Investigation of the selective catalytic reduction of NO by NH3 on Fe-ZSM5 monolith catalysts

被引:167
作者
Kröcher, Oliver [1 ]
Devadas, Mukundan
Elsener, Martin
Wokaun, Alexander
Söger, Nicola
Pfeifer, Marcus
Demel, Yvonne
Mussmann, Lothar
机构
[1] Paul Scherrer Inst, CH-5232 Villigen, Switzerland
[2] Umicore AG & Co KG, Automot Catalysts, D-63403 Hanau, Germany
关键词
Fe-ZSM5; NOx; conversion; monolith; stability; urea SCR; ammonia storage;
D O I
10.1016/j.apcatb.2006.03.012
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-ZSM5 coated on cordierite monolith was investigated in the selective catalytic reduction (SCR) of NO with ammonia over a broad temperature range, applying simulated diesel exhaust gas conditions. The catalyst exhibited over 80% NOx reduction (DeNOx) from 400 to 650 degrees C at very good selectivity. The dosage of variable amounts of ammonia in the catalytic tests revealed that the SCR reaction is inhibited by ammonia. At very high temperatures DeNOx is reduced due to the selective catalytic oxidation (SCO) of ammonia to nitrogen and the oxidation to NO. Water-free experiments resulted in generally higher DeNOx values, which are explained by the inhibiting effect of water on the NO oxidation capability of Fe-ZSM5. The catalyst was stable upon thermal ageing and only 5-15% loss in DeNOx activity was observed after hydrothermal treatment. This loss in DeNOx is in parallel with a loss of ammonia storage capacity of the aged catalyst. Characterization by NH3 TPD and MAS Al-27 NMR spectroscopy revealed dealumination of the zeolite by hydrothermal ageing, which reduces the Bronsted acidity of the catalyst. (c) 2006 Elsevier B.V. All rights reserved.
引用
收藏
页码:208 / 216
页数:9
相关论文
共 36 条
[1]   ALUMINUM SITING IN MORDENITE AND DEALUMINATION MECHANISM [J].
BODART, P ;
NAGY, JB ;
DEBRAS, G ;
GABELICA, Z ;
JACOBS, PA .
JOURNAL OF PHYSICAL CHEMISTRY, 1986, 90 (21) :5183-5190
[2]   TEMPERATURE-PROGRAMMED DESORPTION STUDIES ON ZSM-5 ZEOLITES [J].
CHAO, KJ ;
CHIOU, BH ;
CHO, CC ;
JENG, SY .
ZEOLITES, 1984, 4 (01) :2-4
[3]   Honeycomb reactor washcoated with mordenite type zeolite catalysts for the reduction of NOx by NH3 [J].
Choi, H ;
Ham, SW ;
Nam, IS ;
Kim, YG .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1996, 35 (01) :106-112
[4]   The simultaneous catalytic reduction of NO and N2O by NH3 using an Fe-zeolite-beta catalyst [J].
Coq, B ;
Mauvezin, M ;
Delahay, G ;
Butet, JB ;
Kieger, S .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2000, 27 (03) :193-198
[5]   Catalytic investigation of Fe-ZSM5 in the selective catalytic reduction of NOx with NH3 [J].
Devadas, M ;
Kröcher, O ;
Wokaun, A .
REACTION KINETICS AND CATALYSIS LETTERS, 2005, 86 (02) :347-354
[6]   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
[7]  
Engelhardt G., 1987, HIGH RESOLUTION SOLI
[8]   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
[9]   MEASUREMENT OF THE ACIDITY OF VARIOUS ZEOLITES BY TEMPERATURE-PROGRAMMED DESORPTION OF AMMONIA [J].
HIDALGO, CV ;
ITOH, H ;
HATTORI, T ;
NIWA, M ;
MURAKAMI, Y .
JOURNAL OF CATALYSIS, 1984, 85 (02) :362-369
[10]   Investigation of the ammonia adsorption on monolithic SCR catalysts by transient response analysis [J].
Kleemann, M ;
Elsener, M ;
Koebel, M ;
Wokaun, A .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2000, 27 (04) :231-242