Acta Phys. -Chim. Sin. ›› 2014, Vol. 30 ›› Issue (6): 1155-1162.doi: 10.3866/PKU.WHXB201401252

• CATALYSIS AND SURFACE SCIENCE • Previous Articles     Next Articles

Preparation of Cu/Zn/Al/(Zr)/(Y) Catalysts from Hydrotalcite-Like Precursors and Their Catalytic Performance for the Hydrogenation of CO2 to Methanol

GAO Peng1,2, LI Feng2, ZHAO Ning2, WANG Hui1, WEI Wei1, SUN Yu-Han2,3   

  1. 1 Center for Greenhouse Gas and Environmental Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203, P. R. China;
    2 State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, P. R. China;
    3 Chinese Academy of Sciences Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203, P. R. China
  • Received:2014-02-10 Revised:2014-04-01 Published:2014-05-26
  • Contact: ZHAO Ning, WEI Wei E-mail:zhaoning@sxicc.ac.cn;weiwei@sari.ac.cn
  • Supported by:

    The project was supported by the National Key Technology Research and Development Program of the Ministry of Science and Technology, China (2013BAC11B02) and Strategic Priority Research Program of the Chinese Academy of Sciences (XDA05010109, XDA05010110, XDA05010204).

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Abstract:

Cu/Zn/Al/(Zr)/(Y) hydrotalcite-like compounds with Cu:Zn:Al:Zr:Y atomic ratios of 2:1:1:0:0, 2:1: 0.8:0.2:0, 2:1:0.8:0:0.2, and 2:1:0.8:0.1:0.1 were prepared using the coprecipitation method. The mixed oxides were then obtained by the calcination of the precursors at 500 ℃ in air, and subsequently evaluated in terms of their catalytic performance for the synthesis of methanol from the hydrogenation of CO2. The asprepared samples were characterized by X-ray diffraction (XRD), thermogravimetric (TG) analysis, N2 adsorption, reactive N2O adsorption, H2 temperature-programmed reduction (H2-TPR), and H2/CO2 temperature-programmed desorption (H2/CO2 TPD) techniques. The results of these analyses showed that the BET specific surface area increased significantly with the introduction of Zr and Y, which was related to the amount of H2O and CO2 evolved from the precursors during calcination. The Cu specific surface area and Cu dispersion properties increased in the order of Cu/Zn/Al2 revealed that the CO2 conversion was dependent on the Cu specific surface area, and the CH3OH selectivity increased linearly as the proportion of strongly basic sites increased. The introduction of Zr and Y therefore favored the production of methanol and the maximum CH3OH yield was obtained over the Cu/Zn/Al/Zr/Y catalyst.

Key words: Hydrotalcite-like precursor, Modifier, Cu/Zn/Al catalyst, CO2 hydrogenation, Methanol

MSC2000: 

  • O643