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Article . 2021 . Peer-reviewed
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The Journal of Physical Chemistry C
Article . 2016 . Peer-reviewed
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https://dx.doi.org/10.48550/ar...
Article . 2016
License: arXiv Non-Exclusive Distribution
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Article . 2016
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Disentangling Vacancy Oxidation on Metallicity-Sorted Carbon Nanotubes

Authors: Mowbray, Duncan J.; Paz, Alejandro Pérez; Ruiz-Soria, Georgina; Sauer, Markus; Lacovig, Paolo; Dalmiglio, Matteo; Lizzit, Silvano; +5 Authors

Disentangling Vacancy Oxidation on Metallicity-Sorted Carbon Nanotubes

Abstract

Pristine single-walled carbon nanotubes (SWCNTs) are rather inert to O$_2$ and N$_2$, which for low doses chemisorb only on defect sites or vacancies of the SWCNTs at the ppm level. However, very low doping has a major effect on the electronic properties and conductivity of the SWCNTs. Already at low O$_2$ doses (80 L), the X-ray photoelectron spectroscopy (XPS) O 1s signal becomes saturated, indicating nearly all the SWCNT's vacancies have been oxidized. As a result, probing vacancy oxidation on SWCNTs via XPS yields spectra with rather low signal-to-noise ratios, even for metallicity-sorted SWCNTs. We show that, even under these conditions, the first principles density functional theory calculated Kohn-Sham O 1s binding energies may be used to assign the XPS O 1s spectra for oxidized vacancies on SWCNTs into its individual components. This allows one to determine the specific functional groups or bonding environments measured. We find the XPS O 1s signal is mostly due to three O-containing functional groups on SWCNT vacancies: epoxy (C$_2$$>$O), carbonyl (C$_2$$>$C$=$O), and ketene (C$=$C$=$O), as ordered by abundance. Upon oxidation of nearly all the SWCNT's vacancies, the central peak's intensity for the metallic SWCNT sample is 60\% greater than for the semiconducting SWCNT sample. This suggests a greater abundance of O-containing defect structures on the metallic SWCNT sample. For both metallic and semiconducting SWCNTs, we find O$_2$ does not contribute to the measured XPS O~1s spectra.

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Austria, Spain
Keywords

Condensed Matter - Materials Science, ADSORPTION, Condensed Matter - Mesoscale and Nanoscale Physics, 103018 Materialphysik, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences, DISSOCIATION, OXYGEN, ELECTRONIC-PROPERTIES, SYSTEMS, DENSITY, Mesoscale and Nanoscale Physics (cond-mat.mes-hall), GRAPHENE OXIDE, FUNCTIONALIZATION, SENSITIVITY, 103018 Materials physics

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selected citations
These citations are derived from selected sources.
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
views
OpenAIRE UsageCountsViews provided by UsageCounts
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