Accepted Manuscript

Organic corrosion inhibitors for industrial cleaning of ferrous and

non-ferrous metals in acidic solutions: A review

Madhusudan Goyal, Sudershan Kumar, Indra Bahadur,

Chandrabhan Verma, Eno E. Ebenso

PII: S0167-7322(17)34213-7
DOI: https://doi.org/10.1016/j.molliq.2018.02.045
Reference: MOLLIQ 8687
To appear in: Journal of Molecular Liquids
Received date: 9 September 2017
Revised date: 25 November 2017
Accepted date: 10 February 2018

Please cite this article as: Madhusudan Goyal, Sudershan Kumar, Indra Bahadur,
Chandrabhan Verma, Eno E. Ebenso , Organic corrosion inhibitors for industrial cleaning
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 ACCEPTED MANUSCRIPT

Organic corrosion inhibitors for industrial cleaning of ferrous and non-

ferrous metals in acidic solutions: a review

Madhusudan Goyala, Sudershan Kumarb,* Indra Bahadurc,d,* Chandrabhan Vermac,d, Eno E.

Ebenso c,d,

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a
Department of Chemistry, University of Delhi, Delhi-110007

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b
Department of Chemistry, Hindu College, University of Delhi, Delhi-110007

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c
Department of Chemistry, School of Chemical and Physical Sciences, Faculty of Natural and
Agricultural Sciences, North-West University, Private BagX2046, Mmabatho 2735, South Africa

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d
Material Science Innovation &Modelling (MaSIM) Research Focus Area, Faculty of Natural
and Agricultural Sciences, North-West University, Private Bag X2046, Mmabatho 2735, South
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Africa
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*Corresponding authors; E-mails: [email protected] (Sudershan Kumar)

Tel: +91- 9717952342 (S. Kumar); [email protected] (I. Bahadur); Tel: +27 183892870;
Fax: +27183892052.

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ABSTRACT
Acidic media have been employed extensively in industry particularly during cleaning
processes including industrial acid cleaning, acid pickling and acid-descaling. Hydrochloric,
sulfuric, nitric, phosphoric and acetic acids are a few of the common aggressive solutions that are
used for cleaning purposes. Several types of inhibitors are being employed for inhibition of
metallic dissolution in acidic media in which use of organic inhibitors is one of the most frequent

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and economic methods. The presence of heteroatoms (O, S, N, and P) and π-electrons in the form

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of conjugation are among the most salient features of the organic inhibitors. These parts of the
heteroatom containing molecules act as excellent inhibitors for metals and alloys corrosion in

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aggressive acidic solutions. This review article describes some recent major works in the field of
metallic corrosion monitoring using organic inhibitors in acidic media. A literature investigation

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revealed that heteroatoms of these molecules exist in the form of polar functional groups which
can actively participate in adsorption processes, in addition to the π-electrons of multiple bonds.
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Keywords: Acid solutions, Corrosion inhibitors, Acid inhibition, Adsorption, Langmuir adsorption
isotherm.
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1. Introduction
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1.1. General introduction about corrosion

Corrosion is a spontaneous process of metallic materials dissolution that results into huge
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economic and safety losses [1-3]. The corrosion can initiates by natural or manmade activities. In
the last few years, inhibition of metallic corrosion during several industrial processes like acid
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pickling and acid descaling has attracted substantial courtesy [1-3]. Among the available methods,
the use of synthetic corrosion inhibitors is the most popular and effective method due to their
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association with cost effective synthesis, high effective ness and ease of application [1, 3-5]. The
effectiveness of these organic inhibitors is based on the fact that generally they contain several
heteroatoms in the form of polar functional groups such –OH, -NO2, -OCH3, -COOH, -NH2, -
COOC2H5, -CONH2 etc. and non-bonding and π-electrons in the form of extensive conjugation [3-
8]. The polar functional groups, non-bonding and π-electrons act as adsorption centers during
metal-inhibitor interactions. The adsorption inhibitor films insulate the metallic materials from the
corrosive surroundings and protect them from dissolution. The organic inhibitors may adsorb on
the metallic surface, either by the interaction of appositively charged inhibitor and metallic surface

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through electrostatic force of interactions (physisorption) or by sharing of non-bonding and π-

electrons between the inhibitor and metallic d-orbital (chemisorption) or by an association of both
physisorption and chemisorption [2-10]. Literature survey reveals that in most of the metal-
inhibitor interactions, adsorption of the inhibitors first occurs by physisorption mechanism
followed by chemisorption mechanism.
1.2. Factors affecting corrosion
The corrosion inhibition property of inhibitors depends upon numerous factors such as the

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nature of the corrosive surrounding, solution temperature, electronic structure of inhibitors, etc.

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Generally, an inhibitor with electron releasing group such as methoxy (-OCH3), hydroxyl (-OH),

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amino (-NH2) etc. groups with planar geometry showed better inhibition efficiency as compared
to the inhibitor having electron withdrawing groups such as nitro (-NO2), cyano (-CN), ester (-

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COOC2H5) etc. groups and non-planer geometry. The effect of substituents on the corrosion
inhibition efficiency of the organic corrosion inhibitors can be explained with the value of
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Hammett sigma constant or simply Hammett constant (σ) [11,12]. A negative value of σ (eg. σ =
-0.17 for p-CH3) is consistent with electron releasing nature of the substitute while a positive value
(eg. σ = 0.78 for p-NO2) is related to an electrons withdrawing effect of the substituents [11, 12].
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The inhibition performance of most of the inhibitors increases with increasing concentration,
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however, after a certain limit which is called the optimum concentration, further increase in
concentration does not influence the inhibition characteristics of the concerned inhibitor molecule.
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Initially, the surface coverage of metallic surface and thereby inhibition efficiency increases with
concentrations and inhibitor molecules tend to adsorb by horizontal or flat orientations, but after
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optimum concentration further increase in concentration causes intermolecular force of repulsion

which results into vertical or non-planer adsorption of the inhibitor molecules [13]. Therefore, it
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can be concluded that below optimum concentration inhibitor tend to adsorb by horizontal
orientations while above optimum concentration they tend to adsorb by vertical orientation. The
temperature has very marked effect on the inhibition characteristics of inhibitor molecules. Similar
to most chemical reaction rates, corrosion rate also increases linearly with increasing surrounding
temperature [13, 14]. Presence of humidity, organic and inorganic salts and impurities increases
the corrosion rate due to increase in the charge conductivity of the electrolyte [15, 16]. Along with
all these environmental factors, the rate of metallic corrosion is also influenced by the nature of
corrosion products collected on the surface [17-19]. In flowing condition, these (rusts and scales)

