Autor según el artículo: Li, Xiaomeng; Rosello, Yannick; Yao, Yang-Rong; Zhuang, Jiaxin; Zhang, Xingxing; Rodriguez-Fortea, Antonio; de Graaf, Coen; Echegoyen, Luis; Poblet, Josep M; Chen, Ning
Departamento: Química Física i Inorgànica
e-ISSN: 2041-6539
Autor/es de la URV: De Graaf, Cornelis / Poblet Rius, Josep Maria / Rodríguez Fortea, Antonio / Rosello Marin, Yannick / ZHANG, XIAO
Resumen: © 2021 The Royal Society of Chemistry. For the first time, an actinide nitride clusterfullerene, U2N@Ih(7)-C80, is synthesized and fully characterized by X-ray single crystallography and multiple spectroscopic methods. U2N@Ih(7)-C80 is by far the first endohedral fullerene that violates the well-established tri-metallic nitride template for nitride clusterfullerenes. The novel UNU cluster features two UN bonds with uneven bond distances of 2.058(3) Å and 1.943(3) Å, leading to a rare unsymmetrical structure for the dinuclear nitride motif. The combined experimental and theoretical investigations suggest that the two uranium ions show different oxidation states of +4 and +5. Quantum-chemical investigation further reveals that the f1/f2 population dominantly induces a distortion of the UNU cluster, which leads to the unsymmetrical structure. A comparative study of U2X@C80 (X = C, N and O) reveals that the U-X interaction in UXU clusters can hardly be seen as being formed by classical multiple bonds, but is more like an anionic central ion Xq- with biased overlaps with the two metal ions, which decrease as the electronegativity of X increases. This study not only demonstrates the unique bonding variety of actinide clusters stabilized by fullerene cages, showing different bonding from that observed for the lanthanide analogs, it also reveals the electronic structure of the UXU clusters (X = C, N and O), which are of fundamental significance to understanding these actinide bonding motifs.
Áreas temáticas: Química Materiais Interdisciplinar General chemistry Farmacia Ciências biológicas iii Ciências biológicas i Chemistry, multidisciplinary Chemistry (miscellaneous) Chemistry (all) Astronomia / física
Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/
ISSN: 2041-6520
Direcció de correo del autor: coen.degraaf@urv.cat yannick.rosello@estudiants.urv.cat josepmaria.poblet@urv.cat antonio.rodriguezf@urv.cat
Identificador del autor: 0000-0001-8114-6658 0000-0002-4533-0623 0000-0001-5884-5629
Fecha de alta del registro: 2024-10-12
Versión del articulo depositado: info:eu-repo/semantics/publishedVersion
Enlace a la fuente original: https://pubs.rsc.org/en/content/articlelanding/2021/sc/d0sc04677a#!divAbstract
URL Documento de licencia: https://repositori.urv.cat/ca/proteccio-de-dades/
Referencia al articulo segun fuente origial: Chemical Science. 12 (1): 282-292
Referencia de l'ítem segons les normes APA: Li, Xiaomeng; Rosello, Yannick; Yao, Yang-Rong; Zhuang, Jiaxin; Zhang, Xingxing; Rodriguez-Fortea, Antonio; de Graaf, Coen; Echegoyen, Luis; Poblet, J (2021). U2N@: I h(7)-C80: fullerene cage encapsulating an unsymmetrical U(iv)NU(v) cluster. Chemical Science, 12(1), 282-292. DOI: 10.1039/d0sc04677a
DOI del artículo: 10.1039/d0sc04677a
Entidad: Universitat Rovira i Virgili
Año de publicación de la revista: 2021
Tipo de publicación: Journal Publications