Nitrogen‐Doped Graphene‐Supported Mixed Transition‐Metal Oxide Porous Particles to Confine Polysulfides for Lithium–Sulfur Batteries

Abstract The intricate charge–discharge reactions and bad conductivity nature of sulfur determine the extreme importance of cathode engineering for Li–S batteries. Herein, spinel ZnCo 2 O 4 porous particles@N‐doped reduced graphene oxide (ZnCo 2 O 4 @N‐RGO) are prepared via the combined procedures of refluxing and hydrothermal treatment, consisting of interconnected uniform ZnCo 2 O 4 nanocubes with an average size of 5 nm anchored on graphene nanosheets. The as‐obtained composite can act as an inimitable cathode scaffold to suppress the shuttling of polysulfides by chemical confinement of ZnCo 2 O 4 and N‐RGO for the first time, as demonstrated by the adsorption energy of ZnCo 2 O 4 to Li 2 S 4 via the strong chemical bonding between Zn or Co and S. The RGO nanosheets with a relatively high specific surface area provide a good conductive network and structural stability. The introduction of doped N atoms and numerous ZnCo 2 O 4 porous nanoparticles can inhibit the transfer of lithium polysulfides between the cathode and anode. Due to the unique structural and compositional features, the as‐obtained hybrid materials with the high sulfur loading of 71% and even 82% still deliver high specific capacity, good rate capability, and enhanced cycling stability with exceptionally high initial Coulombic efficiency, which displays a high utilization of sulfur.