Materials Sciences and Applicatio ns, 2011, 2, 1260-1267
doi:10.4236/msa.2011.29170 Published Online September 2011 (http://www.SciRP.org/journal/msa)
The Inhibitive Effect of 3-Methyl 4-Amino 1,2,4
Triazole on the Corrosion of Copper-Nickel
70 - 30 in NaCl 3% Solution
Tayeb Chieb1,2, Kamel Belmokre2, Mohammed Benmessaoud1,3, Sidi El Hassane Drissi3, Najat Hajjaji1,
Abdellah Srhiri1
1Laboratory of Electrochemistry, Materials and Environment (LEME), Faculty of Science, Ibn Tofail University, Kenitra, Morocco;
2Laboratory Corrosion and Surface Treatment (LCST), University of Skikda, Faculty of Sciences, Skikda, Algeria; 3University of
Mohammed V Agdal, Energy Systems Laboratory, Materials and Environment, High School of Technology, Salé Medina,
Morocco.
Received May 3rd, 2011; revised May 26th, 2011; accepted June 11th, 2011.
ABSTRACT
The effect of 3-methyl 4-amino 1,2,4 triazole (MATA) on the corrosion behaviour of copper-nickel 70 - 30 (Monel) in
NaCl 3% solution is investigated at 298 K by weight loss measurements, potentiodynamic polarisation and impedance
spectroscopy (EIS) methods. Preliminary screening of the inhibition efficiency (ECR) was carried out with using weight-
loss measurements. Polarization measurements showed that the organic compound investigated is mixed type inhibitor
(it acts on the cathod ic and the cathodic reac tions), inhibiting the corrosion of Monel by blocking the active sites of the
metal surface. Changes in the impedan ce parameters charge transfer resistance (Rct) and double layer capacitance (Cdl)
are related to adsorption of organic inhibitor of the metal surface, leading to the formation of protective film, which
grows with increasing exposure time. Inhibition efficiencies obtained from cathodic Tafel plots, gravimetric and EIS
methods are in good agreement. Resu lts obtained shows that the (MA T A) is good inhibitor for copper – nickel, and its
efficiency reaches more than 95% at 60 ppm after 30 mn of immersion.
Keywords: Copper-Nickel, Triazole, Inhibitor, Efficiency, Polarisation, Impedance
1. Introduction
Copper and its alloys are widely used in industry because
of their excellent electrical and thermal conductivity and
their corrosion resistance; copper alloys are often used in
heating and cooling system [1-3]. Copper-nickel 70 - 30
(Monel) has been widely used as tubing material con-
densers and heat exchangers in various water cooling
systems [4-9]. However, the presence of certain pollut-
ants such as sulphurs and ammonia compromise their
corrosion resistance especially in sea water. Sure enough,
Macdonald et al. [10,11] studied the impact of sulphur on
the corrosion behaviour of copper nickel in airless sea
water, these authors showed that sulphurs increases cor-
rosion rates. On the other hand Syrett et al. [12] noticed
that the sulphurs are not dangerous in the absence of
oxygen. Other authors [13,14] investigated the effect of
ammonia, they have observed that the presence of am-
monia favour the selective corrosion of copper nickel
alloys by the formation of complexes compounds with
copper. Sure enough, copper complexes which formed
with ammonia molecules destabilize easily corrosion
products layer which generally protect copper alloys [15].
During more then thirty years ago, many techniques have
been used to minimise corrosion of copper-nickel. One of
the techniques used for minimising corrosion is the use
of inhibitors. The effectiveness of the inhibitors va- ries
with its concentration, the corrosive medium and the
surface properties of the alloy. Many inhibitors have
been tested to minimise the corrosion of Monel in dif-
ferent media [16]. Particularly, heterocyclic organic com-
pounds containing nitrogen, sulphur and/or oxygen are
often used to protect metals from corrosion. Among them,
azoles have been intensively investigated as effective
copper corrosion inhibitors [17-20]. Benzotriazole (BTA),
for example, has been studied and found to have excel-

