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Although vanadium (V)-based sulfides have been investigated as cathodes for aqueous zinc-ion batteries (ZIBs), the performance improvement and the intrinsic zinc-ion (Zn2+) storage mechanism revelation is still challenging. Here, VS4@rGO composite with optimized morphology is designed and exhibits ultrahigh specific capacity (450 mA h g−1 at 0.5 A g−1) and high-rate capability (313.8 mA h g−1 at 10 A g−1) when applied as cathode material for aqueous ZIBs. Furthermore, the VS4@rGO cathode presents long-life cycling stability with capacity retention of ∼82% after 3500 cycles at 10 A g−1. The structural evolution, redox, and degradation mechanisms of VS4 during (dis)charge processes are further probed by in situ XRD/Raman techniques and TEM analysis. Our results indicate that the main energy storage mechanism is derived from the intercalation/deintercalation reactions in the open channels of VS4. Notably, an irreversible phase transition of VS4 into Zn3(OH)2V2O7·2H2O (ZVO) during the charging process and the further transition from ZVO to ZnV3O8 during long-term cycles are also observed, which might be the main reason leading to the capacity degradation of VS4@rGO. Our study further improves the electrochemical performance of VS4 in aqueous ZIBs through morphology design and provides new insights into the energy storage and performance degradation mechanisms of Zn2+ storage in VS4, and thus may endow the large-scale application of V-based sulfides for energy storage systems.

Although vanadium (V)-based sulfides have been investigated as cathodes for aqueous zinc-ion batteries (ZIBs), the performance improvement and the intrinsic zinc-ion (Zn