Online International Interdisciplinary Research Journal, {Bi-Monthly}, ISSN2249-9598, Volume-III, Issue-V, Sept-Oct 2013

Corrosion Inhibition of Hexamine for Galvanized Steel in

Hydrochloric Acid Solution
a
Khulood Abid Al-Saade, aHayfaa A.Abas
a
Department of Chemistry, College of science, Baghdad University, Jaderyah,
Baghdad, Iraq

Corresponding author:
Khulood Abid Al-Saade
Department of Chemistry, College of science, Baghdad University, Jaderyah, Baghdad, Iraq

Abstract
The corrosion of galvanized steel in hydrochloric acid solution (pH = 2)
containing different hexamine concentration has been studied at temperature range
(298-328) K, by using computerized potentiostate. Corrosion protection percentage of
galvanized steel using different concentrations and at different temperatures reaches
the range of (51-86)% . The corrosion protection percent was found to increase with
the increase of temperature and to decrease with the increase of hexamine
concentrations. Hexamine cause to decreased penetration loss and weight loss, with
-5 -4
it used in low concentration (7. 4×10 - 3.57×10 ). Hexamine shifted the corrosion
to surface sites where activation energy is lower by block the active sites which have
-2 -
high activation energy. Hexamine was acted as good inhibitor in 1×10 mol.dm
3
HCl for G.S corrosion.

KEYWORDS: Corrosion, Galvanized steel, Hexamine, Inhibitor, Protection

Introduction
Steel galvanization is a sacrificial protection method for steel against
corrosion where, a layer of zinc is applied on the surface of steels either
electrochemically or by dipping of steel in molten zinc(El-Shazly et al., 2011). The
process results in the formation of an outer layer of pure zinc that is under laid by
several zinc –iron alloy layer. Zinc provided protection in two ways. It acts as a
barrier that prevents access of oxygen and moisture to the protected material, and or
acts as sacrificial anode that corrodes in preference to the protected metal(David et al
2009).
Acids have been used for drilling operation ,pickling baths and in de- scaling
processes (Matheswaran et al 2010).Hydrochloric acid is the most difficult of the
common acid to handle from the standpoint of corrosion and materials of
constructions(Ehteram et al 2008) .This acid is very corrosive to most of the metals
and alloys(Fontana 1987). The reason for the aggressiveness of chloride has been
pondered for some time and number of notions has been but forth. Chloride is an
anion of a strong acid and many metal cation exhibit considerable solubility in
chloride solution. Chloride is a relatively small anion with a high diffusivity; it
interferes with passivation, and it is ubiquitous as a contaminant (Galvele 1981) . One
of most vital processes in the field of corrosion and its control is the use of organic
inhibitors. Heteroatom such as nitrogen, oxygen, sulphur present in the inhibitors play
a leading role in this interaction by donating their free electron pairs (Fontana 1987) .

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Aromatic, aliphatic and heterocyclic amine has been extensively investigated as

corrosion inhibitors (Galvele 1981). According to(Hackerman et al 1961). The
inhibitive properties of a series of secondary aliphatic and cyclic amine in acid media
are controlled by the percentage of π – orbital of the free electron on the nitrogen
atom of this compound. (Wang Lin et al 2003). has studied the corrosion inhibition of
zinc in phosphoric acid solution by 2- mercapto benzimidazole .(Vashi et al 2005).
Studied ethanolamines and ethylamines as corrosion inhibition for zinc in phosphoric
acid .Hexamine was reported as effective corrosion inhibition for various metals in
acid (Hackerman et al 1961). The most effective and efficient inhibitors are organic
compounds having heteroatom's and /or π bound in their structures. An efficient
organic compound possesses the ability to be adsorbed on the metal surface by
displacing water molecule from a corroding interface (Zarrouk et al 2010) . In this
research work, the inhibition effects on acid corrosion of galvanized steel in acid
solution was investigated by corrosion monitoring techniques like potentiostate
polarization studies, weight loss and penetration losses measurements.
Experimental Procedure
There are two main reasons why zinc is chosen as a protective coating for
iron steel. The first is the natural resistance of zinc itself against corrosion in the
most atmospheric conditions , and the second is the fact that zinc is electronegative
to iron and can protect it sacrificially. The success of zinc can be largely attributed to
ease of application, low cost and high corrosion resistance. In practical applications,
the structures most commonly provided with protection are constructed of iron or
steel (including stainless steel) and the electrolytes are most often soil and
water. Other metals commonly provided with cathodic protection include, lead
sheathed cables, copper and aluminum piping, galvanized steel, and cast iron
Materials and Chemical
The galvanized steel which has been used in this work has the following
composition. The base metal is carbon steel with typical analysis.
Metal Co Si Mn S P
wt% 0.40 0.25 0.80 0.015 0.015

