Graphene An Introduction to the Fundamentals and Industrial Applications
من سلسلة علم المواد المتقدمة
Advanced Material Series
Madhuri Sharon and Maheshwar Sharon
Walchand Centre of Research for Nanotechnology and Bionanotechnology, India
Contents
Foreword by Hisanori Shinohara xv
Preface xvii
1 Te History of Graphene 1
2 Structure and Properties of Graphene 17
2.1 Te Structure of Graphene 17
2.1.1 Carbon 18
2.1.2 Graphite 19
2.1.3 Graphene 21
2.1.3.1 Bilayer Graphene 22
2.1.4 Graphane 23
2.1.5 Graphone 24
2.2 Disorder in Graphene Structure 25
2.2.1 Ripples 26
2.2.2 Topological Defects 26
2.2.3 Ad-Atom (OR “ADSORBED ATOM”) 27
2.2.4 Cracks or Fractures in Graphene 27
2.3 Properties of Graphene 28
2.3.1 Mechanical Properties 29
2.3.2 Termal Properties 29
2.3.3 Optical Properties 30
2.3.4 Chemical Stability and Reactivity 33
2.3.5 Te Intriguing Electronic Properties (Dirac Point) 35
2.3.6 Semiconductor Properties 37
2.4 Summary 37
3 Nanographene and Carbon Quantum Dots (C-Dots) 39
3.1 Nanographene 40
3.1.1 Structure of Nanographene 42
3.1.2 Properties of Nanographene 42
3.1.3 Fabrication of Nanographene 44viii Contents
3.1.3.1 Physical Methods 44
3.1.3.2 Chemical Methods 45
3.1.4 Applications of Nanographene 45
3.2 Graphene Quantum Dots or Carbon Dots 46
3.2.1 Structure of Carbon Dots 48
3.2.2 Properties of Carbon Dots 49
3.2.2.1 Optical Properties 49
3.2.2.2 Photocatalytic Properties 54
3.2.2.3 Chemical Inertness 54
3.2.2.4 Water Solubility 55
3.2.3 Fabrication of Carbon Dots 55
3.2.3.1 Electrochemical Methods 56
3.2.3.2 Combustion, Termal, Hydrothermal and
Acidic Oxidation of Carbon Precursors 58
3.2.3.3 Pulsed Laser Irradiation of
Carbon Source 59
3.2.3.4 Laser Ablation of Graphite 60
3.2.3.5 Arc Discharge Method 60
3.2.3.6 Plasma Treatment Method 61
3.2.3.7 Opening of Fullerene Cage 61
3.2.3.8 Ultrasonic-/Microwave-Assisted
Synthesis 61
3.2.3.9 Chemical Methods 62
3.2.3.10 Supported Synthetic Procedure 63
3.2.3.11 Biogenic Synthesis 64
3.2.4 Applications of Carbon Dots 66
3.2.4.1 Sensor Designing 66
3.2.4.2 Bioimaging 67
3.2.4.3 Drug Delivery 68
3.2.4.4 Optoelectronics and In Vivo Biosensing
Applications 70
3.2.4.5 Photocatalysis 70
3.2.4.6 SERS 70
3.2.4.7 Health and Bio-Related Applications 71
3.3 Conclusions 71
4 Identifcation and Characterization of Graphene 73
4.1 Introduction 73
4.2 Microscopic Methods 76
4.2.1 SEM, STM and TEM Characterization of Graphene 76
4.2.2 AFM Characterization of Graphene 79Contents ix
4.3 Spectroscopic Methods 81
4.3.1 Raman Spectroscopic Analysis of Graphene 81
4.3.2 FTIR Analysis of Graphene 85
4.3.3 UV-Vis Spectroscopic Analysis of Graphene 87
4.3.4 XRD Analysis of Graphene 88
4.3.5 XPS of Graphene 90
4.3.6 NMR Analysis of Graphene 91
4.3.7 DLS of Graphene 92
4.3.8 DPI of Graphene 92
4.4 Optical Property Analysis 93
4.4.1 Optical Absorption and Nonlinear Kerr E?ect 93
4.4.2 Photoluminescence/Blue-Photoluminescence 95
4.4.3 Optical Band Gap 97
4.5 Measurement of Mechanical Properties 99
4.5.1 Young’s Modulus 99
4.5.2 Poisson’s Ratio 100
4.5.3 Bulge Test 102
4.5.4 Tensile Testing/Tension Testing 103
4.5.5 Gas Leak Rates in Graphene Membranes 105
4.6 Termal Properties and Termal E?ect Analysis 105
4.6.1 Termal Conductivity 105
4.6.2 TGA and Termal Stability 105
4.7 Characterization of Electrical Properties 108
4.7.1 Electronics 108
4.7.2 Electron Transport 108
4.7.3 Electrochemical Redox 109
4.8 Work Function 109
4.9 Anomolous Quantum Hall E?ect 109
4.10 Spin Transport 110
4.11 Summary 111
5 Engineering Properties of Graphene 113
5.1 Introduction 113
5.2 Engineering Magnetic Properties 114
5.3 Engineering Graphene with Enhanced Mechanical
Properties 115
5.3.1 Homogeneously Dispersing Graphene
