Title

Design of Electrocatalysts with Superior Longevity for Polymer Electrolyte Membrane Fuel Cell Applications

Alternative Title

차세대 고분자 전해질막 연료전지 적용을 위한 초장수명 전기화학 촉매 개발

DGIST Authors

Gyan Barimah Caleb ; Yun Hee Jang ; Jong-Sung Yu

Advisor

장윤희

Co-Advisor(s)

Jong-Sung Yu

Issued Date

2025

Awarded Date

2025-08-01

Type

Thesis

Description

Electrocatalyst, PEMFC, Pt-AKEM, ORR, Durability

Table Of Contents

List of Contents
Abstract i
List of contents iii
List of figures v
List of tables xii


I. INTRODUCTION 1
1.1. Motivation 1
1.2. Objective of this thesis 2
1.3. Thesis outline 3
II. BACKGROUND 5
2.1. Introduction to Fuel Cells 5
2.1.1. Fuel Cell types 5
2.1.2. Uses of fuel cells 7
2.2. Polymer Electrolyte Membrane Fuel Cell (PEMFC) 8
2.2.1. Thermodynamics of PEMFC 10
2.2.2. Origin of overpotentials in fuel cells 13
2.2.3. Electrocatalysts for PEMFC 15
2.2.4. Non-platinum group electrocatalyst (Non-PGM) 17
2.2.5. Platinum-alkaline earth metal alloys as promising ORR electrocatalysts. 18
III. High Vacancy Formation Energy Boosts the Stability of Structurally Ordered PtMg in Hydrogen Fuel
Cells 21
3.1. Introduction 21
3.2. Experimental section 24
3.2.1. Chemicals and materials 24
3.2.2. Synthesis of Structurally ordered PtMg alloys 25
3.2.3. Characterization 26
3.2.4. Electrochemical Half-Cell RDE measurement 27
3.2.5. Full cell PEMFC test 29
3.2.6. Computational studies 30
3.3. Results and discussion 31
3.3.1. Catalyst design and characterization 31
3.3.2. Electrochemical Half-cell evaluation 43
3.3.3. Mechanistic Study 47
3.3.4. Membrane electrode assembly (MEA) full cell evaluation 52
3.3.5. Theoretical studies (DFT results) 63
3.4. Conclusion 66
IV. Intermetallic Platinum-Calcium Alloy Breaks the Activity-Stability Trade-off in Fuel Cell for Enhanced
Performance 68
4.1. Introduction 68
4.2. Experimental section 70
4.2.1. Chemicals and materials 70
4.2.2. Synthesis of PtCa, PtBa and PtSr and Pt3Y 70
4.2.3. Characterization 70
4.2.4. Electrochemical half-cell evaluation 71
4.2.5. Full cell PEMFC test 71
4.2.6. Computational details 71
4.3. Results and discussion 72
4.3.1. Electrochemical half-cell and MEA full-cell test 85
4.3.2. Theoretical studies (DFT calculations) 94
4.4. Conclusion 99
V. Metal-N Coordination in a Structurally Ordered PtZn Alloy Propels a Boost in Activity and Stability for
PEMFC 101
5.1. Introduction 101
5.2. Experimental Section 104
5.2.1. Chemicals and Reagents 104
5.2.2. Synthesis of ZIF-8 105
5.2.3. Synthesis of Pt/C, PtCo/C, PtNi/C, and PtFe/C 105
5.2.4. Method2 (Sorption of Metal ions on Carbon support; scaleup approach) 105
5.2.5. Synthesis of PtZn/C, N-PtZn/C, PtCoZn/C, PtNiZn/C and PtFeZn/C 106
5.2.6. Characterization 107
5.2.7. Electrochemical half-cell test 107
5.2.8. MEA Preparation and Fuel Cell Test 107
5.3. Results and discussion 107
5.3.1. Synthesis and structural characterization 107
5.3.2. Half-Cell ORR Measurements 115
5.3.3. Fuel Cell Performance Evaluation 118
5.4. Conclusion 124
VI. Summary 126

URI

https://scholar.dgist.ac.kr/handle/20.500.11750/59784
http://dgist.dcollection.net/common/orgView/200000888193

DOI

10.22677/THESIS.200000888193

Degree

Doctor

Department

Department of Energy Science and Engineering

Publisher

DGIST

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