Methodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes

Hydrogenated small fullerenes (C<i><sub>n</sub></i>, <i>n</i> < 60) are of interest as potential astrochemical species, and as intermediates in hydrogen-catalysed fullerene growth. However, the computational identification of key stable species is difficult due...

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Detalles Bibliográficos
Autores principales: Yuri Tanuma, Toru Maekawa, Chris Ewels
Formato: article
Lenguaje:EN
Publicado: MDPI AG 2021
Materias:
DFT
xTB
Acceso en línea:https://doaj.org/article/0d4a4e52f6de4b4ba902539a360a8ade
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Sumario:Hydrogenated small fullerenes (C<i><sub>n</sub></i>, <i>n</i> < 60) are of interest as potential astrochemical species, and as intermediates in hydrogen-catalysed fullerene growth. However, the computational identification of key stable species is difficult due to the vast configurationally space of structures. In this study, we explored routes to predict stable hydrogenated small fullerenes. We showed that neither local fullerene geometry nor local electronic structure analysis was able to correctly predict subsequent low-energy hydrogenation sites, and sequential stable addition searches also sometimes failed to identify most stable hydrogenated fullerene isomers. Of the empirical and semi-empirical methods tested, GFN2-xTB consistently gave highly accurate energy correlations (r > 0.99) to full DFT-LDA calculations at a fraction of the computational cost. This allowed identification of the most stable hydrogenated fullerenes up to 4H for four fullerenes, namely two isomers of C<sub>28</sub> and C<sub>40</sub>, via “brute force” systematic testing of all symmetry-inequivalent combinations. The approach shows promise for wider systematic studies of smaller hydrogenated fullerenes.