Hexamine

Structure of Hexamine

Hexamethylene Tetramine, more commonly known as Hexamine, was

obtained from BDH with a purity exceeding 99% and was used without further
purifications. The molecular formula is C6H12N4 and the molecular weight is 140.20
g/mole. 1.0 Cm2 pieces of galvanized steel (G. S.), were served as the working
electrode. Platinum was served as the counter electrode, while standard calomel
electrode (SCE) was used as the reference electrode. The electrochemical studies were
conducted with the use of advanced potentiostat winking MLab-200 (2007)
(Germany), [Bank Elektronik-Intelligent]. In this study, the effects of adding different
hexamine concentration to 0.01M HCl acid solutions on the corrosion of G.S have
been investigated in order to determine the percentage of corrosion inhibition at

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different temperatures. Corrosion current icorr was evaluated by extrapolated the

anodic and cathodic Tafel lines for the polarization curves. The open circuit potential
(OCP) was measured and the polarization curves were scanned between (-1.0 - 0.2 V).
The HCl solutions were prepared by using HCl (36% Aldrich) and diluted with De
ionized water (with measured conductivity less than 2 µs ⁄ cm).
1. Results and Discussion
1.1 Polarization Curve
Figure 1, shows the polarization curves for the G.S. in 10-2 mol dm -3 HCl,
containing different concentration of hexamine and at different temperatures 298 -
328 K. Table 1 shows the polarization data, (the corrosion potential Ecorr and the
corrosion current densities Icorr), while Table 2 show the influence of hexamine
concentration on the corrosion current densities , corrosion potentials for the G.S. in
10-2 mol dm-3 HCl solution over the temperature range 298 -328 K. It was observed
from the data of the Table 1, that hexamine addition caused a slight increase in the
corrosion current densities for G.S. with the increase of both hexamine concentration
and the temperature. The corrosion potential is shifting in the noble direction (or to a
less negative potential) with the increase of both hexamine concentration and
temperature. The tendencies of these effects were reflected by the change of the
corrosion current density of the specimen and by the tendency of the specimen for
corrosion. As can be seen in Table 1, the values of the Tafel slopes ba and bc was
obtained within the range 0.05 - 0.1 V decade -1. Increasing the temperature from
298K to 328 K caused only a slight increase in the values of Tafel slopes. A
departure in ba and bc then the expected theoretical values may be attributed to the
variation of the rate –determining step in the metal dissolution reaction or of a change
in the mechanism of anodic and cathodic reaction. A cathodic Tafel slope of - 0.120V
decade-1 may be diagnostic of discharge – chemical desorption mechanism for
hydrogen evolution reaction at the cathode in which the proton discharge is the rate –
determining step. If chemical desorption is the rate –determining step ,then the rate
will be independent of the over potential since no charge transfer occurs in this
process and the rate becomes directly proportional to the concentration or the
coverage θ of the adsorbed hydrogen atoms. The process may occur at a coverage
rang from very small values to almost full surface layer formation .The expected
Tafel slop would then be -0.03V decade-1, when the electrochemical desorption
becomes the rate determining step for the hydrogen evolution reaction on the cathode.
The expected value of bc is -0.04 V decade-1.
1.2. Protection Efficiencies
Table 2 shows the values of protection efficiency P which are calculated
from Eq. 1
p % = I corr u − I corr I / I corr * 100 ……… 1
ICorr u, ICorr I are corrosion current densities for uninhibited and inhibited acid
for the corrosion current obtained by extrapolation of the cathodic and anodic Tafel
lines respectively. Values of the protection efficiency P were highly dependent on
temperature in presence of hexamine as inhibitor. The value of P% increases to
maximum value at about 328 K and is shown in the Figure 2. Figure 3, shows the
relationship between the protection efficiencies of G.S. and various concentration of
inhibitor. The protection efficiency was found to decrease upon the increase of
concentration of hexamine, and then became independent with the increase in
concentration of hexamine.

