Corros Rev 2018; aop

Review

Anees A. Khadom* and Salah N. Farhan

Corrosion inhibition of steel in phosphoric acid

https://doi.org/10.1515/corrrev-2017-0104 phenomenon known as corrosion. A good definition of
Received June 29, 2017; accepted January 6, 2018 corrosion is as follows: “Corrosion is the degradation of a
metal by an electrochemical reaction with its environment”
Abstract: Phosphoric acid has been used in many indus-
(Trethewey and Chamberlain, 1996). The significance of
trial applications and can be in contact with a lot chemi-
corrosion studies is threefold. The most significance is eco-
cal and petrochemical equipment. Most of this equipment
nomic, including the objective of reducing material losses
is made of steel alloys that may be damaged because of
resulting from the corrosion of piping, tanks, metal parts
contact with acid. Corrosion inhibitors can be used for to
of machines, ships, etc. The second is enhanced safety of
protect steel alloys against several forms and various envi-
operating equipment, which through corrosion may fail
ronments of corrosion. In this paper, the efficiency and
with terrible consequences, such as pressure vessels and
applications of organic and inorganic inhibitors in dif-
boilers. The third is safeguarding, applied mainly to metal
ferent environments of phosphoric acid are investigated.
resources whose world supply is limited and their deple-
More than 40 papers were collected and reviewed. Surveys
tion includes corresponding losses of energy and water
of the stated works in phosphoric acid environments are
reserves related with the production and manufacture of
documented. It was concluded that organic inhibitors per-
metal structures. Losses contributed by industry, by the
formed as good corrosion inhibitors and are used widely.
military and by municipalities amount to many billions
The use of inorganic inhibitors was limited. Most of stud-
of dollars annually (Uhlig, 1971). Steel and steel alloys are
ied inhibitors follow Langmuir’s adsorption isotherm,
subjected to the action of acids in many different ways
and the mechanism of the inhibition can be ascribed to
and by many different causes. The exposure can be very
the mixed effect on cathodic and anodic reactions. The
severe, but in many cases, the corrosion can be controlled
synergistic effect was also addressed in the present work.
by means of anticorrosion chemicals. Processes in which
Keywords: alloy; chemistry; corrosion; inhibitor; phos- acids play a very significant role are as follows (George,
phoric acid; steel. 1974): Acid pickling is the removal of unwanted oxide from
metals and for preparing the surface for further opera-
tions, such as enameling and painting. Industrial acid

1 Introduction cleaning is applied essentially for the removal of scale and

undesirable deposits from steam-generating equipment
and from chemical and petrochemical reaction vessels.
In nature, most metals that originate in a chemically joint
Hydrochloric acid is widely used. Sulfuric and phosphoric
state are known as ore. Ores may be oxides, sulfides, car-
acids are also used for chemical cleaning. Oil well acidiz-
bonates, or other complex compounds. In order to sepa-
ing is used for simulations, wherein large quantities of
rate a metal such as iron from one of its ores, e.g. iron
acid are pumped at high rates of flow through the oil well
oxide, a large amount of energy is essential. Therefore,
tubing in the production process. The primary objective is
metals in their uncombined condition are usually in high-
to act on the formation in such a way as to simulate the oil
energy states. Thermodynamic laws tell us that there is
flow. One of the used acids in these processes is the phos-
a high trend for high-energy states to convert into low-
phoric acid. Also, phosphoric acid solutions are an effi-
energy states. It is this tendency of metals to recombine
cient catalyst for organic reactions such as the alkylation
with components of the environment that yields to the
of aromatic hydrocarbons with olefins, the isomerization
of olefins, and the polymerization of normally gaseous
olefins (Khadom, 2000). Therefore, it is very important to
*Corresponding author: Anees A. Khadom, Chemical Engineering
study the corrosion and corrosion prevention of carbon
Department, College of Engineering, Diyala University Alqudis
Street, Diyala 32001, Iraq, e-mail: aneesdr@gmail.com
steel by phosphoric acid. The present work is a step in the
Salah N. Farhan: Chemical Engineering Department, College of direction toward understanding the corrosion of carbon
Engineering, Diyala University Alqudis Street, Diyala 32001, Iraq steel by phosphoric acid (H3PO4) and its inhibition by