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corrosion products accumulated on the surface are continuously removed from the surface which
results in exposure of newer surface to electrolyte for corrosion. However, in static condition, their
corrosion behavior can be best determined by Pilling–Bedworth ratio. Generally, Pilling –
Bedworth ratio is presented as Md/ nmD [17-19]. In this formula, D and M represent the density
and molecular weight of the corrosion product, M and D are the atomic mass and density of the
metal under consideration, while, n denotes the number of metallic atoms in the molecular formula
of corrosion product, for example in the molecular formula of corrosion products Fe3O4, Al2O3

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and Fe2O3 n are equal to 3, 2 and 2, respectively [17-19]. The cases Md/nmD < 1 and Md/nmD >1

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represent the non-protective and protective nature of the corrosion product, respectively.

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1.3. Introduction about types of corrosion Inhibitors

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Corrosion is an expensive and dangerous process and therefore its control is highly
anticipated. Several methods are being employed to control this unwanted process. Alloying and
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de-alloying, organic and inorganic coating and electrochemical plating are some common
corrosion protection measures beside the use of corrosion inhibitors. The inhibitor may be of
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anodic or passivating type that generally precipitates on the anodic region through the formation
of surface oxide layers. The inhibitors can be further divided into oxidizing anions type that can
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forms surface oxide layers in the absence of atmospheric oxygen. Chromate, nitrite and nitrate are
some common oxidizing types of passivating inhibitors. On the other hands, anodic inhibitors may
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be of non-oxidizing anions type that can passivate metallic surface only in the presence of
atmospheric oxygen. Molybdate, tungstate and phosphate are some common examples of non-
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oxidizing anodic inhibitors. The cathodic inhibitors generally precipitate at the cathodic sites and/
or slow down the rate of cathodic hydrogen evolution reaction and thereby ultimately retard the
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corrosive dissolution [20, 21]. They can be further classified as oxygen scavengers, cathodic
precipitates and cathodic poisons types. In general, arsenic and antimony make the association of
hydrogen atoms during cathodic hydrogen evolution and therefore behaved as cathodic poisons.
The magnesium, calcium and zinc in form of their oxides precipitate on cathodic sites and behave
as barrier between metal and electrolytes and thereby act as cathodic precipitates. Further,
hydrazine and sodium sulfite can associate with surrounding oxygen molecules and thereby
perform as oxygen scavengers [22-28]. As per the literature reports organic corrosion inhibitors
are most extensively utilized owing to their ease and facile synthesis, high protection ability, ease

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to apply in the corrosive media. Several forms of organic corrosion inhibitors such as drugs as
inhibitors, plant extract as inhibitors, polymeric compounds as inhibitors etc. have been developed
and being utilized. Literature study revealed that various review papers have been published
addressing the various aspects of corrosion. Some common review articles includes, effect of
organic compounds as corrosion inhibitors [26-28], alternatives to chromate based corrosion
inhibitors and green corrosion inhibitors [29-32], natural products and plants extracts as corrosion
inhibitors [33-35], drugs as corrosion inhibitors [36,37], Molybdates and lanthanides as corrosion

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inhibitors [38,39], passivation of magnesium based alloys for corrosion protection [40],polymeric

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materials as corrosion inhibitors [41,42], recent patents in the field of corrosion inhibition [43],

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volatile corrosion inhibitors (VCI) [44], DFT as tool for inhibitors designing [45,46], pitting
corrosion of aluminum [47], effect of marine biofilms on corrosion [48], surfactants as corrosion

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inhibitors [49], anticorrosive coating [50] etc. Several review articles described the effect of
inhibitors concentration on their inhibition property. Effect of temperature and other atmospheric
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conditions such as effect of pH and acid concentrations have also been described in many articles.
However, reviews on organic corrosion inhibitors for industrial cleaning are very rare and highly
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anticipated.

1.4. Consequences of corrosion

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Nowadays, corrosion becomes the utmost destructive and stimulating problem for the
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industries particularly for acid cleaning, acid descaling, acid pickling and oil well acidification
industries. According to the National Association of Corrosion Engineers (NACE) in 2002, various
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nations including United States, Germany, Australia, Kuwait, Sweden, Japan, China and India loss
around one to five percent of the total Gross National Product (GNP) because of corrosion. As per
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a data published by NACE (National Association of Corrosion Engineers), in the year 1998
corrosion causes loss of around US $276 billion that equates roughly 3.1% of GNP [51,52]. In
United States (U. S.), this cost of corrosion increased to more than US $2.2 trillion in the year
2011. In India, corrosion results into the loss of approximately US $45 billion or Rs. 2 lacks crores
as estimated in 1st Global Corrosion Summit held in New Delhi, India in 2011 [51,52]. These
estimations are out-of-date and now some more closure looks area available on the costs of
corrosion. According to the most recent published data of NACE, worldwide cost of corrosion is
around US $2.5 trillion that constitutes approximately 3.4% of the global GDP [51,52]. The cost

