SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS
Tin-cobalt alloy coatings with a tin content of 5–85 wt.% were synthesized from a polyligand citrate-chloride electrolyte. The surface morphology and composition of tin-cobalt alloy coatings depending on the conditions of their production were studied using EDS and XRD methods. The dynamics of chan...
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Ukrainian Chemistry Journal| _version_ | 1871466099536560128 |
|---|---|
| author | Nikitenko, Vasyl Maltseva, Tetiana Babenkov, Eugen Kublanovsky, Valeriy |
| author_facet | Nikitenko, Vasyl Maltseva, Tetiana Babenkov, Eugen Kublanovsky, Valeriy |
| author_institution_txt_mv | [
{
"author": "Vasyl Nikitenko",
"institution": "Vernadsky Institute of General & Inorganic Chemistry of National Academy of Sciences of Ukraine, Academic Palladin Avenue, 32\/34, Kyiv, 03142"
},
{
"author": "Tetiana Maltseva",
"institution": "V. I. Vernadsky Institute of General and Inorganic Chemistry of the National Academy of Sciences of Ukraine, 32\/34, Academic Palladin Avenue, Kiev, 03142, Ukraine"
},
{
"author": "Eugen Babenkov",
"institution": "Vernadsky Institute of General & Inorganic Chemistry of National Academy of Sciences of Ukraine, Academic Palladin Avenue, 32\/34, Kyiv, 03142"
},
{
"author": "Valeriy Kublanovsky",
"institution": "V. I. Vernadsky Institute of General and Inorganic Chemistry of the National Academy of Sciences of Ukraine, 32\/34, Academic Palladin Avenue, Kiev, 03142, Ukraine"
}
] |
| author_sort | Nikitenko, Vasyl |
| baseUrl_str | https://ucj.org.ua/index.php/journal/oai |
| collection | OJS |
| datestamp_date | 2026-07-22T08:23:55Z |
| description | Tin-cobalt alloy coatings with a tin content of 5–85 wt.% were synthesized from a polyligand citrate-chloride electrolyte. The surface morphology and composition of tin-cobalt alloy coatings depending on the conditions of their production were studied using EDS and XRD methods. The dynamics of changes in the parameters of the equivalent impedance circuit on tin-cobalt alloy coatings in 0.1 mol∙l-1 KOH solution is determined by the process of formation of a cobalt (II) hydroxide layer on the coating surface. The parameters of corrosion resistance and electrocatalytic activity of the coatings in the reaction of hydrogen evolution were calculated from the stationary voltammetry dependences. The corrosion currents on tin-cobalt alloy coatings with a tin content of 33–85 wt.% are about 10-6–10-8 A∙cm-2. An inverse dependence of the hydrogen evolution overvoltage on tin-cobalt alloy coatings on the corrosion current was established. |
| doi_str_mv | 10.33609/2708-129X.91.1.2025.3-11 |
| first_indexed | 2025-09-24T17:43:59Z |
| format | Article |
| fulltext |
3
UDC 541.136 doi: 10.33609/2708-129X.91.1.2025.3-11
SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES
OF TIN-COBALT ALLOY COATINGS.
V.M. Nikitenko*, T.V. Maltseva, E.A. Babenkov, V.S. Kublanovsky
Vernadsky Institute of General and Inorganic Chemistry
of the National Academy of Sciences of Ukraine,
32/34 Academician Palladin Ave., 03142 Kyiv, Ukraine
*e-mail: vasylnikitenko@gmail.com
Tin-cobalt alloy coatings with a tin content of 5–85 wt.% were synthesized from a poly
ligand citrate-chloride electrolyte. The surface morphology and composition of tin-cobalt al-
loy coatings depending on the conditions of their production were studied using EDS and
XRD methods. The dynamics of changes in the parameters of the equivalent impedance cir-
cuit on tin-cobalt alloy coatings in 0.1 mol∙l-1 KOH solution is determined by the process of
formation of a cobalt (II) hydroxide layer on the coating surface. The parameters of corrosion
resistance and electrocatalytic activity of the coatings in the reaction of hydrogen evolution
were calculated from the stationary voltammetry dependences. The corrosion currents on
tin-cobalt alloy coatings with a tin content of 33–85 wt.% are about 10-6–10-8 A∙cm-2. An in-
verse dependence of the hydrogen evolution overvoltage on tin-cobalt alloy coatings on the
corrosion current was established.
Key words: electrodeposition, tin-cobalt alloy, citrate-chloride electrolyte, corrosion re-
sistance, electrocatalytic activity.
INTRODUCTION. Electrolytic coatings of
tin-cobalt alloy are promising anode materi-
als for lithium-ion batteries (LIB) due to their
high specific capacity and stability during cy-
cling [1–3]. Cobalt serves as a kind of buffer,
contributing to an increase in the mechanical
strength of tin during cycling in LIB. In ad-
dition, tin-based alloy coatings are currently
being studied as electrocatalysts for reactions
of hydrogen ion [4–7] and nitrate ion [8, 9]
reduction, oxygen evolution [7], and selective
reduction of carbon dioxide to formate ions
[10, 11].
One of the most effective and controlled
methods of applying coatings with metals and
alloys, allowing to influence their morpho
logy, structure and functional properties, is
electrolytic deposition from aqueous solutions
of complex compounds. Correctly selected li
gands allow to influence purposefully the in-
hibition of the electrode process, the compo-
sition of electrochemically active complexes
4 ISSN 2708-129X. Укр. хім. журн., 2025
SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS.PHISICAL CHEMISTRY
(EAC), the mechanism of the process, and,
consequently, the morphology, structure and
functional properties of the resulting coatings
with metals and alloys [12–14].
