Mo‐O‐C Between MoS2 and Graphene Toward Accelerated Polysulfide Catalytic Conversion for Advanced Lithium‐Sulfur Batteries

MoS2 /C composites constructed with van der Waals forces have been extensively applied in lithium-sulfur (Li-S) batteries. However, the catalytic conversion effect on polysulfides is limited because the weak electronic interactions between the composite interfaces cannot fundamentally improve the intrinsic electronic conductivity of MoS2 . Herein, density functional theory calculations reveal that the MoS2 and nitrogen-doped carbon composite with an Mo-O-C bond can promote the catalytic conversion of polysulfides with a Gibbs free energy of only 0.19 eV and a low dissociation energy barrier of 0.48 eV, owing to the strong covalent coupling effect on the heterogeneous interface. Guided by theoretical calculations, a robust MoS2 strongly coupled with a 3D carbon matrix composed of nitrogen-doped reduced graphene oxide and carbonized melamine foam is designed and constructed as a multifunctional coating layer for lithium-sulfur batteries. As a result, excellent electrochemical performance is achieved for Li-S batteries, with a capacity of 615 mAh g-1 at 5 C, an areal capacity of 6.11 mAh cm-2 , and a low self-discharge of only 8.6% by resting for five days at 0.5 C. This study opens a new avenue for designing 2D material composites toward promoted catalytic conversion of polysulfides.