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of corrosion is now more than US $100-billion and US $ 9.6 billion in India and South Africa,
respectively. By implementing suitable available corrosion monitoring techniques this cost of
corrosion can be reduced from US $ 375 billion (15%) to US $ 875 billion (35%) [51,52]. Despites
the presence of several corrosion monitoring methods, the cost of corrosion is increasing day by
day and also expected to increase in near future. Besides these economic losses, corrosion can
adversely affect our life in other ways. In Guadalajara, Mexico, sever corrosive explosion caused
death of more than 200 people in April 1992 [53]. The series of corrosive blasts have damaged

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over 1600 buildings and injured more than 1500 peoples that ultimately results into loss of

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approximately 75 million USD [54]. Owing to above consequences of corrosion, its control by

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proper implementation of suitable techniques is highly anticipated.
1.5. Forms of corrosion

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Corrosion can be classified on the basis of their appearance on the corroded metallic
surfaces. In most of the forms of corrosion can be identified with the aid of naked eyes, however
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in some cases high magnifications are required for this purpose. There are eight forms of corrosion
namely uniform corrosion (general corrosion), galvanic corrosion (two metals corrosion), pitting
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corrosion, crevice corrosion, selective leaching corrosion (parting corrosion), inter-granular

corrosion, stretch corrosion and erosion corrosion have been identified for corrosion of metals and
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alloys in different corrosive environments [55-57]. Generally, inspection of the corroded metallic
surfaces is carried out before the cleaning of metallic surfaces. Although, the appearance and
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properties of the eight forms of corrosion is unique but most of them are more or less related with
each other. The above classification of forms of corrosion is arbitrary but covers practically all
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corrosion disappointments and complications. The uniform corrosion is the most common form of
corrosion which uniformly precedes over the metallic surface ones it’s get started. Corrosions of
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the metallic surfaces (Zinc, iron) in acidic solutions (HCl, H2SO4) are good examples of uniform
corrosion. Galvanic corrosion is resulted due to potential difference between two interconnected
metals. In the galvanic couple, more reactive metal acts as anode and less reactive metal acts as
cathode. In general, corrosion of cathodic metal is protected in the galvanic couple. Crevices
corrosion is started and propagated through the crevices and other shielded area of the metallic
surface. The pitting corrosion is even more localized form of corrosion which is started from pits/
cracks or holes present on the metallic surface. The pitting corrosion is extremely dangerous form
of corrosion, ones it is started it readily propagates and damaged metallic surface quickly. Since,

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grain boundaries are more active as compared to the matrix and therefore inter-granular corrosion
started from gain boundaries and propagates uniformly. Removal of one or more element(s) from
alloys through a phenomenon of leaching may results into corrosion which is known as selective
leaching corrosion. The erosion corrosion is attributed to the relative motion of corrosive
environments and metallic surface and stress corrosion is resulted due to the cracking resulted by
tensile stress of the metallic surface in the corrosive environments.

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1.6. Brief introduction about organic inhibitors

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Acid cleaning processes in metal finishing, heat exchangers and cleaning of boilers require

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use of acidic solutions particularly acid solutions sulphuric and hydrochloric acid, in order to
remove scales and rust collected on the metallic surfaces, due to their relatively easy availability

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and economic nature. Metallic species (metals and alloys) are highly reactive and therefore they
react with atmospheric components such as moisture and oxygen to form a surface oxide layer,
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and acidic solutions are employed to remove this layer. Removal of these unwanted corrosion
products are essential before using the metallic species for their desired applications. Acidic
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solutions of the phosphoric acids having different concentrations is frequently utilized in the
fertilizers industry as well as several other metallic surfaces such as in chemical coloring,
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electrolytic polishing, cleaning and etching, phosphating and passivating treatments. Literature
study suggests that earlier several forms of organic and inorganic inhibitors including drugs or
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medicines, plant extracts, polymeric materials, ionic liquids, heterocyclic compounds, inorganic
salts, organic-organic and in-organic mixtures have been used to avoid the dissolution of metallic
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materials in to the aggressive solutions. Almost every type of metals such as iron (Fe), zinc (Zn),
copper (Cu), aluminum (Al), magnesium (Mg) and nickel (Ni) etc. and their alloys require cleaning
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before their industrial use with these aggressive solutions. Unfortunately, these acid cleaning
processes result into huge loss of metals and metallic components (of alloys) and therefore these
cleaning processes require some external additives called corrosion inhibitors. Careful inspection
of the literature reveals that these external additives (organic inhibitors) associated with polar
ionizable groups attached to the large hydrocarbon moieties that generally contain extensive
conjugation in the form of benzenoid and non-benzenoid multiple bonds along with the multiple
bonds of polar functional groups [58-70]. It is well documented that phosphorus (P), oxygen (O),
Nitrogen (N) and Sulfur (S) are the most common heteroatoms that constitute the adsorption

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centers, and compounds having these heteroatoms behaved as good inhibitors [71, 72]. The
inhibitive characteristics of these heteroatoms and compounds related with them is attributed to
their high polarizability and lower electronegativity, so that these atoms and the functional groups
constituted by them can cover large metallic surfaces as well as easily transfer their electrons to
the empty orbitals of atoms [73]. It is further documented that nitrogen containing organic
inhibitors are better inhibitors for metallic corrosion in aggressive hydrochloric acid whereas
compounds having sulfur atoms behave as good inhibitors in sulphuric acid. Compounds

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possessing sulfur and nitrogen act as excellent corrosion inhibitors for both media [74].

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The effectiveness of any inhibitor for any particular metal or alloys in aggressive acidic

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solutions depends upon the nature of the inherent inhibitor film accumulated over the surface and
the number and nature of adsorption centers participating in the adsorption phenomenon.

