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Metal Oxides for Hydrogen Activation and Sustainable Chemical Conversions

Miu, Evan V (2023) Metal Oxides for Hydrogen Activation and Sustainable Chemical Conversions. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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Our green, renewable future remains an unsatisfyingly distant reality. Although we are taking actions to suppress anthropogenic harm to the natural world, there is scientific consensus that radical changes are needed today to avoid significant ecological and climate damage. In this direction, a hydrogen-based economy has been proposed as a sustainable alternative to a fossil-based economy. Hydrogen is receiving such attention because it has the potential to be carbon-free, producing only water when used as a fuel. However, the production of hydrogen is currently tightly linked to fossil fuels, and fossil-free methods remain under-developed. Sourcing hydrogen from water and renewable electricity has been proposed as a significant opportunity for making positive steps towards a more sustainable future.

This dissertation focuses on the development of catalytic schemes that combine water electrolysis and hydrogenation chemistries through mediated hydrogen transfers. The specific approach uses metal oxide hydrogen bronzes to electrocatalytically activate hydrogen from water and then supply it for general hydrogenation chemistries. It is worth noting that the chemical industry is the leading consumer of hydrogen, and it will remain so for many decades. This work is driven by the hypothesis that these bronzes offer fine control over the activity of hydrogen and can be tuned
to accommodate specific hydrogenations. Research herein includes fundamental studies of the thermodynamics, transport phenomena, and kinetics of hydrogen intercalation into metal oxides. Additionally, a mediated hydrogenation using tungsten oxide is demonstrated. Overall, this research offers foundational knowledge of bronze-mediated hydrogenations and presents a means for environmentally benign hydrogen utilization, bringing us closer to a sustainable chemical industry.


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Item Type: University of Pittsburgh ETD
Status: Unpublished
CreatorsEmailPitt UsernameORCID
Miu, Evan Vevm24@pitt.eduevm240000-0003-0429-5101
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee CoChairMcKone,
Committee CoChairMpourmpakis,
Committee MemberKeith,
Committee MemberVeser,
Committee MemberGilbertson,
Date: 14 September 2023
Date Type: Publication
Defense Date: 13 June 2023
Approval Date: 14 September 2023
Submission Date: 22 June 2023
Access Restriction: No restriction; Release the ETD for access worldwide immediately.
Number of Pages: 223
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: hydrogen, electrocatalysis, catalysis, metal oxide
Date Deposited: 14 Sep 2023 13:40
Last Modified: 14 Sep 2023 13:40

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