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2      A.A. Khadom and S.N. Farhan: Corrosion inhibition of steel in phosphoric acid
means of a literature review of previous and recent works.
Mass loss and potentiostatic polarization techniques were
used. Corrosion rates, inhibition efficiency, and other cor-
rosion parameters were obtained.
2 C
 orrosion inhibition via organic
inhibitors
The use of organic materials as corrosion inhibitors is one
of the most useful methods for protecting against corro-
sion, and it is becoming progressively more common. The
existing data show that organic inhibitors act by adsorp-
tion on the metal surface and creation of a protective layer.
The adsorption of organic inhibitors at the metal/solution
interface takes place through the replacement of water
molecules by the organic inhibitor materials according to
the following equation (Ramazan et al., 2011):
Org(sol) + xH2O(ads) →  Org(ads) + xH2O(sol) (1)
where Org(sol) and Org(ads) are organic molecules in the
solution and organic molecules adsorbed on the metal
surface, respectively, and x is the number of water mole-
cules replaced by the organic molecules. Generally, acid
inhibitors are organic compounds that contain nitrogen,
sulfur, oxygen or phosphorus with the structure of aro-
matic ring or triple bonds. The efficiency of inhibition
of corrosion decreases according to the following order:
O < N < S < P (Subramanyam et al., 1993). It has also been
found that the molecules containing both nitrogen and
sulfur in their molecular structure have shown better cor-
rosion inhibition efficiency in comparison with those that
only have one of these atoms (Behpour et al., 2009).
Poornima et  al. (2011) studied the effect of 4-(N,N-
diethylamino)benzaldehyde thiosemicarbazone (DEABT)
and its corrosion inhibition on the corrosion of a steel
alloy in 0.67 m H3PO4 solution at 30–50°C by poten-
tiodynamic polarization, electrochemical impedance
spectroscopy (EIS) and weight loss methods. Inhibi-
tion effectiveness of DEABT was found to rise with the
increase in DEABT concentration and decline with the
increase in temperature. The activation energy Ea and
other thermodynamic factors have been assessed and
discussed. The adsorption of DEABT on the steel surface
follows the Langmuir adsorption isotherm model, and
the inhibitor showed mixed-type inhibition performance.
Yaro et  al. (2013) investigated the corrosion inhibi-
tion of low-carbon steel in 1 m phosphoric acid using
apricot juice at variable temperatures in accordance to the
mass loss method. Adsorption, activation, and statistical
studies were reviewed in this work. Adsorption studies
showed that the inhibitor adsorbed on metal surface in
relation to the Langmuir isotherm. The average value of
heat of adsorption was −14.93 kJ/mol that shows a spon-
taneous physical adsorption on a metal surface. Activa-
tion parameters did not change by the addition of the
inhibitor, indicating that there is no change in the reaction
mechanism. Analysis of variance was also applied. This
analysis showed that the corrosion rate is influenced by
temperature, inhibitor concentration, and the combined
interaction of both.
Li et al. (2011) studied the inhibition effect of benzyl-
trimethylammonium iodide (BTAI) on the corrosion of
steel in 7.0 m H3PO4 produced by a dihydrate wet method
process using weight loss, potentiodynamic polarization,
EIS, and scanning electron microscopy (SEM) methods.
The outcomes show that BTAI is a decent inhibitor, and the
adsorption of BTAI follows the Langmuir adsorption iso-
therm. Polarization data show that BTAI acts as a mixed-
type inhibitor. EIS spectra exhibit one capacitive loop and
confirm BTAI’s inhibitive ability. The inhibition action of
BTAI is also evidenced by SEM images. They attributed the
action of the inhibitor to the ionization of BTAI in the acid
according to the following equation:
BTAI → [BTA]+ + I− (2)
Therefore, in aqueous acidic media, BTAI exists as the
organic part (BTA+) and the anion inorganic part (I−). Fur-
thermore, the steel surface can be charged positively in an
acid solution (Li et al., 2009a,b), so it is difficult for BTA+ to
adhere to the steel surface because of repulsion. However,
I− can be oxidized by oxygen dissolved in acidic media and
turns to the yellowish tri-iodide. The oxidization reactions
of iodide ions can be described as follows (Feng et al., 1999):
4I− + O2 + 4O2 → 2I2 + H2O (3)
I2 + I− → I3− (4)
6I − + O2 + 4H+ → 2I 3− + 2H2O (5)
The I−3 ions could accumulate slowly to the steel/
solution interface and be adsorbed, and the BTA+ may be
adsorbed through electrostatic interactions between the
positively charged molecules and the negatively charged
metal surface. In other words, there may be a synergism
between BTA+ and I−3.
Jianguo et  al. (1995) demonstrated that both poly­
vinylpyrrolidone and polyethylenimine are power-
ful for the inhibition of low-carbon steel over a wide
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 A.A. Khadom and S.N. Farhan: Corrosion inhibition of steel in phosphoric acid      3
concentration range of aqueous H3PO4 solutions. Both
polymers retard the anodic and cathodic corrosion reac-
tions with emphasis on the former. The outcomes for
uninhibited acid confirm the kinetic expression proposed
by Mathur and Vasudevan (1982).
Benabdellah et al. (2006) extracted artemisia oil (Ar)
from Artemisia herba alba, and it was confirmed as a
corrosion inhibitor of steel in 2 m phosphoric acid using
weight loss, electrochemical polarization, and EIS proce-
dures. The natural oil decreases the corrosion rate. The
inhibition efficiency was found to increase with oil con-
centration to approach 79% at 6 g/l. Artemisia oil behaves
as a cathodic inhibitor. The influence of temperature on
the corrosion mechanism of steel indicates that the inhi-
bition efficiency of the natural substance decreases with
the rise of temperature. The adsorption isotherm of the
natural product on the steel has been determined. They
proposed that the adsorption of heterocyclic compounds
happens when the aromatic rings are mostly perpendicu-
lar to the steel surface at a low concentration of inhibi-
tor, but at elevated inhibitor concentration, the molecules
are reoriented to the parallel mode, and this result agrees
with the work of Bockris and Yang (1991).
Dadgarinezhad and Baghaei (2009) studied the
effect of 2-phenyl-1-hydrazine carboxamide on the cor-
rosion of low-carbon steel in solutions of H3PO4. The
results obtained revealed that this compound is a good
mixed-type inhibitor. Increasing the acid concentra-
tion increased the metal corrosion but did not affect the
inhibitor efficiency. The optimum inhibitor concentra-
tion remained at 150  ppm for various concentrations of
phosphoric acid. The surface morphologies of specimens
after 1  h of immersion in various solutions were studied
by SEM. The Langmuir adsorption isotherm fitted well
with the experimental data. They also concluded that the
