Carbonate-based electrolytes demonstrate safe and stable electrochemical performance in lithium-sulfur batteries. However, only a few types of sulfur cathodes with low loadings can be employed and the underlying electrochemical mechanism of lithium-sulfur batteries with carbonate-based electrolytes is not well understood. Here, we employ in operando X-ray absorption near edge spectroscopy to shed light on a solid-phase lithium-sulfur reaction mechanism in carbonate electrolyte systems in which sulfur directly transfers to Li₂S without the formation of linear polysulfides. Based on this, we demonstrate the cyclability of conventional cyclo-S₈ based sulfur cathodes in carbonate-based electrolyte across a wide temperature range, from -20 °C to 55 °C. Remarkably, the developed sulfur cathode architecture has high sulfur content (>65 wt%) with an areal loading of 4.0 mg cm^-2. This research demonstrates promising performance of lithium-sulfur pouch cells in a carbonate-based electrolyte, indicating potential application in the future.

中文翻译：

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碳酸盐电解质中的高能硫阴极，通过固相锂-硫转化消除多硫化物。

碳酸盐基电解质在锂硫电池中显示出安全稳定的电化学性能。然而，仅可使用几种类型的低负载硫阴极，并且对基于碳酸盐的电解质的锂硫电池的基本电化学机理还不甚了解。在这里，我们在边缘光谱中通过操作X射线吸收来阐明碳酸盐电解质体系中的固相锂硫反应机理，在该体系中硫直接转移到Li ₂ S而不形成线性多硫化物。基于此，我们证明了传统的cyclo-S ₈的可循环性在-20°C至55°C的宽温度范围内，碳酸盐基电解液中的铝基硫阴极。值得注意的是，已开发的硫阴极结构具有高的硫含量（> 65 wt％），单位面积载荷为4.0 mg cm ^-2。这项研究表明锂-硫袋式电池在碳酸盐基电解质中的应用前景看好，表明其在未来的潜在应用。