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1.3 The surface coverage

The coverage θ of the surface of G.S .immersed in 10 -2 mol dm -3 of
hydrochloric acid containing the inhibitor ( hexamine), with different concentration C
was calculated using Eq. 3. The values for the various inhibitor concentration and
four experimental temperatures are given in Table 4. Values of C and C/θ for the
corrosion of the Galvanized Steel at different Temperatures were calculated using Eq.
4, as shown below:
θ = (Wu - Wi / W u) ………. 3
C/θ =1 /b + C ……… 4
1.4 . Thermodynamic of corrosion
1. A plot of C/θ values against the corresponding values of C was found to be
linear as shown in Figure 4. The term b is the maximum adsorption quantity at
different temperatures and were obtained from the intercepts of the straight lines
of the plot. The later is used to determine the thermodynamic function, H, S
and G as seen from Table -3(Chem2000 and Karaca et al 2008) [3,10]
b= a*exp ( - H ads/RT ) ………. 5
ln b =ln a- (- Ha /R ) * 1/T …….… 6
ln a = S /R ……… 7
G = Hads -T S ..…….. 8
Equation 6 was used to calculated the Hads , by plotting lnb against 1 /T as shown in
Figure 5. The plot gave a linear relationship and the slope represents (- Hads /R), from
which Hads values were calculated.
1.5. Kinetic of Corrosion
The rate of the corrosion of G.S. in the galvanized steel in presence of
inhibitor, is represented by Arrhenius equation:
r = A exp (-Ea /RT) ……….9
Where A and Ea are the pre –exponential factor and energy of activation .The value of
the rate of corrosion r at any temperature was taken to be proportional to the corrosion
current density icorr.Figure 6, shows Arrhenius plot for the various inhibition values of
Ea. Log A have been derived from the slop and intercepts of the plots. Entropy of
activation S* values were calculated from the value of A using the relationship:
A = kT / h e - S* /R ……… 10
Where k, h and R are constants. The kinetic data which have been presented in the
Table 5.
The activation energies were found to be lower than that obtained in the absence of
inhibitor .Thus, the presence of hexamine in the acid medium 10 -2 mol dm -3 HCl
shifted the corrosion to surface site. The calculated Ea was found to be lower than that
obtained in the absence of hexamine. This may arise as a consequence of an electric
field arising at the inhibitor /metal interface which may lower the energy barrier for
corrosion of the metal.

Mechanism of Corrosion
The mechanism of inhibition process of corrosion is believed to be due to the
formation and maintenance of protective film on the metal surface. Macro molecular
size and higher number of N- atoms of hexamine might have covered almost all active
source of G.S. Four nitrogen atom of hexamine having high electron density must
have functioned as the reaction center and the hexamine molecules might have been
chemisorbed to form a thin monolayer on the G.S. surface.

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Hexamine consist of four nitrogen atoms and six CH2 groups. Because of the
presence of three nitrogen atoms, electron is disposed easily in the ring and therefore
it is expected to be an effective inhibitor. The inhibitor action can be accounted by the
interaction of lone pair of electron in the nitrogen atom on the positively charged
metal surface. The presence of six ethylene groups also helps to lead to an
enhancement of electron density at the nitrogen atoms, which enhances its adsorption
on the metal surface. This in turn leads to an increase value of protection efficiency.
The protective effect of the inhibitor is probably due to formation of insoluble films
hence the mechanism of the inhibitive action is possibly due the blocking of anodic
and cathodic sites by adsorption. This enables the formation of a protective insoluble
film (Vashi et al 2010).
The calculated value of Ea calculated from Eq. 9 was found to be higher than
that of uninhibited system. This suggests that the presence of reactive centers on the
inhibitor can block the active sites for corrosion resulting in an increase in Ea.The
enthalpy H values was calculated from Eq. 5, the enthalpy change value was
positive, indicating the endothermic nature of reaction suggesting that higher
temperature favors the corrosion process .(Adeyen 2005) described that if the H < 10
kJ mol-1, the adsorption is probably physisorption and if the H > 10 kJ mol-1 values
indicate that the hexamine strongly adsorbed on G.S. is chemisorptions(Vashi et al
2005).
.

