Vertically Oriented MoS2 with Spatially Controlled Geometry on Nitrogenous Graphene Sheets for High‐Performance Sodium‐Ion Batteries

Inspired by the great success of graphite in lithium‐ion batteries, anode materials that undergo an intercalation mechanism are considered to provide stable and reversible electrochemical sodium‐ion storage for sodium‐ion battery (SIB) applications. Though MoS2 is a promising 2D material for SIBs, it suffers from deformation of its layered structure during repeated intercalation of Na+, resulting in undesirable electrochemical behaviors. In this study, vertically oriented MoS2 on nitrogenous reduced graphene oxide sheets (VO‐MoS2/N‐RGO) is presented with designed spatial geometries, including sheet density and height, which can deliver a remarkably high reversible capacity of 255 mA h g−1 at a current density of 0.2 A g−1 and 245 mA h g−1 at a current density of 1 A g−1, with a total fluctuation of 5.35% over 1300 cycles. These results are superior to those obtained with well‐developed hard carbon structures. Furthermore, a SIB full cell composed of the optimized VO‐MoS2/N‐RGO anode and a Na2V3(PO4)3 cathode reaches a specific capacity of 262 mA h g−1 (based on the anode mass) during 50 cycles, with an operated voltage range of 2.4 V, demonstrating the potentially rewarding SIB performance, which is useful for further battery development. Vertically oriented MoS2 with controlled spatial geometry on N‐RGO favors rapid Na+ diffusion for sodium‐ion batteries, and the dense spatial distance due to the high sheet density and low height enables a high reversible capacity and long stability.