Unlocking Electrochemical-Driven Surface Oxygen Vacancies-Regulated Cathode–Electrolyte Interphase for Stabilizing Li-Ion Cells

Abstract A stable cathode–electrolyte interphase (CEI) significantly enhances the durability of lithium-ion batteries; however, the intricate chemistry underlying its formation makes predesign exceedingly challenging. This work demonstrates that surface oxygen vacancy (OV) concentration dually regulates CEI thickness and composition. We develop an in situ strategy where Li 2 C 4 O 4 incorporation into LiCoO 2 (LCO) spontaneously decomposes during cycling, generating surface OVs. Combined experim