Article 1 de BOULECHFAR Chérifa
Article 1 de BOULECHFAR Chérifa
Article 1 de BOULECHFAR Chérifa
a r t i c l e i n f o a b s t r a c t
Article history: The 2-furaldehyde semicarbazone (FSC), an environmentally safe Schiff base, has been synthesized and
Received 12 August 2021 tested for the first time as a corrosion inhibitor for XC38 carbon steel in an acidic environment. This com-
Revised 10 October 2021 pound’s anti-corrosion properties are assessed using electrochemical, analytical, and characterization
Accepted 16 October 2021
techniques. At 293 K and an FSC concentration of 500 ppm, the inhibitory effectiveness increased with
Available online 27 October 2021
the FSC concentration, reaching a maximum of around 91.5%. Furthermore, an increase in temperature
from 303 to 323 K increased the corrosion rate, most likely due to the inhibitor agent’s desorption from
Keywords:
the steel surface. Scanning Electron Microscope (SEM) and X-ray Fluorescence (XRF) metal surface exam-
Carbon steel
Corrosion
ination revealed that the presence of FSC causes the development of a protective layer. FSC adsorption
Inhibitor isotherms on carbon steel were measured at different temperatures, displaying an exothermic behavior
Schiff bases that corroborated the earlier observations. Electrochemical experiments show that as the inhibitor con-
Molecular dynamics centration increases from 50 to 500 ppm, Icorr decreases from 0.695 to 0.123 mAcm2. At the same time,
DFT the maximum change in Ecorr values is 23.1 mV, leading to the conclusion that this Schiff base (inhibitor)
is a mixed type of (anodic/cathodic) inhibitor. The FSC Electrophilic/nucleophilic attacks on carbon steel
are theoretically studied. MD simulations revealed the FSC molecules’ adsorption process on the steel
surface.
Ó 2021 Elsevier B.V. All rights reserved.
https://doi.org/10.1016/j.molliq.2021.117874
0167-7322/Ó 2021 Elsevier B.V. All rights reserved.
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
various objectives [6]. Nitric, sulfuric, hydrochloric, formic, and molecular behavior and electronic interaction between the metal
acetic acids are widely employed in these applications [7]. and the produced inhibitor molecule.
Every sector relies on metal alloys, mainly carbon steel, because
of their inexpensive cost and high mechanical strength [8]. Metal, 2. Materials and procedures
building, chemical, marine applications, and oil extraction and
refining are a few industries where carbon steel is used. Pipelines 2.1. Synthesis of inhibitors
and equipment, for example, can be severely corroded by such uses
[9–10]. The standard practice of adding an inhibitor to carbon steel Ibrahim et al. [27] published a technique for synthesizing the
to prevent corrosion is to do so. Inhibitors are usually made up of FSC Schiff base. An ethanolic solution of 2-furaldehyde (9.6 g)
organic and inorganic chemicals that adsorb on the metal surface was added dropwise to an aqueous solution (50 cm3) of semicar-
and protect it from corrosion [11]. bazide chloride (11.15 g) and AcONa (20 g). After 1 h of refluxing,
In the realm of corrosion inhibitors, organic type Schiff bases the FSC precipitated, was filtered, and then recrystallized from
have shown promise in preserving carbon steel against corrosion hot water. The reaction produces a product that is 85% pure and
in various harsh conditions [12–13]. Hugo Schiff (a German scien- has a melting point of 461 K. Fig. 1 illustrates the optimum struc-
tist and Nobel Prize laureate) discovered Schiff bases by condens- ture of the resultant molecule.
ing primary amines with carbonyl compounds [14]. They are also
referred to as ‘‘imines,” ‘‘anils,” and ‘‘azomethine.” A functional 2.2. Carbon steel samples
group with a double carbon–nitrogen bond, where the nitrogen
atom is linked to an alkyl or aryl group, distinguishes them. XC38 carbon steel was utilized to create specimens and the
R1HC = N-R2 is their general formula, with R1 and R2 being aryls, working electrode for the gravimetric and electrochemical tests
alkyls, cycloalkyls, or heterocyclic groups that allow for different in the corrosion experiments. Before being submerged in the corro-
substitution processes [15]. sive electrolyte solution, samples were mechanically abraded (us-
Free-electron pairs produced by the metal surface’s interaction ing emery paper with a mesh/in grade ranging from 400 to 2000),
with hetero atoms of the inhibitor structure, such as nitrogen, sul- washed with double distilled water followed by acetone, and lastly
fur, and oxygen, are generally responsible for corrosion inhibition dried in hot air. Samples were cut into cylindrical shapes
[16–17]. Additionally, since the p-orbital interacts with the metal’s (D = 15 mm and H = 5 mm) and implanted in an inert resin with
surface, compounds containing p-bonds have strong inhibitory a 1.77 cm2 exposed surface section for weight loss and electro-
properties. Schiff bases are corrosion inhibitors due to their chemical tests.
‘‘azomethane” group (C@N). Schiff bases applied to steel [18–19],
aluminum [20], and copper [21–22] have been found to be effec- 2.3. Corrosive working solutions
tive in preventing corrosion in acidic environments.
Schiff bases as corrosion inhibitors have gained much interest in In the presence and absence of the FSC inhibitor, corrosive elec-
recent years since they are ecologically friendly and low-cost to trolyte solutions of 0.5 M H2SO4 were produced from laboratory-
make. This is to avoid unfavorable environmental consequences grade H2SO4 and distilled water. The inhibitor concentration was
connected with the manufacturing and use of corrosion inhibitors varied between 25 and 500 ppm.
while ensuring carbon steel’s long-term durability, which has eco-
nomic and operational benefits. Despite this, there is a paucity of 2.4. Weight loss measurements
literature about how Schiff bases prevent carbon steel corrosion
under various working circumstances, particularly at the molecu- A thermostatic waterbath was used to regulate the temperature
lar level. Molecular dynamics (MD) simulations and density func- of cylindrical carbon steel samples submerged in a 0.5 M H2SO4
tional theory (DFT) computations have been demonstrated to solution at a set concentration of the produced inhibitor. Temper-
provide important advances to our knowledge of the fundamental atures at three distinct levels were studied (303, 313, and 323 K).
processes governing molecular interactions between various sub- For comparison, a blank solution (i.e., one without the inhibitor)
stances and solid surfaces [23–24]. This can help with product was utilized. The specimens were taken out, washed with distilled
selection and optimization for specific applications, such as corro- water, and dried after a set time in the water. Steel samples were
sion inhibitors. Some researchers investigated the process of corro- weighed using a Shimadzu AUW220D UniBloc Analytical Balance
sion inhibition using DFT and MD theoretical methods [25–26]. with a precision level of 105 g before and after treatment in cor-
Indeed, these numerical methods promise fundamental guidelines rosive solution. Experiments were done in triplicate at a constant
for tuning the physicochemical properties of molecules better at temperature and inhibitor dosage, assuming the mean mass loss.
acting as inhibitors against specific materials that need to be pro- This enabled the following Eqs to be used to calculate the corrosion
tected from corrosion, which is a novel way of looking at this rate (CR), degree of surface covering (h), and inhibition efficiency
research line. The efficacy of 2-furaldehyde semicarbazone (FSC) (Ew) [28].
Schiff base as a corrosion inhibitor of carbon steel in a 0.5 M sulfu-
ric acid medium was examined in the current study. The inhibition
efficacy at various inhibitor doses and temperatures was evaluated
using electrochemical impedance spectroscopy (EIS), potentiody-
namic polarization (PDP), and weight loss measures. Scanning elec-
tron microscopy (SEM), X-ray fluorescence (XRF), and X-ray
photoelectron spectroscopy (XPS) studies were used to verify the
efficient deposition of the FSC protective coating onto the surface
of carbon steel. Using adsorption thermodynamic models, density
functional theory (DFT) calculations, and molecular dynamics
(MD) simulations, a focused modeling campaign was conducted
to clarify the adsorption process, the reactivity of FSC, and the
interaction of FSC with the steel surface. MD simulations were used
to supplement the experimental results and explain the inter- Fig. 1. Optimized molecular structure ofFSC.
