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Oxide Electronics
Wiley Series in Materials for Electronic &
Optoelectronic Applications
www.wiley.com/go/meoa
Series Editors
Professor Richard Curry, University of Manchester, Manchester, UK
Professor Jun Luo, Chinese Academy of Sciences, Beijing, China
Professor Harry E. Ruda, University of Toronto, Toronto, Canada
Founding Series Editors

Professor Arthur Willoughby, University of Southampton, Southampton, UK
Dr Peter Capper, Ex-Leonardo MW Ltd, Southampton, UK
Professor Safa Kasap, University of Saskatchewan, Saskatoon, Canada
Published Titles
Bulk Crystal Growth of Electronic, Optical and Optoelectronic Materials, Edited by P. Capper
Properties of Group-IV. III–V and II–VI Semiconductors, S. Adachi
Charge Transport in Disordered Solids with Applications in Electronics, Edited by S. Baranovski
Thin Film Solar Cells: Fabrication, Characterization, and Applications, Edited by J. Poortmans and
V. Arkhipov
Dielectric Films for Advanced Microelectronics, Edited by M. R. Baklanov, M. Green, and K. Maex
Liquid Phase Epitaxy of Electronic, Optical and Optoelectronic Materials, Edited by P. Capper and M. Mauk
Molecular Electronics: From Principles to Practice, M. Petty
Luminescent Materials and Applications, A. Kitai
CVD Diamond for Electronic Devices and Sensors, Edited by R. S. Sussmann
Properties of Semiconductor Alloys: Group IV, III–V, and II–VI Semiconductors, S. Adachi
Mercury Cadmium Telluride, Edited by P. Capper and J. Garland
Zinc Oxide Materials for Electronic and Optoelectronic Device Applications, Edited by C. Litton, D. C.
Reynolds, and T. C. Collins
Lead-Free Solders: Materials Reliability for Electronics, Edited by K. N. Subramanian
Silicon Photonics: Fundamentals and Devices, M. Jamal Deen and P. K. Basu
Nanostructured and Subwavelength Waveguides: Fundamentals and Applications, M. Skorobogatiy
Photovoltaic Materials: From Crystalline Silicon to Third-Generation Approaches, Edited by G. Conibeer and
A. Willoughby
Glancing Angle Deposition of Thin Films: Engineering the Nanoscale, Matthew M. Hawkeye, Michael T.
Taschuk, and Michael J. Brett
Physical Properties of High-Temperature Superconductors, R. Wesche
Spintronics for Next Generation Innovative Devices, Edited by Katsuaki Sato and Eiji Saitoh
Inorganic Glasses for Photonics: Fundamentals, Engineering and Applications, Animesh Jha
Amorphous Semiconductors: Structural, Optical and Electronic Properties, Kazuo Morigaki, Sandor Kugler,
and Koichi Shimakawa
Microwave Materials and Applications 2V , Edited by Mailadil T. Sebastian, Rick Ubic, and Heli Jantunen
Molecular Beam Epitaxy: Materials and Applications for Electronics and Optoelectronics, Edited by Hajime
Asahi and Yoshiji Korikoshi
Metalorganic Vapor Phase Epitaxy (MOVPE), Edited by Stuart Irvine and Peter Capper
Optical Properties of Condensed Matter and Applications 2e, Edited by J. Singh
Oxide Electronics, Edited by Asim Ray
Oxide Electronics
Edited by
Asim Ray
Brunel University
London, UK
This edition first published 2021
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Library of Congress Cataloging-in-Publication Data
Names: Ray, Asim K., editor.

Title: Oxide electronics / edited by Asim Ray, Brunel University
London, England, United Kingdom.
Description: First edition. | Hoboken, NJ, USA : John Wiley and Sons, Inc.,
2021. | Series: Wiley series in materials for electronic &
optoelectronic applications | Includes bibliographical references and
index.
Identifiers: LCCN 2020051123 (print) | LCCN 2020051124 (ebook) | ISBN
9781119529477 (hardback) | ISBN 9781119529484 (adobe pdf ) | ISBN
9781119529507 (epub)
Subjects: LCSH: Electronics–Materials. | Metallic oxides. |
Oxides–Electric properties.
Classification: LCC TK7871 .O95 2021 (print) | LCC TK7871 (ebook) | DDC
621.381028/4–dc23
LC record available at https://lccn.loc.gov/2020051123
LC ebook record available at https://lccn.loc.gov/2020051124
Cover Design: Wiley

Cover Images: Courtesy of Subhasish Basu Majumder
Set in 10/12pt WarnockPro by SPi Global, Chennai, India
10 9 8 7 6 5 4 3 2 1
v
Contents
Series Preface xiii

Preface xv
List of Contributors xvii
1 Graphene Oxide for Electronics 1

Fenghua Liu, Lifeng Zhang, Lijian Wang, Binyuan Zhao and Weiping Wu
1.1 Introduction 1
1.2 Synthesis and Characterizations of Graphene Oxide 2
1.2.1 Chemical Reduction of Graphene Oxide (GO) 2
1.2.2 Microwave Method 2
1.2.3 Plasma Method 3
1.2.4 Laser Method 4
1.3 Energy Harvest Applications of Graphene Oxide 5
1.3.1 Solar Cells 5
1.3.2 Solar Thermal Energy Harvest Devices 7
1.4 Energy Storage Applications of Graphene Oxide 7
1.4.1 Supercapacitors 7
1.4.2 Batteries 10
1.5 Electronic Device Applications of Graphene Oxide 12
1.6 Large Area Electronics Applications of Graphene Oxide 13
References 16
2 Flexible and Wearable Graphene-Based E-Textiles 21

Nazmul Karim, Shaila Afroj, Damien Leech and Amr M. Abdelkader
2.1 Introduction to Wearable E-Textiles 21
2.2 Synthesis of Graphene Derivatives 22
2.2.1 Graphene Oxide 22
2.2.2 Reduced Graphene Oxide 24
2.3 Graphene-Based Wearable E-Textiles 25
2.3.1 Graphene-Based Textile Fibres 26
2.3.2 Graphene-Coated Textiles 27
2.3.3 Graphene-Printed Wearable E-Textiles 28
2.3.3.1 Screen Printing 30
2.3.3.2 Inkjet Printing 30
2.4 Surface Pre- and Post-Treatment of Substrates 32
2.5 Applications 34
2.5.1 Sensors 34
vi Contents
2.5.2 Supercapacitor 36
2.5.3 Rechargeable Batteries 38
2.5.4 Optoelectronics 39
2.6 Challenges and Outlook 40
References 41
3 Magnetic Interactions in the Cubic Mott Insulators NiO, MnO, and CoO and the
Related Oxides CuO and FeO 51
David J. Lockwood and Michael G. Cottam
3.1 Introduction 51
3.2 Spin–Spin Interactions 52
3.2.1 Magnetic Ordering Below T N 52
3.2.2 Magnetostriction 53
3.2.3 Magnetic and Electronic Excitations 54
3.3 Spin–Phonon Interactions 59
3.3.1 Phonon and Magnon Temperature Dependences 60
3.3.2 Phonon Mode Splitting Below T N 62
3.4 Other Related Materials 64
3.4.1 Cupric Oxide 64
3.4.2 Iron Monoxide 65
3.5 Conclusions 68
Acknowledgments 68
References 68
4 High-𝜿 Dielectric Oxides for Electronics 75

Tong Zhang, Xiaoyang Zhang, Yi Yang and Weiping Wu
4.1 Introduction of High-𝜅 Dielectric Oxides 75
4.1.1 Group IIIA Dielectric Oxides 77
4.1.2 Group IIIB High-𝜅 Dielectric Oxides 77
4.1.3 Group IVB High-𝜅 Dielectric Oxides 77
4.2 The Deposition of High-𝜅 Oxide Dielectrics 78
4.3 High-𝜅 Dielectric Oxides for Field-Effect Transistors 80
4.3.1 High-𝜅 Dielectric Oxides for the MOSFETs 80
4.3.2 High-𝜅 Dielectric Oxides for Tunnel Field-Effect Transistors 84
4.4 High-𝜅 Dielectric Oxides for Memory Devices 85
4.4.1 High-𝜅 Dielectric Oxides for DRAM 85
4.4.2 High-𝜅 Dielectric Oxides for ReRAM 87
References 88
5 Low Temperature Growth of Germanium Oxide Nanowires by Template Based

Self Assembly and their Raman Characterization 93
Raisa Fabiha, Abigail Casey, Gregory Triplett and Supriyo Bandyopadhyay
5.1 Introduction 93
5.2 Synthesis 93
5.3 Characterization 96
5.4 Raman Measurements 96
5.5 Conclusion 98
References 99
Contents vii
6 Electronic Phenomena, Electroforming, Resistive Switching, and Defect

Conduction Bands in Metal-Insulator-Metal Diodes 101
Thomas W. Hickmott
6.1 Introduction 101
6.2 Experimental 103
6.3 Electroforming, Electroluminescence, and Electron Emission 104
6.3.1 Electroforming of Al-Al2 O3 -Ag Diodes 104
6.3.2 Electroluminescence from Al-Al2 O3 -Ag Diodes 104
6.3.3 Electron Emission from Al-Al2 O3 -Ag Diodes 105
6.3.4 VCNR, EL, and EM in Other Insulators 107
6.3.5 Temperature Dependence of EM 108
6.4 Electrode Effects in Resistive Switching of Nb-Nb2 O5 -Metal Diodes 109
6.4.1 Resistive Switching in Nb-Nb2 O5 -Metal Diodes 109
6.4.2 Resistive Switching at Low Temperatures 109
6.4.3 Structure in I-V Curves of Electroformed Nb-Nb2 O5 -Metal
Diodes 110
6.5 Conduction, Electroluminescence, and Photoconductivity Before
Electroforming MIM Diodes 112
6.5.1 Conduction in Nb-Nb2 O5 -Au Diodes 112
6.5.2 Electroluminescence in Nb-Nb2 O5 -Au Diodes 112
6.5.3 Conduction and Electroluminescence in MIM Diodes with
TiO2 and Ta2 O5 115
6.5.4 Photoconductivity in MIM Diodes 115
6.6 Discussion 118
6.6.1 Defect Conduction Bands in Amorphous Al2 O3 119
6.6.2 Defect Conduction Bands in Amorphous Nb2 O5 121
6.6.3 Defect Conduction Bands in Amorphous Insulators 123
6.7 Summary and Conclusions 125
References 125
7 Lead Oxide as Material of Choice for Direct Conversion Detectors 129

Alla Reznik and Oleksii Semeniuk
7.2 Crystal Structure and Electronic Properties of PbO 130
7.2.1 Crystal Structure of Tetragonal PbO (𝛼-PbO) 131
7.2.2 Crystal Structure of Orthorhombic PbO (𝛽-PbO) 132
7.2.3 Electronic Properties of 𝛼- and 𝛽-PbO 133
7.3 Deposition Process of PbO Layers 135
7.4 Charge Transport Mechanism in Lead Oxide 147
7.4.1 Electron Transport in poly-PbO 148
References 151
8 ZnO Varistors: From Grain Boundaries to Power Applications 157

Felix Greuter
8.2 Manufacturing Process of ZnO Varistors 160
8.3 Microstructure and Grain Boundaries 162
8.4 Grain Boundary Potential Barriers 168
viii Contents
8.5 The ‘Double Schottky Barrier Defect Model’ 174

8.6 Hot Electron Effects Controlling the Breakdown Region 181
8.7 Hot Electron Effects and Dynamic Response 185
8.8 From Single Grain Boundaries to Microstructures and Varistor Devices 196
8.9 Ageing and Long-Term Stability of Varistor Materials 207
8.10 Energy Absorption Capability and High Current Impulse Stresses 218
8.11 Summary and Outlook 223
Acknowledgements 226
References 226
9 Fundamental Properties and Power Electronic Device Progress of Gallium

Oxide 235
Xuanhu Chen, Chennupati Jagadish and Jiandong Ye
9.2 Electronic Properties and Defects of Ga2 O3 236
9.2.1 Bulk Crystals, Epitaxy, and n–type Doping 237
9.2.2 Electronic Band Structure and Feasibility of p–type Doping 240
9.2.3 Defect Behaviour in Bulk Crystals and Epitaxial Films 245
9.3 Basic Device Characteristics 250
9.3.1 Metal-Semiconductor Contact 250
9.3.1.1 Barrier Formation 250
9.3.1.2 Image-Force Lowering 252
9.3.1.3 Carrier Transport and Breakdown 254
9.3.2 Physics of Deep Depletion Ga2 O3 MOSFETs 257
9.3.2.1 Metal-Insulator-Semiconductor Capacitors 257
9.3.2.2 Basic Device Characteristics of Depletion Mode
MOSFETs Based on Ga2 O3 270
9.3.2.3 Approaches to Enhancement-Mode 𝛽-Ga2 O3
MOSFETs 280
9.3.3 Relevant Figure of Merit in Ga2 O3 282
9.4 Ga2 O3 Schottky Rectifiers 286
9.4.1 Edge Terminations 287
9.4.2 Ga2 O3 Schottky Rectifiers 295
9.4.3 Ga2 O3 p-n Heterojunction Diodes 301
9.5 Ga2 O3 Transistors 307
9.5.1 Ohmic Contacts to Ga2 O3 307
9.5.2 Dielectric Materials for Ga2 O3 and MOSCaps 308
9.5.3 Lateral Ga2 O3 FETs 313
9.5.4 𝛽-Ga2 O3 MODFETs 324
9.5.5 Vertical Ga2 O3 MOSFETs 330
9.6 Summary 335
References 336
10 Emerging Trends, Challenges, and Applications in Solid-State Laser Cooling 353

Jyothis Thomas, Lauro Maia, Yannick Ledemi, Younes Messaddeq and Raman
Kashyap
10.2 Theory 355
Contents ix
10.3 Experimental Design Considerations for Cooling 357

