Theoretical routes to advance oxygen electrocatalysis for energy conversion
Abstract/Contents
- Abstract
- Developing sustainable energy technologies is an essential step towards addressing climate change, which remains one of the greatest global challenges of our times. Electrochemistry offers a promising avenue to convert variable renewable energy (VRE), like solar and wind energy, into reliable carbon-neutral fuels, such as hydrogen gas. However, widespread adoption of electrochemical routes of sustainable energy conversion necessitates the development of active, stable, and selective catalysts that are economically viable. In this thesis, we explore various aspects of catalyst design from a theoretical perspective with a focus on electrochemical oxygen reduction (ORR) and evolution (OER). ORR is the rate-limiting reaction of hydrogen fuel cells, which convert hydrogen fuel and oxygen into water and electrical energy. OER limits the overall efficiency of the opposite process in water electrolyzers. To consider approaches to improve catalyst design for these and other electrochemical processes, we first apply density functional theory (DFT) to evaluate the promise of single atom catalysts to achieve high theoretical activity towards ORR and circumvent fundamental activity limitations through strategic design. We then turn our attention to stability considerations by implementing a pre-processing algorithm within the Pymatgen code to improve the efficiency of Pourbaix diagram construction for increasingly complex materials. We apply this algorithm to extract stability trends for a wide range of ternary oxides and build predictive models. By investigating the impacts of catalyst dissolution on activity for Ru-based pyrochlores for OER, we also combine activity and stability considerations to gain a more complete understanding of catalyst performance. Finally, we focus on kinetic modeling of electrochemical steps by studying generalizable trends in activation barriers for proton coupled electron transfers (PCET). We find that these barrier heights are largely governed by the identity of the proton acceptor, which can have profound impacts on simplifying microkinetic modeling and analyzing reaction pathways. Collectively, our findings shine light on thermodynamic activity, stability, and kinetic treatment of catalysts for oxygen electrochemistry.
Description
| Type of resource | text |
|---|---|
| Form | electronic resource; remote; computer; online resource |
| Extent | 1 online resource. |
| Place | California |
| Place | [Stanford, California] |
| Publisher | [Stanford University] |
| Copyright date | 2021; ©2021 |
| Publication date | 2021; 2021 |
| Issuance | monographic |
| Language | English |
Creators/Contributors
| Author | Patel, Anjli M |
|---|---|
| Degree supervisor | Jaramillo, Thomas Francisco |
| Degree supervisor | Noerskov, Jens |
| Thesis advisor | Jaramillo, Thomas Francisco |
| Thesis advisor | Noerskov, Jens |
| Thesis advisor | Reed, Evan J |
| Degree committee member | Reed, Evan J |
| Associated with | Stanford University, Department of Chemical Engineering |
Subjects
| Genre | Theses |
|---|---|
| Genre | Text |
Bibliographic information
| Statement of responsibility | Anjli M. Patel. |
|---|---|
| Note | Submitted to the Department of Chemical Engineering. |
| Thesis | Thesis Ph.D. Stanford University 2021. |
| Location | https://purl.stanford.edu/fj358cx0003 |
Access conditions
- Copyright
- © 2021 by Anjli M Patel
- License
- This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).
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