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or O
2
ions are also formed.
The fact that all the three processes are represented by only
one loop could be attributed either to the overlapping of the
loops of processes, or to the assumption that one process dom-
inates and, therefore, excludes the other processes (Morad,
1999). The other explanation offered to the high frequency
capacitive loop is the oxide lm itself. The origin of the
0 200 400 600 800 1000 1200
0
200
400
600
800
1000
1200
-
Z
I
I
(
o
h
m
c
m
2
)
Z
l
(ohm cm
2
)
0.01M
0.1M
1.0M
Figure 3 Nyquist plot for 6063 aluminium alloy in different
concentrations of H
3
PO
4
at 30 C.
0 2 4 6 8 10 12 14 16
0
2
4
6
8
10
12
14
16
-
Z
"
(
o
h
m
c
m
2
)
Z' (ohm cm
2
)
0.05M
0.25M
0.5M
Figure 4 Nyquist plot for 6063 aluminium alloy in different
concentrations of NaOH at 30 C.
Table 3 Results of Tafel polarization studies and EIS studies of 6063 aluminium alloy in NaOH.
Tafel polarization EIS
NaOH (M) T (K) E
corr
(V vs. SCE) i
corr
(10
5
A cm
2
) b
a
(V dec
1
) b
c
(V dec
1
) t
corr
(mm y
1
) R
p
(X cm
2
) CPE (l F cm
2
)
0.05 303 1.55 40.4 4.84 4.86 4.40 101.8 66
308 1.56 46.9 4.87 4.83 5.11 82.5 72
313 1.57 52.6 5.21 5.31 5.73 80.2 75
318 1.58 57.2 4.83 5.33 6.23 77.3 79
323 1.59 59.8 4.45 5.44 6.51 75.6 85
0.25 303 1.57 209 5.04 4.84 22.78 24.9 76
308 1.59 244 4.90 4.92 26.59 18.3 84
313 1.60 281 5.11 4.47 30.62 17.3 96
318 1.61 307 4.80 4.70 33.46 15.0 107
323 1.62 331 4.93 4.73 36.07 14.4 114
0.5 303 1.59 326 4.92 4.71 35.53 12.2 83
308 1.60 374 4.92 4.91 40.76 11.5 95
313 1.61 424 5.03 4.88 46.21 9.9 101
318 1.62 437 4.67 4.84 47.63 9.7 111
323 1.63 455 4.92 4.96 49.59 8.3 123
4 P. Deepa, R. Padmalatha
Please cite this article in press as: Deepa, P., Padmalatha, R. Corrosion behaviour of 6063 aluminium alloy in acidic and in alkaline
media. Arabian Journal of Chemistry (2014), http://dx.doi.org/10.1016/j.arabjc.2013.07.059
inductive loop has often been attributed to the surface or bulk
relaxation of species in the oxide layer (Morad, 1999). The LF
inductive loop may be related to the relaxation process ob-
tained by adsorption and incorporation of phosphate ions
and hydroxide ions into the oxide lm (Lorenz and Mansfeld,
1981).
An equivalent circuit of nine elements depicted in Fig. 5a
was used to simulate the measured impedance data of the
6063 aluminium alloy, as shown in Fig. 5b. In this equivalent
circuit, R
s
is the solution resistance and R
t
is the charge trans-
fer resistance. R
L
and L represent the inductive elements. This
also consists of constant phase element; CPE (Q) in parallel to
the series capacitors C
1
and C
2
and series resistors R
1
, R
2
, R
L
and R
t
. R
L
is parallel with the inductor L. The polarization
resistance R
p
and double layer capacitance C
dl
are calculated
from Eqs. (2) and (3):
R
p
R
L
R
t
R
1
R
2
; 2
C
dl
C
1
C
2
: 3
The measured value of polarization resistance decreased
with increase while the CPE value increased with increasing
concentration of the phosphoric acid medium and sodium
hydroxide medium, indicating that the rate of corrosion in-
creased with increasing concentration of the phosphoric acid
medium and sodium hydroxide medium. This is in agreement
with the results obtained from potentiodynamic polarization
data.
