Bakhit 2014
Bakhit 2014
a r t i c l e i n f o a b s t r a c t
Article history: Corrosion resistance of Ni–Co alloy and Ni–Co/SiC nanocomposite coatings electrodeposited in a modified
Received 24 December 2013 Watts bath using sediment codeposition (SCD) technique was evaluated by potentiodynamic polariza-
Received in revised form 5 April 2014 tion measurements in the 3.5% NaCl solution and studied as a function of deposition conditions In order
Accepted 6 April 2014
to characterize the morphology, chemical and phase compositions of the coatings, scanning electron
Available online xxx
microscopy (SEM), energy dispersive X-ray spectrometry (EDS) and X-ray diffraction (XRD) were uti-
lized, respectively. It was observed that the cobalt content in the Ni–Co alloy coatings was increased
Keywords:
through an anomalous behavior by increasing the cobalt concentration in the electrolyte. The highest
Nanocomposite coatings
Sediment codeposition
percentage of SiC nano-particles (8.1 vol.%) in the Ni–Co/SiC nanocomposite coatings was achieved at
Microstructure 3 A/dm2 deposition current density and 5 g/l particle concentration. SEM and EDS analysis illustrated
Corrosion resistance that SiC nano-particles were distributed uniformly throughout the nanocomposite coatings. The poten-
tiodynamic polarization tests indicated that the corrosion resistance of the Ni–Co alloy coatings was
varied as a function of the cobalt content, and the corrosion resistance of the Ni–Co/SiC nanocompos-
ite coatings was markedly higher than the corrosion resistance of the Ni–Co alloy coatings. Among the
studied coatings, Ni–Co/SiC nanocomposite coatings containing 8.1 vol.% SiC nano-particles exhibited the
best corrosion resistance.
© 2014 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.apsusc.2014.04.037
0169-4332/© 2014 Elsevier B.V. All rights reserved.
Please cite this article in press as: B. Bakhit, et al., Corrosion resistance of Ni–Co alloy and Ni–Co/SiC nanocomposite coatings electrode-
posited by sediment codeposition technique, Appl. Surf. Sci. (2014), http://dx.doi.org/10.1016/j.apsusc.2014.04.037
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Table 1
Ni–Co alloy and Ni–Co/SiC nanocomposite electrolyte compositions.
Please cite this article in press as: B. Bakhit, et al., Corrosion resistance of Ni–Co alloy and Ni–Co/SiC nanocomposite coatings electrode-
posited by sediment codeposition technique, Appl. Surf. Sci. (2014), http://dx.doi.org/10.1016/j.apsusc.2014.04.037
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Cobalt content in the alloy coatings (Wt.%)
600
50 0 Wt.% Co
400 17 Wt.% Co
45 42 Wt.% Co
200
40
Potential (mV)
0
35
-200
30
-400
25
-600
20
-800
15
-1000
10
-1200
5 -1400
-2 -1 0 1 2 3 4 5 6
0
logi (i in µA.cm-2)
0 5 10 15 20 25 30 35 40 45 50 55
Cobalt concentration in the electrolyte (g/l) Fig. 3. The potentiodynamic polarization curves of the Ni–Co alloy coatings as a
function of the cobalt content.
Fig. 2. The cobalt content in the Ni–Co alloy coatings as a function of the cobalt
concentration in the electrolyte. Co. Therefore, Ni–17Co alloy coatings exhibit the lowest corrosion
rate.
