All‐solid‐state lithium‐sulfur batteries (ASSLSBs) have garnered widespread attention due to their advantages of high energy density and enhanced safety. However, the typical composite structure composed of solid‐state electrolyte (SE), discrete conducting carbon black, and microsized sulfur (μ‐S) with long‐range Li+/e− conducting path and huge volume changes, suffers from sluggish charge transport and severe electrochemical‐mechanical failure. In this work, a unique hierarchical carbon nanocage (hCNC) is applied as a continuous conducting network where nanosized sulfur are confined. Due to the synergistic effects of multi‐dimensional (particle, interface, and electrode) structural engineering, this new sulfur‐carbon composite cathode (S@hCNC39) can achieve uniform distribution of sulfur and carbon, and efficiently constructs triple‐phase interfaces, showing enhanced charge‐carrier transport and improved electrochemical‐mechanical stability. Remarkable cycling performance of 89% after 300 cycles at 0.2 C at 30 °C is realized in ASSLSBs assembled with S@hCNC39. Notably, ASSLSBs achieve an ultrahigh areal capacity of 9.95 mAh cm−2 with stable cycling at 60 °C with high sulfur contents of 40% and high sulfur loadings of 6 mg cm−2. These results provide critical insights into the design of rational sulfur‐carbon composites and offer a viable approach to enhance the overall performance of ASSLSBs.

中文翻译：

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用于高面容量全固态锂硫电池的带有分层碳纳米笼的工程三相界面


全固态锂硫电池 （ASSLSB） 因其高能量密度和增强安全性等优点而受到广泛关注。然而，由固态电解质 （SE）、离散导电炭黑和具有长程 Li+/e− 导电路径和巨大体积变化的微尺寸硫 （μ-S） 组成的典型复合结构存在电荷传输缓慢和严重的电化学机械故障。在这项工作中，将独特的分层碳纳米笼 （hCNC） 用作纳米级硫被限制的连续导电网络。由于多维（颗粒、界面和电极）结构工程的协同效应，这种新型硫碳复合阴极 （S@hCNC39） 可以实现硫和碳的均匀分布，并有效地构建三相界面，表现出增强的电载流子传输和改进的电化学机械稳定性。在与 S@hCNC39 组装的 ASSLSB 中，在 0.2 °C 和 30 °C 下循环 300 次后，实现了 89% 的显着循环性能。值得注意的是，ASSLSB 实现了 9.95 mAh cm-2 的超高面容量，在 60 °C 下稳定循环，硫含量为 40%，硫含量为 6 mg cm-2。这些结果为合理的硫碳复合材料的设计提供了重要见解，并为提高 ASSLSB 的整体性能提供了一种可行的方法。