Structure-Dependent Thermal Defunctionalization of Single-Walled Carbon Nanotubes

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dc.citation.journalTitleACS Nanoen_US
dc.contributor.authorGhosh, Saunaben_US
dc.contributor.authorWei, Fangen_US
dc.contributor.authorBachilo, Sergei M.en_US
dc.contributor.authorHauge, Robert H.en_US
dc.contributor.authorBillups, W.E.en_US
dc.contributor.authorWeisman, R. Bruceen_US
dc.contributor.orgSmalley Institute for Nanoscale Science and Technologyen_US
dc.date.accessioned2015-06-15T18:57:50Zen_US
dc.date.available2015-06-15T18:57:50Zen_US
dc.date.issued2015en_US
dc.description.abstractCovalent sidewall functionalization of single-walled carbon nanotubes (SWCNTs) is an important tool for tailoring their properties for research purposes and applications. In this study, SWCNT samples were first functionalized by reductive alkylation using metallic lithium and 1-iodododecane in liquid ammonia. Samples of the alkyl-functionalized SWCNTs were then pyrolyzed under an inert atmosphere at selected temperatures between 100 and 500 °C to remove the addends. The extent of defunctionalization was assessed using a combination of thermogravimetric analysis, Raman measurements of the D, G, and radial breathing bands, absorption spectroscopy of the first- and second-order van Hove peaks, and near-IR fluorescence spectroscopy of (n,m)-specific emission bands. These measurements all indicate a substantial dependence of defunctionalization rate on nanotube diameter, with larger diameter nanotubes showing more facile loss of addends. The effective activation energy for defunctionalization is estimated to be a factor of ∼1.44 greater for 0.76 nm diameter nanotubes as compared to those with 1.24 nm diameter. The experimental findings also reveal the quantitative variation with functionalization density of the Raman D/G intensity ratio and the relative near-IR fluorescence intensity. Pyrolyzed samples show spectroscopic properties that are equivalent to those of SWCNTs prior to functionalization. The strong structure dependence of the defunctionalization rate suggests an approach for scalable diameter sorting of mixed SWCNT samples.en_US
dc.identifier.citationGhosh, Saunab, Wei, Fang, Bachilo, Sergei M., et al.. "Structure-Dependent Thermal Defunctionalization of Single-Walled Carbon Nanotubes." <i>ACS Nano,</i> (2015) American Chemical Society: http://dx.doi.org/10.1021/acsnano.5b01846.en_US
dc.identifier.doihttp://dx.doi.org/10.1021/acsnano.5b01846en_US
dc.identifier.urihttps://hdl.handle.net/1911/80760en_US
dc.language.isoengen_US
dc.publisherAmerican Chemical Societyen_US
dc.rightsThis is an author's peer-reviewed final manuscript, as accepted by the publisher. The published article is copyrighted by the American Chemical Society.en_US
dc.subject.keywordcovalent functionalizationen_US
dc.subject.keywordpyrolysisen_US
dc.subject.keyworddodecylationen_US
dc.subject.keywordD/G ratioen_US
dc.subject.keywordnanotube fluorescence restorationen_US
dc.titleStructure-Dependent Thermal Defunctionalization of Single-Walled Carbon Nanotubesen_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpost-printen_US
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