Solid electrolytes, developed to address the safety hazards of liquid electrolytes, still face some issues, such as low ionic conductivity, non-flame retardancy, and poor compatibility with electrodes. Herein, an organic ionic liquid lithium salt (named PQ-Li) with good intrinsic conductivity and flame retardancy was synthesized, and a flexible and homogeneous all-solid “polymer in salt” electrolyte, composed of 73.15 wt% PQ–Li and 26.85 wt% poly(ethylene oxide) (PEO), referred to as PQSE, was prepared. This preparation strategy, based on a dual-functional lithium salt, endows PQSE with great electrochemical performance (e.g., an ionic conductivity of 0.11 mS m−1 at 30°C, and an electrochemical stability window of 5.1 V), excellent flame retardancy, and good compatibility with Li electrodes considering the absent short circuits and lithium dendrites. The sound charge/discharge performance of Li|PQSE|LiFePO4 cells (e.g., a discharge capacity of 150.6 mAh g−1 at 0.1 C, Coulombic efficiency beyond 99%, and repeatable power-supply processes for light-emitting diode bulbs) exactly results from the formation of a stable solid–electrolyte interface film with a favorable bilayer architecture. Through molecular dynamic simulation and two-dimensional correlation Raman technique, a dual-channel Li+ conduction mechanism in PQSE under an electric field has been proposed, with the dominant mode relying on the hopping of Li+ in ionic aggregates/bridges, and the auxiliary mode relying on the random movement of PEO segments coordinating with Li+. The developed PQSE provides a trade-off of safety, electrochemical properties, and processibility of electrolytes and represents a promising avenue in solid-state lithium battery technologies.
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