Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates

Autores
Briand, Laura Estefania; Jehng, Jih-Mirn; Cornaglia, Laura Maria; Hirt, Andrew M.; Wachs, Israel E.
Año de publicación
2003
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The present work investigates the number and nature of the surface active sites, selectivity and turnover frequency towards methanol selective oxidation of a series of bulk metal vanadates. The catalysts were synthesized through an organic route and characterized by laser Raman spectroscopy, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and specific surface area analysis (BET). The number of surface active sites (Ns) was determined by measuring the concentration of surface methoxy species adsorbed on the catalysts exposed to an atmosphere of 2000 ppm of methanol in helium at 100 °C. The specific activity values (TOFs) were calculated by normalizing the methanol oxidation reaction rate by the number of surface active sites probed by methanol chemisorption. The comparison of the methanol oxidation products distribution from bulk metal vanadates, pure V2O5 and corresponding metal oxides (NiO, MnO, etc.) strongly suggests that the metal vanadate catalysts consist of only surface vanadium oxide sites. The comparison of the TOF values demonstrated that bulk metal vanadates possess similar activity to monolayer vanadium oxide supported catalysts and are more active than bulk metal molybdates for methanol selective oxidation. Moreover, bulk metal vanadates are as active and selective as the commercial MoO3/Fe2(MoO4)3 catalysts at high methanol conversion. © 2002 Elsevier Science B.V. All rights reserved.
Fil: Briand, Laura Estefania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas "Dr. Jorge J. Ronco". Universidad Nacional de la Plata. Facultad de Ciencias Exactas. Centro de Investigación y Desarrollo en Ciencias Aplicadas; Argentina
Fil: Jehng, Jih-Mirn. National Chung Hsing University; República de China
Fil: Cornaglia, Laura Maria. Universidad Nacional del Litoral. Facultad de Ingeniería Química; Argentina
Fil: Hirt, Andrew M.. Materials Research Laboratories; Estados Unidos
Fil: Wachs, Israel E.. Lehigh University; Estados Unidos
Materia
Bulk Molybdates
Bulk Vanadates
Catalysts
Methanol Chemisorption
Methanol Oxidation
Supported Molybdenum Oxides
Supported Vanadium Oxides
Surface Active Sites
Turnover Frequency
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:11336/62557
Acceder
id CONICETDig_482ff7d314c7765673337fb23ba6eba0
oai_identifier_str oai:ri.conicet.gov.ar:11336/62557
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadatesBriand, Laura EstefaniaJehng, Jih-MirnCornaglia, Laura MariaHirt, Andrew M.Wachs, Israel E.Bulk MolybdatesBulk VanadatesCatalystsMethanol ChemisorptionMethanol OxidationSupported Molybdenum OxidesSupported Vanadium OxidesSurface Active SitesTurnover Frequencyhttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2The present work investigates the number and nature of the surface active sites, selectivity and turnover frequency towards methanol selective oxidation of a series of bulk metal vanadates. The catalysts were synthesized through an organic route and characterized by laser Raman spectroscopy, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and specific surface area analysis (BET). The number of surface active sites (Ns) was determined by measuring the concentration of surface methoxy species adsorbed on the catalysts exposed to an atmosphere of 2000 ppm of methanol in helium at 100 °C. The specific activity values (TOFs) were calculated by normalizing the methanol oxidation reaction rate by the number of surface active sites probed by methanol chemisorption. The comparison of the methanol oxidation products distribution from bulk metal vanadates, pure V2O5 and corresponding metal oxides (NiO, MnO, etc.) strongly suggests that the metal vanadate catalysts consist of only surface vanadium oxide sites. The comparison of the TOF values demonstrated that bulk metal vanadates possess similar activity to monolayer vanadium oxide supported catalysts and are more active than bulk metal molybdates for methanol selective oxidation. Moreover, bulk metal vanadates are as active and selective as the commercial MoO3/Fe2(MoO4)3 catalysts at high methanol conversion. © 2002 Elsevier Science B.V. All rights reserved.Fil: Briand, Laura Estefania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas "Dr. Jorge J. Ronco". Universidad Nacional de la Plata. Facultad de Ciencias Exactas. Centro de Investigación y Desarrollo en Ciencias Aplicadas; ArgentinaFil: Jehng, Jih-Mirn. National Chung Hsing University; República de ChinaFil: Cornaglia, Laura Maria. Universidad Nacional del Litoral. Facultad de Ingeniería Química; ArgentinaFil: Hirt, Andrew M.. Materials Research Laboratories; Estados UnidosFil: Wachs, Israel E.. Lehigh University; Estados UnidosElsevier Science2003-02info: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/11336/62557Briand, Laura Estefania; Jehng, Jih-Mirn; Cornaglia, Laura Maria; Hirt, Andrew M.; Wachs, Israel E.; Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates; Elsevier Science; Catalysis Today; 78; 1-4 SPEC.; 2-2003; 257-2680920-5861CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0920586102003504info:eu-repo/semantics/altIdentifier/doi/10.1016/S0920-5861(02)00350-4info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:39:42Zoai:ri.conicet.gov.ar:11336/62557instacron: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 09:39:42.476CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates
title Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates
spellingShingle Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates
Briand, Laura Estefania
Bulk Molybdates
Bulk Vanadates
Catalysts
Methanol Chemisorption
Methanol Oxidation
Supported Molybdenum Oxides
Supported Vanadium Oxides
Surface Active Sites
Turnover Frequency
title_short Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates
title_full Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates
title_fullStr Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates
title_full_unstemmed Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates
title_sort Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates
dc.creator.none.fl_str_mv Briand, Laura Estefania
Jehng, Jih-Mirn
Cornaglia, Laura Maria
Hirt, Andrew M.
