Lithium–sulfur (Li–S) batteries are deemed as one of the most promising next-generation energy storage systems. However, their practical application is hindered by existing drawbacks such as poor cycling life and low Coulombic efficiency due to the shuttle effect of lithium polysulfides (LiPSs). We herein present an in situ constructed VO₂–VN binary host which combines the merits of ultrafast anchoring (VO₂) with electronic conducting (VN) to accomplish smooth immobilization–diffusion–conversion of LiPSs. Such synchronous advantages have effectively alleviated the polysulfide shuttling, promoted the redox kinetics, and hence improved the electrochemical performance of Li–S batteries. As a result, the sulfur cathode based on the VO₂–VN/graphene host exhibited an impressive rate capability with ∼1105 and 935 mA h g⁻¹ at 1C and 2C, respectively, and maintained long-term cyclability with a low capacity decay of 0.06% per cycle within 800 cycles at 2C. More remarkably, favorable cyclic stability can be attained with a high sulfur loading (13.2 mg cm⁻²). Even at an elevated temperature (50 °C), the cathodes still delivered superior rate capacity. Our work emphasizes the importance of immobilization–diffusion–conversion of LiPSs toward the rational design of high-load and long-life Li–S batteries.

中文翻译：

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针对高硫负荷的Li-S电池 ，在VO ₂ -VN二元主体上同步固定和转化多硫化物†

锂硫（Li–S）电池被认为是最有前途的下一代储能系统之一。然而，由于多硫化锂（LiPSs）的穿梭效应，诸如循环寿命差和库仑效率低之类的现有缺点阻碍了它们的实际应用。我们在此介绍一种原位构建的VO ₂ -VN二元宿主，它结合了超快锚定（VO ₂）和电子导电（VN）的优点，以实现LiPSs的平稳固定-扩散-转化。这样的同步优势有效地减轻了多硫化物的穿梭，提高了氧化还原动力学，并因此改善了锂锂电池的电化学性能。结果，基于VO ₂的硫阴极-VN /石墨烯基质在1C和2C时分别具有约1105和935 mA hg ^-1的速率能力，并保持了长期可循环性，在2C的800个循环中，每个循环的容量衰减低至0.06％。更显着地，在高硫负载（13.2mg cm ^-2）下可以获得良好的循环稳定性。即使在升高的温度（50°C）下，阴极仍可提供出色的倍率容量。我们的工作强调了将LiPS固定化，扩散和转化的重要性，以合理设计高负载和长寿命的Li-S电池。