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Naji, M. |
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Motta, Antonella |
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Taccardi, Nicola |
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Petrov, R. H. | Madrid |
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Kočí, Jan | Prague |
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Ali, M. A. |
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Rančić, M. |
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Ollier, Nadège |
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Azevedo, Nuno Monteiro |
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Gaulding, E. Ashley
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article
Effect of hydrogen on catalyst nanoparticles in carbon nanotube growth
Abstract
<p>The structures of carbon nanotubes grown from catalytic nanoparticles via plasma-enhanced chemical vapor deposition in CH<sub>4</sub> / H<sub>2</sub> mixtures show a strong dependence on the H<sub>2</sub> -to- CH<sub>4</sub> ratio in the feed gas. A suite of characterization techniques, including optical emission, infrared, and Raman spectroscopies combined with convergent-beam and selected-area electron diffraction, and high-resolution (scanning) transmission electron microscopy imaging were used to systematically investigate the interrelation among plasma gas phase composition, catalysts morphology, catalyst structure, and carbon nanotube structure. Hydrogen plays a critical role in determining the final carbon nanotube structure through its effect on the catalyst crystal structure and morphology. At low H<sub>2</sub> -to- CH <sub>4</sub> ratios (∼1), iron catalyst nanoparticles are converted to Fe<sub>3</sub> C and well-graphitized nanotubes grow from elongated Fe <sub>3</sub> C crystals. High (>5) H<sub>2</sub> -to- CH<sub>4</sub> ratios in the feed gas result in high hydrogen concentrations in the plasma and strongly reducing conditions, which prevents conversion of Fe to Fe<sub>3</sub> C. In the latter case, poorly-graphitized nanofibers grow from ductile bcc iron nanocrystals that are easily deformed into tapered nanocrystals that yield nanotubes with thick walls.</p>