Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst
- Autores
- Vecchietti, María Julia; Belletti, Gustavo Daniel; Quaino, Paola Monica; Bonivardi, Adrian Lionel; Collins, Sebastián Enrique
- Año de publicación
- 2023
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- ChemCatChem homepage for more articles in the collection. The mechanism of the low-temperature water gas shift reaction (LTWGS) on an Au/CeO2 catalyst was investigated by means of in situ diffuse reflectance infrared (DRIFT) spectroscopy. Under steady-state LTWGS reaction (373–623 K), the catalyst is partially reduced, and signals from carbonate/formate dominates the infrared spectra. Time-resolved pulse of CO experiment under a constant partial pressure of water at 423 K indicates that Ce4+ can be reduced to Ce3+ and that formate (HCOO) species cannot be directly related to the CO2 production. Further information was obtained by performing modulation excitation spectroscopy (MES) experiments coupled with a phase-sensitive detection (PSD) method. Under periodic modulation of the CO partial pressure while keeping the H2O concentration constant, most of the intense bands of carbonate and formate remained constant, indicating that these species are only spectators. The same is observed for the concentration of Ce3+. Conversely, signals in-phase with the conversion of CO to CO2 are observed and assigned to carboxyl [C(O)OH] and carboxylate (CO2δ−) species, while some monodentate formate (m-HCOO) also changes but at a lower rate. A plausible associative reaction mechanism where carboxyl/carboxylate are key intermediates is postulated.
Fil: Vecchietti, María Julia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina
Fil: Belletti, Gustavo Daniel. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; Argentina
Fil: Quaino, Paola Monica. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; Argentina
Fil: Bonivardi, Adrian Lionel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina
Fil: Collins, Sebastián Enrique. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina - Materia
-
CARBOXYL
CARBOXYLATE
CERIUM OXIDE
FORMATE
GOLD CATALYSTS
MODULATION SPECTROSCOPY - 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:11336/226241
Ver los metadatos del registro completo
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Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria CatalystVecchietti, María JuliaBelletti, Gustavo DanielQuaino, Paola MonicaBonivardi, Adrian LionelCollins, Sebastián EnriqueCARBOXYLCARBOXYLATECERIUM OXIDEFORMATEGOLD CATALYSTSMODULATION SPECTROSCOPYhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1ChemCatChem homepage for more articles in the collection. The mechanism of the low-temperature water gas shift reaction (LTWGS) on an Au/CeO2 catalyst was investigated by means of in situ diffuse reflectance infrared (DRIFT) spectroscopy. Under steady-state LTWGS reaction (373–623 K), the catalyst is partially reduced, and signals from carbonate/formate dominates the infrared spectra. Time-resolved pulse of CO experiment under a constant partial pressure of water at 423 K indicates that Ce4+ can be reduced to Ce3+ and that formate (HCOO) species cannot be directly related to the CO2 production. Further information was obtained by performing modulation excitation spectroscopy (MES) experiments coupled with a phase-sensitive detection (PSD) method. Under periodic modulation of the CO partial pressure while keeping the H2O concentration constant, most of the intense bands of carbonate and formate remained constant, indicating that these species are only spectators. The same is observed for the concentration of Ce3+. Conversely, signals in-phase with the conversion of CO to CO2 are observed and assigned to carboxyl [C(O)OH] and carboxylate (CO2δ−) species, while some monodentate formate (m-HCOO) also changes but at a lower rate. A plausible associative reaction mechanism where carboxyl/carboxylate are key intermediates is postulated.Fil: Vecchietti, María Julia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; ArgentinaFil: Belletti, Gustavo Daniel. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; ArgentinaFil: Quaino, Paola Monica. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; ArgentinaFil: Bonivardi, Adrian Lionel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; ArgentinaFil: Collins, Sebastián Enrique. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; ArgentinaWiley VCH Verlag2023-08info: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/11336/226241Vecchietti, María Julia; Belletti, Gustavo Daniel; Quaino, Paola Monica; Bonivardi, Adrian Lionel; Collins, Sebastián Enrique; Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst; Wiley VCH Verlag; Chemcatchem; 15; 19; 8-2023; 1-231867-3880CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cctc.202300435info:eu-repo/semantics/altIdentifier/doi/10.1002/cctc.202300435info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:39:25Zoai:ri.conicet.gov.ar:11336/226241instacron: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 10:39:25.578CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
dc.title.none.fl_str_mv |
Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst |
title |
Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst |
spellingShingle |
Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst Vecchietti, María Julia CARBOXYL CARBOXYLATE CERIUM OXIDE FORMATE GOLD CATALYSTS MODULATION SPECTROSCOPY |
