For solar fuels applications, efficient catalysis of the water-splitting half reaction is an important process. In nature's photosynthesis, this is accomplished 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 solid-state and molecular systems to allow for more rational design of catalysts. This presentation will describe high-valent metal complexes and clusters, and a detailed mechanism for the evolution of oxygen <i>via</i> water oxidation at a tetranuclear cobalt oxo cubane. An important aspect to this catalysis relates to the manner in which metals cooperate to mediate the multi-electron, multi-proton oxidation of water. To further probe this aspect, the synthesis of a range of related, heterometallic oxo clusters have been targeted.<br/>

Mechanisms of oxidation with heterometallic oxo clusters

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.