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Gas induced formation of inactive Li in rechargeable lithium metal batteries

Author

Listed:
  • Yuxuan Xiang

    (Xiamen University
    Westlake University)

  • Mingming Tao

    (Xiamen University)

  • Xiaoxuan Chen

    (Xiamen University)

  • Peizhao Shan

    (Xiamen University)

  • Danhui Zhao

    (Xiamen University)

  • Jue Wu

    (Xiamen University)

  • Min Lin

    (Xiamen University)

  • Xiangsi Liu

    (Xiamen University)

  • Huajin He

    (Xiamen University)

  • Weimin Zhao

    (Binzhou University)

  • Yonggang Hu

    (Xiamen University)

  • Junning Chen

    (Xiamen University)

  • Yuexing Wang

    (China Academy of Engineering Physics)

  • Yong Yang

    (Xiamen University)

Abstract

The formation of inactive lithium by side reactions with liquid electrolyte contributes to cell failure of lithium metal batteries. To inhibit the formation and growth of inactive lithium, further understanding of the formation mechanisms and composition of inactive lithium are needed. Here we study the impact of gas producing reactions on the formation of inactive lithium using ethylene carbonate as a case study. Ethylene carbonate is a common electrolyte component used with graphite-based anodes but is incompatible with Li metal anodes. Using mass spectrometry titrations combined with 13C and 2H isotopic labeling, we reveal that ethylene carbonate decomposition continuously releases ethylene gas, which further reacts with lithium metal to form the electrochemically inactive species LiH and Li2C2. In addition, phase-field simulations suggest the non-ionically conducting gaseous species could result in an uneven distribution of lithium ions, detrimentally enhancing the formation of dendrites and dead Li. By optimizing the electrolyte composition, we selectively suppress the formation of ethylene gas to limit the formation of LiH and Li2C2 for both Li metal and graphite-based anodes.

Suggested Citation

  • Yuxuan Xiang & Mingming Tao & Xiaoxuan Chen & Peizhao Shan & Danhui Zhao & Jue Wu & Min Lin & Xiangsi Liu & Huajin He & Weimin Zhao & Yonggang Hu & Junning Chen & Yuexing Wang & Yong Yang, 2023. "Gas induced formation of inactive Li in rechargeable lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-022-35779-0
    DOI: 10.1038/s41467-022-35779-0
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    References listed on IDEAS

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    1. Michael A. Hope & Bernardine L. D. Rinkel & Anna B. Gunnarsdóttir & Katharina Märker & Svetlana Menkin & Subhradip Paul & Ivan V. Sergeyev & Clare P. Grey, 2020. "Selective NMR observation of the SEI–metal interface by dynamic nuclear polarisation from lithium metal," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    2. Jun Liu & Zhenan Bao & Yi Cui & Eric J. Dufek & John B. Goodenough & Peter Khalifah & Qiuyan Li & Bor Yann Liaw & Ping Liu & Arumugam Manthiram & Y. Shirley Meng & Venkat R. Subramanian & Michael F. T, 2019. "Pathways for practical high-energy long-cycling lithium metal batteries," Nature Energy, Nature, vol. 4(3), pages 180-186, March.
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