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Adsorption removal of malachite green dye from aqueous solution

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DOI: 10.1515/revce-2016-0041

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Kshitij Tewari, Gaurav Singhal and Raj Kumar Arya*
Adsorption removal of malachite green dye from
aqueous solution
DOI 10.1515/revce-2016-0041
Received September 20, 2016; accepted March 6, 2017; previously
published online May 5, 2017
Abstract: In this review, the state of the art on the removal
of malachite green dye from aqueous solution using
adsorption technique is presented. The objective is to criti-
cally analyze different adsorbents available for malachite
green dye removal. Hence, the available recent literature
in the area is categorized according to the cost, feasibility,
and availability of adsorbents. An extensive survey of the
adsorbents, derived from various sources such as low cost
biological materials, waste material from industry, agri-
cultural waste, polymers, clays, nanomaterials, and mag-
netic materials, has been carried out. The review studies
on different adsorption factors, such as pH, concentra-
tion, adsorbent dose, and temperature. The fitting of the
adsorption data to various models, isotherms, and kinetic
regimes is also reported.
Keywords: adsorption; biological adsorbents; magnetic
adsorbents; malachite green; nanomaterials; polymeric
adsorbents.
1 Introduction
Color is a visual pollutant and one of the most important
hazardous species found in industrial effluents. There are
more than 10,000 dyes that are extensively used in many
process industries such as textile, paper, etc. Malachite
green is a commonly used dye. It is an organic compound,
and its molecular structure is shown in Figure  1 (Saha
et al. 2010a). It is known by many other names as aniline
green, Victoria green B, basic green 4, and diamond green
B. It was first prepared by Fischer in 1877 by condensing
benzaldehyde and dimethylaniline in a molecular ratio of
1:2 and in the presence of dehydrating agent.
*Corresponding author: Raj Kumar Arya, Department of Chemical
Engineering, Thapar University, Patiala, Patiala 147004, Punjab,
India, e-mail: rajarya@thapar.edu, rajaryache@gmail.com.
http://orcid.org/0000-0003-1210-108X
Kshitij Tewari and Gaurav Singhal: Department of Chemical
Engineering, Jaypee University of Engineering & Technology, Guna,
A. B. Road, Raghogarh, Guna 473226, M. P., India
Rev Chem Eng 2018; 34(3): 427–453
Malachite green dye is generally used in agriculture,
food, health, textile, and other industries for several pur-
poses. It is highly carcinogenic for species living on water
like fishes, mammals, etc. It is highly toxic in nature, and
its toxicity increases with exposure time, temperature,
and concentration. It causes carcinogenesis, mutagenesis,
chromosomal fractures, respiratory toxicity, etc. Hence,
there is a need to review the various methods available
for its separation and mitigation before discharging it into
water bodies.
In earlier days, malachite green was widely used in
the fish farming industry because of its price and good
efficiency in prevention and treatment of external fungal
and parasitic infection in fish (Li et  al. 2008, Pan and
Zhang 2009). In earlier studies, the researchers found
that it is a hazardous dye that is very harmful for human
beings when inhaled or ingested by the body and creates
irritation when contacted with skin.
There are several techniques to remove malachite
green dye from waste water. The dye can be removed by
coagulation, flocculation, oxidation/advanced oxida-
tion, precipitation, combined chemical and biochemical
processes, ozonation, aerobic and anaerobic diges-
tion, irradiation, adsorption, membrane treatment,
katox treatment (Bekçi et al. 2009), biosorption, fungal
decolonization, ion exchange, and photo degradation
(Debrassi et al. 2012, Song et al. 2012, Pal and Deb 2013,
Ghaedi et al. 2014, Zhang et al. 2016d). Each technique
has its own merits and limitations. Among all the tech-
niques, adsorption is the most effective technique as it is
cheap, fast, and simple (Debrassi et al. 2012, Song et al.
2012, Pal and Deb 2013, Ghaedi et al. 2014, Zhang et al.
2016b,d).
1.1 M
 alachite green dye removal using
adsorption
Among the different types of dye removal methods,
adsorption of a dye over a solid surface is now recognized
as an effective and economical method for wastewater
treatment. There is a great flexibility in design and opera-
tion in adsorption processes. In many cases, adsorption
will produce high-quality treated effluent. Also, in some
cases, recovery of the dye as well as the adsorbent is also
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428      K. Tewari et al.: Removal of malachite green dye
HCL
OH
CH3
N pared adsorbent was treated with formaldehyde and
CH3 N sulfuric acid. The percentage dye removal was 96%. An
CH3
CH3
Figure 1: Structure of malachite green.
possible. A wide variety of adsorbents have been used for
the removal of malachite green dye from wastewater by
various researchers.
Adsorption is the adhesion of atoms, ions, or
molecules from a gas, liquid, or solid to the surface. It
is usually described by isotherm, which is the amount
of adsorbate on the adsorbent as a function of pressure
and concentration at constant temperature. The various
adsorption isotherms used to explain the data are linear
isotherm, Freundlich isotherm, Langmuir isotherm, BET
isotherm, Kisliuk isotherm, Thomas isotherm, Temkin
isotherm, Dubinin-Radushkevich isotherm, Dubinin
Kaganer Radushkevich isotherm, Frumkin isotherm,
Redlich-Peterson isotherm, Sips isotherm, and Koble-
Corrigan isotherm.
The Langmuir and Freundlich models are most com-
monly used due to ease and better prediction capabilities
of the adsorption data. Langmuir equation states that
αp
θ=
1 + αp

where α is Langmuir adsorption constant, θ is frac-
tional coverage of the surface, and p is gas pressure or
concentration.
In Freundlich isotherm, the concentration of a solute
on the surface of an adsorbent is plotted against the con-
centration of the solute in the liquid with which it is in
contact. The Freundlich isotherm is mathematically
shown as
x
1
= kp n
m in the adsorption with a decrease in pH was attributed to

where x is mass of the adsorbate, m is mass of the adsor-
bent, p is equilibrium pressure of adsorbate, k is constant
for a given adsorbate, and n is constant for adsorbent at
given temperature.
2 M
 alachite green adsorption using
various biological wastes
Garg et  al. (2004) prepared the adsorbent from Prosopis
cineraria sawdust – an agro-industry waste – and used
it to remove malachite green in a batch reactor. The pre-
agro-industry waste contains P. cineraria, which is avail-
able in the northern states of India.
Rahman et al. (2005) made similar studies with acti-
vated carbon derived from bamboo, rice husk, or by spent
tea leaves. Rice husk treated with phosphoric acid, sodium
hydroxide, and nitrogen was used to remove malachite
green. They found that the maximum carbonization tem-
perature for effective adsorption was 500°C and the cor-
responding adsorption capacity was 80 mg/g. The derived
activated carbon also gave good removal efficiency.
