Direct room-temperature synthesis of methyl-functionalized Ti-MCM-41 nanoparticles and their catalytic performance in epoxidation
Methyl-functionalized Ti-MCM-41 nanoparticles with a size of 80 to 160 nm (Me-Ti-MCM-41 NP) were directly prepared via a dilute solution route by the co-condensation of tetraethoxysilane and methylalkoxysilanes in sodium hydroxide medium at room temperature. The characterization results showed the e...
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| Veröffentlicht in: | Journal of catalysis Jg. 263; H. 1; S. 75 - 82 |
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| Sprache: | Englisch |
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01.04.2009
Elsevier Elsevier BV |
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| ISSN: | 0021-9517, 1090-2694 |
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| Abstract | Methyl-functionalized Ti-MCM-41 nanoparticles with a size of 80 to 160 nm (Me-Ti-MCM-41 NP) were directly prepared via a dilute solution route by the co-condensation of tetraethoxysilane and methylalkoxysilanes in sodium hydroxide medium at room temperature. The characterization results showed the existence of ordered hexagonal mesoporous structure and tetrahedral Ti species in the nanoparticles. In the epoxidation of cyclohexene with
tert-butyl hydroperoxide and aqueous H
2O
2, Me-Ti-MCM-41 NP samples displayed higher turnover frequencies (TOFs) for cyclohexene and initial reaction rates compared to Ti-MCM-41 and methyl-functionalized Ti-MCM-41 with normal particle size and to non-functionalized Ti-MCM-41 nanoparticles. Simultaneously, a higher selectivity for cyclohexene epoxide was observed in the case of aqueous H
2O
2, suggesting that the hydrolysis of cyclohexene epoxide with water is reduced on Me-Ti-MCM-41 NP samples. The improved catalytic behavior of Me-Ti-MCM-41 NP is discussed both in terms of the nanosize and methylation of the surface of the catalyst particles. The regeneration of Me-Ti-MCM-41 NP with
tert-butyl hydroperoxide solution was evaluated via washing and calcination approaches.
Methyl-functionalized Ti-MCM-41 nanoparticles display improved catalytic performance in the epoxidation of cyclohexene. |
|---|---|
| AbstractList | Methyl-functionalized Ti-MCM-41 nanoparticles with a size of 80 to 160 nm (Me-Ti-MCM-41 NP) were directly prepared via a dilute solution route by the co-condensation of tetraethoxysilane and methylalkoxysilanes in sodium hydroxide medium at room temperature. The characterization results showed the existence of ordered hexagonal mesoporous structure and tetrahedral Ti species in the nanoparticles. In the epoxidation of cyclohexene with tert-butyl hydroperoxide and aqueous H2O2 , Me-Ti-MCM-41 NP samples displayed higher turnover frequencies (TOFs) for cyclohexene and initial reaction rates compared to Ti-MCM-41 and methyl-functionalized Ti-MCM-41 with normal particle size and to non-functionalized Ti-MCM-41 nanoparticles. Simultaneously, a higher selectivity for cyclohexene epoxide was observed in the case of aqueous H2O2 , suggesting that the hydrolysis of cyclohexene epoxide with water is reduced on Me-Ti-MCM-41 NP samples. The improved catalytic behavior of Me-Ti-MCM-41 NP is discussed both in terms of the nanosize and methylation of the surface of the catalyst particles. The regeneration of Me-Ti-MCM-41 NP with tert-butyl hydroperoxide solution was evaluated via washing and calcination approaches. [PUBLICATION ABSTRACT] Methyl-functionalized Ti-MCM-41 nanoparticles with a size of 80 to 160 nm (Me-Ti-MCM-41 NP) were directly prepared via a dilute solution route by the co-condensation of tetraethoxysilane and methylalkoxysilanes in sodium hydroxide medium at room temperature. The characterization results showed