Heterostructured Mn3O4‐MnS Multi‐Shelled Hollow Spheres for Enhanced Polysulfide Regulation in Lithium–Sulfur Batteries

Abstract

Constructing heterojunctions and hollow multi‐shelled structures can render materials with fascinating physicochemical properties, and have been regarded as two promising strategies to overcome the severe shuttling and sluggish kinetics of polysulfide in lithium–sulfur (Li–S) batteries. However, a single strategy can only take limited effect. Modulating catalytic hosts with synergistic effects are urgently desired. Herein, Mn3O4‐MnS heterogeneous multi‐shelled hollow spheres are meticulously designed by controlled sulfuration of Mn2O3 hollow spheres, and then applied as advanced encapsulation hosts for Li–S batteries. Benefiting from the separated spatial confinement by hollow multi‐shelled structure, ample exposed active sites and built‐in electric field by heterogeneous interface, and synergistic effects between Mn3O4 (strong adsorption) and MnS (fast conversion) components, the assembled battery achieves prominent rate capability and decent cyclability (0.016% decay per cycle at 2 C, 1000 cycles). More crucially, satisfactory areal capacity reaches up to 7.1 mAh cm−2 even with high sulfur loading (8.0 mg cm−2) and lean electrolyte (E/S = 4.0 μL mg−1) conditions. This work will provide inspiration for the rational design of hollow multi‐shelled heterostructure for various electrocatalysis applications.