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High-throughput Li plating quantification for fast-charging battery design

Nature Energy volume 8, pages 450–461 (2023)Cite this article

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Abstract

Fast charging of most commercial lithium-ion batteries is limited due to fear of lithium plating on the graphite anode, which is difficult to detect and poses considerable safety risk. Here we demonstrate the power of simple, accessible and high-throughput cycling techniques to quantify irreversible Li plating spanning data from over 200 cells. We first observe the effects of energy density, charge rate, temperature and state of charge on lithium plating, use the results to refine a mature physics-based electrochemical model and provide an interpretable empirical equation for predicting the plating onset state of charge. We then explore the reversibility of lithium plating and its connection to electrolyte design for preventing irreversible Li accumulation. Finally, we design a method to quantify in situ Li plating for commercially relevant graphite|LiNi0.5Mn0.3Co0.2O2 (NMC) cells and compare with results from the experimentally convenient Li|graphite configuration. The hypotheses and abundant data herein were generated primarily with equipment universal to the battery researcher, encouraging further development of innovative testing methods and data processing that enable rapid battery engineering.

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Fig. 1: Determining irreversible Li plating as a function of charge rate and length.
Fig. 2: Irreversible Li plating and plating onsets with modelling.
Fig. 3: Electrolyte engineering to reduce irreversible Li plating.
Fig. 4: Full-cells electrolyte testing with dead Li estimation and titration.
Fig. 5: Determining irreversible Li in full-cells, comparison with half-cells and titration validation.

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Data availability

All data supporting the findings in this study are available within the paper and the Supplementary Information. Source data are provided with this paper.

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Acknowledgements

This work was largely supported by the Vehicle Technologies Office of the US Department of Energy under the XCEL Fast Charging Program (eXtreme Fast Charge Cell Evaluation of Lithium ion Batteries, XCEL). Part of this work was authored by the National Renewable Energy Laboratory, operated by the Alliance for Sustainable Energy, LLC, for the US Department of Energy (DOE) under contract DE-AC36-08GO28308. H.K.B., D.E.B. and E.J.M. acknowledge support from the National Science Foundation Graduate Research Fellowship Program under grant DGE 1106400. T.-Y.H. gratefully acknowledges support from both the Ministry of Education in Taiwan and UC Berkeley College of Chemistry through the Taiwan Fellowship Program. The authors thank S. Trask, A. Jansen, A. Dunlop and B. Polzin from the Argonne National Laboratory Cell Analysis, Modeling, and Prototyping (CAMP) facility for providing laminate electrodes used in the study. Z.M.K. thanks J. Heo for assistance with the design of Fig. 3e.

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Author notes

  1. Brendan M. Wirtz & Eric J. McShane

    Present address: Department of Chemical Engineering, Stanford University, Stanford, CA, USA

Authors and Affiliations

  1. Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA, USA

    Zachary M. Konz, Brendan M. Wirtz, Tzu-Yang Huang, Helen K. Bergstrom, Matthew J. Crafton, David E. Brown, Eric J. McShane & Bryan D. McCloskey

  2. Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Zachary M. Konz, Tzu-Yang Huang, Helen K. Bergstrom, Matthew J. Crafton, David E. Brown, Eric J. McShane & Bryan D. McCloskey

  3. Energy Conversion and Storage Systems Center, National Renewable Energy Laboratory, Golden, CO, USA

    Ankit Verma & Andrew M. Colclasure

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Contributions

Z.M.K. conceived ideas, performed experiments, developed methods, wrote analysis code and wrote the manuscript and Supplementary Information. B.M.W. developed Fig. 3 methods and analysis with Z.M.K. and provided continuous project and manuscript feedback. A.V. and A.M.C. performed EChem modelling simulations and wrote the corresponding manuscript/Supplementary Information sections. T.-Y.H. helped Z.M.K. to build the titration syringe attachment. H.K.B. helped with experiment design for Li plating on copper and electrolyte conductivity measurements. M.J.C. and T.-Y.H. provided feedback and assistance with titrations. D.E.B. and E.J.M. provided project feedback, troubleshooting ideas and mentorship. A.M.C. also conceived Fig. 2 experiments with Z.M.K., led EChem model modifications and provided continuous project feedback. B.D.M. was lead project supervisor, conceived ideas and was primary manuscript editor. All authors edited and provided feedback on the manuscript.

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Correspondence to Bryan D. McCloskey.

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

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Konz, Z.M., Wirtz, B.M., Verma, A. et al. High-throughput Li plating quantification for fast-charging battery design. Nat Energy 8, 450–461 (2023). https://doi.org/10.1038/s41560-023-01194-y

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