Simultaneous removal of SO2 and NOx from flue gas using a CuO/Al2O3 catalyst sorbent II.: Promotion of SCR activity by SO2 at high temperatures

被引:138
作者
Xie, GY [1 ]
Liu, ZY [1 ]
Zhu, ZP [1 ]
Liu, QY [1 ]
Ge, J [1 ]
Huang, ZG [1 ]
机构
[1] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China
基金
中国国家自然科学基金;
关键词
SO2; promoting effect; NOx; selective catalytic reduction (SCR); ammonia oxidation; CuO/Al2O3;
D O I
10.1016/j.jcat.2004.02.016
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Promoting effect Of SO2 on selective catalytic reduction (SCR) of NO by NH3 over a CuO/Al2O3 catalyst sorbent has been investigated. Transient experiment, X-ray photoelectron spectroscopy (XPS), in situ DRIFT, NH3-TPD, and temperature-programmed reduction (TPR) were used to evaluate the promoting mechanism. The results show that the presence Of SO2 in the reaction stream can significantly promote catalytic activity of NO reduction at temperatures above 300 degreesC due to the formation of sulfate species on the catalyst surface. Sulfate species affect SCR activity by changing the acidity and redox property of the catalyst sorbent. In situ DRIFT shows that only ammonia coordinated on Lewis acid sites is found on the CuO/Al2O3 catalyst sorbent. Sulfation of CuO/Al2O3 catalyst sorbent greatly increases the concentration and strength of Lewis acid sites and the concentration of Bronsted acid sites. However, the ammonia bound to Bronsted acid sites does not play an important role in the SCR reaction in the catalyst system. Moreover, there is a close relationship between the SCR activity and ammonia oxidation activity. Ammonia oxidation experiments and TPR in H-2 suggest that sulfation of the catalyst sorbent weakens the catalyst's oxidation ability and inhibits NH3 oxidation to NO in the process of SCR, which may be another main promoting effect Of SO2 on SCR. (C) 2004 Elsevier Inc. All rights reserved.
引用
收藏
页码:42 / 49
页数:8
相关论文
共 26 条
[11]   Removal of NOx and SO2 by CuO/γ-Al2O3 sorbent/catalyst in a fluidized-bed reactor [J].
Jeong, SM ;
Kim, SD .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2000, 39 (06) :1911-1916
[12]   Selective catalytic reduction of NO by NH3 over a bulk sulfated CuO/γ-Al2O3 catalyst [J].
Jeong, SM ;
Jung, SH ;
Yoo, KS ;
Kim, SD .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1999, 38 (06) :2210-2215
[13]   Characterization of Fe-ZSM-5 catalyst for selective catalytic reduction of nitric oxide by ammonia [J].
Long, RQ ;
Yang, RT .
JOURNAL OF CATALYSIS, 2000, 194 (01) :80-90
[14]   Selective catalytic reduction of nitrogen oxides by ammonia over Fe3+-exchanged TiO2-pillared clay catalysts [J].
Long, RQ ;
Yang, RT .
JOURNAL OF CATALYSIS, 1999, 186 (02) :254-268
[15]   Enhancement of activities by sulfation on Fe-exchanged TiI2-pillared clay for selective catalytic reduction of NO by ammonia [J].
Long, RQ ;
Chang, MT ;
Yang, RT .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2001, 33 (02) :97-107
[16]   INFRARED STUDIES OF THE SURFACE OF ALPHA-FE2O3 [J].
LORENZELLI, V ;
BUSCA, G .
MATERIALS CHEMISTRY AND PHYSICS, 1985, 13 (3-4) :261-281
[17]   Testing of the CuO/Al2O3 catalyst-sorbent in extended operation for the simultaneous removal of NOx and SO2 from flue gases [J].
Macken, C ;
Hodnett, BK ;
Paparatto, G .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2000, 39 (10) :3868-3874
[18]   The catalytic activity of CuSO4/ZrO2 for the selective catalytic reduction of NOx with NH3 in the presence of excess O2 [J].
Pietrogiacomi, D ;
Sannino, D ;
Magliano, A ;
Ciambelli, P ;
Tuti, S ;
Indovina, V .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2002, 36 (03) :217-230
[19]   AMMONIA ADSORPTION ON VANADIA SUPPORTED ON TITANIA-SILICA CATALYST - AN INFRARED SPECTROSCOPIC INVESTIGATION [J].
RAJADHYAKSHA, RA ;
KNOZINGER, H .
APPLIED CATALYSIS, 1989, 51 (01) :81-92
[20]   Adsorption, activation, and oxidation of ammonia over SCR catalysts [J].
Ramis, G ;
Yi, L ;
Busca, G ;
Turco, M ;
Kotur, E ;
Willey, RJ .
JOURNAL OF CATALYSIS, 1995, 157 (02) :523-535