Sulfur-deficient MoS2-carbon hollow nanospheres for synergistic trapping and electrocatalytic conversion of polysulfides

[Display omitted] Lithium-sulfur battery is one of the most promising candidates for next-generation energy storage systems, but the serious shuttle effect and sluggish reaction kinetics of polysulfides impair its practical applications. Herein, sulfur-deficient MoS2/carbon hollow nanospheres (MoS2-CHNs) are firstly synthesized by a NaCl-template pyrolysis and employed as sulfur host for lithium-sulfur batteries. TEM analysis reveals that carbon hollow nanospheres existing in the composite are the backbones that help to immobilize the ultrathin MoS2 nanosheets and ensure their large specific surface area. The MoS2 nanosheets consist of 5–10 layers of MoS2 with rich sulfur vacancies. The first principle calculation demonstrates that sulfur vacancy led to an intensively enhanced binding energy (-4.70 eV) towards Li2S6 compared to the pristine MoS2 (-1.57 eV). It suppressed the shuttle effect efficiently. The catalytic experiments reveal that MoS2-CHNs have a superior ability for the nucleation of Li2S and bidirectional electrocatalytic capability for the conversion of polysulfide. The large storage space inside MoS2-CHNs can work as a reservoir for intermediate polysulfides to substantially reduce the concentration overpotential. Due to this advantageous structural design of MoS2-CHNs electrode, its reversible capacity remains 1139 mAh g−1 after 100 cycles at 0.2C, and 600 mAh g−1 after 500 cycles at 5C with a sulfur loading of 5 mg cm−2. Even though the sulfur loading increases to 10 mg cm−2, the Li-S battery delivers a stable capacity of 978 mAh g−1 after 50 cycles at 0.2C. So the MoS2-CHNs demonstrate a promising application for high-energy Li-S batteries.