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Quantification of reversible and irreversible lithium in practical lithium-metal batteries

Nature Energy volume 7, pages 1031–1041 (2022)Cite this article

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Abstract

Accurate assessment of the reversibility of electrodes is crucial for battery performance evaluations. However, it is challenging to acquire the true reversibility of the Li anode in lithium-metal batteries, mainly because an excessive amount of Li is commonly used. Here we propose an analytic approach to quantitatively evaluate the reversibility of practical lithium-metal batteries. We identify key parameters that govern the anode reversibility and subsequently establish their relationship with the cycle number by considering the mass of active and inactive Li of the cycled Li anode. Using this method, we show that the mass of active Li can be quantitatively distinguished from the mass of inactive Li of the cycled anodes in Amp hour-level pouch cells. This work opens an avenue for accurately assessing degradation and failure in lithium-metal batteries.

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Fig. 1: Reversibility and irreversibility of a cycled LMA.
Fig. 2: The pathways for key parameter calculation.
Fig. 3: Decoupling and quantifying inactive Li0 and active Li0.
Fig. 4: Resolved irreversibility and reversibility from quantified results.
Fig. 5: Dynamic failure model predicted by qualitative and quantitative analysis.

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The datasets analysed and generated during the current study are included in the paper and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

This work was supported by National Natural Science Foundation of China (grant number 52001320, 51872305), ‘Lingyan’ Research and Development Plan of Zhejiang Province (grant number 2022C01071) and China Postdoctoral Science Foundation funded project (grant number 2019TQ0331, 2019M662123). Y.S.M. acknowledges funding support from the Zable Endowed Chair of Energy Technology and the Sustainable Power & Energy Center of UC San Diego. W.D. thanks F. Zhao for helpful discussions about the work; Q. Guo for discussions about mathematical equations; Z. Jiang, Q Han, W. Fang and J. Wang for their help on the pouch cell assembly and tests; and A. Cao, Y. Yu, S. Liu and H. Li for their help on ICP-OES and GC characterizations. W.D. thanks Y. Han for help with GC analysis, Y. Li for Ar-BET characterizations and K. Shen for ICP-OES analysis from the testing centre of NIMTE, CAS.

Author information

Author notes

  1. These authors contributed equally: Wei Deng, Xue Yin, Wurigumula Bao.

Authors and Affiliations

  1. Advanced Li-ion Battery Engineering Laboratory of Zhejiang Province, Key Laboratory of Graphene Technologies and Applications of Zhejiang Province and CAS Engineering Laboratory for Graphene, Ningbo Institute of Materials Technology & Engineering, Chinese Academy of Sciences (CAS), Zhejiang, P. R. China

    Wei Deng, Xue Yin, Xufeng Zhou, Zhiyuan Hu, Bangyi He, Bao Qiu & Zhaoping Liu

  2. Department of NanoEngineering, University of California, San Diego, CA, USA

    Wurigumula Bao & Ying Shirley Meng

  3. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, P. R. China

    Xufeng Zhou, Bao Qiu & Zhaoping Liu

  4. Materials Science and Engineering, University of California, San Diego, CA, USA

    Ying Shirley Meng

  5. Pritzker School of Molecular Engineering, University of Chicago, Chicago, IL, USA

    Ying Shirley Meng

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Contributions

W.D., X.Z., Y.S.M. and Z.L. conceived the concept and the project. W.D. and W.B. performed the analytical procedures and data analysis. W.D. and X.Y. performed the ICP-OES characterizations. W.D., Z.H. and B.H. assembled and tested the pouch cells. W.D., W.B., X.Z., B.Q., Y.S.M. and Z.L. wrote and revised the manuscript. All authors discussed the results and reviewed the manuscript.

Corresponding authors

Correspondence to Xufeng Zhou, Ying Shirley Meng or Zhaoping Liu.

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Supplementary Figs. 1–27, Discussion and Tables 1–12.

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Deng, W., Yin, X., Bao, W. et al. Quantification of reversible and irreversible lithium in practical lithium-metal batteries. Nat Energy 7, 1031–1041 (2022). https://doi.org/10.1038/s41560-022-01120-8

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