For deposition of tin-cobalt alloy coatings,
we selected a polyligand citrate-chloride elect
rolyte, in which the formation of electrochemi-
cally active complexes (EAC) and deposition of
tin (II) into the alloy is limited by the dissocia
tion of electrochemically inactive complexes
(EIC) [SncitCl2]
3–, and this allows us to control
the chemical composition of the alloy by select-
ing the ratio of the electrolyte components and
the deposition conditions. In a polyligand cit-
rate-chloride electrolyte at pH 4-6, tin (II) ions,
in contrast to the citrate electrolyte, exist in the
form of the EIC of the composition [SncitCl2]
3–
[15], while cobalt (II) ions exist in the form of
the EAC of the composition [CoH2cit]+ and
[CoHcit] [14]. Precipitation of tin (II) and co-
balt (II) ions from the monoligand citrate elec-
trolyte in this pH region is limited by mixed
kinetics [16]. The precipitation of tin(II) ions
into a tin-cobalt alloy from a polyligand cit-
rate-chloride electrolyte at pH 4-6, in contrast
to a citrate electrolyte, is limited not by mixed
kinetics, but by a preceding chemical reaction
of dissociation of polyligand electrochemically
inactive complexes [SncitCl2]
3-:
[SncitCl2]
3– ↔ [Sncit]– + 2Cl–. (1)
The presence of electrochemically inactive
[SncitCl2]
3- complexes in the citrate-chloride
electrolyte is an additional factor that allows
us to influence the composition, morpholo-
gy, structure and functional properties of the
resulting tin-cobalt alloy coatings, primarily
their porosity and corrosion resistance. The
presence of citric acid in the proposed cit-
rate-chloride electrolyte allows increasing the
buffer capacity and stability of the electrolyte
during its long-term operation. This work is
devoted to the development of a process for
applying functional tin-cobalt alloy coatings
from a complex citrate-chloride electrolyte for
various functional purposes, as well as studying
their morphology, phase, chemical composi-
tion, corrosion resistance and electrocatalytic
activity in the reaction of hydrogen evolution
in an alkaline medium.
EXPERIMENT AND DISCUSSION OF
THE RESULTS. Tin-cobalt alloy coatings
were applied to copper foil (S = 2 cm2) from
a citrate-chloride electrolyte of the follow-
ing composition, mol∙l-1: SnCl2∙2H2O – 0.05;
CoSO4∙7H2O – 0.10; Na3C6H5O7 – 0.30;
C6H8O7∙H2O – 0.05; Na2SO4∙10H2O – 0.50;
pH 4.6 in a thermostatic cell at a direct current
density of 1-30 mA∙cm-2 and a temperature of
40 0C. A platinum plate (S = 12 cm2) was used
as the anode. Analytical grade reagents were
used to prepare the electrolyte. The surface of
the copper substrate was pre-degreased with
Vienna lime and activated according to the
method [17]. The electrolysis parameters were
set using a PI-50-1 potentiostat and a PR-8
programmer. To obtain good quality coatings,
the citrate-chloride electrolyte was pre-treated
at a current density 0.5 mA∙cm-2 for 4 hours.
The structural characteristics of the coat-
ings were studied by X-ray phase analysis us-
ing a DRON-2UM setup with CuKα radiation
in the angle range from 10 to 85 degrees with
a recording step of 0.04 degrees at an exposure
time of 3 sec. The chemical composition of the
tin-cobalt alloy coatings was determined using
the atomic absorption method. The corrosion
properties of the tin-cobalt alloy coatings were
studied in a 0.1 mol∙l-1 KOH solution at 20 0C.
5https://ucj.org.ua
V.M. Nikitenko, T.V. Maltseva, E.A. Babenkov, V.S. Kublanovsky UCJ № 1 / Vol. 91
The electrochemical impedance spectra and
current-voltage dependencies were obtained
using the AUTOLAB system with GPES4.7
software in the frequency range from 0.1 Hz
to 100 kHz and voltage amplitude of 10 mV.
A saturated silver chloride electrode was used
as a reference electrode. Platinum served as an
auxiliary electrode. The value of the active re-
sistance of the coatings Rz was calculated using
the built-in program “Find circle”. The parame
ters of the electrocatalytic activity of tin-cobalt
alloy coatings in the of hydrogen evolution
reaction were calculated from the linear sec-
tions of the lg j – η dependences. The polari-
zation value was calculated relative to the hy-
drogen electrode based on the potential of the
2H+/H2 pair, which in a 0.1 mol∙l-1 KOH solu-
tion is 0.75 V (pH = 12.7).
Micrographs of the surface of tin-cobalt al-
loy coatings obtained from a citrate-chloride
electrolyte are shown in Fig. 1. At a current
density of up to 3.0 mA∙cm-2, as can be seen
from Fig. 1a, fine-crystalline coatings are de-
posited that are well bonded to the substrate.
The tin-cobalt alloys coatings are well formed,
densely packed, fairly uniform, and are close
in appearance to smooth coatings. With an in-
crease in current density, a scaly structure of
the deposit is observed, and at higher current
densities (from 20 mA∙cm-2 and higher), crys-
talline coatings are deposited, consisting of
spherulites with particle sizes 1–5 µm.
a b c
Fig. 1. Microstructure of the surface of tin-cobalt alloy coatings obtained from citrate-chloride elec-
trolyte at a current density, mA∙cm-2: 3.0 (a); 12.0 (b); 30.0 (c), temperature of 40 0C, stirring speed of
400 rpm, electrolysis time of 20 min.