Kumar et al. (2006) proposed a method for the removal
of malachite green using Pithophora sp., a fresh water
algae. The maximum uptake of the dye was observed at
pH 6. The adsorbent had an adsorption capacity 42.2 mg/g
with a removal of 98.88% at 30°C. The data followed
the first-order kinetics. The dye uptake decreased with
increased adsorbent dosage. This process was found to be
surface diffusion controlled.
Papinutti et al. (2006) used wheat bran to remove the
malachite green. The maximum dye removal was 90% at
pH 7–9. Wheat bran is an inexpensive agricultural residue.
It contains polysaccharides such as starch and cellulose
and is a useful carbon source. This is the main advantage
of wheat bran as compared to other lignocellulosic mate-
rials such as pine sawdust. The maximum dye adsorption
(1)
capacity was 240 mg/g at 28°C.
Hameed and El-Khaiary (2008a) used oil palm trunk
fiber to remove malachite green from an aqueous solution.
The palm trunk was left to dry naturally. The dried trunk
was chopped to pieces 1 in3 in size, ground and sieved to
obtain a particle size range of 0.5 mm. The prepared parti-
cles were washed with boiled water and then dried at 70°C
for 24 h. The maximum dye removal was 82% at pH 10 and
30°C. The maximum adsorption capacity was 149.35 mg/g.
The equilibrium was attained in 140 min. They found that
dye adsorption was unfavorable at pH <4. The decrease
(2)
two reasons. First, as the pH of the system decreased, the
number of negatively charged adsorbents decreased and
the amount of positively charged surface sites increased.
Second, with an excess in H+ ions, lower adsorption of
malachite green took place at acidic pH.
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Khattri and Singh (2009) used neem sawdust as
an adsorbent for the removal of malachite green from
aqueous solution. The neem sawdust was collected from a
local timber industry, boiled with dilute hydrochloric acid
for 30  min, distilled with water, and then dried. It was
finely sieved to particles of 50, 80, and 100  mesh sizes.
The particle size of the adsorbent had significant influ-
ence on the kinetics of adsorption. The adsorption capac-
ity was directly proportional to the total exposed surface
and inversely proportional to the particle diameter. The
adsorption of malachite green increased from 66.75% to
75.78% with a decrease in particle size of the adsorbent
from 50 to 100 mesh at pH 7.2 for solution of 12 mg/l con-
centration. The rate of adsorption increased with the agi-
tation speed. The adsorption process was endothermic in
nature. This adsorbent could not be used on large scale
due to limited availability and high price.
Chowdhury and Saha (2010b) used sea shell powder
to remove the malachite green. Their characterization
showed the presence of -OH, -CO3, and -PO4 functional
groups on the surface of the adsorbent. The maximum
monolayer adsorption capacity was 42.33  mg/g at 303  K
and pH 8. The equilibrium was attained in 2 h. The activa-
tion energy was 15.71 kJ mol−1 for this adsorption process.
Nethaji et  al. (2010) chemically prepared activated
carbon derived from Borassus aethiopum flower and used
it as an adsorbent. They used three different particle sizes
such as 100 μm, 600 μm, and 1000 μm. The maximum
adsorption occurred at pH range from 6 to 8. For the prep-
aration of the biomass, palm flowers were washed and
dried for 48 h and treated with H2SO4 for 48 h. Then, the
carbonized bioadsorbent was washed with water to neu-
tralize and dried at 140°C for 48 h. The dried palm flower
activated carbon (PFAC) was sieved to three mesh sizes
and used as an adsorbent. Malachite green is a basic dye,
and maximum adsorption occurred between pH 6 and 8
for all particle sizes. The percentage adsorption did not
vary much in this range of pH and was 99% for 100 μm,
95% for 600 μm, and 78% for 1000 μm. This shows that
PFAC could be effectively used in this pH range. The effects
of dosages were also studied. The dosages were changed
from 0.0001 g/10  ml to 0.5 g/10  ml. For this change in
dosages, the percentage dye removal was increased from
83% to 99%, 33% to 99%, and 31% to 98% for 100  μm,
600 μm, and 1000 μm size adsorbents, respectively. The
equilibrium was attained at about 1 h for 100 μm, 2 h for
600 μm, and 4 h for 1000 μm size adsorbent.
Chowdhury and Das (2011) used conch shell powder
for the removal of malachite green. The maximum adsorp-
tion capacity was 92.25 mg g−1 at 303 K and pH 8. The data
fitted well to the Langmuir model. The monolayer sorption
K. Tewari et al.: Removal of malachite green dye      429
capacity increased with an increase in the temperature in
the range of 303–333 K. The adsorption was spontaneous
and endothermic in nature. Conch shell powder seems
to be an attractive adsorbent due to its low cost and high
adsorption capacity, and moreover, it does not require any
treatment.
Chowdhury et al. (2011a) used pineapple leaf powder
to remove malachite green. The optimum conditions
found by them were pH: 9.0, initial dye concentration:
50 mg l−1, contact time: 150 min, and bioadsorbent dosage:
5.0 g l−1. The temperature played very important role in this
process. The activation energy was found to be 45.79  kJ
mol−1 for this biosorption process. This study suggested
pineapple leaf powder as potential adsorbent for mala-
chite green removal.
Chowdhury et  al. (2011b) used NaOH treated rice
husk for malachite green removal in batch study. The
adsorption capacity of rice husk also increased with an
increase in the dye concentration from 10 to 100 mg per
liter because it provided the driving force to overcome all
mass transfer resistance between the liquid and the solid
phase. The percentage dye removal was 98.9% at pH 7.
The maximum dye adsorption capacity was 17.98 mg/g at
40°C. The Freundlich isotherm model showed good fit to
the equilibrium data.
Balan et  al. (2012) studied the removal of malachite
green by laccase. The laccase was produced from banana
peel as a solid substrate. They used response surface
methodology to design the optimum conditions. It was
observed that when concentration of malachite green was
95.80  ppm, the concentrations of laccase and 1-hydroxy
benzotriazole were 2.16 U ml−1 and 0.85 m molar, respec-
tively, where 1 enzyme unit (U) is equal to 1 micromole per
minute. The percentage dye removal was 96% in 3.02 h.
Chowdhury and Saha (2012) used chemically modi-
fied rice husk for malachite green removal. The operation
conditions were found using response surface methodol-
ogy. The three independent process variables for optimi-
zation of malachite green were pH of the solution, initial
dye concentration, and adsorbent dose. Their modeling
results showed that maximum dye adsorption will take
place at an initial solution pH of 4 to 10, 100–500  mg/l
initial dye concentration, and 10–50 g/l adsorbent
dosage. The experimentally found optimum conditions
were pH 8.30, 500  mg/l, and 29.31 g/l, respectively, for
initial solution pH, initial dye concentration, and adsor-
bent dose. The removal efficiency was 90.83% at these
conditions. The maximum dye adsorption capacity was
15.49 mg/g.
