ISSN 0012-5016, Doklady Physical Chemistry, 2011, Vol. 441, Part 1, pp. 212–214. © Pleiades Publishing, Ltd., 2011.
Original Russian Text © E.V. Moroz, J.A. Zakharova, V.G. Sergeyev, A.B. Zezin, 2011, published in Doklady Akademii Nauk, 2011, Vol. 441, No. 2, pp. 205–208.
212
The polyelectrolyte complexes with oppositely
charged surfactants are formed spontaneously upon
mixing of aqueous solutions of chemically comple-
mentary components [1]. A fundamental feature of
these complexes is the ability of surfactant ions bound
electrostatically to a polyion to be packed in micelles,
which are able to solubilize organic compounds of dif-
ferent chemical nature. As has been shown previously
[2], even small amounts of solubilized compounds can
considerably affect the solubility of the complexes by
changing the hydrophilic–hydrophobic balance of
particles.
In this paper, we report for the first time ternary
complexes, either soluble or insoluble in aqueous solu-
tions, containing multiwalled carbon nanotubes apart
from the polyelectrolyte and the surfactant.
As the polyelectrolyte, we used positively charged
poly(N-ethyl-4-vinylpyridinium bromide)s prepared
by quaternization of poly-4-vinylpyridine (polymer-
ization degree 2500, manufactured by Polyscience,
Inc., USA) with ethyl bromide in methanol. Accord-
ing to IR spectroscopy, the degree of quaternization of
the samples was 32 ± 5% (PEVP
32
) and 83 ± 5%
(PEVP
83
). The polyelectrolyte concentration in the
solution was expressed as the total base molar concen-
tration of all the PEVP units (base-mol/L) including
nonquaternized moieties.
Sodium dodecyl sulfate (SDS, Serva, used as
received) served as the anionic surfactant.
The multiwalled carbon nanotubes (MNT), manu-
factured by Nanocyl (Belgium) with an average diam-
eter of 10 nm and a length of 1.5 μm were dispersed in
aqueous solutions of SDS (20 or 40 mg of MNT in
20 mL of a 1% aqueous solution of SDS) by a 5-min
ultrasonic treatment in an ice bath. Note that the
ultrasonic treatment of nanotubes in micellar surfac-
tant solutions is a known method for the preparation
of stable nanotube dispersions (see, for example [3–
5]). After dispersion, the solutions were centrifuged on
a MiniSpin microcentrifuge at 13000 rpm for 5 min.
The nanotube concentration in the solution was deter-
mined by spectrophotometry based on the absorption
at 500 nm (ε = 42.2 L g
–1
cm
–1
[6]) on a Perkin-Elmer
Lambda 25 spectrophotometer. The photomicro-
graphs of binary and ternary complexes were obtained
on a Leo912 AB Omega transmission electron micro-
scope (TEM) (Carl Zeiss, Germany) (Fig. 1). Judging
by the high contrast of the MNT surface, upon the
ultrasonic dispersion in SDS, the tube surface
becomes coated by a surfactant layer, whose charge
ensures the dispersion stability of the tubes in aqueous
solutions. In addition, it can be seen that the ultra-
sonic treatment of the MNT in a micellar solution of
SDS results in a noticeable decrease in the average
tube length down to approximately 600 nm but almost
does not affect their diameter. The dispersions remain
stable even on dilution with water to a SDS concentra-
tion of less than 1 × 10
–3
mol/L, which is much lower
than the critical micelle concentration (the CMC of
SDS in water at 25°C is 8 × 10
–3
mol/L [1]).
The PEVP–SDS–MNT ternary complexes were
obtained by dropwise addition (with vigorous stirring)
of an aqueous MNT-SDS dispersion (1 to 2 g/L of
nanotubes, [SDS] = 0.035 mol/L) to solutions of
PEVP in the desired component ratio. The final con-
centration of the polyions in the samples was 0.004–
0.016 base-mol/L. Alternatively, a solution of PEVP
was rapidly added with stirring to a dilute MNT–SDS
dispersion. In the series of samples obtained in this
way, the final SDS concentration was 1.4 × 10
–3
mol/L
and the MNT concentration was 45 mg/L. The result-
ing ternary mixtures were kept for at least 24 h to reach
equilibrium.
The composition of the reaction mixture Z =
[SDS]/[PEVP
+
], where [SDS] is the molar concen-
tration of surfactant ions and the [PEVP
+
] is the molar
concentration of quaternized PEVP units, was varied
from 0 to 1.2.
For separating large aggregates, which are below
referred to as insoluble complexes, the reaction mix-
tures were centrifuged at 13 000 rpm. The PEVP con-
centration in the supernatants was determined by
spectrophotometry. Since at λ 257 nm (the absorption
maximum of PEVP) the absorption of the polymer
is superimposed on the absorption of nanotubes,
PHYSICAL
CHEMISTRY
Ternary Complexes Polyelectrolyte–Oppositely Charged
Surfactant–Carbon Nanotubes: Formation and Properties
E. V. Moroz, J. A. Zakharova, V. G. Sergeyev, and Corresponding Member of the RAS A. B. Zezin
Received May 11, 2011
DOI: 10.1134/S0012501611090077
Moscow State University, Moscow, 119991 Russia