Al2O3-coated cordierite honeycomb supported CuO catalyst for selective catalytic reduction of NO by NH3: Surface properties and reaction mechanism

被引:20
作者
Liu, Qingya [1 ]
Liu, Zhenyu [1 ]
Su, Junhua [2 ]
机构
[1] Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
[2] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
关键词
CuO/Al2O3-coated cordierite; SCR; Surface acidity; NH3; activation; DRIFTS; ON-ALUMINA CATALYSTS; IN-SITU DRIFTS; FT-IR; AMMONIA ADSORPTION; NITRIC-OXIDE; SCR; OXIDATION; ANATASE; SO2; TEMPERATURE;
D O I
10.1016/j.cattod.2010.04.036
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Al2O3-coated cordierite supported CuO catalyst shows high activities for selective catalytic reduction (SCR) of NO by NH3 at 350-500 degrees C after being sulfated by SO2. Its surface properties and reaction mechanism are elucidated in this paper by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) coupled with mass spectroscopy. Results show that the catalyst has both Lewis and Bronsted acid sites, the Bronsted acidity is far weaker than the Lewis acidity and the protonated ammonia on Bronsted sites is less stable than the coordinated ammonia on Lewis sites. Ammonia coordinated on sulfated CuAl2O4 may transfer to NH2-NH2, where aluminum species is responsible for NH3 storage and copper species is responsible for activation of NH3 to NH2. The SCR reaction involves the adsorbed NH2-NH2 and gaseous NO, following Eley-Rideal mechanism. When NH3 is insufficient, NO may convert to NO2 through oxidation by O-2 or to N2O and NO2 through disproportionation. (C) 2010 Elsevier B. V. All rights reserved.
引用
收藏
页码:370 / 376
页数:7
相关论文
共 27 条
[1]   An FT-IR study of ammonia adsorption and oxidation over anatase-supported metal oxides [J].
Amores, JMG ;
Escribano, VS ;
Ramis, G ;
Busca, G .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 13 (01) :45-58
[2]  
Bosch H., 1988, Catalysis Today, V2, P369, DOI [DOI 10.1016/0920-5861(88)80002-6, 10.1016/B978-0-444-98919-2.50005-3, DOI 10.1016/B978-0-444-98919-2.50005-3]
[4]   In situ DRIFTS study of the SCR reaction of NO with NH3 in the presence of O2 over lanthanide doped V2O5/Al2O3 catalysts [J].
Centeno, MA ;
Carrizosa, I ;
Odriozola, JA .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 19 (01) :67-73
[5]   ADSORPTION AND REACTIVITY OF NO ON COPPER-ON-ALUMINA CATALYSTS .2. ADSORBED SPECIES AND COMPETITIVE PATHWAYS IN THE REACTION OF NO WITH NH3 AND O-2 [J].
CENTI, G ;
PERATHONER, S .
JOURNAL OF CATALYSIS, 1995, 152 (01) :93-102
[6]   ADSORPTION AND REACTIVITY OF NO ON COPPER-ON-ALUMINA CATALYSTS .1. FORMATION OF NITRATE SPECIES AND THEIR INFLUENCE ON REACTIVITY IN NO AND NH3 CONVERSION [J].
CENTI, G ;
PERATHONER, S ;
BIGLINO, D ;
GIAMELLO, E .
JOURNAL OF CATALYSIS, 1995, 152 (01) :75-92
[7]   NATURE OF ACTIVE SPECIES IN COPPER-BASED CATALYSTS AND THEIR CHEMISTRY OF TRANSFORMATION OF NITROGEN-OXIDES [J].
CENTI, G ;
PERATHONER, S .
APPLIED CATALYSIS A-GENERAL, 1995, 132 (02) :179-259
[8]   Present status and perspectives in de-NOx SCR catalysis [J].
Forzatti, P .
APPLIED CATALYSIS A-GENERAL, 2001, 222 (1-2) :221-236
[9]   CHARACTERIZATION OF CU-AL2O3 CATALYSTS [J].
FRIEDMAN, RM ;
FREEMAN, JJ ;
LYTLE, FW .
JOURNAL OF CATALYSIS, 1978, 55 (01) :10-28
[10]  
Huang HZ, 2001, PETROCHEM TECHNOL, V30, P325