Purification of single-walled carbon nanotubes synthesized by
the hydrogen arc-discharge method
Pengxiang Hou, Chang Liu, Yu Tong, Shitao Xu, Min Liu, and Huiming Cheng
a)
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy
of Sciences, Shenyang 110016, People’s Republic of China
(Received 29 May 2001; accepted 12 June 2001)
A simple procedure for the purification of the single-walled carbon nanotube (SWNT)
product synthesized by the hydrogen arc-discharge method was proposed and
discussed. The procedure involves ultrasonication in alcohol, oxidation in fixed air, and
soaking in hydrochloric acid. Most of the amorphous carbon and carbon nanoparticles
as well as metal particles in the product was successfully removed, according to the
results obtained from transmission electron microscopy, thermogravimetric analysis,
and resonant laser Raman measurements. With this procedure, a 41 wt% yield of the
SWNTs with a purity of about 96% was achieved after purification.
I. INTRODUCTION
Recently, several methods
1–3
for large-scale synthesis
of single-walled carbon nanotubes (SWNTs) have
opened the door to study their physical and chemical
properties, which were expected to be unique.
4,5
How-
ever, the as-prepared SWNTs synthesized by any method
usually contain a large amount of impurities, such as
metal particles, amorphous carbon, and carbon nanopar-
ticles. These impurities are closely entangled with
SWNTs or stick on the outer surface of the SWNTs. The
impurities present in the as-prepared products are delete-
rious to the precise measurement for the properties
of SWNTs.
Various oxidation methods
6–13
have been explored for
the purification of SWNTs. One simple purification
method is the gas-phase oxidation of the SWNT soot at
elevated temperatures.
6
However, the SWNTs are so
fragile during high-temperature oxidation that the yield is
less than 1 wt%. Tohji
10
et al. used an improved gas
oxidation, in which they incorporated a hydrothermal
treatment for the easy removal of the impurities of both
metal particles and carbonaceous materials; the yield
they obtained increased to some 20 wt%.
In this paper, we report a simple method that appears
to be quite suitable for the purification of SWNTs syn-
thesized by the hydrogen arc-discharge method. The pu-
rification procedure includes ultrasonication, oxidation in
fixed air, and acid washing. With this procedure, the
impurities of metal particles, amorphous carbon, and
carbon nanoparticles could be effectively removed; a
41 wt% yield of the SWNTs with a purity of about 96%
was achieved.
II. EXPERIMENTAL
A. Synthesis of SWNTs
The SWNTs were synthesized by the hydrogen arc-
discharge method, which has been described else-
where.
14
The electric arc was typically operated in a
direct current (dc) mode using 150 A under an atmos-
phere of 200 torr H
2
, with a distance of approximately
2 mm maintained between the two electrodes. Transition
metals, including iron, nickel, and cobalt, were selected
as co-catalysts. A mixture of 2.6 at.% Ni, 0.7 at.% Fe,
0.7 at.% Co, 0.75 at.% FeS, and graphite powders gave a
yield of more than 1 g SWNTs within 3 min of synthesis.
The morphology of the raw sample is usually in large
slices of thin films and weblike substances.
B. Purification procedures of SWNTs
The sample (60 mg) of the as-prepared SWNTs was
first ultrasonicated in alcohol for 30 min to disperse the
SWNTs and dried in air at room temperature. Subse-
quently, the oxidation of the dried sample was conducted
in fixed air at 550 °C for 40 min. After the oxidation
procedure, the black product was soaked in hydrochloric
acid at room temperature to remove metal particles. Fi-
nally, the sample was washed with deionized water and
dried for characterization. About 25 mg of the purified
SWNTs was obtained after drying in an oven at 150 °C
for 12 h.
a)
Address all correspondence to this author.
e-mail: cheng@imr.ac.cn
J. Mater. Res., Vol. 16, No. 9, Sep 2001 © 2001 Materials Research Society 2526