2
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
r ¼ 1=g ð14Þ
The electrophilicity index (x) of ions, atoms, and molecules is
calculated from the electronegativity and hardness values as [35]:
v2
x¼ ð15Þ
2g
The fraction of electrons transferred (DN) from the inhibitor
molecule to the surface of the carbon steelsampleis calculated in
corrosion studies [35]:
4
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
Table 1
FSC, polarization parameters for XC38 steel corrosion in 0.5 M H2SO4.
Parameter Ecorr(mV) Icorr(mAcm2) Rp(O cm2) ba(mV dec1) bc(mVdec1) Eicorr(%) ERp(%)
Blank 428.9 0.695 29.2 129 151.7 – –
50 ppm 435.7 0.516 40.96 88.5 127.1 25.76 28.71
100 ppm 435.6 0.415 45.04 87.2 130.8 40.22 35.16
250 ppm 436.9 0.27 72.53 96.7 139.6 61.15 59.74
400 ppm 413.8 0.19 105.8 81.6 300.0 72.66 72.4
500 ppm 414.1 0.123 170 273.6 583.6 82.26 82.82
in both the anodic (ba) and cathodic (bc) Tafel slopes, confirming The CPE magnitude, angular frequency, CPE exponent, and
that the inhibitor controls reactions at both the anode and cathode imaginary unit are represented by Q, w, a, and j, respectively.
electrodes [43]. These results imply that FSC interacts with the The CPE can alternatively be thought of as a perfect capacitor.
XC38 steel surface in a 0.5 M H2SO4 solution, blocking the active The results show that the inhibitor adsorbs on the metal surface,
sites and improving the metal’s corrosion resistance [44–45]. forming a protective layer. This film also helps increase the thick-
ness of the electric double layer and lower the dielectric constant
4.1.3. Electrochemical impedance spectroscopy (EIS) of the solution, which improves corrosion resistance [49].
Fig. 4 shows the results for the EIS steel XC38/H2SO4 (0.5 M acid The RS, Rct, Rd, and CPEdl components of the circuit (Fig. 5(a) and
concentration) solution interfaces at various FSC concentrations. (b)) represent the solution resistance, charge transfer resistance,
The ‘‘Nyquist plot” depicts the imaginary part of impedance (Zi) diffuse layer resistance, and constant phase element of the double
vs. the real component of impedance (Ri) for each frequency (Zr). layer, respectively.
The semicircular forms seen in Nyquist diagrams suggest that,
while corrosion is occurring, a significant charge transfer process 4.2. Gravimetric analysis
occurs in the studied system [46–47]. The size of these semicircles
grows as the inhibitor concentration rises, improving metal corro- 4.2.1. Effect of the inhibitor concentration
sion resistance and decreasing corrosion rates [48–49]. In a solution of 0.5 M H2SO4 at 293 K for 48 h, gravimetric tests
The metal-electrolyte interface, defined by a double electric on carbon steel corrosion were performed in the presence or
layer, is sensitive to changes in structure or composition when a absence of FSC inhibitor (concentrations ranging from 25 to
new chemical (inhibitor) is introduced. This means that double- 500 ppm). Fig. 6 shows that FSC is an efficient corrosion inhibitor,
layer capacitance measurements (before and after corrosion inhibi- as seen by the monotonic drop-in corrosion rate (CR) and inhibi-
tor inclusion) might aid in the monitoring of inhibitor adsorption tion efficiency (Ew) increase as inhibitor concentration increases.
[50]. When comparing data obtained in the absence of inhibitor to those
Fig. 5 depicts the equivalent electrical circuit corresponding to obtained at the maximum FSC concentration, CR was decreased by
the EIS data. The constant phase element (CPE) replaces the more than one order of magnitude. At 500 ppm FSC, Ew is around
double-layer capacitance in Nyquist plots when looking at 92%. The inhibitor shields the metal from the aggressive acidic
depressed capacitive loops. In the corrosion sector, it is commonly media, most likely by creating a layer adsorbed on the carbon steel
recognized to utilize the CPE in the equivalent circuit. Dynamic surface (Fe-FSC complex that prevents dissolution) [53–54].
electrochemical processes and microscopic material characteristics
(local charge inhomogeneity and surface imperfections) are inti- 4.2.2. Effect of temperature
mately connected to macroscopic impedance [51–52]. The 4.2.2.1. Corrosion parameters. Fig. 7(a) and (b) show the corrosion
double-layer constant phase elements (CPE), solution resistance, rate and inhibition efficiency for samples submerged for 2 h in a
and charge transfer resistance are the elements that define the 0.5 M H2SO4 solution at 303, 313, and 323 K, respectively. At a con-
equivalent circuit. The equation below represents CPE impedance: stant FSC concentration, the inhibition efficiency drops while the
corrosion rate increases with increasing temperature. On the other
1
Z CPE ¼ a ð17Þ hand, at 500 ppm FSC, the CR increased five times when the tem-
Q ðjwÞ
perature increased from 303 to 323 K. This is due to inhibitor des-
orption or, more likely, thermal breakdown of the FSC structure at
elevated temperatures, exposing a larger surface area of carbon
steel to acidic corrosive attack (i.e., a minor coverage degree at a
greater temperature level). This suggests that the inhibitor mole-
cules are physisorbed to the steel surface [55–56]. Finally, the rise
in FSC concentration is good for increased corrosion resistance. Ew
reaches a maximum level of approximately 89% at 500 ppm and
303 K, according to the previously described pattern at 293 K.
5
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
Fig. 5. Equivalent Electrical circuit a) Solution without inhibitor (Blank) and b) Solution containing FSC.
Eq. (17) (see Fig. 8) and Eq. (18) (see Fig. 9). The data were obtained
at various inhibitor doses in an acidic medium.
The activation energy in the presence of FSC is more significant
than in the absence of FSC, suggesting that the dissolving process
of XC38 carbon steel in acidic conditions is delayed [59]. Inhibition
adsorption forms a thick layer on the metal surface, which explains
why corrosion activation energy is more significant in inhibited
systems [60] and the presence of physical adsorption phenomena
by producing an electrostatic adsorptive film on the metal surface
[61].
The positive values of DHa indicate that the corrosion process is
endothermic and that the higher the FSC concentration the more
the dissolution of XC38 carbon steel in the presence of the inhibitor
is more energy demanding [62]. The activation entropy in the pres-
ence of FSC was higher than when it wasn’t (in both cases, the val-
ues were negative).
Calculating activation parameters from corrosion rate data elu-
Fig. 6. Corrosion rates and inhibition efficiency for steel samples vs. FSC concen- cidates the inhibitor adsorption mechanism on metal surfaces. The
tration after 48 h of immersion. activation energy was somewhat higher in the presence of FSC
than in its absence. According to the Arrhenius equation, higher
activation energies result in increased temperature variation in
The corrosion rate (as measured by the weight loss technique)
the reaction rate. This accounts for the temperature-dependent
and the Arrhenius pre-exponential factor (mg cm2h1) are repre-
variation in reaction rate seen in the absence and presence of inhi-
sented by CR and A.
bitor. For both the uninhibited sample and FSC, the rate of corro-
The thermodynamic parameters enthalpy of activation, DHa and sion increased with temperature. Chemisorption occurs when the
entropy of activation, DSa were calculated using the transition state
Ea and DHa levels of the inhibited system are equal to or less than
equation [58]. those of the uninhibited system, while physisorption occurs when
those values are higher [63]. The table demonstrates that
!