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Generally, the inhibition adsorption and inhibition tendency of the inhibitors having different
heteroatoms follow the reverse order of their electronegativities, so that in S, N, O and P, the
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inhibition efficiency obeyed in the order of: O < N < S < P [75]. Several computational studies,
such as molecular dynamic (MD) simulations and density functional theory (DFT), are used to
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corroborate the experimental results obtained from electrochemical and gravimetric studies [76,
77]. Despite the fact that use of organic inhibitors in solution phase and in the form of coating is
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one of the most appropriate and effective corrosion monitoring methods, however neither inhibitor
can retard the metallic corrosion in aggressive solution [78, 79]. The aim of this review is to the
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major works made to the literature on the corrosion inhibitors in various acidic media for different
metals and alloys.
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2. Acid corrosion inhibitors

The synthesis and use of organic inhibitors particularly for iron and its alloys, like mild
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steel and carbon steel, in acid cleaning industries and oil and gas fields, are highly anticipated.
These organic inhibitors very often passivate the metallic surface through adsorption mechanism.
The passivation caused by organic inhibitors has several advantages over the passivation caused
by inorganic inhibitors. For example, organic inhibitors uniformly passivate the metal surface
resulting in the maximum possible protection, while the passive films of inorganic inhibitors are
highly broken and porous, which results in localized corrosion of the metallic surface [80]. The
presence of organic compounds in the acidic solution generally changes the electrochemical
behavior of the acidic media i.e. decreases the aggressiveness of the medium. The most frequently

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employed heterocyclic inhibitors have sulfur (S), phosphorus (P), nitrogen (N) or oxygen (O)
heteroatoms, and these effectively participate in adsorption centers.
Fekry [81] and Sutter et al. [82] studied the influence of a few selected aliphatic and
aromatic heterocyclic inhibitors in different acidic environments. These heterocyclic inhibitors are
characterized through their 13C and 1H NMR spectroscopy methods. Pha et al. [83] reported that
nitrogen containing aliphatic amines like ethylamine, dimethylamine, butylamine, diethylamine,
butyldiethylamine and a few other octylamine derivatives could be used for the inhibition of

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corrosion of steel in acid solution. These authors observed that the investigated amine derivatives

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form a surface protective film by transferring their non-bonding and π-electrons into the metallic

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d-orbital and forming coordination bonds with metal surfaces. Similar observations have also been
observed for the inhibitive effect of aniline and its derivatives [84], p-substituted anilines [85] and

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other amino substituted anilines [86] where substantial interactions with metal surfaces with the
non-bonding electrons of heteroatoms and π-electrons of the conjugated double bonds takes place,
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which results in strong metal-inhibitors coordinate bonds by the investigated aniline derivatives
(Fe–N). Several other straight chain aliphatic amines of low molecular weight for the mild steel
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corrosion [87], o-substituted anilines [88] have been demonstrated. The inhibition by poly(N-
methylaniline) (PNMA) and polyaniline (PANI) electrodeposited on mild steel from an oxalic acid
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bath was studied using cyclic voltammetric (CV) technique methods [89]. These polyaniline
derivatives inhibit steel corrosion through adsorbing on the surface and their adsorption was
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supported by their FTIR analysis.

Inhibition properties of several amino acid based organic compounds have also been
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investigated with the aid of theoretical and experimental methods using several methods in which
good agreement between them has been observed. Similar to most of the organic corrosion
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inhibitors, their adsorption is also accompanied by physisorption and chemisorption mechanisms

which result in co-ordinate bonds between metal and inhibitor molecules. Generally, co-ordination
bonding takes place between non-bonding electrons of heteroatoms (N, S, O, P etc.) and d-orbitals
of the surface metallic atoms. It has been documented that oxide layers present on the metallic
surface can enhance the metal-inhibitor bonding through hydrogen bonding [87-94]. Zhang et al.
[95] demonstrated the inhibition properties of three amino acids, namely cysteine, glutamic acid
and glycine, and illustrated their inter-molecular synergistic behavior on the corrosion of copper
in acidic solution of hydrochloric acid. Till today the inhibition characteristics of more than 150

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aliphatic and aromatic amines and more than 30 amino acids have been illustrated for several
metals and alloys in various aggressive solutions [96]. As far as the corrosion inhibition of Schiff’s
bases is concerned, they exhibit good inhibition and adsorption tendency which is attributed to
their several salient features such as availability of the amine (–C=N–) group, and relatively lower
electronegative N, S and/or O atoms present in their molecular structures. Nowadays, several
Schiff’s bases have been identified as potential inhibitors for metals and alloys in sulphuric acid
[97] as well as in hydrochloric acid [98] media. The inhibition efficiency of three L-lysine based

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corrosion inhibitors having different substituents on steel in 1M HCl solution showed that the

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presence of electron releasing dimethyl amino (-NMe2, SB-3) displayed the highest inhibition

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performance due to its maximum electron donating ability, followed by SB-2 having an electron
releasing hydroxyl group (-OH) and finally SB-1 without any substituent [99]. All these amino

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based compounds are mixed type corrosion inhibitors and their adsorption obeyed the Langmuir
adsorption isotherm. Experimental inhibition efficiency order was complimented by DFT based
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calculations.
In another study, Ashry with his coworkers [100] investigated the adsorption behavior of
hydrazides and Schiff’s bases on metal surfaces in acidic environment using experimental and
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DFT methods. Results computed from DFT study revealed that values of EHOMO and ELUMO
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increase and decrease, respectively, with the order of inhibition efficiency for Schiff’s bases while
for hydrazides just the reverse order was observed. Recently, Hegazy et al. [101] studied inhibition
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properties of new synthesized Schiff bases as inhibitors for carbon steel in acidic 1M hydrochloric
medium and showed that these Schiff’s bases became effective by strongly adsorbing on the
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metallic surface using their non-bonding and π-electrons.

