Lithium solid state batteries are one of the state of the art energy storage systems due to their high safety. However, ionic conductivity in solid electrolytes is a concern, because at present it does not match the ionic conductivity of non-aqueous Li-ion batteries, thus resulting in sluggish electrochemical kinetics. In this report, we enhance the ionic conductivity of Li-argyrodites (Li₆PS₅Cl_0.5Br_0.5) through Si substitution at the P-site using a dry ball milling process. Among the silicon substitutions, Li_6.2Si_0.2P_0.8S₅Cl_0.5Br_0.5 exhibited the high ionic conductivity of 5.12 mS cm⁻¹ compared to pristine Li₆PS₅Cl_0.5Br_0.5 at 4.02 mS cm⁻¹. The Rietveld refinement analysis revealed that after silicon substitution, volume of the unit cell gets increased that allows the lithium at T2-site, that promotes the fast Li-ion transport. Moreover, the optimized solid electrolyte was utilized in a solid state battery system, and demonstrated a high initial capacity of 148.1 mAh g⁻¹ at 0.1 C rate compared to pristine argyrodite (135.1 mAh g⁻¹). Further, we demonstrated the interface phenomena between electrode and solid electrolyte using ex-situ XPS analysis. This confirmed the formation of interface products such as LiCl, Li₂S, lithium polysulfides and P₂S_x, which influence the cycling stability of the ASSLBs.

由于其高安全性，锂固态电池是最先进的储能系统之一。然而，固体电解质中的离子电导率是一个问题，因为目前它与非水锂离子电池的离子电导率不匹配，从而导致电化学动力学缓慢。在本报告中，我们使用干式球磨工艺通过 P 位的 Si 取代提高了锂银锰矿（Li ₆ PS ₅ Cl _0.5 Br _0.5）的离子电导率。在硅取代物中，Li _6.2 Si _0.2 P _0.8 S ₅ Cl _0.5 Br _0.5与原始的 Li ₆ PS ₅ Cl _0.5 Br _0.5在 4.02 mS cm ^-1相比，表现出 5.12 mS cm ^-1的高离子电导率。Rietveld 精修分析表明，在硅取代后，单元电池的体积增加，从而允许锂在 T2 位点，从而促进锂离子的快速传输。此外，优化的固体电解质用于固态电池系统，与原始银铅矿（135.1 mAh g ^-1）相比，在 0.1 C 倍率下显示出 148.1 mAh g ^-1的高初始容量。此外，我们使用非原位证明了电极和固体电解质之间的界面现象XPS 分析。这证实了界面产物如 LiCl、Li ₂ S、多硫化锂和 P ₂ S _{x 的形成}，它们影响了 ASSLB 的循环稳定性。