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Storage of Energy in Chemical Bonds Utilizing Earth-Abundant Molecular Electrocatalysts: Improving Catalyst Design Through an Understanding of Mechanism181 views
Author
Nichols, Asa, Chemistry - Graduate School of Arts and Sciences, University of Virginia0000-0002-8480-5118
Advisors
Machan, Charles, AS-Chemistry, University of Virginia
Abstract
The studies described in this dissertation focus on the use of N<sub>2</sub>O<sub>2</sub> ligands in the CO<sub>2</sub> reduction reaction and the oxygen reduction reaction. The use of Fe and Co metal centers in these ligand frameworks leads to different reactivity profiles. Chapter 2 of this dissertation focuses on the synthesis, characterization, and reactivity of an Fe(N<sub>2</sub>O<sub>2</sub>) compound towards CO<sub>2</sub> under electrochemically reducing conditions in the presence of phenol for the production of formate. These studies are continued in Chapter 3 with a focus on studying how secondary-sphere moieties oriented towards the protonation-sensitive Fe-bound phenolate ligands affect catalytic reactivity towards CO<sub>2</sub>. Chapter 4 focuses on synthesis, characterization, and reactivity of a Co(N<sub>2</sub>O<sub>2</sub>) compound towards the oxygen reduction reaction. These oxygen reduction studies are continued in Chapter 5 with a focus on studying how secondary-sphere moieties oriented towards the catalytically active Co metal center affect catalytic reactivity towards O<sub>2</sub>. Finally, Chapter 6 summarizes the previous chapters and outlines preliminary results and future directions for new projects.
Nichols, Asa. Storage of Energy in Chemical Bonds Utilizing Earth-Abundant Molecular Electrocatalysts: Improving Catalyst Design Through an Understanding of Mechanism. University of Virginia, Chemistry - Graduate School of Arts and Sciences, PHD (Doctor of Philosophy), 2021-04-27, https://doi.org/10.18130/205a-0312.
