Immobilization of Jacobsen type catalysts on modified silica

RESUMEN: Several immobilized Jacobsen type catalysts were covalently anchored on modified SiO2 using 3-aminopropyltriethoxysilane (3-APTES) as a reactive surface modifier. Characterization of the heterogeneous catalysts, as well as their precursors, by FTIR, DR UV–VIS, TGA and AAS confirms the succe...

Full description

Autores:
Grajales González, Edwing Javier
Vásquez Agudelo, Santiago
Montes de Correa, Consuelo
Tipo de recurso:
Article of investigation
Fecha de publicación:
2011
Institución:
Universidad de Antioquia
Repositorio:
Repositorio UdeA
Idioma:
eng
OAI Identifier:
oai:bibliotecadigital.udea.edu.co:10495/5436
Acceso en línea:
http://hdl.handle.net/10495/5436
Palabra clave:
Catalizadores
Catalizador de Jacobsen
Rights
openAccess
License
https://creativecommons.org/licenses/by-nc-sa/4.0/
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repository_id_str
dc.title.spa.fl_str_mv Immobilization of Jacobsen type catalysts on modified silica
dc.title.translated.spa.fl_str_mv Inmovilización de catalizadores tipo Jacobsen en sílica modificada
title Immobilization of Jacobsen type catalysts on modified silica
spellingShingle Immobilization of Jacobsen type catalysts on modified silica
Catalizadores
Catalizador de Jacobsen
title_short Immobilization of Jacobsen type catalysts on modified silica
title_full Immobilization of Jacobsen type catalysts on modified silica
title_fullStr Immobilization of Jacobsen type catalysts on modified silica
title_full_unstemmed Immobilization of Jacobsen type catalysts on modified silica
title_sort Immobilization of Jacobsen type catalysts on modified silica
dc.creator.fl_str_mv Grajales González, Edwing Javier
Vásquez Agudelo, Santiago
Montes de Correa, Consuelo
dc.contributor.author.none.fl_str_mv Grajales González, Edwing Javier
Vásquez Agudelo, Santiago
Montes de Correa, Consuelo
dc.contributor.researchgroup.spa.fl_str_mv Catálisis Ambiental
dc.subject.none.fl_str_mv Catalizadores
Catalizador de Jacobsen
topic Catalizadores
Catalizador de Jacobsen
description RESUMEN: Several immobilized Jacobsen type catalysts were covalently anchored on modified SiO2 using 3-aminopropyltriethoxysilane (3-APTES) as a reactive surface modifier. Characterization of the heterogeneous catalysts, as well as their precursors, by FTIR, DR UV–VIS, TGA and AAS confirms the successful immobilization of chiral Mn(III) salen complexes. These catalysts were examined for the diastereoselective epoxidation of R-(+)-limonene with in situ generated dimethyldioxirane (DMD) as oxidizing agent, yielding 1,2-epoxide as the main product. When compared to homogeneous catalysts, under similar experimental conditions, only a slight selectivity decrease over heterogeneous catalysts was observed. The immobilized catalysts were used three times maintaining the initial selectivity. However, after reusing them more than three times, selectivity to 1,2-epoxide decreased. FTIR results suggest partial degradation of the catalytic species. Despite the immobilization method was chosen to minimize changes in the structure of the homogeneous catalysts the diastereoselectivity (d.e.) of heterogeneous catalysts underwent a remarkable decay.
publishDate 2011
dc.date.issued.none.fl_str_mv 2011
dc.date.accessioned.none.fl_str_mv 2016-11-18T20:14:42Z
dc.date.available.none.fl_str_mv 2016-11-18T20:14:42Z
dc.type.spa.fl_str_mv Artículo de investigación
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dc.identifier.citation.spa.fl_str_mv J. A. Cubillos, E. J. Grajales, S. Vásquez and C. Montes, "Immobilization of Jacobsen type catalysts on modified silica", Rev. Fac. Ing. Univ. Antioquia, no. 57, pp. 38-48, 2011.
dc.identifier.issn.none.fl_str_mv 0120-6230
dc.identifier.uri.none.fl_str_mv http://hdl.handle.net/10495/5436
dc.identifier.eissn.none.fl_str_mv 2422-2844
identifier_str_mv J. A. Cubillos, E. J. Grajales, S. Vásquez and C. Montes, "Immobilization of Jacobsen type catalysts on modified silica", Rev. Fac. Ing. Univ. Antioquia, no. 57, pp. 38-48, 2011.
0120-6230
2422-2844
url http://hdl.handle.net/10495/5436
