Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts

Oxide-derived Cu has an excellent ability to promote C–C coupling in the electrochemical carbon dioxide reduction reaction. However, these materials largely rearrange under reaction conditions; therefore, the nature of the active site remains controversial. Here we study the reduction process of oxi...

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Detalles Bibliográficos
Autores: Lian, Zan, Dattila, Federico, López, Núria
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2024
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:2072/537504
Acceso en línea:http://hdl.handle.net/2072/537504
https://doi.org/10.1038/s41929-024-01132-5
Access Level:acceso abierto
Palabra clave:Química
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spelling Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalystsLian, ZanDattila, FedericoLópez, NúriaQuímica54Oxide-derived Cu has an excellent ability to promote C–C coupling in the electrochemical carbon dioxide reduction reaction. However, these materials largely rearrange under reaction conditions; therefore, the nature of the active site remains controversial. Here we study the reduction process of oxide-derived Cu via large-scale molecular dynamics with a precise neural network potential trained on first-principles data and introducing experimental conditions. The oxygen concentration in the most stable oxide-derived Cu increases with an increase of the pH, potential or specific surface area. In long electrochemical experiments, the catalyst would be fully reduced to Cu, but removing all the trapped oxygen takes a considerable amount of time. Although the highly reconstructed Cu surface provides various sites to adsorb oxygen more strongly, the surface oxygen atoms are not stable under common experimental conditions. This work provides insight into the evolution of oxide-derived Cu catalysts and residual oxygen during reaction and also a deep understanding of the nature of active sites.Springer Nature2024info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersion11 p.application/pdfhttp://hdl.handle.net/2072/537504https://doi.org/10.1038/s41929-024-01132-5RECERCAT (Dipòsit de la Recerca de Catalunya)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésEuropean Union’s Horizon Europe research and innovation programme under the Marie Skłodowska-Curie grant, agreement no. 101064867 (DESCRIPTOR project)Spanish Ministry of Science and Innovation (ref. no. PID2021-122516OB-I00, Severo Ochoa Center of Excellence CEX2019-000925-S)Creative Commons Attribution 4.0 International Licenseinfo:eu-repo/semantics/openAccessoai:recercat.cat:2072/5375042026-05-29T05:05:01Z
dc.title.none.fl_str_mv Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts
title Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts
spellingShingle Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts
Lian, Zan
Química
54
title_short Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts
title_full Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts
title_fullStr Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts
title_full_unstemmed Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts
title_sort Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts
dc.creator.none.fl_str_mv Lian, Zan
Dattila, Federico
López, Núria
author Lian, Zan
author_facet Lian, Zan
Dattila, Federico
López, Núria
author_role author
author2 Dattila, Federico
López, Núria
author2_role author
author
dc.subject.none.fl_str_mv Química
54
topic Química
54
description Oxide-derived Cu has an excellent ability to promote C–C coupling in the electrochemical carbon dioxide reduction reaction. However, these materials largely rearrange under reaction conditions; therefore, the nature of the active site remains controversial. Here we study the reduction process of oxide-derived Cu via large-scale molecular dynamics with a precise neural network potential trained on first-principles data and introducing experimental conditions. The oxygen concentration in the most stable oxide-derived Cu increases with an increase of the pH, potential or specific surface area. In long electrochemical experiments, the catalyst would be fully reduced to Cu, but removing all the trapped oxygen takes a considerable amount of time. Although the highly reconstructed Cu surface provides various sites to adsorb oxygen more strongly, the surface oxygen atoms are not stable under common experimental conditions. This work provides insight into the evolution of oxide-derived Cu catalysts and residual oxygen during reaction and also a deep understanding of the nature of active sites.
publishDate 2024
dc.date.none.fl_str_mv 2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/2072/537504
https://doi.org/10.1038/s41929-024-01132-5
url http://hdl.handle.net/2072/537504
https://doi.org/10.1038/s41929-024-01132-5
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv European Union’s Horizon Europe research and innovation programme under the Marie Skłodowska-Curie grant, agreement no. 101064867 (DESCRIPTOR project)
Spanish Ministry of Science and Innovation (ref. no. PID2021-122516OB-I00, Severo Ochoa Center of Excellence CEX2019-000925-S)
dc.rights.none.fl_str_mv Creative Commons Attribution 4.0 International License
info:eu-repo/semantics/openAccess
rights_invalid_str_mv Creative Commons Attribution 4.0 International License
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 11 p.
application/pdf
dc.publisher.none.fl_str_mv Springer Nature
publisher.none.fl_str_mv Springer Nature
dc.source.none.fl_str_mv RECERCAT (Dipòsit de la Recerca de Catalunya)
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 15,812429

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