Highly Selective and Durable Electrocatalysts for Ambient Ammonia Production via Nitric Oxide Electroreduction in Acidic Medium
- Title
- Highly Selective and Durable Electrocatalysts for Ambient Ammonia Production via Nitric Oxide Electroreduction in Acidic Medium
- Alternative Title
- 산성 매질에서 산화질소 전기환원을 통한 고 선택적이며 고내구성의 상온 암모니아 생산 전기촉매
- Author(s)
- Dhanabal Dinesh
- DGIST Authors
- Dhanabal Dinesh ; Sangaraju Shanmugam ; Soonhyun Kim
- Advisor
- 상가라쥬 샨무감
- Co-Advisor(s)
- Soonhyun Kim
- Issued Date
- 2024
- Awarded Date
- 2024-08-01
- Type
- Thesis
- Description
- Ammonia, nitric oxide electroreduction, nitrogen fixation, nitrogen-doped carbon nanorods, electrocatalysis
- Table Of Contents
-
Abstract i
Table of Contents ii
List of Tables v
List of Figures vii
1. Introduction 1
1.1. Ammonia: Fueling the Future 1
1.2. Global Ammonia Demand Outlook 3
1.3. Beyond Haber-Bosch’s Ammonia 5
1.4. Nitric Oxide Reduction: An Electrochemical Breakthrough 8
1.5. Mechanism of Nitric Oxide Electroreduction 10
1.6. Current Insights and Future Challenges 12
1.7. Objectives of the Thesis 14
2. Experimental Methods 16
2.1. Synthesis of Transition Metal Nanoparticle-Embedded N-Doped Carbon nanorods (TM-NCNR) 16
2.1.1. Chemicals and Materials 16
2.1.2. Synthesis of TM-NCNR and Nomenclature 17
2.1.3. Synthesis of Other Control Samples and Nomenclature 17
2.2. Synthesis of copper nanowires infused porous multi-nano-channel N-doped carbon nanorods (Cu-mNCNR) 18
2.2.1. Chemicals and Materials 18
2.2.2. Synthesis of Cu-mNCNR and Nomenclature 18
2.2.3. Synthesis of control sample (Cu-NCNR) 19
3. Characterization Methods 20
3.1. Physicochemical Characterization 20
3.2. Electrochemical Characterization 21
3.2.1. Electrode Fabrication 21
3.2.2. Electrochemical Cell Setup and Testing 21
3.2.3. Linear sweep voltammetry 22
3.2.4. Chronoamperometry 22
3.2.5. Tafel slope analysis 23
3.2.6. Electrochemical impedance spectroscopy 23
3.2.7. Electrochemical active surface area 23
3.3. The Zn-NO battery assembly and testing 24
3.4. Product Quantification 25
3.4.1. Colorimetric techniques 25
3.4.2. 1H NMR quantification of NH3 28
3.4.3. Gas chromatography quantification of H2 29
3.5. Equations used for the calculations 29
3.5.1. Average yield rate of the product 29
3.5.2. Faradaic efficiency 30
3.5.3. Turn-over frequency 30
4. Results and Discussion 31
4.1. Exploration of Various TM Active Sites with N-doped Carbon Nanorods for Selective Electrosynthesis of NH3 31
4.1.1. Overview 31
4.1.2. Phase formation and analysis 32
4.1.3. Morphological analysis 34
4.1.4. Chemical states analysis 38
4.1.5. Nature of carbon and chemical composition 42
4.1.6. BET surface area and pore size distribution 45
4.1.7. Electrochemical Nitric Oxide Reduction Activity 46
4.1.8. Effect of Graphitization and Porosity 54
4.1.9. Elucidating The Nature of Active Site and Effect of N-Heteroatom Doping .. 62
4.1.10. Robustness of the Ni-NCNR700 and Post-eNORR Study 66
4.1.11. Summary 70
4.2. Development of Copper Nanowires Infused in N-doped Carbon Nanorods for Selective Electrosynthesis of NH3 and Demonstration of Zn-NO Battery 71
4.2.1. Overview 71
4.2.2. Phase evolution and analysis 72
4.2.3. Morphological analysis 74
4.2.4. Raman analysis and chemical composition 79
4.2.5. Surface composition and electronic configurations 80
4.2.6. Electrocatalytic activity of Cu-mNCNR on eNORR 84
4.2.7. Inception of enhanced catalytic activity and N-source identification 92
4.2.8. Robustness of Cu-mNCNR2 and Post-electrolysis Study 97
4.2.9. Zn-NO Battery-A Proof-of-Concept Device 103
4.2.10. Summary 106
5. Conclusion 107
References 109
요 약 문 125
- URI
-
http://hdl.handle.net/20.500.11750/57616
http://dgist.dcollection.net/common/orgView/200000802852
- Degree
- Master
- Department
- Department of Energy Science and Engineering
- Publisher
- DGIST
- Related Researcher
-
-
Shanmugam, Sangaraju
- Research Interests Electrocatalysts for fuel cells; water splitting; metal-air batteries; Polymer electrolyte membranes for fuel cells; flow batteries; Hydrogen generation and utilization
-
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-
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- Appears in Collections:
- Department of Energy Science and Engineering Theses Master
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