Sulfide-based Li-argyrodites (Li_5.5PS_4.5Cl_1.5) are considered as promising solid-state electrolytes for all-solid-state Li–S batteries (ASSLSBs) due to their high ionic conductivity and suitable mechanical properties. However, their hygroscopic nature and intense decomposition behavior when combined with conductive additives at the sulfur cathode introduce many variables that can affect cell performance. This study demonstrates that an optimized amount of ambient air contamination during cycling can enhance cell performance. Multiple spectroscopic analyses reveal that the hydrolysis of Li_5.5PS_4.5Cl_1.5 can incorporate oxygen into the argyrodite structure, thereby increasing the oxidative stability and generating additional redox active sulfur species. Methods, such as monitoring cell impedance growth, open-circuit voltage changes, and ³¹P NMR spectroscopic analysis, are proposed to determine the air-tightness of cell configurations. The research findings suggest that verifying the air-tightness of cell configurations is critical for ASSLSBs research to prevent misleading results.

中文翻译：

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环境空气污染对 Argyrodite 基全固态锂硫电池性能的影响


硫化物基银辉体 （Li_5.5PS_4.5Cl_1.5） 因其高离子电导率和合适的机械性能而被认为是全固态 Li-S 电池 （ASSLSB） 的有前途的固态电解质。然而，当与硫阴极的导电添加剂结合使用时，它们的吸湿性和强烈的分解行为会引入许多可能影响电池性能的变量。本研究表明，在循环过程中优化的环境空气污染量可以提高电池性能。多重光谱分析表明，Li_5.5PS_4.5Cl_1.5 的水解可以将氧掺入 argyrodite 结构中，从而增加氧化稳定性并产生额外的氧化还原活性硫物种。提出了监测电池阻抗增长、开路电压变化和 ³¹P NMR 波谱分析等方法，以确定电池配置的气密性。研究结果表明，验证细胞构型的气密性对于 ASSLSBs 研究以防止误导性结果至关重要。