Activity and durability of Fe/ZSM-5 catalysts for lean burn NOx reduction in the presence of water vapor

被引:487
作者
Chen, HY [1 ]
Sachtler, WMH [1 ]
机构
[1] Northwestern Univ, Ctr Catalysis & Surface Sci, VN Ipatieff Lab, Dept Chem, Evanston, IL 60208 USA
关键词
DeNO(x); SCR; Fe/ZSM-5; H2O effect; sublimation;
D O I
10.1016/S0920-5861(98)00078-9
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A novel method for the preparation of superior Fe/ZSM-5 catalysts is described. FeCl3 is sublimed into the cavities of H/ZSM-5, where it reacts chemically with the acid sites of the zeolite. With this method, Fe/ZSM-5 with an iron loading as high as Fe/Al=1 can be easily achieved. This preparation method is less sensitive to the origin of the zeolite and its synthesis history than the conventional ion-exchange method. HRAEM, FTIR, H-2-TPR and CO-TPR results show that iron is located at the exchange sites of the zeolite. An oxygen bridged binuclear iron complex is a plausible prototype for the active iron species. The iron is reduced from +3 to +2 below 800 degrees C. These catalysts are very active and selective in the catalytic reduction of NO, with iso-butane; they have a high durability under conditions simulating vehicular emission. A conversion of NO to N-2 Of about 76% was observed near 350 degrees C. Remarkably and in contrast to most other M/ZSM-5 catalysts, the performance of the new catalysts was not impaired when 10% H2O was added to the feed. H2O actually enhances the NOx conversion at low temperatures. CO and CO2 are both true primary products of NOx SCR over Fe/ZSM-5 catalysts. (C) 1998 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:73 / 83
页数:11
相关论文
共 34 条
[1]   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
[2]   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
[3]   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
[4]  
BAES CF, 1976, HYDROLYSIS CATIONS, P236
[5]   Potential reaction paths in NOx reduction over Cu/ZSM-5 [J].
Beutel, T ;
Adelman, B ;
Sachtler, WMH .
CATALYSIS LETTERS, 1996, 37 (3-4) :125-130
[6]   Redox chemistry of Cu/ZSM-5 [J].
Beutel, T ;
Sarkany, J ;
Lei, GD ;
Yan, JY ;
Sachtler, WMH .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (02) :845-851
[7]   Copper coordination in zeolite-supported lean NOx catalysts [J].
Blint, RJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (50) :19518-19524
[8]  
BOLT HP, 1994, THESIS U UTRECHT NET, pCH5
[9]  
COTTON FA, 1988, ADV INORG CHEM, P717
[10]   REDOX CATALYSIS IN ZEOLITES - INVESTIGATION OF THE BEHAVIOR OF IRON-EXCHANGED MORDENITE TOWARD CARBON-MONOXIDE REDUCTION [J].
FANG, SM ;
PETUNCHI, J ;
LEGLISE, J ;
MILLMAN, WS ;
HALL, WK .
JOURNAL OF CATALYSIS, 1985, 96 (01) :182-188