Controllable Design of MoS₂ Nanosheets Anchored on Nitrogen-Doped Graphene: Toward Fast Sodium Storage by Tunable Pseudocapacitance

Transition-metal disulfide with its layered structure is regarded as a kind of promising host material for sodium insertion, and intensely investigated for sodium-ion batteries. In this work, a simple solvothermal method to synthesize a series of MoS₂ nanosheets@nitrogen-doped graphene composites is developed. This newly designed recipe of raw materials and solvents leads the success of tuning size, number of layers, and interplanar spacing of the as-prepared MoS₂ nanosheets. Under cut-off voltage and based on an intercalation mechanism, the ultrasmall MoS₂ nanosheets@nitrogen-doped graphene composite exhibits more preferable cycling and rate performance compared to few-/dozens-layered MoS₂ nanosheets@nitrogen-doped graphene, as well as many other reported insertion-type anode materials. Last, detailed kinetics analysis and density functional theory calculation are also employed to explain the Na⁺- storage behavior, thus proving the significance in surface-controlled pseudocapacitance contribution at the high rate. Furthermore, this work offers some meaningful preparation and investigation experiences for designing electrode materials for commercial sodium-ion batteries with favorable performance.