Cu-ZSM-5 (Si/Al=66), Cu-Fe-S-1 (Si/Fe=66) and Cu-S-1 catalysts for NO decomposition: preparation, analytical characterization and catalytic activity

被引:21
作者
Dossi, C
Fusi, A
Recchia, S
Psaro, R
Moretti, G
机构
[1] Univ Milan, Dipartimento Chim Inorgan Metallorgan & Anali, Ctr CSSCMTBSO, CNR, I-20133 Milan, Italy
[2] Univ Insubria, Ist Sci Matemat Fis & Chim, I-22100 Como, Italy
[3] Univ La Sapienza, Dipartimento Chim, CNR, Ctr SACSO, I-00185 Rome, Italy
关键词
Cu-Fe-silicalite; Cu-silicalite; Cu-ZSM-5; Fe-silicalite; NO decomposition;
D O I
10.1016/S1387-1811(99)00020-7
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
We prepared H-ZSM-5 (Si/Al = 66), Fe-S-1 (Si/Fe = 66), and Silicalite-1 (S-1) according to the methods described by Bellussi and coworkers, and compared their ion-exchange capacity for copper ions. The Cu-ZSM-5, Cu-Fe-S and Cu-S-1 samples thus obtained have been investigated as catalysts for the NO decomposition reaction at 773 K. We found that using copper acetate solutions with concentrations in the range 0.004 M less than or equal to[Cu2+]less than or equal to 0.1 M, at room temperature and at 323 K, it is very easy to prepare overexchanged Cu-ZSM-5, Cu-Fe-S-1, and Cu-S-1 catalysts. XRD and Vis-UV DRS techniques show that after thermal treatments of the fresh samples in air at 823 K for 4 h no segregation of bulk CuO phase occurs, suggesting the presence of low nuclearity [CunOx(OH)(y)](q+) species [q=2(n-x)-y greater than or equal to 0]. These results were confirmed by TPR studies. At 773 K, only Cu-ZSM-5 and Cu-Fe-S-1 catalysts showed NO decomposition activity (NO 1% in He, W/F = 0.2 g s cm(-3)). Instead, the activities of Cu-S-1 and of the copper-free matrices (S-1, H-ZSM-5 and Fe-S-1) were not measurable under our experimental conditions. The negative results obtained with Cu-S-1 catalysts clearly demonstrate that the active sites for NO decomposition in Cu-MFI catalysts consist of polynuclear ionic copper species strongly anchored to framework [MO4](-) species (M=Al, Fe). (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:165 / 175
页数:11
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