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Actinide-lanthanide single electron metal-metal bond formed in mixed-valence di-metallofullerenes

Author

Listed:
  • Yingjing Yan

    (Soochow University)

  • Laura Abella

    (Universitat Rovira i Virgili)

  • Rong Sun

    (Peking University)

  • Yu-Hui Fang

    (Peking University)

  • Yannick Roselló

    (Universitat Rovira i Virgili)

  • Yi Shen

    (Soochow University)

  • Meihe Jin

    (Soochow University)

  • Antonio Rodríguez-Fortea

    (Universitat Rovira i Virgili)

  • Coen Graaf

    (Universitat Rovira i Virgili
    ICREA)

  • Qingyu Meng

    (Soochow University)

  • Yang-Rong Yao

    (Soochow University
    University of Science and Technology of China)

  • Luis Echegoyen

    (University of Texas at El Paso, 500 W University Avenue)

  • Bing-Wu Wang

    (Peking University)

  • Song Gao

    (Peking University)

  • Josep M. Poblet

    (Universitat Rovira i Virgili)

  • Ning Chen

    (Soochow University)

Abstract

Understanding metal-metal bonding involving f-block elements has been a challenging goal in chemistry. Here we report a series of mixed-valence di-metallofullerenes, ThDy@C2n (2n = 72, 76, 78, and 80) and ThY@C2n (2n = 72 and 78), which feature single electron actinide-lanthanide metal-metal bonds, characterized by structural, spectroscopic and computational methods. Crystallographic characterization unambiguously confirmed that Th and Y or Dy are encapsulated inside variably sized fullerene carbon cages. The ESR study of ThY@D3h(5)-C78 shows a doublet as expected for an unpaired electron interacting with Y, and a SQUID magnetometric study of ThDy@D3h(5)-C78 reveals a high-spin ground state for the whole molecule. Theoretical studies further confirm the presence of a single-electron bonding interaction between Y or Dy and Th, due to a significant overlap between hybrid spd orbitals of the two metals.

Suggested Citation

  • Yingjing Yan & Laura Abella & Rong Sun & Yu-Hui Fang & Yannick Roselló & Yi Shen & Meihe Jin & Antonio Rodríguez-Fortea & Coen Graaf & Qingyu Meng & Yang-Rong Yao & Luis Echegoyen & Bing-Wu Wang & Son, 2023. "Actinide-lanthanide single electron metal-metal bond formed in mixed-valence di-metallofullerenes," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42165-x
    DOI: 10.1038/s41467-023-42165-x
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    References listed on IDEAS

    as
    1. Josef T. Boronski & John A. Seed & David Hunger & Adam W. Woodward & Joris Slageren & Ashley J. Wooles & Louise S. Natrajan & Nikolas Kaltsoyannis & Stephen T. Liddle, 2021. "A crystalline tri-thorium cluster with σ-aromatic metal–metal bonding," Nature, Nature, vol. 598(7879), pages 72-75, October.
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    3. Jiaxin Zhuang & Roser Morales-Martínez & Jiangwei Zhang & Yaofeng Wang & Yang-Rong Yao & Cuiying Pei & Antonio Rodríguez-Fortea & Shuao Wang & Luis Echegoyen & Coen Graaf & Josep M. Poblet & Ning Chen, 2021. "Characterization of a strong covalent Th3+–Th3+ bond inside an Ih(7)-C80 fullerene cage," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    4. Fupin Liu & Denis S. Krylov & Lukas Spree & Stanislav M. Avdoshenko & Nataliya A. Samoylova & Marco Rosenkranz & Aram Kostanyan & Thomas Greber & Anja U. B. Wolter & Bernd Büchner & Alexey A. Popov, 2017. "Single molecule magnet with an unpaired electron trapped between two lanthanide ions inside a fullerene," Nature Communications, Nature, vol. 8(1), pages 1-9, December.
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