ISSN 0020-1685, Inorganic Materials, 2014, Vol. 50, No. 4, pp. 344–348. © Pleiades Publishing, Ltd., 2014.
Original Russian Text © V.M. Ogenko, L.V. Dubrovina, O.V. Naboka, I.V. Dubrovin, 2014, published in Neorganicheskie Materialy, 2014, Vol. 50, No. 4, pp. 372–376.
344
INTRODUCTION
Carbon-based composites are already in practical
use as sorbents, catalysts of chemical reactions, and
anodes of lithium ion batteries and are potentially
attractive as magnetic, electrically conducting, and
heat-conducting materials. The fabrication of com-
plex-shaped high-temperature heaters (including
flexible configurations), pipes for aggressive media,
and high-temperature thermal shields is based on the
use of carbon–carbon–carbon–carbon composites:
C(exfoliated graphite)–C(pyrolytic carbon)–C(car-
bon fiber)–C(pitch etc.). Exfoliated graphite (EG) is
a relatively new carbon material, which possesses all
the properties of graphite but has a very low bulk den-
sity, large specific surface area, and high plasticity. EG
is characterized by a small thickness of stacks of
graphene layers (20–70 nm) and a high concentration
of pores 2–5 nm in size. Owing to the presence of nan-
opores, EG-based composites can be thought of as
promising sorbents, membranes, and hydrogen stor-
age materials. Moreover, when EG is used as a matrix,
its structural characteristics can be varied via modifi-
cation with pyrolytic carbon [1–6]. Several groups [7–
9] have studied the synthesis conditions, structure,
and properties of EG having metal or metal oxide
nanoparticles supported on its surface, which increase
the capability of the material for adsorption, ion
exchange, and atomic exchange. The use of
microporous carbon–carbon materials is currently
limited by their high cost, so the ability to reduce their
cost remains a priority issue.
The purpose of this work was to fabricate carbon–
carbon composites based on exfoliated graphite mod-
ified with pyrolytic carbon produced via carbonization
of organic and polymeric precursors.
EXPERIMENTAL
As a carbon support for the preparation of pyrolytic
carbon nanostructures, we used exfoliated graphite
(EG) (Sivash Pilot Works, Chuiko Institute of Surface
Chemistry, National Academy of Sciences of
Ukraine). The following carbon precursors, chosen
based on previous results [10, 11], were used: (1) com-
mercially available poly(vinylidene fluoride) (PVDF)
with a characteristic viscosity [η] = 1.2 dL/g, as deter-
mined at 25°C in dimethylformamide (DMFA), and
samples consisting of PVDF and a cobalt(II) chloride
solution in DMFA; (2) a mixture of tolylene 2,4-diiso-
cyanate (70 wt %) and tolylene 2,6-diisocyanate
(30 wt %) (TDI); and (3) IsoPMDI92140 polyisocy-
anate (PIC) (Elastogran, Germany), which is a mix-
ture of 4,4'-diphenylmethane diisocyanate with highly
functional oligomers and isomers (average functional-
ity, 2.7; concentration of NCO groups, 31 wt %).
A PVDF solution (4.0 g/100 mL) and TDI and PIC
solutions in DMFA were used to impregnate EG (at
room temperature). The precursor : matrix ratios were
[PVDF] : [EG] = 1 : 4, [TDI] : [EG] = 1 : 10, and
[PIC] : [EG] = 1 : 5 by weight. Dried samples were
carbonized at 750°C in flowing argon.
The samples were characterized by scanning elec-
tron microscopy (SEM) on a Carl Zeiss Leo Ultra 55
FEG SEM. Before SEM examination, the samples
were applied to a double sided conductive adhesive
tape. The accelerating voltage was 1.5–2.0 kV. The
surface topography of the samples was examined in
secondary-electron mode. The compositional con-
trast was estimated using an EsB low-energy back-
scattered electron detector (filtering grid voltage, 1.3–
1.5 kV). The composition of the carbon samples was
determined by energy dispersive X-ray (EDX) spec-
1
Exfoliated Graphite Modified with Pyrolytic Carbon
V. M. Ogenko
a
, L. V. Dubrovina
a
, O. V. Naboka
a
, and I. V. Dubrovin
b
a
Vernadsky Institute of General and Inorganic Chemistry, National Academy of Sciences of Ukraine,
pr. Akademika Palladina 32/34, Kyiv, 03680 Ukraine
b
Chuiko Institute of Surface Chemistry, National Academy of Sciences of Ukraine,
vul. Generala Naumova 17, Kyiv, 03164 Ukraine
e-mail: divexfoliated@ua.fm
Received June 27, 2013
Abstract—Exfoliated graphite (EG) has been modified with pyrolytic carbon produced by 750°C carboniza-
tion of poly(vinylidene fluoride) (PVDF), tolylene diisocyanate (TDI), and polyisocyanate (PIC) applied to
the EG surface from solutions. The pyrolytic carbon obtained had the form of particles ranging in size from
200 nm to 1 μm. The microstructural characteristics of the carbon–carbon materials depend on the chemical
composition of the carbon precursor: S = 15.8 to 63 m
2
/g; nitrogen sorption from 24.7 to 59.2 cm
3
/g (–
190°C); micropore volume, up to 7.4 mm
3
/g; benzene vapor absorption from 0.07 to 0.27 g/g (20°C).
DOI: 10.1134/S002016851404013X