In literature, N-heterocyclics are demonstrated to be efficient inhibitors for different metals
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and alloys including mild steel and aluminum, whose strong adsorption is generally due to the non-
bonding unshared electron pair of nitrogen atom as well as the presence of multiple bonds such as
double and triple bonds of non-polar (>C=C<, -C≡C-) and polar (>C=O, >C=S, >C=N-, -C≡N)
functional groups of either side chain or of aromatic rings. In addition to this, salient features of
the adsorption of Schiff’s bases at meta/solution interfaces are influenced by several other factors
such as the electrochemical nature of metals and alloys, structure of inhibitors, nature and
aggressiveness of corrosion causing media.

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The inhibition of Azole and its derivatives during pickling processes in acidic media have
been well documented in the literature [102-104]. Similarly, triazole and tetrazole and their
derivatives possess good adsorption and inhibition behavior in acidic media for a variety of metals
and alloys [105-108]. The inhibition performance of triazole, azole and tetrazole derivatives
enhances with their concentrations and is reversed with rise in temperature.
These experimental results are supported by parameters derived from DFT study. Imidazole and
its derivatives were placed in the center of the corrosion inhibitors for metals and alloys in almost

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every types of corrosive media [109-111]. Although imidazole and its derivatives have been

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illustrated to be good inhibitors in a variety of testing media, however their use as inhibition of

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oilfield corrosion is most frequent. The literature insight suggests that imidazole itself and several
its derivatives have been used previously as inhibitors in acidic solution [112]. Additionally,

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pyrazole, pyridine and their several derivatives showed good anti-corrosive nature for metals and
alloys particularly in acid [113-117]. Pyrazine derivatives namely, 2-aminopyrazine (AP), 2-
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methylpyrazine (MP) and 2-amino-5-bromopyrazine (ABP) for cold rolled steel (CRS) in acidic
solution of 1 M S2SO4 using gravimetric and electrochemical methods showed that their inhibition
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efficiencies obeyed the order MP <AP< ABP [118]. Several other nitrogen based heterocyclics
such as 1,2,3-triazole, 1,2,4-triazole, benzotriazole, bipyrazole, pyrimidine, pyridazine, indole,
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benzimidazole, quinolone, purine, tetrazole, benzotriazole etc. and their derivatives [119-130]
have been widely employed for inhibition of metallic and alloys corrosion in aggressive acidic
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solution.
The effects of nicotinic acid (pyridine 3-carboxlic acid) on the corrosion of mild steel in
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unimolar sulphuric acid solution have been illustrated using potentiodynamic polarization and
electrochemical impedance spectroscopy [131]. A significant improvement in the inhibition
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efficiency that is synergistic effect was observed when potassium iodide (KI) was used along with
nicotinic acid. The effect of synergism of KI was observed in every tested inhibition experiment.
The synergistic effects of KI on the inhibition characteristics of phthalazinone on the corrosion
inhibition of mild steel in 1.0 M HCl have been further demonstrated [132]. The synergistic effect
of iodide ions was further illustrated for inhibitive nature of methyl-benzyl quaternary imidazoline
derivative on the steel corrosion in sulphuric acid solution using several techniques. Generally,
sulfur containing compounds exhibit better inhibition performance as compared to nitrogen and
oxygen containing compounds because of the lower electronegativity and high molecular volume

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of the sulfur atom, that offer better metal-inhibitor coordination [133-135]. Literature study
suggested that several sulfur containing compounds such as thiourea, thiosemicarbazide and
thioacetamide exhibited substantial corrosion inhibition for steel, aluminum and nickel in acid
environments [136].
The inhibition effects of some thiourea derivatives, such as N-propyl thiourea (PTU), N-
methyl thiourea (MTU) and N-allyl thiourea (ATU) on iron corrosion in acidic 1M HNO3 solution
of HNO3 and their relative inhibition efficiencies are correlated with thiourea derivatives [137].

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Inhibition efficiencies of several tested organic compounds were demonstrated using various

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commonly used experimental methods like electrochemical and weight loss. The results of these

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analyses were in good correlation. With the aid of computational study, adsorption of these
molecules on steel surface and their most favorable adsorption sites have been described

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appropriately. Li et al. [138] examined inhibition behavior of allyl thiourea on cold rolled steel in
phosphoric acid (H3PO4) solution and demonstrated its acid pickling behavior. The researchers
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investigated thiosemicarbazide and its derivative effective inhibitors for acid corrosion of iron in
2M HCl and 2.5M H2SO4 acid solutions [139,140]. The unshared electron pairs of the sulfur and
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nitrogen atoms are transferred into the d-orbital of surface iron atoms and this provides the strong
meta-inhibitor bonding and results into formation of protective surface barrier. The sodium
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diethyldithiocarbamate tested as efficient inhibitor of cold rolled steel in acidic solution of 0.5 M
hydrochloric acid [141].
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The inhibitive and pickling nature of some sulphonamides and semicarbazone based
organic compounds have been demonstrated as inhibitors for mild steel in aggressive acidic media
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using several experimental methods [142,143]. The inhibition property of a water soluble inhibitor,
namely bis (benzimidazol-2-yl) disulphide, has been studied for mild steel in acidic solution [144].
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The inhibition property and adsorptive nature of a few thiazole derivatives such as 2-
mercaptothiazoline (2MT) and 2-amino-5-mercapto-1,3,4-thiadiazole (2A5MT) at Fe surface in
H2SO4 was studied through commonly employed electrochemical techniques like PDP and EIS
[145]. Both the tested thiazole derivatives acted as potential inhibitors and several experimental
methods showed good agreement in their inhibition performances. Their high inhibition
characteristics are attributed to their strong adoption and formation of inherent inhibitor film. The
strong inherent film of inhibitor on the steel surface was manifested by SEM and AFM studies.
Similar observation was reported by other authors while study the inhibitive nature of

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benzisothiozole-3-piperizine hydrochloride on steel corrosion in sulphuric acid medium (0.5

