We are investigating copper-tungsten binuclear complexes as potential catalysts for hydrogen production and carbon dioxide activation. The square pyramidal environment around tungsten mimics the molybdenum center in carbon monoxide dehydrogenase, which is known to catalyze a reaction similar to water-gas shift reaction. These complexes undergo reversible two-electron redox processes associated with TM(IV)/TM(VI) interconversion. The copper center is bridged to tungsten through a sulfide bond and is known to maintain a +1 oxidation state in the native enzyme. Density functional theory and pseudopotentials have been employed to profile the energetics of the catalytic cycle. To determine the most favorable reaction pathway, a series of analogues involving redox-active ligands have been tested. In this presentation, we describe the influence of metal center and ligand environment on energy profiles.

Carbon monoxide dehydrogenase mimics for catalytic production of hydrogen

248th National Meeting (2014)

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