Gel Polymer Electrolyte Enables Low‐Temperature and High‐Rate Lithium‐Ion Batteries via Bionic Interface Design

Abstract Traditional ethylene carbonate (EC)‐based electrolytes constrain the applications of silicon carbon (Si‐C) anodes under fast‐charging and low‐temperature conditions due to sluggish Li + migration kinetics and unstable solid electrolyte interphase (SEI). Herein, inspired by the efficient water purification and soil stabilization of aquatic plants, a stable SEI with a 3D desolvation interface is designed with gel polymer electrolyte (GPE), accelerating Li + desolvation and migration at the interface and within stable SEI. As demonstrated by theoretical simulations and experiment results, the resulting poly(1,3‐dioxolane) (PDOL), prepared by in situ ring‐opening polymerization of 1,3‐dioxolane (DOL), creates a 3D desolvation area, improving the Li + desolvation at the interface and yielding an amorphous GPE with a high Li + ionic conductivity (5.73 mS cm −1 ). Furthermore, more anions participate in the solvated structure, forming an anion‐derived stable SEI and improving Li + transport through SEI. Consequently, the Si‐C anode achieves excellent rate performance with GPE at room temperature (RT) and low temperature (−40 °C). The pouch full cell coupled with LiFePO 4 cathode obtains 97.42 mAh g −1 after 500 cycles at 5 C/5 C. This innovatively designed 3D desolvation interface and SEI represent significant breakthroughs for developing fast‐charging and low‐temperature batteries.