Journal of Molecular Liquids 266 (2018) 577–590

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Journal of Molecular Liquids

journal homepage: www.elsevier.com/locate/molliq

Review

An overview on plant extracts as environmental sustainable and green

corrosion inhibitors for metals and alloys in aggressive corrosive media
Chandrabhan Verma a,b,⁎, Eno E. Ebenso a,b, Indra Bahadur a,b, M.A. Quraishi c,d,⁎⁎
a
Department of Chemistry, School of Chemical and Physical Sciences, Faculty of Natural and Agricultural Sciences, North-West University, Private BagX2046, Mmabatho 2735, South Africa
b
Material Science Innovation &Modelling (MaSIM) Research Focus Area, Faculty of Natural and Agricultural Sciences, North-West University, Private Bag X2046, Mmabatho 2735, South Africa
c
Department of Chemistry, Indian Institute of Technology, Banaras Hindu University, Varanasi 221005, India
d
Center of Research Excellence in Corrosion, Research Institute, King Fahd University of Petroleum & Minerals, Dhahran 31261, Saudi Arabia

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

Article history: Recently, the development of green corrosion inhibitors and green inhibition strategies are highly demanded be-
Received 17 March 2018 cause of the increasing demand of green chemistry in the area of science and technology. In last few decades, use
Received in revised form 11 June 2018 of plant extracts as metallic corrosion inhibitors has attracted significantly attention. Plant materials are ideal
Accepted 26 June 2018
green candidatures to replace traditional toxic corrosion inhibitors. Reduced environmental risk, lower cost,
Available online 30 June 2018
wide spread availability and high corrosion inhibition effectiveness make the plant extracts as suitable candidates
Keywords:
to replace the expensive and toxic traditional synthetic corrosion inhibitors. Literature survey reveals that differ-
Plant extract ent extracts such as leaf, root, stem, bark, pulp, fruit, etc. have been effectively employed as sustainable inhibitors
Green inhibitors for the corrosion of different metals and alloys. Present review article describes the collection of published work
Phytochemicals that has been carried out on the topic “plant extract as corrosion inhibitors for metals and alloys in aggressive
Green chemistry aqueous solutions”. The article includes extracts of diverse part of the plants for diverse metals and alloys in
Metals and alloys the several electrolytic media.
© 2018 Elsevier B.V. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 578
1.1. General introduction of corrosion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 578
1.2. Green corrosion inhibitors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 578
1.3. Important parameters for extract preparation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 578
1.4. Leaf extracts as corrosion inhibitors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 578
1.4.1. Leaf extracts as corrosion inhibitors for mild steel . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 579
1.4.2. Leaf extracts as corrosion inhibitor: Mild steel: HCl system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 579
1.4.3. Leaf extracts as inhibitors: mild steel: H2SO4 system. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 579
1.4.4. Leaf extracts as inhibitors: Mild steel: HCl and H2SO4 system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 581
1.4.5. Leaf extracts as inhibitors: Mild steel/NaCl, petroleum/CO2 system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 581
1.4.6. Leaf extract as inhibitors for mild steel: CH3COOH, HNO3, H3PO4 system. . . . . . . . . . . . . . . . . . . . . . . . . . . . 581
1.5. Other part of the plant extracts as inhibitors for mild steel . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 581
1.6. Plants extracts as corrosion inhibitors for aluminum . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 583

Abbreviations: WL, Weight loss; GM, Gravimetric; GSM, Gasometric; TM, Thermometric; HE, Hydrogen evolution; EIS, Electrochemical impedance spectroscope; PDP, Potentiodynamic
polarization; LPR, Linear polarization resistance; LP, Linear polarization; CV, Cyclic voltammetry; PM, Potential monitoring; CAM, Chrono-amperometric; SEM, Scanning electron
microscope; FESEM, Field Emission Scanning Electron Microscope; EDX, Electron dispersive X-ray spectroscope; AFM, Atomic force microscope; AAS, Atomic absorption spectroscope;
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; MD, Molecular dynamics; MC, Monte Carlo; QSAR, Quantitative structure–activity
relationship.
⁎ Correspondence to: C. Verma, Department of Chemistry, School of Chemical and Physical Sciences, Faculty of Natural and Agricultural Sciences, North-West University, Private
BagX2046, Mmabatho 2735, South Africa.
⁎⁎ Correspondence to: M.A. Quraishi, Department of Chemistry, Indian Institute of Technology, Banaras Hindu University, Varanasi, 221005, India.
E-mail addresses: chandraverma.rs.apc@itbhu.ac.in, (C. Verma), maquraishi.apc@itbhu.ac.in (M.A. Quraishi).

https://doi.org/10.1016/j.molliq.2018.06.110
0167-7322/© 2018 Elsevier B.V. All rights reserved.
578 C. Verma et al. / Journal of Molecular Liquids 266 (2018) 577–590

2. Phenomenon of synergism . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 583

3. Relative effectiveness of different plant extracts . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 583
4. Challenges and outlooks . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 583
5. Conclusions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 585
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 585
References. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 585

