Accepted Manuscript

An overview on plant extracts as environmental sustainable and

green corrosion inhibitors for metals and alloys in aggressive
corrosive media

Chandrabhan Verma, Eno E. Ebenso, Indra Bahadur, M.A.

Quraishi

PII: S0167-7322(18)31417-X
DOI: doi:10.1016/j.molliq.2018.06.110
Reference: MOLLIQ 9308
To appear in: Journal of Molecular Liquids
Received date: 17 March 2018
Revised date: 11 June 2018
Accepted date: 26 June 2018

Please cite this article as: Chandrabhan Verma, Eno E. Ebenso, Indra Bahadur, M.A.
Quraishi , An overview on plant extracts as environmental sustainable and green corrosion
inhibitors for metals and alloys in aggressive corrosive media. Molliq (2018), doi:10.1016/
j.molliq.2018.06.110

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 ACCEPTED MANUSCRIPT

An overview on plant extracts as environmental sustainable and

green corrosion inhibitors for metals and alloys in aggressive
corrosive media

Chandrabhan Verma1,2*, Eno E. Ebenso1,2, Indra Bahadur1,2 and M. A. Quraishi3,4*

1
Department of Chemistry, School of Chemical and Physical Sciences, Faculty of Natural
and Agricultural Sciences, North-West University, Private BagX2046, Mmabatho 2735,

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South Africa
2
Material Science Innovation &Modelling (MaSIM) Research Focus Area, Faculty of Natural
and Agricultural Sciences, North-West University, Private Bag X2046, Mmabatho 2735,

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South Africa
3
Department of Chemistry, Indian Institute of Technology, Banaras Hindu University,

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Varanasi 221005, India.
4
Center of Research Excellence in Corrosion, Research Institute, King Fahd University of
Petroleum & Minerals, Dhahran 31261, Saudi Arabia
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Corresponding Author’s emails: chandraverma.rs.apc@itbhu.ac.in (CV);
maquraishi.apc@itbhu.ac.in (MAQ)
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Abstract:

Recently, the development of green corrosion inhibitors and green inhibition

strategies are highly demanded because of the increasing demand of green chemistry in the
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area of science and technology. In last few decades, use of plant extracts as metallic corrosion
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inhibitors has attracted significantly attention. Plant materials are ideal green candidatures to
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replace traditional toxic corrosion inhibitors. Reduced environmental risk, lower cost, wide
spread availability and high corrosion inhibition effectiveness make the plant extracts as
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suitable candidates to replace the expensive and toxic traditional synthetic corrosion
inhibitors. Literature survey reveals that different extracts such as leaf, root, stem, bark, pulp,
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fruit, etc. have been effectively employed as sustainable inhibitors for the corrosion of
different metals and alloys. Present review article describes the collection of published work
that has been carried out on the topic “plant extract as corrosion inhibitors for metals and
alloys in aggressive aqueous solutions”. The article includes extracts of diverse part of the
plants for diverse metals and alloys in the several electrolytic media.

Keywords: Plant extract, Green inhibitors, Phytochemicals, Green chemistry, Metals and
alloys.

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1. Introduction
1.1. General introduction of corrosion

Corrosion is a natural and spontaneous phenomenon that results into conversion of

pure metals and their alloys into several stable forms such as their sulfide, oxides, hydroxides
etc. by the chemical and /or electrochemical reactions with the surrounding environments [1-
3]. Corrosion is a damaging phenomenon for assets of industries, buildings, traffic and
railways bridges, and households [4-6]. A very recent study carried out by NACE 2016

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suggests that at global level, corrosion causes economic loss of about 2.5 trillion US dollars
which constitutes nearly 3.4% of total GDP. However, by implementation of existing

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corrosion preventing technologies in a proper way, the cost of corrosion can be reduced up to
15-35% (375-875 billion US dollars). Because of its association with very high economic and

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safety losses, corrosion is an important issue that has to be addressed by scientists and
engineers working in the field of corrosion discipline and engineering throughout the world
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[7-13]. Several methods of corrosion prevention have been developed among which use of
synthetic corrosion inhibitors is one of the most popular and economic methods due to their
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ease of synthesis and application and high effectiveness at relatively low concentration.
These organic compounds adsorb over the surface of metals and alloys through their
heteroatoms and π-electrons and form protective surface barrier thereby protect metals from
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corrosive degradation. Generally, heteroatoms of organic inhibitors exist in polar functional

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groups such as –CN, -NO2, -NH2, -OH, -COOH, -COOC2H5, -OCH3 etc. those act as
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adsorption centers during adsorption of these compounds on the metallic surfaces [14-18].
Additionally, these polar functional groups enhance the solubility of the compounds in the
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polar electrolytic media like H2O, HCl, H2SO4, H3PO4, HNO3 etc. [14-18].

1.2. Green corrosion inhibitors

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The use of traditional corrosion inhibitors, is now limited because of increasing

concept of “green chemistry” in field of science, technology and engineering [19-21]. “Green
chemistry” is a branch of science and technology which utilizes a set of principles that causes
reduction in the discharge of environmentally malignant materials into surrounding
environmental and designing as well as application of environmental friendly chemicals [22-
24]. Recently, the increasing ecological consciousness and strict ecofriendly regulations in all
field of science and technology, have influenced the scientists and engineers working in the
field of corrosion science towards, the synthesis of organic inhibitors using one step multi-

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component reactions (MCRs) that combines three or more reacting molecules in single step.
The MCRs have emerged as substantial tool for the green synthesis of organic compounds
particularly in association with ultrasound and microwave irradiations [23, 25-31]. Further,
the use of different plant extracts [32-35], chemical medicines (drugs) [36-40], and ionic
liquids (designer chemicals) [41-47] have also gained sufficient consideration towards the
development of green corrosion inhibitors. Plants are characterized by their unique property
to convert radiant energy (sunlight) into life providing organic compounds (carbohydrates)

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via the process of photosynthesis. They are also natural source of several raw materials such
as fruit, vegetables, woods, oils, resins, and dyes those have several commercial uses in our
day-today life [48, 49]. In addition to these uses, plants are also characterized by their ability

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to continuous uptake of “greenhouse” CO2 gas, highly toxic metals and other pollutants

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during the process of photosynthesis, which is an essential process from environmental
cleaning point of view. The photosynthesis cleans the surrounding water, soil and aerial
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environments [50, 51]. Literature revision proposes that till today numerous reviews articles
have been documented for corrosion inhibition such as drugs [38, 52-54], DFT as tool for
corrosion study [55, 56], chromate independent green corrosion inhibitors [57-60], organic
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compounds and ionic liquids as inhibitors [16, 17, 19, 61-67], inorganic corrosion inhibitors
[68-70], plant extracts as inhibitors [67, 71-72] and so on. As for as the availability of review
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articles on plants extracts are concerned, they are outdated and have very limited content and
number of cited papers. In contrast, present review article collects several recent and past
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papers in which plant extracts have been tested as corrosion inhibitors for several electrolytic
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media.
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1.3. Important parameters for extract preparation

Nowadays, development of green corrosion inhibitors and inhibition strategies are

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highly demanded because of the increasing demand of green chemistry in all field of science
and technology. Because of their natural and biological origin along with their ecofriendly
isolation, plant extracts can be regarded as green and sustainable materials to be used as
inhibitors for metals and alloys corrosion in aggressive media including HCl, H2SO4, H3PO4
and HNO3 [73]. There are several methods available in literature for preparation of plant
extracts. The detail description of these methods is beyond the scope of the present report.
However, the several parameters that should be considered during preparation of plants
extracts are described briefly:

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(a) Solvents for extraction: Generally, solvent diffused into plant tissue, solubilized and
finally extracted the compounds (phytochemicals) present over there [74, 75].
Therefore, choice of the suitable solvents for extraction is very important for effective
extraction. Extensive literature survey reveals that water is the best solvent owing to
its simplicity, readily availability, non-toxic nature, non-flammable, non-hazardous,
uniquely redox-stable, inexpensive properties [76-79]. However, preparation of some
plant extracts requires organic solvents like ethanol and methanol.

