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Ultrafast deposition of faceted lithium polyhedra by outpacing SEI formation

Nature volume 620, pages 86–91 (2023)Cite this article

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Abstract

Electrodeposition of lithium (Li) metal is critical for high-energy batteries1. However, the simultaneous formation of a surface corrosion film termed the solid electrolyte interphase (SEI)2 complicates the deposition process, which underpins our poor understanding of Li metal electrodeposition. Here we decouple these two intertwined processes by outpacing SEI formation at ultrafast deposition current densities3 while also avoiding mass transport limitations. By using cryogenic electron microscopy4,5,6,7, we discover the intrinsic deposition morphology of metallic Li to be that of a rhombic dodecahedron, which is surprisingly independent of electrolyte chemistry or current collector substrate. In a coin cell architecture, these rhombic dodecahedra exhibit near point-contact connectivity with the current collector, which can accelerate inactive Li formation8. We propose a pulse-current protocol that overcomes this failure mode by leveraging Li rhombic dodecahedra as nucleation seeds, enabling the subsequent growth of dense Li that improves battery performance compared with a baseline. While Li deposition and SEI formation have always been tightly linked in past studies, our experimental approach enables new opportunities to fundamentally understand these processes decoupled from each other and bring about new insights to engineer better batteries.

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Fig. 1: Transition of different dendritic Li to identical faceted Li polyhedra.
Fig. 2: Atomic-resolution cryo-EM of Li rhombic dodecahedra with faceting behaviours.
Fig. 3: Electrochemical analysis of Li plating pathways at ultrafast and low current density regimes.
Fig. 4: Li plating as rhombic dodecahedra in coin cell geometry and its failure mechanism analysis.

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Data availability

The data that support the findings of this study are available from the corresponding author on reasonable request.

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Acknowledgements

We acknowledge the support of the National Science Foundation (CBET-2143677) and the use of the University of California, Los Angeles California NanoSystems Institute EICN Facilities.

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Authors and Affiliations

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

    Xintong Yuan, Bo Liu & Yuzhang Li

  2. California NanoSystems Institute, University of California, Los Angeles, Los Angeles, CA, USA

    Matthew Mecklenburg

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Contributions

X.Y. and Y.L. conceived the project and designed the experiments. X.Y. built the UME set-up and performed electrochemical experiments and SEM characterization. B.L. helped with COMSOL simulations and data analysis. X.Y. and Y.L. carried out cryo-EM experiments. M.M. advised on microscope and imaging analyses. X.Y. and Y.L. co-wrote the manuscript. All authors discussed the results and commented on the manuscript.

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Correspondence to Yuzhang Li.

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

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Yuan, X., Liu, B., Mecklenburg, M. et al. Ultrafast deposition of faceted lithium polyhedra by outpacing SEI formation. Nature 620, 86–91 (2023). https://doi.org/10.1038/s41586-023-06235-w

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