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Employing Electroanalysis as a Diagnostic Tool to Enable Carbon-free Energy Supply

Sawant, Tejal V (2021) Employing Electroanalysis as a Diagnostic Tool to Enable Carbon-free Energy Supply. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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Abstract

Fossil fuel-based energy has been instrumental over the last century to satisfy the socioeconomic welfare of humankind. However, the continuous increase in population and resource consumption places a significant strain on the limited supply of fossil fuels available in the world. Moreover, fossil fuel consumption gives rise to negative environmental impacts, particularly greenhouse gas emissions that contribute to global climate change. Thus, there is a clear and pressing need for the development of carbon-free energy technologies as alternatives to fossil fuels. This dissertation focuses on leveraging the tools of applied electroanalysis to advance the development of a carbon-free energy supply. The work described herein encompasses two overarching research objectives:
1. to improve the energy efficiency of Redox Flow Batteries (RFBs) by developing highly catalytic, robust electrodes for the associated electron-transfer reactions.
2. to increase the long-term stability of nuclear reactors by mitigating the effects of Zircaloy corrosion under the unique photochemical conditions of nuclear fission.
In the field of RFBs, we developed an electroanalytical platform for precise and accurate characterization of interfacial electron transfer kinetics at technologically relevant flow battery conditions. Additionally, we modulated the surface chemistry of carbon and established pretreatment strategies that resulted in ten times faster kinetics for the Fe redox chemistry. In the nuclear energy domain, we confirmed that the passivating oxides that form on Zr under nuclear reactor conditions behave as semiconductor photoanodes, which influences the corrosion performance of Zr-based cladding materials. We further developed a mechanistic understanding of the degradation of Zr oxides under these conditions of high energy radiation. Overall, this work demonstrated the importance of electrochemical catalysis in the design of RFBs and provided an impetus to develop more corrosion resistant alloys for use in nuclear reactors, thus advancing the path toward a carbon-free energy supply.


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Details

Item Type: University of Pittsburgh ETD
Status: Unpublished
Creators/Authors:
CreatorsEmailPitt UsernameORCID
Sawant, Tejal Vtvs8@pitt.edutvs80000-0003-4517-789X
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Thesis AdvisorMcKone, James Rjmckone@pitt.edu
Committee MemberFullerton, Susanfullerton@pitt.edu
Committee MemberVeser, Goetzgveser@pitt.edu
Committee MemberLi, Leilel55@pitt.edu
Date: 13 June 2021
Date Type: Publication
Defense Date: 7 December 2020
Approval Date: 13 June 2021
Submission Date: 9 January 2021
Access Restriction: 1 year -- Restrict access to University of Pittsburgh for a period of 1 year.
Number of Pages: 172
Institution: University of Pittsburgh
Schools and Programs: Swanson School of Engineering > Chemical and Petroleum Engineering
Degree: PhD - Doctor of Philosophy
Thesis Type: Doctoral Dissertation
Refereed: Yes
Uncontrolled Keywords: redox flow battery, electroanalysis, kinetics, catalysis, electrochemical energy storage, interfacial electron transfer, corrosion, high energy radiation, Zircaloy, nuclear reactor, photoelectrochemistry, zirconium oxide
Date Deposited: 13 Jun 2021 18:13
Last Modified: 13 Jun 2021 18:13
URI: http://d-scholarship.pitt.edu/id/eprint/40149

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