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Smart gel polymer electrolytes enlightening high safety and long life sodium ion batteries

Author

Listed:
  • Li Du

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory
    Shandong University of Science and Technology)

  • Gaojie Xu

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Chenghao Sun

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Yu-Han Zhang

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Huanrui Zhang

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Tiantian Dong

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Lang Huang

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Jun Ma

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Fu Sun

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Chuanchuan Li

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Xiangchun Zhuang

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Shenghang Zhang

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Jiedong Li

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Bin Xie

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Jinzhi Wang

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Jingwen Zhao

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Jiangwei Ju

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Zhiwei Hu

    (Max Planck Institute for Chemical Physics of Solids)

  • Fan-Hsiu Chang

    (National Synchrotron Radiation Research Center)

  • Chang-Yang Kuo

    (National Synchrotron Radiation Research Center
    National Yang Ming Chiao Tung University)

  • Chien-Te Chen

    (National Yang Ming Chiao Tung University)

  • André Hilger

    (Helmholtz-Zentrum Berlin für Materialien und Energie)

  • Ingo Manke

    (Helmholtz-Zentrum Berlin für Materialien und Energie)

  • Shanmu Dong

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

  • Guanglei Cui

    (Chinese Academy of Sciences
    Shandong Energy Institute
    Qingdao New Energy Shandong Laboratory)

Abstract

The overall performance of sodium-ion batteries, particularly regarding safety and cycle life, remains below expectations due to severe degradation of electrode materials and the electrode/electrolyte interphase. Herein, we develop a smart gel polymer electrolyte for hard carbon||NaNi1/3Fe1/3Mn1/3O2 batteries through the in situ radical polymerization of a cyanoethylurea-containing methacrylate monomer and an isocyanate-based methacrylate monomer in conventional NaPF6-carbonate-based electrolytes. We demonstrate that the smart gel polymer electrolyte facilitates the formation of robust electrode/electrolyte interphase layers, thus improving the thermal and chem-electrochemical stability of the electrodes. When the temperature exceeds 120 °C, the in situ formed gel polymer electrolyte undergoes further crosslinking through nucleophilic addition reactions between urea and isocyanate motifs. This additional crosslinking blocks ion transportation and inhibits crosstalk effects, thus boosting the safety of pouch-type hard carbon||NaNi1/3Fe1/3Mn1/3O2 batteries. Moreover, the smart gel polymer electrolyte enables hard carbon||NaNi1/3Fe1/3Mn1/3O2 full cells to achieve improved cycle life even at the elevated temperature of 50 °C. The design philosophy behind the development of in situ formed smart gel polymer electrolytes offers valuable guidance for creating high-safety, long-life, and sustainable sodium-ion batteries.

Suggested Citation

  • Li Du & Gaojie Xu & Chenghao Sun & Yu-Han Zhang & Huanrui Zhang & Tiantian Dong & Lang Huang & Jun Ma & Fu Sun & Chuanchuan Li & Xiangchun Zhuang & Shenghang Zhang & Jiedong Li & Bin Xie & Jinzhi Wang, 2025. "Smart gel polymer electrolytes enlightening high safety and long life sodium ion batteries," Nature Communications, Nature, vol. 16(1), pages 1-14, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57964-7
    DOI: 10.1038/s41467-025-57964-7
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