3.3. Effect of temperature
The effect of temperature on the corrosion rate of the 6063 al-
loy was studied by measuring the corrosion rate at the temper-
ature range of 303323 K. Figs. 6 and 7 represent the
potentiodynamic polarization curves of 6063 aluminium alloy
in 1.0 M phosphoric acid medium and 0.5 M sodium hydride
medium at temperature range of 303323 K. Figs. 8 and 9
represent Nyquist plots for the same. From both gures it is
Figure 5 Equivalent circuit t for 6063 Al alloy in 1.0 M H
3
PO
4
at 30 C.
-6.5 -6.0 -5.5 -5.0 -4.5 -4.0 -3.5 -3.0 -2.5 -2.0 -1.5
-1.1
-1.0
-0.9
-0.8
-0.7
-0.6
-0.5
E
(
V
/
S
C
E
)
log i(Acm
-2
)
30
o
C
35
o
C
40
o
C
45
o
C
50
o
C
Figure 6 Tafel polarization curves for 6063 aluminium alloy at
different temperatures in 1 M H
3
PO
4
.
-5.5 -5.0 -4.5 -4.0 -3.5 -3.0 -2.5 -2.0 -1.5
-1.9
-1.8
-1.7
-1.6
-1.5
-1.4
-1.3
E
(
V
/
S
C
E
)
log i (A cm
-2
)
30
o
C
35
o
C
40
o
C
45
o
C
50
o
C
Figure 7 Tafel polarization curves for 6063 aluminium at
different temperatures in 0.5 M NaOH.
Corrosion behaviour of 6063 aluminium alloy 5
Please cite this article in press as: Deepa, P., Padmalatha, R. Corrosion behaviour of 6063 aluminium alloy in acidic and in alkaline
media. Arabian Journal of Chemistry (2014), http://dx.doi.org/10.1016/j.arabjc.2013.07.059
obvious that the corrosion rate increased with an increase in
temperature. This results in the rapid dissolution of the oxide
lm, thereby enhancing the corrosion rate. This is attributable
to the enhanced chemical lm dissolution due to enriched
phosphate ions, OH
4
ions at the
lm/solution interface. Thus with the increasing temperature
the oxide passive lm becomes thin, porous and less protective
as a result of dissolution of the lm by the electrolyte (Foley
and Nguyen, 1982).
The energy of activation of corrosion of 6063 aluminium
alloy was calculated from Arrhenius Eq. (4). The Arrhenius
plot (lnCR vs. 1/T) at all the concentrations of phosphoric
acid medium and sodium hydroxide medium is represented
in Figs. 10 and 11.
lnt
corr
B
E
a
RT
; 4
where B is a constant, R is the universal gas constant, and T is
the absolute temperature.
Enthalpy of activation (DH
a
) and entropy of activation
(DS
a
) were calculated from the transition state theory Eq. (5),
t
corr
RT
Nh
exp
DS
a
R
exp
DH
a
RT
5
where h is Planks constant and N is Avagadros number.
A plot of ln(t
corr
/T) vs 1/T gives a straight line with
slope = DH
a
/T and intercept = ln(R/Nh) +DS
a
/R. The
plots of ln(t
corr
/T) vs. 1/T for the corrosion of 6063 aluminium
alloy in the presence of different concentrations of phosphoric
acid medium and sodium hydroxide medium are shown in
Figs. 12 and 13.
The values of energies of activation, enthalpy of activation
and entropy of activation are listed in Tables 4 and 5.
As indicated in Table 4, except for 0.01 M phosphoric acid
medium, value of energy of activation is greater than
20 kJ mol
1
.
This suggested that at higher strengths of acid, the whole
process is controlled by surface reaction (El-Neami et al.,
1995). This phenomenon may be due to the fact that the
activation energy for the corrosion reaction is independent of
concentration polarization (Oguzie, 2007) and mainly due to
activation polarization. However, in case of sodium hydroxide
medium, energy of activation at all studied concentrations
was less than 20 kJ mol
1
and E
a
decreased with an
increase in sodium hydroxide medium concentration, which
is suggestive of concentration polarization as a main reaction
at electrodeelectrolyte interface.
