Surface Chemistry and Macroscopic Assembly of Graphene for Application in Energy Storage (Springer Theses)

This PhD thesis presents the latest findings on the tunable surface chemistry of graphene/graphene oxide by systematically investigating the tuning of oxygen and nitrogen containing functional groups using an innovative carbonization and ammonia treatment. In addition, novel macroscopic assemblies or hybrids of graphene were produced, laying the theoretical foundation for developing graphene-based energy storage devices. This work will be of interest to university researchers, R&D engineers and graduate students working with carbon materials, energy storage and nanotechnology -- OhioLink Library Catalog Parts of this thesis have been published in the following journal articles: 6 Supervisors' Foreword 7 Acknowledgments 9 Contents 11 1 Literature Review and Research Background 14 1.1 Introduction to Graphene 14 1.2 Summary of Graphene Preparation Methods 15 1.3 The Synthesis and Structure of Graphite Oxide 17 1.4 The Formation of Reduced Graphene Oxide 25 1.4.1 Thermal Annealing 27 1.4.2 Chemical Reduction 30 1.5 Application Prospect of Reduced Graphene 34 1.5.1 Paper/Membrane-Like Materials 34 1.5.1.1 Graphite Oxide Paper 34 1.5.1.2 Electric-Conductive Reduced Graphene Paper 37 1.5.1.3 Transparent Conducting Film 39 1.5.2 Energy Storage Materials 42 1.5.2.1 Supercapacitor 42 1.5.2.2 Li-Ion Cell 47 1.5.3 Other Applications 51 1.6 The Proposal of the Topic and the Main Research Contents 51 References 54 2 Structural Evolution of the Thermally Reduced Graphene NanosheetsDuring Annealing 63 2.1 Introduction 63 2.2 Experimental 64 2.2.1 Preparation of TRG 64 2.2.2 Sample Characterization 64 2.2.3 Electrochemical Measurements 65 2.3 Results and Discussion 66 2.3.1 Structural Evolution 66 2.3.2 Electrochemical Performance 73 2.4 Conclusions 80 References 81 3 Hierarchical Amination of Graphene for Electrochemical Energy Storage 84 3.1 Introduction 84 3.2 Experimental 85 3.2.1 Preparation of Hierarchically Aminated Graphene 85 3.2.2 Sample Characterization 86 3.2.3 Electrochemical Measurements 86 3.3 Results and Discussion 87 3.3.1 The Microstructure of AGHs 87 3.3.2 The Surface Chemistry of AGHs 90 3.3.3 The Electrochemical Capacitance of AGH 97 3.4 Conclusions 104 References 104 4 Free-Standing Graphene Film with High Conductivity by Thermal Reduction of Self-assembled Graphene Oxide Film 108 4.1 Introduction 108 4.2 Experimental 109 4.3 Results and Discussion 110 4.4 Conclusions 118 References 119 5 Template-Directed Macroporous ‘Bubble’ Graphene Film for the Application in Supercapacitors 122 5.1 Introduction 122 5.2 Experimental 123 5.2.1 Synthesis of PMMA Latex Spheres 123 5.2.2 Hard Template Route for Macroporous Graphene Film 123 5.2.3 Structural Characterization 124 5.2.4 Electrochemical Measurements 124 5.3 Results and Discussion 125 5.4 Conclusions 130 References 130 6 SnO2@Graphene Composite Electrodes for the Application in Electrochemical Energy Storage 133 6.1 Introduction 133 6.2 Experimental 135 6.2.1 Pre-graphenization: SnO2@TRG Hybirds 135 6.2.2 Post-graphenization: SnO2@CRG Hybrids 135 6.2.3 Sample Characterization 136 6.2.4 Li-Ion Battery Performance Measurements 136 6.2.5 Supercapacitor Performance Measurements 137 6.3 Results and Discussion 137 6.3.1 Pre-graphenization: Structure of TRG and SnO2@TRG Hybrids 137 6.3.2 Post-graphenization: Structure of SnO2@CRG Hybrids 139 6.3.3 Electrochemcial Performance 143 6.3.3.1 Li-Ion Battery 143 6.3.3.2 Supercapacitor 146 6.4 Conclusions 148 References 149 7 Main Conclusions and Plan of Further Work 152 7.1 Conclusions 152 7.2 Primary Innovation Points 154 7.3 Planning of Future Work 155 Front Matter....Pages i-xiii Literature Review and Research Background....Pages 1-49 Structural Evolution of the Thermally Reduced Graphene NanosheetsDuring Annealing....Pages 51-71 Hierarchical Amination of Graphene for Electrochemical Energy Storage....Pages 73-96 Free-Standing Graphene Film with High Conductivity by Thermal Reduction of Self-assembled Graphene Oxide Film....Pages 97-110 Template-Directed Macroporous ‘Bubble’ Graphene Film for the Application in Supercapacitors....Pages 111-121 SnO2@Graphene Composite Electrodes for the Application in Electrochemical Energy Storage....Pages 123-141 Main Conclusions and Plan of Further Work....Pages 143-146 This PhD thesis presents the latest findings on the tunable surface chemistry of graphene/graphene oxide by systematically investigating the tuning of oxygen and nitrogen containing functional groups using an innovative carbonization and ammonia treatment. In addition, novel macroscopic assemblies or hybrids of graphene were produced, laying the theoretical foundation for developing graphene-based energy storage devices. This work will be of interest to university researchers, R & D engineers and graduate students working with carbon materials, energy storage and nanotechnology