Local structural changes in V–Ti–Cr alloy hydrides with hydrogen absorption/desorption cycling.

Vanadium-based solid solution alloys potentially serve as safe, high-capacity hydrogen storage materials. Low-vanadium-concentration alloys have low durability, and their hydrogen absorption and desorption amounts decrease by 20 % after 100 cycles. In this study, we conducted reverse Monte Carlo modeling on X-ray diffraction patterns and neutron pair distribution functions of the hydrogen-absorbed and desorbed samples of a V 0.10 Ti 0.36 Cr 0.54 alloy to analyze the variations in the local structure. The local structure surrounding the hydrogen atom in the hydrogen-absorbed phase exhibited minimal changes. In contrast, hydrogen occupied both tetrahedral and octahedral sites of the hydrogen-desorbed phase almost equally during the early cycles; however, the amount of hydrogen occupying the tetrahedral sites increased with the number of cycles. It is speculated that hydrogen absorption and desorption cycling induced grain refinement and/or introduced dislocations, which altered both the amount of hydrogen and the sites occupied in the desorbed phase, thereby decreasing the hydrogen storage capacity. [Display omitted] • Degradation mechanism of V–Ti–Cr hydrogen storage alloy revealed by local structure. • Decrease in hydrogen storage consistent with PDF refinements and p – c isotherms. • Cr–H and Ti–H correlations reproduced by a large atomic ensemble in RMC modeling. • Change in hydrogen occupation positions supplemented by inelastic neutron scattering. [ABSTRACT FROM AUTHOR]