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Use of Recycled Plastics in Eco-efficient
Concrete
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Woodhead Publishing Series in Civil and
Structural Engineering

Use of Recycled Plastics in


Eco-efficient Concrete

Edited by

Fernando Pacheco-Torgal
Jamal Khatib
Francesco Colangelo
Rabin Tuladhar
Woodhead Publishing is an imprint of Elsevier
The Officers’ Mess Business Centre, Royston Road, Duxford, CB22 4QH, United Kingdom
50 Hampshire Street, 5th Floor, Cambridge, MA 02139, United States
The Boulevard, Langford Lane, Kidlington, OX5 1GB, United Kingdom

Copyright © 2019 Elsevier Ltd. All rights reserved.


No part of this publication may be reproduced or transmitted in any form or by any means,
electronic or mechanical, including photocopying, recording, or any information storage and
retrieval system, without permission in writing from the publisher. Details on how to seek
permission, further information about the Publisher’s permissions policies and our
arrangements with organizations such as the Copyright Clearance Center and the Copyright
Licensing Agency, can be found at our website: www.elsevier.com/permissions.
This book and the individual contributions contained in it are protected under copyright by
the Publisher (other than as may be noted herein).
Notices
Knowledge and best practice in this field are constantly changing. As new research and
experience broaden our understanding, changes in research methods, professional practices,
or medical treatment may become necessary.

Practitioners and researchers must always rely on their own experience and knowledge in
evaluating and using any information, methods, compounds, or experiments described
herein. In using such information or methods they should be mindful of their own safety and
the safety of others, including parties for whom they have a professional responsibility.
To the fullest extent of the law, neither the Publisher nor the authors, contributors, or editors,
assume any liability for any injury and/or damage to persons or property as a matter of
products liability, negligence or otherwise, or from any use or operation of any methods,
products, instructions, or ideas contained in the material herein.
Library of Congress Cataloging-in-Publication Data
A catalog record for this book is available from the Library of Congress

British Library Cataloguing-in-Publication Data


A catalogue record for this book is available from the British Library
ISBN: 978-0-08-102676-2

For information on all Woodhead publications visit our


website at https://www.elsevier.com/books-and-journals

Publisher: Matthew Deans


Acquisition Editor: Gwen Jones
Editorial Project Manager: Charlotte Rowley
Production Project Manager: Joy Christel Neumarin Honest Thangiah
Designer: Mark Rogers
Typeset by TNQ Technologies
Contents

List of contributors xi

1 Introduction to the use of recycled plastics in eco-efficient concrete 1


F. Pacheco-Torgal
1.1 The waste plastic problem 1
1.2 Outline of the book 4
References 7

2 Techniques for separation of plastic wastes 9


Silvia Serranti and Giuseppe Bonifazi
2.1 Introduction 9
2.2 Plastic waste sources and typologies 10
2.3 The plastic recycling chain 13
2.4 Plastic waste separation technologies 15
2.5 Recycled plastics quality control 28
2.6 Technical challenges in plastic recycling 30
References 33

3 Hydraulic separation of plastic wastes 39


Monica Moroni, Emanuela Lupo and Floriana La Marca
3.1 Introduction 39
3.2 Principles of the hydraulic separation process 40
3.3 Devices for the hydraulic separation within mechanical recycling
plants 46
3.4 The hydraulic separator channel 48
3.5 Separation efficacy of the hydraulic separator channel 54
3.6 Conclusions 65
References 66

4 Production of recycled polypropylene (PP) fibers from industrial


plastic waste through melt spinning process 69
Rabin Tuladhar and Shi Yin
4.1 Introduction 69
4.2 Physical cutting of waste plastic 70
4.3 Mechanical recycling of plastic wastes 71
4.4 Production of recycled plastic fibers 75
vi Contents

4.5 Material characterization 77


4.6 Mechanical properties of recycled PP fibers 80
4.7 Conclusions 82
Acknowledgments 83
References 83

5 Fresh properties of concrete containing plastic aggregate 85


Sheelan M. Hama and Nahla N. Hilal
5.1 Introduction 85
5.2 Mix proportion and design 85
5.3 Workability of fresh concrete containing plastic aggregate 94
5.4 Fresh density of concrete containing plastic aggregate 101
5.5 Self-compacting plastic aggregate concrete 103
5.6 Conclusions 113
References 113
Further reading 114

6 Mechanical strength of concrete with PVC aggregates 115


A.A. Mohammed
6.1 Introduction 115
6.2 Properties of concrete with PVC waste aggregate 117
6.3 Summary 134
References 134

7 Characteristics of concrete containing EPS 137


J.M. Khatib, B.A. Herki and A. Elkordi
7.1 Introduction 137
7.2 Preparation of EPS 139
7.3 Physical properties of EPS 140
7.4 Chemical properties of EPS 141
7.5 Substitution levels of EPS 141
7.6 Production and applications of EPS concrete 146
7.7 Density of concrete containing EPS 146
7.8 Fresh properties of concrete containing EPS 146
7.9 Mechanical properties 148
7.10 Thermal conductivity 153
7.11 Durability-related properties of concrete containing EPS 154
7.12 Structural performance of reinforced concrete beams 156
7.13 Conclusions and recommendations 156
References 158

8 Lightweight concrete with polyolefins as aggregates 167


Francesco Colangelo and Ilenia Farina
8.1 Introduction 167
8.2 Production of expanded granules 168
8.3 Use of recycled polyolefins in different sectors 170
Contents vii

8.4 Use of polyolefins as recycled aggregates in lightweight concrete


(case study) 170
8.5 Future trends 183
References 183
Further reading 186

9 Properties of concrete with plastic polypropylene aggregates 189


Z. Pavlík, M. Pavlíkov
a and M. Z
aleska
9.1 Introduction 189
9.2 Waste polypropylene-based aggregates for concrete 191
9.3 Structural properties of concrete with PP aggregates 197
9.4 Mechanical properties of concrete with PP aggregates 199
9.5 Thermal properties of composites with PP aggregates 207
9.6 Hygric properties of composites with PP aggregates 210
9.7 Possible application of PP in concrete production and future trends 211
Acknowledgments 211
References 211

10 Virgin and waste polymer incorporated concrete mixes for


enhanced neutron radiation shielding characteristics 215
Santhosh M. Malkapur and Mattur C. Narasimhan
10.1 Introduction 215
10.2 Neutron radiation and shielding 216
10.3 Use of hydrogenous aggregates and polymers in radiation
shielding 223
10.4 Use of virgin HDPE powder as partial replacement to sand 227
10.5 Properties of PISCC mixes in their fresh states 231
10.6 Neutron radiation shielding properties of polymer incorporated
concrete mixes 235
References 245

11 Performance of dioctyl terephthalate concrete 249


B. Şimşek, T. Uygunoglu, H. Korucu and M.M. Kocakerim
11.1 Introduction 249
11.2 Dioctyl terephthalate concrete 251
11.3 Comparison of the polyethylene terephthalate and dioctyl
terephthalate concrete 257
11.4 Conclusions and recommendations 262
References 264

12 Recycling of PET in asphalt concrete 269


I. Aghayan and R. Khafajeh
12.1 Introduction 269
12.2 Using PET waste as modifier in asphalt mixture 270
12.3 Conclusion 282
References 283
viii Contents

13 Recycling of different plastics in asphalt concrete 287


M.A. Dalhat, Khaleel Al-Adham and M.A. Habib
13.1 Introduction 287
13.2 Polymer modification of asphalt and the need for plastic
recycling in asphalt concrete 288
13.3 Materials and methods 289
13.4 Results 293
13.5 Future trends 302
13.6 Summary and conclusions 302
Acknowledgments 303
Conflict of interest 303
References 303

14 Replacement of stabilizers by recycling plastic in asphalt concrete 307


Goutham Sarang
14.1 Introduction 307
14.2 Need for stabilization of asphalt concrete 308
14.3 Addition of plastic in asphalt concrete 314
14.4 Performance of asphalt concrete with plastics 315
14.5 Field investigations 317
14.6 Conclusion 318
References 318

15 The use of recycled plastic as partial replacement of bitumen


in asphalt concrete 327
Marta Vila-Cortavitarte, Pedro Lastra-Gonz alez,

Miguel Angel Calzada-Pérez and I. Indacoechea-Vega
15.1 Introduction 327
15.2 Bitumen’s role in asphalt 328
15.3 Modification of asphalt mixtures with polymers 329
15.4 Modification of asphalt mixtures with polystyrene 332
15.5 General Conclusions 344
15.6 Future lines of study 345
References 346

16 Concrete reinforced with metalized plastic waste fibers 349


Ankur C. Bhogayata
16.1 Introduction 349
16.2 Metalized postconsumer plastic wastes: challenges and issues
for management 349
16.3 Feasibility of MPW in concrete: outcomes from pilot studies 350
16.4 Role of MPW fibers in the workability and strength properties
of conventional concrete 355
16.5 Effect of MPW fibers on the deformation due to the axial
compression by modified concrete 360
Contents ix

16.6 Advantages and limitations of the usage of MPW in concrete 364


16.7 Important findings and concluding remarks 365
16.8 Future trends 366
16.9 Sources of further information and advice 366
References 366
Further reading 367

17 Performance of concrete with PVC fibres 369


Senthil Kumar Kaliyavaradhan and Tung-Chai Ling
17.1 Introduction 369
17.2 Performance of concrete with PVC fibres 370
17.3 Conclusions 383
17.4 Future research perspective 383
Acknowledgments 383
References 384

18 Recycled waste PET for sustainable fiber-reinforced concrete 387


Dora Foti
18.1 Introduction 387
18.2 Use of PET in concrete 389
18.3 Tests (summary) and results 398
18.4 Conclusions 408
Acknowledgments 408
References 408
Further reading 410

19 Properties of recycled carpet fiber reinforced concrete 411


Hamid Reza Pakravan, Ali Asghar Asgharian Jeddi, Masoud Jamshidi,
Farnaz Memarian and Amir Masoud Saghafi
19.1 Introduction 411
19.2 Carpet types and fiber recycling methods 412
19.3 Properties of recycled carpet fiber 415
19.4 Physical properties of concrete containing recycled carpet fiber 416
19.5 Durability-related properties of concrete containing recycled
carpet fiber 418
19.6 Mechanical properties of concrete containing recycled
carpet fiber 418
19.7 Future trends 422
References 423

20 Performance of asphalt concrete with plastic fibres 427


Nura Usman and Mohd Idrus Mohd Masirin
20.1 Introduction 427
20.2 Polyethylene terephthalate 428
20.3 The use of polyethylene terephthalate in asphalt mixture 428
x Contents

20.4 Recycled polyethylene terephthalate fiber 429


20.5 Characteristics of recycled PET fiber 430
20.6 Application of recycled PET fiber in asphalt mixture 431
20.7 Conclusion 437
References 438

21 Sustainability of using recycled plastic fiber in concrete 441


Rabin Tuladhar and Shi Yin
21.1 Introduction 441
21.2 Sustainability in construction materials 442
21.3 Comprehensive LCA of recycled plastic fibers used for
reinforcing concrete 448
21.4 Conclusions 458
Acknowledgments 459
References 459

Index 461
List of contributors

I. Aghayan Shahrood University of Technology, Shahrood, Iran


Khaleel Al-Adham Civil & Environmental Engineering Department, King Fahd
University of Petroleum and Minerals, Dhahran, Saudi Arabia
Ali Asghar Asgharian Jeddi Textile Engineering Department, Amirkabir Univer-
sity of Technology, Tehran, Iran
Ankur C. Bhogayata Department of Civil Engineering Marwadi Education
Foundation’s Group of Institutions, Rajkot, India
Giuseppe Bonifazi Department of Chemical Engineering, Materials & Environ-
ment, Sapienza University of Rome, Rome, Italy

Miguel Angel Calzada-Pérez GCS Research Group, University of Cantabria,
Av. de los Castros 44, Santander, Spain
Francesco Colangelo Department of Engineering, University Parthenope of Naples,
Materials Science and Engineering Research GroupdMASERG, Centro Direzionale,
Is. C4, Naples, Italy
M.A. Dalhat Transportation and Traffic Engineering Department, College of
Engineering, Imam Abdulrahman Bin Faisal University, Dammam, Saudi Arabia
A. Elkordi Faculty of Engineering, Beirut Arab University, Beirut, Lebanon
Ilenia Farina Department of Engineering, University Parthenope of Naples,
Materials Science and Engineering Research GroupdMASERG, Centro Direzionale,
Is. C4, Naples, Italy
Dora Foti Department of Civil Engineering Sciences and Architecture, Polytechnic
University of Bari, Bari, Italy
M.A. Habib Civil & Environmental Engineering Department, King Fahd University
of Petroleum and Minerals, Dhahran, Saudi Arabia
Sheelan M. Hama Department of Civil Engineering, University of Anbar, Ramadi,
Iraq
B.A. Herki Faculty of Engineering, Soran University, Erbil, Iraq
Nahla N. Hilal Department of Civil Engineering, University of Anbar, Ramadi, Iraq
xii List of contributors

