Atomic layer deposition of multi-component catalyst systems for the oxygen evolution reaction

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Abstract/Contents

Abstract
Development of catalysts for the OER continues to be a research priority with the aim of improving the efficiency of electrochemical water splitting. One of the best classes of catalysts for the OER in alkaline electrolytes is based on doped nickel oxyhydroxides. In this dissertation, atomic layer deposition (ALD) was utilized to synthesize model catalyst systems for research. First, the role of iron in nickel oxyhydroxide catalysts will be discussed. ALD was used to perform surface-directed modification of nickel oxyhydroxide catalysts. ALD of iron oxide on these nickel oxyhydroxide catalysts was found to deposit iron on the surface without modifying the bulk nickel properties. Through this selective deposition, an iron-doped nickel oxyhydroxide surface was found to be the active site motif required for high OER activity. Second, the role of aluminum as a dopant will be discussed. ALD was utilized to synthesize well-defined, ultra-thin nickel-aluminum oxide films. A study was performed to understand the growth behavior of ALD nickel-aluminum oxide. Nucleation effects of ALD aluminum oxide on surfaces prepared by ALD nickel oxide was found to be the dominant effect resulting in non-constant growth per cycle. With the knowledge obtained in the growth behavior studies, well-defined nickel-aluminum oxide films were deposited for catalysis. To form the final catalyst, an electrochemical conditioning procedure was employed to convert the as-deposited oxide films to the active oxyhydroxide catalyst. Turnover frequencies (TOFs) were determined for each catalyst, and it was found that the highest performing electrocatalysts were the films containing nickel, aluminum and iron, confirming that aluminum exerts a promotion effect on nickel oxyhydroxide catalysts. For the thinnest films, aluminum doping improved the TOF of nickel-iron oxyhydroxide catalysts by over 300%

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 2020; ©2020
Publication date 2020; 2020
Issuance monographic
Language English

Creators/Contributors

Author Baker, Jonathan Grant
Degree supervisor Bent, Stacey
Thesis advisor Bent, Stacey
Thesis advisor Cargnello, Matteo
Thesis advisor Jaramillo, Thomas Francisco
Degree committee member Cargnello, Matteo
Degree committee member Jaramillo, Thomas Francisco
Associated with Stanford University, Department of Chemical Engineering.

Subjects

Genre Theses
Genre Text

Bibliographic information

Statement of responsibility Jonathan G. Baker
Note Submitted to the Department of Chemical Engineering
Thesis Thesis Ph.D. Stanford University 2020
Location electronic resource

Access conditions

Copyright
© 2020 by Jonathan Grant Baker
License
This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).

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