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Growing single-crystalline seeds on lithiophobic substrates to enable fast-charging lithium-metal batteries

Nature Energy volume 8, pages 340–350 (2023)Cite this article

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Abstract

Controlling the nucleation and growth of lithium metal is essential for realizing fast-charging batteries. Here we report the growth of single-crystalline seeds that results in the deposition of dense lithium, even at high current densities. Contrary to the widely accepted practice of using a lithiophilic surface to achieve dendrite-free deposition, we employ a lithiophobic surface made of a nanocomposite of LiF and Fe to deposit hexagonal crystals, which induce subsequent dense lithium deposition. The nanocomposites have uniform Fe sites for nucleation while LiF enables rapid lithium transport. A cell using a 3 mAh cm−2 LiNi0.8Co0.1Mn0.1O2 (LiNMC811) cathode, onefold excess of lithium and 3 g Ah−1 electrolyte cycles at a 1 C rate for more than 130 cycles with 80% capacity retention, a 550% improvement over the baseline cells. Our findings advance the understanding of lithium nucleation and pave the way for realizing high-energy, fast-charging Li-metal batteries.

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Fig. 1: Li nucleation and growth on different substrates.
Fig. 2: Morphology of initial Li deposition on different substrates.
Fig. 3: Cryo-TEM imaging and crystallographic analysis of the single-crystalline Li crystals.
Fig. 4: Cross-sectional morphology and thickness of the deposited Li layer.
Fig. 5: Electrochemical performance of half cells with different substrates.
Fig. 6: Electrochemical performance of full cell with different substrates.

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All relevant data are included in the paper and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

The work was supported by the Office of Vehicle Technologies of the US Department of Energy through the Advanced Battery Materials Research Program (Battery500 Consortium) under contract no. DE-EE0007764. Work done by C.W. and H.L.X. at UCI was supported by the Materials Science and Engineering Divisions, Office of Basic Energy Sciences of the US Department of Energy, under award no. DE-SC0021204. Part of the work used the UCSD-MTI Battery Fabrication Facility and the UCSD-Arbin Battery Testing Facility. Part of the characterization was performed at the San Diego Nanotechnology Infrastructure of UCSD, a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (grant ECCS-1542148). This research used the TEM facility of the Center for Functional Nanomaterials, which is a US Department of Energy Office of Science User Facility, at Brookhaven National Laboratory under contract no. DE-SC0012704.

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Authors and Affiliations

  1. Program of Chemical Engineering, University of California San Diego, La Jolla, CA, USA

    Zhaohui Wu & Ping Liu

  2. Department of Physics and Astronomy, University of California, Irvine, CA, USA

    Chunyang Wang & Huolin L. Xin

  3. Department of NanoEngineering, University of California San Diego, La Jolla, CA, USA

    Zeyu Hui, Haodong Liu, Shen Wang, John Holoubek & Ping Liu

  4. Program of Material Science, University of California San Diego, La Jolla, CA, USA

    Sicen Yu, Xing Xing, Qiushi Miao & Ping Liu

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  1. Zhaohui Wu
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Contributions

Z.W. and P.L. conceived the idea. P.L. and H.L. directed the project. Z.W. and Z.H. performed the electrochemical experiments and SEM characterizations. S.W. performed the FIB-SEM analysis. S.Y. carried out the XPS characterization. X.X. developed the method for the thermal evaporation of iron fluoride. J.H. provided input on data interpretation and manuscript preparation. Q.M. helped with the contact angle measurement. C.W. and H.L.X. performed the TEM measurement and analysis. Z.W., C.W., Z.H., H.L., J.H., H.L.X. and P.L. co-wrote and revised the manuscript.

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Correspondence to Huolin L. Xin or Ping Liu.

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

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Supplementary Figs. 1–27 and Table 1.

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Wu, Z., Wang, C., Hui, Z. et al. Growing single-crystalline seeds on lithiophobic substrates to enable fast-charging lithium-metal batteries. Nat Energy 8, 340–350 (2023). https://doi.org/10.1038/s41560-023-01202-1

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