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Materials and Corrosion 54, 251–258 (2003) Crude oil storage tanks 251

Corrosion inhibition of steel in crude oil storage


tanks
Korrosionsinhibierung von Stahl in Rohöllagertanks
M. A. Khalifa, M. El-Batouti*, F. Mahgoub,
A. Bakr Aknish

The corrosion behavior of steel in water from certain oil fields Mit Hilfe potentiodynamischer Messungen bei pH 5,9 wurde das
with various organic inhibitors was studied by applying potentio- Korrosionsverhalten von Stahl in Wasser aus bestimmen Ölfeldern
dynamic technique at pH 5.9. The inhibitors which were used in- bei Zugabe verschiedener organischer Inhibitoren untersucht. Die
clude 2-methylbenzimidazole (I), 2-mercaptobenzimidazole (II), 2- eingesetzten Inhibitoren beinhalten 2-Methylbenzimidazole (I), 2-
mercapto-5-methylbenzimidazole (III), and 2-mercaptothiazole Mercaptobenzimidazole (II), 2-Mercapto-5-Methylbenzimidazole
(IV). The inhibiting efficiency of the different additives was eval- (III), and 2-Mercaptothiazole (IV). Die Inhibitorwirksamkeit der
uated from their anodic and cathodic polarization curves at different verschiedenen Zusätze wurde aus deren anodischen und kathodi-
temperatures. schen Polarisationskurven bei verschiedenen Temperaturen ermit-
A comparative study of curve fitting procedures using the kinetic telt.
thermodynamic model and those utilizing well-known adsorption Eine vergleichende Untersuchung der Kurvenanpassungen mit
isotherms was undertaken. Three types of isotherms were used, Hilfe des kinetisch-thermodynamischen Modells sowie bekannter
Langmuir, Frumkin and Flory-Huggins isotherm. The results Adsorptionsisotherme wurde durchgeführt. Dabei wurden drei Ar-
show that the kinetic-thermodynamic model and Flory-Huggins ten von Isothermen verwendet, die Langmuir-, die Frumkin- und
isotherms are more suitable to fit the data for the four inhibitors, die Flory-Huggins-Isotherme. Die Ergebnisse zeigen, dass das ki-
at all applied temperatures. From the values of binding constants, netisch-thermodynamische Modell und die Flory-Huggings-Iso-
K, the order of inhibitor efficiency is: therme bei allen untersuchten Temperaturen besser geeignet
III > IV > II > I sind, die Daten für die vier Inhibitoren anzupassen.
and thus 2-mercapto-5-methylbenzimidazole was the most effec- Aus den Werten der Bindungskonstanten K ergibt sich die Rei-
tive inhibitor. The thermodynamic parameters obtained for all the henfolge der Inhibitorwirksamkeit:
compounds used showed low values of Hads, which indicates that III > IV > II > I
the action of these inhibitors is physically adsorptive in nature. Das bedeutet, dass 2-Mercapto-5-Methylbenzimidazol der wirk-
samste Inhibitor war. Die für alle eingesetzten Inhibitoren ermittel-
ten thermodynamischen Parameter zeigten niedrige Werte für Hads,
was darauf schließen lässt, dass die Wirkung dieser Inhibitoren phy-
sikalisch-adsorptiver Natur ist.

