Bioinspired gel polymer electrolyte for wide temperature lithium metal battery

Shuohan Liu; Wensheng Tian; Jieqing Shen; Zhikai Wang; Hui Pan; Xuchen Kuang; Cheng Yang; Shunwei Chen; Xiujun Han; Hengdao Quan; Shenmin Zhu

doi:10.1038/s41467-025-57856-w

Bioinspired gel polymer electrolyte for wide temperature lithium metal battery

Nat Commun. 2025 Mar 12;16(1):2474. doi: 10.1038/s41467-025-57856-w.

Authors

Shuohan Liu¹, Wensheng Tian², Jieqing Shen¹, Zhikai Wang¹, Hui Pan³, Xuchen Kuang¹, Cheng Yang⁴, Shunwei Chen⁵, Xiujun Han⁶, Hengdao Quan⁷, Shenmin Zhu⁸

Affiliations

¹ State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, China.
² State Key Laboratory of Space Power-Sources, Shanghai Institute of Space Power-Sources, Shanghai, China.
³ State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, China. panhui115@sjtu.edu.cn.
⁴ State Key Laboratory of Space Power-Sources, Shanghai Institute of Space Power-Sources, Shanghai, China. yangcheng_811@sina.com.
⁵ School of Materials Science and Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan, Shandong, China.
⁶ School of Materials Science and Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan, Shandong, China. xjhan@qlu.edu.cn.
⁷ School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, China.
⁸ State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, China. smzhu@sjtu.edu.cn.

Abstract

Stable operation of Li metal batteries with gel polymer electrolytes in a wide temperature range is highly expected. However, insufficient dynamics of ion transport and unstable electrolyte-electrode interfaces at extreme temperatures greatly hinder their practical applications. We report a bioinspired gel polymer electrolyte that enables high-energy-density Li metal batteries to work stably in a wide temperature range from -30 to 80 °C. The wide-temperature gel polymer electrolyte is fabricated by using a branched polymer of which side chains are double coupled with their asymmetric analogues. The double dipole coupling regulates the Li⁺ coordination environment to form a weak solvation structure that offers fast and uniform Li⁺ deposition at extreme temperatures. Consequently, the non-flammable gel polymer electrolyte displays an ionic conductivity of 1.03 × 10^-4 S cm^-1 at -40 °C and a Li⁺ transference number of 0.83. The Li metal batteries with LiNi_0.8Co_0.1Mn_0.1O₂ positive electrode deliver initial specific discharge capacities of 121.4 mAh g^-1 at -30 °C and 172.2 mAh g^-1 at 80 °C, with corresponding discharge currents of 18.8 mA g^-1 and 188 mA g^-1, respectively. Additionally, a pouch cell delivers a specific energy up to 490.8 Wh kg^-1.