Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation

Autores
Chanquia, Corina Mercedes; Cánepa, Analía Laura; Winkler, Elin Lilian; Rodríguez Castellon, Enrique; Casuscelli, Sandra Graciela; Eimer, Griselda Alejandra
Año de publicación
2016
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A multi-technique physicochemical investigation including UV–Vis-DRS, Raman spectroscopy, XPS, ESR and FTIRS with pyridine adsorption was performed to analyze the nature of different vanadium nanospecies present on MCM-41 type catalysts. By employing a direct hydrothermal synthesis, vanadium species were incorporated into siliceous structure mainly as tetrahedrally coordinated isolated Vδ+ ions, which would be located inside the wall and on the wall surface of the mesoporous channels. The coexistence of both vanadium oxidation states V4+ and V5+ was also revealed. Acidity measurements permitted to infer about the majority presence of Lewis acid sites, which increase with vanadium content. The catalytic performance of these materials was evaluated in the reaction of α-pinene oxidation with H2O2. The highest intrinsic activity of the sample with lower V loading was attributed to the high dispersion and efficiency of the isolated Vδ+ species that actuate as active sites. A mixture of reaction products arising from competitive processes of epoxidation and allylic oxidation was found.
Fil: Chanquia, Corina Mercedes. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Cánepa, Analía Laura. 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: Winkler, Elin Lilian. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Rodríguez Castellon, Enrique. Universidad de Málaga; España
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
Amorphous Materials
Nanostructures
Surface Properties
Oxidation
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
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CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
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oai:ri.conicet.gov.ar:11336/32030
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oai_identifier_str oai:ri.conicet.gov.ar:11336/32030
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidationChanquia, Corina MercedesCánepa, Analía LauraWinkler, Elin LilianRodríguez Castellon, EnriqueCasuscelli, Sandra GracielaEimer, Griselda AlejandraAmorphous MaterialsNanostructuresSurface PropertiesOxidationhttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2A multi-technique physicochemical investigation including UV–Vis-DRS, Raman spectroscopy, XPS, ESR and FTIRS with pyridine adsorption was performed to analyze the nature of different vanadium nanospecies present on MCM-41 type catalysts. By employing a direct hydrothermal synthesis, vanadium species were incorporated into siliceous structure mainly as tetrahedrally coordinated isolated Vδ+ ions, which would be located inside the wall and on the wall surface of the mesoporous channels. The coexistence of both vanadium oxidation states V4+ and V5+ was also revealed. Acidity measurements permitted to infer about the majority presence of Lewis acid sites, which increase with vanadium content. The catalytic performance of these materials was evaluated in the reaction of α-pinene oxidation with H2O2. The highest intrinsic activity of the sample with lower V loading was attributed to the high dispersion and efficiency of the isolated Vδ+ species that actuate as active sites. A mixture of reaction products arising from competitive processes of epoxidation and allylic oxidation was found.Fil: Chanquia, Corina Mercedes. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Cánepa, Analía Laura. 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: Winkler, Elin Lilian. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Rodríguez Castellon, Enrique. Universidad de Málaga; EspañaFil: 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 Science Sa2016-03info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/32030Eimer, Griselda Alejandra; Casuscelli, Sandra Graciela; Rodríguez Castellon, Enrique; Winkler, Elin Lilian; Cánepa, Analía Laura; Chanquia, Corina Mercedes; et al.; Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation; Elsevier Science Sa; Materials Chemistry and Physics; 175; 3-2016; 172-1790254-0584CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0254058416301626info:eu-repo/semantics/altIdentifier/doi/10.1016/j.matchemphys.2016.03.014info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:44:11Zoai:ri.conicet.gov.ar:11336/32030instacron: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 09:44:11.326CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation
title Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation
spellingShingle Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation
Chanquia, Corina Mercedes
Amorphous Materials
Nanostructures
Surface Properties
Oxidation
