4.6 Article

Radial growth kinetics of epitaxial pyrolytic carbon layers deposited on carbon nanotube surfaces by non-catalytic pyrolysis

Journal

DIAMOND AND RELATED MATERIALS
Volume 123, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.diamond.2022.108857

Keywords

Carbon nanotube; Chemical vapor deposition; Vapor growth

Funding

  1. JSPS KAKENHI [JP19K14837 andJP21K14489, JP19K14837]
  2. [JP21K14489]

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This study discusses the growth mechanism of epitaxial PyC layers on CNT surfaces achieved by low-pressure ethylene pyrolysis, distinct from previous studies using higher gas pressures. The average thickness of deposited PyC layers is calculated by analyzing TEM images, and the crystallinity is evaluated by Raman spectroscopy and X-ray diffraction. A two-stage nonlinear behavior in the growth kinetics of PyC layers is found, indicating the influence of surface active sites on the radial growth rate.
Chemical vapor deposition of pyrolytic carbon (PyC) onto carbon nanotube (CNT) surfaces by hydrocarbon pyrolysis can thicken the nanotube diameter until the desirable size. Vapor-induced thickening of CNTs may require no metal catalysts because the CNT-templated growth can easily convert PyC deposits into epitaxial graphene shells. However, little work has been done on the kinetics of the vapor-induced CNT thickening process during the non-catalytic pyrolysis. In this study, we discuss the growth mechanism of epitaxial PyC layers on CNT surfaces achieved by the low-pressure (<= 1.5 kPa) pyrolysis of ethylene, which is distinct from previous studies using much higher gas pressures (4-100 kPa) for the PyC deposition. The average thickness of deposited PyC layers is calculated by analyzing the transmission electron microscopy images of PyC-coated CNTs. The crystallinity of PyC-coated CNTs is evaluated by Raman spectroscopy and X-ray diffraction. The thickness of PyC layers on CNT surfaces can be adjusted by simply changing the growth time under typical pyrolysis parameters (800 degrees C-1.5 kPa of ethylene). We find a two-stage nonlinear behavior to describe the growth kinetics of PyC layers, indicating that the radial growth rate of PyC layers can be influenced by the number of surface active sites. This study reveals the self-assembly mechanism of graphitic layers on the CNT template, which is expected to promote the diameter-controlled synthesis of CNTs.

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