Kinetics of selective catalytic reduction of NO with NH3 on Fe-ZSM-5 catalyst

被引:127
作者
Huang, HY [1 ]
Long, RQ [1 ]
Yang, RT [1 ]
机构
[1] Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA
基金
美国国家科学基金会;
关键词
Fe-exchanged ZSM-5; selective catalytic reduction; SCR of NO with ammonia; kinetics; activation energy;
D O I
10.1016/S0926-860X(02)00268-5
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
Fe-exchanged ZSM-5 has been found previously to be much more active than commercial vanadia-based catalysts for selective catalytic reduction (SCR) of NO with NH3. The kinetics of the SCR reaction is studied in this work. The results show that the rate of NO conversion on Fe-ZSM-5 is first-order with respect to NO, zeroth-order w.r.t. NH3 and nearly half-order w.r.t. O-2, at 260-300degreesC. This is in good agreement with our previous FTIR result that the catalyst surface is nearly completely covered by ammonia adsorbed species (i.e. NH4+ ions) under reaction conditions. The present results further support that the SCR mechanism on Fe-ZSM-5 involves NO2 as an intermediate and the formation of NO2 from NO oxidation (NO + (1 /2)O-2 --> NO2) is probably the rate-determining step. The apparent activation energy for the reaction is found to be 54 kJ/mol. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:241 / 251
页数:11
相关论文
共 34 条
[1]   KINETIC AND INFRARED SPECTROSCOPIC STUDIES OF FE-Y ZEOLITES FOR THE SELECTIVE CATALYTIC REDUCTION OF NITRIC-OXIDE BY AMMONIA [J].
AMIRIDIS, MD ;
PUGLISI, F ;
DUMESIC, JA ;
MILLMAN, WS ;
TOPSOE, NY .
JOURNAL OF CATALYSIS, 1993, 142 (02) :572-584
[2]  
Bosch H., 1986, CATAL TODAY, V2, P369, DOI DOI 10.1016/0920-5861(88)80002-6
[3]  
Brandin JGM, 1989, CATAL TODAY, V4, P187
[4]   Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts:: A review [J].
Busca, G ;
Lietti, L ;
Ramis, G ;
Berti, F .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 18 (1-2) :1-36
[5]   SELECTIVE CATALYTIC REDUCTION OF NO(X) USING ZEOLITIC CATALYSTS FOR HIGH-TEMPERATURE APPLICATIONS [J].
BYRNE, JW ;
CHEN, JM ;
SPERONELLO, BK .
CATALYSIS TODAY, 1992, 13 (01) :33-42
[6]   MICRODYNAMICS OF METHANE, ETHANE AND PROPANE IN ZSM-5-TYPE ZEOLITES [J].
CARO, J ;
BULOW, M ;
SCHIRMER, W ;
KARGER, J ;
HEINK, W ;
PFEIFER, H ;
ZDANOV, SP .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1985, 81 :2541-2550
[7]   Activity and durability of Fe/ZSM-5 catalysts for lean burn NOx reduction in the presence of water vapor [J].
Chen, HY ;
Sachtler, WMH .
CATALYSIS TODAY, 1998, 42 (1-2) :73-83
[8]   TPD study of mordenite-type zeolites for selective catalytic reduction of NO by NH3 [J].
Choi, EY ;
Nam, IS ;
Kim, YG .
JOURNAL OF CATALYSIS, 1996, 161 (02) :597-604
[9]   Kinetic and mechanistic study of NOx reduction by NH3 over H-form zeolites .1. Kinetic and mechanistic insights into NO reduction over H-ZSM-5 [J].
Eng, J ;
Bartholomew, CH .
JOURNAL OF CATALYSIS, 1997, 171 (01) :14-26
[10]  
Forzatti P, 1996, HETEROGEN CHEM REV, V3, P33, DOI 10.1002/(SICI)1234-985X(199603)3:1<33::AID-HCR54>3.0.CO