An Introduction to the Circular Economy 1536192333, 9781536192339

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ECONOMIC ISSUES, PROBLEMS AND PERSPECTIVES

AN INTRODUCTION TO THE CIRCULAR ECONOMY

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ECONOMIC ISSUES, PROBLEMS AND PERSPECTIVES

AN INTRODUCTION TO THE CIRCULAR ECONOMY

PIERFRANCESCO MORGANTI AND

MARIA-BEATRICE COLTELLI EDITORS

Copyright © 2021 by Nova Science Publishers, Inc. All rights reserved. No part of this book may be reproduced, stored in a retrieval system or transmitted in any form or by any means: electronic, electrostatic, magnetic, tape, mechanical photocopying, recording or otherwise without the written permission of the Publisher. We have partnered with Copyright Clearance Center to make it easy for you to obtain permissions to reuse content from this publication. Simply navigate to this publication’s page on Nova’s website and locate the “Get Permission” button below the title description. This button is linked directly to the title’s permission page on copyright.com. Alternatively, you can visit copyright.com and search by title, ISBN, or ISSN. For further questions about using the service on copyright.com, please contact: Copyright Clearance Center Phone: +1-(978) 750-8400 Fax: +1-(978) 750-4470 E-mail: [email protected].

NOTICE TO THE READER The Publisher has taken reasonable care in the preparation of this book, but makes no expressed or implied warranty of any kind and assumes no responsibility for any errors or omissions. No liability is assumed for incidental or consequential damages in connection with or arising out of information contained in this book. The Publisher shall not be liable for any special, consequential, or exemplary damages resulting, in whole or in part, from the readers’ use of, or reliance upon, this material. Any parts of this book based on government reports are so indicated and copyright is claimed for those parts to the extent applicable to compilations of such works. Independent verification should be sought for any data, advice or recommendations contained in this book. In addition, no responsibility is assumed by the Publisher for any injury and/or damage to persons or property arising from any methods, products, instructions, ideas or otherwise contained in this publication. This publication is designed to provide accurate and authoritative information with regard to the subject matter covered herein. It is sold with the clear understanding that the Publisher is not engaged in rendering legal or any other professional services. If legal or any other expert assistance is required, the services of a competent person should be sought. FROM A DECLARATION OF PARTICIPANTS JOINTLY ADOPTED BY A COMMITTEE OF THE AMERICAN BAR ASSOCIATION AND A COMMITTEE OF PUBLISHERS. Additional color graphics may be available in the e-book version of this book.

Library of Congress Cataloging-in-Publication Data Title: An introduction to the circular economy / Pierfrancesco Morganti, (editor) Professor, Academy of History of Health Care Art, Rome, Italy, Maria-Beatrice Coltelli (editor) . Description: Hauppauge : Nova Science Publishers, 2021. | Series: Economic issues, problems and perspectives | Includes bibliographical references and index. | Identifiers: LCCN 2021019482 (print) | LCCN 2021019483 (ebook) | ISBN 9781536192339 (hardcover) | ISBN 9781536196610 (adobe pdf) Subjects: LCSH: Recycling industry. | Sustainable development. | Environmental policy. Classification: LCC HD9975.A2 .I58 2021 (print) | LCC HD9975.A2 (ebook) | DDC 338.4/76284458--dc23 LC record available at https://lccn.loc.gov/2021019482 LC ebook record available at https://lccn.loc.gov/2021019483 ISBN: 978-1-53619-233-9

Published by Nova Science Publishers, Inc. † New York

This book is dedicated to our families.

Moreover, we thank all the professional contributors who helped us to realize this book on circular economy with the important support of the NOVA Sciences's collaborators, fundamental to disseminate a major knowledge on the existing means necessary to fight against the great problem of waste and pollution.

An idea that is developed is more important than an idea that exists only as an idea. Buddha Progress is impossible without change, and those who cannot change their minds cannot change any things. George Bernard Shaw One of the first conditions of happiness is that the link between man and nature shall not be broken. Leo Tolstoy The earth will not continue to offer its harvest, except with faithful stewardship. We cannot say we love land and then take steps to destroy it for use by future generations John Paolo II

CONTENTS Foreword

xi Amilcare Collina

Preface

xv

Part I. Introduction

1

Chapter 1

Life Expectancy in the World and Relative Variables U. Cornelli, M. Recchia, E. Grossi and G. Belcaro

3

Chapter 2

Circular and Green Economy: Which Is the Difference? Pierfrancesco Morganti and Gianluca Morganti

17

Part II. Building Blocks of Circular Economy

41

Chapter 3

Past, Present and Future of Industrial Symbiosis Sophie Hennequin and Daniel Roy

43

Chapter 4

Development of Indicators of Circular Economy and Their Application in Water Management Juan Carlos Leyva-Díaz, Valentín Molina-Moreno, Jorge Sánchez-Molina and Luis Jesús Belmonte-Ureña

Chapter 5

The Present Contribution of Circular Economy to Stimulate Economic Growth in the World L. Marsullo

Chapter 6

Circular Economy for a Healthy Living Environment P. Morganti and G. Tishchenko

Chapter 7

Circular Economy in China Xing-Hua Gao and He Cong-Cong

67

91 97 113

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Contents

Part III. Waste in Circular Economy Chapter 8

Chapter 9

Chapter 10

Chapter 11

Chapter 12

Chapter 13

Circular Economy in the European Union as an Example of Wasteless Processing of Crustacean’s Waste Galina Tishchenko and Pierfrancesco Morganti Circular Economy: Valorization of Waste Plant Biomass to Produce Active Ingredients with Antimicrobial Activity against Human and Plant Pathogens Giovanna Simonetti, Elisa Brasili and Gabriella Pasqua The Circular Economy and Built Environment. Maintenance, Rehabilitation and Adaptive Reuse: Challenging Strategies for Closing Loops Serena Viola, Stefania De Medici and Patrizia Riganti Waste Valuation for Environmental and Health Improvement on Circular Economy View William Michelon, Aline Viancelli, Apolline P. Mass, Daniel Vicente Filipak Vanin, Rafael Dorighello Cadamuro, Paula Rogovski, Aline Frumi Camargo, Charline Bonatto, Fábio Spitza Stefanski, Thamarys Scapini, Gislaine Fongaro and Helen Treichel Waste Recycling from Construction Sector within the Circular Economy Paradigm Álvaro Sánchez-Quintana, Juan Carlos Leyva-Díaz, Jorge Sánchez-Molina and Valentín Molina-Moreno Circular Economy of Wastewater Streams by Means of Membrane Technologies Marco Stoller

Part IV. Reuse, Reduce, Recycle in Circular Economy Chapter 14

Chapter 15

Sustainable Food Production: The Transition towards a Circular Economy of Plastic Food Packaging Pedro Núñez-Cacho, Rody Van der Gun, Juan Carlos Leyva-Díaz and Valentin Molina-Moreno Bioconverter Insects: A Good Example of Circular Economy, the Study Case of Hermetia illucens Rosanna Salvia and Patrizia Falabella

121 123

143

165

183

205

229

241 243

261

Chapter 16

Chitin and Lignin Waste in the Circular Economy Pierfrancesco Morganti, Alessandro Vannozzi, Adnan Memic and Maria-Beatrice Coltelli

281

Chapter 17

The Use of Coffee Waste to Produce Goods and Energy Andrea Morganti and Pierfrancesco Morganti

297

Contents Chapter 18

Chapter 19

Chapter 20

Chapter 21

Chapter 22

Natural Metabolites as Functional Additive of Biopolymers: Experimental Evidence and Industrial Constraint Arash Moeini, Gabriella Santagata, Antonio Evidente and Mario Malinconico Regenerated Cellulose Sheet as Natural Tissue to Make Biodegradable Baby Diapers Alessandro Gagliardini and Pietro Febo Waste Recycling for Wound Care and Cosmetic Smart Economics: Chitin and Lignin Pierfrancesco Morganti, Gianluca Morganti, Alessandra Fusco and Adone Baroni Biobased and Biodegradable Rigid and Flexible Polymeric Packaging Maria-Beatrice Coltelli, Vito Gigante, Patrizia Cinelli, Alessandro Vannozzi, Laura Aliotta and Andrea Lazzeri Reuse and Recycling of Post-Consumer Textile Waste in Smart Green Cities Natalia A. Vukovic

Chapter 23

Circular Economy in the Fashion Sector and Textile Goods Marco Piu and Mauro Rossetti

Chapter 24

Circular Economy in the Built Environment: A Strategy for Flexible Housing through Flexzhouse Mohd Zairul

ix

309

331

341

365

391 405

421

About the Editors

437

List of Contributors

439

Index

445

FOREWORD For a long time, our economy has been "linear". This means that the raw materials are used to make a product which, after use, becomes waste and is thrown away. Several factors - such as the generation of waste, the exposure to economic risks and the availability of resources, the degradation of natural capital, the evolution of regulations indicate that the linear model is increasingly being challenged by the context in which it operates, and that a more in depth change is needed in the operating system of our economy. In this context, the circular growth model, which aims to dissociate economic growth from the consumption of limited resources and make the economic system less vulnerable to crises, is increasingly considered to be the trajectory of development to be followed. The current paradigm of the linear economic model "production, use and disposal" is destined to be replaced by the circular economy model whose paradigm is "reduce, reuse, recycle". The circular economy is a regenerative industrial system. It replaces the concept of end of life with restoration, directs the use of renewable energies, eliminates the use of toxic chemicals that prevent reuse and return to the biosphere and aims to eliminate waste through better design of materials, products, systems and business models. This economy is based on some simple concepts. First, a circular economy aims to eliminate waste. Waste does not exist: the products are designed and optimized for a disassembly and reuse cycle. Secondly, circularity introduces a rigorous differentiation between the consumables and the durable components of a product. Consumer goods in the circular economy are largely made of organic or "nutrient" ingredients that are at least non-toxic and even better beneficial, and can be safely returned to the biosphere, directly or in a cascade of consecutive uses. Durable goods, on the other hand, are made up of technical substances unsuitable for the biosphere, such as metals and most plastics. These are designed from the beginning to ensure the reuse of the product or its components at the end of the primary use cycle. Thirdly, the energy needed to fuel this cycle should be renewable in order to reduce dependence on resources. Ten principles define how the circular economy should work: •

Waste becomes a resource: it is the basic principle. All the biodegradable material returns to nature and the non- biodegradable is reused.

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Amilcare Collina •

• • • • •

•

•

•

Second use: reintroduce into the economic circuit those products that no longer correspond to the initial needs of consumers. Reuse: reuse products or product components to build new manufactured products. Repair: prolong the life of damaged products. Recycling: use materials present in the waste. Enhancement: exploit the energy deriving from waste that cannot be recycled. Energy from renewable sources: elimination of fossil fuels for production, re-use and recycling. Eco-design: considers and integrates environmental impacts throughout its life cycle for a product. Industrial and territorial ecology: optimized management of stocks and flows of materials, energy and services Economy of functionality: new business models

An important starting point is the design of production processes, products and services: the products must be redesigned to be used for a longer time, repaired, modernized, remanufactured or, in the end, recycled, instead of being thrown away; the production processes must be conceived taking into greater account the possibilities of re-use of products and raw materials, as well as the regenerative capacity of natural resources. The diagram below illustrates the model of the circular economy by schematizing the main phases, each of which offers opportunities in terms of cost cutting, less dependence on natural resources, growth and employment, as well as containing waste and environmentally harmful emissions

Foreword

xiii

The phases are interdependent, as the materials can be used in cascade: for example, companies exchange by-products, products are refurbished or remanufactured. To ensure the effectiveness of the system it is necessary to avoid as far as possible that the resources leave the circle. In the logic of the circular economy, the circle closes with the transformation of waste into resources. (Ellen Macarthur Foundation: Towards a Circular Economy- Business Rationale for an accelerated transition) For this purpose the role of both the Scientific Community and the Industry of the chemical sector is crucial for the development of new technologies. The volumes of potentially transformable waste in resources - with the development of appropriate technologies - is huge. I can mention in this regard a report edited by the Research National Agency ENEA (Study on the potential of carbonation of minerals and industrial residues. Report RdS /2010/48) which analyzes the residues potentially suitable to react with carbon dioxide and be transformed into reusable products generated in Italy by a number of industrial sectors. The development of technologies of reaction of these residues with carbon dioxide has a twofold environmental value: • •

Transformation of a waste into a product Massive up-take of carbon dioxide from sources of emissions with reduction of the environmental impact of these sources

The industrial sectors analyzed in the ENEA Report are the following: • • • • • • •

Iron and steel industry; Energy production; Waste-to-energy treatment; Mining; Cement production; Construction and demolition sector; Paper industry.

In conclusion I would like to point out that waste is an issue that affects the whole European Union. According to the European Commission, altogether, the EU produces up to 3 billion tons of waste every year. On average, each of the 500 million people living in the EU throws away around half a ton of household rubbish every year. This is on top of huge amounts of waste generated from activities such as manufacturing (360 million tons) and construction (900 million tons), while water supply and energy production generate another 95 million tons. Turning waste into a resource is a major key to the circular economy. For this purpose, the availability of a rational set of rules concerning the “end of waste” is crucial.

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Amilcare Collina

Amilcare Collina Responsible for relationships with Scientific Community, MAPEI Group; Member of Technical Committee, CONFINDUSTRIA (Association representing Italian manufacturing and services Companies); Member of Research & Innovation Committee, CEFIC (European Chemical Industry Council)

PREFACE According to the United Nations, one third (i.e., 1.3 billion tons) of all the food produced is thrown away annually along its entire supply chain, representing a major contribution to climate change .On the other hand million tonnes of waste plastics, used as containers or packaging materials, are littering on the oceans surface under the form of micro/nanoparticles because of humans’ incivility. These problems represent one of the main problems of our society, who shows to be irrespective of one million of undernourished people and the environmental problems. Thus the necessity of a sustainable development, achieved by a better governance, an intelligent economy and finance, an increased investment in science and technology and a more aware knowledge of manufacturers and costumers for preserving the natural raw materials and the biodiversity of our planet. The adoption of the so-called circular economy seems to be the best way to reduce or eliminate the negative impact of the actual linear economy. By the circular economy, in fact, it would be possible to encourage activities that preserve the value of energy, labour and materials, avoiding the use of non-renewable resources which favor both human health and natural systems. This new economy, in fact, is based on the prevention and management of the waste created, which redesigned, recycled and reused, will preserve the economic value of the natural raw materials. By the new bio-nanotechnologies, in fact, it is possible to curb food and plastic waste pollution, managing it by mechanical and chemical methodologies. However, in the circular economy the increased collection and selection of the different waste materials, their reuse and recycling also to reduce the carbon footprint, remains as a priority. The book is organized in the following four parts: by Part I Introduction, composed by two chapters, many considerations on the humans’ way of living and life expectancy are reported in chapter 1. Life expectancy and the means to provide food and maintain in health all the family has to be considered at the first place, also for the fastest growing of an aged population projected to reach 2.1 billion by 2050. However, while the increase of life expectancy is evident, life span and longevity in different countries is not fully understood, due to the many variables to be taken in consideration. This chapter consider 17 ancillary variables, recorded as routine in relation to the environment, the demography and the economy of 261 countries. The possibility to live longer and healthy, maintaining the natural raw materials and the planet biodiversity, is the main objective of the circular economy, based on the reuse, recycle and regeneration of the raw materials obtained by a virtuous waste management.

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This the topic of chapter 2, which tries to introduce the lecturer to the meaning of the new circular/green economy trying to persuade her/him in the necessity to leave the linear economy. This innovative circular economy will achieve its target only if governance, economy & finance, science & technology, individual & collective activities will integrate one with the other. According to some international organizations, this new economical approach will permit a more sustainable global development, reducing poverty and giving people freedom together within the fundamental rights. Moreover the circular/ green economy, based on the use of the waste and a redesigning of new goods made applying “zero waste” principles with a reduction of water and energy consumption, could maintain the natural raw materials for the future generations, preserving the earth biodiversity. The concept of industrial symbiosis is reported on chapter 3 by the conduction of a full bibliometric analysis based on the published research works. Thus, the principle of an industrial symbiosis to obtain a sustainable development is discussed, comparing the existing parallelism with the natural processes obtainable at zero waste by the use of a minimum of energy and raw materials. While in the biological ecosystems the sustainability is obtained by allowing high flexibility and adaptability of all the productive processes, the circular economy can be seen as a flexible long term strategy system based on a permanently changing environmental/ market/society conditions. Chapter 4, considering the necessity the circular economy has to avoid scarcity in ecosystems, introduces the important theme of water representing one of the greatest challenges of current sustainability policies. According to the United Nations, it has been reported that at least 25% of world population live with water scarcity. Thus, the necessity of new legislation models to reduce the water consumerism for modifying its current management. Moreover, by the new economic rules it will be necessary to use at the best the digital technologies for stimulating the economy growth. At this purpose a drastic change of the people mentality after years of unbridled consumerism is considered of fundamental importance for the incoming circular economy. This the topic focused on chapter 5 and 6 where it is underlined the importance to produce at zero waste for maintaining a healthy living. It is, in fact, to remember that fishery's byproducts and plant biomass represent a golden waste raw material of around 300 billion tonnes per year, utilized until now for less than 20%. Chapter 7, representing the end of this book section, reports interesting news regarding the actual Chinese programs on circular economy. The Chinese government has becoming to push the population to cut the use of not necessary packaging changing the lifestyle to eliminate the food loss also. The chapter underlines that living green is not penance, but rather a way of pursuing happiness and a less stressful way of life. On the other hand, it is underway the transition from coal toward cleaner sources for developing more green energy, so that special experts have been selected to help govern for placing the hazardous chemical industry in key areas, while ramping up efforts to move plants out of densely populated areas. These the papers reported on PART II: Buildings Blocks of Circular Economy, by five chapters. Chapter 8 and 9 are the first two papers of the PART III: Waste in Circular Economy which, organized by six chapters, tries to give an idea on the industrial use of this waste. Chapter 8 is focused on the current trend of the industrial production of chitin, chitosan and their derived compounds. Thus many examples of these polysaccharides have been reported,

Preface

xvii

because of their increased use due to the skin friendly and environmental friendly activity. At this purpose, a view of the EU scientific publications during the last 10 years has been reviewed. On Chapter 9 it has been underlined as plant biomass represents the most important source of phytochemicals, such as antimicrobial agents active against fungal and bacterial pathogens, as well as new smart ingredients used in both pharmaceutical and cosmetic field for their particular effectiveness and safeness. These ingredients result important not only as natural compounds to be used for making innovative drugs and smart cosmetics, but also to reduce agricultural waste converting it into value added metabolites, active against human and plant pathogens. As industrial examples, some ingredients extracted from olive oil waste and fruit juice are reported. Chapters 10-13 are focused on recycling and valorization of different source of waste for obtaining an improvement of human health and the environment. Chapter 10 discusses the attitude towards maintenance, rehabilitation, and adaptive reuse as a strategy to give new life to decaying and abandoned spatial and social contexts. Principles of the circular economy highlight the need to preserve and increase the value of existing assets as both materials and buildings, when applied to the construction sector. Therefore, there is a growing interest in urban mining from buildings, from both environmental and economic perspectives. Thus, materials hidden in buildings are an interesting alternative to raw materials. Chapter 11 underlines that, rethinking the production process, represents an important strategy for industry, energy and agriculture reflecting on human quality of life. Accordingly to the principles of circular economy, materials reuse and recycling encourage technological innovation, new inspirations and research challenges, aiming the development of cleaner technologies and a more healthy environment. Chapter 12 is focused on the necessity to change the way to produce and consume, transforming the current linear economy in the circular economy model, especially for the construction field that became one of the largest producer of waste and greenhouse (GHGs) emissions. Some suggestions, therefore, are reported to reduce waste and GHGs by the use of the design out principle, recycling the construction materials, and utilizing new technologies and material. In Chapter 13 is underlined the valorization of the product stream and the increase of the membrane longevity. The target of a membrane process, for example, is to separate the feed stream in two separate ones, the process stream and the secondary stream, considered as a waste. In any way, the design of the membrane process aims to reach on the target stream the desired quality in terms of purification, concentration, and separation. Thus according to the circular economy, this process has to be modified by innovative technologies to realize recyclable membranes to be reused. Driving toward a circular economy has became a necessity to save the limited natural raw materials of our planet, increase the production of energy generated though renewable resources, and reduce the increasing waste and pollution. Thus the necessity to rethink our economic future through a circular model based on the so called 3R: reuse, reduce and recycle. This the topic of PART IV: Reuse, reduce, recycle in Circular Economy, composed of 11 Chapters. In Chapter 14 the problem of food packaging is reported and discussed, underlining that today it represents the majority of the non-biodegradable materials through out in the environment. Thus the urgent necessity to solve this great problem by the use of materials that can be recycled indefinitely.

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On one hand, it is remembered that the actual food packaging creates undoubtedly significant advantages because the plastic materials used are cheap, durable, with a low weight and a low energy need during manufacturing, and able to maintain fresh the food for a longer period. However, the durability represents an disadvantage because the materials used are not recyclable and have an high cost of recycling. On the other hand, the use of alternative containers made by glass or aluminum result too expensive and increase the GHGs emissions. Therefore, recycling plastic containers seems at moment the best and more economic option to reduce the negative impact of plastic pollution. This solution, in fact, is characterized by the lowest global warming and energy consumption, compared to incineration or disposal in landfills. Chapter 15 reports an innovative application for bio-converting agro-food waste material into valuable products through the insect H. Illucens. This insect may be used to produce animal feed and/or an alternative energy source, according to the circular economy. On the other hand, some derived compounds obtainable from waste materials during the food processing, such as chitin, chitosan and their derived compounds, can find many possible applications in agricultural, biomedical and pharmaceutical fields. Bio-converting the insects, therefore, can offer the capacity to valorizing organic waste from the agro-food industry through specific processes. In conclusion, the breeding of insects for animal feed and as an alternative energy source could represent one of the solutions to be adopted in the future to convert the food waste into goods. As reported, plastic and food waste represent an important pollution problem for humans and the environment, being actually dumped into land and oceans. Thus the necessity to recycle plastics and reuse food extracting its bioactive ingredients, thus considering this waste a business opportunity and richness for a new economy. Among the other possibilities, Chapter 16 is focused on the way to use fishery's byproducts and plant biomass waste to obtain chitin and lignin respectively. These two polymers, obtained in their micro/nano size by a patented process, have been complexed each to other due to the different electrical charges covering its surface: electropositive charge for chitin and electronegative for lignin. They may be used to produce smart non-woven tissues facial masks, or advanced medications, as result of the different active ingredients entrapped into the fibers obtained by the electrospinning methodology. These tissues applied on the skin, in fact, seem able to release the active ingredient at different time, according to the production method adopted. Another source of waste is represented from both spent grounds and non-biodegradable plastic containers of which are made the many coffee consumed worldwide, remaining in the environment as pollution. According to Chapter 17, billion cups of coffee are drinking daily across the world, while the spent ground is throughout as waste. As consequence, this spent powder decomposes, releasing methane and increasing the greenhouse gas (GHGs) emissions in the atmosphere. On the other hand, coffee grounds, rich of many active ingredients, could be used in the pharmaceutical and cosmetic fields as well as in other industrial sectors to make biofuel, for example, or bio fertilizers. Thus the necessity to utilize coffee waste more intelligently and efficiently, making an important contribution to the waste management by innovative technologies and a sustainable strategy according to the circular economy rules, as focused on this chapter. While packaging represents a great waste problem, on the other hand it is necessary to preserve food from the microorganisms damages. The prevention from mold contamination, in fact, is another big problem regarding the food packaging system. Contaminants, as Penicillum Roquefort and Aspergillus Niger, are the main contaminants dangerous for human

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health. Thus the necessity to design right packaging systems to protect food from any physico-chemical and biological damage, preserving its quality and safety. At this purpose Chapter 18 reports the more common polymers currently distributed in the market for food packaging, focusing the attention on the new biological polymeric composites, active for their biodegradable matrices. Cellulose based nanocomposites and regenerated cellulose are other materials used in packaging as alternative to petroleum-based ones. Their increasing utilization not only for food but also to make biodegradable baby diapers, is due to their light weight, durability, and bio recyclability. Regarding the different fiber organization and size, nano-crystals and bacterial cellulose are continually studied because both possess strong reinforcing effects on nanocomposites, having highly favorable properties, including biodegradability, high surface area, low density and good thermo-mechanical performance. Thus, they are becoming to be used for green applications in baby diapers as reported in Chapter 19. Waste recycling of cosmetic products and drugs for both their content and packaging became a problem for the economy, as previously focused. This the topic of chapter 20 were new biodegradable carriers are reported, obtained from waste materials. These innovative vehicles, capable to overcome the skin barrier, are able to transport and deliver active ingredients across its layers because of their nanosize and surface electrical charges. On the other hand, chapter 21 is dedicated to the potentialities and opportunities of biobased and biodegradable polymeric materials available on the market, considering their regulatory and standardization aspects. Among the polymers reported, PLA-based biocomposites seem to represent currently the more promising alternative to the petrol-based ones. Chapter 22 is focused on the utilization, processing, and reuse of textile waste worldwide in modern cities. Its recycling may be considered a promising base for a new Ecobusiness, thus reducing the waste problem and its harmful effects on the environment, according to the aims of circular economy and reported in chapter 23 also. This chapter underlines the necessity to eliminate the use of hazardous chemicals during fabric processing and organize the traceability of the textile raw materials for verifying the absence of toxic compounds, thus permitting the recyclability and protect the consumer health. For living in good health and without waste and pollution it is necessary to change our way of produce and consume food, cosmetics, drugs and all the goods utilize for our actual lifestyle. Thus our house also has to be made by the recyclable materials to be in line with the circular economy. At this purpose the book ends with chapter 24 which reports the use of the so called flexZhouse business model that combines an innovative leasing with elements of the circular economy useful to provide an affordable housing to the customers for ameliorating their lifecycle chain. This new model is based on innovative strategic business useful to reduce cost of manufacturing and production by economies of scale. In conclusion, this book tries to debate on the significance of circular economy, underlying the necessity to change our way of producing, consuming, and traveling on a daily basis. The passage from a linear economy to a circular economy will help us to reduce the degradation of the environment for avoiding future disastrous consequences, such as depletion of biodiversity, scarcity of raw materials and drinking water, rising waters, etc. The circular economy, therefore, involves designing a product so that it can be recycled or its components reused. Thus, reuse consists of the product back into the economic circuit in its

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original condition as well as repair makes it possible to fix a broken good and recovery consists of reusing its components. This is the significance of the so called 3R strategy, illustrated in this book.

Pierfrancesco Morganti Academy of History of Healthcare Art, R&D Unit, Rome, Italy Visiting Professor, China Medical University Maria Beatrice Coltelli Associated Professor, Department Civil and Industrial Engineering, University of Pisa, Italy

PART I. INTRODUCTION

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 1

LIFE EXPECTANCY IN THE WORLD AND RELATIVE VARIABLES U. Cornelli1,*, M. Recchia2, E. Grossi3 and G. Belcaro4 1

2

Loyola University School of Medicine Chicago, US Department of Biostatistics, University of Lugano, Switzerland 3 Villa Santa Maria Institute, Tavernello, Italy 4 Irwin Labs, University of Chieti, Italy

ABSTRACT Life expectancy in every country can be determined by demographic, ecological, and economical variables. Life expectancy (LE) was compared in 191 countries on the basis of 17 demographic and economic variables. A stochastic approach was used consisting of simple correlation coefficients, followed by principal component analysis, factor analysis and - lastly segmentation analysis. The results ruled out 10 of the 17 variables as non-correlated. The surface area covered by forests, the square kilometers of forests, the ratio of gross domestic product (GDP) to education, the number of hospital beds, the particulate matter, the population and the population density were not found to be determinant. What emerged as directly correlated with LE were the Internet, GDPs (GDP/inhab, GDP2 and GDP3, related to advanced industry and the economy respectively), urban concentration, cars and mobile phones. An inverse correlation was found with GDP1 (related to agriculture, livestock and fishing). LE in the world is not connected with the variables typically linked with the environment, and is more closely connected with economic variables.

Keywords: life expectancy, ecology, gross domestic product, segmentation analysis

*

Corresponding Author’s Email: [email protected].

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U. Cornelli, M. Recchia, E. Grossi et al.

INTRODUCTION Before considering the aspects of circular economy and the relative possibility to be implemented one should consider in which context/s the humans are living. The most important objective of the humans is to live, which means to eat and to provide foods for the family. Because of this, life expectancy (LE) can be considered among the most important variables. Humans in general are not oriented to the environment modifications, provided that they can provide to satisfy the energy necessary to survive. This has to be clearly in mind when efforts are undertaken to modify the human behavior. Life expectancy (LE) has been steadily rising in the past two centuries and projected to continue increasing. From the 40 year in 1990 [1, 2] has doubled since the beginning of the 20th century, and in most developed countries now exceeds 80 years in both man and women [3] with an 80% probability that world population will increase to between 9.6 and 12.3 billion in 2100 [4]. LE is increasing in every area of the world and already in 2010 the International Future modelling system (IFs) was calculating values ranging from 73 to 85 years for males, and 80 to 87 years for females [5]. Particular improvements were forecasted for Sub-Saharian Africa, whereas slower improvements were expected in high-income countries. Considering data deriving from The Global Burden Disease Study 2015 the total death increased by 4.1% from 2005 to 2015, but the age standardized death rate fell by 17% [6]. After 2015 many efforts were made by United Nation to achieve a world of prosperity, equity, freedom and peace -according to the Millennium Development Goals- to stimulate the implementation of primary health care. However, the gap between countries is still existing and occurs for different reasons that should by analyzed with details [7]. Indeed, a wide array of disease and injury sequelae affects the world’s population. Globally, in 2013 only 4.3% of the population had no burden of disease or injury sequelae, slightly up from 4.2% in 1990, and the Years Lived with Disability (YLDs) was also increasing [6]. According to these considerations, globally LE at birth is projected to rise from 70 years in the period 2010-2015 to 77 years in 2045-2050 and achieve 83 years in 2095-2100. Africa seems to gain about 19 years of LE by the end of the century. Such increases are contingent on further reductions in the spread of HIV, and combating successfully other infectious as well as non-communicable diseases. Both Asia and Latin America and the Caribbean are expected to gain 13-14 years of LE at birth by 2095-2100, while Europe, Northern America and Oceania are projected to gain 10-11 years. Globally, population aged 60 or over is the fastest growing. Furthermore, as fertility declines and LE rises, the proportion of the population above a certain age rises and this phenomenon - known as population ageing- is occurring throughout the world. In 2015, there were 901 million people aged 60 or over, comprising 12 per cent of the global population. Europe has the largest percentage of its population at ages 60 or over (24 per cent), and the number of older persons in the world is projected to reach 1.4 billion by 2030 and 2.1 billion by 2050. Population ageing will have a profound effect on the number of workers per retiree in various countries, as measured by the Potential Support Ratio (PSR), defined as the number of people aged 20 to 64 divided by the number of people aged 65 or over. Currently, African countries, on average, have 12.9 people aged 20 to 64 for every person aged 65 or over, while Asian countries have PSRs of 8.0, Latin America and the Caribbean

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7.6, Oceania 4.8, Northern America 4.0 and Europe 3.5. Japan, at 2.1, has the lowest PSR in the world, although seven European countries also have PSRs below 3. By 2050, seven Asian countries, 24 European countries, and four countries of Latin America and the Caribbean are expected to have PSRs below 2, underscoring the fiscal and political pressures that many countries are likely to face in the not-too-distant future in relation to their public health care. The increase of LE is undoubtedly evident, however what is not fully understood is why there are so many differences among countries. Life span and longevity are complex variables and belong to the interaction between environmental, genetic, epigenetic, and stochastic factors that can be influenced also by foods and drugs which according to the common knowledge are considered valid factors to live longer. The aim of our study was to consider the LE as a main variable to correlate with 17 ancillary variables that are recorded as routine in most of the countries in relation to the environment, the demography and the economy. The determinants of LE were measured through the stochastic and non-stochastic analysis to discover the existence of common variables. On the basis of these conditions one may consider where (and when) the circular economy can be implemented.

LIST OF THE COUNTRIES All the 261 countries in the world were analyzed, considering the data of two years 2014 and 2015. Countries without some of the variables that were chosen for the analysis were excluded, and because of this the final sample was limited to 191 countries. The LE in each country was taken by the World Health Statistics Monitoring 2016 [8]. Those not reported such as for Montecarlo and San Marino were taken by the CIA World Factbook 2016 [9]. At the end all the data concerning the year 2015 were reported since those of the 2014 were superimposable. The following 191 countries that have been analyzed are presented in terms of descending order for life expectancy. Monaco; Japan; San Marino; Singapore; Andorra; Swiss; Australia; Sweden; Liechtenstein; Canada; France; Norway; Spain; Island; Nederland; New Zealand; Ireland; Germany; United Kingdom; Greece; Austria; Malta; Luxembourg; Belgium; Taiwan; South Korea; Finland; United States; Denmark; Portugal Bahrein; Chile; Qatar; Cyprus; Czech Republic; Panama; Costa Rica; Cuba; Albania; Slovenia; Dominican Republic; Kuwait; Argentina; Santa Lucia; Lebanon; United Emirates; Uruguay; Paraguay; Brunei; Slovakia; Poland; Morocco; Czech republic; Algeria; Ecuador; Sri Lanka; Bosnia and Herzegovina; Antigua Bermuda; Libya; Lithuania; Tonga; Macedonia; Georgia Brazil; Tunisia; Hungary; Mexico; Saint Kits and Nevis; Columbia; Mauritius; Maldives; China; Barbados; Oman; Salomon Islands; Saint Vincent Grenadine; Saudi Arabia; Romania; Malesia; Venezuela; Bulgaria; Seychelles; El Salvador; Thailand; Armenia; Jordan; Estonia; Grenada; Jamaica; Egypt; Latvia; Turkey; Uzbekistan; Peru; Samoa; Vietnam; Nicaragua; Vanuatu; Palau; Marshall Islands; Philippine; Micronesia; Indonesia; Belarus; Fiji Islands; Bahamas; Azerbaijan; Greenland; Guatemala; Suriname; Lebanon; Cape Verde; Iraq; Honduras; Iran; Bangladesh; Kazakhstan; Russia; Moldavia; Kirghizstan; North Korea; Turkmenistan; Ukraine; Bhutan; Mongolia; Bolivia; Belize; Syria; Guyana; India; Timor Est; Nepal; Tajikistan, Pakistan; Papua New Guinea; Burma; Tuvalu; Ghana; Kiribati; Madagascar; Yemen; Gambia; SãoTomè and Principe; Togo; Cambodia; Kenia; Eritrea; Laos; Equatorial Guinea; Comoros; Sudan; Haiti; Djibouti; Mauritania; Tanzania; Benin;

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Senegal; Ethiopia; Malawi; Guinea; Burundi; Republic of Congo; Liberia; Ivory Coast; Sierra Leon; Cameroon; Democratic Republic of Congo; Zimbabwe; Angola; Mali; Burkina Faso; Niger; Uganda; Botswana; Lesotho; Nigeria; Mozambique; Gabon; Namibia; Zambia; Somalia; Central African Republic; Swaziland; Afghanistan; Guinea-Bissau; South Africa; Chad.

THE VARIABLES The following 17 variables were considered taken by CIA World Factbook 2016 [9]: Population: as number of inhabitants Population density: in terms number of subjects/km2 Urb pop: rate (percentage) of urban population in comparison to the total population GDP/inhab: Gross Domestic Product/inhabitants or the total values/inhabitants of goods and final services related to economical activities, capital investments Unempl: unemployment rate (percentage) of people looking for a job in relation to the labor force GDP 1: GPD rate (percentage) of the Gross Domestic Product in relation to primary industry bound to agriculture, forests, livestock, fishing GDP 2: GDP rate (percentage) of the Gross Domestic Product in relation to industry, mining and construction industry GDP 3: GDP rate (percentage) of the Gross Domestic Product in relation to commerce, transportation, communication, tourism, insurance GDP 2+3: sum of the rate (percentage) related to GDP 2+ GDP 3 Education: rate (percentage) of the investments in public and private instruction in relation to GDP HB: number of hospital beds/1000 inhabitants Forests: as rate (percentage) of surface covered by forests PM: particulate matter (PM2.5 and PM10) in mcg/m3 measured in cities with > 100,000 inhabitants Cars: number of cars/1000 inhabitants Cell: number of mobiles/1000 inhabitants Internet: number of people connected to internet/1000 inhabitants Forests Kmq2: square kilometers of forest/1000 inhabitants. LE was considered as the main variable to compare with all the others using two approaches: stochastic and non-stochastic analysis. The first was based on the simple correlations and on the Main Component Analysis (MCA with rotation Verimax), to explain the correlation among the variables [10, 11]. This evaluation was followed by the Factorial Analysis that used “factor scores” to transform the cluster of observations in more simple structures or Factors [12, 13]. The Segmentation analysis was also used [13] on the base of CHAID (Chi square Automatic Interaction Detection). The methods employed for the analysis were the following: correlation matrix among all the variables, considering as limit of significance the value of r ≥ 0.6. The Main Component

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Analysis (MCA) was applied to explain the correlation among the variables as cause of “non observable” or hidden factors [10, 11]. This was followed by the Factorial Analysis that used the “factor scores” to transform the cluster of observations in more simple structures or Factors [12, 13]. Followed the analysis to measure if the LE was correlated to the mutation of any single Factor. After these three steps, only the factor scores capable to explain a consistent percentage of variability (> 80%) will be considered, with the aim of isolating two orthogonal factors, each consisting of a combination of variables, and project the need to define a target variable191 countries on these two new axis. The segmentation analysis is based on the construction of a decisional tree based on CHAID (Chi Square Automatic Interaction Detection). The method needs at first to identify the target variable that in the current case was the LE that ranges between 45 to 85 years. LE was divided into 4 groups of similar dimension (between 45 to 50 countries) and CHAIDS allows the identification of “optimal splits” that consent to maximize the differences among the groups [13]. In a first step the sample was divided into two clusters of countries according to the most solid “predictor”. The best predictor is chosen among the variables that contain 100% of the variance and were isolated with the MCA (in this case 7 variables). The cluster isolated by the first predictor can be further divided on the base of other predictors. The analysis gives back the probability of a given LE based upon the dimension of the predictors. All the calculations were carried out with JMP 12 SAS (Sas Institute inc. e XLSTAT).

RESULTS Here are summarized the data of 2015 because those of 2104 were practically superimposable to 2015. The correlation matrix is reported in Figure 1 and is limited to variables with r value ≥ 0.6. According to the r ≥ 0.6 cut-off, five variables only were found correlated to LE, namely: GDP 1; GDP 3; Cars; GDP 2 + 3; Internet. This last showed the highest r value (r = 0.7697) Vs LE. In the light of this simple analysis, two other aspects were considered. The first was to isolate those variables that were considered “inhert” because they were not correlated with any other variable. These were 10: population, population density, unemployment rate, GDP 2; Instr/GDP, HB, Forests, PM, Cell, Forests Kmq2. The second was to determine how the remaining variables were mutually crossing, as reported in Figure 1.

Figure 1. Variables that are significantly correlate with “r” ≥ 0.6.

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What can be drown is that GDP in all the aspects is either positively (GDP2 and GDP 3) or negatively (GDP 1) correlated with LE, and the other highly interconnected variables are Internet, Cars and GDP3 or GDP 2+3. GDPs are all correlates among them either in positive or negative way. The proposed exploratory Factor Analysis (with rotation Verimax) that was following allowed to explain the correlation between different variables in terms of a reduced number of factors unobservable or latent. This analysis eliminate 10 of the 17 variables because their information was already contained in the remaining 8. The following variables were excluded: population and population density, unemployment, GPD 2 and GPD 3, HB, Instr/GDP, forests, forest Kmq2, and PM. The seven remaining variables instead were capturing 100% of the variance, namely: urb pop; GPD/inhab; GDP 1; Cars; Cell; GDP2+ GDP 3; Internet (see Figure 2).

Figure 2. Weight of the 7 Factors that have been isolated from the initial 17 variables, Eigenvalues, Percentages and Cumulative Percentages.

Where 1 = urb pop; 2 = GDP/inhab; 3= GDP 1; 4 =Cars; 5 = Cell; 6 = GDP 2+ GDP 3; 7 = Internet. The 7 Numbers were explaining 100 of the variance and two of them (see Numbers 1 and 2 in Figure 2) capture as much as 80% of the variance. The Number 1 contains 66.83% of the variance and represents the combination of the following four variables: urban pop, GDP 2+GDP 3, Cell, and GDP 1. The Number 2 contains 12.83% of the variance and is represented by the combination of the following three variables: GDP/inhab, Cars, and Cell. These two Numbers were called Factor 1 and Factor 2 respectively. The correlations with LE of each variable contained in the Factors was calculated and it was possible to determine the importance of every single variable by the “greatness” of the relative coefficient (Figure 3).

Figure 3. Correlations coefficients of Factor 1 and the Factor 2 Vs the original variables composing the Factors. Analysis with rotation Verimax.

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By their "greatness" one may notice that: Factor 1 decreases with GDP 1 (negative coefficient) and increases with increasing GDP 2 + 3, urban pop, and Cell, whereas GDP/inhab and Cars were almost inconsistent; Factor 2 values increase mainly with the growth of GDP/inhab, Cars, Internet. In this last case pop urb, GDP 1, Cell, and GDP 2 + GDP 3 were shown less consistent. Internet correlation is present in both Factors but its weight prevail in Factor 2. Only values > 0.6 were considered consistent. The “greatness” allowed to identify within the two Factors those variables that were better defining the Factor’s characteristics. For Factor 1 they were represented by urban pop, GDP 1, Cell, and GDP 2+ GDP 3, whereas for Factor 2 they were represented by GDP/inhab, Cars, and Internet. A regressive models comparing LE respectively Vs Factor 1 and Factor 2 was calculated, and the results are represented in the following Figures 4 and 5.

Figure 4. LE of 191 countries in relation to Factor 1 (urb pop, GDP 1, Cell, GDP 2+3).

Figure 5. LE of 190 countries in relation to Factor 2 (GDP/inhab, Cars, Internet).

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The regression line marked in the figure represents the growth of LE as a function of Factor 1. For what concern Factor 2, represented by GDP/inhab, Cars and Internet, the regression line and the points disposition are reported in Figure 5. The last step of the analysis was the connection of the two Factors (Figure 6). This is possible because they explain 80% of the variance and may form a “complex” variable to be used for the final correlation. The results were represented in ascending order in Figure 6, consisting of the new regression LE Vs Factor1 + Factor 2. The correlation is statistically significant: r = 0.77 p < 0.001).

Figure 6. LE in relation to the sum of Factor 1 and Factor 2. Factor 1 (urb pop, GDP 1, Cell, GDP 2+3,) + Factor 2 (GDP/inhab, Cars, Internet).

For the Segmentation analysis four classes of LE were considered: 49-64 years, 65-73 years, 73-77 year and finally > 77 years composed respectively by 47, 44, 53, and 47 countries. The CHAID (Chi square Automatic Interaction Detection) was used to determine the best predictors among the seven variables isolated by the Factor analysis with rotation Verimax (see Figure 3). The first predictor hierarchically most important was Internet presenting two cut-off: >436 and 73 years, whereas the second only the 13%. The second predictor was GDP/inhab > 21633 and 21633 that were concentrating respectively 95% and 86% of the countries with LE >73. The third predictor was Car > 360 and 73 and the second the 100%. In other terms, a country characterized by internet > 436, GDP > 21633, and Cars >360 was offering a LE >77 years with 98% of probability. Without taking into consideration the three predictors, the probability of LE > 77 years was 52% only (52/191countries).

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DISCUSSION This is the first time that LE is compared with many variables that are usually employed to define the condition/performance of a country. The weakness of this study belongs to some points that has to be underlined. They are the precision/quality of some variables, such as the PM, unemployment, and urban population. PM in fact was not taken in a standardized way in terms of the period of the year, number of measures, and cities of a given country. Furthermore, they belong to different origin, ranging from inert matter to very toxic substances. In other terms the PM of cities close to the desert cannot be compared to PM of the industrial areas. The unemployment can fluctuate in some country during the year, and the urban population may be modified quite rapidly by the massive immigrations. The urban population can change due to the emigration, since the war exploding in some countries that can suddenly and dramatically modify the characteristics of the closest areas. However, in general most of the variables can be defined as solid, and among the 191 countries the vast majority was stable and free from dramatic events. The first observation emerging from the analysis concerns those variables that were excluded as determinant for the LE and confirmed in all the type of analysis. The classical and common concerns like PM, the Kmq2 of forests or the forests dimension in a given country, the Instr/GDP, were excluded as direct factors that may have impact on LE. For the extent of the forests, the HB and the Instr/GDP one may only take the data as they are, and the reason why they are not emerging as determinants in above the scope of this research. The PM instead can be matter of discussion due to same particular aspect. PM is a complex mixture of chemical components that should be considered together with many gas such as methane (CH4), ozone (O3), carbon monoxide (CO), sulfate (SO3), nitrogen dioxide (NO2) aerosols and all the possible widespread air pollutants, present wherever people live. These particles are able to penetrate deeply into the respiratory tract and therefore constitute a risk for health by increasing mortality from respiratory infections and diseases, lung cancer, and selected cardiovascular diseases. The WHO estimated in 2000 that the exposure to PM caused 800,000 deaths and 6.4 million YLDs and that the developing countries accounted for two third of this burden [14]. In general the WHO stated that there is no evidence of a safe level of exposure to PM or a threshold below which no adverse health effects occur, and globally > 30% of the population lived in areas exceeding the WHO level Target of 35 mcg/m3. The data recorded for this study represent an average of the cities where the monitoring stations were available. In order to present air quality largely representative for human exposure, measurements of residential areas, commercial and mixed areas were used. Stations characterized as particular “hot spots” or exclusively industrial areas were not included. Furthermore, in some of countries particles 436 and GRD/inhab > 21633 have a probability of 89% to reach a LE > 77 years. The probability increases up to 98% in those countries with Cars > 360. The ANN was detecting more information than the stochastic analysis and found more complex relations among variables. The analysis was confirming that Internet is the most important determinant since it is the node more directly connected with LE nodes (high or low). When LE is low, the other node indirectly connected is unemployment, whereas when LE is high the closest node is GDP 3. The other variables that has been isolated with the previous analysis (GDP/inhab, Cars, urban population, GDP 1, GDP 2, GDP 2+ GDP3) seems to have less impact, but still are “indirectly” connected nodes having some influence. In conclusion the two different analysis, stochastic and non-stochastic, are indicating similar variables that are determinant for LE: GDPs, Internet and Cars are emerging in every analysis. There is no simple explanation of why the “classical threats” seems not involved. Apparently, what can be depicted as the heaven on earth, represented by fresh air, forest, lucky solitude, health, knowledge, resources coming from the environment, and finally “unemployment” are not bound to LE. Much more important are resources deriving from a modern way of leaving, no matter if they are carrying also some troubles.

CONCLUSION The life expectancy (LE) in 191 countries was compared on the base of 17 demographic and economic variables. Two approaches were followed: the stochastic and non-stochastic analysis. The results excluded at least 10 out the 17 variables. The surface covered by Forests, the Kmq2 of forests, the ratio of the Domestic Gross Profit (GDP) with education, the number of hospital beds, the particulate matter, the population and the population density were not considered determinant. What was emerging as directly correlated with LE were internet, GDPs (GDP/inhab, and GDP 2 and GDP 3 related respectively to the advance industry and economy), urban concentration, cars and cellphones. An inverse correlation was found with GDP 1 (related to agriculture, livestock, fishing), The conclusion is that LE in the world is far from the variables typically bound to the environment and more linked to the economic variables. At the end a more holistic point of view should be considered: probably Adam and Eve were kicked out from the Paradise not because of an apple, but to give them the chance to live longer.

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It is a matter of fact that circular economy cannot be applied in every country, since it needs to be implemented in those countries where a complex of factors can be modified and generate stereotypes which than can be transferred to the rest of the world, aimed to an evolution and not as a fashion or even worse a revolution.

ACKNOWLEDGMENTS Funding: No funding was requested for this study. Author contributions: UC and GB conceived the study and collected all the data; UC and MR were making the calculation for the stochastic analysis; EG was applying the non stochastic Neuronal Network Analysis (ANN); UC and GB wrote the paper. Competing interests: There are no competing interests. Data and material availability: All the data are available upon request to the corresponding author (in the form of excel files).

REFERENCES [1] [2] [3] [4] [5]

[6]

[7] [8] [9] [10] [11] [12] [13]

Juvin, H. (2010) The coming of the body. London UK: Verso. ISBN 9781844673100. Lutz, W., Sanderson, W., Scherbov, S. (2008). The coming acceleration of global population ageing. Nature 7, 716-719. Gerland, P., Raftery, A.E., Ševciková, H. et al. (2014) World population stabilization unlikely this century. Science 364, 234-237. United Nation World Population Prospect the 2015 revision. Hugues, B.B., Kuhn, R., Peterson, C.M. et al. (2011) Projection of global health outcomes from 2005 to 2060 using the International Future integrated forecasting model. Bull. World Heath Organ. 89, 478-486. GDB 2015 Mortality and Causes of Death Collaborators. Global, regional, and national LE, all-cause mortality, and cause-specific mortality for 249 causes of death, 19802015: A systematic analysis for the Global Burden of Disease Study 2015. Lancet 388, 1549-1544 (2016). Laaser, U., Brandt, H. Global health in the 21st century. Global Health Action 7, 23694 (2014) http://dx.doi.org/103402/gha.v723694. WHO- Global Health Observatory [GHO)] (2016). The CIA World Factbook 2016. Central Intelligence Agency. Dillon, W., and Goldstein, M. (1984) Multivariate Analysis-Methods and Applications. John Wiley. NY, NY. Cureton, E.E. and D’Agostino R.B. (1983) Factor Analysis- An Applied Approach. Lawrence Erlbaum Associates. Hillsdale, New Jersey. Jae-On, K., Mueller, C.W. (1978) Introduction to factor Analysis. Beverly Hills: Sage. Fabbris, L. (1997) Statistica Multivariata McGraw-Hill Libri Italia.

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[14] Cohen, A.J., Anderson, H.R., Ostro, B. et al. Comparative of Health Risks: Global and Regional Burden of Disease Attributable to Selected Major Risk Factors. 1st ed. Vol. Vol.2. World Health Organization Geneva 2004 p. 1353-1453. [15] Brauer, M., Amann, M., Burnett, R.T. et al. (2012) Exposure assessment for estimation of the global burden of disease attributable to outdoor pollution. Environ. Sci. Technol. 46, 652-660. [16] Lippmann, M., Chen, L.C., Gordon, T. et al. (2013) National Particle Component Toxicity (NPACT) initiative: integrated epidemiologic and toxicologic studies of the health effects of particulate matter component. Res. Rep. Health Eff. Inst. 177, 5-13. [17] Crouse, D.L., Peters, P.A., Brook, J.R. et al. (2015) Ambient PM2.5, O3, and NO2 exposures and associations with Mortality over 16 years of follow-up in the Canadian Census Health and Environment cohort (CanChec). Environmental Health Perspectives 123, 1180-1186. [18] Baccarelli, A.A., Hales, N., Burnett, R.T. et al. (2016) Particulate air pollution, exceptional aging, and rate of centenarians: a nationwide analysis of the United States, 1980- 2010. Environ. Health Perspect. 124: 1744-1750. [19] Henschel, S., Atkinson, R., Zeka, A. et al. (2012). Air pollution and their impact on public health. Int. J. Public Healt 57: 757-768. [20] Adams, K., Greenbaum, D.S., Shaikh, R. et al. (2015) Particulate matter components, sources, and health: systematic approaches to testing effects. J. Air Waste Assoc 65, 544-558. [21] WHO 2016 May. World Health Assembly closes, passing resolution on air pollution and epilepsy, Enviro. [22] WHO- WHO’s Urban Ambient Air Pollution database- Update 2016. [23] Seto, K., Güneralp, B., Hutyra, L.R. (2012) Global forecast of urban expansion to 2030 and direct impacts on biodiversity. PNAS 109, 16083-16088. [24] UN News Centre March 2013. [25] DH Deccan Herald 25 January 2017. [26] Lynn, J. Mobile phones help lift poor out of the poverty: UN study News Centre March October 14 2010.

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 2

CIRCULAR AND GREEN ECONOMY: WHICH IS THE DIFFERENCE? Pierfrancesco Morganti1,2, and Gianluca Morganti3 1

Academy of History of Health Care Art, Rome, Italy 2 China Medical University, Shenyang, China 3 ISCD R&D Nanoscience Center, Rome, Italy

ABSTRACT In the billion year of earth history all the planet' living organisms functioned by natural equilibrate cycles based of a thermodynamic autonomy and interchanging energy and matter with their environment. Energy is neither created nor destroyed, but it is transformed: it is always constant. Nature doesn't produce significant amount of waste that is impossible or very difficult to decompose or lay out for many years. Only humans create wastage materials! Human ecosystems, in fact, being unbalanced are producing a high quantity of municipal and industrial waste that became day by day a tough managing problem. The majority of waste is represented first of all from food lost and nonrecyclable plastics invading lands and oceans in addition to yard trimmings and electronics. Thus, the so called 3Rs, such as the reduction, recycling and reuse of each product help to cut down the amount of waste we throw away, saving money and land, according to the green circular economy. This means a new way of operating and living not only the industrial mode of production, but also the lifestyle and, therefore, the way by which consumers use food and goods. The paper tries to persuade the readers in the necessity to leave the linear economy which can be briefly described as the modality to produce and use products which release in the environment waste and dangerous pollution. On the contrary, the circular economy considers waste a source useful to produce new manufacturing goods or to update what was previously used. According to some international organizations, this new approach will permit a more sustainable global development reducing people living in poverty and giving them the "currently denied fundamental rights and freedom." Moreover, it will strengthen the general well-being,



Corresponding Author’s Email: [email protected].

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Pierfrancesco Morganti and Gianluca Morganti promoting sustainable urban and peri-urban development and preserving natural raw materials, environment and the earth biodiversity for the future generations.

Keywords: circular economy, green economy, recycling, waste, pollution, sustainability, environment, food systems, innovation, green cities

INTRODUCTION In natural ecosystems the flow of materials and energy are perfectly and strictly regulated to guarantee the planet species’ evolution without production of waste. For 4.5 million years the Earth functioned by a circular principle based on the natural cycles according to the well known saying attributed to Lavoisier, "nothing is lost, nothing is created and everything is transformed." Contrariwise, in human ecosystems this equilibrium has been disrupted and both production and consumption leaves a huge variety of increasing waste which invades the environment by toxic materials. Thus, the necessity to organize a more sustainable development for guaranteeing preservation of the natural ecosystems for the future generations [1]. This result would be obtained by the 3R principles of circular economy (reduce, reuse, recycle) reported also as 5R (by the inclusion of remanufacture and repurpose) or 9R as reported in Figure 1 [2, 3].

Figure 1. Linear Economy versus the 9R Circular Economy (by the courtesy of UN).

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All these principles, enabling to increase the product level efficiency, reduce waste generation, safeguarding the natural raw material. Also if through different school of thought, the circular economy is a restorative and regenerative industrial system, where products and processes are redesigned to maximize the value of resources with the aim and hope to decouple economic growth in few years (Figure 2) [3-5].

Figure 2. Circular Economy as a regenerative system (by courtesy of Ellen MacArthur Foundation [5]).

Thus, according to the United Nations Environment program [4], it has been estimated that, by this new way of producing and living, the yearly greenhouse gas (GHG) emissions could be reduced between 79% and 99%. Moreover, it has been supposed that the valueretention processes (VRPs) of circular economy could create new demand and opportunity for skilled labor, favoring and improving all the industrial sectors [4]. The VRPs, in fact, based on remanufacturing, refurbishing, reusing and repairing each product, enables its retention value, creating new value for both the producer and customer, at a reduced environmental impact. "Companies, therefore can unlock the substantial benefits of VRPs through a combination of product redesign, developing performance such as based business models, scaling-up reverse-logistics and collaboration across sectors and along the value chains" [4]. As a consequence, the adoption of VRPs would reduce the new material input requirements together with the embody material energy and emissions. These new methodologies would reduce the energy needs in the production processes, cutting the consequential production waste. Moreover VRPs, creating jobs and offset labor costs, could also increase the

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opportunity of exportation. It has been estimated, for example, that "resource efficiency improvements all along the value chains could reduce material inputs from 17% to 24% by 2030, while a better use of resources could represent for European industry an overall saving potential of €630 billion per year" [2]. In addition to overcoming the market barriers, waste prevention, eco-design, reuse, and recycle could bring a European business net savings of € 600 billion.

LINEAR AND CIRCULAR ECONOMY Which the difference between linear and circular economy? In the linear economy the only source of value is the product and the profit is determined by the difference between the product' final market price and the production cost. Thus, to increase profit, companies try to sell as much as possible, reducing all the productive and distributive' chain costs. The innovation is used only to stimulate costumer for buying new products. In fact, to repair the old ones isdifficult and time and money consuming! The consequence is the production of waste without limits! On the contrary, by the circular economy the producer has to guarantee not only the product longevity, but also its reusing, repairing possibility, with the final recycling. So doing, the safeguard of economic and environmental resources with the consequential social benefits, will be increased (Figure 3).

Figure 3. Linear economy versus circular economy with the relative benefits (by the courtesy of EU [8]).

Naturally, to repair, reuse, restructure and regenerate the final product, a correct ecodesign project is required, guaranteeing its post-use circularity also [6]. At this purpose, "the global community has to work collectively and individually to serve societal needs... at the best," to transform the actual linear economy to the circular ones [6]. The circular green economy requires, in fact, fundamental changes in the production-consumption systems such as a better food use, people mobility and energy consumption and housing. For such transition profound changes in "dominant institutions practices, technologies, policies, lifestyles and thinking" are believed necessary [7-9]. At this purpose, the European 7th

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Environment Action program has given "appropriate signals to producers and consumers for promoting resource efficiency" [8, 9] and changing the lifestyle system by the circular economy, with the aim to achieve the 2050 vision of "living well within the limits of our planet" [7-9]. As a consequence, the circular economy would certainly provide positive effects on actual waste/pollution, reducing the GHG emissions, balancing land recycling and ameliorating urban development and infrastructure, as well as to bettering place-based management, water consume and green energy. However, it is not to be forgotten the important role of forests and green cities, because plants consume daily the dangerous carbon oxide, emitting into the air the precious oxygen, indispensable for human living. Reforesting and making the cities greener, therefore, are other important objectives of the circular economy. A sustainable development and better social-ecological systems, in fact, have to "meet the needs of current generations without compromising the ability of future generations to meet their needs" [2, 3]. Unfortunately, both level of air pollution and releases of nutrients from agriculture and wastewater remain too high, causing acidification and eutrophication in ecosystems, so that the global climate continue to change with loss in the planet biodiversity. Currently the most important impact of air pollution in the environment and biodiversity is, in fact, eutrophication caused by airborne nitrogen deposition to ecosystems, as well as the use of chemical fertilizers in cropland and the incorrect pastures. However according to the new rules adopted by the circular economy, the nitrogen oxide emissions decreased in Europe by approximately 42% between 2000 and 2016 [10]. On the other hand due to the worldwide crisis further raised by the COVID-19 pandemic, the economic growth is slowing worldwide, eroding also food production and security. As a consequence social inequality and poverty are notably increasing, contributing to the 25 per cent of diseases and deaths, attributable to environmental causes [7, 8]. Thus, increasing the resource efficiency and enhancing the ecosystem resilience by the circular economy is considered essential to sustain the socioeconomic progress in a world of finite resources.

Food and Plastic Waste Municipal waste, food and plastic production and consume, solid waste collection represents one of the major problems of urban and rural areas worldwide, first of all, due to the recovered heterogeneous material (Figure 4) [11]. Its management, in fact, requires solutions financially sustainable, technically feasible, socially and legally acceptable and environmentally friendly [12]. Regarding both waste produced and recycled, the major problem to solve is the high quantity of food lost and the different types of non-recyclable plastics wich, especially used as packaging, represents for humans and animals the more dangerous pollutant accumulating in the environment. Just to better understand the problem, roughly one-third of the edible parts of food produced for human consumption is globally lost during its supply chain, representing about 1.3 billion ton per year i.e., 95-115 kg/ year/pro capita in EU and USA and 6/11kg/year in sub-Saharian Africa and South/Southeast Asia.[13]. This not eaten food not only is lost as aliment, while hundreds of millions of people remain undernourished, but produces also a carbon footprint

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that, estimated to 3.3 Gigatonnes of CO2, represents the third top emitter after USA and China (Figure 5). This wastage is, therefore, also a great economical loss for the global economy, estimated in US$ 680 billion in industrialized countries and US$ 310 billion in developing countries. Regarding production and consume of non-biodegradable plastics the problem of their eventual recycling and reusing is more complex and difficult to solve because the living micro-organisms of both animals and environment haven't the enzymes for catabolize these synthetic polymers. Moreover, the majority of the plastic containers are often realized by different types of polymers, impossible to separate each other and to recycle. As a consequence, "95% of plastic packaging material for a value or US$ 80-120 billion/year is lost to the economy, after a short first use" [14]. However, 72% of this plastic material is not recovered at all: 40% is landfilled and 32% is often illegally dumped or mismanaged as the reported overview in Figure 6 [14, 15]. It has been estimated also that at least 5.25 trillion individual plastic particles (i.e., ~269,000 tons) are floating on or near the ocean's surface, remaining in land and oceans as dangerous pollutants. Moreover, plastics without being littered, release in land and water toxic compounds used in their manufacture, such as bisphenols and phthalates, acting as disrupted of endocrine system in terrestrial, aquatic animals and humans [16]. Thus, given the prohibitive cost to remove this particular waste, the solution is focused on preventing its improper disposal, limiting its use or, alternatively producing and using biodegradable bioplastics. However, the reuse and recycling of both food, plastics and their relative waste materials has become a must for our society.

Figure 4. Waste materials ~50 of which is represented from trimmings, food and plastics (by courtesy of UNEP [11]).

Circular and Green Economy: Which Is the Difference?

Figure 5. Food loss is China and the third GHG emissions emitter after USA (by courtesy of World Resources Institute).

Figure 6. Total plastic production and waste (by courtesy of Ellen MacArthur Foundation [5]).

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CIRCULAR AND GREEN ECONOMY Which is the difference between circular economy and green economy? According to the European Environmental Agency (EEA) [8, 9], the circular economy represents the greatest part of the green economy, which fundamentally deals with the human welfare. On the one hand, circular economy refers to an industrial model based on waste management, waste prevention and resource efficiency (Figure 7) [17].

Figure 7. Circular economy versus green economy (by the courtesy of EU [8]).

Reuse, recycle, and regeneration of the raw materials obtained by waste is, therefore, the main objective to achieve, alternatively their extraction from natural products. On the other hand, as previously reported, the green economy has the objective to preserve the natural raw materials but is also focused on an extensive and inclusive human well-being able to preserve the planet' natural capital and natural ecosystems generating increasing prosperity. Thus according to UNEP [18], the green economy can be defined as an evolving economic system based on the production, distribution of goods and services for obtaining human well-being and social equity in the long period, while environmental risks and ecological scarcities are significantly reduced for the future generations, safeguarding the planet ecosystems. Adopting these new rules between 2000 and 2017, the EU resource productivity (i.e., economic output per unit of material used) has been increased by 39% with declined consumption of fossil fuels by 21%, forecasting to further increase by 14% between 2014 and 2030 (Figure 8) [19]. Improvements in resource efficiency, therefore, resulted in a lower consumption of materials, a better economic development and a global increased competitiveness, fundamentally obtained by investments in innovation [20]. The improvement of productivity, in fact, is necessary to increase competitiveness and secure access to raw materials and energy, with a contemporary lowering pressure on the environment by the use of waste materials. About the resource productivity by country, Switzerland in EU has the top position followed by Netherland, UK, Luxembourg and Italy pollution and GHG emissions [20].

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Figure 8. EU resource productivity and domestic material consumption 2000-2017 (by courtesy of EU [8]).

Pollution and GHG Emissions However, according to the 2018 Environmental indicator report, while the EU's natural capital is not jet being protected, some resource efficiency improvements has been obtained. Unfortunately, the overall environmental impact of production and consumption has been not sufficiently reduced. Thus, while the global emissions of air and water pollutants have been substantially reduced, in EU's urban areas persist air and noise pollution with the chronic exposure of the population to complex mixture of chemicals, such as nitrogen dioxides, dust particles, ozone and nitrogen [21]. At this purpose, it is to remember that 75% of the natural resource consumption occurs in cities which produce 50% of the global waste and 60-80% of GHG emissions. As a consequence, EU air pollution is estimated to cause 400,000 premature deaths per year [22]. Cities are therefore the major cause of resource depletion, environmental degradation and climate change so that, "emissions in air are the major concern worldwide due to its direct consequence on human health" [22]. Unfortunately and probably for these reasons, the total GHG emissions and energy consumption in EU households increased while nitrogen losses from agricultural land did not decreased further between 2010 and 2014,as for prevision of the EU Programs. These results may be accounted for the different performances registered between Member States for promoting waste management and recycling [22]. Only six Members, for example, have effectively eliminated landfilling of municipal waste, reducing it from 90% to less than 5% in the past 20 years, reaching recycling rate of 85%,while in the others over 90% of waste is still landfilled and less than 5%recycled [22, 23]. However, the overall rate of EU recycling (material recycling, composting and digestion) increased from 31% in 2004 to 45% in 2016 (Figure 9) [22, 23]. Thus, the necessity to rethink the key actual urban systems such as a new way to make buildings and live the cities mobility by introducing, for example, a greener innovative circular economy is still exists. The Social Challenge of the EU Work Program for 2018-2020 is, therefore, focused on the realization of a greener and more efficient economy in agreement with and supporting the UN's Sustainable Development Goals and the targets of the COP21

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Paris Agreement (www.unfccc.int/paris_agreement/item/9485.phpa) [22, 23]. It has been estimated, in fact, that improving the efficiency along the whole value chain could reduce need for material inputs by 17-24% by 2030, representing an overall savings potential of € 630 billion per year for the European manufacturing industry [22, 23, 24]. Thus the new EU work program, therefore, is based on six priorities: (a) Climate action in support of the Paris Agreement; (b) circular economy; (c) raw materials; (d) water, economy and society (e); innovation cities; (f) protection of cultural assets value. In addition, specific attention is paid to climate change and cooperation with key international partners [22].

Figure 9. Proportion of municipal waste treated by different methods in EU (By courtesy of EEA [14]).

CIRCULAR ECONOMY AND INNOVATION It is interesting to underline that by the circular-green economy all the scientists are trying to solve the same problems which were at the base of the Club of Rome's project, the ideas and proposals of which were published on 1972 by a booklet: The limits to Growth [25]. By the project of this restrict group of 70 multidisciplinary scientists, coming from twenty five Countries and gathered in the year 1968 in the Accademia dei Lincei in Rome, were established the first cyclical economic models. In that occasion it was examined and tried to solve "the complex of problems troubling men of all nations : poverty in the midst of plenty; degradation of the environment; loss of faith in institutions; alienation of youth; rejection of traditional values; inflation and other monetary disruptions." Unfortunately the today problems are still the same world-wide! The hope is the possibility to start solving them by the Circular-green economy representing nevertheless only 9.1% of the global world economy, after 40 years from Rome's club! [6]. However, apart the different economic and ecological perspectives, reported by many popular and scientific papers and scholarly studies on the circular-green economy, its realization is considered fundamental for the majority of

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scientists to preserve the integrity of our Planet. The majority of ideas and proposals to achieve the target of a sustainable green economy have been based on seven key elements [6]: (a) Prioritize Regenerative Resources; (b) Preserve and Extend What's Already Made; (c) Use Waste as Resource; (d) Rethink the Business Model; (e) Design for the Future; (f) Incorporate Digital Technology; and (g) Collaborate to Create Joint Value (Figure 10) [6].

Figure 10. The seven key elements of the Green-Circular economy [by the courtesy of circleeconomy.com).

Figure 11. Four pillars of sustainability (by the courtesy of Anne Taufen Wessels [27]).

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With the many difficulties to overcome and without claiming to offer a definitive solution, these new models of thinking and operating can help us to realize the circular-green economy whilst safeguarding the economic development and preserving both natural capital and the limited amounts of raw materials of the planet. However, it is to underline that vision and objectives of this innovative economy are not based to slow down the current economic growth nor to diminish the benefits for the end users. On the contrary, it is to be considered a process of innovation, transformation of business models, and resources saving, based on the worldwide collaborations by new ideas and innovation between industries and customers [26]. It is, therefore, a new virtuous economic mean able to preserve natural capital, pursuing economic growth by the four pillars of sustainability (Figure 11) [27].

Waste Recycling and Research Despite the higher GDP of both USA and EU estimated about US$ 14 trillion and US$ 16 trillion respectively and depending almost entirely from fossil fuels, new rules are fortunately in progress and at the center of the international debate to build more sustainable economies [28], as previously reported. An example of these debates may be the meeting of the United Nations University held in Maastricht, Holland, on July 2018, where researchers, policymakers and students of UN and university discussed on the Science, Innovation, Technology and Engagement as the sustainable pillar goals of Circular Economy (Figure 12) [29].

Figure 12. The goals of the sustainable development discussed in Maastricht (by the courtesy of Armani SV [29]).

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Figure 13. Skyscrapers in Milano (Italy) made according to the circular economy approach.

To achieve the goal of a green economy possibly at zero waste, in fact, it seems necessary not only to completely innovate the industrial production and distribution chains, but also to increase, by school and mass media, education and training for a better understanding of the sustainability's significance and purposes Research and Knowledge, in fact, lead to intensify and bettering both production processes and services, helping countries to complete and integrate them into the global marketplace [22]. Thus for example, a major use of the socalled white biotechnology, based on the support of enzymes and micro-organisms, would be able to improve the industrial processes for creating products with novel-value-added, generating little or no waste [30]. At this purpose, the European Research Council [22] are supporting fundamental research studies through investments of € 650 million under Horizon 2020 and € 5.5 billion under the Structural Funds, in order to address the transition from a linear to a circular economy. Among the target to achieve the provisional results, there is the necessity to boost, reuse, and recycling municipal waste to a minimum of 65% and increase the recycling rate for packaging waste to 75% by 2030 [22]. The respective goals will be a binding landfill reduction of 10% by 2030 and a further development of markets for the obtained high quality secondary raw materials, useful to increase the business confidence. However, many of the EU measures have the aim to promote reparability, durability of products, along with energy efficiency, to boost use of organic and waste-based natural fertilizers and support both role of bio-nutrients and wastewater reuse. Additionally, it is to underline the strategy on plastics addressed to its recyclability and biodegradability, by the use of biodegradable polymers and the elimination of hazardous substances from the productive process to obtain a sustainable development with the goal to significantly reduce and possibly eliminate the marine littering [12, 14, 15]. All these innovative processes will help to decarbonize industry, making it more efficient and sustainable, thus boosting the European competitiveness. As examples of the EU Research studies done and in loges, it is to

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remember, for example, the Lipid project which developed innovative materials harnessing the sun's power to clean up air and water; the Eco2Co2 project which developed a low cost method to turn carbon dioxide into fine chemicals for products such as perfume or flavorings, ProSum which developed secondary raw materials from building mine waste and BAMB projects that reports pilot projects for more green and smart cities (Figure 13) [31] or nChitopack and PolyBioSkin projects which realized respectively, transparent, bacteriostatic and compostable films for food packaging [32] or surgical and beauty masks (Figure 14) [34] and hard containers (Figure 15) [33] for medical and cosmetic purpose, all produced by the use of chitin nanofibrils and nano-lignin and other polysaccharide polymers obtained from waste biomass [35, 36].

Figure 14. Biodegradable Film (on top) and non-woven tissue made according to the Circular economy approach (by the courtesy of Morganti et al. [32]).

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Figure 15. Hard and soft containers made according to the circular approach (By the courtesy of Cinelli et al. [33]).

CONCLUSION As previously amply focused, circular-green economy represents the actual hope to achieve more sustainable productive processes and a novel way of living, to generate increasing prosperity, maintaining the natural raw materials and biodiversity of our planet (Figure 16).

Figure 16. The Green Economy and circular economy approach(by courtesy of EC [31]).

This novel economical concept requires an interactive and multi-disciplinary approach, involving experts in material, mechanical and biomedical engineering, molecular cell biology, in architecture, bioethics, regulatory affairs, business administration, commercialization and marketing, and naturally in new economic systems. However, at the base of the circular-green economy there is first of all the necessity to involve, bio-nanotechnologies and digital technologies to develop, use and store the relative industrial processes. On the one hand,

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nano-biotechnology as the convergence of engineering and molecular biology, is the branch of nanotechnology applied by biological structures and biochemical means [37, 38]. On the other hand digital technology is an electronic discipline that has risen to be an important" critical determinant of economic growth, national, security, and international competitiveness... having also a profound influence on the world's societal wellbeing" [39, 40]. For these reasons, the electronic technology also plays an important role in the transition towards the Circular-green Economy. In fact, bio-nanotechnology and digital technology deal with the possibility of engineering molecular assemblers or tools which could recorder matter on a molecular or atomic scale, mimicking the natural systems [37, 38]. By these novel techniques, therefore, it may be possible to realize the circular-green economy, utilizing the great advancements in molecular biosciences and biotechnology obtained during the last twenty years. All the methodologies, necessary to recycle products or to made them by waste agro-forestry biomass or industrial by-products, in fact, are based on environmental friendly biodegradation processes, delivered from the molecular biology and the relative biotechnological systems [35, 36]. Thus, waste materials could be drastically reduced, if used on a global scale by bio-based production, as reported by the circular bio-economy. As a consequence supply and value chains have the opportunity to be developed more locally, instead to be originated at the sources of fossil feedstocks with subsequent transportation across oceans and lands, to reduce energy consumption and CO2 emissions [22, 31]. However, as bio-based production is often still more expensive than fossil-based ones, a new generation of R&D companies and research laboratories are necessary to create jobs much closer to biomass feedstocks. As a consequence, new skill workers, specialized technicians and bio-based experts will be required on a large scale from school and university, involving also the political class to take the right decisions through interventions and regulatory initiatives of public acceptance. As has been previously reported, in fact, education and training result "increasingly important in a globalized and knowledge driven economy, where a skilled work force is necessary to complete in terms of productivity, quality, and innovation" [23-28]. Additionally, key stakeholders, workers, mass media and consumers need to be involved in the transition from the linear to the circular bio-economy [22, 31]. They have to better understand the necessity to change the way of producing, consuming, living and thinking for maintaining the natural raw materials for the incoming generations, respecting the planet biodiversity also. A clear reply showing the necessity of a more strict collaboration among industries, consumers and politicians may be given looking to the actual production and use of plastics and bio-plastics. Depending on the consumers demand, in fact, the global plastics size was evaluated US$ 522.66 billion in 2017 expanding at a mean CAGR of ~ 4% and expected to reach US$ 721.14 billion by 2025 [41]. About half of this plastic material is used for packaging purpose with a very low percentage of recycling (Figure 17) [42]. However, its ubiquitous use, such as consumer packaging, healthcare, textiles, food, beverages, etc. has been contributing to the generation of a huge volume of plastic waste with the greatest production of polyethylene as main plastic component (Figure 18) [42].

Circular and Green Economy: Which Is the Difference?

Figure 17. Plastic packaging polymer, its use and relative percentage of recycling (by courtesy of Lemonick [42].

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Figure 18. Global Plastic Packaging 2014-2020 (by courtesy of Zion Research Analysis [43].

In term of location most of the plastic material manufacturers are located in the AsiaPacific region (Figure 19).

Figure 19. Locations of the plastic manufacturers by region (by courtesy of Plastics Europe-Worldwide Institute).

On the other hand the global bioplastic market was evaluated US$ 21.126 million in 2017, and is projected to reach US$ 68.577 million by 2024 with a provisional CARG of~ 30% to 2030 (Figure 20) [43-45] with the major increase in Europe especially due to the adopted and adopting new rules and the changing way of living of consumers.

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Figure 20. Global plastic market versus bioplastic.

However, on the one hand, as reported from OECD[46],the green growth, supported by the development of circular/bioeconomy policies and research (Figure 21), is fostering development, ensuring resources and environmental services on which our well-being relies.

Figure 21. Investments in R&D during the period 2000-2015 (by courtesy of Henry-Nickie et al. [39] and National Science Foundation [40]).

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On the other end the necessity for a better balance between upstream R&D that would be more laboratory based, and downstream research activities that need to create an industrial ecosystem, without creating overlaps and duplication. Thus, all productive bioprocesses and energy policies would be standardized around the world, together with better control over existing practices of illegal trade in important secondary raw materials flows. In conclusion, "the conservative use of the worldwide available resources is a key challenge for business, politics, and society" as well as a novel way for "expanding economic growth to emerging and developing countries." So doing the worldwide poverty will be reduced by the use of a global sustainable development, an increase of R&D innovation, and a change of the citizens' domestic expenditures [22-32, 40, 46]. This the common objectives of EU, OECD, and UN which are based on the actual policy of six key entry points: human wellbeing and capabilities; sustainable and just economies; food systems and nutrition patterns; energy decarbonization and universal access; urban and peri-urban development and global environmental commons (Figure 22) [31, 46, 47].