The corrosion resistance of alloy coatings may be correlated to
coatings and ±250 mV for the nanocomposite coatings with respect simultaneous effects of several important factors such as chemi-
to the Eocp by 1 mV/s sweeping rate. The corrosion current den- cal composition, phase structure, preferred orientation, and grain
sity was calculated according to the Stern–Geary equation from size. In order to explain the chemical composition influence of
the polarization measurement [30]: alloy coatings, it was shown that alloying can affect the corrosion
ˇa × ˇc resistance by changing the nobility of materials [35]. Since cobalt
icorr = (2) is more active than nickel, it is expected that the electrochemi-
2303 × Rp ˇa + ˇc
cal activity of the Ni–Co alloy coatings to be greater than pure
where icorr is the corrosion current density, Rp is the polarization Ni coatings, particularly by increasing the cobalt content [36]. The
resistance, ˇa and ˇc are the anodic and cathodic Tafel slopes, other factor which has a major impact on the corrosion behavior of
respectively. In addition, the polarization resistance was calculated alloy coatings is microstructure. In general, two-phase structures
according to the following equation: are less corrosion resistant than single-phase structures because
galvanic cells can be formed between phases (along grain bound-
dE E aries) and facilitate corrosion attacks, especially when phases have
Rp =
di E=Eocp
≈
i
(3)
different nobilities. Moreover, the corrosion resistance of face cen-
tered cubic (fcc) phases is higher than the corrosion resistance
3. Results of base centered cubic (bcc) phases due to their higher packing
factor. According to obtained results, the phase structure of the
3.1. Ni–Co alloy coatings studied Ni–Co alloy coatings, which was fcc single-phase solid solu-
tion, was not changed by the variation of the cobalt content in the
3.1.1. Electrodeposition coatings. Therefore, the phase structure had an approximately con-
Fig. 2 shows the variation of the cobalt content in the Ni–Co alloy stant influence on the corrosion properties of the studied Ni–Co
coatings as a function of the cobalt concentration in the electrolyte. alloy coatings.
There is a substantial upward trend in the cobalt content from 0 to The preferred orientation is another factor playing a signifi-
45 wt.% Co. The cobalt content in the alloy coatings is significantly cant role in corrosion resistance of coatings. Ramanauskas et al.
higher than the cobalt concentration in the electrolyte. According [37] suggested that the higher corrosion resistance of Zn–Ni alloys
to Brenner [31], this behavior is classified as an anomalous codepo- is owing to the predominant presence of crystallographic planes
sition. The anomalous codeposition of the Ni–Co alloy coatings was with a higher packing density. Fig. 4 shows the influence of the
explained by different mechanisms such as depletion of the diffu- cobalt content on the relative texture coefficient (RTC) of (1 1 1),
sion layer due to the preferential deposition of cobalt cations [32], (2 0 0), and (2 2 0) planes in the studied Ni–Co alloy coatings. Since
two-step codeposition of cobalt cations and decreasing the nickel a preferred orientation of a (hkl) plane is shown by the values of
deposition in the second step [33], and formation and adsorption of RTC(hkl) ≥ 33.33%, it can be seen that the preferred orientation in all
metal hydroxides because of a local increase in the pH, and higher studied Ni–Co alloy coatings is (1 1 1). However, the RTC(hkl) per-
adsorption of cobalt hydroxides [34]. centage of the studied alloy coatings is changed as a function of
the cobalt content. Although the RTC of (2 2 0) planes, which have a
3.1.2. Corrosion properties low packing density in fcc phase structures, is increased noticeably
Fig. 3 illustrates the potentiodynamic polarization curves of the from 0.54% to 28%, the RTC of (2 0 0) planes is approximately halved
Ni–Co alloy coatings. There is no passivation tendency over the from 38% to 16% by increasing the cobalt content in the deposits.
swept range of potentials. The electrochemical data extracted from Moreover, the RTC of (1 1 1) planes, which have the highest packing
the polarization curves are also summarized in Table 2. The low- density in fcc phase structures, is increased by 15% between 0 and
est corrosion current density (icorr ) and the highest polarization 38 wt.% Co. Yet, there is a collapse of 20% in the RTC of (1 1 1) planes
resistance (Rp ) are related to an alloy coating containing 17 wt.% after reaching a peak of 76%. This figure illustrates that the amount
Please cite this article in press as: B. Bakhit, et al., Corrosion resistance of Ni–Co alloy and Ni–Co/SiC nanocomposite coatings electrode-
posited by sediment codeposition technique, Appl. Surf. Sci. (2014), http://dx.doi.org/10.1016/j.apsusc.2014.04.037
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Table 2
Electrochemical data extracted from the potentiodynamic polarization curves of the Ni–Co alloy coatings.
