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

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.