!
RT DSa DH a chemisorption is preferable than physisorption. The drop in the
CR ¼ exp exp ð19Þ preexponential frequency component may account for the pace
Nh R RT
at which corrosion decreases with increasing inhibitor concentra-
The Avogadro’s number is N, and the Planck constant is h. tion. DSa is negative in the absence of FSC and much more in its
Table 2 presents the activation energies values for XC38 deter- presence (Table 2). This indicates that the rate-determining transi-
mined from fitting corrosion rate data to the linearized versions of tion state is more ordered than the reactants, and that an inhibitor
Fig. 7. The influence of FSC concentration at various temperatures on (a) corrosion rate and (b) inhibition efficiency.
6
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
Table 2 lowing the cathodic Tafel slope tabulated in Table 1, we may pre-
Activation thermodynamic parameters at different FSC concentrations sume that in the present case, the reaction shown in eqn (19) is
C(ppm)
Ea (kJmol1)
DHa (kJmol1)
DSa (Jmol1K1) the rate determining step. In fact, all these intermediate steps lead
to a decrease in the randomness in their corresponding transition
Blank (Uninhibited) 37.413 34.810 174.268
25 ppm 38.202 35.600 171.915 states, which is reflected in the negative value for DSa . Again, the
50 ppm 39.034 36.431 169.445 more negative value of DSa in the presence of the inhibitor can
100 ppm 41.927 39.333 160.674
200 ppm 70.003 67.401 73.826
be explained in terms of the blocking of the cathodic and anodic
300 ppm 81.136 78.534 42.067 reaction sites by the inhibitor molecule. For occurrence of any type
350 ppm 72.747 70.145 71.997 of surface reaction, reactants require closer approach or interaction
400 ppm 66.412 63.809 95.110 with a metal surface possessing an inhibitor layer, resulting in
500 ppm 64.757 62.155 102.925
more order during the intermediate stages of the reaction. This also
results in a decrease in the pre-exponential frequency A. Addition-
ally, at 300 ppm FSC, the DSa value becomes less negative (in-
creases) and the DHa value drops, indicating an increase in
disorder at the metallic surface. This strongly suggests that
300 ppm is the saturation level and that it is more than enough
to provide the corrosion preventing effect.
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Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
Table 3
Temperature effect on adsorption thermodynamic parameters
plot was used to produce K ads values, which were then linked to the The DGads values observed in this work range from 23.199 kJ/-
standard free energy of adsorption (DGads ) as follows: mol to 22.214 kJ/mol, showing a spontaneous process including
physisorption and forming an adsorbed FSC layer that shields the
1 DG metal from corrosion via inhibitor-metal electrostatic interactions
K ads ¼ expð ads Þ ð24Þ
55:5 RT [76–79]. As predicted for physisorption, the negative value of DHads
The Gibbs-Helmholtz equation was used to calculate the indicates that the process is exothermic. Finally, the DSads value is
strikingly negative, implying a significant connection between
enthalpy of adsorption, DHads , and the entropy of adsorption, DSads :
the FSC and the carbon still surface, as well as a decrease in entropy
following adsorption [80].
DGads ¼ DHads T DSads ð25Þ
Another calculation method is to take the slope and intercept of 4.3. Surface characterization
the lnðK ads Þ plot versus 1000/T (Fig. 11):
4.3.1. Scanning electron microscopy (SEM)
DHads DS 1 Fig. 12 illustrate the surface morphology of XC38 carbon steel.
lnðK ads Þ ¼ þ ð ads þ ln Þ ð26Þ After immersion in the acidic solution in the absence of the inhibi-
RT R 55:5
tor, the carbon steel surface micrographs show an aggressive
Table 2 shows the estimated values of DGads , DHads and DSads at attack (Fig. 12 (b)). The metal surface has fractures and pits, indi-
various temperatures. Table 2 shows that positive values imply cating that the solution’s corrosive attack has severely harmed it.
attractive lateral interactions in the adsorbed layer, more pro- In comparison to the (b) sample (Fig. 12(b)), the addition of
nounced at higher temperatures. The temperature rise causes a 500 ppm of the inhibitor to the solution (Fig. 12(c)) resulted in a
drop in the adsorption equilibrium constant, and K ads is lowered smoother and more compact surface with very few noticeable frac-
by a factor of around 2.5 from 303 to 323 K, as predicted by earlier tures and pits, showing that the metal was successfully protected
measurements. As a result, the inhibitor tends to desorb from the against corrosive attack. The discrepancy might be explained by
carbon steel surface [74–75]. the deposited FSC molecules covering the working electrode’s steel
surface [37]. This demonstrated that an effective protective layer of
the tested inhibitor was adsorbed on the metal surface and was
influential in inhibiting corrosion.
Fig. 12. SEM images of the carbon steel surface a) before immersion H2SO4, b) after immersion in H2SO4without FSC, c) after immersion in H2SO4 and 500 ppm FSC.
Fig. 13(a) and (b) show three deconvoluted peaks in the C1s
Table 4
XRF studies of the various components of the XC38 carbon steel core level spectra. The first is at 284.48 eV for pure FSC (Fig. 13a)
and 284.53 eV for FSC-treated carbon steel (Fig. 13b), which is
Elements XC38 steel XC38 steel after XC38 steel after
attributed to the existence of AC@C/ACAC in aromatic rings [84].
before immersion in H2SO4 immersion in
immersion (wt. (wt.%) (H2SO4 + FSC) (wt.%) Carbon atoms linked to nitrogen atoms (CAN/C@N) and sulfur
%) atoms (CAS) are responsible for the second peak, situated at
C 0.37 0.456 0.786
285.78 eV for pure FSC and 286.03 eV for both FSC-treated carbon
Ti 0.011 1.094 0.823 steel. For pure FSC and FSC-treated carbon steel, the third contribu-
Si 0.23 0.116 0.185 tion emerges at 288.38 eV and 288.13 eV, respectively, correspond-
Cr 0.077 1.059 0.756 ing to the C@N+ with varying intensities [85]. All of the peaks above
S 0.016 0.018 0.017
indicate that the FSC molecule was adsorbed on the steel surface.
Mn 0.68 0.786 0.423
Fe 98.388 86.154 95.542 The deconvoluted O1s spectra for pure FSC (Fig. 13c) reveal two
Co 0.009 0.012 0.011 significant peaks at 531.38 and 533.28 eV, respectively, indicating
Ni 0.059 1.252 0.401 the existence of C@O and CAOH bonds [86]. The O 1s spectra for
FSC-treated carbon steel, on the other hand, could be divided into
three distinct peaks (Fig. 13(d)): (i) The oxygen atom linked to Fe
4.3.3. XPS analysis (III) in the Fe2O3 and/or Fe3O4 oxides is responsible for the peak
The XPS measurement was performed at 298 K after 24 h of at 529.06 eV [87], (ii) OH of FeOOH [88] is responsible for the peak
immersion in 0.5 M H2SO4 on pure FSC and steel treated with at 531.13 eV and (iii) The oxygen in the adsorbed water might
500 ppm of FSC. C1s, N1s, S2p, O1s, and Fe2p for the FSC-treated explain the peak at 532.43 eV [88].
steel surface were obtained from XPS spectra of pure FSC and Fig. 13(e) depicts the deconvolution of the N 1s spectrum for
C1s, N1s, S2p, O1s, and Fe2p for the FSC-treated steel surface. A pure FSC, revealing one component at 399.7 eV that may be attrib-
deconvolution fitting technique was performed in all XPS spectra uted to the @NA structure [89]. Despite this, the high-resolution N
to reveal the complex forms for the associated species (Fig. 13). 1s spectra of the XC38 treated by FSC showed two peaks at BE
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Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
Fig. 13. The XPS deconvoluted profiles of pure FSC (a) C 1s, (c) O 1s, (e) N 1s and for FSC/Carbone steel (b) C 1s, (d) for O 1s, (f) N 1s (g) S 2p and (h) Fe 2p.
