THESIS
2014
xix, 142 pages : illustrations (some color) ; 30 cm
Abstract
Carbon nanotube (CNT) is a fascinating material with extraordinary electrical thermal and
mechanical properties. Growing vertically aligned CNT (VACNT) arrays on metal substrates
is an important step in bringing CNT into practical applications such as thermal interface
materials (TIMs) and microelectrodes. However, the growth process is challenging due to the
difficulties in preventing catalyst diffusion and controlling catalyst dewetting on metal
substrates with physical surface heterogeneity.
In this work, the catalyst diffusion mechanism and catalyst dewetting theory were studied
for the controlled growth of VACNTs on metal substrates. The diffusion time of the catalyst,
the diffusion coefficients for the catalyst in the substrate materials and the number density of
catalyst...[
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Carbon nanotube (CNT) is a fascinating material with extraordinary electrical thermal and
mechanical properties. Growing vertically aligned CNT (VACNT) arrays on metal substrates
is an important step in bringing CNT into practical applications such as thermal interface
materials (TIMs) and microelectrodes. However, the growth process is challenging due to the
difficulties in preventing catalyst diffusion and controlling catalyst dewetting on metal
substrates with physical surface heterogeneity.
In this work, the catalyst diffusion mechanism and catalyst dewetting theory were studied
for the controlled growth of VACNTs on metal substrates. The diffusion time of the catalyst,
the diffusion coefficients for the catalyst in the substrate materials and the number density of
catalyst nanoparticles after dewetting are identified as the key parameters, based on which
three strategies are developed.
Firstly, a fast-heating catalyst pretreatment strategy was used, aiming at preserving the
amount of catalyst prior to CNT growth by reducing the catalyst diffusion time. The catalyst
lifetime is extended from half an hour to one hour on a patterned Al thin film and a VACNT
height of 106 μm, about twenty fold of that reported in the literature, was attained.
Secondly, a diffusion barrier layer strategy is employed for a reduction of catalyst diffusion
into the substrate materials. Enhancement of VACNT growth on Cu substrates was achieved
by adopting a conformal Al
2O
3 diffusion barrier layer fabricated by a specially designed
atomic layer deposition (ALD) system.
Lastly, a novel catalyst glancing angle deposition (GLAD) strategy is performed to
manipulate the morphology of a relatively thick catalyst on metal substrates with physical
surface heterogeneity, aiming to obtain uniform and dense catalyst nanoparticles after
dewetting in the pretreatment process for enhanced VACNT growth.
We are able to control the VACNT growth conditions on metal substrates in terms of their
distribution, heights and alignments. Catalyst loss is controlled by the catalyst diffusion time
and catalyst diffusion coefficients. A shorter catalyst diffusion time and smaller diffusion
coefficient enhance VACNT growth on metals due to reduced catalyst loss during the
pretreatment process. The dewetting behaviors of the thin film catalysts are influenced by the
physical surface heterogeneity of the substrates which leads to non-uniform growth of
VACNTs. The GLAD process facilitates the deposition of a relatively thick catalyst layer for
the creation of dense and uniform catalyst nanoparticles.
Applications of VACNT-metal structures in TIMs and microelectrodes are demonstrated.
The VACNT-TIMs fabricated on Al alloy substrates have a typical thermal contact resistivity
of 17.1 mm
2∙K/W and their effective application in high-brightness LED thermal management
was demonstrated. Electrochemical characterization was carried out on VACNT
microelectrodes for the development of high resolution retinal prostheses and a satisfactory
electrochemical property was again demonstrated.
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