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以拟薄水铝石为铝源制备浆态床二甲醚合成催化剂

高志华, 黄伟, 李俊芳, 阴丽华, 谢克昌   

  1. 太原理工大学煤科学与技术教育部和山西省重点实验室, 太原 030024
  • 收稿日期:2008-07-04 修回日期:1900-01-01 出版日期:2009-03-10 发布日期:2009-03-10
  • 通讯作者: 黄伟

Liquid-phase Preparation of DME Slurry Catalysts Using Pseudo-boehmite as Aluminum Source

GAO Zhi-Hua, HUANG Wei*, LI Jun-Fang, YIN Li-Hua, XIE Ke-Chang
  

  1. Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
  • Received:2008-07-04 Revised:1900-01-01 Online:2009-03-10 Published:2009-03-10
  • Contact: HUANG Wei

摘要: 利用完全液相法, 以拟薄水铝石(AlOOH)为铝源制备了CuZnAl浆状催化剂, 并通过添加不同的干燥控制化学添加剂(DCCA)对催化剂前驱体进行了修饰, 采用X射线粉末衍射、氮气吸附、X射线光电子能谱和程序升温还原对其进行了表征, 考察了CuZnAl浆状催化剂在一步法合成二甲醚反应中的催化性能. 实验结果表明, 以AlOOH为铝源, 所得样品的Cu和Al间相互作用较强, 生成了CuAl2O4相, 从而减少了催化剂中可还原Cu2O的数量, 降低催化活性. 添加不同DCCA对催化剂性能有显著的影响, 其中加入丙三醇增加了催化剂的比表面积和平均孔径, 改善了催化剂组分的分散性, 抑制了CuAl2O4的形成, 提高了催化剂中的可还原Cu2O量, 从而显著提高了催化剂的二甲醚时空收率和选择性.

关键词: 完全液相法, 拟薄水铝石, 二甲醚, 干燥控制化学添加剂, 浆状催化剂

Abstract: Al-based slurry catalysts using pseudo-boehmite as aluminum source were prepared by a complete liquid-phase technology and the catalyst precursors were modified by different drying control chemical additives(DCCAs). The catalysts were characterized by means of X-ray diffraction, N2 adsorption, X-ray photoelectron spectroscopy and H2 temperature-programmed reduction. The performance of the catalysts was evaluated in a slurry reactor for the synthesis of dimethyl ether(DME) from syngas. The results indicate that using pseudo-boehmite as aluminum source there takes place a strong interaction between copper and aluminum, which induce the formation of CuAl2O4 and decrease the amount of reducible Cu2O. Consequently, the catalyst activity is decreased. Further study shows that the DCCA influences significantly on catalyst's property. When the catalyst precursors are modified by glycerol as DCCA, the catalysts surface area and mean pore size are increased. The active component of the catalyst is dispersed uniformly and the formation of CuAl2O4 is suppressed, meanwhile, the reducible Cu2O is increased. Therefore, the catalyst shows the highest space time yield and selectivity of dimethyl ether.

Key words: Complete liquid-phase technology, Pseudo-boehmite, Dimethyl ether, Drying control chemical additive(DCCA), Slurry catalyst

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