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 re-
cent study carried out by NACE 2016 suggests that at global level, corro-
sion causes economic loss of about 2.5 trillion US dollars which
constitutes nearly 3.4% of total GDP. However, by implementation of
existing corrosion preventing technologies in a proper way, the cost of
corrosion can be reduced up to 15–35% (375–875 billion US dollars). Be-
cause of its association with very high economic and safety losses, cor-
rosion 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 [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 ease of
synthesis and application and high effectiveness at relatively low con-
centration. These organic compounds adsorb over the surface of metals
and alloys through their heteroatoms and π-electrons and form protec-
tive surface barrier thereby protect metals from corrosive degradation.
Generally, heteroatoms of organic inhibitors exist in polar functional
groups such as -CN, -NO2, -NH2, -OH, -COOH, -COOC2H5, -OCH3 etc.
those act as 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 polar electrolytic
media like H2O, HCl, H2SO4, H3PO4, HNO3 etc. [14–18].
1.2. Green corrosion inhibitors
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 con-
sciousness 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-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 particu-
larly 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 develop-
ment of green corrosion inhibitors. Plants are characterized by their
unique property to convert radiant energy (sunlight) into life providing
organic compounds (carbohydrates) via the process of photosynthesis.
They are also natural source of several raw materials such as fruit, veg-
etables, 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 to continuous uptake of “greenhouse”
CO2 gas, highly toxic metals and other pollutants 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 environments [50, 51]. Literature revision pro-
poses that till today numerous reviews articles have been documented
for corrosion inhibition such as drugs [38, 52–54], DFT as tool for corro-
sion study [55, 56], chromate independent green corrosion inhibitors
[57–60], organic compounds and ionic liquids as inhibitors [16, 17, 19,
61–67], inorganic corrosion inhibitors [68–70], plant extracts as inhibi-
tors [67, 71–72] and so on. As for as the availability of review 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 papers in which plant extracts have
been tested as corrosion inhibitors for several electrolytic media.
1.3. Important parameters for extract preparation
Nowadays, development of green corrosion inhibitors and inhibition
strategies are 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 de-
tail description of these methods is beyond the scope of the present re-
port. However, the several parameters that should be considered during
preparation of plants extracts are described briefly:
(a) Solvents for extraction: Generally, solvent diffused into plant tis-
sue, solubilized and finally extracted the compounds (phyto-
chemicals) present over there [74, 75]. Therefore, choice of the
suitable solvents for extraction is very important for effective ex-
traction. Extensive literature survey reveals that water is the best
solvent owing to its simplicity, readily availability, non-toxic na-
ture, non-flammable, non-hazardous, uniquely redox-stable, in-
expensive properties [76–79]. However, preparation of some
plant extracts requires organic solvents like ethanol and metha-
nol.
(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 constit-
uents (phytochemicals). Generally, extraction is being carried
out in the 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 room temperature in shade. However, this
type of drying requires several days, weak, even months; there-
fore oven drying has also gained significant advancement.
1.4. Leaf extracts as corrosion inhibitors
Because of the toxic behaviour of traditional corrosion inhibitors for
living being and their non-biodegradable nature, the demand corrosion
 C. Verma et al. / Journal of Molecular Liquids 266 (2018) 577–590
inhibitors of natural and biological origin that have either no or little ad-
verse effect on environment is highly anticipated [82–84]. In this con-
text plant extracts (phytochemicals) are being utilized extensively as
green and effective alternative of tradition toxic corrosion inhibitors.
Leaf is the phytochemically richest part of the plants where the synthe-
sis of phytochemicals takes place. The consumption of plant extracts as
corrosion inhibitors is a green and environmental friendly approach be-
