物理化学学报 >> 2013, Vol. 29 >> Issue (06): 1289-1296.doi: 10.3866/PKU.WHXB201304162

催化和表面科学 上一篇    下一篇

制备方法对Co-MOR催化剂CH4选择还原NO性能的影响

李滨1,2, 王虹1, 丁福臣1, 李翠清1, 宋永吉1, 柯明2, 任翠涛1   

  1. 1 北京石油化工学院, 北京 102617;
    2 中国石油大学(北京), 北京 102249
  • 收稿日期:2013-02-18 修回日期:2013-04-15 发布日期:2013-05-17
  • 通讯作者: 王虹, 李翠清 E-mail:wanghong@bipt.edu.cn;licuiqing@bipt.edu.cn
  • 基金资助:

    北京市教委科技计划(KM200910017002)和北京市属高等学校人才强教计划(PHR200907129, PHR20110517)资助项目

Effects of Preparation Methods on the Catalytic Performance of Selective Catalytic Reduction of NO with CH4 over Co-MOR Catalysts

LI Bin1,2, WANG Hong1, DING Fu-Chen1, LI Cui-Qing1, SONG Yong-Ji1, KE Ming2, REN Cui-Tao1   

  1. 1 Beijing Institute of Petrochemical Technology, Beijing 102617, P.R.China;
    2 China University of Petroleum, Beijing 102249, P. R. China
  • Received:2013-02-18 Revised:2013-04-15 Published:2013-05-17
  • Supported by:

    The project was supported by the Science and Technology Development of Bejing Education Committee, China (KM200910017002) and Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Municipality, China (PHR200907129, PHR20110517).

摘要:

采用离子交换法、浸渍法制备一系列的Co-MOR 催化剂, 并将其用于CH4选择性催化还原 NOx(CH4-SCR)反应. 运用X 射线衍射(XRD)、X 射线荧光光谱(XRF)、扫描电子显微镜(SEM)、紫外-拉曼(UVRaman)光谱、X射线光电子能谱(XPS)、NO程序升温脱附(NO-TPD)等手段对催化剂进行了表征. 结果表明, 浸渍法制备的催化剂, Co以Co3O4形式存在; 而离子交换法制备的催化剂, Co以离子形式进入丝光沸石(MOR)骨架之中, 在催化剂上形成更多的Co2+和[Co-O-Co]2+, 形成更均匀NO吸附中心和CH4-SCR反应活性中心. 催化剂活性评价表明离子交换法制备的催化剂具有更宽的活性温度区间, Co(0.30)-MOR 催化剂在327-450℃温度范围内NO转化率大于50%.

关键词: Co, 丝光沸石, 离子交换, CH4, NO

Abstract:

A series of Co-mordenite (MOR) catalysts prepared by ion-exchange or impregnation methods were used in the selective catalytic reaction of NO with methane (CH4-SCR). The structure and physicochemical properties of the catalysts were examined by X-ray diffraction (XRD), X-ray fluorescence (XRF), scanning electron microscopy (SEM), UV-Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and temperature-programmed desorption of NO (NO-TPD). The Co species in the catalyst prepared by impregnation is present as Co3O4, whereas in the catalyst prepared by an ion-exchange method, the Co species enter in the mordenite skeleton with the ion form, and the more Co2+ and [Co-O-Co]2+ formed in the catalysts, the more uniform the adsorption of NO centers and the active centers of CH4-SCR. The catalysts prepared by different methods exhibited different activities for CH4-SCR. The catalysts prepared by ion-exchange exhibited activity over a wide activity temperature region, and NO conversion was over 50% at 327-450℃ on the Co(0.30)-MOR catalyst.

Key words: Co, Mordenite, Ion-exchange, CH4, NO

MSC2000: 

  • O643