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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/32027
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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 Técnicas2025-09-03T09:44:16Zoai: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:34982025-09-03 09:44:17.155CONICET 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 |
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CONICET Digital (CONICET) |
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CONICET Digital (CONICET) |
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Consejo Nacional de Investigaciones Científicas y Técnicas |
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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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1842268655901999104 |
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13.13397 |