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

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 LiFePO₄ 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.