The Inhibitive Effect of 3-Methyl 4-Amino 1,2,4 Triazole on the Corrosion of Copper-Nickel 1261
70 - 30 in NaCl 3% Solution
lent inhibition properties in several corrosive environ-
ments [21-25]. This molecule contains nitrogen atoms
and has been found useful in preventing copper staining
and tarnishing. The effectiveness of BTA has been re-
lated to the formation of a [Cu+-BTA−]n film, the film
formed is considered to be insoluble and polymeric [26].
Bag et al. [27] investigated the protective action of azo-
les on the corrosion of 70 - 30 brass in ammonia solution
and concluded that the inhibitors could control corrosion
effectively. Shukla and Pitre [28] studied the electro-
chemical behaviour of brass and the inhibitive effect of
imidazole in acid solution. Walker [29] showed that the
addition of small amounts of the 1,1,3 benzotriazole and
1,2,4 triazole inhibited the corrosion of brass in various
acidic, neutral and alkaline solutions. Fenelon and Bre-
zlin [30] studied the formation of BTA films on copper,
Cu-Zn alloys and Zn in chloride solution. Aramaki et al.
[31] proposed mechanisms of benzotriazole derivatives
on copper in sulphate solution at several values of pH by
an impedance technique and enhanced Raman scattering
spectroscopy. Subramanian and Lakshimina- rayanan [32]
studied the adsorption properties and the effect of some
azoles such as benzotriazole, mercaptobenzotriazole,
benzimidazole, imidazole and tetrazole on the growth of
oxide film on copper in 0.1 M NaOH. All these com-
pounds contain nitrogen and/or sulphur atoms which can
co-ordinate with copper through the lone pair of elec-
trons to form complexes. These complexes are generally
believed to be polymeric in nature and form a protective
film on the copper surface, which acts as a barrier of ox-
ide film formation. The inhibitor action of these azoles
may also be due to physisorption or chimisorption onto
the copper surface. Trachli et al. [33] studied the protect-
tive effect of electropolymerized aminotriazole towards
corrosion of copper in 0.54 M NaCl solution. Nagiub and
Mansfeld [34] investigated the corrosion behaviour of
26,000 brasses in artificial sea water using EIS and ENA
techniques. BTA, gluconic acid sodium salt and poly-
phosphoric acid sodium salt were evaluated as corrosion
inhibitors. Qafsaoui et al. [35] studied the quantitative
characterization of protective film developed on copper
by anodic polarization in a borate buffered solution con-
taining benzotriazole and aminotriazole. Al-kharafi and
Ateya [36] investigated the effect of sulphides on the
electrochemical impedance of copper in benzotriazole-
inhibited media. Tommesani [37] studied protective ac-
tion of 1,2,3-benzotriazole derivative films against cop-
per corrosion. Although there is an extensive literature on
the corrosion properties of triazole such as imidazole and
benzotriazole on steel and copper, there remains little
information on the effect of various functional groups in
the BTA derivatives on the corrosion of copper nickel
alloys. Based on this, the inhibitors have been considered
and synthesized according to the previous report. In the
present investigation, it is proposed to study the electro-
chemical behaviour of copper nickel 70 - 30 in artificial
seawater with 3-Methyl 4-Amino 1,2,4 triazole (MATA).
Weight-loss method and electrochemical studies such as
potentiodynamic polarization, impedance spectroscopy.
Solution analysis was carried out to find out the concen-
tration of Cu and Ni leached out from the copper nickel
alloy using atomic absorption spectroscopy.
2. Experimental Conditions
Monel strips having chemical compositions (wt%): 69.3%
Cu, 29.6% Ni, 0.7% Mn, 0.4% Fe. The NaCl 3% solution
was prepared by dissolving 30 g of pure NaCl in 1 l of dis-
tilled water. The inhibitor: 3-Methyl 4-Amino 1,2,4 triazole
(MATA) was synthesized according to the reported proce-
dures [38] and its structure is shown in Figure 1.
Weight-loss method measurements were performed
with rectangular Monel coupons (5 cm × 3 cm× 0.3 cm).
The coupons were immersed in 300 ml of NaCl 3% solu-
tion with and without inhibitors and allowed to for 5 days
at room temperature (25˚C). Afterwards, the coupons
were rinsed with distilled water and adherent corrosion
products were removed by immersing the coupons in 6%
H2SO4 for 20 s. Then the coupons were rinsed with dis-
tilled water, cleaned with acetone, dried and weighed.
Duplicate tests were conducted with for each experiment.
The corrosion rate CR and the percentage of inhibition
efficiency ECR (%) over the exposure period were calcu-
lated using the following equations [39]:
87.6 W
CR DAT



 (1)

%
inh
CR
CR CR
ECR

100
(2)
Figure 1. 3-Methyl 4-Amino 1,2,4 triazole (MATA).

