Sulfide solid electrolytes (SSEs) have captured plentiful interest on account of their high ionic conductivity and appropriate mechanical strength. However, the poor air stability and cost-intensive preparation process of SSEs limit their applications. Herein, a novel ultimate-energy mechanical alloying (UEMA) approach is applied to rapidly synthesize the argyrodite-type electrolytes in a one-pot process. According to the hard-soft-acid-base theory and the first-principles density functional theory (DFT) calculation, In-doping in Li₆PS₅I is attempted to enhance air stability and the experimental results demonstrate the success of this approach. The synthesized Li_6.5In_0.25P_0.75S₅I electrolyte has a high ionic conductivity (1.06 mS cm^–1), and also presents excellent interfacial stability against Li metal, benefiting from the formation of a LiI-rich interphase layer. The assembled Li–S battery with Li_6.5In_0.25P_0.75S₅I as an interlayer delivers a high discharge capacity (954 mAh g^–1) and presents the capacity retention of 96% after 200 cycles. The In-doped Li₆PS₅I is a novel promising electrolyte with high air stability and ionic conductivity for the application of all-solid-state lithium metal batteries.

中文翻译：

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用于全固态锂金属电池的由极限能量机械合金触发的多功能 Li6.5In0.25P0.75S5I 硫化物电解质

硫化物固体电解质（SSE）由于其高离子电导率和适当的机械强度而引起了广泛的关注。然而，SSEs 的空气稳定性差和成本密集的制备过程限制了它们的应用。在此，采用一种新型的极限能量机械合金化 (UEMA) 方法，在一锅法中快速合成银铅矿型电解质。根据硬-软-酸碱理论和第一性原理密度泛函理论（DFT）计算，尝试在Li ₆ PS ₅ I中掺杂In来增强空气稳定性，实验结果证明了该方法的成功。合成的 Li _6.5 In _0.25 P _0.75 S ₅I 电解质具有高离子电导率 (1.06 mS cm ^–1 )，并且由于形成了富含 LiI 的界面层，因此对 Li 金属具有出色的界面稳定性。以 Li _6.5 In _0.25 P _0.75 S ₅ I 作为中间层的组装 Li-S 电池具有高放电容量（954 mAh g ^–1），并在 200 次循环后显示出 96% 的容量保持率。In掺杂的Li ₆ PS ₅ I是一种新型的、具有高空气稳定性和离子电导率的电解质，可用于全固态锂金属电池。