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Lithium inventory tracking as a non-destructive battery evaluation and monitoring method

Nature Energy volume 9, pages 612–621 (2024)Cite this article

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Abstract

Tracking the active lithium (Li) inventory in an electrode shows the true state of a Li battery, akin to a fuel gauge for an engine. However, non-destructive Li inventory tracking is currently unavailable. Here we used the theoretical capacity of a transition metal oxide to convert capacity into a Li inventory analysis. The Li inventory in electrodes was tracked reliably to show how battery formulations and test methods affect performance. Contrary to capacity, Li inventory tracking reveals stoichiometric variations near the electrode–electrolyte interface. Verifiable results rationalized differences in measurements, clarifying and reducing interferences from cell formulations and experimental manipulations. By tracing four variables from formation to end-of-life, we characterize electrode and cell performance with a thermodynamic framework. Accurate rationalization of subtle differences in Li inventory utilization promises precise battery engineering, evaluation, failure analysis and risk mitigation. The method could be applicable from cell design optimization and fabrication to battery management, improving battery performance and reliability.

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Fig. 1: Test results and Li inventory tracking of nine cells in the formation cycle.
Fig. 2: The charge–discharge profiles of a GITT formation cycle.
Fig. 3: Test results of CA_4.2, 4.4 and 4.6 cells cycled at C/3 rate with three Vmax cut-offs.
Fig. 4: Tracing variations of critical variables in cycle ageing performance in CA_4.2, 4.4 and 4.6 cells.
Fig. 5: Trace of variations in (QTh × Δx) as a function of cycle number.

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Data availability

All data used in this work are contained in the article and Supplementary Information. The datasets are also available at https://doi.org/10.17605/OSF.IO/2W4K3.

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Acknowledgements

The work presented in this article comprised three stages of effort and development that should be recognized. The initial concept was developed in a project supported in part under Idaho National Laboratory’s Laboratory Directed Research and Development programme (project no. 19P45-013FP) for a lithium-ion battery reliability and safety diagnostic study. This work was later supported by a project funded by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy in the Advanced Battery Materials Research Program (Battery500 Consortium) to apply the concept to diagnose the performance and degradation of high-energy rechargeable lithium metal batteries, where the bulk of the data was used in this study. The extension of the experimental work for the analysis is supported under the Earth-Abundant Cathode Material Consortium led by Argonne National Laboratory, and the goal is to assist material research with a better diagnostic tool and approach. Idaho National Laboratory is operated by Battelle Energy Alliance under contract no. DE-AC07-05ID14517 for the US Department of Energy.

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Authors and Affiliations

  1. Energy Storage and Electric Transportation, Idaho National Laboratory, Idaho Falls, ID, USA

    Meng Li, Yulun Zhang & Boryann Liaw

  2. The NorthEast Center for Chemical Energy Storage, Binghamton University (SUNY), Binghamton, NY, USA

    Hui Zhou, Fengxia Xin & M. Stanley Whittingham

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  1. Meng Li
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Contributions

B.L. and M.L. conceived the conceptual approach for the analysis. M.L. and Y.Z. conducted the analyses. H.Z., F.X. and M.S.W. conducted the experiments and produced the data for the analyses. B.L. wrote the paper with the help of all authors.

Corresponding author

Correspondence to Boryann Liaw.

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Competing interests

B.L., M.L. and Y.Z. disclosed that Battelle Energy Alliance has filed US patent applications 17/149,046 and 18/185,018. US Patent 11,740,290 has been issued. The other authors declare no competing interests.

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Nature Energy thanks David Ansean and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Figs. 1–8 and Discussion.

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Li, M., Zhang, Y., Zhou, H. et al. Lithium inventory tracking as a non-destructive battery evaluation and monitoring method. Nat Energy 9, 612–621 (2024). https://doi.org/10.1038/s41560-024-01476-z

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