Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement

Autores
Vaschetto, Eliana Gabriela; Monti, Gustavo Antonio; Herrero, Eduardo Renato; Casuscelli, Sandra Graciela; Eimer, Griselda Alejandra
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Al-containing mesoporous catalysts with MCM-41 structure and high surface area have been successfully prepared by direct hydrothermal synthesis. Various characterization techniques including XRD, N2 adsorption, ICP-OES, NMR, FT-IR and adsorption of pyridine coupled to FT-IR spectroscopy were employed. A detailed study about the relationships existing between the different synthesis parameters, the physico-chemical properties, the acid behavior and the catalytic performance is presented in this contribution. We have suggested that the active sites for the Beckmann rearrangement of cyclohexanone oxime are nest silanols (at structural defects) of very weak Brønsted acid character, which is associated with the introduction of Al into the mesoporous framework. In all the cases, employing soft reaction conditions, we have obtained selectivity to caprolactam of 100%. Finally, a Si/Al initial molar ratio of 20, a stirring of synthesis gel for 7 h and a hydrothermal treatment of 6 days seem to be the optimum synthesis conditions to obtain the highest framework Al incorporation, more abundant weak acid sites (silanol nests) and maximum yield for -caprolactam.
Fil: Vaschetto, Eliana Gabriela. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; Argentina
Fil: Monti, Gustavo Antonio. Universidad Nacional de Córdoba. Facultad de Matemática, Astronomía y Física; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Herrero, Eduardo Renato. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; Argentina
Fil: Casuscelli, Sandra Graciela. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; Argentina
Fil: Eimer, Griselda Alejandra. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; Argentina
Materia
Mesoporous Materials
Al-Mcm-41
Synthesis Time
Gel Stirring
Caprolactam
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/10995
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/10995
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangementVaschetto, Eliana GabrielaMonti, Gustavo AntonioHerrero, Eduardo RenatoCasuscelli, Sandra GracielaEimer, Griselda AlejandraMesoporous MaterialsAl-Mcm-41Synthesis TimeGel StirringCaprolactamhttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2Al-containing mesoporous catalysts with MCM-41 structure and high surface area have been successfully prepared by direct hydrothermal synthesis. Various characterization techniques including XRD, N2 adsorption, ICP-OES, NMR, FT-IR and adsorption of pyridine coupled to FT-IR spectroscopy were employed. A detailed study about the relationships existing between the different synthesis parameters, the physico-chemical properties, the acid behavior and the catalytic performance is presented in this contribution. We have suggested that the active sites for the Beckmann rearrangement of cyclohexanone oxime are nest silanols (at structural defects) of very weak Brønsted acid character, which is associated with the introduction of Al into the mesoporous framework. In all the cases, employing soft reaction conditions, we have obtained selectivity to caprolactam of 100%. Finally, a Si/Al initial molar ratio of 20, a stirring of synthesis gel for 7 h and a hydrothermal treatment of 6 days seem to be the optimum synthesis conditions to obtain the highest framework Al incorporation, more abundant weak acid sites (silanol nests) and maximum yield for -caprolactam.Fil: Vaschetto, Eliana Gabriela. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; ArgentinaFil: Monti, Gustavo Antonio. Universidad Nacional de Córdoba. Facultad de Matemática, Astronomía y Física; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Herrero, Eduardo Renato. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; ArgentinaFil: Casuscelli, Sandra Graciela. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; ArgentinaFil: Eimer, Griselda Alejandra. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; ArgentinaElsevier Science2013-02info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/10995Vaschetto, Eliana Gabriela; Monti, Gustavo Antonio; Herrero, Eduardo Renato; Casuscelli, Sandra Graciela; Eimer, Griselda Alejandra; Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement; Elsevier Science; Applied Catalysis A: General; 453; 2-2013; 391-4020926-860Xenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2012.12.016info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0926860X12007752info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T10:07:24Zoai:ri.conicet.gov.ar:11336/10995instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-03 10:07:24.81CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement
title Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement
spellingShingle Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement
Vaschetto, Eliana Gabriela
Mesoporous Materials
Al-Mcm-41
Synthesis Time
Gel Stirring
Caprolactam
title_short Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement
