Zr2Fe alloy exhibits the advantages of being tritiated water-free and easy to recover in the form of reversible metal hydrides, which make it an ideal material for the trapping of hydrogen isotopes. However, its practical application is significantly limited by its susceptibility to poisoning by impurity gases such as oxygen. While significant progress has been made in understanding the effects of oxygen on hydrogen adsorption, a microscopic-level explanation of this interaction is still lacking. In this work, we employed detailed density functional theory to investigate the microscopic interaction mechanism between O2 and Zr2Fe, as well as the impact on hydrogen adsorption, addressing a gap in the current understanding. Our results reveal that O2 dissociatively adsorbs at hollow sites on the Zr2Fe surface, with oxygen atoms forming strong bonds with Zr and Fe atoms. This interaction blocks key active sites, hindering hydrogen diffusion into the alloy’s interior, as confirmed by climbing-image nudged elastic band calculations. These findings provide new insights into the inhibition mechanism caused by oxygen, offering a deeper understanding for improving the hydrogen storage performance of Zr-based alloys.
Read full abstract