Carbon dioxide emissions have continued to rise in recent years as a result of the ongoing burning of fossil fuels— an issue that has brought significant interest to chemical methods that can use CO2 as a potential feedstock for energy-rich molecules. One method used to improve mechanistic understanding of the CO2 reduction reaction (CO2RR), and thereby aid the development of new electrocatalysts that are inexpensive, robust, and efficient, is to employ electronic structure calculations. Two of the largest challenges in the development of electrocatalysts for CO2RR are (a) designing molecules that can selectively activate CO2 in the presence of water and (b) doing so while maintaining relatively low overpotentials. To date, performance of this kind has been seen in iron porphyrins, and cobalt and nickel tetraaza macrocycles, such as [Ni(cyclam)]2+. Our research is focused on using computational methods to understand the mechanism by which the electrocatalytic reduction of CO2 to CO is facilitated by novel earth-abundant macrocycle-like catalysts, and specifically the role that N-heterocyclic carbene (NHC) ligands can play in stabilizing the metal-CO2 adduct.

Computational studies of earth-abundant macrocycle-like electrocatalysts for CO2 reduction

255th National Meeting (2018)

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