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

ABSTRACT

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.