2
2
The presence of electrochemically inactive [SncitCl2]3- complexes in the citrate-chloride
electrolyte is an additional factor that allows us to influence the composition, morphology, structure
and functional properties of the resulting tin-cobalt alloy coatings, primarily their porosity and
corrosion resistance. The presence of citric acid in the proposed citrate-chloride electrolyte allows
increasing the buffer capacity and stability of the electrolyte during its long-term operation. This
work is devoted to the development of a process for applying functional tin-cobalt alloy coatings
from a complex citrate-chloride electrolyte for various functional purposes, as well as studying their
morphology, phase, chemical composition, corrosion resistance and electrocatalytic activity in the
reaction of hydrogen evolution in an alkaline medium.
EXPERIMENT AND DISCUSSION OF THE RESULTS. Tin-cobalt alloy coatings were applied
to copper foil (S = 2 cm2) from a citrate-chloride electrolyte of the following composition, mol∙l-1:
SnCl2∙2H2O – 0.05; CoSO4∙7H2O – 0.10; Na3C6H5O7 – 0.30; C6H8O7∙H2O – 0.05; Na2SO4∙10H2O
– 0.50; pH 4.6 in a thermostatic cell at a direct current density of 1-30 mA∙cm-2 and a temperature
of 40 0C. A platinum plate (S = 12 cm2) was used as the anode. Analytical grade reagents were used
to prepare the electrolyte. The surface of the copper substrate was pre-degreased with Vienna lime
and activated according to the method [17]. The electrolysis parameters were set using a PI-50-1
potentiostat and a PR-8 programmer. To obtain good quality coatings, the citrate-chloride
electrolyte was pre-treated at a current density 0.5 mA∙cm-2 for 4 hours.
The structural characteristics of the coatings were studied by X-ray phase analysis using a
DRON-2UM setup with CuK radiation in the angle range from 10 to 85 degrees with a recording
step of 0.04 degrees at an exposure time of 3 sec. The chemical composition of the tin-cobalt alloy
coatings was determined using the atomic absorption method. The corrosion properties of the tin-
cobalt alloy coatings were studied in a 0.1 mol∙l-1 KOH solution at 20 0C. The electrochemical
impedance spectra and current-voltage dependencies were obtained using the AUTOLAB system
with GPES4.7 software in the frequency range from 0.1 Hz to 100 kHz and voltage amplitude of 10
mV. A saturated silver chloride electrode was used as a reference electrode. Platinum served as an
auxiliary electrode. The value of the active resistance of the coatings Rz was calculated using the
built-in program “Find circle”. The parameters of the electrocatalytic activity of tin-cobalt alloy
coatings in the of hydrogen evolution reaction were calculated from the linear sections of the lg j –
dependences. The polarization value was calculated relative to the hydrogen electrode based on
the potential of the 2H+/H2 pair, which in a 0.1 mol∙l-1 KOH solution is 0.75 V (pH = 12.7).
Micrographs of the surface of tin-cobalt alloy coatings obtained from a citrate-chloride
electrolyte are shown in Fig. 1. At a current density of up to 3.0 mA∙cm-2, as can be seen from Fig.
1a, fine-crystalline coatings are deposited that are well bonded to the substrate. The tin-cobalt alloys
coatings are well formed, densely packed, fairly uniform, and are close in appearance to smooth
coatings. With an increase in current density, a scaly structure of the deposit is observed, and at
higher current densities (from 20 mA∙cm-2 and higher), crystalline coatings are deposited,
consisting of spherulites with particle sizes 1–5 m.
a b c
Fig. 1. Microstructure of the surface of tin-cobalt alloy coatings obtained from citrate-chloride
electrolyte at a current density, mA∙cm-2: 3.0 (a); 12.0 (b); 30.0 (c), temperature of 40 0C, stirring speed of
400 rpm, electrolysis time of 20 min.
The tin content in tin-cobalt alloy coatings
obtained from citrate-chloride electrolyte de-
pends on the parameters of their deposition
and varies in the range of 5–85%. The X-ray
diffraction pattern of the tin-cobalt alloy coat-
ing (Fig. 2) contains several diffraction peaks. It
should be noted that the number of peaks and
their position in the X-ray diffraction pattern
does not depend on the conditions of coating
production. Electrolysis parameters affect only
the magnitude of the diffraction peaks and
the properties of the resulting coatings. Peaks
characteristic of the tin-cobalt alloy are ob-
served at 2θ deviation angles of 32 and 45 de-
grees. These peaks indicate the presence of an
amorphous or incompletely formed crystalline
phase in the tin-cobalt alloy and do not allow
one to determine a specific phase. In addition
6 ISSN 2708-129X. Укр. хім. журн., 2025
SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS.PHISICAL CHEMISTRY
to the peaks corresponding to the tin-cobalt al-
loy, there are peaks that, by their position, can
be attributed to metallic tin. The presence of a
peak corresponding to metallic copper is due
to its use as a substrate when applying coatings
with a tin-cobalt alloy from a citrate-chloride
electrolyte.
Fig. 2. X-ray diffraction pattern of a tin-cobalt
alloy coating obtained from a citrate-chloride elec-
trolyte at a current density of 4.0 mA cm–2, 40 0C
and an electrolysis duration of 60 min.