cause most of the phytochemicals are water soluble metabolites like or-
ganic 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, biode-
gradable, and biocompatible and ease of application, several plant ex-
tracts 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 im-
portant to mention that extract every plant extract contains several or-
ganic compounds that can effectively adsorb on metallic surface and
behave as corrosion inhibitors. These organic compounds contain het-
eroatoms 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
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 of the surrounding en-
vironment [96]. Additionally, the synthesis of phytochemical by utiliza-
tion of highly toxic greenhouse gas (CO2) through photosynthesis is
important for another aspect of green chemistry. The phytochemicals
are naturally available in huge 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].
1.4.1. Leaf extracts as corrosion inhibitors for mild steel
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 chemical and electrochemical reactions
with the components of the environment, and thus loss of metal com-
ponent occurs due to corrosion. Several attempts have been made pre-
viously in order to mitigate these unwanted reactions particularly
during some common 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 employed as ef-
fective 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 sur-
face 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 hydrochlo-
ric acid. Since hydrochloric acid is more reactive than sulphuric acid,
pickling is generally carried out in hydrochloric acid solution at lower
temperature, while pickling with sulphuric acid requires higher tem-
perature. Apart from that, the residual chloride (ferrous or ferric) pro-
duced from hydrochloric acid pickling process can be rinsed off more
readily than the residual sulphates (ferrous or ferric) produced due to
579
sulphuric acid pickling. Several leaf extracts have been used as effective
inhibitors for mild steel/HCl system. Soltani et al. [106] described the in-
hibition effect of Salvia officinalis leaves extract on 304 stainless steel
corrosion in 1 M HCl solution using 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 several components of the S. officinalis in
order to describe its inhibition performance. These authors postulated
that out of fifteen active components, the inhibition activities of the S.
officinalis extract is mainly attributed due to presence of phenolic com-
ponents such as 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 ad-
sorption centers. Li et al. [107] studied the inhibition property of
Osmanthus fragran leaves extract (OFLE)) on carbon steel in 1 M HCl.
The study was performed using electrochemical, AFM, FT-IR and DFT
methods. Adsorption of the OFLE on carbon steel 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 corrosion inhibition. The inhibition effect of alkaloids
extract (AE) of Geissospermum leave on C38 steel in 1 M HCl was inves-
tigated by Faustin et al. [108] using electrochemical and surface study
(SEM and EDX) methods. They found that AE acted as good corrosion in-
hibitor 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 AE acted as mixed type in-
hibitor. 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 com-
pound 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 effi-
ciency of N. fruticans with that of 1,5-diphenylcarbazone and observed
that at 30 °C N. fruitcans exhibited 75.11% inhibition 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.
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] investigated the inhibition effect
of Aloe Vera leaf extract on mild steel corrosion in 1 M sulphuric acid
using electrochemical and scanning electron microscopic techniques.
Results 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 1 M H2SO4. The ad-
sorption of Citrus aurantium leaves extracts metallic surface obeyed the
Langmuir adsorption isotherm. The extract exhibited maximum inhibi-
tion efficiency of 89% at 10 mL/L concentration. Quantum chemical cal-
culations of active constituents deliver upright sustenance to the
experimental results. The inhibition effect of Sida acuta [153], African
Perquetina [154], Emblica leaves [155], Cassia tora [156], Nicotiana
tabacum [157], Mangnifera indica [158], Achyranthes aspera [159],
African Breadfruit [160], Jatropha curcas [161], Wrightiatinctoria,
Clerodendrumphlomidis, Ipomoeatrilob [162], Sida acuta [163], Nauclea
latifolia [164], Nypa fruticans Wurmb [165], Spondias cytherea [166],
Combretum bracteosum [167], Hyptis suaveolens [168], Polyalthia
580 C. Verma et al. / Journal of Molecular Liquids 266 (2018) 577–590

