Oxygen-atom functionalization of chemical intermediates to generate epoxides and lactones is critical for the production of diverse textiles, plastics, and pharmaceuticals. The wet chemical and thermochemical routes used today suffer from large carbon dioxide footprints, stoichiometric waste products, and hazardous reagents. In this presentation, we will discuss methods by which water can be used as the oxygen source in functionalization reactions, including epoxidation and lactonization, with tailored metal and metal oxide nanoparticle anodic electrocatalysts. At the cathode, hydrogen is selectively generated, reflecting that this reaction can be thought of as a derivative of water splitting, in which the oxidizing equivalents go towards generating a valuable product rather than generating molecular oxygen. Doping the surface with single atoms can provide tunablility over oxygen electrophilicity, a critical parameter in controlling epoxidation rates. We have developed mechanistic understanding of how water is oxidized, providing means by which the selectivity for oxygen-atom functionalization can be rationally improved.

Controlling electrocatalytic oxygen-atom transfer reactions

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