Results in Physics 8 (2018) 728–733

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Results in Physics
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Synthesis and characterization of a novel organic corrosion inhibitor for

mild steel in 1 M hydrochloric acid
Mohammed H. Othman Ahmed a, Ahmed A. Al-Amiery b,⇑, Yasmin K. Al-Majedy b, Abdul Amir H. Kadhum a,
Abu Bakar Mohamad a, Tayser Sumer Gaaz c,⇑
a
Department of Chemical & Process Engineering, Faculty of Engineering & Built Environment, Universiti Kebangsaan, Malaysia
b
Energy and Renewable Energies Technology Center, University of Technology, Baghdad 10001, Iraq
c
Department of Machinery Equipment Engineering Techniques, Technical College Al-Musaib, Al-Furat Al Awsat Technical University, Al-Musaib, Babil 51009, Iraq

a r t i c l e i n f o a b s t r a c t

Article history: The synthesis and characterization of a novel organic corrosion inhibitor (4-(3-mercapto-5,6,7,8-tetrahy
Received 16 October 2017 dro-[1,2,4]triazolo[4,3-b][1,2,4,5]tetrazin-6-yl)phenol), for mild steel in 1 M hydrochloric acid (HCl) has
Received in revised form 16 December 2017 been successfully reported for the first time. The inhibitor evaluated as corrosion inhibitor for mild steel
Accepted 17 December 2017
in 1 M of Hydrochloric acid solution using electrochemical impedance spectroscopy (EIS), and electro-
Available online 10 January 2018
chemical frequency modulation (EFM) measurement techniques. Changes in the impedance parameters
suggested an adsorption of the inhibitor onto the mild steel surface, leading to the formation of protective
Keywords:
films. The results show that the inhibition efficiencies increased with increasing the concentrations of the
Corrosion
Inhibitor
inhibitors and decreased with increasing temperature. The maximum inhibition efficiency up to 67% at
Mild steel the maximum concentration 0.5 mM. This shows that those inhibitors are effective in helping to reduce
EIS spectroscopy and slowing down the corrosion process that occurs to mild steel with a hydrochloric acid solution by
providing an organic inhibitor for the mild steel that can be weakened by increasing the temperature.
The adsorption process of the synthesized organic inhibitor depends on its electronic characteristics in
addition to steric effects and the nature of metal surface, temperature degree and the varying degrees
of surface-site activity. The synthesized inhibitor molecules were absorbed by metal surface and follow
Langmuir isotherms.
Ó 2017 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND
license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

Introduction acidization in industrial cleaning processes [6]. Organic additives

prevent the adsorption of chloride ions and/or the formation of a
Mild steel, also known as low carbon steel, is a low cost and more resistant oxide film on the metal surface [7]. The inhibition
remarkable material in industrial technology because it is exten- efficiency of these compounds depends mainly on the structure
sively used in chemical and allied industries for the handling of and nature of the adsorbed layer on the metal surface [8]. Organic
acid, alkali and salt solutions [1]. However, its tendency to corrode compounds, mainly containing nitrogen, oxygen, sulfur and phos-
makes it unsuitable for exposure to acids. The use of inhibitors is phorus atoms and having multiple bonds, are recognized as effec-
one of the most practical methods for protection against corrosion tive inhibitors for the corrosion of many metals and alloys [9]. O, N,
in acidic media [2]. Corrosion inhibitors are chemical compounds S and P, they found to act as corrosion inhibitors due to their active
that in small quantities can retard the degradation of metals in centers for the process of adsorption on metal surfaces, higher
hostile environments [3]. Organic inhibitors have been widely used basicity as well as electron density. The inhibition efficiency should
due to the ability of these compounds to prevent corrosion in var- follow the sequence O < N < S < P [10]. Adsorption depends mainly
ious corrosive environments [4]. These compounds can adsorb on certain physicochemical properties of the inhibitor group, such
onto the mild steel surface and block active sites, thus decreasing as electron density at the donor atom and orbital character and
the corrosion rate [5]. In addition, a variety of organic compounds electronic structure of the molecule [11]. The adsorption of organic
have been reported to be effective as corrosion inhibitors during molecules at the metal/solution interface is of great interest in sur-
face science and can markedly change the corrosion resistance of
⇑ Corresponding authors. the metal [12]. It is generally accepted that the first step in the
E-mail addresses: [email protected] (A.A. Al-Amiery), taysersumer@ adsorption of an organic inhibitor on a metal surface usually
gmail.com (T.S. Gaaz).

