表面助剂改性对Cu/ZnO/Al2O3甲醇合成催化剂性能的影响

doi:10.3866/PKU.WHXB201306211

Abstract

Abstract:

Surface promoters-modified Cu/ZnO/Al₂O₃ (CZA) catalysts were prepared by a coprecipitationpost impregnation method and evaluated in methanol synthesis fromsyngas. The effects of Zr, Ba, and Mn as promoters, the reaction temperature and run time over CZA and Zr-promoted CZA catalysts on catalytic performance were investigated, respectively. The catalysts were characterized by X-ray diffraction (XRD), N₂-sorption, reactive N₂O sorption, X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption of H₂ (H₂-TPD), scanning electron microscopy (SEM), and high-resolution transmittance electron microscopy (HR-TEM). The results showed that the space-time yield (STY) of methanol can be increased noticeably over the Zr-or Ba-promoted CZA catalyst before and after the heating treatment of the catalysts. The introduction of Mn as a promoter onto the CZA catalyst led to a decrease in the STY of methanol before heating treatment. The introduction of Zr as a promoter onto the CZA catalyst can decrease the temperature at which the STY of methanol reached the highest value and also improve the catalytic stability. A hydrogen molecule can be adsorbed and then activated over Cu⁰ and ZnO. The strong interaction between Cu⁰ and ZnO is favorable for improving the catalytic performance of the CZA catalyst. The decrease in catalytic performance after heating treatment of the CZA catalysts is attributed to a growth of Cu⁰ crystallites. Based on the results of catalytic performance and characterization, a possible "bidirectional but synchronous catalytic reaction course" in methanol synthesis from syngas over a CZA catalyst is proposed.

Key words: Promoter, Zirconium, Barium, Cu/ZnO/Al₂O₃ catalyst, Methanol synthesis, Reaction course

HAO Ai-Xiang, YU Yang, CHEN Hai-Bo, MAO Chun-Peng, WEI Shi-Xin, YIN Yu-Sheng. Effect of Surface Promoters-Modifying on Catalytic Performance of Cu/ZnO/Al₂O₃ Methanol Synthesis Catalyst[J]. Acta Phys. -Chim. Sin. 2013, 29(09), 2047-2055. doi: 10.3866/PKU.WHXB201306211

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Effect of Surface Promoters-Modifying on Catalytic Performance of Cu/ZnO/Al₂O₃ Methanol Synthesis Catalyst

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Effect of Surface Promoters-Modifying on Catalytic Performance of Cu/ZnO/Al₂O₃ Methanol Synthesis Catalyst