Arabian Journal of Chemistry (2019) 12, 4646–4663

King Saud University

Arabian Journal of Chemistry

www.ksu.edu.sa
www.sciencedirect.com

REVIEW

Organic corrosion inhibitors for aluminum and its

alloys in chloride and alkaline solutions: A review
Klodian Xhanari a,b, Matjaž Finšgar a,*

a
University of Maribor, Faculty of Chemistry and Chemical Engineering, Smetanova ulica 17, 2000 Maribor, Slovenia
b
University of Tirana, Faculty of Natural Sciences, Boulevard ‘‘Zogu I”, 1001 Tirana, Albania

Received 12 May 2016; accepted 17 August 2016

Available online 26 August 2016

KEYWORDS Abstract In this review we summarize the research work reported in the last two decades on the
Aluminum; use of organic corrosion inhibitors for aluminum and its alloys in different alkaline (mainly NaOH
Aluminum alloys; and KOH) and chloride solutions. The focus is on the corrosion inhibitor type and its inhibition
Corrosion inhibitor; effectiveness and mechanism. Moreover, the testing conditions and the methodology used for
Chloride solution; corrosion inhibition performance evaluation are presented. As seen herein, the most frequently used
Alkaline solution corrosion inhibitors are the mercapto compounds, azole derivatives, organic dyes, and different
polymers. Weight loss and electrochemical techniques were among the most frequently used tech-
niques to evaluate the corrosion inhibition effectiveness of the studied compounds.
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Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4647
2. Corrosion of aluminum . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4647
2.1. Corrosion of aluminum in alkaline solutions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4647
2.2. Corrosion of aluminum in chloride solution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4648
2.3. The influence of alloy composition on corrosion resistance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4648
3. Organic corrosion inhibitors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4649
3.1. Organic corrosion inhibitors in alkaline solutions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4649
3.1.1. Organic corrosion inhibitors in NaOH solution. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4649
3.1.2. Organic corrosion inhibitors in KOH solution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4652

* Corresponding author.
E-mail address: matjaz.finsgar@um.si (M. Finšgar).
Peer review under responsibility of King Saud University.

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Organic corrosion inhibitors
3.1.3. Organic corrosion inhibitors in other alkaline solutions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
3.2. Organic corrosion inhibitors in chloride solution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
4. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
Appendix A. Supplementary material . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
1. Introduction
Corrosion is a naturally occurring process that leads to the degrada-
tion of the material’s properties through its chemical or electrochemi-
cal interaction with the surrounding environment. The costs related to
corrosion can be either direct (due to the replacement of corroded
structures, implementation and maintenance of corrosion protection,
etc.) or indirect (due to the shutdown of manufacturing plants, product
and efficiency losses, etc.) (Revie and Uhlig, 2008). It has been reported
in earlier studies that the costs related to corrosion can reach up to 3–
5% of the Gross National Product in the most developed countries
(McCafferty, 2010). The economic aspect combined with security
and environmental concerns have provided continuous motivation
for the research community to develop new methods to reduce the
impact of corrosion. Material selection is one of the general
approaches used to prevent corrosion. Apart from specific require-
ments related to the actual application and/or the corrosion environ-
ment, there are also general criteria to be considered in material
selection. The physical and mechanical properties (density, strength,
ductility, hardness, etc.), resistance to corrosion and to service condi-
tions, cost, and availability are among the most important (Ahmad,
2006).
Aluminum has excellent formability, high electrical and thermal
conductivity, a low weight (a density of 2.7 g/cm3), and high reflectiv-
ity. Aluminum has a relatively low cost and is almost twice as abun-
dant as iron. The high strength to weight ratio of some aluminum
alloys is even comparable to that of high-strength structural steels.
In addition, aluminum shows good corrosion resistance when exposed
to the atmosphere and many aqueous environments, due to the forma-
tion of a resistive oxide layer. Furthermore, the corrosion products are
colorless and non-poisonous (Kaufman, 2000; Bardal, 2004; Winston
Revie, 2011). The combination of these properties and others has made
aluminum one of the most attractive materials in several applications,
including as packaging for food, beverages, and pharmaceutical prod-
ucts, sacrificial anodes, automotive, marine, and aerospace parts
(Davis, 2000; Winston Revie, 2011).
Although the oxide layer formed on the aluminum surface protects
it in certain environments, when exposed to many acidic and alkaline
solutions, and especially chloride containing solutions, this oxide layer
is destroyed and the metal corrodes. Several methods and combina-
tions thereof have been used to reduce the corrosion of aluminum
and its alloys in different environments. Anodizing, coatings (conver-
sion, inorganic, organic, or organic-inorganic types) and inhibitors
(inorganic and organic) are among the most common protection meth-
ods tested (Domingues et al., 2003; Liu et al., 2005; Na and Pyun,
2006; Lundvall et al., 2007; Niknahad et al., 2010; Harvey, 2013;
Golru et al., 2015b). Moreover, natural compounds, also known as
green corrosion inhibitors, have been extensively used to protect alu-
minum materials (James and Atela, 2008; Abiola and Tobun, 2010;
Abdallah et al., 2012; Gerengi, 2012; Abdallah et al., 2016a;
Chaubey et al., 2016; Winkler et al., 2016). Furthermore, corrosion
inhibitor research for aluminum and its alloys have been also presented
in several patents (Jung et al., 1989; Lewis and Aklian, 1999; Sinko,
2002; Crotty et al., 2008; Foster and Ciemiega, 2008; Garner, 2014).
The aim of this paper is to present only research articles published
since the review article by Jayalakshmi and Muralidharan
(Jayalakshmi and Muralidharan, 1997) in 1997, on the use of organic
compounds as corrosion inhibitors for aluminum and its alloys. Some
4647
4653
4654
4659
4660
4660
4660
reviews dealing either with the corrosion protection of particular alu-
minum alloys of interest (Snihirova et al., 2016) or on green inhibitors
have also been published (Montemor, 2016). However, to the best of
our knowledge, the review from Jayalakshmi and Muralidharan
(1997) was the last effort to present a comprehensive summary of
the research performed on organic corrosion inhibitors for aluminum
in acidic, alkaline, and neutral solutions. Therefore, herein we discuss
only about the research work published after that review and summa-
rize the latest developments in the field. Herein, the focus is only on
corrosion inhibitors for aluminum and its alloys in alkaline and chlo-
ride corrosive solutions. In this work, we first briefly describe the gen-
eral corrosion process of aluminum and its alloys, followed by a review
of the organic corrosion inhibitors for alkaline and chloride-containing
solutions.
2. Corrosion of aluminum
The standard electrode potential indicates that aluminum is a
thermodynamically reactive metal, second only to magnesium
among the common engineering metals (Revie and Uhlig,
2008). However, the Pourbaix diagram for the aluminum-
water system shows that in the pH range from about 5 to
8.5, aluminum is thermodynamically stable. This stability is
due to the formation of an amorphous oxide layer on the alu-
minum surface with about 2–10 nm thickness (Revie and
Uhlig, 2008; Winston Revie, 2011). The oxide layer prevents
further attack on aluminum from the corrosive environment,
rendering it passive. This passive state can be altered by several
factors, among which pH, temperature, and chloride content
are the most important.
In the following sections the corrosion behavior of alu-
minum and its alloys in alkaline and chloride solutions is pre-
sented. In addition, the effect of the chemical composition on
corrosion resistance is also discussed.
2.1. Corrosion of aluminum in alkaline solutions
Aluminum and many of its alloys are susceptible to corrosion
when exposed to alkaline solutions. This is frequently reported
for sodium and potassium hydroxide. On the other hand, the
low solubility of lime and calcium hydroxide solutions limits
their corrosive action on aluminum materials. High corrosion
resistance is observed in ammonium hydroxide solutions for
most aluminum alloys. The presence of approx. 4 wt.% Mg
in aluminum alloys increases their corrosion resistance in alka-
line solutions, even more so in ammonium hydroxide solutions
(Davis, 2000).
Aluminum is subjected to alkaline solutions (mainly
sodium or potassium hydroxide) in several applications,
among which aluminum-air batteries and alkaline etching are
the most important (Egan et al., 2013; Ma et al., 2013;
Golru et al., 2015a). The performance of aluminum-air batter-
ies is dependent on the mitigation of aluminum corrosion in
4648 K. Xhanari, M. Finšgar

alkaline solution, which otherwise can lead to self-discharge 2.2. Corrosion of aluminum in chloride solution
(Egan et al., 2013).
Pyun and Moon studied the corrosion mechanism of pure Pitting corrosion is the most dangerous type of aluminum cor-
aluminum in alkaline solution, using electrochemical tech- rosion. It occurs as holes and pits of irregular shapes on the
niques (Pyun and Moon, 2000). They reported that aluminum surface of the metal. The diameter and depth of the pits are
dissolution proceeds first through hydroxide film formation dependent on the type of material, the corrosive medium,
and then its dissolution as a partial anodic reaction. The same and the properties of the environment that the aluminum
authors (Moon and Pyun, 1999) previously concluded that this and its alloys are exposed to. Pitting corrosion of aluminum
film is electrochemically formed due to the migration of the takes place frequently in aerated chloride solutions.
hydroxide ions through the oxide layer on the aluminum sur- Chloride ions attack the natural oxide layer, damaging it in
face, as shown in Eq. (1): the weakest parts. On the anodic sites two main reactions
Al þ 3OH ¢ AlðOHÞ3 þ 3e ð1Þ occur:
The aluminum hydroxide film is then chemically dissolved Al ¢ Al3þ þ 3e ð8Þ
by the attack of the hydroxide ions to form soluble aluminate
ions (Eq. (2)): Al3þ þ 3H2 O ¢ AlðOHÞ3 þ 3Hþ ð9Þ
AlðOHÞ3 þ OH 
¢ AlðOHÞ
4 ð2Þ Eq. (9) shows that at anodic sites a more acidic (pH = 3–4)
environment is created. The chloride ions facilitate the anodic
The combination of Eq. (1) and Eq. (2) gives the partial
dissolution of aluminum, forming aluminum chloride. The
anodic dissolution reaction of pure aluminum in alkaline solu-
later hydrolyzes to form the hydroxide and acid, which shifts
tions, as shown in Eq. (3):
the pH to acidic values. Eqs. (10)–(12) show the possible reac-
Al þ 4OH ¢ AlðOHÞ
4 þ 3e

ð3Þ tions at the cathodic sites:
There are two possible partial cathodic reactions, the reduc- AlCl3 þ 3H2 O ¢ AlðOHÞ3 þ 3HCl ð10Þ
tion of oxygen and/or the reduction of water, represented by
Eqs. (4) and (5): 3Hþ þ 3e ¢ 3=2H2 ð11Þ
 
3=4O2 þ 3=2H2 O þ 3e ¢ 3OH ð4Þ
1=2O2 þ H2 O þ 2e ¢ 2OH ð12Þ
 
3H2 O þ 3e ¢ 3=2H2 þ 3OH ð5Þ As seen in Eq. (12), the cathodic sites are more alkaline due
to the local hydroxide formation. The presence of oxygen is
The corrosion reaction can be summarized by combining
crucial for pitting. Cone-shaped accumulations of corrosion
Eqs. (3) and (4):
products are formed at the mouth of the pits due to the precip-
Al þ OH þ 3=4O2 þ 3=2H2 O ¢ AlðOHÞ
4 ð6Þ itation of aluminum hydroxide outside the pits (Winston
and/or by combining Eqs. (3) and (5): Revie, 2011), as seen in Fig. 1.

