The PhD is Vietnamese, the publication is in English.

Graphene is defined as a flat monolayer of sp2-hybridized carbon atoms tightly
packed into a two-dimensional (2D) honeycomb structure. This stringently 2D
material exhibits a broad range of extraordinary properties, such as excellent
electrical and thermal conductivities, and extremely high strength, which hold
great promises in a variety of applications in micro/nanoelectronics, composites,
and clean energy. Of special interests are the physicochemical properties of
graphene materials strongly dependent on synthetic methods, resulting in diverse
practical uses employed. This dissertation mainly aims to develop new approaches
for production of graphene materials using wet chemistry as well as chemical
vapor deposition (CVD) methods. Subsequently, the as-synthesized graphene
materials are employed for applications as flexible and transparent conductors, a
key component for removal of organic contaminants (including oils or organic
solvents) from water, a supporting barrier for growth of carbon nanotubes (CNTs),
and effective fillers for enhancing electron field emission performance of a vacuum
filtered CNT film.
Generally, exfoliation of graphite into graphene sheets by wet chemistry
approaches require intercalating chemicals into interspaces of graphite layers
followed by harsh oxidation and reduction or selecting a solvent with surface
tension close to that of graphite. In our approach, we prepared ethanol soluble fewlayer
graphene nanosheets (FLGs) without adopting the common receipts, thus
avoided using toxic oxidizing/reducing agents or poisonous solvents. Atomic force
microscopy and high-resolution transmission electron microscopy studies reveal
that FLGs have average thicknesses in the range of 2.6–2.8 nm, corresponding to
8–9 layers. A graphene/nafion composite film has a sheet resistance of 9.70 kΩsq-1
at the transmittance of 74.5% (at 550 nm) while the nafion film on polyethylene
II
terephthalate has a sheet resistance of 128 kΩsq-1 at transmittance of 90.0%. For
the cycling/bending test, almost no change in resistance was exhibited when the
film was bent at an angle up to 1400, and no obvious deviation in resistance could
be found after 100 bending cycles. In addition, a FLGs/poly(3,4-
ethylenedioxythiophene): poly(styrenesulfonate) composite layer was
demonstrated as the effective hole transporting layer to improve the hole
transporting ability in an organic photovoltaic device, with which the power
conversion efficiency was enhanced from 3.10% to 3.70%.
We further investigated the hydrophobic properties of the ethanol soluble FLG
material and its combination with a type of commercial sponge. The FLG films
possess strong hydrophobic properties besides their opto/mechano-electrical
properties aforementioned. By coating an appropriate amount of FLGs on the
sponge skeletons with polydimethylsiloxane (PDMS) binder, superhydrophobic
(water contact angle of ~1620) and superoleophilic (oil contact angle of ~00)
graphene-based sponges were obtained. The as-fabricated graphene-based sponges
perform as an efficient absorbent for a broad range of oils and organic solvents
with high selectivity, good recyclability, and excellent absorption capacities up to
165 times their own weight.
In addition to wet chemistry method, we also developed a CVD method to grow
graphene and integrate thin CNT networks on the surface of the graphene film
using the same CVD system. The thickness of graphene and the CNT density on
graphene surface can be controlled properly. Graphene films are demonstrated as
an effective supporting barrier for preventing poisoning of iron nanoparticles
which catalyze the growth of CNTs on copper substrates. Based on this method,
the opto-electronic and field emission properties of the graphene integrated with
CNTs can be remarkably tailored. A graphene film exhibits a sheet resistance of
III
2.15 kΩsq-1 with a transmittance of 85.6% (at 550 nm) while a CNT–graphene
hybrid film shows an improved sheet resistance of 420 Ωsq-1 with an optical
transmittance of 72.9%. Moreover, CNT–graphene films reveal as effective
electron field emitters with low turn-on and threshold electric fields of 2.9 and 3.3
Vμm-1, respectively.
In order to combine the merits of the two-dimensional graphene and onedimensional
CNT nanocarbon materials, many efforts have recently been made to
obtain graphene-CNT hybrid materials or composites. Most studies on these hybrid
materials focused on optoelectronic and electrical properties. Several attempts to
create ohmic contact between CVD grown graphene and CNTs to enhance the field
emission properties have been investigated. However, no studies utilizing reduced
graphene oxide (RGO) nanosheets as the conductive fillers as well as the
secondary emitters for enhancing field emission performance of CNT film have
been reported to date. Herein, the composite films composing of CNTs and
chemically reduced graphene nanosheets were fabricated using the vacuum
filtration method. Compared to other processing methods such as chemical vapor
deposition, electrophoresis, or screen-printing, this method is more beneficial for
fabrication of low-cost field emitters with density controllable and additive
avoidable. The composite films with different weight ratios between CNTs and
graphene oxide (GO) are prepared by varying the volumes of CNTs and GO
dispersions. The results show that the composite film with GO:CNT weight ratio of
1:3 after hydrazine treatment reveals the best field emission performance with low
turn on and threshold fields of 2.82 and 2.98 V/μm, respectively.

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