MH2SO4) [146]. These authors reported that presence of halide ions showed a significant
enhancement of inhibition efficiency by synergism effect. It has been demonstrated in the study
that presence of halide ions not only enhances inhibition tendency of the tested organic inhibitor
but also decreases hydrogen embrittlement.
Addition of halide ion increases inhibition by organic inhibitors and decreases hydrogen
embrittlement. Solmaz et al. [147] investigated the adsorption and inhibitive effect of 2-

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mercaptothiazoline on metallic corrosion and adsorption of hydrogen during acid pickling process

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of iron in acidic media. The inhibitive tendency of benzyl triphenylphosphonium bromide on steel

CR
in H2SO4 at several concentrations and temperatures has been manifested [148]. This compound
acted as a good inhibitor for steel at each tested concentration and temperature. Several

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phosphonium compounds have been tested as inhibitors for nickel corrosion in acidic medium by
other authors [149]. Literature survey revealed that earlier only a few others phosphonium based
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compounds have been demonstrated to have corrosion inhibitive performance [150-152]. Owing
to this, these authors demonstrated the inhibition properties of the new phosphonium based
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corrosion inhibitors for nickel in acidic solution. It is extensively reported that organic inhibitors
with multiple (double or triple) bonds along with high functionality showed good inhibitive and
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adsorptive tendency [153,154].

The inhibition properties of two diols, namely propylene glycol and ethylene glycol and
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one triol, namely glycerol are demonstrated as organic polyhydroxyl inhibitors in highly
aggressive inorganic as well as organic acidic solutions without any neutralization [155]. These
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investigated polyhydroxyl corrosion inhibitors are relatively readily available and cheap organic
compounds that have showed good corrosion inhibitive nature. Due to intermolecular hydrogen
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bonding these polyhydroxyl (diols and triols) compounds also decrease the rate of acid evaporation
and thereby enhance the workability of the testing medium.
The inhibitive nature of macrocyclic cobalt(III) complexes for iron corrosion in pickling
purposes have also been demonstrated in pickling baths by a few researchers. The relative
effectiveness of several cobalt (III) complexes contains nitrogen, sulfur and oxygen on iron
corrosion has been studied in perchloric acid [156,157]. The inhibition efficiencies of the cobalt
(III) based complexes in perchloric acid were supported by their quantum chemical studies and
good relationship between experimental and theoretical results were obtained [156,157].

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Nowadays, several new and effective ecologically friendly inhibitors of synthetic and
natural origins have been developed by several groups of authors working in the field of corrosion.
The development of these green inhibitors has been eagerly anticipated owing to increasing
ecological awareness throughout the entire world. In this direction plant extracts along with
microwave and ultrasound assisted organic compounds and chemical drugs have gained substantial
advancement. The plant extracts are generally rich in chemical compounds such as tannins which
have very complex structures as well as the presence of several heteroatoms through which they

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can adsorb and inhibit corrosion effectively. The inhibition property of the tannin has been

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demonstrated using theoretical and experimental methods in several electrolytic media for

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different metals and alloys [158,159].
The inhibition property of an alkaloid, namely berberine for metal in acidic media has been

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demonstrated using some common computational and experimental methods. [160]. Inhibition
effect and adsorption ability of the berberine on mild steel surface in sulphuric acid is because of
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the interactions between the metallic surface and molecular π-density of berberine molecules.
Pectin has been studied as an effective green environmentally friendly inhibitor for aluminum
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corrosion in hydrochloric acid [161]. Because of their environmentally friendly and safe nature,
several polymeric extracts of leaves and seeds are being employed as effective inhibitors for metals
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and alloys in several common electrolytic media. Souza et al. [162] reported the inhibitive and
adsorptive behavior of caffeine as a green and effective inhibitor for copper corrosion in sulphuric
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acid medium through EIS, complementary adsorption and surface analysis methods. The
investigation showed that caffeine reduces corrosion by strongly and spontaneously adsorbing on
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the copper surfaces in H2SO4 solution. Zenthoxylum alatum extract was used as an ecofriendly
green corrosion inhibitor for mild steel in phosphoric acid solution through weight loss and
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electrochemical methods [163]. The inhibition property of compounds on metallic surfaces was
tested in the 20, 50 and 88% aqueous orthophosphoric acid solutions. The plant extract retarded
the corrosion rate of the metallic specimen more efficiently in the 88% phosphoric acid as
compared to 20% phosphoric acid solution. In addition to the effect of concentration, the influence
of temperature on the corrosion inhibitive nature of tested plant extract for mild steel in the
corrosive media of 20, 50 and 88% phosphoric acid have also been demonstrated at various
temperatures varying from 50 to 80 0C. The experimental demonstration showed that the extract
acts as a good inhibitor for mild steel up to 70 0C in the aggressive solution of phosphoric acid

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(88%). XPS and FT-IR studies were performed in order to find the mechanism of adsorption and
corrosion inhibition in phosphoric acid medium for mild steel.
The inhibition characteristics of the Dendrocalmus sinicus Chia et J.L. Sun leaf (bamboo)
extract (DSCLE) at various acid concentrations of hydrochloric acid and sulphuric acids, ranging
from 1.0 to 5.0 M and 0.5 to 5.0 M respectively, for cold rolled steel (CRS) corrosion were
measured by employing weight loss, atomic force microscopy (AFM) and electrochemical
methods such as EIS and PDP [164]. Results derived from the investigation showed that DSCLE

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is an efficient inhibitor for CRS in the testing media of hydrochloric acid (1.0 M HCl) and

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sulphuric acid (0.5 M H2SO4) and its inhibition efficiency in the testing media obeyed the order:

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HCl > H2SO4. The order of inhibition efficiency derived from weight loss study was supported by
electrochemical measurements. Langmuir adsorption isotherm was best fitted for the adsorption

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of inhibitor (DSCLE) on the metallic (CRS) surface and its mixed nature of corrosion retardation
was manifested by potentiodynamic study.
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Ginkgo leaves extract (GLE) has been demonstrated to be a green and effective corrosion
inhibitor for cold rolled steel (CRS) in the corrosive solution of 1.0–5.0 M HCl as well as 0.5–2.5
M