The entropy of activation is large and negative. This implies
that the activated complex in the rate determining step repre-
sents association rather than dissociation, indicating that a de-
crease in disorder takes place, in going from reactant to the
activated complex (Trowsdale et al., 1996). The value of DS
a
decreased with an increase in acid concentration reveals that
dissolution of alloy is facilitated as the concentration of the
acid medium increases.
0 20 40 60 80 100 120
0
20
40
60
80
100
120
-
Z
I
I
(
o
h
m
c
m
2
)
Z
I
(ohm cm
2
)
30
o
C
35
o
C
40
o
C
45
o
C
50
o
C
Figure 8 Nyquist plots for the corrosion of 6063 aluminium
alloy at different temperatures in 1.0 M H
3
PO
4
.
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5
0.0
0.5
1.0
1.5
2.0
2.5
3.0
3.5
Z' (ohm cm
2
)
-
Z
"
(
o
h
m
c
m
2
)
30
o
C
35
o
C
40
o
C
45
o
C
50
o
C
Figure 9 Nyquist plots for the corrosion of 6063 aluminium
alloy at different temperatures in 0.5 M NaOH.
3.1x10
-3
3.1x10
-3
3.2x10
-3
3.2x10
-3
3.3x10
-3
3.3x10
-3
3.4
3.6
3.8
4.0
4.2
4.4
4.6
4.8
5.0
5.2
5.4
5.6
l
n
(
C
R
)
(
m
m
y
-
1
)
1/T (K
-1
)
0.01M
0.05M
0.1M
Figure 10 Arrhenius plots for the corrosion of 6063 aluminium
alloy in H
3
PO
4
.
6 P. Deepa, R. Padmalatha
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media. Arabian Journal of Chemistry (2014), http://dx.doi.org/10.1016/j.arabjc.2013.07.059
3.4. Scanning electron microscopic study
The SEM images of freshly polished surface of 6063 alumin-
ium alloy are given in Fig. 14 which shows polished surface
with few scratches due to polishing. The surface morphology
of the 6063 aluminium alloy sample was examined by SEM
immediately after corrosion tests in 1.0 M phosphoric acid
medium and 0.5 M sodium hydroxide medium. The SEM
image of corroded sample given in Figs. 15 and 16 shows the
degradation of alloy, with more or less uniform attack in
phosphoric acid medium and sodium hydroxide medium.
Fig. 17 represents EDX spectrum of the polished sample of
the 6063 aluminium alloy. The spectrum shows peaks for
aluminium and oxygen suggesting the presence of aluminium
oxide/hydroxide. Fig. 18 depicts the EDX spectrum for the
corroded sample in the presence of phosphorous indicating
the attack of phosphoric acid medium.
3.1x10
-3
3.1x10
-3
3.2x10
-3
3.2x10
-3
3.3x10
-3
3.3x10
-3
-2.2
-2.0
-1.8
-1.6
-1.4
-1.2
-1.0
-0.8
-0.6
-0.4
-0.2
l
n
(
C
R
/
T
)
(
m
m
y
-
1
K
-
1
)
1/T (K
-1
)
0.01M
0.05M
0.1M
Figure 11 Plots of ln(CR/T) vs. 1/T for the corrosion of 6063
aluminium alloy in H
3
PO
4
.
3.1x10
-3
3.1x10
-3
3.2x10
-3
3.2x10
-3
3.3x10
-3
3.3x10
-3
6.0
6.5
7.0
7.5
8.0
8.5
l
n
(
C
R
)
(
m
m
y
-
1
)
1/T (K
-1
)
0.05M
0.25M
0.5M
Figure 12 Arrhenius plots for the corrosion of 6063 aluminium
alloy in NaOH.