Singh et  al. (2012) used yeast Saccharomyces cerevi-
siae MTCC 174 to remove malachite green dye. Yeast cells
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430      K. Tewari et al.: Removal of malachite green dye
were collected from a 3 l fermentor. The yeast cell sus-
pension was washed with double distilled water, frozen
at −80°C in deep freezer for 24 h and lyophilized for 48 h
and then heat killed. The dead S. cerevisiae cell suspen-
sion was added to 4% (w/v) sodium alginate solutions
in 1:1 volume ratio and mixed thoroughly. Finally, these
beads were washed with sterile distilled water to remove
excess Ca2+ ions and unentrapped cells before being used
for the adsorption process. The maximum dye adsorption
was 96.25% in 60 min at pH 6.88. The adsorbent was used
several times because maximum desorption was up to
61%. The adsorption data followed pseudo-second-order
kinetics. The adsorption process was spontaneous and
exothermic in nature.
Khan et  al. (2013) used unsaturated polyester phos-
phate from plastic waste bottles to remove malachite
green dye. The dye removal was 98% at pH 8. The process
was spontaneous and endothermic in nature. It was con-
cluded that UPECe (IV) P is an effective cation exchanger
and good adsorbent for malachite green removal.
Lv et al. (2013) used deinococcus radio durans R1 for
malachite green removal. The temperature and pH ranges
were found out to be 25–50°C and 6–8, respectively, for
maximum adsorption. The maximum decolorization
efficiency was 97.2% within 30  min. The maximum dye
adsorption capacity was 7.63  mg/g. Their study demon-
strated that this strain was very efficient to degrade mala-
chite green as compared to other microorganism.
Chen et  al. (2014a) used bamboo leaves to adsorb
malachite green dye. This adsorbent surface contained
the carboxyl and hydroxyl groups on the surface, which
were mainly responsible for adsorption. The percentage
dye removal was 97.6%. The maximum dye adsorption
capacity was 48.3 mg/g at pH 6 in 60 min. The data fol-
lowed pseudo-second-order kinetics and fitted well to the
Langmuir model.
Khan et  al. (2014) used waste pea shells to remove
malachite green dye. The particle size of the shell was
greater than 75 μm. The characterization techniques
showed the presence of hydroxyl and carboxyl groups.
The surface of the adsorbent was heterogeneous. The per-
centage dye removal was 96% in 40 min at pH 7. The data
fitted well to the Freundlich model and followed pseudo-
second-order kinetics. The maximum dye adsorption
capacity was 14.49 mg/g. The adsorption process was con-
trolled by intraparticle diffusion and liquid film diffusion.
The process was spontaneous and endothermic in nature.
Kushwaha et al. (2014) used carrot stem powder and
carrot leaves powder for malachite green removal. The
adsorption process was instantaneous and endother-
mic in nature. The data followed pseudo-second-order
kinetics. The intraparticle diffusion and surface adsorp-
tion were the controlling steps. The maximum adsorption
capacities for carrot stem and leave powers were 43.4 and
52.6 mg/g respectively. The adsorption data fitted well to
the Freundlich model. The adsorption process was spon-
taneous and endothermic in nature and was controlled by
physical adsorption mechanism.
Sharma et al. (2014) used potato peel and neem bark
for malachite dye removal. These two bioadsorbents were
chemically modified by HCHO. The adsorption data for
potato peels and neem bark followed the Freundlich and
Temkin models, respectively. The acid-treated adsorbents
showed the chemisorptions process. The data followed
pseudo-second-order kinetics. The potato peels and acid
treated potato peels gave maximum adsorption at pH 12;
however, neem bark and acid-treated neem bark gave
maximum adsorption at pH 2. The adsorption efficien-
cies were 94.4%, 92.7%, 92.2%, and 82.7% for acid-treated
neem bark, neem bark, potato peels, and acid-treated
potato peels, respectively. The dye adsorption capacities
were 111 and 500 mg/g for acid-treated potato peels and
acid-treated neem bark, respectively.
Mary et al. (2015) used Mosambi peal dust to remove
malachite green dye. They found that 20 min was enough
for 94% dye removal at 0.6 g/l dosage at pH 11. Patra et al.
(2015) prepared bioadsorbents using various biowastes
like sugarcane bagasse, neem leaf, and sawdust. All the
biowastes were pretreated to enhance the surface prop-
erties. They studied the effect of various surface treat-
ments on adsorption capacity. They found 97% removal
efficiency when treatment was done using phosphoric
acid, which was much higher than the removal efficiency
of formaldehyde treated, i.e. 89%. They treated the real
waste water and recorded 79% dye removal for 1 g/100 ml
dosage.
Saygili and Guzel (2015) prepared mesoporous carbon
from industrial grape waste. Their adsorption data fol-
lowed pseudo-second-order kinetics, which follow the
Langmuir model. Their adsorption data showed the pres-
ence of other controlling mechanism besides intraparticle
diffusion. The adsorption process was spontaneous and
endothermic in nature. The maximum adsorption capac-
ity was 667 mg/g.
Song et  al. (2015) synthesized bioadsorbent from
sawdust. They used triethylamine as the modifying agent.
The modified adsorbent was 632.98% more efficient than
the unmodified one. Maximum adsorption capacity was
697.8  mg/g in 6  h at pH 5.08. The adsorption data fitted
well with Freundlich model.
Zhou et  al. (2015) chemically modified cellulose
to remove malachite green. It was modified using two
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chemicals, namely phthalic anhydride and maleic anhy-
dride. The adsorption data followed pseudo-second-
order kinetics and fitted well to the Langmuir model. The
maximum dye adsorption capacity was 111 and 370 mg/g
at pH 6 for phthalic anhydride and maleic anhydride mod-
ified cellulose, respectively. The process was spontaneous
and exothermic in nature.
Asfaram et  al. (2016) used the yarrowia lipolytica
ISF7  strain to remove malachite green. They carried out
a modeling study using response surface methodology.
The maximum dye removal was 99.89% at pH 7 and 25°C.
The maximum dye adsorption was 155.09  mg/g. Chukki
and Shanthakumar (2016) used chrysanthemum indicum
flower to remove malachite green dye. They modeled the
experimental data using response surface methodology.
The maximum dye removal was 99.3% at pH 11 and 30°C
in 75 min.
Das et  al. (2016) designed a continuous fixed-bed
reactor for malachite green dye removal. They used pine-
apple leave powder as an adsorbent. The adsorption effi-
ciency was higher at low flow rate as compared to high
flow rate due to more residence time. The breakthrough
time was increased with an increase in bed height due to
more amount of adsorbent and, hence, higher intake of
the dye. The data fitted well to the Thomas model.
Ren et al. (2016) used garlic root for malachite green
removal. The characterization showed the presence of
hydroxyl and carboxyl groups on the adsorbent surface,
which were mainly responsible for the dye adsorp-
tion. The data fitted well to Langmuir model and fol-
lowed pseudo-second-order kinetics. The maximum dye
adsorption was 232.56 mg/g. The process was controlled
by intraparticle diffusion along with external diffusion
in the boundary layer. The adsorption process was physi-
cal in nature.
