Lithium-sulfur (Li-S) batteries have been recognized as one of the most promising technologies for next-generation energy storage. However, their practical implementation is greatly impeded by the sluggish sulfur kinetics and unsatisfactory cyclability. Herein, a novel three-dimensionally ordered macro-microporous metal organic frameworks (3DOM ZIF-8) is developed via self-templated coordination-replication method, which serves as an advanced sulfur reservoir for enhanced Li-S battery performance. The unique hierarchical architecture not only facilitates the electrolyte infiltration and ion/mass transportation, but also increases the surface area for abundant exposure of active interfaces. Moreover, the nanometric ZIF-8 subunits impose strong sulfur immobilization and catalyzation through their chemical interactions with polysulfides, thus rendering significantly inhibited shuttle effect and fast reaction kinetics. Benefiting from these synergistic features, sulfur electrodes based on 3DOM ZIF-8 exhibit excellent electrochemical performance, i.e., prolonged cycling stability with a low capacity decay of 0.028% per cycle over 500 cycles, as well as high areal capacity and decent cyclability under raised sulfur loading and limited electrolyte, demonstrating a great promise in developing practically viable Li-S batteries.

锂硫（Li-S）电池已被公认为是下一代能量存储最有希望的技术之一。但是，其缓慢的硫动力学和不令人满意的可循环性极大地阻碍了它们的实际实施。在本文中，通过自模板配位-复制方法开发了一种新颖的三维有序的宏观微孔金属有机骨架（3DOM ZIF-8），该骨架可用作增强硫锂电池性能的先进硫储存器。独特的分层结构不仅有助于电解质的渗透和离子/质量的运输，而且还增加了表面积，使活性界面充分暴露。此外，纳米级ZIF-8亚基通过与多硫化物的化学相互作用而强加了固硫和催化作用，因此，显着抑制了穿梭效应和快速的反应动力学。得益于这些协同功能，基于3DOM ZIF-8的硫电极表现出出色的电化学性能，即延长的循环稳定性，在500个循环中每个循环的容量衰减低至0.028％，在高硫条件下具有较高的面容量和良好的循环性负载和有限的电解质，这表明在开发实用的Li-S电池方面具有广阔的前景。