The Inhibitive Effect of 3-Methyl 4-Amino 1,2,4 Triazole on the Corrosion of Copper-Nickel
1262
70 - 30 in NaCl 3% Solution
where W is the weight-loss in (mg), T the immersion time
in (hours), A the coupons area in (cm2), D the density of
the specimen in (g/cm3), CRinh and CR are the corrosion
rate of Monel in the presence and absence of inhibitor
respectively.
The potentiodynamic polarization studies were carried
out with Monel strips having an exposed surface area of
1 cm2. The electrodes were abraded mechanically with
silicon carbide papers from 120 to 1200 grit, the elec-
trode was thoroughly washed with distilled water, de-
greased in acetone, rinsed with distilled water and dried.
The cell assembly consisted of Monel as working elec-
trode, a platinum foil as counter electrode and Ag/AgCl
as reference electrode (RE). Polarization studies were
carried out using potentiostat/galvanostat (model PGZ
201). The working electrode was immersed in aerated
NaCl 3% solution and allowed to stabilize for 30 min
[40]. The cathodic and anodic polarization curves for
Monel specimen in the test solution with and without
inhibitors were recorded at a scan rate of 1 mv/s. The
inhibition efficiency of MATA was determined from
corrosion current density using the Tafel extrapolation
method.
Electrochemical impedance spectra (EIS) were carried
out at Ecorr using an electrochemical system response
analyser (model EGG). Monel with the exposed surface
of 1 cm2 was used as the working electrode. A conven-
tional three-electrode electrochemical cell of volume 300
ml was used. The reference electrode is on Ag/AgCl, the
platinum plate electrode was used as the counter. The
EIS were acquired in the frequency range from 100 kHz
to 1 mHz with 10 mV amplitude sine wave generated by
a frequency response analyser.
After the polarization measurements, the solutions were
analysed by atomic absorption spectroscopy to measure
the amount of Cu and Ni leached out from the Monel
samples at the optimum concentration of inhibitor. The
denickelification factor (f) is calculated using the rela-
tion.


Ni Cu
Ni/Cu
s
ol
alloy
f, (3)
where the ratio (Ni/Cu)sol is determined from the solution
analysis and (Ni/Cu)alloy is the weight-percent ratio of the
elements in the alloy.
3. Results and Discussion
3.1. Weight-Loss Method
Table 1 Show the corrosion rate and inhibition efficiency
of Monel by weight-loss measurements at different con-
centrations of inhibitor in NaCl 3% solution at room tem-
Table 1. Inhibition efficiency for various concentration of
(MATA) for the corrosion of Monel in NaCl 3% solution
obtained by weight-loss method.
[Inhibitor] (ppm) CR (×102 mm·year1) ECR (%)
Blank 25.5 -
20 7.65 70.0
40 3.83 84.9
60 1.28 95.0
80 2.8 89
100 3.8 85
perature (25˚C). The results showed that the corrosion
rate of Monel decreased whereas the inhibition effi-
ciency increased with increasing inhibitor concentration.
The maximum E% of the inhibitor (MATA) was achie-
ved at 60 ppm and a further increase in concentration
showed a decrease of inhibitor efficiency. Hence, the
optimum concentration of the inhibitor was found to be
60 ppm.
It is well known that the inhibitive action of organic
compounds containing N, and/or S, are due to the forma-
tion of co-ordinate type of bond between the metal and
the lone pair of electrons present in the additive. The
tendency to form co-ordinate bond and hence the extent
of inhibition can be enhanced by increasing the effective
electron density at the functional group of the additive, in
aromatic or heterocyclic ring compounds, the effective
electron density at the functional group can be varied by
introducing different substituent in the ring leading to
variations of the molecular structure.
The inhibition efficiency of triazolic derivates com-
pounds is due to donor-acceptor interactions between the
π electrons of the inhibitor and the vacant d-orbital of
copper surface or an interaction of inhibitor with already
adsorbed chloride ions [41]. Based on the results, the
organic compound (MATA) showed good performance
in NaCl 3% solution. The high solubility of 3-methyl
4-amino 1,2,4 triazole in the corrosive media and the
presence of NH2 group and CH3 radical allow the com-
pound to inhibit the metal surface in tandem.
3.2. Potentiodynamic Polarization Studies
The cathodic and anodic polarization curves of Monel in
NaCl 3% solution with varying concentrations of MATA
are shown in Figures 2 and 3. The three distinct regions
appearing in the anodic polarization curve were the ac-
tive dissolution region (apparent Tafel region), the ac-
tive-to-passive transition region and the limiting current
region.

