Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U

GGA + U calculations have been carried out to study the complete methanol decomposition on the more stable Ceria surfaces, i.e. (111), (221), (331) and (110). These results have shown that the methanol adsorption is exothermic on oxidized as well as on the partially reduced surfaces though the adsor...

ver descrição completa

Detalhes bibliográficos
Autores: Reimers, Walter Guillermo, Branda, Maria Marta
Formato: artículo
Estado:Versión publicada
Fecha de publicación:2017
País:Argentina
Recursos:Consejo Nacional de Investigaciones Científicas y Técnicas
Repositorio:CONICET Digital (CONICET)
Idioma:inglés
OAI Identifier:oai:ri.conicet.gov.ar:11336/63312
Acesso em linha:http://hdl.handle.net/11336/63312
Access Level:acceso abierto
Palavra-chave:Catalysis
Dft
Methanol Decomposition
Oxide
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
id AR_75f6a351fbb110b101ad80e032e8e901
oai_identifier_str oai:ri.conicet.gov.ar:11336/63312
network_acronym_str AR
network_name_str Argentina
repository_id_str
spelling Methanol decomposition on low index and stepped CeO2 surfaces from GGA+UReimers, Walter GuillermoBranda, Maria MartaCatalysisDftMethanol DecompositionOxidehttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1GGA + U calculations have been carried out to study the complete methanol decomposition on the more stable Ceria surfaces, i.e. (111), (221), (331) and (110). These results have shown that the methanol adsorption is exothermic on oxidized as well as on the partially reduced surfaces though the adsorption energy is greater for the latest. The first dehydrogenation step of methanol is highly probable for all the studied sites with activation barriers smaller than 0.2 eV. The first dehydrogenation reaction could also occur by breaking the C[sbnd]H methyl bond, but we found that this reaction is very unlikely. Reaction and activation energies for the second dehydrogenation – from methoxy to formaldehyde, are very similar for perfect (111) and stepped surfaces but these activation barriers are not negligible, almost ten times as many the first step barriers. Next, the formaldehyde decomposition to formyl and CO species on perfect CeO2(111) have an important energetic cost, therefore these reactions could occur only on stepped surfaces.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: 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 Science2017-02info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/63312Reimers, Walter Guillermo; Branda, Maria Marta; Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U; Elsevier Science; Applied Surface Science; 394; 2-2017; 509-5180169-4332CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0169433216322784info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apsusc.2016.10.154info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2024-05-08T14:19:28Zoai:ri.conicet.gov.ar:11336/63312instacron: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:34982024-05-08 14:19:29.059CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U
title Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U
spellingShingle Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U
Reimers, Walter Guillermo
Catalysis
Dft
Methanol Decomposition
Oxide
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
title_short Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U
title_full Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U
title_fullStr Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U
title_full_unstemmed Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U
title_sort Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U
dc.creator.none.fl_str_mv Reimers, Walter Guillermo
Branda, Maria Marta
author Reimers, Walter Guillermo
author_facet Reimers, Walter Guillermo
Branda, Maria Marta
author_role author
author2 Branda, Maria Marta
author2_role author
dc.subject.none.fl_str_mv Catalysis
Dft
Methanol Decomposition
Oxide
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
topic Catalysis
Dft
Methanol Decomposition
Oxide
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
description GGA + U calculations have been carried out to study the complete methanol decomposition on the more stable Ceria surfaces, i.e. (111), (221), (331) and (110). These results have shown that the methanol adsorption is exothermic on oxidized as well as on the partially reduced surfaces though the adsorption energy is greater for the latest. The first dehydrogenation step of methanol is highly probable for all the studied sites with activation barriers smaller than 0.2 eV. The first dehydrogenation reaction could also occur by breaking the C[sbnd]H methyl bond, but we found that this reaction is very unlikely. Reaction and activation energies for the second dehydrogenation – from methoxy to formaldehyde, are very similar for perfect (111) and stepped surfaces but these activation barriers are not negligible, almost ten times as many the first step barriers. Next, the formaldehyde decomposition to formyl and CO species on perfect CeO2(111) have an important energetic cost, therefore these reactions could occur only on stepped surfaces.
publishDate 2017
dc.date.none.fl_str_mv 2017-02
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/11336/63312
Reimers, Walter Guillermo; Branda, Maria Marta; Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U; Elsevier Science; Applied Surface Science; 394; 2-2017; 509-518
0169-4332
CONICET Digital
CONICET
url http://hdl.handle.net/11336/63312
identifier_str_mv Reimers, Walter Guillermo; Branda, Maria Marta; Methanol decomposition on low index and stepped CeO2 surfaces from GGA+U; Elsevier Science; Applied Surface Science; 394; 2-2017; 509-518
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/pii/S0169433216322784
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apsusc.2016.10.154
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
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
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_ 1799196225348567040
score 15,812455

Registos relacionados