CAREER: Probing and Controlling Acidic Electrocatalytic Oxidation Mechanisms and Catalyst Degradation Processes

As our global energy supply expands to meet growing demands and evolves to incorporate a larger fraction of renewable sources, we must adapt our fuel and chemical production industry to effectively utilize, convert, or store these vital resources. Electrocatalytic processes provide a sustainable route to convert and store renewable electricity in the form of chemical bonds and mitigate spatiotemporal mismatch between variable supply and demand. Fuel- and chemical-producing reduction reactions require an electron donating counter reaction, ideally using an abundant resource such as water. Therefore, the oxidation of water to molecular oxygen, also known as the oxygen evolution reaction (OER), plays a critical role in these technologies. Several mechanisms have been proposed for the OER which involve both coupled and non-coupled proton-electron transfer steps, as well as varying degrees of lattice oxygen activation. However, few of these mechanisms have been experimentally validated, and only for a limited set of catalyst surfaces and reaction conditions. Fundamental understanding of dynamic catalyst properties that activate specific OER mechanisms is critical to effectively design highly active, stable catalysts. The overarching goal of this NSF CAREER proposal is to understand and manipulate the relationship between precisely tuned metal oxide catalysts and OER mechanisms in acidic conditions, addressing the effects of metal electronic structure, lattice oxygen activation, oxygen vacancies, and material stability, to enable optimized catalyst design and operation. The proposed work leverages the PI’s experience in metal oxide materials, oxidative electrocatalysis, and advanced in situ spectroscopy techniques. Tightly integrated with this proposed research is a sustainable plan for attracting and improving retention of diverse students to STEM fields through collaborative development and implementation of new curriculum that emphasizes student engagement and fulfills Next Generation Science Standards, by working with Chicago Public High School teachers.