performance of the inhibitor is attributed to the presence
of electron donor groups (N, O, and the aromatic ring) in
the structure of 2-phenyl-1-hydrazine carboxamide, which
leads to the adsorption on the metal surface.
Ben Hmamou et  al. (2013) investigated the inhibi-
tion effect of alizarin red on the corrosion of carbon steel
in 2 m phosphoric acid solutions at 298 K by using EIS,
potentiodynamic polarization, and weight loss tech-
niques. A main decrease in the corrosion rate of steel was
noticed in the presence of the investigated alizarin red.
Potentiodynamic polarization plots exposed that this
inhibitor acted as a mixed-type inhibitor, affecting both
cathodic and anodic corrosion processes. The adsorp-
tion of the inhibitor on the metal surface was found to
follow the Langmuir adsorption isotherm. Thermody-
namic adsorption parameters of the examined inhibitor
were calculated from the linear formula of the Langmuir
adsorption isotherm.
Li et al. (2017) studied the inhibition effect of the cati-
onic surfactant of tetradecylpyridinium bromide (TDPB)
on the corrosion of steel in 7 m H3PO4 by weight loss and
potentiodynamic polarization methods and EIS and SEM.
Quantum chemical calculation was applied to clarify the
adsorption type of TDPB molecules on a steel surface. The
results show that TDPB acts as a good inhibitor, and its
maximum inhibition efficiency is higher than 90% even
at low concentrations. The adsorption of TDPB obeys the
Langmuir adsorption isotherm. Polarization curves indi-
cate that TDPB bromide acts as a mixed-type inhibitor in
acid. EIS studies show one capacitive loop, which indi-
cates that the corrosion reaction is controlled by charge
transfer process. They also classified TDPB as 1:1 electro-
lyte, and it ionized as [TDP]+ and [Br]−, which agrees with
the explanation of Li et al. (2011).
Wang et al. (2012) studied the corrosion inhibition by
a triazole derivative on low-carbon steel in H3PO4 solution
by weight loss and polarization methods. The experimen-
tal results state that the material has an important inhib-
iting effect on the corrosion of steel in phosphoric acid
solution. It also shows good corrosion inhibition at the
upper concentration level of phosphoric acid. Potentiody-
namic polarization results have shown that the compound
acts as a mixed-type inhibitor, hindering the anodic and
cathodic corrosion reactions with the largest effect on
the cathodic reaction. The values of inhibition efficiency
attained from weight loss and polarization measurements
are in good agreement. The adsorption of this material is
found to follow the Langmuir adsorption isotherm. Some
kinetic and thermodynamic parameters such as apparent
activation energy, frequency factor, and adsorption free
energy have been estimated and discussed. The inhibitor
efficiency decreases slightly with increasing H3PO4 con-
centration; this conclusion agrees with the results of Dad-
garinezhad and Baghaei (2009).
The inhibition effect of dimethylaminobenzylidene
acetone on low-carbon steel corrosion in 1 m H3PO4 solu-
tion was investigated by Saratha and Meenakshi (2011).
The data showed that dimethylaminobenzylidene acetone
was a steel corrosion inhibitor in H3PO4 solution, and the
maximum inhibition performance achieved was 94.9%
at the concentration of 0.04% (w/v) for the immersion
period of 12 h. Temperature studies were carried out, and
thermodynamic parameters such as change in enthalpy,
change in entropy, and change in free energy were evalu-
ated. Adsorption of dimethylaminobenzylidene acetone
on the steel surface in 1 m H3PO4 solution followed the
Temkin adsorption isotherm. EIS measurements showed
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4      A.A. Khadom and S.N. Farhan: Corrosion inhibition of steel in phosphoric acid
an increase in charge transfer resistance. The potentiody-
namic study showed it as a mixed type of inhibitor, con-
trolling both the anodic and cathodic reactions. Surface
analysis by Fourier transform infrared spectroscopy (FTIR)
and SEM confirmed the formation of protective coating on
the mild steel surface.
Belghiti et  al. (2016b) tested three hydrazine deriva-
tives, namely, 1,2-bis(pyrrol-2-ylidenemethyl)hydrazine
(HZ1), 1,2-bis(thiophen-2-ylidenemethyl)hydrazine (HZ2),
and 1,2-bis(furyl-2-ylidenmethyl)hydrazine (HZ3) as cor-
rosion inhibitors of mild steel in phosphoric acid using
experimental and theoretical methods. In the theoretical
part, quantum chemical calculations based on density
functional theory (DFT) and quantitative structure-activ-
ity relationship methods were done to determine the con-
nection between the molecular structure of hydrazines
and their inhibition efficiencies. The quantum chemical
parameters such as the localization of frontier molecular
orbitals, EHOMO, ELUMO, energy gap (∆E), dipole moment (μ),
hardness (ŋ), softness (S), the fractions of electrons trans-
mit (∆N), electrophilicity index (χ), and total energy charge
were calculated and used to clarify the electron transfer
mechanism between the inhibitor molecules and the steel
surface. Furthermore, statistical equations were proposed
using the multiple-linear and the nonlinear regression
analyses. In the experimental part (Belghiti et al., 2016a),
the inhibitory effects of three hydrazine derivatives were
studied using weight loss, electrochemical impedance
spectroscopy, and polarization techniques. It was found
that the inhibition efficiency of the compounds increases
with the increasing inhibitor concentration. The adsorp-
tion of inhibitors on the steel surface obeys the Langmuir
isotherm. The effect of temperature on the corrosion
behavior of mild steel in phosphoric acid solution in the
absence and presence of the inhibitors was also studied.
The inhibitor’s efficiency decreased with the rise in tem-
perature. Polarization curves showed that HZ1 and HZ3
behave as mixed-type corrosion inhibitors in phosphoric
acid solution. The inhibition efficiencies of the inhibitors
follows the order of HZ2 > HZ3 > HZ1. These results agree
with the research that the number of N-heterocyclic com-
pounds in the aromatic or long carbon chain system have
effective inhibitor performance (Dafali et  al., 2002). The
notable inhibitory influence is supported by the presence
of heteroatoms such as sulfur (S), oxygen (O), and nitro-
gen (N) in the ring that simplifies the adsorption on the
metal surface following the sequence of -S- > =N- > -O- >  acted as a mixed-type inhibitor.
(Dafali et al., 2003).
Zarrok et al. (2014) investigated the inhibition of cor-
rosion of carbon steel in phosphoric acid solution by the
use of l-cysteine methyl ester hydrochloride by weight
loss and electrochemical procedures. The performance
of inhibition was increased by increasing the concentra-
tion of the inhibitor and reduced by increasing the tem-
perature. Polarization data showed that l-cysteine methyl
ester hydrochloride behaves as a mixed-type inhibitor.
Electrochemical impedance spectroscopy showed that