the existence of ordered hexagonal mesoporous structure and tetrahedral Ti species in the nanoparticles. In the epoxidation of cyclohexene with tert-butyl hydroperoxide and aqueous H 2O 2, Me-Ti-MCM-41 NP samples displayed higher turnover frequencies (TOFs) for cyclohexene and initial reaction rates compared to Ti-MCM-41 and methyl-functionalized Ti-MCM-41 with normal particle size and to non-functionalized Ti-MCM-41 nanoparticles. Simultaneously, a higher selectivity for cyclohexene epoxide was observed in the case of aqueous H 2O 2, suggesting that the hydrolysis of cyclohexene epoxide with water is reduced on Me-Ti-MCM-41 NP samples. The improved catalytic behavior of Me-Ti-MCM-41 NP is discussed both in terms of the nanosize and methylation of the surface of the catalyst particles. The regeneration of Me-Ti-MCM-41 NP with tert-butyl hydroperoxide solution was evaluated via washing and calcination approaches. Methyl-functionalized Ti-MCM-41 nanoparticles display improved catalytic performance in the epoxidation of cyclohexene. |
| Author | Houthoofd, Kristof Liang, Duoduo Jacobs, Pierre A. Lin, Kaifeng Van Tendeloo, Gustaaf Pescarmona, Paolo P. |
| Author_xml | – sequence: 1 givenname: Kaifeng surname: Lin fullname: Lin, Kaifeng organization: COK, K.U. Leuven, Kasteelpark Arenberg 23-bus 2461, 3001 Heverlee, Belgium – sequence: 2 givenname: Paolo P. surname: Pescarmona fullname: Pescarmona, Paolo P. email: paolo.pescarmona@biw.kuleuven.be organization: COK, K.U. Leuven, Kasteelpark Arenberg 23-bus 2461, 3001 Heverlee, Belgium – sequence: 3 givenname: Kristof surname: Houthoofd fullname: Houthoofd, Kristof organization: COK, K.U. Leuven, Kasteelpark Arenberg 23-bus 2461, 3001 Heverlee, Belgium – sequence: 4 givenname: Duoduo surname: Liang fullname: Liang, Duoduo organization: EMAT, UA, Groenenborglaan 171, 2020 Antwerpen, Belgium – sequence: 5 givenname: Gustaaf surname: Van Tendeloo fullname: Van Tendeloo, Gustaaf organization: EMAT, UA, Groenenborglaan 171, 2020 Antwerpen, Belgium – sequence: 6 givenname: Pierre A. surname: Jacobs fullname: Jacobs, Pierre A. organization: COK, K.U. Leuven, Kasteelpark Arenberg 23-bus 2461, 3001 Heverlee, Belgium |
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| Keywords | Dilute solution route Shorter mesoporous channels Aqueous H 2O 2 Methyl-functionalized Ti-MCM-41 nanoparticles Epoxidation of cyclohexene tert-Butyl hydroperoxide Water Particle size Hydrogen peroxide Nanoparticle Washing Selectivity Condensation Porous material Sodium hydroxide Characterization Particle Synthesis Dilute solution Epoxidation Aqueous H2O2 Structure Catalytic reaction Organic hydroperoxide Reaction rate Mesoporosity Hydrolysis Heterogeneous catalysis Regeneration Epoxide Frequency Methylation Ethylenic compound Catalyst Room temperature |
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| Snippet | Methyl-functionalized Ti-MCM-41 nanoparticles with a size of 80 to 160 nm (Me-Ti-MCM-41 NP) were directly prepared via a dilute solution route by the... |
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| SubjectTerms | Aqueous H 2O 2 Catalysis Chemical synthesis Chemistry Colloidal state and disperse state Dilute solution route Epoxidation of cyclohexene Exact sciences and technology General and physical chemistry Methyl-functionalized Ti-MCM-41 nanoparticles Molecular structure Nanoparticles Physical and chemical studies. Granulometry. Electrokinetic phenomena Porous materials Shorter mesoporous channels tert-Butyl hydroperoxide Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry |
| Title | Direct room-temperature synthesis of methyl-functionalized Ti-MCM-41 nanoparticles and their catalytic performance in epoxidation |
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