https://doi.org/10.1016/j.rinp.2017.12.039
2211-3797/Ó 2017 The Authors. Published by Elsevier B.V.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
 Mohammed H. Othman Ahmed et al. / Results in Physics 8 (2018) 728–733 729

involves replacement of one or more water molecules adsorbed at %) of the mild steel was as follows: Fe, 99.21; C, 0.21; Si, 0.38; P,
the metal surface [13]. The inhibitor may then combine with 0.09; S, 0.05; Mn, 0.05; and Al, 0.01. The specimens were cleaned
freshly generated Fe2+ ions on the steel surface, forming metal according to ASTM standard procedure G1-03 [21]. Measurements
inhibitor complexes [14]. The organic inhibitors function through were conducted in aerated, non-stirred 1.0 M HCl solutions con-
adsorption on the metal surface blocking the active sites by dis- taining different concentrations of the inhibitor. Electrochemical
placing water molecules and forming a compact barrier film to measurements were performed at the steady-state corrosion
decrease the corrosion rate [15]. Acid solutions are widely used potential using a Gamry euro cell. The cell contained three elec-
in industrial applications, such as acid pickling, industrial acid trodes, working, counter and reference electrodes, which were
cleaning, acid descaling and oil well acidizing. As of result of the composed of mild steel, a graphite bar and a saturated calomel
general aggressiveness of acid solutions, inhibitors are commonly electrode (SCE), respectively. The measurements were performed
used to reduce corrosive attack on metallic materials [16]. using the Gamry Instrument Potentiostat/Galvanostat/ZRA (REF
In continuation of previous work [17–20], we focus herein on 600) model (Gamry, Warminster, PA, USA). DC105 and EIS300 soft-
the design our approach to increase the inhibitive properties based ware by Gamry were used to perform the corrosion potential, elec-
on conjugated system and electron density, so to the best of our trochemical impedance spectroscopy (EIS) and electrochemical
knowledge novel corrosion organic inhibitor namely 4-(3-mer frequency modulation (EFM) measurements. EIS measurements
capto-5,6,7,8-tetrahydro-[1,2,4]triazolo[4,3-b][1,2,4,5] tetrazin-6- were performed using the AC signals of the 5 mV peak-to-peak
yl)phenol has been successfully synthesized and employed as a amplitude at the corrosion potential in the frequency range of
corrosion inhibitor for mild steel in 1 M hydrochloric acid. The 100 kHz to 0.1 Hz. All impedance data were fit to appropriate
inhibitory effect was investigated using various electrochemical equivalent circuits (ECs) using the Gamry Echem Analyst software.
measurement techniques such as Electrochemical Impedance EFM measurements were carried out at 0.1 Hz base frequency with
Spectroscopy (EIS), and electrochemical frequency modulation applied AC potential of 10 mV for 20 cycles. The electrochemical
(EFM). measurements began to be collected approximately 30 min after
the working electrode was immersed in the solution to allow the
steady state potential to stabilize. Each measurement was repeated
Materials and methods
five times, and only the average values were reported to verify
reproducibility of the experiments.
Chemistry

Synthesis of corrosion inhibitor (4-(3-mercapto-7,8-dihydro-[1 Results and discussion

