Development of stable metal oxide electrodes for the conversion of electricity to chemical fuels

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Abstract/Contents

Abstract
The conversion of renewable sources of electricity to molecular fuels is widely viewed as an important component of our future energy economy. To accomplish this, stable electrodes are necessary to perform electrochemical reactions of interest for extended periods of operation with high efficiency. In the first part of this thesis, a method to immobilize homogeneous catalysts to a metal oxide electrode through click chemistry on an attached p-azidophenyl phosphonic acid linker is presented. This strategy allows for a convergent approach to surface modification that results in stable attachments while allowing for facile charge transfer between the electrode and the immobilized catalyst. The deposition of p-azidophenyl phosphonic acid to the metal oxide surface and subsequent click with molecules of interest was investigated with Fourier transform infrared spectroscopy, electrochemistry and X-ray photoelectron spectroscopy. The electrochemical oxidation of water to supply the electrons need for fuel synthesis remains a challenge due to the lack of materials which can both efficiently remove four electrons and withstand the harsh oxidative conditions of the reaction. A novel type of dimensionally stable anode utilizing silicon as the base substrate and also as an in-situ photon collector has been developed. It uses a thin amount of titanium dioxide as a protective layer deposited by atomic layer deposition. A thin layer of physical vapor deposited iridium is used as the water oxidation catalyst. Results shown include water oxidation efficiency in both light and dark conditions and over a range of pH values with an emphasis on the operational stability and durability of the anodes.

Description

Type of resource text
Form electronic; electronic resource; remote
Extent 1 online resource.
Publication date 2011
Issuance monographic
Language English

Creators/Contributors

Associated with Prange, Jonathan David
Associated with Stanford University, Department of Chemistry
Primary advisor Chidsey, Christopher E. D. (Christopher Elisha Dunn)
Thesis advisor Chidsey, Christopher E. D. (Christopher Elisha Dunn)
Thesis advisor Stack, T. (T. Daniel P.), 1959-
Thesis advisor Waymouth, Robert M
Advisor Stack, T. (T. Daniel P.), 1959-
Advisor Waymouth, Robert M

Subjects

Genre Theses

Bibliographic information

Statement of responsibility Jonathan David Prange.
Note Submitted to the Department of Chemistry.
Thesis Ph.D. Stanford University 2011
Location electronic resource

Access conditions

Copyright
© 2011 by Jonathan David Prange
License
This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).

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