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

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, Jingwen Zhao, Jiangwei Ju, Zhiwei Hu, Fan-Hsiu Chang, Chang-Yang Kuo, Chien-Te Chen, André Hilger, Ingo Manke, Shanmu Dong and Guanglei Cui ()
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Li Du: Chinese Academy of Sciences
Gaojie Xu: Chinese Academy of Sciences
Chenghao Sun: Chinese Academy of Sciences
Yu-Han Zhang: Chinese Academy of Sciences
Huanrui Zhang: Chinese Academy of Sciences
Tiantian Dong: Chinese Academy of Sciences
Lang Huang: Chinese Academy of Sciences
Jun Ma: Chinese Academy of Sciences
Fu Sun: Chinese Academy of Sciences
Chuanchuan Li: Chinese Academy of Sciences
Xiangchun Zhuang: Chinese Academy of Sciences
Shenghang Zhang: Chinese Academy of Sciences
Jiedong Li: Chinese Academy of Sciences
Bin Xie: Chinese Academy of Sciences
Jinzhi Wang: Chinese Academy of Sciences
Jingwen Zhao: Chinese Academy of Sciences
Jiangwei Ju: Chinese Academy of Sciences
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
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
Guanglei Cui: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-57964-7

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