An in situ temperature dependent IR, EPR and high resolution XANES study on the NO/Cu+-ZSM-5 interaction

被引:94
作者
Prestipino, C
Berlier, G
Xamena, FXLI
Spoto, G
Bordiga, S
Zecchina, A
Palomino, GT
Yamamoto, T
Lamberti, C
机构
[1] Univ Turin, IFM, Dipartimento Chim, I-10125 Turin, Italy
[2] Univ Turin, INFM, UdR, Turin, Italy
[3] Univ Turin, INSTM, UdR, Turin, Italy
[4] Univ Balearic Isl, Dept Quim, Palma de Mallorca 07071, Spain
[5] Kyoto Univ, Dept Mol Engn, Grad Sch Engn, Kyoto 6068501, Japan
关键词
D O I
10.1016/S0009-2614(02)01183-1
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
We report an in situ IR, EPR, and high resolution XANES study on the Cu+(NO) and Cu+(NO)(2) complexes formed at 80 K in Cu+-ZSM-5. Bare Cu2+ ions (<1%) exhibit an axial EPR spectrum, while bare Cu+ ions exhibit well resolved 1s --> 4p(xy) and 1s --> 4p(z) transitions (p(xy)/p(z) splitting of 3.1 eV), reflecting the same local symmetry. Cu+(NO) complex exhibits an anisotropic EPR signal, while XANES spectrum of dinitrosyl adducts presents three resolved components ascribed to the 1s --> 4p(x), 1s --> 4p(y), and 1s --> 4p(z) transitions (p(x)/p(y) and p(y)/p(z) splitting of 3.8 and 2.6 eV, respectively) testifying the rupture of the axial symmetry of Cu+ bare cations upon NO adsorption. Upon increasing the temperature to 300 K, NO oxidizes a fraction of 75-85% of the cuprous ions. (C) 2002 Elsevier Science B.V. All rights reserved..
引用
收藏
页码:389 / 396
页数:8
相关论文
共 37 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]   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
[3]   X-RAY ABSORPTION-EDGE SPECTROSCOPY OF COPPER(I) COMPLEXES - COORDINATION GEOMETRY OF COPPER(I) IN THE REDUCED FORMS OF COPPER PROTEINS AND THEIR DERIVATIVES WITH CARBON-MONOXIDE [J].
BLACKBURN, NJ ;
STRANGE, RW ;
REEDIJK, J ;
VOLBEDA, A ;
FAROOQ, A ;
KARLIN, KD ;
ZUBIETA, J .
INORGANIC CHEMISTRY, 1989, 28 (07) :1349-1357
[4]   Calorimetric and spectroscopic study of the coordinative unsaturation of copper(I) and silver(I) cations in ZSM-5 zeolite -: Room temperature adsorption of NH3 [J].
Bolis, V ;
Bordiga, S ;
Palomino, GT ;
Zecchina, A ;
Lamberti, C .
THERMOCHIMICA ACTA, 2001, 379 (1-2) :131-145
[5]   X-ray photoelectron spectroscopy and x-ray absorption near edge structure study of copper sites hosted at the internal surface of ZSM-5 zeolite:: A comparison with quantitative and energetic data on the CO and NH3 adsorption [J].
Bolis, V ;
Maggiorini, S ;
Meda, L ;
D'Acapito, F ;
Palomino, GT ;
Bordiga, S ;
Lamberti, C .
JOURNAL OF CHEMICAL PHYSICS, 2000, 113 (20) :9248-9261
[6]   THE INTERACTION OF NO WITH COPPER IONS IN ZSM5 - AN EPR AND IR INVESTIGATION [J].
GIAMELLO, E ;
MURPHY, D ;
MAGNACCA, G ;
MORTERRA, C ;
SHIOYA, Y ;
NOMURA, T ;
ANPO, M .
JOURNAL OF CATALYSIS, 1992, 136 (02) :510-520
[7]  
GRUNERT W, 1994, J PHYS CHEM-US, V98, P10832
[8]   Fourier transform IR study of NOx adsorption on a CuZSM-5 DeNO(x) catalyst [J].
Hadjiivanov, K ;
Klissurski, D ;
Ramis, G ;
Busca, G .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1996, 7 (3-4) :251-267
[9]   Identification of neutral and charged NxOy surface species by IR spectroscopy [J].
Hadjiivanov, KI .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2000, 42 (1-2) :71-144
[10]   ENHANCEMENT OF CATALYTIC ACTIVITY OF COPPER ION-EXCHANGED Y-TYPE ZEOLITES FOR THE DECOMPOSITION OF NITROGEN MONOXIDE [J].
IWAMOTO, M ;
YAHIRO, H ;
KUTSUNO, T ;
BUNYU, S ;
KAGAWA, S .
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 1989, 62 (02) :583-584