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; Henghui Xu

doi:10.1038/s41467-025-56324-9

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

Nat Commun. 2025 Jan 23;16(1):962. doi: 10.1038/s41467-025-56324-9.

Authors

Tianyi Hou¹, Donghai Wang², Bowen Jiang¹, Yi Liu¹, Jia Kong¹, Yanbing He³, Yunhui Huang⁴, Henghui Xu⁵

Affiliations

¹ State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, PR China.
² Institute of New Energy for Vehicles, Shanghai Key Laboratory of Development & Application for Metallic Functional Materials, School of Materials Science and Engineering, Tongji University, Shanghai, PR China.
³ Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center and Shenzhen Geim Graphene Center, Institute of Materials Research (IMR), Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, China.
⁴ State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, PR China. [email protected].
⁵ State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, PR China. [email protected].

PMID: 39843477
DOI: 10.1038/s41467-025-56324-9

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||LiNi_0.8Mn_0.1Co_0.1O₂ (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||LiNi_0.9Mn_0.05Co_0.05O₂ (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||LiNi_0.8Mn_0.1Co_0.1O₂ 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.

Abstract

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