Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?

Autores
German, Estefania; Gebauer, Ralph
Año de publicación
2020
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
We use density functional theory based calculations to study the energetics of the oxygen evolution reaction on a monolayer of MoS2. This material, a prototypical example of a layered transition metal dichalcogenide, is intensely studied in the context of many important catalytical applications, in particular for the hydrogen evolution reaction. The second half-reaction of the water-splitting process, the oxygen evolution reaction, is almost never considered on this material, due to its low activity. Based on our calculations, we explain this experimentally observed poor catalytic activity for the oxygen evolution by the weak binding of two key reaction intermediates (hydroxyl and hydroperoxyl) to the substrate. We explore substitutional doping with oxygen and phosphorous as means to facilitate the oxygen evolution on MoS2 layers. The oxygen substitution slightly increases the reaction´s overpotential, but does not significantly change the energetics. The doping with phosphorous, on the other hand, is not a promising way to promote the oxygen evolution on MoS2 layers. We also explore the role of the edges of MoS2 layers. We find that while the adsorption energies of reaction intermediates are strongly influenced by the presence of an edge, the final reaction overpotential remains nearly the same as on a pristine monolayer, meaning that the presence of edges is not favoring the OER.
Fil: German, Estefania. Universidad de Valladolid; España. 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: Gebauer, Ralph. The Abdus Salam. International Centre for Theoretical Physics; Italia
Materia
DENSITY FUNCTIONAL THEORY
MOS2
OXYGEN EVOLUTION REACTION
TRANSITION METAL DICHALCOGENIDE
WATER SPLITTING
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/144076
Acceder
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network_acronym_str CONICETDig
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network_name_str CONICET Digital (CONICET)
spelling Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?German, EstefaniaGebauer, RalphDENSITY FUNCTIONAL THEORYMOS2OXYGEN EVOLUTION REACTIONTRANSITION METAL DICHALCOGENIDEWATER SPLITTINGhttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1We use density functional theory based calculations to study the energetics of the oxygen evolution reaction on a monolayer of MoS2. This material, a prototypical example of a layered transition metal dichalcogenide, is intensely studied in the context of many important catalytical applications, in particular for the hydrogen evolution reaction. The second half-reaction of the water-splitting process, the oxygen evolution reaction, is almost never considered on this material, due to its low activity. Based on our calculations, we explain this experimentally observed poor catalytic activity for the oxygen evolution by the weak binding of two key reaction intermediates (hydroxyl and hydroperoxyl) to the substrate. We explore substitutional doping with oxygen and phosphorous as means to facilitate the oxygen evolution on MoS2 layers. The oxygen substitution slightly increases the reaction´s overpotential, but does not significantly change the energetics. The doping with phosphorous, on the other hand, is not a promising way to promote the oxygen evolution on MoS2 layers. We also explore the role of the edges of MoS2 layers. We find that while the adsorption energies of reaction intermediates are strongly influenced by the presence of an edge, the final reaction overpotential remains nearly the same as on a pristine monolayer, meaning that the presence of edges is not favoring the OER.Fil: German, Estefania. Universidad de Valladolid; España. 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: Gebauer, Ralph. The Abdus Salam. International Centre for Theoretical Physics; ItaliaElsevier Science2020-10-30info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/144076German, Estefania; Gebauer, Ralph; Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?; Elsevier Science; Applied Surface Science; 528; 30-10-2020; 1-7; 1465910169-4332CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.apsusc.2020.146591info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/abs/pii/S0169433220313489info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:25:43Zoai:ri.conicet.gov.ar:11336/144076instacron: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 10:25:44.19CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?
title Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?
spellingShingle Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?
German, Estefania
DENSITY FUNCTIONAL THEORY
MOS2
OXYGEN EVOLUTION REACTION
TRANSITION METAL DICHALCOGENIDE
WATER SPLITTING
title_short Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?
title_full Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?
title_fullStr Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?
title_full_unstemmed Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?
title_sort Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?
dc.creator.none.fl_str_mv German, Estefania
Gebauer, Ralph
author German, Estefania
author_facet German, Estefania
Gebauer, Ralph
author_role author
author2 Gebauer, Ralph
author2_role author
dc.subject.none.fl_str_mv DENSITY FUNCTIONAL THEORY
MOS2
OXYGEN EVOLUTION REACTION
TRANSITION METAL DICHALCOGENIDE
WATER SPLITTING
topic DENSITY FUNCTIONAL THEORY
MOS2
OXYGEN EVOLUTION REACTION
TRANSITION METAL DICHALCOGENIDE
WATER SPLITTING
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv We use density functional theory based calculations to study the energetics of the oxygen evolution reaction on a monolayer of MoS2. This material, a prototypical example of a layered transition metal dichalcogenide, is intensely studied in the context of many important catalytical applications, in particular for the hydrogen evolution reaction. The second half-reaction of the water-splitting process, the oxygen evolution reaction, is almost never considered on this material, due to its low activity. Based on our calculations, we explain this experimentally observed poor catalytic activity for the oxygen evolution by the weak binding of two key reaction intermediates (hydroxyl and hydroperoxyl) to the substrate. We explore substitutional doping with oxygen and phosphorous as means to facilitate the oxygen evolution on MoS2 layers. The oxygen substitution slightly increases the reaction´s overpotential, but does not significantly change the energetics. The doping with phosphorous, on the other hand, is not a promising way to promote the oxygen evolution on MoS2 layers. We also explore the role of the edges of MoS2 layers. We find that while the adsorption energies of reaction intermediates are strongly influenced by the presence of an edge, the final reaction overpotential remains nearly the same as on a pristine monolayer, meaning that the presence of edges is not favoring the OER.
Fil: German, Estefania. Universidad de Valladolid; España. 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: Gebauer, Ralph. The Abdus Salam. International Centre for Theoretical Physics; Italia
description We use density functional theory based calculations to study the energetics of the oxygen evolution reaction on a monolayer of MoS2. This material, a prototypical example of a layered transition metal dichalcogenide, is intensely studied in the context of many important catalytical applications, in particular for the hydrogen evolution reaction. The second half-reaction of the water-splitting process, the oxygen evolution reaction, is almost never considered on this material, due to its low activity. Based on our calculations, we explain this experimentally observed poor catalytic activity for the oxygen evolution by the weak binding of two key reaction intermediates (hydroxyl and hydroperoxyl) to the substrate. We explore substitutional doping with oxygen and phosphorous as means to facilitate the oxygen evolution on MoS2 layers. The oxygen substitution slightly increases the reaction´s overpotential, but does not significantly change the energetics. The doping with phosphorous, on the other hand, is not a promising way to promote the oxygen evolution on MoS2 layers. We also explore the role of the edges of MoS2 layers. We find that while the adsorption energies of reaction intermediates are strongly influenced by the presence of an edge, the final reaction overpotential remains nearly the same as on a pristine monolayer, meaning that the presence of edges is not favoring the OER.
publishDate 2020
dc.date.none.fl_str_mv 2020-10-30
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/11336/144076
German, Estefania; Gebauer, Ralph; Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?; Elsevier Science; Applied Surface Science; 528; 30-10-2020; 1-7; 146591
0169-4332
CONICET Digital
CONICET
url http://hdl.handle.net/11336/144076
identifier_str_mv German, Estefania; Gebauer, Ralph; Why are MoS2 monolayers not a good catalyst for the oxygen evolution reaction?; Elsevier Science; Applied Surface Science; 528; 30-10-2020; 1-7; 146591
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/doi/10.1016/j.apsusc.2020.146591
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/abs/pii/S0169433220313489
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
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

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