,2,4]triazolo[4,3-b][1,2,4,5] tetrazin-6-yl)phenol). Mixture of 4-
hydroxybenzaldehyde (1.22 g, 10 mmol) and 4-amino-5-hydrazi Synthesis
nyl-4H-1,2,4-triazole-3-thiol (Purpald) (1.46 g. 10 mmol) with fer-
ric ammonium sulfate (5.0 g, 10 mmol) in water (50 mL) was The synthesis was carried out by refluxing purpald with
reacted under reflux condition. After 6 h, a solution of ferric ammo- 4-hydroxybenzaldehyde in the presence of with ferric ammonium
nium sulfate (20 mmol, 10 g) in water (50 mL) was added to the sulfate. The molecular weight of the synthesized corrosion
mixture of reaction. The reaction continued for 4 h, the progress inhibitor was 248 g/mol that was calculated based on the molecu-
of the reaction was monitored by TLC, using ethyl acetate: n- lar formula (C9H8N6OS) and supported via mass spectrometry.
hexane (1:1). The mixture of the reaction was cold; the precipitate (4-(3-mercapto-5,6,7,8-tetrahydro-[1,2,4]triazolo[4,3-b][1,2,4,5]
was filtered, washed with water, dried and recrystallized by etha- tetrazin-6-yl)phenol) can be dissolved in acetone, dichloro-
nol. IR: 3305.1 and 3278.8 cm
1 (NH), 3155 cm
1 (OAH), 3082.5 methane, dimethylformamide, dimethylsulfoxide, ethanol or
cm
1 (CAH; aromatic group), and 16132.9 cm
1 (C@N). 1H NMR methanol solutions. Fig. 2- SI, shows a proton-NMR spectrum for
(d 2.053 for Acetone as a solvent): ds, 2.935 NH; s, 3.298 NH; 5.1 the corrosion inhibitor in which absorption bands at 3305.1 and
OH; dd 6.990 and 7.004 for CH aromatic; dd 7.775 and 7.790 for 3278.8 cm
1 for amine NH and azomethane (C@N) and stretching
CH aromatic; 9.837 for SH. 13C NMR (Acetone solvent has d29.45 at 16132.9 cm
1 can be seen. The bands at 3155 and 3082.5 cm
1
and 206.31): 116.45CAH for OHAC@CAH; 125.25 = CAC; (127.39, are from OAH and CAH aromatic respectively. The 1H NMR spec-
129.24, 130.43, 132.79 Aromatic carbons), 146.41C@N, trum exhibits two singlet signals at d2.935 ppm an 3.298 ppm due
159.89CAOH; 161.71C@N; 163.99N@CASH. to the NAH protons groups respectively, d 5.100 (s, 1H, for OH),
To synthesize (4-(3-mercapto-5,6,7,8-tetrahydro[1,2,4]triazolo and d6.990 (d, 1H), 7.004 (s, 1H), 7.775 (d, 1H) and 7.790 (s, 1H) for
[4,3-b][1,2,4,5]tetrazin-6-yl) phenol) as a corrosion inhibitor, the aromatic ring, also at d9.837 (s, 1H, for
SH) (Fig. 2- SI).
reaction sequence outlined in Fig. 1 was followed, starting from Fig. 3- SI, illustrates a 13C NMR, spectrum for the corrosion inhi-
commercially available 4-hydroxybenzaldehyde and (Purpald). bitor in which a signal appears at 163.99 ppm due to the N@CASH
group also 159.89 ppm and 146.41 ppm are from hydroxyl and
Electrochemical measurements azomethane groups respectively. Bands at 127.39, 129.24, 130.43
and 132.79 ppm are from carbon atoms in the aromatic ring.
Mild steel specimens were obtained from Gamry Instruments
Inc. and were used as working electrodes throughout this study, Electrochemical results
each with an active surface area of 4.5 cm2. The composition (wt
Electrochemical impedance spectroscopy (EIS)
EIS is another method to test the effectiveness of corrosion inhi-
bitors that is used to protect the surface of the mild steel in the
acidic solution (1M HCl). Different corrosion system (e.g., charge
transfer control, diffusion control or a mixture type) may show dif-
ferent features in the EIS spectra. Through analyzing the EIS data
(Nyquist plot), the corrosion mechanism of the system can be iden-
tified. In practice, EIS data are often interpreted in terms of electri-
Fig. 1. Chemical synthesis of inhibitor. cal equivalent circuits that can be used to describe the electrical
730 Mohammed H. Othman Ahmed et al. / Results in Physics 8 (2018) 728–733