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 adsorption Remark Ref.

electrolyte (s)

Olea europaea WL, PDP, CV C-steel/2 M HCl Langmuir, mixed type Hydroxytyrosol and oleuropein were active components [110]
Tabernaemont-ana divaricata WL, EIS, PDP, SEM-EDX Fe/1 M HCl Langmuir, mixed type Maximum efficiency of 95% was achieved at 500 ppm [111]
Phyllanthus amarus WL, EIS, PDP, DFT Fe/1 M HCl Langmuir, mixed type Phyllanthin is the main phytochemical present in P. amarus [112]
Eleusine aegyptiaca and Croton WL, EIS, PDP, FT-IR, Cast iron/1 M Langmuir, mixed type Inhibition performance of these leaves extracts was also [113]
rottleri UV–Vis, SEM, X-ray HCl studied with halide additives (KCl, KBr, and KI)
diffraction
Pimenta dioica EIS, PDP, SEM, AFM, DFT Mild steel/0.5 Langmuir, mixed type Eugenol is major active component which showed [114]
M and 1.0 M comparable efficiency to the P. dioica extract
HCl
Thyme WL, EIS, PDP Mild steel/2 M Langmuir, mixed type Thyme leaves extract attained maximum efficiency of 84% [115]
HCl
(Guatteria ouregou and Simira EIS, PDP, OPM Low carbon Langmuir, Mixed Harmane was identified as the main component of S. [116]
tinctoria) steel/1 M HCl type tinctoria extract
Morusalba pendula EIS, PDP, UV–visible, Steel/1 M HCl Langmuir, mixed type Inhibition efficiency increased from 93% to 96% in presence [117]
FT-IR, AFM of 10 mM KI
Ficus hispida WL, EIS, PDP, XRD, FT-IR, Mild steel/1 M Langmuir, cathodic Maximum %IE was 90% at 250 ppm, stigmasterol was main [118]
EDX HCl type active constituent of F. hispida
Solanam Xanthocarpum WL, GSM, EIS, PDP, MM Carbon steel/1 Langmuir, mixed type Maximum %IE of 83.2 was obtained at 800 ppm [119]
M HCl concentration
Gliricidia sepium WL, FT-IR, SEM-EDX Mild steel/1 M Langmuir isotherm Phytochemical screening suggests the presence of [120]
HCl Saponins, Tannins, Flavonoids, Terpenoid
Rosemarinus officinalis L. GM, PM Mild steel/0.1 – 100% leaves extract gave the 98.33% efficiency [121]
M HCl
Eichhornia crassipes GM, DFT and MD Mild steel/5 M – Higher concentrations and lower temperatures enhances [122]
simulations HCl the efficiency
Murraya koenigii (Curry leaves) WL, GSM, EIS, PDP, SEM Mild steel/1 M Langmuir, mixed type 84.6% IE was obtained at 4% in v/v extract [123]
HCl
Petroselinum crispum (Parsley), Eruca EIS, PDP, SEM Carbon steel/1 Langmuir, mixed type Plant extracts inhibits metallic corrosion be becoming [67]
sativa (Arugula), Anethum M HCl adsorbate at metal surface
graveolens
Eucalyptus Camaldulenis GM technique Carbon Steel/3 Langmuir isotherm Adsorption of E. Camaldulenis is spontaneous [124]
M HCl
Emblica Officinalis WL, UV–visible, FT-IR, Mild steel/1 M Langmuir isotherm highest %IE of 88% at 1000 ppm concentration [125]
SEM HCl
Pterocarpus soyauxi WL, Mild Tempkin and P. soyauxi physically adsorbed on the metallic surface [126]
steel/1–2.5 M Freundlich isotherms
HCl
Plumeria alba, Blighia sapida, GM, OPM Low carbon Langmuir isotherm Blighia Sapida exhibited the maximum inhibition efficiency [127]
Secamone Afezeli steel/1 and 2 M
HCl
Emblica Officinalis WL, UV, SEM Mild steel/1 M – Highest %IE of 88% at 1000 ppm concentration [128]
HCl
Sesbania sesban WL, EIS, PDP Carbon steel/1 Langmuir, mixed type 91.08% IE was obtained at 2.00 g/L concentration [129]
M HCl
Bryophyllum pinnatum GM, SEM Mild steel/0.5 Langmuir isotherm 94.27% IE was obtained at 8 g/L concentration at 298 K [130]
M HCl
Azadirachta Excelsa GM, FESEM Mild steel/1 M Langmuir isotherm 78.55% IE was obtained at 800 ppm concentration [131]
HCl
Boscia senegalensis WL, SEM, EIS, PDP, FT-IR, Mild steel/1 M Langmuir, mixed type Saponins, tannins, phlobatins, anthraquinones, cardiac [132]
DFT calculations HCl glycosides, flavonoids, terpenes, and alkaloids were
components
Acalypha indica WL Mild steel/1 M Temkin isotherm 93.26% IE was obtained at 0.7% inhibitor concentration [133]
HCl
Phoenix dactylifera WL, EIS, PDP, SEM Carbon steel/1 Langmuir, mixed type 97.7% IE was obtained at 2 g/l concentration [134]
M HCl
Ruta graveolens WL, EIS, PDP, DFT Mild steel/1 M Langmuir, mixed type 98.25% IE was obtained 4%v/v of inhibitors [135]
calculations HCl
Annona muricata. L WL, EIS, PDP, SEM Mild steel/1 M Mixed type Photochemical analysis shows the presence of several [136]
HCl constituents
Michelia alba EIS, PDP, SEM, FT-IR, DFT Carbon Langmuir, mixed type 98.4% IE was obtained at 1.686 g/L concentration [137]
calculations steel/mild steel
1 M HCl
Anthocleista Djalonensis WL Mild steel/1 M Langmuir isotherm 97.23%was obtained at 0.6 g/L concentration [138,
HCl 139]
Morinda tinctoria WL, EIS, PDP, Mild steel/1 M Langmuir, mixed type Synergism through KBr, KCl and KI showed significant IE [139]
calorimetric tests HCl increase
Vitex negundo WL, GSM, Carbon steel/1 Langmuir, mixed type 79.2% IE was obtained at 800 ppm extract concentration [140]
electrochemical M HCl
Gymnema Sylvestre WL, SEM, UV, FT-IR and Mild steel/1 M Langmuir isotherm Gymnemic acid, Stigmasterol, Lupeol were main [141]
EDX HCl constituents
Argemone mexicana WL, UV–vis, Mild steel/1 M Langmuir, mixed type 92.5% IE was obtained at 500 mg/L extract concentration [142]
electrochemical, SI HCl
Acalypha torta WL, UV–vis, Mild steel/1 M Langmuir, mixed type Nearly 90% efficiency was obtained at 1000 ppm [143]
electrochemical, SEM, HCl concentration
