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De Gruyter Graduate
Leclerc, Gauvin ∙ Functional Materials
Also of Interest
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Functional
Materials

|
For Energy, Sustainable Development and
Biomedical Sciences

Edited by
Mario Leclerc and Robert Gauvin
Editors
Prof. Mario Leclerc Dr. Robert Gauvin
Department of Chemistry Scientific Liaison Officer
Université Laval Québec Center for Functional Materials (CQMF)
Quebec, Canada Quebec, Canada
Email: [email protected] Email: [email protected]

ISBN 978-3-11-030781-8
e-ISBN (PDF) 978-3-11-030782-5
e-ISBN (EPUB) 978-3-11-038819-0

Library of Congress Cataloging-in-Publication Data

A CIP catalog record for this book has been applied for at the Library of Congress.

Bibliographic information published by the Deutsche Nationalbibliothek

The Deutsche Nationalbibliothek lists this publication in the Deutsche Nationalbibliografie;
detailed bibliographic data are available on the Internet at http://dnb.dnb.de.

© 2014 Walter de Gruyter GmbH, Berlin/Boston

Cover image: PASCAL GOETGHELUCK/SPL/Agentur Focus
Typesetting: PTP-Berlin, Protago TEX-Produktion GmbH, www.ptp-berlin.de
Printing and binding: Hubert & Co. GmbH & Co. KG, Göttingen
♾ Printed on acid-free paper
Printed in Germany

www.degruyter.com
Foreword
When asked to write a foreword for this new book on functional materials, I initially
hesitated to comply with the request for a few simple reasons. First of all, new journals
and books on functional materials are sprouting these days like cabbage in the spring.
This is even more the case for original research papers printed in the usual disci-
plinary journals in chemistry, physics, medicine, and engineering. Consequently, it is
almost impossible to critically keep track and differentiate important studies from the
less significant ones. Moreover, not every original contribution contains completely
novel work, as many of them are instead additions to already well-known facts or well-
accepted lines of thought. In addition, the word “functional” implies that the material
serves a specific and defined purpose in a unique manner; but many contributors to
the field forget or overlook the fact that the material under consideration or subject
under study is just one of many components in a device and its function only evolves
through interplay with all the other components in the device. Note that even the sim-
plest of all rechargeable batteries as an example of a device contains at least a dozen
different functional materials, which all need to comply with the overall performance
of the battery. Thus, compatibility of materials is an important issue frequently over-
looked by eager researchers.
These critical remarks should not be misunderstood. We do not argue against aca-
demically motivated research in materials science. On the contrary, we think that high
quality work aiming at improved, optimized, and – to some extent – novel functional
materials is a necessity. We would merely like to express a warning against exagger-
ated promises and hopes that have no basis in the world of practice. After all, research
on functional materials must envisage practical solutions and is never justified as a
purely academic exercise. The clash between academic ideas and the reality of the
industry and the markets is nowhere harsher than in this field of science.
Despite these critical remarks, it is highly appreciated that this book is not simply
a review of the vast body of literature of the recent years, as it holds the focus upon
various aspects of application. Moreover, it selects only a few topics in favor of a solid
and thorough treatment of the relevant aspects. It is particularly pleasing that poly-
mer colloids receive much attention. Polymer colloids have seen an impressive revival
as a subject of academic research. This is a bit surprising at first sight, given the sit-
uation that emulsion and suspension polymerization processes have served as major
industrial processes in the mass production of polymers, to supply markets with ma-
terials for the coatings and adhesives industry, as textile and leather modifiers and as
constituent in cosmetics, just to mention a few. However, the widespread interest in
nanotechnology has guided the researchers to develop methods which not simply aim
at the synthesis of new molecules, but rather target the production of defined objects.
These nanosized objects are not only composed of different molecules, each type of
molecule contributing different functions to the object, but they also exhibit a defined
VI | Foreword

shape and size distribution, have a defined and controllable surface structure, and a
structured internal composition.
Similar cases are characteristic of the synthesis of mesoporous materials, which
have a long history as absorbents and filtering materials in industry, but have also
found new attention, with the desire to embed more functions into these materials
than was previously possible. This includes better control of pore structure and pore
size distribution. Here again, the target of the synthesis is the object, and not the indi-
vidual molecule which would only later be subject to further processing. Similarly,
nanoscale pigments have been available through industrial processes for decades.
Nevertheless, academic interest centers on the development of novel pigments with
particular size distribution, surface structure, and function, as well as specific elec-
tromagnetic properties. The definition of viable conditions for mass production by in-
dustrially acceptable processes is a key to the success of such research.
All of these aspects are treated in this book. In addition, materials for energy
storage (batteries and capacitors) as well as fuel cells are brought to the readers’s
attention. Last but not least, materials aiming towards application in the vast field
of biomedicine are discussed, described, and critically evaluated. Biocompatibility,
safety aspects, and the essential approval by the authorities are important aspects not
to be overlooked in this area, requiring extensive knowledge in both materials science
and medicine.
In summary, this book comes at a good time, when a large body of academic liter-
ature has been accumulated and is waiting for a critical inspection in the light of the
real demands of application. This book will provide valuable information to a critical
readership and should receive wide-spread recognition from the scientific community.