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(b) Extraction temperature: Temperature has very marked effect on the effective plant
extract preparation. A very low temperature limits the effective solubility of the
phytochemicals, while very high temperature cause the decomposition of the active

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constituents (phytochemicals). Generally, extraction is being carried out in the

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temperature range of 60-80 ᴼC in order to find optimal extraction yield [80, 81].
(c) Plant Drying Temperature: Very often, the plant materials are allowed to dry at
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room temperature in shade. However, this type of drying requires several days,
weak, even months; therefore oven drying has also gained significant
advancement.
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1.4. Leaf extracts as corrosion inhibitors

Because of the toxic behaviour of traditional corrosion inhibitors for living being and
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their non-biodegradable nature, the demand corrosion inhibitors of natural and biological
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origin that have either no or little adverse effect on environment is highly anticipated [82-84].
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In this context plant extracts (phytochemicals) are being utilized extensively as green and
effective alternative of tradition toxic corrosion inhibitors. Leaf is the phytochemically richest
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part of the plants where the synthesis of phytochemicals takes place. The consumption of
plant extracts as corrosion inhibitors is a green and environmental friendly approach because
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most of the phytochemicals are water soluble metabolites like organic acids, Quinone’s,
phenolic compounds, flavonoids, alkaloids, catechins, and terpenoids and co-enzymes etc.
including amino acids, plants derived proteins, polysaccharides and vitamins [85-87] that
have no significant adverse effect on living organisms and environment. Because of the low
cost, renewable nature, reliability, versatile, biodegradable, and biocompatible and ease of
application, several plant extracts have been used earlier.

The leaf is the richest part of the organic compounds where their synthesis takes place
via photosynthesis. Several cost effective methods have been developed for preparation of
plant extracts [88, 89]. It is important to mention that extract every plant extract contains

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several organic compounds that can effectively adsorb on metallic surface and behave as
corrosion inhibitors. These organic compounds contain heteroatoms like oxygen, sulfur,
nitrogen and phosphorus in form of polar functional moieties, aliphatic and aromatic
heterocyclic rings that can act as adsorption centers [90-92]. The adsorb inhibitors film
separates the metals and alloys from the corrosive environments. The adsorption behavior of
organic corrosion inhibitors affected by several factors such temperature, nature of metal and
corrosive environment, electronic structure, solubility, and planarity of the inhibitor molecule

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etc. [93, 94]. The use of plant extracts as alternative for organic corrosion inhibitors have
several advances such as reduced environmental risk as majority of plan extracts are
tolerable, biodegradable and non-toxic [95] and are associated with negligible adverse effect

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of the surrounding environment [96]. Additionally, the synthesis of phytochemical by

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utilization of highly toxic greenhouse gas (CO2) through photosynthesis is important for
another aspect of green chemistry. The phytochemicals are naturally available in huge
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amount and can be isolated economically [97, 98]. The plants are widely dispersed
throughout the world and wide range of effectiveness as each plant extract generally contains
various active phytochemicals [99, 100].
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1.4.1. Leaf extracts as corrosion inhibitors for mild steel

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Mild steel is widely used as building materials in different industries due to its high
mechanical strength and low cost [101, 102]. However, it is very reactive by means of
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chemical and electrochemical reactions with the components of the environment, and thus
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loss of metal component occurs due to corrosion. Several attempts have been made
previously in order to mitigate these unwanted reactions particularly during some common
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industrial developments like acid cleaning, acid descaling, acid pickling, etc. among which
use of corrosion inhibitors is one of the best methods. Several leaf extracts have been
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employed as effective corrosion inhibitors for mild steel in different electrolytic media.

1.4.2. Leaf extracts as corrosion inhibitor: Mild steel: HCl system

Before their commercial and industrial applications, the metallic surface often
requires removal of rusts and scales using strong acid such as H2SO4, HCl, HNO3 and H3PO4
[103, 104]. This process of acid cleaning is generally known as acid pickling [105].
Although, hydrochloric acid is more expensive and reactive than sulphuric acid, however, it
is more commonly being used as pickling agent than sulphuric acid because waste liquor can
be recovered more economically in case of hydrochloric acid. Since hydrochloric acid is

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more reactive than sulphuric acid, pickling is generally carried out in hydrochloric acid
solution at lower temperature, while pickling with sulphuric acid requires higher temperature.
Apart from that, the residual chloride (ferrous or ferric) produced from hydrochloric acid
pickling process can be rinsed off more readily than the residual sulphates (ferrous or ferric)
produced due to sulphuric acid pickling. Several leaf extracts have been used as effective
inhibitors for mild steel/ HCl system. Soltani et al. [106] described the inhibition effect of
Salvia officinalis leaves extract on 304 stainless steel corrosion in 1M HCl solution using

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computational and experimental methods. Potentiodynamic polarization study revealed that
S. officinalis leaves extract is acted as mixed type inhibitor. Adsorption of the S. officinalis on
metallic surface obeyed the Langmuir adsorption isotherm. DFT was performed on the

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several components of the S. officinalis in order to describe its inhibition performance. These

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authors postulated that out of fifteen active components, the inhibition activities of the S.
officinalis extract is mainly attributed due to presence of phenolic components such as
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luteolin 7-glucoside, sagecomarin, luteolin 7-glucoronide, rosmarinic, carnosol and
salvianolic acid. The phenolic components possess heteroatoms such as N and O that can act
as adsorption centers. Li et al. [107] studied the inhibition property of Osmanthus fragran
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leaves extract (OFLE)) on carbon steel in 1M HCl. The study was performed using
electrochemical, AFM, FT-IR and DFT methods. Adsorption of the OFLE on carbon steel
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followed the Langmuir adsorption isotherm. Polarization study revealed the OFLE acted as
mixed type inhibitors. DFT study was also performed in order to explain the mechanism of
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corrosion inhibition. The inhibition effect of alkaloids extract (AE) of Geissospermum leave
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on C38 steel in 1M HCl was investigated by Faustin et al. [108] using electrochemical and
surface study (SEM and EDX) methods. They found that AE acted as good corrosion
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inhibitor and gained the maximum inhibition efficiency of 92% at 100 mg/ L concentration.
Adsorption of AE on C38 surface followed the Langmuir adsorption isotherm. Further, the
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AE acted as mixed type inhibitor. SEM and EDX analyses supported the adsorption behavior
of AE on metallic surface. The comparative study of AE of and geissospermine alone
indicated that the geissospermine is the active compound of the AE responsible for the
inhibition performance of the G. leave. Orubite and Oforka [109] investigated the inhibition
performance of extracts of leaves of Nypa fruticans. The test material was mild steel
corrosion in hydrochloric acid solution using weight loss and hydrogen gas evolution
methods. Authors compared the in the inhibitory efficiency of N. fruticans with that of 1,5-
diphenylcarbazone and observed that at 30 ᴼC N. fruitcans exhibited 75.11% inhibition

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performance, while 1,5-diphenylcarbazone only 70.18% at same temperature. Several other

leaf extracts have been investigated as corrosion inhibitors, some of them listed in Table 1.

