Synergistic Molecular and Polymer Network Design Enables Stable LiPF₆-Based Gel Polymer Electrolytes for Lithium Metal Batteries.

Authors

Min Wang, Mengjie Li, Junru Wu, Yuefeng Meng, Lili Lin, Yadong Wang, Hao Du, Xinran Geng, Zhiqiang Fu, Cuiping Han, Baohua Li

Published in

Angewandte Chemie (International ed. in English). Pages e6028878. Aug 26, 2026. Epub Aug 26, 2026.

Abstract

High-voltage lithium metal batteries suffer from severe interfacial degradation and electrolyte decomposition, limiting cycling stability and practical application. In conventional LiPF₆-based electrolytes containing fluoroethylene carbonate (FEC), LiPF₆ decomposition generates Lewis-acid species that trigger FEC defluorination and HF formation, causing progressive interphase degradation. Here we report a multifunctional gel polymer electrolyte (MGPE) that integrates solvation regulation with polymer-network confinement and interrupts the PF₅-FEC degradation pathway via strong PF₆ ^- binding. The fluorinated aromatic additive 1,1,2,2-tetrafluoroethoxybenzene modulates the Li⁺ solvation structure and promotes preferential formation of a stable cathode-electrolyte interphase, enhancing oxidative stability up to 5.0 V. Meanwhile, in situ polymerization of 3,5-bis(trifluoromethyl)styrene constructs a fluorinated aromatic network with strong affinity toward PF₆ ^-, suppressing Lewis‑acidic PF₅ formation. The synergistic interplay between solvation regulation, PF₅ suppression, and fluorinated-network confinement steers interphase evolution toward dense LiF-rich layers on both electrodes, enabling Li||LiCoO₂ cells to retain 82.6% capacity after 400 cycles at 4.5 V and 90.3% after 200 cycles at a cathode loading of ∼11 mg cm^-2. Furthermore, 1.3 Ah pouch cells (N/P = 1.1) show 80.7% capacity retention after 30 cycles under practical conditions. This work provides an electrolyte-engineering strategy to suppress PF₅-induced degradation and stabilize interphase evolution, enabling safer high-energy lithium metal batteries.

PMID:
42655968
Bibliographic data and abstract were imported from PubMed on 27 Aug 2026.

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