Abstract
Argyrodite-based solid-state lithium metal batteries exhibit significant potential as next-generation energy storage devices. However, their practical applications are constrained by the intrinsic poor stability of argyrodite towards Li metal and exposure to air/moisture. Therefore, an indium-involved modification strategy is employed to address these issues. The optimized doping yields a high Li-ion conductivity of 7.5 mS cm−1 for Li5.54In0.02PS4.47O0.03Cl1.5 electrolyte, accompanied by enhanced endurance against air/moisture and bare Li metal. It retains 92.0% of its original conductivity after exposure to air at a low dew point of −60 °C in dry room. Additionally, a composite layer comprising Li–In alloy and LiF phases is generated on the surface of lithium metal anode via the reaction between InF3 and molten Li. This layer effectively mitigates Li dendrite growth by creating a physical barrier from the robust LiF phase, while the Li–In alloy induces uniform Li-ion deposition and accelerates Li transport dynamics across the interphase between the solid electrolyte/Li metal. Moreover, the In-doped electrolyte facilitates the in-situ generation of Li–In alloy within its voids, reducing local current density and further inhibiting lithium dendrite growth. Consequently, the combination of the Li5.54In0.02PS4.47O0.03Cl1.5 electrolyte and the InF3@Li anode provides exceptional electrochemical performances in both symmetric cells and solid-state lithium metal batteries across different operating temperatures. Specifically, the LiNbO3@LiNi0.7Co0.2Mn0.1O2/Li5.54In0.02PS4.47O0.03Cl1.5/InF3@Li cell delivers a high discharge capacity of 167.8 mAh g−1 at 0.5 C under 25 °C and retains 80.0% of its initial value after 400 cycles. This work offers a viable strategy for designing functional interfaces with enhanced stability for sulfide-based solid-state lithium batteries.
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Acknowledgements
This work was supported by the National Key Research and Development Program (2021YFB2500200) and the National Natural Science Foundation of China (52177214, 52222703). We gratefully acknowledge the Analytical and Testing Center of HUST for us to use the facilities. The Basic Science Research Fund in Xidian University (ZYTS24132), the Postdoctoral Science Research Program of Shaanxi (30102230001).
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Enhancing Solid-State Lithium Metal Battery Performance via Indium-based Modification of Electrolyte and Lithium Metal Surfaces: Mechanistic Insights and Optimization
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Wu, Z., Liu, C., Jiang, Z. et al. Enhancing solid-state lithium metal battery performance via indium-based modification of electrolytes and lithium metal surfaces: mechanistic insights and optimization. Sci. China Chem. (2024). https://doi.org/10.1007/s11426-024-2275-2
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DOI: https://doi.org/10.1007/s11426-024-2275-2