| Summary: | Abstract To achieve next‐generation lithium metal batteries (LMBs) with desirable specific energy and reliability, the electrolyte shown simultaneously high reductive stability toward lithium metal anode and oxidative stability toward high‐voltage cathode is of great importance. Here, we report for the first time that high‐concentration lithium bis(fluorosulfonyl)imide (LiFSI) initiates ring‐opening polymerization of 1,3‐dioxolane in presence of ethylene carbonate and ethylmethyl carbonate to produce in‐situ a novel polymeric concentrated quasi‐solid electrolyte (poly‐CQSE). The unique poly‐CQSE with 10 M LiFSI forms a mixed‐lithiophobic‐conductive LiF‐Li3N solid electrolyte interphase on lithium metal anode, and a F‐rich conformal cathode electrolyte interphase on LiNi0.5Co0.2Mn0.3O2 (NCM523) cathode simultaneously. As a result, the poly‐CQSE not only enables stable Li plating/stripping of metallic Li anode at a sound Coulombic efficiency of 95.3% without dendrite growth, but also enables a stable cycling of the Li||NCM523 quasi‐solid‐state LMB at a capacity retention of 94% over 100 cycles.
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