title_short Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation
title_full Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation
title_fullStr Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation
title_full_unstemmed Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation
title_sort Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation
dc.creator.none.fl_str_mv Chanquia, Corina Mercedes
Cánepa, Analía Laura
Winkler, Elin Lilian
Rodríguez Castellon, Enrique
Casuscelli, Sandra Graciela
Eimer, Griselda Alejandra
author Chanquia, Corina Mercedes
author_facet Chanquia, Corina Mercedes
Cánepa, Analía Laura
Winkler, Elin Lilian
Rodríguez Castellon, Enrique
Casuscelli, Sandra Graciela
Eimer, Griselda Alejandra
author_role author
author2 Cánepa, Analía Laura
Winkler, Elin Lilian
Rodríguez Castellon, Enrique
Casuscelli, Sandra Graciela
Eimer, Griselda Alejandra
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Amorphous Materials
Nanostructures
Surface Properties
Oxidation
topic Amorphous Materials
Nanostructures
Surface Properties
Oxidation
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv A multi-technique physicochemical investigation including UV–Vis-DRS, Raman spectroscopy, XPS, ESR and FTIRS with pyridine adsorption was performed to analyze the nature of different vanadium nanospecies present on MCM-41 type catalysts. By employing a direct hydrothermal synthesis, vanadium species were incorporated into siliceous structure mainly as tetrahedrally coordinated isolated Vδ+ ions, which would be located inside the wall and on the wall surface of the mesoporous channels. The coexistence of both vanadium oxidation states V4+ and V5+ was also revealed. Acidity measurements permitted to infer about the majority presence of Lewis acid sites, which increase with vanadium content. The catalytic performance of these materials was evaluated in the reaction of α-pinene oxidation with H2O2. The highest intrinsic activity of the sample with lower V loading was attributed to the high dispersion and efficiency of the isolated Vδ+ species that actuate as active sites. A mixture of reaction products arising from competitive processes of epoxidation and allylic oxidation was found.
Fil: Chanquia, Corina Mercedes. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Cánepa, Analía Laura. 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: Winkler, Elin Lilian. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Rodríguez Castellon, Enrique. Universidad de Málaga; España
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 A multi-technique physicochemical investigation including UV–Vis-DRS, Raman spectroscopy, XPS, ESR and FTIRS with pyridine adsorption was performed to analyze the nature of different vanadium nanospecies present on MCM-41 type catalysts. By employing a direct hydrothermal synthesis, vanadium species were incorporated into siliceous structure mainly as tetrahedrally coordinated isolated Vδ+ ions, which would be located inside the wall and on the wall surface of the mesoporous channels. The coexistence of both vanadium oxidation states V4+ and V5+ was also revealed. Acidity measurements permitted to infer about the majority presence of Lewis acid sites, which increase with vanadium content. The catalytic performance of these materials was evaluated in the reaction of α-pinene oxidation with H2O2. The highest intrinsic activity of the sample with lower V loading was attributed to the high dispersion and efficiency of the isolated Vδ+ species that actuate as active sites. A mixture of reaction products arising from competitive processes of epoxidation and allylic oxidation was found.
publishDate 2016
dc.date.none.fl_str_mv 2016-03
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/11336/32030
Eimer, Griselda Alejandra; Casuscelli, Sandra Graciela; Rodríguez Castellon, Enrique; Winkler, Elin Lilian; Cánepa, Analía Laura; Chanquia, Corina Mercedes; et al.; Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation; Elsevier Science Sa; Materials Chemistry and Physics; 175; 3-2016; 172-179
0254-0584
CONICET Digital
CONICET
url http://hdl.handle.net/11336/32030
identifier_str_mv Eimer, Griselda Alejandra; Casuscelli, Sandra Graciela; Rodríguez Castellon, Enrique; Winkler, Elin Lilian; Cánepa, Analía Laura; Chanquia, Corina Mercedes; et al.; Nature of active vanadium nanospecies in MCM-41 type catalysts for olefins oxidation; Elsevier Science Sa; Materials Chemistry and Physics; 175; 3-2016; 172-179
0254-0584
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0254058416301626
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.matchemphys.2016.03.014
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
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science Sa
publisher.none.fl_str_mv Elsevier Science Sa
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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