Coating Eocp (mV) ˇa (mV/dec) ˇc (mV/dec) Ecorr (mV) icorr (A/cm2 ) Rp (k.cm2 )
of close-packed (1 1 1) planes in the Ni–Co coatings is decreased by properties, which were attained in the previous work at 50 g/l
a further increase in the cobalt content while the amount of (2 2 0) cobalt [23], as well as the highest corrosion properties simulta-
planes, which are not dense, is increased. Hence, it can be deduced neously.
that a part of the higher corrosion resistance of the Ni–17Co alloy The effect of both particle concentration and deposition cur-
coatings is resulted from the presence of an fcc phase with predom- rent density on incorporation of SiC nano-particles is shown in
inant close-packed (1 1 1) planes and the low percentage of (2 2 0) Fig. 5. The SiC nano-particle content in the deposits is decreased by
planes. increasing the particle concentration in the bath. Although there
On the other hand, the grain size of coatings has a considerable is a gradual decrease in the particle content of nanocomposite
effect on the corrosion rate because the grain boundaries are prone coatings deposited at 1 and 4 A/dm2 , the percentage of incorporated
to corrosion attacks, and the corrosion resistance is decreased by particles in nanocomposite coatings deposited at 2 and 3 A/dm2
increasing the density of grain boundaries [38,39]. The grain size of shows a drop between 10 g/l and 15 g/l particle concentration. This
the studied alloy coatings was obtained from XRD peak broaden- decreasing trend can be correlated with nanoparticle agglomera-
ing analysis and calculated from integral width of the (2 0 0) peaks tion [23].
using the Scherrer equation [40] after excluding the instrumen- The transfer rate of suspended particles in the electrolyte is
tal broadening. Results show that the grain size of the coatings related to the hydrodynamic forces resulted from the electrolyte
is reduced strikingly from 48 nm in Ni–17Co coatings to 26 nm in agitation rate and the electrophoretic forces resulted from the
Ni–27Co coatings and then, 15 nm in Ni–42Co coatings. The grain deposition current density. At a constant agitation rate of the elec-
size reduction in the Ni–Co alloy coatings was linked to the forma- trolyte (350 rpm), the SiC nano-particle content shows an upward
tion of metal hydroxides in the electrolyte which are able to absorb trend with a peak at 3 A/dm2 and then a decrease by increasing
on active growth centers, block them and act as grain refiners [41]. the deposition current density. This might be described through a
As a consequence, besides the negative effect of the presence of competitive process between the reduction rate of metallic cations
the low density (2 2 0) planes, another reason for decreasing the and the incorporation rate of suspended particles. At low deposi-
corrosion resistance of the Ni–Co alloy coatings containing more tion current densities, the rate of cation reduction is higher than
than 17 wt.% Co could be related to their grain sizes. Therefore, the rate of particle incorporation. Then, the particle incorporation
higher corrosion resistance of the Ni–17Co alloy coatings is linked rate is increased moderately by raising the deposition current den-
to a moderate grain size, a single-phase fcc structure, and a relative sity until reaching a peak. After that, the reduction rate of metallic
predominance of (1 1 1) preferred orientation. cations is increased again at higher deposition current densities.
2
SiC nano-particle content in the
1 A/dm
2
2 A/dm
2
100 8 3 A/dm
(111) 2
Relative texture coefficient (RTC)
4 A/dm
90 (200)
(220)
80
7
70
60
6
50
40
30 5
20
10 4
0 5 10 15 20
0 8 17 27 38 42 SiC nano-particle concentration
Cobalt content (Wt.%) in the electrolyte (g/l)
Fig. 4. The relative texture coefficient (RTC) percentage of (1 1 1), (2 0 0) and (2 2 0) Fig. 5. The particle content in the Ni–Co/SiC nanocomposite coatings as a function
planes in the Ni–Co alloy coatings as a function of the cobalt content in the deposits. of the particle concentration and deposition current density.