399.43 and 401.23 eV, as shown in Fig. 13(f). Pure FSC contains sig- ðFeSO2
4 ÞAdsorbed $ ðFeSO4 ÞAdsorbed þ 2e ð29Þ
nificantly variable quantities of nitrogen species, including CAN
and the unprotonated N atom (@N-structure) [90]. The nitrogen
cooperation with the steel surface causes the peaks following ðFeSO2 2þ
þ SO2
4 ÞAdsorbed $ Fe 4 ð30Þ
adsorption. Furthermore, the N-Fe bonds can induce peak shifts
to higher binding energies than the uncoordinated @NA structure In the presence of excess, SO2
4 ions that are first adsorbed onto
[91], suggesting that the FSC is adsorbed on the XC38 surface. the positively charged metal surface, the reaction Eq. (28) is also
Fig. 13(g) shows the S 2p high-resolution XPS spectra for XC38 anticipated to proceed extremely fast [92]. Inhibitor, on the other
steel after immersion in inhibited solution, which reveals a single hand, interacts with Fe (II) to create the anticorrosive complex [
signal corresponding to the doublet 2p3/2 and 2p1/2 in the range FeSO2 +
4 , Inhibitor ]. This strong layer prevents aggressive ions from
of 168.17–169.37 eV, indicating SO2 4 ions. the majority of the corrosive solution from reaching the surface of
The Fe 2p spectra for FSC-covered carbon steel surfaces display XC38 steel. The process of cathodic hydrogen evolution is as fol-
two doublets (Fig. 13(h)) associated with high-energy ghost struc- lows [94]:
tures suggesting subsequent steel surface oxidation: 711 eV (Fe
2p3/2) and 724 eV (Fe 2p1/2).
There are four peaks in the Fe 2p3/2 XPS spectra after deconvo- Fe þ Hþ $ ðFeHþ ÞAdsorbed ð31Þ
lution. The initial peak detected at low binding energy (707.28 eV)
is due to iron nitrides (FexN), indicating that the deconvolution
above N 1s is correct (Fig. 13(f)). Ferric compounds such as ðFeHþ ÞAdsorbed þ e $ ðFeHÞAdsorbed ð32Þ
Fe2O3/Fe3O4/FeSO4/FeOOH [53] are responsible for the two signifi-
cant peaks at 710.58 eV and 713.68 eV. The Fe (III) satellite feature
is responsible for the last peak at BE = 716.68 eV [91]. ðFeHÞAdsorbed þ 2Hþ þ 2e ! Fe þ H2 " ð33Þ
+ +
4.4. Mechanism of inhibition Then, in competition with H ions, Inhibitor molecules can be
adsorbed at cathodic sites of XC38 steel, resulting in the decrease
The presence of N1s peaks and a shift of the N1s peak to higher of H+ ions and the evolution of H2 gas [95].
binding energy in the inhibited sulfuric acid solution confirms the
adsorption of the FSC layer onto the steel surface. The interaction Table 5
of protonated inhibitor molecules with iron on a steel surface must The liquid-phase reactivity descriptors
be thoroughly understood. In sulfuric acid solutions, the anodic
Descriptor FSC Protonated FSC
electro-dissolution reactions of iron are represented as follows
EHOMO 5.1973 2.272
[92–93]:
ELUMO 2.3075 1.493
Egap 2.8898 0.779
ðH2 OÞAdsorbed þ SO2 2 v
4 $ H2 O þ ðSO4 ÞAdsorbed ð27Þ 3.7524 1.883
g 1.4449 0.390
x 4.872 4.549
Fe þ SO2 2
4 $ ðFeSO4 ÞAdsorbed ð28Þ DN 0.3694 3.771
10
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
11
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
Fig. 15. Adsorption of FSC on the Fe surface shown from the side view of the cleaved (1 1 0) plane.
Table 7
Calculated adsorption energies (Kcal mol1) for FSC on the Fe (1 1 0) surface
Fig. 16. RDF of the adsorbed FSC on the Fe (1 1 0) surface in acidic solution.
in which Esurfacesolution , Einhibitor and Etotal are the energies of the metal adsorb preferentially on the iron surface as a protonated molecule
surface-solution, the inhibitor alone, and these two systems and effectively eject water molecules.
together, respectively.
Table 7 contains both the binding energies and interactions of 4.5.3. Radial distribution function (RDF)
the inhibitors that were examined. It is worth noting that both The neutral and protonated form of FSC inhibitor interact with
neutral and protonated FSC molecules showed a pronounced neg- the iron surface, as seen by the first significant peak in the RDF
ative interaction energy. One might argue that the protonated form curves. Chemical interactions (peak at 1–3.5 Å) or physical interac-
has a greater capacity for adsorption and a higher adsorption tions (peaks at a distance longer than 3.5 Å) with the iron surface
energy. This study supports the previous findings that FSC may might occur depending on the molecule’s location [96]. In Fig. 16,
12
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
the first g(r) Fe inhibitor peaks occur at distances of less than 3.5. Acknowledgments
This demonstrates that electrovalent bonds regulate Fe-inhibitor
interactions. We would like to thank the ‘‘La Direction Générale de la
Recherche Scientifique et du Développement Technologique
(DGRSDT) ”. The authors are also thankful to the Taif University
5. Conclusions
Researchers Supporting Project number (TURSP-2020/03), Taif
University, Taif, Saudi Arabia.
Weight-loss and electrochemical techniques, scanning electron
microscopy, fluorescence-X, and theoretical calculations were used
References
to investigate the anticorrosive power of FSC Schiff base on XC38
Carbon steel in a 0.5 M H2SO4 medium. [1] W. Sun, S. Nesic, A mechanistic model of H2S corrosion of mild steel, Houst.
The results indicated that the Schiff base studied is an effective Tex. USA 07655 (2007) 1–26.
corrosive inhibitor for the metal in the investigated corrosive solu- [2] M.M. Ibrahim, R.S.A. Hameed, A.-A.-H. Abu-Nawwas, Schiff bases and their
metal complexes as corrosion inhibitors for steel alloys in acidic media, Org.
tion (0.5 M H2SO4), with an inhibition effectiveness of 91.478% for Chem. 9 (12) (2013) 493–499.
500 ppm FSC. On the other hand, the increase in temperature is [3] W. Ebdelly, S. Ben Hassen, X.R. Nóvoa, Y. Ben Amor, Inhibition of carbon steel
harmful to inhibition efficiency, perhaps due to desorption of the corrosion in neutral calcareous synthetic water by eruca sativa extract, Prot.
Met. Phys. Chem. Surf. 55 (3) (2019) 591–602.
inhibitor or a loss in its stability at higher temperatures. Because [4] K. Zakaria, N.A. Negmb, E.A. Khamisc, E.A. Badrb, Electrochemical and quantum
it participates in processes on both the cathode and the anode, chemical studies on carbon steel corrosion protection in 1M H2SO4 using new
the FSC was a mixed inhibitor in the potentiodynamic polarization eco-friendly Schiff base metal complexes, Taiwan Inst. Chem. Eng. (2016) 1–
11.
research. According to a thermodynamic analysis of the data,
[5] O.S.I. Fayomi, I.G. Akande, S. Odigie, Economic impact of corrosion in oil sectors
adsorption follows the Frumkin adsorption model, is spontaneous, and prevention: an overview, J. Phys. Conf. Ser. 1378 (2019) 022037, https://
and happens through physical interactions. Negative values indi- doi.org/10.1088/1742-6596/1378/2/022037.