10.3.1 Experimental Setups Used for Solid-state Laser Cooling 357
10.3.1.1 Crystals 357
10.3.1.2 Glasses 358
10.3.1.3 Silica Glass Optical Fibres 360
10.3.1.4 Semiconductor Nanoribbons 361
10.3.2 Techniques to Analyse Background Absorption (𝛼 b ) Coefficient 361
10.3.3 Temperature Measurement Techniques in Solid-State Laser
Cooling 362
10.3.3.1 Thermal Imaging 362
10.3.3.2 Photoluminescence (PL) Thermometry 363
10.3.3.3 Temperature Measurement Using Fibre Bragg
Gratings 363
10.3.3.4 Thermocouples 364
10.3.3.5 Photothermal Deflection Spectroscopy (PTDS) 364
10.3.3.6 Interferometric Technique 364
10.4 Laser Cooling Materials and Properties 365
10.4.1 Crystals 366
10.4.2 Semiconductors 368
10.4.3 Optical Fibres 370
10.4.4 Nanocrystalline Powders 371
10.5 Oxyfluoride Glass-Ceramics: Recent Developments in Solid-State
Laser Cooling 373
10.5.1 Earth-Doped Oxyfluoride Pseudo-Binary Glasses and
Glass-Ceramics for Optical Refrigeration 375
10.5.1.1 Materials and Methods 376
10.5.1.2 Results and Discussion 376
10.5.1.3 Summary on Pseudo-Binary Oxyfluoride Glass
Ceramics 381
10.6 Optical Cryocooler Devices 382
10.7 Future Prospects and Conclusions 386
References 388
11 Electrode Materials for Sodium Ion Rechargeable Batteries 397

Tania Majumder, Anwesa Mukherjee, Debasish Das and S.B. Majumder
11.1 Introduction – Review of the Constituents Used in Na – Ion Cells 397
11.2 Cathode Materials for Na Ion Rechargeable Cells 397
11.2.1 Transition Metal Oxides with Layered Structure 397
11.2.2 Prussian Blue Analogue 398
11.2.3 Sodium Superionic Conductors (NASICON) 399
11.2.4 Other Cathodes 400
11.3 Current Collectors, Binder, and Electrolyte 400
11.4 Anode Materials for Na Ion Rechargeable Cells 401
11.4.1 Carbonaceous Materials 401
11.4.2 Alloying Type Anodes 401
11.4.3 Conversion Type Anodes 402
11.4.4 Other Anodes 402
11.5 Outstanding Research Issues and Statement of the Problem 402
x Contents
11.6 Synthesis and Electrochemical Characterization of Electrodes 404

11.6.1 Ilmenite NiTiO3 as Anode 404
11.6.1.1 Synthesis and Characterization 404
11.6.2 Electrochemical Characterization 404
11.6.3 Electrophoretic Deposition of NiTiO3 -Based Anode 406
11.6.4 Electrochemical Performance of EPD Grown NTO Anodes 408
11.7 Na2 Ti3 O7 as Anode 409
11.7.1 Synthesis and Characterization 409
11.7.2 Electrochemical Characterization of Pristine NaTO 410
11.7.3 Electrochemical Performance of Carbon-Coated NaTO Anode 411
11.7.4 Electrochemical Performance of NaTO/rGO Composite Anode 413
11.8 PBA as Cathode 414
11.8.1 Nickel Hexacyanoferrate (NiHCF) 415
11.8.2 Iron Hexacyanoferrate (FeHCF) 417
11.9 Summary and Conclusions 418
Acknowledgement 419
References 419
12 Perovskites for Photovoltaics 423

Hooman Mehdizadeh Rad, David Ompong and Jai Singh
12.2 Diffusion Length 424
12.2.1 Methodology 425
12.2.2 Results of Simulated Diffusion Length and Discussions 427
12.3 Open-Circuit Voltage 432
12.3.1 Results of Open-Circuit Voltage and Discussions 433
12.3.2 Bimolecular Recombination 436
12.4 Influence of Density of Tail States at Interfaces 437
12.4.1 Methods 437
12.4.2 Results of Density of States and Discussions 441
12.5 Conclusions 444
References 447
13 Advanced Characterizations of Oxides for Optoelectronic Applications 453

U. Onwukwe, L. Anguilano and P. Sermon
13.1 A Brief History of Optoelectronic Devices 453
13.1.1 Semiconductors 454
13.1.1.1 n-Type Extrinsic Semiconductors 455
13.1.1.2 p-Type Extrinsic Semiconductors 456
13.2 Interaction of Semiconductors and the Optoelectronic Phenomenon 457
13.2.1 Direct Band Gap Semiconductors 457
13.2.1.1 Indirect Band Gap Semiconductors 458
13.2.2 Oxides for Optoelectronics: Introduction 459
13.2.3 Major Types of MO for Optoelectronics 460
13.2.3.1 ITO 460
13.2.3.2 ZnO 460
13.2.3.3 AZO 461
13.2.3.4 IGZO 461
13.2.3.5 Perovskite Oxides 462
Contents xi
13.2.3.6 Reduced Graphene Oxide-Miscellaneous Materials 463

13.2.4 Method of Preparation of Optoelectronic Structures 467
13.2.4.1 Nanowires/Nanorods 467
13.2.4.2 Thin Films 467
13.2.4.3 Mixed Morphologies Fabrication 468
13.3 Characterization Techniques and their Use for Metal Oxide
Optoelectronics 470
13.3.1 Rutherford Backscattering Spectrometry (RBS) 470
13.3.2 Fourier-Transform Infra-Red (FTIR) 471
13.3.2.1 Raman Spectroscopy 473
13.3.3 Scanning Electron Microscopy (SEM) 475
13.3.4 Transmission Electron Microscope (TEM) 477
13.3.5 Luminescence Techniques 480
13.3.6 X-Ray Diffraction 482
13.4 Facilities and Case Studies 484
13.4.1 Case Study I – Leaf Biotemplate Derived TiO2 485
References 488
14 Future Tuning Optoelectronic Oxides from the Inside: Sol-Gel (TiO2 )x -(SiO2 )100-x 497
M.P. Worsley, J.G. Leadley, R.M.A. MacGibbon, T. Salvesen, P.A. Sermon and J.M.
Charnock
14.1 Introduction and Background 497
14.1.1 Photons and Wavetrains 497
14.1.2 Optoelectronic Oxides and Devices 497
14.1.3 TiO2 498
14.1.4 TiO2 -SiO2 498
14.1.5 Alkoxide and Sol-Gel Routes to TiO2 -SiO2 500
14.1.6 Miscibility and the % TiO2 (x) Added in TiO2 -SiO2 500
14.1.7 Doping of TiO2 -SiO2 501
14.1.8 Local Structure in TiO2 -SiO2 501
14.2 Hypothesis 503
14.3 Experimental 504
14.3.1 Materials 504
14.3.2 Preparations 504
14.3.3 Characterization Methods 504
14.4 Characterization Results 505
14.5 Discussion on Future Automated CALPHAD Design, Dip-Coating
Mechanical, and High-Throughput Screening of Novel Optoelectronic
Oxides and Devices 510
14.6 Conclusions on TiO2 -SiO2 Use 510
References 513
15 Binary Calcia-Alumina Thin Films: Synthesis and Properties and Applications 525
Asim K. Ray
15.2 Structural and Physical Properties of C12A7 526
15.2.1 Thermal Stability 528
15.2.2 Ionic Conductivity and Mechanisms of Oxide–Ion Migration 529
xii Contents
15.3 Atomic and Electronic Structure 530

15.3.1 Synthesis of C12A7 531
15.3.2 Single Powders 531
15.3.3 Single Crystal 532
15.3.4 Polycrystalline Bulk 533
15.3.5 Thin Film 535
15.3.6 Ion Doping in C12A7 536
15.3.6.1 Heat Treatment in H2 Atmosphere 537
15.3.6.2 Thermoelectricity 537
15.4 Optical Properties 540
15.4.1 Reflectivity 541
15.4.2 Luminescence 542
15.5 Applications of C12A7 543
15.6 Summary 545
References 546
16 Oxide Cathodes 553

Ian Alberts
16.1 Historical Aspects 553
16.1.1 The Edison Effect 555
16.1.2 Arthur Wehnelt 555
16.1.3 Thermionic Emission Research in the Early Twentieth Century 556
16.1.4 Oxide Cathodes for the CRT 556
16.2 Physics of Thermionic Emission 557
16.2.1 Derivation of the Richardson-Dushman Equation 558
16.2.2 Space Charge and the Child-Langmuir Law 559
16.3 Oxide Cathode Development 560
16.3.1 The Barium-Coated Cathode 561
16.3.2 The Rise and Subsequent Fall of the Impregnated Cathode 562
16.3.3 Cermet Cathodes 565
16.3.4 State of the Art 565
16.4 Future Trends and Ongoing Applications 567
16.4.1 Vacuum X-Ray Tubes 568
16.4.2 Military Telecommunications 568
16.4.3 Klystrons 570
16.4.4 Gyrotron 571
16.4.5 Thermionic Energy Conversion 571
16.4.6 Triboelectric Nanogenerators 573
16.4.7 Frontiers in Thermionic Research: Vacuum Nanoelectronics 575
16.4.8 Field Emission Displays (FED) 575
16.5 Conclusion 577
References 577
Index 583
xiii
Series Preface
Wiley Series in Materials for Electronic and Optoelectronic

Applications
This book series is devoted to the rapidly developing class of materials used for elec-
tronic and optoelectronic applications. It is designed to provide much-needed infor-
mation on the fundamental scientific principles of these materials, together with how
these are employed in technological applications. The books are aimed at (postgradu-
ate) students, researchers, and technologists, engaged in research, development, and the
study of materials in electronics and photonics, and industrial scientists developing new
materials, devices, and circuits for the electronic, optoelectronic and, communications
industries.
The development of new electronic and optoelectronic materials depends not only on
materials engineering at a practical level, but also on a clear understanding of the prop-
erties of materials, and the fundamental science behind these properties. It is the prop-
erties of a material that eventually determine its usefulness in an application. The series
therefore also includes such titles as electrical conduction in solids, optical properties,
thermal properties, and so on, all with applications and examples of materials in elec-
tronics and optoelectronics. The characterization of materials is also covered within the
series in as much as it is impossible to develop new materials without the proper char-
acterization of their structure and properties. Structure–property relationships have
always been fundamentally and intrinsically important to materials science and engi-
neering.
Materials science is well known for being one of the most interdisciplinary sciences.
It is the interdisciplinary aspect of materials science that has led to many exciting dis-
coveries, new materials and new applications. It is not unusual to find scientists with
a chemical engineering background working on materials projects with applications in
electronics. In selecting titles for the series, we have tried to maintain the interdisci-
plinary aspect of the field, and hence its excitement to researchers in this field.
Arthur Willoughby
Peter Capper
Safa Kasap
xv
Preface
Potential applications of oxide electronic materials are vast. Transparent electronics,

optoelectronics, magnetoelectronic, photonics, spintronics, thermoelectric, piezoelec-
tric, resistive switching, power harvesting, hydrogen storage, and environmental waste
management has stimulated huge interests, both academic and industrial, in oxide elec-
tronics. The vast wealth of functional properties of oxides is first rooted in the extreme
diversity of characterizing techniques. Complex transition metal oxides exhibit mani-
fold physical properties comprising high-temperature superconductivity, piezoelectric-
ity, ferroelectricity, magnetism, multiferroicity, and resistive switching. The functional
properties of complex metal oxides are very sensitive to the details of electronic struc-
ture and are thereby strongly influenced by the elemental composition and the presence
of defects or lattice distortions. The nanoscale form of oxides provides a new dimension
due to the increased surface-to-volume ratio.
This handbook contains 16 chapters. These topics have a broader appeal with a view
to satisfying the multidisciplinary need of electrical and electronic engineers, physi-
cists, and material scientists. The format of these chapters is similar to one another.
For example, each begins with an abstract followed by an introduction to the topic
and a clear illustration of contents with relevant equations and graphical illustrations.
Chapters end with a summary of the description. Each chapter contains an adequate
number of supporting references, pointing out the additional contribution to existing
knowledge. All chapters are self-contained with no overlapping in their contents. Dif-
ficult mathematics has been avoided as far as possible in describing the science within
the chapters. The handbook is highly interdisciplinary so that its chapters are valuable
for readers with different backgrounds.
I am very grateful to all the authors for their excellent contributions. Each topic
is multidisciplinary, Therefore, readers with chemistry backgrounds but working in
electrical engineering will may be interested in this handbook. Similarly, physicists
will benefit from this handbook in order to acquire knowledge in materials science.
The authors’ cooperation in delivering their manuscripts during different stages of
production has also been very much appreciated. Sincere thanks are due to Jenny
Cossham and Katrina Maceda for their help over several months in commissioning the
contributions and getting them ready for production.
xvi Preface
It is my great pleasure to thank Professor Safa Kasap for his many helpful suggestions.
He is the Editor-in-Chief of Materials Science: Materials in Electronics. His advice on
the selection of chapters and their authors has been very much appreciated.
Finally, the editor wishes to thank all the members of their family (Arunima, Raj,
Madhurima, Rishabh, Mayan and Reuben).
Asim Ray
London, UK, August 2016
xvii
List of Contributors
Amr M. Abdelkader Supriyo Bandyopadhyay

Department of Design and Engineering Department of Electrical and Computer
Bournemouth University Engineering
Dorset Virginia Commonwealth University
UK Richmond
USA
Shaila Afroj
Centre for Fine Print Research Abigail Casey
The University of West of England Department of Electrical and Computer
Bristol Engineering
UK Virginia Commonwealth University
Richmond
U. Onwukwe, L. Anguilano USA
College of Engineering,
Design and Physical Sciences J.M. Charnock
Brunel University London Nanomaterials and Applications
Uxbridge Laboratory
UK CEDPS, Bragg Building
Brunel University
Ian Alberts Uxbridge
Department of Nuclear Medicine UK
Inselspital, Bern University Hospital
University of Bern Xuanhu Chen
Bern School of Electronic Science and
Switzerland Engineering
and Nanjing University
Nanjing
LG.Philips Displays
China
Lancashire
UK
Michael G. Cottam
Department of Physics and Astronomy
Western University, London
Ontario
Canada
xviii List of Contributors
Debasish Das J.G. Leadley

