Acta Phys. -Chim. Sin. ›› 2011, Vol. 27 ›› Issue (11): 2651-2658.doi: 10.3866/PKU.WHXB20111018

• CATALYSIS AND SURFACE SCIENCE • Previous Articles     Next Articles

Dimethyl Ether Synthesis from CO2 Hydrogenation over CuO-TiO2-ZrO2/HZSM-5 Catalysts

WANG Song, MAO Dong-Sen, GUO Xiao-Ming, LU Guan-Zhong   

  1. Research Institute of Applied Catalysis, School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai 200235, P. R. China
  • Received:2011-05-09 Revised:2011-07-18 Published:2011-10-27
  • Contact: MAO Dong-Sen
  • Supported by:

    The project was supported by the Science and Technology Commission of Shanghai Municipality, China (08520513600), Leading Academic Discipline Project of Shanghai Education Committee, China (J51503) and Shanghai Special Fund for Outstanding Young Teachers, China (yyy10078).

Abstract: A series of CuO-TiO2-ZrO2 mixed oxides with different CuO mass fractions (50%-80%) were prepared by co-precipitation and characterized by X-ray diffraction (XRD), N2 physisorption, temperatureprogrammed reduction of hydrogen (H2-TPR), temperature-programmed desorption of carbon dioxide (CO2-TPD) and hydrogen (H2-TPD), and reactive N2O adsorption techniques. The prepared CuO-TiO2-ZrO2 samples were mixed physically with HZSM-5 zeolite to synthesize dimethyl ether (DME) from CO2 hydrogenation in a fixed bed reactor at 250°C, 3.0 MPa, gas hourly space velocity (GHSV) of 1500 mL·g-1· h-1, and volume ratio of 2.8 for H2 to CO2. We found that the conversion of CO2 increased with an increase in CuO content, reached a maximum at a CuO content of 70% and then decreased. The selectivity of DME increased with an increase in CuO content initially and remained essentially constant when the CuO content was ≥70%. Thus, the yield of DME reached a maximum of 13.2% at 70% CuO content. The productivity of the oxygenated compounds (including methanol and DME) on the CuO-TiO2-ZrO2/HZSM-5 catalysts is closely related to the metallic copper surface area.

Key words: Hydrogenation of CO2, Dimethyl ether, CuO-TiO2-ZrO2 mixed oxide, Zeolite HZSM-5, Bifunctional catalyst