ZrMn 2 alloy was electro-synthesized directly from cathode pellets compacted with powdered mixture of MnO 2 and ZrO 2 in molten calcium chloride. Sintering temperature, cell voltage and electrolysis time were the dominant factors that affected the characteristics of the final product. The results confirmed the formation of pure ZrMn 2 alloy through the electro-deoxidation of the mixed oxide pellets at 3.1 V for 12 h in 900 °C CaCl 2 melt. The X-ray diffraction (XRD) and cyclic voltammetry analysis suggested that the electro-deoxidation proceeded from the reduction of manganese oxides to Mn, followed by ZrO 2 or CaZrO 3 reduction on the pre-formed Mn to ZrMn 2 alloy. The cyclic voltammetry measurements using powder microelectrode showed that the prepared ZrMn 2 alloy has a good electrochemical hydrogen storage property.