Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60
Using density functional theory approaches, we follow the sequential addition of CF3 functional groups to the surface of the metallic endofullerene species Gd@C60. The presence of gadolinium in the interior of the cage strongly influences the addition sequence. The calculations are able to successfu...
| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
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The Royal Society
2018-01-01
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| Series: | Royal Society Open Science |
| Subjects: | |
| Online Access: | https://royalsocietypublishing.org/doi/pdf/10.1098/rsos.180588 |
| _version_ | 1818251166913396736 |
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| author | Chris Ewels Jeremy Rio Hiroyuki Niwa Haruka Omachi Hisanori Shinohara Mark Rayson Patrick Briddon |
| author_facet | Chris Ewels Jeremy Rio Hiroyuki Niwa Haruka Omachi Hisanori Shinohara Mark Rayson Patrick Briddon |
| author_sort | Chris Ewels |
| collection | DOAJ |
| description | Using density functional theory approaches, we follow the sequential addition of CF3 functional groups to the surface of the metallic endofullerene species Gd@C60. The presence of gadolinium in the interior of the cage strongly influences the addition sequence. The calculations are able to successfully identify end points in the addition sequence at Gd@C60(CF3)n, n = 3 and two isomers at n = 5, in predictive agreement with experiment. Inverting the algorithm to determine the most labile groups also identifies the correct positively charged Gd@C60(CF3)4+ isomer, as confirmed by experimental mass spectra. The importance of surface mobility, notably at later stage addition, is discussed. |
| first_indexed | 2024-12-12T16:03:58Z |
| format | Article |
| id | doaj.art-d259be33c82c47c88447a4560f0fc9a8 |
| institution | Directory Open Access Journal |
| issn | 2054-5703 |
| language | English |
| last_indexed | 2024-12-12T16:03:58Z |
| publishDate | 2018-01-01 |
| publisher | The Royal Society |
| record_format | Article |
| series | Royal Society Open Science |
| spelling | doaj.art-d259be33c82c47c88447a4560f0fc9a82022-12-22T00:19:22ZengThe Royal SocietyRoyal Society Open Science2054-57032018-01-015910.1098/rsos.180588180588Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60Chris EwelsJeremy RioHiroyuki NiwaHaruka OmachiHisanori ShinoharaMark RaysonPatrick BriddonUsing density functional theory approaches, we follow the sequential addition of CF3 functional groups to the surface of the metallic endofullerene species Gd@C60. The presence of gadolinium in the interior of the cage strongly influences the addition sequence. The calculations are able to successfully identify end points in the addition sequence at Gd@C60(CF3)n, n = 3 and two isomers at n = 5, in predictive agreement with experiment. Inverting the algorithm to determine the most labile groups also identifies the correct positively charged Gd@C60(CF3)4+ isomer, as confirmed by experimental mass spectra. The importance of surface mobility, notably at later stage addition, is discussed.https://royalsocietypublishing.org/doi/pdf/10.1098/rsos.180588metallofullerenesgadoliniumdensity functional calculationsaddition pathways |
| spellingShingle | Chris Ewels Jeremy Rio Hiroyuki Niwa Haruka Omachi Hisanori Shinohara Mark Rayson Patrick Briddon Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60 Royal Society Open Science metallofullerenes gadolinium density functional calculations addition pathways |
| title | Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60 |
| title_full | Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60 |
| title_fullStr | Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60 |
| title_full_unstemmed | Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60 |
| title_short | Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60 |
| title_sort | determining addition pathways and stable isomers for cf3 functionalization of endohedral gd c60 |
| topic | metallofullerenes gadolinium density functional calculations addition pathways |
| url | https://royalsocietypublishing.org/doi/pdf/10.1098/rsos.180588 |
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