Fe-containing ZSM-11 zeolites as active catalyst for SCR of NOx -: Part I.: Synthesis, characterization by XRD, BET and FTIR and catalytic properties

被引:28
作者
Anunziata, OA [1 ]
Beltramone, AR
Juric, Z
Pierella, LB
Requejo, FG
机构
[1] Univ Tecnol Nacl, Fac Cordoba, CITeQ, Grp Fisicoquim & Neuvos Mat, RA-5016 Cordoba, Argentina
[2] Univ Oklahoma, Sch Chem Engn & Mat Sci, Oklahoma City, OK USA
[3] UNLP, FCE, Dto Fis, La Plata, Buenos Aires, Argentina
[4] Consejo Nacl Invest Cient & Tecn, IFILP, La Plata, Buenos Aires, Argentina
关键词
fe-zeolites; synthesis; NOSCR; active sites; XRD; FTIR;
D O I
10.1016/j.apcata.2003.12.033
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-ZSM-11 zeolites, prepared by novel sol-gel process with Fe2+ and/or Fe3+ as active sites incorporated by reproducible post-synthesis methods were obtained. Investigations of the electron-donor-acceptor (EDA) sites from Fen+-containing zeolite by in situ infrared spectroscopy using pyridine as a probe molecule lead to the conclusion that the NOx conversion is a function of Fe2+ species. Fen+ as counter ions generates new Lewis sites. We differentiated it from the well-known Lewis sites from aluminum in the zeolitic framework. Thus, lower unoccupied molecular orbital (LUMO) of Fen+ and its interaction with the reactant through EDA adduct leading to a coordinative activity with Bronsted acid sites, being successfully applicable to selective catalytic reduction (SCR) of NOx. Moreover, according FTIR in situ analysis of NO adsorbed onto the catalyst, Fe2O3 as isolated species was not detected in the samples, although this specie is found in low proportion in the sample with Fe3+ as active site by XRD analysis. (C) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:93 / 101
页数:9
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]   Expanded regional rate analysis: A novel method to determine regional formation rates in catalyzed reactions [J].
Anunziata, OA ;
Pierella, LB ;
Marino, RG .
APPLIED CATALYSIS A-GENERAL, 1997, 165 (1-2) :35-49
[3]   NATURE OF THE ACTIVE-SITES IN H-ZSM-11 ZEOLITE MODIFIED WITH ZN(2+) AND GA(3+) [J].
ANUNZIATA, OA ;
PIERELLA, LB .
CATALYSIS LETTERS, 1993, 19 (2-3) :143-151
[4]  
ANUNZIATA OA, 2003, UNPUB
[5]   Catalytic behavior of La-Sr-Ce-Fe-O mixed oxidic/perovskitic systems for the NO plus CO and NO+CH4+O2 (lean-NOx) reactions [J].
Belessi, VC ;
Costa, CN ;
Bakas, TV ;
Anastasiadou, T ;
Pomonis, PJ ;
Efstathiou, AM .
CATALYSIS TODAY, 2000, 59 (3-4) :347-363
[6]  
BELTRAMONE AR, 2003, IN PRESS CATAL LETT
[7]  
BOON K, 1986, INORGANIC CHEM CONCE, V9
[8]   Identification of active sites and adsorption complexes in Fe/MFI catalysts for NOx reduction [J].
Chen, HY ;
El-Malki, EM ;
Wang, X ;
van Santen, RA ;
Sachtler, WMH .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2000, 162 (1-2) :159-174
[9]   Reduction of NOx over various Fe/zeolite catalysts [J].
Chen, HY ;
Wang, X ;
Sachtler, WMH .
APPLIED CATALYSIS A-GENERAL, 2000, 194 :159-168
[10]   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