I. Indacoechea-Vega GITECO Research Group, University of Cantabria, Av. de los


Castros 44, Santander, Spain
Masoud Jamshidi School of Chemical Engineering, Iran University of Science and
Technology (IUST), Tehran, Iran
Senthil Kumar Kaliyavaradhan Key Laboratory for Green and Advanced Civil
Engineering Materials and Application Technology of Hunan Province, College of
Civil Engineering, Hunan University, Changsha, China
R. Khafajeh Shahrood University of Technology, Shahrood, Iran
J.M. Khatib Faculty of Engineering, Beirut Arab University, Beirut, Lebanon;
Faculty of Science and Engineering, University of Wolverhampton, Wolverhampton,
United Kingdom
M.M. Kocakerim Department of Chemical Engineering, Çankırı Karatekin Univer-
sity, Uluyazı Campus, Çankırı, Turkey
H. Korucu Department of Chemical Engineering, Çankırı Karatekin University,
Uluyazı Campus, Çankırı, Turkey
Floriana La Marca DICMA-Sapienza University of Rome, Rome, Italy
Pedro Lastra-Gonz alez GITECO Research Group, University of Cantabria, Av. de
los Castros 44, Santander, Spain
Tung-Chai Ling Key Laboratory for Green and Advanced Civil Engineering Mate-
rials and Application Technology of Hunan Province, College of Civil Engineering,
Hunan University, Changsha, China
Emanuela Lupo DICEA-Sapienza University of Rome, Rome, Italy
Santhosh M. Malkapur Department of Civil Engineering, Faculty of Engineering
and Technology, M.S. Ramaiah University of Applied Sciences, Bengaluru, India
Mohd Idrus Mohd Masirin Faculty of Civil and Environmental Engineering,
Universiti Tun Hussein Onn Malaysia, Rarit Raja Johor, Malaysia
Farnaz Memarian Textile Engineering Department, Amirkabir University of
Technology, Tehran, Iran
A.A. Mohammed Department of Civil Engineering, College of Engineering,
University of Sulaimani, Sulaimani, Iraq
Monica Moroni DICEA-Sapienza University of Rome, Rome, Italy
Mattur C. Narasimhan Department of Civil Engineering, National Institute of
Technology Karnataka (NITK) Surathkal, Mangalore, India
F. Pacheco-Torgal C-TAC Research Centre, University of Minho, Guimar~aes,
Portugal
List of contributors xiii

Hamid Reza Pakravan Textile Engineering Department, Amirkabir University of


Technology, Tehran, Iran
Z. Pavlík Department of Materials Engineering and Chemistry, Faculty of Civil
Engineering, Czech Technical University in Prague, Prague, Czech Republic
M. Pavlíkova Department of Materials Engineering and Chemistry, Faculty of Civil
Engineering, Czech Technical University in Prague, Prague, Czech Republic
Amir Masoud Saghafi Technical and Production Director, Savin Carpet Company,
Tehran, Iran
Goutham Sarang Assistant Professor (Senior), School of Mechanical and Building
Sciences (SMBS), Vellore Institute of Technology - Chennai Campus, Chennai, Tamil
Nadu, India
Silvia Serranti Department of Chemical Engineering, Materials & Environment,
Sapienza University of Rome, Rome, Italy
B. Şimşek Department of Chemical Engineering, Çankırı Karatekin University,
Uluyazı Campus, Çankırı, Turkey
Rabin Tuladhar Centre of Tropical Environmental and Sustainability Science, Col-
lege of Science and Engineering, James Cook University, Townsville, QLD, Australia
Nura Usman Faculty of Civil and Environmental Engineering, Universiti Tun
Hussein Onn Malaysia, Rarit Raja Johor, Malaysia; Department of Civil Engineering,
Hassan Usman Katsina Polytechnic, Katsina, Nigeria
T. Uyguno
glu Department of Civil Engineering, Afyon Kocatepe University,
Ahmet Necdet Sezer Campus, Afyon, Turkey
Marta Vila-Cortavitarte GITECO Research Group, University of Cantabria, Av.
de los Castros 44, Santander, Spain
Shi Yin College of Science and Engineering, James Cook University, Townsville,
QLD, Australia
M. Zalesk
a Department of Materials Engineering and Chemistry, Faculty of Civil
Engineering, Czech Technical University in Prague, Prague, Czech Republic
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Introduction to the use of
recycled plastics in eco-efficient 1
concrete
F. Pacheco-Torgal
C-TAC Research Centre, University of Minho, Guimar~aes, Portugal

1.1 The waste plastic problem


Deriving from the Greek word ’’plastikos’’ meaning fit for moulding, plastics
comprise mainly two broad categories (thermoplastics and thermosetting plastics).
The former include plastics (polyethylene, polypropylene, polysterene, polycarbon-
ates, etc.) that can be heated up to form products and if needed can be reheated and
melted again for new forms. In contrast, the latter (polyurethane, polyesters,
phenolic and acrylic resins, silicone, etc.) can be melted and formed, but unlike ther-
moplastics cannot be remelted. The global production of fossil-based plastics has
grown more than 20-fold since 1964 to 322 million ton in 2015 (Wei and Zimmer-
mann, 2017; PlasticsEurope, 2017). Not only the production of plastics consumes
yearly 4%e8% of the global crude oil extraction meaning that if plastics are
disposed instead of being recycled, these resources are lost but the worst part is
that plastic waste is harmful because pigment contains many trace elements that
are highly toxic and need hundreds of years to degrade (Huysman et al., 2017).
More worrying is the several millions of tons of plastic waste that are entering the
ocean each year, for quite some time, whose damaging action has been addressed
by several authors (Eriksen et al., 2014; Jambeck et al., 2015; Sussarellu et al.,
2016; Green et al., 2016; MacArthur, 2017; Lamb et al., 2018). Between 8 and 24
tons of plastic waste enter oceans each minute (Haward, 2018).
According to ten Brink et al. (2018), the annual cost of marine litter is conserva-
tively estimated at US$ 40 billion. And in July 19, 2017 Science magazine published
an article warning that by 2050, we’ll have produced 26 billion tons of plastic waste,
half of which will be dumped in landfills and the environment (Guglielmi, 2017). It’s
then no surprise that target 14.1 of the 2030 Agenda for Sustainable Development
seeks to prevent and significantly reduce marine pollution of all kinds, in particular,
from land-based activities, including marine debris, by 2025. Yes, it’s true that on
17th of April 2018 a paper published in the Proceeding of the National Academy
of Sciences of the United States of America (Austin et al., 2018) reported the discov-
ery of an enzyme that can digest highly crystalline PET and also polyethylene-2,5-
furandicarboxylate (PEF). However, as Oliver Jones, analytical chemist at RMIT
University in Melbourne, recognized “there is still a way to go before you could
recycle large amount of plastic with enzymes” (Gabbatiss, 2018). But a more wise

Use of Recycled Plastics in Eco-efficient Concrete. https://doi.org/10.1016/B978-0-08-102676-2.00001-3


Copyright © 2019 Elsevier Ltd. All rights reserved.
2 Use of Recycled Plastics in Eco-efficient Concrete

position was made by Adisa Azapagic, at the University of Manchester who


mentioned that “A full life-cycle assessment would be needed to ensure the technol-
ogy does not solve one environmental problemdwastedat the expense of others,
including additional greenhouse gas emissions” (Carrington, 2018). And if a lesson
can be extracted from this case, it is that scientists should have some lessons on pub-
lic communication, a problem recognized several years ago (Soapbox Science, 2012;
Goldstein, 2012; Grant, 2016). In the meantime a study published on May of 2018
showed that each liter of sea ice on the Arctic contained around 12,000 particles of
plastic (La Daana et al., 2018). No wonder then that a previous study (Wilcox et al.,
2015) revealed that around 90% of seabirds have plastic waste particles in their gut
that they mistakenly took to be fish eggs. Also, Rochman (2018) recently showed
that the ocean is not the only place to suffer damaging environmental impacts.
Around 26 million tons of plastic waste are generated in Europe every year, which
makes Europe the second largest producer of plastic materials, being responsible for
20% of the world production. Packaging applications, the largest application sector,
represent 39.6% of the total plastic demand (Huysman et al., 2017). In the past years
significant share of European waste plastics leave the EU to be treated in third world
countries, where different environmental standards may apply (EUROSTAT,
EuropePlastics). However, since January of 2018 China decided to ban the imports
of 24 kinds of waste including waste plastic which will aggravate the problem of
plastic waste in Europe. And that is why plastic waste is one of the five priority areas
in the EU action plan for the circular economydCE (EC, 2015a). The CE concept
may have been inspired by Rachel Carson’s Silent Spring and the “limits to growth”
thesis of the Club of Rome in the 1970s (Winans et al., 2017) and is being promoted
by the EU, but several national governments still argue (Geissdoerfer et al., 2017)
that the conceptual relationship between the CE and sustainability is not clear, hav-
ing detrimental implications for the advancement of sustainability science. Others
(Korhonen et al., 2018) mentioned that the CE practice has almost exclusively
been developed and led by practitioners, that is, policy-makers, businesses, business
consultants, business associations, and business foundations and as a result the
research content of the CE concept is superficial and unorganized.
Still in the European Union context, looking into the past is worth remembering that
the previous Directive 94/62/EC had imposed a recycling target which required 22.5%
of waste plastic packaging to be recycled. This target increased toward 55% by 2030
(EC, 2015b) but on March 14 of the 2017 the European Parliament voted for legisla-
tion to aim for a recycling rate target of 70% by 2030, with a proposed 80% target for
packaging materialsdincluding paper, cardboard, plastics, glass, metal, and wood.
This constitutes a high ambition postured by the EU and there is still some controversy
regarding job creation in the field of waste recycling. While the report cited by the Eu-
ropean Parliament mentioned the possibility of creation of 1e3 million jobs (IP, 2017)
the fact is that the European Commission has presented a much lower number of just
170,000 direct jobs (Politico, 2018). Most of these optimistic projections usually tend
to forget that as Cooper and Gutowski (2017) recently pointed the fact that reusing a
product does not guarantee an environmental benefit because of the need to upgrade
old product efficiencies and the fact that more efficient new products can be on the
Introduction to the use of recycled plastics in eco-efficient concrete 3

market. For instance, as contradicting as it may seem, Dunant et al. (2018) showed that
reused steel is somewhat more expensive than new steel elements. Fig 1.1 shows plas-
tic post-consumer waste rates of recycling, energy recovery, and landfill per country in
2016 and also the group of 10 countries that have implemented landfill restrictions.
The figure illustrates in a very clear way the effort that needs to be taken to close
the gap between the state-of-the-art plastic waste recycling and the new recycling tar-
gets. Of course energy recovery is nothing more than incineration (Eriksson and Finn-
veden, 2017).
Also the proof that the new and ambitious waste plastic recycling approved by the
European Parliament could be hard to achieve is given by Karl-H. Foerster, executive
director of industry organization Plastics Europe, who responded to the parliamentary
proposals, saying that: “Taking into account today’s recycling technology, we already

Figure 1.1 Plastic waste rates of recycling, energy recovery, and landfill per country (Plastics, 2017).
4 Use of Recycled Plastics in Eco-efficient Concrete

consider that the 55% plastics packaging preparing for re-use and recycling target pro-
posed by the Commission is challenging. We would therefore like to call on the Pres-
idency of the Council to carefully assess the impact prior to adopting any substantive
amendment to the rules on the calculation initially proposed by the Commission.” That
position however must be seen in the light of the interests of the associates of Plastics
Europe which are in the business of plastic manufacture and not in the business of
waste plastic recycling. Of course, some European countries like the Netherlands,
which in 2014 already recycled 50% of (packaging) plastics, aiming for 52% in
2022 (Gradus et al., 2017) will be in a better position to achieve this requirements.
Be there as it may, the truth is that even countries with top performance concerning
plastic waste recycling like Austria recognized that in order to achieve the proposed
increased target major steps will be needed with respect to both collection and sorting
of waste plastic (Van Eygen et al., 2018). This also means that even in Europe there’s
still much to do in order to aim at a 100% recycling target (zero plastic waste scenario).
In January 16 of 2018 the European Strategy for Plastics in a Circular Economy was
released (COM, 2018). The document confirmed that more than 85% of plastic was
sent to China. The document mentions that internalizing the environmental costs of
landfilling and incineration through high or gradually rising fees or taxes could
improve the economics of plastic recycling. However, this is just wishful thinking
lacking a sound study. More likely it could constitute an incentive for illegal dumping
or for exportation of plastic wastes to Africa as was mentioned in a United Nations
University study (PiP, 2017) meaning that at this moment it is not possible to forecast
how increasing recycling targets and the use of internalizing the environmental costs
through rising fees or taxes may lead to an increase of smuggling waste to third world
countries. The concept of eco-efficiency was firstly coined in the book Changing
Course (Schmidheiny, 1992) in the context of 1992 Earth Summit process. This
concept includes "the development of products and services at competitive prices
that meet the needs of humankind with quality of life, while progressively reducing
their environmental impact and consumption of raw materials throughout their life cy-
cle, to a level compatible with the capacity of the planet.” All of these give an impor-
tant value to the option of recycling waste plastics through concrete, which is the most
consumed material in our planet, about 25 gigatonnes per year around 3.5 ton per
capita (Hossain et al., 2018). Not to mention the several billion tons of asphalt concrete
used by the pavement industry each year. The use of recycled plastics in eco-efficient
concrete can be done mainly by replacing natural aggregates, as binders and also as
recycled fibers, allowing for improvements in the ductility of concrete composites.
Those are the areas covered by this book.