 C. Verma et al. / Journal of Molecular Liquids 266 (2018) 577–590
Table 1 (continued)
Plant name Technique(s) Metal and
electrolyte
CAM
Podranea ricasoliana WL, FT-IR Mild steel/1 M
electrochemical, SEM HCl
Passiflora foetida WL, SEM, AFM Mild steel/1 M
electrochemical HCl
Shorea Robusta WL Mild steel/1 M
HCl
Funtumia elastica WL, FT-IR Mild steel/1 M
electrochemical, DFT, HCl
MD simulations
Tithonia diversifolia PDP, FT-IR 304 SS/1 M HCl
Gnetum africana WL, electrochemical, Mild steel/1 M
HCl
Lactuca sativa, Eruca Sativa, WL Carbon steel/1
Petroselinum crispum, and Anethum M HCl
Graveolens
Longifolia [169], Buddleia perfoliata [170], Bambusa glauscescens [171],
Bitter leaf (Vernonia amygdalina) [172], Cassava leaves (Manihot
esculenta) [173], Oxystelma Esculentum [174], Stachytarpheta indica
[175], Telferia occidentalis (TO), Azadirachta indica (AI), Occimum viridis
(OV) and Hibiscus sabdariffa (HS) [176] leaf extracts have been investi-
gated as potential corrosion inhibitors for mild steel in sulphuric acid so-
lution using several experimental techniques such as weight loss,
electrochemical, surface investigation and DFT methods. Table 2 repre-
sents some common examples of this type of plant extracts.
1.4.4. 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 ex-
tracts 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], Citrus aurantiifolia [183], Jatropha Curcas
[184], Hibiscus sabdariffa [185], Gnetum africanum, Gongronema
latifolium, Chromolena odaratum [186], Phyllanthus amarus [187], lupine
(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 ad-
sorption isotherm. Adsorption of Trifoliate fenugreek [181] on mild
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 tested solutions
obeyed kinetic thermodynamic model.
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 media. Although, several types of organic com-
pounds have been reported as effective corrosion inhibitors however
the use of plant (leaf) extracts as corrosion inhibitors in these media is
relatively scare. Abdel-Gaber and coworkers [189] studied the inhibi-
tion effect of the olive (Olea europaea L) leaf extract on steel corrosion
in brine solution (saturated solution of NaCl) using electrochemical
and chronoamperometry techniques. The extract exhibited high inhibi-
tion efficiency due to development of cytotoxically sedentary complex
of calcium caffeate. Results further showed that extract inhibits the cor-
rosion 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 re-
ported for inhibition effect of Neem and African star apple leaf extracts
on mild steel corrosion in sodium chloride and polluted seawater
581
Nature of adsorption Remark Ref.
(s)
Langmuir, mixed type Maximum IE was obtained at 3 h immersion time [144]
Langmuir, mixed type 94.61% IE was obtained at 130 ppm concentration [145]
Langmuir isotherm 94.5% IE was obtained at 5 g/L concentration [146]
Langmuir, mixed type 90.1% IE was obtained at 1500 mg/L concentration after 24 [147]
h. Immersion time decreased the efficiency
Mixed type 77.27% was obtained at 2 g/L extract concentration [148]
Langmuir, mixed type 98.37 IE was obtained at 0.5 g/L concentration [149]
Langmuir, Freundlich, Petroselinum crispum extract exhibited maximum IE of [150]
and Temkin isotherm 81.39% at 60%v/v extract concentration
media, respectively [191, 192]. Abd-El-Khalek and coworkers [193]
studied the inhibition behavior of Nicotiana leaves extract on steel cor-
rosion in neutral chloride solution using electrochemical techniques.
Results showed that Nicotiana leaves extract acts as mixed type inhibi-
tor. Aribo et al. [194] studied the inhibition effect of Tridax procumbens
and Chromolaena odorata extracts on stainless steel (UNS S31254) cor-
rosion in a CO2-saturated acidizing oilfield environment. Results
showed that over 90% efficiency was obtained at 100 ppm concentra-
tion of inhibitors. The inhibition mechanism involves formation of
monolayer consisted with Langmuir adsorption isotherm. The inhibi-
tion 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 exhibits the inhibition efficiency of 70–80%
and acts as mixed type inhibitors. Adsorption of the extract over metal-
lic surface obeyed the Langmuir adsorption isotherm.
1.4.6. Leaf extract as inhibitors for mild steel: CH3COOH, HNO3, H3PO4
system
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 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 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 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. 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 on mild steel corrosion in 1 M phosphoric
acid. The extract acts as mixed type inhibitor and its adsorption on the
mild steel surface followed the Temkin adsorption isotherm. The inhibi-
tion effect of Rosmarinus officinalis leaf extract in phosphoric acid solu-
tion has also been investigated elsewhere [198]. The inhibition effect
of Aloe barbadensis (Aloe Vera) on mild steel corrosion in nitric acid so-
lution is reported by Pankaj and Gargi using weight loss method [199].
The extract exhibited maximum efficiency of 89.94% at 0.225 × 10–3 g
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 chemicals occur. How-
ever, there are several parts of the plants such as root [200–202], bark
582 C. Verma et al. / Journal of Molecular Liquids 266 (2018) 577–590

