Interfacial Chemistry Regulation via AlPO ₄ Modification Enables Fast Charging and Wide‐Temperature Operation of Graphite Anodes for Lithium‐Ion Batteries

ABSTRACT Graphite remains the dominant anode for commercial lithium‐ion batteries (LIBs), yet it suffers from sluggish reaction kinetics and interphase instability under long‐term cycling and extreme‐temperature conditions, which hinder the high rate performance, longevity and environmental adaptability of LIBs. Herein, an interfacial chemistry regulation strategy via AlPO 4 (APO) surface modification is proposed to address the challenge. APO modification induces more PF 6 − anions entering the solvation structure at interface, which not only reduces the desolvation energy, but also facilitates the generation of inorganic‐rich SEI, promoting the reaction kinetics and thermal/structural stability of SEI. Meanwhile, APO optimizes the electrolyte decomposition reaction route and suppresses gas release, alleviating gas‐induced interfacial structure degradation, further enhances the uniformity and stability of the SEI and graphite. Consequently, the APO‐modified graphite exhibits remarkable performance across a wide temperature range with ordinary electrolyte. It delivers 210.5 mAh g −1 at 2000 mA g −1 with 76.2% retention after 1000 cycles at room temperature, maintains stable cycling at −20°C and providing an unprecedented 345.5 mAh g −1 at 60°C under 2000 mA g −1 and excellent cycle stability. This work demonstrates an effective interfacial chemistry regulation strategy via surface modification to achieve fast‐charging, thermally resilient graphite electrode for high‐performance LIBs.