September 2014 Professor Gerhard Wegner

Emeritus scientific member
Max-Planck Institute for Polymer Research
Mainz, Germany
Preface
Energy, health, and environment are certainly at the top of the list of priorities in the
challenges facing society worldwide for the next 50 years. Functional materials are
providing new solutions and opportunities to ensure sustainable energy and environ-
ment, as well as improved medical care for the future. By its nature, the field of func-
tional materials is highly interdisciplinary, comprising basic sciences such as physics,
chemistry, and biology, as well as applied sciences and engineering. In this regard,
this book brings together the expertise of multiple experts and gives an overview of
emerging trends in this field of research. It allows the reader to associate a multitude
of functional materials with their respective application, in a way that has not pre-
viously been done in existing books covering smart or functional materials. As one
can imagine, this interdependence between synthesis, structure, properties, and per-
formance of functional materials requires applied and theoretical chemistry, physics,
biology, and engineering tools in order to ensure the development of novel and effi-
cient technologies (Fig. 1).

Synthesis

Properties

Structure

Performance

Fig. 1. The field of functional materials is by definition interdisciplinary, involving scientists from
various backgrounds in designing and synthesizing new materials with structure and properties
tailored in order to achieve optimal performance.

This book is addressed to experts as well as graduate students interested in the most
recent developments in the field of functional materials. It includes 15 chapters which
are organized in three sections focusing on (1) the synthesis and applications of func-
tional materials, (2) novel materials for energy applications, and (3) new trends in
functional materials for sustainable development and biomedical applications. The
chapters have been written by recognized experts in their respective fields and cover
topics ranging from fundamental concepts in synthesis to applied research projects.
Recent examples of how functional materials are improving many aspects of technol-
ogy currently available to us on a daily basis are also discussed. The authors are all
VIII | Preface

members of the Quebec Center for Functional Materials (CQMF), a research center lo-
cated in Quebec, Canada, and are internationally known for their work in the devel-
opment of innovative and state-of-the-art functional materials.
In summary, this book provides an overview of the recent advances made in syn-
thesis, characterization, and computer modeling, as well as various applications in-
volving functional materials, and should be of great interest for the scientific commu-
nity working in this area of research. The authors are grateful to Mrs. Patricia Basque
(CQMF), and Mr. Philippe Dufour (NanoULaval) for their collaboration, and to Mrs.
Karin Sora (De Gruyter), Mrs. Julia Lauterbach (De Gruyter), and Mrs. Kathleen Prüfer
(De Gruyter) for their assistance in editing this book. We also acknowledge financial
support from the FRQNT-Strategic Networks Funding Program, which provides the op-
portunity to bring scientists and engineers together in order to develop novel and in-
novative technologies.

Québec, August 2014 Mario Leclerc

Robert Gauvin
Contents
Foreword | V

Preface | VII

Contributing authors | XVII

About the editors | XXIII

R. Gauvin
1 Introduction | 1

Part I: Functional materials: Synthesis and applications

A. Al Shboul, F. Pierre, and J. P. Claverie

2 A primer on polymer colloids: structure, synthesis and
colloidal stability | 9
2.1 Introduction | 9
2.2 Polymer colloids inside out | 10
2.2.1 How many polymer chains per particle? | 10
2.2.2 How many particles? | 10
2.2.3 Are the chains immobile within the nanoparticle? | 12
2.2.4 Morphology of polymeric nanoparticles | 13
2.3 Preparation of polymer nanoparticles | 17
2.3.1 Emulsion polymerization | 18
2.3.2 Miniemulsion polymerization | 22
2.3.3 Microemulsion polymerization | 24
2.3.4 Self-assembly in selective solvents | 25
2.4 Colloidal stabilization | 26
2.4.1 Electrostatic stabilization | 26
2.4.2 Steric stabilization | 30
2.4.3 Depletion stabilization | 31
2.4.4 Future directions | 33

S. Rondeau-Gagné and J.-F. Morin

3 Synthesis, functionalization and properties of fullerenes and
graphene materials | 37
3.1 Introduction | 37
3.2 Fullerenes | 37
X | Contents

