The Smallest Stable Fullerene, M@C28(M = Ti, Zr, U): Stabilization and Growth from Carbon Vapor,Journal of the American Chemical Society

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The Smallest Stable Fullerene, M@C28(M = Ti, Zr, U): Stabilization and Growth from Carbon Vapor
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2012-05-24 , DOI: 10.1021/ja302398h
Paul W. Dunk ₁ , Nathan K. Kaiser ₂ , Marc Mulet-Gas ₃ , Antonio Rodríguez-Fortea ₃ , Josep M. Poblet ₃ , Hisanori Shinohara ₄ , Christopher L. Hendrickson _{1,

2} , Alan G. Marshall _{1,

2} , Harold W. Kroto ₁

Affiliation

The smallest fullerene to form in condensing carbon vapor has received considerable interest since the discovery of Buckminsterfullerene, C(60). Smaller fullerenes remain a largely unexplored class of all-carbon molecules that are predicted to exhibit fascinating properties due to the large degree of curvature and resulting highly pyramidalized carbon atoms in their structures. However, that curvature also renders the smallest fullerenes highly reactive, making them difficult to detect experimentally. Gas-phase attempts to investigate the smallest fullerene by stabilization through cage encapsulation of a metal have been hindered by the complexity of mass spectra that result from vaporization experiments which include non-fullerene clusters, empty cages, and metallofullerenes. We use high-resolution FT-ICR mass spectrometry to overcome that problem and investigate formation of the smallest fullerene by use of a pulsed laser vaporization cluster source. Here, we report that the C(28) fullerene stabilized by encapsulation with an appropriate metal forms directly from carbon vapor as the smallest fullerene under our conditions. Its stabilization is investigated, and we show that M@C(28) is formed by a bottom-up growth mechanism and is a precursor to larger metallofullerenes. In fact, it appears that the encapsulating metal species may catalyze or nucleate endohedral fullerene formation.

中文翻译：

最小的稳定富勒烯，M@C28(M = Ti, Zr, U)：碳蒸气的稳定和生长

自从发现巴克敏斯特富勒烯 C(60) 以来，在冷凝碳蒸气中形成的最小的富勒烯引起了相当大的兴趣。较小的富勒烯仍然是一大类尚未开发的全碳分子，由于大的曲率和在其结构中产生的高度金字塔化的碳原子，预计这些分子将表现出迷人的特性。然而，这种曲率也使最小的富勒烯具有高度反应性，使它们难以通过实验检测。气相通过金属笼包封来研究最小富勒烯的尝试受到了由包括非富勒烯簇、空笼和金属富勒烯在内的汽化实验产生的质谱复杂性的阻碍。我们使用高分辨率 FT-ICR 质谱来克服这个问题，并通过使用脉冲激光汽化簇源研究最小富勒烯的形成。在这里，我们报告说，在我们的条件下，C(28) 富勒烯通过用适当的金属直接从碳蒸气中封装而稳定，作为最小的富勒烯。对其稳定性进行了研究，我们表明 M@C(28) 是通过自下而上的生长机制形成的，并且是较大金属富勒烯的前体。事实上，封装金属物质似乎可以催化或成核内嵌富勒烯的形成。我们报告说，在我们的条件下，通过用适当的金属包封而稳定的 C(28) 富勒烯直接从碳蒸气中形成为最小的富勒烯。对其稳定性进行了研究，我们表明 M@C(28) 是通过自下而上的生长机制形成的，并且是较大金属富勒烯的前体。事实上，封装金属物质似乎可以催化或成核内嵌富勒烯的形成。我们报告说，在我们的条件下，通过用适当的金属包封而稳定的 C(28) 富勒烯直接从碳蒸气中形成为最小的富勒烯。对其稳定性进行了研究，我们表明 M@C(28) 是通过自下而上的生长机制形成的，并且是较大金属富勒烯的前体。事实上，封装金属物质似乎可以催化或成核内嵌富勒烯的形成。

更新日期：2012-05-24

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