Al þ 3H2 O þ OH ¢ 3=2H2 þ AlðOHÞ

4 ð7Þ
Experimental work shows that during the corrosion of pure
aluminum in alkaline solution gas evolves, which confirms that
the aluminum dissolution process goes mainly through the
reduction of water (Eq. (7)).
2.3. The influence of alloy composition on corrosion resistance
Based on the strengthening method used, commercial wrought
aluminum alloys can be divided into two groups. Series 1xxx,
3xxx, 4xxx, and 5xxx alloys are non-heat treatable, while series

Figure 1 Pitting corrosion of a Cu- and Fe-containing aluminum alloy (Winston Revie, 2011).
Organic corrosion inhibitors 4649

chloride-containing solutions published over the last two dec-

Table 1 Composition of the wrought alloys series (Davis,
ades. Fig. 2 presents the most tested organic compounds in
2000; Winston Revie, 2011).
both types of corrosive environment. Tables S1 and S2 (in
Series designation Type of alloy composition the Supplementary Materials) summarize the new findings,
Non-heat treatable alloys including details on the inhibition effectiveness (g) of the com-
1xxx Al pounds tested in alkaline and chloride-containing solutions. As
3xxx Al-Mn-Mg reported by the authors in their publications, only the mini-
4xxx Al-Si mum and maximum inhibition effectiveness values are given
5xxx Al-Mg (1–2.5% Mg) in these tables. The research work is presented in two main
5xxx Al-Mg-Mn (3–6% Mg) parts, based on the solution type (alkaline or chloride), follow-
Heat treatable alloys ing the trend of decreasing aluminum content in the material.
2xxx Al-Cu-Mg (1–2.5% Cu) When possible, the articles are also grouped based on the
2xxx Al-Cu-Mg-Si (3–6% Cu) authors or the compound tested. In the majority of cases,
6xxx Al-Mg-Si the authors report the chemical composition of the aluminum
7xxx Al-Zn-Mg materials tested, including the designation of the alloys. How-
7xxx Al-Zn-Mg-Cu
ever, it can be noticed that there are discrepancies as regards
8xxx Al-Li-Cu-Mg
the element percentages for the same alloy designation
obtained from different providers. Therefore, the chemical
composition and alloy designation as given by the authors
are presented in Table S3 in the Supplementary Materials.
2xxx, 6xxx, and 7xxx alloys are heat-treatable. Table 1 presents
the alloy composition of these series.
3.1. Organic corrosion inhibitors in alkaline solutions
General, galvanic, pitting, stress-corrosion cracking, inter-
granular, and exfoliation are among the most common types
3.1.1. Organic corrosion inhibitors in NaOH solution
of corrosion for aluminum, independent of the corrosive envi-
ronment (Davis, 2000; Winston Revie, 2011). The non-heat Dhayabaran et al. studied the inhibition effectiveness of fluo-
treatable alloys have a higher corrosion resistance toward gen- rescein (a synthetic organic compound with the IUPAC name
eral corrosion compared to the heat treatable alloys. However, 30 ,60 -dihydroxyspiro[2-benzofuran-3,90 -xanthene]-1-one) as a
series 6xxx alloys containing the Al-Mg2Si system also show corrosion inhibitor for commercially pure aluminum in 1.0 N
considerable resistance to general corrosion (Winston Revie, NaOH solution at 30 °C, using the weight loss (WL) and
2011). The same behavior is observed for series 7xxx alloys
that do not contain copper (Al-Zn-Mg). The alloys’ resistance
to pitting corrosion increases significantly with increasing pur-
ity. The pitting corrosion resistance decreases in the order ser-
ies 1xxx > series 5xxx (especially when containing less than
3 wt.% Mg) > series 3xxx > series 6xxx > series
7xxx > series 2xxx (Davis, 2000). Alloys containing more than
0.15 wt.% copper are more susceptible to pitting corrosion,
especially in environments containing chlorides. An increase
in iron content will lead to the promotion of pitting corrosion.
A similar effect is observed in series 6xxx alloys (Davis, 1999).
Aluminum alloys can be susceptible to intergranular corrosion
if second-phase microconstituents are formed at grain bound-
aries. A corrosion potential of the alloy different from that of
the matrix will also cause intergranular corrosion. A balanced
content ratio of the magnesium and silicon present in the 6xxx
series will lead to higher resistance to intergranular corrosion.
The presence of appreciable amounts of soluble alloying ele-
ments, such as copper, magnesium, silicon, and zinc, will make
these alloys susceptible to stress-corrosion cracking. The same
is observed for the heat treatable alloys (series 2xxx and 7xxx,
as well as series 5xxx containing more than 3 wt.% Mg)
(Davis, 2000).

