The development of lithium–sulfur batteries is limited by the poor conductivity of sulfur cathodes and soluble long‐chain lithium polysulfides (LPSs), which cause the low utilization of sulfur and the aversive shuttle effect, and further, give rise to self‐discharge, rapid reversible capacity fading, and low Coulombic efficiency. In this work, a novel configuration is built for high‐performance lithium–organosulfur batteries, in which the organosulfur hybrid material and lithium metal are used as the cathode and the anode, respectively, and are separated by a functional separator decorated with nitrogen and sulfur co‐doped reduced graphite oxide. The organosulfur in the cathode prevents the shuttle effect by inhibiting the formation of long‐chain LPSs. In addition, the functional separator effectively adsorbs LPSs escaping from the cathode by electrostatic interactions and further restrains the shuttle effect. These effects are confirmed by density‐functional theory calculations. As a result, this novel configuration provides a high initial discharge capacity of 1364 mAh g⁻¹ at 0.2 C and a high discharge capacity of 750 mAh g⁻¹ at 1 C after 700 cycles with a very low capacity decay rate of 0.037% per cycle.

中文翻译：

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通过抑制长链多硫化锂和功能分离器的形成来抑制穿梭，从而极大地改善了锂有机硫电池的性能

锂硫电池的发展受到硫阴极和可溶长链多硫化锂（LPSs）导电性差的限制，这会导致硫的利用率低和有害的穿梭效应，并进一步导致自放电，快速可逆容量衰减，库仑效率低。在这项工作中，为高性能锂-有机硫电池构建了一种新颖的配置，其中有机硫杂化材料和锂金属分别用作阴极和阳极，并通过装饰有氮气和硫磺的功能性分隔器进行分隔共掺杂还原氧化石墨。阴极中的有机硫通过抑制长链LPS的形成来防止穿梭效应。此外，该功能性隔板有效地吸附了通过静电相互作用从阴极逸出的LPS，并进一步抑制了穿梭效应。这些影响已通过密度泛函理论计算得到证实。结果，这种新颖的配置提供了1364 mAh g的高初始放电容量^-1在0.2℃和750毫安g的高放电容量^-1，在700次循环的每个周期的0.037％的非常低的容量衰减率后1℃。