According to the phase diagram [18, 19], tin
forms intermetallic compounds with cobalt of
the following composition: CoSn, Co2Sn and
Co3Sn2. The Co3Sn2 compound consists of two
phases Co2Sn + α-CoSn or Co2Sn + β-CoSn.
It should be noted that tin-cobalt alloy coat-
ings, which are a single-phase intermetallic
compound of the CoSn composition, can only
be obtained by the electrolytic method from
complex electrolytes. According to the results
of chemical analysis of the obtained coatings,
with an increase in the current density, the ra-
tio of cobalt to tin in the alloy changes from
1:2 to 2:1, which may indicate a change in the
composition of the intermetallic compounds of
the alloy from CoSn2 to CoSn, Co3Sn2 and fur-
ther to Co2Sn, which is consistent with the data
of [2, 20]. The impedance spectra of tin-cobalt
alloy coatings with a content of 66.7 at. % tin,
obtained from a citrate-chloride electrolyte
at a current density of 3.0 mA∙cm-2, from the
holding time in a 0.1 mol∙l-1 KOH solution, are
shown in Fig. 3.
3
3
The tin content in tin-cobalt alloy coatings obtained from citrate-chloride electrolyte depends on
the parameters of their deposition and varies in the range of 5–85%. The X-ray diffraction pattern of
the tin-cobalt alloy coating (Fig. 2) contains several diffraction peaks. It should be noted that the
number of peaks and their position in the X-ray diffraction pattern does not depend on the
conditions of coating production. Electrolysis parameters affect only the magnitude of the
diffraction peaks and the properties of the resulting coatings. Peaks characteristic of the tin-cobalt
alloy are observed at 2 deviation angles of 32 and 45 degrees. These peaks indicate the presence of
an amorphous or incompletely formed crystalline phase in the tin-cobalt alloy and do not allow one
to determine a specific phase. In addition to the peaks corresponding to the tin-cobalt alloy, there
are peaks that, by their position, can be attributed to metallic tin. The presence of a peak
corresponding to metallic copper is due to its use as a substrate when applying coatings with a tin-
cobalt alloy from a citrate-chloride electrolyte.
Fig. 2. X-ray diffraction pattern of a tin-cobalt alloy coating obtained from a citrate-chloride electrolyte at a
current density of 4.0 mA cm–2, 40 0C and an electrolysis duration of 60 min.
According to the phase diagram [18, 19], tin forms intermetallic compounds with cobalt of the
following composition: CoSn, Co2Sn and Co3Sn2. The Co3Sn2 compound consists of two phases
Co2Sn + -CoSn or Co2Sn+-CoSn. It should be noted that tin-cobalt alloy coatings, which are a
single-phase intermetallic compound of the CoSn composition, can only be obtained by the
electrolytic method from complex electrolytes. According to the results of chemical analysis of the
obtained coatings, with an increase in the current density, the ratio of cobalt to tin in the alloy
changes from 1:2 to 2:1, which may indicate a change in the composition of the intermetallic
compounds of the alloy from CoSn2 to CoSn, Co3Sn2 and further to Co2Sn, which is consistent with
the data of [2, 20]. The impedance spectra of tin-cobalt alloy coatings with a content of 66.7 at. %
tin, obtained from a citrate-chloride electrolyte at a current density of 3.0 mA∙cm-2, from the
holding time in a 0.1 mol∙l-1 KOH solution, are shown in Fig. 3.
3
3
The tin content in tin-cobalt alloy coatings obtained from citrate-chloride electrolyte depends on
the parameters of their deposition and varies in the range of 5–85%. The X-ray diffraction pattern of
the tin-cobalt alloy coating (Fig. 2) contains several diffraction peaks. It should be noted that the
number of peaks and their position in the X-ray diffraction pattern does not depend on the
conditions of coating production. Electrolysis parameters affect only the magnitude of the
diffraction peaks and the properties of the resulting coatings. Peaks characteristic of the tin-cobalt
alloy are observed at 2 deviation angles of 32 and 45 degrees. These peaks indicate the presence of
an amorphous or incompletely formed crystalline phase in the tin-cobalt alloy and do not allow one
to determine a specific phase. In addition to the peaks corresponding to the tin-cobalt alloy, there
are peaks that, by their position, can be attributed to metallic tin. The presence of a peak
corresponding to metallic copper is due to its use as a substrate when applying coatings with a tin-
cobalt alloy from a citrate-chloride electrolyte.
Fig. 2. X-ray diffraction pattern of a tin-cobalt alloy coating obtained from a citrate-chloride electrolyte at a
current density of 4.0 mA cm–2, 40 0C and an electrolysis duration of 60 min.
According to the phase diagram [18, 19], tin forms intermetallic compounds with cobalt of the
following composition: CoSn, Co2Sn and Co3Sn2. The Co3Sn2 compound consists of two phases
Co2Sn + -CoSn or Co2Sn+-CoSn. It should be noted that tin-cobalt alloy coatings, which are a
single-phase intermetallic compound of the CoSn composition, can only be obtained by the
electrolytic method from complex electrolytes. According to the results of chemical analysis of the
obtained coatings, with an increase in the current density, the ratio of cobalt to tin in the alloy
changes from 1:2 to 2:1, which may indicate a change in the composition of the intermetallic
compounds of the alloy from CoSn2 to CoSn, Co3Sn2 and further to Co2Sn, which is consistent with
the data of [2, 20]. The impedance spectra of tin-cobalt alloy coatings with a content of 66.7 at. %
tin, obtained from a citrate-chloride electrolyte at a current density of 3.0 mA∙cm-2, from the
holding time in a 0.1 mol∙l-1 KOH solution, are shown in Fig. 3.
