1T-MoS2 nanosheets with enlarged interlayer spacing vertically bonded on rGO for high-performance lithium-ion capacitors

1T-MoS2 nanosheets, with metallic conductivity and high capacity, hold great potential for lithium-ion capacitors (LICs), but suffer from sluggish reaction kinetics due to dense stacking. Herein, 1T-MoS2 nanosheets with enlarged interlayer spacing, vertically bonded to reduced graphene oxide (rGO) (1T-MoS2/rGO), were designed using a hydrothermal-assisted dispersion and intercalation strategy. The active nitrogen species derived from N, N-dimethylformamide (DMF) not only bridge the rGO and MoS2 through strong Mo–N–C bonds to promote the formation of dispersed MoS2 nanosheets, but also intercalate into the MoS2 structure, further enlarging the interlayer spacing. This unique structure synergistically enhances meso- and microscale mass transfer outside and inside of the few-layered nanosheets, significantly improving electrochemical reaction kinetics and reducing the kinetic mismatch between the anode and cathode. Consequently, the resulting 1T-MoS2/rGO achieves a capacity of 500 mAh g−1 after 500 cycles at 5 A g−1 and a high rate performance of 587 mAh g−1 at a high rate of 10 A g−1. Moreover, the assembled 3D vertical 1T-MoS2/rGO//AC LIC delivers a high energy density of 100.3 Wh kg−1 at a power density of 1.0 kW kg−1, and long cycle stability with capacity retention as high as 91.02% after 5000 cycles at 2 A g−1. This work provides a generalizable strategy for engineering two-dimensional material-based electrodes, offering new insights into high-performance energy storage systems.