3.1x10
-3
3.1x10
-3
3.2x10
-3
3.2x10
-3
3.3x10
-3
3.3x10
-3
0.5
1.0
1.5
2.0
2.5
3.0
l
n
(
C
R
/
T
)
(
m
m
y
-
1
K
-
1
)
1/T (K
-1
)
0.05M
0.25M
0.5M
Figure 13 Plots of ln(CR/T) vs. 1/T for the corrosion of 6063
aluminium alloy in NaOH.
Table 5 Activation parameters for the corrosion of 6063
aluminium alloy in NaOH.
NaOH (M) E
a
(kJ mol
1
) DH
a
(kJ mol
1
) DS
a
(J mol
1
K
1
)
0.05 18.43 15.88 150.54
0.25 15.79 13.24 141.49
0.5 13.25 10.70 128.21
Figure 14 SEM image of freshly polished surface of the 6063
aluminium alloy.
Table 4 Activation parameters for the corrosion of 6063
aluminium alloy in H
3
PO
4
.
H
3
PO
4
E
a
(kJ mol
1
) DH
a
(kJ mol
1
) DS
a
(J mol
1
K
1
)
0.01 13.1958 10.644 180.99
0.1 31.6439 29.0923 109.652
1.0 50.2442 47.6926 37.8584
Corrosion behaviour of 6063 aluminium alloy 7
Please cite this article in press as: Deepa, P., Padmalatha, R. Corrosion behaviour of 6063 aluminium alloy in acidic and in alkaline
media. Arabian Journal of Chemistry (2014), http://dx.doi.org/10.1016/j.arabjc.2013.07.059
For aluminium there is deposition of aluminium phosphate
precipitate on the surface and for 6063 aluminium alloy due to
the alloying elements, it may be attributed to deposition of the
phase Mg
5
Al
8
which makes an anodic phase in the aluminium
matrix and Si acts as cathode and contributes to the intergran-
ular corrosion resulting in uniform attack and making it an
optimum region of dissolution (Scamans et al., 1987). Close
observation of SEM metal images indicates the deposition
of precipitates of aluminium phosphate and magnesium
phosphate on 6063 aluminium alloy.
Fig. 19 depicts the EDX spectrum for the corroded sample
in the presence of sodium hydroxide medium. The spectrum re-
veals the presence of sodium hydroxide medium, the increase
in the amount of oxygen can be attributed to the presence of
aluminium hydroxide lm formed due to the attack of hydrox-
ide ion on the surface of metal.
3.5. Mechanism of corrosion process
Aluminium and its alloys have air formed oxide lm of
amorphous c alumina which initially thickens on exposure to
neutral aqueous solution with the formation of a layer of
crystalline hydrated alumina (Hart, 1957).
In acid solution the mechanism of dissolution of aluminium
is as follows (Obot et al., 2010):
Al H
2
O ! AlOH
ads
H
; 6
AlOH
ads
5H
2
O H
! Al
3
6H
2
O 2e
; 7
Al
3
H
2
O ! AlOH
2
H
; 8
AlOH
2
X
! AlOHX
: 9
Thus soluble complex ion formed leads to the dissolution of
the metal.
In case of sodium hydroxide medium corrosion of metals is
known to proceed by the action of local cells, which are
established by metals, comprising a partial anodic reaction
and a partial cathodic reaction occurring simultaneously on
the metal surface (Uhlig and Revie, 1991). So, in order to
Figure 15 SEM image of 6063 aluminium alloy after immersion
in 1.0 M H
3
PO
4
.
Figure 16 SEM image of 6063 aluminium alloy after immersion
in 0.5 M NaOH.
Figure 17 EDX spectrum of the polished sample of the 6063 aluminium alloy.