3. Organic corrosion inhibitors

Organic compounds have been extensively used as corrosion

inhibitors for aluminum and its alloys due to the fact that they
contain several heteroatoms (N, S, O and P) which serve as
adsorption centers (Xhanari and Finšgar, 2016). Hereinafter,
we discuss the use of organic compounds as corrosion
inhibitors for aluminum and its alloys in alkaline and
Figure 2 The most tested organic compounds as corrosion
inhibitors for aluminum and aluminum alloys in both alkaline and
chloride-containing solutions.
4650
potentiodynamic polarization (PDP) techniques (Dhayabaran
et al., 2004). The inhibition effectiveness of fluorescein
increased with increasing concentration. The addition of
CaO to the solutions containing fluorescein further increased
the inhibition effectiveness. Based on the PDP measurements,
the authors reported that fluorescein acted as an anodic-type
inhibitor.
Al-Juaid investigated the inhibition effectiveness of three
mono azo dyes, i.e., (E)-4-((2-chlorophenyl)diazenyl)naphtha
lene-1,5-diol, (E)-4-(o-tolyldiazenyl)naphthalene-1,5-diol, and
(E)-4-((2-methoxyphenyl)diazenyl)naphthalene-1,5-diol, as
corrosion inhibitors for 99.99% aluminum in 0.01 M NaOH
solution at 30–50 °C, using the WL and galvanostatic polariza-
tion (GSP) techniques (Al-Juaid, 2007). The inhibition effec-
tiveness increased with increasing inhibitor concentration,
following the order (E)-4-((2-methoxyphenyl)diazenyl)naph
thalene-1,5-diol > (E)-4-(o-tolyldiazenyl)naphthalene-1,5-dio
l > (E)-4-((2-chlorophenyl)diazenyl)naphthalene-1,5-diol. An
increase in temperature decreased the inhibition effectiveness
of these compounds. The author attributed the inhibition
action of these compounds to their ability to form insoluble
complexes in combination with the metal cation, which adsorb
on the aluminum surface.
Abdallah et al. tested three N-thiazolyl-2-cyanoacetamide
derivatives, i.e., N-(4-phenylthiazol-2-yl)-2-phenylazo-2-cya
noacetamide, N-(4-phenylthiazol-2-yl)-2-(p-tolylazo)-2-cyanoa
cetamide, and N-(4-phenylthiazol-2-yl)-2-(p-methoxypheny
lazo)-2-cyanoacetamide, as corrosion inhibitors for 99.99%
aluminum in 0.01 M NaOH solution at 30 °C, using the WL
and GSP techniques (Abdallah et al., 2014b). The inhibition
effectiveness of these derivatives increased with increasing
derivative concentration, but decreased with increasing tem-
perature. The data showed that the inhibition effectiveness
decreased in the order N-(4-phenylthiazol-2-yl)-2-(p-methoxy
phenylazo)-2-cyanoacetamide > N-(4-phenylthiazol-2-yl)-2-(p
-tolylazo)-2-cyanoacetamide > N-(4-phenylthiazol-2-yl)-2-phe
nylazo-2-cyanoacetamide. The authors explained this order in
terms of the polar effect of the p-substituents on the phenylazo
group. N-(4-phenylthiazol-2-yl)-2-(p-methoxyphenylazo)-2-cy
anoacetamide has a highly electron donating p-OCH3 group,
which enhanced the delocalized p-electrons on the molecule.
The inhibition effectiveness was further increased upon the
addition of 1 mM MCl2 (M = Mg, Ca, Sr, Ba), following
the order Ba2+ > Sr2+ > Ca2+ > Mg2+. The polarization
measurements suggested that these compounds acted as
mixed-type inhibitors. Abdallah et al. also reported on the
inhibition effectiveness of three bidentate azodye compounds,
i.e., 1-(4-((2-hydroxy-3-nitrophenyl)diazenyl)phenyl)propan-
1-one, 1-(4-((3-amino-2-hydroxyphenyl)diazenyl)phenyl)pro
pan-1-one, and 1-(4-((2,4,6-trihydroxyphenyl)diazenyl)phe
nyl)propan-1-one, as corrosion inhibitors for 99.99% alu-
minum in 0.1 M NaOH solution, using the WL and GSP tech-
niques at 30 °C (Abdallah et al., 2014a). The inhibition
effectiveness increased with increasing concentration of the
compounds and with decreasing temperature. The presence
of the electron-donating group in the chemical structure of
the inhibitors was crucial for the corrosion inhibition effect.
The authors showed that the inhibition effectiveness increased
in the order 1-(4-((2,4,6-trihydroxyphenyl)diazenyl)phenyl)pro
pan-1-one)) > 1-(4-((3-amino-2-hydroxyphenyl)diazenyl)phe
nyl)propan-1-one > 1-(4-((2-hydroxy-3-nitrophenyl) diazenyl)
phenyl)propan-1-one. The polarization measurements showed
K. Xhanari, M. Finšgar
that these compounds acted as mixed-type inhibitors. The
authors attributed the inhibiting effect of the bidentate azo-
dyes to the adsorption of a stable complex formed on the alu-
minum surface. They also evaluated the inhibition
effectiveness of these three compounds with the addition of
1 mM solutions of chlorides of Mg2+, Ca2+, and Ba2+. It
was reported that these additives improve the inhibitive action
of the bidentate azodyes, probably due to the fact that these
cations can chemisorb on the aluminum surface in alkaline
solutions. The enhanced inhibition effectiveness of the three
tested compounds has a synergistic nature. The inhibition
effectiveness of the compounds followed the order
Ba2+ > Ca2+ > Mg2+.
Al-Rawashdeh and Maayta investigated the inhibition
effectiveness of the cationic surfactant cetyl trimethylammo-
nium chloride (CTAC) in the corrosion of 99.95% aluminum
in 0.2 M and 0.5 M NaOH solutions at 30–60 °C, using
the WL and potentiostatic polarization (PSP) techniques
(Al-Rawashdeh and Maayta, 2005). The inhibition effective-
ness increased with increasing surfactant concentration and
decreased with increasing NaOH concentration. Increasing
temperature resulted in a decrease in inhibition effectiveness
and the authors explained this by the increase in aluminum dis-
solution at higher temperatures. In the same article, the
authors tested the inhibition effectiveness of CTAC in 0.2 M
and 0.5 M HCl solution under the same conditions as men-
tioned above (temperature and material type). They concluded
that the inhibition effectiveness of CTAC in NaOH was higher
than in HCl solutions.
Abdel-Gaber et al. tested cetyl trimethyl ammonium bro-
mide (CTAB) as an inhibitor in the corrosion of 99.68% alu-
minum in 2 M NaOH solution, using the PDP technique
(Abdel-Gaber et al., 2010). The inhibition effectiveness
increased with increasing compound concentration. The high-
est inhibition effectiveness was obtained for concentration val-
ues around the CTAB critical micelle concentration
(1.8  104 M). A further increase in the CTAB concentration
led to a decrease in the corrosion current. The authors
reported that CTAB chemisorbed on the aluminum surface.
Chemisorption involved charge transfer from the lyophilic
function groups in the molecules to the metallic surface, form-
ing a coordinate bond.
Princey and Nagarajan reported on the inhibition effective-
ness of 3-hydroxy flavone in the corrosion of 99.59% alu-
minum in 1 M NaOH solution at 30–50 °C, using the WL,
PDP, and electrochemical impedance spectroscopy (EIS) tech-
niques (Princey and Nagarajan, 2012). The inhibition effective-
ness increased with increasing compound concentration, but
decreased with increasing temperature. The addition of quater-
nary ammonium bromide and iodide salts further increased the
inhibition effectiveness. However, the authors do not specify
either the concentration of the quaternary ammonium halide
salts added, or the concentration of the 3-hydroxy flavone
solution. The PDP measurements showed that 3-hydroxy fla-
vone acted as a mixed-type inhibitor.
Maayta studied the inhibition effectiveness of sulfonic acid
(SA), sodium cumene sulfonate (SCS), and sodium alkyl
sulfate (SAS) as corrosion inhibitors for 99.5% aluminum in
0.5 M NaOH solution at 30–60 °C, using the WL technique
(Maayta, 2006). The inhibition effectiveness increased with
increasing concentration of these compounds, following the
order SA > SCS > SAS. A decrease in the inhibition
Organic corrosion inhibitors
effectiveness with increasing temperature was reported. How-
ever, the question that arises in this study is whether the
observed reduction in the corrosion rate is due to the corrosion
inhibition effect or due to the reduction in the pH, as acids
were employed.
Rajendran et al. investigated the inhibition effectiveness of
succinic acid and succinic acid with the addition of zinc sulfate
and diethylene triamine penta (methylene phosphonic acid),
(DETAPMP) in the corrosion of 99% aluminum in 0.01 M
NaOH solution at 30 °C, using the WL and PDP techniques
(Rajendran et al., 2012a). The inhibition effectiveness
increased with increasing succinic acid concentration. A fur-
ther increase in the inhibition effectiveness was reported when
Zn2+ was added. The authors reported that the maximum
inhibition effectiveness (g = 97.5%) was reached for the tern-
ary system (succinic acid + zinc sulfate + diethylene triamine
penta (methylene phosphonic acid)). The PDP measurements
showed that the ternary system acted as a mixed-type
inhibitor.
Rajendran et al. studied the corrosion of 99% aluminum in
0.5 M NaOH solution in the presence of glutaric acid and glu-
taric acid with the addition of zinc sulfate and DETAPMP,
using the WL and PDP techniques (Rajendran et al., 2013).
The inhibition effectiveness of glutaric acid increased with
increasing compound concentration and decreased with
increasing temperature. The addition of zinc sulfate to glutaric
acid increased the inhibition effectiveness from 46.0% to
57.2% for the highest concentration of glutaric acid tested.
The authors reported an even higher difference in the inhibi-
tion effectiveness for the ternary system (glutaric acid + zinc
sulfate + diethylene triamine penta (methylene phosphonic
acid)). The highest inhibition effectiveness obtained in this case
was 93.4%. The PDP measurements showed that this formula-
tion acted as a mixed-type inhibitor. Based on the atomic force
microscopy (AFM) studies, the authors showed that the alu-
minum surface is smoothened as a result of the adsorption
layer formed. Rajendran et al. also studied the inhibition effec-
tiveness of DETAPMP and adipic acid (AA) in the corrosion
of 99% aluminum in 0.01 M NaOH solution at 30 °C in the
presence of Zn2+ ions, using the WL and PDP techniques
(Rajendran et al., 2012b). They found that the inhibition effec-
tiveness of both compounds increased with increasing com-
pound concentration, but only until a certain value. This
increase is limited in the case of DETAPMP. The authors
reported that for concentrations of DETAPMP above
50 ppm the inhibition effectiveness decreased. The same was
observed for AA, for which the limiting concentration was
found to be 240 ppm. When DETAPMP and AA were used
together in the presence of a 20 ppm concentration of Zn2+
the inhibition effectiveness increased remarkably, up to 98%.
The PDP measurements showed that both compounds acted
as mixed-type inhibitors.
Elango et al. investigated the inhibition effectiveness of the
mixture polyaniline and zinc oxide as a corrosion inhibitor for
57S aluminum (97.7% aluminum) in 2 M NaOH solution,
using the WL and GSP techniques (Elango et al., 2009).
According to the authors, polyaniline was dissolved in NMP,
but no explanation was given in the text for this abbreviation.
The abbreviation NMP was used by the same authors in
another article to refer to N-methyl-2-pyrrolidone (Elango
et al., 2010). The authors reported that the inhibition effective-
ness of the polyaniline and zinc oxide mixture increased with
4651
increasing polyaniline concentration. Based on the polariza-
tion measurements, they concluded that the corrosion of 57S
aluminum alloy in the presence of the above-mentioned mix-
ture is under anodic control. The same authors tested zinc
oxide and polyaniline dissolved in N-methyl-2-pyrrolidone as
a corrosion inhibitor for 57S aluminum (no composition given)
in 2 M NaOH solution, using the WL and GSP techniques
(Elango et al., 2010). They reported that the inhibition effec-
tiveness of the mixture increased with increasing polyaniline
concentration.
Umoren et al. reported on polyvinyl alcohol as a corrosion
