物理化学学报 >> 2015, Vol. 31 >> Issue (3): 533-539.doi: 10.3866/PKU.WHXB201501094

催化和表面科学 上一篇    下一篇

Mo-Ni2P/SBA-15催化剂的制备、表征及加氢脱硫催化性能

王周君1, 吴平易1,2, 兰玲2, 刘坤红2, 胡亚琼2, 季生福1   

  1. 1. 北京化工大学, 化工资源有效利用国家重点实验室, 北京 100029;
    2. 中国石油石油化工研究院, 北京 100195
  • 收稿日期:2014-10-31 修回日期:2015-01-07 发布日期:2015-03-06
  • 通讯作者: 季生福 E-mail:jisf@mail.buct.edu.cn
  • 基金资助:

    国家重点基础研究发展规划项目(973) (2006CB202503)及中国石油科技创新基金(2010D-5006-0401)资助

Preparation, Characterization and Hydrodesulfurization Catalytic Performances of Mo-Ni2P/SBA-15 Catalysts

WANG Zhou-Jun1, WU Ping-Yi1,2, LAN Ling2, LIU Kun-Hong2, HU Ya-Qiong2, JI Sheng-Fu1   

  1. 1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China;
    2. Petrochemical Research Institute, PetroChina, Beijing 100195, P. R. China
  • Received:2014-10-31 Revised:2015-01-07 Published:2015-03-06
  • Contact: JI Sheng-Fu E-mail:jisf@mail.buct.edu.cn
  • Supported by:

    The project was supported by the National Key Basic Research Program of China (973) (2006CB202503) and PetroChina Innovation Foundation, China (2010D-5006-0401).

摘要:

以介孔分子筛SBA-15 为载体, 通过分步浸渍硝酸镍、磷酸氢二铵、钼酸铵, 然后在H2气流下程序升温还原(H2-TPR), 制备了一系列不同Mo 含量的Mo-Ni2P/SBA-15 催化剂. 采用X 射线衍射(XRD)、氮气吸脱附(BET)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)对催化剂的结构进行了表征, 评价了催化剂对二苯并噻吩(DBT)的加氢脱硫(HDS)活性. 结果表明, Mo-Ni2P/SBA-15 催化剂仍然保留有介孔结构, 催化剂的物相主要是Ni2P. 催化剂表面的Ni 以Niδ+和Ni2+形式存在; P以Pδ-和P5+形式存在; Mo以Moδ+和Mo6+形式存在. Mo能促进催化性能的提高, 其中Mo含量为1% (w, 质量分数)的Mo-Ni2P/SBA-15 催化剂具有最好的二苯并噻吩加氢脱硫催化活性, 在反应温度为380 ℃, 反应压力为3.0 MPa的条件下, 二苯并噻吩的转化率可达99.03%, 所有考察的Mo-Ni2P/SBA-15都以直接加氢脱硫(DDS)途径为主.

关键词: Mo, Ni2P, 二苯并噻吩, 加氢脱硫, 介孔

Abstract:

A series of Mo-Ni2P/SBA-15 catalysts with various Mo loadings were prepared by impregnating nickel nitrate, diammonium hydrogen phosphate, and ammonium molybdate onto an SBA-15 support, followed by temperature-programmed reduction (TPR) under H2. The structure of the catalysts was characterized by Xray diffraction (XRD), N2 adsorption-desorption, transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The catalytic performance was evaluated in the hydrodesulfurization (HDS) of dibenzothiophene (DBT). The results indicate that the mesoporous structure was maintained and the Ni2P phase was present in all of the catalysts. The chemical states of Ni were Niδ+ and Ni2+, the chemical states of P were Pδ- and P5+, and the chemical states of Mo were Moδ+ and Mo6+. Mo was shown to promote the HDS catalytic performance of Ni2P/SBA-15 catalysts. The Mo-Ni2P/SBA-15 catalysts with 1% (w, mass fraction) Mo loading exhibited the highest HDS activity. The conversion of the DBT reached 99.03%under reaction conditions of 380 ℃ and 3.0 MPa. The HDS of DBT proceeded mainly via the direct desulfurization (DDS) pathway over all of the tested Mo-Ni2P/SBA-15 catalysts.

Key words: Mo, Ni2P, Dibenzothiophene, Hydrodesulfurization, Mesoporous

MSC2000: 

  • O643