Heterobimetallic complexes with effective ligand designing can unravel the novel arenas of reactivity and catalysis with multimetallic cooperativity. Continuous decades of research in conversion of the greenhouse gas, carbon dioxide to the chemical feedstocks has focused our attention to the efficient conversion of CO2 to CO by the carbon monoxide dehydrogenase metalloenzyme. The [NiFe] CO dehydrogenase enzyme performs anaerobic reversible catalytic conversion of CO2 to CO with high rate and turnover numbers. Prior research in this field successfully characterized intermediates with single crystal X-ray crystallography and permitted a proposed mechanistic cycle. However, there is no report of nickel-iron bimetallic molecular systems which can perform the function of enzyme catalytically and reversibly with metal-metal and metal-ligand cooperation. A synthetic route to a novel double decker ligand framework which can enable a cooperative substrate binding was pursued. The heterobimetallic [NiFe] complex system with phosphine ligated nickel atom and nitrogen ligated iron atom was successfully synthesized in good yield and further characterized with NMR and X-Ray crystallography techniques. The preliminary results reveal the reaction of CO2 with the bimetallic complex.

Mimicking of the function of [NiFe] CO dehydrogenase enzyme

ACS Spring 2022

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