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Ab-Initio Computational Studies of the Catalysis Mechanisms on Graphene-Based Materials in Fuel Cell Applications

Ab-Initio Computational Studies of the Catalysis Mechanisms on Graphene-Based Materials in Fuel Cell Applications
Alternative Title
제 1 원리 전산을 이용한 그래핀 기반 재료의 연료전지 촉매 거동 연구
Kwon, In Hye
DGIST Authors
Kwon, In HyeHan, Byung ChanKim, Ho Young
Han, Byung Chan
Kim, Ho Young
Issued Date
Awarded Date
2013. 2
first-principlesdensity functional theoryfuel celloxygen reduction reactiongraphene연료전지제1원리 전산범밀도 함수 이론산소환원반응그래핀
Low temperature fuel cells with noble metal-based catalysts are one of the promising green technologies. However, they have obstacles to wide commercialization largely caused by catalysts with high materials costs, poor electrochemical durability, and low efficient activity. As such, it is highly demanded to develop inexpensive but efficient and stable metal-free catalysts of fuel cells. Recently, it was reported that the electrochemical activity of nitrogen-doped graphene for oxygen reduction reaction (ORR) could be comparable to Pt/C in alkaline fuel cells. In this thesis, catalytic mechanisms of graphene-based materials for Polymer Electrolyte Membrane Fuel Cells (PEMFCs) were studied using first-principles density functional theory (DFT) computations. Thesis work includes the atomic-level structural studies of graphene-based materials, charge distribution analysis by doping, interfacial water layer structures, adsorption energies of various chemical species. These quantum mechanical grade of information is used to construct thermodynamic free energy diagrams and thus, to identify the most viable ORR mechanisms. This thesis confirms that doping with heteroatom in graphene causes charge redistribution, and creates charged sites. Positively charged sites with lower electronegativity between carbon and dopants acted as O2 adsorption sites by reducing overpotential needed in the O2 adsorption. Furthermore, two-electron reaction involving hydrogen peroxide was not preferred on N, B, and P-doped graphene but on pristine graphene. Through this thesis, we found doping with heteroatoms can considerably affect the electronic structures of graphene and alter its ORR mechanisms leading to improving ORR activity. ⓒ 2013 DGIST
Table Of Contents
Chapter 1. Introduction 1
1.1 Overview 1
1.2 Literature Review 4
1.3 Thesis Outline 7
Chapter 2. Methodology 9
2.1 Introduction to the Ab-Initio Computations 9
2.2 Computational Details 10
2.3 Bader Charge Analysis 10
Chapter 3. Results and Discussion 12
3.1 Stable Structures of Nitrogen-Doped Graphene 12
3.2 Charge Density Analysis 14
3.3 Interfacial Water Structures 18
3.4 Adsorption Energies of O2 and OH 23
3.5 Oxygen Reduction Reaction Mechanism 31
Chapter 4. Conclusions 40
References 42
Summary(국문요약) 46
Energy Systems Engineering
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Department of Energy Science and Engineering Theses Master


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