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首页> 外文期刊>Advanced Functional Materials >Strong Electronic Interaction of Amorphous Fe_2O_3 Nanosheets with Single-Atom Pt toward Enhanced Carbon Monoxide Oxidation
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Strong Electronic Interaction of Amorphous Fe_2O_3 Nanosheets with Single-Atom Pt toward Enhanced Carbon Monoxide Oxidation

机译：具有单原子Pt的非晶Fe_2O_3纳米片对增强的一氧化碳氧化的强电子相互作用

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摘要

Platinum-based catalysts are critical to several chemical processes, but their efficiency is not satisfying enough in some cases, because only the surface active-site atoms participate in the reaction. Henceforth, catalysts with single-atom dispersions are highly desirable to maximize their mass efficiency, but fabricating these structures using a controllable method is still challenging. Most previous studies have focused on crystalline materials. However, amorphous materials may have enhanced performance due to their distorted and isotropic nature with numerous defects. Here reported is the facile synthesis of an atomically dispersed catalyst that consists of single Pt atoms and amorphous Fe2O3 nanosheets. Rational control can regulate the morphology from single atom clusters to sub-nanoparticles. Density functional theory calculations show the synergistic effect resulted from the strong binding and stabilization of single Pt atoms with the strong metal-support interaction between the in situ locally anchored Pt atoms and Fe2O3 lead to a weak CO adsorption. Moreover, the distorted amorphous Fe2O3 with O vacancies is beneficial for the activation of O-2, which further facilitates CO oxidation on nearby Pt sites or interface sites between Pt and Fe2O3, resulting in the extremely high performance for CO oxidation of the atomic catalyst.
机译：铂基催化剂对几种化学过程至关重要，但由于某些表面活性位原子参与反应，因此其效率在某些情况下不能令人满意。因此，非常需要具有单原子分散体的催化剂以最大化其质量效率，但是使用可控制的方法来制造这些结构仍然具有挑战性。以前的大多数研究都集中在晶体材料上。但是，无定形材料由于其畸变和各向同性的性质而具有许多缺陷，因此可能具有增强的性能。本文报道了由单个Pt原子和无定形Fe2O3纳米片组成的原子分散催化剂的简便合成方法。合理的控制可以调节从单原子团簇到亚纳米颗粒的形态。密度泛函理论计算表明，协同作用是由于单个Pt原子的牢固结合和稳定以及原位局部锚定的Pt原子与Fe2O3之间的强金属-载体相互作用导致弱的CO吸附。此外，具有O空位的变形的非晶态Fe 2 O 3有利于O-2的活化，这进一步促进了在附近的Pt位点或Pt与Fe 2 O 3之间的界面位点上的CO氧化，从而导致原子催化剂的CO氧化极高的性能。

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