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Amorphous VS 4 (a-VS 4 ) electrode material was synthesized by mechanical milling of crystalline VS 4 (c-VS 4 ). The columbic efficiency of the a-VS 4 cell was significantly improved (ca. 86 %) at the first cycle as compared with the c-VS 4 cell (ca. 77 %), resulting in the improved capacity retention for prolonged cycling. Pair distribution function (PDF) analysis obtained from X-ray total scattering data, revealed that the radial atomic distribution of a-VS 4 at initial stage was similar to that of the low-crystalline VS 4 appeared after the first cycle of c-VS 4 . This is suggestive that the amorphization via mechanical milling process gave rise to the preparation of "first cycled VS 4 " which would contribute to the improved columbic efficiency at the first cycle and the resulting improved capacity retention for prolonged cycling. The structure of a-VS 4 could be visualized by first-principles molecular dynamic calculation of "first-cycled VS 4 ".

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