Transition Metal-Based Electrocatalysts for the Electroreduction of Nitric Oxide to Ammonia
- Title
- Transition Metal-Based Electrocatalysts for the Electroreduction of Nitric Oxide to Ammonia
- Author(s)
- Sethuram Markandaraj Sridhar
- DGIST Authors
- Sethuram Markandaraj Sridhar ; Sangaraju Shanmugam ; Soonhyun Kim
- Advisor
- 상가라쥬샨무감
- Co-Advisor(s)
- Soonhyun Kim
- Issued Date
- 2023
- Awarded Date
- 2023-02-01
- Type
- Thesis
- Description
- Ammonia, Membrane electrode assembly, core-shell nanostructure, nitric oxide reduction, electrolyzer cell
- Table Of Contents
-
Chapter 1 Introduction 1
1.1 Background 1
1.1.1 Nitric Oxide 1
1.1.2 Ammonia 2
1.2 Commercial Haber-Bosch Process 3
1.3 Electrochemical Nitric Oxide Reduction to Ammonia 5
1.4 Mechanism Involved in the Nitric Oxide Reduction Reactions 7
1.5 Types of Electrochemical Cell Configuration 8
1.5.1 H-type Batch Electrolyzer 8
1.5.2 Flow-cell Electrolyzer 9
1.5.3 Membrane-electrode Assembly Electrolyzer 10
1.6 Literature Survey 11
1.7 Remaining Challenges 12
1.8 The objective of the research work 13
1.8.1 Solar Energy-assisted NO Electrolyzer Using a Core-shell Ni@NC as Electrocatalyst to Produce NH3 13
1.8.2 Dual Fe, Ni-sites for Efficient Electrosynthesis of NH3 from NO in a Membrane Electrode Assembly Electrolyzer 14
Chapter 2 Experimental Section 16
2.1 Synthesis of Core-shell Ni@NC Catalyst 16
2.1.1 Chemicals and Materials 16
2.1.2 Synthesis of Prussian Blue Analog (PBA) 16
2.1.3 Preparation of Core-shell Electrocatalysts 17
2.1.4 Preparation of Nickel Electrocatalyst 17
2.1.5 Preparation of NiO Electrocatalyst 17
2.1.6 Preparation of NC Electrocatalyst 17
2.2 Synthesis of Fe, Ni-dual Single-atom Catalyst 18
2.2.1 Preparation of Fe-NCNT 18
2.2.2 Preparation of FeNi-NCNT 18
2.2.3 Preparation of NCNT 19
Chapter 3 Characterization 20
3.1 Instrumentation 20
3.2 Electrochemical Characterizations 21
3.2.1 Batch Electrolysis Operation 21
3.2.2 Zero-gap MEA Electrolysis Operation 22
3.3 Electrochemical Active Surface Area 22
3.4 Nafion Membrane Pretreatment 23
3.5 Electrode Fabrication for Half-cell Test 23
3.6 Ink, Catalyst Layer, and MEA Fabrication for Full-cell Test 23
3.7 Product Quantification 24
3.7.1 Quantification of NH3 24
3.7.2 Quantification of N2H4 26
3.7.3 Quantification of NH2OH 26
3.8 Equations used for the calculation 27
3.8.1 Yield Rate 27
3.8.2 Faradaic Efficiency 27
3.8.3 Energy Efficiency 27
3.8.4 Solar-to-Fuel Efficiency 28
3.8.5 Turnover Frequency 28
Chapter 4 Results and Discussion 29
4.1 Design and Development of Core-shell Nanostructures as Efficient Electrocatalyst for NH3 Synthesis at Low Overpotentials 29
4.1.1 Physicochemical Characterization 29
4.1.2 Electrochemical Characterization 38
4.1.3 Elucidating the Nature of the Active Site and Identification of Reaction Pathway 47
4.1.4 Coupling NORR and OER in the Full-cell Batch Electrolyzer 52
4.1.5 Electrocatalytic NORR Driven by a Solar Cell 54
4.1.6 Post-ENORR Study for a Ni@NC-3 to Evaluate the Chemical and Morphological Features 56
4.1.7 Summary 59
4.2 Atomically Dispersed Fe, Ni- Dual-Metal Site Catalysts for Enhanced NO Electroreduction to NH3 in a Membrane Electrode Assembly Electrolyzer 60
4.2.1 Physicochemical Characterization 60
4.2.2 Electrochemical Characterization 68
4.2.3 Summary 80
Chapter 5 Conclusion 82
- URI
-
http://hdl.handle.net/20.500.11750/45725
http://dgist.dcollection.net/common/orgView/200000659326
- 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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- Appears in Collections:
- Department of Energy Science and Engineering Theses Master
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