Figure 22. The 6 fundamental points of a sustainable development (by the courtesy of UN [42]).

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To meet these targets, governance, economy & finance, science & technology, individual & collective action have to deploy all together. The Circular-Green Economy is going on this direction.

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[16] NIH, Endocrine Disruptors, 2019, National Institute of Environmental Health Scieces, Health & Education, Durham NC USA www.niehs.nih.gov> agents (accessed October 20, 2019). [17] SOER (2015) Green economy: Sustainability transitions, European Environment Information and Observation, Copenhagen, Denmark, may 2015. [18] Fedrigo-Fazio, D. and Ten Brink, P. (2011) Green Economy, UNEP, Nairobi, Kenya. [email protected]. [19] Eurostat: Eurostat regional yearbook 2015, Luxeburg Publications Office of the European Union, 2015 ISBN 978-92-79/49273-0. [20] OECD. (2015) Material resources, productivity and environment. Green Growth Studies, OECD Publishing, Paris, France. [21] EEA (2017) Environmental indicator report 2018. In support to the monitoring of the Seventh Environment Action Programme, Luxemburg. [22] European Commission (2019) Horizon 2020-Work Programme 2018-2020 Climate action, Environment, resource efficiency and raw materials, Brussels, Belgium, 2 July 2019. [23] Ecosense (2012) Resource Efficiency Challenge. Opinions, Examples and Management Tools. eco sense-Forum for Sustainable Development of German Business, Berlin, Germany. [email protected]. [24] Cambridge Econometrics (2014) Modelling the economic and environmental impacts of change opinion raw material consumption. Technical report 2014-2478. Publications Of-fice of the European Union, Luxemburg. [25] Meadows, D. H., Meadows, D. L., Randers, J. and Behrens III W. W. (1972) The limits to Growth, Universe Books, New York, USA. [26] Institut Montaigne (2016) The circular economy: reconciling economic growth with the environment, 2016, Policy Paper, Institut MOINTAGNE, November 2017, Paris, France. www.istitutmointagne.org. [27] Taufen Wessels, A. (2014) Urban Blue Space and "The Project of the Century": Doing Justice on the Seattle Waterfront and for Local Residents, Buildings 4:764-784 doi: 10.3390/buildings4040764. [28] Thistle Praxis, Beyond GDP: The Making of a Sustainable Economy, Medium, May 26, 2017. https://medium.com/@ThistlePraxis/beyond-gdp-the-making-of-a-sustainableeconomy-f6206d547e6c (Accessed October 21, 2019). [29] Ramani, S. V. (2018) Knowledge Sharing for Urban Sustainability and Catching up to a Circular Economy, 2018, UNU-MERIT University Conference, Maastrict, Holland, June 2018 www.merit.unu.edu/how-to-pin-down-and-drive-the-cut. [30] EuropaBio, Industrial or White Biotechnology. Research for Europe, 2019, EuropaBio, Brussels, Belgium.www.bio-economy.net (Accessed on October 25th 2019). [31] EC: Circular Economy Research and Innovation-connecting economic & Environmental gains, 2017. European Commission, Directorate-General for Research and Innovation, Brussels, Belgium August 2017. [32] Morganti, P., Tishchenko, G., Palombo, M., Kelnar, I., Brizova, L., Spirkova, M., Pavlova, E., Korea, L. and Carezzi, F. (2013) Chitin Nanofibrils for Bimimetic Products: Nanoparticles and Nanocomposite Chitosan Films in Health Care. In Kim S. K. (ed.) Marine Biomaterials. Characterization, Isolation and Applications, CRC Press, pp 681-71.

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[33] Cinelli, P., Coltelli, M. B., and Lazzeri, A. (2013) Naturally-Made Hard Containers for Food Packaging: Actual and Future Persoectives. In Morganti P (ed.) Bionanotechnology to Save the Environment. Plant and Fishery's Biomass as Alternative to Petrol, MDPI, Basel, Switzerland, pp 297-318. [34] Morganti, P., Chen, H. D., and Li, Y. H. (2019) Green-Bio - Economy and BioNanotechnology for a More Sustainable Environment. In Morganti, P. (ed.) Bionanotechnology to Save the Environment. Plant and Fishery's Biomass as Alternative to Petrol, MDPI, Basel, Switzerland, pp 39-59. [35] Tishchenko, G., Morganti, P., Stoller, M., Kelnar, I., Mikesova, J., Kovarova, J. et al, (2019) Chitin Nanofibrils-Chitosan Composite Films: Characterization and Properties. In: Morganti, P. (ed.) Bionanotechnology to Save the Environment. Plant and Fishery's Biomass as Alternative to Petrol, MDPI, Basel, Switzerland, pp 191-226. [36] Morganti, P. and Coltelli, M. B. (2019) A new Carrier for Advanced Cosmeceuticals, Cosmetics 6: 10. doi:10.3390/cosetics60100101. [37] Alam Khan, F. (ed.) Biotechnology Fundamentals. (2020) Third Edition. CRC Press, Boca Raton FL, USA. [38] Rosen, Y. and Elman, N. (eds.) (2012) Biomaterials Science. An Integrated Clinical and Engineering Approach, CRC Press, Boca Raton FL, USA. [39] Henry-Nickie, M., Frimpong, K., and Sun. H. (2019) Trends in the Information technology sector, Brooking Report, March, www.brooking.edu/research/trends-ininformation-technology-sector (Accessed October 24, 2019). [40] NSF. (2018) Science & Engineering Indicators 2018, National Science Foundation (NSF), Alexandria, USA .www.nsf.gov/statistics/2018/nss20181/digest/sections/globalr-d-one-measure-of-commitment-to-innovation (accessed October 24, 2019). [41] Gran View Research. (2016) Plastics Market Size, Share & Trends by Product, by Application and by Segment Forecasts, 2019-2025, July 29 (Accessed on October 24th 2019). [42] Lemonick, S. (2018) Chemistry may have solutions to our plastic trash problem, 2018, C&en, 96, issue 25 (accessed on October 24th 2019). [43] Saatnia, A. A. (2016) Global plastics packaging market to hit $375 billion by 2020, Zion Research Analysis, https://pimi.ir/global-plastics-packaging-market-hit-375billion-2020/ (Accessed on October 19th 2020). [44] Energy Gold Pub. (2019) Global Bioplastics Market Predicted to Grow 350% energyandgold.com (Accessed October 29, 2019). [45] Bioplastics News (2019) Bioplastic Market Expected to Reach $68,577.25 Million by 2024, 2029, https://biopasticsnews.com/2019/08/08/global-bioplastics-market-to-growby-20/ (Accessed on October 29, 2019). [46] OECD (2018) Realising the Circular Bioeconomy, OECD Committee for Scientific and Technological Policy, Paper No 2018/60, Berlin, Mexico City, and Washington, 19 October. [47] UN (2019) The Future is Now, Global Sustainable Development Report, United Nations publication, Department of Economic and Social Affairs, NY, USA.

PART II. BUILDING BLOCKS OF CIRCULAR ECONOMY

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 3

PAST, PRESENT AND FUTURE OF INDUSTRIAL SYMBIOSIS Sophie Hennequin* and Daniel Roy University of Lorraine, LGIPM, Metz France

ABSTRACT To explore the concept of industrial symbiosis proposed thirty years ago by R. A. Frosch and N. E. Gallopoulos, we conduct a bibliometric analysis of published research works, capturing more than 100 articles. In this way, an analysis of existing implementation and improvement proposals is carried out, such as the development and study of possibilities offered, both in a theoretical and practical framework considering real industrial applications. To simply describe the principle of industrial symbiosis, we can start from the definition of biological symbiosis, which namely refers to a close, long-term interaction between two different species, from the Greek συμβίωσις: living together. This biological symbiosis, studied since the end of the 19th century, inspired recently many developments that highlighted all possible relationships between firms in industrial parks, whatever their characteristics, to improve their environmental performance, more precisely the waste management and resources use, by cost-effective actions. In this chapter, we therefore detail these works and research orientations in order to emphasize the benefits of drawing inspiration from nature by setting up industrial symbioses into industry but also by pointing out the limitations and main difficulties encountered. We specify the different approaches and methodologies used as well as the tools developed to facilitate the implementation of industrial symbioses and their perpetuation over time. We conclude by developing the perspectives around the concept of symbiosis and the future avenues of research.

Keywords: industrial symbiosis, eco-industrial parks, environmental, economic and social benefits, waste optimization, materials and energy exchange

*

Corresponding Author’s Email: [email protected].

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INTRODUCTION The concept of industrial symbiosis (IS), an industrial ecology subfield stated in 1989 in [1], is defined as an industrial system which “in addition to minimizing waste production in processes, would maximize the economical use of waste materials and of products at the ends of their lives as inputs to other processes and industries” [2]. R. A. Frosch [2] drew a parallel between industrial and natural ecosystems, trying to ensure that industrial ecosystems reuse matters and wastes to reduce the need in raw materials coming from Earth resources. To briefly describe, industrial symbiosis corresponds to an organization of industrial entities so that the unused outputs (used water, steam, heat, waste) of some processes of those entities can serve as inputs (energy, water, raw materials after transformation or not) for some processes of other entities [3] or more generally for other entities, which allows this concept to be registered as a model for circular economy. Applying this concept at the scale of a small industrial area gives rise to eco-industrial parks and networks that exchange materials and realize collective sustainable benefits for firms and states [4]. The first full realization of an industrial symbiosis has been located in Kalundborg in Denmark to reduce both costs and to lessen environmental impact on the community. The involved companies have learned how to use each other's waste to create viable commercial products [5]. Indeed, IS allows converting business problems (like trying to catch any potentially hazardous waste or too costly to transform/treat) into a potential revenue stream by finding ready buyers and increasing profits coming from gains in recycling, reduction in greenhouse gases emissions and of course resource saving [6]. However, it was noted that a close proximity of the firms involved in the IS is necessary and known as an initial driving force for exchange flows [7]. This proximity depends on the geographical distance but also on the mental distance of each engaged actor [8]. Furthermore, the evolutionary characteristics and dynamic behavior of direct (facilitating companies and industries) and indirect (governments) actors can greatly facilitate or on the contrary prevent the implementation of an industrial symbiosis and its sustainability over time [9]. While the case of Kalundborg (still in operation for decades) emphases IS's principles can be efficient and work, the various stakeholders must propose methods, tools, exchange on best practices, etc. in order to develop a viable generic implementation model. This chapter presents the main achievements and research works, and sketches out future challenges to shaping ISs and paving the way towards a climate-neutral circular economy [10-11] where pressure on natural resources including freshwater as well as ecosystems is minimized. It will be divided into 3 main parts as described below. First, we will define the principle of industrial symbiosis, its functioning and advantages, and main challenges. To do this, we will start from a concrete implemented case, the well-known Kalundborg’s one and the analyses carried out. This allows us to highlight the main difficulties of implementation in time and space. Once the complete characterization of the IS’s principle has been defined, we will focus in a second part on describing the different models defined, as well as the projects currently being developed around the world and the pursued objectives, whether or not they are achieved. Finally, we will conclude by presenting some research avenues to guide future activities in terms of industrial symbiosis and the applications that can result from it.

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PAST OF INDUSTRIAL SYMBIOSIS In this section, we begin with the principle of industrial symbiosis (IS), first definitions and prospective models, bounding IS in time and space by introducing the development of eco-industrial parks. At this point, it is important to precise that it was early implemented following local political willing before becoming a field of study. Therefore, we will present the well-known case of Kalundborg in Denmark developed since the 1960’s [12]. This wellknown IS case highlights that IS has been initially developed in an empirical way before becoming a scholarly field with a clear codification [13]. Then, we detail how IS can improve environmental and economic benefits. We also give the main limitations encountered and strategies deployed to address them. In addition, the study of industrial applications extended from American eco-industrial parks [14-15] to Asian industrial cases [16], allow us to describe how this transition was made, with which methods and approaches, analyzing both environmental [17] and economic benefits [18] and the different tools used to assess these performances.

Principle of Industrial Symbiosis The principle of industrial symbiosis is inspired by the relationships and exchanges between living species within biological symbiosis, defined by naturalists in the 1870s and 1880s as a "mutualization" between different species for a common benefit [19-20]. Furthermore, in this living together strategy, Nature does not proceed by a rigid scheme in the role. It assigns to each specie, but It adapts to the particular relationships and needs in each case [19]. It should be noted here that the different identified biological symbioses are between a very small number of species (usually two) even if the number of individuals per specie can be very large. With this in mind, at least two or more independent firms can mutualize by exchanging materials, energy or information and thus achieve mutual gain. The individual benefit may be economic, environmental and/or societal in nature, but industrial symbiosis mainly aims reducing the collective environmental weight of firms in a given territory. The development and reuse of a by-product, waste, water, or available energy (for example heat or steam) thus allows an environmental gain while presenting new business opportunities for symbiotic firms. This biomimicry [21] therefore leads to a reconsideration of the productive system by abandoning a usual linear vision (strong pressure of human activities on the biosphere thus jeopardizing its functioning) in favor of a more circular vision of flows with reuse at the end of the cycle. This is also the basis of the principle of circular economy within an ecosystem in which closed loops of industrial production are implemented in order to have circular industrial production routines. The possibilities of an entity (simply a plant) to achieve symbiotic synergies are illustrated through its synergistic potential in an industrial ecosystem (therefore, in the absolute, not limited to a geographically confined area [22]). The particularity of IS (unlike industrial ecology and circular economy) comes from the fact that it was physically implemented in the 1960’s before being scientifically defined in the 1990’s. This real implementation was done in Denmark as explained below.

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Kalundborg‘s Case The IS in Kalundborg has been initially built between six processing companies, one waste handling company and the Municipality of Kalundborg [23-24] starting from a cooperative project between Saint-Gobain Gyproc and Dansk Veedol in order to construct a pipeline to deliver gas [7]. The IS has evolved to include more companies today and is one of the most perfect examples of IS, even if at the beginning the guiding was more focused on saving resources than on achieving an IS. The philosophy is that the partners exploit each other’s residual or by-products on a commercial basis, see Figure 1. From this partnership (with private and public entities), firms share resources (initially the water) and take advantage of other waste resources as heat, steam and gas. This allows to develop new opportunities (different resources and waste flows) and to develop closed-loop practices without central organization.

Figure 1. Flows of materials and energy in Kalundborg.

At the end, this gradual cooperative partnership results into a network that encourages sustainable collaborative relationships to use each other's by-products and otherwise shared resources [25] with a high level of environmental consciousness. It has to be noticed that this project has not been the result of a careful environmental planning process but of the involvement of participants who are constantly exploring new avenues of environmental cooperation. The overall consumption of water has been reduced by 25%. Furthermore, 19 thousand tons of oil and 30 thousand tons of coal are saved each year that results in 130 thousand tons of CO2 equivalent reduced. The main observed outcomes are: i) reduced consumption of resources and environmental strains by cooperation among industries, and ii) increasing of viability of firms by the continuously cooperation between firms. Furthermore, based on this case, the more companies are involved, the greater the opportunity for symbiosis. The case of Kalundborg has been largely studied and commented in the literature from different point of view. We can cite: organizational [26-28], structural [29-30], functional with studies related to expected gains in sustainable development [31-33] and of exchanged flows [34] in most cases at a strategic/tactical level. All these studies highlight its potential and thus promote the implementation of many other more or less successful applications.

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Eco-Industrial Parks and the Role of IS Most serious environmental problems (air and water pollution, solid waste accumulation and disposal of toxic and hazardous wastes) come from transport and industrial processes of petrochemical plants and refineries, metal smelters, chemical industries, heating and electricity generation... but not only. These pollutions result in diseases, very costly for countries and firms, pushing governments to define strategies (taxes, standards, environmental laws…) to force enterprises to find ways to limit their environmental impacts. However, small and medium-sized companies, especially in developing countries, are not able to define their own pollution control systems. For such companies, IS could be an interesting way of reducing environmental impacts as was the case in Kalundborg. Even if, in this case, it is not a developing country and concerns more large groups, but it can serve as an example for deployments in such contexts. Since this first promising implementation, the United Nations with its United Nations Industrial Development Organization (UNIDO) program has helped, early in the 1970’s, many countries (Ivory Coast, Ethiopia, Iraq, Nigeria, Peru, Vietnam, China and Kazakhstan to cite few of them) to develop sustainable projects and set guidelines for green industrial park consideration, construction and management [35]. With this in mind, a green industrial park, or an eco-industrial park (EIP), is defined as [36]: “a community of manufacturing and service businesses seeking enhanced environmental and economic performance through collaboration in managing environmental and resource issues, including energy, water, and materials… The goal of an EIP is to improve the economic performance of the participating companies while minimizing their environmental impact”. De facto, in an EIP, an industrial symbiosis can exist between small and medium-sized companies in order to limit the consumption of non-renewable resources by moving towards a more eco-friendly solution, such as waste recycling and the use of alternative raw materials. An EIP is considered as an industrial ecosystem in which communities of companies exist, allowing the appearance of an IS such as in a biological ecosystem: a company may not find an interest in its own waste, but this waste could be used as a raw material for another company [3]. Thus, EIPs could include IS since they allow to obtain economic benefits and new business opportunities, reducing environmental impacts (like greenhouse gas emissions, scarcity of natural resources and waste), but also other elements as using renewable energy and green buildings. In accordance with these principles, EIPs all around the world have been developed. The direct environmental benefits include reducing greenhouse gas and toxic air emissions, promoting pollution prevention on the cooperation basis, improving the use of energy and water, the conservation of materials through short circle loops between firms and reducing of waste [37]. Furthermore, EIPs allow promoting green technology development and diffusion and the redevelopment of brown field industrial sites. All this of course makes it possible to obtain important economic gains such as direct benefits coming from cost savings (reduced waste management, improved process and product efficiency) and indirect benefits such as retaining existing business and increasing inducted tax revenue, generating new local employments from innovative firms and new marketing opportunities [22, 38-39]. This emphasis is based on resource recovery including energy cascading, and materials exchange, on a small geographical zone. Industrial symbiosis could then play an important role in the development of EIPs, but a number of drivers and barriers could happen as described below.

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Main Challenges with IS Close distance between enterprises is very important to improve symbiotic connections for the transportation of waste/by-products but also for profitable cooperation [40]. Indeed, the role of geographic proximity is generally considered as an essential component for IS [13]. In particular, the importance of the intensity of exchanges between companies, the interdependence in the choices made about recycling and waste reuse processes, the transformations required in production processes directly raise the question of the geographical dimension. Consequently, the grouping of companies involved in an EIP is a considerable asset in the development of inter-industrial trade, insofar as it facilitates the circulation of material and information flows, while limiting transport costs and transaction costs related in particular to the search for relevant productive partners [41]. Many studies are currently focusing on the spatial dimension and its impact on cooperation [42]. In the case of IS, it is probably also due to the central role played by Kalundborg in the shaping expectations of IS, or perhaps also to the presumed low value of the waste/by-products exchanged. However, authors have shown that the distance traveled by a resource in a synergy does not statistically correlate with the resource value or mass [43]. In China, the EIP of Tianjin [44] and in USA, the EIP of Choctaw [45], show that an IS can appear also between more distant enterprises. The other important key factor is to find options, as to with whom, to form a symbiosis and what resource(s) to exchange. Generally, authors focus on how to optimize already identified industrial symbioses within an eco-industrial park [46-47]. However, symbiosis could be developed also outside the EIP and then offer much more possibilities of exchange and business opportunities. Indeed, the bounded geographical space should not be a limit to the symbiosis as we have seen above (even if it is indeed easier to collaborate and mutualize resources while being close). The only element that can be cleavable in this case could come from the mental distance and the fact that the common objective is less obvious (even if sustainable development is holistic). A low mental distance allows, on one hand simple interactions between individuals and on the other hand easy comprehension between individuals. One way to achieve this would be, as in the case of Kalundborg, to have actors already convinced of the importance of acting in terms of sustainable development and therefore to have a common objective that does not contradict individual objectives. Another way would be a better understanding of the common overall objective as it is possible in a given industrial sector (e.g., agro-food, in which case, the spatial restriction is less severe because the mental distance is smaller). Furthermore, most existing approaches focus on inputs and outputs of the same type inside the EIP [48]. In this way, they may miss opportunities and do not facilitate generalization. Initially, in Kalundborg, the objective was to reduce the water consumption rather than optimize the gypsum inside the IS. Thus, the identification of inputs and outputs was therefore simple, which is not always the case depending on the type of firms and the market. Similarly, many works focus on a particular area to reduce the difficulty like for example in chemical industry [49], construction industry [50-52] or agro-food [53]. However, even in this case, data collection is not always simple. Indeed, the structural and functional heterogeneity of the actors (small companies, large groups) does not facilitate the recovery of homogeneous information (very diverse flows, variable denomination/characterization of materials, etc.). In addition, competition problems may arise that does not facilitate the exchange of data (which can be considered as

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confidential) and problems of interdependence between companies may distort identification. Methods exist that can partially facilitate this identification of inputs and outputs for each concerned company like the Enterprise Input-Output Model which allows to identify all inputs and outputs of a part of an entity like the production processes, or the entity itself [34]. The last point that can make complex the implementation of industrial symbiosis within an EIP is the perception of the common objective relatively with individual objectives. We have already detailed this point, but it deserves to be detailed because of the barriers it can induce. Of course, the main driver pushing firms to mutualize resources in IS is the potential economic benefit resulting from this mutualization [54]. Indeed, below a minimum expected economic gain, companies will not wish to make the effort of cooperation in the IS [55] especially if the economic advantage of a symbiotic cooperation is lower than the minimum expected advantage (the company will not start/maintain an IS relationship). The economic gain corresponds to the difference between costs spent and sales achieved [56]. The sales depend on products traditionally marketed by the firm but also on sales of waste to other firms created by IS relationships. The costs depend on purchase costs, transportation costs, production costs (labor, energy, etc.) and perhaps additional costs required to operate the IS exchanges (like treatment costs of waste which can arise when a waste need a treatment process before it can be used as input for other firms inside the IS) minus reduced waste disposal costs. The treatment can generate supplementary costs since treatments of waste may require changes in the production process and therefore additional investment costs in addition to the consumption of energy and materials required for this treatment. To ensure sustainability, the necessary investments in the production processes require innovating to be sure to maintain sustainability by reducing the number of materials and energy used without impacting the quality of products, by-products and waste produced... But these aspects only concern economic gains, other gains can be obtained resulting from the reduction of environmental (such as reducing greenhouse gas emissions, scarcity of natural resources and reduction of waste) and social impacts (job creation, reduction of health problems caused by various pollutants and awareness of the challenges of sustainable development). Although not directly financial, current thought patterns and societal pressure mean that the gains on these aspects may well be decisive in determining the willingness to integrate an IS. However, these gains could be more complex to characterize. Nevertheless, EIPs have large possibilities of development like site design, park infrastructure, individual facilities, and shared support services with the help of local governments, integration of new actors, etc. which can promote and facilitate an industrial symbiosis strategy [57] and industrial symbiosis can facilitate the management of EIP [58]. Several EIPs are already well developed but most are still in the planning and feasibility stages [59]. In the same way, several projects concerning industrial symbiosis are defined all around the world. In the following section, we propose to detail these projects.

PRESENT OF INDUSTRIAL SYMBIOSIS In this section, we study proposed methods and models offered in the literature to explain concepts behind the design, the management and the control of IS. We will start from current implementations and projects in the world to give the main results and orientations. Then, we

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will study proposed models from a strategic, tactical and operational levels and methods in link with the main challenges defined above. Based on the study of these works, we draw a parallel with industrial ecosystems in order to highlight areas for progress and ways to increase the propagation of this practice.

Projects and Implementations of IS and EIPs in the World Real industrial eco-parks and regional industrial symbioses (at a very local range like Kalundborg in Denmark) have been largely explored around the world [8]. In this way, in North America, when the US President's Council on Sustainable Development defined eco-parks [60] more than 60 projects have been developed in both the USA and Canada [61]. We can cite in USA, the Houston Ship Channel in Texas which is an interesting example of a spontaneously EIP in which the different industries exchanged materials at a large scale [62]. The projects carried out are more in line with efficient industrial development with significant economic gains than in a pure circular economy and IS framework, even if very good results have been obtained [63]. In Mexico, the Altamira-Tampico industrial corridor has been implemented twenty years ago with success [64]. The authors in their study highlight the importance of stakeholder involvement in this success but also in a comprehensive approach of the region since the companies will act also by considering their historical story (industrial culture and commitments). For a given year, this IS allowed savings 44,820 tons of wastewater, 44,400 tons of carbon dioxide, and 26,720 tons of carbon monoxide. However, this success has not been sustained over time and some companies involved at the beginning are not yet invested (as in many other EIP and IS projects). In South America, for the moment to the best of our knowledge, only one project located in the state of Rio de Janeiro in Brazil was completed. It aimed to develop waste synergies and by-products between various industries [37]. However, further efforts are needed to ensure the sustainability of these actions over time. In Asia, Japan has initiated a national program in 1997 to study possibilities of industrial symbioses [65-66] and China initiated its first project in 2001 [67], and since then 108 projects are underway [68]. In China, the Guangxi Guitang Group is an example of the application of the IS to the agro-food industry with the use of by-products of sugar production, first within a single company, then in a broader network including other sugar producers in the city of Guitang and sugar cane farmers [69]. The success of this IS is due to the fact that the first investments were all made within the single company, not between separate companies, and an important reduction of the urban carbon footprint [70]. From this single company, an eco-industrial network has been developed, including other sugar producers and farmers. In Shandong Lubei, another case in China [71], the IS has an important number of activities between different kind of companies like water and wastewater companies, thermal power plants, farms, pharmaceutical company, paper company, cement companies, automobiles and machinery industries, among others. In South Korean, a 15-year plan has been defined to retrofit existing industrial complexes into eco-parks from 2000 to 2015 [72]. In India, the concept and application of IS facilitates industrial and urban developments [8]. All projects carried out are generally very ambitious and medium/long term and therefore the expected results are still pending. We also remark that an important

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number of projects focus on technological improvement of manufacturing processes (including energy). In Europa, through different funds and guidelines from the European Commission [73] more than 130 million euros have been invested since 2006 in different research projects allowing to develop a platform that facilitates the uptake of industrial symbioses by different actors [74]. To give few examples, in Sweden, an IS network permits to create jobs with 5 new companies and to reduce CO2 emissions through resource sharing [75]. This case concerns a small number of companies with a very little diversity, since the symbioses are developed between growers of mushrooms and farmers or between brewers and breeders. In United Kingdom, several projects have been developed [55] highlighting the importance of cooperation and therefore the impact on the results of good coordination [76]. In Germany and Austria, recycling strategy networks are stimulated, based on industries that are not located on the same site, but that are present in a particular Länder (i.e., an administrative or geographic region). In the Netherland, the Industrial EcoSystems project initiative including seven refineries, eleven companies involved in inorganic chemistry and thirteen in petrochemistry has been developed in a district of Rotterdam [42]. This project is based on exchange of residual products between industries in order to obtain both environmental and economic benefits with a calculated reduction in CO2-emission of 2775 tons per year. In Italia, some projects have been developed for specific industrial sector as chemical, automotive, and agro-food industries. In Belgium, at the Herdersbrug Industrial Park, where the main CO2 emissions are due to energy consumption and the incineration plant, 67% of total CO2 emissions can be saved with the renewable energy generated in the park. In the majority of European projects, the impetus of national governments and European support has made possible to develop strategies to significantly reduce emissions and limit waste, but not always in a spirit of circular economy and IS, although efforts are currently being made in this direction [18]. Furthermore, projects are dedicated to specific region and specific activities like in Finland with forestry activities [77]. In Australia, the national government and a local council developed the Australia's first eco-industrial estate, named Synergy Park near Brisbane in 1996. The industrial symbiosis has been limited to two types of resource synergies (based on physical exchanges of materials or by-products) and utility sharing (shared use of infrastructure to provide process water, energy, etc., or common treatment of effluents or wastes). From this project, another project has been launched near Perth [78] with a large regional industrial symbiosis project: the Kwinana Industrial Area Project. The Kwinana project comprises 47 symbiotic projects between 22 firms and is well developed until now with for example one of the cogeneration plants which accepts excess refinery gas from the oil refinery and supplies in return process steam back to the refinery. In Africa, eco-industrial projects have been initiated in Egypt and South Africa with the help of UNO but are still in progress. For some developing countries, IS and EIPs are a very promising means of economic development and enable these countries to participate in sustainable development without making too much investment [79-80]. Furthermore, the case of Beshghardash Region in Bojnourd, Iran [81] allows considering not only environmental specifications (like the desertification) but also the importance of special cultural characteristics of the society in order to obtain sustainable development. The conclusions made by several studies highlight that the most relevant roles in the industrial symbiosis are, apart the proximity of production plants already mentioned, the

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infrastructure, utility, and services availability, the volume and homogeneity of waste, the limited presence of hazardous materials, the homogeneity (sometimes but rarely heterogeneity) of industries, geographical characteristics (cultural, social and also the sustainable development involvement of actors) and finally the number of industries and processes involved in the IS. Many projects are currently being developed around the world (especially in China, the USA and the European Community) to define EIPs including symbiotic synergies. We have not presented all projects in an exhaustive way but the most studied projects in the reference articles. The different studied cases in literature reflect an important variety in the size and types of activity involved in IS. However, even on the most advanced projects, many actions remain to be carried out, such as optimization of IS networks and synergies, comparative analysis of IS developments to characterize an optimal design, assessing benefits of IS developments, optimal strategies linked with regional and local sustainable developments, future trend for IS. Furthermore, these works have very different approaches in the sense that some are oriented towards a very strategic and upstream vision (to set up an IS), others are articulated on more tactical activities and the fact of maintaining an IS over time and finally some works address the operational level of symbiosis. We will develop these ideas in the following considering the possible levers for improvement.

Improvement Strategies for IS First, we focus on strategic works which core on the design of an IS. Then, we study the implementation and sustainability of symbiosis over time and finally describe the levers for operational improvement of ISs. Considering the first point, at the strategic level, a physical representation of firms and links between firms is necessary. It could be obtained by a formal representation of IS grounded in graph theory [30, 82]. In this case, a network study can be conducted as well as the links representing the interactions. This study can therefore assess the network itself, but also its weaknesses and opportunities. However, these studies do not really take into account the social dimension of the network. Another important point is correlated with collaboration within diverse multi-stakeholder groups [27]. To study these collaborations, two main directions are taken. Firstly, a holistic approach with a focus on stakeholders is made. In this case, the characterization of stakeholders and their involvement can be studied based on multi-agent systems [46, 83]. The identified actors could be institutions regulating industrial symbioses, networks of companies or organizations and companies or individuals. The modes of organization are also studied with very top-down government mandates to bottom-up independent programs with self-initiated synergies to facilitated and coordinated IS networks [13]. The approach, coupled with the relationship of these actors to Nature, also depends on how interactions between the actors are organized (ranging from intentional coordination like most of the projects developed to a collective culture like in Kalundborg). In this case, the limitations observed are often linked to the identification of the possibilities offered (subsidies, facilitation and exchange of data, processing of waste in order to make it usable by others, etc.) and the linking and facilitation of cooperation [42]. In addition, stakeholders could enter into the IS collaboration for various strategic reasons and as long as these reasons are met, the collaboration will be successful. The identified reasons are increasing the

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participating firms' chances of survival, obtaining essential scarce resources, pressure from external institutions and norms, gaining legitimacy, publicity and a competitive advantage, and finally reducing costs. Some authors stress the importance of innovation in strategies developed not only at the process level but also in information sharing [26]. They also highlight three key points to be integrated to ensure the sustainability of IS: potential partners, tradable resources and the impact of time in interactions. The other direction concerns the organization and coordination between actors (which may also include their support). We can cite for examples social network analysis [68], their impacts on results and difficulties in information sharing [84]. The proposed works generally have a theoretical approach to the problem, most often omitting the spatial dimension and its impact on the results expected or obtained as part of a symbiosis. However, symbiosis (biological or industrial) develops itself in a given environment (with its own constraints and characteristics). The symbiosis is therefore directly impacted and linked to this environment but will also impact this environment. This point must be included to improve the design of an IS in a given region. As detailed above, an important point concerns the definition of IS relationships into an existing industrial park by identifying possible synergies between companies [13]. At a tactical level, generally, authors try to clearly identify inputs (which can be energy, water, materials) and outputs (waste, used water, steam/heat). Authors proposed to identify all possible inputs/outputs of the same type, for example water and waste water [48]. Otherwise, a design structure matrix which intends to support the identification of substitution opportunities [47] could be defined associated with a graph of the formal IS. This approach allows finding symbiosis opportunities that would not be found by classical input-output matching approach but does not consider possible convert resources and does not allow catching further symbiosis opportunities. Furthermore, this characterization and quantification require clear system boundaries. The evolution of relationships in Kalundborg has been largely studied from a grounded theory approach to highlight key factors. This theory is an inductive, qualitative approach well suited to situations where existing theories do not exist [5]. Then, it allows describing success factors but also organizational barriers [28] such as geographic proximity, which is a well-recognized element that facilitates industrial symbiosis [85]. Other approaches focus on the analysis of environmental gains with analyses conducted in relation to the life cycle assessment [86, 90]. The Material Flow Analysis makes possible to carry out an inventory and to assess the construction models around the diversity and quality of the possible mutualizations. A logistics vision of flows is also envisaged for similar reasons but with the objective of sharing on the supply chain [24]. Logistics makes it possible to encompass all internal or external activities that add value to goods for customers by considering the flows of materials exchanged as well as the flows of information. Energy flows are not often taken into account, but many recent studies integrate environmental impacts into classical supply chain studies [91]. The various studies carried out highlight the importance and characterization (flows, types…) of symbiotic exchanges (from an environmental point of view, although the social dimension could be addressed in the expected benefits). At this tactical level, more technical and less economical approaches are most often used (like life cycle assessment...). However, a more logistical approach makes it possible to integrate concepts such as value creation into a more systemic approach. At an operational level, few works have been developed to the best of our knowledge. The existing approaches consider design optimization but they are still suffering from several

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major problems due to dominance of the global IS optimum over the local individual optimum, limited number of optimization objectives falling into the categories of economic and environmental objectives (forgotten social objectives) and optimization performed without considering possible operational uncertainties. Indeed, transformations within the symbiosis and its evolution over time are never taken into account, which is crucial (as we have seen with many of projects). Two directions can be mentioned. The first concerns the performance within the industrial symbiosis. Thus, in [92], authors propose indicators derived from an agent approach, in [58], authors focus on defining a dashboard to optimize the management of the IS, and in [93], authors focus on the performance obtained at the exchange level. In [94] a semantic approach is proposed to set environmental indicators for IS and in [95] a resilience indicator is proposed for EIPs. The second direction concerns the evaluation of gains in order to improve the results obtained. We can thus cite the definition of mathematical models which allow characterizing gains and improving them under different possible scenarios by simulations. So, in [56] and [96], the authors seek to define optimal material flows based on two objectives: symbiotic profit and economic profit of the industrial park. A bi-objective mathematical model is obtained and the optimal Pareto front is determined. The results obtained make it easier for the decision-maker to take decisions to determine grant or tax levels in order to effectively promote industrial symbiosis. In another work [97], the authors propose a Stakelberg game model for waste recycling based on waste pricing under three scenarios: non-symbiosis, partial symbiosis and complete symbiosis between two firms. Then, based on this game theory model, they show that the internal (like recycling cost, harmless disposal cost and the degree of waste recyclability) and external (like price of raw materials and the government price subsidy) factors affect the existence of symbiotic relationships. They highlight that coordination between enterprises is then needed to promote waste management inside the industrial park. Thus, by studying the structural organization of industrial symbiosis, researchers and practitioners could provide a better understanding of industrial ecosystems that are complex adaptive systems [27]. In this perspective, methods from complex systems permit to examine the evolution and resilience of IS [46, 98]. By studying the functional organization of IS, authors focus on relation between methods and expected results like for example quality [99] and sustainability [100-101] issues. In addition, the identification of environmental gains with minimization of waste, GHGs produced and reuse of materials [102] is essential and therefore widely studied [103-106]. Industrial ecology allows the analysis of the flows of materials and energy considering the life cycle of products, the design of buildings, infrastructure and industrial parks and the reuse, recovery and recycling of resources in a manner which is cleaner and more efficient [41]. Circular economy aims to redefine growth, focusing on positive society-wide benefits. IS and EIPs could then play a major role inside industrial ecology and circular economy for the society as described in the following section.

FUTURE OF INDUSTRIAL SYMBIOSIS We end by a synthesis of evolution of works concerning IS. Thus, we give an overview of industrial symbiosis developments potential in new schemes. We analize selected publications based on the research of articles with keywords "industrial symbiosis" in the title

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as well as in the document in order to identify the largest number of publications. The consulted academic databases comprise the publishers with the greatest number of articles published in this domain such as ACS Publications and Annual Reviews, Elsevier, Emerald Insight, Inderscience Online, IEEE Xplore, MDPI, SAGE Journals, Springer, Taylor & Francis Online, Wiley Online Library instead of Web of Science and Scopus, since they offer more articles (see also [107]). Obtained articles are research articles in journals or conferences, book chapters and editorials with peer-reviewed processes. Looking at the number of publications on IS over time, we can see that in recent years (and more precisely since 2007 and especially since the rise of projects developed in China) this number has exploded exponentially, see Figure 2. the publications could be classified into three main types: theoretical studies, review articles and case studies from real applications and projects in the world. Looking at the potential of applying industrial symbiosis in new places, new categories are defined such as urban industrial symbiosis presented below. Moreover, the most recent works carried out makes it possible to return to and highlight the issues of industrial symbiosis as initially defined (following the Kalundborg case), as we will see in the following. From this analysis, we present the most recent developments and their objectives, integrating the gaps still identified and the avenues for future research. We conclude this section by presenting IS outside a purely industrial framework and show how interesting it can be on other developments than EIPs.

Figure 2. Research works in time relatively with IS.

Potentials of IS IS is generally studied from an issue dealing with limited resources and pollutions but we must not neglect the economic role it can play in the regional development [108]. As we have seen, IS is highly studied at the strategic level with main interest concerning the development of a region and a lot of works focus on geopolitical/geo-economical aspects and interests in terms of sustainable development [31]. However, the spatial dimension and its impact of IS results is rarely studied. Although, the expected gains depend on this spatial dimension and they can also influence it, see Figure 3. Indeed, the culture/history of population and its level of life, the possibilities in terms of raw materials and resources will greatly affect, in a positive or negative way, the implementation of IS. For the Kalundborg’s case, it is evident

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that the success comes from implementation parameters since the involvement of stakeholders also in terms of sustainable development is important for a long time, and the facilitation in collecting different kinds of data since concurrency is lesser important than transparency in Denmark for examples.

Figure 3. Ecosystem and IS.

It should be pointed out here that the ecosystem under consideration is not limited to the study of a limited geographical area (like in an EIP) but may include more distant interactions with other actors (as in a supply chain). As a reminder, an industrial ecosystem has the capacity to maintain itself alone through the efficient use of its resources, whether manufacturing or natural, with an environmental impact that tends towards zero while allowing maximum economic and social benefits (and thus towards sustainability) [109].

New Developments In the most recent developments, many studies are interested in the application of the concept of IS to cities since IS allows to gain advantages involving physical exchange of materials, energy, water, and by-products by mutualization between separate entities in a collective approach. This idea could then be further extended to urban waste and energy exchange from industrial complexes. This concept is known as urban symbiosis [111]. The industrial symbiosis as urbanization has been initially applied in the Japanese Eco-town program [112] in 1997 in order to revitalize local industries and also to extend the life of existing landfill sites, an important aspect in Japan. This program permits to optimize waste management and develop recycling industries. Furthermore, a best quality of life of local population and the appearance of a sense of belonging to a community are obtained. From this program, it is evident that companies could improve their results and productivity with

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short circular loops and reuse of waste as in case of ISs, but the civil society also gains with the improvements of the well-being of communities [111]. So, both IS and urban industrial symbiosis focus on waste recycling, heat/steam exchange and a symbiotic network that can offer benefits to the entire city [113]. Transport, manufacturing and logistics can also be included and helpful dedicated tools like platforms could be developed to facilitate the implantation in cities [114-117]. Another way of research which could be also very interesting in implementation of IS concerns the direct application of biological symbiosis in the definition of relationship between entities into industrial clusters and innovation efficiency. Indeed, two types of relationships deriving from ecological relationships could be defined: i) opposite relationships, which could be predation or competition, and ii) symbiotic relationships with mutualism, commensalism, amensalism and parasitism [118]. In fact, generally in order to obtain the best benefits, symbiotic relationships are developed inside innovation and industrial clusters. However, resulting from the evolution of the market and the concurrency, the first type of relationships could appear. This opposite relationships should be taken into account in the defined study along the evolutional path to address the particular links between stakeholders of different subsystems and entities. From a purely innovation point of view, it has to be noticed that symbiosis occurs mainly between two entities. The first one expresses a particular need and the second ones the solution to this need [119]. Then, the measurement and analysis of the symbiotic modes can allow describing the development and evolution of innovations in a cluster, and it can then allow defining future directions and strategies. The integration of these different kinds of relationships is more vital in the case of vast territory and various marked regional differences to be sure to gain real coordinated ISs. Among these works, almost no work integrates the potential offered by industry 4.0 and the associated new emerging tools. We can still mention the facilitation in data management through big data analysis [120]. Industry 4.0, the fourth industrial revolution initiated in the early 2000s, is a term, which refers to the developmental digitalization process in the management of industry [121]. However, the tools offered in this framework, such as new information and communications technologies and artificial intelligence would most certainly facilitate the design, deployment and implementation, as well as the optimization of ISs. One example is the new ways of storing and securing information, with for example blockchains, that could make it possible to overcome the problems of historization and confidentiality. Industry 4.0 is intended to be the future of the industry in general; it may be the future of industrial symbioses in particular.

CONCLUSIONS Through the analysis of more than 100 articles, we sought to understand what industrial symbiosis represented and how it could act in terms of sustainable development from a circular point of view. Through the analysis of the articles found, we have been able to note that the IS is simple to define but much more complex to implement. The first known implementation of industrial symbiosis was defined in Denmark at Kalundborg early in the 1960s. Since then, it is still up-to-date, still effective and growing. The works having studied this real case have been able to highlight different key elements of this IS (such as geographic

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proximity, stakeholders’ involvement, economic, social and environmental gains). Since then, an important number of projects have been carried out in the world: (i) in developing countries, with the help of the United Nations, to build green industrial zones, also called ecoindustrial parks, and (ii) in developed countries either to revitalize industrial activities or, as in Kalundborg, to build industrial symbiosis on existing or future industrial sites. These real applications of industrial symbiosis are done around projects carried out by the state governments and are therefore registered in a particular region most often restricted in size. Unfortunately, the results are not always there (lack of implications of the actors, difficulty of implementation, too strong constraints...) nor do last either in time (some actors leave the symbiosis or this one disappears). As a result, many authors have proposed ways to improve and eliminate those problems with approaches that are often strategic (to optimize the design of the IS) and tactical (to optimize its deployment and its chances of success). Few works are articulated at the operational level yet decisive in the continuity of implementation. From a strategic point of view, the work focuses mainly on the exchanges and organization of the actors. At a tactical level, a comprehensive and detailed knowledge of the material and energy flows of a given sector or geographical area is generally considered as a prerequisite for IS. To successfully carry out this diagnosis, all data on company’s flows must be identified. This is met with considerable reluctance in a number of industrial sectors, given the high degree of competition that may exist and the resulting culture of confidentiality. The choice of a homogeneous sector can simplify but some opportunities for symbiosis are lost. All works highlight, from upstream to downstream, the models for building collective action and the diversity of possible symbioses. Furthermore, such as for industrial ecology and circular economy, the number of research papers concerning IS explodes. To conclude, if we make a comparison with naturel systems, four main principles [122] should be respected in IS. (1) The roundup capacity: recycling activities like in Nature where the actors involved cooperate through waste material and energy utilization. (2) Locality: actors inside the IS cooperate in diverse interdependent relationships in and outside the IS, but in relation with regional conditions and limiting factors that should not be forgotten. (3) Diversity: the basic idea is similar to biological ecosystems where the sustainability is ensured by allowing high flexibility and adaptability, the existence of diversity can be seen as a long-term survival strategy of ecosystems as a consequence of permanently changing environmental/market/society conditions. (4) gradual change: this point is more difficult to obtain since companies should adapt themselves with rapid changes (due to market, industrial evolution, social and cultural transformations, etc.). However, innovation, resilience and deep learning methods would help firms to adapt to rapid changes. So, to construct a universal design principle of IS, it is necessary to keep in mind these four principles and make regional efforts and initiatives to improve EIPs. Furthermore, as detailed above, it is necessary to inscribe the research carried out in a framework integrating the spatial and temporal dimensions This could be facilitated with the help of tools and methods developed in the context of Industry 4.0. Moreover, a vitally important point is innovation in product and process design to reduce resource inputs per unit of output and to extend the lifecycle of end products through durability, reparability, upgradability, and recyclables, but also in cooperation and mutualization. In this case, the knowledge coming from Nature and ecological symbiosis studies could help to define new strategies for the long-term decisionmaking for industrial ecology and circular economy by integrated new insights.

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[93] Fraccascia, L., Albino, V. and Garavelli, C.A. (2017). Technical efficiency measures of industrial symbiosis networks using enterprise inputoutput analysis, International Journal of Production Economics 183(A): 273-286. [94] Trokanas, N., Cecelja, F. and Raafat, T., (2015). Semantic approach for pre-assessment of environmental indicators in industrial symbiosis. Journal of Cleaner Production 96: 349-361. [95] Valenzuela-Venegas, G., Henríquez-Henríquez, F., Boix, M., Montastruc, L., ArenasAraya, F., Miranda-Pérez J. and Díaz-Alvarado, F.A. (2018). A resilience indicator for eco-industrial parks. Journal of Cleaner Production 174: 807-820. [96] Hennequin S., Ho, V.T., Le Thi, H.A., Nouinou, H. and Roy, D. (2019). “Industrial symbioses: Bi-objective model and solution method”, Optimization of Complex Systems: Theory, Models, Algorithms and Applications, Thi L. and An H. (eds.), Springer, ISBN 978-3-030-21803-4. [97] He, M., Jin, Y., Zeng, H. and Cao, J. (2020). Pricing decisions about waste recycling from the perspective of industrial symbiosis in an industrial park: A game model and its application, Journal of Cleaner Production https://doi.org/10.1016/j.jclepro.2019. 119417 [98] Romero, E. and Ruiz, M.C. (2014). Proposal of an agent-based analytical model to convert industrial areas in industrial eco-systems. Science of the Total Environment, 468,394-405. Cleaner Production 19: 1158-1169. [99] Prosman, E.J. and Wæhrens, B.V. (2019). Managing waste quality in industrial symbiosis: Insights on how to organize supplier integration. Journal of Cleaner Production 234: 113-123. [100] Ren, J., Liang, H., Dong, L., Sun, L. and Gao, Z. (2016). Design for sustainability of industrial symbiosis based on emergy and multiobjective particle swarm optimization. The Science of the Total Environment 562: 789–801. [101] Shi, X. and Li, X. (2019). A symbiosis-based life cycle management approach for sustainable resource flows of industrial ecosystem. Journal of Cleaner Production 226: 324-335. [102] Mohammed, F., Biswas, W.K., Yao, H. and Tadé, M. (2016). Identification of an environmentally friendly symbiotic process for the reuse of industrial byproduct—an LCA perspective. Journal of Cleaner Productio 112: 3376-3387. [103] Taskhiri, M.S., Tan, R.R. and Chiu, A.S.F. (2011). Emergy-based fuzzy optimization approach for water reuse in an eco-industrial park. Resources, Conservation and Recycling 55: 730–737. [104] Liu, Q., Jiang, P., Zhao, J., Zhang, B., Bian, H. and Qian, G. (2011). Life cycle assessment of an industrial symbiosis based on energy recovery from dried sludge and used oil. Journal of Cleaner Production 19: 1700-1708. [105] Mattila, T., Lehtoranta, S., Sokka, L., Melanen, M. and Nissinen, A. (2012). Methodological aspects of applying life cycle assessment to industrial symbioses. Journal of Industrial Ecology 16: 51-60. [106] Kerdlap, P., Choong Low, J.S., Steidle, R., Loong Tan, D.Z., Herrmann, C. and Ramakrishna, S. (2019). Collaboration Platform for Enabling Industrial Symbiosis: Application of the Industrial-Symbiosis Life Cycle Analysis Engine. Procedia CIRP (26th CIRP Conference on Life Cycle Engineering (LCE) Purdue University, West Lafayette, IN, USA May 7-9, 2019) 80: 655-660.

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[107] Neves, A., Godina, R., Carvalho, H., Azevedo, S.G. and Matias, J.C.O. (2020). A comprehensive review of industrial symbiosis, Journal of Cleaner Production, In press. [108] Kokoulina, L., Ermolaeva, L., Patala, S. and Ritala, P. (2018). Championing processes and the emergence of industrial symbiosis, Regional Studies, 1-12. [109] Andrews, C.J. (1999). Putting industrial ecology into place evolving roles for planners, Journal of the American planning association 65(4): 364-375. [110] Cui, H., Liu, C., Cote, R. and Liu, W. (2019). Understanding the Evolution of Industrial Symbiosis with a System Dynamics Model: A Case Study of Hai Hua Industrial Symbiosis, China. Sustainability 10(11). [111] Van Berkel, R., Fujita, T., Hashimoto, S. and Geng, Y. (2009). Industrial and urban symbiosis in Japan: analysis of the Eco-Town program 1997–2006. Journal of Environmental Management 90: 1544-1556. [112] Geng, Y., Liu, Z., Xue, B., Dong, H., Fujita, T. and Chiu, A. (2014). Emergybased assessment on industrial symbiosis: a case of Shenyang Economic and Technological Development Zone, Environmental Science and Pollution Research 21: 13572-13587. [113] Afshari, H. and Jaber, M.Y. (2019). Searcy C. Extending industrial symbiosis to residential buildings: A mathematical model and case study. Journal of Cleaner Production 183: 370-379. [114] Mulrow J.S., Derrible S., Ashton W.S. and Chopra S.S. (2017). Industrial Symbiosis at the Facility Scale. Journal of Industrial Ecology Special Issue: Exploring the Circular Economy 21(3): 559-571. [115] Govindan, K. and Hasanagic, M. (2018). A systematic review on drivers, barriers, and practices towards circular economy: a supply chain perspective. International Journal of Production Research 56(1-2): 278-311. [116] Yeo, Z., Masi, D., Choong Low, J.S., Ting Ng, Y., Tan, P.S. and Barnes, S. (2019). Tools for promoting industrial symbiosis: A systematic review. Journal of Industrial Ecology, 23(5): 1087-1108. [117] Yeo, Z., Choong Low, J.S., Loong Tan, D.Z., Chung, S.Y., Tjandra, T.B. and Ignatius, J. (2019). A collaboration platform for enabling industrial symbiosis: Towards creating a self-learning waste-to-resource database for recommending industrial symbiosis transactions using text analytics. Procedia CIRP (26th CIRP Conference on Life Cycle Engineering (LCE). Purdue University, West Lafayette, IN, USA May 7-9, 2019). 80, pp. 643-648. [118] Zhang, W. and Lee Lam, J.S. (2013). Maritime cluster evolution based on symbiosis theory and Lotka–Volterra model, Maritime Policy & Management 40(2): 161-176. [119] Wang, S., Zhang, J., Fan, F., Lu, F. and L. Yang (2019). The symbiosis of scientific and technological innovation efficiency and economic efficiency in China - an analysis based on data envelopment analysis and logistic model, Technology Analysis & Strategic Management 31(1): 67-80. [120] Tseng, M.L., Tan, R.R., Chiu, A.S.F., Chien, C-F. and Kuo, T.C. (2018). Circular economy meets industry 4.0: Can big data drive industrial symbiosis? Resources, Conservation and Recycling 131: 146-147. [121] Lu, Y. (2017). Industry 4.0: A survey on technologies, applications and open research issues, Journal of Industrial Information Integration 6: 1-10. [122] Korhonen, J. (2001). Four ecosystem principles for an industrial ecosystem, Journal of Cleaner Production 9: 253-259.

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 4

DEVELOPMENT OF INDICATORS OF CIRCULAR ECONOMY AND THEIR APPLICATION IN WATER MANAGEMENT Juan Carlos Leyva-Díaz1,, Valentín Molina-Moreno2, Jorge Sánchez-Molina3 and Luis Jesús Belmonte-Ureña4 1

Department of Chemical and Environmental Engineering, University of Oviedo, Spain 2 Department of Management-1, University of Granada, Spain 3 Department of Chemistry, University of Francisco de Paula Santander, Colombia 4 Department of Economy and Business, University of Almeria, Spain

ABSTRACT One of the main characteristics of circular economy is that it is a restorative and regenerative economy, which means that any input within the production process must be restored. This implies reducing as many negative externalities as possible, thus avoiding scarcity in ecosystems. Circular economy stands as an alternative production and consumption model, whose objective is to solve current environmental challenges and create business and economic growth opportunities. The transition towards an economic model based on circular economy is considered as the only feasible option in order to preserve earth’s resources and eliminate or mitigate those negative externalities produced by the linear economy model. One of the great challenges of current sustainability policies is water management. According to United Nations figures, water redistributive management is not optimal and at least 25% of world population is expected to live in a country affected by chronic and repeated scarcity of fresh water by 2050. Due to all the above, circular economy provides an important opportunity to improve the efficacy and efficiency in water management. In this respect, United Nations sustainable development goals consider that it is essential to change the currently dominant water management model. This model is not viable in the medium and long terms, as the availability of water resources in terms of quantity and quality is at risk. 

Corresponding Author’s Email: [email protected].

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Juan Carlos Leyva-Díaz, Valentín Molina-Moreno, Jorge Sánchez-Molina et al. Despite the strategic importance of water, Spain has not developed any specific policies from the point of view of circular economy. In addition, the available data regarding this topic is scarce. The scientific community and international organizations recommend the introduction of indicators for the evaluation and follow-up of the progress towards a sustainable development, given that they are essential tools when it comes to making decisions in order to improve resource efficiency and minimize waste generation. This chapter puts forth the literature revision of indicators of circular economy and water management, as well as the proposal for their design so as to be applied in the field of wastewater treatment, which allows quantifying the degree of approximation to a circular economy model. In this paradigm, wastewater, which is initially seen as waste, is transformed into a resource or technological nutrient that can be partially reintroduced into the production process. On this basis, the decision-makers from both production sectors and public administrations can incorporate them into the creation of new legislation and sustainability models and, in this way, contribute towards a change of model, from linear to circular economy.

Keywords: circular economy, indicator, water management, bibliometric analysis, sustainability, technological nutrient

INTRODUCTION TO CIRCULAR ECONOMY Economic growth sustainability and environmental protection have become a priority from the beginning of the 21st century. Social awareness is rooted and citizens’ opinions are clear, as environmental damage is a fact and confirms what experts had already anticipated years ago. A political agreement was necessary in order to manage the global production system, including different variables to catalog growth, instead of only considering those that measure richness with economic purposes. Political initiatives were implemented in several climate change and environmental sustainability summits. The most important of them was perhaps the 2015 Paris Climate Summit, where 96 signatory countries (in June 2017, after the US elections, Trump announced US exit from this agreement so as to safeguard the financial interests of the nation) presented their answer in order to mitigate the emissions of polluting gases which are contributing to the greenhouse effect. The main proposal was to restrict those emissions from 2020 onwards, when the agreement would come into effect. The Paris Summit was a consequence of an initial impulse: the 2030 Agenda. With it, the UN General Assembly set the objectives of sustainable development (OSD) in September 2015, with the aim of combining economic prosperity and environmental sustainability. The strategy was clear: to reduce the negative externalities generated by the current production process in both private and public sectors [1]. The purpose is to make those stakeholders participating in the economic system understand the critical situation of the planet and the need for a change in the management of corporate governance [2]. The European Union, as a signatory of the Paris Summit, has maintained an active position in its fight for environmental sustainability. In fact, a roadmap has been designed based on the European Commission regulations (2012, 2015) in order to introduce a lowcarbon production system according to the circular economy model.

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Within this framework, circular economy can be contextualized as the production system that is regenerative and, consequently, environmentally friendly, as the main energy source usually comes from renewable energies [3]. In addition, it is characterized by minimizing resources and obtaining by-products and waste, mainly in the farming sector [4-6]. Due to all the above, production within the circular economy paradigm seeks to optimize production processes and minimize the negative externalities generated thereby. It is regenerative by design, the energy that it uses is renewable and it reduces chemical waste generation [7].

THE NEED FOR WATER MANAGEMENT WITHIN THE CIRCULAR ECONOMY PARADIGM In 2018, the European Commission published a report presenting the need for a system of monitoring indicators so that the implementation of circular economy in various production sectors could be introduced in a gradual and optimal way throughout the EU countries. Regarding water, it is important to highlight that the above mentioned report does not make any reference to variables related to water management, since it is mainly based on the flow management of raw materials and pays particular attention to material recycling and the use of secondary raw materials. However, Spain (and some other EU countries) has developed the draft 2030 Spanish Circular Economy Strategy, along with a proposal for an action plan (2018-2020) containing several guidelines. In chapter 7 of this document, a system of indicators of water management is specified. This shows the necessity to create a specific model of water indicators in order to promote water as a resource or nutrient that must become a referent within the new circular economy paradigm. One of the principles of circular economy is that it is restorative and regenerative, so it is fundamental to minimize and optimize productive inputs, which must be reintroduced into the different production processes. In this respect, water is an essential resource that must be managed efficiently and effectively, inasmuch as it is a dwindling resource. When the creation of indicators is suggested, the various theories of business management indicate that they must be referred to units of reference, of both a material and an economic nature. For instance, being able to determine the economic performance generated by a cubic meter of water used in agriculture, services or industry provides us with essential information when it comes to making decisions about the management of this resource. Within the circular economy paradigm, water is considered as a technological nutrient and thus a productive factor that can be regenerative and restorative as an element of natural wealth. For these reasons, it is important to create indicators that enable us to understand its management within this new paradigm. Hence, the main aim of this chapter is to present the different contributions made within the framework of indicators of circular economy and water management as well as to formulate a design proposal of them in the field of wastewater treatment. In order to do so, scientific articles on this subject published on Scopus database have been analyzed. The

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results show the contributions to this line of research, which allows identifying the principal forcing agents, its future trends and some gaps in critical knowledge.

STATE OF THE ART ABOUT INDICATORS OF CIRCULAR ECONOMY REGARDING WATER MANAGEMENT Evolution of Scientific Production The evolution analysis of the number of scientific articles published and annual citations (Figure 1) shows the variations in this research field during the study period, between 2012 and 2019. No publications were found for the year 2013. Only 1 publication was found for the year 2012, although this figure increases to 15, which represents 39% of total articles, in 2019.

Figure 1. Total of articles published and annual citations in the period 2012-2019.

It should be highlighted that there is a growing interest on this subject since 2018 (8 articles), when the number of annual articles doubles. In 2015, there was a marked increase regarding citations: from an average of 4 annual citations to 92, becoming the year with the greatest number of citations in the period under discussion, since one of the most cited articles (65 citations) belongs to that year. Since that moment, there have been variations, reductions and slight increases, reaching 39 citations in 2019. The first article published in 2012 is entitled “Energy consumption, resource utilization and environmental protection in Beijing - Practice and challenges,” with one citation, and the last article on this subject, which is published in November 2019, is “Recycling of end-of-life reverse osmosis membranes: Comparative LCA and cost-effectiveness analysis at pilot scale,” not cited yet. The most cited article (65) is from 2015, followed by another one from the same year with 27 citations (Table 1). The total count of citations of the ten articles appearing in Table 1 (225) represents 88% of total citations.

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Table 1. Most cited articles in the period 2012-2019 A AN TC Y Quantitative assessment of industrial Wen, Z., Meng, X. 65 2015 symbiosis for the promotion of circular economy: A printed circuit boards industry in China's Suzhou New District. Life Cycle Assessment from food to food: Strazza, C., Magrassi, F., 27 2015 A case study of circular economy from Gallo, M., Del Borghi, A. cruise ships to aquaculture. Mapping Industrial Symbiosis Domenech, T., Bleischwitz, R., 25 2019 Development in Europe_ typologies of Doranova, A., Panayotopoulos, networks, characteristics, performance and D., Roman, L. contribution to the Circular Economy. Towards a Circular Economy in Australian Pagotto, M., Halog, A. 22 2016 Agri-food Industry: An Application of Input-Output Oriented Approaches for Analyzing Resource Efficiency and Competitiveness Potential. Supporting phosphorus management in Zoboli, O., Zessner, M., 21 2016 Austria: Potential, priorities and Rechberger, H. limitations. What gets measured, gets done: Nuñez-Cacho, P., Górecki, J., 17 2018 Development of a Circular Economy Molina-Moreno, V., Corpasmeasurement scale for building industry. Iglesias, F.A. Design of indicators of circular economy as Molina-Moreno, V., Leyva15 2017 instruments for the evaluation of Díaz, J.C., Llorens-Montes, sustainability and efficiency in wastewater F.J., Cortés-García, F.J. from pig farming industry. The low-entropy city: A thermodynamic Pelorosso, R., Gobattoni, F., 12 2017 approach to reconnect urban systems with Leone, nature. Eco-efficiency indicator framework Rönnlund, I., Reuter, M., Horn, 11 2016 implemented in the Metallurgical industry: S., (...), Ylimäki, L., Pursula, T. part 2 - a case study from the copper industry. Proposal of sustainability indicators for the Molina-Sánchez, E., Leyva10 2018 waste management from the paper industry Díaz, J. C., Cortés-García, F. J., within the circular economy model. Molina-Moreno, V., A: article name; AN: name of authors; TC: total number of citations; Y: year of publication of journals.

J Journal of Cleaner Production

Sustainable Production and Consumption Resources, Conservation and Recycling Journal of Industrial Ecology

Science of the Total Environment Sustainability (Switzerland) Water (Switzerland)

Landscape and Urban Planning International Journal of Life Cycle Assessment Water (Switzerland)

the article; J: name of

Distribution of Publications per Subject Category Between 2012 and 2019, the scientific production on indicators of circular economy and water is grouped around five subject categories. The area of Environmental Science represents the main category (76%), with 29 of the total articles (Figure 2). This category has experienced a growing evolution since 2014, acquiring more representative importance since 2017. Since 2012, the second category, Engineering, has maintained itself as one of the categories where a great number of articles are cataloged (26%), with the exception of 2013 and 2017. The area of Social Sciences, with 24% of articles published, has had a growing tendency, mainly since 2017.

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Figure 2. Comparison of growth trends of the subject categories in the research (2012-2019).

Subject categories are useful when it comes to classifying articles in specific journals that deal with this research topic, although its approach will vary depending on each journal. The top five journals publishing 34% of analyzed articles (Resources Conservation and Recycling, Sustainability, Water, Journal of Cleaner Production, Science of the Total Environment) have sustainable management and conservation of natural resources as their main subject.

Evolution of Indicators of Circular Economy Several studies have designed classifications of indicators of circular economy. Table 2 shows various classifications according to different authors. Table 2. Indicators of circular economy for water management [8-11] Code A A1 A2 B B1 B11 B12 B13 B14 B15 B2 B21 B22 B23 B3 B31 C C1 C2

Indicator Abstraction Percentage of water abstracted directly by users with respect to total amount of abstracted water Percentage of desalted water with respect to total amount of abstracted water Supply Use of energy and raw materials Amount of energy used per cubic meter of water Percentage of energy coming from green and renewable sources Amount of energy generated by water services Carbon footprint produced by water supply Use of natural resources for water treatment Infrastructure Leakage in water systems Kilometers of dual water distribution (water supply from different sources depending on the purpose) Materials used for the creation of infrastructures and equipment for water treatment Economic (investment and cost in the water sector) Investment in new infrastructure and equipment Water use Total volume of water used (or registered) Use of water per unit of reference

Development of Indicators of Circular Economy and Their Application … Code C3 D D1 D11 D12 D13 D14 D2 D21 D22 D23 D3 D31 E E1 E11 E12 E13 E2 E21 E3 E31 F F1

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Indicator Water footprint Sanitation and reuse Impacts Volume of wastewater treated Percentage of wastewater treated and reused Volume of reused water Destination of treated water Efficiency Use of energy and raw material per unit of wastewater treated and reused Use of by-products resulting from wastewater treatment Percentage of sludge that is used and its destination Infrastructure and economic Investment in treatment, reutilization and cost Supply Impacts indicators Volume of water for supply Volume of treated wastewater for supply Source of water for supply Efficiency indicators Use of energy and raw material per unit of water for supply Infrastructure and economic Investment in water abstraction, supply and cost Indicators of water environmental condition Environmental condition of water bodies

Table 3 shows how these indicators have been reflected in several scientific studies, between 2014 and 2019. Table 3. Evolution of indicators of circular economy for water management 2014

2015

2016

Strazza et al., 2015 Wen, & Meng, 2015

Rönnlund et al., 2016

A1 A2 B11

B12 B13

B14

Strazza et al., 2015 Wen, & Meng, 2015

Zhao, & Ma, 2014

Strazza et al., 2015 Wen, & Meng, 2015

2017 Laner et al., 2017 Laner et al., 2017

Rönnlund et al., 2016 Rönnlund et al., 2016 Zoboli et al., 2016

Laner et al., 2017

Osorio et al., 2016 Pagotto, & Halog, 2016 Rönnlund et al., 2016 Zoboli et al., 2016

MolinaMoreno et al., 2017 Pelorosso et al., 2017

2018 Dominguez et al., 2018

2019 Gravagnuolo et al., 2019 Oliveira et al., 2019 Oliveira et al., 2019

GarcíaBustamante et al., 2018 Nuñez-Cacho et al., 2018

Ignacio et al., 2019 Oliveira et al., 2019 Kiselev et al., 2019 Rapsikevičienė et al., 2019 Gravagnuolo et al., 2019 Kiselev et al., 2019 Gravagnuolo et al., 2019 Ignacio et al., 2019 Kiselev et al., 2019 Oliveira et al., 2019 Rapsikevičienė et al., 2019 Tretyakova, 2019 Domenech et al, 2019 Kiselev et al., 2019 Niero, & Kalbar, 2019 Rapsikevičienė et al., 2019 Roychand et al., 2020 (*)

GarcíaBustamante et al., 2018 Nuñez-Cacho et al., 2018

MolinaSánchez et al., 2018 Zhong et al., 2018

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Juan Carlos Leyva-Díaz, Valentín Molina-Moreno, Jorge Sánchez-Molina et al. Table 3. (Continued)

B15

2014

2015

2016

Zhao, & Ma, 2014

Huang, 2015

Osorio et al., 2016 Rönnlund et al., 2016 Zoboli et al., 2016

Dominguez et al., 2018 Nuñez-Cacho et al., 2018 Zhong et al., 2018

Wen, & Meng, 2015

Osorio et al., 2016

Nuñez-Cacho et al., 2018

B21

2017

2018

B22 B23

B31

Strazza et al., 2015

Pagotto, & Halog, 2016

C1

C2

C3

D11

Zhao, & Ma, 2014

MolinaMoreno et al., 2017

GarcíaBustamante et al., 2018 MolinaSánchez et al., 2018

Laner et al., 2017

Nuñez-Cacho et al., 2018

GarcíaBustamante et al., 2018 Xiao et al., 2018 MolinaSánchez et al., 2018 NuñezCacho et al., 2018 Xiao et al., 2018 Dominguez et al., 2018

Huang, 2015

Osorio et al., 2016

Laner et al., 2017 Pelorosso et al., 2017

Huang, 2015 Wen, & Meng, 2015

Osorio et al., 2016 Pagotto, & Halog, 2016 Rönnlund et al., 2016 Zoboli et al., 2016

MolinaMoreno et al., 2017

Strazza et al., 2015

D12

D13

D14

Huang, 2015

Zoboli et al., 2016

Laner et al., 2017

Osorio et al., 2016

Pelorosso et al., 2017

Cobo et al., 2018 Dominguez et al., 2018 Dominguez et al., 2018

Dominguez et al., 2018 Nuñez-Cacho et al., 2018

2019 Senán-Salinas et al., 2019 Simon, 2019 Tretyakova, 2019 Aravossis et al., 2019 Gravagnuolo et al., 2019 Rapsikevičienė et al., 2019 Senán-Salinas et al., 2019 Tua et al., 2019 Domenech et al., 2019 Oliveira et al., 2019 Domenech et al., 2019 Oliveira et al., 2019 Domenech et al., 2019 Roychand et al., 2020 (*) Domenech et al, 2019 Kayal et al., 2019 Micari et al., 2019 Niero, & Kalbar, 2019 Rapsikevičienė et al., 2019 Gravagnuolo et al., 2019 Oliveira et al., 2019 Senán-Salinas et al., 2019 Aravossis et al., 2019 Oliveira et al., 2019 Senán-Salinas et al., 2019 Ignacio et al., 2019 Rapsikevičienė et al., 2019 Simon, 2019 Tretyakova, 2019 Micari et al., 2019 Oliveira et al., 2019 Senán-Salinas et al., 2019 Micari et al., 2019 Oliveira et al., 2019

Micari et al., 2019 Oliveira et al., 2019 Senán-Salinas et al., 2019. Aravossis et al., 2019 Niero, & Kalbar, 2019 Senán-Salinas et al., 2019 Tretyakova, 2019

Development of Indicators of Circular Economy and Their Application …

D21

2014 Zhao, & Ma, 2014

D22

2015 Huang, 2015 Huang, 2015

2016 Osorio et al., 2016 Rönnlund et al., 2016 Pagotto, &Halog, 2016 Rönnlund et al., 2016

2017 Pelorosso et al., 2017

Cobo et al., 2018 Zhong et al., 2018

D23

D31

Strazza et al., 2015 Wen, & Meng, 2015

Pagotto, & Halog, 2016 Rönnlund et al., 2016

MolinaMoreno et al., 2017

E11

Zoboli et al., 2016

Laner et al., 2017

E12

Zoboli et al., 2016

Laner et al., 2017

Strazza et al., 2015 Wen, & Meng, 2015

Pagotto, & Halog, 2016

Laner et al., 2017 Pelorosso et al., 2017

Huang, 2015. Strazza et al., 2015

Osorio et al., 2016 Pagotto, & Halog, 2016 Rönnlund et al., 2016 Zoboli et al., 2016

MolinaMoreno et al., 2017. Pelorosso et al., 2017

Strazza et al., 2015 Wen, & Meng, 2015

Pagotto, & Halog, 2016 Rönnlund et al., 2016

MolinaMoreno et al., 2017

E13

E21

E31

Zhao,& Ma, 2014

2018

Cobo et al., 2018 Dominguez et al., 2018 MolinaSánchez et al., 2018 NuñezCacho et al., 2018 Xiao et al., 2018

GarcíaBustamante et al., 2018 Zhong et al., 2018 Cobo et al., 2018 Zhong et al., 2018 GarcíaBustamante et al., 2018 Xiao et al., 2018 GarcíaBustamante et al., 2018 MolinaSánchez et al., 2018 Nuñez-Cacho et al., 2018 Xiao et al., 2018 Zhong et al., 2018 GarcíaBustamante et al., 2018 MolinaSánchez et al., 2018 Nuñez-Cacho et al., 2018 Xiao et al., 2018

75

2019 Ignacio et al., 2019 Roychand et al., 2020 (*) Aravossis et al., 2019 Tua et al., 2019 Micari et al., 2019 Tua et al., 2019

Gravagnuolo et al., 2019 Kayal et al., 2019 Micari et al., 2019 Oliveira et al., 2019 Rapsikevičienė et al., 2019 Roychand et al., 2020 (*) Ignacio et al., 2019 Micari et al., 2019 Oliveira et al., 2019 Senán-Salinas et al., 2019 Micari et al., 2019 Oliveira et al., 2019 Senán-Salinas et al., 2019 Ignacio et al., 2019 Micari et al., 2019 Oliveira et al., 2019 Rapsikevičienė et al., 2019 Aravossis et al., 2019 Ignacio et al., 2019 Kiselev et al., 2019 Niero, & Kalbar, 2019 Roychand et al., 2020 (*) Tua et al., 2019

Gravagnuolo et al., 2019 Micari et al., 2019 Kayal et al., 2019 Rapsikevičienė et al., 2019 Roychand et al., 2020 (*) Tua et al., 2019

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Juan Carlos Leyva-Díaz, Valentín Molina-Moreno, Jorge Sánchez-Molina et al. Table 3. (Continued)

F1

2014 Zhao, & Ma, 2014

2015 Huang, 2015 Strazza et al., 2015 Wen, & Meng, 2015

2016 Albertario, 2016 Pagotto, & Halog, 2016 Osorio et al., 2016 Rönnlund et al., 2016 Zoboli et al., 2016

2017 MolinaMoreno et al., 2017

2018 Cobo et al., 2018 MolinaSánchez et al., 2018 Xiao et al., 2018 Zhong et al., 2018

2019 Gravagnuolo et al., 2019 Ignacio et al., 2019 Kiselev et al., 2019 Niero, & Kalbar, 2019 Rapsikevičienė et al., 2019 Roychand et al., 2020 (*) Simon, 2019 Tretyakova, 2019 Tua et al., 2019

(*) Published in 2019.

METHODOLOGY These bibliometric analysis tools will enable organizing the information regarding this research. In order to do that, it will be necessary to access the information available at the repositories of international scientific information, such as Scopus database. This database is chosen since it is the largest repository of scientific articles in relation to both authors and scientific journals. This research methodology is in line with other studies [12-15]. Once the search was carried out, there was a total of 38 articles, from which it has been possible to obtain information variables about publication years, authors, lists of coauthorships, institutional affiliation, countries and keywords defining the subject of the study. Regarding scientific production indicators, authors’ productivity, countries and institutions were presented taking into account both the total number of papers published on each subject and the citation count. In addition, by using the tool VOSviewer (version 1.65 – Leiden University, The Netherlands) it is possible to present the network maps reflecting the collaboration between authors and countries as well as research trends based on keyword analyses. Network maps, which are especially suitable for studies based on bibliometric analysis, have become a widely used technique in order to process and group words [12, 16, 17].

RESULTS AND DISCUSSION Author’s Productivity, Collaborations and Countries The main characteristics about the authorship of the scientific production that has been published about Indicators of circular economy for water management are presented in Table 4. It is remarkable that among the five authors with the greatest number of publications on the subject, two of them are Spanish. Valentín Molina Moreno, a researcher from the University of Granada, is at the top of the list with the greatest number of articles (3) and citations (41). His most cited article [7] is “What gets measured, gets done: Development of a Circular

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Economy measurement scale for building industry,” from 2018. In total, 140 authors have published on this subject. The five most important researchers have contributed with 11 articles (29% of the total production under analysis) and 56% of total citations, a low percentage that clearly indicates the multiplicity and diversity of authors contributing to this subject. Table 4. Authors with the greatest number of articles in the period 2012-2019 Authors A TC TC/A Insitution C 1st A Last A Molina-Moreno, V 3 41 13.67 University of Granada Spain 2017 2018 Cortés-García, F. J 2 24 12.00 Autonomous University of Chile Chile 2017 2018 Leyva-Díaz, J. C 2 24 12.00 University of Oviedo Spain 2017 2018 Rechberger, H 2 27 13.50 Technische Universitat Wien Austria 2016 2017 Zoboli, O 2 27 13.50 Technische Universitat Wien Austria 2016 2017 A: number of articles; TC: number of citations for all articles; TC/A: number of citations by article; C: country.

H index 8 4 13 27 7

The analysis of the main articles written by these authors evinces the preference of interaction and articulation between authors of the same nationality and/or from the same institution (Figure 3).

Figure 3. Map of collaboration between the main authors.

Italy leads scientific production, with 21% of total published articles coming from this country (Table 5). China stands second, with seven articles, registering the greatest number of citations and Spain is in third place, with six articles and 49 citations. Table 5. Countries with the greatest number of publications in the period 2012-2019 Country A TC TC/A H-index Italy 8 46 5.75 3 China 7 79 11.29 3 Spain 6 49 8.17 4 Australia 2 21 10.50 1 Austria 2 27 13.50 2 A: number of articles; TC: number of citations for all articles; TC/A: number of citations by article.

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Table 6 shows the main collaborations between countries for the publication of research papers. Table 6. Main international collaborations in the period 2012-2019 Country

NC

Main collaborators

IC

TC/A IC NIC Spain 3 Chile, Australia, Poland 50.0% 13.67 2.67 Italy 3 China, Germany, Russian Federation 37.5% 3.67 7.00 Australia 1 España 50.0% 0.00 21.00 China 1 Italy 14.3% 8.00 11.83 Austria 0 0.0% 0.00 13.50 NC: number of collaborators; IC: percentage of articles made with international collaboration; TC/A: number of citations by article; IC: international collaboration; NIC: no international collaboration.

Spain is at the top of the list (50%). Half of the articles has been published with countries in three different continents. Italy has published 37.5% of articles with countries such as Germany, China and Russia (Figure 4).

Figure 4. Map of collaboration between the main countries.

