Catalytic reduction of CO2 represents an attractive approach to the generation of new chemical feedstocks for the production of liquid fuels. However, economic feasibility of such processes requires the development of efficient and robust catalysts. While some of the best catalysts used for CO2 reduction are based on the use of precious metals, there is a growing desire to develop catalysts based on readily available, earth-abundant transition metals. Utilizing thermodynamic insights into the hydricity of transition metal hydrides as a guiding principle, we have developed a series of heteroleptic nickel complexes with bis-N-heterocyclic carbene and diphosphine ligand frameworks. These complexes undergo reversible, two-electron reductions whose potential can be tuned by substitution of simple diphosphine chelates. Tuning the electronics at the nickel center provides a direct method of influencing the hydricity of the corresponding metal hydride, affording a platform to generate species capable of reducing CO2 electrocatalytically.

Tuning the hydricity of nickel hydrides for the electrocatalytic reduction of CO2

255th National Meeting (2018)

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