Jerold and Sivasubramanian (2016) used brown
marine algae Sargassum swartzii for malachite green dye
removal. The maximum dye adsorption was achieved at
pH 10. The data followed the second-order kinetics and
fitted well with the Langmuir model. NH2, C = O, C-O, and
C-H groups were present on the surface of the adsorbent.
The presence of amino group on the surface had tremen-
dously increased the dye adsorption. The maximum dye
adsorption capacity was 76.92 mg/g. In this case, film dif-
fusion was the controlling mechanism. The adsorption
process was instantaneous and endothermic in nature.
Jothirani et  al. (2016) used modified corn pith for
malachite dye removal. They modified corn pith using
ultrasonic waves. The maximum monolayer adsorp-
tion capacity was 488.3  mg/g at neutral pH in 60  min.
The data followed pseudo-first-order kinetics. The
K. Tewari et al.: Removal of malachite green dye      431
adsorption process was spontaneous and exothermic
in nature. The boundary layer diffusion controlled the
adsorption process to some extent because intraparticle
diffusion was not the only controlling step. Arunadevi
and Venkatachalam (2016) used Ananas comosus leaves
to remove malachite green. The adsorbent was activated
in muffle furnace at 1100°C and was finely powdered.
The maximum dye removal was 90% in 50  min. The
optimum pH was between 2 and 6.5. The data followed
pseudo-second-order kinetics. The adsorption was phys-
ical in nature.
Mullick and Neogi (2016) synthesized activated carbon
from used stevia leaves. It was modified by impregnating
with sodium hydroxide at two different weight ratios. The
dye adsorption capacities were 284.45 and 288.67  mg/g
for the adsorbents having sodium hydroxide in the weight
ratios of 1:1 and 1:2, respectively. This proved that more
amount of sodium hydroxide was not able to enhance the
adsorption capacity. However, the process required some
minimum quantity. The data followed the Freundlich
model and fitted well to pseudo-second-order kinetics.
The process was nonspontaneous and endothermic in
nature.
Pragathiswaran et  al. (2016) synthesized activated
carbon from Gloriosa superba stem. 90.5% dye was
removed at 30°C and pH 6.5 using 250  mg dosage. The
data followed pseudo-first-order kinetics. The adsorp-
tion process was physical and spontaneous having an
endothermic nature. Shamel et al. (2016) used sea shell to
remove malachite green. The results showed the presence
of carboxyl groups on the sea shell, which were mainly
responsible for the adsorption. The dye removal was
89.48% at pH 10. The data followed pseudo-second-order
kinetics.
3 M
 alachite green adsorption using
animal waste
Mittal (2006) used hen feathers for the removal of mala-
chite green from water. Hen feathers collected from local
farm were distilled and then cut into small pieces of about
less than 1  mm long. After cutting, obtained barbs were
treated with hydrogen peroxide and then dried in an oven.
The adsorption studies were carried out at 30, 40, and 50°C
temperatures in batch studies. The maximum dye adsorp-
tion took place at pH 5. The percentage dye removal was
85% and maximum adsorption capacity was 2.93  mg/g
at all the temperatures. The equilibrium was found to be
established rapidly in just 90 min.
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432      K. Tewari et al.: Removal of malachite green dye
Chowdhury and Das (2012) used eggshells to remove
malachite green. Eggshells are freely available domestic
waste. Eggshells were characterized by scanning electron
microscopy, Fourier transform infrared spectroscopy, and
BET analysis. Arrhenius and Eyring equations were used
to determine the activation parameters. The maximum
adsorption occurred at pH 9 in 90 min. The high adsorp-
tion capacity and low cost of eggshells make it attractive
option for dye removal.
4 Adsorption using industrial waste
Gupta et al. (2004) used thermal power plant bottom ash
as a potential adsorbent for the toxic textile dye malachite
green. The bottom ash obtained from a thermal power
plant was washed with double distilled water and dried.
The dried material was treated with hydrogen peroxide,
dried at 100°C and then kept at 500°C for 15  min in the
presence of air. The adsorbent thus obtained was sieved
to the desired particle size. Adsorption studies were per-
formed in batch operations at 30, 40, and 50°C. The adsor-
bent behavior of dye over a wide pH range was studied.
The maximum uptake of malachite green took place at
pH 5.06. The percentage dye removal was 100%. The
maximum dye adsorption capacity was 0.71  mg/g. Their
study clearly indicated the protonation of malachite green
in an acidic medium. The adsorption process was endo-
thermic in nature.
Chowdhury and Saha (2010a) used fly ash for mala-
chite green removal. It is very cheap, being an industrial
by-product. It was treated with alkali to modify its surface
properties. The adsorption process was exothermic in
nature. The adsorption activation energy was 56.08  kJ
mol−1. The adsorption mechanism of alkali-treated fly ash
was intraparticle diffusion controlled. The values of ther-
modynamic parameters ΔG° and ΔH° came out to be nega-
tive, which showed the exothermic nature and feasibility
of adsorption.
5 M
 alachite green removal using
clay adsorption
The clay based adsorbents are much stable and have large
surface area and better structural properties as compared
to activated carbon. These adsorbents are cheaper and
much efficient as compared to activated carbon (Kaya
et al. 2016).
Castellini et al. (2008) used sodium exchange kalonite
to remove malachite green. The clay was treated using
sodium hexametaphosphate and sodium disilicate, which
are widely used deflocculants. They concluded that the
adsorption process was greatly affected by defloccu-
lants. The treatment of disilicate deflocculant increased
the physiosorption and hexametaphosphate defloccu-
lant completely preserved it. The data fitted well to the
Frumkin model. The maximum dye adsorption capacity
was 26.5 mg/g.
Gong et  al. (2009) used monosodium glutamate to
treat sawdust. They compared the performances of crude
sawdust and treated sawdust. The results showed that
the functionalized sawdust had high adsorption capac-
ity as compared to the crude sawdust. The percentage dye
removal was 95% at pH 6. The maximum dye adsorption
capacity was 196.08 mg/g for sawdust with monosodium
glucamate. The data fitted well to the Langmuir model
and followed pseudo-second-order kinetics.
Chaudhuri et  al. (2016) developed a new route
to synthesize Si-MCM-41. It was functionalized with
poly(ethylenimine), aspartic acid, and β-cyclodextrin.
The data followed pseudo-second-order kinetics and
fitted well to the Langmuir model. The maximum adsorp-
tion capacity was 561.45 mg/g in Si-MCM-41-β cyclodextrin
in 40 min. The adsorption process was spontaneous and
endothermic in nature.
Kaya et al. (2016) synthesized a new adsorbent from
sepiolite. In this work, sepiolite was treated by plasma.
The sepiolite is an oxide mineral and is composed of two
tetrahedral silica sheets between octahedral sheets of
magnesium oxide hydroxide. The plasma treatment was
able to produce the carbonyl, hydroxyl, and carboxylic
acid on the surface. The plasma-treated sepiolite was 29%
more efficient than the raw sepiolite and has 42% more
surface area than the raw sepiolite. The adsorption data
fitted well to the Freundlich model. The maximum mon-
olayer adsorption capacity was 143 mg/g at pH 8.
