Ion bridging enables high-voltage polyether electrolytes for quasi-solid-state batteries

Tianyi Hou, Donghai Wang, Bowen Jiang, Yi Liu, Jia Kong, Yanbing He, Yunhui Huang () and Henghui Xu ()
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Tianyi Hou: Huazhong University of Science and Technology
Donghai Wang: Tongji University
Bowen Jiang: Huazhong University of Science and Technology
Yi Liu: Huazhong University of Science and Technology
Jia Kong: Huazhong University of Science and Technology
Yanbing He: Tsinghua University
Yunhui Huang: Huazhong University of Science and Technology
Henghui Xu: Huazhong University of Science and Technology

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Polyether electrolytes have been widely recognized for their favorable compatibility with lithium-metal, yet they are hampered by intrinsically low oxidation thresholds, limiting their potential for realizing high-energy Li-metal batteries. Here, we report a general approach involving the bridge joints between non-lithium metal ions and ethereal oxygen, which significantly enhances the oxidation stability of various polyether electrolyte systems. To demonstrate the feasibility of the ion-bridging strategy, a Zn2+ ion-bridged polyether electrolyte (Zn-IBPE) with an extending electrochemical stability window of over 5 V is prepared, which enables good cyclability in 4.5 V Li||LiCoO2 batteries. Ampere-hour-level quasi-solid-state batteries of SiO-graphite||LiNi0.8Mn0.1Co0.1O2 (10 Ah, N/P ratio of 1.12, 303 Wh kg−1 at 0.1 C based on the total weight of the pouch cells) and 60 μm-Li||LiNi0.9Mn0.05Co0.05O2 (18 Ah, N/P ratio of 2.5, 452 Wh kg−1 at 0.33 C based on the total weight of the pouch cells) pouch cells with Zn-IBPE present elevated electrochemical performance, benefiting from adequate interfacial stability. Nail penetration tests evidence high battery safety enabled by Zn-IBPE in 4 Ah graphite||LiNi0.8Mn0.1Co0.1O2 pouch cells without combustion or smoke. This work offers a pathway for designing high-voltage polymer electrolytes and a general solution for achieving high-performance quasi-solid-state batteries.

Date: 2025
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DOI: 10.1038/s41467-025-56324-9

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