Energy-efficient CO2/CO interconversion by homogeneous copper-based molecular catalysts

Abstract

Facile conversion of CO2 to commercially viable carbon feedstocks offer a unique way to adopt a net-zero carbon scenario. Synthetic CO2-reducing catalysts have rarely exhibited energy-efficient and selective CO2 conversion. Here, the carbon monoxide dehydrogenase (CODH) enzyme blueprint is imitated by a molecular copper complex coordinated by redox-active ligands. This strategy has unveiled one of the rarest examples of synthetic molecular complex-driven reversible CO2 reduction/CO oxidation catalysis under regulated conditions, a hallmark of natural enzymes. The inclusion of a proton-exchanging amine groups in the periphery of the copper complex provides the leeway to modulate the biases of catalysts toward CO2 reduction and CO oxidation in organic and aqueous media. The detailed spectroelectrochemical analysis confirms the synchronous participation of copper and redox-active ligands along with the peripheral amines during this energy-efficient CO2 reduction/CO oxidation. This finding can be vital in abating the carbon footprint-free in multiple industrial processes.