Covalent and polyfluorinated lithium salt for stable LiCoO2 batteries at high temperature and high voltage

Qi Xiong, Ruijie Wang, Dedi Li, Ruhong Li, Shuoqing Zhang, Zhiquan Wei, Shimei Li, Dechao Zhang, Shixun Wang, Hu Hong, Li Song (), Qi Liu (), Xiulin Fan () and Chunyi Zhi ()
Additional contact information
Qi Xiong: City University of Hong Kong, Hong Kong Center for Cerebro-Cardiovascular Health Engineering (COCHE)
Ruijie Wang: University of Science and Technology of China, National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, Hefei National Laboratory for Physical Sciences at the Microscale, School of Chemistry and Materials Science
Dedi Li: City University of Hong Kong, Department of Materials Science and Engineering
Ruhong Li: Zhejiang University, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering
Shuoqing Zhang: Zhejiang University, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering
Zhiquan Wei: City University of Hong Kong, Department of Materials Science and Engineering
Shimei Li: City University of Hong Kong, Hong Kong Center for Cerebro-Cardiovascular Health Engineering (COCHE)
Dechao Zhang: City University of Hong Kong, Hong Kong Center for Cerebro-Cardiovascular Health Engineering (COCHE)
Shixun Wang: City University of Hong Kong, Department of Materials Science and Engineering
Hu Hong: City University of Hong Kong, Department of Materials Science and Engineering
Li Song: University of Science and Technology of China, National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, Hefei National Laboratory for Physical Sciences at the Microscale, School of Chemistry and Materials Science
Qi Liu: City University of Hong Kong, Department of Physics
Xiulin Fan: Zhejiang University, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering
Chunyi Zhi: City University of Hong Kong, Hong Kong Center for Cerebro-Cardiovascular Health Engineering (COCHE)

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract Elevating the charge cut-off voltage of the LiCoO2 positive electrode beyond 4.5 V has already been the focus to unlock its energy for portable electronics, whereas the severe phase transitions during the delithiation of LiCoO2 from 4.5 V to 4.7 V can ruin the electrode structure. Besides, the poor thermal and hydrolytic stabilities of traditional lithium salt (LiPF6) prevent batteries from working at high temperatures and increase production costs and environmental pollution. Here, we show that using covalent lithium nonafluoro-n-butanesulfonate as a fluorine-rich lithium salt to create a robust LiF-rich cathode electrolyte interphase, which effectively impedes the surface destruction, we successfully realize a stable LiCoO2 battery at a high voltage of 4.7 V and demonstrate a 2.14 Ah Li|| LiCoO2 pouch cell with a stack-level specific energy of 518 Wh kg−1 (without packaging). Furthermore, its satisfactory thermal stability empowers LiCoO2 to work at a harsh condition of 60 °C and 4.6 V. Even more, its antihydrolytic stability enables the LiCoO2 battery to work with the electrolyte with 200 or even 1000 ppm water contamination. Lithium nonafluoro-n-butanesulfonate presents itself as a potentially viable lithium salt for advanced lithium batteries, offering the prospect of high voltage, improved thermal stability and eco-friendliness.

Date: 2025
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DOI: 10.1038/s41467-025-65256-3

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