Multi-electron, multi-proton processes underpin catalytic transformations that convert energy-poor feedstock molecules into energy-dense fuels. The specific proton-coupled electron transfer reaction mechanisms that a catalyst navigates in a fuel production reaction can dramatically impact the efficiency, durability, and selectivity of the system. The overarching goal of this research program is to develop a detailed understanding of the proton-coupled electron transfer processes that underpin multi-electron, multi-substrate fuel-forming reactions in order to enhance catalyst efficiency, selectivity, and durability.

The proposed research will study the proton-coupled electron transfer pathways by which fuel-forming catalysts and relevant model systems operate. The structural and electronic factors that influence the specific reaction pathways that these species operate through will be identified. The proton-coupled electron transfer reaction kinetics that form key reaction intermediates will be quantified, and used to understand how reaction dynamics influence the product selectivity. Further, the proton-coupled electron transfer reactivity of model complexes will be studied at an electrode interface in order to understand how the local interfacial environment influences the mechanism and kinetics of the reaction.

In the course of this research, key design principles will be identified for catalysts that operate with enhanced efficiency and are highly selective for desired fuel products.