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For improving the electrode characteristics of the Zr-based AB(2)-type alloy, a new kind of composite hydrogen Zr0.9Ti0.1(Ni0.50Mn0.35V0.15)(2)(represented as AB(2)) with a rare storage alloy was successfully prepared by ball-milling I earth-based AB(5)-type alloy (represented as AB(5)) which worked as a surface modifier. Effects of ball-milling on the electrode characteristics and microstructure of Zr0.9Ti0.1(Ni0.50Mn0.35V0.15)(2) alloy and mixtures of AB(2) with AB(5) alloy were investigated. After milling the mixed AB(2) and AB(5) powders (9: 1 in mass ratio) for 10min, XRD and SEM analysis showed that AB(2) and AB(5) maintained their original crystalline states, respectively, some AB(5) particles were adhered onto the surface of AB(2), and some fresh surfaces were formed. It was found that the activation cycles of AB(2)-AB(5) composite alloy was shortened from 14 to 7 and the maximum discharge capacity was increased from 330mAh . g(-1) to 347mAh . g(-1) as compared with AB(2) alloy. The discharge rate capability of AB(2) alloy was also improved by ball milling AB(2) with AB(5) alloy process. The combined effect of ball-milling and mixing with AB(5) alloy is superior to that of sole treatment. It was believed that AB(5) alloy works not only as a regular hydrogen storage alloy, but also as a surface modifier to catalyze the hydriding/ dehydriding process of AB(2) alloy.