Countering Voltage Decay, Redox Sluggishness, and Calendering Incompatibility by Near‐Zero‐Strain Interphase in Lithium‐Rich, Manganese‐Based Layered Oxide Electrodes

Abstract Lithium‐rich, manganese‐based layered oxides are considered one of the most valuable cathode materials for next generation high‐energy density lithium‐ion batteries (LIBs) their high specific capacity and low cost. However, practical implementation in LIBs is hindered by rapid voltage/capacity decay on cycling long‐standing contradictions between redox kinetics volumetric energy due to poor calendaring compatibility. Herein, a coherent near‐zero‐strain interphase constructed grain boundaries secondary particles infusing LiAlO 2 material through reactive infiltration method (RIM). Theoretical calculations, multi‐scale characterizations, electrochemical tests show that this with feature upon (de)lithiation inhibits volume changes lattice structural degradation primary during cycling. More importantly, ionically conductive nanolayer infiltrated can not only promote Li + migration act as barrier protect from corrosion electrolyte but also effectively improve mechanical strength particles. Collectedly, ‐infiltrated display superior cyclability, enhanced rate capability, industrial performance, marking significant step toward commercial implementation.