Acta Chim. Sinica ›› 2017, Vol. 75 ›› Issue (5): 479-484.DOI: 10.6023/A17010031 Previous Articles     Next Articles

Article

Pd/ZSM-5/MCM-41催化剂加氢脱硫性能研究

杨晓东a, 王新苗a, 高善彬a,b, 王安杰c   

  1. a. 中国石油石油化工研究院 大庆 163714;
    b. 中国石油大学理学院重质油加工国家重点实验室 北京 102249;
    c. 大连理工大学精细化工国家重点实验室 大连 116012
  • 收稿日期:2017-01-20 出版日期:2017-05-15 发布日期:2017-02-23
  • 通讯作者: 杨晓东 E-mail:xiaodongyang1983@126.com
  • 基金资助:

    项目受中国石油天然气股份公司基金项目(Nos.2013E-1502,2014B-2508)资助.

Hydrodesulfurization Performances of Pd Catalysts Supported on ZSM-5/MCM-41 Composite Zeolite

Yang Xiaodonga, Wang Xinmiaoa, Gao Shanbina,b, Wang Anjiec   

  1. a. Petrochemical Research Institute, CNPC, Daqing 163714, China;
    b. College of Science, State Key Laboratory of Heavy Oil Processing, China University of Petroleum Beijing, Beijing 102249, China;
    c. State Key Laboratory of Fine Chemical, Dalian University of Technology, Dalian 116012, China
  • Received:2017-01-20 Online:2017-05-15 Published:2017-02-23
  • Contact: 10.6023/A17010031 E-mail:xiaodongyang1983@126.com
  • Supported by:

    Project supported by the China National Petroleum Corporation Fund (Nos. 2013E-1502, 2014B-2508).

Siliceous MCM-41 (Si-MCM-41), two micro-mesoporous materials obtained either by physically mixing Si-MCM-41 with HZSM-5 zeolite (Z-MCM-41-M) or by coating Si-MCM-41 over HZSM-5 zeolite particles (Z-MCM-41), were prepared and characterized by means of XRD, N2 adsorption-desorption, pyridine adsorbed FT-IR. The hydrodesulfurization (HDS) performances of the supported Pd catalysts thereof, were evaluated with dibenzothiophene (DBT) as the model sulfur-containing molecule. The close relationship between the surface area of the support and the HDS performance for the supported Pd catalysts was not observed. The result indicated that the surface area of the support or the dispersion of the catalyst might not be the key parameter affecting the HDS performance of the supported Pd catalyst. However, the HDS performances of Pd catalysts were significantly influenced by the pore structures and acid properties of the supports. Pd catalysts supported on the acidic supports showed the enhancement of HDS and hydrogenation activities that was thought to be the effect of hydrogen spillover. Among the catalysts studied, Pd/Z-MCM-41 exhibited the highest HDS activity and excellent hydrogenation activities. The results demonstrated that mesoporous materials introducing to microporous zeolite was beneficial to the improvement of HDS activities, but only physically mixing Si-MCM-41 with HZSM-5 zeolite couldn't show the combination advantage of pore of mesoporous materials and acid properties of microporous zeolite, and further generate better synergistic catalytic action. Z-MCM-41 composite material with the regular structure and uniform distribution acidity was potential carriers for precious metal catalysts.

Key words: MCM-41, ZSM-5, composite zeolite, Pd, hydrodesulfurization