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Table 1: Leaf extracts as corrosion inhibitors in hydrochloric acid solution including techniques, nature of metal and electrolytes and
nature of adsorption of active constituents.

Plant name Technique(s) Metal and Nature of Remark

P T Ref.(s)

Olea europaea WL, PDP, CV

electrolyte

C-steel/
adsorption

Langmuir,
R I
Hydroxytyrosol and Oleuropein were active [110]
2 M HCl
Mixed type

S C components

Tabernaemont-ana
divaricata
WL, EIS, PDP,
SEM-EDX
Fe/1M HCl

N U
Langmuir,
Mixed type
Maximum efficiency of 95% was achieved at
500 ppm
[111]

Phyllanthus amarus WL, EIS, PDP, Fe/1M HCl

A
Langmuir, Phyllanthin is the main phytochemical present [112]
DFT
M Mixed type in P. amarus

Eleusine aegyptiaca and

Croton rottleri
WL, EIS, PDP,
FT-IR, UV–Vis,
E D
cast iron/1M HCl Langmuir,
Mixed type
Inhibition performance of these leaves
extracts was also studied with halide additives
[113]

SEM, X-ray
diffraction
P T (KCl, KBr, and KI)

Pimenta dioica
AFM, DFT
C E
EIS, PDP, SEM, Mild steel/ 0.5M
and 1.0 M HCl
Langmuir,
Mixed type
Eugenol is major active component which
showed comparable efficiency to the P. dioica
[114]

Thyme
A C
WL, EIS, PDP Mild steel/ 2M
HCl
Langmuir,
Mixed type
extract

Thyme leaves extract attained maximum

efficiency of 84%
[115]

(Guatteria ouregou and EIS, PDP, OPM Low carbon Langmuir, Harmane was identified as the main [116]
Simira tinctoria) steel/1 M HCl Mixed type component of S. tinctoria extract

Morusalba pendula EIS, PDP, UV– Steel/ 1M HCl Langmuir, Inhibition efficiency increased from 93% to [117]
visible, FT-IR,

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AFM Mixed type 96% in presence of 10 mM KI

Ficus hispida WL, EIS, PDP, Mild steel/ Langmuir, Maximum %IE was 90% at 250 ppm, [118]
XRD, FT-IR, cathodic type stigmasterol was main active constituent of F.
EDX 1M HCl hispida

Solanam Xanthocarpum WL, GSM, EIS, Carbon Steel/ 1M Langmuir,

T
Maximum %IE of 83.2 was obtained at 800
P
[119]

Gliricidia sepium
PDP, MM

WL, FT-IR,
HCl

Mild steel/
Mixed type

Langmuir
I
ppm concentration

R
Phytochemical screening suggests the [120]
SEM-EDX 1M HCl
isotherm

S C
presence of Saponins, Tannins, Flavonoids,
Terpenoid

Rosemarinus officinalis L. GM, PM Mild steel/ ----

N U 100% leaves extract gave the 98.33%

efficiency
[121]
0.1M HCl
A
Eichhornia Crassipes GM , DFT and Mild steel/ M ---- Higher concentrations and lower temperatures [122]
MD simulations

E
5M HCl D enhances the efficiency

Murraya koenigii (Curry

leaves)
WL, GSM, EIS,
PDP, SEM
P T
Mild steel/ Langmuir,
Mixed type
84.6% IE was obtained at 4% in v/v extract [123]

Petroselinum Crispum
C E
EIS, PDP, SEM
1M HCl

Carbon Steel/ 1M Langmuir, Plant extracts inhibits metallic corrosion be [67]

(Parsley),Eruca Sativa
(Arugula), Anethum
Graveolens A C HCl Mixed type becoming adsorbate at metal surface

Eucalyptus Camaldulenis GM technique Carbon Steel/ 3M Langmuir Adsorption of E. Camaldulenis is spontaneous [124]
HCl isotherm

Emblica Officinalis WL, UV-visible, Mild Steel/ 1M Langmuir highest %IE of 88% at 1000ppm [125]

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FT-IR, SEM HCl isotherm concentration

Pterocarpus soyauxi WL, Mild Steel/ Tempkin and P. soyauxi Physically adsorbed on the [126]
Freundlich metallic surface
1-2.5 M HCl isotherms

Plumeria Alba, Blighia GM, OPM Low carbon Steel/ Langmuir

T
Blighia Sapida exhibited the maximum
P
[127]
Sapida, Secamone Afezeli
1 and 2 M HCl
isotherm
I
inhibition efficiency

R
Emblica Officinalis WL, UV, SEM Mild steel /
1 M HCl
---

S C
highest %IE of 88% at 1000ppm
concentration
[128]

Sesbania sesban WL, EIS, PDP Carbon Steel/ 1M

HCl
N U
Langmuir,
Mixed type
91.08% IE was obtained at 2.00 g/l
concentration
[129]

A
Bryophyllum GM, SEM Mild steel /
M Langmuir
isotherm
94.27% IE was obtained at 8 g/L
concentration at 298K
[130]
Pinnatum

Azadirachta Excelsa GM, FESEM D

0.5 M HCl

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Mild steel / Langmuir 78.55% IE was obtained at 800 ppm [131]

P T1 M HCl
isotherm concentration

Boscia
senegalensis C E
WL, SEM, EIS,
PDP, FT-IR,
Mild steel/
1M HCl
Langmuir,
Mixed type
saponins, tannins, phlobatins, anthraquinones,
cardiac glycosides, flavonoids, terpenes, and
[132]

Acalypha indica
A
WLC
DFT calculations

Mild steel/ Temkin

isotherm
alkaloids were components

93.26% IE was obtained at 0.7% inhibitor

concentration
[133]
1M HCl

Phoenix dactylifera WL, EIS, PDP, Carbon steel/ Langmuir, 97.7% IE was obtained at 2 g/l concentration [134]
SEM Mixed type
1M HCl

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Ruta Graveolens WL, EIS, PDP, Mild steel/ Langmuir, 98.25% IE was obtained 4%v/v of inhibitors [135]
DFT calculations Mixed type
1M HCl

Annona Muricata .L WL, EIS, PDP, Mild steel/ Mixed type Photochemical analysis shows the presence of [136]
SEM several constituents
1M HCl

P T
Michelia alba EIS, PDP, SEM,
FT-IR, DFT
calculations
Carbon steel/Mild
steel
Langmuir,
Mixed type
R I
98.4% IE was obtained at 1.686 g/L
concentration
[137]

Anthocleista Djalonensis WL
1M HCl

Mild steel/ Langmuir S C

97.23%was obtained at 0.6 g/L concentration [138,
1M HCl
N U
isotherm 139]

Morinda tinctoria WL, EIS, PDP, Mild steel/

A
Langmuir, Synergism through KBr, KCl and KI showed [139]
calorimetric tests
1M HCl M Mixed type significant IE increase

Vitex negundo WL, GSM,

electrochemical
E D
Carbon steel/ Langmuir,
Mixed type
79.2% IE was obtained at 800 ppm extract
concentration
[140]

P T
1M HCl

Gymnema Sylvestre
E
WL, SEM, UV,
FT-IR and EDX
C
Mild steel/
1M HCl
Langmuir
isotherm
Gymnemic acid, Stigmasterol, Lupeol were
main constituents
[141]

Argemone mexicana
A C
WL, UV-vis,
electrochemical,
Mild steel/
1M HCl
Langmuir,
Mixed type
92.5% IE was obtained at 500 mg/L extract
concentration
[142]

