Acta Phys. -Chim. Sin. ›› 2011, Vol. 27 ›› Issue (01): 177-185.doi: 10.3866/PKU.WHXB20110105

• CATALYSIS AND SURFACE SCIENCE • Previous Articles     Next Articles

Synthesis of Highly Efficient WO3-Doped MCF Catalyst and Its Application in the Selective Oxidation of Cyclopentene to Glutaraldehyde

YANG Xin-Li1,2, YIN An-Yuan1, DAI Wei-Lin1, FAN Kang-Nian1   

  1. 1. Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, P. R. China;
    2. School of Chemistry & Chemical Engineering, Henan University of Technology, Zhengzhou 450052, P. R. China
  • Received:2010-08-20 Revised:2010-10-25 Published:2010-12-31
  • Contact: DAI Wei-Lin E-mail:wldai@fudan.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20973042, 20903035), Science & Technology Commission of Shanghai Municipality, China (08DZ2270500), and Research Fund for the Doctoral Program of Higher Education, China (20090071110011).

Abstract:

We synthesized WO3 doped mesocellular silica foam (WO3-doped MCF) catalysts with a high tungsten oxide content of 20% (w, mass fraction) directly using sodium tungstate and tetraethylorthosilicate as precursors. The catalysts showed high thermal stability after calcination at 773 K. Small-angle X-ray scattering, N2 adsorption, and transmission electron microscopy results indicated that the characteristic three dimensional mesocellular structural features of the MCFs were retained after the incorporation of tungsten oxide species. Ultraviolet-Raman and ultraviolet-visible diffuse reflectance spectroscopy data showed that isolated or lowly condensed oligomeric tungsten oxide species were obtained for the WO3- doped MCF catalysts. These oxide species were stable and highly dispersed in the silica-based MCF matrix with a tungsten oxide content lower than 20% (w). We found that the nature of the tungsten species largely depended on its content and the direct synthesis method was beneficial in obtaining highly dispersed tungsten oxide species. In the selective oxidation of cyclopentene (CPE) to glutaraldehyde (GA), the 20% (w) WO3-doped MCF catalyst had a CPE conversion of 100% and a GA yield of 83.5% after reacting for 16 h. Furthermore, very stable catalytic activity after many recycling tests was apparent for the WO3-doped MCF catalyst indicating that almost no tungsten species was leached into the reaction solution. A proper amount of tungsten oxide and its high dispersion accounted for the high activity.

Key words: WO3-doped MCF, Tungsten oxide species, Selective oxidation, Cyclopentene, Glutaraldehyde

MSC2000: 

  • O643