visitante ::
identificación
|
|||||||||||||||
Buscar | Enviar | Ayuda | Servicio de Bibliotecas | Sobre el DDD | Català English Español |
Página principal > Artículos > Artículos publicados > Site-specific axial oxygen coordinated FeN4 active sites for highly selective electroreduction of carbon dioxide |
Fecha: | 2022 |
Resumen: | Regulating the coordination environment via heteroatoms to break the symmetrical electronic structure of M-N active sites provides a promising route to engineer metal-nitrogen-carbon catalysts for electrochemical CO reduction reaction. However, it remains challenging to realize a site-specific introduction of heteroatoms at atomic level due to their energetically unstable nature. Here, this paper reports a facile route via using an oxygen- and nitrogen-rich metal-organic framework (MOF) (IRMOF-3) as the precursor to construct the Fe-O and Fe-N chelation, simultaneously, resulting in an atomically dispersed axial O-coordinated FeN active site. Compared to the FeN active sites without O coordination, the formed FeN-O sites exhibit much better catalytic performance toward CO, reaching a maximum FE of 95% at −0. 50 V versus reversible hydrogen electrode. To the best of the authors' knowledge, such performance exceeds that of the existing Fe-N-C-based catalysts derived from sole N-rich MOFs. Density functional theory calculations indicate that the axial O-coordination regulates the binding energy of intermediates in the reaction pathways, resulting in a smoother desorption of CO and increased energy for the competitive hydrogen production. |
Ayudas: | European Commission 823717 European Commission 101030637 Agencia Estatal de Investigación PID2020-116093RB-C43 Ministerio de Ciencia e Innovación SEV-2017-0706 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-327 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-1246 |
Nota: | Altres ajuts: ICN2 and IREC were funded by the CERCA Programme/Generalitat de Catalunya. |
Derechos: | 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. |
Lengua: | Anglès |
Documento: | Article ; recerca ; Versió publicada |
Materia: | CO generation ; CO2 electroreduction ; FeN4-O active sites ; Metal-organic frameworks ; Single atom catalysts |
Publicado en: | Advanced functional materials, Vol. 32, issue 18 (May 2022) , art. 2111446, ISSN 1616-3028 |
9 p, 2.1 MB |