Chapter 1: Introduction 1 1.1 The global energy scenario and motivation for adopting green energy 1 1.1.1 Excess CO2 concentration: A harmful greenhouse gas 3 1.2 Possibility of renewable source of energy 3 1.2.1 Potential of Solar fuels: What are Solar Fuels 4 1.2.2 Natural Photosynthesis vs. Artificial Photosynthesis 4 1.3 Fundamentals of CO2 photoreduction 5 1.3.1 Challenges in CO2 photoreduction 7 1.3.2 Interaction of CO2 molecule with Semiconductor Photocatalyst Surface 10 1.3.3 Importance of isotopic studies in CO2 photoreduction 10 1.3.4 Pathways for CO2 reduction 11 1.4 Reduced titania: synthesis route, properties and interaction with reactant molecules 13 1.4.1 How are Ti3+ states generated 14 1.4.2 Properties of reduced Titania 20 1.4.3 Principles of H2O and CO2 molecule interaction with reduced titania 22 1.5 Organization of the thesis 25 1.6 References 27 Chapter 2: Characterization techniques and analytical tools 32 2.1 Characterization techniques 32 2.1.1 X-ray diffraction (XRD) 32 2.1.2 Energy dispersive X-ray spectroscopy (EDS or EDX or EDAX) 34 2.1.3 Raman analysis 36 2.1.4 Transmission electron microscopy (TEM) analysis 38 2.1.5 High resolution transmission electron microscopy (HR-TEM) analysis 40 2.1.6 Ultraviolet-Visible diffuse reflectance spectroscopy (UV-Vis DRS) 40 2.1.7 Photoluminescence (PL) spectroscopy 42 2.1.8 X-ray photoelectron spectroscopy (XPS) 43 2.1.9 Ultraviolet photoelectron spectroscopy 44 2.1.10 Electron paramagnetic resonance (EPR) spectroscopy 45 2.1.11 Transient absorption spectroscopy (TAS) analysis 48 2.2 Analytical techniques 48 2.2.1 Gas chromatography 48 2.2.2 Gas chromatography-mass spectroscopy (GC-Master) 55 2.3 CO2 photoreduction setup 60 2.4 References 62 Chapter 3: Highly Enhanced and Stable Activity of Defect Induced Titania Nanoparticles for Solar Light Driven CO2 Reduction into CH4 63 3.1 Introduction 64 3.2 Experimental 67 3.2 Results and Discussions 70 3.4 Conclusions 94 3.5 References 97 Chapter 4: High rate solar-light photoconversion of CO2 into fuel: Controllable transformation from C1 to C2 products 101 4.1 Introduction 102 4.2 Photocatalyst preparation and characterization 105 4.3 Results and discussions 107 4.4 Conclusion 126 4.5 References 128 Chapter 5: CO2, Water, and Sunlight to Hydrocarbon Fuel: A Peak Joule-to-Joule Photoconversion Efficiency of 3.3% 133 5.1 Introduction 134 5.2 Photocatalysts synthesis and characterizations 135 5.3 Results and discussions 137 5.4 Conclusions 149 References 150 Chapter 6: Conclusions and Future Perspectives 154 Appendix 1: Abstract in Korean language 157
Research Interests
Electrocatalysts for fuel cells; water splitting; metal-air batteries; Polymer electrolyte membranes for fuel cells; flow batteries; Hydrogen generation and utilization