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Vol. 8. Issue 6.
Pages 5314-5324 (November - December 2019)
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Vol. 8. Issue 6.
Pages 5314-5324 (November - December 2019)
Original Article
DOI: 10.1016/j.jmrt.2019.08.052
Open Access
Rosuvastatin drug as a green and effective inhibitor for corrosion of mild steel in HCl and H2SO4 solutions
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M.R. Gholamhosseinzadeha, H. Aghaiea, M. Shahidi Zandib,
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meshahidizandi@gmail.com

Corresponding author.
, M. Giahic
a Department of Chemistry, Science and Research Branch, Islamic Azad University, Tehran, Iran
b Department of Chemistry, Kerman Branch, Islamic Azad University, Kerman, Iran
c Depertment of Chemistry, Lahijan Branch, Islamic Azad University, Lahijan, Iran
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Tables (5)
Table 1. Polarization parameters and the corresponding inhibition efficiencies for mild steel in 1.0 M HCl and 0.5 M H2SO4 containing different concentrations of studied drug at 25 0C.
Table 2. Impedance parameters and the corresponding inhibition efficiency values for mild steel in 1.0 mol.L−1 HCl and 0.5 mol.L−1 H2SO4 containing different concentrations of studied drug at 25 ºC.
Table 3. Effect of temperature on the corrosion parameters of mild steel in 1.0 M HCl and 0.5 MH2SO4 containing drug.
Table 4. Activation and thermodynamic parameters of adsorption obtained by potentiodynamic polarization measurements for mild steel in 1.0 mol.L−1 HCl and 0.5 mol.L−1 H2SO4 solution in the absence and presence of 600 ppm of drug.
Table 5. The values of Kads and ΔGads corresponding to polarization, EIS and Tafel data in 1.0 M HCl and 0.5 M H2SO4 solution.
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Abstract

The effect of rosuvastatin drug on the corrosion behavior of mild steel in 1.0 M HCl and 0.5 M H2SO4 solutions was investigated using potentiodynamic polarization, electrochemical impedance spectroscopy (EIS) and Fourier transform infrared (FTIR) techniques. The inhibition efficiency (IE) was found to increase with increasing rosuvastatin concentration up to 600 ppm and then it was decreased. The maximum inhibition efficiency of 92% has been achieved at 600 ppm rosuvastatin concentration in both HCl and H2SO4 solutions. The effect of temperature on the rate of corrosion in the absence and presence of drug was also studied. Some thermodynamic parameters were computed from the effect of temperature on corrosion and inhibition processes. Adsorption of the drug was found to obey Langmuir adsorption isotherm. Potentiodynamic polarization measurements indicated that the inhibitor were of mixed type. The inhibition efficiency values obtained from potentiodynamic polarization showed a reasonable agreement with those arising from EIS measurements.

Keywords:
Rosuvastatin drug
Green inhibitor
Electrochemical impedance spectroscopy
Potentiodynamic polarization
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1Introduction

Acid solutions are widely used in industry, such as acid pickling, industrial acid cleaning, acid descaling and oil well acidizing. Because of the general aggressivity of acid solutions, inhibitors are commonly used to reduce the corrosive attack on metallic materials [1–14]. Inhibitors are substances which, when added in small concentrations to corrosive media, decrease or prevent the reaction of the metal with the media. However, the use of these compounds has been questioned lately, due to the several negative effects that they have caused in the environment. Thus, the development of the novel corrosion inhibitors of natural source and non-toxic or low-toxic type has been considered to be more important and desirable [1–4]. Recently researchers have paid attention to the development of drugs as inhibitors for metallic corrosion [4–12]. Abdallah has described the inhibition effect of ampicillin, cloxacillin, flucloxacillin and amoxicillin in 2 M HCl solution by the formation of stable complex on the aluminium surface [5]. Eddy et al. have performed research in the field of penicillins as mild steel corrosion inhibitors [6,7]. They have explained the inhibitory action of penicillin G and penicillin V in terms of their physical adsorption on the surface of mild steel. Fouda et al. have investigated the effect of ampicillin and benzyl penicillin (penicillin G) on the corrosion behavior of 304 stainless steel in 1.0 M HCl solution [8]. The corrosion inhibition of mild steel in 1 M sulfuric acid using amoxicillin as inhibitor has been investigated by Kumar et al. [9].

