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Dy@D2(21)-C84: isolation and crystallographic characterization of a rare trivalent C84-based monometallofullerene

Shen, Wangqiang ; Lei, Lou ; Yiao Wei ; Bao, Lipiao ; Xu, Guangqing ; Peng, Jin ; Lv, Jun ; Lu, Xing

Inorganic chemistry frontiers, 2023-07, Vol.10 (14), p.4139-4146 [Periódico revisado por pares]

London: Royal Society of Chemistry

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  • Título:
    Dy@D2(21)-C84: isolation and crystallographic characterization of a rare trivalent C84-based monometallofullerene
  • Autor: Shen, Wangqiang ; Lei, Lou ; Yiao Wei ; Bao, Lipiao ; Xu, Guangqing ; Peng, Jin ; Lv, Jun ; Lu, Xing
  • Assuntos: Cages ; Crystallography ; Dysprosium ; Fullerenes ; Hexagons ; High temperature ; Inorganic chemistry ; Rare earth elements
  • É parte de: Inorganic chemistry frontiers, 2023-07, Vol.10 (14), p.4139-4146
  • Descrição: Monometallofullerenes (mono-EMFs), which only contain one metal atom inside the fullerene cage, are the most basic yet crucial prototypes to understand the structures and characteristics of EMFs. However, although trivalent mono-EMFs are relatively abundant, M@C82 dominates the category so that larger fullerene cages (>C82) have seldom been isolated and structurally elucidated possibly because of their low production yield and poor kinetic stability. Herein, for the first time, a dysprosium-containing mono-EMF with a C84 cage, namely, Dy@D2(21)-C84, has been successfully synthesized and obtained by using a facile method involving Lewis-acid treatment and HPLC separations. Unambiguous X-ray results demonstrate that the C84 cage possesses the rare D2(21) symmetry, and all disordered Dy sites distribute along a band of ten contiguous hexagons, demonstrating the unique interaction between the trivalent Dy ion and C84 cage. Notably, this is the first instance of a trivalent M3+ (M = rare earth metals) and a D2(21)-C84 cage-based mono-EMF isomer that has been documented. Further theoretical calculations confirm its prevailing at high temperatures for EMF formation, and also reveal that the encapsulation of a trivalent Dy ion in this carbon cage is energetically more favorable than those of other C84-based mono-EMFs. This work not only adds a precious member with large cages (>C82) to the renowned trivalent mono-EMF family but also provides new insights into the intriguing metal–cage interactions of such novel EMFs for deeply understanding their unique structures and stabilities.
  • Editor: London: Royal Society of Chemistry
  • Idioma: Inglês
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  • Realização: ABCD-USP USP   Logos de Redes Sociais: Freepik

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