features of the electrochemical interfaces [22]. The Nyquist plot As shown in Fig. 3, the impedance response of mild steel is sig-
contains a ‘‘depressed” semicircle with the center under the real nificantly altered after the addition of inhibitor to the corrosive
axis, such behavior characteristic for solid electrodes and often solution. This result can be attributed to an increase in the sub-
referred to as frequency dispersion, which have been attributed strate impedance with increased inhibitor concentration. The next
to roughness and inhomogeneity of the surface [23]. Two ways experiments is using the same concentration of corrosion inhibitor
are used in the literature to describe the EIS spectra for the inho- that is 0.5 mM but at different temperatures which were 30, 40, 50
mogeneous films on the metal surface or rough and porous elec- and 60 °C.
trodes. One is the finite transmission line model [24] and the Based on Fig. 3, we can see that the graph of semi-circle at 60 °C
other is the filmed equivalent circuit model [25], which is usually is the smallest and at 30 °C was greatest. This shows that the diam-
proposed to study the degradation of coated metals [26]. It has eter of the semi-circle is getting smaller with increasing tempera-
been suggested that the EIS spectra for the metal covered by ture. These results suggest that the inhibition of corrosion is
organic inhibitor films are very similar to the failed coating metals significantly reduced with increasing temperature. Increasing the
[27]. The tests were carried out at 30 °C with the absence and the temperature of the solution accelerates the corrosion process that
presence of different concentrations of the corrosion inhibitor occurs due to changes in the operating mechanism of corrosion
ranging from 0.030 to 0.050 mM as shown in Fig. 2. [28]. From Fig. 3, the total impedance of mild steel in the presence
of 0.5 mM decreases with increasing solution temperature. This
behavior is due to desorption of adsorbed inhibitor molecules from
the mild steel surface. The experimental data for the two Figs. are
summarized in Tables 1 and 2. There is a considerable increase in
the total impedance observed with the addition of corrosion inhi-
bitor as shown in Tables 1 and 2. In the impedance spectrum of
mild steel in the presence of response, the Nyquist plots have
two loops: one loop in the high frequency region (HF) and another
at an intermediate frequency (MF), with slight inductive behavior
at low frequencies (LF). The HF and MF loops are attributed to
the electrode and charge-transfer process, respectively. The induc-
tive behavior observed in the LF region is attributed to relaxation of
the adsorption of corrosion products or to the adsorption of inhibi-
tor molecules on the mild steel surface in acidic solution in the
absence and presence of inhibitor, respectively [29–30]. Similar
behavior is observed for all temperatures examined. The corroding
surface of the working electrode is expected to be inhomogeneous
due to its roughness; therefore, the capacitance is presented
Fig. 2. Nyquist plots for mild steel in 1.0 M HCl with various concentrations of the
through a constant phase element (CPE). The EIS results were ana-
inhibitor at 30 °C. lyzed using the equivalent circuit mentioned elsewhere [31], as
shown in Fig. 4. The inhibition efficiencies (IE%) were calculated
from the charge transfer resistance using the Eq. (1):

ðIE%Þ ¼ ðRp
Rp =Rp Þ  100 ð1Þ

where Rop and Rp indicate the charge transfer resistances in the pres-
ence and absence of corrosion inhibitor, respectively.
By using the Gamry Analyst software, EIS experimental data can
be obtained with CPE data matching. In Table 1, Rs is the solution
resistance, CPE is the constant phase element, Rp, is the charge
transfer resistance and Cdl is the double layer charge [32]. Table 1
shows the EIS data for 1.0 M HCl with different corrosion inhibitor
concentrations at 30 °C, where the Cdl values decrease and the Rp
values increase with the increasing of inhibitor concentrations.
This is due to the gradual replacement of water molecules by the
adsorption of the inhibitor molecules on the metal surface, and
decreasing the extent of dissolution reaction. The high Rp values
are generally associated with slower corroding system [33]. While
the decrease in Cdl values resulted from the decrease of the local
Fig. 3. Nyquist plots for mild steel in 1.0 M HCl with 0.5 mM of the inhibitor at dielectric constant and/or from the increase of thickness of the
various temperatures ranging from 30 to 60 °C.
electrical double layer [34]. The corrosion inhibitor molecules

Table 1
CPE data for mild steel in 1.0 M HCl with different corrosion inhibitor concentrations at 30 °C.