School of Nano Science and Technology Nanomaterials and Applications
Indian Institute of Technology Laboratory
Kharagpur CEDPS, Bragg Building
W. Bengal Brunel University
India Uxbridge
UK
Raisa Fabiha
Department of Electrical and Computer Yannick Ledemi
Engineering Department of Electrical Engineering
Virginia Commonwealth University École Polytechnique de Montréal
Richmond Canada
USA
Damien Leech
Felix Greuter Centre for Fine Print Research
Department of Energy & Materials The University of West of England
ABB Corporate Research Bristol
Baden-Daettwil UK
Switzerland
Fenghua Liu
Thomas W. Hickmott Shanghai Institute of Optics and Fine
Department of Physics Mechanics
State University of New York at Albany Chinese Academy of Sciences
Albany Shanghai
USA China
Chennupati Jagadish David J. Lockwood

Department of Electronic Materials Metrology Research Centre
Engineering and ARC Centre of National Research Council Canada
Excellence on Transformative Ottawa, Ontario
Meta-Optical Systems Canada
Research School of Physics
Australian National University, ACT R.M.A. MacGibbon
Canberra Nanomaterials and Applications
Australia Laboratory
CEDPS, Bragg Building
Nazmul Karim Brunel University
Centre for Fine Print Research Uxbridge
The University of West of England UK
Bristol
UK Lauro Maia
Instituto de Física
Raman Kashyap Universidade Federal de Goiás
Department of Engineering Physics Goiânia
École Polytechnique de Montréal Brazil
Canada
List of Contributors xix
S.B. Majumder Asim K. Ray

Materials Science Centre Design & Physical Sciences
Indian Institute of Technology College of Engineering
Kharagpur Brunel University
W. Bengal Uxbridge
India UK
Tania Majumder Alla Rez

Materials Science Centre Physics Department
Indian Institute of Technology Lakehead University
Kharagpur Thunder Bay
W. Bengal Canada
India and
Thunder Bay Regional Health Research
Hooman Mehdizadeh Rad
Institute
College of Engineering
Thunder Bay
IT and Environment
Canada
Charles Darwin University
Darwin
T. Salvesen
Australia
Nanomaterials and Applications
Laboratory
Younes Messaddeq
CEDPS, Bragg Building
Centre d′ optique,
Brunel University
Photonique et Laser
Uxbridge
Université Laval
UK
Québec
Canada
Oleksii Semeniuk
Radiation Medicine Program
Anwesa Mukherjee
Princess Margaret Cancer Centre
Materials Science Centre
Toronto, ON
Indian Institute of Technology
Canada
Kharagpur
W. Bengal
Jai Singh
India
IT and Environment
David Ompong
Darwin
IT and Environment
Australia
Darwin
P. Sermon
Australia
College of Engineering,
Design and Physical Sciences
Brunel University London
Uxbridge
UK
xx List of Contributors
Jyothis Thomas Jiandong Ye

Department of Engineering Physics School of Electronic Science and
École Polytechnique de Montréal Engineering
Canada Nanjing University
Nanjing
Gregory Triplett China
Department of Electrical and Computer
Engineering Lifeng Zhang
Virginia Commonwealth University School of Materials Science and
Richmond Engineering
USA Shaanxi University of Science and
Technology
Lijian Wang Xi’an, Shaanxi
School of Materials Science and China
Engineering
Shanghai Jiao Tong University Tong Zhang
Shanghai School of Electronic Science and
China Engineering
Southeast University
M.P. Worsley Nanjing, Jiangsu
Nanomaterials and Applications China
Laboratory
CEDPS, Bragg Building Xiaoyang Zhang
Brunel University School of Electronic Science and
Uxbridge Engineering
UK Southeast University
Nanjing, Jiangsu
Weiping Wu China
Shanghai Institute of Optics and Fine
Mechanics Binyuan Zhao
Chinese Academy of Sciences School of Materials Science and
Shanghai Engineering
China Shanghai Jiao Tong University
Shanghai
Yi Yang China
School of Electronic Science and
Engineering
Southeast University
Nanjing, Jiangsu
China
1
Graphene Oxide for Electronics

Fenghua Liu 1 , Lifeng Zhang 2 , Lijian Wang 3 , Binyuan Zhao 3 and Weiping Wu 1
1
Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai, China
2
School of Materials Science and Engineering, Shaanxi University of Science and Technology, Xi’an, Shaanxi, China
3
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, China
1.1 Introduction
Graphene, a single layer or a few layers of sp2 -hybridized graphitic carbon, has generated
much attention both in scientific and technological fields due to its unique physical and
chemical properties. As a conducting semimetal, graphene has attracted lots of inter-
ests for the research and applications of electronics. Mass preparation of graphene with
controllable size and economic cost is still a key challenge in its application to electronic
devices. Different synthesis methods of graphene leaded to its various properties. Since
the first successful preparation of graphene using the ‘scotch tape’ method, a series of
methods have been developed for the synthesis of graphene [1]. A significant proportion
of the graphene research has been realized by the graphene oxide (GO) and its reduced
form, the reduced graphene oxide (rGO) as the raw materials.
Graphite oxide is a compound of carbon (C), oxygen (O), and hydrogen (H), and has
been synthesized by Hummers’ method in 1958 [2], using the chemical reaction between
graphite, potassium permanganate (KMnO4 ), sodium nitrate (Na2 NO3 ), and sulfuric
acid (H2 SO4 ). The one-molecule-thick or few-layer version of the substance graphite
oxide is known as graphene oxide (GO). The GO is not conductive but can be reduced
by chemical reactions, thermal treatment, or many other methods, forming conduc-
tive rGO (Figure 1.1) [3]. So far, many methods have been well developed to synthesis
GO and rGO, including the chemical reduction, the microwave method, the plasma
method, the laser method, and the hydrothermal method. Other synthesis methods,
such as chemical vapour deposition (CVD) method, arc discharge method, ball milling
approach, solvent-assisted exfoliation, etc., were also devoted to develop high-quality
graphene, although these synthesis methods all have some trade-offs in terms of high
quality, high yield, and environmental friendliness.
Oxide Electronics, First Edition. Edited by Asim Ray.

© 2021 John Wiley & Sons Ltd. Published 2021 by John Wiley & Sons Ltd.
2 1 Graphene Oxide for Electronics
OH
CO
O
OH O
Oxiation Reduction O
HO OH O
OH O
C O
O
HO
Graphene Graphene Oxide (GO) Reduced Graphene Oxide (rGO)
Figure 1.1 The chemical structures of graphene, graphene oxide (GO), the reduced graphene oxide
(rGO) and the conversion of graphene into GO and rGO via oxidation/reduction reactions. Source:
Reprinted with permission from ref. [3] Copyright 2018, Springer Nature.
1.2 Synthesis and Characterizations of Graphene Oxide

1.2.1 Chemical Reduction of Graphene Oxide (GO)
Chemical reduction of graphene oxide (GO) is a common method to low-cost syn-
thesize graphene [4]. Exfoliation of GO to individual GO sheets (Figure 1.2) could be
chemically reduced to rGO, using, for instance, NaBH4 or hydrazine [5]. However, the
product has problems, such as aggregation and defects. Moreover, the generally used
reducing agents, such as hydrazine or NaBH4 , are toxic. However, it still remained a
great challenge to readily and efficiently synthesis of high-quality graphene with higher
conductivity and less defects. Recently, some emerging methods of producing graphene,
such as microwave method, plasma method, and laser method, have attracted a lot of
interest, which will be presented in the following sections.
1.2.2 Microwave Method

Microwave absorbs heat energy through the medium and conducts micro-gradient
heating from inside the material, which is considered as a unique method for material
4
Height (nm)
3
2
1
0
0.0 0.5 1.0 1.5 2.0
4
Height (nm)
3
2
1
0
0.0 0.5 1.0 1.5 2.0
4
Height (nm)
3
2
1
0
0.0 0.5 1.0 1.5 2.0
Distance (microns)
Figure 1.2 AFM image of exfoliated graphene oxide (GO) sheets with three height profiles acquired in
different locations. Source: Reprinted with permission from ref. [5] Copyright 2007 Elsevier Ltd.
1.2 Synthesis and Characterizations of Graphene Oxide 3
synthesis. The strong microwave absorption capability of graphene oxide (GO) can
quickly remove oxygen-containing functional groups and further exfoliates GO. This
feature has a fatal temptation for the preparation of high-quality and pollution-free
graphene. As early as in 2011, microwave method was employed by Zhu et al. to
exfoliate GO [6]. Through the subsequent activation of KOH, they prepared graphene
with a high specific surface area (SSA) value of 3100 m2 g−1 and a high conductivity of
500 S m−1 . Another example of utilization of microwaves is the exfoliation of graphite
in molecularly engineered ionic liquids [7]. It is supposed that the cation–𝜋 interactions
can improve the affinity of graphene surfaces. The as-exfoliated graphene exhibited a
high single-layer proportion. Besides, I D /I G value of 0.14 and C/O ratio of 30 are close
to the values of the graphite precursor, indicating the excellent structural integrity.
One of the challenges on producing GO and rGO is the use of the toxic chemicals,
such as sulfuric acid and hydrazine hydrate. Lots of methods have been developed
to synthesize rGO by green reduction methods, using hydroiodic acid (HI), citric
acid, plant extracts, phytochemicals, or alternatively by thermal heating in the inert
atmosphere. In 2016, Voiry et al. reported on the fabrication of high-quality graphene
through the microwave reduction of GO [8]. This result attracted much interest because
they used a conventional microwave oven operated at 1000 W to rapidly and efficiently
reduce GO nanosheets with ∼50 μm size (Figure 1.3a). The higher-power microwave
pulses locally and ultra-fast-heated GO up to several thousand degrees to thoroughly
eliminate the oxygen functional groups and reorder the graphene basal plane. The
XPS results (Figure 1.3b) suggest that microwave-reduced GO (MW-rGO) shows a
negligible in-plane oxygen concentrations of ∼4 at. %. This oxygen content is much
lower than the theoretical value of rGO annealed at 1500 K [9]. The Raman spectra
of MW-rGO and other compared samples are shown in Figure 1.3c. The as-prepared
MW-rGO exhibited highly ordered graphene–like Raman features with sharp and
symmetrical 2D and G peaks and a very low I D /I G ratio (<0.1). It is also found that
MW-rGO shows higher I 2D /I G ratios and larger graphene domain sizes as compared
with rGO and solution-exfoliated flakes (Figure 1.3d). Although microwave method
has potential advantages in the efficient preparation of high-quality graphene, it should
be noted that the yield is so low that scale-up fabrication of high-quality graphene
remains a great challenge.
1.2.3 Plasma Method
Plasma etching may not be able to precisely control the microstructure of the product
at the atomic level, and even may entail undefined structural disorders or defects of the
products. However, as a simple and efficient method, plasma etching still was widely
used for etching of carbon materials [10]. Graphene was once prepared by unzipping
of carbon nanotubes (CNTs) through plasma etching with poly(methyl methacrylate)
(PMMA) films [10]. Herein, PMMA protects CNTs as an etching mask during the etch-
ing process. The top side walls of CNTs were etched faster and removed by the plasma.
For 10 seconds of Agron (Ar) plasma etching, 20% of the starting CNTs were converted
into single- or few-layer graphene nanoribbons (GNRs) with ∼10–20 nm width and
2 nm height. Pang et al. reported on the patterned GN synthesized by means of an
oxygen-plasma etching approach from solution-processed GO films [11]. They used
low-cost aluminium as sacrificial metal and protective masks to remove the graphene
Graphite
Intensity (a.u.)
CVD graphene
MWrGO
rGO
–O
C–O C–sp2
C=O 3
GO C=O C–sp
60 μm 292 290 288 286 284 282

Binding energy (ev)
(a) (b)
2.0
CVD-graphene
CVD Graphene
1.5
Intensity (a.u.)
HOPG MWrGO
I2D/IG
Dispersed 1.0
MWrGO
rGO 0.5 Dispersed

graphene
HOPG
GO
GO
rGO
0.0
1250 1500 1750 2700 3000 10 100 1000
Raman shift (cm–1) La (nm)
(c) (d)
Figure 1.3 (a) SEM of GO nanosheets. (b) High-resolution XPS C1s spectra and (c) Raman spectra of
MW-rGO and other compared samples. (d) Evolution of the I2D /IG ratio versus the crystal size (La).
Source: Reprinted with permission from ref. [8] Copyright 2016 The American Association for the
Advancement of Science (AAAS).
regions not covered by the aluminium when the sample was exposed to oxygen plasma.
They argued that oxygen-plasma etching of graphene film with sacrificial aluminium
contact patterns is an effective method for accurately controlling the size of graphene
electrodes. Wang and coworkers reported the preparation of graphene from the GO
using a radio frequency (RF) dielectric barrier discharge plasma system with different
plasma gas, such as O2 , N2 , and CH4 [12].
1.2.4 Laser Method
The laser method for the fabrication of graphene has advantages over the conventional
methods requiring high synthesis temperature or tedious post-treatments. Laser tech-
nologies enabled the process to be simpler and more compatible. Although this tech-
nology still faces the problem of large-scale production, it has been demonstrated to
produce high-quality graphene. El-Kady et al. used a standard LightScribe DVD opti-
cal drive to carry out the direct laser reduction of GO films to GN with high electrical
conductivity (1738 S m−1 ) and SSA (1520 m2 g−1 ), which can be used directly as super-
capacitor electrodes without the binder or current collectors [13]. The LightScribe laser
1.3 Energy Harvest Applications of Graphene Oxide 5
Laser
LSG GO P-LIG-70
Pine
(b) (c)
Side view Side view 3.3A
1 μm 1 μm
(a) (d) (e)
te
bstra
SA su Etching Transfer
PET-P
Graphene / Cu G/PET-PSA Heating Pressure
MG-MSCs &
Micro-patterns MG films
Line-filter device
(f)
Figure 1.4 (a) Preparation illustration of LSG and SEM images of cross-section of the product. Source:
Reprinted with permission from ref. [13] Copyright 2012 The American Association for the
Advancement of Science (AAAS). Morphology characterizations of laser-induced graphene (LIG)
derived from pine: (b) SEM image of pristine pine, (c) SEM, (d) TEM and (e) high-resolution TEM images
of P-LIG-70. The scale bars are 500 μm, 500 μm, 20 nm, and 4 nm, respectively. Source: Reprinted with
permission from ref. [14] Copyright 2017 The Wiley-VCH. (f ) Schematic illustrating the preparation
process of solid-state flexible MG-MSCs. Source: Reprinted with permission from ref. [15] Copyright
2018 Wiley-VCH.
was able to simultaneously reduce and exfoliate the GO sheets to form an open network
of laser-scribed graphene (LSG) (Figure 1.4a). This network structure with open pores
integrates the positive in terms of preventing the agglomeration of graphene sheets and
facilitating the electrolyte accessibility to improve the ionic diffusion.
1.3 Energy Harvest Applications of Graphene Oxide