Please cite this article in press as: B. Bakhit, et al., Corrosion resistance of Ni–Co alloy and Ni–Co/SiC nanocomposite coatings electrode-
posited by sediment codeposition technique, Appl. Surf. Sci. (2014), http://dx.doi.org/10.1016/j.apsusc.2014.04.037
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Fig. 6. The surface morphology of the Ni–Co/SiC nanocomposite coatings deposited at different deposition current densities of (a and e) 1 A/dm2 , (b and f) 2 A/dm2 , (c and
g) 3 A/dm2 , and (d and h) 4 A/dm2 at two different magnifications: 15k× and 30k×.
uniform distribution, the number of agglomerated particles in the Additionally, EDS spectra in Fig. 7 reveal that the intensity of Ni
surface of nanocomposite coatings deposited at 2 and 3 A/dm2 is and Co peaks is lengthened by increasing the deposition current
higher than nanocomposite coatings deposited at 1 and 4 A/dm2 . density. This can be an appropriate proof for the fact that the reduc-
The pyramidal morphology in Fig. 6d and h proves a rapid fall in tion rate of metallic cations is increased as a function of deposition
the particle content because of increasing the reduction rate of current density. In order to study the chemical composition and
metallic cations. Furthermore, the size of agglomerated particles particle distribution uniformity across the nanocomposite coating
is approximately comparable in all studied coatings. Fig. 7 shows thickness, the elemental line scans of Ni, Co, Si and Cu elements
the surface morphologies and Si dot-map patterns of the Ni–Co/SiC are represented on a cross sectional SEM image (Fig. 8). There is
nanocomposite coatings deposited at different current densities. a fairly uniform distribution of the elements approving the SiC
The dot-map patterns confirm that SiC nano-particles have a uni- nano-particle distribution uniformity through the thickness of the
form distribution over the surface of the nanocomposite coatings. nanocomposite coatings. Moreover, the SEM image of a Ni–Co/SiC
Fig. 7. The dot-map and spectra patterns of the Ni–Co/SiC nanocomposite coatings deposited at different deposition current densities of (a, e and i) 1 A/dm2 , (b, f and j)
2 A/dm2 , (c, g and k) 3 A/dm2 , and (d, h and l) 4 A/dm2 .
Please cite this article in press as: B. Bakhit, et al., Corrosion resistance of Ni–Co alloy and Ni–Co/SiC nanocomposite coatings electrode-
posited by sediment codeposition technique, Appl. Surf. Sci. (2014), http://dx.doi.org/10.1016/j.apsusc.2014.04.037
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Fig. 8. Line scan element curves of the Ni–Co/SiC nanocomposite coating (3 A/dm2
and 5 g/l particle concentration).
Fig. 9. Cross sectional image of the Ni–Co/SiC nanocomposite coating (3 A/dm2 and
15 g/l particle concentration).
800
Intensity (cps)
(111)
600
400
(220)
(200)
200
(311)
(222)
Ni-42Co
-2
Ni-Co/SiC, 1 A.dm
-2
Ni-Co/SiC, 2 A.dm
-2
Ni-Co/SiC, 3 A.dm
-2
Ni-Co/SiC, 4 A.dm
Fig. 10. X-ray diffraction patterns of the Ni–42Co alloy and the Ni–Co/SiC nanocomposite coatings deposited at different current densities.
Please cite this article in press as: B. Bakhit, et al., Corrosion resistance of Ni–Co alloy and Ni–Co/SiC nanocomposite coatings electrode-
posited by sediment codeposition technique, Appl. Surf. Sci. (2014), http://dx.doi.org/10.1016/j.apsusc.2014.04.037
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Table 3
Electrochemical data extracted from the potentiodynamic polarization curves of the Ni–Co/SiC nanocomposite coatings as a function of the deposition current density.
