Atmospheric CO2 concentrations have reached their highest to date, which holds immediate and dire consequences for the environment and all areas of human health. Based on these imminent and growing threats, there is an urgent need to transition our current infrastructure from fossil fuels to renewable energy sources. In this context, solar energy could be used to drive the catalytic conversion of CO2 and H2O into energy-rich chemicals whereby energy is stored indefinitely in chemical bonds for on-demand use. One approach is to employ molecular electrocatalysts due to the versatility and tunability of their electronic and geometric parameters. However, despite the number of synthetic catalysts, several challenges remain in the use of earth-abundant or inexpensive materials for CO2 fixation. Conversely, carbon monoxide dehydrogenase (CODH) enzymes are able to extract energy from their environments in order to carry out the reversible conversion of CO to CO2 at high rates and selectivity while operating near the thermodynamic potential. Here, we employ computational chemistry in conjunction with experimental efforts to design molecular electrocatalysts that mimic essential structural features and functions of CODH for CO2 reduction to value-added products.

Understanding the electronic structure and reactivity of carbon monoxide dehydrogenase model systems for carbon dioxide reduction

2019 Fall National Meeting

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