Structure-function relationships in metal oxides and carbon-based catalysts for electrochemical energy conversion reactions

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Abstract/Contents

Abstract
As the imperative to mitigate climate change intensifies, the shift towards sustainable energy practices has never been more crucial. At the heart of this transformation lies electrochemical energy and chemical conversion, which, through the potential-driven control over catalysts, provides a promising pathway to sustainable energy and commodity development over traditional thermochemical methods. This presentation will focus on two electrochemical systems using a combined electrochemical and theoretical approach: the upgrading of biomass to value-added chemicals and the material development and characterization of metal-organic frameworks (MOFs) for the oxygen reduction reaction (ORR) in alkaline hydrogen fuel cells. The electrochemical benzyl alcohol oxidation (BAO) reaction, a model system for studying the biomass upgrading process, can be promoted using Ni-based thin-film catalysts. We will focus on Ni3+ surfaces (lower potential region) under standard operating conditions, correlating BAO onset potentials and the Ni(II/III) redox peak positions across different microenvironments as well as unraveling the mechanisms during BAO. Through the systematic investigation of experimental reaction conditions and computational free energy thermodynamics, this work opens research avenues for the oxidation of related organic molecules from renewable feedstocks. The latter half of the presentation will pivot to the domain of hydrogen fuel cells, centered on the utilization of phthalocyanine-based MOF materials with dual active centers (M-N4 moieties, M1 = amine coordinated metal node, M2 = phthalocyanine center) that can facilitate the ORR. In a combined experimental and theoretical approach, we correlate structural properties (choice and placement of transition metals) with electrochemical performance (activity, selectivity, and material stability) during ORR. Moreover, we highlight metal and site dominance (M1 vs. M2) with insights into possible MOF degradation pathways using preferential metal dissolution profiles. This presentation aims to present a comprehensive understanding of these complex systems and pave the way for practical and scalable solutions to current and future energy challenges.

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 2023; ©2023
Publication date 2023; 2023
Issuance monographic
Language English

Creators/Contributors

Author Wei, Lingze
Degree supervisor Jaramillo, Thomas
Thesis advisor Jaramillo, Thomas
Thesis advisor Bao, Zhenan
Thesis advisor Cargnello, Matteo
Degree committee member Bao, Zhenan
Degree committee member Cargnello, Matteo
Associated with Stanford University, School of Engineering
Associated with Stanford University, Department of Chemical Engineering

Subjects

Genre Theses
Genre Text

Bibliographic information

Statement of responsibility Lingze Wei.
Note Submitted to the Department of Chemical Engineering.
Thesis Thesis Ph.D. Stanford University 2023.
Location https://purl.stanford.edu/wm970pk4006

Access conditions

Copyright
© 2023 by Lingze Wei
License
This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).

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