Chinese Journal of Catalysis ›› 2014, Vol. 35 ›› Issue (1): 108-119.DOI: 10.1016/S1872-2067(12)60720-7

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Catalytic activity of Ag/SBA-15 for low-temperature gas-phase selective oxidation of benzyl alcohol to benzaldehyde

Liang Maa, lihua Jiab, Xiangfeng Guoa, Lijun Xiangb   

  1. a Key Laboratory of Fine Chemicals of College of Heilongjiang Province, Qiqihar University, Qiqihar 161006, Heilongjiang, China;
    b College of Chemistry and Chemical Engineering, Qiqihar University, Qiqihar 161006, Heilongjiang, China
  • Received:2013-08-11 Revised:2013-09-22 Online:2013-12-23 Published:2014-01-17
  • Contact: lihua Jia, Xiangfeng Guo
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21176125), the Science Research Project of the Ministry of Education of Heilongjiang Province of China (12521594, 2012TD012, JX201205), the Natural Science Foundation of Heilongjiang Province of China (B201114, B201313), and the Key Program of Science and Technology of Qiqihar, Heilongjiang Province (GYGG-201108).

Abstract:

Ag/SBA-15 catalysts with different Ag contents were prepared by an impregnation method and were used for the gas-phase selective oxidation of benzyl alcohol to benzaldehyde with O2 as the oxidant. These catalysts were characterized using N2 adsorption-desorption, X-ray diffraction, scanning electron microscopy, high-resolution transmission electron microscopy, inductively coupled plasma mass spectrometry, and X-ray photoelectron spectroscopy. The effects of Ag loading, reaction temperature, and weight hourly space velocity of benzyl alcohol on the catalytic performance were investigated. The results showed that Ag was successfully incorporated into the mesoporous channels of SBA-15 and well dispersed on the surface as a result of the nano-confinement effect of SBA-15, which increased the specific surface area of the active components. Moreover, Ag/SBA-15 had a uniform pore size, a wall of thickness of 3-5 nm, and a high specific surface area of 411-541 m2/g. The catalytic activity of Ag/SBA-15 for the gas-phase selective oxidation of benzyl alcohol to benzaldehyde was enhanced by oxygen spillover of nucleophilic oxygen species from the Ag nanoparticles to the SBA-15 surface. The 5.3%Ag/SBA-15 exhibited excellent low-temperature catalytic properties; when the reaction temperature was 220℃, the conversion of benzyl alcohol and the selectivity for benzaldehyde reached 87% and 95%, respectively. At 240℃, the catalyst displayed the best catalytic properties, achieving a benzyl alcohol conversion of 94% and benzaldehyde selectivity of 97%, which remained almost constant at 240-300℃. This showed that Ag/SBA-15 had excellent thermal gradient stability. The catalyst could be used for 40 h and retained high catalytic activity for oxidation after treatment at 500℃.

Key words: Silver, SBA-15, Low-temperature gas-phase oxidation, Benzyl alcohol, Benzaldehyde