In situ formed LiF-Li3N interface layer enables ultra-stable sulfide electrolyte-based all-solid-state lithium batteries

doi:10.1016/j.jechem.2023.01.007

Abstract

Abstract: Sulfide solid electrolytes are promising for high energy density and safety in all-solid-state batteries due to their high ionic conductivity and good mechanical properties. However, the application of sulfide solid electrolytes in all-solid-state batteries with lithium anode is restricted by the side reactions at lithium/ electrolytes interfaces and the growth of lithium dendrite caused by nonuniform lithium deposition. Herein, a homogeneous LiF-Li₃N composite protective layer is in situ formed via a manipulated reaction of pentafluorobenzamide with Li metal. The LiF-Li₃N layer with both high interfacial energy and interfa-cial adhesion energy can synergistically suppress side reactions and inhibit the growth of lithium den-drite, achieving uniform deposition of lithium. The critical current densities of Li₁₀GeP₂S₁₂ and Li₆PS₅Cl are increased to 3.25 and 1.25 mA cm^-2 with Li@LiF-Li₃N layer, which are almost triple and twice as those of Li-symmetric cells in the absence of protection layer, respectively. Moreover, the Li@LiF-Li₃N/ Li₁₀GeP₂S₁₂/Li@LiF-Li₃N cell can stably cycle for 9000 h at 0.1 mA cm^-2 under 0.1 mA h cm^-2, and Li@LiF-Li₃N/Li₆PS₅Cl/Li@LiF-Li₃N cell achieves stable Li plating/stripping for 8000 h at 0.1 mA cm^-2 under 10 mA h cm^-2. The improved dynamic stability of lithium plating/stripping in Li@LiF-Li₃N/Li₁₀GeP₂S₁₂ or Li₆PS₅Cl interfaces is proved by three-electrode cells. As a result, LiCoO₂/electrolytes/Li@LiF-Li₃N batteries with Li₁₀GeP₂S₁₂ and Li₆PS₅Cl exhibit remarkable cycling stability of 500 cycles with capacity retentions of 93.5% and 89.2% at 1 C, respectively.

Key words: LiF-Li₃N, Sulfide solid electrolytes, Interface modification, High interface energy, All-solid-state batteries

Ming Wu, Mengqi Li, Yuming Jin, Xinshuang Chang, Xiaolei Zhao, Zhi Gu, Gaozhan Liu, Xiayin Yao. In situ formed LiF-Li₃N interface layer enables ultra-stable sulfide electrolyte-based all-solid-state lithium batteries[J]. Journal of Energy Chemistry, 2023, 79(4): 272-278.

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https://www.jenergychem.com/EN/Y2023/V79/I4/272

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In situ formed LiF-Li₃N interface layer enables ultra-stable sulfide electrolyte-based all-solid-state lithium batteries

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