FeSx/MoS2 heterostructure decorated S-coated hydroxylated carbon nanotubes for boosting catalytic activity and mitigating polysulfide shuttling in lithium-sulfur batteries

Heterostructure was widely study to figure out the inferior shuttle effect of intermediate lithium polysulfides and the sluggish kinetics of sulfur redox reaction in lithium-sulfur batteries (LSBs). However, they have low electrical conductivity and no clear discharge/charge catalytic mechanism as LSBs cathode. Combination of heterostructure and functional carbonaceous is a promising choice. Herein, FeSx/MoS2 heterostructure decorated S-coated hydroxylated carbon nanotubes (FSM/SHC) were successfully designed and the catalytic mechanism of FSM was elucidated by in-/ex- situ electrochemical characterizations. Compared to FeSx/MoS2 heterostructure decorated carbon nanotubes (FSM/C)-based sulfur cathode, the chemical adsorption capacity to anchor intermediate polysulfides and the Li-S conversion reaction kinetics of FSM/SHC has been enhanced ascribed to the introduction of polar bonds and functional groups. As a consequence, FSM/SHC-based sulfur modified cathode delivers a marked sulfur reversion (1280 mAh g−1 after 800 cycles at 0.2C and 1048 mAh g−1 after 300 cycles at 4C) and a high capacity retention of 6 mAh cm−2 over 70 cycles at 0.5C (8 mg cm−2). Moreover, the FSM heterostructure demonstrates an accelerated electron transfer caused by the valence change of Fe0/Fe3+ transition, Mo4+/Mo6+ transition and heterointerface, and thus facilitates the redox reaction kinetics of polysulfide. This work reveals the advantages of multi metal-based heterostructures and functional group modification in LSBs.