dissolution of the steel occurs as a result of charge trans-
fer. Adsorption of the inhibitor obeyed the Langmuir
adsorption isotherm. Kinetic and thermodynamic data
were also estimated.
Sivaraju and Kannan (2010) studied the inhibition
effect of Acalypha indica L. alcoholic extract (AIAE) on
mild steel corrosion in 1 N H3PO4 by weight loss and polari-
zation methods in a temperature range of 303–333 K. The
inhibition efficiency increased with increase in the con-
centration of AIAE. The corrosion rate increased with
increase in temperature and decreased with increase in
the concentration of inhibitor compared with the inhibi-
tor-free solution. The adsorption of inhibitor on the mild
steel surface has been found to obey the Temkin adsorp-
tion isotherm. Potentiostatic polarization results revealed
that the extract acts as a mixed-type inhibitor. The values
of the activation energy (Ea), free energy of adsorption
(ΔGads), heat of adsorption (Qads), enthalpy of adsorption
(ΔH), and entropy of adsorption (ΔS) were calculated.
Surface analyses (FTIR and SEM) were also achieved to
establish the mechanism of corrosion inhibition on the
mild steel corrosion in H3PO4 solution.
Noyel et  al. (2015) investigated the adsorption and
corrosion inhibition property of the alcoholic Psidium
guajava (guava) leaf extract on mild steel in 1 m H3PO4
solution medium by mass loss, potentiodynamic polariza-
tion, and electrochemical impedance spectroscopy tech-
niques. The studies showed that the inhibition efficiency
increases with inhibitor concentration up to 800 ppm and
decreases slightly at 1200 ppm. A minor fall in the inhibi-
tor performance at 1200  ppm concentration may be due
to the desorption of the inhibitor molecules into the bulk
on approaching the critical concentration. Desorption
declines the metal-inhibitor interaction resulting in a drop
in inhibition efficiency. The adsorption obeys both the
Langmuir and Temkin adsorption isotherm formulas. The
kinetic and thermodynamic parameters were estimated.
The adsorption was found to follow a comprehensive-
type adsorption dominated by chemisorption. Potentio-
dynamic polarization studies showed that the inhibitor
Balanaga Karthik (2011) tested the influence of allyl
methyl sulfide on the corrosion of mild steel in a H3PO4
solution by the weight loss method in relation to the con-
centration of the inhibitor, acid, and temperature. At room
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 A.A. Khadom and S.N. Farhan: Corrosion inhibition of steel in phosphoric acid      5
temperature, the efficiency of the inhibition increases with
the increase in the concentration of allyl methyl sulfide
for mild steel. The corrosion rate is at a maximum for an
uninhibited solution as compared with that of the inhib-
ited solution at all temperatures. The corrosion rate is
increasing with the increase of temperature. For 1 × 10−2 m
of allyl methyl sulfide concentration, the percentage effi-
ciency decreases with temperature increase because of
decreasing adsorption with increase in temperature. Low
heat of adsorption indicates the physical adsorption. By
increasing the temperature, the free energy change values
decrease; this may be ascribed to the increase in tempera-
ture favoring the corrosion process. As the concentration of
the inhibitor decreases, the free energy change increases.
This shows that with the decrease in the concentration of
allyl methyl sulfide, the corrosion process becomes more
and easier.
Arab and Al-Turkustani (2006) investigated the corro-
sion inhibition of low-carbon steel in 0.67 m phosphoric
acid by phenacyl dimethylsulfonium bromide and six of
its p-substituted derivatives using different chemical, elec-
trochemical, and SEM methods. The order of increasing
inhibition efficiency was correlated with its p-substitution
through the Hammett relation. Potentiodynamic polariza-
tion curves indicated that the compounds acted primar-
ily as mixed-type inhibitors. Electrochemical impedance
spectroscopy showed that the steel dissolution is organ-
ized by a charge-transfer mechanism. The kinetic-ther-
modynamic model of adsorption isotherm described the
experimental findings. The number of active sites, binding
constant, and change of free energy were computed for all
the studied compounds. Depending on the inhibitor, it
was found that each organic molecule substituted one or
two adsorbed water molecules from the steel surface. The
adsorption center was suggested to be the π electrons of
the phenyl ring, and a flat configuration adsorption of the
molecule may occur.
Wang et  al. (2000) used mass loss and polarization
techniques to show that 2-mercaptobenzoxazole is effec-
tive for the inhibition of low-carbon steel over a wide con-
centration range of aqueous H3PO4 solutions. The inhibitor
hinders the anodic and cathodic corrosion reaction with an
emphasis on the former. Results for uninhibited acid solu-
tion confirm the kinetic expression proposed by Mathur.
The corrosion behavior of steel alloy in phosphoric
acid was investigated by various electrochemical methods.
The action of propargyl alcohol as an inhibitor was also
studied over a wide range of acid concentrations and solu-
tion temperatures (Morad, 1999). The results obtained
from both polarization curves and EIS proved that pro-
pargyl alcohol greatly inhibits the hydrogen evolution
reaction on mild steel in phosphoric acid solutions at
temperatures ≥40°C and inhibition occurs by adsorp-
tion of propargyl alcohol molecules. The most favorable
adsorption style is one in which the carbon atoms forming
the triple bond interact with the iron atoms. Inhibition
of the cathodic reaction proposes that adsorption of the
inhibitor is most favorable at a surface partially covered
by hydrogen. A similar mode of inhibition by propargyl
alcohol was suggested by Bartos et al. (1993), Kuteja et al.
(1995), and Bockris and Yang (1991). The results of this
work present no indications of the formation of a polymer
film of propargyl alcohol on the metal surface in the pres-
ence of propargyl alcohol.
Noor (2005) determined the corrosion rates of steel
in concentrated phosphoric acid (1.0–11.0 m) by the mass
loss technique, at three temperatures 298, 308, and 323 K.
The corrosion rate increases with both acid concentra-
tion and temperature. The activation energies, enthalpies,
and entropies of the dissolution process were determined.
The effect of some quaternary N-heterocyclic compounds
as corrosion inhibitors was evaluated. Results obtained
showed that these compounds are good mixed-type inhib-
itors without changing the mechanism of the corrosion
reaction. General, at constant acid concentration, inhibi-
tor performance increased with the concentration of the
inhibitor. On the other hand, at constant inhibitor concen-
tration, inhibitor efficiency decreased with the concentra-
tion of the acid up to a critical concentration above which
it started to increase. The studied compounds seemed to