[6] V. S. Sastri, Corrosion Inhibitors: Principles and Applications | Emerald Insight,
cate that FSC adsorption on the metal surface is of a spontaneous
John Wiley Sons N. Y., 1998, Accessed: Oct. 31, 2020.
chemical kind. According to SEM data, the morphology of the par- [7] H. Ferkous, S. Djellali, R. Sahraoui, Y. Benguerba, H. Behloul, A. Çukurovali,
ent carbon steel was mostly preserved in the presence of the inhi- Corrosion inhibition of mild steel by 2-(2-methoxybenzylidene) hydrazine-1-
bitor. The organic inhibitor adsorption on the metal surface, on the carbothioamide in hydrochloric acid solution: experimental measurements
and quantum chemical calculations, J. Mol. Liq. 307 (2020) 112957, https://doi.
other hand, resulted in an increase in carbon content on the metal org/10.1016/j.molliq.2020.112957.
surface, and the drop in iron content was significantly less marked [8] I. Benmahammed, T. Douadi, S. Issaadi, M. Al-Noaimi, S. Chafaa, Heterocyclic
in the presence of the inhibitor and after exposing the sample to Schiff bases as corrosion inhibitors for carbon steel in 1 M HCl solution:
hydrodynamic and synergetic effect, J. Dispers. Sci. Technol. 41 (7) (2020)
the acidic medium, according to the XRF analysis. The development 1002–1021, https://doi.org/10.1080/01932691.2019.1614038.
of an inhibitor layer comprising FSC molecules with iron oxides [9] M.A. Migahed, M.M. Attya, S.M. Rashwan, M. Abd El-Raouf, A.M. Al-Sabagh,
was confirmed by XPS research. Quantum calculations were used Synthesis of some novel non ionic surfactants based on tolyltriazole and
evaluation their performance as corrosion inhibitors for carbon steel Egypt, J.
to back up the experimental results, and a strong connection was Pet. 22 (1) (2013) 149–160, https://doi.org/10.1016/j.ejpe.2012.09.006.
discovered between theoretical and electrochemical investiga- [10] A.M. Al-Sabagh, N.M. Nasser, A.A. Farag, M.A. Migahed, A.M.F. Eissa, T.
tions. MD simulations were used to identify the FSC molecule’s Mahmoud, Structure effect of some amine derivatives on corrosion
inhibition efficiency for carbon steel in acidic media using electrochemical
adsorption on steel surfaces, as well as the attack of nucleophilic/-
and Quantum Theory Methods, Egypt. J. Pet. 22 (1) (2013) 101–116, https://
electrophilic sites. Finally, FSC has been demonstrated to be an effi- doi.org/10.1016/j.ejpe.2012.09.004.
cient carbon steel corrosion inhibitor. [11] S.K. Shanmughan, J.T. Kakkassery, V.P. Raphael, N. Kuriakose, Electrochemical
and AFM studies on adsorption behavior of a Polynuclear Schiff Base at carbon
steel in HCl medium, Curr. Chem. Lett. 4 (2) (2015) 67–76, https://doi.org/
10.5267/j.ccl.2015.2.001.
6. Data and materials availability [12] M. Behpour, S.M. Ghoreishi, M. Salavati-Niasari, B. Ebrahimi, Evaluating two
new synthesized S-N Schiff bases on the corrosion of copper in 15%
All the data needed to assess the conclusions in work is pre- hydrochloric acid, Mater. Chem. Phys. 107 (1) (2008) 153–157, https://doi.
org/10.1016/j.matchemphys.2007.06.068.
sented in the paper and/or the Supplementary Materials. [13] S. Bilgiç, N. Çaliskan, An investigation of some Schiff bases as corrosion
inhibitors for austenitic chromium–nickel steel in H2SO4, J. Appl. Electrochem.
31 (1) (2001) 79–83, https://doi.org/10.1023/A:1004182329826.
CRediT authorship contribution statement [14] M.S. Hossain, C.M. Zakaria, M. Kudrat-E-Zahan, B. Zaman, Synthesis, spectral
and thermal characterization of Cu(II) complexes with two new schiff base
Chérifa Boulechfar: Investigation, Conceptualization, Method- ligand towards potential biological application, Pelagia Res. Libr. Chem. Sin. 8
(3) (2017) 380–392.
ology, Project administration, Resources, Writing - original draft, [15] R. Sahu, D.S. Thakur, Schiff base: an overview of its medicinal chemistry
Writing - review & editing. Hana Ferkous: Conceptualization, potential for new drug molecules, Int. J. Pharm. Sci. Nanotechnol. 5 (3) (2012)
Methodology, Supervision. Souad Djellali: Conceptualization, 3, https://doi.org/10.37285/ijpsn.2012.5.3.2.
[16] A. Raman, P. Labine, NACE International. Reviews on Corrosion Inhibitor
Methodology, Supervision. Mohammed A. Amin: Writing - review Science and Technology, NACE Houst., vol. 1, 1986, Accessed: Oct. 31, 2020.
& editing. Sihem Boufas: Conceptualization, Supervision. Amel [17] A.K. Singh, M.A. Quraishi, E.E. Ebenso, Inhibitive effect of cefuroxime on the
Djedouani: Conceptualization. Amel Delimi: Conceptualization. corrosion of mild steel in hydrochloric acid solution, Int. J. ElectrochemSci 6
(2011) 5676–5688.
Yasser Ben Amor: Conceptualization. Krishna Kumar Yadav: [18] M.N. Desai, M.B. Desai, C.B. Shah, S.M. Desai, Schiff bases as corrosion
Writing - review & editing. Byong-Hun Jeon: Writing - review & inhibitors for mild steel in hydrochloric acid solutions, Corros. Sci. 26 (10)
editing. Yacine Benguerba: Supervision, Software, Methodology, (1986) 827–837, https://doi.org/10.1016/0010-938X(86)90066-1.
[19] E. Naderi, A.H. Jafari, M. Ehteshamzadeh, M.G. Hosseini, Effect of carbon steel
Writing – review & editing. microstructures and molecular structure of two new Schiff base compounds
on inhibition performance in 1 M HCl solution by EIS, Mater. Chem. Phys. 115
(2-3) (2009) 852–858, https://doi.org/10.1016/j.matchemphys.2009.03.002.
Declaration of Competing Interest [20] A. Aytaç, Ü. Özmen, M. Kabasakaloğlu, Investigation of some Schiff bases as
acidic corrosion of alloy AA3102, Mater. Chem. Phys. 89 (1) (2005) 176–181,
The authors declare that they have no known competing finan- https://doi.org/10.1016/j.matchemphys.2004.09.003.
[21] S.L. Li, H.Y. Ma, S.B. Lei, R. Yu, S.H. Chen, D.X. Liu, Inhibition of copper corrosion
cial interests or personal relationships that could have appeared with schiff base derived from 3-methoxysalicylaldehyde and O-
to influence the work reported in this paper. phenyldiamine in chloride media, Corrosion 54 (12) (1998) 947–954.
13
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
[22] S. Li, S. Chen, S. Lei, H. Ma, R. Yu, D. Liu, Investigation on some Schiff bases as irreversible electron transfers. 1. Theoretical study of the anodic dissolution
HClcorrosioninhibitors for copper, Corros. Sci. 41 (7) (1999) 1273–1287, of metals, J. Phys. Chem. B 109 (10) (2005) 4584–4592, https://doi.org/
https://doi.org/10.1016/S0010-938X(98)00183-8. 10.1021/jp0467954.
