Harnessing structural reconstruction to enhance the electrochemical stability and performance of VS2 for aqueous zinc-ion storage

Layered VS 2 with large interlayer spacing and high conductivity is a promising cathode for aqueous zinc-ion batteries (AZIBs) but suffers from structural instability. Here, a VS 2 /MnS hybrid is designed to stabilize the VS 2 framework through electrochemically induced structural reconstruction. Rietveld refinement of neutron diffraction data confirms the coexistence of hexagonal 1T-VS 2 and cubic MnS, with VS 2 as the dominant phase. Operando synchrotron radiation X-ray diffraction reveals gradual MnS dissolution during the first charge and limited Mn incorporation into VS 2 , forming a stable Mn-intercalated phase (VS 2 -Mn). X-ray absorption spectroscopy and density functional theory demonstrate that VS 2 -Mn exhibits improved structural stability, electrical conductivity, and electron-transfer capability. Benefiting from this reconstruction, the VS 2 -Mn electrode delivers a high capacity of 297.9 mAh g -1 at 0.1 A g -1 , outstanding cycling stability (78.6% after 3000 cycles at 10 A g -1 ), and excellent rate capability. This study highlights structural reconstruction as an effective route to design advanced AZIB cathodes.