Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 16, 2025

Abstract Ionic liquids (IL)‐based quasi‐solid polymer electrolytes (QSPEs) hold promise for safe lithium metal batteries owing to their tunable electrochemical properties and processability. However, traditional design strategy has ignored the interdependencies among “component‐function‐interface”, leading compromised practical applications hindered by sluggish lithium‐ion transport kinetics safety concerns. Herein, a triadic molecular synergy paradigm is proposed decouple conduction mechanisms in flame‐retardant QSPEs. Pentaerythritol tetraacrylate‐lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) provides structural framework, while IL (1‐butyl‐3‐methylimidazole bis (trifluoromethylsulfonyl) imide, BmimTFSI) as plasticizer softens chains weakening intermolecular forces provide an additional ion‐transport pathway imparting properties. Additionally, highly electronegative fluorine atoms of additive (2‐(perfluorohexyl)ethyl methacrylate, PFMA) promote LiTFSI dissociation through electron cloud migration, simultaneously immobilizing TFSI⁻ anions suppressing cationic competition strong PFMA−Bmim + coordination. As proof‐of‐concept, this synergistic achieves high transference number (0.72), forms stable fluoride‐dominated interphases, enhances battery via condensed‐phase mechanism. Experimental validation demonstrates that designed electrolyte significantly cycling stability Li symmetric cells, Li||LiFePO 4 Li||LiNi 0.8 Co 0.1 Mn O 2 cells. The engineering establishes developing high‐performance QSPEs batteries.

Language: Английский