Fig. 3. Nyquist (a) and Bode (b) plots for tin-cobalt alloy samples containing 66.7 at.% tin versus hold-
ing time, min.: 20 (1), 40 (2) and 60 (3) in 0.1 mol∙l-1 KOH solution.
7https://ucj.org.ua
V.M. Nikitenko, T.V. Maltseva, E.A. Babenkov, V.S. Kublanovsky UCJ № 1 / Vol. 91
When comparing the obtained dependencies
with the diagnostic ones shown in Fig. 4 [21, 22],
it can be concluded that an oxide-hydroxide lay-
er of cobalt (II) has formed on the film surface.
After a sufficiently long holding time (60 min.)
of the sample in a 0.1 mol∙l-1 KOH solution the
electrical parameters of the coating (resistance
and capacity) remain constant.
a b
Fig. 4. Equivalent impedance circuits of tin-cobalt alloy coatings and Nyquist and Bode diagnostic
dependences when the coatings are kept in a 0.1 mol l-1 KOH solution for 20 (a) and 60 (b) min.
4
4
Fig. 3. Nyquist (a) and Bode (b) plots for tin-cobalt alloy samples containing 66.7 at.% tin versus holding
time, min.: 20 (1), 40 (2) and 60 (3) in 0.1 mol∙l-1 KOH solution.
When comparing the obtained dependencies with the diagnostic ones shown in Fig. 4 [21, 22], it
can be concluded that an oxide-hydroxide layer of cobalt (II) has formed on the film surface. After a
sufficiently long holding time (60 min.) of the sample in a 0.1 mol∙l-1 KOH solution the electrical
parameters of the coating (resistance and capacity) remain constant.
a
b
Fig. 4. Equivalent impedance circuits of tin-cobalt alloy coatings and Nyquist and Bode diagnostic
dependences when the coatings are kept in a 0.1 mol l-1 KOH solution for 20 (a) and 60 (b) min.
On samples of tin-cobalt alloy with a tin content of 33.3 at. %, obtained at a deposition current
density of 7.5 mA∙cm-2, the Nyquist and Bode dependences have a similar character. In this case,
only the numerical values of the parameters of the equivalent impedance circuit change: the
contribution of the hydroxide layer resistance to the total corrosion resistance of such films is
insignificant (< 5%). Based on the equality of the values of the stationary electrode potentials of
reactions (2) and (3), we can write the reactions:
Sn = Sn 2+ + e, Е2 = 0.136 + 0.0291lg [Sn2+], (2)
Co = Co2+ + e, Е3 = 0.277 + 0.0291lg [Co 2+], (3)
which can occur on the surface of a tin-cobalt alloy in a 0.1 mol∙L-1 KOH solution (pH12.7), it
can be shown that under these conditions, corrosion of the tin-cobalt alloy coating occurs due to the
dissolution of cobalt, since the value of lg([Sn2+]/[Co2+]) is equal to 4.85, that is, in the studied
solution the concentration of ions [Co2+] >> [Sn2+]. According to the Pourbaix diagram of the cobalt
water and tin water systems [23], in the range of values of stationary electrode potentials E2 and
E3, equal to, depending on the tin content in the tin-cobalt alloy, 0.02 0.08 V and 0.23 0.34 V
(table) in a 0.1 mol∙l-1 KOH solution (pH 12.7), a stable hydroxide film consisting of cobalt
hydroxide Co(OH)2 is formed on the surface of the coatings. The dissolution of cobalt with the
formation of hydroxide Co(OH)2 most likely occurs by an electrochemical mechanism according to
the reaction:
Co + 2H2O = Co(OH)2 + 2H+ + 2e, Е4 = 0.095 0.0581pH (4)
The steady-state electrode potential of reaction (4) under these conditions (pH 12.7) is
0.643V. The formation of a poorly soluble compound of hydroxide Co(OH)2 (SE(solubility
equilibrium) = 2.5 10-16) on the surface of the tin-cobalt alloy leads to passivation of the coating
surface and, consequently, to stabilization of the steady-state potential of the electrode. Tin in the
tin-cobalt alloy in 0.1 mol∙l-1 KOH solution (pH 12.7) is practically insoluble. The resulting
hydrogen ions are then reduced on tin. It can be assumed that the processes of formation and growth
over time of the hydroxide layer of cobalt(II) on the alloy surface are accompanied by changes in
other characteristics of the coatings, such as, the resistance of the coating, the capacity of the double
electric layer and the value of the specific surface. The dependence of the coating resistance
measured by impedance spectroscopy on the current density of its production and the holding time
in a 0.1 mol∙l-1 KOH solution is shown in Fig. 5a, from which it is evident that the coating
corrosion resistance decreases with increasing current density and depends insignificantly on the
holding time of the sample in the solution. At the same time, the coating corrosion resistance Rz
increases with increasing tin content in the alloy (Fig. 5b) and is practically independent of the
holding time in a 0.1 mol∙l-1 KOH solution. Obviously, such a dependence of the coating corrosion
On samples of tin-cobalt alloy with a tin
content of 33.3 at. %, obtained at a deposition
current density of 7.5 mA∙cm-2, the Nyquist and
Bode dependences have a similar character.
