While many forms of carbon nanotubes and filamentous carbon have been repor
ted, both a large inside diameter and highly graphitic wall structure have
not been created. This paper describes such tubes from 70 to 1300 nm in dia
meter which were synthesized hydrothermally in the C-H-O-Ni system at 100 M
Pa and 730-800 degreesC by first establishing a post-pyrolysis C-H-O equili
brium followed by an increase in pressure during which time growth of graph
itic carbon occurred. Depending on the size of the Ni catalyst particles, f
lake-like graphite or carbon tubules were formed. Tubes were also synthesiz
ed without water, i.e., in the C-H-Ni system, but these tubes had multiple
internal caps while those produced with water present had very few internal
obstructions and a large inside diameter. The exceptional quality of the t
ube walls is demonstrated by straight and perfect lattice fringing in the t
ube walls and electron diffraction spot patterns free of diffuse amorphous
rings. Raman spectral evidence shows high similarity to the spectra obtaine
d from high purity natural graphite. The high integrity of hydrothermal nan
otubes is demonstrated by the existence of liquid inclusions trapped inside
the tubes during synthesis. The properties of hydrothermal graphite tubes
suggest their use in nano-fluidic devices and as lightweight reinforcement
for composites. (C) 2001 Elsevier Science Ltd. All rights reserved.