Fourier transform IR study of NOx adsorption on a CuZSM-5 DeNO(x) catalyst

被引:151
作者
Hadjiivanov, K [1 ]
Klissurski, D [1 ]
Ramis, G [1 ]
Busca, G [1 ]
机构
[1] UNIV GENOA,FAC INGN,IST CHIM,I-16129 GENOA,ITALY
关键词
adsorption; carbon monoxide; CuZSM-5; FTIR spectroscopy; nitrogen monoxide; nitrogen dioxide; NOx; propane; zeolites;
D O I
10.1016/0926-3373(95)00034-8
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 adsorption and coadsorption of selective catalytic reduction (SCR) reactants and reaction products on CuZSM-5-37 containing 11 wt.-% CuO have been studied by FTIR spectroscopy. The catalyst surface is characterized by both weak acidity and weak basicity as revealed by testing with probe molecules (CO2, NH3, H2O). NO2 adsorption results in formation of different kinds of nitrates. The same species are formed when NO is coadsorbed with oxygen at 180 degrees C. NO adsorption at ambient temperature also leads to formation of nitrates as well as of Cu2+-NO species. In the presence of oxygen the latter are converted according to the scheme: NO --> N2O3 --> N2O4 --> NO2 --> NO3. It is concluded that the surface nitrates are important intermediates in the SCR process. They are thermally stable and resistant towards interaction with CO2, N-2, O-2, and art only slightly affected by H2O and NO. However, they posses a high oxidation ability and are fully reduced by propane at 180 degrees C. It is concluded that one of the most important roles of oxygen in SCR by hydrocarbons is to convert NOx into highly active surface nitrates.
引用
收藏
页码:251 / 267
页数:17
相关论文
共 48 条
[31]  
Nakamoto K, 1966, INFRARED SPECTRA INO
[32]   ON THE ROLE OF NITROGEN-DIOXIDE IN THE MECHANISM OF THE SELECTIVE REDUCTION OF NOX OVER CU-ZSM-5 ZEOLITE [J].
PETUNCHI, JO ;
HALL, WK .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1993, 2 (2-3) :L17-L26
[33]  
PIEPLU T, 1994, P 3 INT C CAT AUT PO
[34]   NH3 FORMATION DURING THE REDUCTION OF NITROGEN MONOXIDE BY PROPANE ON H-CU-ZSM-5 IN EXCESS OXYGEN [J].
POIGNANT, F ;
SAUSSEY, J ;
LAVALLEY, JC ;
MABILON, G .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1995, (01) :89-90
[35]  
Pozdnyakov D., 1973, Kinet. Katal, V14, P760
[36]   FOURIER TRANSFORM-INFRARED STUDY OF THE ADSORPTION AND COADSORPTION OF NITRIC-OXIDE, NITROGEN-DIOXIDE AND AMMONIA ON VANADIA TITANIA AND MECHANISM OF SELECTIVE CATALYTIC REDUCTION [J].
RAMIS, G ;
BUSCA, G ;
BREGANI, F ;
FORZATTI, P .
APPLIED CATALYSIS, 1990, 64 (1-2) :259-278
[37]  
RAMIS G, IN PRESS J CATAL
[38]   FOURIER-TRANSFORM INFRARED STUDY OF THE ADSORPTION AND COADSORPTION OF NITRIC-OXIDE, NITROGEN-DIOXIDE AND AMMONIA ON TIO2 ANATASE [J].
RAMIS, GG ;
BUSCA, G ;
LORENZELLI, V ;
FORZATTI, P .
APPLIED CATALYSIS, 1990, 64 (1-2) :243-257
[39]   IN-SITU DIFFUSE-REFLECTANCE FTIR STUDY OF THE SELECTIVE CATALYTIC REDUCTION OF NO BY NH3 OVER VANADIA-TITANIA AEROGELS [J].
SCHNEIDER, H ;
TSCHUDIN, S ;
SCHNEIDER, M ;
WOKAUN, A ;
BAIKER, A .
JOURNAL OF CATALYSIS, 1994, 147 (01) :5-14
[40]   SPECTROSCOPY OF THERMAL-OXIDATION OF NO IN SOLID OXYGEN AT CRYOGENIC TEMPERATURES [J].
SMITH, GR ;
GUILLORY, WA .
JOURNAL OF MOLECULAR SPECTROSCOPY, 1977, 68 (02) :223-235