Abstract
The operation of high-energy all-solid-state lithium-metal batteries at low stack pressure is challenging owing to the Li dendrite growth at the Li anodes and the high interfacial resistance at the cathodes1,2,3,4. Here we design a Mg16Bi84 interlayer at the Li/Li6PS5Cl interface to suppress the Li dendrite growth, and a F-rich interlayer on LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes to reduce the interfacial resistance. During Li plating–stripping cycles, Mg migrates from the Mg16Bi84 interlayer to the Li anode converting Mg16Bi84 into a multifunctional LiMgSx–Li3Bi–LiMg structure with the layers functioning as a solid electrolyte interphase, a porous Li3Bi sublayer and a solid binder (welding porous Li3Bi onto the Li anode), respectively. The Li3Bi sublayer with its high ionic/electronic conductivity ratio allows Li to deposit only on the Li anode surface and grow into the porous Li3Bi sublayer, which ameliorates pressure (stress) changes. The NMC811 with the F-rich interlayer converts into F-doped NMC811 cathodes owing to the electrochemical migration of the F anion into the NMC811 at a high potential of 4.3 V stabilizing the cathodes. The anode and cathode interlayer designs enable the NMC811/Li6PS5Cl/Li cell to achieve a capacity of 7.2 mAh cm−2 at 2.55 mA cm−2, and the LiNiO2/Li6PS5Cl/Li cell to achieve a capacity of 11.1 mAh cm−2 with a cell-level energy density of 310 Wh kg−1 at a low stack pressure of 2.5 MPa. The Mg16Bi84 anode interlayer and F-rich cathode interlayer provide a general solution for all-solid-state lithium-metal batteries to achieve high energy and fast charging capability at low stack pressure.
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Data availability
The data that support the findings of this study are available within this article and its Supplementary Information. Additional data are available from the corresponding author upon reasonable request.
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Acknowledgements
This work was supported by the US Department of Energy under award number DE-AC05-76RL01830, the Advanced Research Projects Agency for Energy under award number DE-AR0000781 and the National Science Foundation (award number 1805159).
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H.W. and C.W. conceived the idea for the project. H.W., W.Z. and X.H. prepared the materials and carried out electrochemical experiments. Z.W. conducted the simulations. W.Z. prepared the polymer electrolyte and the CCD test for the polymer electrolyte. X.H. prepared the oxide electrolyte and the CCD test for the oxide electrolyte. All authors discussed the results, analysed the data and drafted the manuscript.
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Nature thanks Xiang Chen and Yong Jiang for their contribution to the peer review of this work.
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Supplementary Methods, Discussions, Figs. 1–49, Tables 1–6 and References.
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Wan, H., Wang, Z., Zhang, W. et al. Interface design for all-solid-state lithium batteries. Nature 623, 739–744 (2023). https://doi.org/10.1038/s41586-023-06653-w
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DOI: https://doi.org/10.1038/s41586-023-06653-w
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