Electronic Effects Determine the Selectivity of Planar Au–Cu Bimetallic Thin Films for Electrochemical CO2 Reduction
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INVESTIGACIONMetadatos
Título
Electronic Effects Determine the Selectivity of Planar Au–Cu Bimetallic Thin Films for Electrochemical CO2 ReductionAutoría
Fecha de publicación
2019-04-10Editor
American Chemical SocietyISSN
1944-8244; 1944-8252Cita bibliográfica
Kai Liu, Ming Ma, Longfei Wu, Marco Valenti, Drialys Cardenas-Morcoso, Jan P. Hofmann, Juan Bisquert, Sixto Gimenez, and Wilson A. Smith ACS Applied Materials & Interfaces 2019 11 (18), 16546-16555. DOI: 10.1021/acsami.9b01553Tipo de documento
info:eu-repo/semantics/articleVersión de la editorial
https://pubs.acs.org/doi/abs/10.1021/acsami.9b01553Versión
info:eu-repo/semantics/publishedVersionPalabras clave / Materias
Resumen
Au–Cu bimetallic thin films with controlled composition were fabricated by magnetron sputtering co-deposition, and their performance for the electrocatalytic reduction of CO2 was investigated. The uniform planar ... [+]
Au–Cu bimetallic thin films with controlled composition were fabricated by magnetron sputtering co-deposition, and their performance for the electrocatalytic reduction of CO2 was investigated. The uniform planar morphology served as a platform to evaluate the electronic effect isolated from morphological effects while minimizing geometric contributions. The catalytic selectivity and activity of Au–Cu alloys was found to be correlated with the variation of electronic structure that was varied with tunable composition. Notably, the d-band center gradually shifted away from the Fermi level with increasing Au atomic ratio, leading to a weakened binding energy of *CO, which is consistent with low CO coverage observed in CO stripping experiments. The decrease in the *CO binding strength results in the enhanced catalytic activity for CO formation with the increase in Au content. In addition, it was observed that copper oxide/hydroxide species are less stable on Au–Cu surfaces compared to those on the pure Cu surface, where the surface oxophilicity could be critical to tuning the binding strength of *OCHO. These results imply that the altered electronic structure could explain the decreased formation of HCOO– on the Au–Cu alloys. In general, the formation of CO and HCOO– as main CO2 reduction products on planar Au–Cu alloys followed the shift of the d-band center, which indicates that the electronic effect is the major governing factor for the electrocatalytic activity of CO2 reduction on Au–Cu bimetallic thin films. [-]
Publicado en
ACS applied materials & interfaces, 2019, vol. 11, no 18Proyecto de investigación
China Scholarship Council: 201507565007; Netherlands Organization for Scientific Research (NWO)Derechos de acceso
info:eu-repo/semantics/openAccess
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