The Inhibitive Effect of 3-Methyl 4-Amino 1,2,4 Triazole on the Corrosion of Copper-Nickel 1263
70 - 30 in NaCl 3% Solution
Figure 2. Cathodic polarization curves of Monel in aerated
3% NaCl without and with various concentrations of
MATA at 25˚C:  = 1000 rpm; |dE/dt| = 1 m·Vs1.
Figure 3. Anodic polarization curves of Monel in aerated
3% NaCl without and with various concentrations of
MATA at 25˚C:  = 1000 rpm; |dE/dt| = 1 m·Vs1.
It is evident that in the presence of inhibitor, the ca-
thodic and anodic curves were shifted towards positive
region and the shift was found to be dependent on in-
hibitor concentration. The Table 2 illustrates the corre-
sponding electrochemical parameters. The Ecorr were
marginally shifted in the presence of MATA. This ob-
servation clearly indicated that the inhibitor control the
anodic and cathodic reaction and thus act as mixed type
inhibitor. The current density also decreased with in-
creasing concentration of inhibitor. The corrosion rates
[42] and the inhibition efficiency [43] were calculated
from polarization curves using the following equations:
3
3.27 10
corr
Ew I
CR D

 
 (4)
Table 2. Polarisation parameters and corresponding inh
ibition efficiency for the corrosion of cupper-nickel 70 -
30 in NaCl 3% without and with addition of various c
oncentration of inhibitor.
Solution Blank 20 ppm 40 ppm60 ppm
bc (mV/dec) −288 −238 −218 −196
Ecorr (mV/Ag/AgCl) −222 −214 −195 −167
icorr (A·cm2) 24.5 6.92 3.28 0.8
CR (× 10-2 mm·year1)26.00 7.36 3.49 0.85
E (%) - 71.7 86.6 96.7

%
corrcorr inh
corr
II
EI100


(5)
where CR is the corrosion rate (mm·year−1), D the density
(g·cm−3), EW the equivalent weight of the specimen and

corr inh and corr
I
I
are the corrosion current density
(A·cm−2) values with and without inhibitor respectively.
The values of cathodic Tafel slope (bc) it found to
change with inhibitor concentrations, indicates that in-
hibitor controlled both the reactions. The inhibition effi-
ciency of MATA attained a maximum value of 96.7% at
60 ppm. The values of inhibition efficiency increase with
increasing concentration of inhibitor, indicating that a
higher surface coverage was obtained in a solution with
the optimum concentration of inhibitor. The corrosion
rate in blank solution was found to be 26 × 10−2 mm·year−1
and it was minimized by adding the inhibitor to a lower
value of 0.85 × mm·year−1 for the Monel due to the
presence of MATA on the metal surface.
3.3. Impedance Studies
The impedance diagrams are represented in Nyquist plot,
obtained in solution with and without the MATA inhibit-
tor, for different concentrations, are presented in Figure
4. The electrode was prepolarized at the free corrosion
potential until a steady-state was attained.
The impedance spectra in the absence of MATA pre-
sent one capacitive loop. In the context of a detailed
study published elsewhere [44], this loop is attributed to
a charge transfer process, the value of associated resis-
tance is about 1.5 kOhm·cm2, the capacity is in the order
of 168 F·cm−2. In the presence of inhibitor, we note that
the impedance display of the electrode in MATA con-
taining the solution changes in shape and size, on the
other hand it can be noticed that the impedance modulus
increased dramatically in presence of inhibitor from 20
ppm of MATA. The presence of two capacitive loops
seems to indicate a diffusion contribution to the begin-
ning of the experiment.

The Inhibitive Effect of 3-Methyl 4-Amino 1,2,4 Triazole on the Corrosion of Copper-Nickel
70 - 30 in NaCl 3% Solution
1264
Figure 4. Nyquist plots of copper-nickel 70 - 30 in NaCl 3% with and without various concentration of inhibitor.
Figure 5 shows the impedance diagrams obtained in
corrosive solution at the corrosion potential after the Cu
30 Ni electrode was exposed to the solution for different
immersion times. It maintains the same shape after 30
min of immersion time. As can be seen in this figure, the
impedance diagrams in the Nyquist plot become larger
with time.
It can be seen that Rt and Cd increased with time. The
increase of Rt may be explained by the formation of
copper chloride which protects the copper against the
corrosion. With accumulation of corrosion products, the
surface roughness increased leading to a higher Cd value.
Figure 6 shows the impedance diagrams obtained in
corrosive solution at 60 ppm of MATA at the corrosion
potential after the Monel electrode was exposed to the
solution for different immersion times. It maintains the
same shape after 30 min of immersion time. As can be
seen in this figure, the impedance diagrams in the Ny-
quist plot become larger with time. The increase of the
polarisation resistance with the immersion period is often
reported for the inhibiting action of heterocyclic on cop-
per corrosion. At 30 min of immersion time, we have a
loop in high frequencies (HF) and dispersion in low fre-
quencies range. If we allot the HF loop to the charge
transfer resistance Rt, then associated resistance is about
42 kOhm·cm2. The capacity is of the order 14.8 F·cm2.
The effect of increasing immersion time on impedance
spectra is characterised by the increasing size of the two
capacitive loops observed, reaching a maximum in 20 h.
The percentage inhibition efficiency (E%) is calcu-
lated from the charge transfer resistance values using the
following equation :

