Articles producció científica> Química Física i Inorgànica

U2N@: I h(7)-C80: fullerene cage encapsulating an unsymmetrical U(iv)NU(v) cluster

  • Identification data

    Identifier: imarina:9139079
    Authors:
    Li, XiaomengRosello, YannickYao, Yang-RongZhuang, JiaxinZhang, XingxingRodriguez-Fortea, Antoniode Graaf, CoenEchegoyen, LuisPoblet, Josep MChen, Ning
    Abstract:
    © 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.
  • Others:

    Author, as appears in the article.: Li, Xiaomeng; Rosello, Yannick; Yao, Yang-Rong; Zhuang, Jiaxin; Zhang, Xingxing; Rodriguez-Fortea, Antonio; de Graaf, Coen; Echegoyen, Luis; Poblet, Josep M; Chen, Ning
    Department: Química Física i Inorgànica
    e-ISSN: 2041-6539
    URV's Author/s: De Graaf, Cornelis / Poblet Rius, Josep Maria / Rodríguez Fortea, Antonio / Rosello Marin, Yannick / ZHANG, XIAO
    Abstract: © 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.
    Thematic Areas: Química Materiais Interdisciplinar General chemistry Farmacia Ciências biológicas iii Ciências biológicas i Chemistry, multidisciplinary Chemistry (miscellaneous) Chemistry (all) Astronomia / física
    licence for use: https://creativecommons.org/licenses/by/3.0/es/
    ISSN: 2041-6520
    Author's mail: coen.degraaf@urv.cat yannick.rosello@estudiants.urv.cat josepmaria.poblet@urv.cat antonio.rodriguezf@urv.cat
    Author identifier: 0000-0001-8114-6658 0000-0002-4533-0623 0000-0001-5884-5629
    Record's date: 2024-10-12
    Papper version: info:eu-repo/semantics/publishedVersion
    Link to the original source: https://pubs.rsc.org/en/content/articlelanding/2021/sc/d0sc04677a#!divAbstract
    Licence document URL: https://repositori.urv.cat/ca/proteccio-de-dades/
    Papper original source: Chemical Science. 12 (1): 282-292
    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
    Article's DOI: 10.1039/d0sc04677a
    Entity: Universitat Rovira i Virgili
    Journal publication year: 2021
    Publication Type: Journal Publications
  • Keywords:

    Chemistry (Miscellaneous),Chemistry, Multidisciplinary
    Química
    Materiais
    Interdisciplinar
    General chemistry
    Farmacia
    Ciências biológicas iii
    Ciências biológicas i
    Chemistry, multidisciplinary
    Chemistry (miscellaneous)
    Chemistry (all)
    Astronomia / física
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