SI

Acalypha torta WL, UV-vis, Mild steel/ Langmuir, Nearly 90% efficiency was obtained at 1000 [143]
electrochemical, Mixed type ppm concentration
SEM, CAM 1M HCl

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Podranea ricasoliana WL, FT-IR Mild steel/ Langmuir, Maximum IE was obtained at 3h immersion [144]
electrochemical, Mixed type time
SEM 1M HCl

Passiflora foetida WL, SEM, AFM Mild steel/ Langmuir, 94.61% IE was obtained at 130 ppm [145]
electrochemical, Mixed type concentration
1M HCl

P T
Shorea Robusta WL Mild steel/
1M HCl
Langmuir
isotherm I
94.5% IE was obtained at 5g/L concentration

R
[146]

Funtumia elastica WL, FT-IR Mild steel/ Langmuir,

S C 90.1% IE was obtained at 1500 mg/L [147]
electrochemical,
DFT, MD
simulations
1M HCl

N U
Mixed type concentration after 24 h. Immersion time
decreased the efficiency

A
Tithonia diversifolia PDP, FT-IR 304 SS /
M Mixed type 77.27% was obtained at 2 g/L extract
concentration
[148]

D
1 M HCl

Gnetum africana WL,

electrochemical, E
Mild steel/

T
Langmuir,
Mixed type
98.37 IE was obtained at 0.5 g/L
concentration
[149]

Lactuca sativa, WL
E P1M HCl

Carbon steel/ Langmuir, Petroselinum crispum extract exhibited [150]

Eruca Sativa,
Petroselinum crispum,
C C 1M HCl
Freundlich, and
Temkin
isotherm
maximum IE of 81.39% at 60 %v/v extract
concentration
and Anethum Graveolens
A

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1.4.3. Leaf extracts as inhibitors: Mild steel: H2SO4 system

Similar to hydrochloric acid, sulphuric acid is also being used widely for removal of rusts
and scales from the surface of metals and alloys. In fact sulphuric acid is second most common
acid used for descaling and acid pickling processes. These acid cleaning processes require use of
some additives to prevent the metallic corrosion. Several leaf extracts have been employed as
operative inhibitors for mild steel corrosion in sulphuric acid. Mehdipour et al. [151]

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investigated the inhibition effect of Aloe Vera leaf extract on mild steel corrosion in 1M

IP
sulphuric acid using electrochemical and scanning electron microscopic techniques. Results

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showed that Aloe Vera leaf extract acts as mixed type inhibitor and exhibited maximum
efficiency of 98% at 30% v/v concentration. Hassan and coworkers [152] testified the inhibition
effect of Citrus aurantium leaves extracts on mild steel corrosion in 1M H2SO4. The adsorption

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of Citrus aurantium leaves extracts metallic surface obeyed the Langmuir adsorption isotherm.
The extract exhibited maximum inhibition efficiency of 89% at 10 ml/l concentration. Quantum
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chemical calculations of active constituents deliver upright sustenance to the experimental
results. The inhibition effect of Sida acuta [153], African Perquetina [154], Emblica leaves
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[155], Cassia tora [156], Nicotiana tabacum [157], Mangnifera indica [158], Achyranthes
aspera [159], African Breadfruit [160], Jatropha Curcas [161], Wrightiatinctoria,
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Clerodendrumphlomidis, Ipomoeatrilob [162], Sida acuta [163], Nauclea latifolia [164], Nypa
fruticans Wurmb [165], Spondias cytherea [166], Combretum bracteosum [167], Hyptis
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Suaveolens [168], Polyalthia Longifolia [169], Buddleia perfoliata [170], Bambusa glauscescens
[171], Bitter leaf (Vernonia amygdalina) [172], Cassava leaves (Manihot esculenta) [173],
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Oxystelma Esculentum [174], Stachytarpheta Indica [175], Telferia occidentalis (TO),

Azadirachta indica (AI), Occimum viridis (OV) and Hibiscus sabdariffa (HS) [176] leaf extracts
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have been investigated as potential corrosion inhibitors for mild steel in sulphuric acid solution
using several experimental techniques such as weight loss, electrochemical, surface investigation
and DFT methods. Table 2 represents some common examples of this type of plant extracts.

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Table 2: Leaf extracts as corrosion inhibitors in sulphuric acid solution, nature of metal and electrolytes and nature of adsorption of
active constituents.

Aloe Vera EIS, PDP, Stainless Langmuir isotherm, It was observed that Aloe Vera lef extract [151]
SEM steel/ Mixed type inhibitor

P T
contains Aloesin, Aloin, Aloe and Aloe Resin

1M H2SO4
I
those have –OH, >=O, C-O, and O-heterocyclic
compounds those act as adsorption centers
R
Citrus aurantium WL, SEM Mild steel/
1M H2SO4
Langmuir isotherm

S CCitrus aurantium leaf extract showed highest

inhibition efficiency of 89% at 10 ml/L
concentration.
[152]

Sida acuta (leaf and WL, AAS, FT- Mild steel/

N U
Freundlich adsorption Results showed that both S. acuta leaf and stem [153]
stem) IR, UV
1M H2SO4
isotherm
A extracts act as good inhibitors and their
efficiencies obeyed the order: LV > ST. Results
M of different analyses were in good agreement.

African Perquetina GM, GSM and Mild steel/

TM
E D Langmuir
isotherm
adsorption A. Perquetina showed maximum %IE of 87.78% [154]
at 0.5 g/L concentration. Dubinnin-Radushkevich
2M H2SO4

P T isotherm model showed the adopted corrosion

monitoring techniques were in good agreements.

Emblica leaves WL

C E Mild steel/ --- %IE amplified with rise in concentration and

extreme efficiency of 80% and 65% were
[155]

Cassia tora
A C
WL, FT-IR,
2M H2SO4

Mild steel/ ----

obtained after 24 and 120 hrs immersion time.

C. tora showed the maximum %IE of 95.44% at [156]

SEM 400 ppm concentration. %IE gradually decreases
0.5M H2SO4 on increasing temperature.

Nicotiana tabacum WL, DFT Mild steel/ Langmuir adsorption N. tabacum showed maximum %IE of 94.13% at [157]
isotherm 10 g/L concentration after 6 hrs immersion time.
2M H2SO4 both experimental and DFT analyses were well

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 ACCEPTED MANUSCRIPT

validated each other.

Mango (Mangnifera WL, TM, PDP, Mild steel/ Langmuir isotherm, M. indica showed optimum %IE of 74.09% at [158]
indica) FT-IR mixed type 0.97g/L concentration at 305.33K temperature
1M H2SO4 and 22.76 hrs immersion time.

Achyranthes aspera WL Mild steel/ Langmuir, Frumkin and

P T
Results showed that A. aspera is a good [159]
0.5M H2SO4
Flory-Huggins
adsorption isotherm
I
corrosion inhibitor and showed the optimum
%IE of 92.3%. It adsorb on the mild steel surface
R
by physisorption mechanism.

African breadfrui WL Mild steel/ Freundlich adsorption

Aluminum isotherm S C
A. breadfrui showed optimum %IE of 70.55%
and 78.56% for mild steel and aluminum,
[160]

1M H2SO4
N U respectively.

Jatropha curcas WL Carbon steel/ ----

A J. curcas exhibited optimum %IE of 92.1% (at [161]
0.5M H2SO4 M 1.5g/L) and 55.5% (2.5 g/L) in0.5 M NaCl and
0.5 M H2SO4.
and
NaCl
0.5M

E D
Wrightiatinctoria,
Clerodendrumphlomidi
WL, PDP, EIS,
SEM
P T
Mild steel/ Langmuir isotherm,
Mixed type inhibitor
The optimum %IE was obtained at 200 ppm
concentration at 323 K temperature. The %IE
[162]

s, Ipomoeatriloba

C E 0.5M H2SO4 obeyed the order: C. phlomidis > I.triloba > W.

tinctoria.

