The conversion of solar energy into a useful chemical fuel represents a major scientific goal in the drive towards a society fully powered by renewable energy.  Several potential fuel targets exist including hydrogen from proton reduction, and various hydrocarbons from carbon dioxide reduction. To achieve meaningful rates of fuel production, any of these potential reduction reactions must be coupled to an oxidative reaction that generates electrons and protons. The most sensible candidate to provide these electrons and protons is water, which can be decomposed <i>via</i> the oxygen evolution reaction (OER). For solar fuel applications, this water-splitting half reaction must be catalyzed to make it energetically efficient, as accomplished in nature's photosynthesis by a tetra-manganese oxo cluster (the oxygen-evolving complex, OEC). Indeed, related transition-metal oxo cubane clusters represent intriguing model systems and catalyst design motifs for development of new water-splitting catalysts based on the most abundant metals. Molecularly derived catalysts of this type offer a number of potential advantages, including the synthetic tunability of structure-activity relationships and chemical properties. Also, the study of model, high-valent molecular species can provide key insights into the mechanism of water oxidation, and thereby help bridge the gap between heterogeneous and homogeneous systems to allow for more rational design of catalysts.

Molecular design and stabilization of metal oxo clusters for challenging electrocatalytic, sustainable transformations

2019 Spring National Meeting

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