ZnSe/N-Doped Carbon Nanoreactor with Multiple Adsorption Sites for Stable Lithium–Sulfur Batteries

To commercially realize the enormous potential of lithium–sulfur batteries (LSBs) several challenges remain to be overcome. At the cathode, the lithium polysulfide (LiPS) shuttle effect must be inhibited and the redox reaction kinetics need to be substantially promoted. In this direction, this work proposes a cathode material based on a transition-metal selenide (TMSe) as both adsorber and catalyst and a hollow nanoreactor architecture: ZnSe/N-doped hollow carbon (ZnSe/NHC). It is here demonstrated both experimentally and by means of density functional theory that this composite provides three key benefits to the LSBs cathode: (i) A highly effective trapping of LiPS due to the combination of sulfiphilic sites of ZnSe, lithiophilic sites of NHC, and the confinement effect of the cage-based structure; (ii) a redox kinetic improvement in part associated with the multiple adsorption sites that facilitate the Li+ diffusion; and (iii) an easier accommodation of the volume expansion preventing the cathode damage due to the hollow design. As a result, LSB cathodes based on S@ZnSe/NHC are characterized by high initial capacities, superior rate capability, and an excellent stability. Overall, this work not only demonstrates the large potential of TMSe as cathode materials in LSBs but also probes the nanoreactor design to be a highly suitable architecture to enhance cycle stability.