Concentration (mM) Rs (ohm cm2) Rp (ohm cm2) CPEdl CPEdl IE

Yo (mSsa cm
2) a (mF cm
2) (%)
Blank 1.71 1.71 8983 0.65 152,400 0.00
0.30 3.02 3.02 7208 0.70 181,400 43.45
0.40 3.57 3.57 6473 0.69 156,600 52.07
0.50 4.21 4.21 4134 0.73 116,800 59.36
 Mohammed H. Othman Ahmed et al. / Results in Physics 8 (2018) 728–733 731

Table 2
CPE data for mild steel in 1.0 M HCl with 0.5 mM corrosion inhibitor at different temperatures.

Temp. (°C) Concentration (mM) Rs (ohm cm2) Rp (ohm cm2) CPEdl CPEdl IE
a
2
2
Yo (mSs cm ) a (mF cm ) (%)
30 Blank 1.71 1.71 8983 0.65 152,400 0.00
30 0.50 4.208 4.208 4134 0.73 116,800 59.36
40 Blank 2.77 2.77 21,880 0.58 2,531,000 0.00
40 0.5 3.96 3.96 11,320 0.61 1,238,000 30.05
50 Blank 1.60 1.60 5118 0.73 4,448,000 0.00
50 0.5 2.17 2.17 1145 0.62 4,035,000 26.27
60 Blank 1.51 1.52 5071 0.73 14,460,000 0.00
60 0.5 1.92 1.88 1155 0.63 11,120,000 19.15

Fig. 4. Equivalent model used to fit impedance data for mild steel in 1.0 M HCl in the absence and presence of the inhibitor.

absorbed on the surface of mild steel samples form a protective instead of one. EFM has many advantages over the harmonic
layer on the mild steel. Great resistance transfer charges commen- method, including data validations, a larger current response and
surate with systems that corrode slowly. With the increase in the an insensitivity to harmonics in the perturbation signal.
value of Rp, the efficiency of inhibition (IE) also increased. The inhibition efficiencies of the corrosion inhibitors (IE) were
Table 2 illustrates that the Rp and inhibition efficiency (IE) calculated using the Eq. (2).
decreased when the temperature increased from 30 to 60 °C. This  
could be attributed to the fact that corrosion inhibitor molecules IEð%Þ ¼ ðicorr
icorr =icorr Þ  100 ð2Þ
which are adsorbed on the surface of the mild steel will undergo where i°corr and icorr are the corrosion current density without and
condensation when the temperature increases [35]. Adsorption of
with corrosion inhibitor.
organic compounds can be divided into two main types, physical Table 3 shows the electrochemical parameters of EFM for mild
adsorption and interaction ’chemisorption’. The presence of a
steel in 1.0 M HCl at 30 °C with different concentrations of the cor-
metal having vacant low energy electron orbital and of an inhibitor rosion inhibitor. icorr decreases by increasing the inhibitor concen-
with molecules having relatively loosely bound electrons or het-
tration. The corrosion rate decreased from 174.81mpy to 62.75
eroatoms with lone pair electrons. However, the compound mpy which demonstrates the effectiveness of the corrosion inhibi-
reported is an organic base which can be protonated in an acid
tor. The standard values for CF-2 and CF-3 are 2.0 and 3.0, respec-
medium [36]. As shown in Tables 1 and 2, the Rp values increase
tively. If causality factors differ from 2 to 3, one may conclude that
with increasing concentration but decrease significantly with
the measurement is affected by noise. If the value of the causality
increasing solution temperature. Fig. 4 illustrates the circuit model
factor approximates the standards, a correlation exists between
employed in this work.
the perturbation and response signals; therefore, the data are
accepted. If CF-2 and CF-3 are in the range of 0–2 and 0–3, the
Electrochemical frequency modulation (EFM) EFM data are valid. Any deviation in the causality factor from the
Electrochemical frequency modulation (EFM) is a new corrosion theoretical value may be due to perturbation amplitude that is
measurement technique for determining corrosion rate without too small, in insufficient resolution in the spectrum frequency, or
preliminary knowledge of the Tafel constants [37]. The main an inhibitor that is not functioning properly [39].
advantage of this technique is that corrosion rate, Tafel parameters IE increases with increasing the concentration of the inhibitors
and causality factors are measured in a single data set [38]. While as shown in Table 3. IE decreases with the increment of the tem-
using EFM, a potential perturbation signal composed of two sine perature as it is shown in Table 4. This result suggests that the inhi-
waves is applied to any corroding specimen to obtain a current bitor molecules adsorb physically on the mild steel surface and not
response. EFM has been used for different combinations of metals chemically; therefore, increasing temperature enhances both the
and electrolytes to accurately measure corrosion parameters. This dissolution of metal and the desorption of inhibitor molecules from
technique is similar to the harmonic method which employs a the metal surface.
lower-amplitude (20 mV) sinusoidal perturbation signal but, The corrosion parameters, including corrosion efficiency (IE%),
unlike the harmonic method, is composed of two sine waves corrosion current density (lA cm
2), Tafel constant and causality
732 Mohammed H. Othman Ahmed et al. / Results in Physics 8 (2018) 728–733

