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.

由于高仿生性和优异的催化活性，仿生催化剂引起了广泛的研究兴趣。本文中，我们通过将生物分子（血红素或亚铁酞菁）整合到轮廓分明的Au / CeO _2上，报道了一系列仿生催化剂，这导致了高性能的CO氧化催化剂。该生物分子的强烈电子相互作用，Au和的CeO ₂被证实和CO摄取过氯高铁血红素-金/的CeO ₂比的Au /更大的CeO大致8倍左右₂。基于Au / CeO ₂（111）和hemin-Au / CeO ₂（111）模型，密度泛函理论计算揭示了生物分子辅助催化过程的机理。理论预测表明，CO和O ₂分子优先结合非接触Au原子（低配位位点）的表面，而不是生物分子位点，并且Au结合的CO的加速氧化是通过Langmuir-Hinshelwood机理或氢键进行的。 Mars-van Krevelen机制。因此，这些发现为开发低成本和高活性的仿生催化剂提供了有用的见识。