It is important to remark that there is not a direct relation between the number of citations and the articles with international coauthorship. The articles present different numbers regarding the percentage of citations, which does not vary depending on collaborations. In this collaboration network, Europe has a significant representation with the largest number of countries [5]. Within Europe, Spain and Italy lead participation with the greatest contribution: six out of the fourteen articles published in these two countries were in collaboration. It should be highlighted that the institutions working on these publications are mainly universities. Three Spanish universities (University of Granada, University of Jaén and University of Cantabria) are at the top of the list with seven publications.

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Keyword Analysis The term “Circular Economy” was not included among the keywords nor were some indexed keywords, added to the records by Scopus, since it was considered that they did not accurately represent the thematic content of the documents or provide any further relevance to the analysis. Table 7 shows the top fifteen most frequently used keywords in the 38 articles about Circular Economy for Water Management during the period evaluated (2012-2019). Their importance and evolution were analyzed according to the number of documents containing those terms. “Sustainable development” was the most important term in the period, with 18 occurrences (47.4% of total documents). This keyword first appeared in 2012 and continued appearing regularly (except in 2014) until 2019, when it was included in 6 out of the 15 articles that were published that year. Table 7. Main keywords in the period 2012–2019 Keyword

2012-2019 A Sustainable Development 18 Sustainability 8 Life Cycle Analysis 7 Water Management 7 Environmental Impact 6 Industrial Economics 6 Waste Management 6 Economic Development 5 Economics 5 Energy Utilization 5 Environmental Indicator 5 Life Cycle 5 Life Cycle Assessment (LCA) 5 Recycling 5 Wastewater Treatment 5 A: number of articles; %: percentage of articles in which it appears.

% 47.4% 21.1% 18.4% 18.4% 15.8% 15.8% 15.8% 13.2% 13.2% 13.2% 13.2% 13.2% 13.2% 13.2% 13.2%

The term “Sustainability” is in second place, with eight associated articles. It first appeared in 2016 and remained constant until 2019. The third term is “Life Cycle Analysis,” which was included in seven articles. Since 2016, and until 2019, this term has taken part in the main researches. The keyword analysis was carried out based on bibliometric information maps. These keyword co-occurrence maps reflect the most important terms selected by authors and database managers. The descriptors appearing on network maps were selected by the software (VOSviewer), according to the number of occurrences (at least 5) and the strength between words, indicating and representing the strongest relationships by means of lines and groups of different colors (cluster). Three clusters, representing the structure of the 38 articles analyzed, are identified in Figure 5. The first and most important, with 6 terms (red), indicates the key elements of circular economy, such as the area where it focuses, which is mainly industry, since it transforms the greatest amount of raw material into products by using different energy

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sources and generating emissions and waste of various kinds. “Sustainability,” which is the foundation of this economic model, is also highlighted in this cluster. This term emphasizes the integral management of resources as well as the reduction and substitution of nonrenewable inputs in order to obtain economic, environmental and social benefits. Sustainability evaluation is achieved by means of measuring parameters such as “Environmental Indicators,” a key tool when it comes to implementing the circular economy model, thus the importance of this term in the network.

Figure 5. Map of term co-occurrence.

The second cluster (green) shows five terms that clearly identify the commitment to the model of circular economy and boost mechanisms that contribute to an efficient management of resources by fostering the use of secondary raw materials, recycling materials and incorporating waste and/or by-products into the production processes in order to avoid materials loss of value and extend their life. The third and last cluster (blue), which groups 4 terms, reflects the benefits and advantages of implementing the circular economy model: reduction of environmental impacts, production and use of renewable energies and economic benefits (by reducing raw material costs and avoid payments regarding waste and/or byproducts disposal). All these aspects are oriented towards the achievement of sustainable development. Figure 6 represents the network map with a timeline (2017-2018) of the keywords used in the analyzed studies, which allows us to observe in greater detail how some of them have emerged recently, mainly those related to circular economy implementation strategies, resources that are prioritized for further use and treatment as well as follow-up and evaluation tools.

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Figure 6. Timeline map of keyword evolution.

PROPOSAL FOR INDICATORS OF CIRCULAR ECONOMY IN WASTEWATER TREATMENT Introduction Once the state of the art about indicators of circular economy for water treatment has been analyzed, a proposal for indicators of circular economy will be carried out. These indicators will be applied to wastewater treatment coming from a specific sector. As a consequence of the increasingly restrictive environmental legislation, it is necessary to transform wastewater into technological nutrients which allow its transformation into resources and its subsequent reintroduction within the production process, with the aim of minimizing and reducing its environmental impact [18, 19]. A series of general indicators of circular economy is defined below. These permit evaluating the degree of approximation of a specific production process to that model. The definition of those indicators will be applied to different resources that can be recovered during the wastewater treatment process according to the state of that resource (liquid, solid and gas).

Indicators of Circular Economy for the Liquid Phase Firstly, the indicator of technological nutrient performance for the liquid phase is presented (ILP,TN). This indicator allows evaluating the treated water that can be obtained and reused in the production process from the wastewater generated in that process. It can be evaluated according to Equation (1):

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Juan Carlos Leyva-Díaz, Valentín Molina-Moreno, Jorge Sánchez-Molina et al. ILP,TN =

∑n i=1 Qw,i

(1)

Qww

where Qw,i is the water volumetric flow recovered during stage i of the wastewater treatment process and Qww is the volumetric flow of wastewater generated by a specific sector. Secondly, the indicator of circular economy efficiency for the liquid phase (ILP,CE) is presented. Such indicator provides information about the reduction of the water that is consumed in order to carry out a specific manufacturing process. It can be evaluated according to Equation (2): ILP,CE =

∑n i=1 Qw,i Qw,t

· 100

(2)

where Qw,t is the total water volumetric flow consumed during the production process. This indicator can range between 0 and 100%: 0 means that no water was recovered during the process and 100% is the ideal case of sustainability, with no external water consumption.

Indicators of Circular Economy for the Solid Phase Following a process similar to the one in the previous section, two types of indicators are proposed. The first one, the indicator of technological nutrient performance for the solid phase (ISP,TN), provides information about the amount of sludge recovered during the wastewater treatment process that can be reused in the production process depending on the wastewater generated in that sector. It can be evaluated according to Equation (3): ISP,TN =

∑n i=1 ms,i

(3)

Qww

where ms,i is the mass flow of mineral load recovered during stage i of the wastewater treatment process. The second one, the indicator of circular economy efficiency for the solid phase (ISP,CE), can be determined by Equation (4): ISP,CE =

∑n i=1 ms,i ms,t

· 100

(4)

where ms,t is the mass flow of total generated sludge. This indicator supplies information about the amount of sludge recovered during a specific production process in relation to the amount of total generated sludge. It can range between 0 and 100% according to the proportion of recovered sludge.

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Indicators of Circular Economy for the Gas Phase As in the case of liquid and solid phases, it is possible to define two indicators for the gas phase. The indicator of technological nutrient performance for the gas phase (IGP,TN) indicates the biogas volumetric flow recovered during the wastewater treatment process depending on the wastewater generated by a specific sector, according to Equation (5): IGP,TN =

Qbg

(5)

Qww

where Qbg is the biogas volumetric flow recovered during the wastewater treatment process. In relation to the indicator of circular economy efficiency for the gas phase (IGP,CE), it provides information about the reduction of natural gas consumption during a specific industrial process. That indicator can range between 0 and 100% depending on the supply level of the biogas generated. Equation (6) shows the mathematical form of this indicator. IGP,CE =

Qbg Qng,t

· 100

(6)

where Qng,t is the natural gas volumetric flow consumed in a specific production process.

Application in Paper and Pig Industries Both paper and pig industries generate a great amount of wastewater, which causes a severe impact on the environment and poses a risk for the humans and fauna of the place [2022]. Table 8 shows the different indicators of circular economy in wastewater treatment coming from paper and pig industries. Table 8. Different indicators of circular economy in wastewater treatment coming from paper and pig industries Indicator of circular economy I LP,TN

Paper industry

Pig industry

References

0.90 m3 water m-3 paper mill wastewater

0.97 m3 water m-3 pig manure

Molina-Moreno et al., 2017; Molina-Sánchez et al., 2018

I LP,CE I SP,TN

85.10% 0.70 kg sludge m-3 paper mill wastewater

47.01% 49.40 kg biofertilizer m-3 pig manure

I SP,CE I GP,TN

39.70% -

4.75% 5.33 m3 biogas m-3 pig manure

I GP,CE

-

5.33%

Molina-Moreno et al., 2017; Molina-Sánchez et al., 2018

Molina-Moreno et al., 2017

Consequently, wastewater can be considered as a technological nutrient which can later be reintroduced into the production process, allowing reusing the resources that it contains.

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These indicators offer new measuring tools to each and every production sector so that they become a reference in the area of sustainable production, thus reducing the negative externalities of industrial processes. Taking these indicators of circular economy into account, decision-makers from both production sectors and public administrations can incorporate them to their sustainability model. This can facilitate the transition toward the circular economy model, minimizing waste generation and improving the efficiency in the use of resources.

REFERENCES [1]

Ozsabuneuoglu, I. H. (1996) Evaluation of Negative Externality by Pollutees. Environment and Planning C: Government and Policy 14(IV): 489–500. [2] Plaza-Úbeda, J. A., De Burgos-Jiménez, J. and Belmonte-Ureña, L. J. (2011) Stakeholders. Environmental management and performance: An integrated approach. Cuad. Econ. Dir. Empresa 14: 151–161. [3] Lieder M. and Rashid A. (2016) Towards Circular Economy implementation: A comprehensive review in context of manufacturing industry. Journal of Cleaner Production 115(I): 36– 5. [4] Aznar-Sanchez, J. A., Belmonte-Ureña, L. J., Velasco, J. F. and Manzano-Agugliaro, F. (2019) The worldwide research trends on water ecosystem services. Ecological Indicators 99: 310-323. [5] Honoré, M. N., Belmonte-Ureña, L. J., Navarro-Velasco, A. and Camacho-Ferre. F. (2019) Profit analysis of papaya crops under greenhouses as an alternative to traditional intensive horticulture in southeast Spain. Int. J. Environ. Res. Public Health 16: 2908. [6] Torres, J., Valera, D. L., Belmonte, L. J. and Herrero-Sánchez, C. (2016) Economic and social sustainability through organic agriculture: Study of the restructuring of the citrus sector in the “Bajo Andarax” District (Spain). Sustainability 8: 1–14. [7] Nuñez-Cacho, P., Górecki, J., Molina-Moreno, V. and Corpas-Iglesias, F. A. (2018) What Gets Measured, Gets Done: Development of a Circular Economy Measurement Scale for Building Industry. Sustainability 10: 2340. [8] CONAMA. Congreso Nacional de Medio Ambiente. https:// www.miteco.gob.es/es/ ceneam/recursos/pag-web/documentos/conama.aspx. [9] EUROSTAT. Which indicators are used to monitor the progress towards a circular economy? https://ec.europa.eu/eurostat/web/ circular-economy/indicators. [10] Molina-Moreno, V., Leyva-Díaz, J., Llorens-Montes, F. and Cortés-García, F. (2017) Design of indicators of circular economy as instruments for the evaluation of sustainability and efficiency in wastewater from pig farming industry. Water 9(IX): 653. [11] Molina-Sánchez, E., Leyva-Díaz, J., Cortés-García, F. and Molina-Moreno, V. (2018) Proposal of sustainability indicators for the waste management from the paper industry within the circular economy model. Water 10(VIII): 1014. [12] Abad-Segura, E., Cortés-Garcia, F. J. and Belmonte-Ureña, L. J. (2019) The Sustainable Approach to Corporate Social Responsibility: A Global Analysis and Future Trends, Sustainability 11(IX): 5382.

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[13] Zhang, L., and Eichmann-Kalwara, N. (2019) Mapping the Scholarly Literature Found in Scopus on “Research Data Management”: A Bibliometric and Data Visualization Approach. Journal of Librarianship and Scholarly Communication 7(I). [14] Veer, D. K. and Khiste Gajanan, P. (2017) Digital Library Output in Scopus during 1995-2016: A Bibliometric Analysis. International Journal of Scientific Research in Computer Science, Engineering and Information Technology 2(V): 779-784. [15] Durieux, V. and Gevenois, P. A. (2010) Bibliometric indicators: Quality measurements of scientific publication 1. Radiology 255: 342–351. [16] Sedighi, M. (2016) Application of word co-occurrence analysis method in mapping of the scientific fields (case study: the field of Informetrics). Library Review 65(1/2): 5264. [17] Van Eck, N. J., and Waltman, L. (2007) Bibliometric mapping of the computational intelligence field. International Journal of Uncertainty, Fuzziness and KnowledgeBased Systems, 15(V): 625-645. [18] Molina-Moreno, V., Leyva-Díaz, J. C. and Sánchez-Molina, J. (2016) Pellet as a Technological Nutrient within the Circular Economy Model: Comparative Analysis of Combustion Efficiency and CO and NOx Emissions for Pellets from Olive and Almond Trees. Energies 9(X): 777. [19] Argudo-García, J. J., Molina-Moreno, V. and Leyva-Díaz, J. C. (2017) Valorization of sludge from drinking watertreatment plants. A commitment to circular economy and sustainability. Dyna 92: 71–75. [20] Liu, X. and Xiao, X. (2016) The optimization of cyclic links of live pig-industry chain based on circular economics. Sustainability 8: 26. [21] Pellegrin, V., Juretschko, S., Wagner, M. and Cottenceau, G. (1999) Morphological and biochemical properties of aSphaerotilus sp. isolated from paper mill slimes. Appl. Environ. Microbiol 65: 156– 162. [22] Pokhrel, D. and Viraraghavan, T. (2004) Treatment of pulp and paper mill wastewater—A review. Sci. Total Environ. 333: 37–58.

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Abad-Segura, E., Cortés-Garcia, F. J. and Belmonte-Ureña, L. J. (2019) The Sustainable Approach to Corporate Social Responsibility: A Global Analysis and Future Trends, Sustainability 11(IX): 5382. Albertario, P. (2016) System of self-financing strategy for the policies aimed at the eco-innovation in the productive sectors. Procedia Environmental Science, Engineering and Management 3(I). Aravossis, K. G., Kapsalis, V. C., Kyriakopoulos, G. L., Xouleis and T. G. (2019) Development of a Holistic Assessment Framework for Industrial Organizations. Sustainability 11(XIV): 3946. Argudo-García, J. J., Molina-Moreno, V. and Leyva-Díaz, J. C. (2017) Valorization of sludge from drinking water treatment plants. A commitment to circular economy and sustainability. Dyna, 92: 71–75.

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In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 5

THE PRESENT CONTRIBUTION OF CIRCULAR ECONOMY TO STIMULATE ECONOMIC GROWTH IN THE WORLD L. Marsullo Finpublic & Finenergie Co., Rome, Italy

ABSTRACT The fast increase of the world population in the last thirty years has led to a wild exploitation of the planet's resources which are becoming increasingly inadequate to meet its needs. The circular economy, based on long lasting products and recycling and reuse of raw materials, it is the only possible way to satisfy the needs of the world population without depleting the planet and its resources. First of all it is necessary a drastic change in people mentality after years of unbridled consumerism; then, all the production systems must be adapted to the new economy: two very ambitious goals, not easy to achieve. This is strategically important, considering the present status of the economy, which is oriented towards an “Immaterial Capitalism with the application of digital technologies in the new social conflict”. The contribution of circular economy to Stimulate economic growth.

INTRODUCTION In the last few years CIRCULAR ECONOMY has become a very important topic discussed by economists in association with political agencies, such as international organization like United Nations, OECD, European Commission and various international banks, representing a response for a sustainable growth [1-4]. Linear economy, in fact, has

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Corresponding Author’s Email: [email protected].

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created and continue to create high inequalities and rinsing levels of food insecurity and undernourishment, affecting the quality of life of million people [5]. Certainly, to expand circular economy it is essential to take advantage of the multiple benefits of renewable energy. In fact, renewable energy provides many benefits, both direct and indirect, to facilitate the expansion of circular economy. Renewable energies play, in fact, a basic role in the development of the present socioeconomic and industrial structures among the most important benefits to achieve a sustainable development of industrial as well developing countries. The diffusion of renewable energy has promoted since second half of last decade an increasing development of new sources of production in all sectors such as agriculture, agricultural industry, industry and advanced industries, almost everywhere in the world. Such widespread diffusion of investment in renewable energies has provided an increasing production in various sector such as transport sector, thermal sector and of course electric sector. In the last fifteen years the contribution of aeolian energy has increased and then remained stable. The solar energy has increased of about 10%. [6, 7, 8].

THE POSSIBLE BASIS FOR THE CIRCULAR ECONOMY These is no doubt that the economic growth of our planet has increased considerably in the last one hundred years at an increased speed, soon after the Second World War. This development has been confused and fast: every country producing almost everything with no planning. Just as an example, each EU citizen generates more than 4.5 tonnes of waste annually and almost half of it is disposed of in landfill sites! [1, 2].Today we are in presence of a mature economy of the world. In fact, few decades ago some economists considered seriously that the economic development of our world had increased so much and at a systemic growth rate to suggest that probably the world development was so mature in presence of a rate of growth ZERO, to necessary to consider the globalization of the economy a necessary step. We have been very critical of the so widespread consideration about the globalized economy. In fact, if we consider carefully the trends of many sector and many countries of the world, we have to consider globalization as a necessary step after which it is now much more important to proceed with a “specialization” economy. It is not difficult to underline that the globalization economy has been only an intermediate step which has now been bypassed by some clear evidence at world level. The globalization has been used to show the various problems of a mature growth development close to ZERO RATE [9].

PRESENT SITUATION Among the principal problems stressed by the globalization these is the identification that the world cannot go on and proceed with a clear specialization era. In short, all countries of the world, past the globalization era, have now to identify and determine their needs and choices by a programmed economy. In short, every single country has to consider carefully the new social public and private choices which will determine the shape of a New Past

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Globalization Era. Once problems and solutions have been identified, it will be necessary to admit that after the “globalization era”, it is now time to reconsider the hidden advantages of a circular economy, envisaged by the globalization period. These hidden advantages represent a new production approach which we can call: circular economy. The circular economy, therefore, is represented by the complex of the hidden advantages which now is time to identify seriously and implement in an efficient and not expensive economy. This new approach of a worldwide circular economy demonstrates that is clear that, after globalization, every single country has to develop its own plan and strategy within this new concept utilizing hidden technologies available at a low cost. In simple terms we like to stress that now every single country, after the productive problems of globalization – have to proceed in a new economy in a new direction. A new approach has to be utilized in an economic way using the existing hidden and not utilized opportunities of the world. Let us make a simple example. For instance, every single country has to realize that now it is no more time to proceed every country with the same and old pattern of industrial production. Every single country must admit that it is no more convenient to produce the same old pattern of industrial production as in the past. A good example is the automobile industry sector. Now for every single country is no more convenient to produce what they need but must produce what it would be possible to produce in a new global contest of distribution, according to opportunities of a circular economy at a planetary level of specialization. The automobile industry sector has already, demonstrated that now after the globalization period the world has to proceed with specialization in a new contest of circular economy and specialization. That is to say that is quite clear now that it is wrong and not economic for every single country developing its own automobile industry. Already we assist to a diffused widespread pattern development at world level of the various national automobile industries in large multinational companies merging in groups larger, more powerful commercial and economically and specialized as a result of the application of the scale economy [10-14]. At beginning of the 20 century there were 5 industries producing cars; that after 50 years soon after the Second World War the national automobiles industries increase to about fifty industries. Now from the beginning this new 21 century the twenty years gone have demonstrated that automobile industries will decrease to about 20 groups at world level and later to about 10 - 15 lines of production within the concept of a multinationals groups such as. Italy, USA, France, Japan, Germany, etc., this is exactly the approach of circular economy at world level and for a single sector where specialization imposes to produce and select production in an economic context not of the need of every single country in a new economic strategy scale in economy concept at world level. Collaboration among countries with different specialization increase the different know-how in a wide range of sectors but not in automobile industries. The demonstration of this assumption has been that in the last 20 years many national automobile companies have disappeared and merged in larger groups. This mean that globalization has imposed the diffusion of specialization in a context of worldwide free economy controlled by specialization to implement and achieve the success of the circular economy at a much lower costs and better results [11]. Once this concept of circular economy has been accepted than the world at the whole has to determine policies of every groups of countries, sector by sector. This is a very ambitious goal and program which can be implemented by strengthening the existing international political and economic organization in more efficient bodies from an

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economic point of view. Most likely the existing formal and inefficient international political organization and distribution with a more effective political organization and bodies have to restructure themselves or to be substituted by new organization with effective political force. Thus it will be able to impose the circular economy in every single country to achieve better results and produce more wealth, to fulfill the need and request of the developing countries. In fact this group of countries, which control most of the natural resources of the world, have to combine their industrial capabilities with all other countries in a global contest where every political economic organization has to contribute in an efficient economic way and not only formally. Thus it will be achieved a better result for all those countries which, participating to a new economic development based on these super national organization, will have the possibility to obtain the result of the circular economy. As a consequence, the resources will be fully utilized for the benefit of the humanity. On the whole, perhaps, an example can be considered the organization of the European Union to be designed on new programs and policies at a world efficient economic scale and development level. Only in this way it will be possible to reduce the various gaps between rich and poor countries, agricultural and industrial economies. Between this new economic efficient approach all countries will gain in terms of socio-economic development and education. Also to improve labor prospects of course it is necessary that all countries – one by one – has to understand the advantages of this not socialist economy, but an intelligent economic way to utilize the limited resources of our planet which is becoming more and more smaller and smaller afflicted by economic wars, unemployment and crises caused by limited development with the constant dramatic increase of the rate of development of world population. In 1971 at the headquarter in London at the International Cooperative Alliance, when I was serving as International Secretary for Agricultural Cooperation at world level, in the course of my new responsibility and role I delivered a speech as a master lesson on “The prospects in 1971 of economic development and growth of the world population”. A short summary was published in the press of I.C.A [9] in London UK. New Delhi in India was what I stressed on that occasion, underlining that at the world level there was an urgent need to consider the rapid increase of population in the next few years. In my view I prospected that within in the next 30 years the population at the time (1971) estimated in about 3 billion people would double and reach by year 2000 6 billion people. Now, in 2019, the population is estimated to be about 7,5 billion people. This dramatic explosion of the increase of population rate has been due to many factors: medical assistance, better food, better conditions of life, etc. This trend will continue in the next decade. The fast increase of the world population has been caused by the need of the poorest countries to produce more children so that they could take care of the old generation. I stressed my opinion in July 1972 [15] in Bombay at the important event “India Forum” in presence of politician and many international representatives of UN Organization. On both events I stressed that the world was developing in a wrong way and I argued that to make sure to secure all people of the planet food, housing, human stability, all countries of the world had to organize themselves in a more economic way as far as the utilization of the limited planet resources and that our world was in need (in 1971/72) of a change of terms more health, food, housing, jobs, social security at world level [9, 15]. As from the United Nations Report, in fact, world population from the actual 7.5 billion will reach 9.8 billion in 2050 and 11.2 billion in 2100 [16].

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In the last 40 years the world surface has not changed: but the increase of population has continued and now there in more need of health, food, housing, jobs and social security especially in developing countries of the world [9]. This lack of efficiency has produced the massive immigration and wars in all countries of the world with the natural follow up of revolution of nations (Venezuela, Mexico, Siria, Libia, African countries, etc) and the following deterioration of collaboration of countries and people of the world [17, 18].

CONCLUSION The circular economy can provide an economic tool to solve many of the mentioned problems. There are at least two important sectors by which, applying the circular economy methods and share strategies, it will possible to solve most of the problems of the world today. These two sectors are 1) energy and 2) finance. Our planet is full of energy at all levels and in every country. The planet itself is the most important natural source and deposit of energy. Energy is essential to produce almost everything and often what is needed is a limited amount of energy resources utilizing new technologies. The second sector which can give impulse to fasten and operate circular economy are the finance [9], resources available at all levels with financing available to all countries so that everyone will have the possibility to utilize the hidden resources of the circular economy. As a first conclusion it is possible to indicate that circular economy can be implemented by everybody using doses of energy and finance. Of course we are in a position to demonstrate by facts and projects that by applying increases quantities of finance and energy the countries of the world will be able to produce in a more economical way food, housing, jobs, social security with less wars and drugs and more education. These proposals were also presented during the collaborations I had in the period ’71-‘86 with F.A.O. (Food and Agricultural Organization) and I.F.A.D. (International Fund of Agriculture Development), where a cost-benefit analysis was developed, as previously reported [7, 8, 11]. The above proposals were illustrated by specific problems regarding Renewable energy, Road Infrastructures, Irrigation and Agricultural Development [8, 10, 11]. Among others conferences, I had the occasion to illustrate the situation and prospects of the energy sector in Italy, submitted and illustrated in 2008 at the Italian Embassy in London and at the United Kingdom Energy Research center in London, on behalf at the Italian Minister of Economic Development [8, 11]. The above conclusions are strategically relevant, considering the present status of the economy, which is oriented towards a “Immaterial Capitalism with the application of digital technologies in the new social conflict” which will produce a “NEW ECONOMIC SOCIAL ORDER”, based on resource conservation and and energy efficiency [19].

REFERENCES [1]

WHO. Circular Economy and Healt: Opportunity and Risks. World Health Organization, 2018, EU office, Copenhagen, Danmark.

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[5] [6] [7]

[8] [9] [10]

[11] [12] [13]

[14] [15] [16] [17]

[18]

[19]

L. Marsullo EC. The Circular Economy. Connecting, creating and conserving value, 2014. EU Publication Office ISBN 978-92-79-37819-2. OECD. The Circular Economy in Cities and Regions, 2019, OECD Report, Centre for Entrepreneurship. www.oecd.org/cfe (Accessed February 17, 2020). UN. Prospects for Economic Growth in 2020 in Hinge on Reducing Trade Disputes and Uncertainty, UN finds. United Nations, Department of Economic and Social Affairs, New York, January 16, 2020. UN. Climate Crisis "affecting quality of life and fueling discontent". United Nations, Department of Economic and Social Affairs, New York, January 17, 2020. Marsullo, L. (2000). Project Financing and Program Management for the Jubilee of 2000, LUISS, Rome, 1997 - 2000. Marsullo, L. (Ed) (2013). Evaluation, Control and Monitoring of Public Investment; with preface by Paolo Savona more times Minister and Professor of Political Economy, Mondadori, Rome; Italy. Marsullo, L. (2014). Efficiency of Public Investment in Italy, Conference, Mondadori, Milano, september. Bullettino of the I.C.A. (1971) London, UK. Marsullo, L. (1987). Economic Evaluation of Public Investment Objects.Higher Institute of Public Administration, Office of the Prime Minister, Mondadori, Milano, Italy. Marsullo, L. (2018). Cost - Benefits Analysis of Public Investment, Mondadori, Rome, Italy. Winch, D. M. (1971). Analytical Welfare Economics, 1971, Pergamon Press, Penguin Books, London. MacArthur, Ellen. (2020). The Circular Economy in Detail Ellen MacArthur Foundationfoundation. www.ellenmacharthurfoundation.org (Accessed February 17, 2020). MacArthur, Ellen. (2013). Toward The Circular Economy. Economic and business rationale for an accelerated transition, Report, Ellen MacArthur Foundation. Marsullo, L. (1972). Bullettin of the I.C.A, New Delhi, India. UN. World Population Ageing 2019. Highlight United, Nations Department of Economic and Social Affairs Population Division, New York, USA. Marsullo, L. (1984). Approccio Metodologico Benefici-Costi per la Valutazione Degli Investimenti in Infrastrutture Stradale [Cost-Benefit Methodological Approach for the Evaluation of Investments in Road Infrastructures]. Seminary, Roma "Sapienza" University, Italy, June 11 - 12. Marsullo, L. (2002). Il Cofinanziamento delle Infrastrutture di Trasporto Alla Luce della Legge Obiettivi [Co-financing of Transport Infrastructures In the Light of the Objectives Law], Rivista Trimestrale Sistemi di Trasporto, Rome, Itay. Ecosense. (2012). Resource Efficiency Challenge, Forum for Sustainable Development, Ecosense Report, Berlin, Germany.

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 6

CIRCULAR ECONOMY FOR A HEALTHY LIVING ENVIRONMENT P. Morganti1,2, and G. Tishchenko3 1

ISCD Nanoscience Center, Rome, Italy China Medical University, Shenyang, China 3 Institute of Macromolecular Chemistry of the Academy of Sciences, Praha, Czech Republic 2

ABSTRACT Food processing and food loss, which generate from 45% to 59% of the total waste further increased by industrial by-products and plastic materials, created a great environmental pollution on lands and oceans, no more sustainable. Thus the necessity to use this waste, considering it not as a simple loss but as an interesting richness. Redesigning goods and tissue production to facilitate their recycling, remanufacturing, and reusing has to be considered a necessity for preserving the natural raw materials for the future generations. Natural polymers, such as chitin and lignin, obtainable from food and agro-food waste, as well as bio-polyesters such as polylactic acid (PLA) and Polyhydroxyalcanoates obtained from renewable resources, have been proposed to produce biodegradable products. By these natural polymers it is possible to produce biodegradable films and non-woven tissues which, characterized for their structure ECMlike, may be used in the medical and cosmetic fields. The different activity of these tissues is due not only to the different productive methodology adopted but also to the selected active ingredients embedded into their fibers. It is, in fact, possible to bound to the fibers various ingredients, able to slow down the aging processes or reduce the inflammation phenomena and repair the skin affected by burns or wounds. The effectiveness of these innovative tissues, made prevalently by chitin and lignin, has been reported by the results of the first feasibility research studies conducted in vitro and in vivo on burned skin. In conclusion, redesigning, reproducing, reusing and producing goods obtained by the use of their biodegradable natural polymers, it seems possible to reduce or eliminate the greenhouse gas (GHG) emissions adopting the circular economy' 

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Keywords: polysaccharides, chitin, lignin, natural polyesters, food packaging, waste, pollution, skin scaffold

INTRODUCTION The food sea industry generates between 6 to 8 million metric tons of shrimp and lobster shell waste, while it is estimated that about 1.3 billion tons per year is human food consumption lost or wasted globally every year [1]. The majority of this waste is dumped back into the ocean or into landfills, creating great problems of pollution for the environment [2]. As a consequence, per capita waste by consumers is between 95-115 kg a year in Europe and North America while in sub-Saharian Africa, south and South-Eastern Asia, people throw away no more than 6-11 kg only. According to FAO this global wastage, causing an environmental carbon footprint which impacts on climate, water and biodiversity, could be recycled and used as opportunity for improving food security and production of goods, if opportunely recycled (Figure 1) [3]. Just to remember, a product's carbon footprint is the total amount of greenhouse gas (GHG) emissions emitted throughout its life cycle in kilograms of CO2 equivalents [3]. Thus, the necessity to reduce the food wastage not only to reduce the food cost and bettering its quality, but also to ameliorate the environmental perspective slowing down the GHG emissions.

Figure 1. Food Wastage worldwide (by courtesy of FAO [3]).

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Figure 2. Saving money by the circular economy (by courtesy of Ellen MacArthur Foundation [4]).

It is to underline that the average carbon footprint of food waste is about 500 kg CO2 equivalent, per capita and per year [3]! Apart the prevention measures which occur to reduce or eliminate the food wastage during the production, distribution and consume supply chain, it appears necessary its reuse to obtain raw materials to make goods, according to the circular economy. At this purpose, by a study of Ellen MacArthur Foundation [4] it has been established that applying the circular economy to the actual current business models, 1 trillion USD will be saved by 2025 (Figure 2) [4]. Therefore the necessity to create new products by waste, therefore, is considered an easy method to rethink, reduce, recycle, recover, refurbish, repurpose, remanufacture, reuse and repair, for going towards a circular economy conceptualized as a combination of the 9Rs [5]. The generated waste, in fact depends on the technology used, the nature of raw materials processed and how much of it is discarded at the end of the supply chain. Thus became a must the necessity to consider a new way of living by producing and consuming goods and services more efficiently, possibly at zero waste [6]. At this purpose, the agro-forestry biomass as well as the fishery's by-products can provide a great quantity of raw materials to produce a wide range of innovative value-added products without consuming the precious natural raw materials of our Planet. Beyond the fact that agriculture is responsible for a quarter of the GHG emissions, a better food system can unlock solutions to climate changing, contributing to environmental and health benefits [4]. However cities, where are living around an half of worldwide population are living, can play an important role in sparking a shift to a different food system, becoming centers where food by-products may be transformed in value-added goods. Moreover, marketing food products by appealing people to use more local, available and seasonal ingredients, could increase cities' connection with local farmers, helping their traceability and safety, thus reducing the pollution created from transport from long distances also [4]. It is to underline, in fact, that “for every dollar spent on food, society pays two

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dollars in health, environmental and economic cost.” Just to know, half of these costs are due to the way the food is produced and consumed worldwide, being its global costs estimated in USD 5.7 trillion/year [4]. In conclusion, it should be necessary to use by-products obtained from both agro-forestry and industrial biomass, choosing products coming from recyclable raw materials and marketing fresh food instead of canned ones, using also more recyclable packagings and less non-biodegradable ones. At this purpose from the waste feedstocks and by different methodologies, it is possible to obtain polymeric polysaccharides, such as cellulose starch, pullulan, alginic acid and chitin/chitosan as well as biopolyesters, such as polylactic acid (PLA) and polyhydroxyalkanoates (PHAs and PHBs), based on renewable resources. All these ingredients are natural polymers, 100% biodegradable and biocompatible which may to be used in different industrial fields.

POLYSACCHARIDES Polysaccharides are stable polymers which, providing biomaterials with interesting mechanical properties and aqueous stability, can better withstand different processing conditions, being also easily made into various shapes and sized [7]. They are condensate polymers resulting by a type of covalent linkage known as glycosidic bond, formed between monomeric units of carbohydrates kwon as monosaccharides. However, polysaccharides are the most abundant natural, polymers on the planet, serving as major defensive elements in plants (i.e., cellulose and lignin) and barrier elements in animals(i.e., chitin in arthropods and hyaluronic acid in mammals), or as food storage material (i.e., starch or glycogen). Because of the monosaccharides's stereoisomerism, during the condensation reaction different types of polysaccharides are synthesized, characterized by different properties and functionalities. Thus for the versatility and the possibility to engineering and customizing these natural polymers, it is possible to make, hydrogels, fibers, non-woven tissues and films by innovative and easy technologies, such as micro/nano emulsions, encapsulation, electrospinning and casting for realizing many different products to be used for medical and cosmetic applications also. As consequence, the possibility to develop tissues or films engineered to obtain right interactions between the cellular environment and appropriate and compatible biomaterials, useful for example, to make specialized scaffolds suitable to mimic the human physiology [8]. Due to the vast amount of literature available on polysaccharides, this paper has been restricted on the different use of chitin and chitosan for food, cosmetic, and medical applications.

CHITIN, CHITOSAN AND CHITIN NANOFIBRILS Chitin, easily recovered as waste material, is the second most abundant polysaccharide present in nature after cellulose, unique for its higher content of nitrogen (~7%). It is a composite material of ordered crystalline microfibrils embedded in a matrix of protein and minerals [9]. Like cellulose, in fact, chitin is a long unbranched polymeric chain made of N- acetyl-D-glucosamine units. Found in a crystalline or semi-crystalline form, as the skeletal material of crustaceans and insects, and as component of cell walls of bacteria, mollusks and

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fungi, this polymer works as a resistant material barrier against the environment and parasite aggressions. Its deacetylated molecule is named chitosan (Figure 3).

Figure 3. Chitin and chitosan formule compared to cellulose.

Figure 4. Intra- and inter-molecular hydrogen bonding of chitin (by courtesy of Pillar et al. [10]).

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Figure 5. Chitin needle-like structure at SEM (by Courtesy of Coltelli et al.).

Because of its linear structure with two hydroxyl groups and an acetamide group, chitin is predominantly a crystallin polymer characterized by strong intra- and inter-molecular hydrogen bonding, thus exhibiting high modulus and strength along its axis (Figure 4) [10]. In living tissues, this polymer appears as an ordered semicrystalline hierarchical structure organized in sheets of nanofibrils made by the aggregation of 17-25 chitin chains exhibiting a needle like morphology (Figure 5). These needles are made of more or less pure crystallites containing on their molecule 15% or more amino groups, depending from the industrial productive method. By the industrial methodology adopted and patented by our group it is possible to obtain a 2% suspension of nanofibrils (3 billion/ml) characterized by a mean dimension of 240 x 7 x 5 nm covered by around 15,000 -NH2 groups. Having cationic characteristics, these nanocrystals possess self-assembly capabilities, so that the nanofibrils form micro/nanoparticles in water suspension, when in contact with anionic polymers or molecules, such as Hyaluronic acid and Lignin (Figure 6) [11]. Apart from the amino groups which impart to chitin and chitosan their distinctive biological functions, they have two hydroxyl functionality useful for effecting appropriate chemical modifications [10]. However, both chitin and chitosan are polycationic polymers, odorless, nontoxic, non allergenic, biocompatible, eco-compatible, and easily degraded by human and environmental enzymes to glucosamine, acetyl glucosamine and glucose, used from human cells and environmental microorganisms as food and energy [11]. The degree of deacetylation, that may vary from 60% to 98%, is generally defined as glucosamine/N-acetyl glucosamine ratio. When the percentage of N-acetyl glucosamine is higher than glucosamine, the biopolymer is called chitin [12]. Despite its huge annual production and easy availability, chitin still remains an underutilized polymer, also if its fibers have attracted a great attention for their highly promising applications as interesting biomaterials, which can be easily modified into various forms such as films, beads, sponges, and more complex shapes [13]. However, for its antimicrobial, antioxidant, immunomodulating and skin repairing activities, this natural, polymer is finding application in biomedical and tissue engineering [14-16], especially under the form of chitin nanofibrils, able to facilitate the cell adhesion and proliferation, because of their hydrophilic nature, nano size dimension and enhanced biocompatibility.

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Figure 6. Chitin Nanofibril-Hyaluronan (on top) and chitin Nanofibril-lignin (below).

In any way, any kind of polymeric fibers, having diameters between few nanometers up some microns, can be successfully used for a wide variety of applications such as reinforcement in nanocomposites and nanoparticles for packaging purposes [17,18] or as scaffolds for tissue engineering and/or innovative cosmetic applications [19-20]. The harnessing of biomass is, therefore, at the hearth of bioeconomy from the agro-forestry to aquatic feedstocks through the waste streams and new alternative sources, the acquiring and processing of which is essential to achieving success. As a consequence, the role of new technologies and innovative industrial processes, are at the base for improve efficiencies and lower costs of production. Thus, for example, in the cosmetic field results fundamental to minimize the environmental impact by developing products and containers skin-friendly and environmentally-friendly, characterized by their good usability and beautiful design. Naturally, the access to feedstocks and the efficiency of their use have to be evaluated and developed, as well as the safety assessment of both nanoparticles and nanocomposites used have to be incorporated into a designed and innovative network, well programmed and controlled for its effectiveness and safeness by in vitro and in vivo studies [21-23].

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Figure 7. Chitin and hyaluronic acid have the same backbone.

Chitin nanofibrils and chitosan, therefore, are considered the right polymers candidates for the skin scaffolds, showing many advantages over synthetic biomaterials for their stable and porous structure. Moreover, they are easily manipulable by electrospinning and casting technologies, being also free of cytotoxicity with antimicrobial, immunological, and wound healing activities, as previously reported. Additionally, the N-acetylglucosamine moiety of both chitin nanofibril and chitosan is structurally similar to hyaluronic acid (Figure 7). Moreover, their holding specific interactions with the skin growth factors and the specific receptors and adhesion proteins, shearing similar biochemical characteristics with natural tissues, facilitate for example the regeneration of a burned skin [24-25].

SKIN STRUCTURE AND SKIN SCAFFOLD Skin is the largest organ of the human body that, by less than 2 mm of thickness, provides a protective barrier for a lifetime, keeping microbes and environmental chemicals out from essential body fluid and organs (Figure 8) [26]. Such temporal demands require not only a perfect integrity, but also mechanical strength and durability. Skin is a three-layered selfrenewable structure composed by: epidermis, dermis, and sub-cutaneous tissue. The epidermis, by the outmost layer (i.e., Stratum corneum) and the overlapping structure of keratinocytes, prevents moisture and heat loss as well as the bacterial infiltration from the environment, contemporary modulating permeability and transdermal delivery of every substance applied on its intact surface. The dermis, separated from the epidermis at level of the dermal-epidermal junction, is composed by a scaffold gel-structure, named extra cellular matrix (ECM), composed of fibers binding water as a sponge. The collagen and elastin fibers, synthesized from the fibroblast cells which are living into this gel matrix, result necessary to maintain the skin hydration. This complex hydrated structure is indispensable to slow down the aging phenomena, also because active in neutralizing all the environmental assaults, including the sun harmful ultraviolet radiation (UV) and the air toxic nanoparticulate.

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Figure 8. Skin layers and environmental aggressions.

Just to remember, ECM is mainly composed of both polysaccharide chains, called glycosaminoglycans (GAGs) covalently linked to protein in the form of proteoglycans (PGs) (Figure 9), and fibrous proteins, including collagens, elastin, fibronectin and laminin, possess fundamentally a structural and adhesive function [27]. Collagen provides tensile strength, while elastin and other proteins provide the skin elasticity. However, ECM is embedded in a highly negatively charged gel-network made by linear polysaccharides called glycans which bound to yaluronic acid contribute to protect, stabilize, and maintain the skin hydration state with its barrier function [27, 28]. The glycosylation process of cell membrane proteins, during which the N-acetylglucosamine is involved, plays an important role in cell-cell interactions, cell adhesion, proliferation and differentiations swell as in remodeling the ECM, hydration, and antimicrobial activities (Figure 10) [27, 28]. Moreover, it contains cell receptors and enzymes which, regulating gene and protein expression, defines fate and signals of the skin cell [29]. Thus, ECM acts not only as a space filler and a mechanical scaffold for the cells, but also as a bioactive and dynamic environment capable to mediate the cellular functions [30]. Its components, in fact, regulate

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the cell proliferation, survival, differentiation, and migration, being function of the normal aging process, with a decreased and a disorganized distribution of collagen type 1 [29]. Thus the necessity to know and understand composition and structure of the natural ECM for making synthetic scaffolds. These scaffolds may be utilized in tissue engineering applications to repair burn or wound or trying to rejuvenate a prematurely aged skin by the so called regenerative medicine. This medical brunch, in fact, has the aim to recuperate lost or altered tissues by guiding cell growth and restoring the original tissue architecture [31]. At this purpose chitin scaffold, used from other authors also, [32] has been recently used with success by our group to regenerate a burned skin by the use of tissue-scaffolds made by nanochitin-nanolignin' fibers bound to nanoparticles of nanostructured silver [23]. The obtained results have shown this kind of non-woven tissue is able to repair the burned skin in a shorter time, in comparison with the usual products, without provoking any side effect, such as hypertrophic scar or keloid. Moreover, this innovative tissue is totally biodegradable, showing to have a great compatibility with the skin, possessing sufficient mechanical strength and elasticity also. Additionally the presence of N-acetyl glucosamine, as part of the chitin molecule, probably has a specific positive role, being an important component of the glycation phenomena, as previously reported (Figure 10). Finally, it is to underline that all the active ingredients and polymers used to make this tissue have been obtained from waste materials.

Figure 9. Polysaccharides and glycosaminoglycans in ECM.

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Figure 10. Involvement of N-acetylglucosamine in the glycosylation process.

FOOD WASTE AND PACKAGING The Technological advancement in the field of agro-industry has led to the availability of large quantity of agricultural products and waste, so that it has been estimated that the food processing generates 45-59% of the total industrial pollutants [3, 4]. Food production, in fact, derived from agriculture, horticulture, and fisheries processes, represent an increasingly market driven in a contest of population increase, urbanization and climate change. As previously reported, the waste of food processing contains good amount of biodegradable and nutritionally rich material which may be utilized by appropriate and sustainable technologies to produce for example bioplastic nano-composites. Synthetic plastics, in fact, have a negative outcome for the environment because of the great waste invading land and oceans of the planet from many years. Thus it has been estimated that “at least 5.25 trillion individual particles, weighing around 269,000 tonnes, are floating on or near the oceans surface” [33]. Only in Europe, the total production of plastic material is over 60.000 tons per year, ~50% of which remains as waste and toxic material [34]. Therefore, the necessity to develop new polymeric materials derived from renewable sources as the biomass waste previously reported. These new materials can be used to produce bioplastics, biodegradable, ecocompatible with a positive end-life and skin-friendly activity, thus replacing the petrol-based eco-toxic plastics and reducing the actual pollution [35]. For these reasons the European Council are adopting new rules to restrict many single-use plastic items and introduce recycling targets for plastic bottle also [36]. At this purpose, our group proposed the use of chitin and chitosan to make biodegradable and compostable films for food packaging [37]. One of the major problem in the food

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industry, in fact, is its contamination by microorganisms. The principal, aims of modern food processing, therefore, are (a) to make safe food, (b) to provide high-quality product and (c) to prepare convenient packagings [38]. Thus the necessity to avoid contamination and maintain the right flavor and texture by the use of the proposed active packaging, made by chitin nanofibrils and chitosan [17, 18, 37]. The obtained, biodegradable and protective films, in fact resulted useful for extending the product shelf life, and ensuring its microbial safety, naturally maintaining the quality of the packed food. In conclusion, the main purpose of food processing industry in the global economy is to maintain sustainability of the environment also. Mother Nature still plays a decisive role in the global economy, but its reduced resources have to be maintained, reusing recycling or reprocessing the waste biomass [38]. Thus, a healthy ecosystem is fundamental to realize a sustainable development because food production and the consequential waste-generation, affect both resources consumption and the environment contamination [39]. Further knowledge of the biochemical molecules available in the various food processing waste would facilitate exploitation of appropriate biotechnologies for developing new and innovative goods, representing also a solution to the many pollution problems. The reported studies of our work on biodegradable and compostable films are going in this direction as reported successively.

CONCLUSION Circular economy aims not only to eradicate waste but also to find new value by recycling and reusing the industrials and agro-forestry by-products, as previously reported. Current trends in global consumption of natural resources, in fact, being unsustainable and socially unjust have to be changed possibly by public-private partnerships, in line and according to the last European decisions. At this purpose, EU Directive 2008/98/CE on waste sets the basic concepts and definitions to waste management, introducing the “polluter pays principle” and the “extended producer responsibility.” Moreover, it includes waste prevention programs with new recycling and recovery targets to be achieved by 2020 regarding certain materials from households and recovery of construction and demolition waste. Thus, the waste hierarchy has to be considered a must of our society (Figure 11) so that “Living well, within the limits of our planet protecting the environment” is the EU long-term vision and strategy UNTIL 2050. A healthy living environment, therefore, should results from a circulating economy based on no-waste with maintenance of biodiversity. At this purpose, it has been estimated that using innovative technologies along all the value chains could reduce material inputs in EU by up to 24% by 2030, conserving materials embodies in high-value products and reducing demand for primary raw materials [40]. Moreover, measures beyond waste recycling could further reduce GHG emissions so that, implementing the resource-efficiency by circular economy could represent an annually benefit from EU to 245 billion to 604 billion [41]. In conclusion, the transition from a linear economy to the circular economy could be the best way to realize an healthy living with an environment free of waste and pollution. This is our actual challenge.

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Figure 11. Zero Waste Pyramid according to EU rules.

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[40] Meyer, B. (2011) Macroeconomic modeling of sustainable development and the link between the economy and the environment. Final report, ENV.F.2/2910/0033, Osnabruck. [41] AMEC Environment & infrastructure and Bio Intelligence Service: The opportunities to business of improving resource efficiency-Final report on behalf of the European Commission, 2014, Contract Ref. 070307/2011/610181/ETU/F. 1, Northich.

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 7

CIRCULAR ECONOMY IN CHINA Xing-Hua Gao1 and He Cong-Cong2 1

Engineering Research Center for Theranostics of Immunological Skin Diseases, China 2 Dermatological Department, China Medical University, Shenyang, China

ABSTRACT China has done a lot in the development of circular economy promoting principally development of resources, improvement of resource output and reduction of waste generation, all under the control of Chinese government. This paper describes the current state of China’s circular economy and the outlook for the future, especially for its application in the field of biomedicine, where a lot of further work has to be done.

Keywords: circular, economy, agricultural, garbage, biomedicine

INTRODUCTION Since the reform and opening of China in 1978, its economic development has advanced greatly. The development of light industry and heavy industry has gone hand in hand. At present, the Gross National Product of China ranks N°2 in the world, also if this rapid economic development caused unfortunately great sacrifices and deterioration of the natural environment. Moreover, the large population of the Country and the uneven distribution of resources, has been the leading cause to encounter bottlenecks in the early stages of development. Chinese government has been aware of this problem, so that people has improved both in terms of ideological consciousness and actual action. In 2006, China officially listed the circular economy in the “Eleventh Five-Year Plan”, launching the “Circular Economy Promotion Law” in 2008. Moreover, it was fully implemented in 2009 becoming today a fundamental milestone of progress. The comprehensive reutilization rate of wasted products from 2000-2010 had a general upward trend. Thus, by the year 2010, about 60% of the overall solid waste generation had already been reutilized, representing more than 20% of the total resource requirement [1].

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THE STATUS QUO OF CIRCULAR ECONOMY IN CHINA At present, the main feature of China’s development by the circular economy is to promote the development of resources, improve resource output rate and reduce waste generation through government-led tax incentives, resource integration, and green subsidies to achieve relatively loose connect between national economic growth and resource consumption. At moment, energy conservation is the distinctive feature of circular economy [2]. As early as the 19th century, some fields in China made great efforts in the circular economy so that nowadays, the circular economy has penetrated various fields including agriculture, industrial, information technology and even biomedicine. China is a big agricultural country, which has the main base for maintaining the survival and development of the nation. Therefore, maintaining the sustainable development of the agricultural economy is of vital importance, and the agricultural circular economy has become an indispensable part of it. The agricultural recycling economy is mainly based to minimize the development and consumption of resources, reduce the production of waste, and recycle the waste of agricultural resources, to achieve the highest utilization of them. As an ecological economy, the agricultural circular economy actually achieves high-efficiency with a clean production obtained through resource reduction and low-level waste production, as well as a sustainable use of agricultural resources. So doing economic benefits and ecological benefits can be achieved. These economic models are infiltrating into broad rural areas in China, providing indemnification for the people. Under the circular economy system, garbage disposal needs to be taken as an important content, so that garbage separation and recycling is also an important part of its disposal to replace the traditional waste disposal methods, such as sanitary landfills and incineration. In 2017, in fact, the main method of harmless domestic garbage disposal was sanitary landfill, which accounted for 57% of all methods; followed by incineration, accounting for 40%. This is because the scale of the project is large and the investment is low. However, it is necessary to consider the transportation distance, the topography of the landfill site, geological conditions, water pollution, etc. Moreover, the site selection is difficult also because for landfill is necessary a large area cause of secondary pollution. This the reason why this method has rarely been used in foreign countries to dispose of garbage. The incineration method is widely used in developed countries and countries with small land areas, and is relatively mature. The harmless treatment is more thorough, and the generated heat energy can also be utilized for heat supply and power generation for non-recyclable materials, representing no more than 20% of waste. In the field of biomedicine, the application of natural materials has become the main form of the circular economy. One of the example is the natural biological dressings that temporarily replace the damaged skin to act as a temporary barrier, avoiding and reducing wound infection, and providing an environment conducive to wound healing. Recently, many biomaterial medical dressings have gradually replaced traditional dressings which can only provide the simplest isolation protection. The alginate that Winter et al. [3] first studied is a polysaccharide compound that has good biocompatibility and biosafety with the fastest hemostasis, being able to effectively reduce the amount of bleeding and heal faster. In addition, other natural materials such as chitosan, dextran, hydrocolloid dressings are novel dressings that are beneficial for skin healing. In addition, natural materials are also used in other clinical fields. Collagen and gelatin, which are widely used in the medical field, have the disadvantages of rapid

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degradation and low mechanical strength. In order to enhance their mechanical strength and adjust their degradation rate, they can be cross-linked by heat. Therefore, they are widely used for hemostasis, wound healing and tissue regeneration guidance or induction as well as Polyhydroxyalkanoates (PHA and PHB.) PHB can be degraded into D-3-hydroxybutyric acid, a natural substance found in human blood and therefore, widely used in surgical sutures, artificial skin, and drug release control carrier, tissue-guided regeneration membrane, etc.

Air Pollution in China Air pollution represents in China an important problem especially for the largest cities, caused from the increased gas emissions from industrial production and the circulating vehicles. Thus, since the Environmental Protection Law in 1979, Chinese government passed many laws and regulations to protect the environment, recognizing the severity of air pollution in urban mega cities, as Beijing and Shanghai, during the early stage of economic development. Air pollution, therefore, has been addressed in a series of policies establishing that vehicles, vessels, and non- road mobile machineries must not exceed the stipulated emission standard reported in the State Council Action Plan [4, 5]. Thus, for example, the construction of new industries facilities and vehicles that may affect the atmospheric environment must be preceded by environmental impact assessments and standards for the emission of atmospheric pollutants, which met the key requirements reported in the Act Plan [4, 5]. As a consequence between the years 2013 and 2017, significant improvements to air quality were obtained with a drop of 35% of the micro-particles (PM 2.5), for example in Beijing. Unfortunately, in the end of 2017 only 107 of China’s 338 cities had reached the World Health Organization’ interim standard of 35 micrograms/m3, also if 70 cities have reduced significantly the air pollution and the Government campaign for Bluer skies is continuing [6]. However, the last action plan is focused on ozone too, also if it in China is it not particularly severe -ranging + 11% between 2017-2018- when compared to other Countries [7]. Thus, the Plan regards particularly “large reductions in total emissions of greenhouse gases”, taking detailed measures on the sources of pollution and structural issues, such as transition to a green energy and transportation (Figure 1) [7, 8].

Plastics Waste and COVID-19 Pandemic Plastic, infiltrating almost every aspect of human life and becoming a major commodity on a global scale, has produced a great waste problem also. Among the different uses, plastic packaging is the most significant sector with a 40 per cent consumption by different items which, utilized only once, contribute to 61% of beach litters by 6.3 billion metric tons (MT) worldwide [9]. Regarding plastics, China and Hong Kong imported 72.4% of all plastic waste produced in 2017, of which only 9% has been recycled. Thus China in 2009 introduced a temporary restriction on plastic waste imported by its Green Fence policy to increase its quality, announcing in 2017 a permanent banning to import the non-industrial plastic waste [10, 11]. However, Chinese authorities rolled out new regulation to control plastic pollution

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in the land, to go on versus the circular economy by three major goals during the period 20202025. By 2020 in some pilot areas and sectors will be prohibited and restricted the production, sale and use of some plastics, imposing a total ban of importation. By 2022 the substitution of disposable plastic packaging with other biodegradable one will be promoted. By 2025 will be established a new system for the management of production, circulation, consumption, recycling and disposal of all the biodegradable and non-biodegradable plastic products. Moreover, production and sale of plastic films in agriculture less than 0.01 millimetric thick and plastic bags less then 0.025 millimetric thick will be banned. In China, in fact, every year about 2 million tons of plastic films are used to cover around 200,000 kilometers square of farmland for protecting against pets and helping maintain moisture. At this purpose, Chinese government is encouraging farmers to reuse and recycle old films as possible and/or utilize recyclable ones. In conclusion, it is necessary to eliminate unnecessary plastics rethinking the way of design, produce and use them for going towards a circular economy based on recyclable or compostable plastics made by natural polymers obtained from food waste. At this purpose, the worldwide large use of surgical masks for protecting people from COVID-19 pandemic is not to be forgotten, being made by petrol-derived non degradable polymers. Thus, according to the Chinese Premier Li Keqiang, prevention and control of COVID-19 is at the hearth of the government’s strategy at macro- and micro level for year ahead [12]. The focus of this strategy will be a continuous socioeconomic vigilance to maintain the citizens health, protecting, employment, livelihoods, business and supply chains from collapse. According to Premier Li’s strategy, preventing and controlling COVID19 will go hand in hand with planning, decision- making and implementing of government policy over the coming year by the so called Six Protections: 1. job security; 2. people’s livelihoods; 3. business; 4. food and energy security; 5. stable industrial and supply chains; 6. functioning of the lower levels of the Chinese government’s five-level hierarchy. Differently to Europe-returning the economy and society to normal- China is putting prevention and control of the epidemic at the Centre for the foreseeable future [12]. All the effort towards socioeconomic development must be planned coordinating pandemic prevention and control.

PROSPECT OF CIRCULAR ECONOMY IN CHINA Evolution of Scientific Production In the future, China’s circular economy will have a good development prospect, facing many challenges and difficulties also. So in the face of the new trend of developing circular economy in the world, what should we do? From the perspective of China’s long-term economic development prospects, we must establish a basic strategic goal for national economic and social development. Only in this way, it is possible to effectively overcome the environmental resource crisis that emerged in the process of modernization. We need to experience the transition from a traditional industrial linear economy to a circular economy. This is a great reform against traditional economic development and environmental governance methods. The process of changing, requires the active advocacy and support of the government [13]. At the same time, active innovation and development in the industry

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requires public participation and endorsement. From the government’s point of view, it is necessary to formulate corresponding laws, regulations, plans and policies, to change which is not in line with the circular economy. More attention should be paid to the application of economic incentives and measures, as well as other incentives for civil voluntariness. In terms of industry, the necessity of integrating resource recycling and environmental protection into the overall innovation, by the development of an operative strategy, able to adopt corresponding technologies and management for guiding a consumption and market behavior, conducive to the circular economy [14-16]. From the public’s point of view, values and consumption views have to be in harmony with the environment, voluntarily choosing environmentally friendly lifestyle and consumption patterns.

Figure 1. Trends in CO2 emissions from 2002-2017 in China (by the courtesy of Zheng et al. [8]).

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Many achievements from developed countries in the circular economy are worth learning from. First of all, transforming design ideas and principles, unifying economic, social and environmental benefits, fully paying attention to recycling materials. In the product design process, the necessity to try to be normative, so that the equipment may be easily upgraded without having to scrap the whole machine. At the end of its life cycle, the product has to be easily disassembled and comprehensively used. At the same time, in the product design has to be avoid the use of toxic and hazardous materials, harmful for people’s health and the environment. Scientific and rational design is, therefore, the precondition for the implementation of circular economy. Secondly, for relying on scientific and technological progress, it will be necessary to actively adopt harmless or low-harm new technologies, vigorously reducing the consumption of natural raw materials and energy, achieving less input, high output, low pollution, and eliminating emissions of environmental pollution as much as possible. Thirdly, the comprehensive utilization of resources will be implemented to make waste resources be reduced and harmless, and decrease environmentally harmful waste to a minimum. Finally, the conduction of a scientific and strict management has to be considered a must. Circular economy is a new and advanced economic form, but it cannot be envisaged as an economic form promoted by advanced technology. It has to be considered, in fact, a systematic project that integrates economy, technology and society. Scientific and strict management is an important condition for doing it well. At the same time, the development of a biomedicalrelated circular economy will not only greatly benefit the development of the entire economy, but will also benefit the whole society. In a word, China will have a lot to do in the development of circular economy.

ACKNOWLEDGMENTS Part of the writing was supported by the 111 Project [D18011] (to XHG).

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Li, N., Zhang, T. & Liang, S. (2013). Reutilisation-extended material flows and circular economy in China[J]. Waste Manag, 33(6), 1552-1560. Yu, F., Han, F. & Cui, Z. (2015). Assessment of life cycle environmental benefits of an industrial symbiosis cluster in China[J]. Environ Sci Pollut Res Int, 22(7), 5511-5518. Winter, D. G. (1962). Formation of the scab and the rate of epithelization of superficial wounds in the skin of the young domestic pig. Nature, 193, 293-294. China State Council. Air Pollution Prevention and Control Action Plan, 2013, No 37, September 10. http://en.cleanairchina.org/file/loadFile/26.html. China State Council. The 2016-2020 13th Five-Year Plan for Economic and Social Development of the People’s Republic of China, 2016, htpp://en.ndrc.gov..cn/ newsrelease/201612/P020161207645765233498.pdf. China State Council. 2018-2020 Three-year Action Plan for winning the Blue Sky war. 13th Five-Year Plan for Environment Protection, 2018.

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PART III. WASTE IN CIRCULAR ECONOMY

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 8

CIRCULAR ECONOMY IN THE EUROPEAN UNION AS AN EXAMPLE OF WASTELESS PROCESSING OF CRUSTACEAN’S WASTE Galina Tishchenko1,* and Pierfrancesco Morganti2,3 1

Institute of Macromolecular Chemistry of the Academy of Sciences, Prague, Czech Republic 2 Academy of History of Health Care Art, Rome, Italy 3 China Medical University, Shenyang, China

ABSTRACT In the European Union, the industrial production of chitin, chitosan and products on their base are produced by five commercial companies: France Chitine, Primex (Iceland), BioLog Heppe® Gmb and Heppe Medical Chitosan GmbH (Germany) [1] and Mavi Sud Srl (Italy) [2]. According to the European Chitin Society (1], scientists from all EU countries take part in an ever-expanding study and practical application of these natural polysaccharides due to their biocompatibility with the human body, high chemical reactivity, easy biodegradability, and excellent film-forming ability. In this chapter, we tried to analyze current trends in the study of new materials based on chitin and chitosan, developed in the form of films for packaging food products and in the form of dressings for the treatment of wounds, due to the great social significance of their practical use. Here, there is a review of the publications of the EU scientists working in these directions during the last 10 years.

Keywords: chitosan, chitin nanofibrils, food packaging, active food packaging films, wound dressings, disposable CHITOPACK packaging films

INTRODUCTION Since ancient times, people, “earning their daily bread, working in the sweat of their faces”, used the Environment not caring much about its restoration. Today, the understanding

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comes that the Environment is a Subject that gives the Mankind everything necessary for its survival for many thousands of years. Uncontrolled human activity has led to pollution of the Environment due to the accumulation in it of an enormous number of toxic substances that had never existed in Nature before. The time has come when all the inhabitants of the Earth must unite and invest their knowledge and experience to restore the lost biological balance on the planet and create new “green” technologies that will not pollute the Environment with municipal and industrial waste. Recycling of waste from the fish industry is one of the successful examples for the implementation of the circular economy in the EU. The processing of crustacean’s shells being the by-product of the fish industry for extraction of chitin and chitosan solves simultaneously two important problems: ensures the materials science, biology and medicine with raw materials and stopes the pollution of Environment with industrial waste.

CHITOSAN AND CHITIN NANOFIBRILS IN FOOD PACKAGING One of the important requirements of the world market is to increase the shelf-life of food products to reduce both losses due to their rot and the labor and financial costs invested in their production. The uninterrupted supply of food to people is related to the duration of their storage, which can be increased by improving the quality and preservation of food products together with development of new active packaging films ensuring their longer storage. One of the recent initiatives of the European Commission has been the financing of the nChitopack project as a part of the European program aimed at creating a “blue and green” economy based on environmentally friendly technologies and materials [3]. The idea of using the biodegradable natural polymer such as chitosan having an excellent ability to form films is not new in the industry of food packaging. Nevertheless, chitosan is still the subject of research for new generations of scientists that expands our knowledge about its transformations and new application areas. A general conclusion for all recent publications discussed in this chapter consists in the confirmation of antimicrobial, antioxidative, and barrier properties to water vapor, oxygen, and ultraviolet rays for the developed chitosan-based packaging films. These findings support once more the widely known intrinsic antimicrobial activity of chitosan, which is comparable with that of chemically synthesized antimicrobial polymers. At the same time, modern research methods used by the authors allowed them to obtain more detailed information about the structure and properties of chitosan that is so important for perfecting the production of biodegradable food packaging films. Lecheta I et al. [4] have proved that the set of properties mentioned above does not depend on the molecular weight of chitosan and the content of glycerol in plasticized chitosan films. Fernandez-Sise P et al. [5] have investigated the relationship between the antimicrobial activity of chitosan and the structural features of its film, which was formed in situ by casting chitosan dissolved in acetic acid directly onto an ATR crystal. In ATR-FTIR spectrum of chitosan film, the normalized band centered at 1405 cm‒1 is attributed to the carboxylate groupings (-NH3 -OOCH), which, according to the authors, handle the biocidal activity of chitosan, since a correlation between the level of antimicrobial activity of chitosan and the

Circular Economy in the European Union as an Example of Wasteless Processing … 125 size of this band has been proven. High antibacterial activity has been seen only in the presence of a sufficient amount of carboxylate groupings in chitosan films. It has been also proven that carboxylate groupings are not stable and their number decreases with time. The temperature influenced also on the antimicrobial properties of chitosan films [6]. If films were obtained at 37, 80°C, they had a significant inhibitory effect on both Staphylococcus aureus and Salmonella spp, while the film obtained at 120°C ceased to show antimicrobial properties. The authors have concluded that the proper temperature and humidity control is needed under preparation and storage of chitosan films for their best biocidal activity. The importance of this conclusion is supported by the results of Velásquez-Cock J et al. [7], who compared the antibacterial effect of chitosan films containing bacterial cellulose as a filler and acetic or lactic acid as a solvent for chitosan. The antibacterial activity of the films obtained by using an acetate solution of chitosan was absent, perhaps, because of the inappropriate conditions under their preparation. The nature of acid affected the interactions between chitosan and cellulose that manifested in various mechanical stabilities of the films, which turned out to be significantly higher for the films prepared from the acetate solution of chitosan. The influence of the nature and concentration of plasticizers on properties of chitosan films was studied by several researchers [8-10]. Fundo JF et al. [8] have found that the amount of glycerol in the slurry handles the composition of film, while the chitosan and glycerol ratio in the slurry decides its thickness. The authors have also found that water molecules move freely in the matrix of films, while molecules of glycerol are associated with chitosan chains. Kellnar I et al. [9] have studied the effect of the content and molecular length of polyglycerols on mechanical characteristics of chitosan (85 wt.%) films reinforced with chitin nanofibrils (15 wt.%). At the same content of glycerol, diglycerol or triglycerol in chitosan films, both their strain at break and the tensile strength increased with increase of the length of plasticizer molecule. For the films with the fixed plasticizer type, when its content increased, the strain at break tended to increase but the tensile strength to decrease. Suyatma NE et al. [10] have determined the effect of conditions and duration of storage of chitosan films plasticized with glycerol, ethylene glycol, poly(ethylene glycol), or propylene glycol on the mechanical and surface properties of the films. The increase of storage of the plasticized films from 3 weeks to 20 weeks at the fixed temperature and relative humidity resulted in a decrease of their stretching. Plasticization increased the hydrophilicity of the films. Glycerol and poly(ethylene glycol) turned out to be more suitable as chitosan plasticizers due to their better plasticizing effect and higher stability of the films at storage. Authors have concluded that 20 wt%-concentration of these plasticizers is sufficient to keep the flexibility and good stability of chitosan films for 5 months of storage. Several research priorities have been found at reviewing the recent publications devoted to the development of new chitosan-based films for food packaging and study of their properties. The first priority consists in the use of chitosan together with one or more natural polymers preferably having antibacterial activity also. A distinctive feature of these researches was, first of all, the detection of the antimicrobial properties of new films, although some attention was paid for evaluation of their antioxidative activity, permeability for water vapors and oxygen, and mechanical properties. Films developed by Alzagameem A et al. [11] were based on hydroxypropyl methylcellulose with addition of chitosan and lignin. The properties of these films depended both on the source of origin and the content of lignin, the polyphenolic structure of which and the presence of O-containing functional groups are potentially responsible for not only its

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antimicrobial activity but also free radical scavenging ability. It is especially important that these films suppress the growth of both gram-positive and gram-negative microorganisms both at 35°C and at low temperatures (0-7°C) including the bacteria Brochothrix thermosphacta and Pseudomonas fluorescens, which can grow at low temperatures and spoil food. Increase of the content of lignin and addition of chitosan to the films has enhanced their antimicrobial activity. Crouvisier-Urion K et al. [12] have also studied the chitosan films containing lignin in the form of microparticles, which were obtained by treatment of lignin under the applied high pressure or by high shear homogenization, resulting in preparation of the lignin microparticles with the sizes of 0.6 and 2.5-5 microns, respectively. The surface hydrophobicity of the composite films increased without a significant difference in their antioxidative activity. However, migration of lignin microparticles from the films into the extraction medium was noted, especially, when homogenizing of lignin happened under high pressure. The films prepared by Benbettaïeb N et al. [13] from mixtures of chitosan and gelatin by casting technique showed the improved mechanical stability and barrier properties due to chemical interactions between the components. Belalia R et al. [14] have shown that the developed films and especially coatings from hydroxypropyl cellulose associated with chitosan or N, N, N-trimethylchitosan as biocides inhibited completely the growth of Listeria monocytogenes and Salmonella typhimuriumevaluate. A potentially biologically active food packaging based on paper coated with chitosan was developed by Bordenave N et al. [15]. Chitosan was deeply absorbed into the paper and enveloped the cellulose fibers, instead of forming a layer as expected. Chitosan-modified paper had improved barrier properties to water. This finding supports the assumption by Van den Broek LA et al. [16], who claimed that antimicrobial agents such as chitosan in packaging films will enhance their barrier properties, thus increasing the shelf-life of a packed food product. The films developed by Gomes LP et al. [17] had chitosan and chitosan nanoparticles obtained by the ultrasound treatment of chitosan for 5, 15 and 30 minutes. The mechanical strength and stiffness of these composite films increased but their water permeability decreased. All these films showed the antimicrobial activity against both some gram-positive and gram-negative bacteria. The second priority direction for the researchers in the development of new packaging films consisted in the use of mixtures of natural and synthetic polymers containing various fillers for improving the mechanical stability of films. The flexible and transparent films of hydrophilic nature have been made by Cazón P et al. [18, 19] from bacterial cellulose, chitosan, and poly(vinyl alcohol). The films have shown good barrier properties against UV irradiation, the improved mechanical properties and high ability to adsorb water. Velickova E et al. [20] used chitosan as the basis for the development of films crosslinked with sodium tripolyphosphate, the both surfaces of which were further coated with beeswax. For comparison, the films consisting of an emulsion of chitosan and beeswax only have been also prepared. Crosslinking of chitosan matrix with tripolyphosphate halved both water absorption and the permeability to water vapor of the films but their rigidity increased. The less stiff films from chitosan and beeswax have passed water vapors in almost twofold slower. The composite films based on hydroxypropyl methylcellulose and chitosan have been developed by Möller H et al. [21]. The hydrophobicity of these films increased at their crosslinking by citric acid or association with stearic acid. The films with and without stearic acid have shown antilisterial activity, but the films crosslinked with citric acid lost their antimicrobial activity. Swagan AJ et al. [22] have purposed to prepare the films based on polylactide, the oxygen

Circular Economy in the European Union as an Example of Wasteless Processing … 127 permeability of which would be comparable to that of poly(ethylene terephthalate). After applying 70 alternating two-layer coatings consisting of chitosan and montmorillonite clay to the surface of the extruded polylactide film, its oxygen permeability decreased by 99% and 96%, respectively, at 20°C and 50% relative humidity. Giannakas A et al. [23] used low molecular weight poly(vinyl alcohol), chitosan, and montmorillonite to prepare packaging films with low permeability for water vapor and oxygen and increased antimicrobial activity. Youssef AM et al. [24] have prepared bionanocomposite packaging films from chitosan, carboxymethyl cellulose, and zinc oxide nanoparticles by casting technique. The films showed better mechanical and thermal properties than those without embedded mineral nanoparticles. Analysis of a sample of the soft white cheese packed in this film and stored at 7°C for 30 days have shown that the packaging film helped in increasing the shelf-life of the cheese and displayed good antibacterial activity against gram positive (Staphylococcus aureus), gram negative (Pseudomonas aeruginosa, Escherichia coli) bacteria and fungi (Candida albicans). Other films prepared by the authors [25] for packaging of the soft white cheese had nanoparticles of titanium oxide embedded in matric from chitosan and carboxymethyl cellulose, instead of zinc oxide. The total number of bacteria including Escherichia coli, mold, and yeast gradually decreased and disappeared on the 30th day of storage. Frindy S et al. [26] have compared the effect of various fillers (layered montmorillonite, nanotubular halloysite or microfibrillar sepiolite) embedded in chitosan on properties of the thin films prepared by casting technique. At 5%-content of microfibrillar sepiolite in chitosan matrix, the mechanical properties of films reached their best values. These findings prove that the addition of clays into chitosan phase is one of the ways to resist the shrinkage which is typical for the films from native chitosan. Mura S et al. [27] have developed films composed of chitosan, methylcellulose, and nanoparticles of silica oxide. An excellent improvement of the mechanical properties was obtained for the films with the mass ratio of chitosan and methylcellulose equal to 50:50 and 1%-content (w/v) of the mineral nanoparticles. Nowadays, the packaging films based on biodegradable polymers with addition of various biologically active compounds such as preservatives, chemical fungicides, and various plant extracts with antimicrobial activity are intensively created and studied. This is the third and the most popular priority direction for many researchers [28-57] developing the films for food packaging. These packaging films based on chitosan and other natural polymers are usually named as active ones because of their enhanced antimicrobial properties. Chitosan active films containing the tea of kombucha (1-3%) have been prepared by Ashrafi A et al. [30] using the casting technique. The shelf-life of minced beef samples packed in these active films has extended up to 4 days owing to the retardation of lipid oxidation and microbial growth under the action of polyphenol components of the kombucha. The active chitosan films prepared by Balti R et al. [31] had the Spirulina extract, which improved not only the antioxidative and antimicrobial activity of the films but also their mechanical and barrier properties. Talón E et al. [32] recommend using the active films based on chitosan and thyme extract, which have shown high antioxidative activity in food packaging due to the presence of thyme polyphenols. The active films developed by OteroPazos P et al. [33] based on chitosan and polycaprolactone had α-tocopherol, due to which the antioxidative activity of the films was kept for more than 20 days. Higueras L et al. [34] have developed active films by casting of chitosan-cyclodextrin mixtures, followed by their

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saturation with carvacrol. These active films were used to inhibit the growth of microbes such as mesophiles, psychrophiles, Pseudomonas species, enterobacteria, lactic acid bacteria, yeast, and fungi on the packaged chicken breast fillets. General inhibition of microbes has been shown, but a large amount of carvacrol, which absorbed on the fillets, caused an unacceptable deterioration in taste. Composite films developed by Pereda M et al. [35], as a potential food packaging, consisted of glycerol-plasticized chitosan and dispersions of cellulose nanocrystals with addition of olive oil. The joint use of cellulose nanoparticles and olive oil has improved elastic properties of chitosan films plasticized with glycerol and, at the same time, proved to be an efficient method to reduce their initially high permeability for water vapors. Higueras L et al. [36] have developed glycerol-plasticized chitosan films containing up to 10% of the antimicrobial compound ethyl N (α) dodecanoyl-1-arginate. Upon contact with an aqueous food simulator, this agent was completely released from the films for several hours at 4 and 2°C. The antimicrobial activity of the films against mesophiles, psychrophiles, Pseudomonas spp., Colif, lactic acid bacteria, hydrogen sulfidecontaining bacteria, yeast and fungi has been evaluated after 2, 6 and 8 days on chicken breast fillet packed in both active and chitosan films. The active films prepared by Brink I et al. [37] from a mixture of whey proteins and chitosan with the addition of cranberry or quince juice, as biocides, have stopped the microbiological destruction of turkey meat and the development of pathogenic microorganisms Salmonella typhimurium, Escherichia coli and Campylobacter jejuni in pieces of turkey at their storage for at least 6 days. The level of antimicrobial activity was higher for the films containing the cranberry juice. Akyuz L et al. [38] have developed the chitosan packaging films containing various commercially available oils and fats such as olive, corn and sunflower oils, butter, and animal fats. Chitosan films with olive oil had improved mechanical properties, higher thermal stability, and better surface morphology, along with the highest antimicrobial activity, which was almost equal to the activity of the commercial antibiotic gentamicin. The films based on a mixture of chitosan and zein with the addition of essential oils such as anise, orange and cinnamon developed by Escamilla-García M et al. [39] were transparent and could inhibit the growth of Penicillium spp. and Rhizopus spp. The physical properties of the films improved owing to the multiple chemical interactions between the functional groups of the components in the films. The water permeability of the film containing anise oil was significantly lower, but its mechanical strength was higher than that of a chitosan film. Benbettaïeb N et al. [40] have developed the films from mixtures of chitosan and fish gelatin with addition of natural antioxidants, such as ferulic acid, caffeic acid, and tyrosol. The permeability of these films decreased by more than 30%, and the tensile strength increased to 50% because of molecular interactions between polymer chains and antioxidants. Films containing caffeic acid or a mixture of caffeic and ferulic acids have shown their highest antioxidative activity. Vasile C et al. [41] have investigated the antifungal, antibacterial, and antioxidative activity of commercial essential oils such as thyme, clove, rosemary, and tea tree to assess their biocidal activity in food packaging. They have realized that the essential oil of thyme, clove, and tea tree can be used as antimicrobial agents against the food decay fungi (Fusarium graminearum, Penicillium corylophilum, and Aspergillus brasiliensis) and pathogenic food bacteria (Staphylococcus aureus, Escherichia coli, and Listeria monocytogenes). The thyme and clove oils exhibited the highest inhibitory effect due to the high content of phenols. These essential oils could be suitable alternatives to chemical additives, thus satisfying the consumer demand for naturally preserved food products ensuring their safety. Promising results were obtained by

Circular Economy in the European Union as an Example of Wasteless Processing … 129 incorporation of essential oils both in chitosan emulsions and films, which have shown potential for food packaging. The study performed by Rubilar JF et al. [42] was aimed at optimization of the active packaging films to improve food preservation and shelf-life extension. They used the mathematical modeling to study the release of gallic acid into an aqueous medium from chitosan films containing a grape seed extract and carvacrol. The results on the controlled release of antimicrobial and antioxidative compounds from packaging films during 30 days at temperatures 5, 25 and 45°C are of utmost importance for extending the shelf-life of perishable foods. For extension of the shelf-life of ready to eat meat products, the active packaging systems have been developed by Quesada J et al. [43]. They had an inner surface coated with a chitosan film containing the thyme essential oil (0%, 0.5%, 1%, and 2%) without the direct contact with the meat during 4 weeks of refrigerated storage. For reducing the impact of thyme essential oil on meat sensory properties, its chemotype with low odor intensity was used. The essential oil in films reduced yeast populations, while aerobic mesophilic bacteria, lactic acid bacteria, and enterobacteria were not affected. The packaged meat had better appearance during storage. Thyme odor was perceived as desirable in cooked meat, and the intensity of typical meat odor decreased by increasing the essential oil concentration. A polyelectrolyte material suitable for active coatings of beef steaks has been developed by Kulig D et al. [44], by complexation of chitosan and sodium alginate in a broad range of the component ratios. Application of obtained hydrosols enriched with sodium erythorbate enhanced the color stability of beef steaks during 2-week storage compared with the uncovered beef. The favorable wetting properties of polyelectrolyte films along with their limited solubility were seen. Elchinger PH et al. [45] have shown that the intrinsic antioxidative activity of chitosan film increased by 90% after immobilization of the short-chain peptide with the radical scavenging activity on the surfaces of the film. Albertos I et al. [46] have examined the inhibitory effect of the active chitosan films containing clove oil for ten representative pathogenic bacteria causing food spoilage. The most sensitive bacteria to the films and the most resistant ones were Shewanella putrefaciens and Aeromonas hydrophila, respectively. The microbial load (total aerobic mesophilic, lactic acid bacteria and total coliform) on the trout fillets covered with chitosan films and stored at 4°C during 22 days was lower than that of samples processed under high pressure, and like that of cooked samples, except for coliform counts. Higueras L et al. [47] have prepared the active films from chitosan and cyclodextrin by casting technique and then saturated them with carvacrol for achieving equilibrium. These films were used to inhibit the microbial growth on the packaged chicken breast fillets stored for 9 days at 4°C. The fillets were the main absorbing phase of carvacrol loaded in the active films with average concentrations of 2005000 mg/kg. During the period of storage, a general microbial inhibition against lactic acid bacteria, yeasts and fungi has been observed. However, the large amount of carvacrol absorbed or reacted with the fillet caused unacceptable taste deterioration. Simonaitiene D et al. [48] have investigated the inhibition effect of both chitosan films and composite ones prepared from whey proteins and chitosan containing different amounts of quince or cranberry juice as natural antifungal agents against Penicillium expansum on the simulation medium and on apples. The presence of cranberry and quince juice in the tested films caused a significant increase in elasticity and decrease in tensile strength of the films. Significant inhibition effect of the films against Penicillium expansum growth on a simulated medium and apples has been shown. A longer lag phase and a lower growth rate of Penicillium

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expansum were observed in the films with cranberry juice than with quince one. The active chitosan films containing citrus extract have been prepared and tested by Iturriaga L et al. [49]. The antimicrobial activity of the films against Listeria innocuous was kept after UV irradiation. In comparison with chitosan films, the active chitosan films containing naringin or citrus extract had an increased absorbance in the UV region showing their ability to reduce the lipid oxidation induced by UV light in food. Regardless of the solvent used for dissolution of naringin at preparation of the active films, UV treatment caused modifications of the flavanone depending on its concentration in the film: the higher the concentration, the lower the modification due to crosslinking and the interactions between naringin and chitosan. Vodnar DC et al. [50] have developed active antimicrobial chitosan films containing extracts of green or black tea for controlling Listeria monocytogenes ATCC 19115 on vacuumpackaged ham steak, which was stored at 20°C for 10 days and at 4°C for 8 weeks. The growth of Listeria monocytogenes ATCC 19115 was inhibited with both tea extracts. Chitosan-coated plastic films without addition of tea extracts did not inhibit the growth of Listeria monocytogenes. When tea extracts were incorporated into these films, they gained the antimicrobial properties which were the dose dependent. The highest antimicrobial efficiency had the films containing 4% of green tea extract reducing the initial counts from 3.2 to 2.65 log CFU/cm2 and from 3.2 to 1-1.5 log CFU/cm2 during storage at room temperature and at 4°C, respectively. The obtained knowledge about the antilisterial activity of the extracts of natural tea are useful for developing antimicrobial packaging films saving the quality of ham steak during room and refrigerated storage. Cerqueira MA et al. [51] have studied the application of films from chitosan, galactomannan, or agar, plasticized with glycerol and corn oil for coating on cheese. The solutions consisting of 1.5% of galactomannan, 2.0% of glycerol, and 0.5% of oil showed the best properties for coating the cheese. In contrast to uncoated cheese, the developed composite solution not only prevented the mold growth on the surface of coated cheese but also decreased its respiration rate (oxygen consumption and carbon dioxide production). The results have shown that these coatings can be applied as an alternative to synthetic coatings. Zimet P et al. [52] have investigated the effect of carboxymethyl chitosan added to chitosan containing bacteriocin nisin on the structural properties and antilisterial activity the films. Carboxymethyl chitosan had a plasticizing effect and enhanced the distribution of the bacteriocin within the biopolymer matrix. Nisin led to changes in the macro- and microstructure, as well as in physicochemical properties of the films. Films from chitosan and carboxymethyl chitosan were more effective against Listeria monocytogenes than chitosan ones. The active films based on chitosan and containing a hop extract have been developed by Bajić M et al. [53]. The incorporation of hop extract into chitosan films has caused a reduction in their hydrophilic character and the complete blocking of UV light at wavelengths below 350 nm. A declining trend of the tensile strength by twice and Young’s modulus by an order, as well as a rising trend of strain at break by triple had been also observed. The films showed antibacterial activity against foodborne pathogen Bacillus subtilis. Akyuz L et al. [54] have developed the active chitosan films containing capsaicin, a plant alkaloid with high antioxidative, anti-inflammatory, anti-obesity, anticancer and analgesic properties. The increase in concentration of capsaicin in chitosan films improved continuously their antimicrobial, antioxidative properties and hydrophobicity. The authors believe that the food packaging and wound healing could be the most promising applications of these films. The oil of Camelina sativa seed at different concentrations was incorporated by Gursoy M et al. [55] into chitosan films that resulted in a notable

Circular Economy in the European Union as an Example of Wasteless Processing … 131 enhancement of their thermal stability, antioxidative, anti-quorum sensing and antimicrobial activity. However, the hydrophilicity of these active films increased noticeably that the authors explain by the formation of micelles between molecules of used plasticizers (glycerol and Tween 40]. An active packaging film developed by Giannakas A et al. [56] consisted of nanostructured low-density polyethylene, chitosan, and extract of the essential oils such as rosemary and Melissa, added to improve the antioxidative properties of the films and disguise the food odor. These films had enhanced barrier properties to oxygen and permeability to water vapors owing to the presence of chitosan. The introduction of oils in the films enhanced their antioxidative efficiency. Kurek M et al. [57] have studied the effect of water vapors on barrier and transport properties of chitosan films containing carvacrol. The plasticizing effect of water and carvacrol depended on moisture. At high humidity, it was more pronounced for water, but at low humidity it was higher for carvacrol. The deposition of a thin layer of chitosan on polyethylene reduced its permeability to oxygen and carbon dioxide in both dry and wet conditions. The release of carvacrol from the chitosan matrix had increased with humidity and, to a lesser extent, with increasing temperature from 4 to 37°C.