Sida acuta

A C
WL, HE Mild steel/
1M H2SO4
Freundlich adsorption
isotherm
The effect of synergism has been studied in
presence of iodide concentration. However, %IE
decreases with temperature.
[163]

Nauclea WL, GSM Mild steel/ Thermodynamic-kinetic The %IE follows the order: RT (94.26%) > LV [164]
model of El-Awady et (91.58%) > BK (75.26%) at 4 g/L concentration.
Latifolia (leaf, bark, 1M H2SO4 al.
root)

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 ACCEPTED MANUSCRIPT

Nypa fruticans Wurmb WL Mild steel/ --- N. Wurmb showed optimum %IE of 74.48% at [165]
0.5 g/L concentration in 0.5M H2SO4 at 323 K
0.1, 0.5, 1.0 temperature.
and 2.0M
H2SO4

Spondias WL, GSM Mild steel/ Langmuir and

P T
S. Cytherea extract showed 67.72% and 72.% [129]

I
Freundlich isotherm efficiency for weight loss and gasometric
Cytherea 5M H2SO4 measurements.

Combretum WL, HE Mild steel/ Frumkin adsorption

C R
C. bracteosum showed optimum %IE of 74.76% [167]

S
bracteosum isotherm and 88.31% in 2M and 5M H2SO4, respectively
2M and 5M at 30º C temperature.

Hyptis WL, EIS, PDP,

H2SO4

Mild steel/
N U
Langmuir isotherm, H. Suaveolens exhibited maximum %IE of 95% [168]
FT-IR, XRD,
A
Mixed type inhibitor at 250 ppm concentration.

M
Suaveolens SEM 1M H2SO4

Polyalthia
Longifolia
WL Mild steel/
1M H2SO4
E D Langmuir,
Temkin, Freundlich
The effect of temperature has also been
investigated in the range of 35-75ºC. it showed
[169]

T
optimum %IE of 92% at 1.5% concentration.
adsorption isotherms

Buddleia perfoliata WL, EIS,

PDP,SEM, E P
1018 Carbon Frumkin
steel/
B. perfoliata showed highest %IE of 88% at 500
ppm concentration using EIS technique.
[170]

C
UV-Visible

C 0.5M H2SO4
adsorption isotherm

Bambusa glauscescens
A
GSM and OPM Mild steel/
2M H2SO4
Freundlich adsorption
isotherm
B. glauscescens performances as good corrosion
inhibitor for mild steel in acidic solution and its
%IE rises with concentration and accomplish
[171]

maximum value 400 ppm concentration

Vernonia amygdalina WL, HE, TM Mild steel/ Langmuir adsorption V. amygdalina adsorbed by physisorption [172]
mechanism. It showed 90 %, 84.82 %, 79.65 %

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1.5M H2SO4 isotherm and 76.90 % at 30º, 40º, 50º and 60ºC
temperature at 0.5g /L concentration.

cassava (Manihot WL, PDP, Mild steel/ Langmuir adsorption The inhibition experiment was performed at [173]
esculenta) SEM isotherm 0.1%, 0.5%, 1%, 5% and 10% and, maximum
0.5M H2SO4 efficiency of 85.87% was obtained at 10%
concentration.
P T
Oxystelma esculentum EIS, PDP Mild steel/ Mixed type inhibitor
R I
At 100 ppm concentration it showed %IE of
66.8%. However, in presence of 25 ppm KI %IE
[174]

Stachytarpheta indica WL, HE

0.5M H2SO4

Mild steel/ Langmuir adsorption

C
enhanced up to 81.0%.

S
S. indica spontaneously adsorbed on mild steel [175]
1M H2SO4
isotherm

N U surface by physisorption mechanism.

A
M
E D
P T
C E
A C

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1.4.3. Leaf extracts as inhibitors: Mild steel: HCl and H2SO4 system

There are several leaf extracts that have been reported as green and efficient corrosion
inhibitors for mild steel in hydrochloric as well as in sulphuric acid solutions. Some of the
common and important leaf extracts investigated as inhibitors for mild steel in both the acidic
solutions are Ginkgo (Chinese name Yingxing) [177], Occimum viridis (OV) [178], Occimum
viridis (OV) [179], Dodonaea viscosa [180], Trifoliate fenugreek [181], Kigelia pinnata [182],

T
Citrus aurantiifolia [183], Jatropha Curcas [184], Hibiscus sabdariffa [185], Gnetum africanum,

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Gongronema latifolium, Chromolena odaratum [186], Phyllanthus amarus [187], lupine

CR
(Lupinous albus) [188]. Generally, these leaf extracts act as mixed type corrosion inhibitors,
however, Ginkgo leaf extract [177] acts as mainly cathodic type inhibitor. Adsorption of the
extracts obey Langmuir adsorption isotherm. Adsorption of Trifoliate fenugreek [181] on mild

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steel surface follows Langmuir and Temkin adsorption isotherms in HCl and H2SO4 solutions,
respectively whereas the adsorption of Lupinous albus [188] on mild steel surface in both the
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tested solutions obeyed kinetic thermodynamic model.
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1.4.5. Leaf extracts as inhibitors: Mild steel/ NaCl, petroleum/ CO2 system

Similar to hydrochloric and sulphuric acids, NaCl and CO2 are very common electrolytic
ED

media. Although, several types of organic compounds have been reported as effective corrosion
inhibitors however the use of plant (leaf) extracts as corrosion inhibitors in these media is
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relatively scare. Abdel-Gaber and coworkers [189] studied the inhibition effect of the olive (Olea
europaea L) leaf extract on steel corrosion in brine solution (saturated solution of NaCl) using
CE

electrochemical and chronoamperometry techniques. The extract exhibited high inhibition

efficiency due to development of cytotoxically sedentary complex of calcium caffeate. Results
AC

further showed that extract inhibits the corrosion of steel by controlling the cathodic oxygen
reduction process. The inhibition effect of ethanolic extract of Ricinus communis leaves on mild
steel corrosion in aqueous solution containing 100 ppm NaCl is reported by Sathiyanathan et al.
[190]. The extract showed maximum inhibition efficiency of 84% at 300 ppm concentration.
Similar observation was reported for inhibition effect of Neem and African star apple leaf
extracts on mild steel corrosion in sodium chloride and polluted seawater media, respectively
[191, 192]. Abd-El-Khalek and coworkers [193] studied the inhibition behavior of Nicotiana
leaves extract on steel corrosion in neutral chloride solution using electrochemical techniques.

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Results showed that Nicotiana leaves extract acts as mixed type inhibitor. Aribo et al. [194]
studied the inhibition effect of Tridax procumbens and Chromolaena odorata extracts on
stainless steel (UNS S31254) corrosion in a CO2-saturated acidizing oilfield environment.
Results showed that over 90% efficiency was obtained at 100 ppm concentration of inhibitors.
The inhibition mechanism involves formation of monolayer consisted with Langmuir adsorption
isotherm. The inhibition effect of Ficus Carica leaves extract on steel corrosion in petroleum
solution has been investigated by Anaee and coworkers [195]. Results showed that the extracted

T
exhibits the inhibition efficiency of 70-80% and acts as mixed type inhibitors. Adsorption of the

IP
extract over metallic surface obeyed the Langmuir adsorption isotherm.