1.3.1 Solar Cells
The superior electronic and optical properties of graphene made it an ideal candidate
for various energy harvest device applications. Graphene and rGO could be used as the
I
3.0
Current density (mA/cm2)

1.5
(a)
0.0
Vacuum level
–1 –1.5
LUMO
–2
–3 Conduction band
Excited state S* –3.0
E(eV)
–4 HOMO
–5 Graphene Ground state S
0
–4.5
anode
–6 Valence band spiro- Au
dye
–7 OMeTAD cathod –0.2 0.0 0.2 0.4 0.6 0.8 1.0
TIO2 Voltage (V)
(b) (c)
Figure 1.5 Illustration and performance of solar cell based on graphene electrodes. (a) Illustration of
dye-sensitized solar cell using graphene film as electrode, the four layers from bottom to top are Au,
dye-sensitized heterojunction, compact TiO2 , and graphene film. (b) The energy level diagram of
graphene/TiO2 /dye/spiro-OMeTAD/Au device. (c) I-V curve of graphene-based cell (black) and the
FTO-based cell (grey), illuminated under AM solar light (1 sun). Source: Reprinted with permission from
ref. [16] Copyright 2008 The American Chemical Society.
transparent electrode, counter electrode, or interface layers in solar cell devices. Wang,
Zhi, and Müllen reported the ultra-thin transparent conductive electrode of rGO films
for the solid-state dye-sensitized solar cells (DSSC; Figure 1.5a). The GO produced by
the Hummers method were purified and dispersed in DI water, the 5–20-nm-thick GO
films were deposited on the substrate by dip coating followed by the thermal reduction.
The sheet resistance of the rGO was about 1.8 kΩ/sq, calculated conductivity was about
550 S cm−1 and a transparency of more than 70% over 1000–3000 nm. The work func-
tion of rGO is 4.42 eV (Figure 1.5b), close to the that of FTO electrode (4.4 eV). When
served as the anode, the graphene/TiO2 /dye/spiro-OMeTAD/Au DSSC device demon-
strated a short-circuit photocurrent density (I sc ) of 1.01 mA cm−2 with an open-circuit
voltage (V oc ) of 0.7 V. The calculated filling factor (FF) was 0.36 and the power conver-
sion efficiency was 0.26% (Figure 1.5c) [16].
Eda et al. reported the use of rGO thin films prepared by vacuum filtration and trans-
fer for the organic solar cells [17]. The GO dispersion was filtered through a 25-nm
pore-size mixed cellulose ester membrane, then the obtained films were transferred
onto the substrate and the ester membrane was then removed by acetone washes. The
GO was reduced by the hydrazine vapour and low temperature annealing at 200 ∘ C. The
sheet resistance of the rGO film was very high, about 70 kΩ/sq when the transmittance
of the film is approximately 65%. They successfully reduced the sheet resistance nearly
by a factor of 5 when by dipping in thionyl chloride (SOCl2 ) for 1 hour. The OPV devices
with the rGO films were very low, only about 0.1% due to the very large sheet resistance
(on the order of 105 ).
Wu et al. used the GO as the dual functional interface modifier for improving wetta-
bility and retarding recombination in indium tin oxide (ITO)/GO/CH3 NH3 PbI3-x Clx /
PCBM/ZnO/Al hybrid perovskite solar cells [18]. The GO serviced as the buffer
layer between the perovskite and 2,2′ ,7,7′ -tetrakis-(N,N-di-p-methoxyphenyl-amine)-

9,9′ -spirobifluorene (Spiro-MeOTAD) hole transport layer (HTL). The open-circuit
voltage (V OC ) and the fill factor (FF) improved and the average efficiency greatly
increased by 45.5%, from 10.0% to 14.5%. Wang et al. fabricated high efficiency (up
to 15.6%) solar cells with perovskite materials and the nanocomposites of solvent
exfoliated graphene and TiO2 using low temperature solution processes (no higher
than 150 ∘ C). The graphene nano flakes provide superior charge-collection in the
nanocomposites [19].
1.3.2 Solar Thermal Energy Harvest Devices

The broadband optical absorption properties and the high surface of rGO made
it an ideal candidate for the solar thermal energy harvest and solar thermal energy
ultilizations. Ito et al. reported the use of graphene grown by CVD for the solar absorber
and the heat localization material for steam generation [20], high-energy conversion
efficiency of 80% and fast water evaporation rate of 1.50 kg m−2 h−1 were achieved. Hu
et al. prepare rGO-CNT aerogels and demonstrate high efficiency (83%) solar steam
generation under one sun [20]. Liu et al. design and prepared the carbon–carbon
composite materials based on rGO and carbon cloth by electrochemistry reduction
of GO (Figure 1.6a) [21]. The rGO-carbon cloth has ultra-high solar absorption up
to 93–97%, thus a ultra-high evaporation rate 2.54 kg m−2 h−1 was achieved under
normal illumination of 1 kWm−2 . The conducting nature of the solar optical absorber
layer allows the use of low-voltage electricity as an additional energy input. The
flexible carbon compositing film could reach 389 ∘ C within 10 seconds at only 3.5 V
(Figure 1.6b,c). The electrically powered Joule heating boosted the steam generation
rate by order of magnitude, setting the record high value of the interfacial evaporation
and steam generation up to 45.87 kg m−2 h−1 .
Graphene oxide and rGO have also been used in other energy harvest devices, such
as thermal energy harvesting [22], the mechanical energy harvesting [23], the acoustic
energy [24] harvesting, and so on. Besides using graphene on its own, it can also be
composited or hybrid with other materials to enhance the performance of the energy
harvest devices.
1.4 Energy Storage Applications of Graphene Oxide

1.4.1 Supercapacitors
Since its first application in supercapacitors in 2008 [25], graphene with its high the-
oretical SSA (2630 m2 g−1 ), excellent electronic conductivity, high flexibility, and sur-
face functionalized diversity, is regarded as a potential candidate for both electrical
double-layer capacitance (EDLC) and pseudocapacitance-based supercapacitors. Ruoff
et al. prepared the activated graphene by simple activation with KOH of microwave
exfoliated GO (MEGO) [6]. The MEGO has ultra-high surface area up to 3100 m2 g−1 ,
containing micropores and mesopores with sizes distributed between ∼1 nm and 10 nm.
Supercapacitors based on the MEGO showed a high gravimetric capacitance of 166 F g−1
and an excellent energy density of ∼70 Wh kg−1 .
Although graphene showed excellent power density and cyclic stability, their specific
capacitances still have a large gap compared to the theoretical value of 550 F g−1 [20].
DC
source GO rGO
GO
+ –
E;ectrochemical
deposition Joule heating
Pt plate
Carbon
cloth GO
solution CC GO-CC rGO-CC
(a) (b)
V 210.0
Water vapor
rGO-CC
Porous paper
Polystyrene foam (d) (e)

115.0
Salt water
(c)
20.0
(f) (g)
Figure 1.6 The preparation of GO-CC and rGO-CC composites. (a) The electrochemical deposition of
graphene. (b) The schematic diagram of electrochemical deposition and joule heating process to
obtain rGO on carbon cloth samples. (c) The schematic diagram of rGO-CC composite heating
elements to generate water vapour with low voltage. (d–g) The photographs and infrared photos of
the rGO-CC (flat and bending). Source: Reprinted with permission from ref. [21] Copyright 2020 2020
WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
This is caused by intrinsic aggregation or re-stacking of graphene nanosheets (GNSs)

due to the strong van der Waals forces, resulting in a seriously reduced electrochemical
property. Nevertheless, this has not affected people’s enthusiasm for the application
of graphene in supercapacitors over the past decade. In this section, we will focus
on the following aspects: the emerging preparation methods for graphene, how to
tune the interlayer spacing of graphene to achieve better electrochemical properties,
three-dimensional (3D) porous graphene, and graphene aerogels.
It is generally considered that investigation of how ion transport through complex lay-
ered graphene-based membranes is difficult because of the random distribution of mul-
tiscale complex and imperfect nanoslits or nanochannels within the layered graphenes.
Using a layered graphene gel (LGG) as a target platform prepared following the previ-
ously reported ‘capillary compression’ method, Cheng et al. demonstrated the effects
of tuneable interlayer spacing on the transport properties of ions with experiment and
simulation [26]. The experimentally estimated interlayer spacing (dexp ) can be varied
in the region of below 10 nm (Figure 1.7a Top). Additionally, small angle neutron scat-
tering (SANS) measurement was carried out to probe the restack phenomenon in the
as-compressed LGG membranes (Figure 1.7a, bottom).
8
10
2.4
106
F
2.0
4 1.6
10 0 3 6
I (q) (a.u.)
d (nm)
102 dexp = 7.0 nm
dexp = 3.9 nm
0 dexp = 2.2 nm
10 dexp = 0.5 nm
0.001 0.01 0.1

q (Å–1)
(a) (c) (d)
L
d
(b)
(f)
(e) (g)
Figure 1.7 (a) Top: SEM images of the LGG membranes when compressed to 3.2 nm (left) and 0.5 nm
(right), respectively. Bottom: Smallangle neutron scattering (SANS) patterns of the membranes with
dexp of 3.9 nm (left) and 0.5 nm (right), respectively. (b) A schematic illustration of the formation of
nanoslits array. (c) Reduced 1D SANS data offset from the absolute intensity scale. The upper right
inset is the slope F as a function of dexp . Source: Reprinted with permission from ref. [26] Copyright
2016, The American Association for the Advancement of Science (AAAS). (d) Schematic diagram
illustrating the production of EGM-GO films. (e) Schematic illustration of the ASSC configuration and
digital photos of the solid-state electrolyte, the flexible ASSC, and the ASSC under various bending
angles. (f ) Cross-sectional SEM images of rGO film and (g) EGM-rGO (50% EG) film. Scale bars, 2 μm.
Source: Reprinted with permission from ref. [27] Copyright 2020, Nature Publishing Group.
In order to establish a quantitative relationship among the nanoconfined ion transport

properties in relation to the complex nanoporous structure of the layered membrane,
they constructed a representative structural model to describe the fluidic contours con-
tained in the LGG membranes (Figure 1.7b), in which the height of nanoslits (d), the lat-
eral size of individual nanosheets (L), and the gap distance between the ends of the sheets
(𝛿) are the key geometrical variables of the proposed structural model. The reduced 1D
SANS curves in Figure 1.7c further confirmed that the nanospace and the porous struc-
ture in the LGG membranes remains largely continuous. These results revealed new
insights into the ion transport phenomena confined in a graphene nanochannel and
provided a solid foundation for the application of GNSs in supercapacitors.
Recently, Li et al. prepared a freestanding graphene laminate film electrode with highly
efficient pore utilization for compact capacitive energy storage [27]. The enhancement
of pore utilization was achieved by precisely adjusting the interlayer spacing of this film
through simply changing the ratio of two precursors, graphene oxide (GO) and exfoli-
ated graphene (EG) (Figure 1.7d). Figure 1.7f,g showed the cross-sectional SEM images
of rGO film and EGM-rGO (50% EG) film, respectively. This simultaneously freestand-
ing, dense yet porous electrode optimized the trade-off between gravimetric capaci-
tance (C wt ) and bulk density (𝜌), consequently delivery a high C ssa of 47 μF cm−2 and an
excellent Evol–stack of 88.1 Wh L−1 in an ionic liquid electrolyte. Furthermore, Figure 1.7e
showed that flexible all-solid-state supercapacitor (ASSC) with multiple optional out-
puts and superior stability was assembled by the as-synthesized graphene laminate film
electrode, demonstrating great potential as the power supply in practical applications.
Wang and coworkers prepared graphene by processing GO in different gas plasma,
such as O2 , N2 , and CH4 [12]. They compared the morphology and microstructure of dif-
ferent samples and evaluated their electrochemical properties as symmetrical electrode
of EDLCs. As displayed in Figure 1.8a, the treated GO-CH4 sample exhibited ultra-thin
and flat GNSs, which is similar to other samples synthesized by different plasma gas.
All plasma etching samples shown analogous XRD patterns with a broad peak at ∼24∘
corresponding to graphitic (002) plane (Figure 1.8b), indicating that the pristine GO
was successfully exfoliated into disordered and loosely packed graphene. Figure 1.8c
shows the CV curves of the electrodes at a scanning rate of 20 mV s−1 between the
potential of 0–1 V. All the typical and rectangular shape of CV curves indicate good
EDLCs behaviour. Electrochemical impedance spectroscopy (EIS) measurements were
conducted in the frequency range of 10–100 kHz. The Nyquist plots in Figure 1.8d dis-
play that the as-prepared three samples presented small resistances (6.6 Ω for GO-O2 ,
10.2 Ω for GO-N2 , 10.0 Ω for GO-CH4 ), which are beneficial to the high performance
EDLCs electrode material.
1.4.2 Batteries
Graphene and rGO could form stacked multilayer structures, which can host the ions,
making them be attractive and promising for battery applications. Yoo et al. used the
GNS materials prepared via the chemical reduction of exfoliated graphite oxide, as the
anode of lithium secondary batteries (LIB) [28]. The CNS has much larger specific capac-
ity of 540 mAh g−1 , much larger than that of the graphite anode (372 mAh g−1 ). They
successfully enhanced the specific capacity up to 730 and 784 mAh g−1 through control-
ling of the intergraphene sheet distance of between the GNSs, by hybriding fullerenes
(C60 ) molecules or CNT during the reduction of GO using hydrazine hydrate.
Similar to CNT and graphene, layers or nanotube of TMD materials have wide appli-
cation in batteries and supercapacitors due to their unique structure. Chen, Zhao, and
Wu et al. proposed and demonstrated a unique one-dimensional and two-dimensional
(1D + 2D) structure based on tungsten disulphide (WS2 ) nanotubes with rGO as the
anode for lithium-ion batteries (Figure 1.9a) [29]. The multilayer WS2 nanotube has
the coaxial multilayer structure and the hollow core, offering the space for the lithium
ion storage, but the material suffered from poor conductivity. By compositing with 2D
layered rGO, the electrical conductivity was significant enhanced. Figure 1.9b shows
the galvanostatic charge/discharge profiles of the WS2 -NTs/rGO composite anode in
the 1st, 2nd, 10th, and 50th at a current density of 0.1 A g−1 . The WS2 -NTs/rGO com-
posite anode demonstrated high initial capacity of 996.4 mAh g−1 and it maintained at
GO-CH4
Intensity / a.u.
GO-O2
GO-N2
1 μm GO
8 16 24 32 40
2 Theta / °
(a) (b)
60
Specific capacitance / F g–1
200
GO-N2
45 GO-O2
100 –Z'' / ohm GO-CH4
GO-N2
GO-O2
0 30
GO-CH4
–100
15
–200
0
0.00 0.25 0.50 0.75 1.00 0 15 30 45 60
Potential / V Z' / ohm
(c) (d)
Figure 1.8 (a) TEM image of GO-CH4. (b) XRD patterns of GO and other compared samples processed
by different gas plasma. (c) CV curves and (d) Nyquist plots of three samples using different plasma
gases O2 , N2 , and CH4 . Source: Reprinted with permission from ref. [12] Copyright 2017 Elsevier.
318.6 mA g−1 over 500 cycles at a current density of 1 A g−1 . The batteries based on the
WS2 -NTs/rGO composite anode also showed excellent rate performances (Figure 1.9c).
Composite materials such as graphene oxide/Fe2 O3 [30], Si nanoparticle/rGO [31],
SnS2 -rGO [32] demonstrated excellent performances when served as the anode for
lithium-ion batteries. The introduction of inorganic materials significantly booted the
discharge and charge capacities (over 1000 mAh g−1 ) with good cycling performance
and rate capability.
Lithium-sulphur batteries are one of the most promising battery technologies towards
commercialization. However, this battery experiment suffered from a few issues, includ-
ing rapid capacity degradation, short life span, low efficiency, and safety concerns. Wang
et al. prepared the amino-functionalized rGO [33] used is for the lithium-sulphur batter-
ies. The covalent chemical bond in the functionalized GO strongly stabilized the sulphur
and its discharge products, thus a stable capacity retention of 80% for 350 cycles with
high capacities and excellent high-rate response up to 4C were achieved. Huang et al.
used ultra-thin graphene oxide (GO) membrane to stabilize the lithium− sulfur batter-
ies [34], by using the oxygen electronegative atoms carboxyl groups in the GO as the
ion-hopping sites. The cyclic capacity decay rate was successfully reduced from 0.49%
per cycle to 0.23% per cycle.
Mixing Hydrothermal
reaction
WS2-NTs Graphene oxide WS2-NT/GS
(a)
3.0 3.0
1200 3.0
WS2-NTs WS2-NT/GS composite
2.5 2.5
Voltage vs. Li / Li / V
WS2-NTs/GS
2.5
Voltage vs. Li+ / Li / V
2.0 2.0
WS2-NTs
1000
Capacity (mAh g–1)

