Au Single Metal Atom for Carbon Dioxide Reduction Reaction

CO2 is the gas that contributes the most to the greenhouse effect and, therefore, to global warming. One of the greatest challenges facing humanity is the reduction of the concentration of CO2 in the air. Here, we analyze the possible use of Au1@g-C3N4 electrocatalyst to transform CO2 into add-ed-va...

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Autores: Vidal-López, Anna, Posada-Pérez, Sergio, Solà i Puig, Miquel, Poater Teixidor, Albert
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2023
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:10256/23161
Acceso en línea:http://hdl.handle.net/10256/23161
Access Level:acceso abierto
Palabra clave:Electrocatàlisi
Reducció química
Electrocatalysis
Reduction (Chemistry)
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spelling Au Single Metal Atom for Carbon Dioxide Reduction ReactionVidal-López, AnnaPosada-Pérez, SergioSolà i Puig, MiquelPoater Teixidor, AlbertElectrocatàlisiReducció químicaElectrocatalysisReduction (Chemistry)CO2 is the gas that contributes the most to the greenhouse effect and, therefore, to global warming. One of the greatest challenges facing humanity is the reduction of the concentration of CO2 in the air. Here, we analyze the possible use of Au1@g-C3N4 electrocatalyst to transform CO2 into add-ed-value products. We use density functional theory (DFT) to determine the reaction Gibbs ener-gies for eight electron-proton transfer reaction paths of the electrochemical carbon dioxide reduc-tion reaction (CO2RR) using a single Au atom supported on 2D carbon nitride support. Our sim-ulations classify the Au1@g-C3N4 electrocatalysts as 'beyond CO' since their formation is energet-ically favored, although their strong binding with a Au single atom does not allow the desorption process. DFT calculations revealed that the lowest energy pathway is CO2(g)→ COOH*→ CO*→ HCO*→ HCOH* → CH2OH* → CH2* →CH3* → CH4(g), where the first hydrogenation of CO to HCO is predicted as the rate-limiting step of the reaction with slightly lower potential than pre-dicted for Cu electrodes, the most effective catalysts for CO2RR. Methane is predicted to be the main reaction product after eight proton-electron transfers (CO2 + 8 H+ + 8e− → CH4 + 2H2O). The generation of formaldehyde is discarded due to the large formation energy of the adsorbed moiety and the production of methanol is slightly less favorable than methane formation. Our computa-tional study helps to identify suitable electrocatalysts for CO2RR by reducing the amount of metal and using stable and low-cost supportsThis research was funded by the Spanish Ministerio de Ciencia e Innovación (projects PID2021-127423NB-I00 to A.P. and PID2020-113711GB-I00 to M.S.) and the Generalitat de Catalunya (project 2021SGR0623 and ICREA Academia prize 2019 to A.P.). A.V.-L. is grateful for funding from the pre-doctoral fellowship (PRE2019-089647). S.P.-P. appreciates the economic support of the Marie Curie fellowship (H2020-MSCA-IF-2020-101020330)MDPI (Multidisciplinary Digital Publishing Institute)2023info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionpeer-reviewed12 p.application/pdfhttp://hdl.handle.net/10256/23161http://hdl.handle.net/10256/23161Chemistry, 2022, vol. 5, p. 1395-1406Articles publicats (D-Q)Vidal-López, Anna Posada-Pérez, Sergio Solà i Puig, Miquel Poater Teixidor, Albert 2022 Au Single Metal Atom for Carbon Dioxide Reduction Reaction Chemistry 5 1395 1406reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)Inglésinfo:eu-repo/semantics/altIdentifier/doi/10.3390/chemistry5020095info:eu-repo/semantics/altIdentifier/eissn/2624-8549PID2021-127423NB-I00PID2020-113711GB-I00info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-127423NB-I00info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2020-113711GB-I00Reconeixement 4.0 Internacionalhttp://creativecommons.org/licenses/by/4.0info:eu-repo/semantics/openAccessoai:recercat.cat:10256/231612026-05-29T05:05:01Z
dc.title.none.fl_str_mv Au Single Metal Atom for Carbon Dioxide Reduction Reaction