1.2 Outline of the book


This book thus provides an updated state-of-the-art review on the use of recycled plas-
tics in eco-efficient concrete.
Part I encompasses processing of plastic wastes (Chapters 2e4).
Introduction to the use of recycled plastics in eco-efficient concrete 5

Chapter 2 concerns techniques for the separation of plastic waste namely gravity
separation, electrostatic separation, magnetic density separation, flotation, and
sensor-based sorting. Auxiliary technologies usually found in plastic recycling plants
are also described: magnetic and Eddy current separators. The importance of recycled
plastic quality control and product certification is strongly pointed out, reporting both
traditional and advanced quality measurement techniques.
Chapter 3 discusses hydraulic separation of plastic waste. This chapter presents an
original device for the hydraulic separation of plastic polymers from mixtures. An
extensive experimental campaign was conducted to investigate the effectiveness of
the apparatus, using two geometric arrangements, nine hydraulic configurations, and
three selections of polymers at three stages of a material’s life cycle. Experimental
data were also employed to validate a numerical model developed within the frame-
work of Computation Fluid Dynamics. The separation results were evaluated in terms
of grade and recovery of a useful material.
Chapter 4 presents the case for the production of recycled plastic fibers. The pro-
duction process includes melt-spinning and hot-drawing processes, which increase
crystallinity of the plastic polymer fibers and improve its mechanical properties.
Part II concerns the case of concrete with recycled plastic as aggregate or binder
(Chapters 5e15).
Chapter 5 reviews the fresh properties of concrete with plastic aggregates. The
chapter also reviews the case for fresh properties of self-compacting concrete.
Chapter 6 covers mostly the mechanical strength of concrete with polyvinyl chlo-
ride (PVC) aggregates including compressive and tensile strength and modulus of
elasticity.
Chapter 7 provides a comprehensive review of concrete containing Expanded Poly-
styrene (EPS), covers recent research, including some recent research by the authors,
with some details on the compositions of concrete mixes, presentation, and discussion
of the results obtained. The review includes the influence of different amounts of EPS
as a replacement for natural aggregates on the different mechanical, physical, and dura-
bility properties of lightweight aggregate concretes (LWAC). The chapter also in-
cludes the methods and techniques for recycling waste EPS to be utilized in concrete.
Chapter 8 deals with the use of polyolefin waste aggregates (PWA) obtained from
recycled plastics and used as plastic aggregates to replace the natural ones to produce
lightweight aggregate concrete (LWAC). The mechanical properties (compressive and
tensile strength) and physical properties (porosity, density, and thermal stability) are
determined. Furthermore, the postfire residual mechanical performance, ultrasonic
testing, and compression force are evaluated.
Chapter 9 is concerned with waste polypropylene-based aggregates, in terms of its
physical, mechanical, and hygric properties and, in particular, of thermal attributes and
optimum energy performance in building construction.
Chapter 10 addresses polymers for enhancing neutron radiation shielding of con-
crete. Past research in the field is reviewed. The feasibility issues and concerns while
using virgin and waste pulverized High-density polyethylene (HDPE) polymeric ma-
terials as partial replacement to fine aggregates for making concrete mixes with
enhanced neutron radiation shielding characteristics are discussed. The fresh and
6 Use of Recycled Plastics in Eco-efficient Concrete

hardened properties of these mixes and their effect on neutron radiation shielding are
also discussed.
Chapter 11 reviews the reuse of dioctyl terephthalate (DOTP) obtained from waste
PET into concrete. Fresh properties as well as mechanical properties of hardened con-
crete are reviewed, along with thermal conductivity. Performance comparisons be-
tween DOTP concrete and PET concrete are also reviewed.
Chapter 12 covers studies investigated in the usage of PET wastes in asphalt
mixture. The volume and mechanical properties of asphalt mixtures containing PET
wastes along with the physical characteristic of the PET-modified binder are examined.
Chapter 13 discloses results on a case study of asphalt concrete performance with
different plastic wastes. Mechanical properties and durability parameters are covered.
Emissions footprint is also covered.
Chapter 14 discusses the need of stabilization of asphalt concrete and different sta-
bilizer materials using recycling plastics. Suitable methods for incorporating waste
plastics, advantages of each, performance of waste plastic added mixtures are dis-
cussed in detail with brief information on some field evaluations.
Chapter 15 reviews the use of recycled plastic as partial replacement of bitumen in
asphalt concrete. The need for stabilization of asphalt concrete is reviewed. The per-
formance of asphalt concrete with plastics is also addressed.
Finally, Part III covers concrete with recycled plastic fibers (Chapters 16e22).
Chapter 16 surveys the usage of metalized plastic waste (MPW) as a cement con-
crete constituent in a macrofibrous form. The chapter focuses on how to obtain the op-
timum quantity of MPW fibers with a suitable size to be used in concrete and changes
in the deformation response due to the axial compression along with the evaluation of
preliminary material properties.
Chapter 17 addresses concrete with PVC fibers in the fresh and hardened state. It is
suggested that the use of PVC fibers, either 0.8% (by weight of cement) or 0.2% (by
volume of concrete), could significantly improve the performances of concrete. Lim-
itations and practical issues on the utilization of PVC fibers in concrete mixes are iden-
tified. Hence, recommendations and future research needs on the practical implications
of the use of PVC fibers are given at the end of the chapter.
Chapter 18 addresses the case of polymers added to concrete in the form of binder
or as discrete elements (fibers) or continuous (strips) can limit the presence of cracks
and especially avoid the corrosion processes in reinforced concrete structural elements.
In more detail, the effect of polyethylene terephthalate (PET) on concrete mix is espe-
cially considered. Laboratory results of concrete reinforced with PET fibers derived
from recycled water bottles and with different shapes are analyzed.
Chapter 19 presents an overview of physical and mechanical properties of concrete
containing recycled carpet waste fibers, as well as the carpet structure and fiber
properties.
Chapter 20 gives details of a case study on the performance of asphalt concrete rein-
forced with recycled PET fibers.
Chapter 21 closes Part III with a chapter on the life cycle assessment. The produc-
tion of 100% recycled polypropylene fibers is compared with the environmental im-
pacts of virgin PP fibers and steel reinforcing mesh.
Introduction to the use of recycled plastics in eco-efficient concrete 7

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Techniques for separation of
plastic wastes 2
Silvia Serranti, Giuseppe Bonifazi
Department of Chemical Engineering, Materials & Environment, Sapienza University of
Rome, Rome, Italy

2.1 Introduction
Mechanical recycling, which is the processing of waste by physical means, represents
the main approach to follow in order to recover plastics. This process typically
includes different actions, such as collection, screening, manual and/or automatic
sorting, size reduction, washing, extrusion, and granulation that may occur in different
sequences and more than one at a time, according to the characteristics of the feed plas-
tic waste, in terms of origin, size, shape, and composition (Hopewell et al., 2009;
Ragaert et al., 2017).
Foundation of each mechanical process, finalized to separate a specific material
inside a flow stream containing other materials also, is to know the different properties
of the target material, with respect to the actions to be applied (i.e., comminution,
classification, separation). Important material properties useful to select the best
separation strategies for segregation of plastic waste include: particle size, class
distribution, density, magnetic and electric properties, color, shape, etc. Density
usually represents one of the most utilized properties to perform material separation.
Unfortunately, some polymers are characterized by very close values of density
(Al-Salem et al., 2009); in these cases this property cannot be successfully utilized,
especially to obtain high-quality single polymer streams.
The need of powerful technologies to perform plastic waste separation, being at the
same time cost-effective and able to guarantee high quality of products in terms of pu-
rity is more and more stringent in order to produce secondary plastics that are compet-
itive in the market in comparison with the virgin polymers. In fact, the actual economic
and environmental constraints dramatically increase the interest of many players (i.e.,
industries, recyclers, technology developers, engineers, etc.) both in waste-sorting
technologies, for the production of high-quality secondary polymers, and in devel-
oping automatic sensors for quality assessment of waste-derived secondary polymers.
On December 2015 plastic was in fact identified by the European Commission as a key
priority in the “EU Action Plan for a circular economy” (COM, 2015) and in January
2018 a “European strategy for plastics in a circular economy” (COM, 2018) was
adopted in order to use such a resource in a more sustainable way, including measures
for the improvement in plastic sorting and recycling capacity and in quality of recycled
plastics.

Use of Recycled Plastics in Eco-efficient Concrete. https://doi.org/10.1016/B978-0-08-102676-2.00002-5


Copyright © 2019 Elsevier Ltd. All rights reserved.
10 Use of Recycled Plastics in Eco-efficient Concrete

A mechanical process aimed to perform plastic waste recycling is based on the uti-
lization of fast, accurate, and reliable tools and equipment specifically addressed to
separate and recover single polymer streams, eliminating polluting elements (i.e., other
polymers or other materials) present in the feed. As already stated, recycling plant
layout has to be developed and managed taking into account the different polymers
in the feed as well as the presence of other materials, both aspects in relation to the
plastic waste sources (Ignatyev et al., 2014), that is: virgin and used ones. The
polymer-based products that belong to the first source class (i.e., virgin waste) never
reached the consumer (i.e., runners from injection molding, waste from production,
changeovers, fall-out products, cuttings, and trimmings). These start-of-life plastic
wastes are usually uncontaminated both from other polymers and/or nonpolymers.
Obviously, they represent the higher-quality grades of polymer waste. End-of-life plas-
tic wastes belong to the second source class (i.e., postconsumer waste). These latter can
strongly vary both in quantity and in quality according to the collecting source and/or
the adopted collecting strategies.
Mechanical recycling can be applied to plastic waste sorting following two different
approaches, that is, at macro- or microscale.
Plastic macrosorting is usually performed when the waste flow stream contains the
polymers to be recovered as macroobjects easy to be identified and separated. In this
case, any specific mechanical action (i.e., size reduction/screening) has to be prelimi-
nary applied and waste plastics, usually bottles and containers, are separated. Specific
polymer attributes are first detected by specialized sensing devices and according to
their characteristics further separated, usually following air-blowebased strategies.
Manual separation strategies are also applied and human knowledge is at the base
of the separation, It is a labor-intensive, costly, and inefficient option, even if today
plastic containers are labeled according to the constituting polymer and/or blend of
polymers.
Plastic microsorting is usually applied when waste plastics are recovered as flakes,
that is, individuals resulting from milling actions, inside a flow stream of mixed waste
characterized by different physical chemical attributes. In this case, handling costs
decrease and the quantity of waste strongly increases, but more complex, and often
also sophisticated technologies have to be designed, implemented, set up, and applied.
These technologies (e.g., size reduction, screening, separation, etc.) are usually
sequentially applied. In the latter case, sorting units and related logics, both addressed
to separation and/or recovered polymer flow stream quality assessment play a preem-
inent role.

2.2 Plastic waste sources and typologies


2.2.1 Production of plastic waste
Over the last 50 years the role and importance of plastics in our economy have grown
steadily. World plastic production has increased twentyfold compared to the 1960s
reaching 335 million tonnes in 2016 (Plastics the Facts, 2017), and should double
in the next 20 years. In the EU, plastic production reached 60 million tonnes in
Techniques for separation of plastic wastes 11

2016. The largest plastic producers are China (29%), followed by Europe (19%) and
NAFTA (18%).
Despite the global increase in plastic production, the potential for recycling plastic
waste is still largely unexploited. The reuse and recycling of plastic at the end of life
are very low, especially compared to other materials such as paper, glass, and metal.
The European plastics converter demand by segment in 2016 is reported in Fig. 2.1,
showing that the packaging sector accounts for 39.9%, followed by building and con-
struction (19.7%); automotive (10%); electrical and electronic equipment (6.2%);
household, leisure, and sports (4.2%), agriculture (3.3%). Other sectors, including ap-
pliances, mechanical engineering, furniture, medical, etc., account for the remaining
16.7% (Plastics The Facts, 2017).
In Fig. 2.2 the European distribution of plastic waste generation by segment in 2015
is reported. It is evident that the main source of plastic waste is packaging, accounting
for 59% of the total plastic waste. It can be noticed that from production to waste,
different plastic products are characterized by different life cycles, depending on their
use, for example, plastic packaging has a service life of less than 1 year, plastic for in-
dustrial equipment can have a service life of 40 years or more. That is the reason why
the volume of collected plastic waste in 1 year usually does not match the volume of
plastic production.
About 27.1 million tonnes of plastic waste were collected in Europe in 2016
(Plastics The Facts, 2017), of which 31.1% was collected for recycling, 41.6% for
energy recovery and 27.3% still went to landfill. Even if the percentage of recycled
plastics is quite low, a positive aspect is that in the past 10 years (from 2006 to
2016) plastic waste recycling has increased by 79% and landfill has decreased by
43%. Unfortunately, even if the EU situation is improving, in many countries landfill
is still the first or second option for plastic waste.
Concerning plastic packaging waste treatment, in 2016 recycling was the first
option accounting for 40.9%, followed by energy recovery (38.8%) and landfill
(20.3%).

Plastic demand by different market sectors (%)


Packaging 39.90%

Building &
construction 19.70%

Automotive 10.00%

Electrical & electronic


6.20%

Household, leisure &


sports 4.20%

Agriculture 3.30%

Others 16.70%

Figure 2.1 Plastic demand by different market sectors in 2016.


Plastics The Facts, 2017.
12 Use of Recycled Plastics in Eco-efficient Concrete

EU plastic waste generation (%)


Others 14.00%

Agriculture 5.00%

Non packaging
household 4.00%

Electrical & electronic


8.00%

Packaging 59.00%
Automotive 5.00%

Building & construction


5.00%

Figure 2.2 EU plastic waste generation in 2015.


COM, 2018. A European Strategy for Plastics in a Circular Economy. p. 28.

It was estimated that plastic production and the incineration of plastic waste
generate a total of about 400 million tonnes of CO2 per year (Ellen MacArthur
Foundation, 2016). Increased use of recycled plastics can reduce dependence on fossil
fuel extraction for plastic production and contain CO2 emissions. According to esti-
mates (Rahimi and García, 2017), recycling of plastic waste from around the world
could result in annual energy savings of 3.5 billion barrels of oil.
Alternative types of raw materials are also being developed (for example, bio-based
plastics or plastics produced from carbon dioxide or methane), which offer the same
functionalities of traditional plastics with a potentially lower environmental impact,
but currently represent a very small slice of the market.
Very large quantities of plastic waste, generated both on land and at sea, are
dispersed in the environment, causing considerable economic and environmental dam-
age. Worldwide, between 5 and 13 million tonnes of plastics end up in the oceans each
year, representing between 1.5% and 4% of the world production of this material
(Jambeck et al., 2015). Plastic is estimated to account for over 80% of marine litter.
The plastic residues are transported by sea currents, sometimes even for very long dis-
tances, and can be deposited on land, break up into microplastics, or form dense areas
trapped in oceanic gyres.
The phenomenon is accentuated by the increasing amount of plastic waste gener-
ated every year, also due to the growing diffusion of “single-use” plastic products,
for example, packaging or other consumer products thrown away after only one short
use, rarely recycled, and subject to being dispersed in the environment. These products
include small packaging, bags, disposable cups, lids, straws, and cutlery, in which the
plastic is widely used for its lightness, low costs, and practical features.
New sources of plastic dispersion are also increasing, generating further potential
risks to the environment and human health. Microplastics, defined as tiny plastic frag-
ments smaller than 5 mm, accumulate in the sea, where, due to their small size, they
can be easily ingested by marine fauna, and can also enter the food chain. Recent
studies have found the presence of microplastics in the air, in drinking water, and in
foods, and their impact on human health is still unknown.
Techniques for separation of plastic wastes 13

Furthermore, the increase in the market share of plastics with biodegradable prop-
erties creates new opportunities but also generates risks. In the absence of a clear
labeling for consumers and without proper collection and processing of waste, it could
lead to an increase in the dispersion of plastics and create problems for mechanical
recycling. On the other hand, biodegradable plastics can certainly be useful for
some applications and innovation in this sector is welcomed.

