First-Principles Calculations of the Effect of Ta Content on the Properties of UNbMoHfTa High-Entropy Alloys

Uranium-containing high-entropy alloys (HEAs) exhibit great potential as a novel energetic structural material, attributed to their excellent performance in impact energy release, superior mechanical properties, and high density. This study investigates the effects of Ta content on the phase stability, lattice constant, density, elastic constants, polycrystalline moduli, and electronic structure of (UNbMoHf)54−xTax high-entropy alloys (where x = 2, 6, 10, 14, 18), utilizing a combination of density functional theory (DFT) calculations and the special quasi-random structure (SQS) approach. Our findings confirm that these alloys maintain stable body-centered cubic structures, as evidenced by atomic radius difference and valence electron concentration evaluations. Analysis of elastic modulus, Cauchy pressure, and Vickers hardness indicates that Ta incorporation enhances mechanical properties and increases the anisotropy of these alloys. Furthermore, investigations into the electronic structure reveal that adding Ta reduces metallic character while increasing covalent characteristics, enhancing the contribution of Ta’s d-orbitals to the total density of states and intensifying covalent bonding interactions between Ta and other elements such as Nb, Mo, and U. These findings provide theoretical guidance for the design of high-performance UNbMoHfTa HEAs with tailored properties.