Insight into MoS2–MoN Heterostructure to Accelerate Polysulfide Conversion toward High‐Energy‐Density Lithium–Sulfur Batteries

Abstract Lithium–sulfur batteries are deemed as optimal energy devices for the next generation of high‐energy‐density energy storage. However, several problems such as low energy density and short cycle life hinder their application in industry. Here, MoS 2 –MoN heterostructure nanosheets grown on carbon nanotube arrays as free‐standing cathodes are reported. In this heterostructure, MoN works as a promoter to provide coupled electrons to accelerate the redox reaction of polysulfides while the MoS 2, with a two‐dimensional layered structure, provides smooth Li + diffusion pathways. Through their respective advantages, both MoN and MoS 2 could mutually boost the process of “adsorption‐diffusion‐conversion” of polysulfides, which have a synergy enhancement effect to restrain the lithium polysulfides from shuttling. The designed cathodes show excellent long‐term cycling performances of 1000 cycles at 1C with a low decay rate of 0.039% per cycle and a high rate capability up to 6C. A high initial areal capacity of 13.3 mAh cm −2 is also achieved under a low electrolyte volume/sulfur loading (E/S) ratio of 6.3 mL g −1 . This strategy of promoting polysulfide conversion by heterostructure MoS 2 –MoN as presented in this work can provide a more structured design strategy for future advanced Li–S energy storage systems.