In this case, only the numerical values of the
parameters of the equivalent impedance cir-
cuit change: the contribution of the hydroxide
layer resistance to the total corrosion resistance
of such films is insignificant (< 5%). Based on
the equality of the values of the stationary elec-
trode potentials of reactions (2) and (3), we
can write the reactions:
Sn = Sn 2+ + e−,
Е2 = − 0.136 + 0.0291lg [Sn2+], (2)
Co = Co2+ + e−,
Е3 = − 0.277 + 0.0291lg [Co 2+], (3)
which can occur on the surface of a tin-cobalt
alloy in a 0.1 mol∙L-1 KOH solution (pH 12.7),
it can be shown that under these conditions,
corrosion of the tin-cobalt alloy coating occurs
due to the dissolution of cobalt, since the value
of lg ([Sn2+]/[Co2+]) is equal to −4.85, that is, in
the studied solution the concentration of ions
[Co2+] >> [Sn2+]. According to the Pourbaix
diagram of the cobalt − water and tin − water
systems [23], in the range of values of statio
nary electrode potentials E2 and E3, equal to,
depending on the tin content in the tin-cobalt
alloy, −0.02 −0.08 V and −0.23 −0.34 V (tab
le) in a 0.1 mol∙l-1 KOH solution (pH 12.7), a
stable hydroxide film consisting of cobalt hy-
droxide Co(OH)2 is formed on the surface of
the coatings. The dissolution of cobalt with the
formation of hydroxide Co(OH)2 most likely
occurs by an electrochemical mechanism ac-
cording to the reaction:
Co + 2H2O = Co(OH)2 + 2H+ + 2e−,
Е4 = 0.095 − 0.0581pH (4)
The steady-state electrode potential of re-
action (4) under these conditions (pH 12.7)
is −0.643 V. The formation of a poorly soluble
compound of hydroxide Co(OH)2 (SE(solubi
lity equilibrium) = 2.5 10-16) on the surface of the
tin-cobalt alloy leads to passivation of the coat-
ing surface and, consequently, to stabilization
of the steady-state potential of the electrode.
Tin in the tin-cobalt alloy in 0.1 mol∙l-1 KOH
8 ISSN 2708-129X. Укр. хім. журн., 2025
SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS.PHISICAL CHEMISTRY
solution (pH 12.7) is practically insoluble. The
resulting hydrogen ions are then reduced on
tin. It can be assumed that the processes of for-
mation and growth over time of the hydroxide
layer of cobalt (II) on the alloy surface are ac-
companied by changes in other characteris-
tics of the coatings, such as, the resistance of
the coating, the capacity of the double electric
layer and the value of the specific surface. The
dependence of the coating resistance measu
red by impedance spectroscopy on the cur-
rent density of its production and the holding
time in a 0.1 mol∙l-1 KOH solution is shown in
Fig. 5a, from which it is evident that the coating
corrosion resistance decreases with increasing
current density and depends insignificantly on
the holding time of the sample in the solution.
At the same time, the coating corrosion resis
tance Rz increases with increasing tin content in
the alloy (Fig. 5b) and is practically independ-
ent of the holding time in a 0.1 mol∙l-1 KOH
solution. Obviously, such a dependence of the
coating corrosion resistance Rz on the current
density is due to a decrease in the tin content
in the coating with increasing current density.
Holding tin-cobalt alloy coatings in an al-
kaline electrolyte leads to an increase in the
corrosion resistance of the electrode. This is
accompanied by a shift in the steady-state po-
tential to more positive values.
5
5
resistance Rz on the current density is due to a decrease in the tin content in the coating with
increasing current density.
jk , mA.cm-2
2.5 3.0 3.5 4.0 4.5 5.0 5.5 6.0 6.5
R z
, k
O
hm
0
40
80
120
160
200
2
1
Sn, at. %
30 35 40 45 50 55 60 65 70
R z
, k
O
hm
0
40
80
120
160
200
1
2
a b
Fig. 5. Dependence of corrosion resistance of tin-cobalt alloy coatings on current density (a) and tin content
in the alloy (b); holding time in 0.1 mol∙l-1 KOH solution, min.: 20 (1), 40 (2).
Holding tin-cobalt alloy coatings in an alkaline electrolyte leads to an increase in the corrosion
resistance of the electrode. This is accompanied by a shift in the steady-state potential to more
positive values.
Table 1.
Electrocatalytic and corrosion characteristics of tin-cobalt alloys.
Sn, аt.% Еst, V j = 10, V RZ , kOhm lgjcorr, А∙cm-2
66.7 -0.34 1.4 150 -7.35
40.0 -0.36 0.8 71 -6.15
33.3 -0.23 0.6 46 -5.78
The corrosion current of tin-cobalt alloy coatings decreases from 1.6∙10-6 to 4.5∙10-8 A∙cm-2
as the tin content increases, while the overvoltage of hydrogen ion reduction increases. Thus, an
increase in the cobalt content leads to an increase in the electrocatalytic properties of the alloy in the
hydrogen evolution reaction, and an increase in the tin content leads to an improvement in the
corrosion properties of the alloy.
