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Controlled Syntheses of Multi-walled Carbon Nanotubes from Bimetallic Fe–Co Catalyst Supported on Kaolin by Chemical Vapour Deposition Method

  • A. Oyewemi
  • A. S. Abdulkareem
  • J. O. TijaniEmail author
  • M. T. Bankole
  • O. K. Abubakre
  • A. S. Afolabi
  • W. D. Roos
Research Article - Chemical Engineering
  • 4 Downloads

Abstract

Multi-walled carbon nanotubes (MWCNTs) were synthesized via acetylene gas deposition over bimetallic Fe–Co/kaolin catalyst by chemical vapour deposition method. The effects of synthesis parameters such as calcination temperatures, reaction time, argon and acetylene flow rates on the CNTs yield were examined using \(2^{4}\) full factorial experimental design. The as-prepared nanomaterials were characterized by HRSEM/EDS, HRTEM, TGA, DLS, XRD, XPS and BET. The HRSEM/TGA revealed well dispersion of the metallic particles on the kaolin support with high thermal stability. XRD analysis of the catalyst confirmed the formation of mixed oxides of different intensities which can favour the growth of MWCNTs. The optimum conditions to obtain high catalyst yield of 88.9% were: mixing ratio of 1.6, stirring speed 1000 rpm, calcination temperature \(500\,{^{\circ }}\hbox {C}\) and calcination time 14 h. The HRSEM, HRTEM and XRD analyses showed that optimal controlled conditions to obtain homogeneous growth of high-quality graphitic MWCNTs of different inner and outer diameters were: reaction temperature of \(700\,{^{\circ }}\hbox {C}\), growing time 55 min, argon flow rate 220 mL/min and acetylene flow rate 180 mL/min. The BET analysis showed that the surface area of unpurified MWCNTs was \(275.5~\hbox {m}^{2}/\hbox {g}\) while pure MWCNTs increased to \(330.6~\hbox {m}^{2}/\hbox {g}\) after acid treatment. The statistical analysis showed that deposition temperature and acetylene flow rate positively exerted significant influence on the CNTs yield than other synthesis parameters, an evidence of thermodynamic-controlled mechanism. This study demonstrated that kaolin can act as an excellent substrate for MWCNTs growth compared to other commercial supports such as \(\hbox {CaCO}_{3}\), MgO, \(\hbox {Al}_{2}\hbox {O}_{3}\), \(\hbox {SiO}_{2}\).

Keywords

Bimetallic Fe–Co catalyst Kaolin Multi-walled carbon nanotubes Catalytic chemical vapour deposition Factorial design 

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Notes

Acknowledgements

The authors acknowledged the financial support received from Tertiary Education Trust Fund (TETFund), Nigeria, under a grant number TETFUND/FUTMINNA/2014/025 and Centre for Genetic Engineering and Biotechnology (CGEB), Federal University of Technology, Minna, Nigeria, for allowing the students to conduct the experiment and also use the FTIR, Nano zetasizer and BET facilities. The authors are grateful to the following people for their technical assistance: Dr Remy Bucher (XRD, ithemba Labs, South Africa), Dr. Franscious Cummings (HRTEM, Physics Department, University of the Western Cape (UWC), South Africa), Andrian Joseph (HRSEM, Physics department, UWC, South Africa).

Compliance with Ethical Standards

Conflict of interest

The authors declare that they have no conflict of interest.