inhibitor for AA1060 aluminum alloy in 0.1 M NaOH solu-
tion, at 30 and 40 °C, using the WL and hydrogen evolution
(HE) techniques (Umoren et al., 2007). The inhibition effec-
tiveness increased with increasing inhibitor concentration, per-
forming better at 30 °C compared to 40 °C. Although there is a
good correlation between the inhibition effectiveness values
obtained from the two methods, the values are low (the highest
g obtained was 34.4%). The authors also reported on the syn-
ergistic effect from the addition of potassium halides (KI, KBr,
and KCl). Surface coverage values decreased in the order
Cl > Br > I, indicating the important role of the radii
and electronegativity of the halides in the adsorption process.
Physisorption was the proposed mechanism for this
compound.
Verma et al. tested three organic compounds, i.e., 50 -amino-
2,4-dihydroxy-400 -methyl-1,10 :30 , 100 -terphenyl-40 ,60 -dicarboni
trile (ABDN-1), 50 -amino-2,200 ,4-trihydroxy-1,10 :30 ,100 -terphe
nyl-40 ,60 -dicarbonitrile (ABDN-2), and 50 -amino-2,4,400 -trihy
droxy-300 -methoxy-1,10 :30 ,10 -terphenyl-40 ,60 -dicarbonitrile
(ABDN-3), as inhibitors in the corrosion of AA1060 alu-
minum alloy in 0.5 M NaOH solution (Verma et al., 2015).
The inhibition effectiveness increased with increasing ABDN
concentration. The PDP measurements showed that these
compounds acted as mixed-type inhibitors. The authors con-
cluded that these compounds adsorbed on the alloy surface,
forming a protective film.
Oguzie et al. studied the inhibition ability of Bismarck
brown dye (a basic diazo compound) in the corrosion of
AA1060 aluminum alloy in 0.1 M NaOH solution, using the
WL technique at 25 and 70 °C (Oguzie et al., 2006). The inhi-
bition effectiveness increased with increasing dye concentra-
tion. However, the data indicated that there was no clear
trend in the way the inhibition effectiveness varied when com-
paring the values for 25 and 70 °C. At lower concentrations of
Bismark brown dye (5 mM and 10 mM), the inhibition effec-
tiveness increased slightly with increasing temperature. At
moderate concentrations (15–20 mM), a temperature increase
caused a decrease in the inhibition effectiveness. At the highest
concentration tested (25 mM), the inhibitor behaved the same
as at lower concentrations when the temperature increased
from 25 to 70 °C. Based on the thermodynamic calculations,
the authors reported that at low and high dye concentrations
chemisorption was favored, while for mid-range concentra-
tions physisorption is favored. They attributed the adsorption
behavior to the presence of several possible adsorption centers
in the dye molecule.
Wang et al. reported on the inhibition effectiveness of
L-cysteine as a corrosion inhibitor for AA5052 alloy in 4 M
NaOH solution at 30 °C, using the HE, Tafel extrapolation,
and EIS techniques (Wang et al., 2016). The inhibition effec-
tiveness increased with increasing inhibitor concentration.
4652
The polarization measurements showed that L-cysteine acted
as a cathodic-type inhibitor. Based on the quantum chemical
calculations, the authors concluded that L-cysteine adsorbed
on the aluminum surface through the carboxyl groups. More-
over, they reported that strong hybridization occurred between
the s- and p-orbitals of L-cysteine and the sp-orbital of the alu-
minum atom.
Abd El-Rehim et al. tested polyoxyethylene (20) sorbitan
monooleate (Tween 80) as a corrosion inhibitor for A5754
aluminum alloy in 0.5 M NaOH solution at 25 °C, using
the PDP technique (Abd El-Rehim et al., 2016). The inhibi-
tion effectiveness increased with increasing compound con-
centration, but decreased with increasing temperature. The
PDP measurements showed that Tween 80 acted as a
mixed-type inhibitor. Based on the thermodynamic calcula-
tions, the authors suggested comprehensive adsorption (both
physisorption and chemisorption) of Tween 80 on the alloy
surface.
Kumari et al. (2011a) synthesized the compound 3-ethyl-4-
amino-mercapto-1,2,4-triazole and tested it as an inhibitor in
the corrosion of AA6061 aluminum alloy in 0.05–0.50 M
NaOH solutions at 30–50 °C, using the PDP and EIS tech-
niques. The inhibition effectiveness increased with increasing
compound concentration up to 50 ppm. At concentration val-
ues higher than 50 ppm the inhibition effectiveness decreased.
The authors reported a decrease in the inhibition effectiveness
with increasing temperature. The PDP measurements showed
that 3-ethyl-4-amino-mercapto-1,2,4-triazole acted as a
mixed-type inhibitor, predominantly inhibiting the cathodic
reaction.
Kumari et al. synthesized 3-methyl-4-amino-5-mercapto-1,
2,4-triazole (MAMT) and tested it as a corrosion inhibitor
for AA6061 aluminum alloy in 0.5 M NaOH solution at 30–
50 °C, using the PDP and EIS techniques (Kumari et al.,
2011b). The inhibition effectiveness increased with increasing
MAMT concentration, but decreased with increasing tempera-
ture. The PDP measurements revealed that this compound
acted as a mixed-type inhibitor, predominantly inhibiting the
cathodic reaction. Based on the thermodynamic calculations,
the authors concluded that MAMT physisorbed on the alu-
minum surface.
Abdallah et al. investigated the inhibitive behavior of gelatin
as a corrosion inhibitor for pure aluminum and two aluminum
alloys, i.e., AA6063 and AA20556 (92.47% aluminum), in
0.1 M NaOH solution at 30–60 °C, using the PSP, EIS and cyc-
lic voltammetry (CV) techniques (Abdallah et al., 2016b). The
inhibition effectiveness increased with increasing gelatin con-
centration, but decreased with increasing temperature and
increasing Si content in the alloys. The authors reported that
the inhibition effectiveness of gelatin decreased in the order
pure aluminum > AA6063 > AA20556. According to the
authors, this was due to the lower affinity of gelatin to adsorb
on silicon than on aluminum. They reported that gelatin pro-
tects aluminum and the aluminum-silicon alloys by forming a
barrier film on their surface. Within the same research group,
the same authors tested the corrosion of the same materials
(pure aluminum and two alloys) at the same NaOH concentra-
tion and temperature range in the presence of methyl cellulose
(Eid et al., 2015). The same conclusions were reported regard-
ing the change in inhibition effectiveness with changing inhibi-
tor concentration and temperature, as well as regarding the
same inhibition order reported for gelatin (Abdallah et al.,
K. Xhanari, M. Finšgar
2016b). The PDP measurements showed that methyl cellulose
acted as a mixed-type inhibitor.
Umoren et al. studied the synergistic effect of potassium
halides (KI, KCl, and KBr) and polyethylene glycol (PEG)
in the corrosion of aluminum in 1 M NaOH solution at 30
and 60 °C, using the WL and thermometric techniques
(Umoren et al., 2009). The inhibition effectiveness increased
with increasing PEG concentration and with increasing tem-
perature. The authors reported on the synergistic effect of
the potassium halides when added to PEG. KI in combination
with PEG provided the highest inhibition effectiveness com-
pared to KBr and KCl. The authors suggested chemisorption
as the possible adsorption mechanism for PEG.
Edrah and Hasan studied the inhibition effectiveness of
thiourea, phenyl thiourea, and 4-carboxy phenyl thiourea in
the corrosion of aluminum (the authors report this as commer-
cially available aluminum) in 0.3–1.0 M NaOH solutions at
21 °C, using the WL technique (Edrah and Hasan, 2010).
The authors concluded that these compounds significantly
reduce the corrosion of aluminum in NaOH solution. How-
ever, the highest inhibition effectiveness reported was 28.3%,
too low a value to support their conclusion. The data showed
that the inhibition effectiveness decreased with increasing
NaOH concentration. Phenyl thiourea was found to be the
best inhibitor in all the tested solutions, apart from the sample
immersed in 0.3 M NaOH solution. 4-carboxy phenyl thiourea
gave the highest inhibition effectiveness in 0.3 M NaOH solu-
tion. This compound protected the aluminum surface by form-
ing a film through adsorption.
Santhini and Jeyaraj synthesized the compound 3-(4-hydr
oxy-3-methoxy-phenyl)-1-(2-hydroxy-phenyl)-propenone
(HMPHPP) and tested it as an inhibitor in the corrosion of
aluminum (the authors reported this as commercially available
aluminum) in 0.1 N NaOH solution, at 30 and 50 °C, using the
WL, HE, and electrochemical techniques (Santhini and
Jeyaraj, 2012). The authors concluded that the inhibition effec-
tiveness increased with increasing HMPHPP concentration
and decreased with increasing temperature. The addition of
tetrabutyl ammonium bromide increased the inhibition effec-
tiveness of HMPHPP. The compound was found to be a
mixed-type inhibitor and physisorption was proposed as the
adsorption mechanism.
Beulah et al. synthesized 1-(4-hydroxyphenyl)-3-(2-hydroxy
phenyl)-propenone (HPHPP) and tested it as an inhibitor in
the corrosion of aluminum (the authors report this as commer-
cially available aluminum) in 1 M NaOH solution at 30 and
50 °C, using the WL, HE, and electrochemical techniques
(Beulah et al., 2012). The inhibition effectiveness of HPHPP
increased with increasing compound concentration and
decreased with increasing temperature. The electrochemical
measurements showed that this compound acted as a mixed-
type inhibitor. Thermodynamic calculations suggested that
HPHPP physisorbed on the aluminum surface.
3.1.2. Organic corrosion inhibitors in KOH solution
Shao et al. (2003) tested tartrate ion as a corrosion inhibitor for
pure aluminum (P99.9995%) in 4 M KOH solution at 25 °C,
using the HE and EIS techniques. The inhibition effectiveness
of the tartrate ion under these conditions was low (g = 23%),
but the authors reported a significant synergistic effect when
saturated Ca(OH)2 solution was added (g = 90%). However,
Organic corrosion inhibitors
they also showed that the Ca2+ ion in itself is a better inhibitor
(g = 86%) compared to the tartrate ion.
Mukherjee and Basumallick studied the inhibition effective-
ness of 2-propanol in the corrosion of 99.9% aluminum in 1 M
KOH solution at 25 °C, using the HE and PDP techniques
(Mukherjee and Basumallick, 1996). They reported that the
compound acted as a corrosion promoter (the alloy had a
higher corrosion rate compared to when immersed in non-
inhibited solution) at low concentrations (2–10 vol.%), while
at high concentrations (30–56 vol.%) the corrosion rate was
reduced. They explained this behavior in terms of a weakening
of the barrier-type inner oxide film on aluminum at low
concentrations of 2-propanol and a blocking effect at high
concentrations through interaction via the oxygen center of
the 2-propanol molecule.
Patil and Sharma studied the influence of 3-methylpyridine
and the synthesized 3-nitropyridine on the corrosion rate of
99.95% aluminum in 1 M KOH solution at 20 °C, using the
WL technique (Patil and Sharma, 2014). The inhibition effec-
tiveness of these compounds increased with increasing inhibi-
tor concentration and decreasing temperature. The authors
concluded also that 3-methylpyridine protected aluminum bet-
ter than 3-nitropyridine.
Oguzie studied the inhibition effectiveness of Crystal violet
dye as a corrosion inhibitor for AA1060 aluminum alloy
(98.8% aluminum) in aerated 0.5 M KOH solution at 30–
60 °C, using the WL technique (Oguzie, 2009). The inhibition
effectiveness increased with increasing dye concentration, but
decreased with increasing temperature. Based on the thermo-
dynamic calculations, the authors suggested physisorption as
the possible adsorption mechanism for Crystal violet dye. They
studied the inhibition effectiveness of Crystal violet dye for the
same alloy in 1 M HCl solution and found that this compound
protected the alloy better in HCl than in KOH solution. In