DISPOSABLE PACKAGING FILMS FROM CHITOSAN AND CHITIN NANOFIBRILS In our study, the disposable packaging films named as CHITOPACK have been developed based on chitosan and chitin nanofibrils produced by the Italian company Mavi Sud Srl [2]. The main results of our study have been summarized and published in the book Bionanotechnology to Save the Environment [58]. Since a one-off film is needed to protect a food product from external contamination for a brief time, the mechanical and surface properties, and their dependence on various variables of the producing process was discussed here. Based on our experience, some recommendations for preparing the CHITOPACK films are given so that their producing process was reproducible and sustainable. First, it should be noted that both chitosan and chitin nanofibrils consist of N-acetyl-Dglucosamine linked to D-glucosamine by a β-(1-4) glycosidic linkage into linear molecules. The difference between them consists in that chitin nanofibrils have about 4-5 times more Nacetyl-D-glucosamine molecules compared to chitosan. CHITOPACK films were obtained from chitosan and chitin nanofibrils with an acetylation degree of 21% and 95%, respectively. Due to the similarity of the chemical structure of chitosan and chitin nanofibrils, it is possible to obtain their composites with a high content of chitin nanofibrils (up to 80%) in the chitosan matrix without any signs of phase separation. This feature distinguishes chitin nanofibrils used as cross-linkers of chitosan molecules from mineral fillers, the amount of which in chitosan films does not usually exceed 3-5%. Moreover, chitin nanofibrils have such a strong stabilizing effect on mobile chitosan molecules that the resulting dry films do not change their size when immersed in water. The efficiency of crosslinking the chitosan, increasing with increasing the content of chitin nanofibrils and resulting in formation of the reversible thixotropic gels, was confirmed by Mikesova et al. [59] in the rheological experiments. Addition of a plasticizer (glycerol, diglycerol, triglycerol or poly(ethylene glycol) delayed the onset of gelation of the slurries significantly due to disruption of the bonds between chitosan

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and chitin nanofibrils. The viscoelastic characteristics of the gels have steadily getting worse. After their storage at 6°C for 19 weeks, the microstructure of a thixotropic gel destroyed because of the degradation of chitosan molecules into short fragments. Therefore, it is recommended to cast the freshly prepared slurry on a support for obtaining the reproducible results. The tensile strength, Young modulus, and the strain at break of the CHITOPACK films depend on the molecular weight of chitosan, the content of the chitin nanofibrils, the type and content of plasticizers, the temperature of drying, the type of a modifier of film surfaces and the conditions of their modification. The surface modification of the films by sorption immobilization of poly(lactic acid) or polyglycerol polyricinoleate exhibited significant effect on improvement of both mechanical stability and hydrophobicity of the films. The surface properties of the films depended additionally on the nature of a support used for casting of the slurries. The mechanical stability of CHITOPACK films were better when high-molecular-weight chitosan of about 1000 kDa was used and its deacetylation degree varied within 75-80%. The deacetylation degree of chitin nanofibrils was always considerably low of about 2-5%. The content of chitin nanofibrils varied within of 20-30 wt% decreasing with increasing the molecular weight of chitosan. It was mentioned above [9] that the mechanical stability of the films deteriorated with increasing content of a plasticizer regardless of its type, i.e., elongation increased and the tensile strength of the film decreased. The CHITOPACK films turned out to be comparable in their mechanical stability with commercial wrapping paper that is used nowadays for one-off packaging of some food products in the fast-food restaurants. One more practical recommendation by Gonçalves I et al. [60] could be useful for the researches who are interested in preparation of the colorless chitosan films crosslinked with genipin. A two-stage strategy has been developed by them for decolorization of the blueishcolored genipin-crosslinked chitosan films using recombinant CotA lacaxa from Bacillus subtilis mediated by 2,2’-azinobis- (3-ethylbenzothiazoline-6-sulfonic acid), followed by oxidation with 5% hydrogen peroxide at pH 11 and 40°C for 30 minutes. The applied method did not change both the acid stability and the antioxidant ability of the starting films.

CHITOSAN IN WOUND DRESSING Chronic non-healing ulcers are a severe problem in clinical practice because they are not often the root causes, but only secondary signs of another chronic disease. The current trend in the application of wound dressings for the treatment of complex wounds that often go with cancer or diabetes is the use of multifunctional dressings [61]. Multifunctional or active dressings not only isolate the wound from injuries and microbial infections during the healing process as traditional inactive dressings do, but also take part in the restoration of skin and epidermal tissues, delivering absorbed medicinal substances, growth stimulants and antiseptics that gradually diffuse into the affected tissues, accelerating the restoration of the skin and inhibiting the growth of pathogenic microorganisms [62]. Wound healing is a complex and regulated physiological process, including activation of distinct types of cells at each next stage (homeostasis, inflammation, proliferation, and tissue remodeling) and any

Circular Economy in the European Union as an Example of Wasteless Processing … 133 violation in the correct sequence of healing events can lead to chronic wounds [63]. Since the human body can recognize the biocompatibility of the material in contact with it, some natural polymers, such as polysaccharides and proteins, which have chemical and structural similarities with tissue macromolecules, are widely used in the treatment of wounds and burns [64]. The development of a proper extracellular matrix that can support tissue regeneration and, at the same time, prevent the occurrence of adverse events, is a challenging task. Researchers working in this field believe that a more thorough study of the mechanisms of regeneration processes and development of a new generation of dressings based on natural polymers biocompatible with human skin and having a suitable porous structure will help to solve this problem. Chitosan is widely known as an active participant in skin regeneration, which is an effective accelerator of wound healing. It has been proved that the linear structure of chitosan molecules gives optimal structural properties to the matrix, contributing to the stimulation of cell proliferation and the acceleration of complete skin repair [63]. More effective wound healing began to be observed when chitosan nanoparticles with a large contact surface were introduced into wound dressings [63]. It was noted that noteworthy progress in the treatment of burns and chronic wounds was achieved precisely due to the active participation of chitosan in tissue repair, which was manifested by the absence of scars on the skin after wound healing. The active dressings developed by Sandri G et al. [63] based on chitosan and pullulan associated with chondroitin sulfate or hyaluronic acid have shown high efficiency in wound healing. The chitosan membranes developed by Nordback PH et al. [65] accelerated wound healing, reduced inflammation, and affected the level of serum interleukin IL-4, however, they were destroyed at the wound site after day 7 due to the activity of proteases and other extracellular enzymes. This problem is solved in two ways: by creating composite materials based on the blends of synthetic and natural polymers and by modifying the surface of commercial polymer matrices having a suitable structure and porosity with biopolymers. 3D matrices that mimic the skin and are necessary for the full restoration of its functionality must be insoluble in aqueous fluids. Synthetic polymers are traditionally used as inactive matrices for wound dressings. For example, Aubert-Viard F et al. [66] used a nonwoven textile fabric made of polyethylene terephthalate fibers as a base matrix, biocompatibility of which with the skin was ensured by modifying the surface of the fibers with chitosan cross-linked with genipin, followed by layering the alternating layers of anionic and cationic polymers, methyl βcyclodextrin and chitosan, respectively. The long-term antibacterial effect during wound healing was supported by diffusion of the antiseptic chlorhexidine previously absorbed into the dressing. In another case, Mogrovejo-Valdivia A et al. [67] used a non-woven poly(ethylene terephthalate) textile fabric for the manufacture of an antiseptic dressing by absorbing silver ions within the matrix and then coating it with alternating layers of cationic chitosan and anionic cyclodextrin. Due to the multilayer polyelectrolyte polymer coating, the release of silver slowed down and the antibacterial effect of the dressing persisted for a long time. Casimiro MH et al. [68] used a porous matrix from poly(vinylpyrrolidone) (5%) and chitosan obtained by freeze-drying and gamma irradiation. This dressing successfully supported the adhesion of cells in vitro, viability, and proliferation of the HFFF2 fibroblast cell line. The introduction of chitosan into synthetic polymer composites makes the degradation of the composite material easier and faster. Dorati R et al. [69] have shown that

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the decomposition of nanofibers obtained by electrospinning from a poly(lactide)-copoly(caprolactone) copolymer containing up to 27% suspension of chitosan hydrochloride salt was accelerated in in vitro tests, although only 6% of the amount of chitosan introduced was available on the surface of the fibers. In the treatment of burns, the structure of dressings becomes especially important. A matrix should be microporous to ensure the absorption of exudate, which is formed in increased amounts during burn skin lesions. Stephen-Haynes J et al. [70] have reported that the absorbent wound dressing KytoCel is effective in outpatient and emergency care. The microporous structure supplies more opportunities for adhesion of fibroblasts' proliferation and the process of angiogenesis. Iacob AT еt al. [71] have shown that microporous membranes based on chitosan or on the blends of chitosan and hyaluronic acid, and containing biologically active derivatives of arginine with thiazolidin-4-one, had a high degree of swelling that contributed to the rapid healing process of burn wounds with the complete reepithelization after 15 days. Currently, the techniques such as electrospinning and 3D printing are becoming increasingly popular in the development of porous wound dressings. The undeniable advantage of 3D printing is the creation of porous matrices with a well-defined architecture and molecular orientation at the micro level. Hafezi F et al. [72] used 3D printing to make a matrix of chitosan, a cross-linker (genipin) and plasticizers (glycerol and poly(ethylene glycol). PEG600 plasticized chitosan-genipin films had an acceptable elasticity, excellent adhesive ability to the surface of the epithelium, high water absorption and low cytotoxicity. More than 48% of human skin fibroblast cell lines were viable after 48 hours of contact with these films. An original example of multifunctional wound dressings is the asymmetric membrane developed by Alves P et al. [73]. The idea was to simulate both skin layers in one dressing using electrospinning technology. The protective layer consisted of polycaprolactone and poly(lactic acid), and the underlying layer consisted of methacrylated gelatin and chitosan, which is more compatible with skin tissues and contributes to less painful wound healing. Good adhesion and hemocompatibility of dressings with skin and a noticeable growth and spread of fibroblasts have been shown in in vitro experiments. Recently, there has been an additional steady trend in the development of active wound dressings. Tanha S et al. [74] used a growth factor (recombinant human granulocyte colony stimulating factor) incorporated into chitosan nanoparticles, which, in their turn, were introduced into matrix from nanofibers of poly(ε-caprolactone), the surface of which was then coated with collagen, the type 1. The authors noted that the created dressing contributed to the active growth of fibroblasts, enhanced collagen deposition and the minimal presence of inflammatory cells. A synergistic effect of a nano-fibrous porous membrane imitating the extracellular matrix of the skin was also observed. As an accelerator for the growth and repair of damaged tissues, Vigani B et al. [75] used a biodegradable alginate, which was introduced into the porous matrix during the formation of fibers from solutions of dextran or poly(ethylene oxide) by electrospinning. Then, the surface of the fibers was coated with poly(lactide-co-glycolide) or chitosan to reduce the rate of biodegradation of dressings in contact with wounds. Such a modification of the surface of the fibers increased the adhesion of fibroblasts, their growth and spread, without hindering the diffusion of alginate from the fibers. As have been shown by Patrulea V et al. [76], the migration of human dermal fibroblasts can also be significantly accelerated by a peptide (arginine-glycine-asparagine)

Circular Economy in the European Union as an Example of Wasteless Processing … 135 fixed on chitosan and hyauronic acid, introduced as polyelectrolyte nanocomplexes into foams or gels from functionalized chitosan and chondrotin sulfate. In in vitro tests, the formulations developed stimulated the proliferation of dermal fibroblasts and their migration for 7 days without signs of toxicity. It has been shown by Ghalayani Esfahani A et al. [77] that an active chitosan patch containing clobetasol propionate, a corticosteroid, which is used to treat various skin diseases, is highly effective in treating inflammatory chronic diseases of the oral mucosa. At the same time, many studies have shown that the use of active dressings is often accompanied by allergic and toxic reactions that are provoked by certain substances released from the dressing. Unexpected results were reported by Zelga PJ et al. [78], who tested six active dressings from distinct categories for of acute irritation in rabbits and for sensitization in guinea pigs. Histological analysis has shown that only a dry linen dressing did not have an irritating and sensitizing effect. The rest of the dressings (hydrogel dressing, chitosan sponge, silver nanoparticles, linen dressing, impregnated with linseed or oil fixative) received a cumulative irritation index of 0.00-0.35 and caused a sensitization reaction in up to 20% of animals. The authors note that although, according to the category of skin reaction, these dressings belong to the group of products that do not cause slight irritation and sensitization, a certain risk of an allergic reaction in people still exists with their use. The main obstacle to the widespread use of chitosan is the almost complete absence of its solubility in water and alkaline solutions. To overcome this obstacle, the structure of chitosan is modified, facilitating the preparation of composites or hydrogels. Chitosan derivatives belong to the class of biomaterials useful for various purposes due to the absence of toxicity, low allergic reaction, biocompatibility, and biodegradability [79].

CONCLUSION In the modern world, studies on the creation of composite materials from mixtures of synthetic and natural polymers are becoming increasingly popular. However, it should be borne in mind that during the destruction of the natural polymer in such composites in the Environment, it is contaminated with microparticles of synthetic polymers. They are accumulated in water, fish, and plants due to the long decomposition time of the synthetic micropolymers. The impressive results have been achieved using the designed active packaging films extending the shelf-life of food products. However, a more detailed analysis of the behavior of microorganisms in products packaged in active films would be desirable to assess their sporulation in the presence of inhibitors of their growth and secretion of toxins. It would be necessary to check the safety of the food products themselves when they absorb biologically active ingredients, and especially those that mask the smell of food. Some problems associated with the storage of food will be minimized by perfecting both the production processes for avoiding the overproduction of perishable food products and the organization of their sales. In today’s McDonaldizated world [80], the need for disposable packaging for food products such as various sandwiches, baguettes, rolls, muffins, hot dogs and other ready-toeat (RTE) confectionery products is growing rapidly since these wrappings are needed for

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hygiene purposes. Soon, the public catering in the fast-food restaurants with an everincreasing quality of prepared meals will become one of the traditional elements of a new lifestyle. Currently, in fast-food restaurants and countless cafes, the paper wrappers are traditionally used. Production of the cellulose-based wrappers requires both significant financial costs and huge volumes of wood. Trees grow for 50-100 years to reach their industrial age, and wrapping paper for RTE products is used and discarded within a few minutes to an hour. Obviously, replacing cellulose with renewable natural polymers for the manufacture of food packaging will reduce deforestation, which has been growing at an alarming rate in the recent years. Such a strategy will have a positive effect on the climate of the planet, as trees are involved in restoring the biological balance by purifying air from industrial emissions, absorbing carbon dioxide and enriching the atmosphere with oxygen. An equally important problem that destroys the BioBalance of the planet is environmental pollution by industrial waste. The only way to solve this problem consists in the implementation of the Circular Economy as well as in the designing new “green” technological processes.

ACKNOWLEDGMENTS The authors gratefully acknowledge the financial support of the European Union (Grant 315233).

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Circular Economy in the European Union as an Example of Wasteless Processing … 141 [65] Nordback, P. H., Miettinen, S., Kääriäinen, M., Haaparanta, A. M., Kellomäki, M., Kuokkanen, H., et al. (2015). Chitosan membranes in a rat model of full-thickness cutaneous wounds: healing and IL-4 levels. J Wound Care., 24(6), 245-6, 248-51. [66] Aubert-Viard, F., Mogrovejo-Valdivia, A., Tabary, N., Maton, M., Chai, F., Neut, C., et al. (2019). Evaluation of antibacterial textile covered by layer-by-layer coating and loaded with chlorhexidine for wound dressing application. Mater Sci Eng C Mater Biol Appl., 100, 554-563, 2019. [67] Mogrovejo-Valdivia, A., Rahmouni, O., Tabary, N., Maton, M., Neut, C., Martel, B., et al. (2019). In vitro evaluation of drug release and antibacterial activity of a silverloaded wound dressing coated with a multilayer system. Int J Pharm., 556, 301-310. [68] Casimiro, M. H., Gomes, S. R., Rodrigues, G., Leal, J. P. & Ferreira, L. M. (2018). Chitosan/Poly(vinylpyrrolidone) Matrices Obtained by Gamma-Irradiation for Skin Scaffolds: Characterization and Preliminary Cell Response Studies. Materials (Basel)., 11(12). pii: E2535. [69] Dorati, R., Pisani, S., Maffeis, G., Conti, B., Modena, T., Chiesa, E., et al. (2018). Study on hydrophilicity and degradability of chitosan/polylactide-co-polycaprolactone nanofiber blend electrospun membrane. Carbohydr Polym., 199, 150-160. [70] Stephen-Haynes, J., Toner, L. & Jeffrey, S. (2018). Product evaluation of an absorbent, antimicrobial, haemostatic dressing. Br J Nurs., 27(6), S24-S30. [71] Iacob, A. T., Drăgan, M., Gheţu, N., Pieptu, D., Vasile, C., Buron, F., et al. (2018). Preparation, Characterization and Wound Healing Effects of New Membranes Based on Chitosan, Hyaluronic Acid and Arginine Derivatives. Polymers (Basel)., 10(6). pii: E607. [72] Hafezi, F., Scoutaris, N., Douroumis, D. & Boateng, J. (2019). 3D printed chitosan dressing crosslinked with genipin for potential healing of chronic wounds. Int J Pharm., 560, 406-415. [73] Alves, P., Santos, M., Mendes, S. P., Miguel, S. D., de Sá, K. S. D., Cabral, C., et al. (2019). Photocrosslinkable Nanofibrous Asymmetric Membrane Designed for Wound Dressing. Polymers (Basel)., 11(4), pii: E653. [74] Tanha, S., Rafiee-Tehrani, M., Abdollahi, M., Vakilian, S., Esmaili, Z., Naraghi, Z. S., et al. (2017). G-CSF loaded nanofiber/nanoparticle composite coated with collagen promotes wound healing in vivo. J Biomed Mater Res A., 105(10), 2830-2842. [75] Vigani, B., Rossi, S., Sandri, G., Bonferoni, M. C., Milanesi, G., Bruni, G., et al. (2018). Coated electrospun alginate-containing fibers as novel delivery systems for regenerative purposes. Int J Nanomedicine., 13, 6531-6550. [76] Patrulea, V., Laurent-Applegate, L. A., Ostafe, V., Borchard, G. & Jordan, O. (2019). Polyelectrolyte nanocomplexes based on chitosan derivatives for wound healing application. Eur J Pharm Biopharm., 140, 100-108. [77] Ghalayani Esfahani, A., Altomare, L., Varoni, E. M., Bertoldi, S., Farè, S. & De Nardo, L. (2019). Electrophoretic bottom-up design of chitosan patches for topical drug delivery. J Mater Sci Mater Med., 30(4), 40. [78] Zelga, P. J., Górnicz, M. M., Głuszkiewicz, J. M. & Piasecka-Zelga, J. (2016). Outcomes of acute dermal irritation and sensitisation tests on active dressings for chronic wounds: a comparative study. J Wound Care., 25(12), 722-729.

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[79] Paul, P., Kolesinska, B. & Sujka, W. (2019). Chitosan and Its Derivatives Biomaterials with Diverse Biological Activity for Manifold Applications. Mini Rev Med Chem., 19(9), 737-750. [80] Ritzer, G. (2008). The McDonaldization of Society 5, Pine Forge Press, An Imprint of Sage Publications, Inc.

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 9

CIRCULAR ECONOMY: VALORIZATION OF WASTE PLANT BIOMASS TO PRODUCE ACTIVE INGREDIENTS WITH ANTIMICROBIAL ACTIVITY AGAINST HUMAN AND PLANT PATHOGENS Giovanna Simonetti*, Elisa Brasili and Gabriella Pasqua Department Environmental Biology, La Sapienza University, Rome, Italy

ABSTRACT Plant extracts rich in bioactive compounds represent an alternative to the use of synthetic drugs. Extensive research over the last two decades has identified plant antimicrobials with a broad spectrum of activity against a variety of fungal and bacterial pathogens. Plant biomass wastes from agricultural and agro-industrial processes aim at a “zero waste” economy and represent the most important source of phytochemicals. This review provides information in processing technologies for the valorization of agroindustrial biomass wastes with a dual purpose: to reduce agricultural waste and convert it into value-added metabolites active against human and plant pathogenic microorganisms. In this chapter, published studies on active ingredients against human and plant pathogens obtained from the wine industry, from the olive oil extraction industry and from the fruit juice industry have been considered.

Keywords: plant extracts, agricultural waste, food by-products, human pathogenic microorganisms, plant pathogenic microorganisms, antimicrobial activity, anti-biofilm activity

*

Corresponding Author’s E-mail: [email protected].

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INTRODUCTION Agricultural wastes show considerable interest because are low cost and ease of availability and reusability. A variety of food and agro-wastes have been adopted as sources for new compounds with different biological activities. Some plant wastes and the byproducts, from agricultural and agro-industrial process, contain appreciable amounts of bioactive compounds that can be extracted, purified, concentrated and reused as antimicrobial agents both against human and plant pathogens [1]. Plant wastes can be obtained from various production processes or from different agricultural techniques. Several plant extracts contain a plurality of biological active molecules, but only a small percentage of waste plant biomass has been explored for its antimicrobial activity. A large quantity of antimicrobials is used in the world for medical use, for food production and in agriculture. Consumption of antimicrobials to produce meat and fish products, and their use in agriculture increased the resistance to antimicrobials [2]. Antimicrobial resistance is a global issue and the presence of few antimicrobial agents on the market increases the risk. In the last decades, microbial infections and contaminations have become major concern for devastating consequences such as human and animal infection, food poisoning, resource contamination caused by pathogen microorganisms. Bacterial human pathogens are Gram positive and Gram negative- bacteria. Among the GRAM+ bacteria, Staphylococcus spp and Streptococcus spp cause cutaneous and systemic infections and Listeria monocytogenes, a bacterium ubiquitous in the environment and easily found in food. Among the GRAM- bacteria, Escherichia, Salmonella, Klebsiella, Vibrio, Campylobacter and Helicobacter are responsible of gastro-intestinal infections. Also fungi can be cause of human diseases. The fungal human pathogens cause of skin-related infections, that affect more than 20–25% of the world’s population, are yeasts as Candida spp, Malassezia spp and molds as dermatophytes [3]. Although these are not generally life threatening, they represent a common global problem. Furthermore, the treatments often require long-term therapy that are not resolving in all [4]. In addition to skin infections, fungi can cause severe diseases associated with high morbidity and mortality. The main fungal human pathogens cause of systemic infections are Candida spp., Aspergillus spp, Cryptococcus spp. and the dimorphic fungi [5, 6]. The past two decades have seen an increasing number of infectious diseases in both animals and plants, that have caused die-offs and extinctions in wild species, jeopardizing food security [7]. The main genera of bacterial pathogens that infect plants are Xylella, Pseudomonas, Xanthomonas, Erwinia, Pantoea, Brenneria, Agrobacterium, Ralstonia, Dickeya, and Pectobacterium [8]. The organisms traditionally referred to as phytopathogenic fungi form a very heterogeneous group, which also includes protozoa such as Myxomycota and Oomycota. Genera of fungi that cause important diseases or belonging to toxigenic species, are Botrytis, Colletotrichum, Phytophthora, Alternaria, Pyricularia, Pythium, Rhizoctonia, Fusarium, Aspergillus and Penicillium. The increase in microbial infections in humans and plants makes it necessary to study new antimicrobial agents. Plants are rich in a wide variety of secondary metabolites, such as tannins, terpenoids, alkaloids, and flavonoids, which have been found to have antimicrobial properties. This chapter provides an overview of the published results on extracts, obtained from wastes of vine-wine industry, olive-oil extraction industry, fruit juice industry, with the aim to recover antimicrobials active against human and plant pathogens.

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PLANT BIOMASS FROM AGRO-INDUSTRIAL WASTE: BYPRODUCTS OF VINE-WINE PRODUCTION CHAIN In the vine-wine industry, agro-waste is generated in large quantities. The wastes are of almost zero value and in some cases require an additional cost for disposal. Grape wastes from agronomic and wine industry include pomace (skins and seeds), stalks, seeds, and unripe grapes are source of added-value products. All these by-products, containing phenolic compounds, are source of added-value products [9].

Plant Biomass from Pomace Grape pomace consists of seeds, skins, stalks, and is an important waste of winemaking. Pomace weighs about 20% of the harvest grapes [10]. The compounds identified in grape pomace are anthocyanins, catechins, flavonol glycosides, phenolic acids, alcohols and stilbenes. According to the current EU and national legislation, the pomace, in the oenological establishments, must be disposed of in a short time. The pomace can be spread in the vineyard as it is permitted by European regulations under certain conditions relating to the quantity, time and characteristics of the soils. The spreading of the pomace on the vineyard does not lead to an appreciation of waste and this solution can lead to contamination and infection. Another use of these biomasses is the compost preparation, which can be used in the vineyards, as well as sold it for agricultural and gardening purposes, though it does not have a high fertilizing capacity. Moreover, this waste biomass could be used for energy purposes and for the production of grappa and alcohol. In the last years, the pomace is used in the nutraceuticals, added to some baked goods in order to improve their nutritional properties, as additives and food supplements rich in fibers, usable in the condiments or in yogurt, or in the production of an edible coating to preserve fruit, vegetables and other foods. Moreover, in Europe the use of the pomace has been authorized to produce cold cuts. To date, pomace and its components are used for antioxidant and microcirculation activities. In addition to these activities, pomace extracts have been shown to have antimicrobial activity against specific strains of bacteria and fungi. Several authors have reported the antimicrobial activity of the pomace against human pathogens such as Aeromonas hydrophila, Bacillus cereus, Enterobacter aerogenes, Enterococcus faecalis, Escherichia coli, E. coli O157:H7, Mycobacterium smegmatis, Proteus vulgaris, Pseudomonas aeruginosa, Pseudomonas fluorescens, Salmonella enteritidis, Salmonella Typhimurium, S. aureus. All the bacteria tested were inhibited by extract concentrations of 2.5, 5, 10 and 20% [11, 12]. Pomace extracts coming from wine grape (Vitis vinifera L.) varieties grown in Turkey and collected from local wine processing plants inhibited the growth of the foodborne pathogens such as Enterobacteriaceae (E.coli and Salmonella) and S. aureus in beef patties [11]. Olejar et al. [13] demonstrated the bactericidal activity of pomace extract against S. aureus and E. coli. The minimum concentration (MBC) of the extract were 0.125% (w/v) against S. aureus, and 2.0% (w/v) against E. coli. Tseng and Zhao [14] reported the antibacterial activity of pomace extracts against Listeria innocua ATCC 51142 and E. coli ATCC 25922 with minimal inhibition concentration (MIC) ranged from 3% to 9% against E. coli, and from 2% to 8% against L. innocua. Pomaces from four selected Virginia‐grown grape varieties were assessed

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for their antibacterial activity by Xu et al. [15]. Red grape varieties were Cabernet Franc (Vitis vinifera) and Chambourcin (hybrid grape variety), while white grape varieties were Vidal Blanc (hybrid grape variety) and Viognier (Vitis vinifera). All extracts showed antibacterial activity against L. monocytogenes and S. aureus, but no antibacterial activity was exhibited against E. coli O157:H7 and S. Typhimurium. The minimum inhibition (MIC) and minimum bactericidal concentration (MBC) of all tested pomace extracts against L. monocytogenes ranged from 4.69 to 18.8 mg/mL and from 9.38 to 37.5 mg/mL, respectively. Cabernet Franc pomace extract showed the lowest MIC (4.69 mg/mL) and MBC (9.38 mg/mL) [15]. Sanhueza et al. [16] showed the antibacterial activity of the grape pomace extracts obtained with chloroform and ethyl acetate from the Cabernet Sauvignon and Syrah varieties. The results demonstrated that Cabernet Sauvignon variety have a broad-spectrum antibacterial activity against food transmitted pathogens. Simonetti et al. [17] demonstrated the antifungal activity of crude extracts from non- fermented grape pomace, entrapped in poly(lactic-co-glycolic) acid nanoparticles (NPs), on Candida biofilm. Crude pomace extract entrapped in NPs exerted a significantly higher anti-biofilm activity compared to their free forms. Pomace extract-loaded PLGA NPs destroyed 37% of the C. albicans mature biofilms. In particular, pomace extract-loaded PLGA NPs showed a BMIC50 of 50 µg/mL against C. albicans ATCC 20891 mature biofilm.

Plant Biomass from Grape Seeds In the last decades, several studies have been focused on human health benefits of grape extracts [18]. Seed extracts have been recognized safe by Food and Drug Administration and are used as food additives and in cosmetics. Several authors reported the antimicrobial activity of grape seed extracts [19]. In particular, antibacterial activity against Gram positive human pathogens such as L. monocytogenes [20], S. aureus [21, 22], Streptococcus mutans [23], Enterococcus faecalis and Streptococcus pneumonia [24] has been demonstrated. Among gram negative bacteria, E. coli O157:H7, an enteropathogen responsible for hemorrhagic colitis, bloody diarrhea, and hemolytic uremic syndrome, was inhibited from Vitis rotundifolia grape seed extracts [25]. Muscadine seed extract showed MIC values ranged from 256 to 1024 µg/ml against Helicobacter pylori, etiological agent of peptic ulcer and gastritis [26]. Luther et al. [27] showed bactericidal activity of Chardonnay seed flour extracts against E. coli. Ahn and others [28] reported that grape seed extracts in cooked ground beef reduced the growth of contaminants of meat and poultry products during refrigerated storage. 1.0% of grape seed extract reduced E. coli O157:H7, L. monocytogenes, S. Typhimurim and Aeromonas hydrophila of 1.5, 2, 1 and 3 Log CFU, respectively. Ahn and others demonstrated that grape seed polyphenols caused disruption of the bacterial cell wall [28]. Grape seed extracts were found to be effective in inhibiting Klebsiella pneumoniae [29], Vibrio vulnificus [30] and Campylobacter jejuni [31]. Baydar and colleagues [32] reported the antibacterial activities of the seed extracts coming from three different grapes. The extracts at 5% concentrations showed bactericidal activity against A. hydrophila, Bacillus cereus, E. aerogenes, E. faecalis, E. coli, E. coli O157:H7, K. pneumoniae, M. smegmatis, vulgaris, P aeruginosa, P.s fluorescens, S. enteritidis, S, Typhimurium, S. aureus and Yersinia enterocolitica. Regarding antifungal activity, Simonetti et al. [33] for the first time, demonstrated, in vitro and in vivo, anti-Candida activity of grape seed extracts, obtained from

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wine and table cultivars of Vitis vinifera L., grown in different agronomic conditions. The authors have showed a significant correlation between anti-Candida activity and the content of the flavan-3-ols in grape seed extracts, with a polymerization degree ≥4. Cheng et al. [34] have showed the anti-Candida activity of extracts obtained from Pinot noir and Pinot meunier seeds with MIC values of 0.39 and 50 mg/mL, respectively. Simonetti et al. [35] for the first time, demonstrated the anti‐ dermatophytes and the anti-Malassezia activities of Vitis vinifera seed extracts obtained from different table and wine cultivars. The authors showed GMMIC values ranged from 20 to 97 µg/mL for dermatophytes and from 32 to 161 µg/mL for Malassezia furfur. The activities were correlated with the amount of the polymeric fraction of the flavan-3-ols.

Plant Biomass from Unripe Grapes Unripe grapes are a large source of waste material derived from the wine industry. Unripe grapes are discarded during cluster thinning. Cluster thinning practice is used to increase the size of table grapes and improve berry quality [36]. This waste could be used to obtain extracts rich in bioactive compounds, safe for human health [37]. Karabiyikli and Öncül [38] reported the antibacterial activity of verjuice and five sour grape sauce against B.s cereus, E. coli, L. monocytogenes, S. Typhimurium and S. aureus. The MICs of un-neutralized unripe grape products ranged from 6.25% to 50%. Simonetti et al. [39] demonstrated anti-Candida spp. and anti-dermatophytes activity of unripe grape extracts from agro-industrial wastes. GM MIC of extracts ranged from 53.58 to 214.31 µg/mL for Candida spp. and from 43.54 to 133.02 µg/mL for dermatophytes. The antifungal activity correlated with polymeric flavan-3ols for Candida spp. and with caffeoyl derivatives for dermatophytes. In V. vinifera plant and in their wastes are found stilbenes. Among them, resveratrol and pterostilbene have long been studied due to their positive influence on human health. Moreover, some authors reported their antimicrobial and antibiofilm activity [40-44]. Fungi reported to be sensitive to resveratrol, both against human pathogens such as C. albicans, Saccharomyces cerevisiae and Trichosporon beigelii and against plant pathogens such as Phytophthora palmivora, P. capisci, Aspergillus flavus, Fusarium spp. and Verticillium spp. [45]. One of the advantages of these compounds is their low cytotoxicity. Resveratrol and pterostilbene showed low toxicity in normal hemopoietic stem cells [46] and pterostilbene oral administration to nude mice (100 µg/kg per day) for 8 weeks did not produce signs of acute toxicity [47].

PLANT BIOMASS FROM AGRO-INDUSTRIAL WASTE: BYPRODUCTS OF THE OLIVE-OIL EXTRACTION INDUSTRY Antimicrobial Activity against Human Pathogens Olive-oil production process, fruit harvesting, and tree pruning generates large quantity of wastes and by-products such as crude olive cake, vegetation water, twigs and leaves. Technological innovation and research in recent years have produced new solutions for the management of the by-products of olive processing, which continue to represent an important

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cost item in the economic balance sheet of extra virgin olive oil production. Olive leaves and cakes have been traditionally used for animal feeding, but they can be used in other applications such as food additives, nutraceuticals, and pharmaceutical and cosmetic purposes due to their high content of high added-value compounds with antioxidant and antimicrobial properties [48]. The process of olive oil production is accompanied by generation of a considerable amount of olive mill wastewater (OMWW) [49]. It is estimated that in the world annual production of OMWW is between 7 and over 30 million m3. Research into finding new uses for by-products of olive oil production is of great interest not only to the economy but also to the environment, particularly in areas where olives are grown and OMWW is wasted. In this context, there is an urgent need to find ways of treating this liquid residue and other by-products from the olive oil industry. Several approaches to treat OMWW have been suggested including anaerobic biodegradation, detoxification by fungi, ozonation as well as other new bioremediation and biovalorisation strategies [50-52]. On the other end, OMWW is potentially a rich source of a diverse range of phenols with a wide array of biological activities. Bianco et al. [53] identified 20 phenolic compounds in OMWW using HPLC-MSMS. The prevalent classes of hydrophilic phenols identified include phenyl alcohols, phenolic acids, secoiridoid derivatives, flavonoids (luteolin, luteolin-7- glucoside), and lignans. Solid residues, such as “Patè”, contain peel and seeds and a significant amount of phenolic compounds. Nuezhenide is found only in seeds as a predominant phenol, whereas verbascoside only appears in significant quantities in the seeds and pulp [51, 54]. Tyrosol and hydroxytyrosol have been detected in olive stones, whereas decarboxymethyl oleuropein has been found in the pulp, seeds and stones. The most abundant phenolic compounds are tyrosol and hydroxytyrosol, together with p-coumaric and, to a lesser extent, vanillic acid [55, 56]. Other minor compounds identified include verbascoside, rutin, caffeoylquinic acid, luteolin4-glucoside, 11-methyloleoside, hydroxytyrosol-10-b-glucoside, luteolin-7-rutinoside, and oleoside [56]. Recently, Mulinacci et al. [57] demonstrated that OLIVE-paste and OLIVEwater derived from olive fruit milling and from filtered vegetation water from olive milling, respectively showed a different chemical profile simple phenol (as hydroxytyrosol) and secoiridoids (mainly oleuropein derivatives). OLIVE-paste extract contained several oleuropein derivatives. The total phenols differed greatly between the two extracts in terms of mg/g, but a negligible difference was highlight when the phenols were expressed as nanomol/g. The antioxidant capability of OLIVE-paste was noticeably higher, suggesting that oleuropein derivatives were more active antioxidants than free hydroxytyrosol. Several studies have shown that these compounds are effective as antibacterial, antiviral, and antifungal compounds. Obied et al. [58] reported that the phenolic fraction of OMWW showed antibacterial activities against several bacterial species (S. aureus, B. subtilis, E. coli and P. aeruginosa). Moreover, other studies have shown that the significant bactericidal and fungicidal activities of OMWW are predominantly tied to their phenolic monomer contents, such as hydroxytyrosol and tyrosol. The “Pâté”, essentially consisting of the olive pulp and skin remaining after the separation of the oil phase, preserves, in addition to a small percentage of oleic, palmitic and polyunsaturated acids, many chemical compounds with a high nutraceutical value, such as hydroxytyrosol, tyrosol, secoiridoid derivatives and other biophenols [59, 60]. Spray-dried olive mill wastewater has been tested on the antimicrobial and anti-biofilm against Campylobacter strains isolated from chicken meat. Campylobacter develops biofilms that are resistant to environmental stress, antibiotics, and disinfectants and are becoming a major issue for the food industry. The phenolic profile of spray-dried olive

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mill wastewater mainly consisted of secoiridoid and hydroxycinnamic acid derivatives. Oleuropein-aglycone di-aldehyde (a secoiridoid derivative) was the major constituent. The extract was able, in vitro, to inhibit biofilm formation and to promote biofilm dispersion [61]. Olive mill wastewater extracts, and the olive cake extracts could also reduce the use of drugs in animal production and could represent promising alternatives to antibiotics. Antimicrobial potential of the phenolic has been demonstrated against S. aureus, whereas the biophenols extracts showed more limited activity against E. coli and E. faecalis [62]. Phenolic compounds as well as OMWW extracts were evaluated in vitro for their antimicrobial activity against Gram-positive (S. pyogenes and S. aureus) and Gram-negative bacteria (E. coli and K.a pneumoniae). Most of the tested phenols were not effective against the four bacterial strains when tested as single compounds at concentrations of up to 1000 µg/mL. Hydroxytyrosol at 400 µg/mL caused complete growth inhibition of the four strains. Gallic acid was effective at 200, and 400 µg/ mL against S. aureus, and S. pyogenes, respectively, but not against the gram-negative bacteria. An OMW fraction called AntiSolvent was obtained after the addition of ethanol to the crude OMW. HPLC analysis of AntiSolvent fraction revealed that this fraction contains mainly hydroxytyrosol (10.3%), verbascoside (7.4%), and tyrosol (2.6%). The combinations of AntiSolvent/gallic acid were tested using the low minimal inhibitory concentrations which revealed that 50/100–100/100 µg/mL caused complete growth inhibition of the four strains. These results suggest that OMW specific fractions augmented with natural phenolic ingredients may be utilized as a source of bioactive compounds to control pathogenic bacteria [63]. OMWW extracts and single phenolic compounds were evaluated in vitro for their antimicrobial activity against Gram - positive (S. pyogenes and S. aureus) and Gram-negative bacteria (E. coli and K. pneumoniae). The compounds, found in OMWW, that exhibited antibacterial activity were hydroxytyrosol, oleuropein, 4-hydroxybenzoic acid, vanillic acid, and p-coumaric acid. In particular, hydroxytyrosol at 400 µg mL−1 caused complete growth inhibition [64-67]. OMWW from processing of cvs. Mission and Frantoio olive fruit contained higher total phenol content. Individual biophenols with the exception of verbascoside and a hydroxytyrosol-secoiridoid were also present at higher concentrations in the OMWW produced from Mission cultivar. Antioxidant activities were measured in aqueous (DPPH) and emulsion (BCBT) systems. The Frantoio extract was more active than the Mission extract in the DPPH assay – EC50 values were 28.3 ± 1.7 ppm and 34.7 ± 1.7 ppm, respectively. Activities were reversed in the BCBT, with the Mission extract (EC50 60.6 ± 2.3 ppm) more potent than the Frantoio extract (EC50 79.9 ± 2.0 ppm), and this may be related to the more lipophilic nature of the Mission extract. Both extracts showed broad spectrum antibacterial activity against S. aureus, B. subtilis, E. coli and P. aeruginosa; whereas individual biophenols (hydroxytyrosol, luteolin, oleuropein) showed more limited activity. Molluscicidal activity was measured against Isidorella newcombi and LD50 values were 424 ppm and 541 ppm for Mission and Frantoio extracts, respectively [68]. Polyphenols obtained through solvent-free microwave-assisted extraction from olive leaves, a pruning waste, showed antibacterial activity against S. aureus and S. epidermidis, with a minimum inhibitory concentration (MIC) value of 1.25 mg/mL [69]. Olive polyphenols such as hydroxytyrosol have been found to act in vitro against both Grampositive and Gramnegative bacteria responsible for respiratory and intestinal tract infections. In this study five ATCC standard bacterial strains (H.s influenzae ATCC 9006, Moraxella catarrhalis ATCC 8176, Salmonella Typhi ATCC 6539, Vibrio parahaemolyticus ATCC 17802 and S.s aureus ATCC 25923) and 44 fresh clinical isolates (H.s influenzae,

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eight strains, M. catarrhalis, six strains, Salmonella spp, 15 strains, V.o cholerae, one strain, Vibrio alginolyticus, two strains, Vibrio parahaemolyticus, one strain, S.s aureus, five penicillin-susceptible strains and six penicillin‐resistant strains), causal agents of intestinal or respiratory tract infections in man, were tested for in‐vitro susceptibility. The minimum inhibitory concentrations (MICs) highlighted a broad of antimicrobial activity of hydroxytyrosol against these bacterial strains (MIC values between 0.24 and 7.85 µg/mLfor ATCC strains and between 0.97 and 31.25 µg/mL for clinically isolated strains) [70].

Antimicrobial Activity against Plant Pathogens The intensive and indiscriminate use of synthetic chemicals, released into the environment, has negatively affected the development of different species, including the wildlife fauna. For several years now there has been a great deal of attention in the search for alternatives to chemical pesticides in many crops [71]. Scientific community opinion about the recycling of OMWW in agriculture, is controversial between those considering only the negative side as phytotoxicity and antimicrobial effects of OMWW and those considering only the positive side as soil fertilization [72, 73]. Recently, some studies have demonstrated interesting bactericidal and fungicidal activities of OMWW and especially of its phenolic monomers as hydroxytyrosol and tyrosol [74]. An hydroxytyrosol enriched extract obtained from olive mill wastewaters was tested on two olive tree pathogens, Pseudomonas savastanoi pv. savastanoi (Pss) and Agrobacterium tumefaciens (At). Pss, in particular, is the etiological agent of the olive knot disease responsible of severe production losses. Chemical characterization allowed to identify and quantify hydroxytyrosol as the main constituent along with other low molecular weight phenols. The total extract has proven significant antimicrobial activity against Pss and At in vitro, higher than hydroxytyrosol alone, suggesting an important role also of the minor phenolic components, which synergistically act with this compound [75]. In a recent study, the addition of OMWW to soil exerted significant disease suppression against the soil-borne diseases caused by Rhizoctonia solani and Fusarium solani [76]. In another study, the effect of sterilized and filter sterilized OMWW was tested in vitro: a) on mycelium growth of Fusarium oxysporum f.sp. lycopersici, Pythium spp., Sclerotinia sclerotiorum and Verticillium dahliae on PDA agar plates; b) on sporulation of Penicillium italicum and P. digitatum and B.s cinerea on infested with the pathogens fruit and-vegetables (oranges and red horn peppers) and c) on planta, tomato plants infested with the fungus F. oxysporum f.sp. lycopersici. The results showed that the filter sterilized OMWW inhibits the mycelium growth of all tested fungi in vitro, due to phenolic compounds which are contained in olive OMWW [77]. Xylella fastidiosa, a Gram-negative bacterium that appeared suddenly in 2010, has devastated large areas of olive groves in Salento (Apulia, Italy). Symptoms consist of withering and desiccation of scattered terminal shoots, which rapidly expands to the rest of the canopy, and results in the death of the tree. Moreover, Italy has banned the use of antibiotics for plant diseases management (D.M. 10.08.1971, in G.U. 212 del 23.08.1971) and also in EU a contentious debate has been opened concerning the possible development of antibiotic resistance in human pathogens [78]. Other managing strategies are therefore urgently needed. Since X. fastidiosa is limited to the plant xylem, particular attention has been given to small molecules that can reach the xylem sap flow and that can inhibit the growth

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and movement of the pathogen. Recently, in vitro antibacterial activity of OMWW-derived fractions was for the first time demonstrated to inhibit the growth of bacterium X. fastidiosa at the minimum tested concentration of 1% (v/v) [79]. Verticillium wilt, caused by Verticillium dahliae Kleb., is one of the most devastating plant diseases worldwide and a challenge for producers to find effective means of its control [80]. V. dahliae has a wide host range including economically important crops. The fungus invades the plant through the roots and may spread from there, through the stem to the leaves. Vascular wilts are particularly notorious since, in the vascular system of host plants, the pathogens cannot be reached by many fungicides and few of them are able to cure plants once they are infected. An hydroxytyrosol-rich (29.27% weight/dry weight) olive mill wastewater and a hydroxytyrosolrich (52.67% weight/dry weight) extract were prepared from fresh OMWW using hydrolysis and post-hydrolysis purification processes and were tested as bio-fungicides. The extracts showed strong fungicidal activity in vitro against V. dahliae with minimal fungicidal concentrations (MFCs) of 28–56 mg/L (dry weight). In tomato experiments incorporation of OMWW into the soil reduced significantly Verticillium wilt disease incidence by 86 compared to untreated plants [81].

VALORIZATION OF FRUIT BY-PRODUCTS AS A SOURCE OF BIOACTIVE COMPOUNDS WITH ANTIMICROBIAL ACTIVITY The agro-food processing industry yields a considerable amount of waste or by-products (peels, seeds and pulps), which represents 50% of the raw processed fruit [82]. These byproducts are considered a valuable source of functional ingredients, such as flavonoids, dietary fibres and essential oils with antimicrobial activity [83].

Wastes from Apple Processing Domesticated apple (Malus × domestica Borkh.) belongs to the genus Malus (Rosaceae family) and is one of the most important fruit crops worldwide. According to FAOSTAT (2018) [84], the world production of apple has increased by 424% from 17.0 million tons in 1961 to 89.3 million tons in 2016 and leading production nations include China, USA, Poland, Turkey, Iran, Italy, Russia, Uzbekistan, and Ukraine. Currently, apples are processed into several food products including juice apple sauce, slices (dried, frozen and canned) and cider (sweet and hard) [85]. The increased production of apples as well as the demand for plant-derived food products have resulted in dramatic increase of wastes. In large-scale apple juice production, 75% of the apples are utilized for juice, while the remaining 25% are discarded as waste or utilized rather inefficiently [86]. Apple pomace consists of apple skin, seeds, and flash, and represents about 25% of a fruit’s fresh weight [87]. It was demonstrated that apple pomace contains over 60 different phenolic compounds, insoluble carbohydrates (cellulose, hemicellulose, pectin and lignin), simple sugars (glucose, fructose and sucrose), as well as small amounts of acids, minerals, proteins, vitamins, and others [88-90]. The main bioactive compounds are flavonoids (phloretin and quercetin glycosides, flavone derivatives and catechins) as well as organic acids [91, 92]. In a recent study of Radenkovs et al. [85],

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apple pomace oils from different Malus spp. were analyzed using gas chromatography-mass spectrometry (GC/MS) and reversed-phase-liquid chromatography coupled with fluorescence detector (RP-HPLC/FLD) systems. A plethora of essential fatty acids, tocopherols and phytosterols with antimicrobial activity were identified and quantified. The chemical analysis revealed that Malus cv. “Ola” is rich in linolenic (57.8%), α-linolenic (54.3%), and oleic (25.5%) acids. M. Bernu prieks, followed by M. cv. “Ola”, and M. soulardii pomace oils showed the highest content of total tocopherols such as δ-tocopherol. β-sitosterol was the prevalent compound determined in all tested pomace oils with a percentage distribution of 10.3–94.5%. The main triterpene identified in the oils was lupeol, which varied in the range of 0.1–66.3%. These pomace oils from M. spp. showed differing antimicrobial activity against bacteria. The pomace oil of M. cv. “Ola” showed an inhibition of both Gram-positive and Gram-negative test cultures, while, to a lesser extent, the M. Berzukroga dzeltenais pomace oil had the ability to inhibit only Gram-negative pathogenic bacteria. In particular, the pomace oil of M. cv. “Ola” had a MIC value o f 31.2 mg mL−1 for Gram - pos itive S. aureus. The pomace oil of M. Bernu prieks, M. cv. “Ola”, and M. Berzukroga dzeltenais exhibited an inhibitory activity with MIC value 31.2 mg/ mL against E. coli, while only pomace oil of M. cv. “Ola” and M. Berzukroga dzeltenais were able to suppress the growth of P. aeruginosa at a concentration of 31.2 mg/mL [85]. Interesting, the phytochemical constituents of apple waste were established also as potential antifungal agents for the control of fungal plant diseases. In a recent in vitro study, Oleszek et al. [93] tested crude, purified extracts and fractions of apple pomace to evaluate their antifungal against four crops pathogens, specifically, Botrytis sp., F. oxysporum, Petriella setifera, and Neosartorya fischeri. The phytochemical constituents of the tested materials were mainly represented by phloridzin and quercetin derivatives, as well as monoterpene–pinnatifidanoside D. The apple pomace extracts containing quercetin hexosides possessed stronger antifungal activity against N.fischeri, Botrytis sp and P. setifera at the concentration of 100 µg/mL. Zhang et al. [94] have isolated phenolic compounds from Golden Delicious pomace with five organic solvents (methanol, ethanol, acetone, ethyl acetate, and chloroform), and the antimicrobial activities of these extracts was determined. Phloretin, phloridzin, and ethyl acetate extracts all have activities against both S. aureus and E. coli. Phloretin, which accounted for 41.94% of total flavnoids in ethyl acetate extract, has the highest antimicrobial activity against both S. aureus and E. coli, and in particular against S. aureus ATCC 6538, with zones of inhibition between 16.09 and 39.17 mm for S. aureus and between 12.57 and 28.25 mm for E. coli. Other constituents less studied in the apple, especially in the cuticle waxlayer, such as terpenoids, have been associated with several interesting properties, including antibacterial activity. Among triterpenoids, an important representative is ursolic acid (UA) that it was associated with antimicrobial effects against several bacterial species [95]. The spectrum of MIC values is very broad and the activity depends mainly on the species (strain) tested. The best MIC values (from 2.5 to 8.0 µg/mL) were against Gram-positive species, such as S. aureus, methicillin-resistant S. aureus, vancomycin-resistant enterococci, and M. tuberculosis [96]. As reviewed by Waldbauer et al. [87] apple pomace rich in procyanidins and phloridzin was tested on growth-inhibiting effects against Helicobacter pylori strains, a pathogen that enhances the possibility to develop gastritis, and gastric or duodenal ulcer in infected patients. The 10% hot-water pomace extract did not exhibit any growth-inhibiting effect in agar diffusion test when administered alone. However, in combination with quince juice and wild or cultivated cranberry juice, synergistic growth-inhibiting effects were observed. The 4%

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stock solution of apple skin extract showed a bactericidal activity against E. coli O157:H7, L. monocytogenes RM2199, Salmonella enterica RM1309, and non-MRSA-resistant S. aureus 1200. Dilutions of the apple skin extract stock solution, killing 50% of the afore mentioned pathogens, were > 2.7%, 1.39%, 0.007%, and 0.002%, respectively.

Red Beet By-Products Among the major agro-industrial wastes with antimicrobial properties, red beet byproducts are also found. Red beet pomace from the juice industry, accounts for 15–30% of the raw material and is usually discarded as feed or manure, even though it has a high content of betalains. Betalains are water-soluble nitrogenous pigments, which consist of two main groups, the red betacyanins and the yellow betaxanthins [97]. They confer the color of the beet, and the phenolic portion of the peel has l-tryptophan, p-coumaric and ferulic acids and cyclo-dopa glucoside derivatives. Red beets are considered among the 10 most effective vegetables, in terms of antioxidant capacity, with the largest amount of total phenolics being found in the peel (50%). Thus, it is crucial to explore red beet pulp and peel, as little is known about their antimicrobial activity. Vodnar et al. [98] showed a high antibacterial activity of red beet waste against L. monocytogenes, with a MIC of 1.953 (mg/mL). This result may be due to the content of phenolic compounds like betacyanins compounds including betanidin, isobetanidin, betanidin-5-O-b-glucoside and isobetanidin-5-O-b-glucoside. A high inhibitory activity was also demonstrated against the Gram-negative bacterium, E. coli, by red-beet waste with an MIC of 1.953 (mg/mL) and an MBC of 3.9 (mg/mL). It also demonstrated that red-beet waste extracts exhibited the high inhibitory activities against S. Typhimurius and P. aeruginosa (MIC = 3.9 and MBC = 7.81).

BY-PRODUCTS OF THE POMEGRATE PROCESSING INDUSTRY A fruit bearing-plant that has been widely recognized for its medicinal properties is pomegranate (Punica granatum L.). Pomegranate peel (PoP) is a byproduct of the fruit juice processing industry, comprising nearly 30–40% of fruit portion. PoP has been used by many cultures around the world for treating health, particularly headaches and stomach problems [99]. It is known to be a good source of phenolic acids, tannins (ellagitannins such as punicalin and punicalagin) and flavonoids that exhibit synergistic antibacterial effects towards different pathogenic and drug resistant bacterial strains such as Salmonella sp., Streptococcus sp., Staphylococcus sp, L. monocytogenes, E. coli and P. aeruginosa [100]. Methanolic extracts from PoP at a concentration of 12 mg mL-1 showed antimicrobial activity against S. aureus, Staphylococcus epidermidis, Lactobacillus acidophilus, Actinomyces viscosus, Streptococcus mutans, Streptococcus sanguinis and Streptococcus salivarius having inhibition zones of 12.5, 13.5, 10.0, 6.5, 9.5, 11.5 and 9.5 mm respectively [101]. The watermethanol extracts from PoP demonstrated a remarkable antibacterial activity also against common food-borne pathogens (L. monocytogenes, S. aureus, E. coli and Yersinia enterocolitica) [102]. This activity was related with the large levels (262.5 mg mL-1) of phenolic compounds present in PoP. Pomenagrate peel extracts owned a strong broad-

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spectrum of antibacterial activity against Gram-positive (B.s subtilis and S. aureus) and Gram-negative (K.a pneumonia) bacteria, with MIC ranging from 0.2 to 0.78 mg/mL [103]. It was also reported that methanolic PoP extracts exhibited a significant antibacterial activity against Trichophyton rubrum, S. Typhimurium, Salmonella anatum, P. aeruginosa with MICs of 0.125, 0.25, 0.25 and 0.5 mg/mL respectively, suggesting that PoP powder or extract might be utilized in coating and preservation of cooked food products for improving their shelf life [104]. Pomenagrate peel is also a rich source of antifungal constituents. High levels of tannins and phenolic compounds as punicalgin were attributed to its powerful antifungal properties. Foss et al. [105] reported that the crude extract of PoP showed good antifungal activity against four species of dermatophyte fungi as Trichophyton mentagrophytes, T. rubrum, Microsporum canis and Microsporum gypseum with MICs of 0.125, 0.125 and 0.25 mg mL1 respectively. Punicalagin seems to be the major component of PoP which acts on the conidial and hyphal structures of dermatophytes. Methanolic extracts from PoP at concentrations of 4, 8 and 12 mg mL-1showed antifungal activity against C. albicans with inhibition zones of 6.0, 6.5 and 6.5 mm respectively [101]. A remarkable antifungal activity of water–methanol PoP extracts was observed against A. niger, Candida utilis and Saccharomyces cerevisiae having inhibition zones of 12, 18 and 14 mm respectively [102]. The Pop antibacterial activity is also cultivar-dependent. Rosas-Burgos et al. [106], demonstrated that PoP extracts (5 mg mL-1) from sour–sweet cultivar showed high levels of ellagic acid (16.5 mg g-1) and punicalagins (239 mg g-1) responsible for a strong antifungal activity against Aspergillus flavus, Fusarium verticillioides, Alternaria alternata and B.s cinerea with inhibition values of 39.2, 70.0, 50.0 and 50.8% respectively. Kharchoufi et al. [107] reported that methanolic PoP extracts were effective against Penicillium digitatum and S. cerevisiae and able to change the shape of fungi. The microscopic observations revealed that hyphae were wilted and coiled in P. digitatum plates containing PoP extract compared to elongated and extended ones present in the control. In C. albicans treated with punicalagin extracted from PoP, an irregular budding pattern, pseudo-hyphae, reduced cytoplasmic contents, thickened cell wall and changed space between the cell wall and cell membrane were the alterations observed under the scanning electron microscope [108]. Tehranifar et al. [109] observed significant inhibitory effects of methanolic PoP extracts (500, 1000 and 1500 ppm) on the mycelia growth and spore germination of three postharvest fungi (Penicillium italicum, Rhizopus stolonifer and B.s cinerea).

Citrus By-Products The consumption of citrus fruits, either as fresh produce or in the juice form, is known to be associated to health benefits. The production of juice and other products from citrus fruits results in the generation of large amounts of citrus by-products every year that can be valorized since they contain a wide range of healthy bioactive compounds [110-111]. A large amount of compounds with biological activities including flavanone glycosides, polymethoxylated flavones and flavanones that are unique to citrus have been found to be comparatively rare in other plants [112, 113]. It has been reported that the citrus peel extracts exert antimicrobial effects against food-borne pathogens due to the present quinones, terpenoids, polyphenols, phenolic acids, and tannins [114, 115]. Citrus seeds are other byproducts of citrus fruit processing rich in bioactive compounds [116]. In a recent study,

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Ndayishimiye et al. [117] demonstrated a high antimicrobial activity of oils obtained from a mixture of citrus by-products and extracted by using supercritical carbon dioxide and ethanol at 200 bar against B. cereus and S. aureus (MIC 0.20 and 0.25 mg/mL, respectively). This antimicrobial activity was attributed to compounds as tocopherol, sterols and other lipophilic compounds present in mixture oils, which could contribute to synergism with the volatile compounds including monoterpene hydrocarbons, sesquiterpene hydrocarbons, and oxygenated monoterpenes. These compounds play an important role in bacterial inhibition owing to their hydrophobic property, which enables them partition the lipids of the bacterial cell membrane and mitochondria, distracting the structures and rendering them more permeable, which leads to an outflow of proteins and other cell contents, and therefore the bacteria dies. Geraci et al. [118] investigated the orange peel of 12 cultivars of Citrus sinensis from central-eastern Sicily identifying a plethora of essential oils such as d-limonene (73.9– 97%), linalool, geraniol and nerol with antimicrobial activity against Gram positive and Gram negative bacteria. In particular, the essential oil ‘Sanguinello’ from Paternò showed a MIC value of 15 mg/mL against the two strains of L. monocytogenes, whereas the essential oil ‘Moro Solarino’ was less active, showing a MIC value of 92 mg mL-1against the S. aureus and P. aeruginosa. Recently, Fratianni et al. [119] identified and quantified several polyphenols of peel and pulp of three Citrus taxa: Citrus medica, Citrus bergamia, and Citrus medica cv. Salò, cultivated in the Cosenza province, Southern Italy, including acidic phenols as gallic acid, chlorogenic acid, caffeic acid, coumaric acid, ferulic acid, and flavonoids as rutin, epicatechin, quercetin, apigenin, catechin. These compounds exerted antibacterial activity against E.coli, L. monocytogenes, P. aeruginosa, S. aureus, and Pectobacterium Carotovorum with MIC value < 10 mg/mL. Interesting, polyphenols present in the peel of bergamot showed also the ability to inhibit the formation of biofilms by L. monocytogenes (92.02% of the biofilm was inhibited just with 1.2 mg of citrus peel extract). In addition, 6 mg of such extract inhibited up to 90% of the biofilm formation by S. aureus. These evidences demonstrate that fruit by-products obtained from agro-food processing industry are nontoxic and effective antimicrobial source that inhibits the growth of wide range of pathogenic and food spoilage microbes. Fruit by-products could be added to foods to prevent microbial growth and to reduce food losses caused by microbial decom-position as well as used by pharmaceutical industry for their bacteriostatic and fungistatic activity. However, the mechanism on how plant extracts can inhibit the microorganisms is complex because both major and minor compounds can contribute to the inhibition and further studies are still needed to identify active components of fruit juice by-products, their mechanism of action and effectiveness.

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In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 10

THE CIRCULAR ECONOMY AND BUILT ENVIRONMENT. MAINTENANCE, REHABILITATION AND ADAPTIVE REUSE: CHALLENGING STRATEGIES FOR CLOSING LOOPS Serena Viola1, Stefania De Medici2, and Patrizia Riganti3 1

Department of Architecture, University of Naples Federico II, Italy Department of Civil Engineering Architecture, University of Catania, Satellite Campus of Architecture, Siracusa, Italy 3 School of Interdisciplinary Studies, University of Glasgow, Dumfries, Scotland, UK

2

ABSTRACT This paper discusses attitudes towards maintenance, rehabilitation, and adaptive reuse as strategies to give new life to decaying and abandoned spatial and social contexts (World Economic Forum, 2018). The methodology is based on a mixed deductive and inductive approach, following three main steps: 1) conceptual framework; 2) design actions; 3) best practices screening. Through matching values preservation with resource optimization, life cycle lengthening emerges as a privileged medium for passing past identities to the future. Saving the performance of spaces or devices the approach suggested to fit best within a built system with high prior degrees of stiffness, working procedures, operators, and scheduled times. Integrating new systems and processes along side existing ones is a way to manage aging processes, as well as transferring, planning, and testing final suitability.

Keywords: built environment, maintenance, rehabilitation, adaptive reuse, life cycle



Corresponding Author’s Email: [email protected].

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INTRODUCTION Rapid and uncontrolled urbanization, spatial and social fragmentation, and drastic quality deterioration are some of the processes increasingly triggering the built environment today [1]. A theoretical framework recently outlined by the Ellen MacArthur Foundation [2] counteracts this trend, through an approach based on the hypothesis that ever-growing economic development can happen without ever-growing pressure on the environment. The European Commission recognizes the unique ability of cities to guide global transitions towards a Circular Economy, through a high concentration of resources, capital, data, and talents in a small geographical area [3]. Long relegated to the margins of the debate, built environment management has fully entered the waste reduction process in terms of resources, capabilities, and embedded values [4]. In a scenario marked by the environmental crisis, with emerging societal and economic challenges, theoretical debates and research have begun to focus on tailored approaches and measures aimed at finding compatible technologies to counteract trends of waste. The built environment is among those sectors which put the most pressure on the natural environment so its role in transitioning to a CE is pivotal, through dealing with rapid and uncontrolled quality deterioration, obsolescence, and abandonment. The specific aim of this work is to consider Circular Economy commitments in the light of actions for the quality improvement of built environments. Since the research on circular processes within built environments is still at an early stage [5], our methodology is based on a mixed deductive and inductive approach, following three main steps: 1) the conceptual framework; a critical review of international policies focusing on life cycle lengthening for built environments and quality improvements; 2) design actions (maintenance, rehabilitation and adaptive reuse) aimed at supporting the transition of the built environment towards circular processes through lengthening life cycles; and 3) best practices screening, with the support of a matrix that considers quality indicators given life cycle lengthening strategies in terms of resources, capabilities, and embedded values. Among the multiple meanings and implications given to the closure of loops, one that crosses the architectural field is life cycle lengthening, promoting trade-offs between users’ needs and past performances, and accounting for our planet’s needs. Commitment to quality is fundamental to meeting the multi-faceted demands of the CE for resources, capabilities, and embedded value preservation and promotion. Assuming the built environment as a key legacy of the cultural, economic, and social layering within settlements [6], the closure of loops requires us to not only to redefine solutions, but also to rethink design processes and strategies [7].

BUILDING RENOVATION AS A DRIVING FORCE IN THE CONSTRUCTION MARKET Over the past two decades, the construction industry in the Western world has reflected the trend to increasingly shift production targets from the construction of new buildings to the renovation of the existing building stock, thus reducing soil and raw material consumption.

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Indeed, the rate of building renovation has increased over time compared to that of new constructions, which is gradually decreasing [8-17]. The Construction Intelligence Centre (CIC) revised its global construction industry growth forecast upwards for the period 2018–2022, with an average annual increase of 3.6% [18]. According to the CIC report, growth in construction investment in emerging markets will steadily slow down, mainly reflecting Chinese trends, while it will increase throughout Western Europe. Indeed, European production in the construction industry will grow by an average of 2.4% per year in the period 2018–2022, with investments in building renovation outweighing new construction. In the USA, commitments in the field of building rehabilitation will be considerable; New York is currently experiencing massive redevelopment, and in the major cities construction is also expected to benefit from increased spending to repair hurricane damage (for example in Texas and Florida) [19]. The highest rate of building development in Europe occurred in 2017, with a 4.2% annual increase, the strongest in over 20 years [20]. In 2018 a slowdown started in some areas (e.g., the UK and several Nordic countries), where production growth stopped again. In Europe, total construction production grew by 3.1% in 2018. Nevertheless, the outlook for the forecast period up to 2021 shows a slow development, in the context of weakening economic expansion. The overall scenario is characterized by structural issues, such as demographic pressure, market saturation, and slow authorization and construction procedures, and the leading market in the next three years will be the infrastructure system. The construction sector is still globally based on linear production models. In 2012, as part of the Europe 2020 initiative, the European Commission published a Communication Strategy for the sustainable competitiveness of the construction sector and its enterprises [21]. The document aimed to promote market conditions leading to sustainable growth in the construction sector. The strategy addresses the following five areas: financing and digitalization, in particular for energy-efficient investments in building retrofitting; skills and qualifications for job creation through skills upgrading; resource efficiency, in terms of lowemission construction, recycling, and reuse of construction and demolition waste; a regulatory framework with the aim of reducing administrative burdens for businesses, in particular SMEs; and international competition, encouraging the adoption of the Eurocodes as well as promoting new financial tools and agreements with non-EU countries. Eurostat’s 2017 report states that construction-related activities produced 923 million tonnes of waste in 2016 [22], which in volume terms represents 30% of all waste generated in the European Union. Such data highlight the need to change the linear process characterizing the construction sector, by finding new ways to close the loop. According to Brennan et al. (Figure 1), the recycling and reuse of construction and demolition waste materials can significantly contribute to reducing construction costs and negative environmental impacts from the extraction, processing, and production of construction materials [23-25]. Therefore, there is a growing interest in urban mining from buildings, from both environmental and economic perspectives. Materials hidden in buildings are an interesting alternative to raw materials. In addition, construction activities are responsible for a large proportion of urban waste in many societies [26]. However, the opportunities opened up by the reuse of construction and demolition materials are an extreme solution to promote sustainability in the construction process. The main goal to be pursued in closing the loop is the conservation of the building as a whole, by the extension of its life cycle and its reuse.

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Figure 1. Linear and closed-loop model of CWD. Source: Brennan et al., 2014. Chart redesigned by the authors.

In the European context, Italy is the country with the largest preindustrial building stock; 30% of Italian buildings date back to before the Second World War. Data surveyed by the Centre for Economic and Social Market Research for Construction and Territory (CRESME) show that in Italy the investments for building renovation (including maintenance) increased from 56% to 67% between 2006 and 2013, while those for new buildings decreased from 44% to 33% [27]. Population decrease is one of the main causes of this trend. Such results are also the outcomes of tax incentive policies for building renovation and energy retrofitting, which involved 19.5 million interventions from 1998 to 2019 (over 62.5% of Italian homes, estimated by ISTAT at 31.2 million). Over twenty years the tax incentive measures generated investments of almost 322 billion euros. For preindustrial buildings, a conservation strategy is often necessary, not only to reduce the land and material consumption expected from the construction of new buildings, but also to respond to the need for cultural sustainability. Indeed, according to the widely shared academic view [28-30], as well as referring to the campaigns conducted by the United Nations Educational, Scientific and Cultural Organization (UNESCO) along with United Cities and Local Governments [31], culture is considered as the Fourth Pillar of Sustainable Development. The doctrine of conservation is based on contrasting change as a force capable of eroding the intrinsic value of cultural heritage. The UNESCO’s approach has led to the consideration of the built environment as a driving force for development. Development evolves around change as its intrinsic core component [32].

