A Gel Polymer Electrolyte with 2D Filler‐reinforced for Dendrite Suppression Li‐Ion Batteries

Abstract Gel polymer electrolytes (GPEs) incorporate both the high ionic conductivity of organic liquid electrolyte and the high safety performance of all‐solid‐state electrolytes (ASSEs), greatly improving the electrochemical performance of solid polymer electrolytes (SPEs). However, the practical application of GPEs is still limited by inferior interface compatibility, lithium dendrites, etc. Herein, we prepared GPEs based on poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP) further co‐blended the two‐dimensional sheet inorganic filler hectorite and poly(methyl methacrylate) (PMMA) to improve the mechanical and electrochemical properties of the GPEs. When the content of PMMA and hectorite is optimal, this GPEs have an ionic conductivity of 1.06×10−3 S cm−1 and outstanding lithium symmetric cells cycle time of more than 3000 h, indicating that the introduction of filler effectively inhibits the growth of lithium dendrites at room temperature. Moreover, the GPEs adopt a relatively simple solution casting method to provide a fresh idea for the synthesis of high‐performance GPEs.