物理化学学报 >> 2010, Vol. 26 >> Issue (09): 2461-2467.doi: 10.3866/PKU.WHXB20100937

催化和表面结构 上一篇    下一篇

Ni2P/TiO2-Al2O3催化剂的制备及其加氢脱硫、脱氮性能

宋华, 郭云涛, 李锋, 于洪坤   

  1. 东北石油大学化学化工学院,石油与天然气化工省重点实验室,黑龙江 大庆 163318
  • 收稿日期:2010-03-30 修回日期:2010-05-22 发布日期:2010-09-02
  • 基金资助:

    黑龙江省科技厅(2009G0947-00)资助项目

Preparation, Hydrodesulfurization and Hydrodenitrogenation Performance of a Ni2P/TiO2-Al2O3 Catalyst

SONG Hua, GUO Yun-Tao, LI Feng, YU Hong-Kun   

  1. Provincial Key Laboratory of Oil and Gas Chemical Technology, College of Chemistry and Chemical Engineering,Northeast Petroleum University, Daqing 163318, Heilongjiang Province, P. R. China
  • Received:2010-03-30 Revised:2010-05-22 Published:2010-09-02
  • Supported by:

    The project was supported by the Heilongjiang Science and Technology Agency, China (2009G0947-00).

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摘要：

采用溶胶-凝胶法制备了TiO2-Al2O3复合载体, 采用浸渍法制备了Ni2P/TiO2-Al2O3催化剂, 并用X 射线 衍射(XRD)、N2吸附比表面积(BET)测定、热重-差热分析(TG-DTA)、X 射线光电子能谱(XPS)等技术对催化剂的 结构和性质进行了表征. 催化剂加氢脱硫(HDS)和脱氮(HDN)活性评价在实验室固定床连续反应装置上, 以噻吩 和吡啶为模型反应物进行. 考察了不同载体、Ni2P 负载量、标称Ni/P 摩尔比、催化剂焙烧温度对Ni2P/TiO2-Al2O3 催化剂上同时进行的噻吩加氢脱硫和吡啶加氢脱氮性能的影响. 结果表明, TiO2含量为80%(w)的TiO2-Al2O3复 合氧化物为载体, Ni2P负载量为30.0%(w), 标称Ni/P 摩尔比为1/2, 催化剂焙烧温度为500oC时, TiO2-Al2O3 催化剂加氢脱硫脱氮活性最高. 在360oC, 3.0 MPa, 氢油比800(V/V), 液时体积空速1.5 h-1 的条件下, 噻吩HDS 和吡啶HDN 转化率分别为61.32%和64.43%.

关键词: 磷化二镍, 二氧化钛, 三氧化二铝, 加氢脱硫, 加氢脱氮

Abstract:

We prepared a TiO2-Al2O3 complex support by the sol-gel method. A nickel phosphide catalyst, Ni2P/ TiO2-Al2O3, was prepared by the impregnation method. The catalysts were characterized by X-ray diffraction (XRD), N2-adsorption specific surface area measurements (BET), thermogravimetry-differential thermal analysis (TG-DTA), and X-ray photoelectron spectroscopy (XPS). The catalysts were evaluated using a lab-scale continuous flow fixed-bed reactor for simultaneously hydrodesulfurization (HDS) and hydrodenitrogenation (HDN) of thiophene and pyridine. The effects of different supports, Ni2P loading, Ni/P molar ratio, and calcination temperature on catalyst activity for the HDS and HDN were studied. The catalytic activity of the Ni2P/TiO2-Al2O3 catalyst with a TiO2 mass fraction of 80%, a Ni2P loading of 30.0%(w), a Ni/P molar ratio of 1/2 as well as a calcination temperature of 500oCwas found to be optimal. At a reaction temperature of 360 o, a pressure of 3.0 MPa, a hydrogen/oil ratio of 800 (V/V), and a liquid hourly space velocity of 1.5 h-1, the conversion of thiophene HDS and pyridine HDN were 61.32%and 64.43%, respectively.

Key words: Nickel phosphide, Titaniumdioxide, Aluminiumtrioxide, Hydrodesulfurization, Hydrodenitrogenation