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Wide-temperature range and high safety electrolytes for high-voltage Li-metal batteries

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Abstract

Along with the keeping growing demand for high-energy-density energy storage system, high-voltage Li-metal batteries (LMBs) have attracted many attentions. In view of many defects of the commercial electrolytes, such as flammability, limited operation temperature range, and severe Li dendrite growth, non-flammable phosphate-based localized highly concentrated electrolytes (LHCE) have been explored as one of the safe electrolytes for LMBs. But until now there is rare report on wide-temperature range LMBs using phosphate-based electrolytes. Here, we prepare a wide-temperature LHCE, which is composed of lithium difluoro(oxalato)borate (LiDFOB), triethyl phosphate (TEP), and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (HFE), and explore the applicability in wide-temperature LMBs from −40 to 70 °C. In the LHCE, both TEP and HFE are non-flammable, and Li+ is highly coordinated with TEP and DFOB−, which can effectively inhibit the TEP decomposition on anode, and facilitate the preferential reduction of DFOB−, thus obtain a robust solid electrolyte interphase (SEI) to suppress Li dendrite growth and side reactions. Therefore, this LHCE can not only endow Li/Cu and Li/Li cells with high Coulombic efficiency (CE) and long cycling lifespan, but also be applied to LiFePO4 (LFP)/Li and LiNi0.5Co0.2Mn0.3O2 (NCM523)/Li LMBs. Most importantly, the NCM523/Li LMBs with LHCE can deliver stable cycling performance at 4.5 V high-voltage and high-temperature (70 °C), as well as excellent low-temperature capacity retention even though both charging and discharging process were carried out at −40 °C.

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Acknowledgements

This work is financially supported by the National Natural Science Foundation of China (Nos 22179142 and 22075314). The XPS characterization is supported by Nano-X (Vacuum Interconnected Nanotech Workstation, Chinese Academy of Sciences, Suzhou 215123, China).

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  1. Anran Pan and Zhicheng Wang contributed equally to this work.

Authors and Affiliations

  1. i-lab, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences, Suzhou, 215123, China

    Anran Pan, Zhicheng Wang, Fengrui Zhang, Lei Wang, Jingjing Xu & Xiaodong Wu

  2. Nano Science and Technology Institute, University of Science and Technology of China, Hefei, 230026, China

    Anran Pan & Lei Wang

  3. Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China

    Jieyun Zheng

  4. College of Textile and Clothing Engineering, Soochow University, Suzhou, 215123, China

    Jianchen Hu

  5. Phylion battery Co., Ltd., Suzhou, 215123, China

    Chenglong Zhao

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  1. Anran Pan
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Correspondence to Jingjing Xu, Jieyun Zheng or Xiaodong Wu.

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Pan, A., Wang, Z., Zhang, F. et al. Wide-temperature range and high safety electrolytes for high-voltage Li-metal batteries. Nano Res. 16, 8260–8268 (2023). https://doi.org/10.1007/s12274-022-4655-1

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