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Long cycle life and dendrite-free lithium morphology in anode-free lithium pouch cells enabled by a dual-salt liquid electrolyte

Nature Energy volume 4, pages 683–689 (2019)Cite this article

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Abstract

Cells with lithium-metal anodes are viewed as the most viable future technology, with higher energy density than existing lithium-ion batteries. Many researchers believe that for lithium-metal cells, the typical liquid electrolyte used in lithium-ion batteries must be replaced with a solid-state electrolyte to maintain the flat, dendrite-free lithium morphologies necessary for long-term stable cycling. Here, we show that anode-free lithium-metal pouch cells with a dual-salt LiDFOB/LiBF4 liquid electrolyte have 80% capacity remaining after 90 charge–discharge cycles, which is the longest life demonstrated to date for cells with zero excess lithium. The liquid electrolyte enables smooth dendrite-free lithium morphology comprised of densely packed columns even after 50 charge–discharge cycles. NMR measurements reveal that the electrolyte salts responsible for the excellent lithium morphology are slowly consumed during cycling.

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Fig. 1: Electrochemical behaviour of single- and dual-salt electrolytes.
Fig. 2: SEM characterization of lithium morphology.
Fig. 3: XPS spectra for lithium negative electrodes.
Fig. 4: Electrolyte composition during cycling.

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Data availability

The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request.

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Acknowledgements

This research was financially supported by Tesla Canada and NSERC under the Industrial Research Chairs Program. A.J.L. thanks the Nova Scotia Graduate Scholarship programme and the Walter C. Sumner Memorial fellowship for support. M.G. thanks the NSERC PDF Program. The authors acknowledge Dr J. Li (formerly of BASF) and Dr D. J. Xiong (formerly of Capchem) for providing chemicals used in the electrolytes, as well as S. Trussler for expert fabrication of the parts used in this work.

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Author notes

  1. These authors contributed equally: R. Weber, M. Genovese.

Authors and Affiliations

  1. Materials Engineering, Department of Mechanical Engineering, Dalhousie University, Halifax, Nova Scotia, Canada

    Rochelle Weber

  2. Tesla Canada R&D, Dartmouth, Nova Scotia, Canada

    Rochelle Weber

  3. Physics and Atmosphere Science, Dalhousie University, Halifax, Nova Scotia, Canada

    Matthew Genovese, A. J. Louli, Samuel Hames, Ian G. Hill & J. R. Dahn

  4. Nanotechnology Engineering, University of Waterloo, Waterloo, Ontario, Canada

    Cameron Martin

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Contributions

R.W., M.G., A.J.L. and J.R.D. conceived the idea. R.W., M.G. and A.J.L. designed the experiments with the guidance of J.R.D.; R.W., M.G. and A.J.L. performed the electrochemical measurements with assistance from S.H. and C.M.; R.W. performed the NMR analysis; R.W. performed the XPS analysis with guidance from I.G.H; M.G. and A.J.L. performed the SEM analysis; A.J.L. performed the mechanical pressure measurements. R.W., M.G., A.J.L. and J.R.D. prepared this manuscript with input from all other co-authors.

Corresponding author

Correspondence to J. R. Dahn.

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Rochelle Weber is employed by Tesla Canada R&D.

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Supplementary Figs. 1–14, Supplementary Table 1 and Supplementary refs.

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Weber, R., Genovese, M., Louli, A.J. et al. Long cycle life and dendrite-free lithium morphology in anode-free lithium pouch cells enabled by a dual-salt liquid electrolyte. Nat Energy 4, 683–689 (2019). https://doi.org/10.1038/s41560-019-0428-9

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