Introduced Hierarchically Ordered Porous Architecture on a Separator as an Efficient Polysulfide Trap toward High-Mass-Loading Li-S Batteries.

Abstract

The severe shuttle effect and the depletion of active sulfur result in performance deterioration, presenting two formidable issues that must be overcome to achieve high-mass-loading lithium-sulfur batteries. Herein, we reported a composite separator by introducing carbon photonic crystals with a hierarchically ordered porous structure on a commercial separator. The ordered structure and interconnected hierarchical macro-meso-micropore network of the composite separator facilitate efficient trapping of polysulfides and rapid transport of lithium ions. The high ion diffusivity promotes the conversion of polysulfides enhancing sulfur utilization and mitigating the occurrence of "dead sulfur" on the surface of the separator. Impressively, under a high sulfur loading of 3 mg cm-2, the lithium-sulfur battery with the composite separator displayed a high reversible capacity of 1582 mA h g-1 at 0.1 C and an excellent long-term cycling performance with a decay rate of as low as 0.033% per cycle over 1500 cycles at 1 C. Surprisingly, the battery represented a high reversible capacity of 935 mA h g-1 at 0.2 C even at a sulfur loading of 6.71 mg cm-2. The design of the composite separator underscores the pivotal role of carbon architecture in improving battery performance and brings a bright prospect to enable the commercialization of high-mass-loading lithium-sulfur batteries.