THE CONCEPTUAL FRAMEWORK: THE CIRCULAR ECONOMY AND THE BUILT ENVIRONMENT, A COMMITMENT TO SAVE THE PLANET Within the last 20 years, theoretical studies and visions have been dealing with built environment as a strategy for promoting environmental and social sustainability, progressing

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beyond purely technical matters to broader cultural, social, and economic considerations for sites and their setting. Economic and social transformations connote visions and approaches, contributing to facing issues related with conflicts between fragile resources and latent potentialities. International strategies progressively take into account systems effectiveness, following the increase of awareness about the limits of a development based on uncontrolled consumptions. Since the 1990s, a radical change in cultural perspectives marks the international debate, redesigning the relationships between built environment innovation and conservation, slowly introducing key issues that have significant repercussions on project experiences. A privileged entry point for this review is recognized in the Nara Document on Authenticity [33] which links built diversity protection to the development of settlements (Article 5). Two themes emerge from the document, conditioning the subsequent international debate: the need to favor the extension of the life cycle and to involve a large number of stakeholders. Ten years later, the Vienna Memorandum [34] introduces the issue of change management, focusing on the adaptability of the existing (art. 27). A central concern is to improve the quality of built spaces and their productive efficiency by bringing benefits not only by acting on technical standards (art. 17). In 2007, the Leipzig Charter on Sustainable European Cities returns to the questions raised by the lengthening of the architectural and urban life cycle, emphasizing how the European heritage includes not only historic buildings but also public spaces [35]. The Charter emphasizes the concept of baukultur as the sum of all the cultural, economic, technological, social and ecological aspects that influence the quality and the process of planning and building cities. Making greater use of integrated approaches to urban development policy, reconciling protection and innovation strategies is an objective that can be achieved through the involvement of economic stakeholders and the general public. The 2008 Quebec declaration on the spirit of place preservation contributes to the international debate with a reflection on the potential of the relationships between tangible elements (sites, buildings, landscapes, paths, objects) and intangible elements (memories, narratives, written documents, festivals, commemorations, rituals, traditional knowledge, values, textures, colors, smells, etc.) [36]. In 2010, the Toledo declaration takes into account the urban dimension of the crisis and the role played by cities in emerging challenges [37]. The redevelopment of abandoned or unused areas is a key strategy to contribute to the reduction of urban impacts (art. A.2). All these documents anticipate the principle that only the re-circularization of resources can positively impact on sustainability through a proactive commitment to future generations. The international commitment is based on a widening of approaches and perspectives, along with the possibility of intervening on ancient and modern buildings, historical centres, and suburbs. In 2011, the document Valletta Principles - Historic cities, towns and urban areas [38] recognizes that cities and historical urban areas, as living organisms, are subject to constant change (Article 1). If managed appropriately, these can be an opportunity to improve settlement quality based on the original features (Article 2). The ICOMOS Declaration of Paris of 2011 on heritage as a driver of development outlines the need for a return of attention to constructive culture [39]. The document also underlines the centrality of the economic feasibility of protection and innovation actions, taking into consideration the impact produced by the project on the heritage (Article 4). As part of the Recommendation on the Historical Urban Landscape [6], the heritage is taken, in the material and immaterial components, as a

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key resource to improve the liveability of urban areas; heritage is able to foster economic growth and social cohesion in an evolving global context (Article 3). Traditionally linked to the issues of conservation and enhancement, the architectural culture becomes progressively sensitive, to the problems posed by the closure of loops between resources and waste. The acknowledgment of the wealth of layers, proposed within the Unesco Recommendation becomes a driver for a renewal of approaches to the project, against obsolescence and abandonment. An alliance between stakeholders is pursued through several international documents, as fundamental for the built environment adaptability and flexibility to new uses. By introducing the UN Sustainable Development Goals and the New Urban Agenda, ICOMOS suggests that ancient settlements can be a reference model for development due to an inner attitude in balancing their aging and loss of functions [40]. In 2018, ICOMOS with the EU - Cherishing Heritage - Quality principles for intervention on cultural heritage provides a guidance for any stakeholder directly or indirectly engaged in EU-funded heritage conservation and management [7]. Social innovation and the change in collective practices directly impact on the design approaches by redefining the framework of the involved actors. Cultural heritage is a resource for society, an inheritance or legacy that is not only material, since it embeds ideals, principles, and values that constitute a shared source of remembrance, understanding, identity, cohesion, and creativity for Europe. Dialogue and interaction mark the commitment of owners, users, tenants, professionals with public administrations, the property sector, and finance, through the institutionalization of partnerships. Bottom–up processes for built environments require: a) understanding and respect for the built and its performances; b) precaution in design, promoting authenticity and integrity; c) reversibility of the intervention, minimum intervention and compatibility of the design solutions with the expected uses. Awareness and responsibility are the two poles around which design strategies for the built environment attentive to waste containment, revolve, through extended partnerships between expert knowledge, research centres and cultural institutions, social enterprises and the third sector. Quality in interventions on cultural heritage becomes a crucial and challenging issue for life cycle assuming that stakeholders (citizens, the public sector, the voluntary sector, the private sector, politicians, and heritage professionals) have points of view and expectations on quality. Linking the closure of loops to the imperatives of social cohesion and built environment protection, from this moment on, life cycle lengthening strategies are based on a community active involvement, promoting trade-offs between the users’ needs and design requirements. The Ellen MacArthur Foundation approach to growth crosses all these visions, suggesting that ever-growing economic profitable development can happen without an ever-growing pressure on the environment. Based on a system thinking, aware of relations between economic, human, natural and cultural dimensions, sustainability invests in maximizing values. Reshaping resources through symbiosis turns into a possible solution for past performance realignment or for the provision of new services. Its assumptions are endorsed by the World Economic Forum in 2018 [4]. Recurring to a theoretical simplification, the excursus highlights how, within the last 25 years, the design culture takes on commitments to life cycle lengthening through: 1) stakeholders’ involvements in values preservation, 2) processes and products innovation with the support of devoted technologies, 3) resources optimization and systems effectiveness promotion. The assumption of the system concept applied to buildings and the recognition of the specific technical and constructive characters for the functional–spatial system strictly

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informs design. The systemic approach gives the opportunity to address the issues of materials and techniques renewal for single units, adopting appropriate life cycle controls. Life cycle lengthening is related to the ability to reinvent new performances for systems, spaces and devices, with the redesign of technologies, able to fit within a built system, with high prior degrees of stiffness, imagining working procedures, operators, and scheduled times. Integrating technologies in addition to the existing ones is a way to manage the aging processes, transferring, planning and testing their suitability. Process and product innovation emerge as privileged mediums for passing on to the future past identities. An imbalance between the growing demand for innovation and compatible solutions marks quality improvements for the built environment.

MAINTENANCE, REHABILITATION AND ADAPTIVE REUSE: DESIGN ACTIONS AIMED AT SUPPORTING THE TRANSITION TOWARDS A CIRCULAR ECONOMY The recognition of quality levels offered by the built environment has a long history, dating at least to the mid-1960s. More than fifty years later, defining quality has progressed beyond purely technical matters at the level of single buildings to broader cultural, social and economic considerations for sites and their setting. Matching values preservation with resources optimization, extended life cycles allow past identities to be conveyed to the future, increasing or realigning the performance framework. Introducing CE paradigms into the project for the built environment therefore means focusing on issues of fairness and social justice. According to the change in cultural paradigms introduced by the Circular Economy, reuse, repair and recycling become pivotal levers of waste reduction in the construction sector. Their potential in the closure of loops is linked to the state of health of the built environment, and to the design aptitude when rebalancing the deviation that occurs within the life cycle with the quality expected. Therefore, intervention strategies are tailored to bring the building back to a level of efficiency which will allow it to perform its functions: adaptive reuse - for abandoned buildings that are no longer able to meet their use needs - identifies new uses compatible with the existing building and defines the adaptations required by their new activities; rehabilitation adds new performances or improves current performance levels, according to the evolution of the activities carried out in the building; and maintenance keeps the performance levels that the building is able to provide above the acceptability threshold through periodic interventions. Systemic analysis helps to identify the building’s residual values, assigning new roles not only to materials and components, but also to the relationships in between. The choice of the building renovation strategy derives from the resources to be reused, their conservation status, and the ability of the building system and its parts to perform their functions. Performance-based building design (PBB) is a key element in the evaluation of renovation effectiveness and efficiency. It is “the practice of thinking and working in terms of ends rather than means. It is concerned with what a building or building product is required to do, and not with prescribing how it is to be constructed” [41]. It assesses the building’s quality by comparing user requirements to performance levels. The PBB approach uses

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reliable evaluation tools to assess whether the proposed design solutions meet the specified criteria at a satisfactory level by “[...] quantification of the level of performance which a building material, assembly, system, component, design factor, or construction method must satisfy in order that the building meet the all goals established by society and the client” [42]. All decisions are based on the required performance, and the assessment and testing of the buildings. Figure 2 shows how maintenance, rehabilitation, and reuse can extend the life cycle of a building, maintaining and integrating its performance over time, according to scientific literature on this topic [43-44]. The graph shows time on the x-axis and quality on the y-axis. For a given building, we can assume an initial quality level Q0. Over time, the quality level of the considered building gradually decreases due to natural and anthropogenic causes of degradation and breakdown. A series of maintenance activities helps to extend the life cycle of the building, slowing down the decrease in quality so as to delay reaching the minimum level of acceptability (Qa). With redevelopment or adaptive reuse, the level of building quality can be significantly increased. The result achieved in terms of quality can be less, equal to or greater than the starting level Q0, depending on the intervention implemented; that is, how much the building’s performance levels are increased as well as which and how many new performances are introduced. Rehabilitation projects can increase the lifespan of the building, improving its quality without changing its use. In the case of adaptive reuse, an increase in the building’s life cycle is achieved by changing the use and adapting the building to meet the requirements of the new function. Such strategies are graded according to the building’s state of health. This approach turns the building to be rehabilitated from waste into a resource.

Figure 2. The Performance Based Building approach in the building renovation process.

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BEST PRACTICES SCREENING: TOWARDS CIRCULAR TRANSITIONS FOR BUILT ENVIRONMENTS When focusing on quality improvements in built environment rehabilitation, adaptive reuse and maintenance, according to the conceptual framework, priority is given to bottom-up processes, based on the following key points: a.

Sharing knowledge: participatory processes of reading, understanding and respect for the built environment and its performance; b. Design quality: precaution in design, basing choices on knowledge, promoting authenticity and integrity; c. Focusing on key-requirements: reversibility of the intervention, minimum intervention, compatibility of the design solutions, and flexibility in building use, durability and maintainability. According to ex-post evaluation methodology, examples of rehabilitation, adaptive reuse and maintenance of the built environment have been selected and analyzed by virtue of their attitude towards activating processes of transition to the Circular Economy. The object of observation is the manufacturing landscape; the result of the historic layering of economic, social and natural values and attributes. Deeply rooted in community needs and the skills of the workforce during the 20th century, these places have lost their symbiosis with the living and manufacturing cultures. Long relegated to the margins of the debate on heritage conservation, manufacturing landscape repurposing is today a topic at the forefront of the Eu Green Deal [45]. The practices are observed using a matrix that considers the quality indicators (a, b, c) given the life cycle lengthening strategies in terms of waste reduction for resources, capabilities, and embedded values (Table 1): 1. Stakeholder involvement: waste reduction in terms of capabilities and new alliances between stakeholders; 2. The potential of technologies: combining resource protection and affordability; 3. Embedded values: renewed productivity to preserve values and uses. Table 1. Matrix: quality indicators and life cycle lengthening strategies

a. Sharing knowledge b. Design quality c. Focusing on key requirements

1. Stakeholder involvement Textiles Pigüé Cooperative Rimaflow OfficineZero

2. The potential of technologies Bonotto Fabbrica lenta

3. Embedded values

Borgo Solomeo COM.I.STRA, company of the textile district of Prato

Milan for social Folly for a Flyover

Sugarhouse Studios

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Textiles Pigüé Cooperative The Empresas Recuperadas por sus Trabajadores - companies recovered by the workers – experience in Argentina a business transformation through a change in the legal form and in management control. In 2016, more than 300 companies subiscono questa trasformazione, saving over 15,000 jobs. Emblematic is the Textiles Pigüé Cooperative; where since 2004, the transformation into a social economy company is supported by the redesign of the management and maintenance processes for the buildings where production takes place. Rimaflow Worker buyout, acquisition of ownership, and control of the company by the workers is an emerging model in Italy. The Law n. 49 of 02.27.1985 (Marcora) states that workers can recover companies forced to close, keeping their jobs and avoiding the loss of acquired skills. Significant experience in protecting the production locations in Italy is that of the Rimaflow of Trezzano sul Naviglio, in the province of Milan. Here, in 2012, a group of workers, the majority of whom had been dismissed by Maflow, rehabilitated the previous factory; the citadel of another economy is realized converting spaces and processes from the automotive sector towards the recycling of electrical and electronic equipment. OfficineZero In June 2013, the Oz-Officine Zero project comes to life in the ex Rsi of Rome Portonaccio, as a laboratory for the reconversion of professionals formed around railway maintenance. Training and production are intertwined with solidarity and cooperation between workers also through the reuse of pre-existing production spaces, which are adapted to the needs of artisans, creatives and artists. They share not only places, but above all skills and design visions. Between 2019-20 after the acquisition of the site by BNL BNP Paribas, Officine Zero decides to move to a publicly owned area, in which to experiment publicprivate processes of adaptive reuse. Bonotto Fabbrica Lenta Bonotto Fabbrica lenta, in the province of Vicenza, is a textile manufacturer founded by Luigi Bonotto in 1912 to produce, at first, straw hats. Combining a modern vision of work and business with ancient technologies, in 2015, 60% of the shares are acquired by the Ermenegildo Zegna Group, an Italian leader in men's luxury. The reasons for this success are attributable to a transformation initiated in 2007, with the replacement of digital machines with discarded and disused mechanical looms from the ‘50s. The rehabilitation of the factory wich hosts also a museum is as slow as the production model pursued: each loom is the center of production; a single worker, as a sort of master craftsman, takes care of a special process. Borgo Solomeo Borgo Solomeo in the Umbria region, is the village where Brunello Cucinelli's cashmere knitwear production was born and developed. The settlement was built between the end of the 12th century; during the 16th century, the inhabited nucleus expanded beyond the walls, and in 1729 the town developed along the entire south-east route of the walls themselves. In 1985, Brunello Cucinelli started the rehabilitation, adaptive reuse and maintenance process of the village, making it the seat of his humanistic enterprise. The castle, the ancient Parish Church,

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the seventeenth-century Villa Antinori, and the Cucinelli Theater form the backdrop to a suggestive historical, artistic and landscape reality. With the establishment, in 2013, of the School of Arts and Crafts located in the rooms initially dedicated to the business activity then moved downstream at the foot of the castle, the village has definitively become a citadel dedicated to arts and culture.

COM.I.STRA Several companies from the Prato textile district of Tuscany are committed to combining technological innovation and the reuse of resources in the production of fabrics from discarded clothing. Among them, in January 2020, COM.I.STRA was recognized by the National Geographic as an emblematic site, for its spaces management and production processes. COM.I.STRA makes fibers obtained from the recycling of wool fabrics and from both new and used knitwear cuttings. It adheres to the Global Recycling Standard certification of Textile Exchange, providing the customer with a certified product, thanks also to a careful traceability system, in order to follow the entire process from the raw material to the finished product. Sugarhouse Studios Sugarhouse Studios is an event space in Bermondsey, in the south of London. It was realized in 2017, by the multi-disciplinary collective Assemble, working across architecture, design and art. The site was achieved through the rehabilitation of a former school which should have been demolished to make way for a large housing program. It develops around a core of common structures that enable and support collaboration and it has provision for over 20 studios to host designers, artists, and manufacturers. Milan for Social The exhibition Milan for social in October 2017 testified in an integrated framework, the entrepreneurial initiatives straddling adaptive reuse of abandoned places, the revival of ancient crafts, and solidarity with weak social groups. Organized at Palazzo Morando by the Bracco Foundation under the patronage of the National Chamber of Italian Fashion and the Municipality of Milan, it illustrated the lesser known history of Italian fashion and costume, witnessed by experiences such as: Alice Social Cooperative, Sartoria San Vittore, Milan (since 1992); Social tailoring, the Gelso, Turin (since 1999); Flowers in the buttonhole, multiethnic tailoring laboratory, Milan (since 2014). Folly for a Flyover Folly for a Flyover was a temporary project for London, carried out in 2011, by the multidisciplinary collective Assemble, with the idea of experimenting with the potential for a disused Hackney Wick highway underground to become a new public space for the area. For nine weeks, the venue hosted an extensive cinema program by the sea, a café, workshops in collaboration with the Create Festival, the Barbican Art Gallery and numerous local organizations and businesses. The project claimed the future of the site by reinventing its past. Like a giant construction kit, the madness was built by hand by a team of over 200 volunteers. At the end of the summer, when the initial purpose was exhausted, the materials used for its construction were reused as new play and planting structures for a local primary school.

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The redesign of the productive processes, the adoption of technologies able to fit within communities’ know – how and buildings' life cycle lengthening, are the common features of the selected experiences. The matrix highlights the following connotative dynamics within the Circular Economy transition for the built environment: •

•

•

Sharing and exchange of knowledge have repercussions not only on the skills of the communities, but also on physical spaces. Flexibility connotes places and processes that host participatory experineces of social utility, and of solidarity [44]. Technological innovation supports the return of productions within disused sites, extending their life cycle, promoting unexpected creative contamination through compatible and reversible design solutions. In the analyzed experiences, technology redesigns the production chains, combining digital and mechanical systems and processes. Linking culture and creativity, renewes forms of productivity, preserving values and uses. The productive system durability and maintainability emerges as a design priority in all the observed experiences at the building and technologica scales.

The discussed case studies highlight how the quality and effectiveness of building renovation processes are dependent on multiple variables, which each play a role in defining the decision-making process. This research has led to identifying factors and relationships which enable the circularisation of processes related to the built environment (Figure 3). In particular, the strategic role of the exchange and sharing of knowledge in defining strategies for the successful outcome of building renovation has been highlighted. Moreover, to close the loop in building renovation it is crucial to define the design choices in relation to the following key requirements: use compatibility and reversibility, flexibility, durability, and maintainability of the building system.

Figure 3. Quality and effectiveness in decision-making: factors and relationships in the building renovation process.

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CONCLUSION The principles of the Circular Economy, when applied to the construction sector, highlight the need to preserve and increase the value of existing assets as both materials and as constructions. Buildings are implicitly identified as a resource with tangible and intangible value, which can be used to satisfy needs. The main strategy to be implemented is the maintenance and renovation of existing buildings, in order to safeguard not only the value of the materials that constitute them, but their multiple values as complex systems. The multiplicity of values that can be ascribed to the built environment and the complexity of its relationships require a systemic interpretation of buildings in order to define a set of rules and constraints capable of addressing future interventions to achieve a balance between conservation and transformation. The values of the built environment fall into the following two categories: the intrinsic qualities, such as the value of raw materials, human labour spent on components and transport, transformation and installation; and the values arising from the relationship between the building and its physical, economic, and social context. The Circular Economy model outlined for the construction industry in this chapter shows a different point of view from the theoretical conclusions of Brennan et al., (Figure 1) [24]. A prominent role in the process of circularisation is assigned to maintenance activities and, more generally, to building renovation activities (Figure 4), with the goal of minimizing waste from the building process. Indeed, the built heritage has always been the object of a continuous circular process of use and reuse, which leads to a minimal production of waste, resulting in the end of the life cycle only in exceptional situations.

Figure 4. Closed loops in the construction industry; a model of circular process based on renovation.

Building renovation is the key strategy for economies with a large number of existing buildings, such as in Europe. In this scenario, we can only marginally consider buildings as a

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repository of materials to be re-used, such as in urban mining experiences. The extension of the life cycle of the built heritage is the main goal to close the circle, recognizing the manifold values of buildings, including their being a sign of the constructive culture of a place, of an era, and of a community. Therefore, the challenges are not only focused on the knowledge of the quality, reliability and durability of recycled materials or reusable elements. Further areas of interest in the transition to a Circular Economy should be identified relating to more effective strategies to extend the life cycle of buildings, involving users, private stakeholders, and local authorities in a virtuous circle. Local governments have the challenge of leading citizens towards this change, spreading the culture of building renovation, settling conflicts, and channelling resources towards shared goals. New models of collaboration for building renovation are currently under consideration in order to verify the possibility of their implementation in further contexts. Moreover, there is the need to adopt new business models based on service provision. Building owners are no longer expected to possess all the elements of their properties. Replaceable and reusable components may belong to the manufacturer for their full life cycle, according to a model that encourages re-manufacturing, reuse, and recycling. The theoretical debate on the topic of building renovation over the last thirty years has been showing us the way to overcome the dichotomy between renovation and projects, and between conservation and transformation. The renovation of the built environment today appears to be the most effective strategy to address the sustainability needs of urban areas; it entails the mutual enrichment of the building and its territory, resulting from their multiple connections. Knowledge helps to strengthen such connections, driving the transformation process towards the protection of shared values.

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Serena Viola, Stefania De Medici and Patrizia Riganti construction sector and its enterprises. ; 2012 Accessed 20.10.19. Eurostat, Report. ; 2017 Accessed 15.10.19. European Commission, European Construction Sector Observatory. Trend Paper - EU construction sector: in transition towards a circular economy. ; 2019 Accessed 10.12.19. Brennan, J., Ding, G., Wonschik, C. R. and Vessalas, K. (2014) A closed-loop system of construction and demolition waste recycling. 31st International Symposium on Automation and Robotics in Construction and Mining, ISARC 2014. https://doi.org/10.22260/isarc2014/0066. Marie, I. and Quiasrawi, H. (2012) Closed-loop recycling of recycled concrete aggregates. Journal of Cleaner Production 37: 243-248; https://doi.org/10.1016/ j.jclepro.2012.07.020. Koutamanis, A., van Reijn, B. and van Bueren, E. (2018) Urban mining and buildings: A review of possibilities and limitations. Resources, Conservation and Recycling, 138:32-39; https://doi.org/10.1016/j.resconrec.2018.06.024. CRESME, RI. U. SO 03. Ristrutturazione Edilizia, Riqualificazione Energetica, Rigenerazione Urbana. 2014. HammershØj, L. G. (2009) Creativity as a question of bildung. Journal of Philosophy of Education 43(4):545–558; https://doi.org/10.1111/j.1467-9752.2009.00703.x. Kembel, G. (2012) Preface. Make Space: How to set the stage for creative collaboration, John Wiley & Sons, New York. Martin, Р. (2010) What are Creative Spaces? Making Space for Сreativity, Brighton, University of Brighton. Institut de Cultura Barcelona, Culture: Fourth Pillar of Sustainable Development, ; 2010 Accessed 15.10.19. Pereira Roders, A. and Van Oers, R. (2011) Editorial: bridging cultural heritage and sustainable development. Journal of Cultural Heritage Management and Sustainable Development 1(1):5-4; https://doi.org/10.1108/20441261111129898. ICOMOS, The Nara Document on Authenticity, Paris, ; 1996 Accessed 20.10.19. UNESCO, Vienna Memorandum World Heritage and Contemporary Architecture, Paris, ; 2005 Accessed 15.10.19. EU Ministers Responsible for Urban Development, Leipzig Charter on Sustainable European Cities, ; 2007 Accessed 15.10.19. ICOMOS. Québec Declaration on the Preservation of the Spirit of Place, ; 2008 Accessed 20.10.19. EU Ministers Responsible for Urban Development, Toledo Informal Ministerial Meeting on Urban Development Declaration, ; 2010 Accessed 20.10.19.

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[38] ICOMOS, Valletta Principles for the Safeguarding and Management of Historic Cities, Towns and Urban Areas, ; 2011 Accessed 20.10.19. [39] ICOMOS, The Paris Declaration on Heritage as a Driver of Development, ; 2011 Accessed 15.10.19. [40] ICOMOS, Cultural Heritage, the UN Sustainable Development Goals, and the New Urban Agenda, ; 2016 Accessed 15.10.19. [41] Gibson EJ: Working with the Perfomance Approach in Building. CIB W60 Commission Report 64, Rotterdam, 1982. [42] Averill JD: Performance-based codes: economics, documentation and design. Worcester Polytechnic Institute, US, 1998. [43] Lee, R. (1976) Building maintenance management, London, Crosby Lockwood Staples. [44] Molinari, C. (2002) Procedimenti e metodi della manutenzione edilizia [Procedures and methods of building maintenance], Pozzuoli, Sistemi Editoriali. [45] European Commission, The European Green Deal. Communication from the Commission to the European Parliament, the European Council, the Council, the European Economic and Social Committee and the Committee of the Regions, ; 2019 Accessed 20.12.19. [46] Moretti, E. (2012) The New Geography of Job, Houghton Mifflin Harcourt, Boston and New York.

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 11

WASTE VALUATION FOR ENVIRONMENTAL AND HEALTH IMPROVEMENT ON CIRCULAR ECONOMY VIEW William Michelon1, Aline Viancelli1, Apolline P. Mass1, Daniel Vicente Filipak Vanin1, Rafael Dorighello Cadamuro2, Paula Rogovski2, Aline Frumi Camargo3, Charline Bonatto3, Fábio Spitza Stefanski3, Thamarys Scapini3, Gislaine Fongaro2 and Helen Treichel3,* Universidade do Contestado, Concórdia – Santa Catarina, Brazil Laboratory of Applied Virology, Department of Microbiology, Immunology and Parasitology, Federal University of Santa Catarina, Florianópolis, Santa Catarina, Brazil 3 Laboratory of Microbiology and Bioprocesses, Federal University of Fronteira Sul, Erechim, Rio Grande do Sul, Brazil 1

2

ABSTRACT Rethinking the production process is an essential strategy for the industry, energy, and agriculture, directly reflecting human life. Some researchers recommend thinking globally, with countries sharing data and coordinating industrial policies and trades, motivating organizations to work based on longevity, renewability, reuse, repair, and capacity sharing. In this context, the circular economy approach can be applied to allnatural resources in activities such as eco-building, water reuse, alternative energy generation (biofuels), enzyme production, waste prevention, and waste recycling. The circular economy can improve the economy itself, but it could also bring substantial benefits, for instance, cost savings, increased productivity, job creation, innovation, and raw material efficiency. These are possible when converting linear to circular processes. All these activities are strongly related to Sustainable Development Goals (SDG), including clean water and sanitation (SDG 6), clean energy (SDG 7), decent work and *

Corresponding Author’s Email: [email protected].

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William Michelon, Aline Viancelli, Apolline P. Mass et al. economic growth (SDG) as well as responsible consumption and production (SDG 12). This chapter will address the importance of the circular economy on diverse working fields to improve environmental and health quality, residue reduction and recycling, and by-products value aggregation.

Keywords: eco-building, bioenergy, biofuel, pathogens, emergent contaminants

INTRODUCTION The term circular economy (CE) was almost unknown a few years ago; nevertheless, the concept was applied in China for the first time as a sustainable practice in 2008 [1]. Traditional production of any product or service was based on linear processes, which proved unsustainable, causing severe environmental harm [1]. CE is based on an alternative flow model, where cyclical processes could be applied almost to all working fields [2]. From this perspective, some practices have recently been used diversely, including eco-building, water reuse, alternative energy generation (biofuels), enzyme production, waste prevention, and waste recycling (Figure 1). This perception offers a new scenario for the relationships between markets, customers, and natural resources. All CE alternative pathways are based on developing present activities without compromising future generations’ survival, introducing cost savings, increased productivity, job creation, innovation, and raw material efficiency. All these activities are strongly related to Sustainable Development Goals (SDG), such as clean water and sanitation (SDG 6), clean energy (SDG 7), decent work and economic growth (SDG 8), and responsible consumption and production (SDG 12).

Figure 1. The circular economy concept.

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WATER REUSE, ECO-BUILDING, AND RESPONSIBLE CONSUMPTION AND PRODUCTION In addition to being vital for humans, animals, and plants, water is essential for ecosystem service maintenance. However, in recent years, water distribution in space and time and water quality degradation have concerned researchers and authorities worldwide. For that reason, countries as Japan and China became pioneers in water reuse practices [3] that are near related to the CE concept to reduce water demand during production processes [4]. Moreover, the Environmental Protection Agency (EPA) has been designing water reuse guidelines since 1980, which are frequently updated, with the last meeting in 2019 [5]. Agricultural activities, such as crop and animal protein production, are the significant causes of freshwater pressure, being responsible for 70% to 90% of global water consumption [6]. Furthermore, the animal production chain generates substantial amounts of wastewater that can contaminate more massive quantities of potable water [7, 8]. The CE concept came to unify the solution for these problems (Figure 2). During the wastewater treatment process, the liquid fraction could be collected, treated to remove impurities (nutrients, pathogens), and reused. Some reuse examples are irrigation, cleaning services, industrial processes, groundwater recharge, dust control, construction activity demands, or activities that do not require portability [9, 10].

Figure 2. Waster reuse possibilities in the Circular Economy concept.

Where freshwater is scarce in urban areas, water has been obtained from wastewater treatment systems or rainwater [11]. The reuse practice could be applied to garden irrigation, car washing, street cleaning, firefighting, and industrial cooling processes, where potability is

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not mandatory [12]. Furthermore, in smaller urban areas, decentralized water systems could be implemented in households or buildings and be used, for example, for toilet flushing [13, 14]. On the other hand, water reuse can face barriers as public acceptance, high treatment costs to achieve potability standards, microbial security, and consequent regulatory legislation [5]. Therefore, water reuse for “noble“ activities could be infeasible when higher water quality standards are required [2]. Most of the CE mindset focuses on medium-lived consumer products, leaving behind long-lifetime products, such as those from the construction industry [15]. Nevertheless, awareness of the construction industry’s significant environmental impact was raised at the United Nations Conference on Sustainable Development, Rio+20, held in Rio de Janeiro, Brazil, in 2012 [16]. Since then, CE in the construction industry focused mainly on construction and demolition waste (CDW) management and its impact on environmental and economic aspects [17, 18, 19]. However, other processes can also be assigned as CE practices, namely sustainable building materials made with by-products and supplementary cementitious materials, to reduce cement consumption. Table 1. Circular Economy studies related to the construction industry around the world Circular economyrelated topic

CDW

Sustainable materials made with by-products for the construction industry

Supplementary cementitious materials

Discussion on

Country

Reference

The awareness for CDW minimization CDW minimization and management Structural steel reuse Gypsum end-of-life management CDW management review CDW management towards a cleaner production in China The barriers to CDW adoption 3R principle applied to CDW CDW management overview Oyster shell for artificial stone production Use of electric arc furnace dust for mortar production Cellulose recovered from sewage toilet paper for mortar reinforcement Automobile metal sheet scrap recovery for facade system Slate quarry sludge pozzolanic activity Paper fly ash and blast furnace slag for dry mortar production Biomass ash, metakaolin, and lime hydrates blend for lightweight mortar production

United Kingdom Malaysia United Kingdom Spain Italy/China Italy/China

[20] [18] [21] [22] [17] [17]

Iran China Saudi Arabia Brazil Spain

[19]

Italy/Turkey

[27]

United States

[28]

Spain France

[29] [30]

Czech Republic

[31]

[23] [24] [25] [26]

In recent years (Table 1), countries worldwide have become concerned with the construction industry’s environmental impacts, determining that a more sustainable approach is required to overcome the sector’s shortcomings.

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Most of the CE thinking in the construction industry has focused on minimizing and managing CDW [17, 18, 20, 23, 24] and developing policies to regulate the activity as an alternative to landfill disposal. Mahpour [19] identified the barriers that prevent CDW to be widely used as alternative materials. The author analyzed data from a behavioral, technical or legal perspective and found that using finitely recycled construction materials, ineffective CDW dismantling, sorting, transporting, and recovering processes are ranked first as barriers to implementing CE in the construction industry. As an unstandardized point of view, CE can be achieved by utilizing a by-product, either from the construction industry or other sectors, as secondary raw material. Artificial stones have been obtained through processing oyster shells, a common residue rich in calcium carbonate. The final composite presented exciting properties and can be applied in many situations [25]. Alternatively, electric arc furnace dust, steel dust generated when fusing scrap have been used to produce mortar. This kind of dust is considered hazardous waste due to its heavy metal constituents. The new material presented higher workability and mechanical properties when compared with the control [26]. Treated toilet papers from the sewage system were studied to extract its cellulose material and apply it to mortars. The composite material presented enhancements in lightness, microstructure, moisture buffering, and flexural strength [27]. Industrial symbiosis has been reported to be close to CE sustainable materials. As it is claimed, the direct reuse of steel scrap materials, without the need for smelting, provides both environmental and economic benefits. Hence, direct reuse over recycling can save up to 40% of the total cost and up to 67% of energy consumption [28]. As an alternative to cement consumption, many supplementary cementitious materials (SCM) have been known for a while. Nevertheless, some very recent research has demonstrated that some waste materials can also present pozzolanic activity; therefore, they were added to the list of SCMs. This material can be chemically activated in an alkaline medium to form calcium silicate hydrates, the same hydrates that provide the concrete its strength. Saéz del Bosque et al. [29] reported that slate quarry sludge has this behavior when thermally activated in the presence of Ca(OH)2. Through the statistical analysis, the study found three factors that control the reaction: time, activation temperature, and cement replacement ratio. Additionally, wastepaper sludge ash and ground granulated blast-furnace slag, a wellknown SCM, have been blended to form a binder matrix that could be used as mortar [30]. The authors reported a final compressive strength of 13.7 and 11.1 MPa when activated by calcium chloride and sodium silicate, respectively. Besides, biomass ash from a biomass heating plant, blended with metakaolin and lime hydrates were evaluated as an SCM to produce mortar [31]. The mix presented better performance, compared to lime mortar, in mechanical resistance, increased water vapor permeability, and lower thermal conductivity. Human impact on the environment is primarily related to the consumption of biophysical resources. Nonetheless, the impact reduction can be achieved not only by responsible production, use, and discard based on a complete cycle but also through lower consumption

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altogether. This change can be performed through environmentally accountable choices. Once it is verified, a million people agree to pay for extra-ecofriendly products [32].

ALTERNATIVE ENERGY GENERATION (BIOFUELS) AND ENZYME PRODUCTION Quality of life improvement and industrial production have demanded increasing amounts of energy, especially in the production and transportation sectors. In these areas, innovation development is directly related to energy availability, consequently influencing energy demand [33]. Energy sourcing can be divided into two broad areas, non-renewable and renewable. Among the non-renewable sources, the use of fossil fuels has been intensified since the Industrial Revolution. Consequently, the emission of enormous amounts of toxic gases and particulate matter negatively affecting health quality, environment, and global warming [33]. Considering all the above, renewable energy sources have been studied to develop clean, efficient, safe, and economically viable alternatives [33]. Among the renewable energy sources, waste has been highlighted due to the possibility of treatment, application, and repositioning of municipal solid waste, agricultural, food, sewage, and animal wastes, on the circular economy context [34]. The treatment and management of solid waste in several European countries occur mainly by incineration [35], aiming to generate electrical and thermal energy. For example, Italy recovered 2.7 million MWh of thermal energy and 1.7 MWh of electricity from burning 2.6 million tons of solid waste [36]. However, the incineration process releases extensive amounts of gases (dioxins) and chemicals (heavy metals) harmful to the environment and requires strict process control [37, 38, 39]. Therefore, one of the most promising ways of using waste biomass is biofuels production (biogas, ethanol, biodiesel), especially those considered second-generation, as they do not stimulate land-use competition with food crops [40]. Hence, anaerobic digestion is applied to waste with high organic loads, such as food, household, agricultural, animal, industrial, pharmaceuticals, and cosmetics chains for biogas generation [36, 39]. Biogas production plants are concentrated in the United States and Europe and are found in lower numbers in Asia, where it has been used for cooking and lighting [41]. Commercial ethanol is first-generation mainly, and its raw material is sugar cane used in Brazil, corn in the US, and sugar beet in the European Union [42]. With technological advancement and research incentives, new processes are being applied, aiming to substitute food for residues as a raw material of the fermentation process [43]. Also, waste from pulp and paper industry, fruit, municipal, and agricultural residues contain lignocellulose and produce bioethanol [42, 44, 45, 46, 47, 48, 49]. Bioethanol has a worldwide prominence among biofuels, responsible for two-thirds of the demand estimated for 2018 to 2023. In 2017, ethanol production increased by 3% to 104 billion liters, mainly driven by Brazil, China, India, and Thailand. Furthermore, the predictions for 2023 highlights that China will increase its share of global production, while the United States and Brazil will account for about 80% of the worldwide output [41].

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Additionally, for biodiesel production, the most challenging issue, on an industrial scale, is the high value of raw material (vegetable oil) and manufacturing process, despite the use of food sources. Thus, current biodiesel production technologies are being developed and improved to make this biofuel more competitive with fossil fuels [50, 51]. In general, the cost of biodiesel production can be minimized by incorporating waste into the process. A good example is cooking oil, which annually generates around 15 million tons of residues worldwide [51, 52, 53]. Other residues presenting a promising alternative for biodiesel production are fish, oil extracted from a coffee, plant, chicken fat, peanut oil, and extraction palm oil [54, 55, 56, 57, 58, 59]. The catalysis for biodiesel production is generally chemical or enzymatic, which addresses high cost and high risk because of chemical storage and transportation [59]. In this scenario, waste can be applied as starting materials in catalyst synthesis, reducing biofuel production costs [60]. With this purpose, materials such as eggshells [61], coconut fiber [60], animal bones [62], brewery waste [59], chicken manure [63], mussel hull [64], and glasses waste [65] have been successfully applied. Kaparaju et al. [66] showed that it is more sustainable to produce different fuels from a single residue in an integrated way instead of applying the residue to have only one fuel type. Therefore, the first step towards an integrated system consists of biodiesel production from oil extracted from waste. Then, the oil-free residue follows for saccharification and fermentation into ethanol. Next, the operations unit’s residues are then submitted to anaerobic digestion for biogas production and biofertilizer [67]. Another integrated production system can be performed from the algal biomass. Algae can be cultivated on wastewater with high organic loads, with the consumption of nutrients for algae growth. Subsequently, the algal biomass can be used for biodiesel, bioethanol, and biogas production [68]. These economic models allow an approach related to the CE, providing the prevention, mitigation, and recovery of waste [69].

Enzymatic Technology Enzymatic biocatalysis has been highlighted as an essential tool in biotechnological processes targeting energy production, enzymes, and other high value-added products [70]. Enzymes are advantageous since not require toxic metal ions to act on the substrate, making it environmentally friendly and cost-effective for industrial applications [71]. Some studies have reported that enzymes’ costs are about 44% of the price of raw materials. Thus, if enzyme production occurs through inexpensive raw materials, a significant reduction can be expected, up to 77%, according to research [72, 73]. Moreover, lignin-degrading enzymes are widely used for the pretreatment of lignocellulosic biomass, either for biofuel production or for other applications of biotechnological interest. Such applications include textile, food, paper industries, organic synthesis processes, wastewater treatment, and bioremediation [74]. Furthermore, cellulases, hemicellulases, xylanases, lignin peroxidase, and manganese peroxidase from a specific enzymatic cocktail present synergistic action depolymerization of plant polysaccharides, based on glucose and other essential monosaccharides in the manufacture of second-generation ethanol [75, 76]. Recently, a study evaluated the production of cellulolytic enzymes (cellulases and xylanases) through the CE approach using

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agricultural residues such as rice husk, soybean husk, sugarcane bagasse, and powdered sugarcane bagasse. The microorganisms capable of enzyme production can convert hundreds of kilograms of bagasse into bioavailable cellulosic material for biofuel production and other energy types [77]. Also, peroxidases and laccases act on biomass containing phenolic and non-phenolic compounds, playing a fundamental role in lignin degradation [78]; therefore, presenting a complete application in the textile industry wastewater treatment [79]. Besides, lipases break down long lipids into smaller fatty acid chains [80], applicable in the food, oil and fat, detergent, pulp and paper, cosmetics, leather, and biodiesel industries [81]. Also, amylases catalyze starch in smaller chains such as maltose and glucose. In the starch industry, α-amylases are widely diffused for conversion into fructose and glucose syrups [82]. Nevertheless, they can be used in the detergent, ethanol, food, textile, and paper industries [83]. Likewise, pectinases comprise a heterogeneous group of enzymes related to pectin substances’ hydrolysis present mainly in plants. They are applied in the processing of vegetable fibers, textiles, tea, coffee, oil extraction, and wastewater treatment containing pectin compounds [84]. Finally, keratinase is used for keratin polypeptide hydrolysis and can be widely produced from keratin substrates such as hair, feathers, wool, nails, horns, hooves while degrading the residue. One of the most promising applications is the production of feather meal with an economically and environmentally safe approach. Other potential industries include the fertilizer, leather, detergent, and pharmaceutical sectors [85]. Nonetheless, these and other enzymes can be obtained from a wide range of residual biomass. Commercial enzymes represent a substantial bottleneck for several industrial applications, mainly due to these biomolecules' high cost. Hence, this impasse could be circumvented with research development, enabling low-cost raw materials for enzyme production. Based on these aspects, many of the lost waste could be reintroduced and turned into a system for obtaining high value-added products within the CE.

SANITATION AND SECURITY ASPECTS In addition to recycling urban wastewater for irrigation, some improvements could be made to agriculture techniques, such as using trickle or drip irrigation, allowing a rational use of water while improving crop yields. Agriculture alone accounts for around 70% of global water usage [86, 87]. Furthermore, options such as dry toilets can be used in rural properties because of its water-savings and efficient reuse of organic matter; these systems can reduce pathogens and are easy to use and operate [88]. An alternative to decrease water loss is reusing it. Combining recycling water, decentralized and wastewater treatment are engines working together, aiming towards sustainable systems [89]. Recycled water can be applied to a range of activities (Table 2).

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Table 2. Recommendations for reuse of water according to USEPA [5] Category of reuse Urban Unrestricted Reuse Restricted

Agricultural Food Crops

Impoundme nts

Processed Food Crops and Nonfood Crops Unrestricted Restricted

Potable Reuse

Indirect Potable Reuse Direct Potable Reuse

Description The use of reclaimed water for nonpotable applications in municipal settings where public access is not restricted The use of reclaimed water for nonpotable applications in municipal settings where public access is controlled or restricted by physical or institutional barriers, including fencing, advisory signage, or temporal access restriction The use of reclaimed water to irrigate food crops that are intended for human consumption The use of reclaimed water to irrigate crops that are either processed before human consumption or not consumed by humans The use of reclaimed water in an impoundment in which no limitations are imposed on body-contact water recreation activities The use of reclaimed water in an impoundment where body contact is restricted Augmentation of a drinking water source (surface or groundwater) with reclaimed water followed by an environmental buffer that precedes standard drinking water treatment The introduction of reclaimed water (with or without retention in an engineered storage buffer) directly into a water treatment plant, either collocated or remote from the advanced wastewater treatment system

Environmental Reuse

The use of reclaimed water to create, enhance, sustain, or augment water bodies including wetlands, aquatic habitats, or streamflow

Industrial Reuse

The use of reclaimed water in industrial applications and facilities, power production, and extraction of fossil fuels

Groundwater Recharge – Nonpotable Reuse

The use of reclaimed water to recharge aquifers that are not used as a potable water source

For waste recycling, sanitary security is an essential barrier for agriculture, water reuse processes, and bio fertilization purposes. In this context, hygienic safety is the pathogen, antibiotics, heavy metals, and endocrine disruptor residues. Hence, enteric viruses are of particular concern for water contamination because they are associated with a wide range of gastrointestinal diseases and can replicate on enterocytes, resulting in water non-absorption and gastroenteritis [90]. These viruses are excreted in the stool in amounts around 109 particles per gram of stool, and only a small dose (101 particles) is sufficient to cause infection [91, 92]. These viruses present some characteristics that favor environmental stability (e.g., adsorption on solid), making them resistant to high temperatures, extreme pH, salinity, and natural UV radiation [93]. These characteristics worry when considering that Waste Water Treatment Plants (WWTP) are not designed to eliminate enteric viruses [94]. For this reason, human adenovirus is one of the models of bioindicators used to characterize the presence of enteric viruses in the environment because of their resistance and viability [95, 96]. Other enteric viruses are hepatitis E virus (HEV) and rotaviruses (RVs) that can be found in the slurry, presenting a great significance because of their zoonotic potential [97]. HEVseropositive individuals in developed countries with sporadic hepatitis E cases have been

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associated with pork products’ consumption. Moreover, swine can act as asymptomatic reservoirs, increasing the possibility of seroprevalence in humans who contact them. The contact and interaction with animals may also be a concern for the generation of new RV types because the zoonotic forms have the potential of genetic exchange with human RV [97]. According to the World Health Organization [98], food irrigated with reused water derived from domestic and industrial uses is consumed by more than 10% of the world’s population. This practice is recommended if the fecal microbial indicator amounts are below 104 CFU 100 mL-1 of Escherichia coli; for the Environmental Protection Agency, the maximum concentration must be less than 102 CFU 100 mL-1. E. coli is not a good indicator of nonfecal opportunistic pathogens such as Legionella pneumophila, Mycobacterium avium, Pseudomonas aeruginosa, and Naegleria fowler that cause diarrhea, cholera, or dysentery [99]. Typhoid and paratyphoid fever caused by Salmonella species are commonly associated with vegetables grown with wastewater [100]. The presence of Salmonella typhimurium, Salmonella dysenteriae, and Vibrio cholerae has been reported in chlorinated effluent discharges [101]. Cryptosporidium spp. and Giardia intestinalis is the most common protozoa associated with waterborne outbreaks, mainly due to its environmentally-resilient dispersion forms such as oocysts and cysts that transmit via fecal-oral spread route [102, 103]. These characteristics cause such pathogens to be resistant to treatment and disinfection in various matrices, including water and sewage. Their concentrations can be ten times higher compared to those of bacteria [104, 105]. The exacerbated/incorrect utilization of antibiotics in hospitals, food production, and pharmaceutical industries with consequent contamination of the environment promotes antibiotic-resistant bacteria [106, 107]. Antibiotic resistance occurs primarily through the horizontal transfer of genetic material such as integrons, plasmids, and transposons. This transmission can occur even when antibiotics are not present, primarily via environmental transport and dispersion [108]. The deposition of antibiotics from diverse sources has been widespread via wastewater treatment plants (WWTPs) [109,110]. Therefore, WWTPs exert selective pressure on local bacteria. In addition to favorable conditions such as low antibiotic concentration and prolonged contact time, these treatment plants can act as promoters of resistance gene transfer [111]. Strategies to reduce antibiotic-resistant bacteria in WWTP are membrane separation, ozone, and UV radiation [112]. Studies demonstrated the reduction of bacterial diversity after chlorination and ozone treatment [112, 113]. But other techniques are also efficient, including oxidation, anaerobic treatment, and coagulation [43, 114, 115, 116]. Heavy metals are a substantial source of environmental contamination because of their ubiquity in nature and their toxic effects [93, 117]. Studies showed that soils irrigated with wastewater containing heavy metals could persist in contaminated form for long periods, even when the irrigation is discontinued, leading to contamination of vegetables grown on these lands [117, 118, 119]. Toxic effects are specific to each metal; however, gastrointestinal disorders, diarrhea, tremors, stomatitis, paralysis, ataxia, pneumonia, and neurological disorders such as depression are common for zinc, arsenic, mercury, lead, aluminum, and copper poisoning [118]. These elements can cause severe health effects, including carcinogenesis and teratogenesis, with possible accumulation in humans through the food chain [120].

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Heavy metal removal from waste can be performed using traditional membrane filtration techniques, chelation, chemical precipitation, and ion exchange. Nevertheless, these technologies are expensive and present reduced efficiency for low metal concentrations ¹²¹. Some agricultural waste materials (rice, tea, coffee, coconut, peanut, and groundnut) could be used as alternative adsorbents for heavy metal removal ¹²². Other promising adsorbents for chemicals are nanobubbles, with the possibility of cost reduction and suitability for decentralized systems in developed and developing countries ¹²³. Metals such as iron can increase the interaction between a viral receptor and host cells, increasing infection probability and the emergence of new viral strains [124, 125]. Furthermore, endocrine disruptors (ED) are defined as exogenous substances that promote alterations in the endocrine system [126]. Some of these disruptors are used for various purposes such as herbicides (chloro-S-triazine) and other organochlorine pesticides, combustion residues, or substances used in industry polychlorinated dibenzo-p-dioxins, biphenyls, and dibenzofurans. Compound evaporation and easy adsorption increase these chemicals’ environmental stability and lead to persistent and bioaccumulation in the trophic chain [127; 128]. The removal of ED could be performed by physical removal (absorption by activated carbon or membranes), biodegradation (aerobic and anaerobic processes), or advanced chemical oxidation (NaClO, K2FeO4) [129].

CONCLUSION The CE approach improves environmental health quality and, consequently, public health through pollution decreases and material-efficient use before becoming waste. In this context, society’s role could be guided by responsible consumption and choices. The expectative is that CE transforms the production pathway once theoretical and practical levels are rooted in a sustainable objective and applicable to all working fields. Materials reuse and recycling encourage technological innovation, new inspirations and research challenges, aiming to develop cleaner technologies.

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In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 12

WASTE RECYCLING FROM CONSTRUCTION SECTOR WITHIN THE CIRCULAR ECONOMY PARADIGM Álvaro Sánchez-Quintana1, Juan Carlos Leyva-Díaz2, Jorge Sánchez-Molina3 and Valentín Molina-Moreno1, 1

Department of Management-1, University of Granada, Granada, Spain Department of Chemical and Environmental Engineering, University of Oviedo, Oviedo, Spain 3 Department of Chemistry, University of Francisco de Paula Santander, San José de Cúcuta, Colombia

2

ABSTRACT Human activity and our way of producing and consuming goods and services have a major impact on the socio-ecological system. The global population continues to grow at a dizzying pace, leading to a higher number of buildings and civil constructions, among others. However, natural resources are not infinite and CO2 emissions are very high. That is why there is a need to change the way in which we produce and consume. Moving from a linear to a circular economic model would mean reintroducing waste into the production chain, reducing fuel gas emissions and using natural resources more efficiently. Large construction companies have started to study the possibilities to implement the circular economy model. This sector presents a distinctive feature due to the fact that buildings are traditionally erected to stay up forever and not to be recycled. Besides, this sector became one of the largest producers of waste and greenhouse emissions. In Europe, one third of the waste is produced by this sector. For this, the application of the circular economy model in building and civil infrastructures has a special interest. Design for deconstruction, use of alternative materials in the construction material manufacturing and new ways of waste management are some examples of how circular economy can be introduced in the construction sector. This review analyzes the potential contribution of circular economy to this sector and it argues that building sustainability is possible with the aid of innovations and by rethinking current methods. A

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Corresponding Author’s Email: [email protected].

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Keywords: biomimicry, building information modeling, circular economy, CO2 emission, construction sector, renewable energy, reuse, sustainability, technological nutrient, waste management

INTRODUCTION Traditionally, the production, consumption and use of raw materials have followed a linear approach, which means that materials are obtained, used to produce and then disposed of. Although the negative externalities are significant, this has been possible due to the large amount of natural resources. However, a new approach to the use of raw materials is necessary as a consequence of population growth and the higher cost of resources, on account of a decrease in the amount of resources and an increase in the demand. Circular economy appears as a new way of production, trying to reincorporate waste into the chain, in such a way as to become an input. When it comes to environmental impact, the construction sector has a decisive role due to the large amount of raw material used and the waste generated. It is calculated that the steel demand will have increased by 80% by 2030, being the construction sector the responsible to generate 50% of this [1]. The objective of this review is to investigate how the construction sector can become more circular and how the EU supports this transformation. For this, the review has the following structure. Firstly, our linear production model and its disadvantages are presented so that the reader has a general idea of the problem. Then, the beginning of the circular economy model and the several thinking schools that have facilitated the appearance of this current economic model are explained. Next, the concept and principles of the circular economy model are introduced. Afterwards, it is highlighted how the circular economy affects construction and why it is necessary to change. In addition, several applications of circular economy are presented so that the reader can see the advantages of them. An analysis of clay brick production following the linear model is also introduced. Eventually, the answers to the research questions are discussed. The research questions are: 1) Is it necessary a change in the construction sector? 2) How does the European Union support the circular economy? 3) How can circular economy be implemented in the construction sector?

END OF LINEAR ECONOMY The industrial economy has been based on a linear model which follows an obtainproduce-dispose pattern. Companies use unprocessed materials to create a product and sell it to the customers, who throw it away when it is no longer in use [2]. Buildings have been

Waste Recycling from Construction Sector within the Circular Economy Paradigm 207 designed to be erected, used as a place to live for a certain period and then demolished, recycling only a limited number of materials and generating a large amount of waste [3]. During the water treatment process, waste is generated and disposed of in landfills [4]. The use of raw material has increased in the past years and it is estimated that there will be approximately 82 billion tons by 2020 [2]. The construction sector plays an important role in this issue, becoming one of the largest purchasers of natural resources [5]. With the “aid” of this linear economy, resource demand and scarcity, price squeeze and volatility will get worse before getting better [6]. This is due to the following factors: • •

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Demographic trends. Middle class population is expected to increase by three billion, which means more consumers. This implies a higher resource demand [1]. Infrastructure needs. Not only has the population growth led to the construction of new infrastructures, but also to an improvement in the access to resource reserves. According to McKinsey [1], meeting the challenge of providing the demanded amount of steel, water, cultivation products and energy will be possible with an investment of approximately €3 trillion per year1, which is 50% higher than current investment levels [6]. Political risks and limited opportunities to use remaining resources. Political events can also have an impact on commodity supply and, as a result, they may trigger or worsen resource scarcity and push up prices and volatility levels. About 80% of all available cultivable areas on the planet are in countries with political and infrastructural problems. About 37% of confirmed oil reserves and 19% of confirmed gas reserves are also located in politically risky countries [6]. Globalized markets, due to the impact of one country on others. Hence, regional price shocks can quickly become global. Price volatility also depends on this issue. Some representative examples are Hurricane Iker in the Gulf of Mexico and its impact on the energy market; and the eruption of Eyjafjallajükull in Iceland, which resulted in air travel chaos [5, 6]. Climate. According to the Environmental Protection Agency, changes in climate could have an impact on stream flow, snow cover and glacial patterns, which would lead to changes in fresh water provision, regular erosion, irrigation necessities, and flood management needs. This chain of events would have a very serious effect on the supply of farming products [6].

ORIGIN OF CIRCULAR ECONOMY The idea of circular economy first emerged in the last century. In his report “Economics of the Coming Spaceship Earth” in 1966, Kenneth E. Boulding sketched the meaning of circular economy. He observed the Earth’s limits in both resources and waste management [7]. “The Potential for Substituting Manpower for Energy” is a report published by Walter Stahel and Genevieve Reday in 1976. The report supports circular economy due to the impact it has on job creation, cost reduction and resource savings [8]. In 2006, circular economy promotion was part of a national policy in China [9].

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Permaculture. This concept was introduced by Bill Mollison and David Holmgren in the late seventies. It is a system of principles of agricultural, social, political and economic design based on the patterns and characteristics of the natural ecosystem. Permaculture has aspects from both conventional green agriculture and current innovations and principles [6]. Fair use of natural resources is also considered by this economic standpoint [10]. “Cradle to Cradle” was first introduced by W. Stahel and later refined by B. McDonough and M. Braungart. This new perspective contemplates that the material manipulated in industrial processes is considered a biological and technological nutrient. Industrial material flow can be based on natural flow. This involves a continuous recovery and reutilization of these nutrients [6]. Waste disposal and using sun as renewable energy are both aims of this philosophy [10]. “Biomimicry.” This concept, which has been mainly used in the construction sector, was introduced by J. Benyus in 1997. Biomimicry has nature as a reference: nature as a measure, using an ecological standard based on natural processes to assess our economic and social management [10]; nature as a model, which helps to solve human problems; nature as a mentor, which involves viewing nature as a source of both resources and information [6]. “Industrial Ecology” is a concept introduced by R. Clift. It is an approach which aims at creating processes in which waste is used as an input for the next step, eliminating the notion of an undesirable by-product6. Shifting from a linear production system, in which there is a large amount of waste, to a closed loop system in order to be more efficient and environmentally friendly is a key point [11]. Blue Economy consists in the use of waste as a resource. The Belgian businessman Gunter Pauli and the former CEO of Ecover are the responsible for this movement. This idea follows the premise of learning from nature to reach more efficiency, respecting the environment and creating wealth [12]. Blue economy is a concept introduced by the businessman Gunter Pauli, who published the book “the Blue Economy” in 2010. He argues that “using the resources available in cascading systems, the waste of one product becomes the input to create a new cash flow” [12]. He affirms that products manufacturing needs to be based on how nature works in order to reduce the use of natural resources and waste [6].

THE REVOLUTION OF CIRCULAR ECONOMY Background The pattern of take-make-dispose has been followed since the beginning of the industrial revolution. This linear model of resource consumption leads companies to obtaining natural resources, manufacturing products and using energy in order to sell the product to a final costumer, who throws it away when it does not serve its function any more [6].

Waste Recycling from Construction Sector within the Circular Economy Paradigm 209 During the last century, resource prices have been decreasing and this has supported economic growth in advanced economies [6]. For this, waste management and use of resources have been rarely controlled, while the utilization of natural resources (i.e., water, energy, raw materials, among others] and their prices have increased drastically in recent years [13]. This increasing resource demand represents limits regarding both economy and nature. Moreover, the waste from the production chain is notable. The Sustainable Europe Research Institute (SERI) has calculated that, every year, approximately 21 billion tons of materials that are part of the manufacturing process in Organization for Economic Cooperation and Development (OECD) countries will not be incorporated into the products themselves [6]. Concerning end-of-life waste, Europe has generated 2.7 billion tons of it in 2010, but only about 40% was treated. Construction companies are increasingly aware that a shift is required. Construction material manufacturing requires raw materials which are obtained by mining. Mining and construction material manufacturing related to the production of steel and cement are responsible for approximately 15-20% of human-generated CO2 [14] .Besides, the energy required for the manufacturing of this material usually has a fossil origin and these sources are scarcer [15]. The traditional line has been based on manufacturing a product to be sold and used. The principal idea in circular economy is offering a service during the product lifetime in such a way that the product, i.e., construction material, can be used for other purposes, i.e., other buildings, after its original one [16].

Definition Different definitions of circular economy have been presented. Some of them are presented below: •

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Ellen MacArthur Foundation: “Circular economy refers to an industrial economy that is restorative by intention and design. It aims at enabling effective flows of material, energy, labor and information so that natural and social capital can be rebuilt. It seeks to reduce energy use per unit of output and accelerate the shift to renewable energies by design, treating everything in the economy as a value resource" [6]. European Commission: “A circular economy represents a development strategy that enables economic growth while optimizing the consumption of natural resources, deeply transforming production chains and consumption patterns and re-design industrial systems" [17, 18]. Waste and Resource Action Plan: “A circular economy is an alternative to a traditional linear economy (make, use, dispose) in which we keep resources in use for as long as possible, extract the maximum value from them whilst in use, then recover and regenerate products and materials at the end of each service life” [19].

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A Shift to a New Business Model The economic growth of countries based on linear economy has been hindered. There is no more balance between economic growth based on linear economy and resource demand. In this backdrop, the concept of circular economy plays a key role. In 2010, Ellen MacArthur Foundation introduced this concept as an alternative for linear economy. Ellen MacArthur Foundation is an international think tank that is recognized as an authoritative source of circular economy information. It has the support of the European Commission and it oversees the publication of reports, articles, case studies, among others, related to this topic [16]. Circular economy aims at reducing costs and dependence on natural resources as well as reducing waste. As linear economy does not pay attention to the waste or, if it does, it is not enough to reduce CO2 contamination, circular economy means a big shift in terms of gaining environmental benefits. Circular economy brings profits to companies. It allows maintaining the value of the materials in a world where raw resources scarcity is growing [17, 18]. Industries have already observed the possible gains for improving resource productivity. It has been foreseen that material input needs will be reduced by 17-24% by 2030 [20]. Approximately €630 billion per year could be saved if the use of resources is optimized [21]. Basically, the aim of this new production system is minimizing the use of resources in such a way that fewer resources escape from the circle. All phases are connected so that outputs in a phase become inputs in the next one. In this context, investments should be high but EU policies already support industries by incentives or guides.

Circular Economy Principles Circular economy rests on the following principles: “design out waste, build resilience through diversity, rely on energy from renewable sources, think in systems and waste is food” [6].

Design out Waste Products and services can be designed in such a way as to reduce waste [6]. The idea is to try to give the output a second life after its use by finding its added value [10]. Waste & Resources Action Programme [19] identified five design principles to reduce waste in the construction sector: •

•

Design for Reuse and Recovery: It has been observed that the reuse of components of a building or the entire building reduces environmental issues such as waste or combustion gases. Reused material refers to both those that are on site and from other sites. An inspection of the site takes place to consider if a reuse is possible. If the construction site meets the requirements, its materials and components will be used for other buildings. If this does not happen, demolition will be done carefully to ensure maximum recovery of materials through recycling [19]. Design for Off-site Construction: Waste reduction through off-site construction has been documented when manufactured components of the construction are used extensively. Off-site construction brings changes into the construction site due to the

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fact that conventional activities vary and the amount of trade decreases. This results in a great number of environmental, corporate and social benefits. Modern technology allows manufacturing construction elements in a quick and efficient way, reducing costs and waste [19]. Design for Materials Optimization: This aims at decreasing the utilization of material and waste in every construction phase, maintaining the design. To achieve this, a minimization of excavation and a simplification of materials, among others, need to be considered [19]. Design for Waste-efficient Procurement: Designers need to work with the contractor to provide him with information related to the generation of construction waste. Waste reduction can be reached by design (i.e., designing construction elements that can be efficiently erected), specification (i.e., more information related to waste management) and contracts (i.e., clauses about this issue) [19]. Design for Deconstruction and Flexibility: After the building life cycle, it can be deconstructed. Hence, designers need to have knowledge related to material recovery.

Building Resilience through Diversity Products need to be modular, versatile and adaptive to reach the different purposes in their life cycle [6]. This principle aims at reducing the product obsolescence [10]. A Shift to Renewable Energy Resources Reducing the use of non-renewable energy is an objective. With this and the use of renewable energies, the environmental impact is minor [10]. Moreover, the use of fossil-fuel based energy will decrease [6]. Think in Systems According to Senge [22], “Systems thinking is a discipline for seeing wholes. It is a framework for seeing interrelationships rather than things, for seeing patterns of change rather than static snapshot.” Within the circular economy model, this can be seen as a self-regulating system similar to nature [23]. Ellen MacArthur Foundation argues that think in systems is “the ability to understand how parts influence one another within a whole, and the relationship of the whole of the parts" [6]. A clear example is our body and how all the organs help each other. Waste is Food This supposes a change in the way we see waste. Waste is not rejected anymore, but used for other industries. This can be the summary of circular economy. Everything in the supply chain has an added value [10].

Loops in the Economy Ellen MacArthur Foundation defines this new economic model as the integration of two sorts of materials. First, biological materials from biological origin, such as bio-based waste

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that can be returned to the biosphere, where their role is to be turned into nutrients [6]. The case of biomass pellets is a clear example of this: pellets are used as biomass to get energy [24]. Secondly, technical materials (also known as technological nutrients) are not biodegradable and based on finite resources. These nutrients are reused or recycled and remain in the loop so that the negative externalities due to their disposal decrease.

CIRCULAR ECONOMY AND CONSTRUCTION SECTOR Introduction Circular construction is based on circular economy in the sense that the principles of circular economy are transferred to the construction sector during the building life cycle: from the obtention of building materials, lay-out, designing, production, erection and utilization to the demolition and recycling of materials, water and energy for production. In this way, there is a reduction in the negative environmental impact, use of the construction site, modular construction and manufacturing of prefabricated construction elements. Construction sector consumes a large amount of raw material and energy. Numerous materials used in construction can be recycled or reused, such as concrete, bricks, wood, steel, plastic [25]. Construction industry has increased dramatically in the past decades. This has an impact on the amount of waste that is generated: it is estimated that one person generates 2 kg waste per day [26]. According to the European Commission, construction sector is a priority for the circular economy due to the amount of resources that are used and the fact that the potential reuse and recycling are very high. Half of the extracted resources and energy and roughly a third of the consumed water are used in the construction sector. For this, the transition in this sector has also been stimulated in order to be achieved by the year 2020 [17, 18]. European countries only recycle or reuse approximately 25% waste from the construction and demolition. One reason behind that is that buildings are designed to be constructed but not deconstructed. This implies that transforming those components into recyclable parts is a challenge. For this, there is a constant loss in this sector [6]. Waste quantities vary between 310 and 700 million tons per year in the European Union [17, 18]. Therefore, construction is seen as one of the main waste sources in Europe [27]. For this, it is essential to control this issue through some guidelines or protocols [28]. Construction projects of infrastructures generate a large amount of CO2 emissions from the beginning of the execution until their demolition [29]. As the reduction of the greenhouse gas emissions to 20% is a target of the European Commission, construction sector plays an important role on this matter [30].

European Union Plays a Key Role In Europe, one third of the total amount of waste comes from the Construction and Demolition (C&D) waste. For this, a protocol has been established to reduce the C&D waste. It gives information about waste management and the advantages of recycling [31].

Waste Recycling from Construction Sector within the Circular Economy Paradigm 213 This Protocol agrees with the “Construction 2020” strategy, as well as the “Communication on Resource Efficiency Opportunities in the Building Sector.” It belongs to the more recent and important Circular Economy Package that the European Commission has published. It aims at achieving the target of 70% C&D waste being recycled by 2020, proposed by the Waste Framework Directive, closing the loop of product life cycles and bringing benefits [31]. In other words, the overall objective of this protocol is improving both the C&D waste management and the quality of C&D recycled materials, through the following [31]: •

Better waste analysis and identification: An appropriate planning and management of any demolition or construction project is a key point due to the fact that this addresses important cost savings as well as environmental and health benefits.

Pre-demolition audits must be carried out to identify C&D waste, implementing proper deconstruction techniques and specifying demolition methods. A pre-demolition audit is composed by two parts: 1) Identification of waste materials: quality, quality and location in the construction site. 2) Extra information related to recycling and reuse possibilities. This needs to be carried out by a qualified expert with a deep knowledge in building materials. Once the pre-demolition audit occurs, an efficient waste management plan takes place. This basically consists in gathering information regarding the different demolition steps: who will conduct it, which materials will be obtained and how they will be transported and how hazardous and non-hazardous waste will be managed. •

•

Better logistics: Finding closer treatment plants is important for C&D waste management. Furthermore, the use of information technology allows optimizing the use of road networks. This enables reducing the use of fuel. Trying to reduce distances is essential so that the environmental benefits of recycling are attractive. An important aspect is to guarantee the integrity of the materials to be recycled. A possible mixture with other materials would make recycling difficult. For this, containers need to be clean. A better waste treatment: An appropriate waste hierarchy allows having benefits with regard to resource efficiency, sustainability and cost savings. As there are different waste treatment options, it is important to analyze which one should be applied according to economic, environmental and technical requirements. Some options are the reuse, recycling and recovery of the material and energy.

Depending on their economic value, materials and products must be classified to be reused for other purposes. Special attention needs to be paid to hazardous waste, which needs to be disposed of according to the corresponding national regulations. It must also be considered that this hazardous waste can pollute non-hazardous waste during the demolition stage.

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For a good waste treatment, it is necessary to have a good knowledge. That is why it is important to train adequately the workers that will handle the waste in the construction site [32]. •

Quality Management: C&D waste is used to create recycled construction materials, such as cement and concrete. Their quality depends on their environmental features and technical performance. In this context, quality management is an important tool to ensure the required quality of the products.

The idea is to manipulate waste in order to obtain technological nutrients that may be reused for other purposes [6]. Technological nutrients refer to the waste that can be reintroduced into the loop to become an input for new manufacturing processes [4]. Reducing to zero the negative externalities is a target [17, 18]. During the sewage sludge treatment, it is not possible to reuse the whole amount of water and the remaining sewage sludge is disposed of. However, in the context of circular economy, there are other options such as using the sewage sludge for manufacturing ceramic materials, as an additive in the cement-making process and for construction materials [4].

The Paradigm of Circular Economy Related to Construction According to Arup, the next six actions can explain the paradigm of circular economy related to construction [30]: •

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Regenerate. This implies solutions that enhance the sustainable use of materials and resources, avoid waste and negative externalities, and restore natural systems. These solutions are regenerative by design. The option of deconstruction can also be considered in order to use a piece of the work site for future buildings. Share. Once the building is erected, the use it has is a key point, having an impact on resources such as water or energy. Airbnb is a clear example of sharing. In 2014, a study in US found that Airbnb users use 63% less energy than hotel users. In Europe, the amount of water that has been saved is equivalent to the content of 1110 Olympic-sized swimming pools. Platforms such as WikiHouse enhance designers to share designs with others. This exchange of information aims at the adoption of a better practice. Some principles of this method of sharing are modular construction, design for disassembly and the use of sustainable and circular materials. Optimize. It refers to optimizing system performance, maintaining materials and components at their highest value, maximizing the construction process efficiency, eliminating waste, and promoting reuse and repurposing. Manufacturing off-site construction elements will reduce the waste produced on-site. After the building life cycle, these elements can be reused in other infrastructures, industrial sectors or buildings. Loop. One of the goals of circular economy is the creation of new uses for materials through remanufacturing and recycling. An appropriate design enables companies to

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reuse construction components and materials. Moreover, this looping of primary and recycled materials enables their uses from other industries. The use of repurposed materials within the sector minimizes the need for primary materials. Moreover, the modulation and disassembly of off-site elements reduce construction waste. Caterpillar has remanufactured some parts since the 1970s and they have become leaders in this topic, enabling the reproduction of elements by a small portion of its previous cost. Standardization of components is also a key point, as it enables the recyclability to increase. Virtualize. Building information modelling (BIM) is an innovative digital tool that comprises updated information of a building or civil construction related to all its phases. It allows saving time and decreasing construction resources loss. All stakeholders such as designer, contractors and building operators have access to this system. It supports the efficient performance and maintenance of buildings, as it communicates any negative externalities as well as opportunities for recycling and remanufacture. Exchange. The leasing of construction machinery reduces costs. Reducing the nonrenewable energy systems of production is an objective. It involves a change to new technologies, upgrade or replacement of older ways of doing things. Using alternative materials for manufacturing construction components is also an option [3] which has been observed by different researchers [4].

This approach to circular economy within the construction sector leads to economic benefits [25]. With the implementation of new technology that is totally connected with circular economy, approximately €1010 billion will be saved 5. Moreover, it has been predicted that the GDP will grow by 7% by 2030 due to EU green policy [17, 18].

Application of Circular Economy in the Construction Sector In this section, some activities carried out in the paradigm of circular economy will be mentioned.

Sewage Sludge Within the paradigm of the circular economy, water and its treatment play a very important role. Water is processed in a Drink Water Treatment Plant (DWTP) and waste is generated in the form of sewage sludge. In the last century, other researchers and scientists have observed that sewage sludge ash is appropriate for brick [33] and mortar manufacturing [34], keeping their mechanical properties [35]. However, in the last years, sewage sludge has been disposed of to landfills or dumped into oceans [36]. To respond to the European Zero Waste Directive, new methods have been incorporated to use this sewage sludge in other industries, such as cement manufacturing. In this way, the sludge becomes a technological nutrient as it becomes an input for another process. The sludge changes from being considered waste to be considered a new resource, which is also known as a technological nutrient [4]. Sewage sludge can also be incinerated and used in

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concrete bricks manufacturing. Between 10% and 20% of the cement can be replaced by sewage sludge ash and the properties of the blocks remain unaffected [37]. Moreover, a resource management company has discovered that sewage sludge can be used in plastic and chemical industries due to the fact that it can be converted into valuable bio-polymers through wastewater treatment processes [3]. Hence, this transformation of sewage sludge into a resource belongs to circular economy and contributes to the process of “closing the loop” [17, 18]. As the construction sector is in continuous growth, the use of this waste as a substitute in construction material is a good alternative in order to reduce the use of other natural resources. Moreover, it brings economic benefits, mitigating the exploitation of sources [36], and helps to protect the environment, reducing the space needed for the disposal of this waste [4].

Deconstruction Traditionally, buildings have been designed and erected following a linear model whose last stage is the demolition. Buildings have not been designed to be eventually dismantled and construction materials are major composites that difficult their recycling. This addresses a large use of natural resources. For this, deconstruction is emerging as an alternative to demolition [38]. Construction and demolition waste has increased until about 450 million tons in EU in recent years [39]. Construction and renovation works use 40% of the world’s material flow. For this, design for deconstruction implies resource savings and plays a significant role within the paradigm of circular economy. A study carried out by NAHB Research Center showed that deconstruction would have reduced approximately 75% of construction and demolition waste in the middle of last century, in contrast to demolishing houses [6]. The report “Communication on Resource efficiency opportunities in the building sector” aims at reducing the use of raw material considering the whole life cycle of buildings and, consequently, materials from deconstruction are reused [40]. Design for deconstruction refers to those practices in which construction components could be used at the end of the building’s operating life for other purposes, in such a way that the waste becomes an input [17, 18]. Unlike demolition, deconstruction allows reusing the building elements for future construction works. For this, it is important that buildings have specific characteristics [40]: • • • •

•

Transparency to identify systems easily. Regularity in terms of following a certain pattern to use similar building systems and materials. Simplicity. Limited number of components. It has been observed that structures consisting of a smaller number of larger members are easier to dismantle than those composed by a larger number of smaller components. Easily separable materials. In order to achieve this, it is necessary to avoid composite materials.

Waste Recycling from Construction Sector within the Circular Economy Paradigm 217 The principles of design for deconstruction can be presented in two groups, according to the sort of construction [41]: 1. Architectural: • Use a simple and regular layout to ease the identification of the different components of the construction. • Layer buildings as much as possible to separate the components within the construction so that it can be easily reused or extracted after the building life cycle. 2. Structural: • Use standard components, shapes and connections that can be easily classified and removed. • More removable fasteners, less adhesives. • Avoid multiple types of structural systems. Several studies have shown that building deconstruction has a lower impact on the environment than building demolition [42]. Deconstruction has economic advantages in the short term. However, its success is more notable in the long-term due to the fact that profits are higher and environmental benefits can be observed [43]. The Center for Construction and Environment demonstrated that deconstruction is more cost-effective than traditional demolition by deconstructing six houses during 1999-2000. The reason for this lies in the reduction of landfill disposal cost and the economic value of the recovered material [44].

Materials Passports It refers to a document which provides information about materials and buildings through the whole life of the product in order to learn more about its possibilities of being reused or recycled. It allows the recognition and separation of components and materials [45]. All members in the supply chain has access to it from any location. There are different levels of information: • •

• •

Design phase. Manufacturers and manufacturers’ suppliers exchange information related to the origin and situation of the materials. Manufacturing phase/Remanufacturing phase. Product manufacturers obtain and provide information about the potential reuse, positive impacts, instructions for use and location of the material. Operative phase. Consumers, installers and owners receive information related to the assembly, cleaning and maintenance of the product. Disassembly phase. Deconstructors and disassemblers exchange information about composition, instructions for disassembly, connections and locations.

These materials passports play an important role within the EU Horizon 2020 roadmap. One of their goals is to define the value for recovery, not only concerning materials, but also the whole building [46]. As construction sector generates a large amount of waste, this new tool enables a reduction of waste due to the fact that appropriate information is provided [47].

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Buildings should be seen as a database of information for materials. For this, the material passport can be the link between the building, the design process and the suppliers [48].

3D Printing A large number of new innovations are to appear in the construction sector in the next years in order to reduce the waste. One of them is 3D printing, which is an advanced technology defined as follows: “a process of joining materials to make objects from 3D model data, usually layer upon layer, as opposed to subtractive manufacturing methodologies" [49]. In 2000, contour crafting was the first attempt to apply this new technique. It is a combination of extrusion and trowel-automated construction [59]. After that, there have been numerous innovators developing different processes, such as printing of construction components to be part of the building, giving shape to hollow honeycomb elements to be assembled in the Amsterdam Canal House and the erection of the entire building structure in a non-stop work session [51]. The main goal of this technology is the sustainability of the construction sector with regards to benefits for companies, people and environment [52]. Additive manufacturing of concrete is a clear example of the good performance of this tool. Concrete is an easily-produced material but CO2 emissions are high. For this, 3D printing enables the creation of concrete components reducing this issue [53]. Moreover, it reduces the structural waste and saves time [3]. Some benefits of 3D printing are the following: • • • • • •

Use of biomaterials [54]. Printed products only use the right amount of material during the manufacturing process, which means a reduction of resources and waste [54]. Faster construction [5]. Use of local and renewable resources [5]. Air pollution emission decreases, both during building or infrastructure erection and its operative phase [51]. Reuse of materials and components is easier than with the standard construction method [51].

Although it is an environmentally friendly technique, it still requires further development. As it is a recent technology, more researches must be carried out.

BIM-Building Information Modeling The complexity of construction projects has increased in recent years. For this, new tools are required for their management. Building Information Modeling is an important change in this respect [55]. It is the process of data management of a building during its life cycle [56], based on a 3D modeling dynamic software and real time to save time and to reduce waste both in the plan and building phases [57]. This process generates the building information modeling which is composed by the building geometry, geographic information, used materials, etc. Designers, contractors and building operators have access to this modeling to organize, design, create and manage buildings and infrastructures [3]. This implies having transparent access to shared information by all stakeholders [58].

Waste Recycling from Construction Sector within the Circular Economy Paradigm 219 This technology reduces the use of resources and the environmental impact [59]. BIM plays a key role in green building [60] and, hence, in circular economy. As BIM provides information related to materials, this can help to learn more about the opportunities to recycle and remanufacture [3]. Besides, it has been observed that BIM improves productivity and reduces the project duration and cost [61]. BIM can be a good tool for waste management. Several BIM-based systems have been proposed in order to decrease C&D waste. An example of this is a database which has information related to the demolition waste based on BIM [62].

CASE STUDY: CLAY BRICKS PRODUCTION Explanation of the Clay Brick Production Process Cerámica Tamesis S.A. is a clay brick manufacturing company located in Cucuta (Colombia). This enterprise follows a linear production model as shown in Figure 1.

Figure 1. Manufacturing process of clay bricks.