2.2.2 Typologies of polymers, characteristics, and uses


The term “plastic” is derived from the Greek word “plastikos,” meaning fit for
moulding. This refers to the material’s malleability or plasticity during manufacture,
which allows it to be cast, pressed, or extruded into a variety of shapesdsuch as films,
fibers, plates, tubes, bottles, boxes, and much more. There are two categories of plas-
tics: thermoplastics and thermosets. Thermoplastics can be melted when heated and
hardened when cooled, the process is reversible. Due to their characteristics, they
can be reheated, reshaped, and frozen many times Thermoplastics include polyeth-
ylene terephthalate (PET), low-density polyethylene (LDPE), polyvinyl chloride
(PVC), high-density polyethylene (HDPE), polypropylene (PP), and polystyrene
(PS) among others. On the contrary, thermosets undergo a chemical change when heat-
ed, so they cannot be remelted and reshaped. Thermosets are widely used in electronics
and automotive products. Thermoset plastics include epoxy, polyester, melamine,
phenol formaldehyde, vulcanized rubber, silicone, polyurethane (PUR), etc.
Each plastic is identified by a resin code that was introduced to facilitate recycling
operations (ASTM, 2014). In Table 2.1 a list of the main plastic types, with their
typical applications, is reported.
The most diffused polymers, according to plastic converter demand, are (Fig. 2.3):
PP, LDPE, HDPE, PVC, PUR, PET, and PS. Such polymers are also the most abun-
dant in plastic waste with some variations according to different lifespan of products.
Polyethylene (LDPE and HDPE) is the most abundant polymer in plastic waste, due to
their dominance in packaging applications, followed by PP, forming together the
polyolefin family, accounting for 56.1% of plastic production demand. Other poly-
mers, accounting for 19.3% of the total, are mainly represented by acrylonitrile buta-
diene styrene (ABS), polycarbonate (PC), polymethyl methacrylate (PMMA),
polybutylene terephthalate (PBT), polytetrafluoroethylene (PTFE), utilized in many
different fields, such as medical, electronics, aerospace, etc.

2.3 The plastic recycling chain


The plastic recycling chain can be divided in the following operations:

Manual Material/ Size Extrusion &


Collection sorting Screening polymer reduction Washing granulation
sorting
14 Use of Recycled Plastics in Eco-efficient Concrete

Table 2.1 Main plastic types and their typical applications


Resin
code Polymer name Applications

Polyethylene Terephthalate Drink bottles, detergent bottles, clear


film for packaging, food trays,
carpet fibers
High-Density Polyethylene Detergent bottles, mobile components,
agricultural pipes, pallets, toys

Polyvinyl Chloride Packaging for food, medical materials,


pipes, window frames, cable
insulation
Low-Density Polyethylene Foil and films for dry cleaning, bread,
frozen food, fresh produce and
household garbage, toys, squeezable
bottles
Polypropylene Containers for food, medicine bottles,
bottle caps, bins, automobile
applications
Polystyrene Disposable cutlery, cups and plates,
meat trays, protective packaging for
furniture, electronic items and toys
Other. Use of this code indicates that a Other packaging
package is made with a resin other
than the six listed above, or is made
of more than one resin and used in a
multilayer combination.

European plastics demand by polymer types


19.3% 19.3%
17.5%

12.3%
10.0%

7.4% 7.5%
6.7%

PS PET PUR PVC HDPE LDPE PP Others

Figure 2.3 European plastics converter demand by polymer types in 2016.


Plastics The Facts, 2017.
Techniques for separation of plastic wastes 15

Each step of the chain affects the others. For example, the selection of the sorting
technology will depend on the characteristics of collected plastic waste (types,
composition, etc.) and the final destination of the recovered product will depend
on its quality.
Collection is carried out adopting different systems, depending also on the different
sources, such as plastics from household waste and from industrial waste. Collection
can be, for example, monomaterial, if plastic is collected as source-separated fraction,
or multimaterial, if plastic is collected with other packaging materials (aluminum,
glass, etc.).
Manual sorting is usually necessary at the beginning of the recycling process for the
preliminary removal of films, cardboard, and bulky items and is usually carried out by
operators checking the waste stream on the conveyor belt.
Screening is applied to remove small objects such as glass and stones. Typical
screening equipment are drum or vibrating screens. Usually waste is divided into three
fractions: undersize (<50 mm), middle size (from 50 to 300 mm), and oversize
(>300 mm). Usually plastic is concentrated in the middle size fraction.
Material/Polymer Sorting has the aim to obtain high-quality recycled plastic
products, preferably single polymer stream. Sorting technologies are based on
different physical-chemical properties of waste materials, such as shape, density,
size, color, or chemical composition of objects. Material sorting consists in the
removal of the unwanted contaminants such as pieces of metals, glass, paper, etc.,
from the plastic waste stream. Polymer sorting is applied to separate polymers by
type; this step is of paramount importance in order to obtain high-quality single
polymer stream. The different plastic waste separation technologies are described
in Section 2.4.
Size reduction is usually carried out by shredding or cutting techniques; such oper-
ations can be present before or after the sorting step, depending on the plant layout and
on the typology of plastic waste stream. Plastics are usually shredded in flakes having a
size of 5e10 mm.
Extrusion and granulation: this step is necessary to produce a granulate which is
easier to use for converters than flakes. The polymer flakes are fed into the extruder,
are heated, and then forced through a die to form a continuous polymer product
(strand) which can then be cooled in a water bath before being pelletized. The granu-
lation process is used to reduce the strands to pellets which can then be used for the
manufacture of new products.

2.4 Plastic waste separation technologies


Plastic waste separation has the main aim to remove unwanted contaminants (such as
metals, glass, etc.) and to obtain high purity polymers. In the following sections the
different separation technologies usually adopted in plastic recycling plants are
described. The choice of the technology (or combination of more than one technology)
will depend on the feed characteristics and on the quality requirements for the output
products, for example, single polymer stream or mixed polymer stream.
16 Use of Recycled Plastics in Eco-efficient Concrete

2.4.1 Gravity separation


2.4.1.1 Dry
Air classifier
Air classifiers use air as the medium to separate lighter materials from heavier ones.
The waste stream enters the column with a raising current of air and lighter objects
are blown upward whereas heavier ones are dropped down (Fig. 2.4). Air classifiers
are usually utilized to remove light contaminants such as dust, small foam particles,
paper, glass powders, and polymer foils from the main plastic waste stream. To reach
this goal, aspirators, wind sifters of air-cyclonesebased techniques are utilized. The
separation occurs based on the different behavior of particles when subjected to a
stream of air. Even if the separation principle is quite simple, air-based classification
has to take into account different parameters (i.e., particle density, morphological
and morphometrical characteristics) that interact with single polymer terminal veloc-
ity, thus affecting separation efficiency and corresponding operative setup (Shapiro
and Galperin, 2005). Air classifiers can be utilized after a gravity separation step or
at the beginning of the process before or after a preliminary comminution stage, to
properly handle/separate complex plastic-rich parts from end-of-life durables (e.g.,
automotive-derived parts, electrical and electronic devices, appliances, etc.).

Ballistic separator
Ballistic separation is based on a simple principle, that is, the different movement char-
acteristics of particles of different size, shape, and weight, spatially defined as 2D or
3D structures (Christensen and Fruergaard, 2011). Ballistic separation can be success-
fully utilized both for mixed waste containing plastics and for plastic waste streams. In
the first case, film, paper, cardboard, textiles, and fibrous materials can be assigned to a
2D flat and light class of products; on the contrary, plastic containers, bottles, stone,

Light

Feed
Air stream

Heavy
Figure 2.4 Schematic representation of an air classifier.
Techniques for separation of plastic wastes 17

wood, cans, and ferrous materials can be assigned to a 3D class of rolling and heavy
products. In the second case, films and flakes belong to 2D individual domains; on the
contrary, containers and/or crumpled containers belong to 3D individual domains. In
both cases separation occurs thanks to the utilization of a so-called ballistic separator,
or ballistic screen. Such a device is usually constituted by a series of screening paddles,
or perforated plates, whose number, size, and shape profile can vary according to the
feed rate and physical characteristics of the waste materials, affected by an orbital
motion and characterized by an inclined position, usually ranging from 10 degrees
to 20 degrees. The materials fed to this separator, according to their 2D or 3D structure
and physical characteristics (i.e., weight, morphological and morphometrical charac-
teristics) follow different trajectories with respect to the orbital blades movement.
The 2D and light materials are conveyed to the upper part of the ballistic separator,
whereas 3D, heavier, and “rolling” individuals move toward the lower part of the sepa-
rator. The continuous shaking of the waste produces also a screening effect: particles
characterized by a size smaller than the distance between the different screening pad-
dles pass through, generating a third flow stream.

2.4.1.2 Wet
Sink-float separation
Sink-float separation processes are based on the utilization of the different density
properties of materials. Separation is based on the fact that when materials are intro-
duced in a tank containing a fluid of a specific density, lighter materials will float
and heavier ones will sink (Fig. 2.5). A sink-float separation unit is efficient when
materials are characterized by quite different density values (Callister and Rethwisch,
2010). Therefore this method can be used to separate plastics from heavier materials,
or polymers characterized by different densities (i.e., PET from PP/PE or ABS from

Floating plastic flakes

Sinking plastic flakes

PP, HDPE, LDPE

Float PVC, PET, ABS


plastics with
specific gravity < 1 g/cm3
Water
Sink specific gravity =
plastics with 1 g/cm3
specific gravity < 1 g/cm3

Figure 2.5 Sink-float separation.


18 Use of Recycled Plastics in Eco-efficient Concrete

PS), whereas it cannot be utilized for separation of polymers characterized by quite


close density values, as for example polyolefins (PP, LDPE, HDPE). Presence of con-
taminants, air bubbles on polymer surface, polymer alteration, fillers, and additives can
affect separation efficiency.

Jigging
Jigging is one of the oldest methods of gravity concentration (Hori et al., 2009).
Jigging can be defined as an “enhanced gravity based separation” method: a water
stream is pulsed, or moved by pistons upward and downward, through the material
bed. Individuals are separated according to their densities, but also thanks to the sys-
tematic and repetitive applied pulsation, whose frequency and amplitude is strictly
related to physical, morphological, and morphometrical attributes of materials. With
reference to plastic waste, this procedure is quite efficient in many cases, allowing
to enhance polymer separation with respect to their relatively low density differences.
Thanks to the repetitions of these actions, particles stratify, across the bed height, ac-
cording to their specific density: the heaviest form the lowest layer and the lightest
constitute the highest.

Hydrocycloning
Hydrocycloning is a density sorting technology based on the centrifugal/centripetal
forces and fluid resistance of different particles having different characteristics
(Bradley, 1965).
A slurry is usually fed to the cyclone. A selected solid/liquid ratio and operative
pressure is adopted. As a result, the fluid pressure transfer produces, inside the device,
a rotational fluid motion, thus permitting separation among the different materials (i.e.,
polymer-contaminant or polymer-polymer characterized by different densities).
Lighter fractions will be transported to the upper part of the cyclone, the heavier
ones to the bottom (Fig. 2.6).

Light plastics
stream

Plastic waste
feed

Heavy plastics
stream
Figure 2.6 Plastic hydrocyclone separator.
Techniques for separation of plastic wastes 19

Materials have to be properly milled before hydrocyclone-based sorting. The sep-


aration mechanism can be synthetically summarized as follows. The slurry is tangen-
tially fed to the inlet, causing the material to rotate within the vessel and ultimately to
form a vortex. Heavier materials are forced outward by centrifugal force and down
from the barrel section into the cone section. Materials heavier than fluid (i.e., usually
water) flow down the inner wall and exit through the apex; the lighter materials
sweep into the center vortex by inward fluid motion and are carried out to the outlet.
When hydrocyclones are selected, several factors have to be considered in order to
reach an optimal and efficient utilization: the need of relatively complex fluid-
dynamic circuits (i.e., presence of pumps, storage bins, pipes, valves, etc.) and the
need to perform a strict feed characteristics control (i.e., constancy of water/solids
ratio, polymers particle morphological and morphometrical characteristics, polymers
surface status).

2.4.2 Electrostatic separation


Electrostatic separation is usually applied when dielectric particles are handled.
Dielectric particles, when electrostatically charged, can be separated according to their
polarity charge (Reinsch et al., 2014). The electrostatic separation architecture is
commonly constituted by two electrodes: one positive and the other negative. Particle
charging conditions and modality are of paramount importance in this kind of separa-
tion. Plastic particles charging is usually carried out utilizing the triboelectric effect.
This effect is based on rubbing together plastic waste particles of different character-
istics; as a result they transfer their electrical charge and surfaces are thus affected by
different electrical charges allowing to perform separation inside an electric field
where also charged electrodes are present. For example, charged plastics falling
down freely in the area between two electrodes change their trajectory due to the mobi-
lized attractive/repulsive electrostatic forces and as a consequence can be “easily”
collected and separated (Fig. 2.7). This separation can be successfully applied with
reference to several polymers, according to the triboelectric charging sequence
(Dodbiba et al., 2001):

ðþ Þ ABS  PP  PC  PET  PS  PE  PVC  PTFE ð Þ

When two plastics in this sequence are rubbed against each other, the plastic closer
to the positive end is charged positively and the one closer to the negative end is
charged negatively. For example, if PVC is rubbed against PET, PVC is charged nega-
tively and PET positively. On the contrary, when PET is rubbed against PP, PET is
charged positively and PP negatively.
Main disadvantages of this separation are linked to: (1) the operative conditions
(i.e., plastics and more in general the waste stream have to be dry), (2) particle
size and shape (i.e., particle surface characteristics and particle size affect the “char-
geability”), (3) presence of additives/fillers (Albrecht et al., 2011) and, finally, (4)
presence of dirtiness on particle surface that can change or inhibit particle surface
charging.
20 Use of Recycled Plastics in Eco-efficient Concrete

Plastics waste
Tribocharger
feed

Negatively charged particles

Positively charged particles

Positive Negative
electrode electrode
(+) (–)

Output products
Figure 2.7 Schematic representation of a triboelectric separation process.