References

  1. 1.
    Iijima, S.: Helical microtubules of graphitic carbon. Nature 354, 56–58 (1991)CrossRefGoogle Scholar
  2. 2.
    Voelskow, K.; Becker, M.J.; Xia, W.: The influence of kinetics, mass transfer and catalyst deactivation on the growth rate of multi-walled carbon nanotubes from ethene on a cobalt-based catalyst. Chem. Eng. J. 244, 68–74 (2014)CrossRefGoogle Scholar
  3. 3.
    Yang, G.; Han, H.; Li, T.: Synthesis of nitrogen-doped porous graphitic carbons using nano-CaCO\(_{3}\) as template, graphitization catalyst, and activating agent. Carbon. 50, 3753–3765 (2012)CrossRefGoogle Scholar
  4. 4.
    Kumar, K.; Ando, Y.: Chemical vapor deposition of carbon nanotubes. J. Nanosci. Nanotechnol. 10, 3739–3758 (2010)CrossRefGoogle Scholar
  5. 5.
    Allaedini, G.; Tasirin, S.M.; Aminayi, P.: Bulk production of bamboo-shaped multi-walled carbon nanotubes via catalytic decomposition of methane over tri-metallic Ni–Co–Fe catalyst. React. Kinet. Mech. Catal. 116, 385–396 (2015)CrossRefGoogle Scholar
  6. 6.
    Liu, W.; Chai, S.; Mohamed, A.: Synthesis and characterization of graphene and carbon nanotubes: a review on the past and recent developments. J. Ind. Eng. Chem. 20, 1171–1185 (2014)CrossRefGoogle Scholar
  7. 7.
    Kavecký, Š.; Valúchová, J.; Čaplovičová, M.: Nontronites as catalyst for synthesis of carbon nanotubes by catalytic chemical vapor deposition. Appl. Clay Sci. 114, 170–178 (2015)CrossRefGoogle Scholar
  8. 8.
    Allaedini, G.; Aminayi, P.; Tasirin, S.M.: Methane decomposition for carbon nanotube production: optimization of the reaction parameters using response surface methodology. Chem. Eng. Res. Design. 112, 163–174 (2016)CrossRefGoogle Scholar
  9. 9.
    Toussi, S.M.; Razi, F.; Luqman, C.A.: Effect of synthesis condition on the growth of SWCNTs via catalytic chemical vapour deposition. Sains Malays. 3, 197–201 (2011)Google Scholar
  10. 10.
    Magrez, A.; Seo, J.W.; Smajda, R.: Catalytic CVD synthesis of carbon nanotubes: towards high yield and low temperature growth. Materials 3, 4871–4891 (2010)CrossRefGoogle Scholar
  11. 11.
    Duan, X.; Wang, D.; Qian, G.; Walmsley, J.C.; Holmen, A.; Chen, D.; Zhou, X.: Fabrication of K-promoted iron/carbon nanotubes composite catalysts for the Fischer–Tropsch synthesis of lower olefins. J. Energy Chem. 36, 1–7 (2016)Google Scholar
  12. 12.
    Manikandan, D.; Mangalaraja, R.V.; Avila, R.E.; Siddheswaran, R.; Anathakumar, S.: Montmorillonite-carbon nanotube nanofillers by acetylene decomposition using catalytic CVD. Appl. Clay Sci. 71, 37–41 (2013)CrossRefGoogle Scholar
  13. 13.
    Maccallini, E.; Tsoufis, T.; Policicchio, A.: A spectro-microscopic investigation of Fe–Co bimetallic catalysts supported on MgO for the production of thin carbon nanotubes. Carbon 48, 3434–3445 (2010)CrossRefGoogle Scholar
  14. 14.
    Mhlanga, S.D.; Coville, N.J.: Iron–cobalt catalysts synthesized by a reverse micelle impregnation method for controlled growth of carbon nanotubes. Diam. Relat Mater. 17, 1489–1493 (2008)CrossRefGoogle Scholar
  15. 15.
    Mhlanga, S.D.; Mondal, K.C.; Carter, R.: The effect of synthesis parameters on the catalytic synthesis of multi-walled carbon nanotubes using Fe–CoCaCO\(_{3}\) catalysts. S Afr. J. Chem. 62, 67–76 (2009)Google Scholar
  16. 16.
    Afolabi, A.S.; Abdulkareem, A.S.; Mhlanga, S.D.: Synthesis and purification of bimetallic catalysed carbon nanotubes in a horizontal CVD reactor. J Exp. Nanosci. 6(3), 248–262 (2011)CrossRefGoogle Scholar
  17. 17.
    Bahgat, M.; Farghali, A.A.; El Rouby, W.M.A.: Synthesis and modification of multi-walled carbon nanotubes (MWCNTs) for water treatment applications. J. Anal. Appl. Pyrolysis 92, 307–313 (2011)CrossRefGoogle Scholar
  18. 18.
    Shokry, S.A.; El Morsi, A.K.; Sabaa, M.S.: Study of the productivity of MWCNT over Fe and Fe–Co catalysts supported on SiO\(_{2}\), Al\(_{2}\)O\(_{3}\) and MgO. Egypt. J. Petrol. 23, 183–189 (2014)CrossRefGoogle Scholar
  19. 19.
    Aliyu, A.; Abdulkareem, A.S.; Kovo, A.S.; Abubakre, O.K.; Tijani, J.O.; Kariim, I.: Synthesize multi-walled carbon nanotubes via catalytic chemical vapour deposition method on Fe–Ni bimetallic catalyst supported on kaolin. Carbon Lett. 21, 33–50 (2017)CrossRefGoogle Scholar
  20. 20.
    Cheng, J.; Zhang, X.; Luo, Z.: Carbon nanotube synthesis and parametric study using CaCO\(_{3}\) nanocrystals as catalyst support by CVD. Mater. Chem. Phys. 95, 5–11 (2006)CrossRefGoogle Scholar
