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DOI: 10.1002/aenm. 201601920 class of materials show great potential for the insertion/extraction of multivalent ions (Zn2+, Mg2+, Al3+) owing to the characteristic of large layer spacing and high conductivity. Among all the TMDs, VS2 is a typical family member of TMDs with hexagonal system, which shows similar crystal structure to that of graphite lamellar with an interlayer spacing of 5.76 Å.[25, 30] There is a vanadium layer between two sulfur layers to form a kind of sandwich structure. In VS2 crystal structure, each V atom is arranged around six S atoms and connected with S atoms with covalent bonds. The interlayer spacing of VS2 is so large that enables the convenient insertion/extraction of lithium ions (0.69 Å), sodium ions (1.02 Å), zinc ions (0.74 Å) or their solvation sheath in electrolyte. However, to the best of our knowledge, there is no report about VS2 as the electrode materials for ZIBs.

Herein, the VS2 nanosheets are synthesized via a facile hydrothermal reaction (Supporting Information), which deliver a high capacity of 190.3 mA hg− 1 at a current density of 0.05 A g− 1 and exhibit long-term cyclic stability as the cathode for ZIBs. The electrochemical reaction mechanism of such VS2 electrodes is further investigated systematically through a series of measurements including ex situ X-ray diffraction (XRD), ex situ X-ray photoelectron spectroscopy (XPS), in situ Raman, ex situ transmission electron microscopy (TEM). A reversible insertion/extraction process can be observed from all aspects. Both the ex situ TEM and ex situ XRD results demonstrate that the interlayer space of VS2 can self adapt to the intercalation of Zn2+ with an …