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...
Gespeichert in:
| Veröffentlicht in: | Royal Society open science 2018-09, Vol.5 (9), p.180588-180588 |
|---|---|
| Hauptverfasser: | , , , , , , |
| Format: | Artikel |
| Sprache: | eng |
| Schlagworte: | |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| container_end_page | 180588 |
|---|---|
| container_issue | 9 |
| container_start_page | 180588 |
| container_title | Royal Society open science |
| container_volume | 5 |
| creator | Ewels, Chris Rio, Jeremy Niwa, Hiroyuki Omachi, Haruka Shinohara, Hisanori Rayson, Mark Briddon, Patrick |
| 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. |
| doi_str_mv | 10.1098/rsos.180588 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_royal</sourceid><recordid>TN_cdi_royalsociety_journals_10_1098_rsos_180588</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><doaj_id>oai_doaj_org_article_d259be33c82c47c88447a4560f0fc9a8</doaj_id><sourcerecordid>2188590727</sourcerecordid><originalsourceid>FETCH-LOGICAL-d434t-ce2edd4148a3910577e2d20d20d32793e907004e2ed1adc2bec268794e550bd73</originalsourceid><addsrcrecordid>eNp9kktr3DAQx01paUKaU7-Aj71sOnpZ0qW0bJsHBAJNe-pByNJ4V4ttbSU7ZfPpa8c5ZC8BwYxG__mheRTFRwIXBLT6nHLMF0SBUOpNcUpB8JWQwN6-8E-K85x3AEAEMFnJ98UJA8W0FHBamO84YOpCH_pNab0PQ4h9ubfD9p895NL2vsyDrVssQ44dplw2MZXrS1Y2Y-9msW3Do33Kik2JvY9b9Mm25ZX_uq7gQ_GusW3G82d7Vvy-_PFrfb26vbu6WX-7XXnO-LBySNF7TriyTBMQUiL1FObDqNQMNUgAPquI9Y7W6GilpOYoBNResrPiZuH6aHdmn0Jn08FEG8xTIKaNsWkIrkXjqdA1MuYUdVw6pTiXlosKGmictmpifVlY-7Hu0Dvsh6mgI-jxSx-2ZhMfTEUkCE0mwKdnQIp_R8yD6UJ22La2xzhmQ4lSYqqIzv_-s0hTPEz9iS7gcDC7OKapsdn8vL-7fxBBm2lgBCrQVJjHsDfz2I0wIecRjV6uyxa89Cc6vEYnYOYlOkr5D-KrukQ</addsrcrecordid><sourcetype>Open Website</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2188590727</pqid></control><display><type>article</type><title>Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60</title><source>DOAJ Directory of Open Access Journals</source><source>Elektronische Zeitschriftenbibliothek - Frei zugängliche E-Journals</source><source>Royal Society Open Access Journals</source><source>PubMed Central Open Access</source><source>PubMed Central</source><creator>Ewels, Chris ; Rio, Jeremy ; Niwa, Hiroyuki ; Omachi, Haruka ; Shinohara, Hisanori ; Rayson, Mark ; Briddon, Patrick</creator><creatorcontrib>Ewels, Chris ; Rio, Jeremy ; Niwa, Hiroyuki ; Omachi, Haruka ; Shinohara, Hisanori ; Rayson, Mark ; Briddon, Patrick</creatorcontrib><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.</description><identifier>ISSN: 2054-5703</identifier><identifier>EISSN: 2054-5703</identifier><identifier>DOI: 10.1098/rsos.180588</identifier><identifier>PMID: 30839750</identifier><language>eng</language><publisher>The Royal Society</publisher><subject>Addition Pathways ; Chemistry ; Density Functional Calculations ; Gadolinium ; Metallofullerenes</subject><ispartof>Royal Society open science, 2018-09, Vol.5 (9), p.180588-180588</ispartof><rights>2018 The Authors.</rights><rights>2018 The Authors. 2018</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0001-5530-9601 ; 0000-0001-8513-2982</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC6170591/pdf/$$EPDF$$P50$$Gpubmedcentral$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC6170591/$$EHTML$$P50$$Gpubmedcentral$$Hfree_for_read</linktohtml><link.rule.ids>230,314,723,776,780,860,881,2095,27126,27903,27904,53769,53771,55533,55543</link.rule.ids></links><search><creatorcontrib>Ewels, Chris</creatorcontrib><creatorcontrib>Rio, Jeremy</creatorcontrib><creatorcontrib>Niwa, Hiroyuki</creatorcontrib><creatorcontrib>Omachi, Haruka</creatorcontrib><creatorcontrib>Shinohara, Hisanori</creatorcontrib><creatorcontrib>Rayson, Mark</creatorcontrib><creatorcontrib>Briddon, Patrick</creatorcontrib><title>Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60</title><title>Royal Society open science</title><addtitle>R. Soc. open sci</addtitle><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.