“Deciphering Oxygen-Evolution Catalysis with Synthetic Metalloclusters”

Abstract

Natural and artificial photosynthesis relies on the highly endergonic oxidation of water to dioxygen (the oxygen-evolution reaction or OER) to store solar-derived energy. Multimetallic motifs like the cofactor of photosystem II and heterogeneous metal oxides are adept at catalyzing the OER. Due to the complexity of enzymatic and heterogeneous catalysts, the mechanism of these catalysts has been difficult to elucidate. My work has involved modeling these complex systems with synthetic metalloclusters. I will present on how synthetic manipulations of cobalt-oxo clusters have yielded detailed insights on the structures, reactivity, and kinetic behavior of intermediates in cobalt-catalyzed OER. In addition, I will discuss the approaches for rationally designing new multimetallic architectures and an expeditious strategy to obtain polydentate ligands for metalloclusters.