+
Current Density:100 mA g–1

1.5 1.5 1, 0.5, 0.2, 0.1 Ag–1
50th,10th,2nd,1st
1.0
2.0 1.0
0.5
0.5
800 0.0
0.0 0.1 Ag–1 0 200 400 600 800
1.5 0 200 400 600
Sepecific Capacity (mAh g–1)
800
Sepecific Capacity (mAh g1)
0.2 Ag–1
600 0.5 Ag–1
1.0 50th,10th,2nd,1st 0.1 Ag–1
1 Ag–1
WS2-NTs/GS composite
Current Density:100 mA g–1 400
0.5
0.0 200
0 250 500 750 1000 1250 0 10 20 30 40 50
Sepecific capacity (mAh g–1) Cycle Number
(b) (c)
Figure 1.9 (a) Schematic illustration of the fabrication of 1D + 2D hierarchically structure WS2 -NT/GS
composite.; (b) Discharge/charge voltage profiles of WS2 -NTs/GS composite and WS2 -NTs (inset)
anode at a current density of 100 mA/g; (c) rate capabilities of WS2 -NTs/GS composite and WS2 -NTs
anode, inset: discharge/charge voltage profiles of WS2 -NTs/GS composite at current density of 0.1, 0.2,
0.5, 1 A g−1 . Source: Reprinted with permission from ref. [29] Copyright 2014 The American Chemical
Society.
1.5 Electronic Device Applications of Graphene Oxide

Chemical reduction of graphene oxide (GO), the RGO films reduced by hydrazine solu-
tion have been reported to have a sheet resistance of 103 − 106 Ω/sq [35], which contain
numerous lattice defects and spatial interruptions from various oxygen groups. Besides,
the GO flakes usually need the addition of reducing agents, such as toxic hydrazine to
reduce GO; this method is limited by its low efficiency and relatedly low conductiv-
ity (on the order of 102 S/m) and high sheet resistance [5]. Furthermore, the graphitic
structure cannot be entirely restored after reduction [36], thus the conductivity of RGO
samples cannot match with that of the ‘perfect’ graphene and are highly dependent on
the reduction level. Some groups reported the preparation of graphene/metal nanocom-
posites makes use of GO as the starting materials, to anchor the metallic nanoparticles
(NPs) to the graphene [37].
Since the report on the electric field effect in atomically thin carbon film graphene [1],
graphene has attracted a huge amount of interest when applying it in electronics devices
[7], especially field-effect transistors (FETs) [38]. One of the advantages of using GO
and rGO for electronic devices is that it could be processed using solution or printing
methods. Although graphene oxide demonstrates the field-effect characteristics even

without reduction [39], it is not an ideal material as the active layer of the FET devices,
but could be used as electrodes, or interface layers used to fabricate sensor devices. Lee
et al. used the highly reduced graphene oxide (HRG) as the interfacial material between
gold source/drain contacts and pentacene in TFT devices. The HRG successfully
improved the electrical characteristics and higher effective carrier mobility due to
better charge injection and lower losses at the interface. Graphene oxide has been also
utilized in other electronic devices, such as photosensitive resistors, memories, and
photodetectors.
1.6 Large Area Electronics Applications of Graphene Oxide

The outstanding electrical conductivity, high optical transmittance, and the mechanical
flexibility of graphene made graphene an ideal material for the transparent conductors
(TCs). Based on the basis of the experimental mobility data, monolayer graphene with
a transmittance (T%) of 97.7% [40] will have a theoretical minimum sheet resistance of
∼30 Ω/sq at a carrier density of 1012 cm−2 [41]. Sukanta et al. calculated the fundamental
limitations on the sheet resistance and transmittance of thin graphene films [42], show
that four randomly stacked graphene layers can display T approximate to 90% and
10 Ω/sq if the product of carrier density and mobility reaches nμ = 1.3 × 1017 V−1 s−1 .
For TC applications where cost and environmental robustness are paramount, the
compelling combination of outstanding properties puts graphene in a truly unique
category for applications that require stretchability or flexibility [43]. In particular,
graphene’s mechanical strength and flexibility [44] are advantageous compared to
ITO, which is expensive and brittle. The graphene-based transparent conductive films
were demonstrated a few years ago [45]. Several demonstrations have been made
of graphene TC films and devices employing graphene TCs. Recent reports suggest
that graphene synthesized via CVD with Ni or copper (Cu) are promising candidates
for transparent conducting technologies [46]. More recently, a method to synthesize
ultra-large-scale (∼30 in.) graphene films with a sheet resistance and transparency of
30 Ω/sq at 90% for a doped four-layer graphene film [47], using roll-to-roll transfer
and chemical doping processes, was developed that shows excellent electrical and
physical properties suitable for practical applications on a large scale. The transfer of
CVD growth process, however, requires CVD growth of graphene on a copper foil,
and still has some unsolved issues such as high cost (high temperature, expensive
foils, or substrates) and environment-unfriendly (need to recycle Cu or Ni). Also, it
is a multistep time-consuming process in which graphene film must be etched and
transferred to a flexible substrate and must be repeated several times to achieve such a
low sheet resistance.
The major challenge in CVD driven graphene films is that the non-uniformity in thick-
ness, which usually results in the uniformity of surface roughness and sheet resistance
for multilayer graphene stacks [48]. The poor surface adhesion of graphene to substrate
is still a major concern. To further envision graphene TC technology, it will clearly
be necessary to deposit large area homogeneous graphene films using low tempera-
ture, cost effectively, single/direct step, and environmentally friendly solution processes.
Numerous techniques for the solution deposition of graphene thin films onto transpar-
ent substrates have been demonstrated, for example, spin coating, vacuum filtration,
Langmuir–Blodgett method, and so on. In addition to differing manufacturing complex-
ity, these methods also vary in scalability, film-to-film consistency, and film properties.
Also, sheet resistance of graphene TC by solution process is higher by an order of mag-
nitude or more compared to CVD-grown films.
Liquid-phase exfoliation from natural crystalline graphite can also yield the graphene
in organic solvents with few defects [23]. Consequently, the conductivity of the graphene
films can reach a high value at the range of ∼1500–6500 S m−1 [49, 50]. Liquid-based sus-
pensions of graphene could be ideal for coatings because this would enable the relatively
low-cost methods of spin-coating [51], ink jet printing [52], and roll-to-roll process.
However, because of downstream processing, highly flammable and toxic organic sol-
vents are not desired, and as such, water is the preferred solvent. Aqueous dispersions
of pristine graphene could be prepared by sonicating graphite in the presence of surfac-
tants, such as sodium dodecyl benzene sulfonate (SDBS) [53] and sodium deoxy-cholate
(SDC) [54]. This method is best suited to the scalable production of composite materi-
als and films based on graphene. However, the standard recipes are only able to produce
pristine graphene flakes with no chemical functionalities, thus limiting the performance,
including the optical electrical properties for practical applications.
Graphene-based materials are strongly affected by the way the individual sheets
are stacked. Most of the previous transparent conductive graphene films have been
limited by a trade-off between the electrical conductivity and the optical transparency,
which are controlled by the thickness of graphene in the film. Graphene/metal hybrid
is a novel class and form of graphene-based composite material. Wu et al. decorated
graphene flakes with metal nanoparticles (NPs) and effectively reduced the inter-sheet
resistance between the graphene sheets [55]. It is important to note that Au and Ag
could not be attached to graphene without functionalization. Acid treatment intro-
duces oxygen-containing chemical functional groups (such as −COOH, −OH, etc.)
and creates defects and brings chemically active sites in graphene (Figure 1.10a). This
also enables further functionalization via the initially added groups in the graphene
layers. Interestingly, silver or gold ions might become attached to carboxyl groups,
and thus the reduction takes place on the surface of the exfoliated sheets. The metal
nanoparticles (such as Au NPs and Ag NPs) decorated graphene flakes (Figure 1.10b)
showed significantly enhanced conductivity by forming the conducting points and
charge carrier bridges between the neighbouring sheets. The sheet resistance was
successfully reduced from 1 kΩ/sq to 50–100 Ω/sq at high optical transparency of
85–90% (Figure 1.10c,d). The low sheet resistance allows much more wider applications
of the graphene TCs and higher performance electronic devices, such as touch sensors,
smart windows, displays, imaging sensors, robotic hands, and so on.
Tian et al. demonstrated a novel macroscopic flexible force sensitive capacitive touch
pad by sandwiching the GO films between two layers of Teflon tape (Figure 1.11a,b)
[56]. The use of graphene and flexible Teflon allows the bending operation of the touch
sensor, the device has a notable electrical response of >5 V for 5 Hz touch frequency on
a 2-mm radius of curvature (5% stain, Figure 1.11c). The response time is about 2 ms,
in the same range of the graphene-based touch pad or rGO-based touch pad (2–3 ms).
The on/off ratio is about 60 when there no stain and had some reduction upon the stain.
HNO3 AuCl–4
(a)
85
Transmittance (%)
80
75
Pristine Graphene
70 HNO3 functionalized
Graphene/AuNPs
0.2 μm
100 1000 10000 100000
Sheet Resistance (Ω / sq)
(b) (c) (d)
Figure 1.10 (a) The synthesis of oxygen functionalized graphene and the metal nanoparticle
decorated graphene. (b) The TEM images of the graphene flakes decorated by Au nanoparticles
(AuNPs). (c) an A4-size graphene transparent conductor (TC) on the flexible PET substrate by rod
coating (a roll-to-roll process). (d) The sheet resistance and optical transmittance of the graphene TC
samples produced from the pristine graphene, the nitric acid functionalized graphene and the AuNPs
decorated graphene [55].
Al membrane
Teflon tape GO touch pad 60
20 R
On/OFF Ration
Go film 50
Voltage (V)
Teflon tape 10
40
ITD film
0 30
PET substrate
–10 20
on 2mm radius of curvature 10
–20 5% strain
(a) 0
–0.6 –0.4 –0.2 0.0 0.2 0.4 0.6 0% 1.0% 2.5% 5.0%
Coat with Coat with Coat with Time (s) Bending strain
GO film Tellon tape membrane
(c) (d)
PET/ITO/Teflon tape
subtrate (b)
Figure 1.11 Schematic view of the flexible capacitive touch pad based on graphene oxide (GO) film.
(a) Schematic structure of the GO-based touch pad. The left inset shows the whole device curved on a
peeler. The right inset shows the flexibility of the whole device in hand. (b) Main process flow of the
GO-based touch pad. The as-prepared GO film is fixed on a PET/ITO/Teflon tape substrate. Another
layer of Teflon tape is deposited above the film. Finally, an aluminium membrane is installed above the
film. (c) The measured electrical response for 5 Hz touch frequency on a 2-mm radius of curvature. (f )
The plot of bending strain vs. ON/OFF ratio. It shows the ratio has an inverse relation with the bending
strain, which indicates that the bending strain could be estimated by the ON/OFF ratio. Source:
Reprinted with permission from ref. [56]. Copyright 2012 The Royal Society of Chemistry.
The on/off ratio decrease slightly upon 1% stain, reduced to 35 when the stain is 2.5%,
but could be kept higher than 20 when the strain was 5% (Figure 1.11d).
Graphene derived from graphene oxide finds many other applications for electronics,
such as sensors, heaters, electromagnetic shielding, and RF devices. To fully achieve
its potential, preparations of higher quality samples plays the most important role,
towards graphene with better electrical conductivity, higher stability, and uniformity of
graphene films. Low cost, proper processing methods will be also important to pattern
the graphene, or stacking the layered graphene towards multilayers, or compositing
with other materials for multifunctional purposes.
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21
Flexible and Wearable Graphene-Based E-Textiles