Table 3
Electrochemical frequency modulation (EFM) parameters for mild steel in 1.0 M HCl with various concentrations of the corrosion inhibitor at 30 °C.

Concentration (mM) icorr (mAcm2) b1 (mVdec
1) b2 (mVdec
1) Corrosion Rate (mpy) IEEFM (%) CF-2 CF-3
0.00 0.1965 75.90 88.12 174.81 0.00 1.685 4.027
0.30 0.1271 101.94 114.27 97.45 35.32 1.407 2.77
0.40 0.0977 114.65 120.30 83.85 50.28 0.834 4.207
0.50 0.0648 119.11 131.62 62.75 67.02 0.678 3.448

Table 4
EFM parameters for mild steel in 1.0 M HCl with 0.5 mM of the corrosion inhibitor at various temperatures.

Temp. (°C) Concentration (mM) icorr (mAcm2) b1 (mVdec
1) b2 (mVdec
1) Corrosion Rate (mpy) IEEFM (%) CF-2 CF-3
30 Blank 0.1965 75.90 88.12 174.81 0.00 1.685 4.027
30 0.50 0.0648 119.11 131.62 62.75 67.02 0.678 3.448
40 Blank 0.2785 88.58 119.27 281.57 0.00 1.731 1.715
40 0.5 0.1716 109.79 123.96 165.34 38.38 1.782 3.833
50 Blank 0.3657 91.02 122.13 363.08 0.00 1.855 4.268
50 0.5 0.2953 119.17 131.78 162.94 19.25 1.752 3.493
60 Blank 0.268 96.99 132.07 183.97 26.72 391.5 4.791
60 0.5 0.4951 128.86 142.06 362.86 10.26 3.844 3.112

Conclusions

In this manuscript, we presented for the first time a novel

organic inhibitor which was tested and the changes in electro-
chemical impedance spectroscopy (EIS) and Electrochemical fre-
quency modulation (EFM) measurements were utilized to study
the corrosion inhibition of mild steel in 1.0 M HCl solutions at
30, 40, 50 and 60 °C, with the use of the inhibitor. This inhibitor
exhibited a good inhibition performance as an organic inhibitor.
This inhibitor has heteroatoms, O, and N that are found to have
higher basicity and electron density and thus act as corrosion inhi-
bitors. The acidic corrosion of mild steel was reduced by addition of
appropriate novel inhibitor concentrations. The inhibition efficien-
cies increased with inhibitor concentration but were reduced pro-
Fig. 5. Langmuir’s isotherm adsorption synthesized corrosion inhibitor on the mild portionally with temperature. The inhibitor acts as an efficient
steel surface in 1.0 M HCl at 303 K.
corrosion inhibitor on a mild steel surface with a maximum inhibi-
tion efficiency of 59.36%.
factors (CF-2 and CF-3), are listed in Tables 3 and 4 for different
concentrations of the corrosion inhibitor in 1.0 M HCl at 30 °C
Acknowledgments
and at different temperatures, respectively.

The authors gratefully acknowledge the Universiti Kebangsaan

Adsorption isotherm Malaysia under grant DIP-2012-02.

Adsorption isotherms can provide basic information about the

Appendix A. Supplementary data
interaction between the inhibitor and mild steel surface [40]. The
corrosion inhibition of organic inhibitors on mild steel in sulfuric
Supplementary data associated with this article can be found, in
acid can be explained via the molecular adsorption method. The
the online version, at https://doi.org/10.1016/j.rinp.2017.12.039.
adsorption process is influenced by the structure of the organic
compounds, the charge distribution in the molecules, the nature
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