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Monolithic solid–electrolyte interphases formed in fluorinated orthoformate-based electrolytes minimize Li depletion and pulverization

Author

Listed:
  • Xia Cao

    (Pacific Northwest National Laboratory)

  • Xiaodi Ren

    (Pacific Northwest National Laboratory)

  • Lianfeng Zou

    (Pacific Northwest National Laboratory)

  • Mark H. Engelhard

    (Pacific Northwest National Laboratory)

  • William Huang

    (Stanford University)

  • Hansen Wang

    (Stanford University)

  • Bethany E. Matthews

    (Pacific Northwest National Laboratory)

  • Hongkyung Lee

    (Pacific Northwest National Laboratory)

  • Chaojiang Niu

    (Pacific Northwest National Laboratory)

  • Bruce W. Arey

    (Pacific Northwest National Laboratory)

  • Yi Cui

    (Stanford University)

  • Chongmin Wang

    (Pacific Northwest National Laboratory)

  • Jie Xiao

    (Pacific Northwest National Laboratory)

  • Jun Liu

    (Pacific Northwest National Laboratory)

  • Wu Xu

    (Pacific Northwest National Laboratory)

  • Ji-Guang Zhang

    (Pacific Northwest National Laboratory)

Abstract

Lithium (Li) pulverization and associated large volume expansion during cycling is one of the most critical barriers for the safe operation of Li-metal batteries. Here, we report an approach to minimize the Li pulverization using an electrolyte based on a fluorinated orthoformate solvent. The solid–electrolyte interphase (SEI) formed in this electrolyte clearly exhibits a monolithic feature, which is in sharp contrast with the widely reported mosaic- or multilayer-type SEIs that are not homogeneous and could lead to uneven Li stripping/plating and fast Li and electrolyte depletion over cycling. The highly homogeneous and amorphous SEI not only prevents dendritic Li formation, but also minimizes Li loss and volumetric expansion. Furthermore, this new electrolyte strongly suppresses the phase transformation of the LiNi0.8Co0.1Mn0.1O2 cathode (from layered structure to rock salt) and stabilizes its structure. Tests of high-voltage Li||NMC811 cells show long-term cycling stability and high rate capability, as well as reduced safety concerns.

Suggested Citation

  • Xia Cao & Xiaodi Ren & Lianfeng Zou & Mark H. Engelhard & William Huang & Hansen Wang & Bethany E. Matthews & Hongkyung Lee & Chaojiang Niu & Bruce W. Arey & Yi Cui & Chongmin Wang & Jie Xiao & Jun Li, 2019. "Monolithic solid–electrolyte interphases formed in fluorinated orthoformate-based electrolytes minimize Li depletion and pulverization," Nature Energy, Nature, vol. 4(9), pages 796-805, September.
    • Handle: RePEc:nat:natene:v:4:y:2019:i:9:d:10.1038_s41560-019-0464-5
    DOI: 10.1038/s41560-019-0464-5
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    Cited by:

    1. Yan Zhao & Tianhong Zhou & Timur Ashirov & Mario El Kazzi & Claudia Cancellieri & Lars P. H. Jeurgens & Jang Wook Choi & Ali Coskun, 2022. "Fluorinated ether electrolyte with controlled solvation structure for high voltage lithium metal batteries," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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