Structure-Dependent Thermal Defunctionalization of Single-Walled Carbon Nanotubes

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dc.citation.journalTitleACS Nano
dc.contributor.authorGhosh, Saunab
dc.contributor.authorWei, Fang
dc.contributor.authorBachilo, Sergei M.
dc.contributor.authorHauge, Robert H.
dc.contributor.authorBillups, W.E.
dc.contributor.authorWeisman, R. Bruce
dc.contributor.orgSmalley Institute for Nanoscale Science and Technology
dc.date.accessioned2015-06-15T18:57:50Z
dc.date.available2015-06-15T18:57:50Z
dc.date.issued2015
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.
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.
dc.identifier.doihttp://dx.doi.org/10.1021/acsnano.5b01846
dc.identifier.urihttps://hdl.handle.net/1911/80760
dc.language.isoeng
dc.publisherAmerican Chemical Society
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.
dc.subject.keywordcovalent functionalization
dc.subject.keywordpyrolysis
dc.subject.keyworddodecylation
dc.subject.keywordD/G ratio
dc.subject.keywordnanotube fluorescence restoration
dc.titleStructure-Dependent Thermal Defunctionalization of Single-Walled Carbon Nanotubes
dc.typeJournal article
dc.type.dcmiText
dc.type.publicationpost-print
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