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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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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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.
The authors declare no competing interests.
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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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