A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces

Autores
Reimers, Walter Guillermo; Zubieta, Carolina Edith; Baltanas, Miguel Angel; Branda, Maria Marta
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A systematic theoretical study of the consecutive hydrogenation reactions of the CO molecule for the methanol synthesis catalyzed by different oxides of Zn, Ce and Ga is reported in this work. First, the CO hydrogenation with the formation of formyl species (HCO) was analyzed, followed by the successive hydrogenations that lead to formaldehyde (H2CO), methoxy (H3CO) and, finally, methanol (H3COH). The co-adsorption with H, in almost all the intermediate species, allows the corresponding hydrogenation reaction. Oxygen vacancies promote the reactivity in the generation of both formaldehyde and methoxy species. The formation of these species involves an important geometric difference between the initial and the final states, leading to high activation barriers. Comparing the surfaces studied in this work, we found that ZnO (0001)vacO has shown to be of a greater interest for methanol synthesis. However, the foregoing is not the most relevant of our results, but, instead, that the Brönsted Evans Polanyi (BEP) relationships between the initial or the final states and the transition states (TS) allowed to find a very good correlation between surface structure and reactivity.
Fil: Reimers, Walter Guillermo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Zubieta, Carolina Edith. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina
Fil: Baltanas, Miguel Angel. 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: Branda, Maria Marta. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Materia
CO
DFT
HYDROGENATION
METHANOL
OXIDES
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:11336/91983
Acceder
id CONICETDig_55c33905572638cbd27524851416815b
oai_identifier_str oai:ri.conicet.gov.ar:11336/91983
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfacesReimers, Walter GuillermoZubieta, Carolina EdithBaltanas, Miguel AngelBranda, Maria MartaCODFTHYDROGENATIONMETHANOLOXIDEShttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1A systematic theoretical study of the consecutive hydrogenation reactions of the CO molecule for the methanol synthesis catalyzed by different oxides of Zn, Ce and Ga is reported in this work. First, the CO hydrogenation with the formation of formyl species (HCO) was analyzed, followed by the successive hydrogenations that lead to formaldehyde (H2CO), methoxy (H3CO) and, finally, methanol (H3COH). The co-adsorption with H, in almost all the intermediate species, allows the corresponding hydrogenation reaction. Oxygen vacancies promote the reactivity in the generation of both formaldehyde and methoxy species. The formation of these species involves an important geometric difference between the initial and the final states, leading to high activation barriers. Comparing the surfaces studied in this work, we found that ZnO (0001)vacO has shown to be of a greater interest for methanol synthesis. However, the foregoing is not the most relevant of our results, but, instead, that the Brönsted Evans Polanyi (BEP) relationships between the initial or the final states and the transition states (TS) allowed to find a very good correlation between surface structure and reactivity.Fil: Reimers, Walter Guillermo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaFil: Zubieta, Carolina Edith. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; ArgentinaFil: Baltanas, Miguel Angel. 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: Branda, Maria Marta. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaElsevier Science2018-04-01info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/91983Reimers, Walter Guillermo; Zubieta, Carolina Edith; Baltanas, Miguel Angel; Branda, Maria Marta; A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces; Elsevier Science; Applied Surface Science; 436; 1-4-2018; 1003-10170169-4332CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/abs/pii/S0169433217336929info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apsusc.2017.12.104info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T14:30:47Zoai:ri.conicet.gov.ar:11336/91983instacron: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:34982025-10-15 14:30:47.724CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces
title A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces
spellingShingle A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces
Reimers, Walter Guillermo
CO
DFT
HYDROGENATION
METHANOL
OXIDES
title_short A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces
title_full A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces
title_fullStr A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces
title_full_unstemmed A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces
title_sort A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces
dc.creator.none.fl_str_mv Reimers, Walter Guillermo
Zubieta, Carolina Edith
Baltanas, Miguel Angel
Branda, Maria Marta
author Reimers, Walter Guillermo
author_facet Reimers, Walter Guillermo
Zubieta, Carolina Edith
Baltanas, Miguel Angel
Branda, Maria Marta
author_role author
author2 Zubieta, Carolina Edith
Baltanas, Miguel Angel
Branda, Maria Marta
author2_role author
author
author
dc.subject.none.fl_str_mv CO
DFT
HYDROGENATION
METHANOL
OXIDES
topic CO
DFT
HYDROGENATION
METHANOL
OXIDES
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv A systematic theoretical study of the consecutive hydrogenation reactions of the CO molecule for the methanol synthesis catalyzed by different oxides of Zn, Ce and Ga is reported in this work. First, the CO hydrogenation with the formation of formyl species (HCO) was analyzed, followed by the successive hydrogenations that lead to formaldehyde (H2CO), methoxy (H3CO) and, finally, methanol (H3COH). The co-adsorption with H, in almost all the intermediate species, allows the corresponding hydrogenation reaction. Oxygen vacancies promote the reactivity in the generation of both formaldehyde and methoxy species. The formation of these species involves an important geometric difference between the initial and the final states, leading to high activation barriers. Comparing the surfaces studied in this work, we found that ZnO (0001)vacO has shown to be of a greater interest for methanol synthesis. However, the foregoing is not the most relevant of our results, but, instead, that the Brönsted Evans Polanyi (BEP) relationships between the initial or the final states and the transition states (TS) allowed to find a very good correlation between surface structure and reactivity.
Fil: Reimers, Walter Guillermo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Zubieta, Carolina Edith. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina
Fil: Baltanas, Miguel Angel. 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: Branda, Maria Marta. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
description A systematic theoretical study of the consecutive hydrogenation reactions of the CO molecule for the methanol synthesis catalyzed by different oxides of Zn, Ce and Ga is reported in this work. First, the CO hydrogenation with the formation of formyl species (HCO) was analyzed, followed by the successive hydrogenations that lead to formaldehyde (H2CO), methoxy (H3CO) and, finally, methanol (H3COH). The co-adsorption with H, in almost all the intermediate species, allows the corresponding hydrogenation reaction. Oxygen vacancies promote the reactivity in the generation of both formaldehyde and methoxy species. The formation of these species involves an important geometric difference between the initial and the final states, leading to high activation barriers. Comparing the surfaces studied in this work, we found that ZnO (0001)vacO has shown to be of a greater interest for methanol synthesis. However, the foregoing is not the most relevant of our results, but, instead, that the Brönsted Evans Polanyi (BEP) relationships between the initial or the final states and the transition states (TS) allowed to find a very good correlation between surface structure and reactivity.
publishDate 2018
dc.date.none.fl_str_mv 2018-04-01
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/11336/91983
Reimers, Walter Guillermo; Zubieta, Carolina Edith; Baltanas, Miguel Angel; Branda, Maria Marta; A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces; Elsevier Science; Applied Surface Science; 436; 1-4-2018; 1003-1017
0169-4332
CONICET Digital
CONICET
url http://hdl.handle.net/11336/91983
identifier_str_mv Reimers, Walter Guillermo; Zubieta, Carolina Edith; Baltanas, Miguel Angel; Branda, Maria Marta; A DFT Approach for Methanol Synthesis via Hydrogenation of CO on Gallia, Ceria and ZnO surfaces; Elsevier Science; Applied Surface Science; 436; 1-4-2018; 1003-1017
0169-4332
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/abs/pii/S0169433217336929
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apsusc.2017.12.104
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
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_ 1846082787118940160
score 13.22299

Publicaciones similares