CR
1.4.6. Leaf extract as inhibitors for mild steel: CH3COOH, HNO3, H3PO4 system

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Mild steel is widely used metallic alloy for construction of pipelines through which
transportation of liquid and gaseous chemicals being carried out. However, generally organic
AN
acids of lower molecular weight such as acetic acid are reported as corrosive agents for the
internal wall of pipeline. Although, use of organic corrosion inhibitors is the first line of defense
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against corrosion in this type of medium, however, recently, few plant (leaf) extracts have been
conveyed as corrosion inhibitors. Chaudhari and Vashi [196] reported the inhibition property of
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henna (Lawsonia Inermis) extract (leaves) on mild steel corrosion in acetic acid solution. The
extract performances as virtuous inhibitor for mild steel and behaved as mixed type inhibitor.
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Adsorption of the extract on the metals surface obeyed the Langmuir adsorption isotherm.
Victoria et al. [197] investigated the inhibition behavior of Psidium guajava (guava) leaf extract
CE

on mild steel corrosion in 1M phosphoric acid. The extract acts as mixed type inhibitor and its
adsorption on the mild steel surface followed the Temkin adsorption isotherm. The inhibition
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effect of Rosmarinus officinalis leaf extract in phosphoric acid solution has also been
investigated elsewhere [198]. The inhibition effect of Aloe Barbadensis (Aloe Vera) on mild
steel corrosion in nitric acid solution is reported by Pankaj and Gargi using weight loss method
[199]. The extract exhibited maximum efficiency of 89.94% at 0.225x10-3gms concentration.

1.5. Other part of the plant extracts as inhibitors for mild steel

Although, leaf is the most common part of the plants that have been inspected as corrosion
inhibitors because it is most chemically reach part of the plants where the biosynthesis of these

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chemicals occur. However, there are several parts of the plants such as root [200-202], bark
[203], flower [204-206], fruit [207-210], wood [211], seed [212-218] and peel [219-228] that
have been employed as efficient corrosion inhibitors for mild steel. Literature survey reveals that
there are several extracts that have been prepared and used as corrosion inhibitors for mild steel
and other metallic materials by crushing the whole plants such as Artemisia pallens [229], Black
pepper [230], Santolina chamaecyparissus [231], Mimosa extract [232], Egyptian licorice [233],
Aloe Vera [234], Seaweed [235], Euphorbia falcata [236], Uncaria gambir [237], Pterolobium

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hexapetalum and Celosia argentea [238], Medicago Sative [239], Chenopodium Ambrosioides

IP
[240], Ligularia fischeri [241], Salvia aucheri mesatlantica [242], Gentiana olivieri [243], Olive

CR
pomace [244], Piper nigrum [245], Cuminum cyminum [246], Uncaria gambir [246, 247],
Acacia tortilis [248], Vernonia Amygdalina [249], Rhus verniciflua [250], Black cumin (Nigella

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sativa L.), Halfabar (Cymbopogon proximus), Chamomile (Chamaemelum mixtum L.) and
Kidney bean (Phaseolus vulgaris L.) [251], Coffee ground [252], Watermelon rind [253],
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Pennisetum purpureum [254], Senna alata [255], Acacia Nilotica [256], Justicia gendarussa
[257] and Oxandra asbeckii [258].
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1.6. Plants extracts as corrosion inhibitors for aluminum

ED

Similar to the mild steel, aluminum is the widely used metals in various industries as machinery,
reaction vessels, pipes and chemical battery. The extensive use of the aluminum based on the
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fact that unlike to most of the metals, aluminum resistant to corrosion due to presence of surface
oxide layer [259]. However, when it expose to corrosive environments like acidic or basic
CE

solutions the protective oxide layer dissolves resulting into rapid corrosion of the aluminum
[259]. The use of synthetic corrosion inhibitors is the most common measure for protection of
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the aluminum corrosion. However, several plant extracts have also been employed as effective
corrosion inhibitors for aluminum in various electrolytic media. Oguzie [260] explored the
inhibition effect of Sansevieria trifasciata on aluminum corrosion in 2M HCl and 2M KOH
using gasometric technique. He demonstrated the effect of KI, KBr and KCl on the inhibition
effect of the S. trifasciata. Results showed that in the presence of halide ions %IE follows the
order: KI > KBr > KCl. S. trifasciata inhibits the aluminum corrosion by adsorption mechanism
which follows the Freundlich adsorption isotherm. S. trifasciata exhibited maximum %IE of
93.6% and 82.3% in 2M HCl and 2M KOH, respectively in the presence of KI at 30ºC. There are

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several other different plants extracts that such as Gossipium hirsutum [261, 262], Phyllanthus
amarus [263, 264], Terminalia arjuna (TA) Moringa oleifera (MO), and Mangifera indica (MI)
[265], Piper longum [266], Cannabis sativa (CS), Rauwolfia serpentina (RS), Cymbopogon
citratus (CC), Annona squamosa (AS) and Adhatoda vasica (AV) [267] have been investigated
as effective corrosion inhibitor in NaOH solution. The Jasminum nudiflorum Lindl [268], Raphia
hookeri [269], Thymus algeriensis [270], Cocos nucifera [271], Morinda tinctoria [272],
Nicotiana tabacum [273], Vernonia amydgalina [274], Tender arecanut [275] and Maesobatrya

T
barteri [276], Delonix Regia [277], Opuntia [278], Ambrosia maritime [279], Ocimum basilicum

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[280], Ananas sativum [281], Euphorbia hirta and Dialum guineense [282, 283], Dendrocalamus

CR
brandisii [284], Hibiscus sabdariffa [285], Chlomolaena odorata [286], Brahmi (Bacopa
monnieri) [287], Gongronema latifolium [288], Capparis deciduas [289], Ipomoea Involcrata

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[290], Hibiscus Rosa-sinensis [291], black mulberry (Morus nigra L.) [292], Solanum
melongena L. [293], Ginseng root extract [294], Rosmarinus officinalis L. [295], Azadirachta
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Indica [296], Aspilia Africana [297], Laurus nobilis L. [298], Azwain (Trachyspermum
copticum), [299], garlic extract [300], Newbouldia leavis [301], Rosemary leaves extract [302],
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Anthocleista djalonensis [303], Ocimum gratissimum [304], Beetroot (Betanin) [305], Abrus
precatorius [306], Newbouldia leavis [307] and several other plant extracts have also been
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studied as corrosion inhibitors for aluminum. Table 3 represents the collection of few common
plant extracts that have been studied aluminum.
PT
CE
AC

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Table 3: Leaf extracts as corrosion inhibitors for aluminum in different electrolytic media.

Sansevieria trifasciata Gasometric Al/ 2 M Freundlich Adsorption of the S. trifasciata on Al surface [260]
technique HCl and
2M KOH
adsorption
isotherm
P T
physisorption mechanism. Presence of halide ions
enhances %IE significantly. The phenomenon follows the
I
order: KCl < KBr < KI.

R
Gossipium hirsutum (leaf WL
and seed)
Al/ 2 M
NaOH
--
C
G. hirsutum leaf gave 97% inhibition efficiency while the
G. hirsutum seed showed 94% at the 50% v/v
S
concentration.
[261]

Phyllanthus amarus WL Al/ 2 M Langmuir

N U
Phyllathin hypophyllathin are two main constituents [263]

A
NaOH adsorption present in P. amarus extract. It showed optimum %IE of
isotherm 76% at 20% v/v concentration.

