Electron Microscopic Imaging of a Single Group 8 Metal Atom Catalyzing C鈥揅 Bond Reorganization of Fullerenes

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• 作者：Eiichi Nakamura ; Masanori Koshino ; Takeshi Saito ; Yoshiko Niimi ; Kazu Suenaga ; Yutaka Matsuo
• 刊名：Journal of the American Chemical Society
• 出版年：2011
• 出版时间：September 14, 2011
• 年：2011
• 卷：133
• 期：36
• 页码：14151-14153
• 全文大小：764K
• 年卷期：v.133,no.36(September 14, 2011)
• ISSN：1520-5126

文摘

Heating a bulk sample of [60]fullerene complexes, (畏⁵-C₅H₅)MC₆₀R₅ (M = Fe, Ru, R = Me, Ph), produces small hydrocarbons because of coupling of R and C₅H₅ via C鈥揅 and C鈥揌 bond activation. Upon observation by transmission electron microscopy, these complexes, encapsulated in single-walled carbon nanotubes, underwent C鈥揅 bond reorganization reactions to form new C鈥揅 bond networks, including a structure reminiscent of [70]fullerene. Quantitative comparison of the electron dose required to effect the C鈥揅 bond reorganization of fullerenes and organofullerenes in the presence of a single atom of Ru, Fe, or Ln and in the the absence of metal atoms indicated high catalytic activity of Ru and Fe atoms, as opposed to no catalytic activity of Ln. Organic molecules such as hydrocarbons and amides as well as pristine [60]fullerene maintain their structural integrity upon irradiation by ca. 100 times higher electron dose compared to the Ru and Fe organometallics. The results not only represent a rare example of direct observation of a single-metal catalysis but also have implications for the use of single metal atom catalysis in Group 8 metal heterogeneous catalysis.