Conclusion
Certain conclusion can be derived from this study as in the following:
1. Hexamine was acted as good inhibitor in1× 10-2 mol.dm-3HCl for G.S.
corrosion .
2. Corrosion rate decreased with hexamine addition to1× 10-2 M HCl and
protection efficiency reach to 86.5% at 328 K .
3. Low hexamine concentration lead to shitted corrosion potential to the noble
direction which mean that the inhibitor act as anodic inhibitor. The high
hexamine concentration some time cause to shift the corrosion potential to
active direction which mean the inhibitor act as a cathodic inhibitor. Overall
the hexamine act as mixed inhibitor for anodic and cathodic regions.
4. The protection efficiency increase with increasing the temperature.
5. Kinetic data reveal the following: The activation energies which were
relatively lower than that obtained in the absence of inhibitor. Thus, the
presence of hexamine in the acid medium (1×10 -2 mol. dm -3 HCl ) shift the
corrosion to surface site where Ea is lower than the normal energy of
activation in the absence of hexamine . This may arise as a consequence of an
electric field arising at the inhibitor /metal interface which may lower the
energy barrier for corrosion of the metal .This case is obtained clearly in using
3.57× 10-3 mol.dm-3 hexamine concentration.
6. The thermodynamic and kinetic data appear that the adsorption of hexamine
on the surface of G.S.is chemisorptions type and obey Langmiur isotherm
type.
7. Hexamine cause to decreased penetration loss and weight loss, with it used in
low concentration (7. 4×10-5 - 3.57×10-4).

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298 K 0.5 INH.

-700
308 K

-800 318 K

Potential (mv)
328 K

-900

-1000

-1100

-1200
0.001 0.010 0.100 1.000

logi corr/mA. cm2

pH = 2
Potential (mv)

-700 298 K

308 K

-800 318 K

328 K

-900

-1000

-1100

-1200
0.001 0.010 0.100 1.000

logi corr/ mA. cm2

Fig 1: Typical polarization curve for the corrosion of G.S.in10-2 mol.dm-3 of HCL
solution at 0.5mol.dm-3 concentrations of hexamine at four temperatures in the Rang
298-328 K.

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concentration
Table 1: Values of inhibitor
of corrosion current(Hexamine) at four
Icorr, corrosion temperatures
potential, Tafel in the range
slopes, weightof loss and
(298-328 K).
penetration loss at different concentrations of hexamine at four temperatures in the Rang
298-328 K.

Con. Of Icorr Weight

(-E Corr ) ba - bc Penetration
T/K Hexamine A.cm2 loss P% θ
(V*10-3) V.decade-1 V.decade-1 loss/(mm.y)
mol/dm3 (*10 -6) (g/m2.d)

298 0 162.77 0.94 0.08 0.54 41 2.1 ----- -----

308 278.09 0.92 0.35 0.58 105 5.38 ----- -----
318 459.37 0.92 0.30 0.46 124 6.34 ----- -----
328 735.96 0.92 0.28 0.50 206 10.5 ----- -----
-5
298 7.14*10 54.45 0.92 0.06 0.14 15.7 0.803 61.76 0.62
308 67.11 0.89 0.06 0.08 20.6 1.05 80.51 0.81
318 81.62 0.87 0.05 0.05 23.1 1.18 81.38 0.81
328 98.10 0.86 0.07 0.08 29 1.48 85.93 0.86
298 3.57*10-4 59.40 0.93 0.07 0.12 16.8 0.86 59.05 0.59
308 72.34 0.93 0.08 0.07 22.4 1.15 78.68 0.79
318 87.02 0.92 0.07 0.09 25.2 1.29 79.66 0.80
328 103.51 0.91 0.07 0.10 29.9 1.53 85.49 0.85
298 7.14*10-4 62.75 0.93 0.07 0.34 17 0.87 58.56 0.59
308 76.55 0.94 0.07 0.12 25.3 1.3 75.91 0.76
318 92.22 0.92 0.11 0.23 26.7 1.37 78.49 0.78
328 109.84 0.93 0.13 0.26 31 1.59 84.96 0.85
298 3. 57*10-3 72.55 0.97 0.07 0.15 20.1 1.03 51.07 0.51
308 81.17 0.96 0.09 0.12 25.6 1.31 75.66 0.76
318 Table 2: Values
90.16of protection
0.95 efficiencies
0.11 calculated corr and weight
0.19 from i27.2 1.39loss, for78.08
the 0.78
corrosion of G.S.in10-2 mol.dm-3 of HCL solution at 0.5mol.dm-3 concentrations
328 99.52 0.94 0.19 0.30 27.8 1.42 86.49 0.86
-3
298 7.14*10 58.77 0.94 0.08 0.17 16.3 0.834 60.27 0.60
308 77.09 0.93 0.09 0.13 22.9 1.17 78.26 0.78
318 99.42 0.92 0.13 0.25 33.2 1.7 73.21 0.73
328 126.25 0.93 0.15 0.35 33.5 1.71 83.76 0.84

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Table 2: Values of protection efficiencies calculated from icorr and weight loss, for the
corrosion of G.S.in10-2 mol.dm-3 of HCL solution at 0.5mol.dm-3 concentrations