Jasminum nudiflorum WL, PDP, EIS, Al/ 1M M

Langmuir The extract showed optimum %IE of 93.6% at 1 g/L [268]
Lindl. SEM HCl

E D isotherm,
cathodic type
concentration. It contains several type of phytochemicals
that can adhere on the metallic surface and inhibit

Raphia hookeri WL, TM

P T
Al/ 0.02-
inhibitor

Temkin
corrosion.

R. hookeri showed optimum %IE of 65.30% at 0.5 g/L [269]

C E 2M HCl adsorption
isotherm,
concentration. It spontaneously adsorbed on the metallic
surface through physisorption mechanism. It showed its

A C Kinetic–
Thermodynami
c Model
best %IE in 1M HCl.

Thymus algeriensis WL, GSM, EIS 2024 Al/ Langmuir It showed optimum %IE of 78.7% at 0.75 g/L [270]
1M HCl adsorption concentration. The presence of iodide ions synergistically
isotherm enhanced the %IE.

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Cocos nucifera WL Al/ 0.5M Langmuir C. nucifera showed optimum %IE of 93% at 7.5% v/v [271]
HCl adsorption concentration. It adsorb physically and spontaneously.
isotherm

Morinda tinctoria WL, PDP, EIS, Al/ 0.5M Langmuir M. tinctoria manifest optimum %IE of 96.72% at 7% [272]
SEM HCl adsorption concentration. It adsorbed spontaneously.
isotherm.
P T
Terminalia arjuna (TA),
Mangifera indica (MI)
WL, EIS, PDP,
SEM, AFM
Al/ 1M
NaOH
Langmuir
adsorption
R I
Among the studied extracts, MO showed the maximum
efficiency of 85.3% at 0.6 g/L concentration. SEM and
[265]

and Moringa
oleifera (MO)
isotherm,
mixed type
S C
AFM analyses showed the formation of protective films
by the extracts.

Piper longum WL, PDP, EIS Al/ 1M

NaOH
Langmuir
adsorption
N U
P. longum showed the optimum %IE of 94% at 400 ppm
concentration. It inhibits corrosion by adsorption
[266]

isotherm,
mixed typeA mechanism by creating a barrier for charge transfer.

Nicotiana tabacum WL, EIS, PDP, AA3003A M

Langmuir N. tabacum acted as mixed type but predominantly [273]
SEM, EDX,
AFM, DFT, MD HCl
E D
l/ 0.1 M adsorption
isotherm,
cathodic type inhibitor. It showed maximum efficiency of
80% at 1200 ppm concentration, experimental results

Cannabis sativa (CS), WL, EIS, PDP, P T

Al/ 1M
cathodic type

Langmuir
were supported by DFT and MD results.

Among these five tested plant extracts RS showed the [267]

Rauwolfia serpentina
(RS), Cymbopogon
SEM, AFM

C E NaOH adsorption
isotherm,
maximum %IE 97.1% at 0.2g/L concentration. These
extracts inhibit corrosion by adsorption mechanism which
citratus (CC), Annona
squamosa (AS) and
A C mixed type was supported by SEM and AFM methods.

Adhatoda vasica (AV)

Vernonia amydgalina WL Al/ 1M Langmuir Increase of the solution temperature decreases the %IE. [274]
HCl adsorption V. amydgalina showed maximum %IE of 91% at 0.09w/v
isotherm concentration

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Tender arecanut WL, EIS, PDP, Al/ 0.5M Langmuir T. arecanut acts as efficient inhibitor for aluminum [275]
AFM HCl adsorption corrosion and showed optimum %IE of 96.15% at 4.5g/L
isotherm, concentration. It contains several phytochemicals those
mixed type act as active constituents.

Breadfruit WL Al/ 0.5M Langmuir Breadfruit peel extracts showed the maximum %IE of [160]
H2SO4 adsorption
T
853% at 145 ppm concentration.
P
Maesobatrya barteri WL, TM Al/ 0.5M
isotherm

Freundlich
R I
M. barteri showed optimum efficiency of 49.30% at [276]
and 2M
HCl
adsorption
isotherm C
0.5g/L concentration.

S
N U
A
M
E D
P T
C E
A C

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2. Phenomenon of synergism

Obviously, each plant extract contains several active phytochemicals/ constituents that can
adsorb at the surface of metal and electrolyte. However, addition of some inorganic salts such as
KCl, KBr and KI in the corrosive medium can add significant improvement in the protection
ability of plant extract towards metallic dissolution. Oguzie investigated the inhibition property
of Occimum viridis (OV) extract on mild steel in 2M HCl and 1M H2SO4 gasometric technique at

T
30 and 60°C temperatures [178]. From the results derived in the study several interesting things

IP
were observed. In hydrochloric acidic medium, addition of KCl decreases the protection power

CR
of the plant extract. Whereas, addition of KBr and KI particularly at lower temperature (30°C)
protection efficiency of the extract increased significantly. In sulphuric acid medium, addition of
KCl, KBr and KI enhances the protection ability of the extract. In both electrolytic media, the

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effectiveness of halides obeyed the order: KI > KBr > KCl. He observed similar observation for
the inhibition effect of Hibiscus Sabdariffa on mild steel corrosion in 2M HCl and 1M H2SO4
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[308]. Similar observation has also been reported on the inhibition effect of Garcinia kola on
mild steel in 5M H2SO4 [309]. Obot and coworkers [310] described the synergistic effect of KI
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on the inhibition efficiency of Aningeria robusta in HCl electrolytic solution. Using hydrogen
evolution method, these authors observed that addition of KI at all studied concentration of the
ED

extract causes noteworthy increase in the protection ability at both studied temperatures (30 and
60°C). The A. robusta extract at 50% v/v concentration showed inhibition efficiency of 48%
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only. Addition of KI at 5 mM concentration in the same solution causes increase in the inhibition
efficiency up to 72%. While studding the inhibition effect of Ipomoea invulcrata on aluminum
CE

corrosion in 1M HCl it was observed that addition KSCN and KI showed the synergistic effect
[311]. The KI showed better synergistic effect as compared to the KSCN. The phenomenon of
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synergism by halide ions have also been reported for other plant extracts such as Sida acuta for
mild steel in 1M H2SO4 [163], Telfaria occidentalis for mild steel 1M H2SO4 and 2M HCl [312],
Ocimum basilicum for aluminum in 2M HCl and 2M KOH [280], bamboo leaf extract for cold
rolled steel (CRS) in 0.1 M H3PO4 [313], coconut coir dust extract for mild steel in 0.5 M H2SO4
[314], Nypa Fruticans’ Wurmb for mild Steel in 0.5 M HCl [315], Cordia sebestena L. for mild
steel in 0.5 M H2SO4 [316], Chamaerops humilis for mild steel in 0.5 M H2SO4 [317] and
Pachylobus edulis for mild steel in 2M H2SO4 [318].