8 P. Deepa, R. Padmalatha
Please cite this article in press as: Deepa, P., Padmalatha, R. Corrosion behaviour of 6063 aluminium alloy in acidic and in alkaline
media. Arabian Journal of Chemistry (2014), http://dx.doi.org/10.1016/j.arabjc.2013.07.059
follow the mechanism underlying the corrosion of metals, it is
necessary to explore which partial anodic reactions and partial
cathodic reactions involve and to determine which of them pre-
vails in the gross corrosion reaction to a greater extent. In
addition, the presence of the native surface oxide lm should
be considered in studying the corrosion mechanism of
aluminium in alkaline solution. The anodic aluminium
dissolution reaction in the presence of the oxide lm can be
classied into a direct metal dissolution reaction by the move-
ment of aluminium ions through the lm and an indirect metal
dissolution reaction by consecutive oxide lm formation and
dissolution (Moon and Pyun, 1998; Moon and Pyun, 1999).
It is generally accepted (Wernick et al., 1987; Brock and
Wood, 1967) that the lm formation proceeds electrochemi-
cally by the incorporation of hydroxide ions into the lm
and migration through the lm towards the aluminium/lm
interface in the presence of a thick oxide lm on the surface
of aluminium as (11):
Al 3OH
! AlOH
3
3e
10
The aluminium hydroxide lm formed electrochemically will
be dissolved chemically by OH- attack at the lm/solution
interface:
AlOH
3
OH
! AlOH
4
11
where AlOH
4
represents the aluminate ions. A partial ano-
dic dissolution reaction of aluminium in alkaline solution
can be obtained by combining electrochemical lm formation
(10) and chemical lm dissolution (11), which can be written
as:
Al 4OH
! AlOH
4
3e
12
The electrons produced by the partial anodic Reaction (12)
will be consumed immediately by such partial cathodic reac-
tions as the oxygen reduction reaction:
3=4O
2
3=2H
2
O 3e
! 3OH
13
and/or the water reduction reaction:
3H
2
O 3e
! 3=2H
2
3OH
14
Figure 19 EDX spectrum of 6063 aluminium alloy after immersion in 0.5 M NaOH.
Figure 18 EDX spectrum of 6063 aluminium alloy after immersion in 1.0 M H
3
PO
4
.
Corrosion behaviour of 6063 aluminium alloy 9
Please cite this article in press as: Deepa, P., Padmalatha, R. Corrosion behaviour of 6063 aluminium alloy in acidic and in alkaline
media. Arabian Journal of Chemistry (2014), http://dx.doi.org/10.1016/j.arabjc.2013.07.059
The short-circuited corrosion reaction of pure aluminium in
alkaline solution can be obtained by combining Reactions
(12) and (13):
Al OH
3=4 O
2
3=2 H
2
O ! AlOH
4
15
and/or by combining Reactions (12) and (14):
Al 3H
2
O OH
! 3=2 H
2
AlOH
4
16
As a consequence of the overall corrosion Reaction (15), alu-
minium metal dissolution occurs. On the other hand, hydrogen
evolution takes place simultaneously with the dissolution of
aluminium metal as a result of the overall corrosion Reaction
(16). The observation of gas bubbles on the corroding
aluminium surface shows that the corrosion of aluminium in
alkaline solution proceeds mainly by water reduction (Pyun
et al., 1999) according to Reaction (16).
Therefore, it is concluded that the overall corrosion reac-
tion of aluminium in alkaline solution can be divided into
two substeps of a partial anodic reaction comprising the elec-
trochemical formation and chemical dissolution reactions of
the lm, and a partial cathodic reaction of water reduction
reaction.
4. Conclusions
6063 aluminium alloy undergoes corrosion both in phos-
phoric acid medium and in sodium hydroxide medium.
The corrosion rate increases with an increase in the concen-
tration of phosphoric acid medium as well as sodium
hydroxide medium.
The corrosion rate increases with an increase in
temperature.
The corrosion of 6063 aluminium alloy is more severe in
sodium hydroxide medium than in phosphoric acid
medium.
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Corrosion behaviour of 6063 aluminium alloy 11
Please cite this article in press as: Deepa, P., Padmalatha, R. Corrosion behaviour of 6063 aluminium alloy in acidic and in alkaline
media. Arabian Journal of Chemistry (2014), http://dx.doi.org/10.1016/j.arabjc.2013.07.059