CONCLUSIONS. Tin-cobalt alloy coatings were synthesized from a polyligand citrate-
chloride electrolyte with a tin content of 5-85 wt. Since the deposition of tin (II) into a tin-cobalt
alloy from a citrate-chloride electrolyte is limited by the preceding chemical reaction of dissociation
of polyligand electrochemically inactive complexes [SncitCl2]3–, which makes it possible to
influence the chemical composition and functional properties of the resulting coatings by selecting
the ratio of the electrolyte components and the deposition conditions. The surface morphology was
studied using EDS and XRD methods, and the phase composition of the tin-cobalt alloy coatings
was determined depending on the conditions of their preparation. It was found that with an increase
in current density, the phase composition of the coating’s changes. An increase in the tin content in
the alloy improves the quality of the coatings, increases their corrosion resistance and reduces the
electrocatalytic activity in the reaction of hydrogen ion reduction in an alkaline medium. The
dynamics of the change in the parameters of the equivalent impedance circuit on tin-cobalt alloy
coatings in 0.1 mol l-1 KOH solution was studied, which is associated with the formation of a
hydroxide layer on the coating surface. The corrosion current decreases with increasing tin content
in the alloy. It was found that the overvoltage of hydrogen evolution is lower, the higher the
corrosion current, which can be a criterion for assessing the catalytic activity of the electrode.
a b
Fig. 5. Dependence of corrosion resistance of tin-cobalt alloy coatings on current density (a)
and tin content in the alloy (b); holding time in 0.1 mol∙l-1 KOH solution, min.: 20 (1), 40 (2).
Table 1.
Electrocatalytic and corrosion characteristics of tin-cobalt alloys.
Sn, аt.% Еst , V η j = 10 , V RZ , kOhm lgjcorr , А∙cm-2
66.7 -0.34 1.4 150 -7.35
40.0 -0.36 0.8 71 -6.15
33.3 -0.23 0.6 46 -5.78
9https://ucj.org.ua
V.M. Nikitenko, T.V. Maltseva, E.A. Babenkov, V.S. Kublanovsky UCJ № 1 / Vol. 91
The corrosion current of tin-cobalt alloy co
atings decreases from 1.6∙10-6 to 4.5∙10-8 A∙cm-2
as the tin content increases, while the overvol
tage of hydrogen ion reduction increases. Thus,
an increase in the cobalt content leads to an in-
crease in the electrocatalytic properties of the
alloy in the hydrogen evolution reaction, and
an increase in the tin content leads to an im-
provement in the corrosion properties of the
alloy.
CONCLUSIONS. Tin-cobalt alloy coat-
ings were synthesized from a polyligand cit-
rate-chloride electrolyte with a tin content of
5-85 wt. Since the deposition of tin (II) into a
tin-cobalt alloy from a citrate-chloride elec-
trolyte is limited by the preceding chemical
reaction of dissociation of polyligand electro-
chemically inactive complexes [SncitCl2]
3–,
which makes it possible to influence the chemi
cal composition and functional properties of
the resulting coatings by selecting the ratio of
the electrolyte components and the deposition
conditions. The surface morphology was stu
died using EDS and XRD methods, and the
phase composition of the tin-cobalt alloy coa
tings was determined depending on the condi-
tions of their preparation. It was found that with
an increase in current density, the phase com-
position of the coating’s changes. An increase
in the tin content in the alloy improves the
quality of the coatings, increases their corro-
sion resistance and reduces the electrocatalytic
activity in the reaction of hydrogen ion reduc-
tion in an alkaline medium. The dynamics of
the change in the parameters of the equivalent
impedance circuit on tin-cobalt alloy coatings
in 0.1 mol l-1 KOH solution was studied, which
is associated with the formation of a hydrox-
ide layer on the coating surface. The corrosion
current decreases with increasing tin content
in the alloy. It was found that the overvoltage
of hydrogen evolution is lower, the higher the
corrosion current, which can be a criterion for
assessing the catalytic activity of the electrode.
This work was performed with the fi-
nancial support from the National
Academy of Sciences of Ukraine with-
in the state budget theme “Finishing of
materials in order to give them unique
functional properties” 0123U100650.
СИНТЕЗ, КОРОЗІЙНІ ТА ЕЛЕКТРОКАТАЛІТИЧНІ
ВЛАСТИВОСТІ ПОКРИТТІВ СПЛАВОМ
ОЛОВО – КОБАЛЬТ
В. М. Нікітенко*, Т. В. Мальцева,
Є. А. Бабенков, В. С. Кублановський
Інститут загальної і неорганічної хімії
ім. В. І. Вернадського НАН України,
просп. Академіка Палладіна, 32/34, Київ
03142, Україна
*vasylnikitenko@gmail.com
Синтезовано покриття сплаву олово –
кобальт із полілігандного цитратно-хло-
ридного електроліту. Вміст олова в покрит-
тях сплаву олово – кобальт залежить від па-
раметрів їхнього осадження і змінюється в
широкому діапазоні від 5.0 до 85.0 мас. %.
Осадження олова (II) у сплав олово – ко-
бальт із цитратно-хлоридного електроліту
лімітується попередньою хімічною реакці-
єю дисоціації полілігандних електрохімічно
неактивних комплексів [SncitCl2]
3−-, що доз-
воляє шляхом вибору співвідношення ком-
понентів електроліту та умов осадження
10 ISSN 2708-129X. Укр. хім. журн., 2025
SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS.PHISICAL CHEMISTRY
впливати на хімічний склад і функціональ-
ні властивості одержуваних покриттів. Ме-
тодами EDS і XRD досліджено морфологію
поверхні, встановлено хімічний та фазовий
склад покриттів олово – кобальт залежно
від умов їхнього отримання. Збільшення
вмісту олова в сплаві покращує якість по-
криттів, підвищує їхній корозійний опір і
зменшує електрокаталітичну активність у
реакції відновлення іонів водню в лужному
середовищі.