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 steel/1 Langmuir isotherm, It was observed that Aloe Vera lef extract contains Aloesin, Aloin, Aloe and [151]
SEM M H2SO4 mixed type inhibitor Aloe Resin those have –OH, ≥ O, C-O, and O-heterocyclic compounds those
act as adsorption centers

Citrus aurantium WL, SEM Mild steel/1 M Langmuir isotherm Citrus aurantium leaf extract showed highest inhibition efficiency of 89% at 10 [152]
H2SO4 mL/L concentration.
Sida acuta (leaf and stem) WL, AAS, Mild steel/1 M Freundlich adsorption Results showed that both S. acuta leaf and stem extracts act as good [153]
FT-IR, UV H2SO4 isotherm inhibitors and their efficiencies obeyed the order: LV N ST. Results of different
analyses were in good agreement.
African Perquetina GM, GSM Mild steel/2 M Langmuir adsorption A. Perquetina showed maximum %IE of 87.78% at 0.5 g/L concentration. [154]
and TM H2SO4 isotherm Dubinnin-Radushkevich isotherm model showed the adopted corrosion mon-
itoring techniques were in good agreements.
Emblica leaves WL Mild steel/2 M – %IE amplified with rise in concentration and extreme efficiency of 80% and [155]
H2SO4 65% were obtained after 24 and 120 h immersion time.
Cassia tora WL, FT-IR, Mild steel/0.5 M – C. tora showed the maximum %IE of 95.44% at 400 ppm concentration. %IE [156]
SEM H2SO4 gradually decreases on increasing temperature.
Nicotiana tabacum WL, DFT Mild steel/2 M Langmuir adsorption N. tabacum showed maximum %IE of 94.13% at 10 g/L concentration after 6 h [157]
H2SO4 isotherm immersion time. Both experimental and DFT analyses were well validated
each other.
Mango (Mangnifera WL, TM, Mild steel/1 M Langmuir isotherm, M. indica showed optimum %IE of 74.09% at 0.97 g/L concentration at 305.33 [158]
indica) PDP, FT-IR H2SO4 mixed type K temperature and 22.76 h immersion time.
Achyranthes aspera WL Mild steel/0.5 M Langmuir, Frumkin and Results showed that A. aspera is a good corrosion inhibitor and showed the [159]
H2SO4 Flory-Huggins optimum %IE of 92.3%. It adsorb on the mild steel surface by physisorption
adsorption isotherm mechanism.
African breadfrui WL Mild Freundlich adsorption A. breadfrui showed optimum %IE of 70.55% and 78.56% for mild steel and [160]
steel/aluminum 1 isotherm aluminum, respectively.
M H2SO4
Jatropha curcas WL Carbon steel/0.5 – J. curcas exhibited optimum %IE of 92.1% (at 1.5 g/L) and 55.5% (2.5 g/L) in0.5 [161]
M H2SO4 and 0.5 M NaCl and 0.5 M H2SO4.
M NaCl
Wrightiatinctoria, WL, PDP, Mild steel/0.5 M Langmuir isotherm, The optimum %IE was obtained at 200 ppm concentration at 323 K [162]
Clerodendrumphlomidis, EIS, SEM H2SO4 mixed type inhibitor temperature. The %IE obeyed the order: C. phlomidis N I.triloba N W. tinctoria.
Ipomoeatriloba
Sida acuta WL, HE Mild steel/1 M Freundlich adsorption The effect of synergism has been studied in presence of iodide concentration. [163]
H2SO4 isotherm However, %IE decreases with temperature.
Nauclea Latifolia (leaf, WL, GSM Mild steel/1 M Thermodynamic-kinetic The %IE follows the order: RT (94.26%) N LV (91.58%) N BK (75.26%) at 4 g/L [164]
bark, root) H2SO4 model of El-Awady et al. concentration.
Nypa fruticans Wurmb WL Mild steel/0.1, – N. Wurmb showed optimum %IE of 74.48% at 0.5 g/L concentration in 0.5 M [165]
0.5, 1.0 and 2.0 M H2SO4 at 323 K temperature.
H2SO4
Spondias cytherea WL, GSM Mild steel/5 M Langmuir and Freundlich S. cytherea extract showed 67.72% and 72.% efficiency for weight loss and [129]
H2SO4 isotherm gasometric measurements.
Combretum bracteosum WL, HE Mild steel/2 M Frumkin adsorption C. bracteosum showed optimum %IE of 74.76% and 88.31% in 2 M and 5 M [167]
and 5 M H2SO4 isotherm H2SO4, respectively at 30 °C temperature.
Hyptis suaveolens WL, EIS, Mild steel/1 M Langmuir isotherm, H. suaveolens exhibited maximum %IE of 95% at 250 ppm concentration. [168]
PDP, FT-IR, H2SO4 mixed type inhibitor
XRD, SEM
Polyalthia Longifolia WL Mild steel/1 M Langmuir, Temkin, The effect of temperature has also been investigated in the range of 35–75 °C. [169]
H2SO4 Freundlich adsorption it showed optimum %IE of 92% at 1.5% concentration.
isotherms
Buddleia perfoliata WL, EIS, 1018 Carbon Frumkin adsorption B. perfoliata showed highest %IE of 88% at 500 ppm concentration using EIS [170]
PDP,SEM, steel/0.5 M H2SO4 isotherm technique.
UV–Visible
Bambusa glauscescens GSM and Mild steel/2 M Freundlich adsorption B. glauscescens performances as good corrosion inhibitor for mild steel in [171]
OPM H2SO4 isotherm acidic solution and its %IE rises with concentration and accomplish maximum
value 400 ppm concentration
Vernonia amygdalina WL, HE, TM Mild steel/1.5 M Langmuir adsorption V. amygdalina adsorbed by physisorption mechanism. It showed 90%, 84.82%, [172]
H2SO4 isotherm 79.65% and 76.90% at 30°, 40°, 50° and 60 °C temperature at 0.5 g/L
concentration.
cassava (Manihot WL, PDP, Mild steel/0.5 M Langmuir adsorption The inhibition experiment was performed at 0.1%, 0.5%, 1%, 5% and 10% and, [173]
esculenta) SEM H2SO4 isotherm maximum efficiency of 85.87% was obtained at 10% concentration.
Oxystelma esculentum EIS, PDP Mild steel/0.5 M Mixed type inhibitor At 100 ppm concentration it showed %IE of 66.8%. However, in presence of 25 [174]
H2SO4 ppm KI %IE enhanced up to 81.0%.
Stachytarpheta indica WL, HE Mild steel/1 M Langmuir adsorption S. indica spontaneously adsorbed on mild steel surface by physisorption [175]
H2SO4 isotherm mechanism.

