Mechanistic study of the effect of coexisting H2O on the selective reduction of NO with propene over sol-gel prepared In2O3-Al2O3 catalyst

被引:37
作者
Haneda, M
Kintaichi, Y
Bion, N
Hamada, H
机构
[1] Natl Inst Adv Ind Sci & Technol, AIST, Tsukuba, Ibaraki 3058565, Japan
[2] CNRS ISMRA, UMR 6506, Catalyse & Spectrochim Lab, F-14050 Caen, France
关键词
NO reduction by propene; Ir2O3-Al2O3; kinetic studies; diffuse reflectance FF-IR spectroscopy;
D O I
10.1016/S0926-3373(02)00215-1
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
The effect of coexisting H2O on the catalytic activity of In2O3-Al2O3 prepared by the sol-gel method for NO reduction by propene in the presence of oxygen was studied. No activity depression due to coexisting H2O was observed for In2O3-Al2O3 with an In2O3 loading of more than 5 wt.%, although the catalysts with a lower In2O3 loading (similar to3 wt.%) showed an inhibition effect by H2O. X-ray diffraction (XRD) and X-ray absorption spectroscopy (XANES) revealed the presence of small In2O3 crystallites and relatively large In2O3 particles in the catalysts with lower (similar to3 wt.%) and higher (5 wt.%) In2O3 loadings, respectively. A high H2O tolerance of In2O3-Al2O3 with higher In2O3 loadings of more than 5 wt.% was considered to be due to the presence of the relatively large In2O3 particles interacting with Al2O3. The results of kinetic studies and in situ diffuse reflectance Fourier transform infrared (FT-IR) experiments showed that coexisting H2O suppresses the formation of and/or promotes the desorption of formate and NO3- surface species. The present effect of coexisting H2O was interpreted by the compensation of the following two opposite effects: the removal of the formate species as a spectator species and the promotion of the hydrolysis of the -NCO species (positive effect), and the inhibition of the formation of NO3- species as the initial intermediate (negative effect). (C) 2002 Elsevier Science B.V All rights reserved.
引用
收藏
页码:57 / 68
页数:12
相关论文
共 46 条
[1]   On the mechanism of selective NOx reduction with alkanes over Cu/ZSM-5 [J].
Adelman, BJ ;
Beutel, T ;
Lei, GD ;
Sachtler, WMH .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1996, 11 (01) :L1-L9
[2]  
BAIKER A, 1992, NEW FRONTIERS CATALY, P1257
[3]   Formation and reactions of isocyanic acid during the catalytic reduction of nitrogen oxides [J].
Cant, NW ;
Chambers, DC ;
Cowan, AD ;
Liu, IOY ;
Satsuma, A .
TOPICS IN CATALYSIS, 2000, 10 (1-2) :13-20
[4]   In situ FTIR studies of the selective catalytic reduction of NO by C3H6 over Pt/Al2O3 [J].
Captain, DK ;
Amiridis, MD .
JOURNAL OF CATALYSIS, 1999, 184 (02) :377-389
[5]   Reaction intermediates in the selective catalytic reduction of NOx over Fe/ZSM-5 [J].
Chen, HY ;
Voskoboinikov, T ;
Sachtler, WMH .
JOURNAL OF CATALYSIS, 1999, 186 (01) :91-99
[6]   An FTIR study an the mechanism of the reaction between nitrogen dioxide and propene over acidic mordenites [J].
Gerlach, T ;
Schütze, FW ;
Baerns, M .
JOURNAL OF CATALYSIS, 1999, 185 (01) :131-137
[7]   Reduction of nitrogen dioxide by propene over acidic mordenites: influence of acid site concentration, formation of by-products and mechanism [J].
Gerlach, T ;
Illgen, U ;
Bartoszek, M ;
Baerns, M .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1999, 22 (04) :269-278
[8]   THE RELATION BETWEEN DEACTIVATION OF CUZSM-5 IN THE SELECTIVE REDUCTION OF NO AND DEALUMINATION OF THE ZEOLITE [J].
GRINSTED, RA ;
JEN, HW ;
MONTREUIL, CN ;
ROKOSZ, MJ ;
SHELEF, M .
ZEOLITES, 1993, 13 (08) :602-606
[9]   Role of supported metals in the selective reduction of nitrogen monoxide with hydrocarbons over metal/alumina catalysts [J].
Hamada, H ;
Kintaichi, Y ;
Inaba, M ;
Tabata, M ;
Yoshinari, T ;
Tsuchida, H .
CATALYSIS TODAY, 1996, 29 (1-4) :53-57
[10]   SELECTIVE REDUCTION OF NO BY HYDROCARBONS AND OXYGENATED HYDROCARBONS OVER METAL-OXIDE CATALYSTS [J].
HAMADA, H .
CATALYSIS TODAY, 1994, 22 (01) :21-40