Improvement in the development of transition metal oxides for energy conversion processes will ultimately depend on an improved understanding of interfacial processes and the surface chemistry of these materials. In particular, redox reactions that occur at the surface of these materials will dictate functionality of these systems and have been shown to be strongly dependent on the presence of charge-compensating counter ions, such as protons. Additionally, recent work has shown that metal oxide nanoparticles are capable of acting as proton-coupled electron transfer (PCET) reagents. However, challenges in studying nano-sized materials have led our group to utilize polyoxometalates as atomically precise analogues. POMs posses a comparable morphology, delocalized electronic structure, and high solubility and stability in organic solvents, suggesting that these compounds are promising candidates for modeling PCET-type reactions at metal oxide surfaces. The work presented here demonstrates the ability for polyoxovanadate-alkoxide clusters to act as proton-coupled electron transfer reagents and allows for a detailed analysis of kinetics and mechanisms of these processes.

Polyoxometalates as models for proton-coupled electron transfer type reactions at metal oxide surfaces

ACS Fall 2021

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