Designing TiZrNbTa-Al Medium-Entropy Alloy for Next-Generation Hydrogen Storage

Medium-entropy alloys (MEAs) represent a promising class of materials for solid-state hydrogen storage due to their high hydrogen affinity, structural stability, and tunable properties. In this work, a compositional series of (TiZrNbTa)_{100-x}Al_x (x = 0-10 at. %) MEAs were prepared and systematically investigated to clarify the influence of aluminum addition on microstructure, mechanical response, and hydrogen sorption behavior. The alloys were synthesized by arc melting, homogenized by annealing, and characterized using microscopy, X-ray diffraction, density measurements, microhardness testing, nanoindentation, and hydrogen absorption/desorption experiments. Hydrogen sorption was evaluated by isobaric absorption measurements at 2 MPa H₂ over two consecutive cycles, complemented by thermogravimetric desorption analysis of hydrogenated samples. The results show that aluminum addition significantly affects activation behavior, hydrogen uptake, and residual hydrogen retention, while simultaneously increasing hardness and elastic modulus in a non-linear manner. The alloy containing 5 at. % Al exhibits the most balanced performance, combining reduced activation temperature in the second absorption cycle, relatively high hydrogen capacity, and moderate mechanical stiffness. These findings demonstrate that controlled aluminum alloying is an effective strategy for tailoring hydrogen-metal interactions and optimizing the performance of TiZrNbTa-based MEAs for solid-state hydrogen storage applications.