Due to the poor activation performance and kinetics of Ti50V25Cr25 alloys, the element Zr was added to improve the phase structure of the alloy and achieve a high-performance hydrogen storage alloy. The Ti50-xV25Cr25Zrx (x = 0, 5, 7, and 9) system alloys were prepared by arc melting. The alloys were analyzed using an X-ray diffractometer (XRD), scanning electron microscope (SEM), and differential scanning calorimeter (DSC). The hydrogen storage capabilities of the alloys were also obtained by the Sievert volumetric method. The results indicated that the alloy with Zr added had a combination of the C15 Laves phase and the BCC phase, whereas the Zr-free alloy had a BCC single phase. The partial replacement of Zr with Ti resulted in an increase in the lattice parameters of the main phase. The hydrogen storage kinetic performance and activation of the alloys both significantly improved with an increasing Zr concentration. The time to reach 90% of the maximum hydrogen storage capacity decreased to 2946 s, 230 s, and 120 s, respectively, with the increases in Zr concentration. The initial hydrogen absorption content of the alloys increased and then decreased after the addition of the element Zr. The second phase expanded with an increasing Zr concentration, which in turn decreased the abundance of the BCC main phase. The Ti43V25Cr25Zr7 alloy showed good cycle stability and hydrogen-desorption performance, and it could absorb 90% of the maximum hydrogen storage capacity in around 230 s. The maximum hydrogen-absorption capacity of the alloy was 2.7 wt%. The diffusion activation energy of hydrogen desorption dropped from 102.67 kJ/mol to 92.62 kJ/mol.
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