Three-dimensionally ordered macro-microporous metal organic frameworks with strong sulfur immobilization and catalyzation for high-performance lithium-sulfur batteries

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.