3.2.1 General considerations | 38

3.2.2 Synthesis and purification of fullerenes | 39
3.2.3 Chemical and physical properties of C60 | 40
3.2.4 Chemical functionalization of C60 | 42
3.2.5 Applications | 45
3.3 Graphene | 47
3.3.1 Production of graphene | 49
3.3.2 Graphene in energy conversion devices | 52

J. Florek, R. Guillet-Nicolas, and F. Kleitz

4 Ordered mesoporous silica: synthesis and applications | 61
4.1 Introduction | 61
4.2 Ordered mesoporous silica (OMS) | 62
4.2.1 Principle of synthesis | 63
4.2.2 Mesostructure diversity and tailoring | 69
4.3 Functionalization of ordered mesoporous silica | 78
4.4 Morphology control | 80
4.5 Selected applications of functionalized ordered
mesoporous silica | 82
4.5.1 Functionalized MSNs as controlled drug delivery platforms | 83
4.5.2 Functionalized mesoporous materials for extraction
chromatography (EXC) applications | 88
4.5.3 Mesoporous organic-inorganic hybrid membranes for
water desalination | 91

A. Ritcey
5 Nanoparticles: Properties and applications | 101
5.1 Introduction | 101
5.2 Synthetic methods | 101
5.2.1 Particle nucleation and growth | 102
5.2.2 Synthesis in inverse micelles | 104
5.3 Particle aggregation and stabilization of colloidal suspensions | 105
5.4 Colloidal quantum dots | 107
5.5 Metal nanoparticles | 110
5.6 Metal oxide nanoparticles | 112
5.6.1 Titanium dioxide | 112
5.6.2 Iron oxide | 113
5.6.3 Silica | 115
5.7 Polymeric nanoparticles | 115
5.8 Advanced architectures and hybrid systems | 117
 Contents | XI

N. Allard and M. Leclerc

6 Conjugated polymers for organic electronics | 121
6.1 Introduction | 121
6.2 Processable conjugated polymers | 122
6.3 Applications in renewable energy | 126
6.3.1 Organic solar cells | 126
6.3.2 Conjugated polymers for organic solar cells | 128
6.4 Applications in micro-electronics | 130
6.4.1 Field-effect transistors | 130
6.4.2 Conjugated polymers for field-effect transistors | 132
6.5 Applications in lighting | 133
6.5.1 Light-emitting diodes | 133
6.5.2 Conjugated polymers for light-emitting diodes | 135
6.6 Summary | 136

A. Soldera
7 Theoretical tools for designing microscopic to macroscopic properties
of functional materials | 139
7.1 Methods | 140
7.1.1 The link between microscopic and macroscopic scales | 140
7.1.2 Ab initio methods | 142
7.1.3 Bridging the gap between ab initio and atomistic levels | 146
7.1.4 Atomistic simulation | 147
7.1.5 Bridging the gap between atomistic and mesoscale levels | 151
7.2 Examples | 151
7.2.1 Quantum studies | 152
7.2.2 Atomistic simulation | 156
7.3 Summary | 164

Part II: Development of new materials for energy applications

S. B. Schougaard and D. Bélanger

8 Electrochemical energy storage systems | 171
8.1 Introduction | 171
8.2 Metrics and performance evaluation | 171
8.3 Models and theory of electrochemical charge storage | 173
8.3.1 Battery operation – a Faradaic process | 174
8.3.2 Electrochemical capacitor operation – a non-Faradaic process | 175
8.4 Electrolytes | 178
8.5 Electrode materials | 180
8.5.1 Electrochemical capacitors | 180
XII | Contents

8.5.2 Hybrid electrochemical capacitors | 181

8.5.3 Lithium battery electrode materials | 183
8.5.4 Negative (anode) electrode materials | 184
8.5.5 The positive (cathode) electrode | 185
8.5.6 Electrode production | 186
8.6 Summary | 186

D. Rochefort
9 Functional ionic liquids electrolytes in lithium-ion batteries | 189
9.1 Introduction | 189
9.1.1 Historical overview | 190
9.1.2 What are ionic liquids? | 191
9.1.3 Key properties as electrolytes | 192
9.2 Ionic liquids as Li and Lithium-ion battery electrolytes | 193
9.3 Functional ionic liquid electrolytes | 194
9.3.1 Overview of functional ionic liquids | 195
9.3.2 Solid electrolyte interphase | 196
9.3.3 Transport of lithium ions | 197
9.3.4 Electroactive ionic liquids as redox shuttles | 198
9.3.5 Perspectives | 202