[23] K. Benbouguerra, S. Chafaa, N. Chafai, M. Mehri, O. Moumeni, A. Hellal, [48] K. Rahmouni, S. Joiret, L. Robbiola, A. Srhiri, H. Takenouti, V. Vivier, Corrosion
Synthesis, spectroscopic characterization and a comparative study of the and protection of high leaded tin bronze covered withpatina in NaHCO3+
corrosion inhibitive efficiency of an a-aminophosphonate and Schiff base Na2SO4solution simulating acid rain in urban environment, Bulg. Chem.
derivatives: experimental and theoretical investigations, J. Mol. Struct. 1157 Commun. 37 (2005) 26–34.
(2018) 165–176, https://doi.org/10.1016/j.molstruc.2017.12.049. [49] M.L. Zheludkevich, D.G. Shchukin, K.A. Yasakau, H. Möhwald, M.G.S.
[24] D. Daoud, T. Douadi, H. Hamani, S. Chafaa, M. Al-Noaimi, Corrosion inhibition Ferreira, Anticorrosion coatings with self-healing effect based on
of mild steel by two new S-heterocyclic compounds in 1 M HCl: experimental nanocontainers impregnated with corrosion inhibitor, Chem. Mater. 19
and computational study, Corros. Sci. 94 (2015) 21–37. (3) (2007) 402–411.
[25] D. Wang, S. Li, Y. Ying, M. Wang, H. Xiao, Z. Chen, Theoretical and experimental [50] V.S. Sastri, Green Corrosion Inhibitors: Theory and Practice, Wiley, 2012.
studies of structure and inhibition efficiency of imidazoline derivatives, [51] H. Cesiulis, N. Tsyntsaru, A. Ramanavicius, G. Ragoisha, The study of thin films
Corros. Sci. 41 (10) (1999) 1911–1919, https://doi.org/10.1016/S0010-938X by electrochemical impedance spectroscopy, in: I. Tiginyanu, P. Topala, V.
(99)00027-X. Ursaki (Eds.), Nanostructures and Thin Films for Multifunctional Applications,
[26] C. Öğretir, B. Mihçi, G. Bereket, Quantum chemical studies of some pyridine Springer International Publishing, Cham, 2016, pp. 3–42.
derivatives as corrosion inhibitors, J. Mol. Struct. THEOCHEM 488 (1) (1999) [52] E. Barsoukov, J.R. Macdonald, Impedance Spectroscopy: Theory, Experiment,
223–231, https://doi.org/10.1016/S0166-1280(99)00033-0. and Applications, second ed., John Wiley Sons, 2005.
[27] G. Ibrahim, E. Chebli, M.A. Khan, G.M. Bouet, Metallic complexes from 2- [53] I.B. Obot, N.O. Obi-Egbedi, N.W. Odozi, Acenaphtho [1,2-b] quinoxaline as a
furaldehyde semicarbazone and 5-methyl-(2-furaldehyde) semicarbazone, novel corrosion inhibitor for mild steel in 0.5M H2SO4, Corros. Sci. 52 (3)
Transit. Met Chem 24 (1999) 294–298. (2010) 923–926, https://doi.org/10.1016/j.corsci.2009.11.013.
[28] K. Boumhara et al., Use of artemisia mesatlantica essential oil as green [54] N. Eddy, E. Ebenso, Adsorption and inhibitive properties of ethanol extracts of
corrosion inhibitor for mild steel in 1 M hydrochloric acid solution, Int. J. Musa sapientum peels as a green corrosion inhibitor for mild steel in H2SO4,
ElectrochemSci 9 (2014) 1187–1206. Afr J Pure ApplChem 2 (6) (2008) 46–54.
[29] Z. Tao, S. Zhang, W. Li, B. Hou, Corrosion inhibition of mild steel in acidic [55] I.B. Obot, N.O. Obi-Egbedi, Ipomoea involcrata as an ecofriendly inhibitor for
solution by some oxo-triazole derivatives, Corros. Sci. 51 (11) (2009) 2588– aluminium in alkaline medium, Port. ElectrochimicaActa 27 (4) (2009) 517–
2595, https://doi.org/10.1016/j.corsci.2009.06.042. 524, https://doi.org/10.4152/pea.200904517.
[30] H. Zarrok, A. Zarrouk, B. Hammouti, R. Salghi, C. Jama, F. Bentiss, Corrosion [56] U.F. Ekanem, S.A. Umoren, I.I. Udousoro, A.P. Udoh, Inhibition of mild steel
control of carbon steel in phosphoric acid by purpald – Weight loss, corrosion in HCl using pineapple leaves (Ananascomosus L.) extract, J. Mater.
electrochemical and XPS studies, Corros. Sci. 64 (2012) 243–252, https://doi. Sci. 45 (20) (2010) 5558–5566, https://doi.org/10.1007/s10853-010-4617-y.
org/10.1016/j.corsci.2012.07.018. [57] M.M. Saleh, Inhibition of mild steel corrosion by hexadecylpyridinium
[31] S.A.M. Refaey, F. Taha, A.M. Abd El-Malak, Corrosion and Inhibition of 316L bromide in 0.5M H2SO4, Mater. Chem. Phys. 98 (1) (2006) 83–89, https://doi.
stainless steel in neutral medium by 2-Mercaptobenzimidazole, Int. J. org/10.1016/j.matchemphys.2005.08.069.
Electrochem. Sci. 1 (2006) 80–91, https://doi.org/10.20964/1020080. [58] G. Vengatesh, G. Karthik, M. Sundaravadivelu, A comprehensive study of
[32] P.W. Atkins, J. De Paula, Physical chemistry, 8th edition, Oxf. N. Y. Oxf. Univ. ondansetron hydrochloride drug as a green corrosion inhibitor for mild steel in
Press, 2006. 1 M HCl medium, Egypt. J. Pet. 26 (3) (2017) 705–719, https://doi.org/10.1016/
[33] T. Engel, P. Reid, Physical Chemistry, reviseded, N. Y. Pearson Pub, 2006, j.ejpe.2016.10.011.
Accessed: Nov. 06, 2020. [Online]. Available: /content/one-dot-com/one-dot- [59] T. Poornima, J. Nayak, A. Shetty, Corrosion inhibition of the annealed 18 Ni 250
com/us/en/higher-education/product.html. grade maraging steel in 0.67 M phosphoric acid by 3,4-
[34] T. Aissaoui, Y. Benguerba, I.M. AlNashef, Theoretical investigation on the dimethoxybenzaldehydethiosemicarbazone, Chem. Sci. J. 69 (2012) 1–14.
microstructure of triethylene glycol based deep eutectic solvents: COSMO-RS [60] S. Martinez, I. Stern, Thermodynamic characterization of metal dissolution and
and TURBOMOLE prediction, J. Mol. Struct. 1141 (2017) 451–456, https://doi. inhibitor adsorption processes in the low carbon steel/mimosa tannin/sulfuric
org/10.1016/j.molstruc.2017.04.009. acid system, Appl. Surf. Sci. 199 (1–4) (2002) 83–89, https://doi.org/10.1016/
[35] A. Belakhdar, H. Ferkous, S. Djellali, R. Sahraoui, H. Lahbib, Y. Ben amor, A. Erto, S0169-4332(02)00546-9.
M. Balsamo, Y. Benguerba, Computational and experimental studies on the [61] S.T. Keera, M.A. Deyab, Effect of some organic surfactants on the
efficiency of Rosmarinusofficinalis polyphenols as green corrosion inhibitors electrochemical behaviour of carbon steel in formation water, Colloids Surf.
for XC48 steel in acidic medium, J. Colloids Surf. A Physicochem. Eng. Asp. 606 Physicochem. Eng. Asp. 266 (1–3) (2005) 129–140, https://doi.org/10.1016/
(2020) 125458. j.colsurfa.2005.05.069.
