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Metal-Catalyst-Free Access to Multiwall Carbon Nanotubes/Silica Nanocomposites (MWCNT/SiO2) from a Single-Source Precursor

Mera, Gabriela and Kroll, Peter and Ponomarev, Ilia and Chen, Jiewei and Morita, Koji and Liesegang, Moritz and Ionescu, Emanuel and Navrotsky, Alexandra (2019):
Metal-Catalyst-Free Access to Multiwall Carbon Nanotubes/Silica Nanocomposites (MWCNT/SiO2) from a Single-Source Precursor.
In: Dalton Transactions, Royal Society of Chemistry, pp. 11018-11033, 48, (29), ISSN 1477-9226,
DOI: 10.1039/C9DT01783F,
[Online-Edition: https://pubs.rsc.org/en/content/articlelanding/2019/dt/c9dt0...],
[Article]

Abstract

The present study introduces a facile single-source precursor preparative access to bamboo-like multiwalled carbon nanotubes (MWCNTs) highly dispersed within a mesoporous silica-rich matrix. The metal-free single-source precursor was synthesized via a one-pot sol-gel process using tetramethyl orthosilicate (TMOS) and 4,4′-dihydroxybiphenyl (DHBP) and converted subsequently via pyrolysis in argon atmosphere into MWCNT/silica nanocomposites. The in-situ segregation of the highly defective bamboo-like MWCNTs was carefully investigated and has been shown to occur within the mesopores of the silica-rich matrix at relatively low temperatures and without the use of a metal catalyst. The experimental results have been supported by extensive computational simulations, which correlate the molecular architecture of the single-source precursor with the structural features of the carbon phase segregating from the silica matrix. Furthermore, the role of hydrogen on the stability of the prepared nanocomposites as well as on the high-temperature evolution and morphology of the segregated MWCNTs has been discussed based on vibrational spectroscopy, calorimetric studies and empirical potential calculations. The results attained within the present study may allow for designing highly-defined nanocarbon-containing composites with tailored structural features and property profiles.

Item Type: Article
Erschienen: 2019
Creators: Mera, Gabriela and Kroll, Peter and Ponomarev, Ilia and Chen, Jiewei and Morita, Koji and Liesegang, Moritz and Ionescu, Emanuel and Navrotsky, Alexandra
Title: Metal-Catalyst-Free Access to Multiwall Carbon Nanotubes/Silica Nanocomposites (MWCNT/SiO2) from a Single-Source Precursor
Language: English
Abstract:

The present study introduces a facile single-source precursor preparative access to bamboo-like multiwalled carbon nanotubes (MWCNTs) highly dispersed within a mesoporous silica-rich matrix. The metal-free single-source precursor was synthesized via a one-pot sol-gel process using tetramethyl orthosilicate (TMOS) and 4,4′-dihydroxybiphenyl (DHBP) and converted subsequently via pyrolysis in argon atmosphere into MWCNT/silica nanocomposites. The in-situ segregation of the highly defective bamboo-like MWCNTs was carefully investigated and has been shown to occur within the mesopores of the silica-rich matrix at relatively low temperatures and without the use of a metal catalyst. The experimental results have been supported by extensive computational simulations, which correlate the molecular architecture of the single-source precursor with the structural features of the carbon phase segregating from the silica matrix. Furthermore, the role of hydrogen on the stability of the prepared nanocomposites as well as on the high-temperature evolution and morphology of the segregated MWCNTs has been discussed based on vibrational spectroscopy, calorimetric studies and empirical potential calculations. The results attained within the present study may allow for designing highly-defined nanocarbon-containing composites with tailored structural features and property profiles.

Journal or Publication Title: Dalton Transactions
Volume: 48
Number: 29
Publisher: Royal Society of Chemistry
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Dispersive Solids
Date Deposited: 25 Jul 2019 05:30
DOI: 10.1039/C9DT01783F
Official URL: https://pubs.rsc.org/en/content/articlelanding/2019/dt/c9dt0...
Projects: Deutsche Forschungs Gemeinschaft, Grant IO 83/2-1, National Science Foundation (NSF), CMMI-1634448, National Science Foundation (NSF) through award CMMI-1634448, Deutsche Forschungs Gemeinschaft, Grant IO 64/14-1, A.P. Sloan Foundation Deep Carbon Observatory
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