Active site structure sensitivity in N2O conversion over FeMFI zeolites

被引:133
作者
Pérez-Ramírez, J
Kapteijn, F
Brückner, A
机构
[1] Oil & Energy Res Ctr, N-3907 Porsgrunn, Norway
[2] Delft Univ Technol, DelftChemTech, NL-2628 BL Delft, Netherlands
[3] Inst Appl Chem Berlin Adlershof, D-12484 Berlin, Germany
关键词
N2O decomposition; N2O reduction; FeMFI; steam treatment; iron species; active site; isolated ions; oligonuclear species; iron oxide; reaction mechanism;
D O I
10.1016/S0021-9517(03)00087-3
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
Preparation of steam-activated Fe-silicalite containing mainly isolated iron species in extraframework positions was essential for deriving structure-activity relationships in various N2O conversion reactions over iron zeolite catalysts. Characterization by UV-Vis/DRS revealed that any significant clustering of iron did not occur in this sample. Other steam-activated FeMFI zeolites, with different framework compositions or treated at higher temperatures, showed various degrees of clustering. The activity of the cluster-free Fe-silicalite was significantly higher in N2O reduction with C3H8 and CO. However, some level of association of iron species leads to higher activities in direct N2O decomposition. Due to the intrinsic reaction mechanism, this result demonstrates the sensitivity of reactions for the form of the iron species in Fe-zeolites, rather than the existence of a unique active site. (C) 2003 Elsevier Inc. All rights reserved.
引用
收藏
页码:234 / 238
页数:5
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