Tian et al. (2016) used diatomite for malachite green
dye removal. They found that diatomite consists of cir-
cular sieve tray type structure and had very high surface
area 46.09  m2 g−1. The pore sizes were in the range of
80–250  nm. The equilibrium was achieved in 90  min
at pH 7 and the maximum dye removal was 93.72%.
The maximum adsorption capacity was 23.64  mg/g at
25°C. The data followed pseudo-second-order kinetics
and fitted well to the Langmuir model. The adsorption
process was spontaneous and endothermic in nature and
was not only controlled by intraparticle diffusion mecha-
nism. They observed the chemisorption as the controlling
mechanism.
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6 M
 alachite green removal using
radiation
Behnajady et  al. (2008) used radiations/ultrasonic tech-
niques to remove malachite green from aqueous solution.
The dye degradation followed first-order kinetics and
hydroxyl radicals had an important role in the degrada-
tion of malachite green. The dye degradation increased
with the increase in temperature.
Han et al. (2010) used natural zeolite to remove mal-
achite green. The microwave irradiations were used to
enhance the adsorption through the regeneration of the
adsorbent. The data were analyzed using the Koble-Corri-
gan model. The adsorption data followed pseudo-second-
order kinetics. The maximum adsorption capacity was
27.34 mg/g at pH 2 and 45°C.
7 Polymeric adsorbent
Chen et  al. (2009) prepared an adsorbent using a series
of polyethylene glycol surfactants for the extraction of
malachite green from aqueous solution. They found that
there was no significant effect of malachite green between
pH 2 and 6.5. The extraction efficiency of malachite green
increased with temperature in the range of 20–60°C and
leveled off beyond 60°C. This happened because the criti-
cal micelle concentration of nonionic surfactant decreased
at a higher temperature, which tends to increase the
micelle amount. Therefore, the extraction efficiency of the
solute increased with the increase in temperature. The dye
removal was 92.14% at 69°C and pH 6.5.
Kagalkar et al. (2011) developed a cell culture, Blumea
malcolmii hook, in a laboratory and used it for malachite
green removal. These cells are highly capable of degrad-
ing a high concentration of dye with a percentage removal
of 93.5% within 24 h at 23–27°C for an initial dye concen-
tration of 20  mg l−1. They studied the effect of dye con-
centration also and found that percentage decolorization
decreased with the increase in dye concentration.
Hasnain et al. (2012) activated poly(urea) using bio-
logical method. This activated poly(urea) was used for
malachite green removal. They prepared polymer metal
complex using condensation polymerization with tran-
sition metals. Transition metal poly(urea) treated with
toluene 2,4-diisocyanate was able to remove 84.60% of
the dye. Leite et al. (2012) used poly(urethane) foam for
malachite green removal. This foam was treated with
sodium dodecylsulfate before use. The data followed sec-
ond-order kinetics. The dye removal was 96% in 60 min.
K. Tewari et al.: Removal of malachite green dye      433
There was no effect of pH on dye removal between pH 2
and 10.
Zhang et  al. (2012) used macroporous versicolor
laccase to remove malachite green. Trametes versicolor
laccase was encapsulated in strong basic exchange resin
D201. The laccase was added into the dye solution and
was magnetically stirred at 25°C. This hybrid biocatalyst
had outstanding resistance and high regeneration ability.
The percentage dye removal was 87% at pH 3–7 and tem-
perature 30–60°C.
Dong et al. (2013) prepared poly(urethane)-attapulgite
porous adsorbent from poly(ether polyol), acid-activated
attapulgite, and toluene diisocyanate. They also used
sodium bicarbonate as foaming agent. Dibutylbis tin was
used as catalyst. Silicon oil was used as a stabilizer. The
percentage dye removal was 99.51%. The maximum dye
adsorption capacity was 47.985  mg/g. The data followed
pseudo-second-order kinetics. The adsorption was spon-
taneous and endothermic in nature.
Bildik et  al. (2014) used crosslinked poly(styrene)-
based quaternary ethyl piperazine resin for malachite
green removal. The maximum dye adsorption capacity
was 450 mg/g. The adsorption data followed second-order
kinetics.
Patel and Hota (2014) synthesized poly(acrylonitrile)
nanofibers membrane using electrospinning method.
These membranes were modified using sodium bicarbo-
nate and sodium hydroxide. The pore size of the fiber was
3.48 nm. These nanofibers were excellent in dye removal
and 99% dye was removed in 30 min at pH 5. The maximum
dye adsorption was 1038 mg/g, which was 5 times higher
than for unmodified poly(acrylonitrile) nanofiber mem-
brane. The data followed pseudo-second-order kinetics
and fitted well with the Langmuir model. The adsorption
was spontaneous and endothermic in nature.
Pourjavadi et al. (2014) synthesized hydrogel of kappa-
carrageenan grafted poly(acrylic acid)/TiO2-NH2. Kappa-
carrageenam is a biopolymer. This nanocomposite was
prepared using graft copolymerization. Their characteri-
zation showed 3D porous network in the gel. The presence
of negative charged ion, i.e. OSO−3 , -COO−, hydroxyl group
polymer chains, and amine (-NR2), was mainly responsi-
ble for dye adsorption. The data followed pseudo-second-
order kinetics and fitted well to the Langmuir model. The
maximum adsorption capacity was between 833.33 and
666.66  mg/g for kappa-carrageenan grafted poly(acrylic
acid) and kappa-carrageenan grafted poly(acrylic acid)/
TiO2-NH2, respectively, at pH 7.
Qin et  al. (2014) synthesized graphite oxide/
poly(urethane) foam for malachite green removal. It was
prepared using foaming technique. The prepared foam
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434      K. Tewari et al.: Removal of malachite green dye
had more interconnected open pores of 0.136 mm diameter
size. The percentage dye removal was 99.7% at 50°C in 3 h.
The maximum dye adsorption capacity was 68.823 mg/g.
The data followed pseudo-second-order kinetics and
fitted well to the Langmuir model. The adsorption process
was spontaneous and endothermic in nature. This process
was chemically controlled.
Sarkar et  al. (2014) synthesized the biodegradable
grafted copolymer for malachite green removal. It was
synthesized using poly(acrylic acid) and amylopectin.
The point of zero charge was 5.51 and the polymer network
expanded at pH higher than the point of zero charge
due to chain dissociation to form carboxyl group, which
enhanced the dye adsorption due electrostatic attraction
between dye and polymer chains. The percentage dye
removal was 99.05% in 30  min. The maximum adsorp-
tion capacity was 352.11 mg/g at 35°C. The data followed
pseudo-second-order kinetics and fitted well to the Lang-
muir model. The adsorption process was spontaneous
and endothermic in nature. The authors suggested simul-
taneous intraparticle diffusion and surface adsorption in
this case.