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Strip Mining The production process starts with the exploitation of the raw material in open-pit mining, once a license is provided. If not, the clay is bought to suppliers. The clay is obtained by diggers, bulldozers and carriers. The energy used and the amount of clay produced by each machine are specified below: • • •

Digger: 250 l of fuel /h – 66 ton of clay/h. Bulldozer: 170.3 l of fuel/h – 144 ton of clay/h. Carrier: 772 l of fuel/h – 36 ton of clay/h.

The total energy required in this phase is 10200 KWh.

Storage The material is stored indoors. There must be enough material for at least 15 days of production. Preparation of Clay The clay is mixed with the sand, taking into account that sand must be 20% of the mixture. Then, the mixture is sent to the mill. Grinding of Clay Hammer mills are used to grind the material due to the fact that the humidity is 7%. In this part of the process, 10000 kWh are used to obtain 3000 ton of clay/h. Sieving The mixture is carried to the rotatory screen. The material which passes through the holes in the screen goes to storage silos. The remaining material, whose dimension is too large to fall through the holes in the screen, is carried back to the mill in order to reduce its size. Mixture and Moisture If the humidity is not enough to have the required plasticity, water is added until the humidity is 16-18%. Extrusion It is the process carried out to manufacture the required objects of a fixed cross-sectional profile. Roof tiles, floor tiles and bricks are produced and cut with a wire cutter to give them the appropriate length. The energy consumption is 1000 kWh. Drying The resultant pieces from the previous step undergo a process of drying with the aim of reducing the moisture. Depending on the requirements of the material, the drying can be natural -in indoor spaces without temperature and ventilation control-or artificial-drying tunnels where both temperature and ventilation are regulated depending on the pieces size and the clay source.The moisture content needs to be 3-6% before the mixture is taken to the stove. The energy consumption is 6000 kWh.

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Firing Bricks are burned at high temperature to gain strength, durability and density. This occurs in a beehive oven (Figure 2). The process of burning in the beehive furnaces takes place in three stages: heating, “hurried” fire and leveling. In the first stage, the temperature reaches approximately 110°C and the burning process lasts for 12 hours. During the “hurried” fire stage, coal is charged into the burners more frequently, rapidly raising a temperature of 600ºC. This temperature is considered to be the point at which the furnace has sufficient heat for the complete burning of the coal, ending with temperatures between 900°C and 1000°C. During the last stage, the temperature is increased allowing the upper and lower temperatures to be equalized in the internal area of the furnace until the final temperature of the designed curve is reached. Carbon waste (unburned) is collected at the bottom of the burners. In Cerámica Tamesis S.A. this takes 40 hours. In every burning, 3000 m2 clay bricks are produced, whilst the use of coal is 20 tons. The energy consumption is 27000 kWh.

Figure 2. Beehive oven.

Problem Analysis and Potential Solutions CO2 Emission In relation to the combustion gas during the firing phase, the analysis is done after 18 hours of firing, for which coal is employed. In one hour, 416.5 Kg coal are used, generating 1159.5 Kg CO2. This amount of CO2 is due to the firing. CO2 from decarbonation needs to be added to that process. Decarbonation takes 10 hours and each decarbonation generates 722.9 kg CO2. For this, the total amount of CO2 is:

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kg CO2 722.9 kg CO2 kg CO2 + = 1231.8 h 10 h h

Carbon footprint, which is the relation between the generation of CO2 and the production of the company, is used in order to measure the impact of CO2. Taking into account that 65 tons of bricks are manufactured in each firing process, which lasts for 40 hours, the tons of bricks per hour will be calculated as follows: 65 tons of bricks = 1.625 tons of bricks/h 40 h

Hence, the carbon footprint will be: kg CO2 kg CO2 h = 758 tons of bricks ton of bricks 1.625 h 1231.8

The resulting figure regarding the carbon footprint is five times higher than the carbon footprint for this process in Spain, which is 135 Kg CO2/ton. Therefore, this needs to be changed [63]. Circular economy aims at reducing waste CO2. Reducing is a challenge, but its use as a carbon resource may be a good solution for this issue. Hölscher et al.[64] observe in their review paper about the alternative use of carbon dioxide as carbon resource that technology allows obtaining carbon from CO2. This will help to reduce both the carbon footprint and coal exploitation.

Use of Coal As 18 tons coal are used in each firing and 10 firing processes are carried out every month, the use of coal per month is the following: 18

tons of coal firing tons of coal · 10 = 180 firing month month

Waste Generated by Coal Mining Waste is generated during coal extraction and, consequently, it is necessary to find an alternative use for that waste. Some waste is the following: fly-ash, coal mine drainage and coal-bed methane. The last one has a negative impact on the environment. Within the circular economy paradigm, the challenge is the reuse and recycling of this waste [65]. In our case, coal fly-ash is generated in the process of burning and only 75% of coal is burned [66]. The rest is coal fly-ash, which is easy to be moved by wind and if it is not well treated, it can affect the environment through dust generation [67]. For this, it is convenient to find other purposes. Some of its potential uses are:

Waste Recycling from Construction Sector within the Circular Economy Paradigm 223 •

•

Adding it to other materials to produce colored bricks. These bricks will make the use of clay reduce in such a way that the fly-ash will be part of the loop by becoming an input [65]. Moreover, the colored bricks will be sold at a more expensive price, giving them an added value. In the cement industry, due to the good properties it has. Besides, it improves its flame-resistant capability [65].

Renewable Energies As the use of carbon has a negative impact on environment, it is necessary to find an alternative [68], for example, solar energy. It has been observed that it can have a good performance during the firing process. Coal is replaced by solar energy, which together with solar concentrators allows reaching high temperatures [69]. Moreover, with this energy source, brick quality increases due to heat uniformity. Biomass can be incorporated into brick manufacturing. The use of pelleted biomass as a source of energy contributes to a reduction of fuel energy. Several researches have demonstrated that replacing 20% of carbon fuel in the firing process by pelleted biomass does not generate significant changes in the process. Moreover, the length of the process remains the same [70]. Besides, the level of CO2 emissions is lower than the one established by European countries. Depending on the origin of the pellets, the combustion efficiency levels vary between 87.7% and 86.3% [24].

Conclusion This is a very practical case of how production following a linear economy involves negative externalities. CO2 emissions are seven times higher than those established in Spain, which means that a change is imperative. New technologies have been developed during the last years and the manufacturing process of clay is suffering a change. This is due to the fact that companies are worried about the scarcity of natural resources. For clay manufacturing, big temperatures need to be reached and this implies the high use of coal. However, other energy sources can be taken into account, such as biomass and solar energy. The coal fly-ash generated by the firing can be added to other industries to manufacture recycled materials and promote, in this way, circular economy.

CONCLUSION The answer to the research questions are provided in this section: Is it necessary to make a change in the construction sector? The erection of building and civil infrastructures requires a huge amount of raw material and energy. This is mainly because the sector has followed a linear economy. The linear economy has been based on a take-make-dispose pattern. This has also made the sector

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become the one generating the highest amount of waste. Buildings have been designed to be erected but not deconstructed. This implies that demolition techniques are not really focused on waste management. The manufacturing of construction materials generates a large amount of CO2 emissions. As population and raw material scarcity are increasing, the construction sector plays a key role. Those are some of the reasons why a shift is necessary. How does the European Union support circular economy? Waste has become a big issue within the construction sector. For this, circular economy has relevance because it aims at designing out waste. It is clear that this is a big challenge for companies but the European Commission helps them through different protocols. The shift to circular economy is necessary in the construction sector due to the big amount of waste that it generates. With the aid of the EU Construction & Demolition Waste Management Protocol, companies gain information to put circular economy into practice. According to the European Commission, zero waste needs to be reached by 2020. It is clear that the importance of this issue is indisputable and the European Union is aware of it. Besides, companies are working hard to provide governments with practical solutions. How can circular economy be implemented in the construction sector? Using the design out waste principle is a strategic approach in order to implement circular economy in construction. As it has been mentioned above, this sector generates a large amount of waste. This must be reduced and this is the reason why the European Commission has developed a protocol. Recycled construction materials are also a good approach. They have appropriate functional characteristics and also enable the reduction of waste. Not only are they made from other construction materials previously used but also from waste coming from water treatment, such as sewage sludge ash. This implies both the reduction of waste and impact on the environment due to the fact that a lower amount of raw material is required. Building deconstruction is related to circular economy, as the components of an old building become those of a new one. This is known as a technological nutrient. This will take time to be widespread. However, several companies have already started to use this technique. Technology growth is determinant in this sector and enables the application of circular economy. BIM, resource passport and 3D printing are revolutionizing this market. Resources are efficiently used and the costs are reduced. It is important that materials are reintroduced into the circle and with the resource passport and BIM identification, their recognition and separation become possible.

ACKNOWLEDGMENT This research was supported by the European Regional Development Fund (European Union), the Government of Spain (Research Projects ECO2013-47027-P and ECO201784138-P), and the Regional Government of Andalusia (Research Project P11-SEJ-7294).

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[56] Lee, G., Sacks, R., Eastman, C.M. (2006). Specifying parametric building object behavior (BOB) for a building information modeling system. Automat. Constr. 15(6): 758-776. [57] Holness, G. V. (2008). BIM Building Information Modeling Gaining Momentum. ASHRAE Journal. [58] Grilo, A., Jardim-Goncalves, R. (2010). Value proposition on interoperability of BIM and collaborative working environment. Automat. Constr. 19(5): 522-530. [59] Spence, R., Mulligan, H. (1995). Sustainable development and the construction industry. Habitat Int. 19(3): 279-299. [60] Zuo, J., Zhao, Z. (2014). Green building research - current status and future agenda: A review. Renew. Sust. Energ. Rev. 30: 271-281. [61] Eastman, C.; Teicholz, P.; Sacks, R.; Liston, K. (2011). BIM Handbook: A Guide to Building Information Modeling for Owners, Managers, Designers, Engineers, and Contractors. Wiley, New York, USA. [62] Park, J., Cha, G., Hong, W., Seo, H. (2014). A Study of the Establishment of Demolition Waste DB System by BIM Based Building. Appl. Mech. Mater. 522-524: 806-810. [63] Diaz, R. (2014). Repercusión medio ambiental del uso de la cerámica estructural en España: Energía Embebida y Huella de Carbono [Environmental impact of the use of structural ceramics in Spain: Embedded Energy and Carbon Footprint]. Thesis, E.T.S. de Edificación (UPM), Spain. [64] Hölscher, M., Gurtler, C., Keim, W., Muller, T.E., Peters, M., Leitner, W. (2012). Carbon Dioxide as a Carbon Resource – Recent Trends and Perspectives. Z. Naturforsch 67(10): 961-975. [65] Haibin, L., Zhenling, L. (2010). Recycling utilization patterns of coal mining waste in China. Resour. Conserv. Recy. 54(12): 1331-1340. [66] Bautista, J. (2002). Optimización de la operación de secado de tableta y enfriamiento de tableta y bloque en Cerámicas Támesis [Optimization of the tablet drying and tablet and block cooling operation in Támesis Ceramics] S.A. Thesis, University of Francisco de Paula Santander, San José de Cúcuta, Colombia. [67] Xiaojun, H. (2007). Environmental damage and new uses technology of fly-ash. Guangdong Chemical Industry. [68] Conte, E. (2018). Sustainable use and management of natural resources in buildings and in the built environment. Sustainability 10(7): 2472. [69] Villeda Muñoz, G. (2010). Horno solar de alta temperatura para el cocimiento de tabiques de arcilla [High temperature solar oven for firing clay partitions]. Thesis, Instituto Politécnico Nacional, Querétaro, Mexico. [70] Garcia-Ubaque, C., Vaca-Bohorquez, M., Talero, G. (2013). Use of Pelleted Biomass in the Brick Industry in Bogota-Colombia: Energy and Environmental Analysis. Información Tecnológica 24(3): 115-120.

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 13

CIRCULAR ECONOMY OF WASTEWATER STREAMS BY MEANS OF MEMBRANE TECHNOLOGIES Marco Stoller Department Chemical Materials Environment Engineering, La Sapienza University, Rome, Italy

ABSTRACT In this Chapter the circular economy possibilities on membranes used for wastewater treatment processes are exploited. Circular economy in this case can be performed on two different aspects of the same technology: on the product streams and on the membrane modules. The first is performed by valorization of the waste stream, that is the stream separating in the membrane module and that is not considered to be the process one. In most cases, this stream correspond to the concentrate, and in the past was always discharged as a waste. The latter one can be achieved by increasing the longevity of the membrane module and, once exhausted, to think about after life applications. In the past, exhausted membrane modules were seen as a solid waste in line with consumables. Achieving circular economy in membrane technology is therefore not a simple task, and requires proper process design to be achieved.

Keywords: circular economy, membranes, fouling, valorization, reuse

INTRODUCTION Membranes are not an invention of man, but of nature. Indeed, membranes permit our body to perform many life supporting tasks for our survival. Membranes are encountered as main structure of single cells, but also in more complex organs such as kidney, liver and intestine. All these biological units have the capability to selective mass exchange, to separate 

Corresponding Author’s Email: [email protected].

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life supporting substances from those poisoning our body. Separating substances within a feed stream is the main application of membrane technology. The productivity of these biological units is enough to sustain life but are relatively low. In these mild operating conditions, membrane fouling is almost reversible and controlled. With the absence of membrane fouling, the biological membrane performances were maintained over a long period of time, avoiding membrane substitution or immediate organ failures. The only phenomena that may affect the performances over time are poisoning and aging. The latter one is unavoidable and will lead at some moment to biological membrane failures and, worst case, the death of the body. It must be noted that nature adopts circular economy strategies by disassembling the used membranes of dead bodies to reuse the materials in the environment. The process can be avoided by proper treatment (mummification, tanning), but requires in case direct man intervention. Nevertheless, when it comes up to industrial application, despite the choice of nature to use low operating conditions, there is a tendency to operate the membranes in harsh conditions such as high-pressure values and high solute concentrations. Therefore, the process quickly overcomes osmotic pressure and solubility values, and, at the end, triggers severe membrane fouling that sensibly reduces the longevity of artificial membrane modules [1]. Due to membrane fouling the modules requires substitution and the exhausted one needs to be dismissed. As simple these complex aspects are presented in this Introduction, at a first glance circular economy aspects in membrane technology in the industrial context should follow the same guidelines of nature, and can be identified to three fields of interest, that is: the valorisation of the stream exiting the membrane module that is not the main process stream, the reuse of exhausted after-life membrane modules and proper membrane engineering. In all cases, the minimization of waste formation and using new resources should be aimed, and many times, all three aspects are connected to each other and should be considered simultaneously, without sacrificing production targets and needs and without compromising economic feasibility of the process.

CIRCULAR ECONOMY BY VALORIZATION OF STREAMS The target of a membrane process is to separate the feed stream in two separate ones, the process stream and the secondary stream. The process stream may be the concentrate or the permeate stream, depending on the process targets. For ease of an example, in case of juice concentrates, the concentrate stream is the target one [2]; on the contrary, in water purification or desalination processes, the target stream is represented by the permeate one [3]. The design of the membrane process aims to reach on the target stream the desired quality in terms of purification, concentration and separation. At a starting stage of process design, the secondary stream is not considered much, and attention is focused to shift all or most undesired substances from the feed stream to this latter one. The result is that the target stream is well controlled by the membrane characteristics and process operation, whereas the secondary stream is forced to uptake regardless all substances that were separated.

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In many cases, the secondary stream is seen as a waste of membrane processes. Much effort is put to minimize this stream, by increasing the recovery rates of the process. Nevertheless, the formation of a secondary stream is unavoidable, and by increasing the recovery rates, the concentration of substances in this stream is more consistent. Consequently, the secondary stream can be hardly reused in other processes, for other purposes or to seek secondary products. As a first example, circular economy by means of waste stream valorization was performed on olive mill wastewater streams [4]. This wastewater is produced during olive oil production and contains a large amount of suspended solids and organic matter, in particular polyphenols such as tyrosol and hydroxytyrosol [5]. The treatment of the wastewater stream comprehend some separation steps in series such as ultrafiltration, nanofiltration and reverse osmosis. At the end, most of the waste stream is obtained as purified water compatible to the municipal sewer system. The rest (25%) are concentrates, that can be prepared for other applications: the ultrafiltration concentrate can be used in the biogas or fertilizer production; the nanofiltration concentrate exhibits highest amount of polyphenols, that can be recovered back, by post processes, as purified polyphenolic solutions for cosmetics and nutraceuticals; the reverse osmosis concentrates are suitable for membrane washing operations and diminishes the need of service water. At the end, exceeding a minimum plant capacity of 30m3 d-1, overall treatment costs are in the range of 5 Euro m-3, which is comparable to those paid nowadays by olive mill owners to discharge this wastewater on terrain or lagoons (7 Euro m-3) [6]. These latter practices are low cost but against EU directives and are permitted by specific national legislation. A second example is the treatment of tannery waste water streams by membrane technologies [7]. A main concern is the use of chromium in the tannery process, that represent one of the most dangerous pollutant for the environment. If irreversible fouling of the membranes is avoided, keeping OPEX costs of the treatment plant very low, economic feasibility of the process is reached. In particular, the use of a treatment plant of mediumlarge capacity may achieve a total cost saving of 28%. Concerning the nanofiltration section, the final recovery of 90% of Cr free water is achieved. Therefore, the environmental impact of the tannery industry would result sensibly reduced. The concentrate is sent back to the process, for an almost complete Cr reuse. Only 5% of the initial volume raises as industrial waste.

CIRCULAR ECONOMY BY REUSE OF AFTER-LIFE MEMBRANE MODULES Membranes will be exposed to unavoidable fouling issues during operation, that will lead to a reduction of the performances of the modules in terms of productivity. As soon as the productivity drops below a critical value, that is the project value of the plant capacity, the membranes requires a complete substitution to new ones. In this respect, the destiny of exhausted membrane modules appears to be relevant. In the past, exhausted membrane modules were treated under the legislation of special solid waste. The dismissal of these membrane modules follows the same route as other industrial and civil solid waste and disposed to landfills. As membrane technology

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applications increased in the recent past in number, a greater amount of exhausted membrane modules was produced every day world-wide, making this approach not sustainable. For this reason, much effort is performed to seek to new opportunities for exhausted membrane modules. To reuse a membrane module, there are two main aspects to consider: the extend of the degradation of the membrane performances and the hazard of the attached fouling material to the membrane surface. For the first aspect, not much can be done, since substitution of the membrane module was performed due to decrease of the performances, and the new application must use these membranes in fouled conditions. In some treatment processes, this can be of great advantage. For example, in wastewater treatment process ultrafiltration membranes can be initially used to purify the wastewater. As soon as fouling develops, the productivity of the membrane will be reduced, but parallel to this, the fouling layer may increase the membrane selectivity. At the end, a more selective and less productive membrane module is obtained [8]. This membrane modules can be used in between new ultrafiltration membrane modules and nanofiltration membrane processes for protection of the latter one of increased concentration values of pollutants in the permeate stream. The same approach may be used for treatment and separation of the milk proteins [9]. Membrane fouling triggers irreversible solid layer formation over the membrane surface and within membrane pores of material contained in the feed stream. Although during the membrane life most of these substances will be found in the secondary stream, part of it solidifies to the membrane. As soon as the layer grows, membrane performances will reduce to insufficient values. Removing the exhausted membrane module, this layer of deposited solid material will be removed together. This may inhibit the use of exhausted membrane modules as impermeable membranes for some applications such as underground water confinement [10], geotextiles [11] or packaging [12]. Another approach is to use the membranes in incinerators for energy recovery [13] or converting tight membranes in looser ones [14].

CIRCULAR ECONOMY BY MEMBRANE ENGINEERING Membrane fouling is the main factor to the longevity of the membrane modules and thus affects the timing of circular economy procedures. Inhibiting fouling is surely one of the most important issues but in this context, it is not mandatory to define and describe with scientific precision the phenomena of membrane fouling. For liquid-liquid separation processes, Field et al., introduced the concept of critical flux for microfiltration, stating that there is a permeate flux below which fouling is not promptly observed [15]. In subsequent years, research identifies critical flux values for ultrafiltration (“UF”) and nanofiltration (“NF”) membranes, too [16]. The concept is suitable to the need to avoid fouling triggering operating conditions, and as a consequence, to avoid fouling at all. Nowadays, the critical flux concept is well accepted by both scientists and engineers as a powerful membrane process optimization tool as long critical fluxes apply [17]. In time it was observed that many systems treating real waste water streams did not strictly follow the critical flux theory. Le Clech et al., noticed that sub critical flux operations

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may not be sufficient in order to have no fouling rate [18]. Moreover, the measurement of critical fluxes was often not possible, and in order to overcome this problem, the identification of “apparent” critical points was used. Given this situation, Field and Pearce introduced for the first time the concept of the threshold flux [19]. Briefly summarizing the concept, the threshold flux is the flux that divides a low fouling region, characterized by a nearly constant rate of fouling, from a high fouling region, where flux dependent high fouling rates can be observed. The introduction of the threshold flux permitted to describe the behaviour of those systems not following the critical one and represent a powerful membrane process optimization tool which found positive feedback and successful validation. The main drawback of these concepts is that the determination of the values cannot be theoretically predicted, but only experimentally determined by time consuming experiments at a certain time moment. Moreover, different threshold flux values can be measured on the same system, depending on various factors, such as hydrodynamics, temperature, feed stream composition and membrane surface characteristics [17, 20-22]. Feed stream composition and operating time are the main responsible of ever-changing threshold flux values, and this is especially true for real wastewater streams treatment by membranes, since the entering feedstock quality is not constant during the year. An additional factor is given in case of batch membrane processes, which are used to limit the amount of required membrane area and thus saving investment costs and irremediably lead to sensible feedstock changes during operation. It appears that threshold flux values do not remain constant as a function of time. This represent a major difficulty in fine-tuning optimal operating conditions and to apply this tool successfully to membrane process design purposes. Nevertheless, critical and threshold flux theories were quickly applied by researchers and membrane process designers in order to inhibit membrane fouling in many systems. As an illustration of popularity of the use of these concepts, more than 6400 papers were published in international scientific journals in the last 5 years [23]. The concepts are not able to describe and explain the fouling phenomena, but give advice how to avoid it and this may be fully sufficient to proper design membrane plants. The problem to define correctly ever changing critical and threshold flux values leads to confusion among membrane practitioners. Even in research, among academics, the confusion about the correct use of the theory exists. Some researchers publish comprehensive review papers about the correct use of the concepts. Critical fluxes were defined in different types, such as strong form, weak form and for irreversibility. Despite these efforts, the introduction of new critical flux definitions increased the confusion and the erratic use among membrane practitioners, and has become even worse with the introduction of the threshold flux concept. Since late 2011, only 32 papers were published using correctly the term of threshold flux on international scientific journals, covering the treatment of wastewater streams, beside those exiting the olive oil, the fruit juice, textile and biotech (algae) industries [23, 24-32]. Many papers still relay on a wrong use of the older critical flux concept on those systems where threshold fluxes suit more precisely. In order to overcome these problems, many designers use the sustainable flux as project parameter. This latter flux is equal to the set point value of the control system of the membrane plant in order to achieve the productivity targets, even if fouling is formed at such a rate that it does not affect the output over long periods of time. Compared to the other definitions, the sustainable flux has a subjective characteristic, trying to fill the knowledge

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gap by the experience of the designer, and as such, cannot be considered a valid engineering tool for design purposes, although it was successfully adopted many times. The sustainable flux concept was never taken into account as a possible parameter in order to develop design tools. In the past years, before the concept of the threshold flux was introduced, many papers on olive vegetation waste water (OVW) purification by membranes, mainly ultrafiltration and nanofiltration, always determining critical fluxes, were published by the authors [33-36]. Irreversible fouling arises quickly on the membranes due to the high concentration of pollutants when wastewater is purified without any pretreatment, and different pretreatment processes influence to a variable extent the critical flux values [37-40]. Therefore, proper and optimal designed pretreatment processes on the given feedstock must be developed in order to maximize productivity and minimize fouling: this objective will be referred from now on as the concept of pretreatment tailoring of membrane processes. The Authors observed in previous research works the change of fouling regime by using olive mill wastewater. Despite the applied optimization methods were based on modified critical flux measurements, before the threshold flux concept ever existed, successful fouling control was accomplished on this system, and in detail justified by means of the threshold flux in 2013 [28]. The developed tools were successfully validated, but dependent of the existence of many different concepts, thus resulting complicated. Field et al., suggested that the correct application of the threshold flux is de facto very near to the sustainable one [19]. Moreover, critical and threshold flux concepts share many common aspects which merge perfectly into a new concept, that is the boundary flux. The introduction of the new boundary flux concept does not extend by addition of new theory or knowledge the critical and threshold flux concepts. On the other hand, it tries to simplify the use of these concepts in future works. Referring to one single concept will reduce sensibly the incorrect use of both the critical and threshold flux concepts, and permits the development of simplified design tools for membrane engineers. Once these tools are widely available, by proper boundary flux knowledge or determination, the membrane process sustainability may be reached or, at least, roughly estimated. The boundary flux shares all known aspects of the critical and threshold flux concepts, without adding something new. The advantage to use a general boundary flux concept relies in the impossibility to misinterpret its value, and eliminates the confusion among membrane practitioners to discriminate between different flux types. The boundary flux will be the guideline flux, and all successive considerations, starting from the optimal membrane performances down to the optimal membrane process design and plant construction, will be based on this. Membrane fouling, expressed as a permeate flux reduction as a function of time given by some phenomena different than polarization and/or aging of the membrane, can be subdivided in three main typologies: 1

2

A reversible fouling; this kind of fouling strictly follows the driving force amplitude, e.g., operating pressure values. As soon as the pressure over the membrane is reduced, this fouling is eliminated after a certain (short) period of time by the same quota. A semi-reversible fouling; this kind of fouling accumulates over the membrane surface and cannot be easily eliminated. The only way to eliminate this kind of fouling is to stop the separation process and clean or wash the membranes, with

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water or aqueous solution of chemicals, respectively. Although this kind of fouling is after the cleaning/washing procedure almost eliminated, it represents a problem in the continuous process operation since it forces to process shut-down at timed intervals. An irreversible fouling; once formed, this kind of fouling is not possible to eliminate by any procedure. It is the main cause of membrane failure concerning productivity.

In all cases, in case of tangential cross flow separation by membranes, all three fouling types will unavoidably appear and form. The existence of different fouling typologies affecting membranes were previously explained by Bacchin et al., and Oringer et al., and are based on the assumption of possible local conditions triggering different liquid/gel phases over the membrane and in the membrane pores due to the concentration profiles by polarization [41, 42]. For systems which exhibit only reversible fouling at low pressure conditions, critical flux concepts apply best. In this case, although strictly not correct, membrane aging may be considered the only type of irreversible fouling affecting this system. Concerning the critical flux Jc, hereafter used in terms of critical flux for irreversibility, the following fitting equations apply: dm/dt = 0; Jp(t) ≤ Jc

(1)

dm/dt = B (Jp(t) – Jc); Jp(t) > Jc

(2)

where m is the permeability of the membrane, B is a fitting parameter and Jp(t) the permeate flux at time t. As soon as eq.2 applies, irreversible fouling starts to form. Semi-reversible fouling may be hardly observed in all the applied pressure range, and is therefore neglected. If semireversible fouling appears at low operating pressures, the system fits well the threshold flux theory. Concerning the threshold flux Jth, the proposed equations by Field et al., are as follows [19]: dm/dt = a; Jp(t) ≤ Jth

(3)

dm/dt = a + b (Jp(t) - Jth); Jp(t) > Jth

(4)

where a, b are both fitting parameters. In case eq.3 is valid, both reversible and semi-reversible fouling are observed, whereas irreversible fouling may be neglected. As soon as eq.4 applies, irreversible fouling sensibly adds to the previous fouling phenomena. It is interesting to notice that the threshold flux equations are similar to the critical flux equations and differ only by the presence of the “a” parameter. In fact, if the case of “a” equal to zero is admitted, eq.(3) and eq.(4) may reduce to eq.(1) and eq.(2), respectively. The parameter “a” value measures below threshold flux conditions the constant permeability loss rate of the membrane in time. If this value is equal to zero, no permeability will be lost in time and therefore no fouling is triggered. This is valid only below critical flux

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conditions, and therefore eq. (3) includes eq.[1] if a = (0,∞). It appears that the parameter “a” is related to the semi-reversible fouling of the membrane system. Above critical and threshold flux conditions, fouling behaves in similar way by exponential permeability loss rates in time. Again, if a = (0,∞), eq.(4) fits eq.(2). The only difference between these systems is that in critical flux characterized systems fouling is not affected by the continuous presence of a constant fouling permeability loss rate as in threshold flux characterized systems. Beside this theoretical difference of the two systems, the Authors want to point out that this aspect is of limited practical importance, since the exponential part of eq.(2) and eq.(4) will quickly overwhelm the linear contribution of the parameter “a” in eq.(4). Summarizing, both critical and threshold fluxes divide the operation of membranes in two regions: a lower one, where no or a small, constant amount of fouling triggers, and a higher one, where fouling builds up very quickly. The introduction of the new boundary flux concept does not extend by addition of new theory or knowledge the critical and threshold flux concepts. On the other hand, it tries to simplify the use of these concepts in future works. Referring to one single concept will reduce sensibly the incorrect use of both the critical and threshold flux concepts. By introducing a new flux, that is the boundary flux Jb, the previous equations may be written as: dm/dt = - α; Jp(t) ≤ Jb

(5)

dm/dt = - α + β (Jp(t) - Jb); Jp(t) > Jb

(6)

where: •

•

α, expressed in [l h-2 m-2 bar-1], represents the constant permeability reduction rate suffered by the system and will be hereafter called the sub-boundary fouling rate index. α is a constant, valid for all flux values. β, expressed in [h-1 m-2 bar-1], represents the fouling behaviour in the exponential fouling regime of the system, and will be hereafter called super-boundary fouling rate index. β appears to not be a constant, and changes with TMP.

The method to measure the boundary flux is similar to the ones used to measure critical flux values, but needs a different approach in order to determine the value of α at first, the value of β successively. Beside experimental data, the extended method requires the use of eq.(5) and eq.(6) to separate the two different operating regimes, that is at the end a region where irreversible fouling may be neglected from another region where irreversible fouling is formed. The validity of eq.(5) excludes the validity of eq.(6): as long as eq.(5) holds, sub boundary flux conditions are met. This approach needs a simple mathematical model to fit pressure cycle experimental data. As soon as the dm/dt value diverges from constancy, the first point is the boundary one, and the relevant TMP value is equal to TMPb. The boundary flux values are sensibly influenced by those parameters affecting the critical and threshold flux, hereafter listed:

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Hydrodynamics Temperature Membrane properties Time Feedstock characteristics Washing and cleaning of membranes

Adopting circular economy concepts means to increase the longevity of the membrane module, and therefore to operate at sub boundary flux conditions.

CONCLUSIONS Performing a circular economy within the membrane technology framework means to consider all the aspects presented in this Chapter together without sacrificing technical and economic feasibility. In Figure 1, all approaches are merged together to report a possible procedure to meet the targets.

Figure 1. Scheme of circular economy for wastewater stream valorization in membrane technologies.

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[2]

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[19] Field, R. W. and Pearce, G. K. (2011) Critical, sustainable and threshold fluxes for membrane filtration with water industry applications, Advances in Colloid and Interface Science 164(1-2): 38-44,. [20] Stoller, M. and Chianese, A. (2006) Optimization of membrane batch processes by means of the critical flux theory, Desalination 191: 62-70. [21] Stoller, M. and Chianese, A. (2007) Influence of the Adopted Pretreatment Process on the Critical Flux value of Batch Membrane Processes, Industrial Engineering Chemistry Research 8(46): 2249-2253. [22] Lipp, P., Lee, C. H., Fane, A. G. and Fell, C. J. D. (1988) A fundamental study of the UF of oil-water emulsions, Journal of Membrane Science 36: 161-177. [23] Data Taken from Scopus, Dec 2013, http://www.scopus.com. [24] Cicci, A., Stoller, M., Bravi, M. (2013) Microalgal Biomass Production by Using Ultraand Nanofiltration Membrane Fractions of Olive Mill Waste Water, Water Research 47(13): 4710-4718, doi: 10.1016/j.watres.2013.05.030. [25] Ochando-Pulido, J. M., Stoller, M., Bravi, M., Martinez-Ferez, A. and Chianese, A. (2012) Batch membrane treatment of olive vegetation wastewater from two-phase olive oil production process by threshold flux based methods, Separation and Purification Technology, 101: 34-41, doi: 10.1016/j.seppur.2012.09.015, 2012. [26] Stoller, M., De Caprariis, B., Cicci, A., Verdone, N., Bravi, M., Chianese A. (2013) About proper membrane process design affected by fouling by means of the analysis of measured threshold flux data, Separation and Purification Technology 114: 83-89, doi: 10.1016/j.seppur.04.041. [27] Stoller, M., De Caprariis, B., Cicci, A., Verdone, N., Bravi, M., Chianese, A. (2013) About proper membrane process design affected by fouling by means of the analysis of measured threshold flux data, Separation and Purification Technology 114: 83-89, doi: 10.1016/j.seppur..04.041. [28] Stoller, M., Ochando Pulido, J. M., Chianese, A. (2013) Comparison of Critical and Threshold Fluxes on Ultrafiltration and Nanofiltration by Treating 2-Phase or 3-Phase Olive Mill Wastewater, Chemical Engineering Transactions 32: 397-402. doi: 10.3303/ CET1332067. [29] Stoller, M. A (2013) Three Year Long Experience of Effective Fouling Inhibition by Threshold Flux Based Optimization Methods on a NF Membrane Module for Olive Mill Wastewater Treatment, Chemical Engineering Transactions 32: 37-42. doi: 10. 3303/CET1332007. [30] Luo, J., Zhu, Z., Ding, L., Bals, O., Wan, Y., Jaffrin, M. Y., Vorobiev, E. (2013) Flux behavior in clarification of chicory juice by high-shear membrane filtration: Evidence for threshold flux, Journal of Membrane Science 435: 120-129. [31] Barredo-Damas, S., Alcaina-Miranda, M. I., Iborra-Clar, M. I., Mendoza-Roca, J. A. (2012) Application of tubular ceramic ultrafiltration membranes for the treatment of integrated textile wastewaters, Chemical Engineering Journal 192: 211-218. [32] Wicaksana, F., Fane, A. G., Pongpairoj, P., Field, R. (2012) Microfiltration of algae (Chlorella sorokiniana): Critical flux, fouling and transmission, Journal of Membrane Science 387-388: 83-92. [33] Stoller, M. (2008) Technical optimization of a dual ultrafiltration and nanofiltration pilot plant in batch operation by means of the critical flux theory: a case study, Chemical Engineering & Processing Journal 47/7: 1165-1170.

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[34] Iaquinta, M., Stoller, M., and Merli C. (2009) Optimization of a nanofiltration membrane process for tomato industry wastewater effluent treatment, Desalination 245: 314-320. [35] Stoller, M., Di Palma, L., and Merli, C. (2011) Optimisation of batch membrane processes for the removal of residual heavy metal contamination in pretreated marine sediment, Chemistry and Ecology 27: 171-179, doi: 10.1080/02757540.2010.534083. [36] Stoller, M., and Chianese, A. (2006) Technical optimization of a batch olive wash wastewater treatment membrane plant, Desalination 200: 734-736. [37] Stoller, M. (2011) Effective fouling inhibition by critical flux based optimization methods on a NF membrane module for olive mill wastewater treatment, Chemical Engineering Journal 168(3): 1140-1148. [38] Stoller, M., and Bravi, M. (2010) Critical flux analyses on differently pretreated olive vegetation waste water streams: some case studies, Desalination 250(2): 578-582. [39] Lim, A.L., and Rembi, B. (2003) Membrane fouling and cleaning in MF of activated sludge wastewater, Journal of Membrane Science 216: 279-290. [40] Stoller, M. (2009) On the effect of flocculation as pre-treatment process for membrane fouling reduction, Desalination 240: 209-217. [41] Aimar, P., Bacchin, P. (2010) Slow colloidal aggregation and membrane fouling, Journal of Membrane Science 360: 70–76. [42] Ognier, S., Wisniewski, C., Grasmick, A. (2004) Membrane bioreactor fouling in subcritical filtration conditions: a local critical flux concept, Journal of Membrane Science 229: 171–177.

PART IV. REUSE, REDUCE, RECYCLE IN CIRCULAR ECONOMY

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 14

SUSTAINABLE FOOD PRODUCTION: THE TRANSITION TOWARDS A CIRCULAR ECONOMY OF PLASTIC FOOD PACKAGING Pedro Núñez-Cacho1, , Rody Van der Gun2, Juan Carlos Leyva-Díaz3 and Valentin Molina-Moreno2 1

Department of Business Organization, University of Jaén, Spain 2 Department of Management, University of Granada, Spain 3 Department of Chemical and Environmental Engineering, University of Oviedo, Spain

ABSTRACT The food packaging industry mainly uses plastic as the base material. In this chapter we review the state of the matter, the advantages and disadvantages of plastic in this sector, the mechanical and chemical processes for recycling, the position of the sector and its stakeholders before the Circular Economy and the measure of the transition of companies from this industry towards this new paradigm of production.

Keywords: circular economy, plastic, food packaging industry, transition, stakeholders

INTRODUCTION Since the first piece of plastic was created in 1862, this material has become increasingly popular and is currently used for food packaging. For instance, in 2015, the plastic containers used were responsible for 42% of the total plastics used. In addition, more than 90 percent of flexible containers are made of plastic [1]. The Ellen Mac Arthur Foundation (EMF) for Circular Economy [2] said that the volumes of plastic containers will continue their strong growth in the coming years, to double over a time horizon of 15 years. 

Corresponding Author’s Email: [email protected].

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The packaging traditionally contains a product, protects and informs about the product inside. “The container must protect what it sells and sell what it protects” [3]. The value for the consumer is derived not only from the packaging itself. The value that comes from the packaging is the consumer experience of the total offer. In the food industry, plastic food packaging includes both, the packaging itself, and the product derived from distribution. The Circular economy (CE) aims to minimize any waste, including emissions. This could be done by creating products that can be recycled indefinitely [4]. For this reason, the food industry needs to find a balance between plastic reduction, prolonged shelf life and food protection for reasons of consumer safety [5]. Minimizing plastic containers that flow through the supply chain is important because packaging is the main source of plastic waste.

STATE OF THE QUESTION OF PLASTIC FOOD PACKAGING Undoubtedly, there are significant advantages derived from the plastic food packaging, being used for food packaging due to multiple reasons. Firstly, plastic is a cheap, low weight and durable material [6]. To start, this light weight reduces logistic costs. Secondly, this material can be easily formed and shaped in all desirable ways, for each specific product [7]. The material allows varying the size of the portions and improves the information to consumers. Thirdly, plastics are cheap to produce and they need low energy during manufacturing. The food is both, well preserved and protected by plastics. The food stays fresh, which increases the quality. As an example, the plastic wrap extends the shelf life of a cucumber from three to fourteen days. In addition, the food is safe in a plastic container, because plastics survive in extreme environments. With plastic packaging, it is possible that food has a greater expiration date, which, at the same time reduces food waste [8]. On the other hand, there are disadvantages of plastic food containers. For example, a 39.7% percent of plastic was used in Europe for packaging and just a 40.8% of this plastic packaging was recycled in 2016 [9]. Thus, we face the main problem: Most of plastics are used once and thrown away after the use. Besides, plastics never disappear completely in landfills or oceans. This durability is becoming a disadvantage when plastics are not recycled. Plastics in the oceans, for example, break down into small pieces, called micro plastics. Animals like fish ingest these micro plastics, which leads them to the human food chain. On the other hand, plastics often contain a chemical mixture of substances, which poses possible consequences for human health and the environment [19]. Another disadvantage of plastics is the cost of recycling, compared to the cost of creating new plastics. It is currently cheaper to produce new plastic bottles than to recycle them. Cleaning and repairing plastics requires a lot of water, energy and effort. The expansion of plastic production keeps the prices of new plastics relatively low. The price of transparent PET recycled sometimes exceeded the price of transparent virgin PET for short periods of time [11]. Apart from this, more than 14% collected for recycling, just a 5% of plastic containers are retained for its subsequent use [12]. In addition, there are a lot of losses during the recycling process, during collection, separation and classification of post-consumer food containers. For these reasons we argue that plastic food packaging is creating negative externalities. The negative external effects are the costs and benefits [8] that are felt beyond or “external

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to” those that cause the effect [13], such as greenhouse emissions from production and environmental pollution for leaks of plastics in natural systems. This causes a market failure because people who create, use and dispose of plastic do not pay the price of pollution.

Disposable and Recyclable Plastic Containers Apart from the recycling issues, we found another problem from plastic material. Not all plastics are recyclable. Plastic bags, straws and coffee cups are examples of plastics that are not recyclable. In this case, the problem must be addressed through reuse whenever possible. Plastic products have a short shelf life. According to Wooward [14], a plastic bag has an estimated shelf life of 12 minutes. Packaging can be classified correctly and profitably and that there is a market for circular plastics produced. On the other hand, replacing plastic food containers with other materials (glass, steel, aluminum, wood, fiber and paper) would increase energy use, water consumption and solid waste, and increase greenhouse gas emissions. Therefore, it is needed another solution to recycling, incineration or disposal in landfills are the three options for handling plastic waste. Recycling is the one with the lowest global warming and lowest energy consumption. Therefore, recycling plastic food containers is an important step to reduce the negative impact of plastic pollution. The main problem here is how we use plastic food containers after use. In Europe, approximately 40 percent of the packaging is discarded after being used only once [15]. This results in a loss of energy, money and generates plastic waste.

Primary Recycling of Plastic Food Containers The terminology for plastic recycling is complex. Several solutions can be found for the treatment of plastic waste, recycling, down cycle or production of chemical components, fuel or energy [16]. With regard to recycling and recovery activities, one can distinguish between primary, secondary, tertiary and quaternary recycling. Primary means; reuse. The secondary recycling process, means that plastic waste is recycled and manufactured in other plastic products. Also known as, “open loop recycling.” Tertiary recycling converts discarded plastic products into petrochemical products or high value fuel raw materials. And finally, quaternary recycling is not considered recycling because it is used to recover the energy concept of plastic waste. The recovery and degradation of plastic food containers are forms of secondary and tertiary recycling. Only primary recycling is considered in this investigation; applications that produce the same or similar products. Important for closed circuit recycling is that the waste stream can be classified, depending on the different types of plastic containers. Due to the separation of the type of plastic, the different recycling loops are not contaminated with other types of plastics. Incorrect or incomplete classification of plastics disrupts their recycling process and results in poor quality or even decomposition of processes [6, 16].

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THE PROCESS OF MECHANICAL AND CHEMICAL RECYCLING OF PLASTIC FOOD CONTAINERS A key principle of a CE is that plastic food containers circulate at the highest value at all times. According to Plastics Recyclers Europe [9], primary mechanical recycling is the most preferable technique, over the other two types of recycling: Mechanical recycling in open loops and chemical recycling. According to the president of the World Plastics Council, mechanical recycling has the greatest potential in the context of the Circular Economy. Mechanical recycling is the physical process of grinding, crushing and melting plastic waste [10]. This technique has the possibility of transforming post-consumer plastics into plastic products: there is therefore talk of closed circuit recycling. All types of thermoplastics can be recycled mechanically [9]. Before mechanical recycling can be performed successfully, plastics must be classified in their type, according to their chemical composition. According to Suez [17], in the case of mixed plastics are converted into energy or recycled at a high cost, there is no primary recycling possible. Plastic waste comes from different currents (industrial, municipal, commercial or agricultural). This results in differences in terms of resin composition and level of contamination. As regards the collection of used plastic containers, there are currently three collection systems, deposit, industrial waste and collection in the cities. The plastic packaging may be made of a type of thermoplastic (“mono-material”), or it may be made of various types of plastics (“multilayer plastic packaging”). Multilayer means that different types of plastics are combined in a single package improves the performance of the package but decreases the value after use. Currently, plastic is mostly recycled mechanically. All types of plastic with a main component (mono-material) of PET, PE or PP that has the potential to be recycled. The size and thickness of the packaging are important, if the plastic packaging is too small, too large, or too thin, it is more complex, costs the process, and is not usually recycled. In addition, there is the theme of color. In the recycling process, the infrared scanner does not process the black plastic packaging or the inner wrap during the mechanical recycling process. In addition, if the infrared scanner cannot recognize the number of a plastic, it ends up as waste and is discarded (not recyclable). Therefore, transparent plastics are the easier ones to recycling. Other types of plastics that are not suitable for recycling and they will be incinerated. PET, PE and PP packages that are suitable for recycling are separated by sorting on an assembly line. The efficiency of mechanical recycling depends on the purity of the incoming plastic waste [18]. After the plastics are separated, they are washed with water and finally melted into plastic grains. “Recycling and cleaning are more important for the environmental result than the direct impact of the packages” [19]. Those grains can be used to make new plastic packages.

CIRCULAR ECONOMY AND PLASTIC FOOD PACKAGING There is a worldwide trade of plastic waste. It mainly flows from western countries to Asian countries, specific to China. Because of cheap labor costs and reduced environmental

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standards. However, recycling companies state that they cannot even handle to recycle all domestic plastic. Therefore, the plastic waste eventually – according to British recycling companies – still goes to East Asia countries, after being ‘laundered’ into the country generator. For example, in 2018, China banned plastic waste from Europe. Therefore over three quarters were shipped to countries within Europe and plastic waste is reused domestically [20]. The packaging sector is one of the largest plaintiffs in plastics, and therefore one of the largest generators of negative externalities. The perspective of the linear economy, which “manufactures uses and discards,” supports this production model. The consequence is that we produce plastic that is discarded after a single use. To evolve towards the CE model in the sector food industry, it is required that the materials used to package food be reusable or recyclable in a cost-effective manner [21]. Food plastics recycling is the solution when consumers do not reuse containers or when containers are not suitable for reuse. Currently, the plastic collected from post-consumer waste is not transformed back into plastic containers. Additionally, the mechanically recycled plastic from municipal waste does not meet the necessary hygiene requirements for use in packaging. The European Food Safety Authority (EFSA] stated that recycled plastic could be used under certain conditions and n materials in contact with food. The different types of (plastic) containers that they can segregate to recycle and end up mixing materials can confuse consumers. If the collection and classification of plastic waste improves, the efficiency of recycling would also increase [22](BIO Intelligence Service, 2013). The European strategy of the CE pursues, in 2025, to raise the recycling rate of waste from packaging to 70% [21]. However, this objective is ambitious, especially under the pressure of the plastics industry. According to Plastics Recyclers Europe, the 55% recycling target can be achieved in 2025, or even 65% if exports are included. What is presented as essential is the creation of closed circuits for the collection, separation and recycling of plastic food containers. The materials to be recycled would enter a closed circuit recycling process in which plastics would maintain the highest possible value. This would positively influence the quality of the recycled product, providing a successive recycling system. In addition, in this type of closed circuit material flow there would be no resource leakage’s in 2017, the European model for dealing with plastic waste was predominantly based on incinerators (roughly 40 percent), landfills (around 30 percent) and exports (more or less 12 percent), primarily to China.

STAKEHOLDERS AND TRANSITION TO THE CIRCULAR ECONOMY For sustainable development, cooperation between stakeholders is essential [23]. In 1984, Richard Freeman defined stakeholders as ‘’any group or individual who can affect or is affected by the achievement of the firm’s objectives.’’ However, this definition is criticized while it is too broad. Therefore, in this research stakeholders are those individuals or groups that hold power over the company. The following primary stakeholders can be identified, plastic producers, food producers, retailers, consumers and waste managers. Besides there are two secondary stakeholders who hold power in the supply chain of plastic food packaging, the government and NGOs. All stakeholders need to communicate and collaborate in order to

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create a secure circular supply chain [24]. Because the government and NGOs not active participating in the supply chain, no behavioral changes are described for them. Within Europe, the European Commission demands from stakeholders to act regarding their voluntary pledges to increase the amount of recycled plastics. By new business strategies and initiatives from stakeholders, market failures can be reduced – or maybe even be resolved.

Producers of Plastic Packaging Within the food industry supply chain, the plastic packaging producers are the first economic player. They have a corporate social responsibility; they also need to adjust their strategies based on their responsibility, which is also extended to the producer. The transition to the CE model requires an environmental management strategy [25]. To achieve the objective of increasing recyclability, the highlights are: Collaboration with food producing companies, the exploration of the use of recycled materials, and the improvement of packaging design. It is also necessary to establish production control mechanisms and determine the degree to which these packages will be recycled [26]. The consensus between and collaboration between the entire supply chain members is an essential element to transition to the CE [13, 27], this collaboration between the different actors, facilitates the transmission of information and experience within the entire supply chain, being able to incorporate best practices related to the CE from another organization. The sustainable strategy of the producers of plastic packaging should focus on reducing the negative external environmental effects of the company. This strategy can be supported by the Cradle-to-Cradle [C2C) philosophy applied to plastic food containers. C2C is an “ecoeffective” solution that maximizes the benefits for the ecological and economic system [28]. The C2C paradigm is one of the main pillars of the CE [29]. The materials maintain their greatest value during their useful life, due to the closed circuits. According to the architect and chemist of the C2C paradigm, McDonough and Braungart [28], a container must be designed to be reused or fully recycled, within a closed circuit process, in which there is no loss of material performance [30]. Therefore, C2C means reducing the impact on future generations, due to this higher recycling rate. McDonough and Braungart argue that C2C containers can be 100 percent recycled if a closed cycle technical nutrient recycling system is used. To facilitate C2C strategies, a comparative evaluation of the product’s life cycle (LCA) can help in decision-making for plastic packaging companies, considering the environmental impacts of the container’s life cycle. LCA is becoming an integral part of industrial decision-making processes (Global Protocol on Packaging Sustainability 2.0). By creating plastic, the possibilities of the end of life should be taken into account; the design must allow its reuse and/or recyclability [31, 32]. In addition, plastic containers should be easier to separate for consumers and waste managers. Mutual coordination and shared responsibility are necessary with collaboration between stakeholders. The actors within the value chain should not focus on addressing the problems of plastic packaging within their own internal processes and strategies. The best would be a lightweight plastic food container made only from recycled materials and designed for reuse [19].

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Plastic Producers Within the supply chain of the food industry, the plastic producers are one of the first economic actors. They must fulfill a corporate social responsibility. In addition, plastic producers need to adjust their strategy, based on their extended responsibility on the part of the producer, following a greener strategy, encouraging “green” production [33]. The transition to evolve the CE requires an environmental management strategy, including aspects such as the increase of the recyclability rate of plastic packaging. Besides, the collaboration with food producing companies, the research and development of recycled materials, the improvement of packaging design according to the approaches of the CE and the design of controls mechanism to identify the degree of recycling [26]. In order to transition to the Circular economy, plastic packaging producers should focus on reducing their negative externalities or negative external environmental effects [34, 35]. The use of clean and renewable energy should be promoted, in order to reduce the CO2 footprint strategy. Another aspect to consider would be the reduction of the water footprint of the producing company. The sector is intensive in the use of chemical products and must follow procedures that guarantee the progressive reduction of its water footprint. In addition, the use of the cradle-to-cradle (C2C) design philosophy can boost that of the plastic food packaging industry in a circular model. C2C is an “eco-effective” solution; maximizing the benefit for ecological and economic systems [28]. The C2C paradigm is one of the main pillars of the CE [29]. It can facilitate the implementation of the C2C philosophy, the comparative evaluation and the analysis of the product life cycle (LCA) as it helps in making decisions for the companies that produce plastic containers in each phase of the product's life, promoting the reduction of environmental impacts, in each of the life cycles of the container. LCA is becoming an integral part of industrial decision-making processes (Global Protocol on Packaging Sustainability 2.0). Thus, when the plastic is manufactured, the possibilities of the end of the life must be taken into account, using a design should allow its reuse and/or recyclability [31, 32].

Food Producers In 2018, the Ellen Mac Arthur Foundation, in collaboration with U.N. Environment, launched the Global Commitment to the New Plastic Economy. This is that more than 290 organizations share a harmonized vision, committed to that in 2025, 100% of the manufactured containers are reusable, recyclable or compostable. These commitments and the work in partnership, jointly designing sustainable strategies, is essential to achieve CE implementation. Government organizations can create and stimulate cooperation between corporations in product chains [36, 37]. For example, with the EU and the strategy for plastics in a CE of 2018. Recipients of these drivers are the large food producing companies, although they also depend on the plastic containers they receive. Therefore, the use of the Extended Producer Responsibility (EPR) policy can convey pressure from food producers to plastic producers.

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Retailers Retailers create the link between the final consumer and the production industry. Therefore, they can influence food producing companies, based on the consumer’s desire to receive more sustainable products. On the other hand, retailers are free to decide which brands they sell, this translates into an influence on other actors in the supply chain, such as food and plastic producers. The retailer can also present the CE as a marketing strategy, since there is a great awareness and concern on the part of consumers about the use of plastic packaging in the food industry. Therefore, retailers must evolve towards a circular model, favoring reverse logistics, creating spaces to return products while maintaining value. The retailer can thus become a central collection point, where consumers can buy and eventually return the plastic packaging of the food they consumed [24], by driving the reverse supply chain.

Consumers Consumer behavior and perceptions are essential for the success of a CE. Consumption behavior is changing over time. Food consumption patterns have increased the waste of plastic containers [31]. Especially, due to the higher consumption of “take-out” food and people buy more food, packed in portions for a single person. The change in behavior in consumers occurs through awareness of sustainability aspects and knowledge of the CE. Consumers are a fundamental link in the implementation of the CE and their behavior can boost or curb the proposals of the other actors in the supply chain. Here it is necessary to take into account on the one hand the needs of consumers and on the other, the value proposition of plastic food containers. The needs are determined by the information that consumers receive, by the price range and by the regulatory framework. Consumers are the starting point for the return of plastic food containers; they are the first actor to make a CE possible in the first place. Therefore, it is essential how they behave with respect to their plastics; reuse, recycle or discard. Plastic recycling begins with the reverse flow of plastics [38]. Demand, through individual purchasing choices made by consumers, can also drive a change in behavior in other actors, who need to meet the needs of their customers. In this way, the consumer will drive a change throughout the supply chain, which can result in a decrease of the amount of plastic used. The formation and dissemination of environmental culture is essential, as consumers often do not know the environmental problems caused by their consumption behavior [39]. The compensations that consumers face to commit to the CE relate to the awareness, understanding and expectations about the durability and recyclability of plastic food containers.

Waste Managers The CE pursues the creation of closed circuit waste streams. This means that plastic food containers, must be recycled so that the same product can be recreated. In this process, those

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responsible for collecting solid waste (plastics) play a strategic role. Most European cities, a source separation system is applied in which households keep their own separate empty plastic containers. However, each city can decide what kind of methodology they apply to the collection of plastic waste. Plastic recycling companies pay them for every ton of plastic they collect. The pretreatment of homes by separating their plastics, increases the quality of recycling and reduces recycling costs, since this depends on the quality of the plastic material delivered by households [49]. After of collection of the plastic waste, the next step is to recycle them. Recycling is essential to know what requirements the plastic must meet, the same represents for all parties involved in the collection and classification. The complexity in the current recycling network makes the application of the cradle principles to cradle, or the closed circuit recycling model “is almost impossible to achieve 100% [41]. The main reason is that the flows of plastic waste are contaminated by other waste (plastic), what translates into losses of value of the plastic materials to return to be transformed in plastic of in closed circuit. Another stream of waste containing plastic is municipal solid waste (MSW), which is mainly composed of organic material, paper, plastic, glass, metal and textile [20]. Plastics collected through MSW are not adequate for the recycling of closed circuit food containers, since in this flow the waste is contaminated by non-food applications, so this waste flow does not comply with European safety standards when plastic waste is mechanically recycled. The domestic separation and classification of plastic containers increase, the amount of plastics available for closed circuit recycling. The classification of plastic waste is the most important step in the recycling cycle, better communication with the other actors in the supply chain is needed, plastic waste that cannot be classified will end in incineration, which forms a barrier to a CE [42].

Drivers to a CE and Sociological Institutional Theory The willingness of the actors involved in the supply chain of the food industry helps to adopt a CE that reduces the negative environmental impacts of plastic waste derivatives. The three drivers are based on the Sociological Institutional theory. The number of rules and regulations are an operationalization of the coercive drivers. The rules and regulations directly influence corporate strategies, but also force consumers to execute a certain behavior. Normative isomorphism is divided into two aspects: stakeholder pressure and awareness raising, accounts for consumers and businesses. Governments and society pressure companies to be more legitimate in the context of sustainability [43]. It could be defined legitimation as how to do the right thing. Besides, consumers in uncertain situations are more likely to imitate high value people in their behavior. Social pressure is necessary for consumers to do the right thing. On the other hand, thanks to the promoters of the CE, organizations are adopting a successful strategy so as not to fall behind their competition.

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Barriers to a CE The objectives to create a CE are highlighted in the strategies and policies established by governments and organizations. However, there are still numerous barriers to its implementation, which must be overcome in order for the transition to the CE to be possible. Barriers inhibit certain behaviors [44]. Lozano [45, 46] related barriers to attitude and described three categories of attitude barriers; behavioral, emotional and informative. The behavioral aspect can be observed directly and it is the action of a person with respect to an idea. The tendency to behave in accordance with the principles of the CE may encounter a barrier if the behavior of organizations and/or consumers hinders the transition. On the other hand, the emotional aspect is related to the feelings and values (positive, neutral or negative) that the individual has regarding the idea or action, in this case the CE. To the extent that consumers and/or organizations are willing to change the status quo. Emotional barriers are not directly observable, but they can be translated into barriers derived from traditional values, non-rational thinking or emotional reactions contrary to the CE. Finally, the attitude barrier is informative. The informative component is the belief and information available about an idea. This refers to unclear strategies of organizations, which do not focus on sustainability and do not help raise consumer awareness. Barriers also appear due to lack of information or incompetence to obtain and process new information. Vermeulen [47] described six implications, which can create barriers. First, the economic barrier, you have to change linear routine practices and not only focus on short term gains and goals. It is also necessary that all actors implied in the supply chain, cooperate in an active way, to transition to the CE, otherwise a behavioral barrier appears [48]. The information level receive by the actor must also be taken into account, which can act as an impulse for the CE in some cases or as a barrier in others, for example when decisions are made based on incorrect or missing information. Another important barrier is the so called technical barrier, which arises when the lack of technology and investment hinders the implementation of the CE. Finally, the regulatory barrier. In this case, the lack of legislation can act as a barrier, since changes in companies could be implemented faster than the creation of a new law.

MEASUREMENT OF THE TRANSITION TO THE CIRCULAR ECONOMY: FRAMEWORKS AND INDICATORS The transition to a CE transforms the economy. According to PBL (2018), the greater the degree of circularity in the economy, the greater the environmental benefits. The CE contributes positively to climate objectives, to the preservation of world resources, creates local jobs and generates competitive advantages [49, 50]. In 2018, the EU developed a scorecard to measure the transformation towards the CE. It included ten key indicators, which measure the circularity in the different phases of the life cycle of a product. National governments play a vital role in promoting this transformation, through their investment, taxation and incentives policy.

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To measure a change, different frames can be applied. The frameworks can help companies ensure better decision making in favor of a CE [35]. The objective is to investigate which framework is the most applicable to the food industry, to create a closed circuit for plastic food packaging. Closing the cycle of plastic food containers directly influences the amount of waste generated and the reduction of the amount of virgin material resources needed to create new products. Resource efficiency is a process to deliver more, with less natural resources [49]. A European study shows that, at the country level, the efficiency of waste resources can be measured by the amount of recycled waste. With regard to the use of materials, there are the following indicators: Consumption of domestic material; direct entry of material and domestic extraction.

Cradle-to-Cradle Design Frame According to the Cradle-to-Cradle (C2C) principle, a plastic package must be recycled in a closed loop process with zero losses in material performance. McDonough and Braungart (2002) distinguish two material cycles: technical and biological. These authors argue that the containers in the C2C must to be 100% recycled if recycling cycles of technical or biological nutrients of closed cycle are performed. In the case of plastic food containers, the focus is on the technical cycle. The technical cycle means that a product, if designed correctly, can be recycled. The C2C uses five criteria: Material health, reuse of materials, renewable energy and carbon management, water management and social equity [51]. Only two indicators within the C2C framework focus on the use of plastic food packaging material, so it is necessary to complete this framework with some additional ones.

Life Cycle Assessment Framework The life cycle assessment (LCA) is part of the life cycle sustainability assessment framework (LCSA) and consists of three pillars: Environment, Social aspects and economic aspects. This framework is the most complete to analyze and evaluate the environmental impact of goods and services at each stage of the supply chain. The LCA is a quantitative tool to measure the environmental performance of a product system during its life cycle. For companies in the food industry, the LCA can be used to choose between different packaging alternatives in order to reduce the negative impact on the environment of their products. For packaging, circularity strategies are important and maintain the maximum value of materials at each step of their life cycle. For example, increase the collection rate, light, weight and waste prevention. Arena [52] perform the LCA analysis of a plastic container recycling system, with the objective of quantifying the real advantage in the recycling of plastic containers, both from an environmental and economic perspective. Ross and Evans [53] present a LCA analysis that evaluates the effects of reuse and recycling strategies of plastic containers in reducing flows to landfill. To investigate the best solution for plastic food packaging, the following question must be answered: If the disposable plastic food packaging was replaced with a single type of recycled plastic food packaging, how would be the environmental impacts be affected?

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The impact measurement categories addressed in this analysis include: energy demand, water consumption, solid waste and effects on climate change [54].

Material Circularity Indicator Framework The EMF determined the Material Circularity Indicator (MCI), which measures how well a product works in the context of the CE. This indicator analyzes four aspects, firstly the entry of material in the supply chain. Secondly both, the amount of tons of plastics entering the market, and the amount of recycled and non-recycled products that return to the market. Thirdly, there are an important number of indicators during the phase of use of the good, such as the number of minutes that it is used, before disposal. A qualitative aspect is also important here; for example, the levels of separation of plastic containers after use. Finally, the fourth indicator reflects the quantities of plastics that are directly discarded to landfill. You can also calculate the amount of plastics that re-enter the system, thus obtaining the primary recycling rate. The MCI calculates the product level and provides a value between zero and one. The higher the value, the more the degree of circularity [2]. This contributes to the increase in the reuse rate, greater utility during use, a greater amount of recycled plastic and greater efficiency in the recycling process. To measure the transition to the CE, relevant, specific and measurable indicators are needed, both quantitative (e.g., recycling percentages), and qualitative. Besides, it is important to measure the level of cooperation between supply chain actors. Apart from this, the transition to the CE could be measure in three economic levels: First, at the micro level (products, companies, consumers). Second, at the meso level (regional, eco-industrial parks) and third at the macro level (national, global and general industrial structure [55].

Quantitative Indicators Homes are the largest source of plastic waste [9]. Therefore, it is very important to classify and collect plastic containers after consumption. Thus, a first quantitative indicator is the amount of post-consumer packaging recovered. A second indicator, related to the previous one, measures the supply of places where containers can deposit their plastic food containers, that is, the amount of plastic waste delivered by the consumer. Quality directly influences the third indicator: The recycling rate of food packaging. The efficiency of the collection system can be measured in the amount of waste from food containers collected versus the amount available for collection. The fourth indicator would be the amount of plastics that re-enter the system. Recycled materials replace in that case the newly extracted resources; reduce the environmental footprint of production and consumption. In this indicator, the pressure from the demand of the food industry (recycled packaging VS not recycled) increases the amount of recycled packaging. Finally, the last indicator is about the competitiveness and innovation that are measured. This indicator includes the volume of private investments, patents related to recycling, value added and employment, related to the CE.

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Qualitative Indicators There are a number of benefits derived from the transition to the CE, which cannot be quantified numerically. For this, qualitative indicators are examined. This research proposes new qualitative indicators that measure the effect of the CE on the physical, mental and social well-being of people. They are indicators such as the quality of life of human beings, subjective well-being, and satisfaction with life, happiness and optimism. Recycling behavior increases people’s well-being. There is a significant relationship between recycling rates and the level of happiness expressed [56]. This is known as “sustainable happiness” and contributes to global well-being, without exploitation of the environment and the sustainability of the system for future generations. Another indicator is about social impact and awareness. The more companies and people involved in the CE, the more positive its effect on the environment. Collaboration along the value chain of plastic food containers is important to increase the quality of PET recycled food containers. By adopting the CE, it can give the feeling of active participation in the society in which they live. The feeling that individual behavior is important; Inclusivity is also important. The more actor’s tare integrated in the CE, the faster and bigger is the movement towards a more sustainable food industry will be.

CONCLUSIONS To summarize, the design of plastic package must be based on the CE principle, using the C2C and LCA frameworks. Besides, the use of plastic must be compared with other package options, keeping into consideration the environmental effects of it use. The implementation of a long term CE will depend on the perception that consumers have of benefit. In addition, thanks to the awareness created, the CE can contribute to a better quality of life because there will be less plastic pollution. Daily exposure to plastic waste in landfills and/or oceans influences the experience of life. The global problem of plastic pollution can be experienced as a risk. Environmental risk can jeopardize the physical security of an individual, making people feel less secure on earth, which can damage perceived well-being. When creating a CE, a possible solution is founded for an urgent problem. This can make people feel more optimistic about the future. Finally, the circularity of the plastic food container industry can be evaluate the application of the MCI.

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In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 15

BIOCONVERTER INSECTS: A GOOD EXAMPLE OF CIRCULAR ECONOMY, THE STUDY CASE OF HERMETIA ILLUCENS Rosanna Salvia and Patrizia Falabella Department of Sciences, University of Basilicata, Potenza, Italy

ABSTRACT The production cycle based on extraction, transformation, production, consumption and waste has not been sustainable for years. The goal is to have production cycles capable of self-regeneration, and therefore to identify a new way of managing byproducts is needed, one that would turn them into a resource. In the production cycle of the food industry, losses and waste account for about 1,3 billion of tons a year, and thus around 1/3 of world production for human consumption. Insects can represent a valid solution to the reuse and valorization of food industry by-products. In environmental and economic fields, an innovative application is offered by the capacity of some insects to bioconvert waste material into valuable products. Bioconverter insects can valorize organic waste from the agrifood industry through bioconversion. This process allows to obtain numerous products of high biological and economic value: proteins and lipids of animal origin, chitin and residues from the bioconversion process (frass of insect and partially digested organic material, rich in in uric acid and chitin, comparable to soil conditioner for agriculture and therefore usable for crop fertilization). Proteins and lipids deriving from some insect species could be used for feed production, and lipids can be exploited for the production of biodiesel or could find application in cosmetics field. Moreover, insect’s chitin and its derivative chitosan can find many possible applications in agricultural, biomedical, pharmaceutical and industrial fields as well as in wastewater treatment. The breeding of insects for animal feed and as an alternative source of energy could represent one of the solutions to be adopted in the future. To date, in Europe the larval biomass obtained from bioconversion process can be marketed for the feeding of game animals, reptiles, fur animals and other insectivorous species (EU Reg. 68/2013, EU Reg. 142/2011); they can also be 

Corresponding Author’s Email: [email protected].

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Rosanna Salvia and Patrizia Falabella transformed into processed animal proteins (PAP) and then in flours with high nutritional content, to replace or supplement the protein and lipid quotas present in conventional feeds. The specific conditions of processing, production, storage, transport and use of insect flour for aquaculture (fish farming) has been governed by the European Regulation 2017/893 that allows the use of proteins for fish feed derived only from seven species, including the dipteran Hermetia illlucens. In the present paper, we describe the sustainable use of H. illucens to bioconvert agrifood by-products and produce proteins, lipids, chitin and its derivatives; furthermore, we shall outline their applications in the view of a zero-waste circular economy.

Keywords: circular economy, insects, Hermetia illucens, bioconversion process, proteins, lipids, chitin

1. INTRODUCTION In recent times we have heard more and more about circular economy. The United Nations 2030 Agenda for Sustainable Development and the Paris Agreement on Climate Change, both adopted in 2015, represent fundamental contributions to guide the transition towards an economic model of development that aims to social progress and environmental protection. In this context, a crucial aspect is a most rational and sustainable management of natural resources for which it is necessary to implement a transition from the linear model of economy based on extraction, transformation, production, consumption and waste to the circular model which aims to recycle and reuse products by extending their life cycle, valorizing them and helping to reduce waste. Food losses and food waste (FLW) have become a global concern in recent years: one third of the annual food produced in the world for human consumption, approximately 1.3 billion tons, gets lost or wasted [1]. Food waste is synonymous with waste of resources, primarily water resources but also energy, labor and capital; furthermore, it produces excessive greenhouse gas emissions, and contributes to climate change. For instance, FAO [2] estimates that FLW generate more than 3.3 gigatons of CO2 equivalent/year. Food waste is the biggest paradox of our time if one considers our need to increase food production by 60-70% to feed an ever growing population. By 2050 the world population will reach 10 billions and the nutritional needs will require to produce at least 800 million tons of proteins [1]. Currently, about 3.73 billion hectares, almost 75% of the planet land, is dedicated to livestock grazing [3], and the demand for meat is expected to grow 58% by 2050 [4]. The real challenge of the 21st century will be to produce animal protein from sustainable sources. Current sources, consisting in particular of cattle farms, are neither sustainable from an ecological point of view, as they are responsible for the increase in greenhouse gas emissions during the entire production cycle, nor from an economic point of view due to the enormous use of water. Moreover, to date the worldwide growing demand for protein sources to breed omnivorous and carnivorous farm animals can no longer be satisfied by intensive fishing to produce high-protein fishmeal, nor by intensive use of agricultural land for protein crops. Indeed, fishmeal for animal nutrition is commonly replaced with other sources of

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proteins, such as soy, but the substitution is not acceptable, due to the lower protein digestibility and less valuable amino acid content [5]. It is thus necessary to replace the current protein sources, consisting mainly of fishmeal, with new sustainable protein sources, and insects offer the solution. Insect proteins can play an important role in the progressive substitution of soy and fishmeal proteins, commonly used to feed animals, and, in country where it is allowed, as novel food for human nutrition [6]. The greatest advantage of insect breeding is the lower environmental impact: less greenhouse gas emissions than any other conventional animal farming, and lower water footprint per gram of produced protein [6]. Moreover, some insect species offer a great opportunity to valorize agrifood by-products, since they are able to grow on different types of organic waste and bioconvert them in larval biomass; such biomass is a good source of protein and fat, and may be applied to both animal feed and human food, but also to industrial, pharmaceutical, or energy purposes, fully embracing the concept of circular economy (Figure 1).

Figure 1. Schematic representation of a circular economic model based on bioconverter insects reared on agrifood by-products. Larvae at the end of the bioconversion process can be used for the production of feed for acquaculture and poultry.

2. FROM AGRIFOOD BY-PRODUCTS TO NOVEL FEED AND FOOD: A PROCESS MEDIATED BY BIOCONVERTER INSECTS 2.1. Bioconverter Insects With over a million species described, insects represent the largest group in the animal kingdom. Thanks to their high biodiversity, subjected to evolution for millions of years, insects have developed the ability to adapt and survive even in hostile environments.

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Bioconverter insects are those species capable of growing on decaying organic substrates. During larval stages these species can convert inedible decaying organic substrates of low biological value into valuable biomass, and represent an opportunity to reduce the 1.3 billion tons of food that is wasted every year [7, 8]. At present, only few species are used for bioconversion of organic wastes, they include crickets, locusts Locusta migratoria, black soldier flies Hermetia illucens, green bottle flies Lucilia sericata, the codling moth Cydia pomonella, and several mealworm species, including the yellow mealworms Tenebrio molitor [7, 9, 10, 11]. The countries in which they are most used for bioconversion processes are China, USA, Canada, Cambodia, Sweden and Indonesia. They are reared on different substrates from decaying fruits and vegetables, peels of yam, spent coffee, spent grain and restaurant waste. Table 1. Bioconverter insects and their corresponding bioconversion outputs [11] Species Black soldier fly (Hermetia illucens)

Housefly (Musca domestica)

Codling moth (Cydia pomonella) Cambodian field crickets (Teleogryllus testaceus) Yellow mealworm (Tenebrio molitor)

Organic waste Rice straw (30%) Restaurant waste (70%) Rice straw Coffee pulp, husk Reject material from pears, banana, and cucumber (5:3:2) Spent distiller grain Fruits and vegetables Corn stover Corncob Sorghum Cowpea Cassava peel Vegetable trimmings, spent coffee grounds, and tea leaves Vegetables, peels of yam, cassava, plantain Restaurant waste (70%) Whole plant corn silage, sawdust (30%) Starch and cheese wastewater sludge Cassava plant tops, spent grain, mung bean sprout waste, field weeds Wheat straw, bruised cabbage leaves Corn stover

Country

Bioconversion output

China Indonesia El Salvador, Indonesia Sweden

Biofuel Biomass Biomass, fertilizer Biomass

USA Canada China China USA USA Indonesia USA, Hong Kong

Biomass Biomass Biofuel, soil amendment Biofuel Biomass Biomass Biomass Biomass

Ghana

Biomass

China Canada

Biomass, biofuel, fertilizer Biomass

Cambodia

Biomass

China

Biomass

China

Biofuel

Insects have a high food conversion efficiency; on average, they can convert 2 kg of feed into 1 kg of mass, while a cattle needs 8 kg of feed to produce the increase of 1 kg of body weight [10]: for example the production of 1 kg of crickets requires 1.7 kg of feed [12]. Another important aspect is the food bioconversion index as efficiency of food transformation into optimal body weight. It has been estimated that domestic crickets are able to convert more than 90% of ingested food into body mass, making it twice as efficient as chicken, at least four times more than pig and twelve times more than cattle. The bioconversion processes can be optimized in controlled conditions, such as temperature and humidity so to

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favor a faster fitness in bioconverting insects. In this way industrial insect rearing can efficiently turn many tons of food waste feedstock into valuable products. Some species of scavengers are extremely suitable for this purpose because they can be bredwith agrifood by-products from various production chains, transforming waste into a source of protein and other organic molecules. Among the species one may considered of extraordinary interest for the production of feed, H. illucens. The larval stages are extremely voracious (they consume a quantity of food substrate equal to twice their weight on a daily basis) and can grow on different organic waste, including food industry and agricultural processed waste, zootechnical waste, urban wet waste [13, 14, 15, 16, 17]. It has also been shown that larvae fed on manure are able to modify the substrates’ microflora, and thus to reduce the charge of bacteria, such as Escherichia coli and Salmonella enterica [18]: this is related to the ability of H. illucens to produce antimicrobial peptides that are particularly effective against different bacterial strains [19] Numerous studies have shown that the flour obtained from this insect’s prepupal stage has a high content of proteins with an equally high nutritional value, if compared to that present in fishmeal [19]. These flours have been used as raw material for the production of feed for different animals’ breeding (chickens, pigs, rainbow trout, catfish, tilapia and salmon) with satisfactory results [19]. In the case of the feed used for aquaculture, quite encouraging data are reported since, replacing fishmeal with different percentages (25, 50 and 100%) of H. illucens’ flours, the farmed species showed good growth performance and no variation in the histological indices or in the fillet quality [19].

2.2. Regulations Insect consumption by humans has always been a worldwide practice, and the nutritional value of insects has been widely recognized since WHO considers insects as a suitable food to meet the protein needs of starving individuals [20]. Yet, the regulatory framework governing the use of insects for human consumption and for the production of feed are still largely absent. In developed countries, the absence of clear laws and regulations to guide the use of insects as food and feed is one of the main limiting factors that hinder the production of insects for food and feed at industrial scale. In developing countries, the use of insects for human or animal consumption is a widespread practice. Interest is growing in the potential benefits of using insects in food and animal feed, but it is necessary to evaluate the risks in potential biological and chemical hazards as well as allergenicity and environmental dangers associated with the use of farmed insects as food and feed. For this reason the European Food Standards Agency (EFSA) has published the “opinion on the risk profile of insects as food and feed” [21], pointing out that lack of knowledge related to possible hazards and notes that there are not systematically collected data on animal and human consumption of insects. Moreover, EFSA highlights how it is important to take into account the entire chain, from farming to the final product. However, EFSA concludes by making a recommendation in favor of further studies. On January 1st, 2018, EU Regulation 2283/2015 [22] relating to the novel food (including insect consumption) came into force. An innovative aspect of such regulation is the introduction of insect’s consumption for human use (food), as well as the use of insects as a protein source in animal feed. However, for the sole purpose of food use, insects and their

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derivatives are configured as ‘novel food’, and at present no species of insect (or its derivative) are authorized as food. With reference to article 35 of Regulation (EU) 2283/2015 [22] on "Transitional measures," it should be clarified that some Member States have authorized the marketing of some insect species at a national level under a "tolerance" regime. Moreover, the EU regulation 893/2018 allow the use of only seven insect species (Hermetia illucens, Musca domestica, Tenebrio molitor, Alphitobius diaperinus, Acheta domesticus, Gryllodes sigillatus, Gryllus assimilis) for the production of PAP (Porcessed Animal Protein) for acquaculture, as long as they are raised on agrifood by-products, while insect meal as feed for pigs and poultry remains prohibited [23].

