In situ polyphenyl derivatisation and the effect of thermal decomposition of adsorbed and chemisorbed polyphenyls on the structure of multi-wall carbon nanotubes

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Abstract

This study presents the exploitation of an alternative reaction route of deamination of arylamines to perform in situ derivatisation of multi-walled carbon nanotubes (MWCNTs) with polyphenyl (PPh) species of various masses. As a result of consecutive derivatisation, high conversion of PPh grafting of the MWCNTs was realised with the collateral outgrowth of physical modification with adsorbed additional PPhs. Applied derivatisation process exceeds the monolayer coverage related superficial saturation limitations in the overall grafting yield of the nanotubes. Thus, a linear relationship was recognized between the overall quantities of chemisorbed PPhs composed of D5-phenylene oligomers and the applied excess of diazonium activated reagents, corresponding to 2H MAS NMR spectroscopy results. According to mass spectrometry (MS) investigations, uniform thermal decomposition of the chemisorbed PPhs modified MWCNTs was found besides the more intense and altered decomposition characteristic-featured adsorbate-chemisorbate PPhs contained MWCNTs during sequential pyrolysis under inert atmosphere. This is attributed to the pyrolysis provoked isomerisation, decomposition and the formation of adsorbed and chemisorbed PPh moieties. As a result, a mediated and an even more pronounced degradation in the order of graphitic lattice of the MWCNTs were evidenced in the adsorbate-chemisorbate and the chemisorbate PPhs contained samples by FT-Raman spectroscopy and transmission electron microscopy (TEM), respectively. 2H MAS NMR supplied results of relevant amount of deuterium in the chemisorbate PPh contained sample without traces of aromatic related MS detected volatile products, these allow us to conclude about a thermally stable derivatisation that is interpreted as an endohedral modification of the nanotubes.

Original languageEnglish
Pages (from-to)6212-6219
Number of pages8
JournalApplied Surface Science
Volume257
Issue number14
DOIs
Publication statusPublished - May 1 2011

Fingerprint

Carbon Nanotubes
Carbon nanotubes
Pyrolysis
Adsorbates
Nanotubes
Mass spectrometry
Decomposition
Deuterium
Isomerization
Oligomers
Nuclear magnetic resonance spectroscopy
Raman spectroscopy
Monolayers
Nuclear magnetic resonance
Transmission electron microscopy
Degradation

Keywords

  • MWCNTs
  • Polyphenyls
  • Sequential derivatisation
  • Thermal decomposition

ASJC Scopus subject areas

  • Surfaces, Coatings and Films

Cite this

@article{8e4aa61f651d4881b1664a0718373e75,
title = "In situ polyphenyl derivatisation and the effect of thermal decomposition of adsorbed and chemisorbed polyphenyls on the structure of multi-wall carbon nanotubes",
abstract = "This study presents the exploitation of an alternative reaction route of deamination of arylamines to perform in situ derivatisation of multi-walled carbon nanotubes (MWCNTs) with polyphenyl (PPh) species of various masses. As a result of consecutive derivatisation, high conversion of PPh grafting of the MWCNTs was realised with the collateral outgrowth of physical modification with adsorbed additional PPhs. Applied derivatisation process exceeds the monolayer coverage related superficial saturation limitations in the overall grafting yield of the nanotubes. Thus, a linear relationship was recognized between the overall quantities of chemisorbed PPhs composed of D5-phenylene oligomers and the applied excess of diazonium activated reagents, corresponding to 2H MAS NMR spectroscopy results. According to mass spectrometry (MS) investigations, uniform thermal decomposition of the chemisorbed PPhs modified MWCNTs was found besides the more intense and altered decomposition characteristic-featured adsorbate-chemisorbate PPhs contained MWCNTs during sequential pyrolysis under inert atmosphere. This is attributed to the pyrolysis provoked isomerisation, decomposition and the formation of adsorbed and chemisorbed PPh moieties. As a result, a mediated and an even more pronounced degradation in the order of graphitic lattice of the MWCNTs were evidenced in the adsorbate-chemisorbate and the chemisorbate PPhs contained samples by FT-Raman spectroscopy and transmission electron microscopy (TEM), respectively. 2H MAS NMR supplied results of relevant amount of deuterium in the chemisorbate PPh contained sample without traces of aromatic related MS detected volatile products, these allow us to conclude about a thermally stable derivatisation that is interpreted as an endohedral modification of the nanotubes.",
keywords = "MWCNTs, Polyphenyls, Sequential derivatisation, Thermal decomposition",
author = "Andr{\'a}s Gergely and K{\'a}lm{\'a}n {\'U}jsz{\'a}szy and Csaba Peltz and P{\'e}ter Kir{\'a}ly and G{\'a}bor T{\'a}rk{\'a}nyi and Judith Mih{\'a}ly and Erika K{\'a}lm{\'a}n",
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language = "English",
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T1 - In situ polyphenyl derivatisation and the effect of thermal decomposition of adsorbed and chemisorbed polyphenyls on the structure of multi-wall carbon nanotubes

