High-throughput calculations to develop high-entropy alloys for hydrogen storage applications

A high-throughput computational alloy design framework was employed to accelerate the discovery of non-equiatomic Ti–Zr–V–Cr–(Co,Fe) HEAs capable of forming the targeted dual-phase architecture consisting of body-centered cubic (BCC) and Laves phase (C14/C15), required for efficient hydrogen storage at room-temperature without activation. Thermodynamic and physical parameters were calculated using semi-empirical models, and phase predictions were performed using Thermo-Calc for 1451 alloys in each Ti–Zr–V–Cr–Fe and Ti–Zr–V–Cr–Co alloy systems to generate the screening dataset. This approach led to identify Ti 20 Zr 10 V 10 Cr 25 Co 35 and Ti 20 Zr 10 V 15 Cr 30 Fe 25 (at.%) HEAs exhibiting dual-phase microstructures with 70–80% Laves phase fraction. Experimental investigations of the fabricated alloys confirmed the predicted phase constituents and demonstrated immediate hydrogen sorption at room temperature without prior activation. The Fe-containing alloy achieved 1.7 wt% of hydrogen absorption within 60 min and showed a reversible desorption of ∼0.6 wt% at ambient conditions. The alloys exhibited an excellent capacity retention with the reversible performance remaining constant in subsequent cycles. Its superior performance is attributed to lower VEC (5.8), larger lattice volume, higher BCC fraction, and favourable interphase boundaries that promote rapid hydrogen diffusion and hydride nucleation. These findings validate that integrating high-throughput computational screening with targeted microstructural design represents a powerful pathway for developing high-performance alloys as next-generation solid-state hydrogen storage materials.