Dissertation
Density Functional Theory Study on Catalytic Activity of Single-Atom Electrocatalysts for Oxygen Reduction Reaction
Washington State University
Doctor of Philosophy (PhD), Washington State University
2022
DOI:
https://doi.org/10.7273/000005195
Abstract
Single transition metal (TM) and nitrogen-coordinated carbon materials (M–N–C) have been extensively studied as promising electrocatalysts due to their excellent catalytic activity towards oxygen reduction reaction (ORR). However, the ORR catalytic activity of these single-atom electrocatalysts (SACs) is normally not as good as Pt-based electrocatalysts, especially, in acidic media. In this project, the first-principles density functional theory (DFT) methods are used to study the ORR catalytic activity of single-atom iron/cobalt electrocatalysts (Fe/Co SACs) in acidic media. The ORR catalytic performance of Fe SAC can be improved by doping N atoms around the Fe–N4 moiety through replacing C atom with N atom. For the Co SAC, the ORR catalytic activity is improved by reducing the number of Co-coordinated N atoms through replacing the N atom with C atom. The electronic occupancy of metal dz2 orbtial in pristine SACs can be used as a descriptor of ORR catalytic activity.
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Details
- Title
- Density Functional Theory Study on Catalytic Activity of Single-Atom Electrocatalysts for Oxygen Reduction Reaction
- Creators
- Hong Zhong
- Contributors
- Scott P Beckman (Advisor)Yuehe Lin (Committee Member) - Washington State University, Mechanical and Materials Engineering, School ofSoumik Banerjee (Committee Member) - Washington State University, Mechanical and Materials Engineering, School of
- Awarding Institution
- Washington State University
- Academic Unit
- Mechanical and Materials Engineering, School of
- Theses and Dissertations
- Doctor of Philosophy (PhD), Washington State University
- Publisher
- Washington State University
- Number of pages
- 84
- Identifiers
- 99901019235901842
- Language
- English
- Resource Type
- Dissertation