Rational electrolyte engineering for practical pouch cells remains elusive because the correlation between the cathode/solid-electrolyte interphase layer and cell-level reaction behavior is poorly understood. Here, by combining multiscale characterization and computational modeling, we show that—counter to the conventional perception of polysulfide-incompatible additives—the spontaneous reaction of sparingly solvated polysulfides with Lewis acid additives (LAAs) can induce in situ formation of a homogeneous interphase on thick and tortuous S cathode. Multiscale synchrotron X-ray characterization consistently affirms that such interface design could effectively eliminate the notorious problems of polysulfide shuttle and lithium corrosion and, more importantly, provide an interconnected “ion transport highway” to alleviate the uneven ion transport within the tortuous S cathode. Hence, this design dramatically reduces the reaction heterogeneity of lithium-sulfur (Li-S) pouch cells under lean electrolyte conditions. This work resolves controversy around the role of polysulfide-incompatible additives in high-energy Li-S pouch cells and highlights the importance of suppressing reaction heterogeneity for practical batteries.

中文翻译：

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多硫化物不相容添加剂抑制锂硫电池的空间反应异质性


实际软包电池的合理电解质工程仍然难以捉摸，因为人们对阴极/固体电解质中间相层与电池级反应行为之间的相关性知之甚少。在这里，通过结合多尺度表征和计算模型，我们表明，与多硫化物不相容添加剂的传统看法相反，少量溶剂化的多硫化物与路易斯酸添加剂（LAAs）的自发反应可以诱导在厚的材料上原位形成均匀界面相。和曲折的S阴极。多尺度同步加速器X射线表征一致证实，这种界面设计可以有效消除臭名昭著的多硫化物穿梭和锂腐蚀问题，更重要的是，提供互连的“离子传输高速公路”，以缓解曲折的S阴极内的不均匀离子传输。因此，这种设计极大地降低了锂硫（Li-S）软包电池在贫电解质条件下的反应不均匀性。这项工作解决了有关多硫化物不相容添加剂在高能锂硫软包电池中的作用的争议，并强调了抑制实际电池反应不均匀性的重要性。