The present paper describes the study of the inhibition action of rosuvastatin on corrosion of mild steel in 1.0 M HCl and 0.5 M H2SO4 solutions using potentiodynamic polarization and electrochemical impedance spectroscopy (EIS) techniques.

2Materials and methods2.1Materials

The concentrated acid solutions (HCl and H2SO4) were purchased from Merck Company. The rosuvastatin drug was obtained from Sigma–Aldrich and used without any further purification. Fig. 1 shows the chemical structure of rosuvastatin drug. The employed working electrodes (WEs) with surface area of 100 mm2 were prepared from mild steel. The chemical composition of mild steel was comprised of (wt%): C (0.15), Mn (0.73), Si (0.72) and Fe (balance).

Fig. 1.

Structure of rosuvastatin drug.

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2.2Methods

Potentiodynamic polarization and EIS measurements were used to study the corrosion behavior of mild steel in 1.0 M HCl and 0.5 M H2SO4 solutions without and with addition of rosuvastatin at different concentrations. The specimens were connected to a copper wire at one end, and then sealed using epoxy resin with the other end exposed as the WE surface. Before performing experiments, the WE surface was abraded by wet abrasive papers through 600-2500-grade, washed with distilled water, degreased with ethanol and finally dried in air.

Potentiodynamic polarization and EIS experiments were conducted using a potentiostat/galvanostat Autolab 302 N (Eco Chemie, Netherlands) supported by a frequency response analyzer FRA-2 and Nova 1.6 software. A platinum rod with area of 100 mm2 was used as the counter electrode (CE) and a saturated (KCl) Ag/AgCl electrode as reference electrode. The electrochemical measurements were conducted in a three-electrode arrangement. To obtain the stabilized open circuit potential (OCP), the samples were immersed 30 min in the solution before measurements.

A sinusoidal potential perturbation of 10 mV versus OCP in the 100 kHz–10 mHz frequency range was used in the EIS measurements. The Nyquist plots of the impedance data were analyzed with Nova 1.9 software.

In potentiodynamic polarization study, polarization curves were recorded from −250 to +250 mV with respect to OCP at a scan rate of 1 mV/s and Nova software was used for determination of corrosion current densities and polarization parameters.

Fourier transform infrared (FTIR) spectra were recorded in a Bruker Tensor 27 spectrophotometer (Bruker, Ettlingen, Germany) which extended from 700 to 4000 cm−1, using KBr disk technique. A small portion of each of the pure drugs was mixed with KBr and pressed into a disk. Then the FTIR spectra were recorded. The steel specimens (11.3 cm in diameter and 0.5 cm in thickness) were abraded using abrasive papers (grades 600–2500), washed with distilled water and acetone and finally dried at room temperature. After 24 h of immersion in 1.0 M HCl and 0.5 M H2SO4 solutions in presence of inhibitor; the specimens were cleaned with distilled water and dried at room temperature. Then, the thin adsorbed film on the steel surface was rubbed with a small amount of KBr powder in an agate mortar and a KBr disk was prepared using this powder.

3Results and discussion3.1Potentiodynamic polarization

Fig. 2 shows the potentiodynamic polarization curves of mild steel in 1.0 M HCl and 0.5 M H2SO4 solutions in the absence and presence of various concentrations of rosuvastatin drug.

Fig. 2.

Polarization curves for mild steel in (a) 1.0 M HCl and (b) 0.5 M H2SO4 solutions in the absence and presence of different concentrations of of rosuvastatin drug at 25 °C.

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It is obvious that the cathodic branch displays a typical Tafel behavior. This makes it possible, as will be seen, to make an accurate evaluation of the cathodic Tafel slope (βc) as well as corrosion currents (jcorr) by the Tafel extrapolation method. On the other hand, the anodic polarization curve does not display the expected log/linear Tafel behavior over the complete applied potential range. The curvature of the anodic branch may be attributed to the deposition of the corrosion products or impurities in the steel (e.g., Fe3C) to form a non-passive surface film [15]. Therefore, due to the absence of linearity in the anodic branch, it is impossible to obtain the accurate evaluation of the anodic Tafel slope by Tafel extrapolation of the anodic branch.

