A Universal Strategy toward the Precise Regulation of Initial Coulombic Efficiency of Li‐Rich Mn‐Based Cathode Materials

Li-rich Mn-based cathode materials (LRMs) are potential cathode materials for high energy density lithium-ion batteries. However, low initial Coulombic efficiency (ICE) severely hinders the commercialization of LRM. Herein, a facile oleic acid-assisted interface engineering is put forward to precisely control the ICE, enhance reversible capacity and rate performance of LRM effectively. As a result, the ICE of LRM can be precisely adjusted from 84.1% to 100.7%, and a very high specific capacity of 330 mAh g^-1 at 0.1 C, as well as outstanding rate capability with a fascinating specific capacity of 250 mAh g^-1 at 5 C, are harvested. Theoretical calculations reveal that the introduced cation/anion double defects can reduce the diffusion barrier of Li⁺ ions, and in situ surface reconstruction layer can induce a self-built-in electric field to stabilize the surface lattice oxygen. Moreover, this facile interface engineering is universal and can enhance the ICEs of other kinds of LRM effectively. This work provides a valuable new idea for improving the comprehensive electrochemical performance of LRM through multistrategy collaborative interface engineering technology.