ISSN 1023-1935, Russian Journal of Electrochemistry, 2012, Vol. 48, No. 4, pp. 375–387. © Pleiades Publishing, Ltd., 2012.
Published in Russian in Elektrokhimiya, 2012, Vol. 48, No. 4, pp. 413–426.
375
INTRODUCTION
As it was shown in our preceding work [1], charge
transfer processes with participation of particles capa-
ble to reduce/oxidize on the surface of metal clusters
included into electroactive polymer films can be
described in terms of diffusion equations (for concen-
trations of such particles) complicated with accompa-
nying electrochemical reactions in the film interior. In
the cited paper, it was also mentioned that the same
approach might be used in case of pristine polymer
films containing populations of different pores, which
completely or partially penetrate such films. In our
opinion, the necessity of the corresponding consider-
ation is stipulated by the well-known fact that real
polymer films are porous systems [2–4]. In this con-
nection, one can also remind the previously estab-
lished data on the hydrazine electrooxidation at Prus-
sian blue (PB) modified electrodes [5], The interesting
result of that study was the observed dependence of the
measured currents on the amount of PB deposited on
the electrode substrate. Though the authors of [5] have
treated this finding in scope of traditional representa-
tions, other two explanations seem also possible. In
particular, one could try to explain the observed
dependence by assuming that hydrazine molecules are
inculcated into the film volume and react with ox–
fragments of the film, i.e. a volume electrochemical
reaction takes place in the film interior. It is also nec-
essary to additionally suppose that the so-called
kinetic layer thickness of such volume reaction [6, 7] is
significantly higher than the film thickness, so that the
maximum currents could be achieved only in the limit
of thick films.
An alternative explanation can be based on the
assumption that the real border between the film and
the bathing electrolyte solution exceeds significantly the
visible film/solution interface due to a microcrystalline
character of PB films [8] or, in other words, the exist-
ence of some surface invaginations and/or pores pene-
trating the films. If one supposes the hydrazine elec-
trooxidation to exclusively proceed on such a physical
border, the observed increase of limiting currents with
increasing the film thickness can be referred to some
deepening of the presumed invaginations and/or pores,
which accompanies the rise of the film width. It is well
known that such an effect of changing the real electrode
surface usually takes place under electrodeposition of
metals. One can therefore expect the same phenome-
non for electropolymerization processes on modified
electrodes. As it will be shown in the next part of the
paper, simulation procedures corresponding to the
indicated mechanisms coincide in their main physical
features, though the conclusions derived for heteroge-
Electrical Currents Resulting from Reduction/Oxidation Processes
of Tested Particles on “Inner” and “Outer” Surfaces
of Electroactive Polymer Films
1, 2
V. V. Malev
a, b, z
and O. V. Levin
a
a
Department of Chemistry, St-Petersburg State University
b
Institute of Cytology, Russian Academy of Sciences, St-Petersburg
Received March 16, 2011
Abstract—Heterogeneous reactions of tested particles proceeding on electroactive films with different kinds
of thin pores are described formally in terms of diffusion equations complicated with an accompanying vol-
ume reaction inside the film interior. As it is shown, in polarization curves of such processes, there might
appear limiting flows, which are essentially smaller than the limiting diffusion flow of tested particles in the
bathing electrolyte. These flows should not depend on a film pores’ topology, but be determined by the ratio
of the total surface of pores and the visible film one. The obtained results are compared with those followed
for the case when tested particles actually inculcate into the film matrix and react with either ox- or red-frag-
ments of the film. Identification criteria of the compared mechanisms are discussed.
Keywords: electroactive films, film pores, tested particles, limiting flow, volume and heterogeneous reactions,
electrode potential
DOI: 10.1134/S102319351203007X
1
Published on the basis of the materials of the IXth International
Frumkin Symposium “Materials and Technologies of Electro-
chemistry of the XXIst Century” (Moscow, October, 2010).
2
The article was translated by the authors.
z
Corresponding author: elchem@rbcmail.ru (V.V. Malev).