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Abstract A class of organic‐inorganic hybrid electrolyte with ion pair integrated network (X‐POSS‐IL‐LiTFSI) has been prepared by crosslinking of oligomeric octasilsesquioxanes grafted with imidazolium‐based ionic liquids for solid state lithium ion battery applications. X‐POSS‐IL‐LiTFSI is thermally stable and highly amorphous, and shows high ionic conductivities and excellent electrochemical stability. With further immobilization of a small fraction of ionic liquid, the ionic conductivity of X‐POSS‐IL‐LiTFSI has been significantly improved, e. g. 1.4×10⁻⁴ S/cm at ambinet temperature, to the level required by the practical battery applications, while maintaining the demensional integity. The coin cells of lithium batteries with the plasticized X‐POSS‐IL‐LiTFSI electrolytes exhibit high specific capacities at both ambient and elevated temperatures. 

The use of highly conductive solid-state electrolytes to replace conventional liquid organic electrolytes enables radical improvements in the reliability, safety and performance of lithium batteries. Here, we report the synthesis and characterization of a new class of nonflammable solid electrolytes based on the grafting of ionic liquids onto octa-silsesquioxane. The electrolyte exhibits outstanding room-temperature ionic conductivity (∼4.8 × 10 −4 S cm −1 ), excellent electrochemical stability (up to 5 V relative to Li + /Li) and high thermal stability. All-solid-state Li metal batteries using the prepared electrolyte membrane are successfully cycled with high coulombic efficiencies at ambient temperature. The good cycling stability of the electrolyte against lithium has been demonstrated. This work provides a new platform for the development of solid polymer electrolytes for application in room-temperature lithium batteries.