Lithium–sulfur chemistry, despite being a promising candidate for energy storage due to its higher theoretical capacity, is faced with several critical challenges. Practical operation of Li–S batteries demonstrates lower capacity, poor rate capability, and insufficient cycle life, which can be related to the underlying physicochemical interactions at the electrodes. Typical carbon-based porous cathodes undergo coupled electrochemical, chemical, and microstructural evolution during operation. In this work, the mesoscale interaction resulting from the underlying chemical/electrochemical complexations and microstructural evolution is studied in order to elucidate the transient impedance behavior in Li–S battery mesoporous carbon cathodes. The discharge product (e.g., Li₂S) precipitation is shown to affect impedance evolution with correlational dependence on the porous cathode microstructure attributes. This mesoscale impedance analytics can be a valuable virtual probing tool for Li–S battery electrochemical performance.

中文翻译：

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探测锂硫电池电极的阻抗和微观结构演变

尽管锂硫化学由于其较高的理论容量而成为有潜力的储能材料，但它仍面临着数项严峻的挑战。Li-S电池的实际操作显示出较低的容量，较差的倍率能力以及不足的循环寿命，这可能与电极上潜在的物理化学相互作用有关。典型的碳基多孔阴极在操作过程中会发生电化学，化学和微观结构的耦合演化。在这项工作中，研究了由潜在的化学/电化学络合物和微观结构演变引起的介观相互作用，以便阐明Li-S电池介孔碳阴极中的瞬态阻抗行为。放电产物（例如，Li ₂S）沉淀显示出对阻抗演化的影响，并且对多孔阴极微结构的属性具有相关性。这种中尺度阻抗分析可以成为锂-锂电池电化学性能的宝贵虚拟探测工具。