Articles producció científica> Química Física i Inorgànica

Probing the formation of halogenated endohedral metallofullerenes: Predictions confirmed by experiments

  • Dades identificatives

    Identificador: imarina:3672884
    Autors:
    Moreno-Vicente A., Mulet-Gas M., Dunk P., Poblet J., Rodríguez-Fortea A.
    Resum:
    The functionalization of endohedral metallofullerenes by halogenation has not been previously reported and remains a challenging endeavor in carbon nanoscience. In this work, we show that halogenation of endohedral metallofullerenes is predicted to be feasible based on thermodynamic grounds by means of DFT computations, combined with in situ experimental investigations. Computed bond energies for the chlorination, fluorination and hydrogenation of endohedral metallofullerenes that span a range of cage sizes are found to be comparable to those of known halogenated and hydrogenated empty fullerenes. Therefore, we propose that new forms of functionalized metallofullerenes should be synthesized under appropriate experimental conditions, despite many prior unsuccessful attempts. Indeed, we experimentally show for the first time that M@C2n (M = metal) metallofullerenes and the prototypical Sc3N@C80 clusterfullerene can be fluorinated by two different routes under the typical 'harsh' gas phase conditions of metallofullerene plasma synthesis, and at lower extents that could avoid cage degradation. The combination of halogenation and metal encapsulation offers the potential to create new radical-quenched, functionalized endohedral metallofullerenes that possess stable, large-gap carbon cages. These results open new avenues for the synthesis and stabilization of encapsulated molecular nanocarbons.
  • Altres:

    Autor segons l'article: Moreno-Vicente A., Mulet-Gas M., Dunk P., Poblet J., Rodríguez-Fortea A.
    Departament: Química Física i Inorgànica
    Autor/s de la URV: Poblet Rius, Josep Maria / Rodríguez Fortea, Antonio
    Paraules clau: Fullerenes
    Resum: The functionalization of endohedral metallofullerenes by halogenation has not been previously reported and remains a challenging endeavor in carbon nanoscience. In this work, we show that halogenation of endohedral metallofullerenes is predicted to be feasible based on thermodynamic grounds by means of DFT computations, combined with in situ experimental investigations. Computed bond energies for the chlorination, fluorination and hydrogenation of endohedral metallofullerenes that span a range of cage sizes are found to be comparable to those of known halogenated and hydrogenated empty fullerenes. Therefore, we propose that new forms of functionalized metallofullerenes should be synthesized under appropriate experimental conditions, despite many prior unsuccessful attempts. Indeed, we experimentally show for the first time that M@C2n (M = metal) metallofullerenes and the prototypical Sc3N@C80 clusterfullerene can be fluorinated by two different routes under the typical 'harsh' gas phase conditions of metallofullerene plasma synthesis, and at lower extents that could avoid cage degradation. The combination of halogenation and metal encapsulation offers the potential to create new radical-quenched, functionalized endohedral metallofullerenes that possess stable, large-gap carbon cages. These results open new avenues for the synthesis and stabilization of encapsulated molecular nanocarbons.
    Àrees temàtiques: Química Medicina iii Medicina i Materials science, multidisciplinary Materials science (miscellaneous) Materials science (all) Materials science Materiais Interdisciplinar General materials science General chemistry Farmacia Ensino Engenharias iv Engenharias iii Engenharias ii Ciências biológicas ii Ciências biológicas i Ciências ambientais Chemistry, physical Chemistry (miscellaneous) Chemistry (all) Biotecnología Astronomia / física
    ISSN: 00086223
    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: 2024-09-07
    Versió de l'article dipositat: info:eu-repo/semantics/acceptedVersion
    Enllaç font original: https://www.sciencedirect.com/science/article/abs/pii/S0008622317312897
    URL Document de llicència: https://repositori.urv.cat/ca/proteccio-de-dades/
    Referència a l'article segons font original: Carbon. 129 750-757
    Referència de l'ítem segons les normes APA: Moreno-Vicente A., Mulet-Gas M., Dunk P., Poblet J., Rodríguez-Fortea A. (2018). Probing the formation of halogenated endohedral metallofullerenes: Predictions confirmed by experiments. Carbon, 129(), 750-757. DOI: 10.1016/j.carbon.2017.12.056
    DOI de l'article: 10.1016/j.carbon.2017.12.056
    Entitat: Universitat Rovira i Virgili
    Any de publicació de la revista: 2018
    Tipus de publicació: Journal Publications
  • Paraules clau:

    Chemistry (Miscellaneous),Chemistry, Physical,Materials Science,Materials Science (Miscellaneous),Materials Science, Multidisciplinary
    Fullerenes
    Química
    Medicina iii
    Medicina i
    Materials science, multidisciplinary
    Materials science (miscellaneous)
    Materials science (all)
    Materials science
    Materiais
    Interdisciplinar
    General materials science
    General chemistry
    Farmacia
    Ensino
    Engenharias iv
    Engenharias iii
    Engenharias ii
    Ciências biológicas ii
    Ciências biológicas i
    Ciências ambientais
    Chemistry, physical
    Chemistry (miscellaneous)
    Chemistry (all)
    Biotecnología
    Astronomia / física
  • Documents:

  • Cerca a google

    Search to google scholar