Zheng et  al. (2014) prepared several granular com-
posite hydrogels via facile polymerization. They used
chitosan as backbone and acrylic acid and itaconic acid
as monomers. They used 5% attapulgite, and it was
enough to enhance the adsorption rate and capacity of
the adsorbent. The presence of large amount of -COOH
groups enhanced the electrostatic attraction between dye
and adsorbent. The maximum adsorption capacity was
2433 mg/g between pH 4 and 10.
Zhou et  al. (2014) modified cellulose to remove
the malachite green. The equilibrium was reached in
180  min at pH 7 and 40°C. The percentage dye removal
was 95% and the maximum dye adsorption capacity was
131.93  mg/g. The data fitted well to the Langmuir model
and followed pseudo-second-order kinetics. The adsorp-
tion process was spontaneous and endothermic in nature.
The used adsorbent was regenerated using HCl and was
used six times without loss of adsorption efficiency.
El-Bouraie (2015) functionalized poly(urethane) foam
with salicylate, a renewable material, to remove malachite
green. They used this adsorbent to treat the textile waste-
water. The maximum dye removal was 95% at pH 10. The
adsorption was physical in a monolayer formation. The
adsorption process was spontaneous and endothermic in
nature.
Kaith et  al. (2015) synthesized gum rosin alcohol-
poly(acrylamide) adsorbent using N,N″-methylene-
bis-acrylamide. They used potassium persulphate as a
crosslinking agent. This adsorbent was able to remove
83% dye. The maximum adsorption capacity was 1.4 mg/g.
The adsorption data followed pseudo-second-order kinet-
ics and fitted well to the Langmuir model. The adsorp-
tion process was not spontaneous and was exothermic in
nature.
Li et al. (2015b) prepared composite foam of chitosan
and poly(urethane). They changed the chitosan content
from 5 to 25  wt%. The foam prepared had an open cell
structure. The maximum percentage dye removal was
95.60% in 12  h at 20% chitosan, pH 9, and 30°C. The
adsorption data followed pseudo-second-order kinetics
and fitted well to the Langmuir model. The maximum
adsorption capacity was 16.67 mg/g.
Zheng et  al. (2015b) synthesized granular hydrogel
using poly(acrylic acid) and gelatin was grafted in it.
The presence of abundant functional groups in gelatin
enhanced the adsorption capacity by manifold. The
maximum adsorption capacity of this gelatin grafted
granular hydrogel was 1370 mg/g. This adsorption mecha-
nism was controlled by electrostatic mechanism.
Dash et  al. (2016) fabricated inexpensive
poly(ethyleneimine) functionalized coal fly ash for mala-
chite green removal. The modification was done using
the wet impregnated method. The functionalized fly ash
had particle size in range of 25–55  nm and were in the
shape of a nanorod. The characterization showed the
presence of nitrogen containing function groups on the
surface of modified fly ash. These groups enhanced the
dye adsorption to a large extent. The data followed sec-
ond-order kinetics and fitted well to the Langmuir model.
The maximum adsorption capacity was 174.83  mg/g at
pH 8 and 35°C. There was no change in the structure of
adsorbent, which confirmed that adsorption was physical
in nature. The adsorption was instantaneous and endo-
thermic in nature. The entire adsorption process was con-
trolled by intraparticle diffusion along with external mass
transfer.
Fu et  al. (2016) synthesized poly(dopamine) micro-
spheres by facile oxidation polymerization. The point of
zero charge was at 3. The surface area was 13 m2 g−1. The
results showed very good adsorption for cationic dyes.
The presence of hydroxyl groups on the adsorbent surface
played an important role in the dye adsorption. The per-
centage dye removal was 91.98%. The adsorption data fol-
lowed pseudo-second-order kinetics and fitted well to the
Langmuir model.
Kaith et  al. (2016) synthesized nanocompoiste using
gum zanthan/psyllium. It was prepared using microwave
synthetic route. The nanocomposite was semicrystalline
in nature and the shape was cubic of size 100 nm. The dye
removal was 83% in 28 h. However, 67% was removed in
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12 h and the maximum adsorption capacity was 3.21 mg/g.
The data fitted well to the Freundlich model.
Kumari et  al. (2016) synthesized lignin-based
poly(urethane) foam. They used lignocellulosic biomass
to functionalize poly(urethane). They synthesized
poly(urethane) using polyol. The adsorption of dye was
spontaneous and endothermic in nature. The maximum
adsorption capacity was 80 mg/g and the adsorbent was
repeatedly used 20 times without much loss of efficiency.
The data followed pseudo-second-order kinetics and
fitted well to the Langmuir model. They suggested chem-
isorption as the controlling step for this case.
Tang et  al. (2016) synthesized mesoporous material
based on lignin sulfonate. It was prepared by grafting
poly(acrylic acid r-acrylamide) onto a lignin sulfonate
molecule. They observed a 37% difference in adsorption
capacities of mesoporous and normal lignin sulfonate.
The maximum dye adsorption was 97  mg/g at pH 7 in
240 min. The data followed pseudo-second-order kinetics
and fitted well to the Langmuir model. In this case, the
intraparticle diffusion step was not the only controlling
step. The adsorption energy data suggested the physical
adsorption process. The adsorption was instantaneous
and endothermic in nature.
8 M
 alachite green removal using
membrane adsorption
Sayılkan et  al. (2007) used nanofiber membrane coated
with Sn doped TiO2. The prepared nanofiber membranes
were used to degrade malachite green dye under UV irra-
diation. The organic compounds present in TiO2 film were
broken down in the presence of ultraviolet light. These
nano-TiO2-coated membranes were repeatedly used to
degrade malachite green. The degradation of dye was
90–94% at 240°C for initial dye solution of 5.2 mg l−1. This
application had not been used commercially because of
the cost and difficulty in the separation of TiO2 nanoparti-
cles for the suspension.
Yin et al. (2016) synthesized coal-based carbon mem-
brane for malachite green removal. The coal-based carbon
membrane was made of anode that was coupled with an
electric field. The dye was completely adsorbed by the
membrane within 0.5 to 1 h in the absence of electric field.
The membrane got saturated in 3 h and malachite green
started coming out from the membrane. The dye never
appeared again in the presence of electric field. The dye
removal was enhanced significantly due to electrochemi-
cal anodic oxidation.
K. Tewari et al.: Removal of malachite green dye      435
9 M
 alachite green removal using
oxidation
Moumeni and Hamdaoui (2012) used bromide ion to
degrade malachite green. They used sonochemical oxi-
dation process for the destruction of malachite green
from water. In this process, bromide ions worked as a
degrading agent for malachite green. The adsorption of
malachite green on bromide ions was a viable oxidation
process. Bromide ions had better advantage as compared
to the other oxidation processes due to its natural environ-
ment. The degradation efficiency was 87% at 25°C and pH
5.3 for an initial dye concentration of 5 mg/l.
10 M
 alachite green adsorption
using nanomaterials
Dong et al. (2012) used mesoporous carbon CMK-3 for mal-
achite green removal. The pore size was around 3–4 nm.
The surface area and pore volume were 1335  m2 g−1 and
1.42 cm3 g−1, respectively. The equilibrium was achieved in
30 min. The maximum adsorption capacity was 625 mg/g.
