Catalytic reduction of nitric oxide by methane in the presence of oxygen on palladium-exchanged mordenite zeolites

被引:66
作者
Descorme, C
Gelin, P
Lecuyer, C
Primet, M
机构
[1] Univ Lyon 1, CNRS, UMR 5634, Lab Applicat Chim Environm, F-69622 Villeurbanne, France
[2] GAZ FRANCE, Direct Rech, CERSTA, F-93211 La Plaine St Denis, France
关键词
SCR; palladium; mordenite; dealumination; nitric oxide; methane;
D O I
10.1006/jcat.1998.2112
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
Pd was introduced by exchange in non-dealuminated and dealuminated mordenites. After activation under oxygen at 500 degrees C, NO adsorption revealed the presence of isolated Pd2+ ions and Pd/PdO particles. Two types of Pd ions were shown: the first one would be located in the small cavities and leads to the formation of dinitrosyl complexes, whereas the second one, probably sitting in the main channels, is responsible for the obtainment of mononitrosyl complexes. Pd/PdO particles are active in the direct combustion of CH4 by oxygen and poorly active in the selective reduction (SCR) of NO. Pd ions are active for the NO SCR; the ions in the main channels are thought to be more active than the ions in the small cavities for accessibility reasons. In the case of the non-dealuminated mordenite catalyst, an activation under reactants is observed. Moreover, the activity is increased by the addition of 10 vol% water which is the opposite of the classical behavior of metal-loaded zeolites. Both phenomena are attributed to a migration of Pd ions from hidden to accessible sites. For the dealuminated sample, the observed deactivation seems to be due to a migration of isolated Pd ions into PdO particles located outside the zeolite matrix. (C) 1998 Academic Press.
引用
收藏
页码:352 / 362
页数:11
相关论文
共 44 条
[1]   The effect of zeolitic protons on NOx reduction over Pd/ZSM-5 catalysts [J].
Adelman, BJ ;
Sachtler, WMH .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 14 (1-2) :1-11
[2]   Mechanistic cause of hydrocarbon specificity over Cu/ZSM-5 and Co/ZSM-5 catalysts in the selective catalytic reduction of NOx [J].
Adelman, BJ ;
Beutel, T ;
Lei, GD ;
Sachtler, WMH .
JOURNAL OF CATALYSIS, 1996, 158 (01) :327-335
[3]   State of Pd on H-ZSM-5 and other acidic supports during the selective reduction of NO by CH4 studied by EXAFS/XANES [J].
Ali, A ;
Alvarez, W ;
Loughran, CJ ;
Resasco, DE .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 14 (1-2) :13-22
[4]  
ALMANZA LO, 1993, ESIS LYON 1 U
[5]   THE UNUSUAL HYDROTHERMAL STABILITY OF CO-ZSM-5 [J].
ARMOR, JN ;
FARRIS, TS .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1994, 4 (01) :L11-L17
[6]   CATALYTIC REDUCTION OF NITROGEN-OXIDES WITH METHANE IN THE PRESENCE OF EXCESS OXYGEN - A REVIEW [J].
ARMOR, JN .
CATALYSIS TODAY, 1995, 26 (02) :147-158
[7]  
Aylor AW, 1996, STUD SURF SCI CATAL, V101, P661
[8]   Investigations of the dispersion of Pd in H-ZSM-5 [J].
Aylor, AW ;
Lobree, LJ ;
Reimer, JA ;
Bell, AT .
JOURNAL OF CATALYSIS, 1997, 172 (02) :453-462
[9]  
Breck D.W, 1974, ZEOLITE MOL SIEVES
[10]   SELECTIVE REDUCTION OF NITROGEN-OXIDES BY HYDROCARBONS UNDER LEAN-BURN CONDITIONS USING SUPPORTED PLATINUM-GROUP METAL-CATALYSTS [J].
BURCH, R ;
MILLINGTON, PJ .
CATALYSIS TODAY, 1995, 26 (02) :185-206