Growth of Single-Walled Carbon Nanotubes from Solid Carbon Nanoparticle Seeds via Cap Formation Engineering with a Two-Step Growth Process and Water Vapor Supply.

Solid carbon nanoparticles are promising growth seeds to prepare single-walled carbon nanotubes (SWCNTs) at high temperatures, at which the SWCNT crystallinity should be improved significantly but conventional metal catalyst nanoparticles are unstable and suffer from aggregation. The noncatalytic nature of solid carbon nanoparticles, however, makes SWCNT growth inefficient, resulting in a limited growth yield. In this study, we develop a two-step chemical vapor deposition process to efficiently synthesize high-crystallinity SWCNTs at high temperatures from solid carbon nanoparticles obtained from nanodiamond. Based on thermodynamic considerations, the growth conditions are separately adjusted to supply different growth driving forces which are suitable for the formation of the initial cap structures and for the stationary elongation of SWCNTs. This process, called cap formation engineering, improves the nucleation density of the cap structures. We examined the changes in crystallinity, amorphous carbon deposition, diameter, and yield of SWCNTs with respect to the synthesis conditions. By controlling the initial growth conditions, high-quality SWCNTs are grown with improved yield. With the addition of water vapor as the etchant, deposition of amorphous carbon at high temperatures was further prevented. The results provide a pathway for precise growth control of SWCNTs from unconventional solid growth seeds.