Integrating Competitive Li+ Coordination with Immobilized Anions in Composite Solid Electrolyte for High‐Performance Li Metal Batteries
Abstract Poly(vinylidene fluoride) (PVDF)‐based polymer electrolytes have attracted widespread attention due to their unique Li+ transport mechanism. However, their low ionic conductivity and porous structure, as well as residual solvent limit their application at high current densities. Here, a com...
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Wiley
2025-04-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202413875 |
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| author | Ziyang Liang Chang Liu Xiang Bai Jiahui Zhang Xinyue Chang Bo Zhang Mengxue Xia Huayun Du Hao Huang Bing Wu Chengkai Yang Shi Wang Wen Liu Qian Wang |
| author_facet | Ziyang Liang Chang Liu Xiang Bai Jiahui Zhang Xinyue Chang Bo Zhang Mengxue Xia Huayun Du Hao Huang Bing Wu Chengkai Yang Shi Wang Wen Liu Qian Wang |
| author_sort | Ziyang Liang |
| collection | DOAJ |
| description | Abstract Poly(vinylidene fluoride) (PVDF)‐based polymer electrolytes have attracted widespread attention due to their unique Li+ transport mechanism. However, their low ionic conductivity and porous structure, as well as residual solvent limit their application at high current densities. Here, a composite solid electrolyte (CSE) is developed by integrating poly(vinylidene‐co‐trifluoroethylene) [P(VDF‐TrFE)] in its all‐trans conformation with aminofunctionalized metal–organic framework (ZIF‐90‐NH2). In such a CSE, all F atoms located on one side of the polymer chain, providing fast Li+ transport channels. Concurrently, the functionalized ZIF‐90‐NH2 can effectively anchor the residual N, N‐dimethylformamide (DMF) in CSEs while weakening Li+‐DMF solvent coordination, inducing the rearrangement of Li+ solvation structure and inhibiting the decomposition of DMF at the interface. Synergistically, ZIF‐90‐NH2 can immobilize anions in Li salts, promoting their dissociation. Based on integrating competitive Li+ coordination with immobilized anions, the obtained CSEs exhibit a high Li+ transference number (0.77). The full cells with LiFePO4 cathode can run stably over 400 cycles at 5 C, while the Li || LiNi0.7Co0.1Mn0.2O2 full cells deliver a high capacity retention (>85%) after 200 cycles at a charge cutoff voltage of 4.5 V. This work opens up a new path for building CSEs with high interfacial stability and fast Li+ transport. |
| format | Article |
| id | doaj-art-dd3dbcd8406c46bc84052e82a0d67e1e |
| institution | OA Journals |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-dd3dbcd8406c46bc84052e82a0d67e1e2025-08-20T02:16:22ZengWileyAdvanced Science2198-38442025-04-011214n/an/a10.1002/advs.202413875Integrating Competitive Li+ Coordination with Immobilized Anions in Composite Solid Electrolyte for High‐Performance Li Metal BatteriesZiyang Liang0Chang Liu1Xiang Bai2Jiahui Zhang3Xinyue Chang4Bo Zhang5Mengxue Xia6Huayun Du7Hao Huang8Bing Wu9Chengkai Yang10Shi Wang11Wen Liu12Qian Wang13College of Materials Science and Engineering Taiyuan University of Technology Taiyuan Shanxi 030024 ChinaCollege of Materials Science and Engineering Taiyuan University of Technology Taiyuan Shanxi 030024 ChinaShanxi Energy Internet Research Institute Taiyuan Shanxi 030024 ChinaShanxi Energy Internet Research Institute Taiyuan Shanxi 030024 ChinaShanxi Energy Internet Research Institute Taiyuan Shanxi 030024 ChinaCollege of Materials Science and Engineering Taiyuan University of Technology Taiyuan Shanxi 030024 ChinaCollege of Materials Science and Engineering Taiyuan University of Technology Taiyuan Shanxi 030024 ChinaCollege of Materials Science and Engineering Taiyuan University of Technology Taiyuan Shanxi 030024 ChinaCollege of Materials Science and Engineering Taiyuan University