1 Introduction 11]. Heterocyclic compounds, such as 2-mercaptobenzothia-


zole [12, 13] and 2-mercaptobenzimidazoles [14, 15] have
Corrosion is a serious problems in oil and gas productions. been used to inhibit corrosion in neutral aqueous solutions.
Both general and localized corrosion types are encountered in The choice of inhibitors was based upon three considerations.
this industry. The extent of the problems depends on the fluid The first is that these derivatives of the investigated imidazole
composition, e.g. oil types, oil/water ratio, water salinity and are organic compounds whose composition and molecular
gas type and content [1]. Water is one of the main factors af- structure provide good conditions for inhibition. Secondly,
fecting the corrosion rates. It is found in some degree with all they are intermediary or secondary products of reactions in
the petroleum produced [2 – 4]. The use of corrosion inhibitors the pharmaceutic industry and, therefore, were relatively
in petroleum production is the most common method for cor- cheap. Thirdly, they are environmentally friendly [16]. The
rosion control in these highly corrosive environments. imidazole molecule shows three different anchoring sites sui-
The compounds most often used as corrosion inhibitors are table for surface bonding, the nitrogen atom with a lone Sp2
nitrogen containing organic compounds (aliphatic and aro- electron pair, the C(4)H-C(5)H „edge“, and the aromatic ring
matic amines) [5 – 7], oxygen, and sulfur-containing com- [17]. The present study aims to throw more light on the effect
pounds [8 – 9]. Several of these compounds have been studied of temperature on the corrosion rate of mild steel in produced
as corrosion inhibitors for steel in different environments [10, water in the presence and absence of the inhibitors. Polariza-
tion technique is used in order to calculate the thermodynamic
and activation parameters of the dissolution process of mild
steel. The application of kinetic-thermodynamic model to ob-
* M. El-Batouti, M. A. Khalifa tain thermodynamic (adsorption equilibrium values and hence
Chemistry Department, Faculty of Science, Alexandria Univer- DGads, DHads, and DSads) parameters is used to describe the
sity, P.O. 426, Alexandria 21321 (Egypt) corrosion characteristics of steel surface and the effectivensss
F. Mahgoub, A. Bakr Aknish of these compounds as inhibitors from a quantitative point of
University of Alexandria Research Center, Alexandria (Egypt) view.

F 2003 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 0947-5117/03/0404-0251$17.50þ.50/0


252 Khalifa, El-Batouti, Mahgoub and Bakr Aknish Materials and Corrosion 54, 251–258 (2003)

Table 1. Chemical composition of steel specimens


Tabelle 1. Chemische Zusammensetzung der Stahlproben

Elements C S Mn P Si Ni Cr V Al

Amount% 0.14 0.035 0.56 0.032 0.17 0.01 0.01 0.01 0.031

2 Experimental procedures Table 2. Analysis of the produced water of the oil field
Tabelle 2. Analyse des erzeugten Wassers des Ölfeldes
The efficiency of imidazole derivatives as steel corrosion
inhibitors in water was investigated using electrochemical Corrosive Elements (ppm) Produced Water
methods based on potentiodynamic polarization, the Tafel ex-
trapolation measurements were achieved by connecting the – Total dissolved solids (TDS) 8190
– Sodium as Naþ 4840
cell to a working potentiostat model MP87. The cell has three – Potassium as Kþ 570
electrodes; the working electrode which is the electrode to be – Calcium as Ca2þ 980
2
studied, the counter electrode, which serves to supply the re- – Magnesium as Mg2þ 2 267
quired current, and the reference electrode, which acts as a 
– Chloride as Cl 8020
probe suppying the feedback signal. Commercial mild steel – Bicarbonate as HCO 3 759
with chemical composition recorded in Table 1 was used as – Sulphate SO24 518
working electrode. – Carbon dioxide (CO2) 37
– Hydrogen sulphide (H2S) 384
Specific conductivity 3200 ls/cm at 25 8C
2.1 Test solution
pH 5.9
The analysis of the produced water of the oil field is shown
in Table 2. The test solution must be free of oils and greases.
Stock solutions of the inhibitors were prepared in dimethyl In general, the variations of the percentage inhibition with
formamide. All test solutions contained 10 vol. percent of di- the logarithmic concentration of the four inhibitors at different
methyl formamide to maintain inhibitors completely soluble. temperatures, have the characteristic of adsorption mechan-
ism for the inhibition process. Inspection of the curves ob-
tained shows that the inhibition efficiency decreases as the
2.2 Working procedure temperature increases from 25 to 60 8C and the corrosion
The sample was metallographically prepared and ultrasoni-
cally cleaned. Potentiodynamic studies were conducted by
connecting the polarization cell to the potentioscan. The stea-
dy state open circuit corrosion potential was recorded and the
sweeping rate used in this study was 0.03 volt/min. Experi-
ments were carried out under aerated condition and thermo-
stated at the required test temperature. The effect of addition
of varying concentrations of the different investigated inhibi-
tors on the current-potential curves was tested at 25, 40, 50
and 60 8C.
The chemical formulas of different inhibitors investigated
are shown in the schematic diagram of Fig. 1. The four com-
pounds were obtained from Aldrich chemical company. The
purity of 2-mercapto-5-methylbenzimidazole was 99%, and
the others were 98% pure.