addition, the inhibition effectiveness of Crystal violet dye fur-
ther increased upon the addition of KI, but the increase was
more significant in 0.5 M KOH solution compared to the
1 M HCl solution.
Oguzie et al. used the WL technique at 30 and 60 °C to test
Congo Red dye (the sodium salt of benzidinediazo-bis-1-naph
thylamine-4-sulfonic acid) as an inhibitor in the corrosion of
AA1060 aluminum alloy in 2 M KOH solution (Oguzie
et al., 2005). The inhibition effectiveness increased with
increasing Congo Red dye concentration and decreased with
increasing temperature. The authors claimed that the addition
of potassium halides (KI, KBr, and KCl) increased the inhibi-
tion effectiveness in general due to the synergistic effect, which
is more pronounced at higher temperature. However, this is
not the case for KCl. The data showed that the inhibition
effectiveness slightly decreased with the addition of KCl to
Congo Red dye at 30 °C (from 31.72% to 29.15%). The oppo-
site behavior is seen at 60 °C. In the case of the addition of
KBr, there is only a slight increase in g at 30 °C (from
31.72% to 34.71%). However, the inhibition effectiveness val-
ues in general are too low, 31.72% at 30 °C and 19.32% at
60 °C when just Congo Red dye was added and 48.63% and
41.90% in the case of the further addition of KI.
3.1.3. Organic corrosion inhibitors in other alkaline solutions
Eduok et al. investigated the inhibition effectiveness of 4-(4-
nitrophenylazo)-1-naphthol (44NIN) as a corrosion inhibitor
4653
for 99.145% aluminum in a binary alkaline medium of
0.1 M NaOH and 0.1 M KOH solution at 30–60 °C, using
the WL technique (Eduok et al., 2013). The inhibition effec-
tiveness increased with increasing 44NIN concentration, but
decreased with increasing temperature. Based on the thermo-
dynamic calculations, the authors concluded that 44NIN phy-
sisorbed on the aluminum surface. They used UV–VIS
measurements to conclude that the inhibition effectiveness of
44NIN is probably due to the formation of an aluminum-
44NIN type complex that covered the metal’s surface.
Amin et al. studied the influence of three polyacrylic acids
(PAA) with different molecular weights (MW) on the corro-
sion inhibition of 99.99% aluminum in weakly alkaline solu-
tions of 0.217 M Na2CO3 containing 0.821 M NaHCO3 (pH
8 and 10) at 30 °C (Amin et al., 2009). The WL, electrochem-
ical (PDP, EIS, and electrochemical frequency modulation
(EFM)), and ex-situ EDX techniques were used. The PDP
measurements showed that these polymers acted as mixed-
type inhibitors. The inhibition effectiveness of these com-
pounds increased with increasing compound concentration,
molecular weight, and immersion time. Their inhibition effec-
tiveness is higher at pH = 8 compared to pH = 10.
Soliman evaluated the inhibition effectiveness of 8-
hydroxyquinoline (8-HQ) on the corrosion inhibition of
99.8% commercial aluminum and Al-HO411 alloys in 0.2 M
NaOH solution, using the WL technique (Soliman, 2011).
The inhibition effectiveness of both alloys increased with
increasing compound concentration up to a certain value
and then did not change (constant value). The corrosion rates
of Al-HO411 alloy are lower than those of the commercial
99.8% aluminum. The authors attributed that to the presence
of Mg2Si, Mg5Si6, SiO2, Al3Mn, and Cu3Ti phases in Al-
HO411 alloy. The adsorbed compound molecules and their
complexes showed a blocking effect on the sample surface
against the penetration of aggressive ions (OH). It has to
be pointed out that the authors used considerably high concen-
trations of the corrosion inhibitor. In fact, the highest inhibi-
tion effectiveness (g = 95%) was reported at 46 mM 8-HQ
in 0.2 M NaOH solution for the Al-HO411 alloy. Under the
same conditions (46 mM inhibitor in 0.2 M NaOH solution)
the 99.8% commercial aluminum was less protected
(g = 66%).
Kalaivani et al. investigated the inhibition effectiveness of
polymethacrylate (PMMA) as a corrosion inhibitor for 95%
aluminum in well water (pH = 11) using the WL, PDP, and
alternating current (AC) impedance techniques (Kalaivani
et al., 2013a). The inhibition effectiveness of PMMA increased
with increasing concentration. A further increase in the inhibi-
tion effectiveness was reported when 25 ppm Zn2+ was added
to solutions with concentrations up to 150 ppm PMMA, and
then stayed constant. Instead, when 50 ppm Zn2+ was added
the inhibition effectiveness decreased compared to the solution
containing only PMMA. However, the corrosion rates
reported are high (2.7–7.3 mdd). Based on the PDP measure-
ments, the authors concluded that PMMA acted as a mixed-
type inhibitor. The AC impedance measurements revealed that
PMMA protects aluminum by forming a protective film on its
surface. Based on the Fourier transform infrared spectroscopy
(FTIR) analysis, the authors concluded that this protective
film consisted of a PMMA-Zn2+ complex and Zn(OH)2. The
corrosion of 95% aluminum in well water (pH = 11) was
studied by the same authors also in the presence of
4654
carboxymethylcellulose as a corrosion inhibitor, using the WL
and AC impedance techniques (Kalaivani et al., 2013b). The
inhibition effectiveness of carboxymethylcellulose increased
with increasing concentration and was further enhanced by
the addition of Zn2+. The increase in the concentration of
Zn2+ (from 25 to 50 ppm) resulted in a lower increase in the
inhibition effectiveness. The authors reported a decrease in
the inhibition effectiveness with increasing immersion period,
from 1 to 7 days. However, the corrosion rates reported by
the authors are high (0.9–9.4 mm/y). Based on the AC impe-
dance measurements, they concluded that the inhibition action
of carboxymethylcellulose is due to the formation of a protec-
tive film on the aluminum surface.
3.2. Organic corrosion inhibitors in chloride solution
Sherif and Park evaluated the inhibition effectiveness of 1,4-
naphtoquinone (NQ) as a corrosion inhibitor of 99.99% alu-
minum in aerated and de-aerated 0.5 M NaCl solutions at
25 °C, using the PDP and EIS techniques (Sherif and Park,
2006). The inhibition effectiveness in both aerated and de-
aerated solutions increased with increasing NQ concentration.
The highest inhibition effectiveness was obtained for the addi-
tion of 1 mM NQ. The addition of the inhibitor shifted the
corrosion and breakdown potentials to more positive poten-
tials. The shifts are larger in de-aerated than aerated solution.
Based on the scanning electron microscope (SEM) images and
quartz crystal analyser measurements, the authors concluded
that NQ molecules strongly adsorb on the aluminum surface,
protecting it from further anodic dissolution. Sherif and Park
also investigated the ability of 1,5-naphthalenediol to protect
99.99% aluminum in 0.5 M NaCl solution, using different
electrochemical techniques (Sherif and Park, 2005). The inhibi-
tion effectiveness increased with increasing compound concen-
tration. The compound decreased both the cathodic and
anodic current, and consequently the corrosion current and
shifted the corrosion and breakdown potentials to more
positive potentials. The authors concluded that the 1,5-
naphthalenediol molecules are adsorbed on the aluminum sur-
face, covering up the preformed pits and protecting them from
further anodic dissolution. In addition, it was suggested that
the aluminum oxides/hydroxides are blocked by the corrosion
inhibitor from forming complexes with chloride ions. Sherif
reported on the effects of 3-amino-1,2,4-triazole-5-thiol
(ATAT) on the corrosion inhibition of 99.99% aluminum in
freely aerated stagnant 3.5 wt.% NaCl solution, using the cyc-
lic polarization (CP) and EIS techniques (Sherif, 2012). The
inhibition effectiveness increased with increasing concentration
of ATAT. The presence of this compound increased the polar-
ization resistance of aluminum in chloride solution. The catho-
dic and anodic corrosion and passive currents decreased upon
the addition of ATAT, while the corrosion and pitting poten-
tial were shifted to more negative potentials. According to the
authors, the ATAT molecules not only repaired the flawed
areas on the oxide film on the aluminum surface, but also pre-
vented the formation of the soluble aluminum chloride and
oxychloride complexes.
El-Shafei et al. reported on the use of indole, tryptamine
and tryptophane as corrosion inhibitors for pure aluminum
in 0.1 M NaCl solution, using the PDP technique (El-Shafei
et al., 2004). The authors reported that the inhibitive action
K. Xhanari, M. Finšgar
was dependent on the number of active centers in the corrosion
inhibitor molecule, molecular size, and the mode of adsorp-
tion. The inhibition effectiveness was found to increase with
increasing compound concentration and followed the order
indole < tryptophane < tryptamine.
Garrigues et al. studied the role of 8-HQ as a corrosion
inhibitor for aluminum with purity higher than 99% in neutral
(0.5 M NaCl) and acidic solutions (pH = 3), using the PDP
and EIS techniques (Garrigues et al., 1996). The authors
showed that the passive aluminum layer is strengthened, par-
ticularly for long immersion times, due to the formation of
an aluminum-chelate complex. They concluded that the
adsorption of 8-HQ prevented the adsorption of chloride ions
and the destruction of the oxide layer on the aluminum surface
in acidic solutions (pH = 3). The authors found that 8-HQ
does not modify the corrosion mechanism of aluminum, due
to the solubility of the aluminum chelate in acidic media.
Zor and Saǧdinç reported on the inhibition effectiveness of
sulfathiazole in the corrosion of 99.9% aluminum in 0.1 M
NaCl solution at 22–60 °C, using the PDP technique (Zor
and Saǧdinç, 2014). The inhibition effectiveness increased with
increasing inhibitor concentration. The PDP measurements
showed that sulfathiazole acted as a mixed-type inhibitor.
Based on the SEM analysis, the authors suggested that the cor-
rosion is inhibited by the formation of a protective layer on the
aluminum surface. Quantum chemical studies showed that this
adsorption occurs through the oxygen and nitrogen atoms.
The protonated form of sulfathiazole showed a considerable
tendency to adsorb on the metal surface. The authors reported
that the adsorption process has a mixed nature (physisorption
and chemisorption).
Solmaz et al. investigated the inhibition effectiveness of
citric acid as a corrosion inhibitor for 99.9% aluminum in
2 M NaCl (pH = 2) solution, using the PDP, polarization of
resistance (Rp), and EIS techniques (Solmaz et al., 2008).
The inhibition effectiveness increased with increasing citric
acid concentration up to 1  105 M of inhibitor added and
then decreased for higher concentrations. However, the results
presented showed a poor correlation between the g calculated
values from the PDP and EIS, on one hand, and Rp measure-
ments, on the other, especially at low concentrations of citric
acid. The lowest values reported, for the same concentration
of citric acid added, are 37.5% and 70.2%, from the PDP
and EIS measurements, respectively. The PDP measurements
showed that citric acid acted as a mixed-type inhibitor.
Jevremović and Misković-Stanković studied the inhibition
effectiveness of monoethanolamine (MEA) in the corrosion
of 99.7% aluminum in 3 wt.% NaCl solution saturated with
CO2 at 20 °C, using the EIS, linear sweep voltammetry
(LSV), and WL techniques (Jevremović and Stanković,
2012). The inhibition effectiveness of MEA increased with
increasing concentration up to 5 mM, and then decreased for
higher concentration values. The polarization measurements
showed that upon the addition of MEA a shift in the corrosion
potential toward more positive values occurred without a sig-
nificant change in the anodic and cathodic Tafel slopes. Based