2.4.3 Magnetic density separation


Magnetic density separation (MDS) is a density-based sorting process realized utiliz-
ing a “magnetic fluid” constituted by a liquid (i.e., water) and magnetic particles (i.e.,
iron oxide particles of about 10e20 nm) suspended in the liquid (Bakker et al., 2009).
Through a special magnetic field (Rem et al., 2013) an artificial gravity is produced, as
a magnetic force. Such a force varies exponentially in the vertical direction, and the
effective density of the liquid also varies accordingly in the same direction. The result
is that waste particles (i.e., plastic particles) will float in the liquid at a level where the
effective density is equal to their own density. In other words, particles characterized
by different densities are suspended at different heights (Hu et al., 2013). Adopting this
strategy, it is thus possible to separate plastic particles characterized by very close den-
sity values, such as PP and PE (Serranti et al., 2015) (Fig. 2.8) and PVC and rubber
from construction and demolition waste (Luciani et al., 2015). Particular care has to
be addressed to the correct fulfilling of the following fundamental steps: (1) wetting,
to make the polyolefin surface hydrophilic (Hu et al., 2010), (2) feeding, separating,
and collecting to avoid turbulence in the flow stream, before, during, and after the sep-
aration, negatively affecting particle flow inside the magnetic fluid.
Techniques for separation of plastic wastes 21

Magnet

PP
Plastic waste Splitter
feed
PE
PP Ferro fluid
PE Mixing zone Separation zone Collection zone

Figure 2.8 Schematic representation of a magnetic density separation system for PP and PE.

Such technology is very useful to produce high-quality secondary raw materials,


that is, single polymer stream with a very low presence of impurities.

2.4.4 Flotation
Flotation processes are based on the different surface wettability properties of mate-
rials (Wang et al., 2015). In principle, flotation works very similarly to a sink and float
process, where the density characteristics of the materials, with respect to that of the
medium where they are placed are at the base of the separation. Sometimes a centrif-
ugal field is applied to enhance separation. Flotation works in a different way in the
sense that in a liquid medium, usually water, a “carrier” is introduced, air bubbles,
responsible to float hydrophobic particles that adhere to the bubbles with respect to
the hydrophilic ones that sink. According to surface plastic characteristics, this tech-
nique can be profitably applied, in principle, to separate waste polymers (Fraunholcz,
2004). To enhance or reduce plastic surface characteristics (i.e., hydrophobic or hydro-
philic) appropriate collectors, conditioners (Singh, 1998; Shen et al., 2002), and flota-
tion cell operative conditions (i.e., air flow rate, agitation) can be utilized. Usually
plastic flotation is carried out in alkaline conditions (Takoungsakdakun and
Pongstabodee, 2007). Once floated, hydrophobic polymers are recovered as well as
the sunk ones (i.e., hydrophilic) at the bottom of the cell. This technique, even if it
is well-known (Buchan and Yarar, 1995) and in principle quite powerful is not widely
used mainly for three reasons: (1) it is a wet technique, this means that water has to be
recovered and processed before reutilization, due to the presence of the reagents and
contaminants, (2) polymer surface status (i.e., presence of dirtiness/pollutants and/or
of physical/chemical alteration) can strongly affect floatability, and (3) large variation
of waste plastics feed in terms of composition. Flotation allows to separate PS, PVC,
PET, PC, and mixed polyolefins (MPO).

2.4.5 Sensor-based sorting


Plastic sorting, with respect to other materials, and/or different polymers, is usually
carried out utilizing specific materials’/polymers’ physical properties allowing separa-
tion. Separation often occurs defining handling architectures (i.e., separation
22 Use of Recycled Plastics in Eco-efficient Concrete

equipment) designed and set up in order to enhance how waste particles behave in
respect of the selected property to perform separation. This behavior is usually accom-
plished, as previously stated, through particle trajectory changes at the device output/s
and/or through concentration in different section of the separation equipment. The
mechanical removal of these different streams generates concentrates, wastes and, in
some cases, one or more intermediate compositional product classes, called “mid-
dlings.” Material physical property can be thus considered as the “direct” responsible
of separation.
The adoption of sensors to perform sorting means to follow a different approach,
requiring the utilization and the implementation of online analytical logics and robotic
units to perform the separation. Materials in fact, have to be first detected, then
identified and topologically assessed in the stream; after these steps automated devices
realize the sorting.
Following this approach, it substantially means to take into account two aspects.
The first one is linked to the sensing principle selected to perform materials identifica-
tion and the second one is related to the required actuators logics/architectures utilized
to collect the materials of interest from the investigated waste flow stream. Sensor-
based sorting techniques are thus substantially classified according to these principles
(i.e., sensing and collection). In all cases there are three main components of the
sorting architecture: a conveyor belt for materials feeding, a sensor connected to a
computer analyzing data collected from the waste stream on the conveyor belt, and
a pneumatic system to mechanically separate materials (Fig. 2.9). Sensors do not
require contact with the materials and are nondestructive.

2.4.5.1 Visible spectroscopy


Sorting in the visible range is mainly focused on the utilization of spectroscopic analyt-
ical techniques, performed in the wavelength range 400e700 nm, or on the adoption of
digital imaging. Both the approaches are not particularly efficient in the case of plastic
recycling, being that the detection principle is mainly based on what is detectable
according to investigated individuals’ pictorial attributes, that is, visible spectra,
when spectroscopy analysis is performed, or digital color components (RGB, HSY,
etc.), size, shape, and surface textural attributes when imaging is applied (J€ahne, 1993).

Feed waste Sensor

Air gun

Conveyor belt
Material 1 Material 2

Figure 2.9 Schematic representation of a sensor-based sorting system.


Techniques for separation of plastic wastes 23

Both the approaches are not very efficient to perform polymer sorting; for this reason,
they are not widely utilized except sometimes at the beginning of the process and when
polymers are constituted by large products (i.e., several centimeters) whose color and/
or shape (Zhu and Basir, 2006) can be associated to a known specific polymer-based
manufactured product (i.e., container, pipe, frame, etc.). They can be used also at the
end of a plastic recycling process to sort by color a monomaterial stream of plastics, as
for example, green, blue, and transparent PET.

2.4.5.2 Near infrared spectroscopy


Near infrared spectroscopy (NIR) is probably the most utilized technology in plastic
recycling. It is based on the collection of reflected spectra of polymers properly ener-
gized by a light source (Beigbeder et al., 2013). The investigated wavelength range is
usually 1000e700 nm; in some cases it is extended to the SWIR region
(1000e2500 nm). The NIR sensor sorting system includes: a conveyor belt, illumina-
tion system and optical sensor, a separation unit with compressed air nozzles. Many
different polymers can be separated by near infrared sensors as they are characterized
by different spectral signature in such wavelength range (i.e., PP, PE, PVC, PET, PS,
etc.). Plastics can be also separated from other materials, as paper, wood, glass, stones,
etc. The reasons of the wide use of this technique are mainly related to: (1) NIR does
not require any direct contact with the investigated object, (2) it can be applied defining
very flexible architectures, thanks to the possibility to largely utilize fiber opticse
based architectures both to energize and to collect the spectral response of plastics
(i.e., analysis and identification, in respect of previously set up reference spectral
libraries of the different polymers’ infrared absorption bands), (3) high detection/iden-
tification speed, (4) multiple detection (i.e., multiple check of the same sample), and
(5) no color interference. The size of flakes to be sorted as well as flakes disposal
on the conveyor belt plays an important role, affecting the sensor detection. Sensing
probes, in fact, are characterized by a physical dimension that influences the investi-
gated image field and, as a consequence, the analytical spatial resolution of the single
sensing unit (i.e., usually installed as an array). Black or very dark polymers are almost
impossible to be identified due to their low surface reflectance.

2.4.5.3 Hyperspectral imaging


Hyperspectral imaging (HSI) is an innovative fast, and nondestructive technique able
to collect both spectral and spatial information from an object. The collected informa-
tion generates a data structure defined “hypercube,” that is a dataset containing both
spatial data (i.e., pixel coordinates: x and y axis) and spectral data (i.e., z axis, repre-
senting the spectrum associated to each pixel). The investigated spectral range depends
on the sensor mounted on the device and can vary from VIS to NIR, SWIR, or MWIR
regions, depending on applications. The application of this technique dramatically
grew in these last years in many sectors (i.e., chemical, pharmaceutical, agricultural,
food industry, etc.) and also in recycling: glass recycling (Bonifazi and Serranti,
2006), compost product quality control (Dall’Ara et al., 2012), recycled aggregates
24 Use of Recycled Plastics in Eco-efficient Concrete

from concrete (Serranti and Bonifazi, 2014; Bonifazi et al., 2015, 2018b) and charac-
terization of different plastic waste (Serranti et al., 2012a,b; Hu et al., 2013; Ulrici
et al., 2013).
This large use is intimately linked to some intrinsic characteristics of the HSI
sensing device (Bonifazi and Serranti, 2014) as: (1) the possibility to perform a contin-
uous monitoring of waste large flow streams as disposed on a conveyor belt thanks to
the scan line camera architecture, (2) easy topological definition of the individual to
sort, (3) utilization of different time scaleerelated sampling strategies, in case of
specific product oriented control/quality actions to develop, (4) implementation of
fast and reliable recognition logics, strongly linked to HSI detectors characteristics
(e.g., possibility handle spectra, images, or both spectra and images), (5) total absence
of environmental impacts and/or safety constraints related to the HSI utilized device,
and finally (6) relatively low cost of the device. With reference to polymer recycling,
HSI is particularly powerful (Jansen et al., 2012) allowing to implement online sorting
and/or quality control strategies, thanks to the possibility to identify the spectral
regions, in the NIR/SWIR range (1000e1700 or 1000e2500 nm), where polymer
molecules absorb light by overtone or combination vibrations (Workman and Weyer,
2007). This behavior produces spectral signature characteristics of the polymer thus
allowing its identification (Bonifazi et al., 2018a). In the last years, high-speed spectral
cameras working in the MWIR wavelength range were introduced in the market in
order to sort black polymers that are not classified by sensors working in the
commonly investigated spectral ranges (400e2500 nm) due to the higher light absorp-
tion and the consequent low reflectance (e.g.,: Rozenstein et al., 2017).
HSI-based sorting architectures are usually constituted by a conveyor unit (i.e., belt)
carrying materials to sort (Serranti et al., 2006). A sensing unit inspects and continu-
ously acquires spectra at a fixed rate. Spectra are then processed by a classification
engine previously set up, according to a material spectral reference library, and indi-
vidual/s recognition is performed. An array of compressed air nozzles mounted at
the end of the conveyor belt provides to separate through a shot of air the recognized
individuals (Tatzer et al., 2005; Picon et al., 2010).

2.4.5.4 X-ray fluorescence


Sorting based on X-ray fluorescence (XRF) is based on the detection of the emitted
wavelengths, as well as of the released energy, by a sample previously energized by
X-ray whose atoms release energy generating an X-ray fluorescence radiation. The
elements contained in the sample influence the emission both in terms of wavelengths
and energy. Such a technique is quite powerful and it is largely used in the waste
sector, mainly in wood recycling (Blassino et al., 2002) to evaluate the presence of
potential harmful elements (i.e., arsenic, chromium, copper, etc.).
In the waste plastic sector, this technique is primarily utilized to sort PVC from PET
(Brunner et al., 2015). The use of this technique is expected to increase in the future, as
it can be applied to the separation of brominated plastic from an input stream of
shredded plastics. Bromine is in fact largely used as flame-retardant, especially in elec-
tronic devices. Other XRF-based approaches have been proposed as the Energy
Techniques for separation of plastic wastes 25

Dispersive X-ray Fluorescence (EDXRF) (Bezati et al., 2011) adding tracers to the
polymer matrix.
Sorting architectures are similar in both cases (i.e., XRF and EDXRF). Referring to
EDXRF, the operative unit is constituted by an X-ray beam energizing the waste flow
stream (i.e., particles transported on a conveyor belt) to analyze and sort. X-ray beam is
focused and passed through the material until it reaches the detector. The signal
collected by the detector is processed, the presence of tracers identified, their amount
evaluated, and according to predetermined rules, the corresponding plastic individuals
blow out by air.
XRF does not require any sample preparation/collection; it can identify black and/
or very dark polymers, as well the presence of contaminants on polymers surface and
as individuals. The disadvantages of this technique in plastic sorting is that it is not able
to distinguish between polymers. Furthermore, there are some safety constraints
related to the utilization of X-ray sources.

2.4.5.5 Laser-induced breakdown spectroscopy


Laser-induced breakdown spectroscopy (LIBS) is an analytical technique based on the
utilization of high power laser pulse that performs an ablation of the sample to analyze,
thus producing plasma plumes (Cremers and Radziemski, 2006). The radiation
produced by the ablated portion of the investigated material is then analyzed by a
CCD-based spectrometric device (Gondal et al., 2007). Following this approach
(i.e., identification of the atomic emission lines), it is thus possible to analyze the prop-
erties of waste in terms of constituent materials (Sattler and Yoshida, 1993) and/or, as
in the case of polymers, elements present as carbon and hydrogen and their resulting
line intensity ratio (C/H) (Anzano et al., 2008).
Recently a compact and reliable architecture was proposed to perform the recogni-
tion of polymer particles following a statistical analysis starting from the information
collected by the so-called laser-induced plasma spectroscopy (LIPS) and processed
performing linear and rank correlations, in the wavelength interval: 200e800 nm
(Anzano et al., 2006) or performing, as previously outlined, instant ratio analysis of
molecular bands to identify the different energetic materials (Anzano et al., 2011).
Following this latter approach PVC, PS, PET, PP, LPDE, and HDPE can be identified.
Sorting architecture is constituted by mechanical units that, according to the LIPS
based detection, sort polymers into their respective bins.