function through general adsorption following the ther-
modynamic-kinetic adsorption isotherm.
Messali et al. (2017) studied the effect of guar gum as
a water-soluble, green, biodegradable, and biocompat-
ible inhibitor for the corrosion inhibition of carbon steel
in 2 m H3PO4 solution. The characteristic effect of guar
gum on the steel corrosion was studied at concentration
ranges from 0.1 to 1.0 g/l at 298 to 328 K by weight loss and
electrochemical methods. The results showed that the
inhibition efficiency of guar gum decreased slightly when
the temperature increased and increased by increas-
ing the inhibitor concentration reaching the maximum
value at 1.0 g/l. The adsorption of guar gum on the metal
surface obeyed the Temkin adsorption isotherm. EIS
measurements indicate that the values of the polarization
resistance of carbon steel in the presence of guar gum are
significantly higher than that of the untreated surface. A
steel surface coated with guar gum was analyzed by SEM,
FTIR, and X-ray diffraction. The quantum calculations
using the DFT method and molecular dynamic simula-
tions were achieved to define the relationship between
the inhibition performance of the investigated compound
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6      A.A. Khadom and S.N. Farhan: Corrosion inhibition of steel in phosphoric acid
and their molecular structure. The performance of guar
gum is due to the adsorption on the metal surface that
depends largely on the molecular structure of the tested
inhibitor, which contains reactive sites such as oxygen
atoms and -OH groups. Furthermore, the steel corrosion
in acidic medium mainly contains two simultaneous elec-
trochemical reactions (anodic and cathodic reactions).
From the observations reported in the electrochemical,
theoretical, and surface analysis results, it can be deter-
mined that the guar gum is possibly adsorbed on the
anodic sites of the metal surface by chelate formation
with Fe2+ present on those sites involving an endocyclic
“O” atom of the mannose unit together with the oxygen
atom of the same monosaccharide unit. The -OH groups
are mainly responsible for adsorption of tested guar on
the cathodic sites of the steel surface.
The summary of the above literature review is shown
in Table  1. It is seen that the inhibition performance of
sulfur-containing compounds is greater than that of nitro-
gen-containing compounds. This may be attributed to the
presence of two electron pairs available for organization.
Furthermore, iron is well known for its coordination affin-
ity to ligands possessing a heteroatom. An increase in
inhibition performance with an increase in inhibitor con-
centration shows that the inhibition action is due to the
adsorption on the steel surface, and this agrees with the
conclusion of Ebenso et al. (1999).
3 C
 orrosion inhibition via inorganic
inhibitors
Inorganic inhibitors can be categorized as anodic and
cathodic inhibitors. Anodic inhibitors (also called pas-
sivation inhibitors) act by reducing the anodic reaction
that blocks the anode reaction and supports the natural
formation of a passivation metal surface, also due to the
formation of a layer adsorbed on the metal surface. In
general, the inhibitors react with the corrosion product,
initially formed, resulting in a solid and insoluble layer
on the steel surface. Cathodic corrosion inhibitors inhibit
the cathodic reaction of the metal from happening. These
inhibitors have metal ions able to produce a cathodic reac-
tion due to alkalinity, thus producing insoluble products
that precipitate selectively on cathodic sites. A compact
and adherent layer deposits over the metal, restricting
the diffusion of reducible species at these sites and thus
increasing the impedance of the surface and the diffusion
restriction of the reducible species, that is, the oxygen
diffusion and electrons conductive in these areas. These
anticorrosion chemicals cause high cathodic inhibition
(Roberge, 1999; Talbot & Talbot, 2000).
Alaoui et al. (2008) studied the influence of phosphate
of aluminum on the corrosion inhibition of low-carbon
steel in H3PO4 solution using the mass loss and electro-
chemical methods. The inhibition efficiency of inhibi-
tor increases with concentration to attain 84% at 10−2 m
of phosphate of aluminum in 0.33 m H3PO4. Polarization
studies proved that phosphate of aluminum is a mixed-
type inhibitor and acts both on the cathodic and anodic
reactions without changing the mechanism of the hydro-
gen evolution reaction. The inhibition efficiency of phos-
phate of aluminum is temperature-dependent. Phosphate
of aluminum adsorbs on the steel surface according to the
Langmuir adsorption isotherm via physical adsorption.
Khadom (2012) evaluated the corrosion of mild steel
in H3PO4 at different temperatures in the absence and
presence of potassium iodide (KI) as a corrosion inhibitor.
Mass loss and polarization methods were used to estimate
the corrosion rate data. Two mathematical models were
suggested to represent the corrosion rate data. Polynomial
and exponential models were used. A computer program
was used to estimate the constants of these models. Both
models successfully represented the corrosion rate data
with high correlation coefficients.
Khadom and Yaro (2011) studied the corrosion of
low-carbon steel in 2.5 m H3PO4 at a temperature range of
30–60°C in the presence and absence of potassium iodide
as an inorganic inhibitor in the range of 0.02–0.05 m at
static conditions. Mass loss and polarization techniques
were employed in this investigation. The maximum value
of inhibitor efficiency obtained was 99.95% at 50°C in the
presence of 0.05 m inhibitor concentration. The fraction
of surface covered calculated from corrosion rates obeyed
the Langmuir adsorption isotherm. Polarization experi-
ments showed that for a given temperature, the curves
were shifted toward the potential axis, leading to lower
corrosion rates as the inhibitor concentration increased.
Potassium iodide inhibits carbon steel corrosion in phos-
phoric acid by altering both anodic and cathodic partial
reactions with the anodic reaction being more prevailing.
Yaro and Khadom (2010) discussed the nonlinear
region of the polarization curve near the corrosion poten-
tial, depending on potential data as a function of current
densities. These data were analyzed by suggesting a math-
ematical model, taking into account the effect of mass
transfer on the activation process. This model was used
to evaluate the values of polarization resistance in the
presence and absence of potassium iodide as a corrosion
inhibitor of mild steel in H3PO4 at different temperatures.
The values of polarization resistance obtained by the
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Table 1: Summary of organic corrosion inhibitor for steel in phosphoric acid in terms of steel type, acid concentration (C), inhibitor type,
temperature range (T), adsorption isotherm, and maximum efficiency (IE).