C. de Bonis, A. D’Epifanio, B. Mecheri, S. Licoccia, and A. C. Tavares

10 Solid polymer proton conducting electrolytes for fuel cells | 207
10.1 Introduction | 207
10.2 Proton exchange membranes | 209
10.2.1 Nafion® | 210
10.2.2 Alternative sulfonated ionomers and membranes | 213
10.3 Characterization of solid polymer electrolytes | 218
10.3.1 Proton conductivity | 218
10.3.2 States of water and water mobility | 222
10.4 Summary | 233

P. Bénard, A.-M. Beaulieu, D. Durette, and R. Chahine

11 Supercritical adsorption of hydrogen on microporous adsorbents | 241
11.1 Introduction | 241
11.2 Fundamentals of supercritical adsorption | 242
11.3 Supercritical adsorption isotherms | 246
11.3.1 Virial expansion of the excess density in terms of pressure | 246
11.3.2 Basic analytic models of the adsorption isotherm | 252
11.3.3 Self-consistent approaches | 256
11.4 The thermodynamics of adsorption | 257
11.4.1 Properties of surface potential | 259
 Contents | XIII

11.5 Microporous adsorbents for hydrogen storage | 261

11.5.1 Activated carbons | 261
11.5.2 Single wall nanotubes | 262
11.5.3 Metal organic frameworks | 263

Part III: New trends in sustainable development and biomedical

applications

D. Mantovani, L. Levesque, G. Sabbatier, M. Leroy, D. G. Seifu, R. Tolouei,

V. Montaño, M. Cloutier, I. Bilem, C. Loy, M. Byad, C. Paternoster, C. A. Hoesli,
B. Drouin, G. Laroche
12 Advanced materials for biomedical applications | 277
12.1 Introduction | 277
12.2 History of biomaterials | 278
12.3 Basics in material science for biomaterial applications | 280
12.3.1 Biomaterial properties | 280
12.3.2 Biometals | 280
12.3.3 Bioceramics | 281
12.3.4 Biosynthetic polymers | 282
12.3.5 Natural polymers | 284
12.4 Biomedical applications | 286
12.4.1 Cardiovascular system | 286
12.4.2 Musculoskeletal system | 291
12.4.3 Visceral organs | 300
12.4.4 Nervous system and sensory organs | 304
12.4.5 Esthetic applications | 310
12.4.6 Skin | 312
12.5 Future trends | 319
12.5.1 Tissue engineering basic concepts | 319
12.5.2 Scaffolds | 319
12.5.3 Surface modification | 323
12.5.4 Stem cells | 323
12.5.5 Bioreactors | 324
12.5.6 Computational models | 324
12.6 Summary | 326

M.-A. Fortin
13 Nanoparticles for magnetic resonance imaging (MRI) applications
in medicine | 333
13.1 The basics of MRI in medicine | 337
13.2 Relaxivity: the performance of MRI contrast agents | 339
XIV | Contents

13.3 Synthesis and characterization of magnetic nanoparticles | 340

13.3.1 Synthesis of magnetic nanocrystals | 340
13.3.2 Nanoparticle coatings for MRI applications | 344
13.3.3 Physicochemical characterization | 346
13.4 Physical properties of magnetic nanoparticles | 347
13.5 MR relaxation properties of magnetic nanoparticles | 352
13.5.1 Relaxivity of paramagnetic CAs | 353
13.5.2 Relaxivity of superparamagnetic CAs | 356
13.5.3 Relaxometric performance of MRI CAs at clinical magnetic field
strengths | 358
13.6 Biological performance of magnetic nanoparticles for MRI | 358
13.6.1 In vivo barriers | 360
13.6.2 Impact of nanoparticle size and surface on colloidal stability and
blood retention | 361
13.6.3 Directing nanoparticles in vivo | 362
13.6.4 Toxicity | 363
13.7 Summary | 364

J. Greener
14 Microfluidics for synthesis and biological functional materials:
from device fabrication to applications | 375
14.1 Introduction | 375
14.2 A practical introduction to microfluidic reactors for
material synthesis | 376
14.2.1 Microfluidic reactor geometries | 376
14.2.2 Device fabrication materials | 377
14.2.3 Fabrication of polymer-based planar microreactors
and components | 380
14.3 Manipulating and measuring precursor reagent streams
in microchannels | 383
14.3.1 High surface area to volume ratios in microchannels | 383
14.3.2 Rapid heat transfer | 384
14.3.3 Control of concentrations | 384
14.3.4 Controlling “time on chip” | 386
14.3.5 Control of hydrodynamics and mass transfer | 386
14.3.6 Characterization in microchannels | 389
14.4 Microfluidics for polymer microparticles | 391
14.4.1 Manipulating the shaping of liquid precursors | 392
14.4.2 Effect of the channel wall | 392
14.4.3 Emulsification of precursor droplets | 393
14.4.4 Channel geometries to achieve emulsified droplets | 393
14.4.5 Multiple emulsions | 395
 Contents | XV

