Kinetics, acid sites and deactivation of H-mordenite during the SCR of NOx with CH4

被引:12
作者
Ribotta, A
Lezcano, M
Kurgansky, M
Miro, E
Lombardo, E
Petunchi, J
Moreaux, C
Dereppe, JM
机构
[1] UNL, CONICET, Inst Invest Catalisis & Petroquim, RA-3000 Santa Fe, Argentina
[2] Univ Catholique Louvain, Chim Phys Lab, B-1348 Louvain, Belgium
关键词
SCR of NO with CH4; H-mordenite; deactivation; acid sites; kinetic parameters;
D O I
10.1023/A:1019064112577
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
H-mordenites are active for the SCR reaction but they suffer irreversible partial deactivation after being on stream for one hour at 650 degrees C. The reaction orders and activation energies are not significantly affected by deactivation. This indicates that deactivation originates in a decrease in the number of active sites due to dealumination and possible pore blockage. The NO disappearance rate correlates with TPD NH3 between 300 and 700 degrees C:; FTIR confirms these results. Xe-129 NMR of adsorbed xenon shows that pore blockage occurs and is due to the presence of aluminum species in the main zeolite channels. The overall deactivation process and the role of acid sites is discussed in terms of the current literature.
引用
收藏
页码:77 / 85
页数:9
相关论文
共 26 条
[1]   THE UNUSUAL HYDROTHERMAL STABILITY OF CO-ZSM-5 [J].
ARMOR, JN ;
FARRIS, TS .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1994, 4 (01) :L11-L17
[2]   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
[3]   THE RATE-DETERMINING STEP IN THE SELECTIVE REDUCTION OF NITRIC-OXIDE BY METHANE OVER A CO ZSM5 CATALYST IN THE PRESENCE OF OXYGEN [J].
COWAN, AD ;
DUMPELMANN, R ;
CANT, NW .
JOURNAL OF CATALYSIS, 1995, 151 (02) :356-363
[4]   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
[5]   CHANGES IN MORDENITE UPON VARIOUS PRETREATMENTS .1. STRUCTURAL REARRANGEMENTS [J].
HA, BH ;
GUIDOT, J ;
BARTHOMEUF, D .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1979, 75 :1245-1253
[6]   SULFATE-PROMOTED METAL-OXIDE CATALYSTS FOR THE SELECTIVE REDUCTION OF NITROGEN MONOXIDE BY PROPANE IN OXYGEN-RICH ATMOSPHERE [J].
HAMADA, H ;
KINTAICHI, Y ;
TABATA, M ;
SASAKI, M ;
ITO, T .
CHEMISTRY LETTERS, 1991, (12) :2179-2182
[7]  
HAYS GR, 1984, ZEOLITES, V4, P373
[8]  
IMOBERDORF G, IN PRESS
[9]   SELECTIVE REDUCTION OF NITROGEN-OXIDES WITH HYDROCARBONS OVER SOLID ACID CATALYSTS IN OXYGEN-RICH ATMOSPHERES [J].
KINTAICHI, Y ;
HAMADA, H ;
TABATA, M ;
SASAKI, M ;
ITO, T .
CATALYSIS LETTERS, 1990, 6 (02) :239-244
[10]  
Lezcano M, 1996, STUD SURF SCI CATAL, V101, P971