Abstract
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 3,000 cycles at 10 A g(-1)), and excellent rate capability. This study highlights structural reconstruction as an effective route to design advanced AZIB cathodes.