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

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 b...

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Main Authors: Tianyi Hou, Donghai Wang, Bowen Jiang, Yi Liu, Jia Kong, Yanbing He, Yunhui Huang, Henghui Xu
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-56324-9
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author Tianyi Hou
Donghai Wang
Bowen Jiang
Yi Liu
Jia Kong
Yanbing He
Yunhui Huang
Henghui Xu
author_facet Tianyi Hou
Donghai Wang
Bowen Jiang
Yi Liu
Jia Kong
Yanbing He
Yunhui Huang
Henghui Xu
author_sort Tianyi Hou
collection DOAJ
description 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.
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issn 2041-1723
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spelling doaj-art-37994def7e344f5199a6967ff789b96d2025-01-26T12:40:38ZengNature PortfolioNature Communications2041-17232025-01-0116111210.1038/s41467-025-56324-9Ion bridging enables high-voltage polyether electrolytes for quasi-solid-state batteriesTianyi Hou0Donghai Wang1Bowen Jiang2Yi Liu3Jia Kong4Yanbing He5Yunhui Huang6Henghui Xu7State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and TechnologyInstitute of New Energy for Vehicles, Shanghai Key Laboratory of Development & Application for Metallic Functional Materials, School of Materials Science and Engineering, Tongji UniversityState Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and TechnologyState Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and TechnologyState Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and TechnologyShenzhen 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 UniversityState Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and TechnologyState Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and TechnologyAbstract 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.https://doi.org/10.1038/s41467-025-56324-9
spellingShingle Tianyi Hou
Donghai Wang
Bowen Jiang
Yi Liu
Jia Kong
Yanbing He
Yunhui Huang
Henghui Xu
Ion bridging enables high-voltage polyether electrolytes for quasi-solid-state batteries
Nature Communications
title Ion bridging enables high-voltage polyether electrolytes for quasi-solid-state batteries
title_full Ion bridging enables high-voltage polyether electrolytes for quasi-solid-state batteries
title_fullStr Ion bridging enables high-voltage polyether electrolytes for quasi-solid-state batteries
title_full_unstemmed Ion bridging enables high-voltage polyether electrolytes for quasi-solid-state batteries
title_short Ion bridging enables high-voltage polyether electrolytes for quasi-solid-state batteries
title_sort ion bridging enables high voltage polyether electrolytes for quasi solid state batteries
url https://doi.org/10.1038/s41467-025-56324-9
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AT bowenjiang ionbridgingenableshighvoltagepolyetherelectrolytesforquasisolidstatebatteries
AT yiliu ionbridgingenableshighvoltagepolyetherelectrolytesforquasisolidstatebatteries
AT jiakong ionbridgingenableshighvoltagepolyetherelectrolytesforquasisolidstatebatteries
AT yanbinghe ionbridgingenableshighvoltagepolyetherelectrolytesforquasisolidstatebatteries
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