Stress-driven lithium dendrite growth mechanism and dendrite mitigation by electroplating on soft substrates

Abstract

Problems related to dendrite growth on lithium-metal anodes such as capacity loss and short circuit present major barriers to next-generation high-energy-density batteries. The development of successful lithium dendrite mitigation strategies is impeded by an incomplete understanding of the Li dendrite growth mechanisms, and in particular, Li-plating-induced internal stress in Li metal and its effect on Li growth morphology are not well addressed. Here, we reveal the enabling role of plating residual stress in dendrite formation through depositing Li on soft substrates and a stress-driven dendrite growth model. We show that dendrite growth is mitigated on such soft substrates through surface-wrinkling-induced stress relaxation in the deposited Li film. We demonstrate that this dendrite mitigation mechanism can be utilized synergistically with other existing approaches in the form of three-dimensional soft scaffolds for Li plating, which achieves higher coulombic efficiency and better capacity retention than that for conventional copper substrates.

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Fig. 1: Cu thin film wrinkling during Li plating and dendrite mitigation by using soft substrate.
Fig. 2: Optical microscope observation of Cu current collectors during and after Li plating.
Fig. 3: Profilometer observation of Cu current collectors during and after Li plating.
Fig. 4: Scanning electron microscopy observation of Li morphology after plating on soft and hard substrates.
Fig. 5: Stress-driven Li whisker growth model.
Fig. 6: Fabrication and comparison of 3D Cu@PDMS substrates.

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Acknowledgements

We gratefully acknowledge the use of facilities within the LeRoy Eyring Center for Solid State Science at Arizona State University. L.H. F.W. and M.T. acknowledge support from the DOE BES Physical Behaviour of Materials Program under grant no. DE-SC0014435. The research also uses HPC resources supported in part by the Big-Data Private-Cloud Research Cyberinfrastructure MRI-award funded by the NSF under grant CNS-1338099 by Rice University. We appreciate the discussion with C. Chan at Arizona State University on the full-cell characterization.

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X.W., W.Z. and H.J. designed the experiments. X.W., W.Z., W.X., H.Y., F.W., H.D. and H.J. carried out experiments and analysis. L.H. and M.T. developed the theory. X.W., M.T. and H.J. wrote the paper.

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Correspondence to Huigao Duan or Ming Tang or Hanqing Jiang.

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Supplementary Information

Supplementary Figures 1–16, Supplementary Discussion, Supplementary References.

Videos

Supplementary Video 1

Optical observation of 200 nm-thick Cu/PDMS soft substrate during Li plating

Supplementary Video 2

Optical observation of 400 nm-thick Cu/PDMS soft substrate during Li plating

Supplementary Video 3

Optical observation of 800 nm-thick Cu/PDMS soft substrate during Li plating

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Wang, X., Zeng, W., Hong, L. et al. Stress-driven lithium dendrite growth mechanism and dendrite mitigation by electroplating on soft substrates. Nat Energy 3, 227–235 (2018). https://doi.org/10.1038/s41560-018-0104-5

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