化工学报 ›› 2014, Vol. 65 ›› Issue (3): 921-928.DOI: 10.3969/j.issn.0438-1157.2014.03.022

• 催化、动力学与反应器 • 上一篇    下一篇

超顺磁催化剂H3PW12O40/Fe3O4@SiO2的制备、结构表征及在汽油烷基化脱硫中的应用

熊小龙1, 刘自力1, 许翠霞2, 秦祖赠2   

  1. 1 广州大学化学化工学院, 珠江三角水质安全与保护教育部重点实验室, 广东 广州 510006;
    2 广西大学化学化工学院, 广西 南宁 530004
  • 收稿日期:2013-09-06 修回日期:2013-12-18 出版日期:2014-03-05 发布日期:2014-03-05
  • 通讯作者: 刘自力
  • 作者简介:熊小龙(1989—),男,硕士研究生。
  • 基金资助:

    国家自然科学基金项目(21076047, 21276054)。

Preparation and structure characterization of superparamagnetic supported catalyst H3PW12O40/Fe3O4@SiO2 and its application in olefinic alkylation desulfurization

XIONG Xiaolong1, LIU Zili1, XU Cuixia2, QIN Zuzeng2   

  1. 1 Key Laboratory of Ministry of Education for Water Quality Security and Protection in Pearl River Delta, School of Chemistry & Chemical Engineering, Guangzhou University, Guangzhou 510006, Guangdong, China;
    2 School of Chemistry & Chemical Engineering, Guangxi University, Nanning 530004, Guangxi, China
  • Received:2013-09-06 Revised:2013-12-18 Online:2014-03-05 Published:2014-03-05
  • Supported by:

    supported by the National Natural Science Foundation of China (21076047, 21276054).

摘要: 采用改进Stöber法制备超顺磁Fe3O4@SiO2复合粒子作为催化剂载体,再通过浸渍法将H3PW12O40(HPW)负载在Fe3O4@SiO2载体上,制备了一系列超顺磁负载型催化剂HPW/Fe3O4@SiO2。并使用X射线衍射(XRD)、傅里叶红外(FT-IR)、氨的程序升温脱附(NH3-TPD)、扫描电镜(SEM)、N2吸附-脱附和振动样品强磁计(VSM)对催化剂进行表征。结果表明,HPW固定并均匀分散在Fe3O4@SiO2载体上,40% HPW/Fe3O4@SiO2催化剂具有较高的饱和磁强度 (30.1 emu·g-1)和较大的比表面积 (303.6 m2·g-1),并可用外加磁场进行分离。采用40% HPW/Fe3O4@SiO2催化噻吩与1-辛烯组成的模拟汽油的烷基化脱硫反应,在160℃下反应2 h,噻吩转化率达到85.5%,有较好的催化脱硫性能,且可以多次循环利用。

关键词: 超顺磁性, 烷基化, 磷钨酸, 催化剂, 复合材料, 二氧化硅

Abstract: Fe3O4@SiO2 nanocomposite was prepared via modified Stöber method and used as catalyst support. Superparamagnetic supported catalystsprepared by loading H3PW12O40 (HPW) onto Fe3O4@SiO2 support through a wet impregnation method, were used for alkylation reaction, and characterized by X-ray diffraction (XRD), Fourier transform infrared (FT-IR), NH3-temperature programmed desorption (TPD), scanning electron microscope (SEM), N2-adsorption and vibrating sample magnetometer (VSM). Their physicochemical characterization revealed that HPW had been immobilized and dispersed on Fe3O4@SiO2. Moreover, 40%(mass) HPW loading catalyst, been of high magnetization 30.1 emu·g-1, mesoporous structure and the surface area 303.6 m2·g-1, could be considered to be a proper catalyst for olefinic alkylation of thiophenic sulfur (OATS) and they can be easy separated by external magnetic field. In addition, their catalytic activity was also investigated in alkylation reaction of a model mixture of thiophene and 1-octene, and the conversion of thiophene was up to 85.5% after 2 h at 160℃.

Key words: superparamagetism, alkylation, phosphotungstic acid, catalyst, composites, silica

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