Acta Phys. -Chim. Sin. ›› 2015, Vol. 31 ›› Issue (6): 1129-1136.doi: 10.3866/PKU.WHXB201503272

• CATALYSIS AND SURFACE SCIENCE • Previous Articles     Next Articles

Influence of Catalyst Structure on Performance of Cu/SiO2 in Hydrogenation of Methyl Acetate

QIU Kun-Zan, GUO Wen-Wen, WANG Hai-Xia, ZHU Ling-Jun, WANG Shu-Rong   

  1. State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, P. R. China
  • Received:2015-01-19 Revised:2015-03-27 Published:2015-06-05
  • Contact: WANG Shu-Rong E-mail:srwang@zju.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (51276166), National Science and Technology Supporting Plan through Contract, China (2015BAD15B06), and Program of Introducing Talents of Discipline to University, China (B08026).

Abstract:

Cu/SiO2 catalysts for the hydrogenation of methyl acetate (MA) to ethanol were prepared using the urea hydrolysis method. The catalysts were characterized using N2-physisorption, X-ray diffraction (XRD), temperature-programmed reduction (TPR), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The effects of the copper loading and reduction temperature on the catalyst structure and catalytic performance were investigated. Experimental studies of the influence of the copper loading showed that a 20% (mass fraction, w) Cu/SiO2 catalyst had uniformly dispersed copper particles and a large number of active centers, and therefore gave the best hydrogenation performances among the three catalysts with the copper loadings of 10%, 20%, and 30%, respectively. Then 20% (w) Cu/SiO2 was reduced at different temperatures (270, 350, and 450 ℃). The results showed that 20% (w) Cu/SiO2 reduced at 350 ℃ had the best catalytic activity. This was attributed to the homogeneous distribution of copper nanoparticles, and appropriate Cu0/(Cu0+Cu+) molar ratio, which achieved simultaneous dissociation of hydrogen and MA activation. Under the optimum reaction conditions, the MA conversion and ethanol selectivity reached 97.8% and 64.9% (theoretical maximum value: 66.6%), respectively.

Key words: Methyl acetate, Ethanol, Hydrogenation, Cu/SiO2, Urea hydrolysis method, Cu0/(Cu0+Cu+) molar ratio

MSC2000: 

  • O643