2.4.6 Auxiliary separation technologies


Auxiliary separation technologies, referred to as plastic waste recycling, are those
allowing to clean the plastic waste stream from the presence of other materials with
different characteristics and/or nature. They are usually applied at the beginning
(i.e., scalping) or at the end (i.e., refining) of the process. Materials usually removed
through such techniques are: (1) ferrous metals, as low-grade stainless steel, nickel
alloys, etc., (2)nonferrous metals, as aluminum. Magnets (Wills, 2016) and Eddy cur-
rent (Rem, 1999) based separators, respectively, are commonly utilized.
26 Use of Recycled Plastics in Eco-efficient Concrete

2.4.6.1 Magnetic separation


The magnetic separation is commonly applied utilizing belt magnets, magnetic head
pulleys, and drum magnets (Svoboda, 2004). Schematic representations of the
different typologies of magnetic separators are reported in Fig. 2.10. In belt magnets,
the magnet is usually installed above the plastic waste flow stream (Fig. 2.10a).

Belt magnet
Feed waste

(a)

Conveyor belt
Magnetic particles
Non magnetic particles

Feed waste

(b) Magnetic head pulley

Conveyor belt
Magnetic particles
Non magnetic particles

Feed waste

(c)

Conveyor belt
Magnetic particles
Non magnetic particles
Magnetic
drum

Figure 2.10 Different typologies of magnetic separators. (a) Overbelt magnetic separator; (b)
Magnetic head pulley separator; (c) Magnetic drum separator.
Techniques for separation of plastic wastes 27

The overhead magnetic field has a belt moving across its surface at approximately a
90 degree angle to the material flow. Ferrous metal particles are thus attracted,
removed from plastics, and discharged, as the moving belt of the separator turns
away from the magnetic field. Magnetic head pulleys are usually installed at the end
of a conveyor belt, beneath the belt (Fig. 2.10b). Ferrous metal particles are thus
held to the belt, while plastics can be downloaded. Drum magnets are commonly
installed inside feeder chutes, between chutes and conveyors (Fig. 2.10c). Ferrous
metals are held by the drum, until a divider provides to its discharge; on the contrary,
plastic wastes continue their flow. All the previous mentioned devices are normally
positioned at the beginning of the plastics recycling plant having the aim to remove
large magnetic polluting individuals. To perform a strong refining/control of the final
products, high-intensity permanent magnets are usually utilized (Svoboda and Fujita,
2003.).

2.4.6.2 Eddy current separation


Eddy current separation is based on the use of a high speed magnetic rotor system and
is used to remove nonferrous metals (i.e., aluminum and copper) from waste plastic
streams. Due to the high speed of the rotor, an electric current, called Eddy current,
is induced into conducting metals. The induced electric current produces a magnetic
field, opposed by the field created by the rotor, repelling the conducting metals. The
remaining materials such as plastics, glass, and other dry recyclables will simply free-
fall over the rotor, separating them from the repelled metals (Fig. 2.11). Eddy current
separators are usually located in the preliminary stages of the process. Such a choice is
mainly due to the fact that Eddy current separation process is highly dependent on the
size of the feed particles according to its separation principle. The magnitude of the
repulsive forces depends on the specific conductivity, mass, morphological and mor-
phometrical characteristics of the particles, and on the intensity and distribution of the
magnetic field (Van der Walk et al., 1986).

Feed waste

Magnetic
high-speed rotor

Conveyor belt
Non metal particles
Non ferrous metal particles
Figure 2.11 Schematic representation of an eddy current separator.
28 Use of Recycled Plastics in Eco-efficient Concrete

2.5 Recycled plastics quality control


The quality certification of recycled plastic products is fundamental to increase their
economic value and to foster their penetration in the market. Product quality assess-
ment is an important aspect in all industrial manufacturing sectors, but this is particu-
larly true for the recycled materials whose market is still hindered by many barriers.
Recycled polymeric materials are expected to have the same high quality and
performance characteristics of those of the corresponding virgin polymers; however,
the achievement of high quality levels requested by the end users through the mechan-
ical recycling process is not an easy task. Furthermore, many plastic brand owners and
manufacturers distrust recycled plastics and fear that they cannot assure their need of
high volumes of reliable material with clearly defined constant quality specifications.
As a consequence, there is a low demand for recycled plastic, especially in high value
products, and its use is often limited to low-value or niche applications (COM, 2018).
It is evident that there is a strong need not only to ensure and to improve quality of
plastic recycled products through technological innovation in the recycling process,
but also to develop and define specific quality standards for recycled plastic products.
The quality requirements must be related to the different applications of plastic prod-
ucts such as food contact or durable goods like electronics and automobiles.
Recycled plastics can vary from virgin resins in a number of ways, including
contamination originated from multiple sources (e.g., impurities, the use-phase,
misuse, degradation, improper separation of materials, legacy substances, or cross-
contamination during waste collection). Such incidental contaminants can affect the
quality and safety of recyclates and therefore fast, cost-effective quality control strate-
gies should be developed and implemented at plastic recyclers’ premises, in order to
produce a certified output that meet customer specifications (Vilaplana and Karlsson,
2008).

2.5.1 Recycled plastics quality measurements


The quality assessment of recycled plastic products should be based not only on the
same testing equipment commonly utilized for virgin resins, but also on specific char-
acterization measurements related to the possible contamination and degradation of a
plastic recycled material.
Traditionally the basic measurements to evaluate plastic product quality and perfor-
mance in different applications are rheological and mechanical properties (e.g., melt
flow rate, tensile and impact strength, etc.). For recycled plastics it is important to
assess also other important properties that can affect quality, such as the degree of
mixing, in terms of presence of polymeric impurities in a single polymer stream, the
level of degradation (chemical and structural/textural alteration), and the presence of
low-molecular weight compounds such as contaminants, additives, etc. (Karlsson,
2004; Vilaplana et al., 2007).
One of the main challenges related to the production of plastic recycled materials
lies in the fact that different polymers are incompatible and immiscible at molecular
level; even low levels of contaminations will affect the quality of the target stream,
Techniques for separation of plastic wastes 29

for example, the presence of small amounts of PVC in a PET stream will make it brittle
and yellowish when recycled (Hahladakis and Iacovidou, 2018). It follows that plastic
must be recycled as much as possible in single polymer streams. For a plastic producer,
stability in composition of the plastic raw material fed to the plant is very important,
since even small variations in melting point or other properties can affect the produc-
tion, in terms of functionality, strength, or durability of products that is not acceptable
for some high-tech applications such as medical devices or automobile components.
This means that a constant and stable composition of a recycled plastic stream must
be assured.
The methods commonly utilized to check the quality of a single polymer recycled
stream in terms of presence of other polymers are applied at laboratory scale, which
means time-consuming operations, involving the presence of a trained operator, a
sample collection, and preparation step. Examples of commonly adopted techniques
at laboratory scale are DSC (Differential Scanning Calorimetry) and FT-IR (Fourier-
Transform Infrared Spectroscopy). An alternative solution to check the quality of the
recycled plastic products is the use of hyperspectral imaging that can be applied
online directly on the conveyor belt without any sample preparation (Serranti
et al., 2011; Luciani et al., 2015) (Fig. 2.12). Polymer mixing evaluation can be
achieved through the definition of classification models, allowing the identification
of different plastics at the same time. HSI in the NIR/SWIR wavelengths ranges
(1000e1700/2500 nm) coupled with chemometrics were successfully applied to
set up fast and reliable quality control strategies at recycling plant scale (i.e., better
and more strict control of sorting and separation process stages) with reference to
many different polymers, including PP, HDPE, LDPE, PET, PVC, etc. (Bonifazi
et al., 2018a).

Spectral-imaging
instrumentation Monitor

Illuminant Moving
belt

Console

PC

Figure 2.12 HSI platform working in the NIR range (1000e1700 nm) developed for quality
control of different recycled polymers.
30 Use of Recycled Plastics in Eco-efficient Concrete

The possible presence of harmful substances can also limit the use of recycled
plastic as secondary raw materials, especially in applications related to food pack-
aging, due to possible dangerous contamination. X-ray fluorescence can be used to
check the presence of hazardous materials and elements, such as brominated flame
retardants and chlorine-containing materials, both of which can only be detected at
the elemental level through X-ray analysis. Other analytical techniques can be
used to determine the presence of additives in plastics, such as inductively coupled
plasma optical emission spectrometry (ICP-OES) or LIBS (Vilaplana and Karlsson,
2008).

2.6 Technical challenges in plastic recycling


In the following sections, some of the main current hot research topics on plastic recy-
cling are introduced.

2.6.1 PP-PE separation


Polypropylene and polyethylene, belonging to the family of polyolefins, are the most
produced plastics at global level. A mixture of PP-PE is commonly an output of a recy-
cling plant treating plastics, especially when dealing with household waste due to their
wide use in packaging. However, in order to produce high-quality secondary polyole-
fins that means single polymer streams, a purity of at least 97% must be reached
(Bakker et al., 2009). MDS, as already mentioned in Section 2.4.3, was proposed as
a powerful technology to separate PP and PE (Fig. 2.8). Its innovation is based on
the use of a medium characterized by a gradient of density, allowing to separate not
only materials with very low differences in density, as PP and PE, but also more
than two materials in one single step (Serranti et al., 2015).

2.6.2 LDPE-HDPE separation


LDPE and HDPE are both semicrystalline polymers but the degree of crystallinity is
higher for HDPE and lower for LDPE, due to the different number of polymer
branches (da Silva and Wiebeck, 2017). Their mechanical separation is not an easy
task, due to their very similar physical characteristics, and especially their density
(i.e., LDPE: 0.926e0.939 g/cm3 and HDPE: 0.940e0.965 g/cm3).
The possibility to correctly identify these two polymers by fast and reliable
methods working online is still a challenge and represents an important goal to reach.
In a recent study, an innovative strategy based on SWIR-HSI was explored allowing
LDPE, HDPE, and other polymers to be recognized in one shot in a plastic waste
flow stream (Serranti et al., 2018) (Fig. 2.13). The study was carried out at
laboratory-scale, but it is very promising and it could be applied in the near future
also at plant-scale, thanks to the fast growing of HSI technologies and corresponding
computing power.
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From somewhere close by there came gently wafted the delicious
penetrating fragrance of lilies. Was it a wonder that Gilles' thoughts should
at once have flown to Jacqueline? and that an uncontrollable ache should
suddenly grip his heart?

Throughout his long adventurous life he had seen so many women—had


kissed a few, and loved none; and now Fate had placed in his path just the
one woman in the whole wide world whom at first sight he had loved with
unbounded passion, and who was as far removed from him as was the gold-
crowned steeple of St. Géry far away, and infinitely more unattainable. For
the first time in his life Gilles had looked into a woman's eyes, felt that they
held in their depths a promise of paradise, only to realize that that promise
could never be made to him.

The scent of the lilies brought with it a murmur of spring, of awakening


nature, of twitter of birds, and the man who listened to that murmur, who
thrilled at its insistent call, knew that he must for ever remain lonely, that
the call of springtide for him must for ever remain unsatisfied.

Standing there alone, he was not ashamed of his emotion, not ashamed
that hot tears welled up involuntarily to his eyes. But with a half-impatient
gesture and a smile at his own folly, he brushed these with his hand
resolutely away.

When the mist of tears was cleared from his eyes, he suddenly saw her—
his dream—standing before him. She was in the window embrasure, with
the flood of sunshine wrapping her like a mantle of gold. On the window
sill beside her lay a bunch of white lilies. Her little hand—Gilles thought he
had never seen such an exquisite little hand—held back the curtain, behind
which she had apparently been sitting. A soft breeze blew in through the
half-open window and stirred with its delicate breath the soft tendrils of her
ardent hair. Her face against the light was in a tender, grey shadow, through
which her eyes shone like a peep of azure sky, and on her cheek that tiny
mole was provocatively asking for a kiss.

The apparition had come upon Gilles so suddenly, the transition from
dark melancholy to joy was so abrupt, that he—poor man!—weak, sick,
unnerved by weariness and constant strain, not only found nothing to say,
but he clean forgot all the amenities of social life which the equerry of a
prince of the House of Valois should have had at his finger-tips.

Jacqueline, too, strangely enough, felt embarrassed for the moment,


angry with herself for being tongue-tied. What was there to be confused
about? Messire Gilles de Crohin could not possibly guess that she had been
sitting here in the window embrasure, waiting to see him pass, just because
she desired to have news of his master. He could not guess that it had taken
all her reserves of diplomacy to so explain to Monseigneur when he
questioned her, what she knew of the events of the past night that, without
being greatly angered against M. de Landas, he should feel sufficient
compunction to send promptly for news of Messire le Prince de Froidmont.
Certainly Messire's equerry could not guess that Madame Jacqueline's heart
had been touched and her mind tickled when Monseigneur placed before
her the naïve effusion of Maître Jehan, and that her own common sense and
unerring feeling for justice had filled in the gaps which the worthy servant's
missive had left in his exposé of what had actually occurred.

Therefore it was not the fear of what Messire de Crohin might think or
guess that kept Jacqueline momentarily speechless and shy, rather was it a
curious and undefinable sense of something strange—familiar yet
mysterious—about the personality of this man who stood, equally silent,
before her. It took her several seconds to free herself from this spell which
appeared to have been cast over her, several seconds of fighting angrily
with herself for the constraint which rendered her tongue-tied and shy.
Fortunately he appeared quite unaware of her embarrassment, waited
somewhat awkwardly, she thought, for her to speak.

'You are Messire de Crohin?' she contrived to say at last.

'At your service, Madame,' he replied.

'Equerry to Monseigneur le Prince de Froidmont?'

He bowed in affirmative response.

'And ... I have no doubt ... devoted to his person?'


He smiled.

'Why should Madame conclude that?' he asked.

She gave a little start. Somehow his tone—that bantering smile, had
accentuated that feeling of familiarity which rendered his person so
strangely mysterious.