in Polymers 116
5.3.2 Chemical Cross-Linking 117
5.3.3 Hydrogenation 117
5.4 Engineering the Field Emission (FE) Properties 119x Contents
5.5 Engineering Band Gap or Energy Gap of Graphene 120
5.6 Engineering the Electronic Properties of Graphene 122
5.6.1 Engineering Electronic Properties of Graphene
for its Application in Transistors 123
5.6.2 Engineering the Electronic Properties of
Graphene for Solar Cell Application 126
5.6.2.1 p:n Junction Solar Cell 126
5.6.2.2 Schottky Junction Solar Cell 127
5.6.2.3 Dye Sensitized Solar Cell (DSSC) or
Organic Photovoltaic Cell (OPV) 127
5.6.3 Engineering the Electronic Properties of
Graphene for Patterning Graphene 128
5.6.4 Engineering the Electronic-Chemical
Properties of Graphene for Supercapacitor 129
5.6.5 Engineering the Piezoelectric Properties
of Graphene 131
5.6.6 Engineering Electronic Properties of Graphene
for its Use in Fuel Cells 132
5.7 Engineering Structural Properties of Graphene 132
5.7.1 Engineering Hybrid Structures of Graphene 133
5.7.1.1 Graphene Hybridized with SnO2 133
5.7.1.2 Graphene Hybridized with TiO2 134
5.7.1.3 Graphene Hybridized with NiO 134
5.7.1.4 Graphene Coated with Transparent Tin
Ferroelectric (P (VDF-TrFE)) Polymer 135
5.7.1.5 Graphene?Metal Nanowire Hybrid
Structures 136
5.7.2 Engineering Super Structures of Graphene 136
5.7.2.1 Engineering Graphene Super
Structure Using Ru 136
5.7.2.2 Engineering Graphene Super
Structure Using Cu 137
5.7.2.3 Engineering Graphene Super
Structure Using Ni 139
5.7.3 Engineering Hetero Structures of Graphene 139
5.7.3.1 Engineering Graphene Hetero
Structure Using Silicon di-oxide
(SiO2) as Substrate 140
5.7.3.2 Engineering Graphene Hetero
Structures Based on Ultrathin
Hexagonal Boron Nitride (h-BN) 140Contents xi
5.7.4 Introducing Imperfections in Graphene 141
5.7.4.1 Imperfections to Improve
Graphene Sensors 141
5.7.4.2 Engineering Single Carbon Atom
Point Defects in Graphene to Induce
Magnetism 142
5.8 Summary 142
6 Applications of Graphene 145
6.1 Application Possibilities 146
6.1.1 High Specifc Strength Related Applications of
Graphene 146
6.1.2 High Surface Area Related Applications of
Graphene 146
6.1.3 Graphene for Electrical Energy Storage 147
6.1.4 Termal Management by Graphene 148
6.1.5 High Flexibility Related Applications
of Graphene 149
6.1.6 Electronic and Optoelectronic Devices
Using Graphene 150
6.1.7 Graphene as Lightweight Electrical Conductor 150
6.1.8 Transparent, Flexible, Conductive and Oxidation
Resistant Films of Graphene 151
6.1.9 Graphene Film’s Impermeability Related
Applications 154
6.1.10 Reinforcements of Polymer Composites 155
6.1.11 Sensors 155
6.1.11.1 Graphene for Biosensors 155
6.1.11.2 Graphene as Gas Sensors 156
6.1.11.3 Graphene for Chemi-Sensors 157
6.1.11.4 Graphene for Pressure-Sensors 158
6.1.11.5 Graphene for Strain-Gauge 158
6.1.12 Graphene for Electric Power Generation 159
6.1.12.1 Fuel Cells 159
6.1.12.2 Solar Cells 160
6.1.13 Graphene as a Compliant Substrate 161
6.1.14 Graphene as Template for New Materials 161
6.1.15 Biodevices Based on Graphene’s
Chemical Properties 162
6.1.16 Graphene in Healthcare 162
6.1.16.1 Cytotoxicity a Concern 162xii Contents
6.1.16.2 Graphene for Drug Delivery 163
6.1.17 Graphene in Textiles and Fabrics 164
6.2 Summary 164
7 Towards Mass Production of Graphene: Lab to
Industry (Scaling Up) 167
7.1 Exfoliation of Graphite: A Top-Down Approach 168
7.1.1 Micro-Mechanical Exfoliation or Repeated
Peeling of Graphite 168
7.1.2 Liquid Phase Chemical Exfoliation of Graphite 169
7.1.3 Liquid Phase Aqueous Exfoliation of
Graphite Oxide 170
7.1.4 Termal Aqueous Phase Exfoliation of
Graphite Oxide 171
7.2 Length-Wise Unzipping of Carbon Nanotubes (CNT) 171
