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Homogeneous and mechanically stable solid–electrolyte interphase enabled by trioxane-modulated electrolytes for lithium metal batteries

Author

Listed:
  • Qian-Kui Zhang

    (Beijing Institute of Technology
    Beijing Institute of Technology)

  • Xue-Qiang Zhang

    (Beijing Institute of Technology
    Beijing Institute of Technology)

  • Jing Wan

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Nan Yao

    (Tsinghua University)

  • Ting-Lu Song

    (Beijing Institute of Technology)

  • Jin Xie

    (Tsinghua University)

  • Li-Peng Hou

    (Tsinghua University)

  • Ming-Yue Zhou

    (Tsinghua University)

  • Xiang Chen

    (Tsinghua University)

  • Bo-Quan Li

    (Beijing Institute of Technology
    Beijing Institute of Technology)

  • Rui Wen

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Hong-Jie Peng

    (University of Electronic Science and Technology of China)

  • Qiang Zhang

    (Tsinghua University)

  • Jia-Qi Huang

    (Beijing Institute of Technology
    Beijing Institute of Technology)

Abstract

The solid–electrolyte interphase (SEI) in lithium (Li) metal batteries is often heterogeneous, containing a diverse range of species and has poor mechanical stability. The SEI undergoes constant cracking and reconstruction during electrochemical cycling, which is accompanied by the exhaustion of active Li and electrolytes, hindering practical applications of the batteries. Here we propose an in situ structural design of SEI to promote its homogeneity and improve its mechanical stability. A bilayer structure of SEI is tailored through trioxane-modulated electrolytes: the inner layer is dominated by LiF to improve homogeneity while the outer layer contains Li polyoxymethylene to improve mechanical stability, synergistically leading to mitigated reconstruction of SEI and reversible Li plating/stripping. The coin cell consisting of an ultrathin Li metal anode (50 μm) and a high-loading cathode (3.0 mAh cm−2)—with the tailored bilayer SEI—achieves 430 cycles tested at 1.2 mA cm−2, while the cell with an anion-derived SEI undergoes only 200 cycles under same conditions. A prototype 440 Wh kg−1 pouch cell (5.3 Ah), with a low negative/positive capacity ratio of 1.8 and lean electrolytes of 2.1 g Ah−1, achieves 130 cycles.

Suggested Citation

  • Qian-Kui Zhang & Xue-Qiang Zhang & Jing Wan & Nan Yao & Ting-Lu Song & Jin Xie & Li-Peng Hou & Ming-Yue Zhou & Xiang Chen & Bo-Quan Li & Rui Wen & Hong-Jie Peng & Qiang Zhang & Jia-Qi Huang, 2023. "Homogeneous and mechanically stable solid–electrolyte interphase enabled by trioxane-modulated electrolytes for lithium metal batteries," Nature Energy, Nature, vol. 8(7), pages 725-735, July.
  • Handle: RePEc:nat:natene:v:8:y:2023:i:7:d:10.1038_s41560-023-01275-y
    DOI: 10.1038/s41560-023-01275-y
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    Cited by:

    1. Jiawei Chen & Daoming Zhang & Lei Zhu & Mingzhu Liu & Tianle Zheng & Jie Xu & Jun Li & Fei Wang & Yonggang Wang & Xiaoli Dong & Yongyao Xia, 2024. "Hybridizing carbonate and ether at molecular scales for high-energy and high-safety lithium metal batteries," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Yanhua Zhang & Rui Qiao & Qiaona Nie & Peiyu Zhao & Yong Li & Yunfei Hong & Shengjie Chen & Chao Li & Baoyu Sun & Hao Fan & Junkai Deng & Jingying Xie & Feng Liu & Jiangxuan Song, 2024. "Synergetic regulation of SEI mechanics and crystallographic orientation for stable lithium metal pouch cells," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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