Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol che...

Autores
Briand, Laura Estefania; Farneth, William E.; Wachs, Israel E.
Año de publicación
2000
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A detailed study of the methanol chemisorption and oxidation processes on oxide surfaces allowed the development of a method to quantify the number of surface active sites (Ns) of metal oxide catalysts. In situ infrared analysis during methanol adsorption showed that molecular methanol and surface methoxy species are co-adsorbed on an oxide surface at room temperature, but only surface methoxy species are formed at 100°C. Thermal stability and products of decomposition of the adsorbed species were determined with temperature programmed reaction spectroscopy (TPRS) experiments. Controlled adsorption with methanol doses resulted in a stable monolayer of surface methoxy species on the oxide surfaces. The stoichiometry of methanol chemisorption resulted in one surface methoxy adsorbed per three Mo atoms for polymerized surface molybdenum oxide structures, regardless of surface molybdenum oxide coordination. The activity of the catalysts per surface active sites (turnover frequencies TOF) was calculated in order to quantitatively compare the reactivity of a series of monolayer supported molybdenum oxide catalysts. The TOF value trends reflect the influence of the bridging Mo-O-Support bond and the electronegativity of the metal cation of the oxide support.
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 ; Argentina
Fil: Farneth, William E.. E. I. du Pont de Nemours and Company; Estados Unidos
Fil: Wachs, Israel E.. Lehigh University; Estados Unidos
Materia
Molybdenum Oxide Catalyst
Surface Active Sites
Methanol Oxidation
Methanol Chemisorption;
Turnover Frequency
Tprs
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:11336/42624
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/42624
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalystsBriand, Laura EstefaniaFarneth, William E.Wachs, Israel E.Molybdenum Oxide CatalystSurface Active SitesMethanol OxidationMethanol Chemisorption;Turnover FrequencyTprshttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2A detailed study of the methanol chemisorption and oxidation processes on oxide surfaces allowed the development of a method to quantify the number of surface active sites (Ns) of metal oxide catalysts. In situ infrared analysis during methanol adsorption showed that molecular methanol and surface methoxy species are co-adsorbed on an oxide surface at room temperature, but only surface methoxy species are formed at 100°C. Thermal stability and products of decomposition of the adsorbed species were determined with temperature programmed reaction spectroscopy (TPRS) experiments. Controlled adsorption with methanol doses resulted in a stable monolayer of surface methoxy species on the oxide surfaces. The stoichiometry of methanol chemisorption resulted in one surface methoxy adsorbed per three Mo atoms for polymerized surface molybdenum oxide structures, regardless of surface molybdenum oxide coordination. The activity of the catalysts per surface active sites (turnover frequencies TOF) was calculated in order to quantitatively compare the reactivity of a series of monolayer supported molybdenum oxide catalysts. The TOF value trends reflect the influence of the bridging Mo-O-Support bond and the electronegativity of the metal cation of the oxide support.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 ; ArgentinaFil: Farneth, William E.. E. I. du Pont de Nemours and Company; Estados UnidosFil: Wachs, Israel E.. Lehigh University; Estados UnidosElsevier Science2000-11info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/42624Briand, Laura Estefania; Farneth, William E.; Wachs, Israel E.; Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts; Elsevier Science; Catalysis Today; 62; 2-3; 11-2000; 219-2290920-5861CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/S0920-5861(00)00423-5info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0920586100004235info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:48:33Zoai:ri.conicet.gov.ar:11336/42624instacron: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 09:48:33.702CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts
title Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts
spellingShingle Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts
Briand, Laura Estefania
Molybdenum Oxide Catalyst
Surface Active Sites
Methanol Oxidation
Methanol Chemisorption;
Turnover Frequency
Tprs
title_short Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts
title_full Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts
title_fullStr Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts
title_full_unstemmed Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts
title_sort Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts
dc.creator.none.fl_str_mv Briand, Laura Estefania
Farneth, William E.
Wachs, Israel E.
author Briand, Laura Estefania
author_facet Briand, Laura Estefania
Farneth, William E.
Wachs, Israel E.
author_role author
author2 Farneth, William E.
Wachs, Israel E.
author2_role author
author
dc.subject.none.fl_str_mv Molybdenum Oxide Catalyst
Surface Active Sites
Methanol Oxidation
Methanol Chemisorption;
Turnover Frequency
Tprs
topic Molybdenum Oxide Catalyst
Surface Active Sites
Methanol Oxidation
Methanol Chemisorption;
Turnover Frequency
Tprs
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv A detailed study of the methanol chemisorption and oxidation processes on oxide surfaces allowed the development of a method to quantify the number of surface active sites (Ns) of metal oxide catalysts. In situ infrared analysis during methanol adsorption showed that molecular methanol and surface methoxy species are co-adsorbed on an oxide surface at room temperature, but only surface methoxy species are formed at 100°C. Thermal stability and products of decomposition of the adsorbed species were determined with temperature programmed reaction spectroscopy (TPRS) experiments. Controlled adsorption with methanol doses resulted in a stable monolayer of surface methoxy species on the oxide surfaces. The stoichiometry of methanol chemisorption resulted in one surface methoxy adsorbed per three Mo atoms for polymerized surface molybdenum oxide structures, regardless of surface molybdenum oxide coordination. The activity of the catalysts per surface active sites (turnover frequencies TOF) was calculated in order to quantitatively compare the reactivity of a series of monolayer supported molybdenum oxide catalysts. The TOF value trends reflect the influence of the bridging Mo-O-Support bond and the electronegativity of the metal cation of the oxide support.
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 ; Argentina
Fil: Farneth, William E.. E. I. du Pont de Nemours and Company; Estados Unidos
Fil: Wachs, Israel E.. Lehigh University; Estados Unidos
description A detailed study of the methanol chemisorption and oxidation processes on oxide surfaces allowed the development of a method to quantify the number of surface active sites (Ns) of metal oxide catalysts. In situ infrared analysis during methanol adsorption showed that molecular methanol and surface methoxy species are co-adsorbed on an oxide surface at room temperature, but only surface methoxy species are formed at 100°C. Thermal stability and products of decomposition of the adsorbed species were determined with temperature programmed reaction spectroscopy (TPRS) experiments. Controlled adsorption with methanol doses resulted in a stable monolayer of surface methoxy species on the oxide surfaces. The stoichiometry of methanol chemisorption resulted in one surface methoxy adsorbed per three Mo atoms for polymerized surface molybdenum oxide structures, regardless of surface molybdenum oxide coordination. The activity of the catalysts per surface active sites (turnover frequencies TOF) was calculated in order to quantitatively compare the reactivity of a series of monolayer supported molybdenum oxide catalysts. The TOF value trends reflect the influence of the bridging Mo-O-Support bond and the electronegativity of the metal cation of the oxide support.
publishDate 2000
dc.date.none.fl_str_mv 2000-11
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/11336/42624
Briand, Laura Estefania; Farneth, William E.; Wachs, Israel E.; Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts; Elsevier Science; Catalysis Today; 62; 2-3; 11-2000; 219-229
0920-5861
CONICET Digital
CONICET
url http://hdl.handle.net/11336/42624
identifier_str_mv Briand, Laura Estefania; Farneth, William E.; Wachs, Israel E.; Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts: I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts; Elsevier Science; Catalysis Today; 62; 2-3; 11-2000; 219-229
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/doi/10.1016/S0920-5861(00)00423-5
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0920586100004235
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
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_ 1844613507811639296
score 13.070432

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