Interfacial Structure and Reactivity
Can we control, and autonomically respond to, the reactions at the oxide-electrolyte interface by leveraging a robust, molecular-scale understanding of its structure and reactivity?
The transport of ions across the electrode/electrolyte interface can lead to kinetic barriers and over-potentials, as well as side reactions associated with interface-specific reaction pathways. Decomposition at electrode potentials that exceed the stability window of the electrolyte is associated with buildup of secondary products, broadly referred to as the “solid electrolyte interphase.” Also, the well-known problem of solid-phase instabilities at extreme potentials, exemplified by metal dissolution from manganese (Mn)-based electrode surfaces at the extreme potentials found in next-generation lithium-ion battery systems, remains poorly understood and is a severe technological limitation. These interfacial aspects of electrochemistry introduce substantial challenges, but simultaneously offer many avenues for controlling and guiding reactivity through interfacial modification.