of Technology Taiyuan Shanxi 030024 ChinaEmergency Research Institute Chinese Institute of Coal Science (CICS) Beijing 100013 ChinaKey Laboratory of Advanced Materials Technology College of Materials Science and Engineering Fuzhou University Fuzhou 350108 ChinaState Key Laboratory of Organic Electronics & Information Displays (SKLOEID) Institute of Advanced Materials (IAM) Nanjing University of Posts & Telecommunications Nanjing 210023 ChinaState Key Lab of Chemical Resource Engineering College of Science and College of Energy Beijing University of Chemical Technology Beijing 100092 ChinaCollege of Materials Science and Engineering Taiyuan University of Technology Taiyuan Shanxi 030024 ChinaAbstract Poly(vinylidene fluoride) (PVDF)‐based polymer electrolytes have attracted widespread attention due to their unique Li+ transport mechanism. However, their low ionic conductivity and porous structure, as well as residual solvent limit their application at high current densities. Here, a composite solid electrolyte (CSE) is developed by integrating poly(vinylidene‐co‐trifluoroethylene) [P(VDF‐TrFE)] in its all‐trans conformation with aminofunctionalized metal–organic framework (ZIF‐90‐NH2). In such a CSE, all F atoms located on one side of the polymer chain, providing fast Li+ transport channels. Concurrently, the functionalized ZIF‐90‐NH2 can effectively anchor the residual N, N‐dimethylformamide (DMF) in CSEs while weakening Li+‐DMF solvent coordination, inducing the rearrangement of Li+ solvation structure and inhibiting the decomposition of DMF at the interface. Synergistically, ZIF‐90‐NH2 can immobilize anions in Li salts, promoting their dissociation. Based on integrating competitive Li+ coordination with immobilized anions, the obtained CSEs exhibit a high Li+ transference number (0.77). The full cells with LiFePO4 cathode can run stably over 400 cycles at 5 C, while the Li || LiNi0.7Co0.1Mn0.2O2 full cells deliver a high capacity retention (>85%) after 200 cycles at a charge cutoff voltage of 4.5 V. This work opens up a new path for building CSEs with high interfacial stability and fast Li+ transport.https://doi.org/10.1002/advs.202413875composite solid electrolytesimmobilized anionsLi metal batteriesLi+ coordinationZIF‐90‐NH2 |
| spellingShingle | Ziyang Liang Chang Liu Xiang Bai Jiahui Zhang Xinyue Chang Bo Zhang Mengxue Xia Huayun Du Hao Huang Bing Wu Chengkai Yang Shi Wang Wen Liu Qian Wang Integrating Competitive Li+ Coordination with Immobilized Anions in Composite Solid Electrolyte for High‐Performance Li Metal Batteries Advanced Science composite solid electrolytes immobilized anions Li metal batteries Li+ coordination ZIF‐90‐NH2 |
| title | Integrating Competitive Li+ Coordination with Immobilized Anions in Composite Solid Electrolyte for High‐Performance Li Metal Batteries |
| title_full | Integrating Competitive Li+ Coordination with Immobilized Anions in Composite Solid Electrolyte for High‐Performance Li Metal Batteries |
| title_fullStr | Integrating Competitive Li+ Coordination with Immobilized Anions in Composite Solid Electrolyte for High‐Performance Li Metal Batteries |
| title_full_unstemmed | Integrating Competitive Li+ Coordination with Immobilized Anions in Composite Solid Electrolyte for High‐Performance Li Metal Batteries |
| title_short | Integrating Competitive Li+ Coordination with Immobilized Anions in Composite Solid Electrolyte for High‐Performance Li Metal Batteries |
| title_sort | integrating competitive li coordination with immobilized anions in composite solid electrolyte for high performance li metal batteries |
| topic | composite solid electrolytes immobilized anions Li metal batteries Li+ coordination ZIF‐90‐NH2 |
| url | https://doi.org/10.1002/advs.202413875 |
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