It has been shown that in the Tafel extrapolation method, the use of both the anodic and cathodic Tafel regions is undoubtedly preferred over the use of only one Tafel region [16]. However, the corrosion rate can also be determined by Tafel extrapolation of either the cathodic or anodic polarization curve alone. If only one polarization curve alone is used, it is generally the cathodic curve which usually produces a longer and better defined Tafel region (as in our case here).

For the calculation of anodic current density from the experimental data the Tafel line of the cathodic polarization curve was first extended back to zero overvoltage, and then the anodic current density was calculated using equation [16]:

where the subscripts a and c refer the anodic and cathodic directions, respectively. Thus, the anodic current density is the sum of the experimentally observed anodic current density and the extrapolated cathodic current density.

The relevant parameters are listed in Table 1 as corrosion current density (icorr), corrosion potential (Ecorr), anodic and cathodic Tafel slopes (βa, βc). The corrosion current density decreased as the concentration of inhibitor increased up to 600 ppm. Addition of drug to acid media affected both cathodic and anodic branches of the potentiodynamic polarization curves. Therefore, this drug behaved as mixed inhibitor.

Table 1.

Polarization parameters and the corresponding inhibition efficiencies for mild steel in 1.0 M HCl and 0.5 M H2SO4 containing different concentrations of studied drug at 25 0C.

C/ppm  icorr/μA.cm−2  −Ecorr/mV  βa/mV.decade−1  βc/mV.decade−1  IEP(%) 
Blank:HCl           
433  492  72  122  – 
100  91  492  47  106  79 
200  87  487  52  111  80 
400  52  482  49  110  88 
600  34  470  51  115  92 
800  44  476  55  110  90 
Blank:H2SO4           
699  493  82  142  – 
100  132  474  48  105  81 
200  99  476  46  101  86 
400  84  470  45  106  89 
600  55  466  51  93  92 
800  74  476  57  106  89 

Table1 also presents values of the corrosion inhibition efficiency (IE) for which the expression in this case is [17]:

where icorr and icorr' are corrosion current densities in the uninhibited and inhibited cases, respectively. An increase in the inhibitor concentration up to 600 ppm increased the IE value. These results also show that rosuvastatin acts as effective inhibitor.

It can be observed that an increase in the concentration of inhibitor causes a decrease in the current density value (icorr') and a corresponding increase in the IE value. This situation is a result of increasing surface coverage (θ) by the inhibitor, leading to the equation of θ = IE/100 [18].

According to surface coverage values an attempt was made to test the Langmuir, Temkin and Frumkin isotherms. The Langmuir adsorption isotherm was found to fit well with the experimental data (Fig. 3), which can be expressed as:

or:
where θ is the surface coverage, C is the inhibitor concentration and K is the adsorption equilibrium constant. The plots of C/θ versus C for the drug (Fig. 3) yielded straight line with correlation coefficient close to 1.0, confirming that the adsorption of drug is well described by the Langmuir adsorption isotherm.

Fig. 3.

Langmuir adsorption isotherm of the inhibitor in (a) 1.0 M HCl and (b) 0.5 M H2SO4 solutions by using surface coverage values calculated by Tafel polarization results.

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3.2Electrochemical impedance spectroscopy

Nyquist diagrams of EIS for mild steel in 1.0 M HCl and 0.5 M H2SO4 solutions in the absence and presence of various concentrations of drug are shown in Fig. 4. It is apparent from Fig. 4 that the impedance response of mild steel changes significantly with increasing the concentration of drug up to 600 ppm.

Fig. 4.

Nyquist plots for mild steel in (a) 1.0 M HCl and (b) 0.5 M H2SO4 solutions in the absence and presence of different concentrations of rosuvastatin drug at 25 °C.

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Fig. 5 shows the electrical equivalent circuit employed to analyze the impedance plots. In this figure, Rs is the solution resistance and Rct is the charge transfer resistance. The impedance of the constant phase element (CPE) is defined as follows [19,20]:

where Y0 is the CPE constant (F.cm−2.sn-1 or sn.Ω−1.cm−2), j equals −1, ω is the angular frequency and n is the CPE exponent. The correct equation to convert the CPE constant, Y0, into the double layer capacitance, Cdl, is the following equation [21]:
where ωmax is the angular frequency at which the imaginary component of the impedance is maximum. Table 2 lists impedance parameters in the absence and presence of different concentrations of drug. As it can be seen from Table 2, the Rct values increased as the concentration of inhibitor increased up to 600 ppm. On the other hand, the values of Cdl decreased with increasing the inhibitor concentration up to 600 ppm.

