Li+-migration influencing factors and non-destructive life extension of quasi-solid-state polymer electrolytes
Abstract Polymer-based quasi-solid-state electrolytes (QSSE) are believed to be the most feasible candidates for solid-state batteries, but they are hindered by relatively lower ionic conductivity and narrower electrochemical window. Here, we synthesize a series of ether-free acrylates containing Li...
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Nature Portfolio
2025-04-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-59020-w |
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| author | Peiying Li Jinjin Hao Shuang He Zenghua Chang Xiaolei Li Rennian Wang Wen Ma Jiantao Wang Yuhao Lu Hong Li Liqun Zhang Weidong Zhou |
| author_facet | Peiying Li Jinjin Hao Shuang He Zenghua Chang Xiaolei Li Rennian Wang Wen Ma Jiantao Wang Yuhao Lu Hong Li Liqun Zhang Weidong Zhou |
| author_sort | Peiying Li |
| collection | DOAJ |
| description | Abstract Polymer-based quasi-solid-state electrolytes (QSSE) are believed to be the most feasible candidates for solid-state batteries, but they are hindered by relatively lower ionic conductivity and narrower electrochemical window. Here, we synthesize a series of ether-free acrylates containing Li+-ligands for high-voltage-stable QSSEs. Our findings demonstrate that the polymer-involved solvation structure is critical in determining the ionic conductivity, and low-temperature crystallization of the polymer can be used for non-destructive life extension of batteries. The prepared polymers do not contain ether unit and exhibit a polymerization degree of 99% in cells without residual double-bonded monomer, endowing them with high antioxidation capability and compatibility with high-voltage positive electrodes including LiNi0.85Co0.075Mn0.075O2, 4.6 V LiCoO2 and 4.8 V Li1.13Ni0.3Mn0.57O2. The confinement of liquid in QSSEs effectively suppresses the interfacial reactions, but the residual interface reactions still gradually consume liquid electrolytes and cause capacity fading, due to the limited diffusion of the confined solvent to wet the interface. Through crystallizing the polymer matrices at −50 °C, the confined liquid in QSSEs is released and re-wets the Li-metal/polymer interface, thereby recovering the capacity and extending the life of solid-state batteries in a non-destructive manner. |
| format | Article |
| id | doaj-art-4bcc95bf42d84565aba05109b077662c |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-4bcc95bf42d84565aba05109b077662c2025-08-20T02:17:56ZengNature PortfolioNature Communications2041-17232025-04-0116111410.1038/s41467-025-59020-wLi+-migration influencing factors and non-destructive life extension of quasi-solid-state polymer electrolytesPeiying Li0Jinjin Hao1Shuang He2Zenghua Chang3Xiaolei Li4Rennian Wang5Wen Ma6Jiantao Wang7Yuhao Lu8Hong Li9Liqun Zhang10Weidong Zhou11Beijing Advanced Innovation Center for Soft Matter Science and Engineering, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical TechnologyBeijing Advanced Innovation Center for Soft Matter Science and Engineering, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical TechnologyBeijing Advanced Innovation Center for Soft Matter Science and Engineering, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical TechnologyChina Automotive Battery Research Institute Co. Ltd. BeijingBeijing Advanced Innovation Center for Soft Matter Science and Engineering, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical TechnologyChina Automotive Battery Research Institute Co. Ltd. BeijingNingde Amperex Technology Limited (ATL), Key Laboratory of Consumer Lithium-Ion Battery in FujianChina Automotive Battery Research Institute Co. Ltd. BeijingNingde Amperex Technology Limited (ATL), Key Laboratory of Consumer Lithium-Ion Battery in FujianKey Laboratory for Renewable Energy, Institute of Physics, Chinese Academy of SciencesBeijing Advanced Innovation Center for Soft Matter Science and Engineering, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical TechnologyBeijing Advanced Innovation Center for Soft Matter Science and Engineering, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical TechnologyAbstract Polymer-based quasi-solid-state electrolytes (QSSE) are believed to be the most feasible candidates for solid-state batteries, but they are hindered by relatively lower ionic conductivity and narrower electrochemical window. Here, we synthesize a series of ether-free acrylates containing Li+-ligands for high-voltage-stable QSSEs. Our findings demonstrate that the polymer-involved solvation structure is critical in determining the ionic conductivity, and low-temperature crystallization of the polymer can be used for non-destructive life extension of batteries. The prepared polymers do not contain ether unit and exhibit a polymerization degree of 99% in cells without residual double-bonded monomer, endowing them with high antioxidation capability and compatibility with high-voltage positive electrodes including LiNi0.85Co0.075Mn0.075O2, 4.6 V LiCoO2 and 4.8 V Li1.13Ni0.3Mn0.57O2. The confinement of liquid in QSSEs effectively suppresses the interfacial reactions, but the residual interface reactions still gradually consume liquid electrolytes and cause capacity fading, due to the limited diffusion of the confined solvent to wet the interface. Through crystallizing the polymer matrices at −50 °C, the confined liquid in QSSEs is released and re-wets the Li-metal/polymer interface, thereby recovering the capacity and extending the life of solid-state batteries in a non-destructive manner.https://doi.org/10.1038/s41467-025-59020-w |
| spellingShingle | Peiying Li Jinjin Hao Shuang He Zenghua Chang Xiaolei Li Rennian Wang Wen Ma Jiantao Wang Yuhao Lu Hong Li Liqun Zhang Weidong Zhou Li+-migration influencing factors and non-destructive life extension of quasi-solid-state polymer electrolytes Nature Communications |
| title | Li+-migration influencing factors and non-destructive life extension of quasi-solid-state polymer electrolytes |
| title_full | Li+-migration influencing factors and non-destructive life extension of quasi-solid-state polymer electrolytes |
| title_fullStr | Li+-migration influencing factors and non-destructive life extension of quasi-solid-state polymer electrolytes |
| title_full_unstemmed | Li+-migration influencing factors and non-destructive life extension of quasi-solid-state polymer electrolytes |
| title_short | Li+-migration influencing factors and non-destructive life extension of quasi-solid-state polymer electrolytes |
| title_sort | li migration influencing factors and non destructive life extension of quasi solid state polymer electrolytes |
| url | https://doi.org/10.1038/s41467-025-59020-w |
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