Magnesium hydrides are considered as the potential hydrogen storage materials.However, high work temperature, slow reaction kinetics and hard activation process limit the practical application of Mg-based hydrides system. Recently, the reaction ball milling (RBM) technique has been successfully introduced to prepare hydrogen storage materials [1,2]. It combines the courses of sample preparation, activation and hydrogenation into one step. Pure Mg milled under the hydrogen atmosphere was studied by Gennari [3]. In his study, the metastable -MgH 2 was generated by the RBM process. A reduction of particle and crystallite size and an increase of specific surface were observed. Unfortunately, only half of Mg was transformed into hydrides and the crystallite size was still very big. Moreover, it took many hours to finish the hydriding process. Some researchers tried to improve the reaction efficiency between In this work, Ti 37.5 V 25 Cr 37.5 (bcc structure) alloy was used as catalyst due to good hydriding properties and high hydrogen storage capacity [7]. Ti 37.5 V 25 Cr 37.5 alloy was prepared using arc melting with electromagnetic stirring (EMS) in an argon atmosphere. The starting materials were of a purity of 99.9% and the alloy was turned and melted for four times to improve the homogeneity. Then the as-cast alloy was crushed into powder, which passed through a 0.5mm screen. Finally, the powder of the as-cast alloy (30wt. %) was mixed with Mg (purity>99%, 100 mesh) and then mechanically milled in a SPEX8000 machine. A cylindrical stainless steel vial was used with the stainless steel balls and the ball to powder ratio is 20:1. The vial was sealed by an O-ring and connected to a gas reservoir under an initial pressure of 1 MPa, as shown in Fig. 1 [8,9]. The total volume of the system was 260 cm 3 and about 2.7 g material could be produced. The milling was carried out for the duration of 5 h.During the milling, small changes in the hydrogen pressure representing absorption of hydrogen by the sample were monitored continuously. The method proposed by Bab et al [9] was adopted to measure the absorption kinetics. Subsequently, the mixture of magnesium powder and the as-cast alloy powder was also milled under the same condition as mentioned above. At selected time, small amount of powder was successively taken out of the vial to characterize the phase structure. For the sake of comparison, the as-cast Ti 37.5 V 25 Cr 37.5 alloy powder was separately milled under the same condition as mentioned above. The powder was characterized at different duration during the milling. Phase structure of the powder was examined using an X-ray diffraction (XRD) machine equipped with a monochromator with Cu Kα The time dependence of the hydrogen absorption during the milling is shown in Fig. 4.In the initial 10 min, an amount of hydrogen, about 1.05 wt % is absorbed quickly;Journal of Materials Science Letters, accepted July 2003 4 then, the hydrogen absorption is slowed down in the following 1 h. The hydrogen content increases rapid...