</description><subject>Addition Pathways</subject><subject>Chemistry</subject><subject>Density Functional Calculations</subject><subject>Gadolinium</subject><subject>Metallofullerenes</subject><issn>2054-5703</issn><issn>2054-5703</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><sourceid>DOA</sourceid><recordid>eNp9kktr3DAQx01paUKaU7-Aj71sOnpZ0qW0bJsHBAJNe-pByNJ4V4ttbSU7ZfPpa8c5ZC8BwYxG__mheRTFRwIXBLT6nHLMF0SBUOpNcUpB8JWQwN6-8E-K85x3AEAEMFnJ98UJA8W0FHBamO84YOpCH_pNab0PQ4h9ubfD9p895NL2vsyDrVssQ44dplw2MZXrS1Y2Y-9msW3Do33Kik2JvY9b9Mm25ZX_uq7gQ_GusW3G82d7Vvy-_PFrfb26vbu6WX-7XXnO-LBySNF7TriyTBMQUiL1FObDqNQMNUgAPquI9Y7W6GilpOYoBNResrPiZuH6aHdmn0Jn08FEG8xTIKaNsWkIrkXjqdA1MuYUdVw6pTiXlosKGmictmpifVlY-7Hu0Dvsh6mgI-jxSx-2ZhMfTEUkCE0mwKdnQIp_R8yD6UJ22La2xzhmQ4lSYqqIzv_-s0hTPEz9iS7gcDC7OKapsdn8vL-7fxBBm2lgBCrQVJjHsDfz2I0wIecRjV6uyxa89Cc6vEYnYOYlOkr5D-KrukQ</recordid><startdate>20180901</startdate><enddate>20180901</enddate><creator>Ewels, Chris</creator><creator>Rio, Jeremy</creator><creator>Niwa, Hiroyuki</creator><creator>Omachi, Haruka</creator><creator>Shinohara, Hisanori</creator><creator>Rayson, Mark</creator><creator>Briddon, Patrick</creator><general>The Royal Society</general><scope>7X8</scope><scope>5PM</scope><scope>DOA</scope><orcidid>https://orcid.org/0000-0001-5530-9601</orcidid><orcidid>https://orcid.org/0000-0001-8513-2982</orcidid></search><sort><creationdate>20180901</creationdate><title>Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60</title><author>Ewels, Chris ; Rio, Jeremy ; Niwa, Hiroyuki ; Omachi, Haruka ; Shinohara, Hisanori ; Rayson, Mark ; Briddon, Patrick</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-d434t-ce2edd4148a3910577e2d20d20d32793e907004e2ed1adc2bec268794e550bd73</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2018</creationdate><topic>Addition Pathways</topic><topic>Chemistry</topic><topic>Density Functional Calculations</topic><topic>Gadolinium</topic><topic>Metallofullerenes</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ewels, Chris</creatorcontrib><creatorcontrib>Rio, Jeremy</creatorcontrib><creatorcontrib>Niwa, Hiroyuki</creatorcontrib><creatorcontrib>Omachi, Haruka</creatorcontrib><creatorcontrib>Shinohara, Hisanori</creatorcontrib><creatorcontrib>Rayson, Mark</creatorcontrib><creatorcontrib>Briddon, Patrick</creatorcontrib><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><collection>DOAJ Directory of Open Access Journals</collection><jtitle>Royal Society open science</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ewels, Chris</au><au>Rio, Jeremy</au><au>Niwa, Hiroyuki</au><au>Omachi, Haruka</au><au>Shinohara, Hisanori</au><au>Rayson, Mark</au><au>Briddon, Patrick</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60</atitle><jtitle>Royal Society open science</jtitle><stitle>R. Soc. open sci</stitle><date>2018-09-01</date><risdate>2018</risdate><volume>5</volume><issue>9</issue><spage>180588</spage><epage>180588</epage><pages>180588-180588</pages><issn>2054-5703</issn><eissn>2054-5703</eissn><abstract>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.</abstract><pub>The Royal Society</pub><pmid>30839750</pmid><doi>10.1098/rsos.180588</doi><tpages>1</tpages><orcidid>https://orcid.org/0000-0001-5530-9601</orcidid><orcidid>https://orcid.org/0000-0001-8513-2982</orcidid><oa>free_for_read</oa></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 2054-5703 |
| ispartof | Royal Society open science, 2018-09, Vol.5 (9), p.180588-180588 |
| issn | 2054-5703 2054-5703 |
| language | eng |
| recordid | cdi_royalsociety_journals_10_1098_rsos_180588 |
| source | DOAJ Directory of Open Access Journals; Elektronische Zeitschriftenbibliothek - Frei zugängliche E-Journals; Royal Society Open Access Journals; PubMed Central Open Access; PubMed Central |
| subjects | Addition Pathways Chemistry Density Functional Calculations Gadolinium Metallofullerenes |
| title | Determining addition pathways and stable isomers for CF3 functionalization of endohedral Gd@C60 |
| url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-01-24T04%3A23%3A53IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_royal&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Determining%20addition%20pathways%20and%20stable%20isomers%20for%20CF3%20functionalization%20of%20endohedral%20Gd@C60&rft.jtitle=Royal%20Society%20open%20science&rft.au=Ewels,%20Chris&rft.date=2018-09-01&rft.volume=5&rft.issue=9&rft.spage=180588&rft.epage=180588&rft.pages=180588-180588&rft.issn=2054-5703&rft.eissn=2054-5703&rft_id=info:doi/10.1098/rsos.180588&rft_dat=%3Cproquest_royal%3E2188590727%3C/proquest_royal%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=2188590727&rft_id=info:pmid/30839750&rft_doaj_id=oai_doaj_org_article_d259be33c82c47c88447a4560f0fc9a8&rfr_iscdi=true |