The energy efficient conversion of atmospheric CO2 into useful chemical feedstocks via earth-abundant catalysts has long been a desired goal in the field of synthetic chemistry. Nature has developed the metalloenzyme NiFe carbon monoxide dehydroganse which is able to catalyze the conversion between CO2 and CO reversibly only using protons and electrons. The active C-cluster of the enzyme has been shown to cooperatively bind CO2 between two metal centers, poising it for reactivity. Utilizing design elements derived from the enzyme, a set of nickel bimetallic complexes in an “open-face” pincer ligand were synthesized. Biomimetic NiFe and NiSn complexes were targeted for their potential cooperative CO2 activation and subsequent reduction. The novel dianionic ligand allows for the isolation of Ni(II)M(II) complexes with and without bridging ligands. Further reduced oxidation states were isolated and structurally characterized. The reactivity with CO2 was explored for both metal pairings.

Bioinspired nickel complexes in a metallopincer framework

ACS Spring 2022

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