3 Results and discussion

3.1 Tafel-extrapolation-measurements

Fig. 2 – 5 show polarization curves for steel in the produced


water in absence and presence of varying concentrations of the
four compounds at 25 8C. The cathodic and anodic polariza-
tion curves obtained from the four compounds exhibit Tafel-
type behaviour. It is clear that the corrosion rate (Icorr) de-
creases as the concentration of the inhibitor was increased.
The results also indicated that the presence of these inhibitors
retarded both the dissolution process and the cathodic process
of the metal and that these compounds act as mixed type in- Fig. 1. The structure of the four different investigated compounds
hibitors which retard mainly the anodic reaction. Abb. 1. Struktur der vier untersuchten Verbindungen
Materials and Corrosion 54, 251–258 (2003) Crude oil storage tanks 253

Table 3. Electrochemical parameters of the corrosion of mild steel in the produced water of oil field in the presence and absence of
different concentrations of 2-mercapto-5-methylbenzimidazole (III) at 25 8C
Tabelle 3. Elektrochemische Parameter der Korrosion von unlegiertem Stahl in dem erzeugten Wasser des Ölfeldes bei An- bzw. Ab-
wesenheit von verschiedenen Konzentrationen an 2-Mercapto-5-Methylbenzimidazol (III) bei 25 8C

Conc. (M)  Ecorr(V) Icorr lA/cm3 %Inhibi. ba (V/decad)  bc (V/decade)


0.0 M 0.800 112.2 0.00 0.082 0.113
1  108 0.760 108.49 3.30 0.085 0.115
1  107 0.750 102.77 8.40 0.083 0.117
7
5  10 0.725 91.46 18.48 0.083 0.121
6
1  10 0.735 75.89 32.36 0.085 0.120
5  106 0.710 66.29 40.91 0.085 0.122
1  105 0.70 56.32 49.88 0.090 0.122
4
1  10 0.672 48.11 57.12 0.090 0.120
3
1  10 0.650 42.17 62.41 0.094 0.120
1  102 0.625 39.62 64.68 0.090 0.125

Table 4. Electrochemical parameters of the corrosion of mild steel in the produced water of oil field in the presence and absence of
different concentrations of 2-mercapto-5-methylbenzimidazole (III) at 40 8C
Tabelle 4. Elektrochemische Parameter der Korrosion von unlegiertem Stahl in dem erzeugten Wasser des Ölfeldes bei An- bzw. Ab-
wesenheit von verschiedenen Konzentrationen an 2-Mercapto-5-Methylbenzimidazol (III) bei 40 8C

Conc. (M)  Ecorr (V) Icorr lA/cm2 %Inhibi. ba (V/decad)  bc (V/decade)


0.0 M 0.810 137.57 2.60 0.084 0.112
8
1  10 0.800 137.57 2.60 0.084 0.112
7
1  10 0.790 133.72 5.33 0.083 0.115
5  107 0.772 123.14 12.82 0.081 0.116
1  106 0.760 109.61 22.40 0.083 0.122
6
5  10 0.740 97.16 31.21 0.085 0.120
5
1  10 0.726 85.11 39.74 0.090 0.120
1  104 0.700 73.85 47.73 0.092 0.122
3
1  10 0.680 64.56 54.28 0.094 0.125
2
1  10 0.660 62.48 55.70 0.092 0.125

rate increases which increasing the temperature. At a given capto-5-methylbenzimidazole (III) at 25, 40, 50, and 60 8C.
inhibitor concentration, the protection efficiency changes ac- The curves have characteristic S-shaped adsorption isotherms.
cording to the following order Inspection of these curves show that the corrosion is greatly
reduced, and the efficiency increases as the concentration of
III > IV > II > I the inhibitor increases. This is also depicted from Fig. 7 which
shows the relation between the corrosion current density (Icorr)
A typical corrosion behavior of the four compounds may be and the logarithm of inhibitor concentration at the given tem-
explained by considering the behavior of compound III which perastues. Fig. 8 shows that the Ecorr increases (anodic shift)
was found to have the highest corrosion protection efficiency. by increasing inhibitor concentration. In this case the highest
The electrochemical parameters of the steel in the produced Ecorr value was observed at a concentration of 102 M. On the
water of the oil field in the presence and absence of different other hand, increasing the temperature was found to decrease
concentrations of 2-mercapto-5-methylbenzimidazole(III) are the Ecorr value to about  0.83 volt at 60 8C and an inhibitor
given in Tables 3 – 6. It is clear that the corrosion rate (Icorr) concentration of 108 M.
decreases with increasing the concentration of inhibitor The effect of the inhibitor on the electrochemical para-
(III) in the medium. Fig. 6 gives the variation of percentage meters of the steel in the produced water, as given in Tables
inhibition with the logarithm of the concentration of 2-mer- 3 – 6, shows two important characteristics:
254 Khalifa, El-Batouti, Mahgoub and Bakr Aknish Materials and Corrosion 54, 251–258 (2003)