Nazmul Karim 1 , Shaila Afroj 1 , Damien Leech 1 and Amr M. Abdelkader 2
1
Centre for Fine Print Research, The University of West of England, Bristol, UK
2
Department of Design and Engineering, Bournemouth University, Dorset, UK
2.1 Introduction to Wearable E-Textiles

Wearable electronic textiles (e-textiles) are perceived as a way to add features into
commonly used textiles, such as radio frequency identification (RFIDs), electrocardiog-
raphy (ECG), electromyography (EMG) sensors, energy harvesting devices, field-effect
transistors, antennas, touch sensitive buttons, pressure sensors, and mobility assistive
devices [1–4]. In recent years, wearable e-textiles have seen an exponential growth,
especially in the field of health care, military uniforms, sportswear, space exploration,
and gaming. Wearable e-textiles are becoming increasingly popular, due to their
ability to make human life safer, healthier, and more comfortable. Such technologies
enabled the manufacturing of truly multifunctional, highly innovative, and intelligent
textiles that can perform as a sensor, actuator, power generator, and energy storage
device all at the same time [5]. This could potentially provide a personalized wearable
garment that can interface with the human body and continuously monitor, collect,
and communicate various physiological parameters, such as temperature, humidity,
heart rate, and activity monitoring [6].
The concept of wearable electronics was introduced by mathematician Edward O.
Thorp and Claude Shannon in 1961. However, research on wearable e-textiles remained
merely a part of hobby electronics until the mid-1990s. During this early stage, the
wearable electronics were created by assembling the electronic equipment in a back-
pack or a small bag. These were heavy, stiff, and uncomfortable, rather than becoming
an integrated part of the clothing. More garment-like wearable electronics started to
appear with the introduction of conducting yarns. Such conductive yarns are mainly
the intertwining of copper, gold, or stainless-steel threads with other textile fibres, in
order to provide electrical conductance to the yarn. The conductive yarns are then inte-
grated into a garment by embroidery, sewing, knitting, weaving, or braiding techniques
to produce wearable e-textiles. Additionally, conductive gripper snaps, Velcro, or but-
tons are used for temporary and removable connections on cloths. Wearable electronics
became more flexible and comfortable to wear as various coating or printing processes
Oxide Electronics, First Edition. Edited by Asim Ray.

© 2021 John Wiley & Sons Ltd. Published 2021 by John Wiley & Sons Ltd.
22 2 Flexible and Wearable Graphene-Based E-Textiles
such as sputtering, conductive polymer coating, chemical vapour deposition, screen

printing, and inkjet printing of conductive inks were introduced. Such conductive inks
contain a range of conductive materials such as metal particles, organometallic com-
ponent, or conductive polymers; however, the majority of commercial conductive inks
are based on metal inks. The demand for such textiles has been growing rapidly with an
estimated market size of USD 5Bn by 2027 [7]. However, there are a number of chal-
lenges that need to be overcome in order to meet growing need including the complex
and time-consuming manufacturing processes, and the use of expensive, toxic, non-
biodegradable, and unstable metallic conductive materials.
Graphene, a two-dimensional single atom thick allotrope of sp2 hybridized carbon
atoms in a honeycomb lattice, has opened a wide range of wearable electronics
applications due to its outstanding electrical [8], mechanical [9, 10], and thermal [11]
properties. Reduced graphene oxide (rGO), a form of graphene, has shown promise for
wearable e-textiles applications due to (i) the scalable synthesis process of its precursor,
graphene oxide (GO), (ii) facile fabrication of rGO-based textiles via existing textiles
dyeing, coating, and printing process, and (iii) flexible and washable e-textiles via suit-
able bonding with textiles fibres. In this chapter, we explore fabrication and applications
of graphene-based wearable electronics, with a focus on rGO-based e-textiles.
2.2 Synthesis of Graphene Derivatives

The unique properties of graphene are mostly associated with the individual sheets.
Therefore, in order to maintain those properties, it is very important that a bulk amount
of graphene be produced in a processable form that does not agglomerate. However,
graphene sheets, unless physically well separated from each other, have a tendency to
agglomerate and even re-stack to form graphite through van der Waals interactions [12].
Graphene-based materials, such as GO and rGO, have shown commercial potential, as
they can be processed into a scalable quantity of stable dispersions [13, 14].
2.2.1 Graphene Oxide

GO is a single atom carbon layer with both surfaces modified by oxygen-containing
functional groups such as hydroxyl, carboxyl, epoxy, and others [15, 16] (Figure 2.1a).
Like graphene and other two-dimensional (2D) materials, it can have single, bi-, tri-,
and multi-layer forms [19], where the layers are separated by the functional groups
attached to each individual layer. GO has been a popular starting point in the early
years of large-scale graphene production, as it can form stable aqueous colloids
through a simple and cheap solution process. However, the properties of GO are far
from that of pristine graphene resulting in lower electrical conductivity and higher
chemical activity. The structure of graphene can partially be restored by reducing GO
to rGO (Figure 2.1b), which contains structural defects due to an incomplete reduction
process. Nevertheless, GO provides a flexible platform to tune the optical transparency,
electrical, and thermal conductance via controlled reduction to rGO and the addition
of various functional groups to its structure.
The synthesis of GO involves intercalation and oxidation of graphite powder. As
reviewed previously [20], the well-known methods for graphite oxide synthesis are
2.2 Synthesis of Graphene Derivatives 23
(a) CO2H (b)

CO2H
HO2C
CO2H
CO2H
CO2H
HO2C
HO2C
(c) C-O (d) C-C

C-C C-O
C=O
Intensity (a.u.)
282 284 286 288 290 292 Intensity (a.u.) 282 284 286 288 290 292
Binding Energy (eV) Binding Energy (eV)
(e) (f) D (g)
G
Intensity (a.u.)
rGo
Go
1200 1400 1600 1800 2000

Wavenumber (cm–1)
Figure 2.1 (a) The chemical structure of graphene oxide and (b) restoration of graphene structure
after reduction. Source: Modified from [17]. High-resolution C (1s) XPS spectrum of (c) GO and (d) rGO
[6]. Photographs of aqueous dispersion of graphene oxide (0.5 mg ml−1 ) (e) before and (g) after
reduction [18]. (f ) Raman spectra of GO and rGO shows characteristic peaks at ∼1344.78 and
1605.95 cm−1 corresponding to D and G bands. The intensity ratio of the D to G band (ID /IG ) is
increased after reduction, from ∼0.98 for GO to up to ∼1.75 for rGO [2].
Brodie method [21], Staudenmaier method [21], Hofmann method [22], and Hummers
method [23], and also their modified and improved forms. Such methods involve the
chemical reaction of graphite with acids (HCl, H2 SO4 , and HNO3 ), which is then
followed by intercalation of alkali metals (KClO3 , KMnO4 , NaNO3 , etc.) into the
graphitic layers to break them into small pieces. The Hummers-Offeman method uses
a mixture of concentrated H2 SO4 , NaNO3 , and KMnO4 or its modified or improved
methods [24], which are the most popular. Because of the slow kinetic of the chemical
intercalation process, an electrochemical oxidation alternative has been developed
[25]. In the electrochemical oxidation, a graphite anode is subjected to several oxide
anions that can intercalate between the graphene layers and lead to exfoliation. The
electrochemical parameters and the types of ions in the electrolyte control the oxidation
level of the graphene and the number of layers of the produced materials. In general,
24 2 Flexible and Wearable Graphene-Based E-Textiles
the anions can intercalate to few nanometres deep from the graphite grain surface,
leading to huge expansion and flakes peeling off the electrode before full oxidation or
exfoliation. Using a membrane to hold the physically detached flakes as part of the
anode increases the oxygen content to almost 34%, which is the typical value for GO
produced by the Hummer process, the most widely used GO synthesis process, due to
a high yield and low processing time.
2.2.2 Reduced Graphene Oxide
rGO has a graphene-like structure, and similar mechanical and electronic properties
to pristine graphene [26]. Though numerous efforts have been made to produce
pristine graphene-like materials via reduction of GO to rGO, only partial restoration
of graphene-like structure is possible with residual functional groups and structural
defects present [27]. However, the residual functional groups of rGO make it a desirable
material for washable and flexible wearable e-textiles applications [2, 6]. A wide range
of GO reduction methods have been reported, which could broadly be categorized into
three main processes: [15] physical (thermal), chemical, and in-situ reduction.
The thermal reduction is a relatively simple and a ‘green’ approach, and it is based
on heating the sample in an inert or reducing atmosphere at elevated temperatures.
The thermal gravimetric analysis of GO in nitrogen or Ar showed that most of the
oxygen functional groups on the surface are removed either by pyrolysis or by react-
ing with carbon from the basal plan to for carbon oxide gases. As a result, structural
damage was reported on the graphene sheets after the thermal treatments. Introduc-
ing reducing gas, such as hydrogen, improves the quality of the resulting graphene by
reducing the reaction with the carbon from the graphene sheets. In addition, the typical
temperature range for thermal reduction is between 400 and 1200 ∘ C, which makes it
difficult to apply in a liquid medium or in GO films on organic and most inorganic sub-
strates. For that reason, thermal reduction of GO prints or coatings on textile surfaces
is not suitable for wearable e-textiles applications, due to the structural degradation and
de-polymerization of textile fibres at higher temperatures [28, 29]. Furthermore, ther-
mal reduction requires specialist equipment and a particular environment to maintain
a higher temperature.
The chemical reduction of rGO is based on the chemical interaction between a reduc-
ing agent and the oxygen-containing groups of GO. The exact processes vary depending
on the reducing agent added; however, this process is, in general, cheaper than thermal
annealing due to the lessened need for specialist heating equipment, and often takes
place at temperatures around or just above room temperature. Hydrazine hydrate is
one of the most popular reducing agent for the chemical reduction of GO, however,
it is a toxic and potentially explosive material [30], and is therefore not considered to
be suitable for wearable e-textiles application. The well-known inorganic and organic
reducing agents that effectively restore GO to graphene include ascorbic acid (vita-
min C), phenyl hydrazine, sodium borohydride, glucose, hydroxylamine, hydroquinone,
pyrrole, amino acids, strongly alkaline solutions, and urea. Other wet chemical pro-
cess used a stronger reducing agent, such as metal powder, in HCl solutions and have
been reported to produce more conductive materials with a very low C/O ratio pro-
cedure [31–33]. Hybrid reduction methods that combine both thermal and chemical
reduction have been reported in the literature [34]. These methods are mimicking sim-
ilar technologies developed mainly for metal oxide reduction [35, 36]. The synergic of
2.3 Graphene-Based Wearable E-Textiles 25
strong reducing agents, such as Li or Na, with the high-temperature molten salts were
reported to remove most of the oxide groups, and even was able to recover some of pris-
tine graphene properties by healing the defects in GO [34]. Electrochemical reduction
in high-temperature molten salts allows the functionalization and doping of graphene
simultaneously with the reduction and produced materials with specific surface area as
high as 2800 m2 g−1 [37–39].
Although the reduction of GO is a popular approach, a major problem associated
with this route is that rGO aggregates in aqueous solution due to its hydrophobic
nature, especially in higher concentration. To prevent re-stacking of graphene flakes,
surface characteristics can be modified by adding the functionality to the surface
in an in-situ reduction process of GO in polymers. Such functional groups can be
added via either covalent bonding or noncovalent interactions [40, 41]. Covalent
bonds are usually achieved by atom doping or reaction with the residual functional
groups of graphene; whereas noncovalent bonds are generally formed by van der Waals
force, hydrogen bonding, electrostatic interaction, p–p stacking interactions, and
coordination bonds. When graphene’s unique electrical property and large surface area
are expected, the modification by forming noncovalent bonds is typically preferred.
They are comparatively weaker than covalent bonds but multiple noncovalent bonds
working in harmony can yield highly stable modifications. Moreover, these noncovalent
bonds are easy to achieve over the entire graphene surface. On the other hand, covalent
bonding is commonly preferred when stability and the strong mechanical properties of
modified graphene are required. In our studies we functionalized the rGO surface using
poly(styrenesulfonate) (PSS)/polyvinyl alcohol (PVA) during in-situ chemical reduction
with ascorbic acid and sodium hydrosulphite, which improved the dispersibility and
stability of the rGO in aqueous media polyvinyl alcohol (PVA). We then used those
dispersions to either coat or print textile yarns or fabrics for wearable e-textiles
applications [2, 4, 6] (Table 2.1).
2.3 Graphene-Based Wearable E-Textiles

Recently, wearable e-textiles have gained remarkable attention from scientists and
researchers due to their wide application scope in the field of sportswear, health
care, environmental monitoring, and military uniform. The current trend of wearable
electronics market is moving away from stitched electronics to full integration into the
garment, which is invisible or more comfortable to wear. There is a growing interest
into incorporating various electronic devices into textiles, such as RFID, sensors
(temperature, strain, humidity), ECG/EMG/Eye tracker, and energy storage devices
[48]. Graphene is a material that has the potential to create ‘disruptive technology’ with
its unique and outstanding properties and hence achieved remarkable attention from
both experimental and theoretical scientists. It is considered to be the most promising
material for next generation electronic applications due to its outstanding properties,
as mentioned in the earlier section. Graphene materials such as graphene, GO, or rGO
can be incorporated in or onto textiles via mainly three ways:
1) Spinning fibres or mixing with fibre polymers before spinning;
2) Coating textile yarn or fabrics;
3) Printing onto fabrics.
Among them, coating at the fabric stage is the most widely employed compared to the
other two methods, due to the ease of fabrication and scalability.
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Title: La Comédie humaine - Volume 14

