Autor según el artículo: Poblet, JM; Luis Echegoyen; Ning Chen; Rodriguez-Fortea, A; Wenting Cai; Roser Morales-Martínez; Xingxing Zhang; Daniel Najera; Elkin L. Romero; Alejandro Metta-Magaña; Skye Fortier
Departamento: Química Física i Inorgànica
Autor/es de la URV: POBLET RIUS, JOSEP MARIA; Luis Echegoyen; Ning Chen; RODRÍGUEZ FORTEA, ANTONIO; Wenting Cai; Roser Morales-Martínez; Xingxing Zhang; Daniel Najera; Elkin L. Romero; Alejandro Metta-Magaña; Skye Fortier
Resumen: Charge transfer is a general phenomenon observed for all endohedral mono-metallofullerenes. Since the detection of the first endohedral metallofullerene (EMF), La@C82, in 1991, it has always been observed that the oxidation state of a given encapsulated metal is always the same, regardless of the cage size. No crystallographic data exist for any early actinide endohedrals and little is known about the oxidation states for the few compounds that have been reported. Here we report the X-ray structures of three uranium metallofullerenes, U@D3h-C74, U@C2(5)-C82 and U@C2v(9)-C82, and provide theoretical evidence for cage isomer dependent charge transfer states for U. Results from DFT calculations show that U@D3h-C74 and U@C2(5)-C82 have tetravalent electronic configurations corresponding to U4+@D3h-C744− and U4+@C2(5)-C824−. Surprisingly, the isomeric U@C2v(9)-C82 has a trivalent electronic configuration corresponding to U3+@C2v(9)-C823−. These are the first X-ray crystallographic structures of uranium EMFs and this is first observation of metal oxidation state dependence on carbon cage isomerism for mono-EMFs.
Grupo de investigación: Química Quàntica
Áreas temáticas: Química Química Chemistry
Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/
ISSN: 2041-6520
Identificador del autor: 0000-0002-4533-0623; ; ; 0000-0001-5884-5629; ; ; ; ; ; ;
Fecha de alta del registro: 2019-01-14
Página final: 5290
Volumen de revista: 8
Versión del articulo depositado: info:eu-repo/semantics/publishedVersion
URL Documento de licencia: https://repositori.urv.cat/ca/proteccio-de-dades/
Entidad: Universitat Rovira i Virgili
Año de publicación de la revista: 2017
Página inicial: 5282
Tipo de publicación: Article Artículo Article
Repositori URV