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Origin of dendrite-free lithium deposition in concentrated electrolytes

Author

Listed:
  • Yawei Chen

    (University of Science and Technology of China)

  • Menghao Li

    (Southern University of Science and Technology
    Harbin Institute of Technology)

  • Yue Liu

    (Soochow University)

  • Yulin Jie

    (University of Science and Technology of China)

  • Wanxia Li

    (University of Science and Technology of China)

  • Fanyang Huang

    (University of Science and Technology of China)

  • Xinpeng Li

    (University of Science and Technology of China)

  • Zixu He

    (University of Science and Technology of China)

  • Xiaodi Ren

    (University of Science and Technology of China)

  • Yunhua Chen

    (NIO Incorporation)

  • Xianhui Meng

    (NIO Incorporation)

  • Tao Cheng

    (Soochow University)

  • Meng Gu

    (Southern University of Science and Technology)

  • Shuhong Jiao

    (University of Science and Technology of China)

  • Ruiguo Cao

    (University of Science and Technology of China)

Abstract

The electrolyte solvation structure and the solid-electrolyte interphase (SEI) formation are critical to dictate the morphology of lithium deposition in organic electrolytes. However, the link between the electrolyte solvation structure and SEI composition and its implications on lithium morphology evolution are poorly understood. Herein, we use a single-salt and single-solvent model electrolyte system to systematically study the correlation between the electrolyte solvation structure, SEI formation process and lithium deposition morphology. The mechanism of lithium deposition is thoroughly investigated using cryo-electron microscopy characterizations and computational simulations. It is observed that, in the high concentration electrolytes, concentrated Li+ and anion-dominated solvation structure initiate the uniform Li nucleation kinetically and favor the decomposition of anions rather than solvents, resulting in inorganic-rich amorphous SEI with high interface energy, which thermodynamically facilitates the formation of granular Li. On the contrary, solvent-dominated solvation structure in the low concentration electrolytes tends to exacerbate the solvolysis process, forming organic-rich mosaic SEI with low interface energy, which leads to aggregated whisker-like nucleation and growth. These results are helpful to tackle the long-standing question on the origin of lithium dendrite formation and guide the rational design of high-performance electrolytes for advanced lithium metal batteries.

Suggested Citation

  • Yawei Chen & Menghao Li & Yue Liu & Yulin Jie & Wanxia Li & Fanyang Huang & Xinpeng Li & Zixu He & Xiaodi Ren & Yunhua Chen & Xianhui Meng & Tao Cheng & Meng Gu & Shuhong Jiao & Ruiguo Cao, 2023. "Origin of dendrite-free lithium deposition in concentrated electrolytes," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38387-8
    DOI: 10.1038/s41467-023-38387-8
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    References listed on IDEAS

    as
    1. J.-M. Tarascon & M. Armand, 2001. "Issues and challenges facing rechargeable lithium batteries," Nature, Nature, vol. 414(6861), pages 359-367, November.
    2. John Holoubek & Haodong Liu & Zhaohui Wu & Yijie Yin & Xing Xing & Guorui Cai & Sicen Yu & Hongyao Zhou & Tod A. Pascal & Zheng Chen & Ping Liu, 2021. "Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature," Nature Energy, Nature, vol. 6(3), pages 303-313, March.
    3. Chaojiang Niu & Hongkyung Lee & Shuru Chen & Qiuyan Li & Jason Du & Wu Xu & Ji-Guang Zhang & M. Stanley Whittingham & Jie Xiao & Jun Liu, 2019. "High-energy lithium metal pouch cells with limited anode swelling and long stable cycles," Nature Energy, Nature, vol. 4(7), pages 551-559, July.
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    Cited by:

    1. Zhuangzhuang Cui & Zhuangzhuang Jia & Digen Ruan & Qingshun Nian & Jiajia Fan & Shunqiang Chen & Zixu He & Dazhuang Wang & Jinyu Jiang & Jun Ma & Xing Ou & Shuhong Jiao & Qingsong Wang & Xiaodi Ren, 2024. "Molecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries," Nature Communications, Nature, vol. 15(1), pages 1-12, 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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