3. THE DIPTERAN HERMETIA ILLUCENS EMBRACES THE CONCEPT OF CIRCULAR ECONOMY 3.1. Hermetia Illucens’ Etology Hermetia illucens (L.) (Diptera: Stratiomyidae), also known as Black Soldier Fly (BSF), is a non-pest insect distributed throughout warm temperate regions and the tropics [24]. The family Stratiomyidae contains 260 known species, and in the southeastern United States it is abundant during late spring and early fall, and develops three generations per year in Georgia [25]. As most holometabolous insects, its life cycle is divided into four phases: egg, larva (5 or 6 larval stages), pupa and adult (Figure 2).

Figure 2. H. illucens’ stages of development, from left eggs, larvae, pupae and adult fly.

Adults mate 48 hours after flickering and the eggs are laid within a few days in the proximity of the larval habitat, and therefore in the presence of preferably decomposing organic substrates [26]. Under appropriate conditions (temperature of 27-30°C and food substrate humidity up to 60%), the larvae reach the prepupa phase in 15-20 days. The only BSF larvae activity is eating: they feed decaying organic material and, after they are ready to pupate, move to a dry and hidden area to go through transformation [27]. BSF, unlike other Diptera such as Musca domestica (L.) (Diptera: Muscidae), Calliphora vomitoria (L.) (Diptera: Calliphoridae) or Chrysomya spp. (Robineau-Desvoidy) (Diptera: Calliphoridae), is a non-pest fly, because even if larvae fed on decomposing organic matter, adult fly does not take up any of such food: they can survive with reserves collected during larval stages [28]. Males try to find spots in the lekking area when it is time to mate, and females do not mate

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with males that have no territory on which to mate [29]. H. illucens is not extremely competitive, and, if another male comes in the area, the two fight only if a female is coming and the winner takes the territory [29, 30]. After mating, females lay their eggs on cracks and crevices [31]. Light affects mating because direct sunlight fosters it, in fact, H. illucens does not mate on rainy or snowy days because the light level is low [31]. After larval stage, they reach the prepupal stage, which is the last larval stage before pupating. As prepupae, they turn black from releasing melanin that increases skin durability [32]. At all stages, the black soldier fly can live in a range of temperatures between 27-30°C. After oviposition, the eggs take about 3-4 days at 27°C to hatch; the larval stage and the pupal stage take two weeks each, but this time may increase to four months in cases of limited resources [33]. A particular characteristic of BSF is that it is no pest- insect, since, for example, it is able to control the proliferation of Musca domestica, both by subtracting food resources and by emitting short-lived interspecific chemical signals [33, 34, 35]. Moreover, the adult fly is not equipped with a mouth parts, and it is thus unable to feed or bite: consequently, it cannot be a vector of diseases.

3.2. Bioconversion Mediated by Hermetia Illucens The black soldier fly (BSF) is a saprophagous insect, and has become one of the most important insects in the world for bioconversion of organic wastes. It can be considered a scavenger of organic matter: females oviposit on or near decaying organic substrates, and after hatching, the larvae feed until the prepupal stage. They are able to feed on a wide variety of decomposing organic material, both of animal and vegetable origin [14], such as manure [34, 36], waste from agrifood chain [37, 38], distiller grains [39, 40] and many others [37]. Environmental conditions and substrate characteristics are very important for efficient bioconversion. The optimal moisture content of substrate is about 60% [13], and optimal temperatures range from 27° to 32°C [29, 41]. Under the rearing conditions of 28°C and 75% RH, the total larval cycle lasts 20–35 days [42]. During lsuch stage, larvae can feed on different decomposing substrates and can reduce the dry matter by 50 – 80%; then, they convert up to 20% into larval biomass within 14 days [42, 43, 44]. In addition to reducing decomposing organic substances, BSF larvae can also reduce Escherichia coli and Salmonella enterica in both chicken and cattle manure [18, 45], and human faeces [46]. This is related to the production of those antimicrobial peptides (AMPs) that are particularly effective against different bacterial strains [19]. Antimicrobial peptides are some of the key components of the humoral innate response. One of the most important features of BSF larvae is the ability to bio-convert large quantities of organic substrates in products of high biological and commercial value in a relatively short time corresponding to their life cycle. While they are eating, larval biomass increases considerably in comparison to the newly-born larva, increasing their biomass by 600 times. The weight gained, the larvae’s nutritional composition, and the reduction of organic waste are strictly linked to the substrate [37, 47, 48, 49, 50, 51, 52, 53]. Spranghers et al. (2017) [54] found that rearing H. illucens larvae on vegetable waste could provide a high-quality resource with a strong potential for incorporation in animal feed. It has been demonstrated that crude protein content and amino acid profile is not substrate dependent, while fat and ash contents appear to be on the rearing substrate. In fact, when larvae are reared on energy dense substrates, they turn into prepupae

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with a high fat content, which is most rich in medium chain fatty acids, and may provide them with an added value in comparison to conventional feed resources [54]. On a different note, Nguyen et al. [37, 55] found a great change in protein and fat acid content, depending on diversified organic substrate on which larvae feed. Nutritional analysis revealed that different dietary treatments (mix of fruit and vegetables (1:1), liver, fish, manure and kitchen waste) affects the chemical composition of BSF prepupae: the fish-based diet increases the total fat content and affects the fatty acid composition of prepupae,: such process results in a high percentage of long and medium chain saturated fatty acids (e.g., lauric, myristic and palmitic acids). Protein content also was affected, indeed larvae feed on kitchen waste and on liver, shows protein amounts significantly higher than larvae feed on other diet Finally, larvae fed on manure and fruit and vegetables-based diets have the lowest fatty acid and protein contents. All these findings put in evidence how important the characteristics of original organic substrate and the different life cycle stages are, in order to define the best bioconversion ratio and the best quality of H. illucens larvae, prepupae and pupae. Nowadays BSF is considered as a potential environmentally sustainable nutritional alternative to conventional livestock, poultry and aquaculture feed, since the dietary values are comparable to classical fish and soybean meals [51, 56]. Consequently, studies need to enhance the knowledge of the H. illucens nutrient aspects, and take in consideration the future usage of insects as an alternative green, environmentally friendly and sustainable source of food for human diet. In addition to larval biomass, the bioconversion process also provides high quality secondary products: at the end of the process, in fact, the bioconversion residue, made of frass and not converted organic matter, is comparable to organic fertilizer. It shows a great potential for improving soil fertility and therefore it is suitable for crop fertilization, as a valid alternative to chemical fertilizers [46, 57]. Moreover, the bioconversion process also provides other high-quality secondary products, such as chitin and its derivative chitosan and lipids [55, 58, 59, 60]. It is important, accordingly to the EU regulations reported above, [22, 23], that H. illucens must be bred on agrifood by-products to be used in the production of feed of high biological value.

3.3. Hermetia Illucens, a Sustainable Source of Molecules of High Economic and Biological Value: Proteins, Lipids and Chitin 3.3.1. Why Insect Proteins? Hermetia Illucens, One of the Most Source The production of animal feed protein is at the heart of the activities of numerous companies that have been founded all over the world, including AgriProtein Technologies (South Africa), Enterra Feed Corporation (Canada), Protix (Holland), Unique (China). Moreover, many small companies and innovative start-ups are also springing up since the breeding of bioconverter insects is increasingly considered a booming business, e.g., Blue Protein (Marocco), Entocycle Ltd (UK), Goterra (Australia), Grubbly Farms (USA), Magalarva (Indonesia), Onto (bio-onto.ru) (Russia) Ynsect (France), XFLIES (Italy) and many others. The presence of all essential amino acids makes the flour derived from the larvae of Hermetia illucens similar to fishmeal, and this is of great interest to fish feed manufacturers,

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since they are constantly looking for alternative, sustainable and quality sources. Carnivorous fish require a diet that contains at least 45% protein while for herbivorous ones the minimum required protein content varies between 15% and 30% [61]. For rainbow trouts, for example, the optimal protein content should be 35% [62]. Aquaculture requires large quantities of fishmeal, and in order to produce them, more than 20 million tons of small fish are caught each year, in addition to 60-65 million tons of fish and seafood earmarked for human consumption. The continuous depletion of the seas and the high costs of fishmeal have led to consider possible alternative and innovative solutions, such as the use of H. illucens. In fact, for some years now, in Europe, feeds whose fishmeal content has been partially or completely replaced by the flour obtained from H. illucens larvae have been tested. St Hilaire et al. (2007) [16] fed rainbow trout with diets in which from 25% to 50% of fishmeal (normally present in them) was replaced by flours or fats from H. illucens, and the control groups did not register differences in weight gain. Sealey et al. (2011) [63] reared H. illucens larvae on substrates enriched with fish processing waste, and concluded that the flours obtained from these larvae can replace up to 50% of fishmeal in trout’s diet without affecting its growth. In an Atlantic salmon farm, Lock et al. (2014) [64] replaced up to 25% of fishmeal with the flour obtained from H. illucens, without negative consequences on performances. In a study on sole, up to 33% of defatted larvae of H. illucens were included in the diet with no effects on palatability and growth [65]. The larvae of H. illucens could also be used for feed of chickens and pigs. Poultry, for example, needs feed with 18% to 20% crude protein content [66]. BSF wholemeal flour has already been used as a component of complete diets for poultry, swine, and several commercial species of fish [66], since they were found to support good growth: it was generally concluded that BSF larvae can be a suitable protein source for animal feed. Generally speaking, insects, but even more H. illucens contain high amounts of the essential amino acids, lysine, threonine and methionine, which are limiting amino acids in low-protein cereal- and legume-based diets for pigs and poultry [6, 66]. The protein content and quality of H. illucens prepupae, reared on different substrates, make in prepupae reared on the black soldier fly could an interesting protein source for animal feeds.

3.3.2. Characterization and Applications of Insect Lipids: Hermetia Illucens as an Interesting Source The possibility of extracting lipids and producing biodiesel from larval biomass represents a good alternative to the use of classical raw materials such as starch, vegetable oils (oilseed rape, sunflower or others) or animal lipids [36]. The use of such resources as well as that of agricultural soil for fuel production, rather than for food industry, appears to be currently unsustainable. Indeed, since, at the end of its life cycle larval biomass is composed of up to 39% of saturated and unsaturated fatty acids, it can be used for high quality biodiesel. The properties of this biodiesel (density, viscosity, flash point and Cetane index) fit in the recommended range of international standards (https://dieselnet.com/tech/fuel_biodiesel_ std.php). A study conducted by Surendra et al. [7], on larvae fed on a mix of organic waste, showed that in the BSF prepupae oil the concentration of medium chain saturated fatty acids (C12:0 ‒ C16:0) (67% of total fatty acids) was higher when compared to soybean (11% of total fatty acids) and palm oil (37% of total fatty acids); furthermore, the concentration of unsaturated fatty acids (28% of total fatty acids) was lower than in soybean oil (85%) and

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palm oil (55%) [7]. These characteristics have a great impact on the quality of the biodiesel produced [67]; high concentrations of long chain saturated fatty acids turn into biodiesel with poor cold flow property. Moreover, biodiesel derived from oil that is rich in polyunsaturated fatty acids has poor oxidative stability, and this decreases storability [67]. For these reasons, the high concentration of medium chain saturated fatty acids and the low concentration of the polyunsaturated fatty acids makes the biodiesel derived from H. illucens prepupae a good source for high quality biodiesel [7]. Another application of insect lipids, and in particular of fats deriving from H. illucens, is in the field of cosmetics. Triglycerides typically act as emollients that soften the skin [68]. Indirectly, they also moisturize the skin by reducing the transepidermal water loss [69]. The properties of the fats can vary in relation to the fatty acid profile, and the healing (e.g., using linoleic acid for dry skin) or skin-protective functions of the creams can be enhanced. The fats are also used in cream formulations for their emulsifying properties [70]. Among the valuable fatty acids that are part of the lipid component extracted from the larvae of H. illucens, one of the most abundant is lauric acid [53, 71, 72, 73]. Such acid, extracted traditionally from matrices of vegetable origin (palm seed oil), is commercially used as a primary component for many personal care products (soaps, detergents, shampoos) because of its antimicrobial properties [75, 76, 77, 78]. Moreover, the qualitative fatty acid composition of lipids in H. illucens larvae can be modified according to the different food substrate [54, 71].

3.3.3. Insects, an Innovative Source of Chitin, and Hermetia Illucens as One of the Most Promising Sources Chitin is one of the most abundant biopolymer in nature. It was isolated for the first time in 1811 from fungi by the French professor Henri Braconnot and named fungine [79]. Subsequently, in 1823, Antoine Odier modified the name in chitin a polysaccharide composed by chains of the monosaccharide, N‐acetylglucosamine. Chitin can be considered ubiquitously present on earth and to date the estimated annual production is about 28.000 tons [80, 81]. It is an important component of diverse solid structures, such as exoskeletons of arthropods, the cell walls of fungi and at least 19 phyla in animal kingdom as well as in bacteria, such as fungi, yeast and algae [82]. Multi paralleled-organized chains form chitin sheets [83] that, when located next to each other, interact [84] and form highly crystalline fibers. Based on chitin sheet orientation, three crystalline allomorphic forms are reported: α-, β-, and γ-chitin. α‐chitin is the most abundant form [84] and is commonly found in insects, crustaceans, fungi, and yeast cell walls [85]. It presents the sheets (each composed of parallel chitin chains) arranged in antiparallel way, and this maximizes the number of hydrogen bonds that give a very high crystalline structure; as consequence, it is characterized by a remarkably high stability and rigidity, and thus resulting in an insoluble product [86]. In β‐chitin sheets are positioned in a parallel way with a reduced number of hydrogen bonds. For this reason, β‐chitin is a more soluble and less stiff material [85, 87]. Finally, γ‐chitin can be considered a mixture of α‐ and β‐chitin, with sheets granted parallel and antiparallel arrangements, and combining the properties of both α- and β-form [86, 87, 88]. Chitin and its derivatives, generally obtained through deacetylation processes such as chitosan, have many important properties, such as no-toxicity, biodegradability, heavy metal absorption capacity and antimicrobial ones [89, 90]. Both chitin and chitosan have been used for some time in several different biomedical applications, such as drug delivery, wound

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dressing, antibacterial coating and tissue engineering [90, 91]. Chitin and chitosan have the ability to stimulate plants’ natural defense systems, and for this reason they are used in agriculture as well [92]. A very interesting application is the production of biopolymeric films for food packaging to contain the microbial contamination and growth, extending the fresh food shelf life [93]. It is easily deductible how the economic value of these biopolymers new bio-compatible and very versatile functional of natural origin is strongly growing, and how the market interest is increasingly relevant [82, 84]. In nature, a large part of chitin derives from aquatic species [82, 94, 95, 96, 97, 98, 99, 100, 101], but the most accessible sources are found in the exoskeleton of several species of the Phylum Artropoda. Nowadays the most part of chitin distributed on the markets is obtained by waste deriving from the marine food industry, and mainly from the exoskeleton of crustaceans [102] (shrimp, krill, crab, and lobster) [94, 103, 104, 105]. The consequences of using mainly aquatic species as a source of chitin have strong ecological and social implications due to very high CO2 emissions, associated to transport from the coastal regions, where the raw material is available, to the mainland, as well as to the depletion of aquatic species in the oceans, with the consequent alteration of the delicate balance in marine environments [106]. Moreover, crustacean exoskeleton as main source of chitin is subject to seasonality, and crustaceans farming is not environmentally friendly [97]. Furthermore, the methods generally used to extract chitin from the waste produced in the fishing industry is not very efficient since the yields are rather low (chitin about 6%, chitosan 2.5%). For all these reasons, sustainability of chitin and chitosan from marine biomass must be considered a serious problem [106]. Insects exoskeleton represent a very interesting alternative and rich source. The composition of insect’s exoskeleton is different from the crustacean one. Indeed, insects’ cuticules are rich in catecholamines, proteins, lipids, lipo-proteins and minerals. Chitins are crosslinked with proteins, lipo-proteins and catecholamines by o‐quinones derived from tyrosine metabolism [107]. Insects’ exoskeletons contain mainly α‐Chitin responsible as well as in crustaceans, for the particularly resistant cuticle structure able to protect them against chemical, physical damages and working as the first barrier of insect immunity against the pathogen entry [107]. The content of chitin in insects is significantly different in the different stages of development and among different species [108]. Although the percentage of chitin content in the exoskeleton of crustaceans (20-31%) and insects (10-36%) is very similar, the extraction of chitin from insects is receiving increasing attention, since they represent a promising and novel source. Insects as a source of chitin show several advantages, such as the ease and cheapness of their breeding, due to their prolificity, fruitfulness, shortness of the biological cycle, the adaptation to different food substrates, including, for some detritivorous and saprophic species, waste products [109]. Moreover, chitin extracted from insects could overcome the potential allergenicity of products derived from crustaceans. To date there is a still reduced commercial interest regarding insects as a source of chitin, and this is due to the low accumulation of residue derived from insect differently from crustaceans. The recent interest in using insect species able to bioconvert agricultural residues to obtain protein and lipid for sustainable pet food and feed, has greatly increased the breeding of these insect species.

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Among them, Hermetia illucens (Black Soldier Fly; BSF) is considered very attractive for its ability to bioconvert organic by-products [110] deriving from the agri-food industry. Indeed, bioconversion transforms low economic and biological value substrates, in products of high biological and economic value. Generally, the larvae are utilized for the production of protein and lipid. Pupae and adults, essential to obtain eggs and then larvae in a complete life cycle, can be considered a kind of waste in massive rearing. In other words, chitin contained in the exoskeleton of pupae and adult flies constitutes the only by-product of the process that aims to produce animal feed (i.e., insect flours).

CONCLUSION Insects are often viewed with prejudice as something harmful and to be eliminated, but this is not always true, if we think about the many ecological services insects offer, thus allowing human survival. First come, the pollinating insects of plants: indeed, it is estimated that around 100,000 pollinating species have been identified and almost 98% are insects [111]. Furthermore, insects improve soil fertility through the bioconversion of waste. Cockroaches, larvae, flies, ants and termites clean up dead plant matter, breaking down organic substance until it can be consumed by fungi and bacteria. In this way, minerals and nutrients become available for absorption by plants. Furthermore, parasitoid insects carry out a natural biocontrol for phytophagous species, balancing these harmful species below the threshold of economic damage, thus reducing the use of pesticides. It must also be noted how precious bees are for the production of honey, propolis, royal jelly or silkworms which produce more than 90,000 tons of silk [111]. Insects are also applied in medical fields such as maggot therapy. Moreover, they represent a source of molecules, such as antimicrobial peptides or chitosan, and represent a source of inspiration in biomimicry [10, 110]. A demanding challenge for the future will be to meet the food demands of a constantly growing world population, and to make the best and sustainable use of resources, such as arable land and water, while limiting environmental pollution. In order to meet the growing demand for food, it is necessary to increase the production of feed for animal breeding and face the serious problem of the disposal of food waste: one third of the product of the world agrifood chain is now lost or eliminated as waste. These crucial challenges require innovative solutions and strategies aimed at finding new food resources, creating new production and consumption cycles, and designing new systems for the treatment, recycling and disposal of waste. Insects represent a potential source of animal protein for feed production and, at the same time, a solution for the reduction of organic waste that can be biotransformed into proteins with high nutritional content. Therefore, the possibility of breeding bioconverter insects on agrifood by-products represents a great opportunity for innovative modern entrepreneurs. Nevertheless, two challenges remain: the increased market and consumer acceptance and the updating of legislation. However, given these considerable potentials, scientific research in the field of basic and applied entomology, biology, nutrition sciences, animal production and aquaculture can provide a solid knowledge base from which it will be possible to develop new industrial processes of high technological content and contribute contributing to the development of a circular economy system.

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CONFLICT OF INTEREST The authors declare that there is no conflict of interest.

ACKNOWLEDGMENT We thank Prof. Manuela Gieri for the English editing.

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In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 16

CHITIN AND LIGNIN WASTE IN THE CIRCULAR ECONOMY Pierfrancesco Morganti1,2,, Alessandro Vannozzi3, Adnan Memic4 and Maria-Beatrice Coltelli5 1Academy

of History of Health Care Art, Rome, Italy Medical University, Shenyang, China 3National Interuniversity Consortium of Materials Science and Technology (INSTM), research unit of University of Pisa, Italy 4Center of Nanotechnology, King Abdul Azuz, University of Jeddah, Saudy Arabia 5Department of Civil and Industrial Engineering, University of Pisa, Italy 2China

ABSTRACT Food and packaging waste, produced by food industries and consumers, cause an increasing pollution if not correctly managed. Recycling opportunities must be exploited to maintain our health and wellbeing, preserving the planet’ natural raw materials and biodiversity for the future generations. Thus, the necessity to transform the linear economy, cause of people inequality and waste, in a circular economy based on economic prosperity, cultural vitality, social equity and environmental sustainability. For a sustainable community development, it will be necessary to recycle the industrial and agricultural waste and redesign and manufacture new products taking into account their end of life management and considering, through Life Cycle Assessment investigations, to maintain a low consume of energy and water. Among the different waste materials recovered worldwide, chitin and lignin, obtainable from food and agroforestry by-products respectively, represent the greatest source of natural raw materials available at low cost and underutilized. By many studies it has been shown that both chitin, lignin and the relative complexes, may be electro-spun with other natural polysaccharides to obtain antibacterial, immunomodulant, antioxidant and skin-repairing non-woven tissues. These



Corresponding Author’s Email: [email protected].

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Pierfrancesco Morganti, Alessandro Vannozzi, Adnan Memic et al. innovative tissues, embedded by selected active ingredients, may be used to make facial beauty masks and/or advanced medications.

Keywords: food waste, plastic waste, pollution packaging, cosmetics, chitin nanofibrils, lignin, beauty masks, advanced medications, circular economy

INTRODUCTION The worldwide food and plastic waste represent actually an important problem for humans and the environment. According to the Waste and Resources Action Program (WRAP) [1] only 12% of food waste (i.e., ~1.3 billion/tons/year) and 14% of plastic waste packaging (i.e., ~ 275 million tons in 2010) is currently recycled each year with 40% going to landfill, and 32% dumped in the environment and oceans [2, 3]. This waste is considered a hazardous material for the human health and source of pollution for the environment. On the contrary if the food waste is recycled and reused, its extract content in bio-active ingredients, may be used in the medical and cosmetic fields, utilizing their health promoting properties [4]. This is the case, for example, of vitamin C, E, A and other vitamins which, together with many micro ingredients, may be recovered from vegetable and fruits waste.

Figure 1. Secondary metabolites for the plant regrowth and defense (by courtesy of prof. Susan Murch [8]).

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Moreover, some ingredients, such as chitin and lignin obtained from waste materials, could be used in agriculture as eco-friendly compounds active as plant growth factors or biopesticides [5]. Many of the plant metabolites, such as for example melatonin, are not only directly involved in plant growth but result also essential for its environment adaptation (Figure 1). They, in fact, provide defense mechanisms for the plant survival, such as the prevention of antimicrobial activity, insecticidal activity and UV protection [6-8]. Alternatively, many plant metabolites, such as melatonin, chitoolisaccharides, and chitin nanofibrils obtained by innovative biotechnological methods, play a major role as active ingredients in human medicine and in the cosmetic fields [9, 10]. On the other hand, as also reported in other chapters of this book, plastics is actually a great source of environmental concern [2, 3]. Of about 280 million tons of plastic produced globally each year, in fact, only a very small part is recycled. Thus according to the Food and Agriculture Organization of the United Nations (FAO), food wastage, representing economically a loss equivalent to the GDP of Switzerland, has to be reduced during all its production, distribution and retailing chain and successively recycled [11]. Thus the necessity to reviewing how plastic and food waste may be managed, safeguarding their economical values and obtaining benefits for the worldwide community. In this contest waste has to be considered a business opportunity and a richness for a new economy that, looking to a sustainable development, has to be based on social, environmental and economic requirements integration [12]. At this purpose it is to underline that currently, by innovative technologies, it is possible, for example to sort from municipal waste and recycle the poly(ethylene terephthalate) (PET) used for drinking bottles and plastic food jars [13]. By this technology it is possible to draw a line between the different polymers through a mechanical treatment process, necessary to separate plastic from non-plastic products, and then separate chemically the mixed PET into different polymers, removing any impurity and contaminant by an efficiency of 95% and more. The obtained PET has the same physicochemical characteristics of the virgin one, but considered unfoundedly of inferior quality [13]. Several methodologies were investigated for controlling recycled PET melt viscosity for optimizing its processing [14-15] and recycled PET is currently used in textile, packaging and in toughened blends [16-17], obtained thanks to properly selected compatibilization methodologies [18-20]. These latter can be used in household appliances, shopping carts [21] and many other applications [22] (Figure 2).

Figure 2. Some prototypes based on post-consumer PET blends [16]: (a) thermoformable sheet; (b) vacuum cleaner; (3) DUST-CART, the sweeper robot [22].

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Unfortunately, the use of these methodologies for fossil based post-consumer materials is not yet widely diffused although it could result environmentally and commercially useful as part of the circular economy. In the meanwhile, much interest for biobased and compostable materials is arisen, for using them in applications with a short life cycle, like packaging or personal care applications [23], where the recycling seems not easy. Natural polymers, coming from waste, can be thus utilized in several applications. As previously reported, chitin and lignin, extracted from agrofood waste and accounting for about 300 billion tons per year, may be considered an interesting natural source of polysaccharides, actually used for no more than 20% [24]. Thus the industrial interest to use this underutilized waste for preserving the natural raw materials for the future generations, according to the circular economy.

CHITIN NANOFIBRILS (CN) Chitin, distributed widely in nature as the skeletal material of crustaceans and insect and as a component of cell walls of bacteria and fungi, is a (1-4)-linked polysaccharide consisting of N-glucosamine units [25]. This polymer, similarly to silk and cellulose, is a glucose based polysaccharide, hierarchical organized in micro-fibrillar sheets arranged as an helicoidal structure (Figure 4) [16].

Figure 3. Chitin microfibrillar twisted plywood structure (by courtesy of Nikolov et al. [27]).

The sheets, holding in place by a number of intra-free hydrogen bonds, including the rather strong C-O...NH bonds, maintain their molecular chains at a distance of about 0.47 nm along the axis of the unit cell. The respective linear molecules are oriented in parallel manner consisting of alternate D- amorphous and crystalline domains [26-29]. On the other hand, the alpha-chitin nanocrystals, covered on their surface by many polar groups positively charged, when produced industrially have the aspect of nano-fibers with a needle-like structure and mean dimension of 240 x 7 x 5 nm (Figure 5) [30].

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Figure 4. Chitin nanofibers as observed by Scanning Electron Microscopy (SEM) at different enlargements [30].

Thus for example, when the chitin (CN) nanofibers’ water suspension enters in contact with negatively charged polymers, such as yaluronic acid and nanochitin (NC), all the polymers assemble easily forming micro/nanoparticles (Figure 5).

Figure 5. Micro/nanoparticles of chitin-Lignin at SEM.

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Figure 6. Scaffold’s of Chitin Nanofibrils (left) and extracellular matrix (right) by SEM.

For their particular physicochemical and biological characteristics, CN and its complexes show an interesting medical and cosmetic interest. By the use of the right methodology, such as elettrospinning, in fact, they form scaffolds which mimic the native extracellular matrix (ECM) (Figure 7) [31, 32].

Figure 7. Lignin structure.

These natural scaffolds, acting as innovative carriers, are able to load and transport various active ingredients, releasing them at different skin layers when used in the form of non-woven tissues or films to make innovative medications or beauty facial masks [9]. Controlling and mimicking the nano-bio molecules, these new ingredient carriers may be used in the regenerative medicine as well as to produce smart biodegradable cosmeceuticaltissues for aging skin [31, 32]. The main purpose of these cosmeceutical-tissues, in fact, is to replace senescence and/or diseases cells, reestablishing their anatomical and physiological state [33]. It is to underline, in fact, that CN is a polymer made by units of glucosamine and acetyl glucosamine, forming the building blocks of the native ECM also [34]. Moreover, the

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incorporation of the complex chitin nanofibrils-nanolignin (CN-NL) into different polysaccharides, enhances the biocompatibility of the electro-spun tissue in terms of cell attachment and proliferation, reinforcing its structure by its nanofiller function [25, 35, 36]. These the reasons why the high crystallinity and strength of CN and its nanocomposites are gaining an increased interest for potential biomedical and cosmetic applications, intrinsically related to their non-toxicity, biocompatibility and biodegradability. Moreover, both CN and NL are polymers at a potential low cost and easy to be processed and, as biomaterials, are able to establish appropriate interactions with the surrounding skin layers, without inducing adverse host responses [25, 35, 36]. In addition, possessing a high surface area to weight ratio, these polymers are readily available for chemical functionalization [26, 35]. Additionally, it is interesting to underline that CN is not only obtained from waste materials, but is also easily degraded by human and environmental, enzymes to molecules, such as glucosamine, acetyl-glucosamine and glucose, utilized as food and energy from both cells and microorganisms [24, 25, 36, 37]. At this purpose, it has been shown in vitro on human keratinocytes that both CN and its complexes with nanolignin, as component of non-woven tissues and films, possess antioxidant, immunomodulatory and skin repairing activity [37-41]. Moreover, the interesting results obtained in vivo have confirmed the skin repairing effectiveness of these non-woven tissues/films, probably due to the activity of the content in biomolecules, capable to stimulate a more regular and modulated production of collagen and elastin, by a more balanced cellular metabolism [40]. In conclusion CN and its complexes, ameliorating the intercellular communication and decreasing the oxidative phenomena caused by UV and air particulate, could be used to make innovative films and non-woven tissues to be used as active carriers for aged or diseased skin. To better understand the supposed effectiveness of the CN complexes it seems useful to report some information regarding the nano-lignins’ activities.

LIGNIN Lignocellulosic biomass are estimated to exceed 2 trillion of tonnes per year worldwide, offering a vast source for the Lignin extraction [42, 43]. The biomass material is a compound of biopolymers with cellulose interwined (35-83%) by hemicellulose (0-30%), lignin(143%)and some extra complexes (tannins etc.). Lignin, rich of basic phenyl propane units and accounting for up 30% of the organic carbon on earth and 15-40% of dry weight of woody plants, is amply studied, especially as one of the most promising raw material to produce energy [42, 43]. Based on the annual biomass growth rates, the every year production of this polymer by paper and pulp sector is around 50-million tons, of which no more than 2% is used to make value added products, while 98%is burned to obtain energy [44]. Lignin is a highly irregularly branched polyphenolic polyether, consisting of primary monolignols, such as p-coumaryl alcohol, coniferyl alcohol, and synapyl alcohol, connected together by aromatic and aliphatic bonds as well as non-aromatic CC-bonds (Figure 8) [45, 46].

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Figure 8. Mitocondrion Redox activity and ROS.

It is a nano-polysaccharide that helps to protect the plant swift tissues from microbial and fungal attack thanks to its content in phenolic groups. Thus nanolignin is an important source of natural antibacterial compounds, also if its antiseptic effectiveness depends from the origin plant species and the processing method of extraction [47]. Moreover, the nano-sized lignin offers a high surface area and, therefore, more functional groups and polyphenolic side chains able to increase its antimicrobial activity. However, similarly to nano-chitin, this polymer may be used as biochemical compound and filler to provide strength for innovative nanocomposites, just as it provides mechanical support for the plant as primary element of its cell wall [48]. Thus, by this function and for its antioxidant and sun protective activity, lignin may be used, for example, as high performance broad spectrum sunscreens for innovative cosmetic products [45]. This polymer, in fact, may be considered a natural sun blocker due to the free radical scavenging ability of its phenolic and ketone groups, as well as an effective antioxidant compound for its structural intramolecular hydrogen bonds. Thus as antioxidant compound, lignin stabilizes in plant the reactions induced by the oxygen reactive species (ROS), as well as slows down the aging phenomena of all the biological systems [48]. The right oxygen’ equilibrium for a balanced respiration of the human biological, tissues, in fact, is a necessary mean for preventing its lack by the continuous UV oxidation, cause of cell mitochondria dysfunction of the premature aged skin (Figure 9). Moreover, the activity of the many phenolic groups of lignin, seems having the ability to inhibit the opportunistic microorganisms’ growth, probably balancing the skin microbiota, as part of its protective barrier [49]. It is to remember, in fact, that the major function of the human skin to protect the body against the environmental aggressions, is also performed

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thanks to the symbiosis between its cells and the microbial layers, established during the lifetime [50]. Therefore, the skin microbiota together with keratins, lipids, lactic acid and minerals result vital to keep healthy both human skin and the body, not only protecting them against the unwanted microorganisms, but also supporting indirectly the hydration and protective activity against the UV damages [50, 51]. Last but not least, the more intensive use of this polymer could help to reduce the agro-agricultural and food waste, preserving the consume of the natural raw materials, according to one of the aims of the green economy [24]. Thus, lignin for its interesting physicochemical and biomimetic characteristics, being biodegradable, eco-compatible, biocompatible and free of side effects, opens new outlooks for making innovative formulations, such as hydrogels, nano-composites and smart tissues/films to be used in the medical, and cosmetic fields. At this purpose, it is to underline the interesting skin activity shown by the nanochitin-nanolignin (CN-NL) complexes, which have evidenced anti-bacterial, anti-inflammatory, cicatrizing and anti-aging effectiveness, when bound to the fibers of non-woven tissues made by natural polysaccharides [20, 52-53]. These innovative tissues probably facilitate the cell communications and growth by the combined activity of the tissue-polysaccharides hydrolyzed in glucose, glucosamine and acetyl-glucosamine and the active ingredients bound to the produced tissues [10, 24, 31-33, 52, 53]. To remain healthy and functional, in fact, skin cells need to be correctly integrate each to others, and able to assimilate and use in the best quantity nutrients, such as, lipids, oligosaccharides and proteins.

CIRCULAR ECONOMY AND FOOD WASTE As reported previously and elsewhere in the book, one of the more unsolved problem is the food waste that represents around one third of all the food produced, while more than 820 million people in the world is undernourished and 2 billion experience moderate or severe food insecurity [54, 55]. On the one hand, chitin waste is underutilized also if around 10 trillion/tons of this polymer are produced annually from organisms living in the oceans [56]. On the other hand, an healthy lifestyle paired with an increasing awareness of the need for a sustainable and responsible consumption of resources, form part of the outlook of the today’s consumers [57]. The majority of customers, in fact, agree that being “better for the environment is the number one reason for buying natural products”. As an example of the UK consumers attitudes towards recycling products, 49%of people seem to be interested in buying fashion intensity made wholly/partially from recycled plastic; 72% are interested in buying products with packaging made wholly/partially from recycled plastic; 73% like to see more food/drink guaranteed to be sourced from unpolluted water, while 79% seems to be incentivized to recycled plastic [57]. Thus, the chitin extraction from fishery’s waste (ranging around 150 billion tons per year!) [38], and its use to make valuable goods, has become a necessity, also to eliminate its negative impact on both human health and the environment, being usually thrown out in the sea, burned, landfilled, or simply left out to spoil [58]. Therefore, in the incoming years, our society has to rethink its business models, making waste free products, following the proposals of the circular/green economy. According to UNEP, in fact, a green economy does not favor one political perspective over another but it is relevant to all economies, as a

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market-led [59], able to follow both the industrial necessities and the actual consumers attitudes. According to the Mintel report [57], in fact, “young people will expect Company to offer support when it comes to their health and well-being as well as get more involved in their education and development”. Moreover, 42% of all consumers believe that natural products are more suitable for the environment, while providing more sustainable benefits without a reduction in sensory performance. On the other hand, in contrast to the take-make waste linear economy, the circular economy has based on a regenerative economic development designed to benefit the industrial business needs with the consumers necessities for health and wellbeing and the protection of the environment [60, 61]. Thus, for example, it has been foreseen by nine month study of experts that by adoption of the circular economy principles, Europe would increase the industrial competitiveness delivering better societal outcomes, resulting in overall benefits of €1.8 trillion by 2030 with a 48% reduction of the Carbon dioxide emissions [62].

CONCLUSION In conclusion, the use of Chitin and Lignin as raw materials obtained from agro-food and industrial by-products respectively, are in line with the Circular Economy goals and the consumers requests for natural product respective of the environment. These interesting natural polymers, in fact, may be not only used to produce innovative cosmeceuticals and advanced medications, but could contribute also to reduce both the land/oceans pollution and the green-house emissions, promoting health and well-being. Thus, as reported, Chitin and Lignin could be utilized, for example, to produce smart non-woven tissue facial masks [10, 24, 30-33] able to load and release active bio-ingredients effective, for example, as cosmetic anti-aging agents. At this purpose, it is Interesting to underline that these smart cosmeceutical tissues utilized as innovative carriers, are free of surfactant/emulsifier which have a devastating effect on the diversity of the protective skin microbiota [51, 52]. Moreover, the same tissues bound to different bio-ingredients have shown to be effective to quickly repair the skin affected by first and second grade’ burns, without evidencing unwanted side effects, such as hypertrophic scars or keloids [36-40]. However, it is also to underline that the packaging material actually utilized, for example in the cosmetic field, represents around 120 billion of units produced annually most of which are not recyclable. For these reasons the cosmetics customers are increasingly demanding zero waste, 100% recyclable packaging and fair trade practices [61, 62]. For all these reasons the cosmetic companies, implementing innovative solutions and eco-systems, are becoming to place importance on products more effective for human health and the environment, guaranteeing security and sustainability of both active ingredients and packaging materials used [63, 64]. We hope that this new productive approach, strongly stimulated from consumers also, will represent the future goal for all the industries. So doing and according to the circular economy and UN guidelines, it seems possible in the incoming years to reduce pollution by a decarbonization program, make food, agricultural and forest production systems more resilient to conserve and restore the biodiversity, organize more sustainable green cities and communities, manage at the best artificial intelligence and communications, finally increasing education and the social protection systems to reduce the

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inequality and promote health and wellbeing for all. This should be the goal of a modern Society.

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In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 17

THE USE OF COFFEE WASTE TO PRODUCE GOODS AND ENERGY Andrea Morganti1 and Pierfrancesco Morganti2,3, Caffe’ Morganti R&D Unit, Rome, Italy Academy of History of Health Care Art, Rome, Italy 3 China Medical University, Shenyang, China 1

2

ABSTRACT Coffee is the world’s favorite drink with a global consumption of 165,345 million bags per year. Also, if its beans are reach of over 1,500 active interesting compounds, each year around 3,000 tons of spent coffee grounds go to landfill as dangerous waste. Thus the necessity to recycle this waste by the circular economy rules, to stop damage to both humans and the environment. The chapter tries to give an overview of coffee consume and waste, reporting data and proposals to reuse its spent grounds

Keywords: waste, environment, coffea arabica, coffea canephora, coffea liberica, spent coffee, cappuccino, caffè espresso, caffe’ macchiato, marocchino, recycling

INTRODUCTION Coffee is among the largest most traded commodities worldwide and represents one of the most popular and valuable product. In years 2018/2019, it ranged the global consumption of 165,346 million bags, 53,896 of which in European Union, 36,742 in Asia and Oceania, 30,454 in North America,27,128 in South America, 11,724 in Africa and Central America, and 5,402 in Mexico. Brazil was the greatest exporting country (Figure 1) while Europe was the greatest importing country [1]. 

Corresponding Author’s Email: [email protected].

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Figure 1. The major coffee producers.

As a beverage, more than 400 billion cups are consumed each year in the world, and each coffee drinker consumes around three and half cups each day. The world’s biggest coffee drinkers are Finland with 12 kg per capita per year, Norway 9.9, Iceland 9, with Italy 5.8 and Cyprus 4.8 among the others (Figure 2). According to International Coffee Organization [1, 2] in 2016 UK customers paid more than any other per pound instant coffee i.e.,US$16.29, followed by Malta at US$ 13.33 and Italy at US $7.45 per pound of roasted coffee (Figure 3).

Figure 2. Coffee consumption in different countries pro capita in 2016.

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Figure 3. Per capital coffee consumption.

It is interesting to underline that today people are drinking more coffee than ever before, and “grabbing a cup of coffee on the way to the office has become a daily ritual for many workers around the world” [2]. However in UK latte, cappuccino and americano coffee remain among the most preferred beverages (Figure 4), while the most branded coffee chains in Europe and the US are Costa and Starbucks respectively (Figure 5) [2]. But which is the coffee waste?

Figure 4. Favourite coffee drinks in UK.

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Figure 5. The most branded coffee in EU and USA.

Unfortunately, each year we produce around 3,000 tons of spent coffee grounds, 93% of which go to landfill and 7% only is collected, processed and used as composting material. Just to remember, spent coffee grounds (SCG) refers to coffee waste produced by the espresso coffee extraction process. Thus, while such amount of waste contributes to rinsing pressure on landfill, its decomposition contributes to green-house gas (GHG) emissions. At this purpose it is interesting to underline that SCG contain many active ingredients which, extracted, could be used in the pharmaceutical and cosmetic field, while alternatively it may be useful as a low cost composting for plants, due to its content of high nutrient ingredient levels, active against pathogens also. When coffee is extracted by water most of its hydrophobic compounds (oils, lipids, fatty acids, insoluble carbohydrates, proteins, etc.) remain in the grounds and could be recycled in order to use its rich content for active ingredients [3].

COFFEE INGREDIENTS AND WASTE Coffee ingredients are represented from over 1,500 chemicals and substances, of which 850 are volatile and 700 soluble compounds. Thus, its brewed beverage contains lignins, phenolic compounds, caffeine and many aroma producing essential oils, which characterize

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its aroma and bitter acidic taste, according to the different varieties. These the reasons to roast together different coffee species (i.e., arabica, robusta and liberica), in order to give acidity, aroma and body’s taste to the final coffee cup, produced by the final ground coffee used. Arabica (Coffea Arabica) has the highest quality in terms of taste and aroma and dominates the international market by around 65%, Robusta (Coffea Canephora) has the highest caffeine content and represents around 33% of world production, while Coffea Liberica with 2% is almost not considered. However, we should consider that on one hand, about two thirds of roasted coffee consumed worldwide is Arabica and one third is Robusta, while on the other hand, around a half of wet weight of the whole coffee bean, including its pulp, at present is discarded, despite its richness in carbohydrates, proteins, minerals, tannins, caffeine and potassium [1, 3]. Thus we should underline that two tons of green coffee produces one ton of coffee pulp that remain in the environment as waste, polluting material. Coffee berries can be processed in two ways, dry (natural) and wet (fermented and washed), considering the last as the best way to have an higher quality product. The quality of coffee beans starts to degrade few hours after being picked from the farm, so that it has to be processed immediately [4]. The dry method is the simplest one with minimum pollution potential but requires a large space and sunny countries with no or low raining seasons. Coffee berries, in fact, after picking are left under the sun, until moisturizing content reach a minimum of 10%. The wet method, in which the coffee berry is subjected, is based on mechanical and biological operations to separate seed from exocarp, and represents a process used by half of the world. The dry method is the simplest with minimum pollution potential, while the wet processing system uses large volume of water (i.e., ~15-20 L to 1 kg of coffee beans), generating high volume of pollution such as pulp (43%), mucilage (12%) and parchment (6.1%), generally discharged in rivers [5]. Just to remember, the coffee berry (Figure 6) is composed by an outer skin, pulp, pectine layer, parchment and silver skin that represent the waste materials released from the coffee processing.

Figure 6. The coffee berry structure.

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These by-products discharged in water, decrease its oxygen content, creating anaerobic conditions which, together with the released toxic chemicals such as tannins, phenolic compounds and alkaloids, result fatal to the aquatic inhabitants. Another coffee waste is represented from the spent grounds, which include those obtained from the soluble coffee industry, as well as those produced after brewing at cafeterias or at home [5]. From 1 g of ground coffee, in fact, we get about 0.91 g of spent coffee grounds, while about 2 kg of wet spent coffee grounds are produced for every kilogram of instant coffee made [5, 6]. However, it is to underline that around 6 million tons of spent coffee grounds are produced each year and from 2000 to 2012 global green coffee production increased by 17% so that in 2016, 7,200,000 tons all coffee beans were exported [6, 7].

COFFEE IN ITALY In Italy, where coffee, as Espresso, Cappuccino, Macchiato and Marocchino, represent the highest consumption per capita in Europe, the market is dominated by its use as an hot drink during the day work break (Figure 7) [8]. Espresso coffee, in fact, has originated in Italy both as regards the espresso makers and for the production method, based on machines the prototype of which was introduced from Italy to the Paris World Expo in 1855. The coffee consumption started in Venice in 1600, sold in Pharmacies as a remedy for the digestive tract and successively appreciated by Pope Clement VIII as a fragrant new drink, became in few decades the Italian and European word caffè. Thus the first coffee houses were opened becoming “places where artists and intellectuals would meet to exchange ideas and discuss the matters of the days” [8]. Italian coffee is normally drunk in a bar by a ritual that doesn’t take longer than 6-7 mins in total, while enjoying a peaceful moment completely by yourself or chatting with friends (Figure 8). The coffee dose for a perfect espresso is 7 g made in about 30 sec by 25/30 ml of hot water. It has to be drunk at a temperature of about 60 C degrees, no more than 2 minutes after being made. Even if you don’t add sugar to your coffee, you still need to mix it to distribute well the blend’s aroma and flavor.

Figure 7. Cappuccino (left) and caffe’ espresso (right) are the most frequent Italian drinks.

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Figure 8. Italians in a bar (By courtesy of Gran Caffe’ Gambrinus).

Coffee taste depends of the different quality and quantity of beans used, time of roasting, water and temperature used to brew it. However, Italian coffees is made mainly by Arabica, known for its full flavor and low caffeine content, blended with Robusta. Roasting time, must be done taking great care to the fact that the blend as Robusta beans need to be roasted longer than Arabica [9]. Thus a common phrase says: “coffee is a pleasure. If it’s not good what pleasure is it?” On the other hand a famous Italian writer and food connoisseur has written about the Italian espresso: “This precious drink that spreads a great deal of excitement throughout the body was called the intellectual drink, the friend of writers, scientists and poets because, jointing the nerves, it brightens ideas, it makes up imagination more alive and thought more rapid.” Thus we are what we drink and eat (Figure 9).

Figure 9. We are what we eat and drink.

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THE COFFEE WASTE PROBLEM IN ITALY In Italy there are about 800 companies involved in coffee manufacturing and 149,000 coffee shops which consume about 1.2 kg of coffee a day to prepare an average of 175 coffee based drinks, while the roasted coffee industry releases the silver skin tegument as roasting residue which, known as “chaff,” comprises 4.2% of green coffee beans. Thus, the necessity to transform in richness the residual spent coffee waste estimated in about 150,000 kg/day. Caffè Morganti is one of the oldest Italian Companies settled in 1890 by apothecary Romeo Morganti (Figure 10). He started in Rome, at Via Ripetta, a roasting coffee company with a distillery. At that time coffee would come from Brazil and Central America to Ripa Grande (big shore) fluvial port of Rome, via Tiber river, aboard a steamboat called Garibaldi. Romeo Morganti in order to roast coffee designed and built a machine consisting of two large metal spheres, which, filled with raw coffee, were placed on a furnace fueled by woodfire (Figures 11 and 12). Since then, Caffè Morganti has grown out to the present days, combining modern production systems to the artisanal care which has always distinguished it from the beginning, allowing the company to produce coffee blends with unique taste.

Figure 10. Coffee shop behind the warehouse in late 1800’.

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Figure 11. Roasting machine.

Figure 12. Promotional Sign.

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COMPANY PROGRAM At present Caffè Morganti Company roasts an average of 7.5 tons of coffee per week, meaning around the same weight of spent coffee grounds. Considering this waste as a richness, we are programming to collect the spent coffee grounds from our customers during the same days we deliver our roasted coffee. Verified the interest of our customers to participate in our coffee grounds recycling program, we have in progress a recovery program as follows. Spent coffee, recovered from every drinking cup produced daily, will be collected into a special container, previously given to each customer. Its capacity is sufficient to collect a week of spent coffee grounds and may preserve them from the air contamination, considering that the coffee machine practically sterilizes the coffee grounds. In the factory the spent coffee will be collected into special closed containers air free to be used in different ways. One option is to collaborate with an Italian Company that use the spent coffee grounds as a growth medium for the mushrooms production. Another in study option is to organize an anaerobic digestion by microorganisms to produce both methane rich biogas, to be used in our factory as energy for the roasting process, and a nutrient rich biological fertilizer.

CONCLUSION The worldwide food and agroforestry’s industries produce annually large volumes of wastes consuming billion tons of the planet resources [10, 13]. Particularly, food loss along the supply chain (~30%) and production of by-products not only cause serious pollution problem to humans and the environment, but induce one million people to be undernourished while the worldwide population is growing. Thus the need of more food to be produced, which put more pressure on natural resources, contributing to increase the greenhouse gas (GHG) emissions [10]. This is why reducing food loss will induce the necessity to use raw materials more intelligently and efficiently making an important contribution to waste management by a sustainable strategy, according to the circular economy aims by the use of innovative biotechnologies [11-13]. As previously reported, coffee is the world’s favorite drink and one of the most valuable international commodities, represented by about 20 million coffee farming families in over 80 countries, while around 100 million people depend on coffee for their liveli-hoods and its export value in 2009/10 ranged US$ 15.4 billion [14]. Coffee cups, in fact, are drunk not only at home but also at the work places and especially in bars and coffeehouses. Consequently, its spent grounds, thrown away and leftovers as waste, release into the atmosphere methane, with a global warming potential much greater than carbon dioxide. Thus, waste and coffee by-products, which represent about 50% of the coffee fruit and ranged worldwide millions of tons, need to be recycled to stop both damages to human and the environment and the money loss. As previously reported the next goal is to try to utilize not only the spent coffee grounds coming from our Company but to involve other industries to join us in this project and contribute towards the circular economy.

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REFERENCES [1] [2] [3] [4]

[5]

[6]

[7]

[8] [9] [10]

[11]

[12] [13] [14]

International Coffee Organization, Trade Statistics - October 2019. www.ico.org (Accessed on November 27th 2019). Jones, L. (2019) Coffee: Who grows, drinks and pays the most? News, 13 April 2018 (Accessed on November 27th 2019). Padmapriya, R., Tharian, J. E. and Thirunalasundari, T. (2013) Coffee waste management-An overview. Int J Curr Sci 9: E 83-91. ISSN 2250-1770. Ljanu, E. M., Kamaruddin, M. A. and Norashiddin, F. A. (2019) Coffee processing wastewater treatment: a critical review on current treatment technologies with a proposal alternative. Applied Water Science 10: 11. https://doi.org/10.1007/s13201-0191091-9. Blink, L., Sirotiak, M., Bartosova, A. and Soldan, M. (2017) Review: Utilization of waste from coffee production, Research Papers Faculty of Materials Science and Technology Slovak University of Technology 25(40): 91-101. Campos-Vega, R., Loarca-Pina, G., Vergara-Castaneda, H. A. and Oomah, B. D. (2015) Spent coffee grounds: A review on current research and future prospects. Trends Food Sci Technol 45: 24-36. Vitezova, M., Jancikova, S., Dordevic, D., Vitez, T., Elbl, J., Hanksakova, N. et al., (2019) The Possibility of Using Spent Coffee Grounds to Improve Wastewater Treatment Due to Respiration Actuvity of Microorganisms. Appl Sci. 9: 3155. doi: https://19.3390/app9153155. USDA foreign Agricultural Service (2010) TAIN Report, No IT 1047, March 12, 2010. Demetri, J. (2019) The World of Italian Coffee. Food and Wine, October 25. https:// www.lifeinitaly.com/food/the-world-of-italian-coffee/ (accessed on October 4th 2020). Gustavsson, J., Cederberg, C., Sonesson, U. van Otterdijk, R. and Meybeck, A. (2011) Global Food Losses and Food Waste, Food and Agriculture Organization of the United Nations, Rome, Italy http://www.fao.org/fileadmin/user_upload/suistainability/pdf/ Global_Food_Losses_and_Food_Waste.pdf (accessed on October 4th 2020). Sustainable Industries, Resource Efficiency Challenge (2012) Edition Econsense. https://econsense.de/app/uploads/2018/06/econsense_Ressource-Efficiency-Challenge_ 2012.pdf (accessed on October 4th 2020). WHO. Circular Economy and Health: Opportunity and Risks. World Health Organization Publication. ISBN 978 92 899 5334 1. Morganti, P. (ed.) (2019) Biotechnology to Save the Environment. Plant and Fishery’s Biomass as Alternative to Petrol, MDPI, Basel, Switzerland. Didanna, H. L. (2014) A critical review on feed value of coffee waste for livestock feeding. World Sci Rer J 2(5): 72-86 ISSN 2331-1894.

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 18

NATURAL METABOLITES AS FUNCTIONAL ADDITIVE OF BIOPOLYMERS: EXPERIMENTAL EVIDENCE AND INDUSTRIAL CONSTRAINT Arash Moeini1,2, Gabriella Santagata1, Antonio Evidente2 and Mario Malinconico1,* 1

Institute for Polymers, Composites, and Biomaterials, National Research Council, Pozzuoli, Italy 2 Department of Chemical Sciences, University of Naples "Federico II", Naples, Italy

ABSTRACT One of the biggest problems in the food packaging system is the prevention of food from mold contamination. Indeed, food mold infestation is very dangerous for human health and can also considerably raise the financial cost. In particular, in bakery products, Penicillium roqueforti and Aspergillus niger are the main contaminators. On the other hand, the food packaging system is responsible for protecting food substrates from physical damage, chemical and biological contaminations. Besides, packages are designed to preserve food quality and safety, extending their shelf-life. However, due to the environmental impact of conventional polymers, recently, the attention of scientific research and industrial sectors is mainly focused on the use of bioactive biopolymerbased package systems. Antimicrobial food packaging is known as an active package in which natural bioactive compounds, such as plant metabolites, incorporated into the polymer or biopolymer matrices can reduce, inhibit or hinder the growth of microorganisms on the packaged food surface. This chapter examined the application of some biopolymers in food packaging along with a brief introduction of the common biopolymers applied for food packaging. Furthermore, it gave an overview of three natural antifungal metabolites with potential applications in the bakery bio-packaging industry.

Keywords: biopolymers, food packaging, natural metabolites, antifungal properties 

Corresponding Author’s Email: [email protected].

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INTRODUCTION Natural products include all secondary metabolites that are synthesized by a living organism. Plant and microorganisms are the main sources of bioactive secondary metabolites, which can have very different structural diversity and unique biological properties with a wide range of applications in different fields such as agriculture [1, 2], medicine [3, 4] and packaging [5]. Molds can cause a serious risk for the health of humans and animals. In particular mycotoxigenic fungi may cause allergic reactions and respiratory problems in both animals and humans. The capability of mold to grow in harsh conditions (low temperature and water) is a huge threat to fresh food products such as bakery, dairy, fruits, and vegetables. The most common molds as food contaminators are Alternaria, Aspergillus, Penicillium, Eurotium, Botrytis, Rhizopus, Monilia, Cladosporium, Geotrichum, and Wallemia [5]. Among them, Aspergillus, Penicillium, and specifically P. roqueforti and A. niger can produce mycotoxins able to contaminate food products. In particular, they are considered the main spoilage of bakery products [6]. Several attempts have been performed in order to avoid food contamination from molds. Formerly, the antifungal additives were directly added to the foods as active ingredients with the main drawback of altering the taste, flavor, and food quality. Over time and by the development of the packaging industry, the new concept of food packaging known as ‘active packaging’ took place; it consisted in formulating different active and antimicrobial substances directly into the package systems to both increase the food shelf-life, preserve their organoleptic properties and safety from microbial infestation, and to maintain or improve the food quality [7]. In the active package materials, the functional compounds can release or absorb substances from the package to the environment surrounding the food. Secondary metabolites from plants and fungal microorganisms could be exploited as potential and promising bioactive substances to be incorporated in polymer packaging systems. This chapter reports an overview of oil-derived and biodegradable polymers commonly used as matrices inactive food packaging. Particular emphasis will be placed on the inclusion of natural antifungal compounds in eco-sustainable polymers for the bakery food packaging industry.

SYNTHETIC POLYMERS Nowadays, based on Plastics Europe, the consumption of plastics has been significantly increased from 65 to more than 350 million tons; 18.5% of this amount is produced in Europe, and more than one-third of this amount belongs to short-life materials such as packaging. Polyolefins and other thermoplastics are the primary matrices of commodities since their plasticity in form and function. Moreover, petroleum-based plastics show wideranging benefits, hovering from the low cost, long-lasting, lightweight, excellent resistance to chemicals and water to suitable mechanical and thermo-optical performances. Packaging represents one of the most important applications of plastics. The most common food packaging materials are polyethylene terephthalate (PET), high-density polyethylene (HDPE), polyvinyl chloride (PVC), low-density polyethylene (LDPE), polypropylene (PP), and polystyrene (PS). Their selection is strongly related to the specific application. As an

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example, PET shows good mechanical and optical properties but melts very easily, making it ideal for cold liquids [8]. HDPE is used for foods where a strong material is needed, but clarity is not required [9]. PVC is used for clear plastic wrapping because of its cheap cost and stretching capabilities as well as being easy to extrude into sheets [10]. Food storage bags are mainly based on LDPE because it is very low cost and evidence a large stretch capacity and excellent barrier properties [11]. PP is the main component of rigid containers like baby bottles and cups, and bowls because of its high strength properties [12]. PS is commonly used in Styrofoam food containers and cups as well as meat and egg trays that require a rigid form or heat resistance [13]. Anyway, as concerning waste management and environmental both issue and perspective, the main drawbacks associated with petrochemical plastics come from the large volumes of plastic waste materials generated, not biodegradable and/or compostable. This is due to their biological inertia, which in turn provokes a waste management problem, particularly emphasized for plastic materials with short shelf life, such as packaging materials. Just to give you an idea, the European Commission report established that less than 25% of post-used plastic is recycled while about 50% goes to landfills and the others to oceans [14]. Nevertheless, since the Sustainable Development Goals of 2030 will be mainly focused on the drastic reduction of plastic pollution of all kinds, including marine litter [15], scientific and industrial communities are increasingly paying attention to the development of biodegradable packaging materials coming from biological resources, such as biopolymers, as valid substitution of oil-based polymers and as a potential solution to waste management and environmental issues [15].

BIOPOLYMERS According to European Bioplastic’s definition, “Biopolymer” is a term used to describe two different kinds of plastic materials, the polymers synthesized from renewable sources (or bio-based polymers) and the biodegradable and compostable polymers according to the standard EN 13432, ASTMD 6400. It is worthy of underlining that the two definitions aren’t mutually exclusive. This means that a polymer can be bio-based, biodegradable/compostable, or both [16]. Biodegradability is the end-of-life process of bioplastics based on the action of microorganisms able to completely transform the post-used polymers in new eco-friendly products in a timely, safe, and effective way. Since the biodegradation occurs by means of biological processes by which microorganisms assimilate and utilize carbon substrates as food for their life processes, phenomena like oxo-hydro-chemo-photo - degradability refer to abiotic mechanisms finalized to deteriorate the optical, thermos, mechanical performances of the polymers, inducing physical modification of their macromolecular structure, such as depolymerization and disintegration. These modifications are far from biodegradability. When disposed of in bioactive environments, biodegradable polymers can be degraded by the enzymatic action of microorganisms, such as bacteria, fungi, and algae, and converted into biomass, carbon dioxide, water, or methane, depending on if the degradative environment is aerobic or anaerobic. Hence, at the end of bioplastic lifetime, biodegradation will start by means of bacteria flora (biodegradation in soil) or in the presence of other organic material (biodegradation in compost), under specific temperature and humidity conditions, in order to

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generate carbon-rich compost [17]. Therefore, it is absolutely relevant to know the disposal environment in which biodegradation occurs, soil, composting, or marine sediment, in order to modulate the rate of the process. Biopolymers have several advantages, like easy availability since they come from natural renewable sources (replenishable agricultural or marine food resources), biocompatibility, and non-toxicity. These properties, together with the possibility to tailor the specific performances by modulating the intrinsic biopolymer chemico-physical features, make biopolymers exploitable for several applications, from the packaging, paper coating, biomedical (surgical sutures, implants, and drug delivery) areas, to food science and agriculture fields. Specifically, as far as the packaging sector concerns, the bioplastics have to be renewable and compostable to reduce the widespread diffusion and consumption of petroleum-derived polymers. Biopolymers (or “bioplastics”) can be classified according to two different criteria, the source of the raw materials and the biodegradability of the polymer. This means that, as a rule, biopolymers can be made from renewable raw materials (biobased), both biodegradable or not, and they can be produced from raw fossil sources, likewise being biodegradable. The biodegradable bio-based biopolymers, produced or by biological systems (microorganisms, plants, and animals) or by chemical synthesis from biological starting materials (e.g., corn, sugar, starch, etc.), include synthetic polymers from renewable resources such as poly(lactic acid) (PLA), biopolymers produced by microorganisms, such as PHA, naturally occurring biopolymers, such as polysaccharides coming from vegetable and animal sources (cellulose, starch, alginate, chitosan, etc.) or proteins biosynthesized by various routes in the biosphere. The non-biodegradable biopolymers coming from biomass or renewable resources mostly include specific polyamides, polyesters based on biopropanediol, biopolyethylene etc. The oil-derived biodegradable biopolymers, such as synthetic aliphatic polyesters made from crude oil, are polycaprolactone (PCL), poly(butylenesuccinate) (PBS), and some aliphaticaromatic copolyesters [18]. Due to their easy availability and cost-effectiveness, biodegradable biopolymers directly obtained from natural sources could be considered the most promising materials in substituting synthetic ones in several applications [19].

ADDITIVE AND BIOPOLYMERS IN FOOD PACKAGING The materials which protect food from the environment (moisture, oxygen, carbon dioxide, and other gases), chemical (flavors and aromas), and physical (breakage) challenges are recognized as food package. The key role played by a food package material is extending the food shelf-life by preserving its organoleptic and sensorial properties [20]. The food packaging history started in France during the Napoleon Bonaparte era by Nicolas Appert, who used glass bottles with cork seals as food containers for the soldiers and used them for food heating. However, due to glass bottles' fragility, they were fastly replaced with metal cans. Only after the Second World War, when plastic materials developed for army purposes, polyethylene was introduced in the food packaging industry [21]. Actually, nowadays, the packaging is an integral part of the food processing industry. Indeed, the “food package” is the entity that works as the physical barrier between the food contents and the outside environment [22].

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The main roles of packaging are identified in food protection (active packaging), information (intelligent packaging); and transport. Due to the increasing demand for plastic packaging showing tailored specific properties in protecting food, the traditional passive packaging, based on food distribution and storage, is not effective and out-dated. In the second half of the twentieth century, the modern concept of food packaging developed when natural and artificial additives were introduced into the package system during the manufacturing process, to both improve polymer processing and performances and extend the shelf life of processed foods, as in the case of active packaging [23]. Hence, additives are mainly classified on the basis of their functions rather than their chemistry. For instance, additives as plasticizers, lubricants, nucleating and blowing agents, optical brighteners, ultraviolet light stabilizers, antioxidants, flame retardants are usually introduced in polymeric matrices to enhance the productivity of the machinery and to improve the mechanical, thermo-photo-optical performances of the packages in accordance with their end use. In addition, since foods are spoiled by a variety of microbial strains, generally attacking food surfaces [24], the introduction of antimicrobial additives, tightly immobilized inside the polymer during the processing, is the proper answer to consumers' request for food without preservatives. The antimicrobial active packaging technology is based on antimicrobial agents physically incorporated inside the plastic resins or chemically immobilized within the polymeric structure before film casting [25]. Thus, in the active packaging, great efforts are making to develop polymer systems proactive in protecting food from microbial contamination. To this aim, in active packaging, oxygen, moisture, or ethylene scavengers are being used to protect foods from the oxidation of sensitive components like fatty acids, carotenoids, meat pigments, and vitamins, as well as to avoid the emission of ethanol and peculiar flavors, thus extending the shelf life of food products [26]. As previously detailed, the increased use of oil-derived plastics has created serious ecological concerns because of their resistance to biodegradation. Biopolymers can be used as a valid alternative as they easily degrade in the environment and generally mimic the outstanding properties of conventional polymers. In particular, biopolymers could be considered excellent materials for short-term and disposable applications in the food packaging industry, representing a key innovation in supporting the drastic reduction of the environmental impact of plastic production [27]. Poly (lactic acid) (PLA), polybutylene succinate (PBS), Mater Bi® (MBi), and chitosan (CH) are the most common biopolymers applied in Food Packaging Industry. In the following part, each of these biopolymers will be briefly introduced.

Poly (Lactic Acid) (PLA) Poly (lactic acid) (PLA) belongs to the biodegradable aliphatic polyesters derived from 100% renewable sources [28]. It is obtained from lactic acid or (2-hydroxypropanoic acid) (LA), a monomer existing in two enantiomeric forms L-lactic acid and D-lactic acid (see Figure 2), from which three PLA stereoisomers could be driven, poly(L-lactide) (PLLA), poly(D-lactide) (PDLA), and poly(DL-lactide or Meso-lactide). Despite LA can be produced by chemical processes, almost 90% of the total LA is obtained by bacterial fermentation [29] and the remaining portion is produced synthetically by the hydrolysis of lactonitrile [30]. The chemical synthesis route usually produces D-LA

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and LLA, whereas an optically pure LA can be obtained by microbial fermentation of agricultural biomasses, depending on the strain selected [31–33]. Among the methods, the microbial fermentation production of lactic acid has gained more attention thanks to being environmentally friendly. Sugars in pure form (glucose, sucrose, lactose) or sugar-containing materials like whey, sugarcane and cassava bagasse, potato, tapioca, wheat, and barley could be a source for microbial fermentation [34]. There are three methods for the production of high molecular weight PLA, the direct polycondensation, the azeotropic dehydrative condensation and the polymerization through lactide formation (Figure 1).

Figure 1. Three methods for the production of high molecular weight PLA.

The most cost-effective way to synthesize PLA is the direct polycondensation, although it is hard to remove solvent and, as a consequence, a low-intermediate molecular weight poly(lactic acid) is obtained. Ring-opening polymerization (ROP) is the most common method to achieve high molecular weight polymers [35]. In this process, the LA cyclic dimer (lactide) opens in the presence of a catalyst. Although the process is quite complex and expensive, it results in high molecular weight PLA. The configuration of the monomer affects the polymer melting point as well as the rate and extent of polymer crystallization. On the other side, the other processing parameters, such as temperature, annealing time, crystallization rate, and extent, drastically influence the chemical-physical properties of the final polymer performances. In general, commercially produced PLA contains 98–99% of PLLA and less than 1–2% PDLA. The crystallinity of PLLA is about 37%, while the glass transition temperature is in the range of 50°C - 60°C and the melting point between 170°C -

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180°C. On the other hand, the PLLA/PDLA blend shows a higher melting temperature and hydrolysis resistance than pure PLLA or PLDA. The degradation rate is controlled by modifying the crystallinity. Indeed, the degradation rate decreased by increasing the percentage of crystallinity. However, it also depends on other parameters such as molecular weight, temperature, pH, relative humidity as well as on the presence of additives such as plasticizers. PLA is becoming an alternative for green food packaging material because, as widely confirmed by literature data, it was found that for several applications, its performances were better than synthetic plastic materials [36]. Indeed, due to its high molecular weight, water solubility resistance, good processability, by means of common thermoforming routes used for oil-derived thermoplastic materials, and biodegradability, PLA is a challenging and promising alternative to traditional food packaging material [37]. PLA shows the tensile strength modulus, flavor and odor barrier of polyethylene and PET or flexible PVC, the temperature stability and processability of polystyrene, as well as the printability of polyethylene. PLA can be processed in the form of films, containers, and coatings for paper and paper boards. As concerning active packaging, several types of research have been published and patented regarding the use of PLA as a polymer matrix of antimicrobial package [38]. The antimicrobial properties of films depend on the processing methods, antimicrobial agents' properties such as their polarity, molecular weight, compatibility, thermal stability, and kind of food. Tawakkal et al. listed the wide range of substances such as organic acids, bacteriocins (nisin), plant extracts (for example, lemon extract), essential oils and extracts (thymol), enzymes (lysozyme), chelating agents (EDTA), metals (for example, silver) incorporated into PLA polymer matrix as antimicrobial agents [39]. Among them, natural antimicrobial agents like nisin, lysozyme, and silver zeolite, incorporated into or coated on the surface of PLA, showed inhibitory activity against Listeria monocytogenes, Escherichia coli, Staphylococcus aureus, and Micrococcus lysodeikticus [39–42]. The growing interest in using PLA as an active antimicrobial package results from the consumer demands to avoid any preservatives inside the food.

Poly Butylene Succinate (PBS) Poly(butylene succinate) (PBS) is one of the most promising biodegradable and compostable thermoplastic polyesters synthesized by polycondensation of dimethyl succinate and 1,4-butanediol (Figure 2). Succinic acid is a colorless crystalline solid, soluble in water and derived from fossil raw materials and bio-based feedstocks. The chemical synthesis of succinic acid occurs via the catalytic hydrogenation of maleic acid or its anhydride. On the other hand, bio-based production of succinic acid happens through the bacteria fermentation of feedstocks such as cane molasses, whey, glycerol, lignocellulosic hydrolyzates, and cereals and following conversion of glucose to succinic acid. There are several routes for the synthesis of PBS. The first one consists of a two-step method, esterification, and polymerization for the synthesis of average molecular weight (Mw) PBS; it starts with the catalytic reaction of dimethyl succinate with 1,4-butanediol followed by polycondensation in melt or solution. Titanium (IV) butoxide is commonly used as a catalyst in this method, and the reaction occurs at 180 °C. The direct polymerization with a catalyst to obtain high molecular weight PBS can occur by direct melt polymerization in which PBS is produced

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from dicarboxylic acid and diol or by the solution polymerization in which all reactants are dissolved in a solvent (xylene or decaline). The polymerization by condensation route finalized to obtain high molecular weight polymer requires the use of a chain extender, such as biscaprolactamate and bisoxazoline, whose two reactive functional groups are able to couple two PBS macromolecular chains by increasing its molecular weight and, of course, its thermal and mechanical properties. Bionolle® company, for instance, synthesizes PBS by melt condensation method followed by chain extensions. Hexing chemical and Anhui produce PBS by direct polycondensation [43]. In addition, it is a highly crystalline polyester with its melting point at around 115 °C, glass temperature (Tg) in the interval between -45 to -10 °C, and heat distortion temperature at 97 °C; these parameters are crucial for PBS applications at high temperatures; in addition, they will match with the ones of common thermoplastic polymers coming from fossil sources, such as PP. Even mechanical performances deserve mentioning; the yield tensile strength of unoriented specimens reaches 30–35 MPa similarly to polypropilene, whereas its elongation at break is about 560% (PBS 1000 BIONOLLE) comparable to LDPE strain at the break; finally, its Young’s modulus ranging between 300–500 MP resembles that of polypropylene, depending on the degree of crystallinity. Being a thermoplastic polymer, PBS has various potential applications. It can be processed like other commodity plastics by many techniques such as blown films, fibers spinning, injection molding, thermoforming, or blow molding. For instance, itis possible to use PBS in electronics and other consumer goods applications, such as thin systems for packaging bags, netting and foam trays for fresh food (meat, fish, vegetables, and fruits), and cutlery, filaments, blown bottles, hygiene commodities, Thanks to its biodegradability (according to DIN EN 13432), PBS can also be used for applications where compostability is important, i.e., in agricultural mulching films. Moreover, it is widely reported the exploitation of PBS in active food packaging. Petchwattana et al. evidenced the bioactivity of films based on PBS and ZnO [44]. Mallardo et al. included b-cyclodextrin/D-limonene complex inside Poly(butylene succinate] to realize antimicrobial films for packaging [45].

Figure 2. Poly (butylene succinate) structure.

Chitosan Chitin or poly-β-(1→4)-N-acetyl-D-glucosamine is the most abundant natural marine biopolymer with potential production of about one trillion tons per year. The main chitin derivative is chitosan or β-(l-4)-2-amino-2-deoxy-D-glucopyranose, a linear polysaccharide including N-acetyl-glucosamine and N -glucosamine units, obtained through N-deacetylation of chitin (Figure 3) [4]. Chitosan is the second most abundant polysaccharide in the world, and since it can be obtained from primary wastes of crustacean shellfishes industry.

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Therefore, it is renewable and easily commercially available. From this point of view, chitosan could be a low-cost material, a worthy point if considering its application in packaging. The degree of deacetylation (DDA) depends on the number of N-glucosamine units and is responsible for the maim chitosan physicochemical properties and immunological activity. Chitosan is biocompatible, biodegradable, non-toxic, physiologically inert, and has a remarkable affinity to proteins, hemostatic, fungistatic, antitumor anticholesteremic activities. For this reason, it is widely used in several application fields, such as biomedical and drug delivery sectors [46, 47]. It has been approved as a food additive in Korea and Japan since 1995 and 1983, respectively. Shrimp-derived chitosan was submitted to the US Food and Drug Administration (FDA) and considered as safe for use in foods (GRAS) since 2001 [48]. It shows film-forming ability and, due to its carbocationic behavior, displays antimicrobial activity against a wide range of foodborne filamentous fungi, yeast, and gram-negative and gram-positive bacteria. These worthy chemico-physical and intrinsic properties have made chitosan one of the most used biopolymers for active packaging with the ability to inhibit the growth of microorganisms and improve food safety [49]. Chitosan is a versatile polysaccharide whose applications in food packaging could be exploited as films and coatings with good mechanical properties, suitable oxygen permeability, and excellent antimicrobial activity. Nevertheless, chitosan is not a thermoplastic material since it degrades before its melting point; therefore, it cannot be extruded or molded, and the films cannot be heat-sealed. This behavior drastically narrows its application window. For this reason, the blending of chitosan with other thermoplastic biopolymers, such as PLA, PBS, or starch-based polymer, could be a valid strategy to overcome this drawback [50]. Actually, the polysaccharide could be or added as a coating of the outer layer of the package or included inside the packaging system in the form of bioactive chitosan micro-nano particles.

Figure 3. Chitin (a) and chitosan (b) structure.

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Mater-Bi Among biopolymers, starch is one of the most widely investigated, as it is widely available and easily modified to get a thermoplastic polymer [51]. Nevertheless, due to the hydrophilic nature, responsible for fast degradation via hydrolysis, thermoplastic starch applications are limited [52]. To overcome this experimental drawback, starch is generally modified by blending with synthetic polymers, such as polyesters or vinyl alcohol copolymers. This approach has been adopted by Novamont under the Mater-Bi trademark [53]. Target markets of Mater-Bi include packaging materials, disposable cutlery, consumer goods, and agricultural tools [54]. There are several grades of Mater-Bi showing different properties, as well as biodegradation and compostability kinetics. According to the company, the highest degradation rate is under industrial composting and anaerobic bacteria. There are five classes of Mater-Bi for different applications [53]. Class Z, made with thermoplastic starch and poly-ɛ-caprolactone and is used for bags, nets, paper lamination, mulching films, twines, wrapping film. Class Y, including cellulose derivatives, is used as cutlery, flower pots, seedling planter trays, golf tees, and pens. Class V finds application in packaging foams and soluble cotton swabs as a replacement for polystyrene. Class A and N, based on starch and ethylene-vinyl alcohol and poly(butylene adipate-coterephthalate), respectively, are used where mechanical resistance of the films has to be assured for long time-life [55]. To achieve an enhancement in processability and performance, Mater-Bi-based composites have been prepared by using different cellulose fibers [56–60]. As a matter of fact, the improvement of mechanical properties, decreasing of water sorption and tailoring of biodegradation kinetics have been observed due to the fiber presence [56]. Thermoplastic starch relies on specific additives to obtain products that fulfill the market demands [61]. Several categories of natural and synthetic additives are available, such as processing aids, plasticizers, stabilizers, and antibacterial additives.

BIOACTIVE NATURAL METABOLITES IN BIOPOLYMERS AS BAKERY BIOACTIVE FOOD PACKAGING MATERIALS In the latest study about the application of secondary active natural metabolites in the food packaging industry, as a preliminary investigation, Valerio et al. examined the potential antifungal properties of 12 bacterial, fungi, and plant metabolites against P. roqueforti and A. niger [5]. Among them, ungeremine and α-costic acid showed the most promising fungicide properties against both fungal strains. Ungeremine showed MIC90 lower than 0.003 mg/mL after 48 h of incubation and 0.025 mg/mL at 72 h against P. roqueforti. The MIC90 value for A. niger was 0.2 mg/mL at 48 h for both compounds. The α-costic acid generally showed MIC values at 48 and 72 h higher than ungermine [5]. In another study, Santagata et al. evidenced the cavoxin inhibitory effect against P. roqueforti IBT18687 and A. niger ITEM5132; they compared the cavoxin activity with calcium propionate, which is a chemical preservative for bakery products (European directive, 1995/2/CE). The results indicated that cavoxin influenced the growth of both fungal strains lowering 100 fold their concentration with respect to calcium propionate; they could also highlight cavoxin activity up to 72 hours

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[62]. The second part of this section will be focused on the discussion of the bioactivity of each metabolite opportunely vehicled by a biopolymer matrix.

Ungeremine Ungeremine (UNG) is betaine type alkaloids isolated from Pancratium maritimim L., a known species of Amaryllidaceae collected on Egypt's northern coasts [63]. It can also be synthesized by SeO2 oxidation of lycorine, which is the main Amaryllideacea alkaloids (Figure 4) [63]. Sternbergia lutea Ker Gawl (Amaryllidaceae) is the best source of lycorine and wild grow on the coasts of the Apulia region in South Italy [64].

