Au Single Metal Atom for Carbon Dioxide Reduction Reaction
Vidal-López, Anna (Universitat Autònoma de Barcelona. Departament de Química)
Posada-Pérez, Sergio (Universitat de Girona. Institut de Química Computacional i Catàlisi)
Solà i Puig, Miquel (Universitat de Girona. Institut de Química Computacional i Catàlisi)
Poater, Albert (Universitat de Girona. Institut de Química Computacional i Catàlisi)

Data:	2023
Resum:	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 added-value products. We use density functional theory (DFT) to determine the reaction Gibbs energies for eight electron-proton transfer reaction paths of the electrochemical carbon dioxide reduction reaction (CO2RR) using a single Au atom supported on 2D carbon nitride support. Our simulations classify the Au1@g-C3N4 electrocatalysts as "beyond CO" since their formation is energetically 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 predicted 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 computational study helps to identify suitable electrocatalysts for CO2RR by reducing the amount of metal and using stable and low-cost supports.
Ajuts:	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-0623 Ministerio de Ciencia e Innovación PRE2019-089647 European Commission 101020330
Nota:	Altres ajuts: ICREA Academia
Drets:	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.
Llengua:	Anglès
Document:	Article ; recerca ; Versió publicada
Matèria:	Electrocatalysis ; Carbon dioxide reduction ; Au single metal atom ; Carbon nitride ; Computational hydrogen electrode ; Methane production
Publicat a:	Chemistry (Switzerland), Vol. 5, Issue 2 (June 2023) , p. 1395-1406, ISSN 2624-8549

DOI: 10.3390/chemistry5020095

12 p, 1.8 MB

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