A novel cerium-based metal-organic framework supported Pd catalyst for semi-hydrogenation of phenylacetylene

IF 5.3 2区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Applied Nano Materials Pub Date : 2024-10-31 DOI:10.1039/d4qi02225d

Xiangdi Zeng, Zi Wang, Meng He, Wanpeng Lu, Wenyuan Huang, Bing An, Jiangnan Li, Li Mufan, Ben Spencer, Sarah Day, Floriana Tuna, Eric J L McInnes, Martin Schroder, Sihai Yang

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Abstract

Phenylacetylene is a detrimental impurity in the polymerisation of styrene, capable of poisoning catalysts even at ppm levels and significantly degrading the quality of polystyrene. The semi-hydrogenation of phenylacetylene to styrene instead of ethylbenzene is, therefore, an important industrial process. We report a novel cerium(IV)-based metal-organic framework (denoted as Ce-bptc), which is comprised of {Ce6} clusters bridged by biphenyl-3,3’,5,5’-tetracarboxylate linkers. Ce-bptc serves as an ideal support for palladium nanoparticles and the Pd@Ce-bptc catalyst demonstrates an excellent catalytic performance for semi-hydrogenation of phenylacetylene, achieving a selectivity of 93% to styrene on full conversion under ambient conditions with excellent reusability. In situ synchrotron X-ray powder diffraction and electron paramagnetic resonance spectroscopy revealed the binding domain of phenylacetylene within Ce-bptc and details of the reaction mechanism.

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用于苯乙炔半加氢的新型铈基金属有机框架支撑钯催化剂

苯乙炔是苯乙烯聚合过程中的一种有害杂质，即使在百万分之几的水平上也能毒害催化剂，并显著降低聚苯乙烯的质量。因此，将苯乙炔半氢化成苯乙烯而不是乙苯是一种重要的工业工艺。我们报告了一种新型的基于铈（IV）的金属有机框架（称为 Ce-bptc），它由联苯-3,3',5,5'-四羧酸链节桥接的 {Ce6} 簇组成。Ce-bptc 是钯纳米粒子的理想载体，Pd@Ce-bptc 催化剂在苯乙炔的半加氢反应中表现出优异的催化性能，在环境条件下完全转化时对苯乙烯的选择性达到 93%，并具有极佳的重复利用率。原位同步辐射 X 射线粉末衍射和电子顺磁共振光谱揭示了苯乙炔在 Ce-bptc 中的结合域和反应机理的细节。

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来源期刊

ACS Applied Nano Materials Multiple-

CiteScore

8.30

自引率

3.40%

发文量

1601

期刊介绍： ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.