Fig. 5.

The equivalent circuit used to fit the experimental data.

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Table 2.

Impedance parameters and the corresponding inhibition efficiency values for mild steel in 1.0 mol.L−1 HCl and 0.5 mol.L−1 H2SO4 containing different concentrations of studied drug at 25 ºC.

C /ppm  Rs/Ω cm2  Rct/Ω cm2  106 Y0/F cm−2 sn−1  Cdl/μF cm−2  IEEIS (%) 
Blank:HCl             
1.2  38  0.895  159  87.8  – 
100  4.9  100  0.888  86  47.1  62 
200  1.5  150  0.872  105  46.2  74 
400  1.2  196  0.891  72  43.0  81 
600  1.3  326  0.893  59  36.8  88 
800  5.0  245  0.867  95  52.8  84 
Blank:H2SO4             
1.8  24  0.906  230  134.1  – 
100  1.4  108  0.924  56  37.0  78 
200  1.8  158  0.926  50  34.1  85 
400  1.5  174  0.926  41  27.6  86 
600  1.7  249  0.918  45  26.1  90 
800  1.3  181  0.918  48  31.4  87 

Inhibition efficiencies in Table 2 were calculated through the following expression:

where Rct and Rct' represent the charge transfer resistance, before and after addition of the inhibitor to the corrosion media, respectively. Inhibition efficiencies increased with increasing the concentration of inhibitor up to 600 ppm and a further increase in the inhibitor concentration decreased the inhibition performance of the inhibitor. The IE values obtained from the EIS technique (Table 2) are in good agreement with those obtained from the polarization method (Table 1).

The decrease of the inhibition efficiency as the concentration of the inhibitor increases beyond the optimal value is consistent with the results obtained from the polarization method and might be due to the saturation of the metallic surface with inhibitor molecules, which also could lead to a deterioration of the layer of the inhibitor on the steel surface [22].

Plots of the data for each isotherm showed the EIS data are agreed with the Langmuir isotherm (Fig. 6).

Fig. 6.

Langmuir adsorption isotherm of the inhibitor in (a) 1.0 M HCl and (b) 0.5 M H2SO4 solutions by using surface coverage values calculated by EIS results.

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3.3Temperature effect and thermodynamic parameters

In order to evaluate the adsorption of inhibitor and to calculate activation energy and thermodynamic parameters of the corrosion process of mild steel in acidic media, potentiodynamic polarization measurements were performed in the temperature range of 25–55 ºC in the absence and presence of various concentrations of drug. The polarization curves at different acid media in the absence and presence of 600 ppm drugare illustrated in Figs. 7 and 8, respectively. The corrosion parameters at different acid media and temperatures are listed in Table 3. The results obtained from polarization curves showed an increase in current density and a decrease in IE% with increasing temperature. Generally, the reduction of the inhibition efficiency with increasing temperature may be explained by the fact that the time lag between the process of adsorption and desorption of inhibitor molecules over the metal surface is becoming shorter with increasing temperature [23]. Hence, the metal surface remains exposed to the acid environment for a longer period, thereby increasing the rate of corrosion with increasing temperature and therefore IE% falls at elevated temperatures.

Fig. 7.

Effect of temperature on the polarization curves in 1.0 M HCl solution (a) without inhibitor, (b) in the presence of 600 ppm of drug.

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Fig. 8.

Effect of temperature on the polarization curves in 0.5 M H2SO4 solution (a) without inhibitor, (b) in the presence of 600 ppm of drug.

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Table 3.

Effect of temperature on the corrosion parameters of mild steel in 1.0 M HCl and 0.5 MH2SO4 containing drug.

T/oC/ppm  icorr/μA cm−2  IE%  θ 
Blank:HCl         
25  506  –  – 
  600  23  95  0.950 
35  997  –  – 
  600  56  94  0.940 
45  1608  –  – 
  600  116  93  0.930 
55  3908  –  – 
  600  408  90  0.900 
Blank:H2SO4         
25  532  –  – 
  600  79  85  0.850 
35  1209  –  – 
  600  196  84  0.838 
45  2558  –  – 
  600  436  83  0.830 
55  6161  –  – 
  600  1199  81  0.810 

The inhibition efficiency of the drug showed a slight change with the rise of temperature indicating the stronger adsorption bond of drug on the surface. This was an evidence for chemisorption of the drug. Therefore, it can be deduced that besides physisorption, chemisorption would also be involved.