title_full Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement
title_fullStr Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement
title_full_unstemmed Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement
title_sort Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement
dc.creator.none.fl_str_mv Vaschetto, Eliana Gabriela
Monti, Gustavo Antonio
Herrero, Eduardo Renato
Casuscelli, Sandra Graciela
Eimer, Griselda Alejandra
author Vaschetto, Eliana Gabriela
author_facet Vaschetto, Eliana Gabriela
Monti, Gustavo Antonio
Herrero, Eduardo Renato
Casuscelli, Sandra Graciela
Eimer, Griselda Alejandra
author_role author
author2 Monti, Gustavo Antonio
Herrero, Eduardo Renato
Casuscelli, Sandra Graciela
Eimer, Griselda Alejandra
author2_role author
author
author
author
dc.subject.none.fl_str_mv Mesoporous Materials
Al-Mcm-41
Synthesis Time
Gel Stirring
Caprolactam
topic Mesoporous Materials
Al-Mcm-41
Synthesis Time
Gel Stirring
Caprolactam
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv Al-containing mesoporous catalysts with MCM-41 structure and high surface area have been successfully prepared by direct hydrothermal synthesis. Various characterization techniques including XRD, N2 adsorption, ICP-OES, NMR, FT-IR and adsorption of pyridine coupled to FT-IR spectroscopy were employed. A detailed study about the relationships existing between the different synthesis parameters, the physico-chemical properties, the acid behavior and the catalytic performance is presented in this contribution. We have suggested that the active sites for the Beckmann rearrangement of cyclohexanone oxime are nest silanols (at structural defects) of very weak Brønsted acid character, which is associated with the introduction of Al into the mesoporous framework. In all the cases, employing soft reaction conditions, we have obtained selectivity to caprolactam of 100%. Finally, a Si/Al initial molar ratio of 20, a stirring of synthesis gel for 7 h and a hydrothermal treatment of 6 days seem to be the optimum synthesis conditions to obtain the highest framework Al incorporation, more abundant weak acid sites (silanol nests) and maximum yield for -caprolactam.
Fil: Vaschetto, Eliana Gabriela. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; Argentina
Fil: Monti, Gustavo Antonio. Universidad Nacional de Córdoba. Facultad de Matemática, Astronomía y Física; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Herrero, Eduardo Renato. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; Argentina
Fil: Casuscelli, Sandra Graciela. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; Argentina
Fil: Eimer, Griselda Alejandra. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Centro Cientifico Tecnologico Cordoba. Centro de Investigacion y Tecnologia Quimica; Argentina. Universidad Tecnologica Nacional. Facultad Regional Cordoba; Argentina
description Al-containing mesoporous catalysts with MCM-41 structure and high surface area have been successfully prepared by direct hydrothermal synthesis. Various characterization techniques including XRD, N2 adsorption, ICP-OES, NMR, FT-IR and adsorption of pyridine coupled to FT-IR spectroscopy were employed. A detailed study about the relationships existing between the different synthesis parameters, the physico-chemical properties, the acid behavior and the catalytic performance is presented in this contribution. We have suggested that the active sites for the Beckmann rearrangement of cyclohexanone oxime are nest silanols (at structural defects) of very weak Brønsted acid character, which is associated with the introduction of Al into the mesoporous framework. In all the cases, employing soft reaction conditions, we have obtained selectivity to caprolactam of 100%. Finally, a Si/Al initial molar ratio of 20, a stirring of synthesis gel for 7 h and a hydrothermal treatment of 6 days seem to be the optimum synthesis conditions to obtain the highest framework Al incorporation, more abundant weak acid sites (silanol nests) and maximum yield for -caprolactam.
publishDate 2013
dc.date.none.fl_str_mv 2013-02
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/10995
Vaschetto, Eliana Gabriela; Monti, Gustavo Antonio; Herrero, Eduardo Renato; Casuscelli, Sandra Graciela; Eimer, Griselda Alejandra; Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement; Elsevier Science; Applied Catalysis A: General; 453; 2-2013; 391-402
0926-860X
url http://hdl.handle.net/11336/10995
identifier_str_mv Vaschetto, Eliana Gabriela; Monti, Gustavo Antonio; Herrero, Eduardo Renato; Casuscelli, Sandra Graciela; Eimer, Griselda Alejandra; Influence of the synthesis conditions on the physicochemical properties and acidity of Al-MCM-41 as catalysts for the cyclohexanone oxime rearrangement; Elsevier Science; Applied Catalysis A: General; 453; 2-2013; 391-402
0926-860X
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2012.12.016
info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0926860X12007752
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science
publisher.none.fl_str_mv Elsevier Science
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
_version_ 1842270002868125696
score 13.13397

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