2D carbon nitride as a support with single Cu, Ag, and Au atoms for carbon dioxide reduction reaction
Posada-Pérez, Sergio (Universitat de Girona. Departament de Química)
Vidal-López, Anna (Universitat Autònoma de Barcelona. Departament de Química)
Solà i Puig, Miquel (Universitat de Girona. Departament de Química)
Poater, Albert (Universitat Autònoma de Barcelona. Departament de Química)

Date:	2023
Abstract:	The electrochemical conversion of CO into value-added chemicals is an important approach to recycling CO. In this work, we have combined the most efficient metal catalysts for this reaction, namely Cu, Ag, and Au, as single-atom particles dispersed on a two-dimensional carbon nitride support, with the aim of exploring their performance in the CO reduction reaction. Here, we report density functional theory computations showing the effect of single metal-atom particles on the support. We found that bare carbon nitride needed a high overpotential to overcome the energy barrier for the first proton-electron transfer, while the second transfer was exergonic. The deposition of single metal atoms enhances the catalytic activity of the system as the first proton-electron transfer is favored in terms of energy, although strong binding energies were found for CO adsorption on Cu and Au single atoms. Our theoretical interpretations are consistent with the experimental evidence that the competitive H generation is favored due to the strong CO binding energies. Our computational study paves the road to finding suitable metals that catalyze the first proton-electron transfer in the carbon dioxide reduction reaction and produce reaction intermediates with moderate binding energies, promoting a spillover to the carbon nitride support and thereby serving as bifunctional electrocatalysts. Single metal atoms supported on 2D carbon nitride are promising electrocatalysts for carbon dioxide reduction reaction and produce reaction intermediates with moderate binding energies, promoting a spillover to the carbon nitride support and thereby serving as bifunctional electrocatalysts.
Grants:	European Commission 101020330 Agencia Estatal de Investigación PID2021-127423NB-I00 Agencia Estatal de Investigación PID2020-113711GB-I00 Agència de Gestió d'Ajuts Universitaris i de Recerca 2021/SGR-623
Note:	Altres ajuts: Red Española de Supercomputación (QHS-2022-1-0017 and QHS-2022-2-0012)
Rights:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original.
Language:	Anglès
Document:	Article ; recerca ; Versió publicada
Published in:	Physical chemistry chemical physics, Issue 12 (February 2023) , p. 8574-8582, ISSN 1463-9084

DOI: 10.1039/d3cp00392b
PMID: 36883855

9 p, 1.5 MB

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