Proton-coupled electron transfer (PCET) processes play an important role in facilitating the multi-electron, multi-proton reactions such as water oxidation, C–H activation, CO2 reduction, and proton reduction. While many catalysts have been developed to improve the efficiency and selectivity of these fuel forming reactions, there is a dearth of mechanistic information regarding how we can control and fine-tune the PCET reactivity of catalytic intermediates (i. e., metal-oxo and metal-hydride species) that underpin the aforementioned metrics. Herein, structural and electronic modifications of molecular complexes have enabled isolation of elusive intermediates and illuminated key mechanistic insights into how these reactive species mediate PCET reactions. The fundamental understandings gained from these studies enable construction of structure-activity relationships and elucidation of design principles for promoting PCET reactivity relevant to fuel forming catalysis.

Controlling proton-coupled electron transfer processes underpinning fuel forming catalysis through synthetic modifications

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ACS Fall 2022

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