'Monseigneur le Prince de Froidmont,' she rejoined coldly, 'is sure to


command the devotion of those who serve him. He is brave and chivalrous
——'

'That was not Madame's opinion of him last night——' he broke in dryly.
Then, seeing that his tone had caused her to turn her eyes on him with
unfeigned surprise he added somewhat lamely: 'At least ... that is ... that is
what Monseigneur gave me to understand last night——'

'It was all a misunderstanding,' she said gently. 'Will you say that to
Monseigneur?'

'If Madame desires.'

'I do desire it. And since you know all about the incident, Messire, will
you, I pray you, tell your master how deeply I regret the erroneous
judgment which I formed of his conduct? Those abominable varlets all
crowding round him——'

'Appearances were against Monseigneur, no doubt.'

'And I behaved like a vixen, Messire,' she said with a smile.

'Then give me an army of vixens!' he retorted impulsively.

'Why, Messire, you were not there to see——'

'No! But I imagine now that vixens must be adorable.'

'Do not jest, Messire,' she rejoined more earnestly. 'I was shrewish last
night and ill-tempered and unjust. Will you tell your master that this
morning——'

'I will tell him, Madame, that this morning you are perfect, whatever you
may have been last night.'

Poor Gilles by now would have given all that he possessed in the world
to be allowed to go. He felt that this interview, which he had neither sought
nor hoped for, was like a dangerous trap into which Fate and his own
temperament might hurl him headlong. Every minute that he spent in this
woman's company rendered her more desirable to him, rendered him more
completely a slave to her charm. But for some strange and subtle reason she
seemed disinclined to let him go just yet, and even now when, remembering
his best manners, Gilles started on the preliminaries of a most elaborate
farewell bow, she went on with a quick catching of her breath and a slight
hesitation, which brought a soft glow to her cheeks:

'Messire Gilles——'

'At your service, Madame.'

'Was Monseigneur de Froidmont very angered with me?'

'He was,' Gilles admitted, 'last night.'

"But ... but....'

'His anger hath since melted like snow in the spring.'

'Even before you came hither at the bidding of my guardian?'

'Even before that, Madame.'

'Did he tell you so?'

'I guessed it.'

'Do you know his innermost thoughts, then?'

'Most of them—yes, Madame.'


'You are very intimate with Monseigneur le Prince de Froidmont?' she
asked, with a certain shy hesitancy which Gilles found adorable, because it
caused a delicate flush of pink to suffuse her cheeks. This caused him, in his
turn, to be confused and tongue-tied, staring at her with eyes that seemed as
if they would devour her loveliness.

She had to repeat her question.

'Oh!—ah!—er!' he stammered vaguely. 'That is—yes! Yes, Madame! I


am on ultimate terms with Monseigneur.'

'And—do tell me, Messire—is Monseigneur handsome?'

'No, by the Lord!' exclaimed Gilles with a loud laugh. Then he caught
her look: it was not one of surprise, rather of amusement not unmixed with
quaint, roguish mischief. He could not interpret that look rightly, and began
to stammer, worse confused than before.

'Madame—I—that is——'

'You are no judge of your master's looks, shall we say?' she retorted with
an enigmatic little smile. 'But you must remember that, though I found
Monseigneur of noble bearing, I have no notion how he looks, for I have
never seen him without a mask—that is——'

This time Gilles was quite sure that she was doing her best to suppress a
laugh.

'Do you think,' she said, 'that you could persuade His Magnificence to
pay his respects to me unmasked?'

'Monseigneur will, I feel sure,' he rejoined stiffly, 'be honoured by the


command, but——'

'But what, Messire?'

'He is strangely ill-favoured, Madame.'


'Oh! a woman is the best judge of that. Some of the ugliest men have
proved most attractive.'

'But—but Monseigneur is scarred—badly scarred. He——'

'What matter? There is naught so glorious as scars on a soldier's face.


When I was a child I once saw the Duc de Guise—le Balafré! With that
great cut across his cheek, he was still the most notable man in a room filled
to overflowing with clever, brave and handsome men!'

'But—but, Madame, Monseigneur is also pock-marked. Yes, that's it!


Pock-marked! An illness contracted in early childhood—Madame
understands?'

'I do,' she replied with a little sigh of sympathy, and looked with those
enchanting blue eyes of hers straight on poor Gilles. 'I do. It is very sad.'

'Very sad indeed, Madame.'

'Scarred and pock-marked. No wonder Monseigneur is shy to show his


face. But no matter,' she continued gaily. 'He hath such a lovely voice, and
oh! such beautiful hands! Slender and full of nerve and power! I always
take note of hands, Messire,' she said with well-feigned ingenuousness.
'They indicate a man's character almost more than his face. Do you not
think, so too?'

'I—Madame—that is——'

Gilles had, quite instinctively, drawn the lace of his sleeve over his left
hand, even while Madame still looked at him with that tantalizing glance
which had the effect of turning his brain to putty and his knees to pulp. Now
she laughed—that merry, rippling laugh of hers—and I do verily assure you
that the poor man was on the verge of making a complete fool of himself.
Indeed, it were difficult to say whether or no the next second would have
witnessed his complete surrender to Jacqueline's magic charm, his total loss
of self-control and the complete downfall of Madame la Reyne de Navarre's
cherished plan, for poor Gilles had lost consciousness of every other feeling
and thought save that of a wild longing to fall on his knees and to kiss the
tiny foot which peeped beneath the hem of that exquisite woman's gown, a
wild longing, too, to hold out his arms and to fold her to his breast, to kiss
her hair, her eyes, her lips, that tiny mole which had wrought the whole
mischief with his soul. For the moment he forgot his past life, his present
position, the Duc d'Anjou and Madame la Reyne: he had forgotten that he
was a penniless adventurer, paid to play an unworthy trick upon this
innocent girl, sworn to infamy on pain of greater infamy still! He had
forgotten everything save that she was adorable and that an altogether new
and ardent love had taken possession of his soul.

Of a truth it is impossible for a prosy chronicler to state definitely what


might have happened then, if Monseigneur the governor had not chosen that
very moment for coming out of his room and walking down the corridor, at
one end of which Gilles was standing spell-bound before the living
presentment of his dream of long ago. He heard Monseigneur's heavy
footstep, pulled himself vigorously together, and with an impatient gesture
which was habitual to him, he passed his left hand slowly across his
forehead.

When he looked on Jacqueline again she was staring at him with an


expression that appeared almost scared and wholly bewildered, and with a
strange, puzzled frown upon her smooth forehead. For the space of a second
or two it seemed as if she wanted to say something, then held back the
words. After a slight hesitation, however, she finally went forward a step or
two to meet her guardian, without looking again on Gilles.

'I was glad,' she said quietly to d'Inchy, 'to have had an opportunity of
seeing Messire de Crohin and of begging him to offer to Monseigneur le
Prince de Froidmont, his master, my sincere regrets for what occurred last
night.'

'Messire has already assured me,' rejoined d'Inchy suavely, 'that


Monseigneur harbours no resentment against any of us. Is that not so,
Messire?'

'Indeed it is, Monseigneur,' replied Gilles stiffly. 'Whatever Monseigneur


may have felt last night, I in his name do assure you that at this hour the
incident of last night hath faded from his memory.'
He bowed now, ready to take his leave. But Jacqueline was apparently
not yet ready to dismiss him. Something had gravely puzzled her, that was
clear; and it was that something which seemingly made her loth to let him
go.

'What, think you, Messire,' she said abruptly, 'caused Monseigneur to


forget his resentment so quickly?'

'A journey, Madame,' he replied, looking her boldly between the eyes
this time, 'which his thoughts took skywards, astride upon a sunbeam.'

She smiled.

'And did Monseigneur's thoughts wander far on that perilous journey?'

'As far as the unknown, Madame.'

'The unknown? Where is that?'

'There where we sow our dreams.'

'Where we sow our dreams? You speak in metaphors, Messire. If, as you
say, we sow our dreams, what do we reap?'

'A perfect being such as you, Madame, can only reap joy and happiness.'

'But you, Messire?'

'Oh, I, Madame!' he replied with a shrug of his broad shoulders. 'What


can a poor soldier of fortune garner from a crop of dreams save a bunch of
memories?'

'Happy memories, I trust,' she said gently, as she finally extended her
dainty hand for his kiss.

'Happiness is such an ephemeral flower, Madame: memory is its lasting


perfume.'
For one brief moment her exquisite little hand, white, soft and tensely
alive, like the petals of a fragrant lily, lay upon his own: for one brief
moment of unalloyed happiness his lips rested upon her finger-tips, and he
felt them quivering beneath his kiss, as if something of the passion which
was searing his heart had been communicated to her through that kiss.

The moment went by like a flash: the next, Monsieur le Baron d'Inchy
was already bidding him farewell with many an unctuous word, which
Gilles never even heard. He had eyes and ears only for Jacqueline—
Jacqueline, whom he had seen and loved at first sight, when she had been
alternately proud and dignified, demure and arch, reproachful and
contemptuous; but before whom he could now bend the knee in adoration
when a softened mood filled her eyes with tears and caused her perfect lips
to quiver with unexpressed sympathy.

'I entreat you, Messire,' she said finally, 'when you return to your master,
to urge upon him the necessity of extreme prudence. Strangers are none too
welcome in Cambray these days, and Monseigneur de Froidmont hath
already made many enemies, some of whom are unscrupulous, others
merely hot-headed; but all, alas! dangerous. Guard him with your life,
Messire,' she urged, with a quaint little catch in her throat. 'And, above all, I
pray you to assure him that Jacqueline de Broyart would give much to undo
the miserable work of the past night.'

She bowed her head in token that he was dismissed at last, and he—poor
wretch!—could not at that moment have uttered a single word in response,
for his throat was choked and his very sinews ached with the effort to
appear calm and unconcerned before Monseigneur the governor.

So, I fear me, that Gilles de Crohin defied every social rule laid down by
the aforesaid Maître Calviac, and that Monseigneur the governor was
seriously shocked when he saw a mere equerry taking an unduly hasty leave
from himself and from Madame Jacqueline de Broyart, who was Duchesse
et Princesse de Ramèse, in rank far above any Sire de Crohin.

Monseigneur d'Inchy gave a quick sigh of impatience. The comedy


invented by the Queen of Navarre was beginning to tax his powers of
endurance heavily. Were it not for the great issues at stake, he would never
have humbled himself before any man as he had done before a profligate
Valois prince who was not worthy to lick the dust that stained Madame
Jacqueline's velvet shoes. He looked down with conscious pride on his
beautiful ward, more beautiful at this moment, he thought, than she had
ever looked before. She was gazing straight down the length of the corridor;
her lips were parted in an enigmatic smile which greatly puzzled her old
guardian, a soft blush mantled over her cheeks and throat, and as she gazed
—on nothing seemingly—her blue eyes shone with a strange, inward
excitement.

And yet, all that there was to see down the corridor was the retreating
figure of that somewhat ill-mannered equerry, Messire Gilles de Crohin.

CHAPTER XIV

WHICH TREATS OF THE DISCOMFITURE OF M.


DE LANDAS

We may take it that M. le Baron d'Inchy, at whose invitation the Duc


d'Anjou had come to Cambray, was not likely to let the matter of the
midnight duel remain unpunished, the moment he learned the full facts
about the affair. The epistle of Maître Jehan had put him on the scent, and it
must be remembered that M. le Baron d'Inchy ruled over Cambray and the
Cambrésis with the full autocratic power of a conqueror, and that he had
therefore more than one means at his disposal for forcing the truth from
unwilling witnesses if he had a mind.
That truth, as confessed by the night watchmen, was nothing short of
appalling. Monseigneur the governor's first thought had been one of ample
—not to say, obsequious—apologies to His Highness for the outrage against
his person. But Monsieur being sick, and etiquette forbidding Monseigneur
the governor's visit to so humble an hostelry as that of 'Les Trois Rois,' M.
d'Inchy had bethought himself of Messire Gilles de Crohin, the equerry, had
sent for him and begged him to transmit to His Highness all those excuses
which he—the governor—would have wished to offer in person.
Fortunately, the equerry had been able to assure Monseigneur that His
Highness appeared inclined to look on the affair with leniency. Whereupon
d'Inchy had seen him depart again, feeling still very wrathful but decidedly
easier in his mind.

Then he sent for de Landas.

De Landas was sick of his wounds, feverish and in the leech's hands; but
the order to present himself before the governor was so peremptory that he
dared not refuse. He knew well that nothing but unbridled anger would
cause Monseigneur to issue such an arbitrary order and that it would neither
be wise nor even safe to run counter to his will.

So de Landas had his wounds re-dressed and bandaged; he took the


cooling draught which the leech had prepared for him, and then he ordered
four of his men to carry him on a stretcher to the Archiepiscopal Palace. But
all this show of sickness did not have the effect of softening Monseigneur's
mood. He ordered de Landas very curtly to dismiss his stretcher-bearers,
then he motioned him to a seat, himself sat down behind his desk and fixed
searching eyes upon his young kinsman.

'I have sent for you, José,' he began sternly, 'and for you alone, rather
than for the whole of your gang, because you have constituted yourself their
leader, and they invariably follow you like so many numskulls, in any
mischief which you might devise.'

'Mon cousin——' stammered de Landas, abashed, despite himself, by


d'Inchy's dictatorial tone.
'One moment,' broke in the latter harshly. 'Let me tell you at once that
explanations and prevarications are useless. I received a hint of what
occurred last night primarily from an outside source, but you will
understand that a clue once obtained can very easily be followed up. We
questioned your varlets, put the night watchmen to the torture; they
confessed everything, and you, M. le Marquis de Landas, my kinsman, and
half a dozen of your precious friends, stand convicted of an attempt at
assassination against the person of a stranger, who happens to be my guest.'

De Landas, feeling himself cornered, made no attempt to deny. It


certainly would have been useless. Unfortunately he had allowed his
jealousy to get the better of his prudence, and last night had made more than
one mistake—such, for instance, as not killing the watchmen outright
instead of merely overpowering them, and employing his own men rather
than a few paid spadassins, who could not afterwards have been traced. So
he sat on, sullen and silent, his arm resting on that of the chair, his chin
buried in his hand.

'For that attempted crime,' resumed Monsieur le Baron d'Inchy, after a


slight pause, and speaking in a trenchant and staccato tone, 'I have decided
to expel you and your five friends out of the city.'

