A Hydrothermally Stable Single-Atom Catalyst of Pt Supported on High-Entropy Oxide/Al2O3: Structural Optimization and Enhanced Catalytic Activity

A catalyst with high-entropy oxide (HEO)-stabilized single-atom Pt can afford low-temperature activity for catalytic oxidation and remarkable durability even under harsh conditions. However, HEO is easy to harden during sintering, which results in a few defective sites for anchoring single-atom metals. Herein, we present a sol-gel-assisted mechanical milling strategy to achieve a single-atom catalyst of Pt-HEO/Al₂O₃. The strong interaction between HEO and Al₂O₃ effectively inhibits the growth of HEO microparticles, which leads to generation of more surface defects because of the nanoscale effect. Meanwhile, another strong interaction between Pt and HEO stabilizes single-atom Pt on HEO. Temperature-programmed techniques further verify that the reactivity of surface lattice oxygen species is enhanced because of the Pt-O-M bonds on the surface of HEO. Unlike conventional single-atom Pt catalysts, Pt-HEO/Al₂O₃ as a heterogeneous catalyst not only exhibits superior stability against hydrothermal aging but also presents long-term reaction stability for CO catalytic oxidation, which exceeds 540 h. The present work opens a new door for rational design of hydrothermally stable single-atom Pt catalysts, which are highly promising in practical applications.