Conc./
T/K P% / from weight loss P% / from I Corr
Mol.dm-3
298 61.76 66.54
308 80.51 75.87
7.14*10-5
318 81.38 82.23
328 85.93 86.67
298 59.05 63.51
308 78.68 73.99
3.57*10-4
318 79.66 81.06
328 85.49 85.94
298 58.56 61.45
308 75.91 72.47
7.14*10-4
318 78.49 79.93
328 84.96 85.08
298 51.07 55.42
308 75.66 70.81
3. 57*10-3
318 78.08 80.37
328 86.49 86.48
298 60.27 63.90
308 78.26 72.28
7.14*10-3
318 73.21 78.36
328 83.76 82.85

90 90

85

80 80

75
P ( %)

70 70
P%

7.14E-05
3.57E-04 65
7.14E-04
60 60 298k
3.57E-03
7.14E-03 308K
55 318K
328K
50 50
290 300 310 320 330 0 0.5 1 1.5
T/ K C /mol. dm-3
Fig.2: Relationships between the Fig.3: relationship between the protection
protection efficiencies of the G.S.corrosion efficiencies of G.S. corrosion and various
and temperature with different concentration of inhibitor at different
concentration of hexamine. Temperature.

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Table 3: The thermodynamic functions ∆H, ∆S and ∆G of the adsorption processes for the
corrosion of the Galvanized Steel at different Temperatures.
∆H / ∆S / ∆G
1/T
b lnb kJ.mol-1 J.mol-1.K-1 kJ.mol-1
K

6963.788301 8.848479 0.003356 130.52 511.5604 -21.92

38358.26621 10.55473 0.003247 130.53 -27.02
540540.5405 13.20032 0.003145 127.77 -34.89
581395.3488 13.27319 0.003049 131.59 -36.19

Table 4: Values of concentration C and concentration over

surfaces coverage C/ θ for the corrosion of the G. S
at different Temperatures.

T/K C*10-5 C/θ*10-5

7.14 11.56
35.71 60.49
298 71.43 121.97
357.14 699.37
714.29 1185.10
7.14 8.87
35.71 45.39
308 71.43 94.09
357.14 472.05
714.29 912.73
7.14 8.78
35.71 44.83
318 71.43 91.00
357.14 457.42
714.29 908.00
7.14 8.31
35.71 41.77
328 71.43 84.07
357.14 412.93
714.29 830.00

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1400
20
298
1200 18
308
1000 16
C/θ*10-5 318
800
328 14

lnb
600
12
400
10
200

0
8
0.003 0.0031 0.0032 0.0033 0.0034
0 200 400 600 800
C*10-5 1/T K-1

Fig. 4: A plot of C/θ values against Fig 5: values of log b plotted verses
the corresponding values of C at 1/T for various inhibitor
different temperatures in the range concentrations for G.S. in 10-2 mol
298 -328K. dm -3 hydrochloric acid systems

2.2 7.14E-05
3.57E-04 60
Log(A) Molecules/cm2.S *10^23

7.14E-04
Log(Icorr.)

2.1
3.57E-03
7.14E-03
2 40

1.9
20
1.8

1.7
0
0.003 0.0031 0.0032 0.0033 0.0034
5 15 25 35 45
1/T K-1 E a kJ/mol

Fig.6: Arrhenius plot relating log icorr Fig.7: Variation of the activation energy (Ea)
with 1/T for the corrosion of G.S. with pre-exponential factor (log A) for the
in 10 -2 mol .dm-3 of hydrochloric corrosion of G.S. in 10-2 mol. dm-3
acid solution. hydrochloric acid solution.

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Table 5: Kinetic data of activation energy (Ea) , pre exponential

factor (A) and the entropy of activation ( S*) for the
corrosion of G.S. in 10 -2 mol dm -3 HCl.

Conc. A*1024 S*
Additive T/ K -1 -3 Ea / KJ.mol-1
/ Mol .dm / molecules.cm-2.S-1 / J.K-1 .mol-1
298 389.88
308 -5 389.60
7.14*10 40.8791 14308.57
None 318 389.34
328 389.08
298 297.11
308 -4 296.83
3.57*10 15.9477 0.204
318 296.57
328 296.31
298 294.81
308 -4 294.54
7.14*10 15.0477 0.155
318 294.27
328 294.01
298 295.67
308 -3 295.40
3.57*10 15.1684 0.172
318 295.13
Hexamine
328 294.88
298 274.71
308 -3 274.43
7.14*10 8.56069 0.014
318 274.17
328 273.91
298 313.75
308 -5 313.47
7.14*10 20.7172 1.512
318 313.21
328 312.95

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