Date of Award:

5-2016

Document Type:

Thesis

Degree Name:

Master of Science (MS)

Department:

Chemistry and Biochemistry

Committee Chair(s)

Yujie Sun

Committee

Yujie Sun

Committee

Tianbiao Liu

Committee

Nicholas E. Dickenson

Abstract

The growing global energy demand and the increasing concentration of CO2 in the atmosphere have encouraged the development of renewable energy to replace carbon-based fossil fuels. Electrocatalytic water splitting to form H2 and O2 and reduction of CO2 to CO are appealing processes and we can be directly utilize H2 and CO as fuels or commodity chemicals in mature industrial processes, which will not alter the current carbon cycle. However, the O2 evolution reaction of water splitting is a reaction of four-proton and four-electron transfer process, whose kinetics is very sluggish under normal conditions. Similarly, the large-scale deployment of CO2 reduction is also challenging because of the thermodynamic stability of CO2. The thermodynamic potential of CO2 reduction to CO is -0.53 V vs standard hydrogen electrode (SHE) at pH 7, while the H2 evolution reaction requires a less negative potential of -0.413 V (vs SHE). Therefore, it is imperative to develop CO2 reduction catalysts with a particularly high selectivity over H2 evolution reaction in the presence of H2O or other proton sources. At present, typical water oxidation and CO2 reduction catalysts are mostly based on noble metals. However, practical applications are limited by their scarcity. The lack of molecular-level mechanistic understanding of catalytic active sites also impedes their further development.

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