Transition-metal coordination compounds provide versatile platforms for mechanistic studies of reductive catalysis in artificial photosynthesis. Our work focuses on the application of transient methods, including laser and radiation techniques, augmented by advanced theoretical modeling to characterize transient intermediates formed during the catalytic reduction of CO2 and protons. In particular, the use of pulse radiolysis with IR detection enables the production and detailed characterization of highly reactive transient intermediates such as metal–CO2, metal–CO, and metal–H species.1,2 This in turn allows one to interrogate the advanced stages of a catalytic cycle, where steady state concentrations of intermediates are typically small. We will present new results on such intermediates using [CoII(L)]2+ (L = 5,7,7,12,14,14-hexamethyl-1,4,8,11-tetraazacyclotetradeca-4,11-diene) and [CoIIL′(Cl)]Cl (L′ = N,N-bis(2-pyridinylmethyl)-2,2′-bipyridine-6-methanamide or its derivatives).

Intermediates in catalytic CO2 and proton reduction investigated by pulse radiolysis

2019 Spring National Meeting

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