Dual Strategy of Morphology Optimization and Interlayer Expansion in VS₂ Cathode Toward High-Performance Mg-Li Hybrid Ion Batteries

Combining the merits of the dendrite-free formation of a Mg anode and the fast kinetics of Li ions, the Mg-Li hybrid ion batteries (MLIBs) are considered an ideal energy storage system. However, the lack of advanced cathode materials limits their further practical application. Herein, we report a dual strategy of morphology optimization and interlayer expansion for the construction of hierarchical flower-like VS₂ architecture coated by N-doped amorphous carbon layers. This tailored hierarchical flower-like structure coupled with homogeneous N-doped amorphous carbon layers cooperatively provide more active sites and buffer volume changes, thus realizing the enhancement of capacity and structural stability. Moreover, the enlarged interlayer spacing caused by the cointercalation of polyvinylpyrrolidone and ammonium ions can effectively promote the charge transfer rate and facilitate the rapid ion diffusion, as further demonstrated by electrochemical results and theoretical calculations. These features endow the hierarchical flower-like VS₂ cathode with superior specific energy density (644.4 Wh kg^-1, average voltage of 1.2 V vs Mg²⁺/Mg) and excellent rate capability (181.1 mAh g^-1 at 2000 mA g^-1). Systematic ex situ characterization measurements are employed to reveal the ion storage mechanism, which confirms that Li⁺ storage plays a leading role in the capacity contribution of MLIBs. Our strategy is in favor of providing useful insights to design and construct MLIBs with high energy density and excellent rate performance.