[36] A.A. Hermas, M.S. Morad, A comparative study on the corrosion behaviour of [62] M. Abdallah, E. Helal, A. Fouda, Aminopyrimidine derivatives as inhibitors for
304 austenitic stainless steel in sulfamic and sulfuric acid solutions, Corros. corrosion of 1018 carbon steel in nitric acid solution, Corros. Sci. 48 (7) (2006)
Sci. 50 (9) (2008) 2710–2717, https://doi.org/10.1016/j.corsci.2008.06.029. 1639–1654.
[37] F.S. de Souza, A. Spinelli, Caffeic acid as a green corrosion inhibitor for mild [63] A. Popova, E. Sokolova, S. Raicheva, M. Christov, AC and DC study of the
steel, Corros. Sci. 51 (3) (2009) 642–649, https://doi.org/10.1016/ temperature effect on mild steel corrosion in acid media in the presence of
j.corsci.2008.12.013. benzimidazole derivatives, Corros. Sci. 45 (1) (2003) 33–58.
[38] I. Ahamad, M.A. Quraishi, Mebendazole: New and efficient corrosion inhibitor [64] R. Idouhli, Y. Koumya, M. Khadiri, A. Aityoub, A. Abouelfida, A. Benyaich,
for mild steel in acid medium, Corros. Sci. 52 (2) (2010) 651–656, https://doi. Inhibitory effect of Senecio anteuphorbium as green corrosion inhibitor for
org/10.1016/j.corsci.2009.10.012. S300 steel, Int. J. Ind. Chem. 10 (2019) 133–143.
[39] J. Cinatl, B. Morgenstern, G. Bauer, P. Chandra, H. Rabenau, H. Doerr, [65] S. Szabo, I. Bakos, Hydrogen deposition as a rate determining step in metal
Glycyrrhizin, an active component of liquorice roots, and replication of corrosion, Corros. Rev. 22 (3) (2004) 183–192.
SARS-associated coronavirus, The Lancet 361 (9374) (2003) 2045–2046, [66] E.A. Noor, A.H. Al-Moubaraki, Thermodynamic study of metal corrosion and
https://doi.org/10.1016/S0140-6736(03)13615-X. inhibitor adsorption processes in mild steel/1-methyl-4[40 (-X)-
[40] M. Tian, H. Yan, K. Row, Extraction of glycyrrhizic acid and glabridin from styrylpyridinium iodides/hydrochloric acid systems, Mater. Chem. Phys. 110
licorice, Int. J. Mol. Sci. 9 (4) (2008) 571–577, https://doi.org/10.3390/ (1) (2008) 145–154, https://doi.org/10.1016/j.matchemphys.2008.01.028.
ijms9040571. [67] F. Bentiss, C. Jama, B. Mernari, H.E. Attari, L.E. Kadi, M. Lebrini, M. Traisnel, M.
[41] K. Stanly Jacob, G. Parameswaran, Corrosion inhibition of mild steel in Lagrenée, Corrosion control of mild steel using 3,5-bis(4-methoxyphenyl)-4-
hydrochloric acid solution by Schiff base furointhiosemicarbazone, Corros. Sci. amino-1,2,4-triazole in normal hydrochloric acid medium, Corros. Sci. 51 (8)
52 (1) (2010) 224–228, https://doi.org/10.1016/j.corsci.2009.09.007. (2009) 1628–1635, https://doi.org/10.1016/j.corsci.2009.04.009.
[42] H. Hamani, T. Douadi, M. Al-Noaimi, S. Issaadi, D. Daoud, S. Chafaa, [68] M.B. Valcarce, M. Vázquez, Carbon steel passivity examined in solutions with a
Electrochemical and quantum chemical studies of some azomethine low degree of carbonation: The effect of chloride and nitrite ions, Mater. Chem.
compounds as corrosion inhibitors for mild steel in 1M hydrochloric acid, Phys. 115 (1) (2009) 313–321, https://doi.org/10.1016/
Corros. Sci. 88 (2014) 234–245, https://doi.org/10.1016/j.corsci.2014.07.044. j.matchemphys.2008.12.007.
[43] X. Li, S. Deng, H. Fu, T. Li, Adsorption and inhibition effect of 6- [69] R.-M. Saedah, Inhibition of mild steel corrosion using Juniperus plants as green
benzylaminopurine on cold rolled steel in 1.0M HCl, ElectrochimicaActa 54 inhibitior, Afr. J. Pure Appl. Chem. 8 (1) (2014) 9–22.
(16) (2009) 4089–4098, https://doi.org/10.1016/j.electacta.2009.02.084. [70] M.A. Deyab, Hydrogen generation during the corrosion of carbon steel in
[44] F. El-TaibHeakal, S. Haruyama, Impedance studies of the inhibitive effect of crotonic acid and using some organic surfactants to control hydrogen
benzotriazole on the corrosion of copper in sodium chloride medium, Corros. evolution, Int. J. Hydrog. Energy 38 (31) (2013) 13511–13519, https://doi.
Sci. 20 (7) (1980) 887–898, https://doi.org/10.1016/0010-938X(80)90121-3. org/10.1016/j.ijhydene.2013.08.016.
[45] R. Solmaz, E. Altunbasß, G. Kardasß, Adsorption and corrosion inhibition effect of [71] H. Amar, A. Tounsi, A. Makayssi, A. Derja, J. Benzakour, A. Outzourhit, Corrosion
2-((5-mercapto-1,3,4-thiadiazol-2-ylimino)methyl)phenol Schiff base on mild inhibition of Armco iron by 2-mercaptobenzimidazole in sodium chloride 3%
steel, Mater. Chem. Phys. 125 (3) (2011) 796–801, https://doi.org/10.1016/ media, Corros. Sci. 49 (7) (2007) 2936–2945, https://doi.org/10.1016/
j.matchemphys.2010.09.056. j.corsci.2007.01.010.
[46] P.R. Roberge, R. Beaudoin, Evaluation of charge transfer resistance by [72] M. Behpour, S.M. Ghoreishi, N. Soltani, M. Salavati-Niasari, M. Hamadanian, A.
geometrical extrapolation of the centre of semicircular impedance diagrams, Gandomi, Electrochemical and theoretical investigation on the corrosion
J. Appl. Electrochem. 18 (1) (1988) 38–42. inhibition of mild steel by thiosalicylaldehyde derivatives in hydrochloric acid
[47] J.J. García-Jareño, D.X. Giménez-Romero, M. Keddam, F. Vicente, Graphical solution, Corros. Sci. 50 (8) (2008) 2172–2181, https://doi.org/10.1016/
analysis of electrochemical impedance spectroscopy of two consecutive j.corsci.2008.06.020.
14
Chérifa Boulechfar, H. Ferkous, S. Djellali et al. Journal of Molecular Liquids 344 (2021) 117874
[73] S. Paul, B. Kar, Mitigation of mild steel corrosion in acid by green inhibitors: Appl. Surf. Sci. 389 (2016) 952–966, https://doi.org/10.1016/j.
yeast, pepper, garlic, and coffee, Int. Sch. Res. Netw. 2012 (2012) 1–8, https:// apsusc.2016.07.115.
doi.org/10.5402/2012/641386. [86] H. Lahbib, S. Ben Hassen, H. Gerengi, M. Rizvi, Y. Ben Amor, Corrosion
[74] Q. Qing, H. Zhengzheng, L. Lei, B. Wei, L. Yongjun, D. Zhongtao, Synthesis and inhibition performance of dwarf palm and Cynaracardunculus leaves extract
evaluation of Tris-hydroxymethyl-(2-hydroxybenzylidenamino)-methane as a for St37 steel in 15% H 2 SO 4: a comparative study, J. Adhes. Sci. Technol.
corrosion inhibitor for cold rolled steel in hydrochloric acid, Corros. Sci. 51 (3) (2020) 1–32, https://doi.org/10.1080/01694243.2020.1819701.
