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载体形态对Pt/α-Fe₂O₃催化剂上3-硝基苯乙烯选择性加氢制3-乙烯基苯胺的影响

Support Morphology Effect on Selective Hydrogenation of 3-Nitrostyrene to 3-Vinylaniline over Pt/α-Fe O Catalysts.

作者信息

Dai Chengshan, Zhang Ying, Chen Junnan, Zhong Xia, Zhang Liyun, Zhang Bingsen

机构信息

Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang, 110016, P. R. China.

School of Materials Science and Engineering, University of Science and Technology of China, 72 Wenhua Road, Shenyang, 110016, P. R. China.

出版信息

Chemistry. 2022 Jun 15;28(34):e202200199. doi: 10.1002/chem.202200199. Epub 2022 May 11.

DOI:10.1002/chem.202200199
PMID:35543283
Abstract

Selective hydrogenation of substituted nitroaromatic compounds is an extremely important and challenging reaction. Supported metal catalysts attract much attention in this reaction because the properties of metal nanoparticles (NPs) can be modified by the nature of the support. Herein, the support morphology on the catalytic performance of selective hydrogenation of 3-nitrostyrene to 3-vinylaniline was investigated. Pt NPs supported on octadecahedral α-Fe O supports with a truncated hexagonal bipyramid shape (Pt/α-Fe O -O) and rod-shaped α-Fe O supports (Pt/α-Fe O -R) were prepared by glycol reduction method. Detailed characterizations reveal that the electronic structure and dispersion of Pt NPs can be modified by the supports. The Pt/α-Fe O -O catalyst exhibited superior catalytic performance for hydrogenation of 3-nitrostyrene because of its low coordinated Pt sites and the small Pt NPs size, which is benefit from the high-index exposed surfaces of truncated hexagonal bipyramid-shaped α-Fe O support. The structural evolution during the catalytic reaction was investigated in detail by identical location transmission electron microscopy (IL-TEM) method, which found that the high cycling activity of Pt/α-Fe O -O catalyst during the cycle experiment results from the stability of Pt NPs.

摘要

取代硝基芳烃化合物的选择性氢化是一个极其重要且具有挑战性的反应。负载型金属催化剂在该反应中备受关注,因为金属纳米颗粒(NPs)的性质可通过载体的性质进行修饰。在此,研究了载体形态对3-硝基苯乙烯选择性氢化为3-乙烯基苯胺催化性能的影响。通过乙二醇还原法制备了负载在具有截顶六方双锥形状的十八面体α-Fe₂O₃载体(Pt/α-Fe₂O₃-O)和棒状α-Fe₂O₃载体(Pt/α-Fe₂O₃-R)上的Pt NPs。详细表征表明,载体可修饰Pt NPs的电子结构和分散性。Pt/α-Fe₂O₃-O催化剂对3-硝基苯乙烯氢化表现出优异的催化性能,这归因于其低配位的Pt位点和较小的Pt NPs尺寸,这得益于截顶六方双锥形状的α-Fe₂O₃载体的高指数暴露表面。通过相同位置透射电子显微镜(IL-TEM)方法详细研究了催化反应过程中的结构演变,发现Pt/α-Fe₂O₃-O催化剂在循环实验中的高循环活性源于Pt NPs的稳定性。

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