Ultrathin VSe2 Nanosheets with Fast Ion Diffusion and Robust Structural Stability for Rechargeable Zinc‐Ion Battery Cathode

The realizing of high‐performance rechargeable aqueous zinc‐ion batteries (ZIBs) with high energy density and long cycling life is promising but still challenging due to the lack of suitable layered cathode materials. The work reports the excellent zinc‐ion storage performance as‐observed in few‐layered ultrathin VSe2 nanosheets with a two‐step Zn2+ intercalation/de‐intercalation mechanism verified by ex situ X‐ray diffraction (XRD) and X‐ray photoelectron spectroscopy (XPS) characterizations. The VSe2 nanosheets exhibit a discharge plateau at 1.0–0.7 V, a specific capacity of 131.8 mAh g−1 (at 0.1 A g−1), and a high energy density of 107.3 Wh kg−1 (at a power density of 81.2 W kg−1). More importantly, outstanding cycle stability (capacity retention of 80.8% after 500 cycles) without any activation process is achieved. Such a prominent cyclic stability should be attributed to its fast Zn2+ diffusion kinetics (DZn2+ ≈ 10−8 cm−2 s−1) and robust structural/crystalline stability. Density functional theory (DFT) calculation further reveals a strong metallic characteristic and optimal zinc‐ion diffusion pathway with a hopping energy barrier of 0.91 eV. The present finding implies that 2D ultrathin VSe2 is a very promising cathode material in ZIBs with remarkable battery performance superior to other layered transitional metal dichalcogenides. Ultrathin VSe2 nanosheets with a thickness of ≈2.1 nm are developed as a promising cathode material for rechargeable aqueous zinc‐ion batteries. The few‐layered VSe2 nanosheets exhibit fast Zn2+ diffusion kinetics with a solid‐state diffusion coefficient of ≈10−8 cm−2 s−1. Density functional theory (DFT) calculation further reveals a strong metallic characteristic, optimal zinc‐ion diffusion pathway with a hopping energy barrier of 0.91 eV.