Catalytic properties and electronic structure of copper ions in Cu-ZSM-5

被引:120
作者
Yashnik, SA [1 ]
Ismagilov, ZR [1 ]
Anufrienko, VF [1 ]
机构
[1] RAS, SB, Boreskov Inst Catalysis, Novosibirsk 630090, Russia
关键词
Cu-ZSM-5; copper-exchanged zeolite; copper electron state; ESR; UV-vis DRS; EXCHANGED ZSM-5 ZEOLITES; NITRIC-OXIDE; SELECTIVE REDUCTION; NITROGEN MONOXIDE; NO DECOMPOSITION; IN-SITU; REDOX BEHAVIOR; ACTIVE-SITES; MECHANISM; CU/ZSM-5;
D O I
10.1016/j.cattod.2005.09.029
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The effect of ion exchange conditions, such as Si/Al ratio, precursor copper salt, pH and concentration of the solution, on the catalytic activity in SCR of NO by propane and on the electronic state of copper ions in Cu-ZSM-5 has been studied. The NO conversion in NO SCR by C3H8 has been found to reach a maximum value at Cu/Al ratio about 0.37-0.4 and remain constant at higher Cu/Al. ESR and UV-vis DR spectroscopy have been used to elucidate stabilization conditions of copper ions in Cu-ZSM-5 zeolites as isolated Cu2+ ions, chain copper oxide structures and square-plain oxide clusters. The ability of copper ions for reduction and reoxidation in the chain structures may be responsible for the catalytic activity of Cu-ZSM-5. These transformations of copper ions are accompanied by the observation of intervalence transitions Cu2+-Cu+ and CTLM of the chain structures in the UV-vis spectra. (c) 2005 Elsevier B.V. All rights reserved.
引用
收藏
页码:310 / 322
页数:13
相关论文
共 65 条
[1]   STUDY OF CU-2+-DOPED ZEOLITE NAH-ZSM-5 BY ELECTRON-SPIN-RESONANCE AND ELECTRON-SPIN ECHO MODULATION SPECTROSCOPIES [J].
ANDERSON, MW ;
KEVAN, L .
JOURNAL OF PHYSICAL CHEMISTRY, 1987, 91 (15) :4174-4179
[2]   MECHANISM OF THE LEAN NOX REACTION OVER CU/ZSM-5 [J].
ANSELL, GP ;
DIWELL, AF ;
GOLUNSKI, SE ;
HAYES, JW ;
RAJARAM, RR ;
TRUEX, TJ ;
WALKER, AP .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1993, 2 (01) :81-100
[3]   A study of linear copper oxide structures in the channels of the ZSM-5 zeolite by electronic diffuse reflectance spectroscopy [J].
Anufrienko, VF ;
Yashnik, SA ;
Bulgakov, NN ;
Larina, TV ;
Vasenin, NT ;
Ismagilov, ZR .
DOKLADY PHYSICAL CHEMISTRY, 2003, 392 (1-3) :207-211
[4]   Detection of O- radical anions in Cu-ZSM-5 zeolites after heat treatment [J].
Anufrienko, VF ;
Bulgakov, NN ;
Vasenin, NT ;
Yashnik, SA ;
Tsikoza, LT ;
Vosel, SV ;
Ismagilov, ZR .
DOKLADY CHEMISTRY, 2002, 386 (4-6) :273-276
[5]  
Baester C.F., 1976, HYDROLYSIS CATIONS, P267
[6]   Evolution of Fe species during the synthesis of over-exchanged Fe/ZSM5 obtained by chemical vapor deposition of FeCl3 [J].
Battiston, AA ;
Bitter, JH ;
de Groot, FMF ;
Overweg, AR ;
Stephan, O ;
van Bokhoven, JA ;
Kooyman, PJ ;
van der Spek, C ;
Vankó, G ;
Koningsberger, DC .
JOURNAL OF CATALYSIS, 2003, 213 (02) :251-271
[7]   INFLUENCE OF THE PREPARATION METHOD ON THE SELECTIVE REDUCTION OF NITRIC-OXIDE OVER CU-ZSM-5 - NATURE OF THE ACTIVE-SITES [J].
CHAJAR, Z ;
PRIMET, M ;
PRALIAUD, H ;
CHEVRIER, M ;
GAUTHIER, C ;
MATHIS, F .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1994, 4 (2-3) :199-211
[8]   Copper active sites for the selective reduction of nitrogen monoxide by propane on Cu-MFI catalysts and non-zeolitic supported-copper solids [J].
Chajar, Z ;
Le Chanu, V ;
Primet, M ;
Praliaud, H .
CATALYSIS LETTERS, 1998, 52 (1-2) :97-102
[9]   EPR STUDY OF COPPER(II) ION PAIRS IN Y-TYPE ZEOLITES [J].
CHAO, CC ;
LUNSFORD, JH .
JOURNAL OF CHEMICAL PHYSICS, 1972, 57 (07) :2890-&
[10]  
Cho B.K., 1994, J CATAL, V155, P84