Activity and deactivation of Fe-MFI catalysts for benzene hydroxylation to phenol by N2O

被引：85
作者：
Meloni, D
Monaci, R
Solinas, V
Berlier, G
Bordiga, S
Rossetti, I
Oliva, C
Forni, L
机构：
[1] Univ Milan, Dipartimento Chim Fis & Elettrochim, I-20133 Milan, Italy
[2] Univ Turin, Dipartimento Chim Inorgan Fis & Mat, I-10125 Turin, Italy
[3] Univ Cagliari, Dipartimento Sci Chim, I-09042 Cagliari, Italy
来源：
JOURNAL OF CATALYSIS | 2003年 / 214卷 / 02期
关键词：
Fe-MFI catalyst; benzene hydroxylation by N2O; catalyst acidity; catalyst coking;
D O I：
10.1016/S0021-9517(03)00013-7
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：
Isomorphously substituted Fe-MFI zeolite catalysts with various Si/Al and/or Si/Fe ratios were synthesized and characterized by many different techniques, such as ICP, XRD, SEM, TPR, microcalorimetry, FTIR, and EPR. Under standard reaction conditions the best catalyst gave 20% benzene conversion and over 90% selectivity to phenol. For Fe-ZSM5 catalysts, addition of steam to the feed improved catalyst activity, selectivity, and durability. Phenol formed onto Fe-based sites only. Active sites could very likely be composed of oxygen-bridged, extraframework binuclear Fe redox species, charge-compensating the framework Fe3+ or Al3+ ions. Surface acidity was not responsible for activity in the main reaction, but it was heavily involved in catalyst deactivation by coking. Catalyst deactivation derived mainly from the decomposition-condensation of phenol onto acid sites; the stronger the latter, the quicker was the coking rate. (C) 2003 Elsevier Science (USA). All rights reserved.
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页码：169 / 178
页数：10
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