Deposition current density (A/dm2 ) Co (wt.%) SiC (vol.%) Eocp (mV) ˇa (mV/dec) ˇc (mV/dec) Ecorr (mV) icorr (A/cm2 ) Rp (k.cm2 )
-160 100
Ni-Co/SiC 0 g/l nano SiC
Ni-42Co 5 g/l nano SiC
-200 0 10 g/l nano SiC
15 g/l nano SiC
-240 20 g/l nano SiC
-100
Potential (mV)
Potential (mV)
-280
-200
-320
-300
-360
-400
-400
-500
-440
-4 -3 -2 -1 0 1 2 3 4
-480
0 10 20 30 40 50 60 70 logi (i in µA.cm-2)
Time (min) Fig. 13. The potentiodynamic polarization curves of the Ni–Co/SiC nanocomposite
coatings as a function of the particle concentration in the electrolyte.
Fig. 11. The open circuit potential (Eocp ) variation of a Ni–Co/SiC nanocomposite
coating and Ni–42Co alloy coating in the 3.5% NaCl corrosive medium.
coatings containing 55 wt.% Co and 8.1 vol.% SiC nano-particles.
Therefore, the Ni–Co/SiC nanocomposite coatings electrodeposited
200 at 3 A/dm2 exhibits better corrosion resistance.
2
1 A/dm
2 Fig. 13 shows the potentiodynamic polarization curves of the
100 2 A/dm
3 A/dm
2 Ni–Co/SiC nanocomposite coatings electrodeposited at different
4 A/dm
2 particle concentrations in the electrolyte. Based on the electro-
0
chemical data extracted from these curves (Table 4), the icorr for
Potential (mV)
Table 4
Electrochemical data extracted from the potentiodynamic polarization curves of the Ni–Co/SiC nanocomposite coatings as a function of the particle concentration in the
electrolyte.
SiC particle concentration (g/l) Co (wt.%) SiC (vol.%) Eocp (mV) ˇa (mV/dec) ˇc (mV/dec) Ecorr (mV) icorr (A/cm2 ) Rp (k.cm2 )
Please cite this article in press as: B. Bakhit, et al., Corrosion resistance of Ni–Co alloy and Ni–Co/SiC nanocomposite coatings electrode-
posited by sediment codeposition technique, Appl. Surf. Sci. (2014), http://dx.doi.org/10.1016/j.apsusc.2014.04.037
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electrolyte enhances particle incorporation, and it causes improv- enhanced significantly the corrosion resistance of the Ni–Co alloy
ing the properties of nanocomposite coatings [21]. Therefore, coatings. The highest corrosion resistance was obtained for the
the chemical composition of the Ni–Co matrix has two different Ni–Co/SiC nanocomposite coatings containing 8.1 vol.% SiC nano-
detrimental and beneficial effects on the corrosion resistance of particles. The corrosion properties of the nanocomposite coatings
Ni–Co/SiC composite coatings. Besides the chemical composition, were discussed based on the chemical composition of the coatings,
phase structure is also another considerable factor affecting the particle content, formation of corrosion micro-cells, diminishing
corrosion properties of composite coatings. The XRD patterns show of the effective metallic area, and increasing and hindering of the
that the phase structure of the alloy matrix is not changed by parti- corrosion paths.
cle incorporation. Accordingly, a part of the corrosion resistance of
the studied coatings can be related to the single-phase fcc structure
of the Ni–Co matrix. Moreover, the most major impact of matrix in
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posited by sediment codeposition technique, Appl. Surf. Sci. (2014), http://dx.doi.org/10.1016/j.apsusc.2014.04.037
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Please cite this article in press as: B. Bakhit, et al., Corrosion resistance of Ni–Co alloy and Ni–Co/SiC nanocomposite coatings electrode-
posited by sediment codeposition technique, Appl. Surf. Sci. (2014), http://dx.doi.org/10.1016/j.apsusc.2014.04.037