on the thermodynamic calculations, the authors suggested that
MEA physisorbed on the aluminum surface.
Banerjee et al. tested phthalic acid, o-phenylenediamine, and
anthranilic acid as corrosion inhibitors for 99.15% aluminum
alloy in 0.6 M NaCl solution at 30 °C, using the PDP technique
(Banerjee et al., 2011). The authors reported that the inhibition
Organic corrosion inhibitors
effectiveness of all three compounds first increased with
increasing compound concentration and then at a certain con-
centration decreased. The inhibition effectiveness followed
the order phthalic acid < o-phenylenediamine < anthranilic.
However, this was true only for the optimum concentration
(4  105 M), but not for the lowest and highest concentration
values. The authors attributed the inhibition order of the com-
pounds to the existence of the NAO donor atom combinations
in the molecules.
Popoola et al. investigated the inhibition effectiveness of
ferrous gluconate as a corrosion inhibitor for 98.99% alu-
minum alloy in 0.05 M NaCl solution at 28 °C, using the
WL, Rp, and PDP techniques (Popoola et al., 2013). The inhi-
bition effectiveness of ferrous gluconate first increased with
increasing compound concentration, up to 1.0 g/mL, and then
decreased for higher concentrations. The PDP measurements
showed that ferrous gluconate acted as a mixed-type inhibitor.
Lakshmi et al. reported on the inhibition effectiveness of
diisopropyl thiourea (DISOTU) in the corrosion of 98.25%
aluminum in 3.5 wt.% NaCl solution, using the WL, HE,
PDP, and EIS techniques (Lakshmi et al., 2013). The inhibi-
tion effectiveness increased with increasing DISOTU concen-
tration. The PDP measurements showed that DISOTU acted
as a cathodic-type inhibitor.
Hakeem et al. studied the inhibition effectiveness of calcium
gluconate as a corrosion inhibitor for 95% aluminum in aque-
ous solution containing 60 ppm Cl (pH = 11) with and with-
out the addition of Zn2+, using the WL, PDP, and AC
impedance techniques (Hakeem et al., 2014). The inhibition
effectiveness increased with increasing calcium gluconate con-
centration. A further increase in the inhibition effectiveness
was observed upon the addition of Zn2+, as shown by the
WL measurements. However, there is a poor correlation
between the inhibition effectiveness values calculated with
the two electrochemical techniques under the same conditions
(the g calculated from PDP was 55% while the AC impedance
resulted in g = 25%). The authors attributed the inhibition
action of calcium gluconate to the formation of a protective
film on the aluminum surface consisting of Al3+-calcium glu-
conate complex and Zn(OH)2. The existence of this film was
confirmed by SEM and AFM analyses. The same was previ-
ously reported, which would suggest that this is the possible
mechanism involving organic corrosion inhibitors and Zn2+
(Kalaivani et al., 2013a).
Ho et al. investigated cerium dibutylphosphate (Ce(dbp)3)
as a corrosion inhibitor for AA2024-T3 aluminum alloy in
0.001 M NaCl solution, using the WL, PDP, and CV tech-
niques (Ho et al., 2006). The inhibition effectiveness increased
significantly with increasing exposure time and with increasing
compound concentration. The authors suggested that Ce
(dbp)3 is a better corrosion inhibitor for aluminum at higher
chloride concentrations due to easier deposition of the inhibit-
ing film when some corrosion has already taken place. Based
on the focused ion beam secondary-ion mass spectroscopy
analysis, the authors reported the presence of a 300–500 nm
thick cerium-containing layer on the aluminum surface after
10 days of immersion. Next, Ce(dbp)3 was also tested as corro-
sion inhibitor for AA2024-T3 in 0.05 M NaCl solution, using
the EIS and SEM- energy dispersive X-ray spectroscopy
(EDS) techniques (Garcia et al., 2013). The authors concluded
that the inhibition action of Ce(dbp)3 is due to the formation
of cerium oxide on Cu-rich areas, combined with the
4655
deposition of the dibutylphosphate on the surface. As a result,
a stable organic layer was formed that isolated the aluminum
surface from the Cl ions and enhanced the Ce deposition
on Cu-rich sites. In addition, Garcı́a et al. investigated the
influence of pH on the inhibition effectiveness of Ce(dbp)3 as
an inhibitor in the corrosion of AA2024-T3 aluminum alloy
in 0.1 M NaCl solution, using the PDP and high-throughput
(multielectrode) technique (Garcı́a et al., 2010). The inhibition
effectiveness of Ce(dbp)3 was studied as a function of pH, at
pH values 2, 4, 5.5, 7, 9, and 11. The solution’s pH was
adjusted by the addition of NaOH and HCl. The inhibition
effectiveness of Ce(dbp)3 at 104 M concentration is highly
affected by the pH of the solution. The authors reported the
highest anticorrosive properties in the neutral pH range (5.5–
7). According to them, both techniques presented similar
trends as regards protection throughout nearly the full pH
range. However, it is clear from the data that there is a poor
correlation between the protection efficiencies calculated from
the two techniques. This is true for the whole pH range stud-
ied. In two cases (pH = 2 and 9) the two techniques yield dif-
ferent conclusions as regards the performance of the inhibitor
(one suggested protection and the other the acceleration of
corrosion). The authors attribute these changes to solution
changes due to speciation and precipitation in solution rather
than to the multielectrode setup. Moreover, the highest inhibi-
tion effectiveness values are not obtained only for the neutral
range (pH = 5.5–7), as claimed by the authors. The inhibition
value at pH = 9 is high as well (g = 88.22% as reported from
the PDP measurements). Moreover, in our opinion, the addi-
tion of HCl is not the best way to adjust pH as one introduces
additional source of chlorides in the solution that additionally
increases the corrosion rate. This will lead to an overestimation
of the pH influence on the corrosion rate.
Lamaka et al. studied the inhibition effectiveness of eleven
organic compounds, i.e., salicylaldoxime (SAL), 2-
mercaptobenzothiazole, 8-HQ, thioacetamide, quinaldic acid,
a-benzoionoxime, 2-(2-hydroxyphenyl) benzoxazole, dithioox-
amide, cuprizone, and cupferron, in the corrosion of AA 2024-
T3 aluminum alloy in 0.05 M NaCl solution (Lamaka et al.,
2007). The highest inhibition effectiveness was achieved for sal-
icylaldoxime, 8-HQ, and quinaldic acid. The authors attribu-
ted the inhibition effect to the passivation of active
intermetallic zones, as well as to the formation of a chelate
layer on the alloy surface. According to the authors, the
chemisorption and precipitation of complexes occur on the
alloy surface, including active S-phases (these are intermetallic
zones, present in about 60% of all intermetallic inclusions, and
are composed of Al2MgCu). They showed that these com-
pounds acted as mixed-type inhibitors. On the other hand,
Snihirova et al. (2015) also studied the inhibition effectiveness
of 8-HQ, SAL and 2,5-dimercapto-1,3,4-thiadiazolate
(DMTD) and the combinations of these compounds as well
as with Ce3+, as corrosion inhibitors for AA2024-T3 alu-
minum alloy in 0.05 M NaCl solution, using the EIS tech-
nique. Based on attenuated total reflectance FTIR
Kretschman spectroscopy the authors concluded that 8-HQ
and SAL adsorb on the aluminum surface forming a thin film.
In case of DMTD the SEM-EDS analysis showed formation of
precipitates or adsorbates on the Cu-rich intermetallic particles
of the alloy. The inhibition effectiveness of these compounds
increased when combined. Based on the EIS measurements
the authors reported that for short immersion times the highest
4656
inhibition effectiveness was observed for the SAL-8-HQ mix-
ture. The mixture Ce-SAL performed better at long immersion
times.
Zheludkevich et al. investigated the inhibition effectiveness
of four triazole and thiazole derivatives, i.e., 1,2,4-triazole
(TA), 3-amino-1,2,4-triazole (ATA), benzotriazole (BTA),
and 2-mercaptobenzothiazole (2-MBT), in the corrosion of
AA 2024 alloy in neutral chloride solutions (0.05 M NaCl),
using the direct current (DC) polarization and EIS techniques
(Zheludkevich et al., 2005). The data showed that 2-MBT and
BTA are the most effective inhibitors for long-term protection
of the 2024 aluminum alloy under these conditions. As a result
of the usage of 2-MBT precipitation, a deposit occurs on the
copper-rich particles, reducing the anodic and cathodic reac-
tions of the corrosion couple.
Hu et al. synthesized cerium tartrate and tested it as a cor-
rosion inhibitor for AA2024-T3 aluminum alloy in 0.05 M
NaCl solution (Hu et al., 2015). The authors reported that this
compound affected both anodic and cathodic corrosion pro-
cesses, rapidly forming a protective film on the alloy surface.
Surface characterization revealed that this protective film
inhibited the dealloying of the Al2CuMg phase in the initial
stage and then cerium ions transformed into cerium oxide/
hydroxides and appeared at the Al2CuMg phase, blocking fur-
ther corrosion at those corrosion sites.
Shi et al. synthesized cerium cinnamate and tested it as an
inhibitor in the corrosion of AA2024-T3 aluminum alloy in
0.05 M NaCl solution, using electrochemical and surface ana-
lytical techniques (Shi et al., 2011). The authors reported that
this compound significantly inhibits corrosion during the ini-
tial 72 h of immersion and that it acts as an anodic-type inhi-
bitor. However, the PDP measurements showed that this
ability became less effective after 168 h of immersion. The elec-
trochemical techniques (PDP and EIS) indicated a change
from anodic inhibition through film deposition, to mixed-
type inhibition by the cinnamate group and cerium ions. The
XPS measurements showed that the carboxylic group in the
cinnamate bonded with the Al matrix, while Ce3+ transformed
into cerium oxide/hydroxide with valences of Ce(III) and Ce
(IV). The PDP measurements showed that cerium cinnamate
acted as a mixed-type inhibitor retarding the onset of corro-
sion from the second phase particles and surrounding Al
matrix.
Markley et al. tested cerium diphenyl phosphate (Ce(dpp)3)
and mischmetal diphenyl phosphate (Mm(dpp)3) as inhibitors
in the corrosion of AA2024 aluminum alloy in 0.1 M NaCl
solution, using the CP technique (Markley et al., 2007). Ce
(dpp)3 inhibited the cathodic reaction, while Mm(dpp)3 acted
as a mixed-type inhibitor. Mm(dpp)3 gave higher inhibition
effectiveness under the studied conditions (after 30 min and
24 h of immersion) compared to Ce(dpp)3. The authors
employed Raman mapping and confirmed the presence of
the inhibitors on the alloy surface.
Catubig et al. investigated the inhibition effectiveness of
cerium mercaptoacetate (Ce(Macet)3) and praseodymium mer-
captoacetate (Pr(Macet)3) as corrosion inhibitors for AA2024-
T3 aluminum alloy in 0.1 M NaCl solution (pH = 6), using
the PDP and SEM techniques (Catubig et al., 2014). Based
on the PDP measurements, the authors reported that the
increase in concentration of these compounds led to the dom-
inance of the inhibition of the cathodic reaction, while inhibi-
tion of the anodic reaction dominated with increasing
K. Xhanari, M. Finšgar
immersion time. They concluded that Pr(Macet)3 is a better
inhibitor than Ce(Macet)3.
Zhou et al. studied the inhibition effectiveness of a mixture
of sodium dodecylbenzenesulfonate (SDBS) and lanthanum
chloride in the corrosion of AA2024-T3 in 0.58 g/L NaCl solu-
tion (pH = 10), using the electrochemical and surface analysis
methods (Zhou et al., 2015). The authors reported a reduction
in the corrosion current density with increasing SDBS concen-
tration. The inhibition effectiveness of the two compounds
after 24 h was lower than that of their mixture; therefore, no
synergistic effect was observed. According to the authors, in