%
ctct inh
ct
RR
ER100

 (6)
where Rct(inh) and Rct are the charge transfer resistance
values with and without inhibitor respectively. The im-
pedance parameters derived from these investigations are
given in Tables 3 and 4. It is found that Rct values in-
creased in the presence of inhibitor and with immersion
time, whereas Cdl values found to be decreased. The de-
crease in Cdl values was due to the adsorption of MATA
on the metal surface. The inhibition efficiency reached
88.8 and 96.3% at 40 and 60 ppm respectively after 30
min of immersion, and it was not affected by the immer-
sion time (95.2% after 20 h in the presence of inhibitor at
60 ppm).

The Inhibitive Effect of 3-Methyl 4-Amino 1,2,4 Triazole on the Corrosion of Copper-Nickel 1265
70 - 30 in NaCl 3% Solution
Figure 5. Nyquist plots of copper-nickel 70 - 30 in NaCl 3%
after 0.5 h, 10 h and 20 h of immersion.
Figure 6. Nyquist plots of copper-nickel 70 - 30 in NaCl 3%
containing optimum concentration of MATA after 0.5 h, 10
h and 20 h of immersion.
Table 3. Impedance parameters for the corrosion of cupper-
nickel 70 - 30 in NaCl 3% in the absence and presence of
inhibitor in different concentrations.
Concentration (ppm) Rct (k·cm2) Cdl (µF·cm2) E (%)
0 1.5 168 -
20 7 23.8 73.3
40 13.50 18.8 88.8
60 40.75 9.76 96.3
3.4. Solution Analysis
The results of solution analysis and the corresponding
denickelification factor (f) in the presence and absence of
MATA at its optimum concentration level in NaCl 3%
solution for Monel are given in Table 5.
The results revealed that both copper and nickel were
present in the solution. The nickel/copper ratio in solu-
tion was found to be higher than that of the bulk alloy.
This indicates that the growth of surface film and the
dissolution of the alloy were controlled by diffusion [45],
which is related to the difference between the ionic rayon
of Ni2+ and Cu+ ions, 0.085 nm and 0.096 nm respec-
tively. It is also observed that the inhibitor is able to re-
tard the dissolution of both copper and nickel. This ob-
servation suggests that the inhibitor excellently control
the denickelification of Monel in NaCl 3% solution,
which is also reflected in the values of denickelification
factor
4. Conclusions
Electrochemical study showed that MATA product tested
is good inhibition efficiency for Monel in NaCl 3% solu-
tion both after a short and long immersion time. Polariza-
tion measurements showed that the organic compound
investigated are mixed type inhibitor, inhibiting the cor-
rosion of Monel by blocking the active sites of the metal
surface. The inhibitor easily adsorb on the Monel surface
at the corrosion potential and form a protective complex
with the Cu (I) ion, controlling Monel from corrosion.
Impedance studies showed that the change in charge
transfer resistance (Rct) and double layer capacity (Cdl)
are related to the adsorption of organic inhibitor on the
metal surface, leading to the formation of a protective
Table 4. Impedance parameters for the corrosion of cupper-
nickel 70 - 30 in NaCl 3% in the absence and presence of 60
ppm of MATA after different immersion times.
Solution Time (h)Rt (k·cm2) Cdl (F·cm2)E (%)
0.5 1.5 106 -
10 3.8 92 -
Blank
20 5.8 61 -
0.5 42 14.8 94.6
10 81 4.8 95.360 ppm MATA
20 120.5 3.5 95.2
Table 5. Effect of optimum concentration of MATA on the
denickelification of Monel in NaCl 3% solution.
SolutionCu (ppm)Ni (ppm) Factor (f) Cu (%)Ni (%)
blank 10.46 37.34 8.32 - -
60 ppm0.732 2.24 7.14 93 94

The Inhibitive Effect of 3-Methyl 4-Amino 1,2,4 Triazole on the Corrosion of Copper-Nickel
1266
70 - 30 in NaCl 3% Solution
film, which grows with increasing exposure time. Solu-
tion analysis revealed that the MATA excellently control
the denickelification of monel in NaCl 3% solution.
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