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3. Relative effectiveness of different plant extracts

There are several articles are available in literature in which inhibition efficiency of more than
one parts of the plant extract have been evaluated as corrosion inhibitors on the same metal/ alloy
using same electrolytic medium. Umoren and coworkers reported the inhibition behavior of
leaves and stem extracts of Sida acuta on mild steel 1 M H2SO4 using hydrogen evolution and
weight loss methods [153]. These authors observed that at 0.5g/L concentration leaves extract

T
showed the inhibition efficiency of 59%, while at the same concentration stem extract showed

IP
the inhibition efficiency of only 15%. The difference in the inhibition efficiencies of different

CR
extracts of the same plant is attributed to the presence of different constituents/phytochemicals in
the extracts of different plant parts. Generally, leaves are relatively richer part of the plants
where the chemical synthesis of the phytochemicals takes place by the process of photosynthesis

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therefore leaves extract should show higher protection ability as compared to the other plant
extract that was observed by Umoren and coworkers. In another study the roots, stem and leaves
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extracts of olive (Olea europaea L.) have been investigated as effective corrosion inhibitors
towards mild steel corrosion in 1M HCl [319]. In the study the authors again observed that
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leaves extract showed the highest inhibition efficiency of 89.83%. Results showed that all
extracts showed the inhibition efficiencies of more than 88% and act as mixed type corrosion
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inhibitors. Among the root (RT) and leaf (LV) extracts of Maesobatrya barteri, the LV showed
better inhibition efficiency towards mild steel dissolution in 1M H2SO4 [320]. The adsorption
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behavior of RT and LV extracts obeyed the Langmuir adsorption isotherm. While, among the
root (RT), seeds (SD) and leaves (LV) extracts of Azadirachta Indica, towards the inhibition
CE

efficiency of mild steel corrosion in 2.0 M H2SO4 follows the order: SD > RT > LV [321].
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4. Challenges and outlooks

The use of plant extracts as metallic corrosion inhibitors is recommended for future research in
the area of corrosion inhibition because they are cost-effective, easily available, biodegradable,
biocompatible, non-hazardous, removable materials, highly effective and environmentally
benign. Recently, application of ionic liquids and compounds synthesized from multicomponent
reactions (MCRs), ultrasound and microwave irradiations and plant extracts has emerged as
green practices for metallic corrosion inhibition. However, numerous aspects need to be taken
into account prior to their use in the real testing environments. Before testing them in real

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environment, the toxicity, bioaccumulation and biodegradability experiments need to be

performed in order to comprehend what is green and what is not. In most of the literature and
articles presented herein, these types of experiments were not carried out and this allows an
exposed subject for the forthcoming studies. Since plant extracts and drugs are derived from
natural and biological systems, there is a high potential to use them as environmentally benign
corrosion inhibitors. Several drugs, chemical compounds and plants extracts were applied
already for diverse industrial applications, where the non-hazardous behaviour was mentioned

T
indirectly (eg. LD50, LC50 and EC50). It has been well established that only a few specific

IP
components of a plant extract are responsible for the inhibition of metallic corrosion and

CR
therefore it is recommended that separation and corrosion inhibition behaviour of each and every
constituent should be carried out. The isolation of the extract constituents (phytochemicals) can

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be easily achieved using GC-MS and HPLC-MS techniques. Additionally, processing (extraction
method) of the extract is one of the most important techniques because of several problematic
AN
aspects such as long processing time and high processing temperature in conventional extraction
procedures. Therefore, there is a high demand of unconventional extraction practices which
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require relatively low processing time and optimum operating temperature. Moreover, the effect
of solvents undertaken for extract preparation on the surrounding environment has also be
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considered as traditional extraction procedures which require the use of highly harmful organic
solvents. Supercritical fluids represent a new class of alternative solvents for the preparation of
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plant extracts which permit selective separation of phytochemicals from the extracts at moderate
temperatures and optimum processing time. Although some reports are available on the effect of
CE

halide and other inorganic ions on the inhibition behavior of plant extras however still there are
sufficient space to use explore phenomenon of synergism. From the reports described herein it
AC

can be predicted that plant extracts are the most effective inhibitors towards metallic corrosion.
Roots, stem, seed and other parts plant extracts have been evaluated but their leaves extract have
not been evaluated therefore it is also recommended that leaves extracts of these plants should be
studied. Considering the huge availability of literature on plant extracts as corrosion inhibitors
particularly for mild steel and aluminum, the use of the extracts should be explored to other
metals and alloys like zinc, nickel and magnesium. In the majority of the researches reported so
far the computational methods are not taken into so much consideration. Recently, computational
techniques particularly density functional theory based quantum chemical calculations and

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molecular dynamics (MD) and/ or Monte Carlo (MC) simulations have emerged as new tools to
describe the effectiveness of a given series of compounds tested as corrosion inhibitors. Each
plant extract contains several constituents (phytochemicals) therefore their relative effectiveness
towards the metallic surface should be determined by these relatively newer and greener
computational techniques. The greenness of these techniques are based on the facts that they
employed software simulations that give reasonably satisfactory prediction about the chemical
reactivity and adsorption behavior of the chemical compounds at the metal/ electrolyte interfaces

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without using any toxic chemicals and solvents. The MD and MC simulation studies can provide

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orientations (horizontal or vertical) of inhibitors (phytochemicals) at the interfaces. In view of

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this, the application of DFT and simulations (MD and MC) studies should be explored in the
field of metallic corrosion inhibition using plant extracts. In summary, isolation and analysis of

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each phytochemicals/ constituents, phenomenon of synergism, use of leaves extracts and
computational (DFT, MD and MC) techniques should be explored in the field of metallic
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corrosion inhibition using plant extracts.

5. Conclusions
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From the ongoing discussion it can be concluded that plant extracts are ideal candidates to
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replace traditional expensive and toxic inorganic and synthetic organic corrosion inhibitors. The
plant extracts contain several phytochemicals/ constituents that can easily adsorb and inhibit
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metallic corrosion. Several types such as leaves, roots, stem and other extracts have been
examined as effective corrosion inhibitors for mild steel, carbon steel, aluminum and other
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metals and alloys in acidic (HCl, H2SO4, HNO3, H3PO4), basic (NaOH) and neutral (NaCl)
media. It is observed that leaf is the phytochemically richest part of the plant where the synthesis
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of phytochemicals takes place. Phenomenon of synergism has also be searched and described
particularly in the presence of halide ions (KX). A significant enhancement in the protecting
ability of the plant extracts have been observed in the presence of halide ions which facilitate the
adsorption of phytochemicals at the metal/electrolyte interfaces. Generally, leaves extract
showed better inhibition performance as compared to the extract of other extracts of the same
plants.

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Acknowledgments

Dr. Verma, thankfully acknowledges the North-West University, Mafikeng Campus South
Africa for providing financial support and scholarship under postdoctoral scheme.

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Abbreviation
WL: Weight loss

GM: Gravimetric

GSM: Gasometric

TM: Thermometric

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HE: Hydrogen evolution

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EIS: Electrochemical impedance spectroscope

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PDP: Potentiodynamic polarization

LPR: Linear polarization resistance

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LP: Linear polarization
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CV: Cyclic voltammetry

PM: Potential monitoring

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CAM: Chrono-amperometric

SEM: Scanning electron microscope

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FESEM: Field Emission Scanning Electron Microscope

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EDX: Electron dispersive X-ray spectroscope

AFM: Atomic force microscope

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AAS: Atomic absorption spectroscope

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OPM: Optical microscope

SI: surface imaging

MM: Metallurgical microscope

XRD: X-ray Powder Diffraction

FT-IR: Fourier-transform infrared spectroscope

UV-Vis: Ultraviolet–visible spectroscope or ultraviolet-visible spectrophotometry

DFT: Density functional theory

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MD: Molecular dynamics

MC: Monte Carlo

QSAR: Quantitative structure–activity relationship

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HIGHLIGHTS
 Present review article describe the collection of green and sustainable corrosion inhibitors

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derived from plants.

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 Based on the literature results, mechanism of phytochemicals has been described.
 Nature adsorption isotherm tested for phytochemicals adsorption have also been

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described.
 Important methods and parameters for extracts preparation have been described.

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 Effect of halide ions (synergism) on inhibition effect of plant extracts have been
surveyed.
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Graphics Abstract