Chinese Journal of Catalysis ›› 2017, Vol. 38 ›› Issue (9): 1613-1620.DOI: 10.1016/S1872-2067(17)62815-8

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Effect of the degree of dispersion of Pt over MgAl2O4 on the catalytic hydrogenation of benzaldehyde

Feng Yana,b, Caixian Zhaoa, Lanhua Yia, Jingcai Zhangb, Binghui Gec, Tao Zhangb, Weizhen Lib   

  1. a Key Laboratory of Environmentally Friendly Chemistry and Applications of Ministry of Education, School of Chemistry, Xiangtan University, Xiangtan 411105, Hunan, China;
    b State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
    c Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
  • Received:2017-02-14 Revised:2017-03-15 Online:2017-09-18 Published:2017-09-06
  • Contact: 10.1016/S1872-2067(17)62815-8
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21403213, 21673226, 21376236, U1462121), the "Hundred Talents Programme" of the Chinese Academy of Sciences, and National Key R&D Program of China (2016YFA0202801), and the "Strategic Priority Research Program" of the Chinese Academy of Sciences (XDB17020100), Department of Science and Technology of Liaoning province under contract of 2015020086-101, and the Natural Science Foundation of Hunan Province (2016JJ2128).

Abstract:

One of the central tasks in the field of heterogeneous catalysis is to establish structure-function relationships for these catalysts, especially for precious metals dispersed on the sub-nanometer scale. Here, we report the preparation of MgAl2O4-supported Pt nanoparticles, amorphous aggre-gates and single atoms, and evaluate their ability to catalyze the hydrogenation of benzaldehyde. The Pt species were characterized by N2 adsorption, X-ray diffraction (XRD), aberration-corrected transmission electron microscopy (ACTEM), CO chemisorption and in situ Fourier transform infra-red spectroscopy of the chemisorbed CO, as well as by inductively coupled plasma atomic emission spectroscopy. They existed as isolated or neighboring single atoms on the MgAl2O4 support, and formed amorphous Pt aggregates and then nanocrystallites with increased Pt loading. On the MgAl2O4 support, single Pt atoms were highly active in the selective catalytic hydrogenation of ben-zaldehyde to benzyl alcohol. The terrace atoms of the Pt particles were more active but less selec-tive; this was presumably due to their ability to form bridged carbonyl adsorbates. The MgAl2O4-supported single-atom Pt catalyst is a novel catalyst with a high precious atom efficiency and excellent catalytic hydrogenation ability and selectivity.

Key words: Platinum, MgAl2O4 spinel, Single-atom catalyst, Selective hydrogenation, Benzaldehyde, Benzyl alcohol