Abstract

Multi-walled carbon nanotubes (MWCNTs) were grown by plasma-enhanced chemical vapor deposition (PECVD) in a bell jar reactor. A mixture of methane and hydrogen (CH4/H2) was decomposed over Ni catalyst previously deposited on Si-wafer by thermionic vacuum arc (TVA) technology. The growth parameters were optimized to obtain dense arrays of nanotubes and were found to be: hydrogen flow rate of 90 sccm; methane flow rate of 10 sccm; oxygen flow rate of 1 sccm; substrate temperature of 1123 K; total pressure of 10 mbar and microwave power of 342 Watt. Results are summarized and significant main factors and their interactions were identified. In addition a computational study of nanotubes growth rate was conducted using a gas phase reaction mechanism and surface nanotube formation model. Simulations were performed to determine the gas phase fields for temperature and species concentration as well as the surface-species coverage and carbon nanotubes growth rate. A kinetic mechanism which consists of 13 gas species, 43 gas reactions and 17 surface reactions has been used in the commercial computational fluid dynamics (CFD) software ANSYS Fluent. A comparison of simulated and experimental growth rate is presented in this paper. Simulation results agreed favorably with experimental data.

Highlights

  • Since their discovery by Iijima in 1991 [1], carbon nanotubes have generated much interest due to their quasi one-dimensional structure and their unique combinations of electronic, field emission, mechanical and chemical properties coupled with the new ability to grow them aligned on a substrate

  • For microwave plasma-enhanced chemical vapor deposition (PECVD) nanotube synthesis we developed an experimental protocol composed by three steps: 1) thermal annealing of Ni/Si substrates, 2) hydrogenation of Ni catalyst, 3) nanotube growth

  • Atomic force microscopy (AFM) of the as produced by thermionic vacuum arc (TVA) Ni/Si substrates and annealed at 850 ̊C during 20 minutes hydrogenated with pure hydrogen plasma during 10 minutes was carried out to determine the surface morphology

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Summary

Introduction

Since their discovery by Iijima in 1991 [1], carbon nanotubes have generated much interest due to their quasi one-dimensional structure and their unique combinations of electronic, field emission, mechanical and chemical properties coupled with the new ability to grow them aligned on a substrate. This opened unlimited possibilities of applications such as field emitters, sensors, high-density energy storage devices, photonic crystals, active media for lasers, non-linear optical media etc. The addition of a controlled amount of a weak oxidizer as oxygen or water into the growth ambient of CVD was reported to significantly enhance the activity and lifetime of the catalyst resulting in efficient nanotubes growth [6] [7]

Experimental
Modeling Approach
Geometry and Assumptions
Gas-Phase Chemistry
Surface Chemistry
Initial and Boundary Conditions
Computational Procedure
Experimental Results
Modeling Results
Conclusions
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