Autor segons l'article: Cai, Wenting; Morales-Martinez, Roser; Zhang, Xingxing; Najera, Daniel; Romero, Elkin L; Metta-Magana, Alejandro; Rodriguez-Fortea, Antonio; Fortier, Skye; Chen, Ning; Poblet, Josep M; Echegoyen, Luis
Departament: Química Física i Inorgànica
Autor/s de la URV: Morales Martínez, Roser / Poblet Rius, Josep Maria / Rodríguez Fortea, Antonio
Resum: 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- C74(4 -) and U4+@C2(5)-C82(4-) . Surprisingly, the isomeric U@C2v(9)-C82 has a trivalent electronic configuration corresponding to U3+@C2v(9)-C82(3-) . 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.
Àrees temàtiques: Química Materiais Interdisciplinar General chemistry Farmacia Ciências biológicas iii Ciências biológicas i Chemistry, multidisciplinary Chemistry (miscellaneous) Chemistry (all) Astronomia / física
Accès a la llicència d'ús: https://creativecommons.org/licenses/by/3.0/es/
Adreça de correu electrònic de l'autor: josepmaria.poblet@urv.cat antonio.rodriguezf@urv.cat
Identificador de l'autor: 0000-0002-4533-0623 0000-0001-5884-5629
Data d'alta del registre: 2024-10-12
Versió de l'article dipositat: info:eu-repo/semantics/publishedVersion
Enllaç font original: https://pubs.rsc.org/en/content/articlelanding/2017/sc/c7sc01711a
URL Document de llicència: https://repositori.urv.cat/ca/proteccio-de-dades/
Referència a l'article segons font original: Chemical Science. 8 (8): 5282-5290
Referència de l'ítem segons les normes APA: Cai, Wenting; Morales-Martinez, Roser; Zhang, Xingxing; Najera, Daniel; Romero, Elkin L; Metta-Magana, Alejandro; Rodriguez-Fortea, Antonio; Fortier, (2017). Single crystal structures and theoretical calculations of uranium endohedral metallofullerenes (U@C-2n, 2n=74, 82) show cage isomer dependent oxidation states for U. Chemical Science, 8(8), 5282-5290. DOI: 10.1039/c7sc01711a
DOI de l'article: 10.1039/c7sc01711a
Entitat: Universitat Rovira i Virgili
Any de publicació de la revista: 2017
Tipus de publicació: Journal Publications