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The effects of Co as a substituent for Ni on microstructure and electrochemical capacity of hydrogen storage alloys MI(NiCoMnAl)5.4 at -30～ +80 ℃, in which the content of Co was 0, 1.31%, 2.63%, 3.94%, 5.25%, and 6.56% (mass fraction), respectively, were reported. All of the alloys were prepared by vacuum induction melting followed by melt-spinning. It is found that the electrochemical capacity of alloys at different temperature depends upon the compositions and preparation methods. The electrochemical capacity of alloys increases at higher temperature (40 ～ 80 ℃ )and decreases at lower temperature ( - 30 ～ 0 ℃ ) with an increasing cobalt content. With an increasing temperature,melt-spinning is more favorable for improved capacity of the alloys than casting. Analyses of the charging/discharging potential curves illustrate that higher cobalt content and melt-spinning techniques are more effective to increase the capacity at higher temperature because of the higher hydrogen evolution potential. On the contrary, the capacity of alloys at lower temperature can be increased by decreasing cobalt content and casting, which is ascribed to higher hydrogen evolution potential and delayed hydrogen evolution reaction, as well as reduced potential drop in the charging/discharging process.XRD patterns confirm that all of the specimens present a single hexagonal CaCu5-type structure and an increased lattice parameters with increasing Co content. The FWHM of the main peak of melt-spun ribbons reduces because of more homogeneous composition and less lattice strain defects.