title Au Single Metal Atom for Carbon Dioxide Reduction Reaction
spellingShingle Au Single Metal Atom for Carbon Dioxide Reduction Reaction
Vidal-López, Anna
Electrocatàlisi
Reducció química
Electrocatalysis
Reduction (Chemistry)
title_short Au Single Metal Atom for Carbon Dioxide Reduction Reaction
title_full Au Single Metal Atom for Carbon Dioxide Reduction Reaction
title_fullStr Au Single Metal Atom for Carbon Dioxide Reduction Reaction
title_full_unstemmed Au Single Metal Atom for Carbon Dioxide Reduction Reaction
title_sort Au Single Metal Atom for Carbon Dioxide Reduction Reaction
dc.creator.none.fl_str_mv Vidal-López, Anna
Posada-Pérez, Sergio
Solà i Puig, Miquel
Poater Teixidor, Albert
author Vidal-López, Anna
author_facet Vidal-López, Anna
Posada-Pérez, Sergio
Solà i Puig, Miquel
Poater Teixidor, Albert
author_role author
author2 Posada-Pérez, Sergio
Solà i Puig, Miquel
Poater Teixidor, Albert
author2_role author
author
author
dc.subject.none.fl_str_mv Electrocatàlisi
Reducció química
Electrocatalysis
Reduction (Chemistry)
topic Electrocatàlisi
Reducció química
Electrocatalysis
Reduction (Chemistry)
description CO2 is the gas that contributes the most to the greenhouse effect and, therefore, to global warming. One of the greatest challenges facing humanity is the reduction of the concentration of CO2 in the air. Here, we analyze the possible use of Au1@g-C3N4 electrocatalyst to transform CO2 into add-ed-value products. We use density functional theory (DFT) to determine the reaction Gibbs ener-gies for eight electron-proton transfer reaction paths of the electrochemical carbon dioxide reduc-tion reaction (CO2RR) using a single Au atom supported on 2D carbon nitride support. Our sim-ulations classify the Au1@g-C3N4 electrocatalysts as 'beyond CO' since their formation is energet-ically favored, although their strong binding with a Au single atom does not allow the desorption process. DFT calculations revealed that the lowest energy pathway is CO2(g)→ COOH*→ CO*→ HCO*→ HCOH* → CH2OH* → CH2* →CH3* → CH4(g), where the first hydrogenation of CO to HCO is predicted as the rate-limiting step of the reaction with slightly lower potential than pre-dicted for Cu electrodes, the most effective catalysts for CO2RR. Methane is predicted to be the main reaction product after eight proton-electron transfers (CO2 + 8 H+ + 8e− → CH4 + 2H2O). The generation of formaldehyde is discarded due to the large formation energy of the adsorbed moiety and the production of methanol is slightly less favorable than methane formation. Our computa-tional study helps to identify suitable electrocatalysts for CO2RR by reducing the amount of metal and using stable and low-cost supports
publishDate 2023
dc.date.none.fl_str_mv 2023
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
peer-reviewed
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10256/23161
http://hdl.handle.net/10256/23161
url http://hdl.handle.net/10256/23161
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.3390/chemistry5020095
info:eu-repo/semantics/altIdentifier/eissn/2624-8549
PID2021-127423NB-I00
PID2020-113711GB-I00
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-127423NB-I00
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2020-113711GB-I00
dc.rights.none.fl_str_mv Reconeixement 4.0 Internacional
http://creativecommons.org/licenses/by/4.0
info:eu-repo/semantics/openAccess
rights_invalid_str_mv Reconeixement 4.0 Internacional
http://creativecommons.org/licenses/by/4.0
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 12 p.
application/pdf
dc.publisher.none.fl_str_mv MDPI (Multidisciplinary Digital Publishing Institute)
publisher.none.fl_str_mv MDPI (Multidisciplinary Digital Publishing Institute)
dc.source.none.fl_str_mv Chemistry, 2022, vol. 5, p. 1395-1406
Articles publicats (D-Q)
Vidal-López, Anna Posada-Pérez, Sergio Solà i Puig, Miquel Poater Teixidor, Albert 2022 Au Single Metal Atom for Carbon Dioxide Reduction Reaction Chemistry 5 1395 1406
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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