Wachs, Israel E.
author Briand, Laura Estefania
author_facet Briand, Laura Estefania
Jehng, Jih-Mirn
Cornaglia, Laura Maria
Hirt, Andrew M.
Wachs, Israel E.
author_role author
author2 Jehng, Jih-Mirn
Cornaglia, Laura Maria
Hirt, Andrew M.
Wachs, Israel E.
author2_role author
author
author
author
dc.subject.none.fl_str_mv Bulk Molybdates
Bulk Vanadates
Catalysts
Methanol Chemisorption
Methanol Oxidation
Supported Molybdenum Oxides
Supported Vanadium Oxides
Surface Active Sites
Turnover Frequency
topic Bulk Molybdates
Bulk Vanadates
Catalysts
Methanol Chemisorption
Methanol Oxidation
Supported Molybdenum Oxides
Supported Vanadium Oxides
Surface Active Sites
Turnover Frequency
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv The present work investigates the number and nature of the surface active sites, selectivity and turnover frequency towards methanol selective oxidation of a series of bulk metal vanadates. The catalysts were synthesized through an organic route and characterized by laser Raman spectroscopy, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and specific surface area analysis (BET). The number of surface active sites (Ns) was determined by measuring the concentration of surface methoxy species adsorbed on the catalysts exposed to an atmosphere of 2000 ppm of methanol in helium at 100 °C. The specific activity values (TOFs) were calculated by normalizing the methanol oxidation reaction rate by the number of surface active sites probed by methanol chemisorption. The comparison of the methanol oxidation products distribution from bulk metal vanadates, pure V2O5 and corresponding metal oxides (NiO, MnO, etc.) strongly suggests that the metal vanadate catalysts consist of only surface vanadium oxide sites. The comparison of the TOF values demonstrated that bulk metal vanadates possess similar activity to monolayer vanadium oxide supported catalysts and are more active than bulk metal molybdates for methanol selective oxidation. Moreover, bulk metal vanadates are as active and selective as the commercial MoO3/Fe2(MoO4)3 catalysts at high methanol conversion. © 2002 Elsevier Science B.V. All rights reserved.
Fil: Briand, Laura Estefania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas "Dr. Jorge J. Ronco". Universidad Nacional de la Plata. Facultad de Ciencias Exactas. Centro de Investigación y Desarrollo en Ciencias Aplicadas; Argentina
Fil: Jehng, Jih-Mirn. National Chung Hsing University; República de China
Fil: Cornaglia, Laura Maria. Universidad Nacional del Litoral. Facultad de Ingeniería Química; Argentina
Fil: Hirt, Andrew M.. Materials Research Laboratories; Estados Unidos
Fil: Wachs, Israel E.. Lehigh University; Estados Unidos
description The present work investigates the number and nature of the surface active sites, selectivity and turnover frequency towards methanol selective oxidation of a series of bulk metal vanadates. The catalysts were synthesized through an organic route and characterized by laser Raman spectroscopy, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and specific surface area analysis (BET). The number of surface active sites (Ns) was determined by measuring the concentration of surface methoxy species adsorbed on the catalysts exposed to an atmosphere of 2000 ppm of methanol in helium at 100 °C. The specific activity values (TOFs) were calculated by normalizing the methanol oxidation reaction rate by the number of surface active sites probed by methanol chemisorption. The comparison of the methanol oxidation products distribution from bulk metal vanadates, pure V2O5 and corresponding metal oxides (NiO, MnO, etc.) strongly suggests that the metal vanadate catalysts consist of only surface vanadium oxide sites. The comparison of the TOF values demonstrated that bulk metal vanadates possess similar activity to monolayer vanadium oxide supported catalysts and are more active than bulk metal molybdates for methanol selective oxidation. Moreover, bulk metal vanadates are as active and selective as the commercial MoO3/Fe2(MoO4)3 catalysts at high methanol conversion. © 2002 Elsevier Science B.V. All rights reserved.
publishDate 2003
dc.date.none.fl_str_mv 2003-02
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/11336/62557
Briand, Laura Estefania; Jehng, Jih-Mirn; Cornaglia, Laura Maria; Hirt, Andrew M.; Wachs, Israel E.; Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates; Elsevier Science; Catalysis Today; 78; 1-4 SPEC.; 2-2003; 257-268
0920-5861
CONICET Digital
CONICET
url http://hdl.handle.net/11336/62557
identifier_str_mv Briand, Laura Estefania; Jehng, Jih-Mirn; Cornaglia, Laura Maria; Hirt, Andrew M.; Wachs, Israel E.; Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates; Elsevier Science; Catalysis Today; 78; 1-4 SPEC.; 2-2003; 257-268
0920-5861
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0920586102003504
info:eu-repo/semantics/altIdentifier/doi/10.1016/S0920-5861(02)00350-4
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
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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