[203], flower [204–206], fruit [207–210], wood [211], seed [212–218]
and peel [219–228] that have been employed as efficient corrosion in-
hibitors 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 hexapetalum and Celosia argentea [238], Medicago
Sative [239], Chenopodium ambrosioides [240], Ligularia fischeri [241],
Salvia aucheri mesatlantica [242], Gentiana olivieri [243], Olive pomace
[244], Piper nigrum [245], Cuminum cyminum [246], Uncaria gambir
[246, 247], Acacia tortilis [248], Vernonia Amygdalina [249], Rhus
verniciflua [250], Black cumin (Nigella sativa L.), Halfabar (Cymbopogon
proximus), Chamomile (Chamaemelum mixtum L.) and Kidney bean
(Phaseolus vulgaris L.) [251], Coffee ground [252], Watermelon rind
[253], Pennisetum purpureum [254], Senna alata [255], Acacia nilotica
[256], Justicia gendarussa [257] and Oxandra asbeckii [258].
 C. Verma et al. / Journal of Molecular Liquids 266 (2018) 577–590
1.6. Plants extracts as corrosion inhibitors for aluminum
Similar to the mild steel, aluminum is the widely used metals in var-
ious industries as machinery, reaction vessels, pipes and chemical bat-
tery. The extensive use of the aluminum based on the 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 envi-
ronments like acidic or basic solutions the protective oxide layer dis-
solves resulting into rapid corrosion of the aluminum [259]. The use of
synthetic corrosion inhibitors is the most common measure for protec-
tion of 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 2 M HCl and 2 M
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 N KBr
N KCl. S. trifasciata inhibits the aluminum corrosion by adsorption mech-
anism which follows the Freundlich adsorption isotherm. S. trifasciata
exhibited maximum %IE of 93.6% and 82.3% in 2 M HCl and 2 M KOH, re-
spectively in the presence of KI at 30 °C. There are 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 barteri [276],
Delonix regia [277], Opuntia [278], Ambrosia maritime [279], Ocimum
basilicum [280], Ananas sativum [281], Euphorbia hirta and Dialum
guineense [282, 283], Dendrocalamus brandisii [284], Hibiscus sabdariffa
[285], Chlomolaena odorata [286], Brahmi (Bacopa monnieri) [287],
Gongronema latifolium [288], Capparis deciduas [289], Ipomoea Involcrata
[290], Hibiscus Rosa-sinensis [291], black mulberry (Morus nigra L.)
[292], Solanum melongena L. [293], Ginseng root extract [294],
Rosmarinus officinalis L. [295], Azadirachta indica [296], Aspilia Africana
[297], Laurus nobilis L. [298], Azwain (Trachyspermum copticum), [299],
garlic extract [300], Newbouldia leavis [301], Rosemary leaves extract
[302], Anthocleista djalonensis [303], Ocimum gratissimum [304], Beet-
root (Betanin) [305], Abrus precatorius [306], Newbouldia leavis [307]
and several other plant extracts have also been studied as corrosion in-
hibitors for aluminum. Table 3 represents the collection of few common
plant extracts that have been studied aluminum.
2. Phenomenon of synergism
Obviously, each plant extract contains several active phytochemi-
cals/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
2 M HCl and 1 M H2SO4 gasometric technique at 30 and 60 °C tempera-
tures [178]. From the results derived in the study several interesting
things were observed. In hydrochloric acidic medium, addition of KCl
decreases the protection power of the plant extract. Whereas, addition
of KBr and KI particularly at lower temperature (30 °C) protection effi-
ciency 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 effectiveness of halides obeyed the order:
KI N KBr N KCl. He observed similar observation for the inhibition effect
of Hibiscus sabdariffa on mild steel corrosion in 2 M HCl and 1 M H2SO4
[308]. Similar observation has also been reported on the inhibition effect
of Garcinia kola on mild steel in 5 M H2SO4 [309]. Obot and coworkers
583
[310] described the synergistic effect of KI on the inhibition efficiency
of Aningeria robusta in HCl electrolytic solution. Using hydrogen evolu-
tion method, these authors observed that addition of KI at all studied
concentration of the extract causes noteworthy increase in the protec-
tion ability at both studied temperatures (30 and 60 °C). The A. robusta
extract at 50% v/v concentration showed inhibition efficiency of 48%
only. Addition of KI at 5 mM concentration in the same solution causes
increase in the inhibition efficiency up to 72%. While studding the inhi-
bition effect of Ipomoea invulcrata on aluminum corrosion in 1 M 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 synergism by halide ions have also been re-
ported for other plant extracts such as Sida acuta for mild steel in 1 M
H2SO4 [163], Telfaria occidentalis for mild steel 1 M H2SO4 and 2 M HCl
[312], Ocimum basilicum for aluminum in 2 M HCl and 2 M KOH [280],
bamboo leaf extract for cold rolled steel (CRS) in 0.1 M H3PO4 [313], co-
conut 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 2 M H2SO4
[318].
3. Relative effectiveness of different plant extracts
There are several articles are available in literature in which inhibi-
tion 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 be-
havior 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 0.5 g/L concentration leaves extract showed the inhibi-
tion efficiency of 59%, while at the same concentration stem extract
showed the inhibition efficiency of only 15%. The difference in the inhi-
bition efficiencies of different 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 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 extracts of olive (Olea europaea L.) have been investi-
gated as effective corrosion inhibitors towards mild steel corrosion in
1 M HCl [319]. In the study the authors again observed that leaves ex-
tract 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 inhibitors. Among the root (RT) and leaf
(LV) extracts of Maesobatrya barteri, the LV showed better inhibition ef-
ficiency towards mild steel dissolution in 1 M H2SO4 [320]. The adsorp-
tion behavior of RT and LV extracts obeyed the Langmuir adsorption
isotherm. While, among the root (RT), seeds (SD) and leaves (LV) ex-
tracts of Azadirachta indica, towards the inhibition efficiency of mild
steel corrosion in 2.0 M H2SO4 follows the order: SD N RT N LV [321].
4. Challenges and outlooks
The use of plant extracts as metallic corrosion inhibitors is recom-
mended 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 environmen-
tally benign. Recently, application of ionic liquids and compounds syn-
thesized from multicomponent reactions (MCRs), ultrasound and
microwave irradiations and plant extracts has emerged as green prac-
tices for metallic corrosion inhibition. However, numerous aspects
need to be taken into account prior to their use in the real testing envi-
ronments. Before testing them in real environment, the toxicity, bioac-
cumulation and biodegradability experiments need to be performed in
584 C. Verma et al. / Journal of Molecular Liquids 266 (2018) 577–590

