RESEARCH ARTICLE

 

The synthesis of nitrogen-doped multiwalled carbon nanotubes using an Fe-Co/CaCO₃ catalyst

 

 

Z.N. Tetana^I; S.D. Mhlanga^I; G. Bepete^I; R.W.M. Krause^II; N.J. Coville^{I, *}

^IDST/NRF Centre of Excellence in Strong Materials and the Molecular Sciences Institute, School of Chemistry, University of the Witwatersrand, Johannesburg, WITS, 2050, South Africa
^IIDST/NRF Centre of Excellence in Strong Materials, Department of Chemical Technology, University of Johannesburg, P.O. Box 17011, Doornfontein, 2028, South Africa

 

 

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ABSTRACT

A CVD method was used to prepare high-quality nitrogen-doped multiwalled carbon nanotubes (N-MWCNTs) using acetonitrile as the nitrogen and carbon source and acetylene as a carbon source over an Fe-Co/CaCO₃ catalyst in the temperature range 700-850 °C. This represents a continuation of earlier work in which Fe-Co on CaCO₃ was used to make undoped carbon nanotubes. The effect of synthesis parameters (growth temperature and CH₃CN vaporization temperature) on the yield, size, quality, morphology and thermal stability of the N-MWCNTs was studied. The resulting materials were characterized by TEM, SEM, TGA, BET, XPS, CN elemental analysis and Raman spectroscopy. TEM analysis revealed that the nanotubes exhibit bamboo-like structures with rough surfaces and a relatively uniform diameter. The bamboo compartment distance decreased with increase in synthesis temperature due to the increased nitrogen content in N-MWCNTs. The SEM examination showed that at high synthesis temperatures carbon spheres (CSs) with chain-like morphology and large sizes were also formed along with the N-MWCNTs. The XPS and CN elemental analysis revealed that nitrogen atoms were successfully doped into the carbon walls. The amount of nitrogen incorporated in the N-MWCNTs varied with increasing growth time and CH₃CN vaporization temperature.

Keywords: Carbon nanotubes, CVD synthesis, nitrogen doping, acetonitrile, Fe-Co/CaCO₃ catalyst

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Full text available only in PDF format.

 

Acknowledgements

The authors would like to thank the National Research Foundation, DST/NRF Centre of Excellence in Strong Materials, CSIR and the University of the Witwatersrand for financial support. We gratefully acknowledge the Department of Physics and Astronomy at Rutgers University, USA, for XPS assistance and M.F. Philpott from the ARC- Institute for Soil, Climate and Water, for C and N elemental analysis. We also thank R.M. Erasmus for his assistance with Raman spectroscopy analysis. The technical support given by the University of the Witwatersrand Microscopy and Microanalysis Unit is also appreciated (special thanks are due to M.J. Witcomb, A. Ziegler and the late A.R. Seema).

 

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Received 11 August 2011
Revised 12 December 2011
Accepted 30 January 2012

 

 

Submitted by invitation to celebrate 2011 the 'International Year of Chemistry'.
* To whom correspondence should be addressed. E-mail: neil.coville@wits.ac.za