title_short |
Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst |
title_full |
Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst |
title_fullStr |
Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst |
title_full_unstemmed |
Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst |
title_sort |
Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst |
dc.creator.none.fl_str_mv |
Vecchietti, María Julia Belletti, Gustavo Daniel Quaino, Paola Monica Bonivardi, Adrian Lionel Collins, Sebastián Enrique |
author |
Vecchietti, María Julia |
author_facet |
Vecchietti, María Julia Belletti, Gustavo Daniel Quaino, Paola Monica Bonivardi, Adrian Lionel Collins, Sebastián Enrique |
author_role |
author |
author2 |
Belletti, Gustavo Daniel Quaino, Paola Monica Bonivardi, Adrian Lionel Collins, Sebastián Enrique |
author2_role |
author author author author |
dc.subject.none.fl_str_mv |
CARBOXYL CARBOXYLATE CERIUM OXIDE FORMATE GOLD CATALYSTS MODULATION SPECTROSCOPY |
topic |
CARBOXYL CARBOXYLATE CERIUM OXIDE FORMATE GOLD CATALYSTS MODULATION SPECTROSCOPY |
purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
dc.description.none.fl_txt_mv |
ChemCatChem homepage for more articles in the collection. The mechanism of the low-temperature water gas shift reaction (LTWGS) on an Au/CeO2 catalyst was investigated by means of in situ diffuse reflectance infrared (DRIFT) spectroscopy. Under steady-state LTWGS reaction (373–623 K), the catalyst is partially reduced, and signals from carbonate/formate dominates the infrared spectra. Time-resolved pulse of CO experiment under a constant partial pressure of water at 423 K indicates that Ce4+ can be reduced to Ce3+ and that formate (HCOO) species cannot be directly related to the CO2 production. Further information was obtained by performing modulation excitation spectroscopy (MES) experiments coupled with a phase-sensitive detection (PSD) method. Under periodic modulation of the CO partial pressure while keeping the H2O concentration constant, most of the intense bands of carbonate and formate remained constant, indicating that these species are only spectators. The same is observed for the concentration of Ce3+. Conversely, signals in-phase with the conversion of CO to CO2 are observed and assigned to carboxyl [C(O)OH] and carboxylate (CO2δ−) species, while some monodentate formate (m-HCOO) also changes but at a lower rate. A plausible associative reaction mechanism where carboxyl/carboxylate are key intermediates is postulated. Fil: Vecchietti, María Julia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina Fil: Belletti, Gustavo Daniel. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; Argentina Fil: Quaino, Paola Monica. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; Argentina Fil: Bonivardi, Adrian Lionel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina Fil: Collins, Sebastián Enrique. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina |
description |
ChemCatChem homepage for more articles in the collection. The mechanism of the low-temperature water gas shift reaction (LTWGS) on an Au/CeO2 catalyst was investigated by means of in situ diffuse reflectance infrared (DRIFT) spectroscopy. Under steady-state LTWGS reaction (373–623 K), the catalyst is partially reduced, and signals from carbonate/formate dominates the infrared spectra. Time-resolved pulse of CO experiment under a constant partial pressure of water at 423 K indicates that Ce4+ can be reduced to Ce3+ and that formate (HCOO) species cannot be directly related to the CO2 production. Further information was obtained by performing modulation excitation spectroscopy (MES) experiments coupled with a phase-sensitive detection (PSD) method. Under periodic modulation of the CO partial pressure while keeping the H2O concentration constant, most of the intense bands of carbonate and formate remained constant, indicating that these species are only spectators. The same is observed for the concentration of Ce3+. Conversely, signals in-phase with the conversion of CO to CO2 are observed and assigned to carboxyl [C(O)OH] and carboxylate (CO2δ−) species, while some monodentate formate (m-HCOO) also changes but at a lower rate. A plausible associative reaction mechanism where carboxyl/carboxylate are key intermediates is postulated. |
publishDate |
2023 |
dc.date.none.fl_str_mv |
2023-08 |
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/11336/226241 Vecchietti, María Julia; Belletti, Gustavo Daniel; Quaino, Paola Monica; Bonivardi, Adrian Lionel; Collins, Sebastián Enrique; Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst; Wiley VCH Verlag; Chemcatchem; 15; 19; 8-2023; 1-23 1867-3880 CONICET Digital CONICET |
url |
http://hdl.handle.net/11336/226241 |
identifier_str_mv |
Vecchietti, María Julia; Belletti, Gustavo Daniel; Quaino, Paola Monica; Bonivardi, Adrian Lionel; Collins, Sebastián Enrique; Time-resolved DRIFT Spectroscopy Study of Carbonaceous Intermediates during the Water Gas Shift Reaction over Au/Ceria Catalyst; Wiley VCH Verlag; Chemcatchem; 15; 19; 8-2023; 1-23 1867-3880 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://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cctc.202300435 info:eu-repo/semantics/altIdentifier/doi/10.1002/cctc.202300435 |
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 |
Wiley VCH Verlag |
publisher.none.fl_str_mv |
Wiley VCH Verlag |
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 |