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介孔氧化铁负载金纳米颗粒用于增强 CO 氧化反应。

Gold nanoparticles supported on mesoporous iron oxide for enhanced CO oxidation reaction.

机构信息

Australian Institute of Innovative Materials (AIIM), University of Wollongong, North Wollongong, New South Wales 2500, Australia.

出版信息

Nanoscale. 2018 Mar 8;10(10):4779-4785. doi: 10.1039/c7nr08895g.

Abstract

Herein, we report the synthesis of gold (Au)-loaded mesoporous iron oxide (FeO) as a catalyst for both CO and NH oxidation. The mesoporous FeO is firstly prepared using polymeric micelles made of an asymmetric triblock copolymer poly(styrene-b-acrylic acid-b-ethylene glycol) (PS-b-PAA-b-PEG). Owing to its unique porous structure and large surface area (87.0 m g), the as-prepared mesoporous FeO can be loaded with a considerably higher amount of Au nanoparticles (Au NPs) (7.9 wt%) compared to the commercial FeO powder (0.8 wt%). Following the Au loading, the mesoporous FeO structure is still well-retained and Au NPs with varying sizes of 3-10 nm are dispersed throughout the mesoporous support. When evaluated for CO oxidation, the Au-loaded mesoporous FeO catalyst shows up to 20% higher CO conversion efficiency compared to the commercial Au/FeO catalyst, especially at lower temperatures (25-150 °C), suggesting the promising potential of this catalyst for low-temperature CO oxidation. Furthermore, the Au-loaded mesoporous FeO catalyst also displays a higher catalytic activity for NH oxidation with a respectable conversion efficiency of 37.4% compared to the commercial Au/FeO catalyst (15.6%) at 200 °C. The significant enhancement in the catalytic performance of the Au-loaded mesoporous FeO catalyst for both CO and NH oxidation may be attributed to the improved dispersion of the Au NPs and enhanced diffusivity of the reactant molecules due to the presence of mesopores and a higher oxygen activation rate contributed by the increased number of active sites, respectively.

摘要

在此,我们报告了负载金(Au)的介孔氧化铁(FeO)作为 CO 和 NH 氧化的催化剂的合成。介孔 FeO 是使用由不对称三嵌段共聚物聚(苯乙烯-b-丙烯酸-b-乙二醇)(PS-b-PAA-b-PEG)制成的聚合物胶束首先制备的。由于其独特的多孔结构和大表面积(87.0 m g),与商业 FeO 粉末(0.8 wt%)相比,所制备的介孔 FeO 可以负载相当高量的 Au 纳米颗粒(Au NPs)(7.9 wt%)。Au 负载后,介孔 FeO 结构仍得以很好地保留,Au NPs 的尺寸在 3-10nm 之间分散在整个介孔载体中。在评估 CO 氧化时,负载 Au 的介孔 FeO 催化剂与商业 Au/FeO 催化剂相比,CO 转化率效率提高了高达 20%,尤其是在较低温度(25-150°C)下,这表明该催化剂在低温 CO 氧化方面具有很大的应用潜力。此外,负载 Au 的介孔 FeO 催化剂在 200°C 时对 NH 氧化的催化活性也更高,转化率为 37.4%,而商业 Au/FeO 催化剂(15.6%)。负载 Au 的介孔 FeO 催化剂对 CO 和 NH 氧化的催化性能显著提高,可能归因于 Au NPs 的分散性得到改善,以及介孔的存在使反应物分子的扩散性增强,同时增加的活性位点数使氧的活化速率提高。

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