M H2SO4 solutions using weight loss, electrochemical (EIS and PDP) and SEM (scanning electron
microscopy) methods [165]. Measurements showed that the leaf extract acts as an excellent
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inhibitor for in both media i.e. in 1.0 M HCl as well as in 0.5 M H2SO4, however the inhibition
efficiency of the extract showed somewhat superior performance in hydrochloric acid solution as
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compared to the sulphuric acid solution. Again adsorption of the plant extract follows the most
common Langmuir adsorption isotherm and its mixed nature of corrosion inhibition was
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demonstrated by polarization investigation in hydrochloric acid while in sulphuric acid medium it

acts as a cathodic type of inhibitor. Additionally, Spirulina platensis was established as a novel
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and effective corrosion inhibitor in aggressive solutions of 1M HCl and 1M H2SO4 for mild steel
[166]. In both media, inhibition efficiency of the Spirulina platensis increases with increasing
concentration. The increasing demand for green corrosion inhibitors has led to the use of several
drug molecules as effective and eco-friendly corrosion inhibitors for mild steel in acidic solutions.
Several classes of drugs have been demonstrated to be effective corrosion inhibitors in several
electrolytic media. Because of their origin from natural and biological sources, these chemical
medicines are green and sustainable alternatives to be used in place of toxic volatile corrosion
inhibitors. The employment of carbocyclic compounds along with heterocyclic compounds has

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been very common in the field of corrosion inhibition for acidic corrosion. Among the cyclic
compounds, five- and six-membered ring compounds have been used most extensively, including
furans, pyridines, imidazoles, thiophenes, isoxazoles derivatives and several others moieties which
have been identified in the chemical structure of several drug molecules [167-169].
The inhibition property of tinidazole drug for protection of mild steel disintegration in HCl
solution has been studied [170]. Results of the demonstration showed that tinidazole is a good
inhibitor for steel in acidic solution and furnished the optimum efficiency of 90.5% at as low as

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400 ppm concentration. In addition the inhibition effects of several plant extracts have also been

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studied, owing to their green nature. The inhibition of mild steel corrosion using an ecofriendly

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green inhibitor, namely Hibiscus cannabinus extract was studied in 0.5M H2SO4 solution [171].
The inhibition efficiency of Hibiscus cannabinus increases with increasing concentration.

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Moreover, several other attempts have been made to develop green corrosion inhibitors from time
to time, among them the use of diamine in 1M HCl for mild steel [172], acidic inhibition of mild
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steel by 1,3-diketone malonates [173], use of Bis (benzimidazol-2-yl) disulphide in aggressive
H2SO4 [174], and eco-friendly derivatives of chitosan for mild steel in H2SO4 medium [175] have
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been well established studies. Some other common studies include hydrogen evolution monitoring
using electrochemical techniques in sulphuric acid media for mild steel [176], ketoconazole in
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acidic solution [177], natural polysaccharides and their chemically modified derivatives as
sustainable inhibitors for mild steel [178].
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The effect of iodide concentration on the inhibition effect of methyl benzyl quaternary
imidazoline has been demonstrated in sulphuric acid for mild steel corrosion and a good synergistic
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effect was observed in the presence of iodide ions [179]. Singh, et al. [180] studied the inhibition
and adsorption of an amino acid, namely L-leucine for inhibition of mild steel in acidic solutions.
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The inhibition characteristics of xanthene and xanthione in sulphuric acid are also considered as
green methods of corrosion protection [181,182]. The use of alkylimidazolium based ionic liquids
as inhibitor for aluminum in HCl medium is another step towards green corrosion inhibition [183].
The synthesis and inhibitive action of nonionic surfactants on carbon steel corrosion in acidic
solution was demonstrated [184]. The inhibition property of tacrine was studied using DFT based
quantum chemical calculations for steel corrosion in the corrosive media of 0.5 M H2SO4 and 1.0
M HCl solution [185]. The inhibitive and adsorption behavior of tacrine was described with the
help of several commonly used parameters among which good correlations have been observed.

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The inhibition efficiency of diethanolamine on mild steel corrosion has been studied by Singh et
al. [186] in 0.5 M sulphuric medium. Polarization studies revealed that diethanolamine is a mixed
type corrosion inhibitor and it adsorption on the metal surface obeyed the physisorption
mechanism. The inhibition of micro-plasma arc welded stainless steels in the acidic solution of
phosphoric acid has also been demonstrated at different temperatures [187].
Azghandi and coworkers [188] studied the inhibition effect of acrylic terpolymer (ATP),
butyl acrylate/ methyl methacrylate /acrylic acid for SAE1018 steel in acidic solution under static

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and hydrodynamic conditions of 0–2000 rpm. It was observed that corrosion rate increases with

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increasing rotation. The inhibition property of benzotriazole (BTAH), 3-amino-1,2,4-triazole

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(ATA) and 1-hydroxybenzotriazole (BTAOH) for copper was demonstrated using experimental
and simulation methods [189]. Both corrosion monitoring methods showed that inhibition

