Yuyeon Song. (2024). Development of Electrocatalysts for Selective Ammonia Production from Nitric Oxide Reduction. doi: 10.22677/THESIS.200000803073
Type
Thesis
Description
Nitric Oxide Reduction Reaction, Ammonia Production, Core-shell Nanostructure, Metal Phosphide Nanocluster, Non-noble Metal Catalysts
Table Of Contents
List of Contents Abstract i List of Contents ii List of Tables v List of Figures vi CHAPTER 1. INTRODUCTION 1 1.1. Background 1 1.1.1. Nitric Oxide 1 1.1.2. Ammonia 2 1.2. Conventional Haber-Bosch Process 3 1.3. Electrochemical Ammonia Synthesis from Nitric Oxide 4 1.4. Nitric Oxide Reduction Reaction Mechanisms 5 1.5. Types of Cell Configurations for Nitric Oxide Reduction Reaction 7 1.5.1. H-type Batch Cell 7 1.5.2. Zn-NO Battery 8 1.6. Literature Survey and Current Issues 9 1.7. Objectives of This Research Work 12 CHAPTER 2. EXPERIMENTAL SECTION 14 2.1. Synthesis of Core-Shell Ni@NC Electrocatalyst 14 2.1.1. Materials 14 2.1.2. Synthesis of Covalent Organic Framework (RIO-12) 14 2.1.3. Synthesis of Ni@RIO-12 15 2.1.4. Synthesis of COF-derived Core-Shell Electrocatalysts 16 2.1.5. Synthesis of Nickel Nanoparticle Electrocatalysts 16 2.1.6. Synthesis of NC Electrocatalysts 17 2.2. Synthesis of Atomically Dispersed Cu3P embedded in N-doped carbon nanorods (Cu3P/NCNR) Catalyst 17 2.2.1. Chemicals and Materials 17 2.2.2. Preparation of Cu3P Catalyst by Electrospinning method 18 2.2.3. Preparation of Control Samples 19 CHAPTER 3. CHARACTERIZATION 20 3.1. Instrumentation 20 3.2. Electrochemical Measurements 20 3.3. Zn-NO Battery. 22 3.4. Fabrication of Electrode 22 3.5. Nafion Membrane Pretreatment 23 3.6. Electrochemical Active Surface Area 23 3.7. Product Quantification 23 3.8. Quantification of NH3 (Indophenol Blue Method) 24 3.8.1. Quantification of NH2OH 25 3.8.2. Quantification of N2H4 (Watt and Chrisp method) 26 3.8.3. 1H NMR Quantification of NH3 27 3.8.4. Quantification of H2 29 3.9. Equations used for the Calculation 30 3.9.1. NH3 yield rate 30 3.9.2. Faradaic Efficiency 30 3.9.3. Turnover Frequency 31 CHAPTER 4. RESULT AND DISCUSSION 32 4.1. Development of Core-shell Nanostructures as High-performance Electrocatalysts for NH3 Synthesis at Low Overpotentials 32 4.1.1. Physicochemical Characterization 32 4.1.2. Morphology Analysis 33 4.1.3. Surface Composition and Electronic Structure (XPS Analysis) 36 4.1.4. Raman Analysis 38 4.1.5. Electrochemical Characterization 39 4.1.6. Elucidating the Nature of the Active Site 45 4.1.7. Identification of N-source and Optimization of Catalyst Loading 47 4.1.8. Stability Performance 48 4.1.9. Post-NORR Study for Ni@NC-700 to Evaluate the Chemical and Morphological Features. 50 4.1.10. Summary. 52 4.2. Efficient Electrosynthesis of NH3 from NO Reduction Over Atomically Dispersed Cu3P Nanocluster in N-doped Carbon Nanorod Catalysts 53 4.2.1. Structural Analysis 53 4.2.2. Morphological Analysis 54 4.2.3. Surface Chemical Composition and Nature of Carbon 59 4.2.4. Elemental Analysis 63 4.2.5. Electrochemical NORR Activity of Cu3P/NCNR catalyst 64 4.2.6. GC Quantification of H2 70 4.2.7. 1H NMR Quantification of H2 70 4.2.8. Investigation of Intrinsic Catalyst Property 73 4.2.9. Elucidating the Nature of the Active Site and Identification of N-Source 74 4.2.10. Effect of Catalyst Loading on GDE 77 4.2.11. Robustness of Cu3P/NCNR-2 and Post-Analysis Study 78 4.2.12. Zn-NO Battery Performance 84 4.2.13. Summary. 87 CHAPTER 5. CONCLUSION 88 References 90
