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Anion-enrichment interface enables high-voltage anode-free lithium metal batteries

Author

Listed:
  • Minglei Mao

    (Beijing National Laboratory for Condensed Matter Physics
    Huazhong University of Science and Technology)

  • Xiao Ji

    (Huazhong University of Science and Technology)

  • Qiyu Wang

    (Beijing National Laboratory for Condensed Matter Physics)

  • Zejing Lin

    (Beijing National Laboratory for Condensed Matter Physics)

  • Meiying Li

    (Beijing National Laboratory for Condensed Matter Physics)

  • Tao Liu

    (Beijing National Laboratory for Condensed Matter Physics)

  • Chengliang Wang

    (Huazhong University of Science and Technology)

  • Yong-Sheng Hu

    (Beijing National Laboratory for Condensed Matter Physics)

  • Hong Li

    (Beijing National Laboratory for Condensed Matter Physics)

  • Xuejie Huang

    (Beijing National Laboratory for Condensed Matter Physics)

  • Liquan Chen

    (Beijing National Laboratory for Condensed Matter Physics)

  • Liumin Suo

    (Beijing National Laboratory for Condensed Matter Physics)

Abstract

Aggressive chemistry involving Li metal anode (LMA) and high-voltage LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode is deemed as a pragmatic approach to pursue the desperate 400 Wh kg−1. Yet, their implementation is plagued by low Coulombic efficiency and inferior cycling stability. Herein, we propose an optimally fluorinated linear carboxylic ester (ethyl 3,3,3-trifluoropropanoate, FEP) paired with weakly solvating fluoroethylene carbonate and dissociated lithium salts (LiBF4 and LiDFOB) to prepare a weakly solvating and dissociated electrolyte. An anion-enrichment interface prompts more anions’ decomposition in the inner Helmholtz plane and higher reduction potential of anions. Consequently, the anion-derived interface chemistry contributes to the compact and columnar-structure Li deposits with a high CE of 98.7% and stable cycling of 4.6 V NCM811 and LiCoO2 cathode. Accordingly, industrial anode-free pouch cells under harsh testing conditions deliver a high energy of 442.5 Wh kg−1 with 80% capacity retention after 100 cycles.

Suggested Citation

  • Minglei Mao & Xiao Ji & Qiyu Wang & Zejing Lin & Meiying Li & Tao Liu & Chengliang Wang & Yong-Sheng Hu & Hong Li & Xuejie Huang & Liquan Chen & Liumin Suo, 2023. "Anion-enrichment interface enables high-voltage anode-free lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36853-x
    DOI: 10.1038/s41467-023-36853-x
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    1. Shitao Geng & Xiaoju Zhao & Qiuchen Xu & Bin Yuan & Yan Wang & Meng Liao & Lei Ye & Shuo Wang & Zhaofeng Ouyang & Liang Wu & Yongyang Wang & Chenyan Ma & Xiaojuan Zhao & Hao Sun, 2024. "A rechargeable Ca/Cl2 battery," Nature Communications, Nature, vol. 15(1), pages 1-8, 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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