  21. 21.
    Motchelaho, M.A.M.; Xiong, H.; Moyo, M.: Effect of acid treatment on the surface of multiwalled carbon nanotubes prepared from Fe–Co supported on CaCO\(_{3}\): correlation with Fischer–Tropsch catalyst activity. J. Mol. Catal. A: Chem. 335, 189–198 (2011)CrossRefGoogle Scholar
  22. 22.
    Aroke, U.O.; El-Nafaty, U.A.; Osha, O.A.: Properties and characterization of Kaolin Clay from Alkaleri, North-Eastern Nigeria. Int. J. Emerg. Technol. Adv. Eng. 3, 387–392 (2013)Google Scholar
  23. 23.
    Hassan, U.J.; Abdu, S.G.: Structural analysis and surface morphology of kaolin. Sci. World J. 9(3), 33–37 (2014)Google Scholar
  24. 24.
    Osabor, V.N.; Okafor, P.C.; Ibe, K.A.: Characterization of clays in Odukpani, South Eastern Nigeria. Afr. J. Pure Appl. Chem. 3, 079–085 (2009)Google Scholar
  25. 25.
    Khorrami, S.A.; Manuchehri, Q.S.: Magnetic properties of cobalt synthesized by hydrothermal and co-precipitation methods: a comparative study. Int. J. Chem. Eng. 10, 1155–1160 (2013)Google Scholar
  26. 26.
    Couteau, E.; Hernadi, K.; Seo, J.W.: CVD synthesis of high-purity multi-walled carbon nanotubes using CaCO\(_{3}\) catalyst support for large-scale production. Chem. Phys. Lett. 378, 9–17 (2003)CrossRefGoogle Scholar
  27. 27.
    Chiwaye, N.; Jewell, L.L.; Billing, B.G.; Naidoo, D.; Ncube, M.; Coville, N.J.: In situ powder XRD and Mössbauer study of Fe–Co supported on CaCO\(_{3}\). Mater. Res. Bull. 56, 98–106 (2014)CrossRefGoogle Scholar
  28. 28.
    Kathyayini, H.; Vijayakumar Reddy, K.; Nagy, J.B.: Synthesis of carbon nanotubes over transition metal ion supported on Al(OH)\(_{3,}\). Indian J. Chem. 47A, 663–668 (2008)Google Scholar
  29. 29.
    Ratković, S.; Kiss, E.; Bošković, G.: Synthesis of high-purity carbon nanotubes over alumina and silica supported bimetallic catalysts. Chem. Ind. Chem. Eng. Q. 15, 263–270 (2009)CrossRefGoogle Scholar
  30. 30.
    Welch, M.: Advanced synthesis of carbon nanotubes. Catalysis 18, 353 (2011)Google Scholar
  31. 31.
    Pełech, I.; Narkiewicz, U.; Kaczmarek, A.; Jędrzejewska, A.: Preparation and characterization of multi-walled carbon nanotubes grown on transition metal catalysts. Pol. J. Chem. Technol. 16, 117–122 (2014)Google Scholar
  32. 32.
    Angulakshmi, V.S.; Karthikeyan, S.; Syed Shabudeen, P.S.: Effect of synthesis temperature on the growth of multi-walled carbon nanotubes from Zea mays oil as evidenced by structural, raman and XRD analyses. Rasayan J. Chem. 8, 1–7 (2015)Google Scholar
  33. 33.
    Abdulkareem, A.S.; Afolabi, A.S.; Iyuke, S.E.; Piennar, C.H.Z.: Synthesis of carbon nanotubes by swirled floating catalyst chemical vapour deposition method. J. Nanosci. Nanotechnol. 7, 1–6 (2007)CrossRefGoogle Scholar
  34. 34.
    Mohammed, I.A.; Bankole, M.T.; Abdulkareem, A.S.; Ochigbo, S.S.; Afolabi, A.S.; Abubakre, O.K.: Full factorial design approach to carbon nanotubes synthesis by CVD method in argon environment. S Afr. J. Chem. Eng. 24, 17–42 (2017)Google Scholar
  35. 35.
    Yardimci, A.I.; Yılmaz, S.; Selamet, Y.: The effects of catalyst pretreatment, growth atmosphere and temperature on carbon nanotube synthesis using Co–Mo/MgO catalyst. Diam. Relat. Mater. 60, 81–86 (2015)CrossRefGoogle Scholar

Copyright information

© King Fahd University of Petroleum & Minerals 2019

Authors and Affiliations

  • A. Oyewemi
    • 1
  • A. S. Abdulkareem
    • 1
    • 6
  • J. O. Tijani
    • 3
    • 6
    Email author
  • M. T. Bankole
    • 3
    • 6
  • O. K. Abubakre
    • 2
    • 6
  • A. S. Afolabi
    • 4
  • W. D. Roos
    • 5
  1. 1.Department of Chemical EngineeringFederal University of Technology MinnaMinnaNigeria
  2. 2.Department of Mechanical EngineeringFederal University of Technology MinnaMinnaNigeria
  3. 3.Department of ChemistryFederal University of Technology MinnaMinnaNigeria
  4. 4.Department of Chemical, Materials and Metallurgical EngineeringBotswana International University of Science and Technology (BIUST)PalapyeBotswana
  5. 5.Department of PhysicsUniversity of the Free StateBloemfonteinRepublic of South Africa
  6. 6.Nanotechnology Research Group, Centre for Genetic Engineering and BiotechnologyFederal University of Technology MinnaMinnaNigeria

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