期刊
JOURNAL OF CATALYSIS
卷 214, 期 2, 页码 169-178出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/S0021-9517(03)00013-7
关键词
Fe-MFI catalyst; benzene hydroxylation by N2O; catalyst acidity; catalyst coking
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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