The data followed pseudo-second-order kinetics and
fitted well to the Langmuir model.
Geng et  al. (2012) synthesized reduced graphene
oxide-Fe3O4 nanoparticles for malachite green removal.
The nanoparticle size was highly tunable. The pore size
was around 10 nm. This adsorbent had very unique prop-
erties, like high surface area and excellent dye adsorption
for multi dye cocktail.
Chang et al. (2013) synthesized porous carbon nano-
sphere using hydrothermal activation with zinc chloride.
The structure of porous carbon nanospheres was tuned
from micropores to mesopores by adjusting the mass frac-
tion of zinc chloride, carbon nanosphere, and activation
temperature. The maximum dye adsorption capacity was
1455 mg/g. The data followed pseudo-second-order kinet-
ics and fitted well to the Langmuir model. The process
was chemical controlled. The adsorbent was used in
five consecutive cycles without any loss in dye removal
efficiency.
Shirmardi et  al. (2013) functionalized multiwalled
carbon nanotubes by acid treatment. These functional-
ized multiwalled carbon nanotubes were used to remove
malachite green. The percentage dye removal was nearly
98%. The maximum adsorption capacity was 142.85 mg/g
at pH 11. The data fitted well to the Langmuir model and
followed pseudo-first-order kinetics.
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436      K. Tewari et al.: Removal of malachite green dye
Ghaedi and Mosallanejad (2014) prepared activated
carbon loaded with cadmium hydroxide nanowires. The
adsorbent prepared had 1271 m2 g−1 surface area and pore
size of 35 Å with average particle size of less than 50 Å. The
maximum dye adsorption capacity was 80.6 mg/g at pH 5
and 25°C. The data fitted well with the Langmuir model.
The adsorption kinetics was of second order. The adsorp-
tion process was spontaneous and endothermic in nature.
Ghaedi et  al. (2014) synthesized activated carbon
loaded with zinc oxide nanoparticles. The surface area,
pore sizes, and particle sizes were >603  m2 g−1, <61 Å,
and <100 Å, respectively. The presence of highly reac-
tive atoms and functional groups was mainly responsi-
ble for the dye removal. The percentage dye removal was
95% at pH 7 in 15 min. The maximum adsorption capac-
ity was 322.58  mg/g. The data followed pseudo-second-
order kinetics and fitted well to the Langmuir model. The
intraparticle diffusion was the rate controlling step in the
system studied.
Roosta et  al. (2014) removed malachite green using
activated carbon loaded with gold nanoparticles. The
particle sizes were in the range of 20–60 nm. The surface
area of the adsorbent was 1229 m2 g−1. They optimized the
adsorption conditions using central composite design and
response surface methodology. The experimental data
fitted well to the Langmuir model and followed pseudo-
first-order kinetics. The percentage dye removal was 99.6%
in 4.4 min at pH 7. The maximum adsorption capacity was
172  mg/g. The adsorption process was spontaneous and
endothermic in nature.
Naseri et  al. (2015) used graphene nanosheets for
malachite dye removal. The adsorption data followed
pseudo-second-order kinetics and fitted well to the Lang-
muir model. The removal of dye was spontaneous and
endothermic in nature. The optimum pH for the adsorp-
tion was 5.
Abou-Gamra and Ahmed (2015) synthesized titania
nanopartciles using the sol-gel process to remove mala-
chite green. They used chitosan to increase surface area
and to control the pore and particle structure. The parti-
cles prepared were around 25  nm. The dye removal was
very fast and 85% dye was removed in 30 min. The adsorp-
tion process was spontaneous endothermic process with
second-order kinetics. Their data indicated film diffusion
as the controlling mechanism. The maximum adsorption
capacity was 6.3 mg/g.
Azad et  al. (2015) prepared activated carbon loaded
with zinc oxide nanorod. They used this adsorbent with
ultrasonic wave for malachite green removal. The adsorp-
tion was enhanced to a great extent due to high-pressure
shock waves from the ultrasonic waves. Dye removal
efficiency was 99% at pH 6. The amount of dye adsorbed
was 59.17  mg/g. The adsorption data fitted well to the
Langmuir model which, suggested the monolayer adsorp-
tion mechanism as the controlling step.
Banu and Maheswaran (2015) impregnated Eichor-
nia crassipes biomass with transition metal salt to get
nanocrystalline embedded activated carbon. This was
used to remove malachite green. The size of the adsor-
bent particle was 7.2958  nm. The scanning electron
microscope graphs confirmed the presence of macropo-
res and mesopores. The nanocrystallites present in the
activated carbon showed the catalytic effect. The adsorp-
tion kinetics followed pseudo-second-order mechanism
and adsorption isotherm followed the Freundlich model.
The maximum adsorption capacity of the adsorbent was
121.1  mg/g. Their calculated apparent adsorption energy
came out to be −198.9 J mol−1, which indicated the physical
sorption.
Gautam et  al. (2015) synthesized bimetallic Fe-Zn
nanoparticles using coprecipitation method for mala-
chite green dye removal. The adsorption data followed
pseudo-second-order kinetics and fitted well to the Lang-
muir model. The adsorption process was spontaneous
and endothermic in nature. They found that ion exchange
was the controlling mechanism for dye adsorption. The
maximum dye removal was 95% and maximum dye
adsorption of 21.74  mg/g was observed in 60  min at pH
9. The adsorbent was reused seven times with more than
70% removal efficiency.
Geetha et  al. (2015) synthesized alginate nanopar-
ticles crosslinked with calcium using green method for
malachite green removal. The analysis showed the pres-
ence of carbonyl and hydroxyl groups on the adsorbent
surface. 98.5% dye was removed in 5  min at pH 10 and
60°C. The data followed pseudo-second-order kinetics
and fitted well to the Langmuir model, which confirmed
the monolayer adsorption mechanism. The adsorption
process was spontaneous and endothermic in nature.
Hashemian et  al. (2015) synthesized manganese
ferrite spinel using coprecipitation method for malachite
green removal. The synthesized adsorbent particles were
of nanosize. Maximum adsorption was achieved in 30 min
at pH 2. The adsorption process followed pseudo-second-
order kinetics.
Mohammadifar et al. (2015) prepared nano-γ-alumina
nanoparticles to adsorb malachite green dye. These par-
ticles were modified using sodium dodecylsulfate. The
maximum sorption capacity was 72.4  mg/g. Roosta et  al.
(2015) synthesized copper nanowires and loaded them on
activated carbon for malachite green removal. They opti-
mized the adsorption condition using central composite
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design. The dye removal was over 99% in a very short time.
The adsorption capacity was 34 mg/g in 6 min at pH 5.5.
Sadegh et  al. (2015) used carboxylate functionalized
multiwalled carbon nanotubes to remove malachite green.
They got the maximum adsorption capacity of 49.45 mg/g
at 298 K and pH 6 in 50 min. The adsorption isotherm fol-
lowed the Langmuir model with pseudo-first-order rate
kinetics. They studied microwaves assisted adsorption of
malachite green.