Steel type   C   Inhibitor   T (°C)  Adsorption type/isotherm   IE (%)   References

Aged maraging   0.67 m   4-(N,N-Diethylamino)   30–50  Predominantly physical   92.17   Poornima

steel (0.015 wt% C) benzaldehyde thiosemicarbazone adsorption/Langmuir et al.
(2011)

Mild steel   1m   Plant extract/apricot juice   30–60  Physical adsorption/   75   Yaro et al.
(0.199 wt% C) Langmuir (2013)
Cold rolled steel   7m   Benzyltrimethylammonium iodide   20–50  Comprehensive   98   Li et al.
(0.07 wt% C) adsorption/Langmuir (2011)

1010 grade low-   1–9 m   Polyvinylpyrrolidone   30–70  Physical adsorption/   89   Jianguo

carbon steel Langmuir 90 et al.
(1995)

and polyethylenimine

Steel (0.21 wt% C)   2 m   Plant extract/artemisia oil   25–75  Physical adsorption/   79   Benab­

Langmuir dellah
et al.
(2006)

Mild steel   1–3 m   2-Phenyl-1-hydrazine   25  Langmuir   98.9   Dadgar­

(0.05 wt% C) carboxamide inezhad
and
Baghaei
(2009)
Carbon steel   2m   Alizarin red   25  Comprehensive   93.6   Ben
(0.37 wt% C) adsorption/Langmuir Hmamou
et al.
(2013)

Cold rolled steel   7m   Tetradecylpyridinium bromide   20–50  Comprehensive   92.2   Li et al.

(0.07 wt% C) adsorption/Langmuir (2017)

Mild steel   2, 7, 9 mole/dm3   3-Phenyl-4-amino-5-mercapto-   30  Predominantly chemical   97   Wang et al.

(0.05 wt% C) 1,2,4-triazole adsorption/Langmuir (2012)

Mild steel   1m   Dimethylaminobenzylidene   30–70  Predominantly chemical   90   Saratha

(0.039 wt% C) adsorption/Temkin and
Meena­kshi
(2011)

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Table 1 (continued)

Steel type   C   Inhibitor   T (°C)  Adsorption type/isotherm   IE (%)   References

Mild steel   2m   Hydrazine derivatives   35  Comprehensive   88.14   Belghiti

(0.21 wt% C) adsorption/Langmuir (HZ1) et al.
89.42 (2016a, b)
(HZ2) 88.5
(HZ3)

Carbon steel   2m   l-Cysteine methyl ester   35–55  Physical adsorption/   93.5   Zarrok
(0.37 wt% C) hydrochloride Langmuir et al.
(2014)

Mild steel   1 N   Plant extract/Acalypha indica L.   30–60  Physical adsorption/   90.38   Sivaraju
(0.017 wt% C) Temkin and Kannan
(2010)
Mild steel (0.2 wt%   1 m   Plant extract/Psidium guajava   30–80  Comprehensive   89   Noyel et al.
C) (guava) adsorption/Langmuir and (2015)
Temkin
Mild steel   1m   Allyl methyl sulfide   30–65  Physical adsorption/   96.87   Balanaga
(0.07 wt% C) Langmuir Karthik
(2011)

Mild steel   0.67 m   Phenacyl dimethyl sulfonium   30  Physical adsorption/   66.39 (A)   Arab and
(0.17 wt% C) bromide (A) kinetic-thermodynamic 84.71 (B) Al-Turkus­
69.41 (C) tani (2006)
74.96 (D)
79.83 (E)
67.90 (F)
    4-Methylphenacyl dimethyl        
sulfonium bromide (B)

    4-Chlorophenacyl dimethyl        
sulfonium bromide (C)

    4-Bromophenacyl dimethyl        
sulfonium bromide (D)

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 A.A. Khadom and S.N. Farhan: Corrosion inhibition of steel in phosphoric acid      9

Table 1 (continued)

Steel type   C   Inhibitor   T (°C)  Adsorption type/isotherm   IE (%)   References

    4-Nitrophenacyl dimethyl        
sulfonium bromide (E)

    4-Methoxyphenacyl dimethyl        
sulfonium bromide (F)

1010 grade low-   3m   2-Mercaptobenzoxazole   30  N/A   94   Wang et al.

carbon steel (2000)
Mild steel   1–9 m   Propargyl alcohol   35–50  N/A   97.2   Morad
(1999)
Mild steel   2m   N-Heterocyclic compounds:   30–70  Physical adsorption/   96.49 (I)   Noor
(0.21 wt% C) Langmuir 95.91 (II) (2005)
99.95 (III)
           

           

           

Carbon steel   2m   Plant extract/guar gum   25–55  Comprehensive   95.8   Messali

(0.37 wt% C) adsorption/Temkin et al.
(2017)

