Electronic Theses and Dissertations

Date of Award

1-1-2021

Document Type

Dissertation

Degree Name

Ph.D. in Chemistry

Department

Chemistry and Biochemistry

First Advisor

Jared H. Delcamp

Second Advisor

Jonah W. Jurss

Third Advisor

Walter Cleland

Relational Format

dissertation/thesis

Abstract

Molecular CO2 and H+ reductive catalysts, whether they be electro- or photocatalytic, have been shown to be possible routes of harnessing solar energy in a clean, renewable manner. There are few electrocatalysts operating at reasonable overpotentials to prove useful in artificial photosynthetic systems, and there are a number of environmental factors within these systems that have yet to be evaluated. Photo-driven catalysis is rare, difficult to control, and rarely provides high-value CO2 reduction products. I report herein an exceptionally low overpotential H+ reduction catalyst, a method of modulating electrocatalysts in-situ to improve performance, a first-of-its-kind mononuclear proton reduction photocatalyst, a method of predicting the best labile ligand for a photocatalyst, and a series of highly durable macrocyclic nickel complexes shown to produce methane via visible light.

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