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Investigations of Copper Catalyzed CO2 Reduction With Molecular Copper Models, Technoeconomics, and Green Policy / Walter D Johnsen.

Dissertations & Theses @ University of Pennsylvania Available online

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Format:
Book
Thesis/Dissertation
Author/Creator:
Johnsen, Walter D., author.
Contributor:
University of Pennsylvania. Chemistry, degree granting institution.
Language:
English
Subjects (All):
Inorganic chemistry.
Energy.
Chemistry.
Chemistry--Penn dissertations.
Penn dissertations--Chemistry.
Local Subjects:
Inorganic chemistry.
Energy.
Chemistry.
Chemistry--Penn dissertations.
Penn dissertations--Chemistry.
Physical Description:
1 online resource (225 pages)
Distribution:
Ann Arbor : ProQuest Dissertations & Theses, 2023
Contained In:
Dissertations Abstracts International 85-08B.
Place of Publication:
[Philadelphia, Pennsylvania] : University of Pennsylvania, 2022.
Language Note:
English
Summary:
Decarbonizing the chemical sector, which is responsible for 8% of annual greenhouse gas emissions, is an acute challenge. The reduction of carbon dioxide (CO2) to multi-carbon products by copper heterogenous electrocatalysts offers an avenue to produce high value chemicals at low carbon intensities. State of the art copper catalysts are unselective and inefficient, preventing their commercialization. However, adding electronegative dopants on the copper surface and Lewis acid additives to reaction conditions can increase the selectivity of copper catalysts for multi-carbon products. Herein, we examine these chemical strategies using non-catalytic molecular dinuclear copper complexes as models for the copper surface. With voltammetry, high pressure electrochemistry, and spectroelectrochemistry, we measure kinetic and thermodynamic parameters of key elementary steps in the CO2 reduction pathway. Our results suggest that additives and electron-withdrawing dopants increase the affinity of copper with CO - an intermediate in CO2 reduction. We also ask what performance targets do copper photoelectrocatalysts and electrocatalysts need to achieve to become market viable and answer this question using a technoeconomic analysis. The thesis concludes by looking at re-tooling existing financial mechanisms to support equitable deployment of emergent green technologies, such as CO2 electrochemical and photochemical reduction systems.
Notes:
Source: Dissertations Abstracts International, Volume: 85-08, Section: B.
Advisors: Goldberg, Karen I.; Mallouk, Thomas E.; Committee members: Schelter, Eric J.; Tomson, Neil C.; Berry, Donald H.
Department: Chemistry.
Ph.D. University of Pennsylvania 2023.
Local Notes:
School code: 0175
ISBN:
9798381510829
Access Restriction:
Restricted for use by site license.

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