Influence of catalyst thickness and temperature
gradient on MWCNT growth and morphology in
TCVD process
M.H. Kara
1, 2, *
, A. Awang Teh
1, 2
, R. Ahmad
1, 2
, M. Rusop
2
, and Z. Awang
1, *
1
Microwave Technology Centre;
2
NANO-ElecTronic Centre;
Faculty of Electrical Engineering, Universiti Teknologi MARA
40450 Shah Alam, Selangor, Malaysia
*Email: mohsenkara@yahoo.com , zaiki.awang@gmail.com
Abstract— In this article the effect of catalyst thickness and
reaction temperature on the formation of horizontal multi-wall
carbon nanotube (MWCNT) was discussed to control product
growth and morphology. MWCNTs were synthesized from
methane by double-heater thermal catalytic vapor deposition
method (TCVD) using a mixture of methanol and ammonia as
active agents to promote the growth of nanotubes and nickel as a
catalyst and are characterized by scanning electron microscopy
(SEM) and Raman spectroscopy.
Results from SEM indicated that, the diameter and density of
tubes increased with increasing the catalyst thickness, whereas the
effect of reaction temperature was on the growth efficiency and
purity of nanotubes and lifetime of the catalyst. The most
favorable temperature for the highest growth efficiency and
purity was around 900 °C. However the optimal catalyst thickness
was around 4 nm.
Keywords:, TCVD, SEM, multiwalled carbon nanotubes,
growth parameters, raman spectroscopy.
I. INTRODUCTION
Carbon nanotubes (CNTs) which consist of graphene sheets
rolled up as hollow cylinders, first identified by Iijima in
1991[1]. Due to their extraordinary electronic, thermal, and
mechanical properties, CNTs offer a promising route for
enormous applications such as electronic devices, field
emission displays, chemical, physical and bio-sensors,
scanning probes, hydrogen storage, etc. [2-5]. Among other
approaches for CNT synthesis, catalytic chemical vapor
deposition (CVD), which has a broad category, including
plasma enhanced CVD (PECVD), thermal CVD (TCVD), and
hot filament CVD (HFCVD) [6 - 8], is the most common
method, due to relatively lower reaction temperature, high
purity, high yield and in-situ selective CNT growth on
catalytically patterned substrates [9 - 11].
In our previous work [12], we found that the new precursor
consist of CH3OH / NH3 with ratio of 8 to 5 respectively to
enhance the growth of CNTs in methane ambient using TCVD
method at fixed reaction temperature of 850°C. However the
dimensions and structure of CNTs critically depend on the
synthesis parameters, such as reaction temperature, synthesis
time, carbon source gas, catalyst structure and thickness [13,
14]. Therefore, optimization of synthesis parameters is crucial
for controlling product morphology in order to produce high
quality aligned CNT.
In this paper, we extended our systematic study through
SEM observations by varying reaction temperature (800 – 1000
°C), and catalyst thickness (1 - 20 nm). The effect of synthesis
time and carbon source gas flow rate on the CNT growth will
be studied later in our next paper.
II. EXPERIMENTAL DETAILS
The fabrication of CNTs on P-type silicon substrates; size 1
cm by 1 cm, thickness 525 ± 25 μm and resistivity 1-10 cm
were done using nickel (Ni) as catalyst. The first process is to
remove any impurity and oxidization on the Si substrate
surface. Then, a thin Ni film was deposited on cleaned
substrates as catalyst using electron beam evaporator and the
substrates were placed on an alumina boat before placed inside
a double-heater TCVD. The first heater was set at 1000 °C to
decompose methane, while the second was set at (800-1000
°C) for pre-treatment of the catalytic film. As A. Awang Teh
et al. proposed [12] a precursor of ammonia and methanol
solution at ratios of 5:8 was placed within the first heater to
enhance the growth of CNT, while the substrates were located
in the second heater. The second heater was first switched in
flowing Argon at 200 bubbles /min. When the temperature of
the second heater reached setting point and stayed stable, first
heater was then switched on. As the temperature of the latter
reached 1000 °C, the Ar supply was switched to methane gas at
flow rate of 100 bubbles /min. The total growth time of the
CNTs was 120 min. Finally, when both heaters were shut off,
methane gas was then switched back to Argon to eliminate any
air. After fabrication is completed, The CNT morphology was
examined using JEOL JSM6360L SEM.
978-1-4577-0255-6/11/$26.00 ©2011 IEEE 783 TENCON 2011