The La–Mg–Ni–Co-based AB2-type alloys, namely La0.7Sm0.3MgNi3·6Co0.4xwt.%Ni (x = 0,5,10, 15, 20), were synthesized through ball milling. The study focused on investigating the impact of Ni content on the structures and electrochemical properties. The structures of the samples were analyzed using X-ray diffraction (XRD), scanning electron microscopy (SEM) and Transmission electron microscope (TEM). It has been demonstrated that the experimental samples consist of a primary phase, LaMgNi4, and a secondary phase, LaNi5. The abundance of phases undergoes significant changes with variations in Ni content, while the phase composition remains constant. The results indicate that a rise in Ni concentration results in an elevation of the LaNi5 phase and a reduction of the LaMgNi4 phase. Additionally, ball milling and the addition of nickel contribute to the refinement of the alloy grains. As the nickel concentration reached 20 wt%, the cycle retention rate(S30) of the composite alloy electrode achieved its maximum value of 73.42 %. In addition, the electrochemical kinetic test findings demonstrated that the maximum D value of the hydrogen diffusion system was 1.807 × 10−10 cm2/s and that the maximum current density of the composite hydrogen storage alloy electrode was 723 mA/g when x = 0 wt%.
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