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通过在钯纳米立方体上组装MIL-101(Fe)金属有机框架实现钯上的协同氢化反应。

Synergistic Hydrogenation over Palladium through the Assembly of MIL-101(Fe) MOF over Palladium Nanocubes.

作者信息

Bakuru Vasudeva Rao, Kalidindi Suresh Babu

机构信息

Materials science division, Poornaprajna Institute of Scientific Research, Bidalur post, Devanahalli, Bengaluru, 562164, India.

Graduate Studies, Manipal University, Manipal-, 576104, India.

出版信息

Chemistry. 2017 Nov 21;23(65):16456-16459. doi: 10.1002/chem.201704119. Epub 2017 Oct 30.

DOI:10.1002/chem.201704119
PMID:28990695
Abstract

Enhancing catalytic performance of metal nanoparticles is highly sought for many industrial catalytic processes. In this regard, assembly of crystalline porous super-tunable metal-organic frameworks (MOFs) around preformed metal nanoparticles is an attractive prospect as this strongly influences the activity of the entire nanoparticle surface. Herein, we assembled a MlL-101(Fe) MOF onto the Pd nanocubes and evaluated the catalytic properties of the hybrid material for the hydrogenation of the α,β-unsaturated carbonyl compounds cinnamaldehyde, crotonaldehyde, and β-ionone. Owing to the synergestic effects originating from the Lewis acid sites present on MOF and Pd active sites, striking improvements in the activities and selectivities were observed for the Pd⊂MIL-101(Fe) hybrid material. The turnover frequency (TOF) values increased up to roughly 20 fold and in all three studied substrates, C=C was preferentially hydrogenated compared to C=O. Furthermore, the Pd⊂MIL-101(Fe) catalyst was readily reusable and highly stable.

摘要

提高金属纳米颗粒的催化性能在许多工业催化过程中备受关注。在这方面,围绕预制金属纳米颗粒组装结晶多孔超可调金属有机框架(MOF)是一个有吸引力的前景,因为这会强烈影响整个纳米颗粒表面的活性。在此,我们将MlL-101(Fe) MOF组装到钯纳米立方体上,并评估了该杂化材料对α,β-不饱和羰基化合物肉桂醛、巴豆醛和β-紫罗兰酮氢化反应的催化性能。由于MOF上的路易斯酸位点和钯活性位点产生的协同效应,Pd⊂MIL-101(Fe)杂化材料的活性和选择性有显著提高。周转频率(TOF)值增加了约20倍,并且在所有三种研究的底物中,与C=O相比,C=C优先被氢化。此外,Pd⊂MIL-101(Fe)催化剂易于重复使用且高度稳定。

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