Figure 4. The synthesis of ungeremine by lycorine oxidation.

Ungermine is thermally stable; this feature is essential for the formulation of metabolite into the package system because most of the industrial processing methods used for the formulation, or incorporation of an additive into the packaging system, such as extrusion, film blowing, and compression molding, need high processing temperatures. However, UNG is a zwitterion, and the presence of positive and negative charges acts as an obstacle for its direct formulation into the polymer matrices. Indeed, the attractive and repulsive force between UNG molecules resulted in a heterogeneous dispersion of the molecules in the matrices. Figure 6 showed some of the unsuccessful trials in which UNG was directly included inside the polymer matrices. In order to solve this problem, Moeini et al, encapsulated ungermine into chitosan polymer matrix by using sodium tripolyphosphate (TPP) as the crosslinking agent and prepared microbeads in order to investigate their properties against P. roqueforti. They investigated the effect of pH and TPP concentration on chemico-physical properties of the films [65]. The result showed that the releasing kinetics of UNG from the chitosan-TPP microbeads was directly related to the different pH. In the next step of this work, the same authors prepared sub-micro particles of chitosan-TPP-UNG and formulated it into MBi polymer matrix in two different ratios; the composite blends were prepared by extrusion, and the films were obtained by compression molding. The antifungal activity of the films was tested against P. roqueforti [66]. The microparticles of chitosan-TPP -ungeremine were homogeneously distributed into the polymeric matrix, as evidenced by morphological analysis detailed in the paper cited above. Due to the interaction between the polysaccharide components of the microparticles, i.e., chitosan and the starch fraction of MBi, the rigidity and tensile strength of the films increased at the expense of ductility. In addition, the microparticles could improve water permeability and decrease oxygen permeability. The antimicrobial test was performed in different media (Bread Extract Broth (BEB) and Potato

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dextrose agar (PDA)) at different pH (4.9, 5.7, and 6.2). Activated films showed three days of inhibition against P. roqueforti in both media at different pH [66]. A different approach consisted in the inclusion of UNG as a core of PLA/PEG nanofibers by using electrospinning [67]. The kinetics of releasing depended on PEG concentration, even if traces of UNG were found in PLA too. Thus, the authors could hypothesize a structure in which the high concentration of UNG zwitterions resulted in a bolded charged spherical agglomeration distributed inside the nanofibers [67].

Cavoxin Cavoxin (CVX), phytopathogenic pentasubstituted benzoic acid, along with cavoxone, a close chroman-4-one (Figure 5), are produced in vitro culture by Phomacava isolated from chestnut (Castaneaspp) [68]. As already mentioned above, cavoxin is an antifungal metabolite particularly active against both A. niger and P. roqueforti. On the other hand, a quantitative analysis was needed for the packaging application to determine the most suitable method for having a larger amount of cavoxin among two culture methods (stirred and static) for Phoma cava. Consequently, Masi et al. developed a precise and quick quantitative HPLC method to quantify CVX in different fungal culture filtrates. They proved that the amount of CVX produced when the fungus was grown in stirred culture was significantly higher than the static condition [69]. The main drawback of cavoxin for the food packaging application is its thermal instability. Indeed, at high temperatures, cavoxin converts to cavoxone, which is biologically inert. Therefore, studies mainly focus on cavoxin and its potential application in different fields [70, 71]. As far as packaging systems are concerned, Santagata et al. formulated cavoxin into polybutylene succinate (PBS), and films from casting were obtained. PBS-CVX films evidenced 72 h inhibition against the two food contaminants A. niger and P. roqueforti [62].

Figure 5. Cavoxin (a), and Cavoxone (b) structures.

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α-Costic Acid The last metabolite recently considered in the smart packaging system because of its biological activity against P. roqueforti and A. niger is α-costic acid (α-CA) (Figure 6), a sesquiterpenoid acid isolated from Dittrichia viscosa (syn. of Inula viscosa), a native Mediterranean basin plant [72]. Besides α-CA, four other bioactive metabolites, characterized as new bi and tricyclic new phytotoxins belonging to different sesquiterpene subgroups and named inuloxins A-D, were extracted from the aerial part of the plant [72]. α-CA was formulated into PLA polymer matrix by casting from solvent. In this case, due to the strong physical interaction occurring between α-CA and PLA, proved by NMR and FTIR-ATR, no antimicrobial activity was observed in the formulated biofilm. On the other side, a worthy plasticization effect was exploited by α-CA, as evidenced by a significant decrease of PLA Tg, following to the increase of polymer chain mobility, and by an improved PLA mechanical performances [73].

Figure 6. α-Costic acid structure.

INDUSTRIAL CONSTRAINT Although the wide range of benefits comes from the exploitation of plant metabolites as bioactive compounds, which are vehicles by biodegradable polymer matrices, several constraints limited the industrial development of this novel, eco-friendly kind of bioactive package (Figure 7). The main drawback is represented by the likely toxicity of these plants; indeed, deep and proper investigations are required in order to evaluate the interaction between food components and doped biopolymers during processing and storage; metabolite migration from the package to food could occur and, moreover, no studies, except for some metabolites, have yet been given on plant cytotoxicity. However, in this regard, the authors are deeply engaged, experimental texts are in progress, and the first results will be objects of forthcoming papers. The metabolites are extracted from a plant belonging to nature and, for this reason, recognized as renewable sources; anyway, the plant availability and harvesting are often correlated to environmental conditions, to the age of the plant, the harvesting season, as well as to the plant healthy, indeed, sometimes, pests and diseases can alter the growth of the plant.

Figure 7. Industrial constraints of natural metabolites usage in the industrial segment.

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Figure 8. Commercial appraisal of raw material used for food packaging.

In addition, the metabolite extraction and purification processes are quite expensive if compared to the final amount of bioactive compound obtained. All these aspects seriously limit the pilot and industrial scaling up of the whole process. This is why the current scientific line is increasingly geared towards new extractive methods mainly based on the drastic reduction of solvents and methodology steps while drawing attention to greener actions. In this way, the whole process will be addressed towards an eco-sustainable, cost-effective, and reproducible approach. Another worthy concern is related to metabolite thermal resistance. Actually, this intrinsic property represents a focal issue since all the industrial processing methods used for the packaging industry occur at high temperatures. Hence, all the metabolite compounds included in polymer matrices should be thermally stable and, overall, preserving their bioactivity even at high temperatures.

CONCLUSION Antimicrobial packaging is a promising form of active food packaging successfully used to increase the shelf life of foods by protecting them from microbial infection. It matches the consumer demands to provide safe and high-quality products. Petroleum-based polymers are still the most commonly used matrices for food packaging material since their excellent performance, easy processing technology, and, overall, low-cost. Anyway, the growing environmental awareness has led to the development of biodegradable packaging based on raw materials coming from the natural feedstock, marine sources, and by-products of the agro-food industry. Biopolymers help in reducing the environmental impact of plastic production and processing since they are renewable, easily available, and, in a way, costeffective sources. Biopolymer-based antimicrobial films are based on a biodegradable polymeric matrix containing natural bioactive compounds. In this chapter, a brief screening of

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the main exploited biopolymers in food packaging, such as PLA, PBS, chitosan, and MBi has been provided together with their main performances and ability to incorporate bioactive metabolites coming from plants, such as ungeremine, and α-costic acid, and fungi as cavoxin from The antibacterial properties against two fungi contaminating bakery products, Penicillium roqueforti and Aspergillus niger, have been successfully proved and detailed, together with the releasing kinetics and chemico-physical properties of the films and composites. At different concentrations, the natural additives evidence suitable thermal stability able to preserve their structure and antibacterial properties even at high temperature and different pH while generally preserved the mechanical properties of the material. Moreover, the films and composites evidenced prolonged antibacterial properties, enabling producing packaging materials with tunable bioactivity. Nevertheless, some drawbacks, far from negligible, have been adequately highlighted, severely restricting they are scaling up from laboratory to pilot and industrial scale. Indeed, more in-depth investigations are due to overcome general plant toxicity and to improve the green and cost-safe approach for metabolite extraction. Thus, green, environmentallyfriendly, biodegradable, low cost and easy-to-obtain polymers should be ideal candidate substrate materials for biodegradable food packaging.

ACKNOWLEDGMENTS The authors wish to thank the European Union (FSE, PON Ricerca e Innovazione 20142020, Azione I.1 “Dottorati Innovativi con caratterizzazione Industriale,” for funding a Ph.D. grant to Arash Moeini. The authors MM and GS wish to thank European Union’s Horizon 2020 research and innovation program under grant agreement No. 860407 BIO-PLASTICS EUROPE (https://bioplasticseurope.eu/)

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In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 19

REGENERATED CELLULOSE SHEET AS NATURAL TISSUE TO MAKE BIODEGRADABLE BABY DIAPERS Alessandro Gagliardini and Pietro Febo R&D Unit Atertek, Pescara, Italy

ABSTRACT The easiest way to make the diaper more biodegradable is to increase its content in cellulosic fibers such as cellulose fluff and cotton. However, these fibers have limits imposed by nature as the size and shape of the cellulose fluff and cotton fibers that could not allow the access to modern nonwoven fabrics manufacturing technologies. Regenerated cellulose fibers are not subjected to these bottlenecks as they can be produced in the required sizes and shapes to permit their use into non-woven manufacturing processes. In addition, over the years the manufacture of regenerated cellulose fibers have been made more and more efficient and clean, starting from a responsible management of forests or facilitating the use of recycled cellulosic materials.

Keywords: non-woven, topsheet, ADL (Acquisition Distribution Layer), baby diaper, regenerated cellulose, viscose, lyocell, circular economy, PLA (Poly Lactic Acid), PHA (Poly Hydroxy Alkanoates), PBS (Poly Butylene Succinate), PBAT (PolyButylene Adipate Terephthalate), CMC (Carboxy Methyl Cellulose)

INTRODUCTION An infant needs up to 7000 diaper changes in his first three years of life. The 450 billion disposable diapers used each year contribute nearly 77 million tons of solid waste to landfills. It is estimated that a disposable diaper takes at least 500 years to degrade [1]. At present, the only alternative to landfill is incineration. Moreover, the end of life of the fossil-based products is causing much concern because of their difficult post-consumer management. In

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the case of sanitary pads, incineration and landfill is still much significant. Although the problem is quite complex and necessitates a holistic approach, bioplastics, biopolymers and biomolecules can certainly allow to outperform fossil-based products not only in biocompatibility but also in their end of life management. In recent times another potential solution to make the disposable baby diaper more sustainable has been to recycle it after usage using innovative and dedicated processes [2-5]. Modern baby diapers products have a layered construction, which allows the transfer and distribution of urine to an absorbent core structure where it is locked in. The topsheet closest to the skin is made of soft nonwoven fabric and transfers urine quickly to the layers underneath. The distribution layer receives the urine flow and transfers it on to the absorbent core. The absorbent core structure is the key component and is made out of a mixture of cellulose pulp and superabsorbent polymers. The backsheet is typically made of “breathable” polyethylene film or a nonwoven and film composite which prevents wetness transfer to the bed or clothes. According to EDANA [6] the average baby diaper composition is reported in Figure 1.

Figure 1. Average baby diaper composition from EDANA [2].

A biodegradable baby diaper made with bio-materials (e.g., from sustainable and renewable sources) could lead to a significant reduction to these impacts. In 2000 the Mexican company Absormex created a disposable “bioactive” diaper that degraded 200 percent faster than ordinary baby diapers. The technology is based on a catalyst additive added to the plastic to enhance biodegradation [7, 8]. However, in this case the plastic (mainly polyolefins), adhesives, elastics and superabsorbent polymer remain fossil-based. Cellulosic materials, e.g., cellulose pulp and cotton can be used as absorbent materials for the baby diaper’s core as well in some types of nonwoven fabrics such as air-laid nonwovens and paper sheets. However there are types of non-woven fabrics where the characteristics of the cellulose or cotton pulp do not allow their use or allow a marginal use, as in the case of

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non-woven fabrics manufactured with spunlace, air-though bonded technologies, thermal bonded, resin bonded, needle-punched and spunbond [9].

BIODEGRADABLE BABY DIAPERS Biodegradable baby diapers can be made with existing technologies and there are several examples on the market, for example the Naturaè in the Italian market [10]. Looking to this baby diaper it is claimed to be compostable according to UNI EN 13432:2000 and EN 14995:200. Its composition is based on a fibrous topsheet made with PLA fibers, an absorbent core made with cellulose fluff pulp and a bio-based superassorbent polymer and a backsheet based on a compostable plastic film. To note, looking the market offer and patent literature most of the bio-based superabsorbent polymers are based on starch or cellulose derivatives such as crosslinked carboxymethyl cellulose. Most of the compostable films produced in Europe are based on biodegradable polyesters such as Ecovio from BASF and MaterBi from Novamont [11, 12]. The absorbent core is the key element for urine absorption and safe retention into the baby diaper. In today’s diapers two absorbent materials are used in combination to optimize absorbency: cellulose pulp fluff fibers and superabsorbent particles. While cellulose fluff pulp is biodegradable the superabsorbent is not. Polyacrylates, obtained from the polymerization of monomers such as acrylic acids and acrylamides (non -renewable sources), constitute a major portion of the commercially available superabsorbents [13, 14]. However their biodegradability is questionable, especially for high molecular weight polymers. Polyacrylates generally contain small amounts of residual monomeric starting materials (i.e., acrylic acids and acrylamides) possessing both toxic and allergenic potential. Superabsorbent polysaccharide-based grafted-polymers are obtained via the grafting of an unsaturated monomer (acrylonitrile, acrylic acid, acrylamide) onto starch, or, less frequently, cellulose. The so-obtained polymers, also called “super slurper,” have shown a water absorption ranging from 700 to 5300 g/g in deionized water, and up to 140 g/g in a 0.9% saline solution. Despite their very high water absorption capability, the grafted polysaccharides, prepared by graft polymerization, are not known to be biodegradable or hypoallergenic, nor are they prepared from renewable sources. CMC and carboxymethylstarch (CMS) [15] constitute other known polysaccharide-based superabsorbents. Cost has always been an issue with these superabsorbents, and they can therefore not be used alone in order to compete with the synthetic polymers. Natural polysaccharide-based superabsorbents constitute a very attractive class of polymers, considering that they can be biodegradable and hypoallergenic, in addition to the fact that they are made from renewable sources such as starch. An example of such kind of natural-based, cross-linked starch-based superabsorbent is described in patent [16].

REGENERATED CELLULOSE FIBERS The first attempts to dissolve cellulose or cellulose containing material such as cotton were described about 150 years ago [17]. Since then a huge variety of cellulose solvents have

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been developed or discovered. Thus the first man-made fiber, Chardonnet silk [18] was obtained with a soluble cellulose derivative and the first man-made plastics, Parkesine [19] and Celluloid [20]were prepared via the same modification reaction. Rayon is a manufactured fiber made from natural resources such as wood and cotton that are regenerated as cellulose fiber. More in particular rayon is classified as “a fiber formed by regenerating natural materials into a usable form” [21]. Specific type of rayon includes viscose, modal and lyocell, each of which differs in the manufacturing process and the properties of the finished product. Rayon is made from purified cellulose, harvested primarily from wood pulp, which is chemically converted into a soluble compound. It is then dissolved and forced through a spinneret to produce filaments which are chemically solidified, resulting in fibers of nearly pure cellulose. The first method to produce true regenerated cellulose was the xanthate method. In the xanthate method cotton or wood cellulose can be dissolved following treatment with alkali and carbon disulphide [22]. The viscous yellow solution (called “viscose”) could be coagulated in an ammonium sulphate bath and then converted back to pure cellulose using dilute sulphuric acid. Using a spinning bath containing a mixture of sulphuric acid and a salt. Despite its environmental problems caused by the by-products and the volatile and odoriferous CS2 solvent, the viscose process is still the most important method for the shaping of cellulose. The xanthate viscous solution can be used to make both rayon and cellophane. Rayon has historically had many environmental issues, especially air and water pollution and depleted forest cover. Recently rayon producers have focused on sourcing from 100% certified forests and applying closed-loop manufacturing technologies, limiting the release of pollutants to water and air. Rayon from leading manufacturers if fully renewable, biodegradable, has reduced the use of water and chemicals, and won’t release microfibers that collect in waterways and oceans [23]. In particular regarding biodegradability in soil burial and sewage sludge rayon was found to be more biodegradable than cotton being compostable and biodegradable in soil, aqueous and marine conditions [23, 24]. Lyocell process relies on dissolution of cellulose products in a solvent, Nmethylmorpholine N-oxide. The process starts with woody sources of cellulose and involves dry jet-wet spinning. It was developed at the now defunct American Enka and Courtlands Fibers. Lensing’s Tencel brand is an example of currently available lyocell fibers [25-27]. Another advantage of rayon is its price advantage compared to cotton and natural or fossil based biodegradable fibers such as PLA, PHA, PBAT and PBS based fibers. Rayon prices do vary with changes in supply and demand in the market; however rayon generally has a price advantage over other natural fibers such as cotton and silk [28]. Regards physical structure of rayon staple fibers used in the manufacture of baby diapers nonwovens, their size generally vary from 0.9 to 4 dtex and their length from 2 to more than 60 mm. Rayon can be mechanically or chemically crimped. Regards fibers shape, viscose fibers are available at different shapes, e.g., irregular, round, multilobal. Rayon fibers are naturally very bright, but the addition of delustering pigments cuts down on this natural brightness [20]. In Table 1 are reported the main characteristics and applications of rayon fibers used into baby diapers nonwovens:

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Table 1. Rayon fibers characteristics and application in baby diapers nonwovens Nonwoven manufacturing technology Spunlacing and needle-punching processes

Typical titer and length of rayon fibers 0.9 to 6.7 dtex and 25 to 60 mm

Specialty papers both via wet-laid and air-laid processes

0.5 to 1.7 dtex and 3 to 12 mm

Typical use into the baby diaper or other hygienic products Diaper topsheet, acquisition distribution layer and core, mainly for femcare products Acquisition and distribution layer and absorbent core

Regards the shape of fibers, the hollow shaped fibers are claimed to be more absorbent while the multilobal fibers (e.g., the trilobal) may have both absorbency benefits and can improve coverage and uniformity of nonwovens while maintaining equivalent fabric strength and softness.

Figure 2. Typical viscose fibers shape, retrieved from [29].

Figure 3. Typical Lyocell fiber shape, retrieved from [30].

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Figure 4. Hollow viscose fiber retrieved from [31].

Figure 5. Trilobal viscose fiber retrieved from [32].

END OF LIFE OF USED BABY DIAPERS The waste disposal for post-consumer diapers (or commonly called “soiled” diapers) is a significant environmental problem as explained in the introduction. The proven technologies so far have always been the use of direct incineration for energy recovery (popular in Europe) or converting soiled diapers into refuse derived fuel to generate heat in industrial applications. Biodegradable baby diapers can be submitted to a composting facility. To note, the components of the diaper are mainly made up of carbon, hydrogen and oxygen, so that the decomposition of the diaper could be seen as a sort of cold combustion not capable of bringing useful elements to the compost. However, into used diapers is present bodily secretion such as urine, feces and menses blood, materials that after proper decomposition treatment could increase the quality of the compost. To further improve the quality of the compost from soiled biodegradable baby diapers a relatively simple modification would be to substitute sodium hydroxide used during the manufacture of superabsorbents (both

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conventional and bio-based ones) to neutralize carboxylic groups with potassium hydroxide. In this simple way the quality of the compost could be enriched with potassium, a valuable plant nutrient instead of sodium. Regarding baby diaper recycling, a few technologies that recycle diapers are under evaluation such as Knowaste, TerraCycle and FaterSmart [4, 5], but these technologies were (so far) never economically sustainable by themselves or able to manage large enough volumes to justify their immediate cloning to multiple locations worldwide. Most of these initiatives are in the development “demo” phase and the future will tell about their feasibility at large scale.

Figure 6. Baby diaper recycling process scheme, retrieved from [4].

In particular the best-known prototype factories for post-consumer diaper recycling are those operated by P&G-Fater in Treviso, Italy, a process using a rotating autoclave and raw material separation with a mesh [5]. Another interesting post-consumer project is using the biomass in the soiled diapers for hydrogen generation, and ozone bleaching to recycle the pulp, proposed by Unicharm [33]. In 2015, the company overcame a major hurdle by creating a system that extracts high-quality pulp which is safe and recyclable from waste diapers by decomposing them with water, then sterilizing the byproduct with ozone. The system can recover several hundred kilograms of high-quality pulp from 4 tons of used diapers while emitting 30% less greenhouse gases than incineration. Recently the company developed a way to use microbial fuel cells to generate power using waste water from the recycling process. A microbial fuel cell - a bioelectrical system that contains bacteria in the negative electrode - generates power through bacteria’s ability to extract electrons from food sources, such as organic materials, or in the case of dirty diapers, from waste water produced during recycling. All recycling processes have a potential issue: for a typical diaper recycling process to work, it needs to separate all plastic components, like polyethylene and polypropylene into pellets that can be used later in other industries, such as plastic injection, to mention an example. For that to work in the most efficient way, they need to feed the machine with only synthetic products, anything else could be detrimental to the quality of the pellets, or an additional separation process needs to be added.

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Figure 7. Unicharm’s diaper recycling process.

Another emergent consumer’s trend is to prefer the use of natural materials such as plantbased components, starch-based films, PLA, different kind of viscose (from bamboo, pine or eucalyptus) and the use of biodegradable SAPs. Adding hydrophobic cotton into the mix with the nonwoven used for the topsheet or in the backsheet is not really a big problem with regards to recycling because the cotton can be extracted and combined with the cellulose as a single output. However, mixing natural films or plant-based plastics with the synthetics may contaminate the resulting plastics or can make the recycling process more complex. The problem is that we will need to separate plant-based products from those made with synthetic components for the post-consumer recycling process to work efficiently.

CONCLUSION The circular economy [34] is an economic system aimed at eliminating waste and the continual use of resources. Circular systems employ reuse, sharing, repair, refurbishment, remanufacturing and recycling to create a close-loop system, minimising the use of resource inputs and the creation of waste, pollution and carbon emissions [35]. The circular economy aims to keep products, equipment and infrastructure in use for longer, thus improving the productivity of these resources. All ‘waste’ should become ‘food’ for another process: either a by-product or recovered resource for another industrial process, or as regenerative resources for nature, e.g., compost. This regenerative approach is in contrast to the traditional linear economy, which has a ‘take, make, dispose’ model of production. [36]. Regenerated cellulosic fibers, e.g., rayon, can be a key component to make the baby diaper biodegradable and bio-based. In particular the regenerated cellulosic fibers are very versatile fibers that can be tailored to be compatible with most of the modern nonwoven technologies. Regenerated cellulosic fibers are 100% biobased and biodegradable. Last but not least their price is significant inferior compared to other bio-based or biodegradable fibers such as those based on PLA, PBS, PBAT, polycaprolactone etc. Depending on the recycling system adopted rayon fibers could be reused as fibers or they could be re-dissolved to make novel rayon fibers [37]. However “circularity” or regenerated cellulose fibers depend on the disposal of soiled baby diapers. If diapers are incinerated or landfilled any chance to recover the rayon (or any

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other part of the diaper) will be lost. In this case the sustainability advantages are due respectively to the fact that rayon is bio-based and biodegradable. Novel processes under development in Europe, US and Japan [4, 5, 33] open home for a potential reuse of the baby diaper’s rayon. In this case the rayon could be recovered as a fiber and recycled as a “secondary raw material” e.g., to make paper, cardboard, textiles, or it could be dissolved to make novel viscose returning to the loop.

CONFLICTS OF INTEREST The authors whose names are listed immediately below certify that they have NO affiliations with or involvement in any organization or entity with any financial interest (such as honoraria; educational grants; participation in speakers’ bureaus; membership, employment, consultancies, stock ownership, or other equity interest; and expert testimony or patent-licensing arrangements), or non-financial interest (such as personal or professional relationships, affiliations, knowledge or beliefs) in the subject matter or materials discussed in this manuscript.

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http://www.worldwatch.org/system/files/M-A%2007%20Life-cycle.pdf. Kim, K. S. and Cho, H. S. (2017) Pilot Trial on Separation Condition for Diaper Recycling, Waste Manag. 67:11-19. Patent EP 2596811 B1, “Apparatus and Process for Sterilizing Absorbent Sanitary Products.” https://www.knowaste.com/. https://www.fatersmart.com/en/how-it-works-recycling-plant. edana-sustainability-report-baby-diapers-and-incontinence-products---2005.pdf. http//www.epi-global.com/en/epi-technology.php. Patent US 2001003797A1, “Degradable Disposable Diaper.” Ajmeri J. R., Ajmeri C. J., “Developments in the use of Nonwovens for Disposable Hygiene Products;” Advances in Technical Nonwovens, 2016, pages 473-496. Naturaè compostable Baby diapers: https://www.naturae.com/ecopannolino/come_ fatto/. Mater-bi: http://www.novamont.com/eng/mater-bi (12/11/2017). Ecovio: https://www.plasticsportal.net/wa/plasticsEU/portal/show/content/products/ biodegradable_plastics/ecovio (12/11/2017). Kabiri, K. (2003) Synthesis of fast-swelling superabsorbent hydrogels: effect of crosslinker type and concentration on porosity and absorption rate. European Polymer Journal. 39 (7): 1341–1348. Bucholz, F. L., Graham, A. T. (1998) Modern Superabsorbent Polymer Technology; Eds., Wiley-VCH, New York. Patent US 8,710,212 B2. British Patent 283, 1855.

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Alessandro Gagliardini and Pietro Febo French Patent 165,349 (1884). British Patent 235, 1856. US Patent 50,359, 1865. Swicofil company website, “Viscose CV” (https://www.swicofil.com/commerce/ products/viscose/278/introduction) (accessed on October 4th 2020). British Patent 8,700, 1892. British Patent 10094, 1906. Park, C. H., Kang, Y. K. and Im, S. S. (2004) Biodegradability of Cellulose Fabrics. Journal of Applied Polymer Science. 94: 248. https://www.edana.org/docs/default-source/product-stewardship/biodegradability-ofviscose.pdf?sfvrsn=32f4fbee_2. US Patent 3,508,941, 1970. US Patent 4,145,532, 1979. Nechwatal, A., Michels, C., Kosan, B., Nicolai, M. (2004) Cellulose 11: 265. Wirz, M. (January 7, 2011) “The Touch, The Feel – Of Rayon,” Wall Street Journal, Money and Investment section, p. c1. http://kelheim-fibres.com/en/viskosefaser/danufil-medical/. Chen, J., “Synthetic Textile Fibers,” in Textiles and Fashion, 2015. http://kelheim-fibres.com/en/viskosefaser/bramante/. http://kelheim-fibres.com/en/viskosefaser/galaxy/. https://asia.nikkei.com/Business/Unicharm-turning-dirty-diapers-into-clean-energy. “Circularity Indicators.” www.ellenmacarthurfoundation.org. Geissdoerfer, M., Savaget, P., Bocken, N. M. P., Hultink, E. J. (2017) The Circular Economy – A new sustainability paradigm? Journal of Cleaner Production. 143: 757– 768. Towards the Circular Economy: an economic and business rationale for an accelerated transition. Ellen MacArthur Foundation. 2012. p. 24. Archived from the original on 2013-01-10. Retrieved 2012-01-30. https://www.texile-plastic-materials-recycling.com/viscous.php.

In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 20

WASTE RECYCLING FOR WOUND CARE AND COSMETIC SMART ECONOMICS: CHITIN AND LIGNIN Pierfrancesco Morganti1,2,, Gianluca Morganti3, Alessandra Fusco4 and Adone Baroni5 1

Academy of History of Health Care Art, Rome, Italy 2 China Medical University, Shenyang, China 3 ISCD Nanoscience Center, Rome, Italy 4 Department Mental Health and Physics and Preventive Medicine, Unit of Experimental Medicine, Campania University Luigi Vanvitelli, Naples, Italy 5 Department Mental Health, Phisics and Preventive Medicine, Campania University Luigi Vanvitelli, Dermatol Unit, Naples, Italy

ABSTRACT Skin is a barrier between the human body and the external environment. In fact, maintaining its integrity together with all the organs of the body, it plays an important role in regulation of homeostasis. For this reason, chronic wounds and burns represent a big problem for the health of the individual, also for the partially devastating physical and emotional consequences, constituting a serious social and financial burden also. Thus the interest for the regenerative medicine which has the function to restore or replace cells, tissues or organs by the use of biomimetic materials able for transplanting or stimulating the body’s own self-repair mechanisms. But, the transdermal delivery of any applied substance is very difficult, because of the great impenetrability of the skin barrier. Therefore, to overcome this barrier, modify its integrity and impenetrability, and facilitate and enhance the penetration of active ingredients, specific nanoparticles (NPs) and nanocarriers (NCs) have been developed. Moreover, the population increase with consequential increase of goods consumption and general gross mismanagement of waste, represents a high problem for the environment. This the reason for the relentless 

Corresponding Author’s Email: [email protected].

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Pierfrancesco Morganti, Gianluca Morganti, Alessandra Fusco et al. increase of biomaterial of natural origin, used for both cosmetic/medical formulations and biodegradable packaging. Thus the necessity to select the right biomaterials which, included into NPs, are generally loaded and transported by natural carriers (vehicles). These vehicles, made by biopolymeric degradable non-woven tissues and films, in fact, may be obtained by the use of varies polymeric polysaccharides (Nanocomposites) extracted from waste biomaterials. At this purpose, among the more available and at low cost biopolymers, both chitin, lignin, and their complexes have shown to be ideal carriers to transport and deliver bioactive molecules across the skin boundaries, because of their pore sizes, surface electrical charges and particular structure, as well as for their degradation properties. Thus, they may represent an interesting raw material that, obtained from agro-forestry biomass and fishery’s by - products respectively, could result of high interest to reduce use and consume of the natural raw materials, preserving them for the future generations and maintaining the Planet Biodiversity.

Keywords: skin, nanoparticles, nanocomposites, nanocarrier, scaffolds, biopolymers, chitin nanofibrils, nanolignin, waste, recycling

INTRODUCTION The skin is the first line of defense which protects the body from mechanical insults, microorganisms and environmental chemicals, modulating transepidermal water loss also, by the function of epidermis, dermis and sub-cutaneous tissue (Figure 1) [1]. It represents an important barrier greatly dependent on the structure and composition of its uppermost layer, the stratum corneum (SC). This first layer is composed of corneocytes, dead flattened anucleate cells, enclosed by keratin filaments aggregated by filaggrin surrounded by highly organized lipid matrix [1, 2]. The layer under the SC, is composed of cells known as keratinocytes, which play a further defense forming both a physical barrier and an immunological shield that alert the immune system, producing proinflammatory mediators such as cytokines and chemokines, and antimicrobial peptides (AMPs) [1, 2]. Cytokines are biological molecules that act as soluble mediators of natural immunity and the immune response. They are described as multifunctional molecules, which together with chemokines and adhesion molecules, which play important biological activities helping hematopoiesis, immunity, infectious diseases, tumorigenesis, homeostasis and tissue repair, growth and cell development. Moreover, AMPs, reflecting and affecting the composition of the skin microorganisms (i.e., bacteria, fungi and yeasts) at different sites and ages, have the aim to mitigate the pathogen colonization. However, antimicrobial peptides and cytokines are a “functional module” of the innate immune system (Radek and Gallo 2007) communicating with cells of the adaptive immune system also. Thus, the skin plays an important role of homeostasis, maintaining the integrity of all the body’s organs. But, because of the great impenetrability of its barrier capacity, the transdermal delivery of any substance applied on its surface result very difficult. Therefore, to overcome this barrier, modify its integrity and impenetrability, and facilitate and enhance the penetration of active ingredients, specific nanoparticles (NPs) and nanocarriers (NCs) have been developed [3]. These innovative means have the capacity to increase the ingredients’

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temporary penetrability through the skin, re-establishing its integrity, also when compromised by traumatic or chronic events, such as burns or wounds [3-5]. This the aim of NPs and NC developed in the form of hydrogels, foams, films, non-woven tissues etc. and made by engineered nanocomposites. Naturally the nanocomposites, loaded by varies active ingredients, have to be selected for releasing these ingredients at level of the different tissue/cells, depending to the activity they are designed for [6, 7]. It is important to remember that the new approach of tissue engineering has to be developed to modulate the active ingredients penetration and/or reduce the limitation of the conventional treatments used to repair the damaged tissues. Thus smart films and non-woven tissues (Figure 2) are continually designed and programmed to actively interact with aged skin or wound bed. However, they must be able to provide an optimum an environment for the skin surface and wound dressing interface, maintaining hydration and preventing infection. So doing the microorganisms’ biofilm can be eliminated, encouraging and helping both epithelialization and tissue formation [7-9]. At this purpose it is to underline that skin wounds and burns became a major social and financial burden for million people suffering from the partially devastating physical and emotional consequences.

Figure 1. The skin as line of defense from the environmental insults.

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Figure 2. Non-woven (on top) tissue and film (on bottom) micrographs obtained by SEM.

World Health Organization (WHO), in fact, has estimated that actually and worldwide nearly 180,000 death are annually caused by burns, occurring in the home and workplace, while nearly 9 million were injured in 2017 by fire, heat and hot substances, according to USA Institute for Health Metrics and Evaluation (IHME) [10, 11]. Moreover in 2018, million people was affected by wounds with or without infections with a cost for treatments estimated between US$ 28.1 billion and 96.8 US$ billion [12]. This the reason why the wound care market is expected to reach US$ 15- 22 billion by 2024, due also to an increased aging population with an increased obesity and diabetes. Thus, in EU it has been foreseen that by 2080 there will be 66.1 milłion people aged 80 years and over, who desire to maintain good health and younger appearance (Figure 3) [13].

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Figure 3. Previsional aging of women and man.

On the other hand, the beauty cosmetic market is expected to register an annual growth rate of 7.14% during the 2018-2023 period reaching up US$ 805.61 billions. As a consequence, the necessity to invent and produce more effective and smart cosmetic products and medical dressings, contemporary developing policies and prevention programs of education for the more vulnerable populations. Together with the increasing diseases, aged population suffer also for the secondary but important problem connected with her/him appearance. Skin wrinkling and fine lines, in fact, are the most evident signs visible on elderly, especially on face and neck, while they don’t like to feel old but wish to maintain a youthful look, possibly forever. This is because, according to Kligman, “those who are gain advantages and the unattractive suffer throughout the life cycle, because what is young and beautiful is good” and “unattractive elderly individuals are perceived less favorably” [14]. However, people live longer and take better care of their health appearance and wellbeing because they want to remain active, contributing to society and maintaining an ageless attitude towards life [15]. Additionally, with the worldwide population boom and the increased consume of drugs, food, cosmetic and sanitary products, a consequent increase of plastic packaging occurred, creating a complex waste problem to be solved.

WASTE PROBLEM AND RECYCLING The increasing number of worldwide inhabitants are consuming an high quantity of drugs, food, adsorbent hygiene and medical products (baby diapers, feminine Sanitary

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napkins, adult incontinent pads, and wound care medications), the majority of which are packed by plastic containers. These non-biodegradable packaging is causing an increasing and difficult waste problem difficult to solve. Its planning and management, in fact, became a critical politic point, affecting also the daily health, productivity and cleanliness of all the communities worldwide. Thus billion packaging are thrown out every year (Figure 4) and remain in the environment as pollution, where alternatively, by the “right politic decisions, there are the possibility to increase plastic recycling rates, reducing plastic consumption or developing plastic recycling end markets” [15].

Figure 4. Plastic packaging in the Environment with a low quantity recycled.

Moreover, with the population and levels of goods consumption increase, the general gross mismanagement of waste represents a high problem for the environment. Thus, work, together with new means and ideas, necessary for waste reduction possibly to zero, has to be financed by priority funding competing and reserved to clean water, education and health care [16]. At this purpose it has to be remembered that in 2016 the World population generated two billion waste per year, 242 million tonnes of which are represented by plastics (i.e.,~ 12% of the global waste and 19% of the packaging waste) (Figure 5) [17, 18]. This plastic waste produced 1.6 billion tonnes of CO2 equivalent, estimated to increase to 2.6 billion tonnes by 2050! [16-19]. Just as an example, 9000 tonnes of sanitary waste has produced every year from India (as heavy as about the Eiffel Tower!), 90% of which is made by plastics. In USA, the biggest generator of waste (800 kg/year for each citizen), the sanitary waste represents 30% of the non-degradable ones [16, 17]. On the other hand in the EU28 in 2016 was generated around 300 tonnes of plastic waste in 2016, equivalent to 30% of the total waste generated [16]. Moreover, according to varies authors [19-22], 120 billion units of packaging are produced globally by the cosmetic industry each year, most of which are nonbiodegradable.

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Figure 5. Per cent of plastic waste on packaging material in EU, 2016.

On the other hand, consumers, from 25 to 34 years old, are pushing the beauty industry to produce cosmetics, following the sustainable rules of the circular economy. Thus, in 2019, 73% the senior decision-makers of cosmetic industry have seen sustainability an opportunity, so that 51% have created packaging with sustainable features in the past 12 months, while 52% have little or no knowledge of legislation and packaging regulations affecting their industries [20-23]. However, the rise of the actual more conscious consumer is pushing retailers to be more transparent and aware of how the beauty products are made and where they are coming from. In any way, driven by rapid urbanization and growing population expected to increase from 7.5 billion to ~9.5 billion by 2050 [24], global annual waste should jump to 3.4 billion tonnes over the next 30 years, up from 2.01 billion in 2016 [16-19]. Thus, while on one hand plastics have many recognized benefits, on the other hand their production and use created and are creating global and complex waste problems. United Nations [25], in fact, have predicted that “under current consumption rates and waste management practices, around 12 billion tonnes of plastic waste, damped into landfills and oceans, will be leaked into the environment by 2050.” This high quantity of plastics, added to the 9 billion tonnes produced in the past century, has invaded our lands and oceans, provoking intolerable pollution and environmental disasters worldwide (Figure 6) [25]. New eco design strategies, therefore, are necessary to ensure better coherence between the manufacturing/distribution politics and the waste management processes to prevent the production of by-products, increase the quality of recycling methodologies and go versus the consumer requested and desired. Thus the need to ameliorate and increase the marketing communications to consumers, remembering and underlining by correct messages the toxicity

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of the petrol based plastics compared to plant-based bioplastics [21, 23]. In conclusion it became a must for the medical and cosmetic industries the necessity to pass from the actual linear economy to the circular economy. Any product would be redesigned, reused and recycled by a zero waste hierarchy (Figure 7) by the use of renewable energy, necessary to eliminate or reduce waste and prevent the negative effects on the natural environment. As a consequence the need to realize, for example, food, cosmetics, adsorbent hygiene products, drugs and advanced medications by the use of bio-ingredients and bio-carriers obtainable managing more efficiently natural resources, and improving technologies and logistics, according to the consumer requests.

Figure 6. Billion tonnes of plastic bottles remain in the Environment as non-degradable pollution.

Figure 7. The necessity to go from a linear economy based on a zero waste hierarchy.

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NATURAL PRODUCTS, BIO CARRIERS AND CONSUMER REQUESTS Also in developing countries, consumers today are re-evaluating their spending habits, looking to more value, high quality, unique and differentiated products, which convey certain level of status, maintaining the environmental equilibrium [25]. Thus, they demand for food and cosmetic products made by natural ingredients, while the post- consumer presence of the polluting plastic packaging is considered negatively. Consequently, 29%of consumers are looking for all-natural ingredients in skincare products, while ingredients transparency is sought by 19% of who are becoming increasingly sensitive to issues of plastic waste. The shopping habits are changing, so that customers are willing to pay more for products with plant derived eco- ethical ingredients (i.e., phytonutrients) and recyclable packaging. A “plastic free world,” therefore, seems to be the future goal for a more environmental conscious lifestyle consumer, based on innovation and zero waste. This the reason of the relentless increase of biomaterial of natural origin, used for both cosmetic/medical formulations and biodegradable packagings. It is considered biomaterial, in fact, any substance of natural or synthetic origin that, engineered to interact with biological systems, may offer the possibility to recover or replace an aged tissue and speed up the healing process of a wounded/burned skin [26]. These natural ingredients, in fact, are engineered as scaffolds able to interact with biological systems for replacing tissues or organs and/or speed up the healing process [27]. For these reasons, it is rapidly increasing the use of natural biocomposites to make bio-carriers and biomolecules safeness and effectiveness, able to facilitate both regeneration and repair of aged or diseased skin. This is also the aim of the EU research project PolyBioSkin (polybioskin.eu) by which biodegradable sanitary, cosmetic, and wound care products have been realized (Figure 8). However, the use of biomaterials, characterized for their biomimetic architecture, biocompatibility, biodegradability and bioresorbability, result fundamental, being also not immunogenic and free of toxicity [28]. Additionally, the scaffolds made from natural or natural derived polymers have to be made by the same structure of natural extracellular matrix (ECM) and therefore able to resemble the skin’s native tissue [29, 30]. ECM, in fact, is a scaffold that coordinating tissue development and arrangement, has the regenerative ability to guide the cells by specific signals providing them an appropriate environment. As a consequence the necessity of making these biomimetic scaffold’s is increasing day by day. These ECM-mimicking structures, in fact, when made by natural polymers and embedded by natural and synthetic nanoparticles (biomaterial), have the capacity to regenerate the skin aged, wounded, or burned. Both these biomimetic carriers and nanoparticles offer several advantages over traditional delivery systems, such as environmental protection of bioactive components, increased bioavailability as well as controlled delivery and release at the site of action [31]. NPs, in fact, possess a high overall material surface area to volume ratio that, together with their electrical charges, result beneficial allowing large numbers of cells to attach and migrate into porous scaffolds and skin. Moreover, the electrical charges, covering their surface play a key role in guiding cell behavior and fate, being the primary interface for cell interaction.

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Figure 8. The aims of the EU Research project Polybioskin.

Actually, the more used natural polymeric biomaterials are proteins such as silk, collagen, gelatin, keratin, etc, and polysaccharides, such as cellulose, lignin, dextran, pullulan, chitin and its derived compounds. All these polymers have excellent biocompatibility and viability but limited physicochemical and mechanical stability. On the other hand, the synthetic polymeric biomaterials, characterized for their less biocompatibility but more stability, are represented from Polylactic acid (PLA), Polyvinylalcohol (PVA), Polyurethane (PU), Polyhydroxyalcanoates (PHA), etc. Thus, to overcome the disadvantages of both natural and synthetic scaffolds, composite mixture of polymers are continually designed and realized by different technologies, such as casting and electrospinning to realize scaffolds ECM-same [32].

SCAFFOLD ACTIVITY AND FUNCTIONS IN REGENERATIVE MEDICINE The ideal scaffold should have sufficient mechanical strength to resist the physiological mechanical environment of the different tissues such as, for example, bone and skin [33]. Moreover it must have the ability to degrade in parallel to the rate of new tissue for maintaining their structural integrity until the new grown tissue has replaced the scaffold’s supporting function, without releasing toxic secondary products. However, the scaffold has to have the fundamental functions to: 1. 2. 3. 4.

Act as barrier for preventing microbial infection and nano-particulate infiltration Support cell adhesion, migration and proliferation Act as delivery vehicle for cells, growth factors and genes Act as reinforcement of the damaged tissue to restore its function and regeneration.

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Moreover, it has to possess the following requirements: 1. A three-dimensional structure with interconnected pores of 200-500 um, a size that, acting similarly to the native ECM, results a necessary network for cell growth, transport of nutrients and metabolic waste. 2. Biocompatible and bioresorbable activity with no or minimum immune response, and a controllable degradation without production of toxic compounds 3. Suitable surface chemistry for cell attachment, proliferation and differentiation 4. Mechanical properties to match those of the tissues at the site of implantation. Thus, the biocompatibility, good polymer cell interaction, and the porosity of the scaffold structure result fundamental for the cell adhesion to the skin-substrate. For all these reasons, a right scaffold, made by the same characteristics of the native ECM, could result of great interest to repair the skin structure, modified by aging and/or photo-aging phenomena and/ or by traumatic effects or diseases [33]. This the aim of tissue engineering used in regenerative medicine and cosmetic dermatology which, as interdisciplinary field of life science, have been developed to restore, regenerate and replace tissues or organs by a combination of biomaterials, biologically active molecules, and cells [34]. One of the goal in tissue engineering, in fact, is to mimic the ECM cellular environment by a 3D structure acting not only as a physical framework for cells, but also as a complex dynamic environment for their reproduction and survival [29, 33]. Applied application of biomaterials in biomedical engineering and healthcare represent, therefore, a mean to replace the biological functions of ECM with its fibers, such as collagen and elastin. Collagen, in fact, has made by the main ECM protein that, by the orientation of its fibers, provides the mechanical support to contrast the forces necessary for resisting to eventual repetitive skin plastic deformation phenomena and age related changes, also during its regenerative processes in wounds or burns [35]. On the other hand, elastin provides the skin elasticity, by its microfibrils. At this purpose it is to remember that, during the aging processes, the gradual reduction of elastic fibers significantly reduces the skin’s ability to bend, while the modified organization, disposition and structure of the collagen fibers reduces its mechanical activity [26, 36, 37]. Moreover, the SC’ lipid levels, broadly reduced together with the level of Normal Moisturizing Factors (NMF) and the production of its precursor filaggrin, cause skin dehydration (Figure 9) [38, 39]. In addition, it appears a gradual decline in immune function and reduced allergen responses also, with a higher threshold for cutaneous inflammation, compared to young adult and infant skin [40]. However, it is also to underline the importance of the cell-cell communication mediated, for example, by the extracellular vesicles (EVs). EVs regulate the cell response, proliferation and migration which are slowing down in aging and probably in normal wound healing also [41]. In addition it is to not forgotten the skin microbiome, that certainly influences the activity of both normal, aged and diseases skin. The skin resident microbes, known as microbiome, play important roles in the maturation and homeostasis of cutaneous immunity. It regulates, for example, the expression of antimicrobial peptides (AMPs) and interleukin 1a (IL-1a), modulating the cutaneous immune system [42]. Microbiome, therefore, has the ability to shift markedly the inflammation cascade, thus impacting human health.

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Figure 9. The Reduction of the filaggrin synthesis causes Reduction of NMF with appearing of skin dehydration.

In addition, as previously reported, the dysfunction or partial/total loss of an organ or tissue’ functions, resulting from aging injuries or diseases, is one of the most important public health problems. On the other hand, advanced materials used in regenerative medicine, such as natural polysaccharides or natural derived compounds, represent a key tool for advanced development and manufacturing of a sustainable circular economy. Regenerative medicine, in fact, has the function to restore or replace cells, tissues or organs by the use of transplantation or stimulation of the body’s own self-repair mechanisms by biomimetic materials. Thus the necessity to select the right biomaterials, which includes the utilization of micro/ nanoparticles (NPs) (Figure 10) with highly controlled diameter and different geometries. NPs, in fact, result useful for their capacity to be loaded and transported by carries made by bio-polymeric degradable polysaccharides (nanocomposites) used, for example, to produce non-woven tissues and films (Figure 12) [43, 44]. All these natural or natural derived biopolymers, in fact, are used to make scaffolds for regenerative purposes due to their similarity to ECM, mechanical tunability, and high biocompatibility and water holding capacity. It is also to underline that NPs, having unique properties and sub cellular size dimension, may be easily embedded into different nanocomposite fibers used to make both non-woven tissues and films (carriers). However the entrapment of active ingredients into

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NPs, loaded on nanocomposite polymers (carriers), have the ability to change the pharmacokinetics and bio-distribution characteristics of the payload-carrier, as these characteristics are dictated by the carrier and not by the physicochemical properties of the ingredients designed. Therefore, the engineering new smart carriers open up new possibility for tuning the overall ingredient performance, enhancing its permeability and retention capacity (EPR) [45]. Naturally, the versatility of these innovative vehicles make possible multiple applications, because of their capability to be also embedded by several different molecules, which will characterize activity and effectiveness of the final product. Thus it is possible to create a new category of biodegradable medications or cosmetic products at zero waste, utilizing these skin-friendly tissues and films as smart carriers. They, in fact may be realized by the use of natural or natural derived polysaccharide and nanocomposites made, for example, by chitin and lignin, which available as waste material, is obtained respectively from industrial fishery’s by- products and agro-forestry biomass [46].

Figure 10. Nanoparticles of chitin nanofibrils-hyaluronic acid block polymers(top) and nanochitinnanolignin (down) respectively obtained by the gelation method.

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POLYSACCHARIDE NANOCOMPOSITES Polysaccharide nanocomposites are comprising of nanoscale material such as chitin nanofibrils and nanolignin incorporated in a bulk of natural nanocomposite polymers made, for example, by pullulan or starch as well as by man-made biopolymers natural derived such as PLA, Polycaprolactone (PO), etc. [47-50]. Thermal resistance and tensile strength of these nanocomposites have been increased by our group [51-55] using micro/nano fillers, such as chitin and lignin, etc. These natural polymers, singularly or complexed each to others by the gelation method, are utilized not only as fillers but also to entrap different active ingredients (Figure 11) [5155].

Figure 11. The gelation method to obtain block polymeric nanoparticles.

Both nanochitin and nanolignin, in fact, may be easily complexed in water solution, being polymers covered in their surface by electropositive and electronegative electrical charges respectively. While the biopolymers act as matrices, the nanofillers are dispersed among the polymeric fibers to improve the functionality such as the physicochemical and mechanical properties, transparency and water permeability or UV-blocking effect, of tissues made by electrospinning or films by casting (Figure 12) [48-51]. Thus, the properties of the final tissue/film are gained by the nanofillers Chitin-Lignin (CN-NL) and naturally by the active ingredients entrapped into the different nanocomposite-fibers. It is to remember that CN-NL complexes have shown to be beneficial to nanocomposite as nanofillers for their high surface/ weight ratio which leads to a large boundary are between the biopolymer matrices (nanocomposites) as well as for the capacity to entrap different ingredients, charactering and finalizing activity and effectiveness of both non-woven tissues and films [46-52]. The selection of nanocomposites and nanofillers plays, therefore, an active and important role to obtain the right effectiveness and safeness at skin level of films and tissues to be realized [7, 53, 54]. Thus, on one hand CN has been used to produce flexible films optically transparent made by casting and air-drying with the use of aqueous based solvent [50, 52]. Once water has evaporated the film can be peeled off, obtaining the desired thickness and the designed characteristics, according to the solution conditions and the ingredients used. However, the film can be water soluble or insoluble, according to the polymers used as well as partially or totally biodegradable, but always multifunctional and skin-friendly and ecofriendly [53-55]. On the other hand, it has been shown that CN and its NL complexes increase, for example, their antioxidant and antibacterial effectiveness, also enhancing skin

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cell adhesion, reproduction and growth, when entrapped into non- woven tissues [55-57]. It is to remember that Radical Oxygen Species (ROS) and Radical Nitrogen, Species (RNS) are at the base of the environmental chemical insults, causing damage to cell membrane and impairing the normal cell function with a consequential its apoptosis and/or mutations [56, 57]. These ECM-like structures, in fact, release easily and slowly the active ingredients entrapped into their fibers, and are metabolized by the chitotriosidases in glucosamine, acetyl glucosamine and glucose, utilized as cell food and nutrients necessary to promote the proliferation of keratinocytes and fibroblasts [58, 59]. Used in vivo on first and second grade’ burns or on wounded skin, these innovative tissues have shown to faster the rate of healing and skin repairing activity, notably reducing the inflammatory process, compared to traditional based wound dressings [60, 61]. They among other activities stimulate the skin production of natural antimicrobial peptides (AMPs) such as the defensins, which have an antimicrobial activity as well as function to link innate and adaptive immune responses [7, 53, 60-62]. Defensins, are endogenous antibiotic molecules acting in the defense of the organism against Gram-positive and Gram-negative bacteria, fungi and the envelope of some viruses. Being involved in the innate immune response, their release is induced by pro-inflammatory cytokines, endogenous stimuli, infections or wounds, thus serving as the first line of skin defense [63, 64].

Figure 12. Tissue (up) and film (down) made by polysaccharides by the electrospinning and the casting technology respectively.

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SKIN BARRIER AND AGING As previously reported, the skin provides an important protective barrier against air pollutants and invading microorganisms, helping our body directly and indirectly by the immune system also. By the continuous environmental aggressions and the passing of time (chronological aging) skin undergoes structural and molecular modifications which modify its barrier structure and functions, such as antimicrobial barrier, epidermis permeability, calcium gradient, lipid synthesis and processing, cytokine production, the SC’ acidic pH and skin hydration [65]. Moreover when, during the life time, the skin has been exposed to excessive sunlight, the signs of chronological aging (intrinsic aging) are increased by the so called photoaging (extrinsic aging) [66]. However, both aging and photoaging are caused by several factors capable of deteriorating ECM and cell modifications, provoking among other fine lines and wrinkling. Skin, in fact, modifies its structures especially at the level of type I collagen, the fibers of which lose their regular disposition and functions (Figure 13) [66, 67]. These and other damages, caused by the oxidative stress and mediated through UVA and UVB adsorptions, lead to the generation of ROS and RNS. Moreover, as reported previously, the oxidative stress plays a role in the development and acceleration of cell apoptosis and different skin diseases [56, 66]. In any way the photo damaged areas, being more visually apparent on face and hands, influence the individual’s life. Thus, the necessity to formulate cosmetic products which, natural-oriented and made by effectiveness and safeness formulations, may be able to erase the effect of age, possibly in a short time and accordingly to the consumer requests. At this purpose, according to the upcoming Mintel report on health management trends for 2020 [68], adult consumers, women and men, are most motivated to “set beauty and wellness goals to improve their health, feel happier, look better and take control of their wellbeing.” They would like to slowdown the aging process with the hope of looking younger longer, improving good health and longevity.

Figure 13. Different cell modifications on aged and photo aged skin compared to young ones.

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Figure 14. Human wellbeing and lifestyle.

Figure 15. Two of the seventeen priority recommended from UNESCO for a sustainable development.

Thus the adoption of strategies for maintaining a younger looking skin and global appearance by the use of anti-aging preparations together with preventive and protective means, such as the routine use of clothing, hats, sunglasses and sunscreens, while avoiding sun during the peak hours from 10 a.m. to 4 p.m. [69]. In 2020, and beyond, therefore, “actions that incorporate physical and emotional benefits, such as walking or stretching, will take over as wellness driven activities available to everyone” (Figure 14) [68]. In addition, it is increasing the routine daily use of cosmetics and diet supplements, as well as the utilization at home of face mask at the end of a long day, instead of going out. Moreover, a holistic and sustainable approach is becoming a key motivator of consumer behavior, while the increased global population and climate crisis are forcing people to reduce their waste production and energy consumption, for safeguarding health and the environment. On the other hand, the manufacturing companies are becoming to change their production modalities going versus the circular economy, adopting the UN’ sustainable development goals by the use of natural

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raw materials and processes, based on a drastic reduction of green-house gas (GHGs) emissions [70]. At this purpose, United Nations have given very clear guidance not only for citizens, but also for corporations on how the sustainable future should look like. If based on Industry responsible production and Innovation and consumer consumption (Figure 15) [71]. However, on the one hand a changing of the way of living is necessary for citizens, who have to better understand the meaning of biodegradability and the possibility to select waste in the right way [72]. On the other hand, new eco design strategies are needed to ensure better coherence between the manufacturing and waste management processes, to prevent waste where possible and to increase the quantity and quality of recyclables.

CONCLUSION Waste recycling, therefore, would be considered as a basic and fundamental priority to save humans and the environment from the disasters we are living worldwide by the waste invasion, further increased for the recent massive use of the non-degradable surgical masks, provoked by the actual COVID-19 pandemic [73-75]. Thus both customers and manufacturers would have a good and safe behavior in consuming and making more biodegradable products such as innovative beauty masks, cosmetics and advanced medications with surgical masks. On one hand, consumers have to re-evaluate their spending habits demanding for convenience and immediacy, searching authentic natural derived differentiated cosmetics, characterized not only for their effectiveness and safeness, but also because free of waste [25]. They, in fact, living longer are taking better care of their health, appearance and wellbeing and want to remain active to society, maintaining an angeless attitude towards life. For all these reasons consumers are “increasingly aware about products’ ingredients, their potential efforts on health and how eco-friendly is their origin” [76]. On the other hand, manufacturers are increasingly focusing on R&D of materials science for recovering new ingredients and innovative natural raw materials. As a consequence, they are becoming to produce cosmeceuticals and advanced medications characterized for maintaining a good relationship between the product effectiveness/safeness and the sustainability principles of its production, based on realistic, economic and social approaches [77, 78]. Thus their action on environmental sustainability is based on the improvement of process efficiency to reduce the consumption of energy and water and to minimize emissions, pollution and waste. Thus, the majority of cosmetic manufacturing are becoming to use for their products, recycled, recyclable biomaterials and bio-sources for making primary and secondary packaging also. Demand for cosmetics made by eco-friendly natural ingredients, in fact, is continuously increasing among the consumers who are looking for skin care product based by all-natural sustainable ingredients. Moreover, the majority of them are becoming increasingly sensitive to plastic waste of cosmetic packaging also, knowing that around 63% of the relative containers are made by non-biodegradable plastic, because of the versatility and durability of this material [78]. Thus, manufactures are looking for biopolymers, such as polysaccharides, to make innovative cosmetic/drugs, gel/emulsions and smart non-woven tissue/films, because of their natural origin and capacity to improve the adhesion of both

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keratinocytes and fibroblasts, when used to make micro/nanocomposites and chitin-based scaffold’s [79]. Biopolymers, in fact as previously reported, may be utilized in a variety of biomedical and cosmetic applications such as pharmaceuticals tissues, tissue regeneration scaffolds, drug/cosmetic masks, delivery agents and imaging agents, because of their mechanical tunability, water holding capacity and biocompatibility due to their ECM-simile structures. Among the more available and at low cost biopolymers, both chitin and lignin fibers and their complexes have shown to be ideal carriers [51-55, 58-62] to transport and deliver bioactive molecules across the skin boundaries, because of their micro/nano dimension, surface electrical charges covering their surface and the particular structure organization as well as for their degradation properties. All these characteristics directly influence transport properties and effectiveness of these carriers both in term of storage and release of the active ingredients loaded. The micro/nanoparticles of the CN-NL complexes, in fact, may be loaded by different active ingredients, entrapped into various natural polymers, easily controllable for their diameters as well as for their capacity to deliver the biomolecules to the target sites at the designed time [43, 80]. Moreover, they are globally biodegraded from the human and environment’ enzymes to safe and useful compounds. In conclusion, the environmental sustainability implies the maintenance of natural resources and long term ecological balance characterized by the reduction of GHGs emissions and, therefore, by a new way of producing and consuming at zero waste [17, 76, 81]. Thus, the use of biopolymers, such as nano-chitin and nano- lignin, for making smart non-woven tissues and films for wound care and cosmetics, may represent an interesting and innovative raw material. Additionally, these smart biopolymers, obtained from agro-forestry biomass and fishery’s by-products respectively, could result of high interest to reduce use and consume of the natural raw materials, with the aim to preserve them for the future generations and maintain the Planet Biodiversity. This the actual challenge for industries and consumers, complicated from the global economy under pressure for the actual political and geopolitical instability further increased from the in progress COVID-19 pandemic [82, 83].

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In: An Introduction to the Circular Economy Editors: P. Morganti and Maria-Beatrice Coltelli

ISBN: 978-1-53619-233-9 © 2021 Nova Science Publishers, Inc.

Chapter 21

BIOBASED AND BIODEGRADABLE RIGID AND FLEXIBLE POLYMERIC PACKAGING Maria-Beatrice Coltelli*, Vito Gigante, Patrizia Cinelli, Alessandro Vannozzi, Laura Aliotta and Andrea Lazzeri Department of Civil and Industrial Engineering, University of Pisa, Italy

ABSTRACT The present chapter is dedicated to the potentialities and opportunities of biobased and biodegradable polymeric materials currently available on the market for producing packaging. After some definitions considering regulatory and standardization aspects, these materials are described and classified. Biopolyesters and biopolymers are mainly used for these products in the form of blends or biocomposites, often in combination with additives based on biobased molecules. For flexible packaging blown film extrusion or flat die extrusion of poly(lactic acid) (PLA) based materials or starch based materials are currently the main options on the market. For rigid packaging, obtained mainly by injection molding or thermoforming, PLA blends or composites are the more promising alternatives, because of their good balance of properties and cost. The control of their processability and final properties is thus fundamental.

Keywords: biobased, biodegradable, flexible packaging, rigid packaging, poly(lactic acid), PLA, starch

*

Corresponding Author’s Email: [email protected].

366 Maria-Beatrice Coltelli, Vito Gigante, Patrizia Cinelli, Alessandro Vannozzi et al.

INTRODUCTION Materials Correlation with the Environment: Definitions There is a growing concern worldwide about plastic disposal since waste produced using plastics based on not degradable polymers is persistent. This issue is particularly bound to plastic waste generated by packaging disposal, because of their short life cycle. Waste policy in most countries follows the so-called waste hierarchy concept, expressed by the Waste Framework Directive 2008/98/EC, 19 November 2008 [1], of the European Parliament that gives specific attention to prevention, reuse and recycling. For this policy, the best options (Figure 1) are: • • • •

Reduction of waste by prevention of waste production, Recycling (organic or material recycling), Energy recovering, Disposal in landfill.

Figure 1. Priority scale of waste management (Waste Framework Directive 2008/98/EC).

The option of recycling includes composting and anaerobic digestion as a type of organic recycling. For organic waste, the waste framework legislation encourages recycling in agriculture through composting since this is considered the most environmentally friendly option for organic waste management. In addition, recycling as re-processing of production scraps in industries is highly recommended. Recently, the European Commission has adopted an ambitious Circular Economy Package, that [2] sets clear targets for reduction of waste and establishes an ambitious and credible long-term path for waste management and recycling. Key elements of the revised waste proposal include:

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A common EU target for recycling 65% of municipal waste by 2030; A common EU target for recycling 75% of packaging waste by 2030; A binding landfill target to reduce landfill to maximum of 10% of municipal waste by 2030; A ban on landfilling of separately collected waste; Promotion of economic instruments to discourage landfilling; Simplified and improved definitions and harmonized calculation methods for recycling rates throughout the EU; Concrete measures to promote re-use and stimulate industrial symbiosis, turning one industry’s by-product into another industry’s raw material; Economic incentives for producers to put greener products on the market and support recovery and recycling schemes (e.g., for packaging, batteries, electric and electronic equipment, vehicles).

In the field of materials recycling, the plastic materials represent the fraction most difficult to be managed. In fact, several different polymers are currently employed in packaging to respect the requirements necessary for different foods and beverages protection. Poly(ethylene), poly(propylene), poly(ethylene terephthalate) and poly(styrene) are the most employed, but also multilayer packaging are currently used. These plastic materials, usually derived from petrol, cannot be recycled without being separated from each other. In principle, each polymer could be recycled by processing it at high temperature to obtain a viscous melt. Nevertheless, if a preliminary separation is not carried out, polymer blends with low performances are obtained because of the immiscibility and incompatibility of the different polymers. Consequently, there is a growing interest both in producers and consumers versus the use of bioplastic. Scientific efforts toward the design, synthesis, and production of sustainable or green materials have expanded exponentially in the last two decades [3]. At present, bioplastics share about 1% of the total market of 359 million tons of plastic produced annually [4]. Even if bioplastics already play an important role in the fields of packaging, agriculture, electronics and automotive parts, etc., the industry for production and marketing of biodegradable and bio-based plastics is relatively young and growing fast. For this reason, in the area of bioplastics, there is currently a lot of confusion on terminology. In Europe and worldwide, there are several industrial associations related to bioplastics. Due to a high confusion regarding appropriate terms, the main associations in the sector have proposed a list of definitions. The SPI Plastic Industry Trade Association, Bioplastics Council, [5] defined bioplastics the plastic that is biodegradable, has bio-based content, or both. On the other hand, Biodegradable Plastic is a plastic that undergoes biodegradation (process where the action of naturally-occurring micro-organisms such as bacteria, fungi, and algae induce the degradation of the material) accepted as industrial standards. Since 2008, accepted industry standard specifications are: ASTM D6400, ASTM D6868, ASTM D7081 or EN 13432 [6–9]. The Bio-based content of a material is the fraction of the carbon content made up of biological materials or agricultural resources versus fossil carbon content, where the biobased content is measured following the procedures set by ASTM D6866. In this latter the product’s biobased carbon content is determined as a fraction of total organic carbon content

368 Maria-Beatrice Coltelli, Vito Gigante, Patrizia Cinelli, Alessandro Vannozzi et al. (TOC) [10], while other analytical standard methods such as EN 16440 and ISO 16620-2 allow bio-based results to be reported as a fraction of total carbon (TC). In fact they specify a calculation method for the determination of the bio-based carbon content in monomers, polymers, and plastic materials and products, based on the 14C content measurement [11, 12]. It is evident that bio-based and biodegradable have not the same meaning. The term “biobased” means just that the material or product is (partly) derived from biomass, but its biodegradability must be assessed. Some bio-based products can biodegrade in municipal or commercial composting facilities, home composting, and aquatic and roadside environments, while others will only biodegrade in extremely specific environments and some will not biodegrade at all. For example, poly(lactic acid) is compostable while bio-poly(ethylene) is not. Biodegradation refers to a chemical process carried on by micro-organisms that are present in the environment. These micro-organisms convert the organic carbon in the materials into natural substances such as water, carbon dioxide, and compost. The process of biodegradation depends on the surrounding environmental conditions (e.g., location or temperature), on the material and on the application. When defining a material to be biodegradable, the environment should be also specified. Thus, some polymers can biodegrade in compost, but not in soil, some can degrade in marine water and some not, etc. Composting is considered as an organic recycling of material. In particular, industrial composting is performed under controlled composting conditions at high temperature in large-scale composting plants. Nevertheless, home composting is performed at ambient temperature in a reduced scale. The Packaging Directive 94/62/EC [13], and most recent amendments, addressed the amounts of biodegradable waste that can be land-filled or incinerated, and thus also compliance with the Landfill Directive, but does not affect recycling of bio-waste as defined in the Waste Framework Directive. The following European standards provide a framework to support the claim that packaging follows the essential requirements for packaging to be placed on the market as defined in the following directives: • • •

• • • •

EN 13431:2000—Packaging. Requirements for Packaging Recoverable in the Form of Energy Recovery Including Specification of Minimum Inferior Calorific Value. EN 13432:2000—Packaging. Requirements for Packaging Recoverable Through Composting and Biodegradation. Test Scheme and Evaluation Criteria for the Final. CR 13695-1—Packaging. Requirements for Measuring and Verifying the Four Heavy Metals (Cr, Rd, Hg, Pb) and Their Release into the Environment, and Other Dangerous Substances Present in Packaging. EN 13427:2000—Packaging. Requirements for the Use of European Standards in the Field of PackagingWaste (“Umbrella Norm”). EN 13428:2000—Packaging. Requirements Specific to Manufacturing and Composition. Prevention by Source Reduction. EN 13429:2000—Packaging. Reuse EN 13430:2000—Packaging. Requirements for Packaging Recoverable by Material Recycling.

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Following the EN 13432, endorsed by the European Commission and therefore considered a harmonized EU standard with a juridical value, a product is compostable if: • •

•

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The product contains at least 50% organic matter and may not exceed the heavy metal limits specified in the standard. The product should mineralize for at least 90% within six months under controlled composting conditions, where mineralization is defined as the conversion of the organic C to Carbon dioxide (CO2) and biomass, and this characteristic is linked to the chemical composition of the sample. The product, in the form which enters the market, should, within a timeframe of 12 weeks, fragment in parts smaller than 2 mm under controlled composting conditions. It must be outlined that this requirement refers to the physical form of the product instead of to the chemical composition. These characteristics are connected mostly to the thickness and the physical construction (e.g., laminate, coating, etc.) of the sample, and can result tricky to be met also for packaging based on biodegradable materials. The compost obtained at the end of the composting trial, which can also contain some no degraded residuals from the product, must not have any negative effects on the germination and growth of plants.

Thus, we can say that compostability comprises more than just biodegradability. A packaging that is compostable is always biodegradable, while a packaging which is biodegradable may not be compostable (since it might be too thick for disintegration or might release in the compost toxic substances). To avoid confusion on terminology to be selected and standards to be applied, several authorities have decided to promote (or even mandate) the definition “compostable” versus the definition “biodegradable”. Being bio -based or compostable does not necessary mean that the material considered is more environmentally sustainable than the counterpart fossil-based or not compostable, but, for example, recyclable. For this reason, it is important to evaluate the sustainability and ecological benefits of a bio-based polymer in term of raw materials, production, applications and end of life. This evaluation can be performed through a Life Cycle Assessment (LCA) study. The LCA represents an internationally standardized methodology that consists of four phases (ISO 14040, 2006 and ISO 14044, 2006) [14, 15]: 1. 2. 3. 4.

Goal and scope definition, Life cycle inventory analysis, Life cycle impact assessment, Life cycle interpretation.

The LCA study allows to estimate with a rigorous methodology the environmental impact of a process or of a material. Hence it is also a powerful method to investigate and assess the environmental impact related to a bio-based material.

370 Maria-Beatrice Coltelli, Vito Gigante, Patrizia Cinelli, Alessandro Vannozzi et al.

BIOPOLYMERS AND BIOPLASTICS With respect to other materials, polymers show a higher versatility thanks to the possibility of modulating their macromolecular structure by controlling the industrial synthesis thus achieving specific final properties. The structural materials “selected by nature” in plants and animals are based on polymers too and they belong to the class of biopolymers. Biopolymers are generally not easily processable with the industrial methodologies typical of the fossil plastic industrial sector to obtain flexible and rigid packaging. In general, polymers can be natural, artificial, or synthetic. An example of a natural polymer is cellulose, contained in paper or cotton fabric; among natural polymers there are also the polymers produced by microorganisms, such as poly(hydroxyalcanoates) (PHAs). An example of an artificial polymer, obtained by chemical modification of natural polymers, is nitro cellulose, much used in varnish, enamels, and propellants industry [16]. The natural and artificial polymers show the advantage of being renewable. Examples of synthetic polymers are given, in the packaging sector, by the so-called commodities, consisting of polyethylene (PE), polypropylene (PP), poly(ethylene terephthalate) (PET) or polystyrene (PS). Currently biosynthetic polymers are distinguished from synthetic polymers because they were industrially produced by traditional polymerization methods, but starting from monomers available from natural sources [17]. Hence, they are renewable. Poly(lactic acid) (PLA) is an example of biosynthetic polymer. The advantage of biosynthetic polymers with respect to natural and artificial polymers is the possibility of controlling the primary structure of the polymer and, consequently, its processability and its properties. From the point of view of biodegradability [4, 18] usually natural polymers are biodegradable where biodegradability is the capability of a material to undergo a complete oxidation in the environment giving CH4, CO2 and other simple compounds. This is typical of all polymers, but for synthetic polymers exceptionally long times—centuries—are required. Artificial polymers can be biodegradable, but usually it depends much on the achieved degree of chemical modification. For instance, cellulose acetate, that can have an acetylation degree between 0 and 3, is reported to be biodegradable only with an acetylation degree below 2.5 [19]. Biosynthetic polymers are usually both bio-based and biodegradable, such as PLA, but also polymers defined as synthetic, such as PE, traditionally obtained by petrochemicals, can now be produced from natural sources. These polymers are not biodegradable. In addition, in bioplastics also the polymers currently not yet synthesized by biotechnology but from not biobased monomers, such as poly(butylene succinate) (PBS), polycaprolactone (PCL) and poly(butylene adipate-co-terephthalate) (PBAT) et cetera, are included, because they are biodegradable. The bioplastics family thus regroups polymers coming from renewable and/or biodegradable sources [20]. Biopolyesters are quite relevant and they are biodegradable. Poly(ethylene terephthalate) (PET) and poly(butylene terephthalate) (PBT), are not renewable and not compostable. Interestingly, the PBAT is only partially renewable but it is compostable, as well as PBS and PCL. They will be fully renewable in the future as their monomers will be fully produced by renewable sources. PLA and PHA are both renewable and compostable (Figure 2).

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Figure 2. Different commercial polyesters: PET and PBT are not renewable and not compostable; PBAT is compostable; PCL and PBS are not yet fully renewable, but they are compostable; the PLA and PHA are both renewable and compostable.

In the field of packaging, the most interesting options for polymers in applications depend much on the end-life option [21, 22]. While in durable applications biodegradability is not an interesting property, in the food-packaging sector it could be so, especially if the perspective of composting is selected for the waste packaging. More important than biodegradability is compostability. As stated in the previous section, biodegradable and compostable products should be certified according to EN 13432/14995 standards [9, 23], defining procedures for testing the effective compostability, granting the correct behavior of the material in the composting plants. The other possible option for packaging management is recycling, which requires the preliminary separation of the different polymers, avoiding contamination, as well as good durability and stability of the plastic material, especially in re-processing conditions. Thus, it is an option suitable for mono-material packages, whereas for multilayer packaging it is obviously more difficult. Considering bioplastics that can be employed in packaging preparation, those polymers produced on an industrial scale, yet available in the market and also validated in processes commonly used in plastic industry seem the most promising. Two different types of basic formulations were developed on a mature technological level: starch-based materials and poly(lactic acid) (PLA)-based materials. Starch is a natural polymer, consisting of amylose and amylopectin, with the former being linear and water soluble, and the latter branched and water insoluble. The processing of starch was possible since some decades ago by controlling the plasticizing effect of water [24], culminating in the thermoplastic processing of starch at approximately its natural water content (about 15%) at a temperature of about 100°C. Amorphous thermoplastic starch (TPS) was thus obtained. An important characteristic of thermoplastic starch formation is the thermal and mechanical (shear-based) structural disorganization (destructuration) of the starch granules, to form, through swelling, a homogeneous melt. In particular, the gelatinization of starch occurs [25] thanks to the processing, in which the starch granules

372 Maria-Beatrice Coltelli, Vito Gigante, Patrizia Cinelli, Alessandro Vannozzi et al. become swollen and destructured and loose amylose by diffusion. This process, having a typical temperature dependent on the water content, results in the destruction of amylopectin crystallites and molecular order in the granules. The gelatinization represents an undesired state. Hence the range of temperature for processing is superiorly limited by the gelatinization point. From a rheological point of view TPSs show the possibility of being processed only in a restricted screw speed range, but in that range the behavior is shear thinning, similar to the one of low density polyethylene, with apparent viscosity decreasing with the increase of screw speed [26]. Destructured starch behaves as a thermoplastic polymer and can be processed as a traditional plastic; when alone, however, its sensitivity to humidity makes it unsuitable for most of the applications. The main use of destructured starch alone is in soluble compostable foams such as loose-fillers, and other expanded items as a replacement for polystyrene. The attaining of processable starch-based formulations suitable for flexible film production was possible by blending starch with thermoplastic hydrophilic synthetic polymers such as poly(caprolactone) [27] and poly(ethylene-vinyl alcohol) [28]. Usually plasticizers such as glycerol [29] or polyethylene glycols [24] are used for optimizing TPS processing. Cassava, also known as manioc or yucca, is a plant producing tuberous roots, typical of South America. Ezehoa et al. [30] reported the preparation of cassava starch-based formulations employed for preparing films by blown film extrusion. The films were obtained by adding poly(vinyl alcohol) (PVA), which is the matrix in the system. Ali et al. [31] also reported the preparation of films for packaging containing starch, but these films consisted mainly of polyethylene. However, in general it is not possible to employ starch for packaging films without blending it with plasticizers and polymers. The granules available on the market and widely employed for soft packaging, especially for pouches, were developed by considering this approach. NOVAMONT, which is the main producer of MATER-BI material, also follows this approach, but using renewable and biodegradable selfproduced additives. These intermediates are produced by vegetable oils and are defined polymeric complexing agents [32]. In fact, they interact with the starch, incorporating it. Hence the processing and mechanical properties were easily modulated, and the starch is protected by environmental humidity by the barrier properties of the host polymers/additives. Another promising material for packaging application, because of its cost, which currently is not significantly higher than the one of PS (at about 2 €/kg in Europe [33]), is poly(lactic acid) (PLA), which is renewable and biodegradable. Because of its rigidity it is not suitable alone for flexible packaging applications. However, commercial granules suitable for flexible packaging applications are available. In fact, in the last decade, many studies were carried out about PLA blends with other biodegradable polyesters or plasticizers. Plasticized and nano-filled films were prepared by flat die extrusion by Scatto et al. [34]. A good miscibility of the plasticizer is important, to avoid demixing and loss in transparency of films. Moreover, the plasticizer should not migrate out of the film.

Bioplastic Blends Biopolymers have great potentialities and many advantages, but also a lot of drawbacks, hence they need to be modified to meet market requirements. For this reason, the fine-tuning of these materials properties is the subject of much scientific research [35]. The blending is a

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pursued solution because it requires low cost compared to the development of new monomers and polymerization techniques. Moreover, tailored properties for a certain application can be achieved optimizing the material performances. Briefly, as theoretical background, it is interesting to underline that completely miscible blends have Gibbs free energy of mixing Gm