催化学报 ›› 2008, Vol. 29 ›› Issue (2): 167-173.

• 研究论文 • 上一篇    下一篇

不同放大级Fe/Cu/K/SiO2催化剂的表征及其浆态床费托合成反应性能

侯文娟1,2,吴宝山1,白亮1,相宏伟1,李永旺1   

  1. 1 中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西太原 030001; 2 中国科学院研究生院, 北京 100049
  • 收稿日期:2008-02-25 出版日期:2008-02-25 发布日期:2012-01-15

Characterization and Slurry Fischer-Tropsch Synthesis Performance of Fe/Cu/K/SiO2 Catalysts with Different Scaled Up Levels

HOU Wenjuan1,2, WU Baoshan1*, BAI Liang1, XIANG Hongwei1, LI Yongwang1   

  1. 1 State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, The Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China; 2 Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2008-02-25 Online:2008-02-25 Published:2012-01-15

摘要: 采用连续共沉淀和喷雾干燥成型相结合的方法,制备了实验室级和放大级微球状费托(FT)合成Fe/Cu/K/SiO2催化剂. 实验室级催化剂的颗粒尺寸为5~15 μm, 放大级催化剂的颗粒尺寸为40~60 μm. 利用低温N2物理吸附、H2程序升温还原、CO2程序升温脱附、穆斯堡尔谱和X射线衍射等表征手段考察了催化剂的织构性质、还原行为、碳化行为及物相变化. 结果表明,与实验室级催化剂相比,放大级催化剂具有较大的晶粒尺寸和孔径、较小的比表面积和较弱的表面碱性,催化剂的还原和碳化受到抑制. 浆态床FT合成反应及扫描电子显微镜结果表明,放大级催化剂经诱导期达到稳定状态后,转化率可达到实验室级催化剂的水平,且具有很高的稳定性、重质烃选择性及抗磨损性.

关键词: 费托合成, 浆态床, 铁/铜/钾/二氧化硅催化剂

Abstract: Two spherical Fe/Cu/K/SiO2 catalysts with different preparation scale for slurry Fischer-Tropsch (FT) synthesis were prepared by a combination of co-precipitated and spray drying method. The pellet size of the catalyst with a laboratory scale is 5-15μm, whereas that is 40-60μm for the scaled-up catalyst. N2 physical adsorption, H2 temperature-programmed reduction, CO2 temperature-programmed desorption, Mössbauer spectroscopy, and X-ray diffraction were used to characterize the textural properties, reduction and carburization behavior, and phase transformation of the two catalysts. The results show that the scaled-up catalyst has larger crystallize size and pore volume, lower BET surface area, and lower surface basicity than the laboratory-scale catalyst. Moreover, the scaled-up catalyst was more difficult to be reduced and carburized. However, the results of FT synthesis in a slurry bed indicate that the scaled-up catalyst exhibits comparative activity, better reaction stability, and higher selectivity for olefin and heavy hydrocarbons. Scanning electron microscopy results suggest a better attrition resistance of the scaled-up catalyst during the FT reaction tests.

Key words: Fischer-Tropsch synthesis, slurry bed, Fe/Cu/K/SiO2 catalyst