14.4.6 Forming linear threads and two-dimensional interfaces | 395

14.4.7 Converting liquid precursors into solid micro-materials | 397
14.4.8 Scale up: a circuit analysis of microfluidic flow in a highly
parallelized microreactor | 397
14.5 Microfluidics for synthesis of functional nanoparticles | 400
14.5.1 Microfluidics for highly controlled nanoparticle synthesis | 401
14.6 Biomaterials | 402
14.6.1 Tissue engineering and membranes | 403
14.6.2 Microenvironments for encapsulated cells | 404
14.6.3 Biofilms | 406
14.6.4 Microdevices utilizing functional biomaterials | 407
14.7 Summary | 410

T. Lefèvre, F. Byette, I. Marcotte, and M. Auger

15 Protein- and peptide-based materials: a source of inspiration
for innovation | 415
15.1 Introduction | 415
15.2 Basics of proteins, peptides and polypeptides | 417
15.2.1 Polypeptides are sequences of amino acids | 417
15.2.2 Polypeptides can adopt various conformations | 418
15.2.3 Polypeptides possess various levels of structural organization | 419
15.3 Functional materials from fibrous proteins | 420
15.3.1 Resilin & abductin | 421
15.3.2 Byssus (mussel anchoring threads) | 422
15.3.3 Silk | 425
15.4 Functional materials from globular proteins | 429
15.4.1 Natural proteins | 429
15.4.2 Artificial proteins | 430
15.5 Functional materials from synthetic peptides | 432
15.6 Summary | 435

B. Riedl, V. Vardanyan, W. N. Nkeuwa, A. Kaboorani, V. Landry, B. Poaty, M. Vlad,

and C. Sow
16 Nanocomposite coatings | 443
16.1 Introduction | 443
16.2 Coating formulations | 446
16.2.1 Chemical components | 446
16.2.2 Mixing techniques | 447
16.2.3 Application and curing | 449
16.3 Nanoparticle additives | 449
16.4 Coating characterization | 454
16.4.1 Mechanical properties | 454
XVI | Contents

16.4.2 Optical properties | 456

16.4.3 X-ray imaging and particle aggregation | 459
16.4.4 Weathering and artificial aging | 459
16.5 Bio-based coatings | 460
16.6 Future developments | 462
16.7 Summary | 463

Index | 465
Contributing authors
Nicolas Allard Ibrahim Bilem
Department of Chemistry Department of Mining, Metallurgical
Université Laval and Materials Engineering
Quebec, QC, Canada Université Laval
e-mail: [email protected] and
Chapter 6 Centre de recherche du CHU de Québec
Québec, QC, Canada
Ahmad Al Shboul e-mail: [email protected]
Department of Chemistry Chapter 12
Université du Québec à Montréal (UQAM)
Montréal, QC, Canada Michael Byad
e-mail: [email protected] Department of Mining, Metallurgical
Chapter 2 and Materials Engineering
Université Laval
Michèle Auger and
Department of Chemistry Centre de recherche du CHU de Québec
Université Laval Québec, QC, Canada
Quebec, QC, Canada e-mail: [email protected]
e-mail: [email protected] Chapter 12
Chapter 15
Frédéric Byette
Ann-Marie Beaulieu Department of Chemistry
Research Institute on Hydrogen Université du Québec à Montréal
Université du Québec à Trois-Rivières (UQTR) and
Trois-Rivières, QC, Canada Université de Montréal
e-mail: [email protected] Montréal, QC, Canada
Chapter 11 e-mail: [email protected]
Chapter 15
Daniel Bélanger
Department of Chemistry Richard Chahine
Université du Québec à Montréal (UQAM) Department of Electrical Engineering and
Montréal, QC, Canada Computer Engineering
e-mail: [email protected] Université du Québec à Trois-Rivières
Chapter 8 Trois-Rivières, QC, Canada
e-mail: [email protected]
Pierre Bénard Chapter 11
Research Institute on Hydrogen
Université du Québec à Trois-Rivières (UQTR) Jerome P. Claverie
Trois-Rivières, QC, Canada Department of Chemistry
e-mail: [email protected] Université du Québec à Montréal (UQAM)
Chapter 11 Montréal, QC, Canada
e-mail: [email protected]
Chapter 2
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