the earlier stage the DBS (an ion from SDBS) adsorbed on
the aluminum alloy surface, promoting Al dissolution by the
formation of Al(OH)3, which induces passivation. On the
other hand, the oxides or hydroxides of lanthanum and La
(DBS)3 deposited on the surface, forming a layer that mitigates
corrosion. The passive layer was damaged with time due to the
formation of pits around the Cu-rich phases from the galvanic
effect between the inclusion and the aluminum substrate.
Balaskas et al. evaluated the performance of 2-MBT, BTA,
and 8-HQ as corrosion inhibitors for AA2024-T3 aluminum
alloy in 3.5 wt.% NaCl solution, using the EIS, PDP, and
image-assisted electrochemical noise techniques (Balaskas
et al., 2015). However, from the experimental data it can be
noticed that there is a poor correlation between the data
obtained with the different techniques. PDP showed that only
2-MBT significantly decreased both the anodic and cathodic
reaction rates. 2-MBT protected the second phase particles,
preventing dealloying, trenching, and the initiation of corro-
sion. BTA retarded only the anodic reaction. By comparing
PDP curves for the 8-HQ-inhibited and non-inhibited solu-
tions, a similar behavior was observed. On the other hand,
8-HQ was previously studied as a corrosion inhibitor for
AA2024 aluminum alloy, but in lower concentrations of the
corrosive media (0.05 M NaCl) by Lamaka et al. (2007). They
found that saturated 8-HQ is an effective inhibitor and that it
decreased the corrosion rates of both the anodic and cathodic
reactions. In addition, Li et al. reported on the corrosion
behavior of AA2024-T3 aluminum alloy in 3.5 wt.% NaCl
solution in the presence of 8-HQ and 8-hydroxy-quinoline-5-
sulfonic acid (HQS), using the PDP and EIS techniques (Li
et al., 2007). The PDP measurements showed that 8-HQ acted
as a mixed-type inhibitor by blocking the active sites of the
metal surface, while HQS promoted corrosion by activating
the cathodic reaction. The authors reported that 8-HQ
absorbed on the metal surface, leading to the formation of a
protective layer. They concluded that the inhibition action of
8-HQ is due to the insoluble aluminum-chelate Al(HQ)3, which
prevents the adsorption of the chloride ion. According to the
authors, HQS breaks down the oxide film.
Li et al. studied the efficiency of tryptophan as an inhibitor
in the corrosion of AA2024 aluminum alloy in 3.5 wt.% NaCl
and 20 wt.% CaCl2 solutions using the WL, polarization, and
EIS techniques (Li et al., 2011). The inhibition effectiveness
increased with increasing tryptophan concentration. The com-
pound acted as an anodic inhibitor in both 20 wt.% CaCl2 and
3.5 wt.% NaCl solutions. Based on the quantum chemical cal-
culations, the authors reported that interactions between the
metal surface and tryptophan occur mainly over the indole
ring plane.
Balbo et al. evaluated the inhibition effectiveness of four
anionic surfactants, i.e., sodium salts of N–lauroylsarcosine
Organic corrosion inhibitors
(NLS), N–lauroyl–N–methyltaurine (NLT), dodecybenzensul-
fonic acid (DBS), and sodium lauryl sulfate (LS), in the
corrosion of AA2198 aluminum alloy in 0.01 M NaCl solu-
tions, 1–168 h of immersion at 25 °C, using the PDP, LSV,
and EIS techniques (Balbo et al., 2013). These surfactants
affected both the cathodic and anodic corrosion reactions,
shifting the breakdown potential to more positive potentials.
NLS and DBS were the most efficient inhibitors. The addition
of these surfactants rendered the natural aluminum passive
layer hydrophobic. The Al-surfactant salt precipitation
plugged the pores in the passive layer, further increasing in this
manner the inhibition effectiveness.
Shahrabi et al. tested 2-butine-1,4-diol and potassium
sodium tartrate as corrosion inhibitors for AA3003 aluminum
alloy in 0.5 wt.% NaCl solution at room temperature, using
the PDP and EIS techniques (Shahrabi et al., 2008). The inhi-
bition effectiveness of both compounds increased with increas-
ing compound concentration. The Tafel curve measurements
indicated that these compounds acted as mixed-type inhibitors.
Thermodynamic calculations showed that these compounds
physisorbed on the aluminum surface. The inhibition effective-
ness increased further when the two compounds were com-
bined. The authors reported that the optimum concentration
ratio of potassium sodium tartrate to 2-butine-1,4-diol is 2:1.
Yazdzad et al. studied the inhibition effectiveness of
propargyl alcohol and potassium sodium tartrate, as well as
their mixture in the corrosion of AA3003 aluminum alloy in
0.5 wt.% NaCl solution, using the Tafel extrapolation and
EIS techniques (Yazdzad et al., 2008). The inhibition effective-
ness increased with increasing compound concentration. Both
inhibitors showed optimum protection at concentrations of 1–
1.5 mM when used separately. The inhibition effectiveness of
potassium sodium tartrate was previously investigated by the
same group (Shahrabi et al., 2008) and the values presented
here are in accordance with those. The polarization measure-
ments showed that these compounds acted as mixed-type inhi-
bitors. Thermodynamic calculations indicated that both
compounds physisorbed on the aluminum surface. When com-
bined together, a synergistic effect was observed, resulting in
higher inhibition effectiveness. The authors reported that the
optimum concentration ratio of potassium sodium tartrate to
propargyl alcohol is 5:2.
Wang et al. reported on the use of 8-aminoquinoline (8-
AQ) and 8-nitroquinoline (8-NQ) as effective corrosion inhibi-
tors for AA5052 aluminum alloy in 3 wt.% NaCl solution,
using the WL and electrochemical techniques (Wang et al.,
2015). 8-NQ was found to be a better inhibitor for the alloy
compared to the 8-AQ. The authors concluded that both inhi-
bitors form a protective film on the alloy surface, retarding the
anodic reaction. Based on density functional theory calcula-
tion it was reported that a strong hybridization occurs between
the p-orbital of reactive sites in the inhibitor molecules and the
sp-orbital of the Al atom.
Hill et al. reported on the corrosion resistance of 7000 series
aluminum alloys, i.e., AA7022, AA7050, and AA7075, in
0.1 M NaCl solution in the presence of ceryl diphenyl phos-
phate, using the EIS technique (Hill et al., 2011). There is no
significant change in the inhibition effectiveness values calcu-
lated from the EIS measurements taken at 30 min, 3 days,
and 6 days. The inhibition effectiveness for the same concen-
tration of ceryl diphenyl phosphate slightly increased in the
order AA7075 > AA7022 > AA7050. ToF-SIMS data
4657
indicated the presence of a complex Ce/Al organophosphate
film, not necessarily homogeneous on the surface. The authors
proposed that this film consisted of hydrolysis products of the
inhibitor and aluminum oxide.
Liu et al. tested 8-HQ as a corrosion inhibitor for AA7075
aluminum alloy in 3.5 wt.% NaCl solution, using the EIS and
PDP techniques. 8-HQ was tested in aqueous 3.5 wt.% NaCl
and ethanol 3.5 wt.% NaCl solutions (Liu et al., 2014). The
inhibition effectiveness increased with increasing compound
concentration. However, it has to be noted that there is a poor
correlation between the data obtained from the two different
techniques, especially for lower concentrations. Based on the
PDP measurements, the authors concluded that 8-HQ inhib-
ited the corrosion process by reducing the rate of the anodic
and cathodic reactions on the alloy surface. This is in agree-
ment with what was found when 8-HQ was used as a corrosion
inhibitor for AA2024 alloy in 0.05 M NaCl and in 3.5 wt.%
NaCl solutions (Lamaka et al., 2007; Li et al., 2007).
Yurt et al. performed quantum chemical studies on the
inhibition effectiveness of six amino acids, i.e., glycine, aspartic
acid, valine, alanine, phenylalanine, and glutamic acid at
pH = 5, and six hydroxy carboxylic acids, i.e., glucolic acid,
malic acid, lactic acid, mandelic acid, benzylic acid, and citric
acid at pH = 8, in the corrosion of AA7075 aluminum alloy in
0.05 M NaCl solution (Yurt et al., 2005). The authors con-
cluded that both physisorption and chemisorption played an
important role in the inhibition of pitting corrosion.
Qafsaoui et al. investigated the role of 1-pyrrolidine dithio-
carbamate (PDTC) as a corrosion inhibitor for pure aluminum
and AA2024-T3 aluminum alloy in 0.2 g/L NaCl solution,
using the WL and electrochemical techniques (Qafsaoui
et al., 2015). They concluded that PDTC has only a small influ-
ence on the corrosion of pure aluminum, but strongly inhibited
the alloy corrosion. According to the authors, this is due to the
presence of copper-rich particles in the alloy. PDTC increased
the galvanic coupling resistance through strong interaction
with the Cu-rich cathodic sites associated with the inter-
metallics through its sulfur atoms. The active cathodic surface
sites are reduced as a result of a stable and adherent Cu(I)-
PDTC complex formed by the interaction between PDTC
and these particles. SEM-EDX analysis showed that PDTC
adsorbed preferentially on the Al-Cu-Mg particles.
Vrsalović et al. reported on the inhibition effectiveness of
sinapinic acid as a corrosion inhibitor for Al-2.5 Mg (97.5%
aluminum) alloy in 0.5 M NaCl solution, using a rotating disk
electrode at 20–50 °C and the PDP, Rp, and EIS techniques
(Vrsalovic et al., 2007). The inhibition effectiveness increased
with increasing concentration of sinapinic acid, but decreased
with increasing temperature. The PDP measurements showed
that this compound acted as a cathodic-type inhibitor. Based
on the EIS measurements, the authors concluded that a thicker
protective film formed on the aluminum surface as a result of
the sinapinic acid adsorption. Physisorption was the proposed
adsorption mechanism for this compound. Vrsalović et al.
investigated two phenolic acids, i.e., sinapinic and gentisic
acid, as corrosion inhibitors for Al-0.8 Mg aluminum alloy
(98.9% aluminum) in 0.5 M NaCl solution at 20 °C, using
the PDP, Rp, and EIS techniques and a rotating disk electrode
(Vrsalović et al., 2009). The inhibition effectiveness increased
with increasing acid concentration, but decreased with increas-
ing electrode rotation rate. Sinapinic acid was found to be a
better inhibitor than gentisic acid under the same conditions.
4658
The PDP measurements showed that both phenolic acids acted
as cathodic-type inhibitors. The authors explained the inhibi-
tion action of these acids with the formation of complex mole-
cules with aluminum ions, which protected the metal through
deposition in places where the oxide film was destroyed. They
proposed physisorption as the possible adsorption mechanism
for both acids. The same conclusions were previously reported
for the corrosion inhibition of Al-2.5 Mg (97.5% aluminum) in
0.5 M NaCl solution by sinapinic acid using a rotating disk
electrode (Vrsalovic et al., 2007).
Önal and Aksüt studied the inhibition effectiveness of tolyl-
triazole (TTA) as a corrosion inhibitor for four aluminum
alloys, i.e., Al-8%Si-3%Cu, Al-4%Cu, Al-12%Cu, and Al-
22%Cu-4%Fe, in 1 M NaCl solution (pH = 6 and 11), at
15–35 °C, using the PDP and Rp techniques (Önal and
Aksüt, 2000). The inhibition effectiveness increased with
increasing TTA concentration, but decreased with increasing
temperature and pH. The authors tested TTA in 1 M HCl
solution (pH = 0.5) as well, in which TTA performed better
than in solutions at pH 6 and 11. Moreover, it was shown that
TTA is a more effective inhibitor at pH = 6 than at pH = 11.
The PDP measurements showed that TTA acted as a mixed-
type inhibitor in all solutions. The authors concluded that
the inhibition effect of TTA is due to its adsorption on Cu par-
ticles and the formation of a Cu(I)-TTA film. They suggested
that this film is formed from the interaction of CuCl 2 complex

