Hierarchical zeolites prepared by organosilane templating : a study of the synthesis mechanism and catalytic activity

A.J.J. Koekkoek, C.H.L. Tempelman, V. Degirmenci, M. Guo, Z. Feng, Can Li, E.J.M. Hensen

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Abstract

The crystallization of hierarchical ZSM-5 in the presence of the organosilane octadecyl-dimethyl-(3-trimethoxysilyl-propyl)-ammonium chloride as the mesoporogen was investigated as a function of time and temperature. The synthesis by this method proceeds in two steps. The rapid formation of a predominantly amorphous disordered mesoporous aluminosilicate precursor phase is followed by the formation of globular highly mesoporous zeolite particles involving dissolution of the precursor phase. It is difficult to completely convert the initial phase into the final hierarchical zeolite. This limits the amount of aluminium built into the MFI network and the resulting Brønsted acidity. In the presence of iron, more crystalline hierarchical zeolite is obtained. These Fe-containing zeolites are excellent catalysts for the selective oxidation of benzene to phenol. Their hierarchical pore structure leads to higher reaction rates due to increased mass transfer and increased catalyst longevity despite more substantial coke formation.
Original languageEnglish
Pages (from-to)96-111
Number of pages16
JournalCatalysis Today
Volume168
Issue number1
DOIs
Publication statusPublished - 2011

Fingerprint

Zeolites
Catalyst activity
Catalysts
Aluminosilicates
Pore structure
Acidity
Coke
Phenols
Reaction rates
Benzene
Dissolution
Mass transfer
Crystallization
Iron
Crystalline materials
Aluminum
Ammonium Chloride
Oxidation
Phenol
Temperature

Cite this

Koekkoek, A.J.J. ; Tempelman, C.H.L. ; Degirmenci, V. ; Guo, M. ; Feng, Z. ; Li, Can ; Hensen, E.J.M. / Hierarchical zeolites prepared by organosilane templating : a study of the synthesis mechanism and catalytic activity. In: Catalysis Today. 2011 ; Vol. 168, No. 1. pp. 96-111.
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Hierarchical zeolites prepared by organosilane templating : a study of the synthesis mechanism and catalytic activity. / Koekkoek, A.J.J.; Tempelman, C.H.L.; Degirmenci, V.; Guo, M.; Feng, Z.; Li, Can; Hensen, E.J.M.

In: Catalysis Today, Vol. 168, No. 1, 2011, p. 96-111.

Research output: Contribution to journalArticleAcademicpeer-review

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AU - Koekkoek, A.J.J.

AU - Tempelman, C.H.L.

AU - Degirmenci, V.

AU - Guo, M.

AU - Feng, Z.

AU - Li, Can

AU - Hensen, E.J.M.

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AB - The crystallization of hierarchical ZSM-5 in the presence of the organosilane octadecyl-dimethyl-(3-trimethoxysilyl-propyl)-ammonium chloride as the mesoporogen was investigated as a function of time and temperature. The synthesis by this method proceeds in two steps. The rapid formation of a predominantly amorphous disordered mesoporous aluminosilicate precursor phase is followed by the formation of globular highly mesoporous zeolite particles involving dissolution of the precursor phase. It is difficult to completely convert the initial phase into the final hierarchical zeolite. This limits the amount of aluminium built into the MFI network and the resulting Brønsted acidity. In the presence of iron, more crystalline hierarchical zeolite is obtained. These Fe-containing zeolites are excellent catalysts for the selective oxidation of benzene to phenol. Their hierarchical pore structure leads to higher reaction rates due to increased mass transfer and increased catalyst longevity despite more substantial coke formation.

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