N-doped ordered mesoporous carbon as a multifunctional support of ultrafine Pt nanoparticles for hydrogenation of nitroarenes

被引:43
|
作者
Liang, Jifen [1 ]
Zhang, Xiaoming [2 ]
Jing, Lingyan [2 ]
Yang, Hengquan [2 ]
机构
[1] Shanxi Univ, Inst Mol Sci, Taiyuan 030006, Shanxi, Peoples R China
[2] Shanxi Univ, Sch Chem & Chem Engn, Taiyuan 030006, Shanxi, Peoples R China
基金
中国国家自然科学基金;
关键词
N-doped mesoporous carbon; Multifunctional support; Ultrafine platinum nanoparticle; Hydrogenation reaction; Halogenated nitrobenzene; METAL NANOPARTICLES; PHENOL HYDROGENATION; GOLD NANOPARTICLES; AEROBIC OXIDATION; CATALYSIS; SPHERES; NANOSPHERES; INTERFACES; ALCOHOLS; PHASE;
D O I
10.1016/S1872-2067(17)62833-X
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Due to the advantages of high surface areas, large pore volumes and pore sizes, abundant nitrogen content that favored the metal-support interactions, N-doped ordered mesoporous carbons are regarded as a kind of fascinating and potential support for the synthesis of effective supported catalysts. Here, a N-doped ordered mesoporous carbon with a high N content (9.58 wt%), high surface area (417 m2/g), and three-dimensional cubic structure was synthesized successfully and used as an effective support for immobilizing Pt nanoparticles (NPs). The positive effects of nitrogen on the metal particle size enabled ultrasmall Pt NPs (about 1.0 +/- 0.5 nm) to be obtained. Moreover, most of the Pt NPs are homogeneously dispersed in the mesoporous channels. However, using the ordered mesoporous carbon without nitrogen as support, the particles were larger (4.4 +/- 1.7 nm) and many Pt NPs were distributed on the external surface, demonstrating the important role of the nitrogen species. The obtained N-doped ordered mesoporous material supported catalyst showed excellent catalytic activity (conversion 100%) and selectivity (>99%) in the hydrogenation of halogenated nitrobenzenes under mild conditions. These values are much higher than those achieved using a commercial Pt/C catalyst (conversion 89% and selectivity 90%). This outstanding catalytic performance can be attributed to the synergetic effects of the mesoporous structure, N-functionalized support, and stabilized ultrasmall Pt NPs. Moreover, such supported catalyst also showed excellent catalytic performance in the hydrogenation of other halogenated nitrobenzenes and nitroarenes. In addition, the stability of the multifunctional catalyst was excellent and it could be reused more than 10 times without significant losses of activity and selectivity. Our results conclusively show that a N-doped carbon support enable the formation of ultrafine metal NPs and improve the reaction activity and selectivity. (C) 2017, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
引用
收藏
页码:1252 / 1260
页数:9
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