The Use of Cognate Cosolvent to Mediate Localized High-Concentration Electrolytes for High-Voltage and Long-Cycling Lithium-Metal Batteries
Localized high-concentration electrolytes (LHCEs) are promising systems for improving the high-voltage performance and interfacial stability of lithium-metal batteries (LMBs). Unfortunately, they are always challenged by liquid–liquid phase separation during solution preparation. Further investigati...
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2025-04-01
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| author | Ying Hu Dandan Wang Qijie Yu Ziyi He Fengrui Deng Hao Yan Tinglu Song Jin-Cheng Zheng Yang Dai |
| author_facet | Ying Hu Dandan Wang Qijie Yu Ziyi He Fengrui Deng Hao Yan Tinglu Song Jin-Cheng Zheng Yang Dai |
| author_sort | Ying Hu |
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| description | Localized high-concentration electrolytes (LHCEs) are promising systems for improving the high-voltage performance and interfacial stability of lithium-metal batteries (LMBs). Unfortunately, they are always challenged by liquid–liquid phase separation during solution preparation. Further investigation is always required when the prepared electrolyte has encountered liquid–liquid phase separation previously. Here, we propose a “cognate cosolvent” strategy to mediate phase-separated LiBF<sub>4</sub>/fluoroethylene carbonate (FEC)|ethyl trifluoroacetate (TFAE) mixtures with ethyl acetate (EA), forming effective LiBF<sub>4</sub>/FEC/EA/TFAE-based LHCEs (B-LHCEs). Because of their unique solvation structure, the B-LHCEs exhibit high oxidative stability, facilitating Li<sup>+</sup> transport. The optimized B-LHCEs help single-crystal LiMn<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub>/Li batteries form robust interphases, improving interfacial stability. As a result, distinct performance can be obtained (4.5 V, 500 cycles, ~90%, 1400, ~70%; 25 C, 128 mAh g<sup>−1</sup>, 4.7 V, 500, 82.5%). This work turns the “impossible” into an “effective” high-voltage electrolyte design, transcending the previous paradigms of electrolyte investigation and enriching LHCE preparation research. |
| format | Article |
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| institution | OA Journals |
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| language | English |
| publishDate | 2025-04-01 |
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| series | Batteries |
| spelling | doaj-art-b6756a63db984b2bb71fb7a6b7e99f9d2025-08-20T02:24:42ZengMDPI AGBatteries2313-01052025-04-0111415610.3390/batteries11040156The Use of Cognate Cosolvent to Mediate Localized High-Concentration Electrolytes for High-Voltage and Long-Cycling Lithium-Metal BatteriesYing Hu0Dandan Wang1Qijie Yu2Ziyi He3Fengrui Deng4Hao Yan5Tinglu Song6Jin-Cheng Zheng7Yang Dai8Department of Chemical Engineering, Shanghai University, Shangda Road 99, Shanghai 200444, ChinaDepartment of Chemical Engineering, Shanghai University, Shangda Road 99, Shanghai 200444, ChinaDepartment of Chemical Engineering, Shanghai University, Shangda Road 99, Shanghai 200444, ChinaDepartment of Chemical Engineering, Shanghai University, Shangda Road 99, Shanghai 200444, ChinaDepartment of Chemical Engineering, Shanghai University, Shangda Road 99, Shanghai 200444, ChinaDepartment of Chemical Engineering, Shanghai University, Shangda Road 99, Shanghai 200444, ChinaExperimental Center of Advanced Materials School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, ChinaDepartment of Physics, Xiamen University, Xiamen 361005, ChinaDepartment of Chemical Engineering, Shanghai University, Shangda Road 99, Shanghai 200444, ChinaLocalized high-concentration electrolytes (LHCEs) are promising systems for improving the high-voltage performance and interfacial stability of lithium-metal batteries (LMBs). Unfortunately, they are always challenged by liquid–liquid phase separation during solution preparation. Further investigation is always required when the prepared electrolyte has encountered liquid–liquid phase separation previously. Here, we propose a “cognate cosolvent” strategy to mediate phase-separated LiBF<sub>4</sub>/fluoroethylene carbonate (FEC)|ethyl trifluoroacetate (TFAE) mixtures with ethyl acetate (EA), forming effective LiBF<sub>4</sub>/FEC/EA/TFAE-based LHCEs (B-LHCEs). Because of their unique solvation structure, the B-LHCEs exhibit high oxidative stability, facilitating Li<sup>+</sup> transport. The optimized B-LHCEs help single-crystal LiMn<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub>/Li batteries form robust interphases, improving interfacial stability. As a result, distinct performance can be obtained (4.5 V, 500 cycles, ~90%, 1400, ~70%; 25 C, 128 mAh g<sup>−1</sup>, 4.7 V, 500, 82.5%). This work turns the “impossible” into an “effective” high-voltage electrolyte design, transcending the previous paradigms of electrolyte investigation and enriching LHCE preparation research.https://www.mdpi.com/2313-0105/11/4/156localized high-concentration electrolytesinterfacial stabilityhigh voltagesingle-crystal Ni-rich layered cathode |
| spellingShingle | Ying Hu Dandan Wang Qijie Yu Ziyi He Fengrui Deng Hao Yan Tinglu Song Jin-Cheng Zheng Yang Dai The Use of Cognate Cosolvent to Mediate Localized High-Concentration Electrolytes for High-Voltage and Long-Cycling Lithium-Metal Batteries Batteries localized high-concentration electrolytes interfacial stability high voltage single-crystal Ni-rich layered cathode |
| title | The Use of Cognate Cosolvent to Mediate Localized High-Concentration Electrolytes for High-Voltage and Long-Cycling Lithium-Metal Batteries |
| title_full | The Use of Cognate Cosolvent to Mediate Localized High-Concentration Electrolytes for High-Voltage and Long-Cycling Lithium-Metal Batteries |
| title_fullStr | The Use of Cognate Cosolvent to Mediate Localized High-Concentration Electrolytes for High-Voltage and Long-Cycling Lithium-Metal Batteries |
| title_full_unstemmed | The Use of Cognate Cosolvent to Mediate Localized High-Concentration Electrolytes for High-Voltage and Long-Cycling Lithium-Metal Batteries |
| title_short | The Use of Cognate Cosolvent to Mediate Localized High-Concentration Electrolytes for High-Voltage and Long-Cycling Lithium-Metal Batteries |
| title_sort | use of cognate cosolvent to mediate localized high concentration electrolytes for high voltage and long cycling lithium metal batteries |
| topic | localized high-concentration electrolytes interfacial stability high voltage single-crystal Ni-rich layered cathode |
| url | https://www.mdpi.com/2313-0105/11/4/156 |
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