Lithium metal batteries promise ultrahigh energy density but suffer from interfacial instability, dendrite growth, and safety risks. Gel polymer electrolytes are a promising solution, but conventional designs suffer from poor interfacial compatibility and lithium dendrite growth. Here, we design an in situ formed nonflammable gel polymer electrolyte (NGPE) that integrates two molecular-level strategies: hydrogen-bond anchoring and solvation-shell regulation. Hydrogen bonds among TMP, PVDF-HFP, and TFSI- immobilize anions, enhancing ionic conductivity and Li+ transference. Fluoroethylene carbonate reshapes Li+ solvation, leading to the formation of inorganic-rich interphases that suppress dendrites and stabilize interfaces. The optimized NGPE achieves stable Li||Li cycling for over 2800 h and Li||LFP full cells with 74.3% capacity retention after 1000 cycles at 2 C. Pouch cells further demonstrate mechanical robustness and exceptional safety under flame tests. This dual molecular strategy provides a general design principle for safe, dendrite-free quasi-solid-state lithium metal batteries.
Gao et al. (Wed,) studied this question.