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efficiencies of these compounds obeyed the order: BTAH >ATA >BTAOH. Kamal et al. [190]
worked on the inhibition effect of Caulerpin, a bis-indole alkaloid derived from Caulerpa racemosa
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a green algae obtained from marine world for carbon steel in acid solution. Analysis showed that
the inhibition of steel corrosion occurs due to the adsorption of inhibitors on the metallic surface
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in the acidic solution. Other green and effective inhibitors include Schinopsis lorentzii extract for
carbon steel in 1 M HCl [191], Mesoporous silica nanoparticles for active corrosion protection
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[192] and piper guineense [193], nonionic surfactant TRITON-X-405 on ferritic steel [194]. The
inhibition efficiencies of these inhibitors generally increases with increasing concentrations. The
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inhibition effect of n-alkyl quaternary ammonium salts on stainless steel in 2M H2SO4 solution has
been demonstrated in another study using several methods [195]. The pH dependency of 2024-T3
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aluminum alloy corrosion was tested using potentiodynamic and high-throughput multi-electrode
and potentiodynamic methods [196]. A good correlation of the results of both the analyses was
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observed. Results showed that decrease in the pH of aggressive solution results in decrease in the
inhibition efficiency.
3. Mechanism of corrosion inhibition
From the reports available in literature is can be concluded that interactions of organic inhibitors
with metallic surfaces involves donor-acceptor interactions. Most of the reported inhibitors are
compounds that have heteroatoms either in their aliphatic or aromatic ring(s) or in side chain. In
aggressive acidic media, these heteroatoms having unshared electron pairs easily protonate and
therefore in acid solution one or more heteroatoms (S, N, P, O) undergo protonation and exit in

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their cationic forms [197,198]. On the other hands, rapid oxidation of metallic elements in the
aggressive solution makes the metallic surface positively charged that attracts the negatively
charge counter ions such as chloride and sulfate ions of hydrochloric and sulphuric acids,
respectively. The negatively charged counter ions adsorb on the surface and make it negatively
charged. Therefore, in acidic solutions positively charged inhibitor molecules and negatively
charged metallic surface attracted each other through electrostatic interactions. The process of
adsorption can be regarded as physisorption [197-199]. However, as soon as inhibitor molecules

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come onto the metallic surface through physisorption, further oxidation of surface metallic atoms

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results into the production of electrons that consume by protonating hydrogen and eliminate

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hydrogen gas. Thereby, cationic inhibitor molecules return their neutral form and heteroatoms with
lone pairs of electron can transfer their lone pair of electrons into the d-orbitals of the surface metal

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atoms that results into the phenomenon of chemisorption. However, this kind of electrons transfer
causes their accumulation in the d-orbitals of metallic atoms that result into inter-electronic
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repulsions. In order to avoid this repulsions a reverse transfer of electrons from d-orbitals of surface
metallic atoms to the unoccupied (empty) anti-bonding molecular orbitals of inhibitor molecules.
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This process of electron transfer is known as retro-donation. It is reported that greater donation of
electrons results into greater retro-donation and thereby donation and retro-donation strengthen
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each other through synergism [197-199]. Thus it can be predicted that adsorption of organic
corrosion inhibitors on the metallic surfaces in aggressive acidic solution takes place in two steps
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namely, physisorption followed by chemisorption. The adsorption tendency of organic inhibitors

on the metallic surface depends upon numerous factors such as nature of corroding metal and
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corrosive medium, solution temperature and electronic structure of inhibitor molecules [198-200].
Generally, inhibitor molecules having electron releasing substituents such as –NH2, -OH, -OCH3,
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-CH3 etc. act as better corrosion inhibitors as compared to the inhibitor molecules having electron
withdrawing substituents such as –NO2, -CN, -COOH etc. An organic inhibitor with planer
geometry covers larger surface area and thereby behaves better corrosion inhibitor as compared to
the organic inhibitor having non-planer geometry [200-203]. The diagrammatic illustration of
adsorption of organic corrosion inhibitors in acidic medium in our previous reported article is
presented in Fig. 1.
4. Conclusion

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Present review article deals with the effect of organic compounds as corrosion inhibitors
for metals and alloys in aggressive acidic solutions. The article also describes the general
introduction about corrosion and factors affecting it. Consequences, forms and mechanism of
corrosion have also been described in the present article. The article survey reveals that several
types of compounds/ inhibitors have been employed corrosion inhibitors in aggressive acidic
solutions, among them application of synthetic organic compounds is the most common and
practical methods because of their economic and ease synthesis and ease of application along with

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their high protection ability. Study reveals that organic compounds having heteroatoms (N, S, O

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and P) act as better corrosion inhibitors as compared to the compounds devoid of these

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heteroatoms. The heteroatoms with lone pair of electrons adsorb on the metallic surface thorough
physisorption mechanism followed by chemisorption mechanism. Literature survey also reveals

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that in acidic solution heteroatoms of the corrosion inhibitors exist in their cationic forms.
Generally, rate of metallic dissolution is very high in the absence of inhibitors; however presence
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of organic inhibitors in the corrosive medium significantly reduced the rate of the dissolution. It is
also observed that the inhibition efficiencies of organic inhibitors increase with increases in their
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concentration and decreases with increase in temperature. An inhibitor with electron releasing
substitutes and planer geometry acts as better corrosion inhibitor as compared to the inhibitor
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having electron withdrawing substituents and/ or non-planer geometry. The role of acid solution
in corrosion inhibition studies is likely to increase in the future, as the focus of investigations shifts
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toward complicated chemical mechanisms. The inhibition characteristics of these organic

compounds are attributed to their adsorption through polar functional groups such as –CN, -NO2,
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-COOH, -COOC2H5, -CONH2, -OH, -NH2, -OCH3, -OH etc. and π-electrons.
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Acknowledgements
The first author, Madhusudan Goyal, is grateful to the University Grant Commission, New Delhi,
India for awarding senior research fellowship to carry out his research work. The authors also
thank Department of Science and Technology, New Delhi (DST) for providing instrumental

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facilities. C. Verma thankfully acknowledges the North-West University, South Africa for
providing scholarship under Postdoctoral Fellowship Scheme.

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Fig. 1: Adsorption behavior of organic corrosion inhibitors (DHATs) on mild steel in 1 M
HCl solution.
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Highlights

 Heteroatoms (O, S, N, and P) and π-electrons in the form of conjugation were discussed.
 Acidic environment is a powerful tool to study the corrosion inhibition efficiency.
 The inhibition effect of several classes of compounds have been described.

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