物理化学学报 >> 2010, Vol. 26 >> Issue (12): 3285-3290.doi: 10.3866/PKU.WHXB20101137

催化和表面结构 上一篇    下一篇

CuxCo1-x/Al2O3/FeCrAl整体式催化剂上甲苯催化燃烧

赵福真1, 曾鹏辉1,2, 季生福1, 杨肖1, 李成岳1   

  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. 中国石油大学(北京)重质油国家重点实验室, 北京102200
  • 收稿日期:2010-06-09 修回日期:2010-07-29 发布日期:2010-12-01
  • 通讯作者: 季生福 E-mail:jisf@mail.buct.edu.cn
  • 基金资助:

    国家自然科学基金(20473009)资助项目

Catalytic Combustion of Toluene over CuxCo1?x/Al2O3/FeCrAl Monolithic Catalysts

ZHAO Fu-Zhen1, ZENG Peng-Hui1,2, JI Sheng-Fu1, YANG Xiao1, LI Cheng-Yue1   

  1. 1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China;
    2. State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102200, P. R. China
  • Received:2010-06-09 Revised:2010-07-29 Published:2010-12-01
  • Contact: JI Sheng-Fu E-mail:jisf@mail.buct.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20473009).

摘要:

以FeCrAl 合金薄片为基底, Al2O3浆料为过渡胶体, 不同摩尔比的Cu、Co为催化活性组分, 制备了一系列CuxCo1-x/Al2O3/FeCrAl(x=0-1)新型整体式催化剂. 采用X射线粉末衍射(XRD), 扫描电子显微镜(SEM), X光电子能谱(XPS)和程序升温还原(TPR)等手段对催化剂的结构进行了表征. 在微型固定床反应器上评价了催化剂的催化甲苯燃烧性能. 研究结果表明: 在所制备的整体式催化剂上, 当Cu含量比较低时, 形成了Cu-Co-O固溶体; 当Cu含量比较高时, 可以测得CuO的衍射峰. 催化剂表面颗粒大小和形貌与Cu、Co摩尔比密切相关.在催化剂表面, Co以Co2+和Co3+价态存在, 而Cu主要以Cu2+价态存在. 催化剂中的Cu可以改善Co的氧化还原性, 从而有利于催化剂活性的提高. 在所制备的催化剂中, Cu0.5Co0.5/Al2O3/FeCrAl 催化剂具有最好的活性, 甲苯在374 oC可以完全催化燃烧消除.

关键词: FeCrAl, 整体式催化剂, 甲苯催化燃烧, X射线粉末衍射, X光电子能谱

Abstract:

A series of CuxCo1-x/Al2O3/FeCrAl (x=0-1) catalysts were prepared using an FeCrAl alloy as support, a boehmite primer sol as the first washcoat layer and copper as well as cobalt oxides as the active washcoat layer. The structure of the catalysts was characterized using X-ray powder diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS) and temperatureprogrammed reduction (TPR). Toluene was chosen as the model compound to evaluate the catalytic activity in a conventional fixed-bed quartz reactor. Results indicate that a Cu-Co-O solid solution phase was present when the content of Cu in the catalysts was low and a CuO phase was present when the content of Cu was high. Both Co2+ and Co3+ were present on the surface of the obtained monolithic catalysts while Cu2+ was the main Cu species. The addition of a proper amount of copper oxide improved the reducibility of the cobalt oxide, which enhanced the catalytic activity of the catalysts. All the obtained catalysts showed good activity for the catalytic combustion of toluene. The Cu0.5Co0.5/Al2O3/FeCrAl catalyst had the best catalytic activity, and toluene was totally oxidized at 374 °C over it.

Key words: FeCrAl, Monolithic catalyst, Toluene catalytic combustion, X-ray powder diffraction, X-ray photoelectron spectroscopy

MSC2000: 

  • O643