Table 5. Electrochemical parameters of the corrosion of mild steel in the produced water of the oil field in the presence and absence of
different concentrations of 2-mercapto-5-methylbenzimidazole (III) at 50 8C
Tabelle 5. Elektrochemische Parameter der Korrosion von unlegiertem Stahl in dem erzeugten Wasser des Ölfeldes bei An- bzw. Ab-
wesenheit von verschiedenen Konzentrationen an 2-Mercapto-5-Methylbenzimidazol (III) bei 50 8C

Conc. (M)  Ecorr Icorr lA/cm2 %Inhib ba (V/decade)  bc (V/decade)


0.0 M 0.815 158.50 0.00 0.078 0.098
1  108 0.816 155.36 1.98 0.085 0.112
1  107 0.803 152.23 3.95 0.084 0.110
7
5  10 0.792 140.66 11.25 0.085 0.110
6
1  10 0.778 132.49 16.41 0.085 0.113
5  106 0.759 115.37 27.21 0.087 0.116
1  105 0.750 104.71 33.93 0.090 0.120
4
1  10 0.725 90.32 43.01 0.090 0.123
3
1  10 0.700 97.43 49.88 0.092 0.123
1  102 0.670 77.18 51.30 0.90 0.124

Table 6. Electrochemical parameters of the corrosion of mild steel in the produced water of the oil field in the presence and absence of
different concentrations of 2-mercapto-5-methylbenzimidazole (III) at 60 8C
Tabelle 6. Elektrochemische Parameter der Korrosion von unlegiertem Stahl in dem erzeugten Wasser des Ölfeldes bei An- bzw. Ab-
wesenheit von verschiedenen Konzentrationen an 2-Mercapto-5-Methylbenzimidazol (III) bei 60 8C

Conc. (M)  Ecorr Icorr lA/cm2 %Inhibi. ba (V(decade)  bc (V/decade)

0.0 M 0.840 199.50 0.00 0.077 0.097


8
1  10 0.830 197.10 1.20 0.080 0.119
7
1  10 0.820 193.71 2.90 0.082 0.118
5  107 0.810 183.99 7.77 0.084 0.116
1  106 0.797 173.16 13.20 0.087 0.210
6
5  10 0.787 153.81 22.90 0.085 0.240
5
1  10 0.770 139.33 30.16 0.085 0.230
1  104 0.759 125.60 37.04 0.087 0.230
3
1  10 0.730 112.20 43.75 0.090 0.125
2
1  10 0.700 110.72 44.50 0.094 0.125

1 – The first one is that, on increasing the concentration of 4 Adsorption isotherm analysis
the inhibitor, there is a small effect on the slopes of the catho-
dic and anodic Tafel lines indicating that the adsorption of the A comparative study of the data for the investigated com-
2-mercapto-5-methylbenzimidazole molecules at the steel pounds by applying the Frumkin, Flory-Huggins and Kinetic-
surface retards the corrosion by the screening effect only thermodynamic equations are given in Table 7. The data show
and there is no effect of the inhibitor on the mechanism of certain agreement between the values of the binding constant
the corrosion process. “K”of the inhibitors molecules obtained from the Flury-Hug-
2 – The second characteristic is the strong effect of the in- gins and Kinetic-thermodynamic model at all temperatures
crease in the concentration of the inhibitor on the corrosion used. However, these values are in poor agreement with the
potential Ecorr of the steel in the produced water. Fig. 8 indi- “K” values obtained by applying the Frumkin model. For
cates that there is a shift of about 0.18 Volt toward more po- all the investigated compounds, there is also poor agreement
sitive values in the corrosion potential Ecorr of the steel due to between the values of the number of active sites occupied by
the increase of inhibitor concentration from 0.0 to 102 M. one inhibitor molecule (1/y) obtained from the fit of the Ki-
This large effect of the inhibitor on the corrosion potential netic-thermodynamic model (Table 7) and the values of the
Ecorr of the steel may be explained on the basis of the adsorp- size ratio parameter (x), (number of surface water molecules
tion of 2-mercapto-5-methylbenzimidazole compound at the replaced by a single inhibitor molecule), obtained from the fit
steel-solution interface. of the Flory-Huggins isotherm. It is also clear that for all the
Materials and Corrosion 54, 251–258 (2003) Crude oil storage tanks 255