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10      A.A. Khadom and S.N. Farhan: Corrosion inhibition of steel in phosphoric acid
Table 2: Summary of inorganic corrosion inhibitor for steel in phosphoric acid in terms of steel type, acid concentration (C), inhibitor type,
temperature range (T), adsorption isotherm, and maximum efficiency (IE).
Steel type   C (m)  Inhibitor  
Mild steel (0.05 wt% C)   0.33  Phosphate of  
aluminum, AlPO4
Carbon steel (0.041 wt% C)  2.5  Potassium iodide, KI  30–60  N/A (mathematical modeling)   98  Khadom (2012)
Carbon steel (0.041 wt% C)  2.5  Potassium iodide, KI  30–60  Chemical/Langmuir
Carbon steel (0.041 wt% C)  2.5  Potassium iodide, KI  30–60  N/A (electrochemical modeling)  99  Yaro and Khadom (2010)
mathematical model were compared with those obtained
by Tafel parameters. The maximum value of polarization
resistance was 5049.13 Ω cm2 at 30°C in the presence of
0.05 m KI, while the minimum value was 1.885 Ω cm2 at
60°C in the absence of KI. These results indicate that the
polarization resistance values increased with the increase
of KI concentration and decreased with the increase of
temperature. The summary of inorganic corrosion inhibi-
tor for steel in phosphoric acid was shown in Table 2.
4 Corrosion inhibition via
­synergistic effect inhibitors
Promotion of the inhibition effect of organic inhibitors
is another important criteria, as most of these inhibitors
are very definite in their action and the corrosion process
is complicated. Extensive studies have thus been under-
taken to identify the synergistic effects with other additives
(Onuchukwu & Lori, 1984; Zucchi et  al., 1994; Aramaki,
2002; Jabeera et  al., 2006). Synergism is described as a
joint action of compounds with greater in total effect than
the sum of the individual effects. For corrosion inhibitor
systems, synergism usually arises either as a consequence
of the interaction between components of the inhibitor
formulation or due to the interaction between the inhibi-
tor and one of the ions present in the aqueous media. The
synergistic effect can be explained according to syner-
gistic parameter, Sθ, obtained from the surface coverage
values (θ) of the anion, cation, and both. Khadom (2015)
calculated the synergism parameter, Sθ, using the follow-
ing equation:
1 − θ 1+ 2
Sθ =
1 − θ*1+2 (6)
where θ1+2 = (θ1 + θ2)  −  (θ1θ2), θ1 is the surface coverage by
anion, θ2 is the surface coverage by cation, and θ*1+2 is
the measured surface coverage by both the anion and the
cation. If Sθ approaches 1, no interaction between inhibi-
tors exists, while S > 1 refers to a synergistic effect. While
T (°C)  Adsorption type/isotherm   IE (%)  References
25–65  Physical/Langmuir   85  Alaoui et al. (2008)
  99.95  Khadom and Yaro (2011)
if S < 1, the antagonistic interaction prevails, which may be
attributed to competitive adsorption (Khadom, 2015). In
competitive adsorption, the anion and cation are adsorbed
at different sites on the metal surface, while in cooperative
adsorption; the anion is adsorbed on the metal surface and
followed by the adsorption of the cation on a layer of anion.
The effects of single o-phenanthroline and the mixture
of various concentrations of NaCl and 0.0002 m o-phen-
anthroline on the corrosion of steel in H3PO4 were inves-
tigated by Guan et  al. (2004). The research showed that
steel in phosphoric acid was more efficiently inhibited
by o-phenanthroline in the presence of NaCl than single
o-phenanthroline, and inhibition efficiency increases
with increasing concentration of NaCl in the presence of
0.0002 m o-phenanthroline. At a higher concentration of
NaCl, there is the synergistic influence between o-phen-
anthroline and NaCl. The adsorption of inhibitor follows
the Langmuir adsorption isotherm. Polarization results
showed that the inhibitor mainly acts as a mixed-type
inhibitor for steel in 1.0 m H3PO4. The results obtained
from weight loss and polarization methods are in good
agreement. They attributed the synergistic effect to the
smaller degree of hydration of chloride ions, and it can
bring excess negative charges in the area of the interface
due to the adsorption, then positively charged ions may
adsorb onto the metal surface. o-Phenanthroline may be
protonated in the acid solution as follows:
o-phenanthroline + xH ↔ [o-phenanthroline ⋅ Hx ] (7)
+ x+
Subsequently, the steel surface contains posi-
tive charges in the acid solution, and the results can be
described on the assumption that in the presence of Cl−, the
negatively charged Cl− would align to the positively charged
surface. Then, near the interface, the concentrations of Cl−
and protonated o-phenanthroline are much higher than
those in the bulk solution. The protonated o-phenanthro-
line do not attach directly to the positively charged steel
surface because of the repulsive interaction between the
protonated o-phenanthroline and the positively charged
steel surface. The protonated o-phenanthroline, however,
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 A.A. Khadom and S.N. Farhan: Corrosion inhibition of steel in phosphoric acid      11
can attach to the steel surface by means of electrostatic
interaction between Cl− and protonated o-phenanthroline.
Qu et al. (2008) investigated the corrosion inhibition
of cold rolled steel in 0.1 m aerated H3PO4 in the presence
of dodecylamine (DDA) and potassium iodide (KI) by
the Tafel polarization curve and EIS at 20°C. The results
achieved from the polarization curve show that the inhibi-
tion efficiency of DDA with and without KI increases with
the increase in concentration of DDA, but the inhibition
efficiency of DDA without KI is lower. A synergistic effect
exists when DDA and KI are combined together to avoid
steel corrosion in 0.1 m H3PO4. All impedance spectra in
EIS tests exhibit one capacitive loop that indicates that
the corrosion reaction is controlled by a charge-transfer
process. Inhibition efficiencies obtained from Tafel polari-
zation and transfer resistance (Rt) are reliable. Clearly,
dodecylamine is a nitrogen-containing organic com-
pound, which contains unshared electron pair and p elec-
trons. Therefore, dodecylamine can be absorbed onto the
