Fluorinated polyester electrolytes have been recognized as promising candidates for solid-state Li metal batteries owing to their exceptional oxidative stability. However, traditional fluorinated polyester electrolytes still encounter poor SEI chemistry and slow bulk Li+ conduction. Herein, by tuning the trifluoromethyl of poly-(trifluoroethyl methacrylate) (PTFMA) to trifluoromethylsulfonamido of poly-(2-(Trifluoromethylsulfonamido)ethyl methacrylate) (PTFSMA), a side-chain engineering of fluorinated polyesters is proposed to achieve the integration of Li metal compatibility and fast Li+ transportation. Ab initio molecular dynamic (AIMD) calculations revealed that the easily cleaved C-S bond of PTFSMA accelerates the formation of LiF and Li2S enriched SEI to suppress further interfacial degradation while guaranteeing unobstructed Li+ diffusion. Molecular dynamic (MD) simulations identified the coupling effect between S=O and −CF3 significantly enhances the Li+ solvation ability of the fluorine atom, endowing high Li+ conductivity of 0.81 mS cm−1. Impressively, the PTFSMA-based gel polymer electrolyte exhibits stable cycling over 5000 and 2800 cycles in LiFePO4 full cells at 5C and 10C, respectively, and the high-loading LiNi0.5Co0.2Mn0.3O2 full cells (2.8 mAh cm−2) maintain 88.9 % capacity retention after 300 cycles. This finding highlights the significance of polymer architecture design on the interfacial SEI chemistry and Li+ transport dynamics of polymer electrolyte for long-cycle Li metal batteries.
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