催化学报

催化学报 ›› 2014, Vol. 35 ›› Issue (4): 546-552.DOI: 10.1016/S1872-2067(14)60028-0

• 研究论文 • 上一篇    下一篇

有机改性对粘土负载镍催化剂的促进作用及其萘加氢性能

任世彪, 文宏志, 曹先中, 王知彩, 雷智平, 潘春秀, 康士刚, 水恒福   

  1. 安徽工业大学化学与化工学院, 安徽省煤洁净转化与利用重点实验室, 安徽马鞍山243002
  • 收稿日期:2013-12-07 修回日期:2014-01-07 出版日期:2014-03-20 发布日期:2014-03-21
  • 通讯作者: 任世彪，水恒福
  • 基金资助:

    国家自然科学基金委员会-神华集团有限公司煤炭联合基金（U1361125，U1261208）；国家自然科学基金（21176001，51174254）；煤资源的加工转化与洁净利用安徽省创新团队项目；煤洁净转化及其催化技术安徽工业大学创新团队项目.

Promotion of Ni/clay catalytic activity for hydrogenation of naphthalene by organic modification of clay

Shibiao Ren, Hongzhi Wen, Xianzhong Cao, Zhicai Wang, Zhiping Lei, Chunxiu Pan, Shigang Kang, Hengfu Shui   

  1. Anhui Key Laboratory of Clean Coal Conversion and Utilization, School of Chemistry and Chemical Engineering, Anhui University of Technology, Ma'anshan 243002, Anhui, China
  • Received:2013-12-07 Revised:2014-01-07 Online:2014-03-20 Published:2014-03-21
  • Supported by:

    This work was supported by the Project of Coal Joint Fund from Natural Science Foundation of China and Shenhua Group Corporation Limited (U1361125, U1261208), the Natural Scientific Foundation of China (21176001,51174254), the Provincial Innovative Group for Processing & Clean Utilization of Coal Resource, and Innovative Research Team in Anhui University of Technology.

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675

被引次数

14

摘要：

以有机改性后的十六烷基三甲基溴化铵柱撑蒙脱石（CTAB-MMT）为载体，采用浸渍法制备了Ni/MMT催化剂. 通过傅里叶红外光谱、X射线衍射、H2程序升温脱附、N2物理吸附以及紫外漫散射等物理化学手段对催化剂进行了表征；并结合微型高压反应釜萘加氢反应，评价了催化剂的加氢性能. 结果表明，有机改性显著改善了Ni/MMT催化剂的金属Ni分散度和织构性质，且所制催化剂表现出优异的萘加氢性能，Ni萘转化率达到88.2%，不仅远高于未处理催化剂（13.1%）和Al2O3柱撑处理催化剂（24.2%），而且高于Ni/SBA-15催化剂（68.2%）. 鉴于CTAB有机柱撑体在催化剂还原过程因热解而消除，其对催化剂所起的作用主要发生于浸渍过程，提出了有机改性在浸渍过程对Ni/MMT催化剂的促进作用机制.

关键词: 镍, 有机蒙脱石, 高活性, 萘, 加氢

Abstract:

A Ni/montmorillonite (MMT) catalyst was prepared by an impregnation method using cetyltrimethylammonium bromide (CTAB)-pillared MMT as the supporting matrix and was characterized using infrared spectroscopy, X-ray diffraction, H2 temperature-programmed desorption, N2 adsorption-desorption, and ultraviolet diffuse reflectance spectroscopy. The catalytic activity of the Ni/MMT for the hydrogenation of naphthalene was also evaluated. The results show that the organic modification of MMT greatly improved the Ni dispersion and textural properties of the Ni/MMT catalyst. The as-prepared Ni/MMT catalyst showed high naphthalene conversion (88.2%) in the hydrogenation reaction; this is much higher than those achieved using Ni supported on pristine MMT (13.1%), Al2O3-pillared MMT (24.2%), and SBA-15 (68.2%). As a result of thermal decomposition of CTAB pillars during reduction of the Ni/MMT catalyst, the CTAB pillars mainly play a role in the Ni/MMT catalyst during impregnation. A mechanism for the promotion of the Ni/MMT catalytic activity by organic modification during impregnation is proposed.

Key words: Nickel, Organic montmorillonite, High activity, Naphthalene, Hydrogenation