Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study
- Autores
- Belletti, Gustavo Daniel; Colombo, Estefanía; Cabana García, Nancy Cecilia; Quaino, Paola Monica; Collins, Sebastián Enrique
- Año de publicación
- 2022
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- The mechanism of methanol oxidation on a Au/TiO2 catalyst was investigated by combining in situ modulation-excitation diffuse reflectance infrared spectroscopy (MES-DRIFT) with periodic density functional theory (DFT). Adsorbed reaction intermediates and spectators were identified. Methanol dissociatively adsorbs as a methoxy (CH 3O) species on the titania surface, and stepwise oxidizes to formate, carboxyl and CO, carbonates and CO2 at the Au/TiO 2 interface. The role of the metal-support interface is clearly observed experimental and theoretically according to a metal–Au-assisted Mars van Krevelen mechanism. Energy barriers were calculated for each elementary step, and the methoxy oxidation was found to be the rate-limiting step in the proposed scenario.
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: Colombo, Estefanía. 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: Cabana García, Nancy Cecilia. 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: 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
-
COMBUSTION
DFT
IN SITU INFRARED
REACTION PATHWAY
VOLATILE ORGANIC COMPOUNDS - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
- Repositorio
.jpg)
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/216531
Ver los metadatos del registro completo
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Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT StudyBelletti, Gustavo DanielColombo, EstefaníaCabana García, Nancy CeciliaQuaino, Paola MonicaCollins, Sebastián EnriqueCOMBUSTIONDFTIN SITU INFRAREDREACTION PATHWAYVOLATILE ORGANIC COMPOUNDShttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The mechanism of methanol oxidation on a Au/TiO2 catalyst was investigated by combining in situ modulation-excitation diffuse reflectance infrared spectroscopy (MES-DRIFT) with periodic density functional theory (DFT). Adsorbed reaction intermediates and spectators were identified. Methanol dissociatively adsorbs as a methoxy (CH 3O) species on the titania surface, and stepwise oxidizes to formate, carboxyl and CO, carbonates and CO2 at the Au/TiO 2 interface. The role of the metal-support interface is clearly observed experimental and theoretically according to a metal–Au-assisted Mars van Krevelen mechanism. Energy barriers were calculated for each elementary step, and the methoxy oxidation was found to be the rate-limiting step in the proposed scenario.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.; ArgentinaFil: Colombo, Estefanía. 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: Cabana García, Nancy Cecilia. 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: 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; ArgentinaSpringer/Plenum Publishers2022-05info: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/11336/216531Belletti, Gustavo Daniel; Colombo, Estefanía; Cabana García, Nancy Cecilia; Quaino, Paola Monica; Collins, Sebastián Enrique; Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study; Springer/Plenum Publishers; Topics In Catalysis; 65; 7-8; 5-2022; 915-9251022-5528CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1007/s11244-022-01620-7info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:06:22Zoai:ri.conicet.gov.ar:11336/216531instacron: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:34982025-10-22 11:06:22.643CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
| dc.title.none.fl_str_mv |
Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study |
| title |
Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study |
| spellingShingle |
Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study Belletti, Gustavo Daniel COMBUSTION DFT IN SITU INFRARED REACTION PATHWAY VOLATILE ORGANIC COMPOUNDS |
| title_short |
Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study |
| title_full |
Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study |
| title_fullStr |
Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study |
| title_full_unstemmed |
Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study |
| title_sort |
Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study |
| dc.creator.none.fl_str_mv |
Belletti, Gustavo Daniel Colombo, Estefanía Cabana García, Nancy Cecilia Quaino, Paola Monica Collins, Sebastián Enrique |
| author |
Belletti, Gustavo Daniel |
| author_facet |
Belletti, Gustavo Daniel Colombo, Estefanía Cabana García, Nancy Cecilia Quaino, Paola Monica Collins, Sebastián Enrique |
| author_role |
author |
| author2 |
Colombo, Estefanía Cabana García, Nancy Cecilia Quaino, Paola Monica Collins, Sebastián Enrique |
| author2_role |
author author author author |
| dc.subject.none.fl_str_mv |
COMBUSTION DFT IN SITU INFRARED REACTION PATHWAY VOLATILE ORGANIC COMPOUNDS |
| topic |
COMBUSTION DFT IN SITU INFRARED REACTION PATHWAY VOLATILE ORGANIC COMPOUNDS |
| purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
| dc.description.none.fl_txt_mv |
The mechanism of methanol oxidation on a Au/TiO2 catalyst was investigated by combining in situ modulation-excitation diffuse reflectance infrared spectroscopy (MES-DRIFT) with periodic density functional theory (DFT). Adsorbed reaction intermediates and spectators were identified. Methanol dissociatively adsorbs as a methoxy (CH 3O) species on the titania surface, and stepwise oxidizes to formate, carboxyl and CO, carbonates and CO2 at the Au/TiO 2 interface. The role of the metal-support interface is clearly observed experimental and theoretically according to a metal–Au-assisted Mars van Krevelen mechanism. Energy barriers were calculated for each elementary step, and the methoxy oxidation was found to be the rate-limiting step in the proposed scenario. 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: Colombo, Estefanía. 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: Cabana García, Nancy Cecilia. 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: 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 |
The mechanism of methanol oxidation on a Au/TiO2 catalyst was investigated by combining in situ modulation-excitation diffuse reflectance infrared spectroscopy (MES-DRIFT) with periodic density functional theory (DFT). Adsorbed reaction intermediates and spectators were identified. Methanol dissociatively adsorbs as a methoxy (CH 3O) species on the titania surface, and stepwise oxidizes to formate, carboxyl and CO, carbonates and CO2 at the Au/TiO 2 interface. The role of the metal-support interface is clearly observed experimental and theoretically according to a metal–Au-assisted Mars van Krevelen mechanism. Energy barriers were calculated for each elementary step, and the methoxy oxidation was found to be the rate-limiting step in the proposed scenario. |
| publishDate |
2022 |
| dc.date.none.fl_str_mv |
2022-05 |
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info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion http://purl.org/coar/resource_type/c_6501 info:ar-repo/semantics/articulo |
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article |
| status_str |
publishedVersion |
| dc.identifier.none.fl_str_mv |
http://hdl.handle.net/11336/216531 Belletti, Gustavo Daniel; Colombo, Estefanía; Cabana García, Nancy Cecilia; Quaino, Paola Monica; Collins, Sebastián Enrique; Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study; Springer/Plenum Publishers; Topics In Catalysis; 65; 7-8; 5-2022; 915-925 1022-5528 CONICET Digital CONICET |
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http://hdl.handle.net/11336/216531 |
| identifier_str_mv |
Belletti, Gustavo Daniel; Colombo, Estefanía; Cabana García, Nancy Cecilia; Quaino, Paola Monica; Collins, Sebastián Enrique; Mechanistic Investigation of Methanol Oxidation on Au/TiO2: A Combined DRIFT and DFT Study; Springer/Plenum Publishers; Topics In Catalysis; 65; 7-8; 5-2022; 915-925 1022-5528 CONICET Digital CONICET |
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eng |
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eng |
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info:eu-repo/semantics/altIdentifier/doi/10.1007/s11244-022-01620-7 |
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openAccess |
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application/pdf application/pdf application/pdf |
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Springer/Plenum Publishers |
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Springer/Plenum Publishers |
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CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas |
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dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar |
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