Catalytic performance of Fe-ZSM-5 catalysts for selective catalytic reduction of nitric oxide by ammonia

被引:162
作者
Long, RQ [1 ]
Yang, RT [1 ]
机构
[1] Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA
关键词
selective catalytic reduction of NO with NH3; Fe-ZSM-5; catalyst; Fe-mordenite catalyst; Fe-Y catalyst; Fe-MCM-41catalyst;
D O I
10.1006/jcat.1999.2674
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
A series of Fe-exchanged molecular sieves were studied as catalysts for the selective catalytic reduction (SCR) of NO with ammonia. It was found that Fe-ZSM-5 and Fe-mordenite catalysts were highly active for the SCR reaction. Nearly 100% NO conversions were obtained at 400-500 degrees C under conditions with a high space velocity (GHSV = 4.6 x 10(5) l/h). However, Fe-Y and Fe-MCM-41 with larger pore sizes showed lower activities for this reaction. For Fe-ZSM-5 catalysts, the SCR activity decreased with increasing Si/Al ratio in the zeolites. As the Fe-exchange level in the Fe-ZSM-5 catalysts was increased from 58 to 252%, NO conversion increased at lower temperatures (e.g., 300 degrees C), but decreased at high temperatures (e.g., 600 degrees C). Compared with the commercial vanadia catalyst, based on the first-order rate constants, the Fe-ZSM-5 catalyst was five times more active at 400 degrees C and seven times more active at 450 degrees C. It also functioned in a broader temperature window produced only N-2 (rather than N2O) and H2O, and showed a substantially lower activity for oxidation of SO2 to SO3. (C) 1999 Academic Press.
引用
收藏
页码:332 / 339
页数:8
相关论文
共 28 条
[1]   Selective catalytic reduction of nitric oxide by hydrocarbons [J].
Amiridis, MD ;
Zhang, TJ ;
Farrauto, RJ .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1996, 10 (1-3) :203-227
[2]   SYNTHESIS OF ALUMINUM-RICH MCM-41 [J].
BORADE, RB ;
CLEARFIELD, A .
CATALYSIS LETTERS, 1995, 31 (2-3) :267-272
[3]  
Bosch H., 1986, CATAL TODAY, V2, P369, DOI DOI 10.1016/0920-5861(88)80002-6
[4]  
Brandin JGM, 1989, CATAL TODAY, V4, P187
[5]   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
[6]   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
[7]   MECHANISM OF POISONING OF THE V2O5 TIO2 CATALYST FOR THE REDUCTION OF NO BY NH3 [J].
CHEN, JP ;
YANG, RT .
JOURNAL OF CATALYSIS, 1990, 125 (02) :411-420
[8]   Iron oxide and chromia supported on titania-pillared clay for selective catalytic reduction of nitric oxide with ammonia [J].
Cheng, LS ;
Yang, RT ;
Chen, N .
JOURNAL OF CATALYSIS, 1996, 164 (01) :70-81
[9]   Kinetic and mechanistic study of NOx reduction by NH3 over H-form zeolites .2. Semi-steady-state and in situ FTIR studies [J].
Eng, J ;
Bartholomew, CH .
JOURNAL OF CATALYSIS, 1997, 171 (01) :27-44
[10]   FeZSM-5: A durable SCR catalyst for NOx removal from combustion streams [J].
Feng, XB ;
Hall, WK .
JOURNAL OF CATALYSIS, 1997, 166 (02) :368-376