Growth of novel carbon phases by methane infiltration of free-standing single-walled carbon nanotube films

High-temperature methane infiltration of thin, free-standing films of acid-treated single-walled carbon nanotubes (SWCNT) has been studied by means of scanning electron microscopy, transmission electron microscopy and Raman spectroscopy. In the early stages of infiltration, carbon nuclei form predominantly at SWCNT bundle intersections. Further growth proceeds via the formation of graphite nanosheets – without further influence of the nanotube support. Both sheet edges and their structural imperfections act as reaction centers for subsequent deposition, likely giving rise to autocatalytic deposition kinetics. In contrast, infiltration with a H2:CH4 (24:1) mixture leads to the reductive activation of residual Ni/Co impurities embedded in the precursor SWCNT-felt. This is associated with a different predominant carbon deposition mode in which multiwalled carbon nanotubes grow out from the substrate.