with TTA (TTAH+ 2 , TTAH or TTA form).
Harvey et al. reported on the inhibition effectiveness of Na-
mercaptopropionic acid, BTA, Na-(diethyl(dithiocarbamate)),
Na-4-mercaptobenzoate, Na-(6-mercaptonicotinate), Na-
mercaptoacetic acid, 2-mercaptobenzothiazole, thiophenol,
2-mercaptobenzimidazole, 2-mercaptopyrimidine, 6-amino-2-
mercaptobenzothiazole, and Na-2-mercaptobenzoate as corro-
sion inhibitors for AA2024 aluminum alloy in 0.1 M NaCl at
21 °C, using the WL technique (Harvey et al., 2011). The same
technique was used to study the corrosion resistance of
AA7075 aluminum alloy in 0.1 M NaCl solution in the
presence of Na-(diethyl(dithiocarbamate)), 6-amino-2-
mercaptobenzothiazole, BTA, 2-mercaptobenzothiazole,
Na-(6-mercaptonicotinate), 2-mercaptobenzimidazole, 4,5-
diaminopyrimidine, Na-mercaptoacetic acid, 4,5-diamino-2,
6-dimercaptopyrimidine, Na-2-mercaptobenzoate, Na-4-
mercaptobenzoate, and Na-2-mercaptonicotinate. The authors
reported that the corrosion of AA2024 aluminum alloy was
promoted and not inhibited in the presence of pyrimidine,
Na-benzoate, pyridine, Na-(4-phenylbenzoate), Na-4-
hydroxybenzoate, Na-nicotinate, Na-isonicotinate, Na-
salicylate, and Na-acetate. In the case of AA7075 aluminum
alloy, corrosion was promoted by pyrimidine, Na-benzoate,
pyridine, Na-(4-phenylbenzoate), Na4hydroxybenzoate, Nani-
cotinate, Na-isonicotinate, Na-3-mercaptobenzoate, Na-
salicylate, and 2,5-dimercapto-1,3,4-thiadiazole. It was found
that several functional groups or the presence of certain atoms
significantly improved the corrosion inhibition ability of the
corrosion inhibitor. According to the authors, the presence
of a thiol group, para- and ortho-positions of carboxylate on
a monoaromatic ring, and the substitution of N for C in an
aromatic ring where it may form a coordinating site with the
carbonyl or nitrogen, play an important role therein. They
concluded that the presence of a hydroxyl group in the corro-
sion inhibitor structure was slightly inhibitive, while the car-
boxylate group provided little or no corrosion inhibition on
K. Xhanari, M. Finšgar
its own. Thiol-containing compounds were more effective on
AA2024 alloy than on AA7075 alloy, and the authors attribu-
ted that to the higher amount of Cu in the former. Two
compounds, i.e., 6-amino-2-mercaptobenzothiazole and 4,5-d
iamino-2,6-dimercaptopyrimidine, show good corrosion inhi-
bition for both alloys at lower concentration (approx. 0.1
and 0.5 mM, respectively, according to their maximum solubil-
ity). Compounds having the (HSAC‚S) group were also
found to be very effective corrosion inhibitors.
Qafsaoui et al. studied the inhibition effectiveness of BTA
in the corrosion of 99.999% aluminum and AA2024-T3 alu-
minum alloy in a 0.1 M Na2SO4 + (0.001–0.5) M NaCl mix-
ture, using the electrochemical noise technique (Qafsaoui
et al., 2009). The authors reported that at high chloride con-
centrations (0.5 M NaCl) the addition of BTA inhibited uni-
form corrosion, resulting in a decrease in the amplitude of
the potential and current fluctuations. Moreover, SEM analy-
sis confirmed that neither the Al matrix nor the Cu-rich parti-
cles were attacked. The authors attributed the inhibition effect
of BTA to its ability to form a polymeric film with Cu(I),
which hinders the oxygen reduction reaction. However, BTA
was unable to prevent 99.999% aluminum corrosion. At low
chloride concentrations (0.001 and 0.1 M NaCl), the authors
reported that BTA protected the AA2024 aluminum alloy
from pitting corrosion, even after one week of immersion
(lower potential and current fluctuations were observed in
the inhibited solutions).
Rodič and Milošev tested cerium(III) acetate as a corrosion
inhibitor for 99% aluminum and AA2024-T3 and AA7075-T6
alloys in 0.1 M NaCl solution at 25 °C, using the PDP tech-
nique (Rodič and Milošev, 2016). The authors attributed the
inhibitory action of this compound to the type of substrate
and the type and concentration of the anion. The inhibition
effectiveness was found to decrease with increasing Ce(Ac)3
concentration (from 1 to 4 mM, in the case of 99% aluminum,
and from 1 to 5 mM, in the case of the AA7075-T6 aluminum
alloy). The authors also tested two other inorganic cerium(III)
salts, i.e., cerium(III) nitrate and chloride. They reported that
Ce(Ac)3 was the most effective inhibitor for all three materials
studied. The authors also showed that the corrosion inhibition
effectiveness of Ce(Ac)3 followed the order AA7075-
T6 > 99% Al > AA2024-T3. The changes in pH with the
addition of Ce(Ac)3 not only affect the stability of the inter-
metallic particles, but also that of the surrounding aluminum
oxide matrix.
Sherif studied the corrosion of 99.99% aluminum in aer-
ated Arabian Gulf Seawater (AGS) and 3.5 wt.% NaCl solu-
tion in the presence of 3-amino-5-mercapto-1,2,4-triazole
(AMTA), using the CP and EIS techniques (Sherif, 2011).
The measurements showed that AGS is more corrosive than
the 3.5 wt.% NaCl solution. However, AMTA protects alu-
minum better in AGS than in 3.5 wt.% NaCl solution. The
inhibition effectiveness increased with increasing AMTA con-
centration. The corrosion and pitting potentials of aluminum
were shifted toward less negative values when AMTA is added
to the corrosion environment. The compound reduced the cor-
rosion rate by preventing the formation of soluble chloride and
oxychloride complexes on the aluminum surface.
Marcelin and Pébère showed that 8-HQ and BTA are two
effective corrosion inhibitors for AA2024 aluminum alloy in
a mixture of 0.1 M Na2SO4 + 0.05 M NaCl (Marcelin and
Pébère, 2015). The mixture of these two inhibitors showed a
Organic corrosion inhibitors
synergistic effect, with BTA acting mainly on the Cu-rich inter-
metallic particles, while 8-HQ acted on the aluminum matrix
due to the chelating properties. The galvanic coupling between
the aluminum matrix and the intermetallic particles is strongly
limited when the inhibitor mixture is used compared to the
inhibitors used separately.
Boisier et al. tested sodium decanoate as a corrosion inhibi-
tor for AA2024 aluminum alloy in a mixture of 0.1 M Na2-
SO4 + NaCl at pH values of 4, 6, 8, and 10, using different
electrochemical techniques (Boisier et al., 2010). This com-
pound formed a hydrophobic layer on the aluminum surface
(as shown from the high contact angle values at pH = 6 solu-
tion), preventing the attack on the passive layer by the chloride
ions. Moreover, the addition of sodium decanoate limited the
galvanic coupling between the intermetallic particles and the
surrounding matrix. The EIS data showed that at pH 6 and
8, the pH range where the alloy was in the passive state, the
inhibitor efficiency was constant and higher than for the lowest
(pH = 4) and highest (pH = 10) pH values.
Sherif investigated the corrosion resistance of 99.99% alu-
minum in naturally aerated stagnant Arabian Gulf seawater
with and without the addition of 3-amino-1,2,4-triazole-5-
thiol (ATAT), using the EIS, CP, and potentiostatic current-
time techniques (Sherif, 2013). The authors reported an
increase in both the solution and polarization resistances, as
well as a shift in the corrosion and pitting potentials to more
negative potentials when ATAT was added, indicating a
decrease in the uniform corrosion rate. These findings are in
accordance with what was reported previously when the same
compound (ATAT) was studied in the corrosion of 99.99%
aluminum in 3.5 wt.% NaCl solution (Sherif, 2012). The inhi-
bition effectiveness increased with increasing ATAT concen-
tration. There is a good correlation between the inhibition
effectiveness reported by the author in aerated stagnant Ara-
bian Gulf seawater (Sherif, 2013) and in aerated stagnant
3.5 wt.% NaCl solution (Sherif, 2012), for the same aluminum
sample (99.99% Al) and the same ATAT concentrations used
(1 mM and 5 mM). The authors concluded that the ATAT
molecules adsorbed on the aluminum surface, increasing in
this manner the stability of aluminum oxide.
Rosliza et al. (2008) studied the corrosion of AA6061 alu-
minum alloy in tropical seawater (no composition given) in
the presence of sodium benzoate (SB), in static and air circula-
tion conditions, using the PDP, EIS, and SEM techniques. SB
acts as a cathodic-type inhibitor and no change occurred in the
corrosion process due to an increase in either the immersion
time or the inhibitor concentration. Under static conditions,
the highest inhibition effectiveness was achieved after 180 days
of exposure to the corrosive environment, while under air cir-
culation conditions, after 60 days. The EIS measurements
showed that the corrosion process was mainly kinetically-
controlled. The charge transfer resistance increased with the
addition of the inhibitor, while the capacitance decreased, indi-
cating the formation of a surface film.
Rosliza et al. reported on the effect of vanillin on the cor-
rosion inhibition of AA6061 aluminum alloy in seawater at
25 °C, using the PDP, Rp, and EIS techniques (Rosliza et al.,
2010). The inhibition effectiveness increased with increasing
compound concentration. The PDP measurements showed
that vanillin acted as a mixed-type inhibitor. The EIS measure-
ments showed that the corrosion process in the presence of
vanillin was mainly kinetically-controlled, without changing
4659
the corrosion mechanism compared to the non-inhibited solu-
tions. The authors concluded that vanillin reduced the overall
corrosion rates by the formation of a thin film of precipitate on
the aluminum surface.
Wan Nik et al. studied the corrosion of AA6063 aluminum
alloy in seawater (no composition given) at room temperature
in the presence of SB, using the WL, PDP, and EIS techniques
(Wan Nik et al., 2013). The authors concluded that the inhibi-
tion effectiveness of SB decreased with increasing immersion
time (30–180 days). However this was valid only up to
120 days of immersion. After 120 days the inhibitor efficiency
increased again (to values close to those of 30 days) and then
decreased again after 180 days. PDP data showed that SB
acted as a cathodic-type inhibitor. The authors concluded that
the corrosion process was mainly kinetically-controlled and no
change in the corrosion mechanism occurred due to either the
immersion time or the addition of inhibitor.
Zor and Özkazanç tested benzamide (BA), 4-
aminobenzenesulfonamide (ABSA), and thioacetamide
(TAA) as inhibitors in the corrosion of aluminum in 0.1 M
NaCl solution, using the PDP and EIS techniques (Zor and
Özkazanç, 2010). The inhibition effectiveness increased with
increasing compound concentration and followed the order
TAA > ABSA > BA. The EIS measurements showed that
the charge transfer resistance increased with increasing inhibi-
tor concentration, while the double layer capacitance
decreased. The authors reported that these compounds
adsorbed on the aluminum surface, forming a protective layer.
Ren et al. reported on the inhibition effectiveness of triiso-
propanolamine (TIPA) as a corrosion inhibitor for ADC12
aluminum alloy (no composition given) in 3 wt.% NaCl solu-
tion, at 25 °C, using the WL, PDP, and EIS techniques (Ren
et al., 2015). The inhibition effectiveness increased with
increasing TIPA concentration. The PDP measurements
showed that TIPA acted as a mixed-type inhibitor. Based on
the thermodynamic and kinetic parameters calculations, the
authors suggested a mixed-type (both physisorption and
chemisorption) adsorption mechanism for TIPA. The authors
used quantum chemical calculations to conclude that TIPA
adsorbed on the aluminum surface through the oxygen atom.
4. Conclusions
In this review we present the latest developments in the field of organic
corrosion inhibitors for aluminum and its alloys in various alkaline
(mainly KOH and NaOH) and chloride-based solutions.
As seen in this review, the most widely employed compounds were
azole derivatives, mercapto compounds, quinolines (especially 8-
hydroxyquinoline), organic dyes, and polymers. The materials studied
in inhibited alkaline solutions were mainly pure aluminum, and series
1xxx and 6xxx alloys. On the other hand, in chloride solutions, the inhi-
bition of the corrosion of pure aluminum, series 2xxx and 7xxx alloys,
was primarily investigated. The highest temperature tested was 70 °C
for the alkaline solutions and 60 °C for the chloride solutions. In most
of the publications, the concentration of the corrosive environment var-
ied from 1 mM up to 4 M concentration of the alkaline solutions, while
NaCl solutions with concentrations from 1 mM to 2 M were tested. In
the case of chloride solutions, the pH of the corrosive environment
was found to vary from 0.5 to 11. The pH of the alkaline solutions
was reported only in a few cases. Weight loss and several electrochemical
techniques, including polarization resistance, potentiodynamic, poten-
tiostatic, and galvanostatic polarization, and electrochemical impe-
dance spectroscopy, were most frequently used to evaluate the
corrosion inhibition effectiveness of the studied compounds.
4660
The inhibition effectiveness usually increased with increasing inhi-
bitor concentration and decreased with increasing temperature. Differ-
ent authors also reported that synergistic effect can be achieved with
the addition of cations, such as Zn2+, Mg2+, Ca2+, Sr2+, and
Ba2+, besides the conventional halides (chloride, bromide, and espe-
cially iodide). The inhibition mechanism was usually attributed to
the formation of a surface layer or a film formed after the adsorption
of compounds on the aluminum surface. Moreover, several authors
reported that this film it consists of Al3+ - inhibitor complexes.
Acknowledgments
This work was supported by the Slovene Research Agency
(Grant No. Z1-6737).
Appendix A. Supplementary material
Supplementary data associated with this article can be found,
in the online version, at http://dx.doi.org/10.1016/j.arabjc.
2016.08.009.
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