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Dynamical evolution of CO2 and H2O on garnet electrolyte elucidated by ambient pressure X-ray spectroscopies

Author

Listed:
  • Nian Zhang

    (Chinese Academy of Sciences
    Chinese Academy of Sciences)

  • Guoxi Ren

    (Chinese Academy of Sciences)

  • Lili Li

    (Chinese Academy of Sciences)

  • Zhi Wang

    (Chinese Academy of Sciences)

  • Pengfei Yu

    (Chinese Academy of Sciences)

  • Xiaobao Li

    (Chinese Academy of Sciences)

  • Jing Zhou

    (Chinese Academy of Sciences)

  • Hui Zhang

    (Chinese Academy of Sciences
    Chinese Academy of Sciences)

  • Linjuan Zhang

    (Chinese Academy of Sciences)

  • Zhi Liu

    (Shanghai Tech University)

  • Xiaosong Liu

    (Chinese Academy of Sciences
    Shanghai Tech University
    University of Science and Technology of China)

Abstract

Garnet-type Li6.5La3Zr1.5Ta0.5O12 (LLZO) is considered a promising solid electrolyte, but the surface degradation in air hinders its application for all-solid-state battery. Recent studies have mainly focused on the final products of the LLZO surface reactions due to lacking of powerful in situ characterization methods. Here, we use ambient pressure X-ray spectroscopies to in situ investigate the dynamical evolution of LLZO surface in different gas environments. The newly developed ambient pressure mapping of resonant Auger spectroscopy clearly distinguishes the lithium containing species, including LiOH, Li2O, Li2CO3 and lattice oxygen. The reaction of CO2 with LLZO to form Li2CO3 is found to be a thermodynamically favored self-limiting reaction. On the contrary, the reaction of H2O with LLZO lags behind that of CO2, but intensifies at high pressure. More interestingly, the results provide direct spectroscopic evidence for the existence of Li+/H+ exchange and reveal the importance of the initial layer formed on clean electrolyte surface in determining their air stability. This work demonstrates that the newly developed in situ technologies pave a new way to investigate the oxygen evolution and surface degradation mechanism in energy materials.

Suggested Citation

  • Nian Zhang & Guoxi Ren & Lili Li & Zhi Wang & Pengfei Yu & Xiaobao Li & Jing Zhou & Hui Zhang & Linjuan Zhang & Zhi Liu & Xiaosong Liu, 2024. "Dynamical evolution of CO2 and H2O on garnet electrolyte elucidated by ambient pressure X-ray spectroscopies," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47071-4
    DOI: 10.1038/s41467-024-47071-4
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    References listed on IDEAS

    as
    1. Jürgen Janek & Wolfgang G. Zeier, 2016. "A solid future for battery development," Nature Energy, Nature, vol. 1(9), pages 1-4, September.
    2. Jie-Nan Zhang & Qinghao Li & Chuying Ouyang & Xiqian Yu & Mingyuan Ge & Xiaojing Huang & Enyuan Hu & Chao Ma & Shaofeng Li & Ruijuan Xiao & Wanli Yang & Yong Chu & Yijin Liu & Huigen Yu & Xiao-Qing Ya, 2019. "Trace doping of multiple elements enables stable battery cycling of LiCoO2 at 4.6 V," Nature Energy, Nature, vol. 4(7), pages 594-603, July.
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