Immobilization of highly active Pd nano-catalysts on functionalized mesoporous silica supports using mercapto groups as anchoring sites and their catalytic performance for phenol hydrogenation

doi:10.1016/S1872-2067(12)60603-2

Chinese Journal of Catalysis ›› 2013, Vol. 34 ›› Issue (8): 1519-1526.DOI: 10.1016/S1872-2067(12)60603-2

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Immobilization of highly active Pd nano-catalysts on functionalized mesoporous silica supports using mercapto groups as anchoring sites and their catalytic performance for phenol hydrogenation

Jiaxi Zhang^a, Gaowei Huang^a, Cheng Zhang^a,b, Qunhua He^b, Chao Huang^a, Xu Yang^c, Huiyu Song^a, Zhenxing Liang^a, Li Du^a,d, Shijun Liao^a,d

a School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, Guangdong, China;
b Guangdong Environmental Monitoring Center, Guangzhou 510640, Guangdong, China;
c Key Laboratory of Renewable Energy and Gas Hydrate, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, Guangdong, China;
d The Key Laboratory of Fuel Cell Technology of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, Guangdong, China

Received:2013-03-24 Revised:2013-04-18 Online:2013-08-16 Published:2013-07-30
Supported by:
This work was supported by the National Natural Science Foundation of China (51102099, 21003052), the Natural Science Foundation of Guangdong Province (S2011040000964), the Training Project for the Outstanding and Innovative Talents in Guangdong Colleges and Universities (Yumiao Project, 2011), and the Fundamental Research Funds for the Central Universities, SCUT.

Abstract

Abstract: Highly active and highly dispersed Pd-loaded nano-catalysts using mercapto group (-SH) functionalized mesoporous silica supports, namely, Pd-SH-MCM-41 and Pd-SH-SBA-15, were prepared using an impregnation-reduction approach. The surface -SH groups are believed to facilitate the high distribution and immobilization of the Pd nanoparticles within the silica supports through an anchoring interaction. The catalysts featured long-range ordered structures, uniform pore size, high surface area, and highly dispersed Pd nanoparticles as characterized by X-ray diffraction, N₂ adsorption-desorption, and transmission electron microscopy. The catalysts showed activity five times higher than that of commercial Pd/C catalyst and three times higher than those of Pd/MCM-41 and Pd/SBA-15 catalysts. Within 1 h of reaction at 80℃ and 1.0 MPa, the conversion of phenol attained was greater than 99%, and the selectivity for cyclohexanone was 98%.

Key words: Mesoporous silica, Mercapto group functionalization, Palladium, Anchoring, Supported catalyst, Phenol hydrogenation

Jiaxi Zhang, Gaowei Huang, Cheng Zhang, Qunhua He, Chao Huang, Xu Yang, Huiyu Song, Zhenxing Liang, Li Du, Shijun Liao. Immobilization of highly active Pd nano-catalysts on functionalized mesoporous silica supports using mercapto groups as anchoring sites and their catalytic performance for phenol hydrogenation[J]. Chinese Journal of Catalysis, 2013, 34(8): 1519-1526.

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Immobilization of highly active Pd nano-catalysts on functionalized mesoporous silica supports using mercapto groups as anchoring sites and their catalytic performance for phenol hydrogenation

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