surface of metal through the transference of lone-pair elec-
trons of nitrogen atoms to the d orbital in the iron atom,
but in acid solution, dodecylamine may be protonated,
leading to positive charge in the molecule as follows:
C12H25NH2 + H+ → [C12H25NH3 ] (8)
The steel surface contains a positive charge in an
acid solution; thus, it is difficult for the positively charged
dodecylamine to reach the positively charged steel surface
because of repulsion forces, and for this reason, the single
dodecylamine cannot act as excellent inhibitor for steel
corrosion in 0.1 m H3PO4 solution without KI. The added
Table 3: Summary of synergistic effect corrosion inhibitor for steel in phosphoric acid in terms of steel type, acid concentration (C), inhibi-
tor type, temperature range (T), adsorption isotherm, and maximum efficiency (IE).
Steel type   C (m)  Inhibitor
Cold rolled steel   1  o-Phenanthroline + sodium chloride
(0.1 wt% C)
Cold rolled steel   0.1  Dodecylamine + potassium iodide
(0.1 wt% C)
Cold rolled steel   1–4  Cetyltrimethylammonium bromide + sodium chloride
(0.1 wt% C)
Cold rolled steel   1–10  Red tetrazolium + uracil
(0.07 wt% C)
KI can facilitate the adsorption process of dodecylamine
and hence improve its performance. This explanation is in
agreement with the previous discussion (Guan et al., 2004).
Li et al. (2008) studied the effect of chloride ions on
the inhibitive performance of cetyltrimethylammonium
bromide in 1–4 m of phosphoric acid for steel using weight
loss and polarization techniques. The influence of acid
concentration on corrosion inhibition has been exam-
ined. The results reveal that a synergistic effect has been
observed for cetyltrimethylammonium bromide with NaCl
at each acid concentration. In 1 m phosphoric acid, the
polarization curves show that the inhibitor-NaCl blend is
a mixed-type inhibitor. The explanation of cetyltrimethyl-
ammonium bromide-NaCl action was in good agreement
with the works of Guan et al. (2004) and Qu et al. (2008).
Li et al. (2009b) investigated the synergistic inhibition
effect of red tetrazolium and uracil on the corrosion of cold
rolled steel (CRS) in 1.0–10.0 m H3PO4 solution by weight
loss and potentiodynamic polarization methods. Atomic
force microscopy provided the CRS surface conditions. The
results showed that red tetrazolium had a moderate inhibi-
tive effect, and the adsorption of red tetrazolium followed
the Freundlich adsorption isotherm. Polarization curves
proved that red tetrazolium was a mixed-type inhibitor in
phosphoric acid. For uracil, it had a weak inhibition effect
and acted as a cathodic inhibitor. However, a combina-
tion of red tetrazolium with uracil significantly improved
the inhibition performance. The inhibition efficiency (IE)
for red tetrazolium in combination with uracil was higher
than the summation of IE for a single red tetrazolium and a
single uracil, which was synergistic in nature. Polarization
  T (°C)  Adsorption   IE (%)  References
type/isotherm
  30–45  Chemical/   97.3  Guan et al. (2004)
Langmuir
  20  N/A   98.4  Qu et al. (2008)
  40  N/A   <90  Li et al. (2008)
  20–50  Physical/   98.8  Li et al. (2009b)
Freundlich
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12      A.A. Khadom and S.N. Farhan: Corrosion inhibition of steel in phosphoric acid
studies revealed that the red tetrazolium/uracil mixture
acted as a mixed-type inhibitor, which extremely inhibited
both anodic and cathodic reactions. The synergistic inhi-
bition effect of red tetrazolium and uracil could also be
evidenced by atomic force microscopy images. Depending
on the results, the synergism mechanism was discussed
from the viewpoint of co-adsorption. The combination of
red tetrazolium and uracil significantly improved inhibi-
tion efficiency, and all the values of synergism parameter
(Sθ) are higher than unity, which specifies that there is a
real synergistic effect of red tetrazolium and uracil in phos-
phoric acid. A positively charged steel surface in acidic
media was also stated. When red tetrazolium was mixed
with uracil in phosphoric acid, Cl− (the anion part of red
tetrazolium) may first adsorb on the positively charged
steel surface by electrostatic attraction. Then the proto-
nated red tetrazolium and uracil could easily approach the
steel surface, followed by transference of electrons from
nitrogen heteroatoms and oxygen atoms to the d orbital of
the iron atom (chemical adsorption) at the steel/solution
interface. The summary of synergistic effect of corrosion
inhibitor for steel in phosphoric acid was shown in Table 3.
5 Conclusion
Phosphoric acid is one of the most important mineral
acids. Corrosion control using inhibitors is a powerful way
to protect steel and its alloys in different environments of
phosphoric acid. Literature on the effects of organic and
inorganic inhibitors and synergistic effect of some compo-
nents was reviewed, and the following conclusions were
obtained:
1. Corrosion of steel in phosphoric acid increased with
temperature and acid concentration and decreased
with inhibitor concentration.
2. Phosphoric acid concentration has no significant
effect on inhibitor performance.
3. Organic inhibitors are widely used in different concen-
trations of phosphoric acid, and these inhibitors can be
adsorbed physically, chemically, or comprehensively
on steel surfaces, forming a barrier to the corrosive
environment. Physical adsorption was more applied.
4. Generally, the adsorption follows the Langmuir
adsorption isotherm, suggesting a formation of a
monolayer on the metal surface.
5. Plant extracts were also used as clean, green, cheap,
and environmentally friendly corrosion inhibitors.
6. Inorganic inhibitors are used to a lesser extent. Potas-
sium iodide was one of the most efficient corrosion
inhibitor with maximum inhibitor efficiency approach-
ing 99.8%.
7. The synergistic effect between organic corrosion
inhibitors and other components improved the inhibi-
tor performance.
8. In general, the efficiency of inhibitors increased with
inhibitor concentration and decreased with a rise in
temperature.
Acknowledgments: Special thanks go to Prof. Dr. Aprael S.
Yaro for his continuous support and encouragement.
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