Vanadium Molybdenum Disulfide Nanosheets Anchoring on Carbon Cloth as High‐Energy Density Cathode for Magnesium–Lithium Hybrid Batteries

Abstract Magnesium–lithium‐ion hybrid batteries (MLIBs) have gained significant attention since the combination of a dendrite‐free and low‐cost magnesium anode with lithium‐ion storage cathodes. However, the lack of high‐performance cathodes has severely hindered their development, limited by the lower operating voltages of electrolytes. Herein, vanadium molybdenum disulfide nanosheets anchoring on flexible carbon cloth (VMS@CC) are constructed as high‐performance cathodes for MLIBs, which inherit the electrochemical properties of high‐voltage VS2 and high‐capacity MoS2, simultaneously. By adjusting the V and Mo atomic ratio, the VMS@CC cathode for MLIBs delivers a record maximum energy density of 275.5 Wh kg−1 with a high working voltage of 1.07 V at 50 mA g−1. Meanwhile, under the synergistic effects of the conductive carbon cloth matrix, abundant hetero‐interfaces and defects, as well as expanded interlayer spacing, the VMS@CC cathode displays superior rate capability and long‐term cycling stability. Ex situ analyses demonstrate the VMS nanosheets cathode exhibits a Li+/Mg2+ co‐insertion/extraction mechanism in MLIBs, following the in situ insertion of organic species in the hybrid electrolyte during the aging process. The fabricated flexible cathode herein provides a new insight into the construction of high‐energy density cathodes for MLIBs.