Sulfide all-solid-state lithium-ion batteries represent one of the most promising energy storage technologies duo to higher safety and ionic conductivities. To further improve its energy density and application, high-voltage LiNi_0.5Mn_1.5O₄ (LNMO) spinel cathode is highly desirable due to its high energy density, low cost, environmental friendliness and Co-free nature. However, sulfide solid electrolyte is not compatible with LNMO cathode, for which issue the reported solutions majorly focus on surface coating. In this work, we propose an efficient approach to sulfurize LNMO itself for an essentially new LNMOS cathode, which not only suppresses interfacial side-reactions but also improve ionic/electronic conductivity of the cathode. This method ultimately improves the interfacial compatibility and consequently the LNMOS/sulfide all-solid-state-battery performances, including 3 times higher initial discharge capacity and much better reversible cycling stability. Detailed analyses on the interface are performed for in-depth understanding and further development of high-energy-density sulfide all-solid-state batteries using 5V-class spinel cathodes.

由于具有更高的安全性和离子电导率，硫化物全固态锂离子电池代表了最有前途的储能技术之一。为进一步提高其能量密度和应用，高压LiNi _0.5 Mn _1.5 O ₄（LNMO）尖晶石阴极由于其高能量密度、低成本、环境友好和无钴性质而备受青睐。然而，硫化物固体电解质与 LNMO 正极不兼容，对此问题报道的解决方案主要集中在表面涂层上。在这项工作中，我们提出了一种有效的方法来硫化 LNMO 本身，用于基本上新的 LNMOS 阴极，这不仅可以抑制界面副反应，还可以提高阴极的离子/电子电导率。这种方法最终提高了界面兼容性，从而提高了 LNMOS/硫化物全固态电池的性能，包括提高 3 倍的初始放电容量和更好的可逆循环稳定性。