物理化学学报 >> 2012, Vol. 28 >> Issue (12): 2924-2930.doi: 10.3866/PKU.WHXB201209281

催化和表面科学 上一篇    下一篇

TiO2柱撑海泡石负载Ni2P的噻吩加氢脱硫性能

廖辉1, 徐香兰1, 谌伟庆1, 石秋杰1, 刘文明1, 王翔1,2   

  1. 1 南昌大学化学系, 南昌 330031;
    2 南昌大学应用化学研究所, 南昌 330031
  • 收稿日期:2012-07-18 修回日期:2012-09-18 发布日期:2012-11-14
  • 通讯作者: 王翔 E-mail:xwang23@ncu.edu.cn
  • 基金资助:

    国家自然科学基金(20863006)及南昌大学“赣江”特聘教授启动基金资助项目

Ni2P Catalysts Supported on TiO2-Pillared Sepiolite for Thiophene Hydrodesulfurization

LIAO Hui1, XU Xiang-Lan1, CHEN Wei-Qing1, SHI Qiu-Jie1, LIU Wen-Ming1, WANG Xiang1,2   

  1. 1 Department of Chemistry, Nanchang University, Nanchang 330031, P. R. China;
    2 Institute of Applied Chemistry, Nanchang University, Nanchang 330031, P. R. China
  • Received:2012-07-18 Revised:2012-09-18 Published:2012-11-14
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20863006) and “Ganjiang” Professor Research Funding of Nanchang University, China.

摘要:

以氢氧化镍为镍源, 亚磷酸为磷源, TiO2柱撑海泡石(Ti-Sep)为载体, 采用浸渍法制备了含磷化镍前驱体的样品, 然后采用程序升温还原法制备了Ni质量分数(w)为5%-25%的Ni2P/Ti-Sep催化剂, 并考察了其噻吩加氢脱硫性能. 采用X射线衍射(XRD)、N2吸附-脱附、热重分析(TGA)、透射电子显微镜(TEM)和傅里叶变换红外(FTIR)光谱对催化剂样品进行了表征. 结果表明, 海泡石经TiO2柱撑之后层间距增大, 比表面积和孔容都明显变大, 热稳定性增强, 活性组分Ni2P能很好地分散在海泡石层间及表面, 并且没有破坏海泡石的层状结构. 上述原因导致Ni2P/Ti-Sep催化剂的噻吩加氢脱硫活性明显优于Ni2P/Na-Sep(NaCl改性海泡石)和Ni2P/HCl-Sep(HCl改性海泡石)催化剂. 当Ni负载量为15% (w)时, Ni2P/Ti-Sep催化剂具有最好的噻吩加氢脱硫性能; 在反应温度为400℃时, 噻吩转化率达100%.

关键词: Ni2P, TiO2, 柱撑海泡石, 噻吩, 加氢脱硫

Abstract:

Samples containing a nickel phosphide precursor were synthesized by the impregnation method using TiO2-pillared sepiolite (Ti-Sep) as a support, nickel hydroxide as a nickel source, and phosphorous acid as a phosphorus source. From these precursor samples, Ni2P/Ti-Sep catalysts with Ni content ranging from 5%-25% (w, mass fraction) were prepared by temperature-programmed reduction. Thiophene hydrodesulfurization (HDS) was used to investigate the HDS activity of the catalysts. The catalysts were characterized by X-ray powder diffraction (XRD), N2 adsorption-desorption, thermal gravity analysis (TGA), transmission electron microscope (TEM), and Fourier transform infrared spectroscopy (FTIR). The results demonstrated that the specific surface area and pore volume of Ti-Sep were enlarged and catalyst thermal stability was improved. In addition, the layer spacing of sepiolite was also increased. As a consequence, the active component, Ni2P, can be well dispersed on the interlayer and outer surface of Ti-Sep. Moreover, the layered sepiolite structure remained intact in the Ni2P/Ti-Sep catalysts. Consequently, thiophene conversion on Ni2P/Ti-Sep is improved compared with Ni2P/Na-Sep (NaCl-modified sepiolite) and Ni2P/HCl-Sep (HCl-modified sepiolite), which were prepared on sepiolite without Ti-pillaring. Ni2P/Ti-Sep with a Ni loading of 15% (w) shows the highest activity among all of the studied catalysts, on which the conversion of thiophene can reach 100% at 400℃.

Key words: Ni2P, TiO2, Pillared sepiolite, Thiophene, Hydrodesulfurization