Metal-Organic Frameworks;Cu active sites;Reconstruction;Electrochemical CO2 reduction
Table Of Contents
Abstract i List of Contents ii List of Tables iv List of Figures v
Ⅰ. Introduction 1.1 Electrochemical CO2 Reduction Reaction 1 1.2 Cu-based Electrocatalyst for CO2RR 4 1.3 Metal-Organic Frameworks 4 1.4 Reconstruction of Cu-based Catalyst 6 1.5 Research Motivation and Strategy 7
Ⅱ. Theoretical Background 2.1 Fundamental Theory of Electrochemical CO2RR 9 2.1.1 Electrochemical Reaction 9 2.1.2 Mechanisms of CO2 Reduction 9 2.1.3 Performance Evaluation Indicators of CO2 Reduction Catalyst 12 2.2 CO2RR Electrolyzer 14 2.2.1 Development of GDE 14 2.2.2 Characteristics of Flow-type Cell 14 2.3 Chemical State Transformation of Cu 17 2.3.1 Change of Cu State by Alkaline Electrolyte 17 2.3.2 Change of Cu State by Reduction Potential 19
Ⅲ. Experimental 3.1 Material Synthesis 21 3.1.1 Synthesis of Cu-BTC and Cu-BDC 21 3.1.2 Fabrication of Cu/C-BTC and Cu/C-BDC 22 3.1.3 Fabrication of i-Cu-BTC and i-Cu-BDC 22 3.2 Material Characterization 22 3.3 Electrode Preparation 23 3.4 Evaluation of CO2 Reduction Performance 24
Ⅳ. Results and Discussion 4.1 Reconstruction of Cu active sites based on morphology and Cu initial state 25 4.1.1 Catalyst Synthesis and Characterization 25 4.1.2 CO2RR Performance Evaluation 46 4.1.3 Real-time Analysis of Reaction Intermediates 49 4.2 Unveiling the Reconstruction of Cu Active Sites in MOFs 51 4.2.1 Strategy for Revealing the Reconstruction Mechanism of MOFs 51 4.2.2 Characterization of i-Cu-BTC and i-Cu-BDC 53 4.2.3 CO2RR Performance Evaluation 63 4.2.4 Proposed MOFs Reconstruction Mechanism 65