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通过表面催化环脱氢反应由芳香族前体合成富勒烯。

Fullerenes from aromatic precursors by surface-catalysed cyclodehydrogenation.

作者信息

Otero Gonzalo, Biddau Giulio, Sánchez-Sánchez Carlos, Caillard Renaud, López María F, Rogero Celia, Palomares F Javier, Cabello Noemí, Basanta Miguel A, Ortega José, Méndez Javier, Echavarren Antonio M, Pérez Rubén, Gómez-Lor Berta, Martín-Gago José A

机构信息

Instituto de Ciencia de Materiales de Madrid (CSIC), Cantoblanco, 28049 Madrid, Spain.

出版信息

Nature. 2008 Aug 14;454(7206):865-8. doi: 10.1038/nature07193.

Abstract

Graphite vaporization provides an uncontrolled yet efficient means of producing fullerene molecules. However, some fullerene derivatives or unusual fullerene species might only be accessible through rational and controlled synthesis methods. Recently, such an approach has been used to produce isolable amounts of the fullerene C(60) from commercially available starting materials. But the overall process required 11 steps to generate a suitable polycyclic aromatic precursor molecule, which was then dehydrogenated in the gas phase with a yield of only about one per cent. Here we report the formation of C(60) and the triazafullerene C(57)N(3) from aromatic precursors using a highly efficient surface-catalysed cyclodehydrogenation process. We find that after deposition onto a platinum (111) surface and heating to 750 K, the precursors are transformed into the corresponding fullerene and triazafullerene molecules with about 100 per cent yield. We expect that this approach will allow the production of a range of other fullerenes and heterofullerenes, once suitable precursors are available. Also, if the process is carried out in an atmosphere containing guest species, it might even allow the encapsulation of atoms or small molecules to form endohedral fullerenes.

摘要

石墨汽化提供了一种生产富勒烯分子的不受控制但高效的方法。然而,一些富勒烯衍生物或不寻常的富勒烯物种可能只能通过合理且可控的合成方法获得。最近,这种方法已被用于从市售起始原料生产可分离量的富勒烯C(60)。但整个过程需要11个步骤来生成合适的多环芳族前体分子,然后该前体分子在气相中脱氢,产率仅约为1%。在此,我们报告了使用高效的表面催化环脱氢过程从芳族前体形成C(60)和三氮杂富勒烯C(57)N(3)。我们发现,在沉积到铂(111)表面并加热到750 K后,前体被转化为相应的富勒烯和三氮杂富勒烯分子,产率约为100%。我们预计,一旦有合适的前体,这种方法将能够生产一系列其他富勒烯和杂富勒烯。此外,如果该过程在含有客体物种的气氛中进行,甚至可能允许原子或小分子被包封以形成内嵌富勒烯。

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