Fig. 2. Polarization curves of mild steel in the produced water of the oil field containing different concentrations of 2-Methylbenzimi-
dazole at 25 8C
Abb. 2. Polarisationskurven für unlegierten Stahl in dem erzeugten Wasser des Ölfeldes mit verschiedenen Konzentrationen an 2-Me-
thylbenzimidazol bei 25 8C

Fig. 3. Polarization curves of mild steel in the produced water of the oil field containing different concentrations of 2-Mercaptobenzi-
midazole at 25 8C
Abb. 3. Polarisationkurven für unlegierten Stahl in dem erzeugten Wasser des Ölfeldes mit verschiedenen Konzentrationen an 2-Mer-
captobenzimidazol bei 25 8C

investigated compounds, the data don’t fit to Langmiur iso- sorbed molecules and the metal surface are stronger at low
therm at all the temperatures used. The Kinetic-thermody- temperatures (giving better inhibition efficiency).
namic model presents a good fit to the corrosion data obtained
primarily from a kinetic type experiment, leading to the design
of a better class of inhibitors for a given metal and chemical 5 Application of kinetic-thermodanymic model
environment.
As can be seen from Table 7, the value of the binding con- A comparative study of the thermodynamic parameters of
stant “K” decreased with increasing the temperature. This the four investigated compounds by the application of the
clearly indicates that the electrical interactions between ad- thermodynamic model is presented in Table 8. From these
256 Khalifa, El-Batouti, Mahgoub and Bakr Aknish Materials and Corrosion 54, 251–258 (2003)

Fig. 4. Polarization curves of mild steel in the produced water of the oil field containing different concentrations of 2-Mercapto-5-Methyl-
benzimidazole at 25 8C
Abb. 4. Polarisationskurven für unlegierten Stahl in dem erzeugten Wasser des Ölfeldes mit verschiedenen Konzentrationen an 2-Mer-
capto-5-Methylbenzimidazol bei 25 8C

Fig. 5. Polarization curves of mild steel in the produced water of the oil field containing different concentrations of 2-Mercaptobenzothia-
zole at 25 8C
Abb. 5. Polarisationskurven für unlegierten Stahl in dem erzeugten Wasser des Ölfeldes mit verschiedenen Konzentrationen an 2-Mer-
captobenzothiazol bei 25 8C
Materials and Corrosion 54, 251–258 (2003) Crude oil storage tanks 257

Fig. 6. Variation of the percentage inhibition with the logarithmic


concentration of 2-mercapto-5-methylbenzimidazole at different Fig. 8. Variation of the Ecorr (v) with the logarithmic concentration
temperatures of 2-mercapto-5-methylbenzimidazole at different temperatures
Abb. 6. Veränderung der prozentualen Inhibierung mit dem Loga- Abb. 8. Veränderung von Ecorr mit dem Logarithmus der Konzen-
rithmus der Konzentration von 2-Mercapto-5-Methylbenzimidazol tration von 2-Mercapto-5-Methylbenzimidazol bei verschiedenen
bei verschiedenen Temperaturen Temperaturen

The protection efficiency of the four studied compounds


obtained at a temperature of 25 8C are summarized in Table 9
and may be further explained as follows:
At a given concentration of the inhibitors, the protection
efficiency decreases in the order.

III > IV > II > I

Compound (III) and (IV) are structurally related except that


compound (III) has an extra methyl group attached to the phe-
nyl ring. This methyl group is expected to increase the elec-
tron density and accordingly compound (III) is expected to
have higher protection efficiency than compound (IV). How-
ever, since the S atom has a higher inhibition efficiency com-
pared to the N atom, the presence of S in compound IV is ex-
pected to increase its relative protection efficiency. The com-
bined effects of these two factors resulted in nearly equally
values of protection efficiency for the two compounds (III
and IV). In this approach we have used an empirical method
in which each functional group of an inhibitor molecule con-
Fig. 7. Variation of Icorr with the logarithmic concentration of 2- tributes a unique, independent, and additive increment of cor-
mercapto-5-methylbenzimidazole at different temperatues rosion inhibition. This is the approach proposed by Sastri et al.
Abb. 7. Veränderung von Icorr mit dem Logarithmus der Konzen- [18] and Wang et al. [19] and could also be applied to explain
tration von 2-Mercapto-5-Methylbenzimidazol bei verschiedenen the relative corrosion behavior of compounds I and II.
Temperaturen

