Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam

Autores
Vaschetto, Eliana Gabriela; Pecchi Sanchez, Gina Angela; Casuscelli, Sandra Graciela; Eimer, Griselda Alejandra
Año de publicación
2014
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Al-MCM-41 type nano-structured catalysts with different Al contents were prepared by direct hydrothermal synthesis. All the materials were characterized by XRD, N2 adsorption, TEM, SEM, ICP-OES, FT-IR and adsorption of pyridine coupled to FT-IR spectroscopy. The relationship between the Al contents in the synthesis gel and final solid, the degree of Al introduction in tetrahedral coordination into the framework, the formation of nest silanols and the relative density of the acidic hydroxyl sites has been exhaustively analyzed. We could corroborate that hydroxyl groups present in silanol nests are the direct responsible of the weakly acid character of our materials. Moreover, a critical concentration of framework Al seems to be necessary to generate such nests, after which the acid sites density is strongly increased, according the framework Al amount increasing. The enhancement in the density of acidic nest silanols (active sites for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam) reached by increasing the Al content, permitted to us achieve a cyclohexanone oxime conversion about 66%. The ɛ-caprolactam selectivity was 100% for all the evaluated catalysts, indicating that the acidic strength was kept sufficiently weak to not catalyze the formation of by-products.
Fil: Vaschetto, Eliana Gabriela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Pecchi Sanchez, Gina Angela. Universidad de Concepción; Chile
Fil: Casuscelli, Sandra Graciela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Eimer, Griselda Alejandra. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Materia
Al Contents
Al-Mcm-41
Silanol Nests
Acidic Strength
Ɛ-Caprolactam
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/32027
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/32027
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactamVaschetto, Eliana GabrielaPecchi Sanchez, Gina AngelaCasuscelli, Sandra GracielaEimer, Griselda AlejandraAl ContentsAl-Mcm-41Silanol NestsAcidic StrengthƐ-Caprolactamhttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2Al-MCM-41 type nano-structured catalysts with different Al contents were prepared by direct hydrothermal synthesis. All the materials were characterized by XRD, N2 adsorption, TEM, SEM, ICP-OES, FT-IR and adsorption of pyridine coupled to FT-IR spectroscopy. The relationship between the Al contents in the synthesis gel and final solid, the degree of Al introduction in tetrahedral coordination into the framework, the formation of nest silanols and the relative density of the acidic hydroxyl sites has been exhaustively analyzed. We could corroborate that hydroxyl groups present in silanol nests are the direct responsible of the weakly acid character of our materials. Moreover, a critical concentration of framework Al seems to be necessary to generate such nests, after which the acid sites density is strongly increased, according the framework Al amount increasing. The enhancement in the density of acidic nest silanols (active sites for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam) reached by increasing the Al content, permitted to us achieve a cyclohexanone oxime conversion about 66%. The ɛ-caprolactam selectivity was 100% for all the evaluated catalysts, indicating that the acidic strength was kept sufficiently weak to not catalyze the formation of by-products.Fil: Vaschetto, Eliana Gabriela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; ArgentinaFil: Pecchi Sanchez, Gina Angela. Universidad de Concepción; ChileFil: Casuscelli, Sandra Graciela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; ArgentinaFil: Eimer, Griselda Alejandra. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; ArgentinaElsevier Science2014-08info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/32027Eimer, Griselda Alejandra; Casuscelli, Sandra Graciela; Pecchi Sanchez, Gina Angela; Vaschetto, Eliana Gabriela; Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam; Elsevier Science; Microporous and Mesoporous Materials; 200; 8-2014; 110-1161387-1811CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.micromeso.2014.08.030info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S1387181114004648info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:34:00Zoai:ri.conicet.gov.ar:11336/32027instacron: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:34982025-09-29 09:34:00.636CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam
title Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam
spellingShingle Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam
Vaschetto, Eliana Gabriela
Al Contents
Al-Mcm-41
Silanol Nests
Acidic Strength
Ɛ-Caprolactam
title_short Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam
