Biomimetic Au/CeO₂ Catalysts Decorated with Hemin or Ferrous Phthalocyanine for Improved CO Oxidation via Local Synergistic Effects.

ABSTRACT: Biomimetic catalysts have drawn broad research interest owing to both high specificity and excellent catalytic activity. Herein, we report a series of biomimetic catalysts by the integration of biomolecules (hemin or ferrous phthalocyanine) onto well-defined Au/CeO₂, which leads to the high-performance CO oxidation catalysts. Strong electronic interactions among the biomolecule, Au, and CeO₂ were confirmed, and the CO uptake over hemin-Au/CeO₂ was roughly about 8 times greater than Au/CeO₂. Based on the Au/CeO₂(111) and hemin-Au/CeO₂(111) models, the density functional theory calculations reveal the mechanisms of the biomolecules-assisted catalysis process. The theoretical prediction suggests that CO and O₂ molecules preferentially bind to the surface of noncontacting Au atoms (low-coordinated sites) rather than the biomolecule sites, and the accelerating oxidation of Au-bound CO occurs via either the Langmuir-Hinshelwood mechanism or the Mars-van Krevelen mechanism. Accordingly, the findings provide useful insights into developing biomimetic catalysts with low cost and high activity.

SUBMITTER: Fan L 

PROVIDER: S-EPMC7721650 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature