Methodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes

Hydrogenated small fullerenes (Cn, n < 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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Autores principales:	Yuri Tanuma, Toru Maekawa, Chris Ewels
Formato:	article
Lenguaje:	EN
Publicado:	MDPI AG 2021
Materias:	fullerene hydrogenation DFT functionalisation growth xTB Crystallography QD901-999
Acceso en línea:	https://doaj.org/article/0d4a4e52f6de4b4ba902539a360a8ade
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spelling	oai:doaj.org-article:0d4a4e52f6de4b4ba902539a360a8ade2021-11-25T17:18:24ZMethodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes10.3390/cryst111113342073-4352https://doaj.org/article/0d4a4e52f6de4b4ba902539a360a8ade2021-11-01T00:00:00Zhttps://www.mdpi.com/2073-4352/11/11/1334https://doaj.org/toc/2073-4352Hydrogenated 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.Yuri TanumaToru MaekawaChris EwelsMDPI AGarticlefullerenehydrogenationDFTfunctionalisationgrowthxTBCrystallographyQD901-999ENCrystals, Vol 11, Iss 1334, p 1334 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	fullerene hydrogenation DFT functionalisation growth xTB Crystallography QD901-999
spellingShingle	fullerene hydrogenation DFT functionalisation growth xTB Crystallography QD901-999 Yuri Tanuma Toru Maekawa Chris Ewels Methodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes
description	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.
format	article
author	Yuri Tanuma Toru Maekawa Chris Ewels
author_facet	Yuri Tanuma Toru Maekawa Chris Ewels
author_sort	Yuri Tanuma
title	Methodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes
title_short	Methodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes
title_full	Methodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes
title_fullStr	Methodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes
title_full_unstemmed	Methodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes
title_sort	methodological investigation for hydrogen addition to small cage carbon fullerenes
publisher	MDPI AG
publishDate	2021
url	https://doaj.org/article/0d4a4e52f6de4b4ba902539a360a8ade
work_keys_str_mv	AT yuritanuma methodologicalinvestigationforhydrogenadditiontosmallcagecarbonfullerenes AT torumaekawa methodologicalinvestigationforhydrogenadditiontosmallcagecarbonfullerenes AT chrisewels methodologicalinvestigationforhydrogenadditiontosmallcagecarbonfullerenes
_version_	1718412511186780160

Methodological Investigation for Hydrogen Addition to Small Cage Carbon Fullerenes

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