Electronic Theses and Dissertations

Date of Award

2019

Document Type

Thesis

Degree Name

M.S. in Chemistry

Department

Chemistry and Biochemistry

First Advisor

Jonah Jurss

Second Advisor

Walter Cleland

Third Advisor

Jared H. Delcamp

Relational Format

dissertation/thesis

Abstract

Since the Industrial Revolution, the consumption of fossil fuels has increased dramatically worldwide. The combustion of fossil fuels leads to the generation of carbon dioxide (CO2) emissions. CO2 is a greenhouse gas, but also a C1 feedstock that could be utilized for the generation of renewable fuels and commodity chemicals. However, CO2 is chemically inert and typically demands strong chemical reductants or very negative potentials before it undergoes conversion into reduced carbon products. The desire to carry out CO2 conversion in the presence of water presents a significant challenge, as protons may be reduced to hydrogen gas rather than facilitating the proton-coupled reduction of CO2. Thus, catalysts that are selective for CO2 reduction over proton reduction are required. In this context, our strategy for accessing renewable energy involves the design of new homogeneous catalysts employing polyaromatic ligand platforms, which aim to lower the overpotential for CO2 conversion or be utilized as tunable and stable redox shuttles for more efficient dye-sensitized solar cells (DSCs). The rational design, synthesis, and characterization of new transition metal complexes, and their application in electrocatalytic CO2 reduction or in DSC solar-to-electric energy technologies are discussed.

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