Effect of zinc-based active sites on porous carbon and electrochemical properties in lithium-sulfur batteries

• Zinc-based active sites allow the morphology/pore size distribution of porous carbon to be customized. • Reasonable morphology of p-HPC-X materials achieves good physical limitation of polysulfides. • Reasonable configuration of polar sites improves the catalytic and adsorption capacity of polysulfide. Hierarchically porous carbon (HPC) is considered as one of the promising cathodes of lithium-sulfur batteries (LSBs) owing to its appealing merits. However, it is still preventing the shuttle effect poorly due to the weak interaction between nonpolar carbon and polar polysulfide (LiPS). Herein, we report a facile method to prepare polar hierarchically porous carbon by in-situ loading the different amounts of zinc-based active sites (p-HPC-X) onto the HPC materials. The close combination of a carbon interconnected skeleton and ZnS nanoparticles derived zinc-based active sites forms the strong interaction that suppresses the soluble polysulfide shuttle effect and catalyzes the kinetics redox reactions of lithium polysulfide/sulfide. Moreover, the effect of polar sites introduced in situ on the morphology/porosity of carbon materials is also focused on. Crystallization of zinc-based active sites during the freeze-drying process and self-assembly during carbonization allow the pore size distribution of porous carbon to be customized, which offers fast lithium-ion and electron transport channels. Due to the synergistic effect of the hierarchical pore structure and suitable polarity sites, the p-HPC-X exhibits high capacity and good cycling performance. Especially p-HPC-1, it yields a high reversible capacity of 683.7 mAh g −1 and a low fading rate of 0.041% per cycle over 900 cycles at a current density of 1 C. This work offers novel insights into realizing the effect of in-situ loaded active sites on pore structure and electrochemical performance in LSBs.