(2009) 569–574, https://doi.org/10.1016/j.corsci.2008.12.010. [87] W. Temesghen, P. Sherwood, Analytical utility of valence band X-ray
[75] M.A. Hegazy, H.M. Ahmed, A.S. El-Tabei, Investigation of the inhibitive effect of photoelectron spectroscopy of iron and its oxides, with spectral
p-substituted 4-(N, N, N-dimethyldodecylammonium bromide)benzylidene- interpretation by cluster and band structure calculations, Anal. Bioanal.
benzene-2-yl-amine on corrosion of carbon steel pipelines in acidic medium, Chem. 373 (7) (2002) 601–608, https://doi.org/10.1007/s00216-002-1362-3.
Corros. Sci. 53 (2) (2011) 671–678, https://doi.org/10.1016/ [88] K. Babić-Samardžija, C. Lupu, N. Hackerman, A.R. Barron, A. Luttge, Inhibitive
j.corsci.2010.10.004. properties and surface morphology of a group of heterocyclic diazoles as
[76] M. Lebrini, M. Lagrenée, H. Vezin, M. Traisnel, F. Bentiss, Experimental and inhibitors for acidic iron corrosion, Langmuir 21 (26) (2005) 12187–12196,
theoretical study for corrosion inhibition of mild steel in normal hydrochloric https://doi.org/10.1021/la051766l.
acid solution by some new macrocyclic polyether compounds, Corros. Sci. 49 [89] M. Outirite, M. Lagrenée, M. Lebrini, M. Traisnel, C. Jama, H. Vezin, F. Bentiss, ac
(5) (2007) 2254–2269, https://doi.org/10.1016/j.corsci.2006.10.029. impedance, X-ray photoelectron spectroscopy and density functional theory
[77] M. Lebrini, F. Robert, A. Lecante, C. Roos, Corrosion inhibition of C38 steel in studies of 3,5-bis(n-pyridyl)-1,2,4-oxadiazoles as efficient corrosion inhibitors
1M hydrochloric acid medium by alkaloids extract from Oxandraasbeckii for carbon steel surface in hydrochloric acid solution, ElectrochimicaActa 55
plant, Corros. Sci. 53 (2) (2011) 687–695, https://doi.org/10.1016/ (5) (2010) 1670–1681, https://doi.org/10.1016/j.electacta.2009.10.048.
j.corsci.2010.10.006. [90] M. Lebrini, M. Lagrenée, M. Traisnel, L. Gengembre, H. Vezin, F. Bentiss,
[78] A.M. Badiea, K.N. Mohana, Effect of temperature and fluid velocity on corrosion Enhanced corrosion resistance of mild steel in normal sulfuric acid medium by
mechanism of low carbon steel in presence of 2-hydrazino-4,7- 2,5-bis(n-thienyl)-1,3,4-thiadiazoles: electrochemical, X-ray photoelectron
dimethylbenzothiazole in industrial water medium, Corros. Sci. 51 (9) spectroscopy and theoretical studies, Appl. Surf. Sci. 253 (23) (2007) 9267–
(2009) 2231–2241, https://doi.org/10.1016/j.corsci.2009.06.011. 9276, https://doi.org/10.1016/j.apsusc.2007.05.062.
[79] S. Martinez, I. Stern, Thermodynamic characterization of metal dissolution and [91] A. Galtayries, R. Warocquier-Clérout, M.-D. Nagel, P. Marcus, Fibronectin
inhibitor adsorption processes in the low carbon steel/mimosa tannin/sulfuric adsorption on Fe–Cr alloy studied by XPS, Surf. Interface Anal. 38 (4) (2006)
acid system, Appl. Surf. Sci. 199 (1) (2002) 83–89, https://doi.org/10.1016/ 186–190, https://doi.org/10.1002/(ISSN)1096-991810.1002/sia.v38:410.1002/
S0169-4332(02)00546-9. sia.2295.
[80] J. Marsh, Advanced Organic Chemistry, third ed., Wiley East, New Delhi, 1988, [92] P. Okafor, V.I. Osabor, E. Ebenso, Eco-friendly corrosion inhibitors: Inhibitive
https://doi.org/10.1002/jps.3030491220. action of ethanol extracts of Garcinia kola for the corrosion of mild steel in
[81] J.H. Hong, S.H. Lee, J.G. Kim, J.B. Yoon, Corrosion behaviour of copper H2SO4 solutions, Pigment Resin Technol. 36 (5) (2007) 299–305, https://doi.
containing low alloy steels in sulphuric acid, Corros. Sci. 54 (2012) 174–182, org/10.1108/03699420710820414.
https://doi.org/10.1016/j.corsci.2011.09.012. [93] E. Kowsari, M. Payami, R. Amini, B. Ramezanzadeh, M. Javanbakht, Task-
[82] B. Mezhoud, M. Bouchouit, E.M. Said, L. Messaadia, A. Belfaitah, H. Merazig, A. specific ionic liquid as a new green inhibitor of mild steel corrosion, Appl. Surf.
Chibani, S. Bouacida, A. Bouraiou, Erratum to: Synthesis, X-ray structure and Sci. 289 (2014) 478–486, https://doi.org/10.1016/j.apsusc.2013.11.017.
theoretical study of benzazolethioether and its zinc complex as corrosion [94] A. Döner, R. Solmaz, M. Özcan, G. Kardasß, Experimental and theoretical studies
inhibitors for steel in acidic medium, Res. Chem. Intermed. 43 (4) (2017) 2691, of thiazoles as corrosion inhibitors for mild steel in sulphuric acid solution,
https://doi.org/10.1007/s11164-016-2783-5. Corros. Sci. 53 (9) (2011) 2902–2913, https://doi.org/10.1016/
[83] H. Gerengi, I. Uygur, M. Solomon, M. Yildiz, H. Goksu, Evaluation of the j.corsci.2011.05.027.
inhibitive effect of Diospyros kaki (Persimmon) leaves extract on St37 steel [95] Y. Zhou, L. Guo, S. Zhang, S. Kaya, X. Luo, B. Xiang, Corrosion control of mild
corrosion in acid medium, Sustain. Chem. Pharm. 4 (2016) 57–66. steel in 0.1 M H2SO4 solution by benzimidazole and its derivatives: an
[84] M. Tourabi, K. Nohair, M. Traisnel, C. Jama, F. Bentiss, Electrochemical and XPS experimental and theoretical study, RSC Adv. 7 (39) (2017) 23961–23969,
studies of the corrosion inhibition of carbon steel in hydrochloric acid pickling https://doi.org/10.1039/C7RA02192E.
solutions by 3,5-bis(2-thienylmethyl)-4-amino-1,2,4-triazole, Corros. Sci. 75 [96] S.-W. Xie, Z. Liu, G.-C. Han, W. Li, J. Liu, Z. Chen, Molecular dynamics simulation
(2013) 123–133, https://doi.org/10.1016/j.corsci.2013.05.023. of inhibition mechanism of 3,5-dibromo salicylaldehyde Schiff’s base, Comput.
[85] M. Bouanis, M. Tourabi, A. Nyassi, A. Zarrouk, C. Jama, F. Bentiss, Corrosion Theor. Chem. 1063 (2015) 50–62, https://doi.org/10.1016/
inhibition performance of 2,5-bis(4-dimethylaminophenyl)-1,3,4-oxadiazole j.comptc.2015.04.003.
for carbon steel in HCl solution: gravimetric, electrochemical and XPS studies,
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