Large Destabilization of (TiVNb)-Based Hydrides via (Al, Mo) Addition: Insights from Experiments and Data-Driven Models

High-entropy alloys (HEAs) represent an interesting alloying strategy that can yield exceptional performance properties needed across a variety of technology applications, including hydrogen storage. Examples include ultrahigh volumetric capacity materials (BCC alloys → FCC dihydrides) with improved thermodynamics relative to conventional high-capacity metal hydrides (like MgH2), but still further destabilization is needed to reduce operating temperature and increase system-level capacity. In this work, we demonstrate efficient hydride destabilization strategies by synthesizing two new Al0.05(TiVNb)0.95–xMox (x = 0.05, 0.10) compositions. We specifically evaluate the effect of molybdenum (Mo) addition on the phase structure, microstructure, hydrogen absorption, and desorption properties. Both alloys crystallize in a bcc structure with decreasing lattice parameters as the Mo content increases. The alloys can rapidly absorb hydrogen at 25 °C with capacities of 1.78 H/M (2.79 wt %) and 1.79 H/M (2.75 wt %) with increasing Mo content. Pressure-composition isotherms suggest a two-step reaction for hydrogen absorption to a final fcc dihydride phase. The experiments demonstrate that increasing Mo content results in a significant hydride destabilization, which is consistent with predictions from a gradient boosting tree data-driven model for metal hydride thermodynamics. Furthermore, improved desorption properties with increasing Mo content and reversibility were observed by in situ synchrotron X-ray diffraction, in situ neutron diffraction, and thermal desorption spectroscopy.