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

• Published in: iScience Vol. 23; no. 12; p. 101852
• Main Authors: Fan, Longlong, Dai, Jiajun, Huang, Zhongliang, Xiao, Jingran, Li, Qingbiao, Huang, Jiale, Zhou, Shu-Feng, Zhan, Guowu
• Format: Journal Article
• Language: English
• Published: Elsevier Inc 18.12.2020; Elsevier
• Subjects: Chemistry; Engineering; Inorganic Chemistry: Catalysis; Inorganic Chemistry: Catalysis; Engineering; Chemistry
• ISSN: 2589-0042; 2589-0042
• DOI: 10.1016/j.isci.2020.101852

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. [Display omitted] •Biomimetic catalysts were prepared by the integration of biomolecules with Au/CeO2•The experimental TOF of hemin-Au/CeO2 was ca. 30 times higher than that of Au/CeO2•Strong electronic interactions facilitate the adsorption and activation of CO molecule•DFT calculations reveal the mechanisms of enhanced activity of biomimetic catalysts Chemistry; Inorganic Chemistry: Catalysis; Engineering