Вивчено динаміку зміни параметрів
еквівалентної схеми імпедансу на покрит-
тях сплавом олово – кобальт зі вмістом 33.3,
40.0 і 66.7 ат. % олова в 0.1 моль·л-1 розчині
KOH. Показано, що динаміка зумовлена
утворенням гідроксидного шару кобальту
(II) на поверхні покриттів. Методом імпе-
дансної спектроскопії підтверджено утво-
рення гідроксидного шару на поверхні по-
криттів у лужному середовищі. Виходячи з
рівності значень стандартних електродних
потенціалів олова (II) та кобальту (II) у
водних розчинах, показано, що за цих умов
корозія покриття сплаву олово – кобальт
відбувається внаслідок розчинення кобаль-
ту з утворенням на поверхні сплаву стійкої
плівки гідроксиду кобальту Co(OH)2. Із
вольт-амперних залежностей розраховано
показники корозійної стійкості та електро-
каталітичної активності покриттів у реак-
ції відновлення іонів водню в лужному се-
редовищі. Показано, що витримка покрит-
тів у 0.1 моль·л-1 розчині KOH призводить
до збільшення їхнього корозійного опору й
зменшення струму корозії. При підвищенні
вмісту олова в сплаві струм корозії зменшу-
ється від 3∙10-6 до 1∙10-8 А·см-2. Перенапруга
реакції виділення водню при струмі реакції
10 мА·см-2 зростає з підвищенням вмісту
олова в сплаві від 0.6 В до 1.4 В. Встановле-
но антибатну залежність перенапруги виді-
лення водню на покриттях сплаву олово –
кобальт від струму корозії. Перенапруга
тим менша, що більший струм корозії.
Ключові слова: електроосадження, оло-
во-кобальтовий сплав, цитратно-хлорид-
ний електроліт, корозійна стійкість, елек-
трокаталітична активність.
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Стаття надійшла 02.10.2024.
|
| id | oai:ojs2.1444248.nisspano.web.hosting-test.net:article-705 |
| institution | Ukrainian Chemistry Journal |
| keywords_txt_mv | keywords |
| language | English |
| last_indexed | 2026-07-23T01:12:33Z |
| publishDate | 2025 |
| publisher | V.I.Vernadsky Institute of General and Inorganic Chemistry |
| record_format | ojs |
| resource_txt_mv | ucjorgua/d5/03297054861073aa93916509215648d5.pdf |
| spelling | oai:ojs2.1444248.nisspano.web.hosting-test.net:article-7052026-07-22T08:23:55Z SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS Nikitenko, Vasyl Maltseva, Tetiana Babenkov, Eugen Kublanovsky, Valeriy electrodeposition, tin-cobalt alloy, citrate-chloride electrolyte, corrosion resistance, electrocatalytic activity. Tin-cobalt alloy coatings with a tin content of 5–85 wt.% were synthesized from a polyligand citrate-chloride electrolyte. The surface morphology and composition of tin-cobalt alloy coatings depending on the conditions of their production were studied using EDS and XRD methods. The dynamics of changes in the parameters of the equivalent impedance circuit on tin-cobalt alloy coatings in 0.1 mol∙l-1 KOH solution is determined by the process of formation of a cobalt (II) hydroxide layer on the coating surface. The parameters of corrosion resistance and electrocatalytic activity of the coatings in the reaction of hydrogen evolution were calculated from the stationary voltammetry dependences. The corrosion currents on tin-cobalt alloy coatings with a tin content of 33–85 wt.% are about 10-6–10-8 A∙cm-2. An inverse dependence of the hydrogen evolution overvoltage on tin-cobalt alloy coatings on the corrosion current was established. V.I.Vernadsky Institute of General and Inorganic Chemistry 2025-02-25 Article Article Physical chemistry Физическая xимия Фізична xімія application/pdf https://ucj.org.ua/index.php/journal/article/view/705 10.33609/2708-129X.91.1.2025.3-11 Ukrainian Chemistry Journal; Vol. 91 No. 1 (2025): Ukrainian Chemistry Journal; 3-11 Украинский химический журнал; ##issue.vol## 91 ##issue.no## 1 (2025): Ukrainian Chemistry Journal; 3-11 Український хімічний журнал; Том 91 № 1 (2025): Ukrainian Chemistry Journal; 3-11 2708-129X 2708-1281 en https://ucj.org.ua/index.php/journal/article/view/705/354 Copyright (c) 2025 Vasyl Nikitenko, Tetiana Maltseva, Eugen Babenkov, Valeriy Kublanovsky https://creativecommons.org/licenses/by-nc/4.0 |
| spellingShingle | Nikitenko, Vasyl Maltseva, Tetiana Babenkov, Eugen Kublanovsky, Valeriy SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS |
| title | SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS |
| title_full | SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS |
| title_fullStr | SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS |
| title_full_unstemmed | SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS |
| title_short | SYNTHESIS, CORROSION AND ELECTROCATALYTIC PROPERTIES OF TIN-COBALT ALLOY COATINGS |
| title_sort | synthesis, corrosion and electrocatalytic properties of tin-cobalt alloy coatings |
| topic_facet | electrodeposition tin-cobalt alloy citrate-chloride electrolyte corrosion resistance electrocatalytic activity. |
| url | https://ucj.org.ua/index.php/journal/article/view/705 |
| work_keys_str_mv | AT nikitenkovasyl synthesiscorrosionandelectrocatalyticpropertiesoftincobaltalloycoatings AT maltsevatetiana synthesiscorrosionandelectrocatalyticpropertiesoftincobaltalloycoatings AT babenkoveugen synthesiscorrosionandelectrocatalyticpropertiesoftincobaltalloycoatings AT kublanovskyvaleriy synthesiscorrosionandelectrocatalyticpropertiesoftincobaltalloycoatings |