Études philosophiques
Author: Honoré de Balzac
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Language: French
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*** START OF THE PROJECT GUTENBERG EBOOK LA COMÉDIE

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Au lecteur
Table
ŒUVRES COMPLÈTES
DE
H. DE BALZAC
LA
COMÉDIE HUMAINE
QUATORZIÈME VOLUME
DEUXIÈME PARTIE
ÉTUDES PHILOSOPHIQUES
PARIS.—IMPRIMERIE DE PILLET FILS AINÉ
RUE DES GRANDS-AUGUSTINS, 5.
IMP. S RAÇON
LE MARCHAND DE CURIOSITÉS.
Une barbe grise et taillée en pointe
cachait le menton de cet être bizarre.
(LA PEAU DE CHAGRIN.)
ÉTUDES
PHILOSOPHIQUES
TOME I
La Peau de chagrin
Jésus-Christ en Flandre. — Melmoth réconcilié. — Le Chef-
d’œuvre inconnu. — La Recherche de l’absolu.
PARIS
V e AL E XA NDRE HO USSIAUX, ÉD IT EUR
RUE DU JARDINET SAINT-ANDRÉ DES ARTS, 3.
1870
ÉTUDES
P H I L OS OP H I QU E S.
LA PEAU DE CHAGRIN.
A MONSIEUR SAVARY,
MEMBRE DE L’ACADÉMIE DES SCIENCES.
Sterne (Tristram Shandy, ch. CCCXXII.)
LE TALISMAN.
Vers la fin du mois d’octobre dernier, un jeune homme entra dans

le Palais-Royal au moment où les maisons de jeu s’ouvraient,
conformément à la loi qui protége une passion essentiellement
imposable. Sans trop hésiter, il monta l’escalier du tripot désigné
sous le nom de numéro 36.
—Monsieur, votre chapeau, s’il vous plaît? lui cria d’une voix
sèche et grondeuse un petit vieillard blême, accroupi dans l’ombre,
protégé par une barricade, et qui se leva soudain en montrant une
figure moulée sur un type ignoble.
Quand vous entrez dans une maison de jeu, la loi commence par
vous dépouiller de votre chapeau. Est-ce une parabole évangélique
et providentielle? N’est-ce pas plutôt une manière de conclure un
contrat infernal avec vous en exigeant je ne sais quel gage? Serait-
ce pour vous obliger à garder un maintien respectueux devant ceux
qui vont gagner votre argent? Est-ce la police tapie dans tous les
égouts sociaux qui tient à savoir le nom de votre chapelier ou le
vôtre, si vous l’avez inscrit sur la coiffe? Est-ce enfin pour prendre la
mesure de votre crâne et dresser une statistique instructive sur la
capacité cérébrale des joueurs? Sur ce point l’administration garde
un silence complet. Mais, sachez-le bien, à peine avez-vous fait un
pas vers le tapis vert, déjà votre chapeau ne vous appartient pas
plus que vous ne vous appartenez à vous-même: vous êtes au jeu,
vous, votre fortune, votre coiffe, votre canne et votre manteau. A
votre sortie, le Jeu vous démontrera, par une atroce épigramme en
action, qu’il vous laisse encore quelque chose en vous rendant votre
bagage. Si toutefois vous avez une coiffure neuve, vous apprendrez
à vos dépens qu’il faut se faire un costume de joueur. L’étonnement
manifesté par l’étranger quand il reçut une fiche numérotée en
échange de son chapeau, dont heureusement les bords étaient
légèrement pelés, indiquait assez une âme encore innocente. Le
petit vieillard, qui sans doute avait croupi dès son jeune âge dans les
bouillants plaisirs de la vie des joueurs, lui jeta un coup d’œil terne et
sans chaleur, dans lequel un philosophe aurait vu les misères de
l’hôpital, les vagabondages des gens ruinés, les procès-verbaux
d’une foule d’asphyxies, les travaux forcés à perpétuité, les
expatriations au Guazacoalco. Cet homme, dont la longue face
blanche n’était plus nourrie que par les soupes gélatineuses de
d’Arcet, présentait la pâle image de la passion réduite à son terme le
plus simple. Dans ses rides il y avait trace de vieilles tortures, il
devait jouer ses maigres appointements le jour même où il les
recevait; semblable aux rosses sur qui les coups de fouet n’ont plus
de prise, rien ne le faisait tressaillir; les sourds gémissements des
joueurs qui sortaient ruinés, leurs muettes imprécations, leurs
regards hébétés, le trouvaient toujours insensible. C’était le Jeu
incarné. Si le jeune homme avait contemplé ce triste Cerbère, peut-
être se serait-il dit: Il n’y a plus qu’un jeu de cartes dans ce cœur-là!
L’inconnu n’écouta pas ce conseil vivant, placé là sans doute par la
Providence, comme elle a mis le dégoût à la porte de tous les
mauvais lieux; il entra résolument dans la salle où le son de l’or
exerçait une éblouissante fascination sur les sens en pleine
convoitise. Ce jeune homme était probablement poussé là par la
plus logique de toutes les éloquentes phrases de J.-J. Rousseau, et
dont voici, je crois, la triste pensée: Oui, je conçois qu’un homme
aille au Jeu; mais c’est lorsque entre lui et la mort il ne voit plus que
son dernier écu.
Le soir, les maisons de jeu n’ont qu’une poésie vulgaire, mais
dont l’effet est assuré comme celui d’un drame sanguinolent. Les
salles sont garnies de spectateurs et de joueurs, de vieillards
indigents qui s’y traînent pour s’y réchauffer, de faces agitées,
d’orgies commencées dans le vin et prêtes à finir dans la Seine; la
passion y abonde, mais le trop grand nombre d’acteurs vous
empêche de contempler face à face le démon du jeu. La soirée est
un véritable morceau d’ensemble où la troupe entière crie, où
chaque instrument de l’orchestre module sa phrase. Vous verriez là
beaucoup de gens honorables qui viennent y chercher des
distractions et les payent comme ils payeraient le plaisir du
spectacle, de la gourmandise, ou comme ils iraient dans une
mansarde acheter à bas prix de cuisants regrets pour trois mois.
Mais comprenez-vous tout ce que doit avoir de délire et de vigueur
dans l’âme un homme qui attend avec impatience l’ouverture d’un
tripot? Entre le joueur du matin et le joueur du soir il existe la
différence qui distingue le mari nonchalant de l’amant pâmé sous les
fenêtres de sa belle. Le matin seulement arrivent la passion
palpitante et le besoin dans sa franche horreur. En ce moment vous
pourrez admirer un véritable joueur, un joueur qui n’a pas mangé,
dormi, vécu, pensé, tant il était rudement flagellé par le fouet de sa
martingale; tant il souffrait travaillé par le prurit d’un coup de trente et
quarante. A cette heure maudite, vous rencontrerez des yeux dont le
calme effraie, des visages qui vous fascinent, des regards qui
soulèvent les cartes et les dévorent. Aussi les maisons de jeu ne
sont-elles sublimes qu’à l’ouverture de leurs séances. Si l’Espagne a
ses combats de taureaux, si Rome a eu ses gladiateurs, Paris
s’enorgueillit de son Palais-Royal, dont les agaçantes roulettes
donnent le plaisir de voir couler le sang à flots, sans que les pieds du
parterre risquent d’y glisser. Essayez de jeter un regard furtif sur
cette arène, entrez... Quelle nudité! Les murs, couverts d’un papier
gras à hauteur d’homme, n’offrent pas une seule image qui puisse
rafraîchir l’âme; il ne s’y trouve même pas un clou pour faciliter le
suicide. Le parquet est usé, malpropre. Une table oblongue occupe
le centre de la salle. La simplicité des chaises de paille pressées
autour de ce tapis usé par l’or annonce une curieuse indifférence du
luxe chez ces hommes qui viennent périr là pour la fortune et pour le
luxe. Cette antithèse humaine se découvre partout où l’âme réagit
puissamment sur elle-même. L’amoureux veut mettre sa maîtresse
dans la soie, la revêtir d’un moelleux tissu d’Orient, et la plupart du
temps il la possède sur un grabat. L’ambitieux se rêve au faîte du
pouvoir, tout en s’aplatissant dans la boue du servilisme. Le
marchand végète au fond d’une boutique humide et malsaine, en
élevant un vaste hôtel, d’où son fils, héritier précoce, sera chassé
par une licitation fraternelle. Enfin, existe-t-il chose plus déplaisante
qu’une maison de plaisir? Singulier problème! Toujours en opposition
avec lui-même, trompant ses espérances par ses maux présents, et
ses maux par un avenir qui ne lui appartient pas, l’homme imprime à
tous ses actes le caractère de l’inconséquence et de la faiblesse. Ici-
bas rien n’est complet que le malheur. Au moment où le jeune
homme entra dans le salon, quelques joueurs s’y trouvaient déjà.
Trois vieillards à têtes chauves étaient nonchalamment assis autour
du tapis vert; leurs visages de plâtre, impassibles comme ceux des
diplomates, révélaient des âmes blasées, des cœurs qui depuis
long-temps avaient désappris de palpiter, même en risquant les
biens paraphernaux d’une femme. Un jeune Italien aux cheveux
noirs, au teint olivâtre, était accoudé tranquillement au bout de la
table, et paraissait écouter ces pressentiments secrets qui crient
fatalement à un joueur:—Oui.—Non! Cette tête méridionale respirait
l’or et le feu. Sept ou huit spectateurs, debout, rangés de manière à
former une galerie, attendaient les scènes que leur préparaient les
coups du sort, les figures des acteurs, le mouvement de l’argent et
celui des râteaux. Ces désœuvrés étaient là, silencieux, immobiles,
attentifs comme l’est le peuple à la Grève quand le bourreau tranche
une tête. Un grand homme sec, en habit râpé, tenait un registre
d’une main, et de l’autre une épingle pour marquer les passes de la
Rouge ou de la Noire. C’était un de ces Tantales modernes qui
vivent en marge de toutes les jouissances de leur siècle, un de ces
avares sans trésor qui jouent une mise imaginaire; espèce de fou
raisonnable qui se consolait de ses misères en caressant une
chimère, qui agissait enfin avec le vice et le danger comme les
jeunes prêtres avec l’Eucharistie, quand ils disent des messes
blanches. En face de la banque, un ou deux de ces fins
spéculateurs, experts des chances du jeu, et semblables à d’anciens
forçats qui ne s’effraient plus des galères, étaient venus là pour
hasarder trois coups et remporter immédiatement le gain probable
duquel ils vivaient. Deux vieux garçons de salle se promenaient
nonchalamment les bras croisés, et de temps en temps regardaient
le jardin par les fenêtres, comme pour montrer aux passants leurs
plates figures, en guise d’enseigne. Le tailleur et le banquier
venaient de jeter sur les ponteurs ce regard blême qui les tue, et
disaient d’une voix grêle:—Faites le jeu! quand le jeune homme
ouvrit la porte. Le silence devint en quelque sorte plus profond, et les
têtes se tournèrent vers le nouveau venu par curiosité. Chose
inouïe! les vieillards émoussés, les employés pétrifiés, les
spectateurs, et jusqu’au fanatique Italien, tout en voyant l’inconnu
éprouvèrent je ne sais quel sentiment épouvantable. Ne faut-il pas
être bien malheureux pour obtenir de la pitié, bien faible pour exciter
une sympathie, ou d’un bien sinistre aspect pour faire frissonner les
âmes dans cette salle où les douleurs doivent être muettes, la
misère gaie, le désespoir décent! Eh bien! il y avait de tout cela dans
la sensation neuve qui remua ces cœurs glacés quand le jeune
homme entra. Mais les bourreaux n’ont-ils pas quelquefois pleuré
sur les vierges dont les blondes têtes devaient être coupées à un
signal de la Révolution? Au premier coup d’œil les joueurs lurent sur
le visage du novice quelque horrible mystère: ses jeunes traits
étaient empreints d’une grâce nébuleuse, son regard attestait des
efforts trahis, mille espérances trompées! La morne impassibilité du
suicide donnait à son front une pâleur mate et maladive, un sourire
amer dessinait de légers plis dans les coins de sa bouche, et sa
physionomie exprimait une résignation qui faisait mal à voir. Quelque
secret génie scintillait au fond de ses yeux, voilés peut-être par les
fatigues du plaisir. Était-ce la débauche qui marquait de son sale
cachet cette noble figure jadis pure et brûlante, maintenant
dégradée? Les médecins auraient sans doute attribué à des lésions
au cœur ou à la poitrine le cercle jaune qui encadrait les paupières,
et la rougeur qui marquait les joues, tandis que les poètes eussent
voulu reconnaître à ces signes les ravages de la science, les traces
de nuits passées à la lueur d’une lampe studieuse. Mais une passion
plus mortelle que la maladie, une maladie plus impitoyable que
l’étude et le génie, altéraient cette jeune tête, contractaient ces
muscles vivaces, tordaient ce cœur qu’avaient seulement effleuré
les orgies, l’étude et la maladie. Comme, lorsqu’un célèbre criminel
arrive au bagne, les condamnés l’accueillent avec respect, ainsi tous
ces démons humains, experts en tortures, saluèrent une douleur
inouïe, une blessure profonde que sondait leur regard, et
reconnurent un de leurs princes à la majesté de sa muette ironie, à
l’élégante misère de ses vêtements. Le jeune homme avait bien un
frac de bon goût, mais la jonction de son gilet et de sa cravate était
trop savamment maintenue pour qu’on lui supposât du linge. Ses
mains, jolies comme des mains de femme, étaient d’une douteuse
propreté; enfin depuis deux jours il ne portait plus de gants! Si le
tailleur et les garçons de salle eux-mêmes frissonnèrent, c’est que
les enchantements de l’innocence florissaient par vestiges dans ses
formes grêles et fines, dans ses cheveux blonds et rares,
naturellement bouclés. Cette figure avait encore vingt-cinq ans, et le
vice paraissait n’y être qu’un accident. La verte vie de la jeunesse y
luttait encore avec les ravages d’une impuissante lubricité. Les
ténèbres et la lumière, le néant et l’existence s’y combattaient en
produisant tout à la fois de la grâce et de l’horreur. Le jeune homme
se présentait là comme un ange sans rayons, égaré dans sa route.
Aussi tous ces professeurs émérites de vice et d’infamie, semblables
à une vieille femme édentée, prise de pitié à l’aspect d’une belle fille
qui s’offre à la corruption, furent-ils prêts à crier au novice:—Sortez!
Celui-ci marcha droit à la table, s’y tint debout, jeta sans calcul sur le
tapis une pièce d’or qu’il avait à la main, et qui roula sur Noir; puis,
comme les âmes fortes, abhorrant de chicanières incertitudes, il
lança sur le tailleur un regard tout à la fois turbulent et calme.
L’intérêt de ce coup était si grand que les vieillards ne firent pas de
mise; mais l’Italien saisit avec le fanatisme de la passion une idée
qui vint lui sourire, et ponta sa masse d’or en opposition au jeu de
l’inconnu. Le banquier oublia de dire ces phrases qui se sont à la
longue converties en un cri rauque et inintelligible: Faites le jeu!—Le
jeu est fait!—Rien ne va plus. Le tailleur étala les cartes, et sembla
souhaiter bonne chance au dernier venu, indifférent qu’il était à la
perte ou au gain fait par les entrepreneurs de ces sombres plaisirs.
Chacun des spectateurs voulut voir un drame et la dernière scène
d’une noble vie dans le sort de cette pièce d’or; leurs yeux arrêtés
sur les cartons fatidiques étincelèrent; mais, malgré l’attention avec
laquelle ils regardèrent alternativement et le jeune homme et les
cartes, ils ne purent apercevoir aucun symptôme d’émotion sur sa
figure froide et résignée.
—Rouge, pair, passe, dit officiellement le tailleur.
Une espèce de râle sourd sortit de la poitrine de l’Italien lorsqu’il
vit tomber un à un les billets pliés que lui lança le banquier. Quant au
jeune homme, il ne comprit sa ruine qu’au moment où le râteau
s’allongea pour ramasser son dernier napoléon. L’ivoire fit rendre un
bruit sec à la pièce, qui, rapide comme une flèche, alla se réunir au
tas d’or étalé devant la caisse. L’inconnu ferma les yeux doucement,
ses lèvres blanchirent; mais il releva bientôt ses paupières, sa
bouche reprit une rougeur de corail, il affecta l’air d’un Anglais pour
qui la vie n’a plus de mystères, et disparut sans mendier une
consolation par un de ces regards déchirants que les joueurs au
désespoir lancent assez souvent sur la galerie. Combien
d’événements se pressent dans l’espace d’une seconde, et que de
choses dans un coup de dé!
—Voilà sans doute sa dernière cartouche, dit en souriant le
croupier après un moment de silence pendant lequel il tint cette
pièce d’or entre le pouce et l’index pour la montrer aux assistants.
—C’est un cerveau brûlé qui va se jeter à l’eau, répondit un
habitué en regardant autour de lui les joueurs qui se connaissaient
tous.
—Bah! s’écria le garçon de chambre, en prenant une prise de
tabac.
—Si nous avions imité monsieur? dit un des vieillards à ses
collègues en désignant l’Italien.
Tout le monde regarda l’heureux joueur dont les mains
tremblaient en comptant ses billets de banque.
—J’ai entendu, dit-il, une voix qui me criait dans l’oreille: Le Jeu
aura raison contre le désespoir de ce jeune homme.
—Ce n’est pas un joueur, reprit le banquier, autrement il aurait
groupé son argent en trois masses pour se donner plus de chances.
Le jeune homme passait sans réclamer son chapeau; mais le
vieux molosse, ayant remarqué le mauvais état de cette guenille, la
lui rendit sans proférer une parole; le joueur restitua la fiche par un
mouvement machinal, et descendit les escaliers en sifflant di tanti
palpiti d’un souffle si faible, qu’il en entendit à peine lui-même les
notes délicieuses. Il se trouva bientôt sous les galeries du Palais-
Royal, alla jusqu’à la rue Saint-Honoré, prit le chemin des Tuileries
et traversa le jardin d’un pas irrésolu. Il marchait comme au milieu
d’un désert, coudoyé par des hommes qu’il ne voyait pas, n’écoutant
à travers les clameurs populaires qu’une seule voix, celle de la mort;
enfin perdu dans une engourdissante méditation, semblable à celle
dont jadis étaient saisis les criminels qu’une charrette conduisait du
Palais à la Grève, vers cet échafaud, rouge de tout le sang versé
depuis 1793. Il existe je ne sais quoi de grand et d’épouvantable
dans le suicide. Les chutes d’une multitude de gens sont sans
danger, comme celles des enfants qui tombent de trop bas pour se
blesser; mais quand un grand homme se brise, il doit venir de bien
haut, s’être élevé jusqu’aux cieux, avoir entrevu quelque paradis
inaccessible. Implacables doivent être les ouragans qui le forcent à
demander la paix: de l’âme à la bouche d’un pistolet. Combien de
jeunes talents confinés dans une mansarde s’étiolent et périssent
faute d’un ami, faute d’une femme consolatrice, au sein d’un million
d’êtres, en présence d’une foule lassée d’or et qui s’ennuie. A cette
pensée, le suicide prend des proportions gigantesques. Entre une
mort volontaire et la féconde espérance dont la voix appelait un
jeune homme à Paris, Dieu seul sait combien se heurtent de
conceptions, de poésies abandonnées, de désespoirs et de cris
étouffés, de tentatives inutiles et de chefs-d’œuvre avortés. Chaque
suicide est un poème sublime de mélancolie. Où trouverez-vous,
dans l’océan des littératures, un livre surnageant qui puisse lutter de
génie avec ces lignes: Hier, à quatre heures, une jeune femme s’est
jetée dans la Seine du haut du Pont-des-Arts. Devant ce laconisme
parisien, les drames, les romans, tout pâlit, même ce vieux
frontispice: Les lamentations du glorieux roi de Kaërnavan, mis en
prison par ses enfants; dernier fragment d’un livre perdu, dont la
seule lecture faisait pleurer ce Sterne, qui lui-même délaissait sa
femme et ses enfants. L’inconnu fut assailli par mille pensées
semblables, qui passaient en lambeaux dans son âme, comme des
drapeaux déchirés voltigent au milieu d’une bataille. S’il déposait
pendant un moment le fardeau de son intelligence et de ses
souvenirs pour s’arrêter devant quelques fleurs dont les têtes étaient
mollement balancées par la brise parmi les massifs de verdure,
bientôt saisi par une convulsion de la vie qui regimbait encore sous
la pesante idée du suicide, il levait les yeux au ciel: là, des nuages
gris, des bouffées de vent chargées de tristesse, une atmosphère
lourde, lui conseillaient encore de mourir. Il s’achemina vers le pont
Royal en songeant aux dernières fantaisies de ses prédécesseurs. Il
souriait en se rappelant que lord Castelreagh avait satisfait le plus
humble de nos besoins avant de se couper la gorge, et que
l’académicien Auger avait été chercher sa tabatière pour priser tout
en marchant à la mort. Il analysait ces bizarreries et s’interrogeait lui-
même, quand, en se serrant contre le parapet du pont, pour laisser
passer un fort de la halle, celui-ci ayant légèrement blanchi la
manche de son habit, il se surprit à en secouer soigneusement la
poussière. Arrivé au point culminant de la voûte, il regarda l’eau d’un
air sinistre.—Mauvais temps pour se noyer, lui dit en riant une vieille
femme vêtue de haillons. Est-elle sale et froide, la Seine! Il répondit
par un sourire plein de naïveté qui attestait le délire de son courage,
mais il frissonna tout à coup en voyant de loin, sur le port des
Tuileries, la baraque surmontée d’un écriteau où ces paroles sont
tracées en lettres hautes d’un pied: SECOURS AUX ASPHYXIÉS. M.
Dacheux lui apparut armé de sa philanthropie, réveillant et faisant
mouvoir ces vertueux avirons qui cassent la tête aux noyés, quand
malheureusement ils remontent sur l’eau: il l’aperçut ameutant les
curieux, quêtant un médecin, apprêtant des fumigations; il lut les
doléances des journalistes, écrites entre les joies d’un festin et le
sourire d’une danseuse; il entendit sonner les écus comptés à des
bateliers pour sa tête par le préfet de la Seine. Mort, il valait
cinquante francs, mais vivant il n’était qu’un homme de talent sans
protecteurs, sans amis, sans paillasse, sans tambour, un véritable
zéro social, inutile à l’État, qui n’en avait aucun souci. Une mort en
plein jour lui parut ignoble, il résolut de mourir pendant la nuit, afin
de livrer un cadavre indéchiffrable à cette société qui méconnaissait
la grandeur de sa vie. Il continua donc son chemin, et se dirigea vers
le quai Voltaire, en prenant la démarche indolente d’un désœuvré
qui veut tuer le temps. Quand il descendit les marches qui terminent
le trottoir du pont, à l’angle du quai, son attention fut excitée par les
bouquins étalés sur le parapet; peu s’en fallut qu’il n’en marchandât
quelques-uns. Il se prit à sourire, remit philosophiquement les mains
dans ses goussets, et allait reprendre son allure d’insouciance où
perçait un froid dédain, quand il entendit avec surprise quelques
pièces retentir d’une manière véritablement fantastique au fond de
sa poche. Un sourire d’espérance illumina son visage, glissa de ses
lèvres sur ses traits, sur son front, fit briller de joie ses yeux et ses
joues sombres. Cette étincelle de bonheur ressemblait à ces feux
qui courent dans les vestiges d’un papier déjà consumé par la
flamme: mais le visage eut le sort des cendres noires; il redevint
triste quand l’inconnu, ayant vivement retiré la main de son gousset,
aperçut trois gros sous.
—Ah! mon bon monsieur, la carita! la carita! catarina! Un petit
sou pour avoir du pain! Un jeune ramoneur dont la figure bouffie était
noire, le corps brun de suie, les vêtements déguenillés, tendit la
main à cet homme pour lui arracher ses derniers sous. A deux pas
du petit Savoyard, un vieux pauvre honteux, maladif, souffreteux,
ignoblement vêtu d’une tapisserie trouée, lui dit d’une grosse voix
sourde:—Monsieur, donnez-moi ce que vous voulez, je prierai Dieu
pour vous... Mais quand l’homme jeune eut regardé le vieillard, celui-
ci se tut et ne demanda plus rien, reconnaissant peut-être sur ce
visage funèbre la livrée d’une misère plus âpre que n’était la sienne.
—La carita! la carita! L’inconnu jeta sa monnaie à l’enfant et au vieux
pauvre en quittant le trottoir pour aller vers les maisons, il ne pouvait
plus supporter le poignant aspect de la Seine.—Nous prierons Dieu
pour la conservation de vos jours, lui dirent les deux mendiants.

