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 frst-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 specifc 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

Stability and lifetime of diffusion-trapped oxygen in oxide-derived copper CO2 reduction electrocatalysts / Lian, Zan; Dattila, Federico; López, Núria. - In: NATURE CATALYSIS. - ISSN 2520-1158. - (2024). [10.1038/s41929-024-01132-5]

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

Federico Dattila;
2024

Abstract

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 frst-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 specifc 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
File in questo prodotto:
File Dimensione Formato  
s41929-024-01132-5.pdf

accesso aperto

Descrizione: Main text
Tipologia: 2a Post-print versione editoriale / Version of Record
Licenza: Creative commons
Dimensione 2.08 MB
Formato Adobe PDF
2.08 MB Adobe PDF Visualizza/Apri
Pubblicazioni consigliate

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11583/2987483