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Homogeneous polymer-ionic solvate electrolyte with weak dipole-dipole interaction enabling long cycling pouch lithium metal battery

Author

Listed:
  • Likun Chen

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

  • Tian Gu

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

  • Jinshuo Mi

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

  • Yuhang Li

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

  • Ke Yang

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

  • Jiabin Ma

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

  • Xufei An

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

  • Yuyuan Jiang

    (Tsinghua Shenzhen International Graduate School, Tsinghua University)

  • Danfeng Zhang

    (Tsinghua Shenzhen International Graduate School, Tsinghua University)

  • Xing Cheng

    (Tsinghua Shenzhen International Graduate School, Tsinghua University)

  • Shaoke Guo

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

  • Zhuo Han

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

  • Tingzheng Hou

    (Tsinghua Shenzhen International Graduate School, Tsinghua University)

  • Yidan Cao

    (Tsinghua Shenzhen International Graduate School, Tsinghua University)

  • Ming Liu

    (Tsinghua Shenzhen International Graduate School, Tsinghua University)

  • Wei Lv

    (Tsinghua Shenzhen International Graduate School, Tsinghua University)

  • Yan-Bing He

    (Tsinghua Shenzhen International Graduate School, Tsinghua University)

  • Feiyu Kang

    (Tsinghua Shenzhen International Graduate School, Tsinghua University
    Tsinghua University)

Abstract

Solid polymer electrolytes (SPEs) are considered as promising electrolytes for high-voltage lithium metal batteries. Whereas, the strong dipole-dipole interaction in polymer electrolytes limits the enhancement of the ionic conductivity. Here, we propose the 1,1,2,2-Tetrafluoroethyl-2,2,3,3-Tetrafluoropropylether (TTE) diluent to significantly regulate the dipole-dipole interaction in polymer-ionic solvate electrolytes (TPISEs). The TTE encapsulates ionic solvate to reduce the dipole-dipole interaction of ionic solvate with the polymer matrix, which promotes their homogeneous distribution, creating a continuous ion percolating network among the polymer matrix. The ion conductivity of TPISEs is therefore enhanced to 1.27×10−3 S cm−1 at 25 °C. Meanwhile, the TTE induces the ionic solvate to transform from contact ion pairs to aggregates, contributing to a stable lithium/electrolyte interface with exchange current density 190 times larger than that without TTE. The Li||LiNi0.8Co0.1Mn0.1O2 full cells exhibit good cycling stability from −30 °C to 60 °C. The practical pouch cells consisting of a thin Li metal foil (50 μm) and a high-areal-capacity positive electrode (3.58 mAh cm−2) achieve a high specific energy of 354.4 Wh·kg−1 and maintain 78.1% capacity after 450 cycles at 54 mA g−1 and 25 °C. This work provides a design strategy for SPEs beyond the bottleneck of ionic conductivity for practical solid-state batteries.

Suggested Citation

  • Likun Chen & Tian Gu & Jinshuo Mi & Yuhang Li & Ke Yang & Jiabin Ma & Xufei An & Yuyuan Jiang & Danfeng Zhang & Xing Cheng & Shaoke Guo & Zhuo Han & Tingzheng Hou & Yidan Cao & Ming Liu & Wei Lv & Yan, 2025. "Homogeneous polymer-ionic solvate electrolyte with weak dipole-dipole interaction enabling long cycling pouch lithium metal battery," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-58689-3
    DOI: 10.1038/s41467-025-58689-3
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