Mo-Ni2P/SBA-15催化剂的制备、表征及加氢脱硫催化性能

doi:10.3866/PKU.WHXB201501094

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

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. 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-Yi^1,2, LAN Ling², LIU Kun-Hong², HU Ya-Qiong², JI Sheng-Fu¹

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/Abstract

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Ni^δ+和Ni²⁺形式存在; P以P^δ-和P⁵⁺形式存在; Mo以Mo^δ+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 Ni^δ+ and Ni²⁺, the chemical states of P were P^δ- and P⁵⁺, and the chemical states of Mo were Mo^δ+ 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

王周君, 吴平易, 兰玲, 刘坤红, 胡亚琼, 季生福. Mo-Ni₂P/SBA-15催化剂的制备、表征及加氢脱硫催化性能[J]. 物理化学学报, 2015, 31(3), 533-539. doi: 10.3866/PKU.WHXB201501094

WANG Zhou-Jun, WU Ping-Yi, LAN Ling, LIU Kun-Hong, HU Ya-Qiong, JI Sheng-Fu. Preparation, Characterization and Hydrodesulfurization Catalytic Performances of Mo-Ni₂P/SBA-15 Catalysts[J]. Acta Phys. -Chim. Sin. 2015, 31(3), 533-539. doi: 10.3866/PKU.WHXB201501094

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201501094

https://www.whxb.pku.edu.cn/CN/Y2015/V31/I3/533

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Mo-Ni₂P/SBA-15催化剂的制备、表征及加氢脱硫催化性能

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

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