title_full Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam
title_fullStr Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam
title_full_unstemmed Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam
title_sort Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam
dc.creator.none.fl_str_mv Vaschetto, Eliana Gabriela
Pecchi Sanchez, Gina Angela
Casuscelli, Sandra Graciela
Eimer, Griselda Alejandra
author Vaschetto, Eliana Gabriela
author_facet Vaschetto, Eliana Gabriela
Pecchi Sanchez, Gina Angela
Casuscelli, Sandra Graciela
Eimer, Griselda Alejandra
author_role author
author2 Pecchi Sanchez, Gina Angela
Casuscelli, Sandra Graciela
Eimer, Griselda Alejandra
author2_role author
author
author
dc.subject.none.fl_str_mv Al Contents
Al-Mcm-41
Silanol Nests
Acidic Strength
Ɛ-Caprolactam
topic Al Contents
Al-Mcm-41
Silanol Nests
Acidic Strength
Ɛ-Caprolactam
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv Al-MCM-41 type nano-structured catalysts with different Al contents were prepared by direct hydrothermal synthesis. All the materials were characterized by XRD, N2 adsorption, TEM, SEM, ICP-OES, FT-IR and adsorption of pyridine coupled to FT-IR spectroscopy. The relationship between the Al contents in the synthesis gel and final solid, the degree of Al introduction in tetrahedral coordination into the framework, the formation of nest silanols and the relative density of the acidic hydroxyl sites has been exhaustively analyzed. We could corroborate that hydroxyl groups present in silanol nests are the direct responsible of the weakly acid character of our materials. Moreover, a critical concentration of framework Al seems to be necessary to generate such nests, after which the acid sites density is strongly increased, according the framework Al amount increasing. The enhancement in the density of acidic nest silanols (active sites for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam) reached by increasing the Al content, permitted to us achieve a cyclohexanone oxime conversion about 66%. The ɛ-caprolactam selectivity was 100% for all the evaluated catalysts, indicating that the acidic strength was kept sufficiently weak to not catalyze the formation of by-products.
Fil: Vaschetto, Eliana Gabriela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Pecchi Sanchez, Gina Angela. Universidad de Concepción; Chile
Fil: Casuscelli, Sandra Graciela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Eimer, Griselda Alejandra. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
description Al-MCM-41 type nano-structured catalysts with different Al contents were prepared by direct hydrothermal synthesis. All the materials were characterized by XRD, N2 adsorption, TEM, SEM, ICP-OES, FT-IR and adsorption of pyridine coupled to FT-IR spectroscopy. The relationship between the Al contents in the synthesis gel and final solid, the degree of Al introduction in tetrahedral coordination into the framework, the formation of nest silanols and the relative density of the acidic hydroxyl sites has been exhaustively analyzed. We could corroborate that hydroxyl groups present in silanol nests are the direct responsible of the weakly acid character of our materials. Moreover, a critical concentration of framework Al seems to be necessary to generate such nests, after which the acid sites density is strongly increased, according the framework Al amount increasing. The enhancement in the density of acidic nest silanols (active sites for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam) reached by increasing the Al content, permitted to us achieve a cyclohexanone oxime conversion about 66%. The ɛ-caprolactam selectivity was 100% for all the evaluated catalysts, indicating that the acidic strength was kept sufficiently weak to not catalyze the formation of by-products.
publishDate 2014
dc.date.none.fl_str_mv 2014-08
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/11336/32027
Eimer, Griselda Alejandra; Casuscelli, Sandra Graciela; Pecchi Sanchez, Gina Angela; Vaschetto, Eliana Gabriela; Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam; Elsevier Science; Microporous and Mesoporous Materials; 200; 8-2014; 110-116
1387-1811
CONICET Digital
CONICET
url http://hdl.handle.net/11336/32027
identifier_str_mv Eimer, Griselda Alejandra; Casuscelli, Sandra Graciela; Pecchi Sanchez, Gina Angela; Vaschetto, Eliana Gabriela; Nature of the active sites in Al-MCM-41 nano-structured catalysts for the selective rearrangement of cyclohexanone oxime toward ɛ-caprolactam; Elsevier Science; Microporous and Mesoporous Materials; 200; 8-2014; 110-116
1387-1811
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.micromeso.2014.08.030
info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S1387181114004648
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
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
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score 13.070432

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