dc.language.iso.spa.fl_str_mv eng
language eng
dc.relation.ispartofjournalabbrev.spa.fl_str_mv Rev. Fac. Ing. Univ. Antioquia
dc.relation.citationendpage.spa.fl_str_mv 48
dc.relation.citationissue.spa.fl_str_mv 57
dc.relation.citationstartpage.spa.fl_str_mv 38
dc.relation.ispartofjournal.spa.fl_str_mv Revista Facultad de Ingeniería Universidad de Antioquia
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dc.publisher.spa.fl_str_mv Universidad de Antioquia, Facultad de Ingeniería
dc.publisher.place.spa.fl_str_mv Medellín, Colombia
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spelling Grajales González, Edwing JavierVásquez Agudelo, SantiagoMontes de Correa, ConsueloCatálisis Ambiental2016-11-18T20:14:42Z2016-11-18T20:14:42Z2011J. A. Cubillos, E. J. Grajales, S. Vásquez and C. Montes, "Immobilization of Jacobsen type catalysts on modified silica", Rev. Fac. Ing. Univ. Antioquia, no. 57, pp. 38-48, 2011.0120-6230http://hdl.handle.net/10495/54362422-2844RESUMEN: Several immobilized Jacobsen type catalysts were covalently anchored on modified SiO2 using 3-aminopropyltriethoxysilane (3-APTES) as a reactive surface modifier. Characterization of the heterogeneous catalysts, as well as their precursors, by FTIR, DR UV–VIS, TGA and AAS confirms the successful immobilization of chiral Mn(III) salen complexes. These catalysts were examined for the diastereoselective epoxidation of R-(+)-limonene with in situ generated dimethyldioxirane (DMD) as oxidizing agent, yielding 1,2-epoxide as the main product. When compared to homogeneous catalysts, under similar experimental conditions, only a slight selectivity decrease over heterogeneous catalysts was observed. The immobilized catalysts were used three times maintaining the initial selectivity. However, after reusing them more than three times, selectivity to 1,2-epoxide decreased. FTIR results suggest partial degradation of the catalytic species. Despite the immobilization method was chosen to minimize changes in the structure of the homogeneous catalysts the diastereoselectivity (d.e.) of heterogeneous catalysts underwent a remarkable decay.ABSTRACT: Varios catalizadores tipo Jacobsen fueron inmovilizados por enlace covalente en sílica amorfa previamente funcionalizada con 3-aminopropiltrietoxisilano (3-APTES). La caracterización de estos catalizadores y sus precursores por FTIR, DR UV–VIS, TGA y AAS permitió confirmar la inmovilización de los complejos de salen de Mn(III). Los catalizadores heterogéneos se evaluaron en la epoxidación diastereoselectiva de R-(+)-limoneno utilizando dimetildioxirano (DMD) generado in situ como agente oxidante, obteniéndose 1,2-epóxido como producto mayoritario. Bajo las mismas condiciones de reacción, los catalizadores heterogéneos mostraron una leve reducción en la selectividad en comparación con el catalizador homogéneo. La selectividad inicial se mantuvo en tres ensayos consecutivos de los catalizadores. Sin embargo, después de tres reusos, se observó pérdida de selectividad del catalizador inmovilizado. Los resultados FTIR sugieren la degradación parcial del catalizador heterogenizado. A pesar de que el método de inmovilización se seleccionó de tal manera que se minimizaran los cambios en la estructura del catalizador homogéneo, el exceso diastereomérico (d.e.) se redujo considerablemente con los catalizadores inmovilizados.10application/pdfengUniversidad de Antioquia, Facultad de IngenieríaMedellín, Colombiahttps://creativecommons.org/licenses/by-nc-sa/4.0/https://creativecommons.org/licenses/by-nc-sa/2.5/co/Atribución-NoComercial-CompartirIgual 2.5 Colombia (CC BY-NC-SA 2.5 CO)info:eu-repo/semantics/openAccesshttp://purl.org/coar/access_right/c_abf2CatalizadoresCatalizador de JacobsenImmobilization of Jacobsen type catalysts on modified silicaInmovilización de catalizadores tipo Jacobsen en sílica modificadaArtículo de investigaciónhttp://purl.org/coar/resource_type/c_2df8fbb1https://purl.org/redcol/resource_type/ARThttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionRev. Fac. Ing. Univ. 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