The dependence of corrosion rate on temperature can be expressed by the Arrhenius equation [24,25]:

where icorr is corrosion current, A is a constant, Ea is the activation energy of the metal dissolution reaction, R is the gas constant and T is the absolute temperature. The Ea values can be determined from the slopes of Arrhenius plots [log icorr versus 1/T (Figs. 9 and 10)]. Calculated activation energies for the corrosion process in the absence and presence of 600 ppm inhibitor are given in Table 4. Activation energy values obtained for the corrosion of mild steel in HCl solution (53.6 kJ.mol−1) agree with those obtained in other studies [24]. An increase in corrosion activation energy in the presence of 600 ppm inhibitor compared to its absence is frequently interpreted as being suggestive of formation of an adsorption film [26,27]. The increase in Ea indicates that the energy barrier for the corrosion interaction is also increased. In other words, the adsorption of the inhibitor on the electrode surface leads to the formation of a physical barrier that reduces the metal reactivity in the electrochemical reactions of corrosion.

Fig. 9.

Arrhenius plots for mild steel in 1.0 M HCl solution in the absence and presence of 600 ppm inhibitor.

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Fig. 10.

Arrhenius plots for mild steel in 0.5 M H2SO4 solution in the absence and presence of 600 ppm inhibitor.

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Table 4.

Activation and thermodynamic parameters of adsorption obtained by potentiodynamic polarization measurements for mild steel in 1.0 mol.L−1 HCl and 0.5 mol.L−1 H2SO4 solution in the absence and presence of 600 ppm of drug.

Drug  Ea (kJ.mol−1Kads (M−1ΔGads (kJ.mol−1ΔHads (kJ.mol−1ΔSads (J.K−1.mol−1
Blank (HCl)  53.58  –  –  –  – 
Rosu  75.79  18975  −34.39  −24.85  34.14 
Blank (H2SO465.73  –  –  –  – 
Rosu  72.71  35088  −35.88  −7.774  94.317 

The value of adsorption equilibrium constant, Kads, is calculated from the reciprocal of the intercept of isotherm line (Fig. 3). The free energy of the adsorption of inhibitor on mild steel surface can be evaluated from the following equation;

where, R is the gas constant and T is the absolute temperature (K). The values of Kads and ΔGoads derived from Langmuir adsorption isotherms for the studied inhibitors (Fig. 3) are given in Table 4. Table 5 summarizes Kads and ΔGoads values obtained through Tafel polarisation and electrochemical impedance measurements. Satisfactory agreement was found between the two methods.

Table 5.

The values of Kads and ΔGads corresponding to polarization, EIS and Tafel data in 1.0 M HCl and 0.5 M H2SO4 solution.

  TafelEIS
Drug  Kads (M−1ΔGads (kJ.mol−1Kads (M−1ΔGads (kJ.mol−1
Rosu (HCl)  18975  −34.36  10152  −32.81 
Rosu (H2SO435088  −35.88  39840  −30.92 

Generally, values of ΔG°ads around −20 kJ mol−1 or less negative are consistent with the electrostatic interaction between charged molecules and the charged metal surface (physisorption); those around −40 kJ mol−1 or more negative involve charge sharing or transfer from organic molecules to the metal surface to form a coordinate type of metal bond (chemisorption) [28]. In the present work, the calculated ΔG°ads values are the intermediate case indicating that the adsorption of inhibitor molecules is not merely physisorption or chemisorption but obeying a comprehensive adsorption (physical and chemical adsorption).

Another form of Langmuir equation may be expressed as below [29]:

where θ is surface coverage, ΔSads is entropy of adsorption, C is concentration, R is gas constant, T is absolute temperature, and ΔHads is enthalpy of adsorption.

The plot of ln(θ/(1-θ)) versus 1/T at constant additive concentration gives a straight line as shown in Figs. 11 and 12. The slope of the straight line is −ΔHoads/R. The obtained values of ΔHoads for adsorption of inhibitors are given in Table 4. The negative values of ΔHoads reflect the exothermic behavior of inhibitors on the mild steel surface.

Fig. 11.