De Landas, forgetting his wounds and his sickness, jumped to his feet as
if he had been cut with a lash.

'Expel me——?' he stammered. He could scarcely frame the words. He


was grey to the lips and had to steady himself against the table or he would
have measured his length on the floor.

'You and your friends,' reiterated d'Inchy with uncompromising severity.


'Would you perchance prefer the block?'

But already de Landas had recovered some of his assurance.

'This is monstrous!' he exclaimed hotly. 'I, your kinsman! Herlaer,


Maarege—some of your most devoted friends...!'
'No one is a friend,' retorted d'Inchy firmly, 'who is a law-breaker and a
potential assassin!'

'Monseigneur!' protested de Landas.

'Well! What else were you all last night?'

'We had no intention of killing the rogue.'

'And attacked him, six to one!'

'His impudence deserved chastisement. We only desired to administer a


lesson.'

'In what form, I pray you?' queried d'Inchy with a short ironical laugh.

'We had some sticks in reserve——"

'Sticks!' thundered d'Inchy, who at the words had jumped to his feet and
in his wrath brought down his clenched fist with a crash upon the table.
'Sticks!! You had thought ... you would dare ... to raise your hands against ...
against ... Oh, my God!' he exclaimed in horror as he sank down once more
into his chair and, resting his elbows on the table, he buried his face in his
hands. Evidently he was quite unnerved.

De Landas had remained silent. Of a truth he had been struck dumb by


this extraordinary show of what amounted almost to horror on the part of
his usually dignified and self-contained kinsman. It seemed as if he—de
Landas—had said something awful, something stupendous when he spoke
of administering chastisement to a vagabond. A vagabond indeed! What
else was this so-called Prince de Froidmont? Whence did he come? What
was his purpose in coming to Cambray? And why should Monseigneur the
governor be so completely unnerved at the bare possibility of any one
laying hands on so obscure a personage?

But this was obviously not the moment for demanding an explanation.
De Landas, ere he left his own fatherland in order to seek fortune in
Flanders, had already been well schooled in those arts of diplomacy and
procrastination for which Spanish statesmen were famous. He scented a
mystery here, which he then and there vowed to himself that he would
fathom; but this was not the time to betray his own suspicions. He knew
well enough that these wooden-headed Flemings were for ever hatching
plots for the overthrow of their Spanish conquerors, that His Majesty the
King of Spain had hardly one faithful or loyal subject among these boors,
who were for ever prating of their independence and of their civil and
religious liberties. De Landas' quick, incisive mind had already jumped to
the conclusion that, in this mystery which surrounded the personality of this
enigmatic Prince de Froidmont, there was no doubt the beginnings of one of
those subtle intrigues, which had already filched from the kingdom of Spain
more than one of her fair Flemish provinces. But the young man had up to
now been too indolent and too self-indulgent to trouble himself much about
the dangers which threatened his country through the brewing of these
intrigues. He was of a truth ready to find fortune in Flanders and to marry
the richest heiress in the land if he could, and then to remain loyal to the
country of his adoption if it continued to suit his purpose so to do; but if, as
he began now vaguely to fear, his plans with regard to Jacqueline were
thwarted for the sake of some unknown suitor, however highly placed, if the
golden apple which he had hoped to gather in this mist-laden land turned to
dead-sea fruit in his hand, then he would no longer consider himself bound
by allegiance to this alien country; rather would his loyalty to King Philip
of Spain demand that he should combat every machination which these
abominable Flemings might set afoot, for the overthrow of Spanish power.

But all this was for the future. De Landas was astute enough not to
betray a single one of his thoughts at the moment—not until he had
surveyed the whole situation in cold blood and discussed it with his friends.
For the nonce, conciliation was the only possible—the only prudent—
course of action, and humility and resignation the only paths thereto.

So he waited a minute or two until d'Inchy had mastered his


extraordinary emotion. Then he said meekly:

'Monseigneur, you see me utterly confounded by your anger. On my


honour, I and my friends sinned entirely in ignorance. We thought the
stranger presumptuous in the presence of Madame Jacqueline de Broyart,
who in our sight is almost a divinity. We desired to teach a malapert a
lesson for daring to approach the greatest lady in Flanders otherwise than
on bended knees. We had no thought,' he added insidiously, 'that in so doing
we might be attacking a personage whom Monseigneur desires to hold in
especial honour.'

'Even if the stranger was a person of no consequence,' rejoined d'Inchy


more calmly, 'your conduct was outrageous——'

'As it is, I am humbled in the dust at thought that it put a spoke in the
wheel of some deep-laid political plans.'

'I did not say that——' broke in d'Inchy quickly.

'Oh, Monseigneur!' protested de Landas gently, 'you deign to belittle


mine intelligence. I may be a young jackanapes, but I am not such a crass
fool as not to realize that the person whom I only thought to chastise, as I
might some insignificant groundling, must be a gentleman of more than
ordinary consequence, else you would not punish me so severely for so
venial an offence.'

'It is my duty——'

'To expel six noble gentlemen from their homes for laying hands on an
unknown adventurer? Fie, Monseigneur! Your estimate of my reasoning
powers must of a truth be a very low one.'

'You have gravely erred against the laws of hospitality.'

'I am prepared to lick the dust in my abasement.'

'You have offended a stranger who was my guest.'

'I will offer him my abject excuses, tell him that I mistook him for a
caitiff.'

'He would not accept your excuses.'

'Is he such a high and mighty prince as all that?' retorted de Landas.
It was an arrow shot into the air, but it evidently hit the mark, for d'Inchy
had winced at the taunt.

'M. le Prince de Froidmont has been too gravely affronted,' he said


stiffly, 'for excuses to be of any avail.'

'Let me try them, at any rate,' riposted de Landas, almost servilely now.

'I don't know—I——'

'Ah! but Monseigneur, I entreat you, listen. I am your friend, your


kinsman, have served this land faithfully, devotedly, for years! I have no
wish to pry into your secrets, to learn anything of which you desire to keep
me in ignorance. But think—think!! Others would not be so scrupulous as I.
Gossip flies about very quickly in this city, and rumours would soon take
wider flight, if it became known that you had punished with such
unyielding rigour six of your best friends, one of them your own kinsman,
for daring to quarrel with a masked stranger whom nobody knows, and who
has entered this city in the strictest incognito. People will deduce unpleasant
conclusions: some will call the stranger a Spanish spy, and you,
Monseigneur, a paid agent of Spain. At best, rumour will be busy with
speculations and conjectures which will jeopardize all your plans. In
pleading for mercy, Monseigneur,' urged de Landas with well-feigned
ingenuous enthusiasm, ''tis not so much mine own cause that I advocate, but
rather that of your own peace of mind and the fulfilment of all your secret
desires.'

D'Inchy made no immediate reply. No doubt the Spaniard's specious


arguments had struck him as sound. He knew well enough how difficult it
was, these days, to keep tongues from wagging, and until the affair with
Monsieur Duc d'Anjou, was irrevocably concluded, gossip would prove a
deadly danger, not only to the plans which he and de Lalain had laid so
carefully, but also to themselves and to their adherents. This knowledge
caused him to weaken in his attitude toward de Landas. He sat there,
frowning, silent, obviously hesitating already.

We must always remember also that the Flemings—whether lords or


churls—had never been able to hold their own against Spanish diplomacy
and Spanish cunning. Their mind was too straightforward, too simple, yes!
too childish, to understand the tortuous subtleties practised by these past
masters of mental craftiness.

D'Inchy, de Lalain, de Montigny and their friends had plunged up to the


neck in a sea of intrigue. They were already floundering, out of their depth.
D'Inchy, ingenuous and inherently truthful, had never suspected de Landas
of duplicity—had, of a truth, never had cause to suspect him—therefore
now he took the young Spaniard's protestations, his meekness, his well-
timed warning, entirely at their face value. De Landas was looking him
straight in the face while he spoke, and d'Inchy was duly impressed by the
air of straightforwardness, of youthful enthusiasm, wherewith the young
man punctuated his impassioned tirade; and the latter, quick to note every
change in the Fleming's stern features, pursued his advantage, pressed home
his pleadings, half certain already of success.

'Let me go forthwith, Monseigneur,' he begged, 'to offer my humble


apologies to—to—Monsieur—er—le Prince de Froidmont. Though you
may think that we tried to murder him last night, we crossed swords with
him like loyal gentlemen. I and my friends will meekly admit our errors. He
is too chivalrous, believe me, not to forgive.'

Obviously d'Inchy was yielding. Perhaps he had never been very


determined on punishing those young coxcombs, had been chiefly angered
because he feared that in his wrath Monsieur Duc d'Anjou, might
incontinently shake the dust of inhospitable Cambray from off his velvet
shoes. Above all things, d'Inchy dreaded gossip about the affair, and de
Landas had indeed proved himself a master in the art of self-defence when
he prophesied the birth of countless rumours if wholesale expulsions and
punishments followed the midnight brawl.

'Have I your permission to go, Monseigneur?' insisted de Landas. 'Sick


as I am, I can yet crawl as far as the hostelry where lodges the enigmatic
Prince de Froidmont.'

Again d'Inchy winced. He felt his secret escaping from the safe haven of
his own keeping. He sat on in silence, meditating for awhile. After all,
Monsieur's equerry had assured him that His Highness was disposed to look
leniently on the episode, and who could be more royalist then the King?
more Catholic than the Pope? Gradually the tensity of his attitude relaxed,
the dark frown disappeared from between his brows; he still looked sternly
on his young kinsman, but the latter saw that the look was no longer
menacing.

A few minutes later Monseigneur d'Inchy had spoken the word which
caused de Landas to give a deep sigh of relief.

'Very well!' he said. 'You may try. But understand,' he added inflexibly.
'If Monsieur—I mean, if M. le Prince de Froidmont does not accept your
apology, if he demands your punishment, you leave Cambray to-night.'

'I understand, Monseigneur,' said de Landas simply.

'And if the Prince does accept your apology, and I do condone your
offence this time, your punishment will be all the more severe if you
transgress again. It would not be a sentence of expulsion then, but one of
death. Now you may go!' he concluded curtly. 'My leniency in the future
will depend upon your conduct.'

After which, he dismissed de Landas with a stiff inclination of the head,


and the young Spaniard left the presence of the autocratic governor of
Cambray with rage in his heart and a veritable whirlpool of conjectures, of
surmises and of intrigues seething in his fertile brain.

II

But right through the wild medley of hypotheses which ran riot in de
Landas' mind there raged also furious, unbridled wrath—wrath at his own
humiliation, his own impotence—hatred against the man who had brought
him to this pass, and mad, ungovernable jealousy whenever his thoughts
turned to Jacqueline.

Somehow—it was only instinct, no doubt—he felt that all this pother
about the masked stranger centred round the personality of Jacqueline. The
first hint which Monseigneur had of last night's affray must of necessity
have come from Jacqueline. She alone was there—varlets and wenches did
not count—she alone could have a personal interest in putting Monseigneur
on the scent.

A personal interest? De Landas' frown became dark and savage when


first that possibility rose before his mind. He had ordered his servants, very
curtly, to go and wait for him in the main entrance hall, for after his
interview with the governor he felt the want of being alone for a few
moments, to think over the situation as it so gravely affected him. He was in
the same corridor where a couple of hours ago Jacqueline had waylaid and
spoken with Messire Gilles de Crohin. On his right was the row of tall
windows with their deep embrasures, which gave view upon the park. De
Landas felt sick and fatigued, as much from choler and nerve-strain as from
the effect of his wounds, and he sat down on one of the wide window-seats
to think matters over.

A personal interest?

Yes! That was it. Jacqueline, capricious, hot-headed, impulsive, had been
attracted by the mysterious personality of the stranger, and for the moment
was forgetting the lover of her youth, the man who felt that he had an
inalienable claim upon her allegiance. De Landas had heard rumours of a
masked minstrel having serenaded Madame beneath her windows. Pierre,
his own henchman, had received a broad hint to that effect from Nicolle,
who was Madame's waiting-woman. Was it possible that the masked
troubadour and the enigmatic Prince de Froidmont were one and the same
person? and was it likely that Jacqueline's romantic fancy had been captured
by his wiles?

A wild, unreasoning rage gripped at de Landas' heart at the thought:


sheer physical pain caused him to groan aloud. He felt stifled and giddy,
and with a rough, impatient gesture, he threw open the casement-window
and leaned out, in order to inhale the pure, fresh air which rose from the
park. As he did so, he caught sight of Jacqueline, who was wandering in
and among the bosquets, attended only by one of her maids. She was
dressed in a dark gown and had a hood over her head, but even thus garbed
she looked adorable, and de Landas muttered an angry oath as he looked
down on her, watching her sedate movements, the queenly walk, that quaint
air of demureness and dignity which became her so well. He suddenly
realized all that the past few days—nay! weeks—had meant in the shaping
of his destiny. Monseigneur the governor's stern decree had already placed
her out of his reach; she was slipping away from him, dragged from his side
by her accession to wealth and power, by the political intrigues which
centred around her—aye! and she was also slipping away from him through
the gradual cooling of her attachment for him; that fact he could no longer
disguise from himself. He had succeeded in winning her, when she was so
young and so inexperienced that she fell readily enough—almost
unconsciously—into his arms. He had ensnared her like the skilful fowler
succeeds in trapping a fledgling unawares. Since then, so many things had
changed. Jacqueline, from an obscure little country wench—almost the
handmaid of an adulated brother—had become one of the most important
personages in the land. She was fêted, courted, admired, on every side,
surrounded by all that was most handsome, most chivalrous, in Europe. She
had not actually turned from the lover of her girlhood—no! even de Landas
was forced to admit that—but she had learned to appraise him in the same
crucible as other men; and, with teeth set, and shame and anger gnawing in
his heart, de Landas had to tell himself that she had apparently found him
wanting. Time was when nothing on earth would have turned her
admiration away from him, when, whatever the appearances might be, she
would look up to him as the fount of all bravery and of all honour. But last
night she had only been gentle and pitying, and a few hours later had led
Monseigneur into investigating the whole affair.

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