Regulating the interaction between Zr-based support and Pt for enhanced room-temperature hydrogen elimination

Hydrogen leakage safety concerns and the limited performance of conventional oxide-supported Pt catalysts have motivated the development of Pt-based catalysts supported on Zr-based multi-component alloys. In this study, a series of Pt-based catalysts (Pt/γ-Al₂O₃, Pt/ZrFe, Pt/ZrVFe, and Pt/ZrVFeTi) were synthesized via chemical reduction method. The phase structure, surface morphology, redox properties, and surface chemical states of the catalysts were characterized using various analytical techniques. Their hydrogen elimination performance was evaluated in a fixed-bed reactor under simulated operating conditions. The results indicate that Zr-based alloy-supported Pt catalysts exhibit superior catalytic activity for hydrogen elimination. Among them, Pt/ZrVFeTi catalyst demonstrates the highest performance, achieving a dynamic H₂ conversion rate of 96.8 %, compared to 92.9 % for Pt/γ-Al₂O₃. In static tests, Pt/ZrVFeTi achieves a hydrogen elimination initiation threshold below 0.5 vol%, an initiation time of merely 2 mins, and a hydrogen elimination rate of 5.22 g H₂·(kg·min)^-1 highlighting its exceptional performance under ambient conditions. To unveil the underlying mechanism, density functional theory calculations were employed to analyze hydrogen adsorption energy, the Pt 3d orbital density of states, and interfacial charge transfer behavior. The calculations indicate that the enhanced performance of Pt/ZrVFeTi arises from the multi-component synergy of the ZrVFeTi support, which optimizes metal-support interaction, improves Pt dispersion, facilitates H₂ adsorption, and promotes interfacial electron transfer, collectively leading to superior catalytic activity.