In recent years, CO2 emissions have risen as a result of the increased burning of fossil fuels, an issue that has brought new interest to chemical methods that can convert CO2 into energetically favorable fuels. One way to better understand the mechanism for the CO2 reduction reaction (CO2RR) and therefore develop electrocatalysts that are inexpensive, robust, and efficient, is to employ electronic structure calculations. One of the largest challenges in the development of electrocatalysts for CO2RR is designing molecules that can selectively activate CO2 in the presence of water while maintaining relatively low overpotentials. To date, performance of this kind has been seen in iron porphyrins, cobalt and nickel polyamine macrocycles, such as [Ni(cyclam)]2+. In 2011, the Chang group developed nickel N-heterocyclic carbene-pyridine complexes that displayed high selectivity for the electrocatalytic reduction of CO2 in the presence of water. Our research has focused on using computational methods to better understand the mechanism by which the electrocatalytic reduction of CO2 to CO is facilitated by nickel macrocycle-like catalysts, specifically the role that ligand dissociation may play in stabilizing the Ni-CO2 adduct.

Computational investigations of nickel based electrocatalysts for CO2RR

254th National Meeting (2017)

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