7.2.1 Selective Etching or Plasma Etching Method 172
7.2.2 Oxidizing Method 173
7.2.3 Alkali-Metal Atom Insertion Method 175
7.2.4 Catalytic Unzipping of Carbon Nanotubes 177
7.2.5 Hydrothermal Method 177
7.2.6 Sonochemical Unzipping of Multi Wall
Carbon Nanotubes (MWNTs) 178
7.3 Chemical Vapor Deposition (CVD) Method 179
7.4 Epitaxial growth of Graphene on Silicon Carbide 181
7.5 Reduction of Graphene Oxide (GO) 184
7.5.1 Termal Reduction of GO 184
7.5.2 Hydrothermal Reduction of GO 185
7.5.3 Solvothermal Reduction of GO 186
7.5.4 Chemical Reduction of GO 187
7.5.5 Electrochemical Reduction of GO 189
7.5.6 Reduction of GO by Hydrogen Plasma 189
7.5.7 Reduction of GO by Xenon Flashtubes 190
7.5.8 Reduction of GO by an
Expansion-Reduction Agent 191
7.5.9 Photocatalytic Reduction of GO 191
7.5.10 Multi Step Reduction 192
7.6 Arc-Discharge Method 194
7.7 Solvothermal Method 194
7.8 Substrate-Free Gas Phase Synthesis Of Graphene 195
7.9 Other Growth Methods 196
7.10 Summary 196Contents xiii
8 Direct Transfer or Roll-To-Roll Transfer of Graphene
Sheet onto Desired Substrate 197
8.1 Introduction 197
8.2 Direct Transfer of Graphene by Etching and
Scooping Method 199
8.3 Direct Transfer of Graphene by Etching and Scooping
Method Using a Graphene Protecting Media 200
8.3.1 PMMA 200
8.3.2 PC (Poly (bisphenol A Carbonate) 202
8.3.3 Transfer on Pre-Stretched Substrate, PDMS 202
8.3.4 Direct Transfer of Graphene onto Flexible
Polyethylene Terephthalate (PET) 202
8.4 Roll-to-Roll Synthesis and Transfer of Graphene 205
8.4.1 Roll-to-Roll Continuous Transfer Using
Termal Tape 205
8.4.2 Roll-to-Roll Transfer on to Ethylene-Vinyl
Acetate Copolymer (EVA) Coated Transparent
Poly-Ethylene Terephthalate (PET) Sheets by
Hot Press Method 206
8.4.3 Roll-to-Roll Transfer Using Photo-Curable
Epoxy Resin onto a PET Film 207
8.5 Apparatus Used for Roll-to-Roll Transfer of
Graphene Sheet 208
8.5.1 Patented Apparatus for Roll-to-Roll Graphene
Synthesis and Transfer by the Research and
Business Foundation at Sungkyunkwan University 208
8.5.2 Four Roller Roll to Roll System 209
8.5.3 Yamada’s Method 211
8.6 Considerations for Minimizing Defects or Cracking
During Transfer 212
8.6.1 Selecting Proper Target Substrate 212
8.6.2 To Avoid the Use of Etchants 213
8.7 Summary 214
9 Graphene in Industry, Commercialization Challenges and
Economics 217
9.1 Introduction 217
9.2 Graphene Industries 219
9.2.1 Companies Producing Graphene and
Graphene-Based Applications 220xiv Contents
9.2.2 Companies Supporting Graphene
Related Activities 230
9.2.2.1 Graphite Mining Companies 230
9.2.2.2 Companies Making
Graphene-Manufacturing Equipment 232
9.2.2.3 Companies Providing Sofware,
Technology or other Services for
Graphene Industries 233
9.2.3 End-User Markets and Target Customers 238
9.2.3.1 Te Automotive Industries 238
9.2.3.2 Electronic Industries 238
9.2.3.3 Aerospace Industries 238
9.2.3.4 Energy Sectors 239
9.2.3.5 Graphene Solar Cells 241
9.2.3.6 Manufacturing Sectors 242
9.3 Graphene Commercialization 244
9.3.1 Challenges in Graphene Commercialization 245
9.3.1.1 Producing Desired Band Gap 245
9.3.1.2 High Production Cost 246
9.4 Economics of Graphene and Graphene-Related Products 246
9.5 Graphene and the Future Possibilities 249
9.5.1 Flexible Electronic Screens 250
9.5.2 Graphene Composites of Very High
Mechanical Strength 251
9.5.3 Graphene to Replace Flash Memory of SD Cards 251
9.5.4 Next Generation Speakers 251
9.5.5 Faster Computer Chips and Broadband 251
9.5.6 Super-Strong Bulletproof Body Armor
Using Graphene 252
9.5.7 Graphene Drones 252
9.6 Graphene and Fantasies 253
9.7 Summary 255
References 257
Index 27
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