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Oxide Electronics 1st Edition Asim K.

Founding Series Editors

Limit of Liability/Disclaimer of Warranty

Library of Congress Cataloging-in-Publication Data

Names: Ray, Asim K., editor.

Cover Design: Wiley

Set in 10/12pt WarnockPro by SPi Global, Chennai, India

Series Preface xiii

1 Graphene Oxide for Electronics 1

2 Flexible and Wearable Graphene-Based E-Textiles 21

4 High-𝜿 Dielectric Oxides for Electronics 75

5 Low Temperature Growth of Germanium Oxide Nanowires by Template Based

6 Electronic Phenomena, Electroforming, Resistive Switching, and Defect

7 Lead Oxide as Material of Choice for Direct Conversion Detectors 129

8 ZnO Varistors: From Grain Boundaries to Power Applications 157

8.5 The ‘Double Schottky Barrier Defect Model’ 174

9 Fundamental Properties and Power Electronic Device Progress of Gallium

10 Emerging Trends, Challenges, and Applications in Solid-State Laser Cooling 353

10.3 Experimental Design Considerations for Cooling 357

11 Electrode Materials for Sodium Ion Rechargeable Batteries 397

11.6 Synthesis and Electrochemical Characterization of Electrodes 404

12 Perovskites for Photovoltaics 423

13 Advanced Characterizations of Oxides for Optoelectronic Applications 453

13.2.3.6 Reduced Graphene Oxide-Miscellaneous Materials 463

15.3 Atomic and Electronic Structure 530

16 Oxide Cathodes 553

Wiley Series in Materials for Electronic and Optoelectronic

Potential applications of oxide electronic materials are vast. Transparent electronics,

Amr M. Abdelkader Supriyo Bandyopadhyay

Debasish Das J.G. Leadley

Chennupati Jagadish David J. Lockwood

S.B. Majumder Asim K. Ray

Tania Majumder Alla Rez

Jyothis Thomas Jiandong Ye

Graphene Oxide for Electronics

Oxide Electronics, First Edition. Edited by Asim Ray.

Graphene Graphene Oxide (GO) Reduced Graphene Oxide (rGO)

1.2 Synthesis and Characterizations of Graphene Oxide

1.2.2 Microwave Method

1.2.3 Plasma Method

60 μm 292 290 288 286 284 282

rGO 0.5 Dispersed

1.2.4 Laser Method

Side view Side view 3.3A

(a) (d) (e)

Graphene / Cu G/PET-PSA Heating Pressure

1.3 Energy Harvest Applications of Graphene Oxide

Current density (mA/cm2)

layer between the perovskite and 2,2′ ,7,7′ -tetrakis-(N,N-di-p-methoxyphenyl-amine)-

1.3.2 Solar Thermal Energy Harvest Devices

1.4 Energy Storage Applications of Graphene Oxide

Polystyrene foam (d) (e)

This is caused by intrinsic aggregation or re-stacking of graphene nanosheets (GNSs)

0.001 0.01 0.1

In order to establish a quantitative relationship among the nanoconﬁned ion transport

WS2-NTs Graphene oxide WS2-NT/GS

Capacity (mAh g–1)

Current Density:100 mA g–1

1.5 Electronic Device Applications of Graphene Oxide

methods. Although graphene oxide demonstrates the ﬁeld-eﬀect characteristics even

1.6 Large Area Electronics Applications of Graphene Oxide

Flexible and Wearable Graphene-Based E-Textiles

2.1 Introduction to Wearable E-Textiles