Plot of ln (θ/1–θ) vs. 1/T for mild steel in 1.0 M HCl solution containing 600 ppm of drug.

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Fig. 12.

Plot of ln (θ/1–θ) vs. 1/T for mild steel in 0.5 M H2SO4 solution containing 600 ppm of drug.

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Entropy of adsorption (ΔSoads) can be calculated using the following equation:

The calculated values of ΔSoads along with the other parameters are recorded in Table 4. The adsorption of organic inhibitor molecules from the aqueous solution can be regarded as a quasi-substitution process between the organic compounds in the aqueous phase and water molecules at the electrode surface [36]. The adsorption of inhibitor on the mild steel surface is accompanied by desorption of water molecules from the surface. Thus, while the adsorption process for the inhibitor is believed to be exothermic and associated with a decrease in entropy of the solute, the opposite is true for the solvent. The thermodynamic values obtained are the algebraic sum of the adsorption of organic molecules and desorption of water molecules [37]. Hence, the gain in entropy is attributed to the increase in solvent entropy and to more positive water desorption enthalpy [38]. The positive values of ΔSoads also suggest that an increasing in disordering takes place in going form reactants to the metal/solution interface [39], which is the driving force for the adsorption of inhibitor onto the mild steel surface.

3.4Fourier transform infrared (FTIR) spectroscopy

It has been confirmed that FTIR spectrometer can be used to determine the type of bonding for organic inhibitors adsorbed on the alloy surfaces [30–32]. The FTIR spectra of adsorbed layer on steel surface can be obtained for determining the presence of drug on the sample surface. The present drug can be studied by FTIR because the drug molecules are weakly adsorbed on steel surface and the adsorbed layer can be transferred into KBr powder by rubbing the steel surface with KBr.

Figs. 13–15 show the FTIR spectra of rosuvastatin drug along with the spectra of adsorbed layer formed on mild steel surface after 24 h immersion in 1.0 M HCl and 0.5 M H2SO4 containing 600 ppm drug. By comparison, we find that the majority of the bands observed in the spectra of adsorbed layer on mild steel closely resemble those appearing in the drug spectrum.

Fig. 13.

FTIR spectra of rosuvastatin drug.

(0.12MB).
Fig. 14.

FTIR spectra of the adsorbed layer formed on mild steel after 24 h immersion in 1.0 M HCl solution +600 ppm of drug.

(0.1MB).
Fig. 15.

FTIR spectra of the adsorbed layer formed on mild steel after 24 h immersion in 0.5 M H2SO4 solution +600 ppm of drug.

(0.11MB).

Characteristics peaks of aromatic NH stretching and CO stretching at about 3430 cm−1 and 1730 cm−1 appeared, respectively. A broad band at around 3400 cm−1 in all three spectra is attributed to OH stretching, which further indicates the adsorbed film contains H2O. The weak bands near 2900 cm−1 are attributed to the aromatic CH stretching vibrations.

The lack of CO stretching band of carboxylic group in the drug spectrum (Fig. 13) means that oxygen atom of carboxylic group can form an intra-hydrogen bonding with the hydrogen of adjacent OH group. The appearance of the CO stretching vibration at about 1730 cm−1 in the adsorbed drug (Figs. 14 and 15) may reveal that the oxygen atom of carboxylic group can act as an active center in adsorption.

The bands at 1633.7 and 1635.9 cm−1 which appeared in the adsorbed spectra (Figs. 14 and 15) and also the observed band at 1654.3 cm−1 in the drug spectrum (Fig. 13) are assigned to CC stretching vibrations. Thus, it can be concluded that the inhibitor are really present on the mild steel surface by the adsorption.

4Conclusion

The adsorption and inhibition effects of rosuvastatin drug on the corrosion behavior of mild steel in 1.0 M HCl and 0.5 M H2SO4 solutions were studied using electrochemical techniques. Our results obtained from potentiodynamic polarization and EIS measurements demonstrated that the adsorption of drug on mild steel in acid solutions followed the Langmuir isotherm. The calculated values of free energy and enthalpy of adsorption indicated that both physical and chemical adsorption may take place. The IE and ΔGoads values obtained from EIS measurements of drug showed a reasonable agreement with those obtained from potentiodynamic polarization measurements.

Conflicts of interest

The authors declare no conflicts of interest.

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