Supported Au/MIL-53(Al): a reusable green solid catalyst for the three-component coupling reaction of aldehyde, alkyne, and amine
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- 作者：Lili Liu ; Xishi Tai ; Nana Zhang…
- 关键词：Metal–organic frameworks ; MIL ; 53(Al) ; Three component coupling reaction ; Propargylamines ; Gold
- 刊名：Reaction Kinetics, Mechanisms and Catalysis
- 出版年：2016
- 出版时间：October 2016
- 年：2016
- 卷：119
- 期：1
- 页码：335-348
- 全文大小：785 KB
- 刊物类别：Chemistry and Materials Science
- 刊物主题：Chemistry
Catalysis
Industrial Chemistry and Chemical Engineering
Physical Chemistry - 出版者：Akad茅miai Kiad贸, co-published with Springer Science+Business Media B.V., Formerly Kluwer Academic
- ISSN：1878-5204
- 卷排序：119
文摘
MIL-53(Al) was synthesized in a mixture of aluminum nitrate, 1,4-benzenedicarboxylic acid, and water using the hydrothermal and reflux methods. A metal–organic-framework-supported Au-based heterogeneous catalyst (Au/MIL-53(Al)) was prepared using the impregnation method under mild conditions with HAuCl4·4H2O as the Au precursors. The physicochemical properties of the samples were characterized by X-ray diffraction (XRD), infrared spectroscopy (IR), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TG), transmission electron microscopy (TEM), and inductively coupled plasma atomic emission spectroscopy (ICP–AES). MIL-53(Al) indicates excellent chemical stability without structure degradation during the loading and catalysis process. The XPS spectra indicate that the catalyst Au/MIL-53(Al) contains coexisting Au0 and Au3+ ions. The catalytic performance of the catalyst was examined in one-pot synthesis of structurally divergent propargylamines via three component coupling of aldehyde, alkyne, and amine (A3) in 1,4-dioxane. The results showed that the catalyst Au/MIL-53(Al) displayed high activity without any additives or an inert atmosphere (the yield reached 97.9 % for 5 h at 120 °C). Au/MIL-53(Al) has proven to be applicable to a wide range of substrates. Various aromatic/aliphatic aldehydes, aromatic alkynes, and piperidine were able to undergo A3 coupling on the catalyst Au/MIL-53(Al). In addition, the catalyst could be recovered easily by centrifugation and reused three times.