AU - Gergely, András

AU - Újszászy, Kálmán

AU - Peltz, Csaba

AU - Király, Péter

AU - Tárkányi, Gábor

AU - Mihály, Judith

AU - Kálmán, Erika

PY - 2011/5/1

Y1 - 2011/5/1

N2 - This study presents the exploitation of an alternative reaction route of deamination of arylamines to perform in situ derivatisation of multi-walled carbon nanotubes (MWCNTs) with polyphenyl (PPh) species of various masses. As a result of consecutive derivatisation, high conversion of PPh grafting of the MWCNTs was realised with the collateral outgrowth of physical modification with adsorbed additional PPhs. Applied derivatisation process exceeds the monolayer coverage related superficial saturation limitations in the overall grafting yield of the nanotubes. Thus, a linear relationship was recognized between the overall quantities of chemisorbed PPhs composed of D5-phenylene oligomers and the applied excess of diazonium activated reagents, corresponding to 2H MAS NMR spectroscopy results. According to mass spectrometry (MS) investigations, uniform thermal decomposition of the chemisorbed PPhs modified MWCNTs was found besides the more intense and altered decomposition characteristic-featured adsorbate-chemisorbate PPhs contained MWCNTs during sequential pyrolysis under inert atmosphere. This is attributed to the pyrolysis provoked isomerisation, decomposition and the formation of adsorbed and chemisorbed PPh moieties. As a result, a mediated and an even more pronounced degradation in the order of graphitic lattice of the MWCNTs were evidenced in the adsorbate-chemisorbate and the chemisorbate PPhs contained samples by FT-Raman spectroscopy and transmission electron microscopy (TEM), respectively. 2H MAS NMR supplied results of relevant amount of deuterium in the chemisorbate PPh contained sample without traces of aromatic related MS detected volatile products, these allow us to conclude about a thermally stable derivatisation that is interpreted as an endohedral modification of the nanotubes.

AB - This study presents the exploitation of an alternative reaction route of deamination of arylamines to perform in situ derivatisation of multi-walled carbon nanotubes (MWCNTs) with polyphenyl (PPh) species of various masses. As a result of consecutive derivatisation, high conversion of PPh grafting of the MWCNTs was realised with the collateral outgrowth of physical modification with adsorbed additional PPhs. Applied derivatisation process exceeds the monolayer coverage related superficial saturation limitations in the overall grafting yield of the nanotubes. Thus, a linear relationship was recognized between the overall quantities of chemisorbed PPhs composed of D5-phenylene oligomers and the applied excess of diazonium activated reagents, corresponding to 2H MAS NMR spectroscopy results. According to mass spectrometry (MS) investigations, uniform thermal decomposition of the chemisorbed PPhs modified MWCNTs was found besides the more intense and altered decomposition characteristic-featured adsorbate-chemisorbate PPhs contained MWCNTs during sequential pyrolysis under inert atmosphere. This is attributed to the pyrolysis provoked isomerisation, decomposition and the formation of adsorbed and chemisorbed PPh moieties. As a result, a mediated and an even more pronounced degradation in the order of graphitic lattice of the MWCNTs were evidenced in the adsorbate-chemisorbate and the chemisorbate PPhs contained samples by FT-Raman spectroscopy and transmission electron microscopy (TEM), respectively. 2H MAS NMR supplied results of relevant amount of deuterium in the chemisorbate PPh contained sample without traces of aromatic related MS detected volatile products, these allow us to conclude about a thermally stable derivatisation that is interpreted as an endohedral modification of the nanotubes.

KW - MWCNTs

KW - Polyphenyls

KW - Sequential derivatisation

KW - Thermal decomposition

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U2 - 10.1016/j.apsusc.2011.02.040

DO - 10.1016/j.apsusc.2011.02.040

M3 - Article

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JO - Applied Surface Science

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SN - 0169-4332

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