Sulfide-based all-solid-state lithium metal batteries (ASSLMBs) are viable options for electric vehicles due to their promising high energy densities. However, the poor stability of sulfide towards air/moisture and lithium metal anode inhibits their development. Herein, we tailored the Bi-O dual-doping amount to enhance the chemical/electrochemical stability of Li5.5PS4.5Cl1.5 electrolyte for ASSLMBs. The optimized Li5.54P0.98Bi0.02S4.47O0.03Cl1.5 demonstrates improved air/moisture stability in various environments with different dew points due to the formation of oxysulfide units PS3O and LiBiS2 phases. Incorporating Bi-O into the structure leads to enhanced Li dendrites suppression and accelerated the transport rate of Li-ion at the interface. This improvement arises from the uniform current distribution and the formation of the of the composite SEI, which includes phases such as LiCl, Li2O, and Li-Bi alloy. The Li5.54P0.98Bi0.02S4.47O0.03Cl1.5 exhibits enhanced compatibility with Li metal and yields superior cycling performance when applied the Li metal anode in both lithium symmetric cells and ASSLMBs combined with LiCoO2 and high-nickel LiNi0.9Mn0.05Co0.05O2 at various operating temperatures (-20 ℃, 25 ℃, and 60 ℃). When cycled at 0.2 C at 25 ℃, LiCoO2-based electrode delivers a notable initial discharge capacity of 156.6 mAh g−1. Even after 150 cycles, the battery maintains a significant portion of this capacity, retaining 79.7 %. This dual-doping strategy provides a guideline for designing solid electrolytes for high-performance ASSLMBs.

中文翻译：

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增强全固态锂金属电池电化学性能的 Bi-O 双掺杂 Li5.5PS4.5Cl1.5 电解质的见解


硫化物基全固态锂金属电池（ASSLMB）由于其高能量密度而成为电动汽车的可行选择。然而，硫化物对空气/湿气和锂金属负极的稳定性较差，阻碍了它们的发展。在此，我们定制了 Bi-O 双掺杂量，以增强 ASSLMB 的 Li5.5PS4.5Cl1.5 电解质的化学/电化学稳定性。优化后的 Li5.54P0.98Bi0.02S4.47O0.03Cl1.5 由于形成硫氧化物单元 PS3O 和 LiBiS2 相，在不同露点的各种环境中表现出更高的空气/湿度稳定性。将 Bi-O 纳入结构中可以增强锂枝晶的抑制并加速界面处锂离子的传输速率。这种改进源于均匀的电流分布和复合 SEI 的形成，其中包括 LiCl、Li2O 和 Li-Bi 合金等相。 Li5.54P0.98Bi0.02S4.47O0.03Cl1.5 表现出增强的与锂金属的兼容性，当将锂金属负极与 LiCoO2 和高镍 LiNi0.9Mn0.05Co0 结合应用于锂对称电池和 ASSLMB 时，可产生优异的循环性能.05O2 在各种工作温度（-20℃、25℃和60℃）下。当在 25 ℃、0.2 C 下循环时，LiCoO2 基电极具有 156.6 mAh g−1 的显着初始放电容量。即使在 150 次循环后，电池仍保持大部分容量，保留 79.7%。这种双掺杂策略为高性能 ASSLMB 的固体电解质设计提供了指导。