The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTx
Autor(a) principal: | |
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Data de Publicação: | 2022 |
Outros Autores: | |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
Texto Completo: | http://hdl.handle.net/10773/35732 |
Resumo: | Density functional theory is used to investigate the origins of the excellent catalytic activity of the Mo2CTx MXene for the water gas shift reaction. By considering different possibilities for the MXene surface termination (Tx = none, O, F, or a mixture of O and F), we conclude that its ideal composition should contain both F and O adatoms, essential for controlling the exothermicity of the reaction and avoiding saturation by oxygenated species. More precisely, while Mo2CO2 and Mo2CF2 are too inert towards water adsorption and dissociation and the bare Mo2C MXene is inactivated upon coverage by oxygenated species, our calculations predict that regions near one or two O adatoms in the midst of F surface terminations should be the active catalytic sites. Indeed, in the vicinity of the O adatoms, water adsorbs with moderate strength, dissociates with a very low energy barrier (0.14–0.20 eV), and the dissociation is moderately exothermic. |
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The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTxWater gas shift reaction2D materialsCarbidesDensity functional theoryPeriodic modelsDensity functional theory is used to investigate the origins of the excellent catalytic activity of the Mo2CTx MXene for the water gas shift reaction. By considering different possibilities for the MXene surface termination (Tx = none, O, F, or a mixture of O and F), we conclude that its ideal composition should contain both F and O adatoms, essential for controlling the exothermicity of the reaction and avoiding saturation by oxygenated species. More precisely, while Mo2CO2 and Mo2CF2 are too inert towards water adsorption and dissociation and the bare Mo2C MXene is inactivated upon coverage by oxygenated species, our calculations predict that regions near one or two O adatoms in the midst of F surface terminations should be the active catalytic sites. Indeed, in the vicinity of the O adatoms, water adsorbs with moderate strength, dissociates with a very low energy barrier (0.14–0.20 eV), and the dissociation is moderately exothermic.Elsevier2023-01-11T12:18:03Z2022-07-23T00:00:00Z2022-07-23info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10773/35732eng0920-586110.1016/j.cattod.2022.07.016Gouveia, José D.Gomes, José R. B.info:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2024-02-22T12:08:35Zoai:ria.ua.pt:10773/35732Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-20T03:06:35.424432Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse |
dc.title.none.fl_str_mv |
The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTx |
title |
The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTx |
spellingShingle |
The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTx Gouveia, José D. Water gas shift reaction 2D materials Carbides Density functional theory Periodic models |
title_short |
The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTx |
title_full |
The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTx |
title_fullStr |
The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTx |
title_full_unstemmed |
The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTx |
title_sort |
The determining role of Tx species in the catalytic potential of MXenes: Water adsorption and dissociation on Mo2CTx |
author |
Gouveia, José D. |
author_facet |
Gouveia, José D. Gomes, José R. B. |
author_role |
author |
author2 |
Gomes, José R. B. |
author2_role |
author |
dc.contributor.author.fl_str_mv |
Gouveia, José D. Gomes, José R. B. |
dc.subject.por.fl_str_mv |
Water gas shift reaction 2D materials Carbides Density functional theory Periodic models |
topic |
Water gas shift reaction 2D materials Carbides Density functional theory Periodic models |
description |
Density functional theory is used to investigate the origins of the excellent catalytic activity of the Mo2CTx MXene for the water gas shift reaction. By considering different possibilities for the MXene surface termination (Tx = none, O, F, or a mixture of O and F), we conclude that its ideal composition should contain both F and O adatoms, essential for controlling the exothermicity of the reaction and avoiding saturation by oxygenated species. More precisely, while Mo2CO2 and Mo2CF2 are too inert towards water adsorption and dissociation and the bare Mo2C MXene is inactivated upon coverage by oxygenated species, our calculations predict that regions near one or two O adatoms in the midst of F surface terminations should be the active catalytic sites. Indeed, in the vicinity of the O adatoms, water adsorbs with moderate strength, dissociates with a very low energy barrier (0.14–0.20 eV), and the dissociation is moderately exothermic. |
publishDate |
2022 |
dc.date.none.fl_str_mv |
2022-07-23T00:00:00Z 2022-07-23 2023-01-11T12:18:03Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://hdl.handle.net/10773/35732 |
url |
http://hdl.handle.net/10773/35732 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
0920-5861 10.1016/j.cattod.2022.07.016 |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
application/pdf |
dc.publisher.none.fl_str_mv |
Elsevier |
publisher.none.fl_str_mv |
Elsevier |
dc.source.none.fl_str_mv |
reponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação instacron:RCAAP |
instname_str |
Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
instacron_str |
RCAAP |
institution |
RCAAP |
reponame_str |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
collection |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
repository.name.fl_str_mv |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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1799137721604636672 |