6 References

data, it is possible to conclude that the thermodynamic para- [1] A. A. El-Hosary, R. M. Salem, A. O. Abdelfattah, 85EIC,
meters obtained from all compounds show low values Ann. Univ. Ferrara, N.S., Sez. V, 1995, 10, 1269.
ofDHoads , indicative that these compounds are physically ad- [2] C. C. Nathan, Corrosion Inhibitors, 1973 63.
sorptive in nature. The free energy of adsorption DGoads , for [3] H. E. Green Well, Corrosion 1963, 9, 307.
[4] K. D. Efird, R. J. Jasinski, Corrosion 1989, 45, 165.
the investigated compounds changes in the following order: [5] H. Kaesche, N. Hackerman, J. Electrochem. Soc. 1958, 105,
191.
IV > III > II > I [6] B. E. Blomgren, J. O. M. Bockris, J. Phys. Chem. 1959, 63,
1459.
258 Khalifa, El-Batouti, Mahgoub and Bakr Aknish Materials and Corrosion 54, 251–258 (2003)

Table 7. The curve fitting of the data of compounds I, II, III and IV to Frumkin, Flory-Huggins and Kinetic-Thermodynamic model
Tabelle 7. Kurvenanpassung der Daten der Verbindungen I, II, III und IV an das Frumkin-, das Flory-Huggins- und das kinetisch-thermo-
dynamische Modell

Comp. Temp. 8C Frumkin Flory-Huggins Kinetic-Therm.


a K x K 1/y K

Comp. (I) 25  1.2 6.3  104 – – 1.8 1.1  104


40 – – 2.8 9.0  103 1.79 9.3  103
50 – – 2.0 7.0  103 1.77 6.1  103
60  0.7 4.6  103 – – 1.64 2.9  103
Comp. (II) 25  0.85 6.3  104 3.4 2.0  104 1.8 1.6  104
40  0.8 3.1  104 2.7 1.8  104 1.8 1.1  104
50  0.65 1.2  104 2.3 1.0  104 1.77 7.1  103
60 – – – – 1.64 3.5  103
Comp. (III) 25  1.15 1.2  106 4.6 2.7  105 1.95 1.26  105
40  1.25 6.4  105 – – 2.06 4.3  104
50  1.1 1.9  105 5.2 3.8  104 2.02 2.7  104
60  1.05 1.0  105 5.3 1.8  104 1.86 2.0  104
Comp. (IV) 25  1.0 8.5  105 3.85 1.6  105 1.85 1.0  105
40  1.2 5.5  105 3.6 6.9  104 1.8 6.0  104
50  1.5 3.8  105 3.0 6.6  104 1.77 3.6  104
60  1.4 2.8  105 – – 1.73 2.5  104

Table 8. Thermodynamic parameters of the compounds I – IV ob- Table 9. Inhibition percent of the four inhibitors at concentrations
tained by applying the Kinetic-thermodynamic model of 1  107, 1  105 and 1  102 M and at a temperature of
Tabelle 8. Durch Anwendung des kinetisch-thermodynamischen 25 8C
Modells ermittelten thermodynamischen Parameter der Verbindun- Tabelle 9. Prozent der Inhibierung für die vier Inhibitoren bei Kon-
gen I – IV zentrationen von 1  107, 1  105 und 1  102 M und bei einer
Temperatur von 25 8C
Compounds DHoads DSiads DGoads
(KJ/mol) (KJ/mol) (KJ/mol) Conc. (M) %Inhib. (I) %Inhib. (II) %Inhib. (III) %Inhib. (IV)
7
I  29.9  21.6  23.5 1  10 1.96 2.11 8.40 6.23
II  34.3  24.8  26.9 1  105 24.54 28.42 49.88 48.40
III  38.6  33.3  28.7 1  102 48.22 55.16 64.68 63.39
IV  39.0  33.2  29.1

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and Technology, Plenum Press, New York 1970, 1, 147.
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