High-energy and fast-charging lithium metal batteries enabled by tuning Li+-solvation via electron-withdrawing and lithiophobicity functionality
Abstract The solvent fluorination almost always improves electrochemical stability of electrolytes against both lithium anodes and high-voltage cathodes in lithium metal batteries. However, how exactly fluorination affects Li+-solvation and interphasial chemistries remains unclear, hindering rationa...
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Nature Portfolio
2025-05-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-59967-w |
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| author | Guangzhao Zhang Tong Zhang Zhen Zhang Ruilin He Qingrong Wang Shang-Sen Chi Yanming Cui Meng Danny Gu Zhongbo Liu Jian Chang Chaoyang Wang Kang Xu Yonghong Deng |
| author_facet | Guangzhao Zhang Tong Zhang Zhen Zhang Ruilin He Qingrong Wang Shang-Sen Chi Yanming Cui Meng Danny Gu Zhongbo Liu Jian Chang Chaoyang Wang Kang Xu Yonghong Deng |
| author_sort | Guangzhao Zhang |
| collection | DOAJ |
| description | Abstract The solvent fluorination almost always improves electrochemical stability of electrolytes against both lithium anodes and high-voltage cathodes in lithium metal batteries. However, how exactly fluorination affects Li+-solvation and interphasial chemistries remains unclear, hindering rational design of electrolytes and interphases with both wide electrochemical stability window and fast ion transport kinetics that are required for energy-dense and fast-charging LMBs. Here we introduce the trifluoromethylation (-CF3) at one end of 1,2-dimethoxyethane and generate 1,1,1-trifluoro-2-(2-methoxyethoxy) ethane, which as a single solvent of electrolyte simultaneously meets energy-dense and fast-charging requirements when dissolving 2 M lithium bis(fluorosulfonyl)imide. Beside the electron-withdrawing effect of -CF3, we find that its lithiophobic nature against Li+ significantly alters the solvation structures, which favors the formation of anion-dominated clusters that lead to superior interphasial chemistries in layered structure and fast Li+ transport kinetics. In such electrolyte, lithium metal batteries constructed with 50-μm-thin Li||high-loading-NMC811 in both coin and pouch cell configurations achieve >400 cycles under fast-charging condition, and >100 cycles in 14-Ah-level industrial pouch cell with a high energy density over 510 Wh kg−1 at cell-level. |
| format | Article |
| id | doaj-art-d41f03cd4ac94794ab9d98796bb32919 |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Nature Portfolio |
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| series | Nature Communications |
| spelling | doaj-art-d41f03cd4ac94794ab9d98796bb329192025-08-20T01:53:23ZengNature PortfolioNature Communications2041-17232025-05-0116111210.1038/s41467-025-59967-wHigh-energy and fast-charging lithium metal batteries enabled by tuning Li+-solvation via electron-withdrawing and lithiophobicity functionalityGuangzhao Zhang0Tong Zhang1Zhen Zhang2Ruilin He3Qingrong Wang4Shang-Sen Chi5Yanming Cui6Meng Danny Gu7Zhongbo Liu8Jian Chang9Chaoyang Wang10Kang Xu11Yonghong Deng12Department of Materials Science and Engineering, Southern University of Science and TechnologyDepartment of Materials Science and Engineering, Southern University of Science and TechnologyDepartment of Materials Science and Engineering, Southern University of Science and TechnologyDepartment of Materials Science and Engineering, Southern University of Science and TechnologyDepartment of Materials Science and Engineering, Southern University of Science and TechnologyDepartment of Materials Science and Engineering, Southern University of Science and TechnologyZhejiang Funlithium New Energy Technology Co., Ltd.Eastern Institute for Advanced Study, Eastern Institute of TechnologyShenzhen CAPCHEM Technology Co. LtdDongguan Key Laboratory of Interdisciplinary Science for Advanced Materials and Large-Scale Scientific Facilities, School of Physical Sciences, Great Bay UniversityResearch Institute of Materials Science, South China University of TechnologySolidEnergy Systems LLCDepartment of Materials Science and Engineering, Southern University of Science and TechnologyAbstract The solvent fluorination almost always improves electrochemical stability of electrolytes against both lithium anodes and high-voltage cathodes in lithium metal batteries. However, how exactly fluorination affects Li+-solvation and interphasial chemistries remains unclear, hindering rational design of electrolytes and interphases with both wide electrochemical stability window and fast ion transport kinetics that are required for energy-dense and fast-charging LMBs. Here we introduce the trifluoromethylation (-CF3) at one end of 1,2-dimethoxyethane and generate 1,1,1-trifluoro-2-(2-methoxyethoxy) ethane, which as a single solvent of electrolyte simultaneously meets energy-dense and fast-charging requirements when dissolving 2 M lithium bis(fluorosulfonyl)imide. Beside the electron-withdrawing effect of -CF3, we find that its lithiophobic nature against Li+ significantly alters the solvation structures, which favors the formation of anion-dominated clusters that lead to superior interphasial chemistries in layered structure and fast Li+ transport kinetics. In such electrolyte, lithium metal batteries constructed with 50-μm-thin Li||high-loading-NMC811 in both coin and pouch cell configurations achieve >400 cycles under fast-charging condition, and >100 cycles in 14-Ah-level industrial pouch cell with a high energy density over 510 Wh kg−1 at cell-level.https://doi.org/10.1038/s41467-025-59967-w |
| spellingShingle | Guangzhao Zhang Tong Zhang Zhen Zhang Ruilin He Qingrong Wang Shang-Sen Chi Yanming Cui Meng Danny Gu Zhongbo Liu Jian Chang Chaoyang Wang Kang Xu Yonghong Deng High-energy and fast-charging lithium metal batteries enabled by tuning Li+-solvation via electron-withdrawing and lithiophobicity functionality Nature Communications |
| title | High-energy and fast-charging lithium metal batteries enabled by tuning Li+-solvation via electron-withdrawing and lithiophobicity functionality |
| title_full | High-energy and fast-charging lithium metal batteries enabled by tuning Li+-solvation via electron-withdrawing and lithiophobicity functionality |
| title_fullStr | High-energy and fast-charging lithium metal batteries enabled by tuning Li+-solvation via electron-withdrawing and lithiophobicity functionality |
| title_full_unstemmed | High-energy and fast-charging lithium metal batteries enabled by tuning Li+-solvation via electron-withdrawing and lithiophobicity functionality |
| title_short | High-energy and fast-charging lithium metal batteries enabled by tuning Li+-solvation via electron-withdrawing and lithiophobicity functionality |
| title_sort | high energy and fast charging lithium metal batteries enabled by tuning li solvation via electron withdrawing and lithiophobicity functionality |
| url | https://doi.org/10.1038/s41467-025-59967-w |
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