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Oxidation of Benzene to Phenol by N2O on an Fe2+-ZSM-5 Cluster: A Density Functional Theory Study
Date
2009-08-27
Author
Fellah, Mehmet Ferdi
van Santen, Rutger A.
Önal, Işık
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Density functional theory (DFT) calculations were carried out in a study of the oxidation of benzene to phenol by N2O on an Fe2+-ZSM-5 cluster. The catalytic cycle has been studied oil a model [Si6Al2O9H14Fe] cluster. It is found that Fe2+ is preferred over Fe1+ as a site for phenol oxidation. A high desorption value of 126.4 kJ/mol suggests that at low temperature phenol desorption is the rate limiting step on the Fe2+-ZSM-5 cluster. It competes with the N2O decomposition step. The computed activation energy for phenol desorption is in good agreement with the experimental activation energy value of 125.94 kJ/mol reported in the literature for benzene oxidation to phenol by N2O on Fe-ZSM-5.
Subject Keywords
Nitrous-oxide decomposition
,
Bridged iron sites
,
One-step oxidation
,
Selective oxidation
,
Active-sites
,
Mfi zeolites
,
Dinitrogen monoxide
,
Fe/Mfi catalysts
,
Alpha-Form
,
Fe-Zsm-5
URI
https://hdl.handle.net/11511/31056
Journal
JOURNAL OF PHYSICAL CHEMISTRY C
DOI
https://doi.org/10.1021/jp904224h
Collections
Graduate School of Natural and Applied Sciences, Article
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Fellah, Mehmet Ferdi; Önal, Işık; van Santen, Rutger A. (2010-07-29)
Density functional theory calculations were carried out in a study of the oxidation of benzene to phenol by N2O on a model (FeO)(1+)-ZSM-5 cluster: the [(SiH3)(4)AlO4(FeO)] cluster. This cluster models the reactivity of Fe3+ oxidic clusters. Results are to be compared with an earlier study (J. Phys. Chem. C 2009, 113, 15307) on a model Fe2+-ZSM-5 cluster. The true activation energies for the elementary reaction step in which phenol is produced appear to be comparable. The major difference between the two sy...
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Density functional theory (DFT) calculations were carried out in the study of oxidation of benzene to phenol by N2O on relaxed [(SiH3)(4)AlO4M] (where M=Fe, Co) cluster models representing Fe- and Co-ZSM-5 surfaces. The catalytic cycle steps are completed for both Fe-ZSM-5 and Co-ZSM-5 clusters. The general trend of the results that were obtained in terms of activation barriers for the Fe-ZSM-5 cluster is in agreement with the experimental and theoretical literature. It was observed that the phenol formatio...
A DFT Study of Direct Oxidation of Benzene to Phenol by N2O over [Fe(mu-O)Fe](2+) Complexes in ZSM-5 Zeolite
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Density functional theory (DFT) calculations were carried out in a study of the mechanism of benzene oxidation by N2O to phenol over an extra framework dimeric [FeOFe](2+) species in ZSM-5 zeolite represented by a [Si6Al2O9H14(Fe(mu-O)Fe)] cluster model. The catalytic reactivity of such a binuclear species is compared with that of mononuclear Fe2+ and (FeO)(+) sites in ZSM-5 investigated in our earlier works at the same level of theory (J. Phys. Chem. C 2009, 113, 15307; 2010, 114, 12580). The activation en...
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M. F. Fellah, R. A. van Santen, and I. Önal, “Oxidation of Benzene to Phenol by N2O on an Fe2+-ZSM-5 Cluster: A Density Functional Theory Study,”
JOURNAL OF PHYSICAL CHEMISTRY C
, pp. 15307–15313, 2009, Accessed: 00, 2020. [Online]. Available: https://hdl.handle.net/11511/31056.