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

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

Gossipium hirsutum (leaf and seed) WL Al/2 M NaOH – G. hirsutum leaf gave 97% inhibition efficiency while the G. [261]
hirsutum seed showed 94% at the 50% v/v concentration.
Phyllanthus amarus WL Al/2 M NaOH Langmuir adsorption Phyllathin hypophyllathin are two main constituents present [263]
isotherm in P. amarus extract. It showed optimum %IE of 76% at 20% v/v
concentration.
Jasminum nudiflorum Lindl. WL, PDP, EIS, Al/1 M HCl Langmuir isotherm, The extract showed optimum %IE of 93.6% at 1 g/L [268]
SEM cathodic type inhibitor concentration. It contains several type of phytochemicals that
can adhere on the metallic surface and inhibit corrosion.
Raphia hookeri WL, TM Al/0.02-2 M Temkin adsorption R. hookeri showed optimum %IE of 65.30% at 0.5 g/L [269]
HCl isotherm, concentration. It spontaneously adsorbed on the metallic
Kinetic–Thermodynamic surface through physisorption mechanism. It showed its best
Model %IE in 1 M HCl.
Thymus algeriensis WL, GSM, EIS 2024 Al/1 M Langmuir adsorption It showed optimum %IE of 78.7% at 0.75 g/L concentration. [270]
HCl isotherm The presence of iodide ions synergistically enhanced the %IE.
Cocos nucifera WL Al/0.5 M HCl Langmuir adsorption C. nucifera showed optimum %IE of 93% at 7.5% v/v [271]
isotherm concentration. It adsorb physically and spontaneously.
Morinda tinctoria WL, PDP, EIS, Al/0.5 M HCl Langmuir adsorption M. tinctoria manifest optimum %IE of 96.72% at 7% [272]
SEM isotherm. concentration. It adsorbed spontaneously.
Terminalia arjuna (TA), Mangifera indica WL, EIS, PDP, Al/1 M NaOH Langmuir adsorption Among the studied extracts, MO showed the maximum [265]
(MI) and Moringa oleifera (MO) SEM, AFM isotherm, mixed type efficiency of 85.3% at 0.6 g/L concentration. SEM and AFM
analyses showed the formation of protective films by the
extracts.
Piper longum WL, PDP, EIS Al/1 M NaOH Langmuir adsorption P. longum showed the optimum %IE of 94% at 400 ppm [266]
isotherm, mixed type concentration. It inhibits corrosion by adsorption mechanism
by creating a barrier for charge transfer.
Nicotiana tabacum WL, EIS, PDP, AA3003Al/0.1 Langmuir adsorption N. tabacum acted as mixed type but predominantly cathodic [273]
SEM, EDX, M HCl isotherm, cathodic type type inhibitor. It showed maximum efficiency of 80% at 1200
AFM, DFT, ppm concentration, experimental results were supported by
MD DFT and MD results.
Cannabis sativa (CS), Rauwolfia serpentina WL, EIS, PDP, Al/1 M NaOH Langmuir adsorption Among these five tested plant extracts RS showed the [267]
(RS), Cymbopogon citratus (CC), Annona SEM, AFM isotherm, mixed type maximum %IE 97.1% at 0.2 g/L concentration. These extracts
squamosa (AS) and Adhatoda vasica (AV) inhibit corrosion by adsorption mechanism which was
supported by SEM and AFM methods.
Vernonia amydgalina WL Al/1 M HCl Langmuir adsorption Increase of the solution temperature decreases the %IE. V. [274]
isotherm amydgalina showed maximum %IE of 91% at 0.09 w/v
concentration
Tender arecanut WL, EIS, PDP, Al/0.5 M HCl Langmuir adsorption T. arecanut acts as efficient inhibitor for aluminum corrosion [275]
AFM isotherm, mixed type and showed optimum %IE of 96.15% at 4.5 g/L concentration.
It contains several phytochemicals those act as active
constituents.
Breadfruit WL Al/0.5 M Langmuir adsorption Breadfruit peel extracts showed the maximum %IE of 853% at [160]
H2SO4 isotherm 145 ppm concentration.
Maesobatrya barteri WL, TM Al/0.5 M and Freundlich adsorption M. barteri showed optimum efficiency of 49.30% at 0.5 g/L [276]
2 M HCl isotherm concentration.

order to comprehend what is green and what is not. In most of the liter-
ature 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 bi-
ological systems, there is a high potential to use them as environmen-
tally benign corrosion inhibitors. Several drugs, chemical compounds
and plants extracts were applied already for diverse industrial applica-
tions, where the non-hazardous behaviour was mentioned indirectly
(eg. LD50, LC50 and EC50). It has been well established that only a few
specific components of a plant extract are responsible for the inhibition
of metallic corrosion and 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 (phytochemi-
cals) can be easily achieved using GC–MS and HPLC-MS techniques. Ad-
ditionally, processing (extraction method) of the extract is one of the
most important techniques because of several problematic aspects
such as long processing time and high processing temperature in con-
ventional extraction procedures. Therefore, there is a high demand of
unconventional extraction practices which require relatively low pro-
cessing time and optimum operating temperature. Moreover, the effect
of solvents undertaken for extract preparation on the surrounding envi-
ronment has also be 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 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 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 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 partic-
ularly for mild steel and aluminum, the use of the extracts should be ex-
plored 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 tech-
niques particularly density functional theory based quantum chemical
calculations and 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
 C. Verma et al. / Journal of Molecular Liquids 266 (2018) 577–590
their relative effectiveness towards the metallic surface should be deter-
mined 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 predic-
tion about the chemical reactivity and adsorption behavior of the chem-
ical compounds at the metal/electrolyte interfaces without using any
toxic chemicals and solvents. The MD and MC simulation studies can
provide orientations (horizontal or vertical) of inhibitors (phytochemi-
cals) at the interfaces. In view of this, the application of DFT and simula-
tions (MD and MC) studies should be explored in the field of metallic
corrosion inhibition using plant extracts. In summary, isolation and
analysis of each phytochemicals/constituents, phenomenon of syner-
gism, use of leaves extracts and computational (DFT, MD and MC) tech-
niques should be explored in the field of metallic corrosion inhibition
using plant extracts.
5. Conclusions
From the ongoing discussion it can be concluded that plant extracts
are ideal candidates to replace traditional expensive and toxic inorganic
and synthetic organic corrosion inhibitors. The plant extracts contain
several phytochemicals/constituents that can easily adsorb and inhibit
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 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 of phytochemicals takes place. Phenomenon of
synergism has also be searched and described particularly in the pres-
ence 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.
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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