Agarwal et  al. (2016a) prepared Ni(OH)2 nanoplates.
They used these nanoplates to modify the activated carbon
for malachite green dye removal. The modified activated
carbon had a very high surface area, i.e. 960 m2 g−1, and
a very low pore size of less than 3.5 nm. The presence of
negative hydroxyl ion had tremendously improved the
adsorption capacity of the cationic dye. These properties
of the adsorbent enhanced the malachite green removal
to a very large extent. Around 99.8% dye was removed in
20 min at pH 6.5. The maximum adsorption capacity was
76.92 mg/g. The adsorption data followed pseudo-second-
order kinetics and fitted to the Langmuir model. The
adsorption process was spontaneous and endothermic in
nature.
Agarwal et  al. (2016b) synthesized iron nanoparti-
cle loaded ash from Rosa canina L. leaves for malachite
green dye removal. The dye adsorption was rapid, and
maximum adsorption was achieved in 5 min and equilib-
rium was achieved in 30 min. The dye removal was 81% in
30 min. The maximum adsorption capacity was 500 mg/g.
The data followed pseudo-second-order kinetics and
fitted well to the Langmuir model. The adsorption was
instantaneous and endothermic in nature.
Ghaedi et  al. (2016) synthesized zinc oxide nanorod
loaded activated carbon. This adsorbent was used to
adsorb malachite green dye. The adsorption data followed
pseudo-second-order kinetics and fitted well to the Lang-
muir model. They optimized the conditions using genetic
algorithm and central composite design.
Li et  al. (2016) prepared a novel adsorbent. The
adsorbent was prepared by N-doping of carbon nano-
tubes into CU2O nanoparticles. The hybrid mesoporous
structure of this adsorbent gave an excellent adsorption
capacity of 1495.46 mg/g for malachite green dye, which
was more than 3 times that of pure carbon nanotubes,
i.e. 417.58  mg/g. The percentage dye removal was more
than 99%. The data followed pseudo-second-order kinet-
ics. Their data showed that the chemical reaction might
be controlling the adsorption process. The adsorption
process was spontaneous and endothermic in nature.
Liu et al. (2016b) synthesized octahedral zinc oxide/
ZnFe2O4. This synthesis was surfactant-free and had a
K. Tewari et al.: Removal of malachite green dye      437
heterogeneous structure. The prepared adsorbent had a
surface area of 60.45 m2 g−1, pore volume of 0.94 cm3 g−1,
and average pore of 39.9  nm. They tested this adsorbent
on several dyes. The percentage dye removal was 99.5%.
The adsorption capacity for malachite green of this adsor-
bent was tremendously high and was 4983  mg/g. They
observed three distinct regions during the adsorption
process: a clear intraparticle diffusion, dye diffusion into
the pore, and a flat region on top showing the exhausted
pore volume. The adsorption data fitted well to the Lang-
muir model.
Mansa et  al. (2016) prepared glycine-modified silica
nanoparticles using sol-gel process to adsorb malachite
green dye. The adsorption data followed pseudo-first-
order kinetics and fitted well to the Langmuir model. The
optimum pH for this adsorbent was 10 with 92.5% removal
efficiency.
Nekouei et  al. (2016) synthesized cuprous iodide-
cupric oxide nanocomposite loaded on activated carbon
for malachite green removal. The nanocomposite was
synthesized using solvothermal method and worked well
at neutral pH. The equilibrium was achieved in 20  min.
The maximum adsorption capacity was 136.57 mg/g. The
adsorption process was very spontaneous and endo-
thermic in nature, which followed pseudo-second-order
kinetics.
Rajabi et  al. (2016) used multiwalled carbon nano-
tubes for malachite green removal. These multiwalled
nanotubes were functionalized using carboxylate group.
The optimum pH and time were 9 and 10 min, respectively.
The data followed pseudo-second-order kinetics and fitted
well to the Langmuir model. The hydroxyl groups, carbox-
ylic groups, and aromatic rings were mainly responsible
for dye adsorption and the maximum adsorption capacity
was 11.73 mg/g.
Rong et  al. (2016) prepared multiwalled carbon
nanotubes functionalized with glucose for malachite
green removal. The percentage dye removal was 84.7%
in 60 min. The data followed pseudo-second-order kinet-
ics and fitted well to the Langmuir model. Tripathi et al.
(2016) synthesized large-pore, high-surface-area carbon
nanoparticles using sol-gel process for malachite green
removal. The surface area of this adsorbent was 1441 m2 g−1
with large pore volume of 1.7 cm3 g−1. The maximum dye
adsorption was 1390 mg/g.
Zhang et  al. (2016a) removed malachite green using
zinc nanoparticles. The dye removal was extremely high
due to strong electrostatic attraction, hydrogen bonding,
and chemical precipitation. The maximum dye adsorp-
tion capacity was 2963 mg/g in 120 min. The data followed
pseudo-second-order kinetics. The adsorbent showed
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438      K. Tewari et al.: Removal of malachite green dye
good repeated use until five cycles without any loss in
adsorption efficiency. The process was spontaneous and
endothermic in nature and was controlled by external
mass transfer followed by intraparticle diffusion.
Dil et al. (2017) prepared activated carbon loaded with
copper oxide nanoparticles. The adsorbent particle sizes
were in the range of 50–100 nm and were almost spheri-
cal in shape. The adsorbent prepared was assisted by
ultrasonic waves to enhance the malachite green removal.
They used chemometric optimization and modeling tech-
nique to treat the data. The maximum adsorption capac-
ity was 87.719  mg/g in 5  min at pH 6. The data followed
pseudo-second-order kinetics and fitted well to the Lang-
muir model.
11 M
 alachite green adsorption
using metal organic framework
Huo and Yan (2012) synthesized metal-organic framework
MIL-100(Fe) for malachite green removal. This framework
was highly porous, with heterogeneous surface due to
presence of various functional groups. The maximum dye
adsorption capacity was 146 mg/g at pH 5. The adsorption
data followed pseudo-second-order kinetics and fitted
well to the Freundlich model. The process was spontane-
ous and endothermic in nature. The authors suggested
that intraparticle diffusion mechanism was not the con-
trolling mechanism.
Luo et al. (2017) synthesized the sulfonic acid modi-
fied metal organic framework for malachite green
removal. This framework had a very high surface area due
to the presence of mesopores and pores of big volume. The
framework’s particle size was in the range of 100–300 nm.
It had anionic groups, which enhanced its cationic dye
removal efficiency. The maximum dye adsorption capac-
ity was 596  mg/g. The data followed pseudo-second-
order kinetics and fitted well to the Langmuir model. The
adsorption was spontaneous and endothermic in nature.
The intraparticle diffusion mechanism was the controlling
step in this case.
12 M
 alachite green adsorption
using magnetic nanomaterials
Debrassi et  al. (2012) prepared magnetic nanoparticles
using iron oxide and N-benzyl-O-carboxymethylchitosan
for malachite green removal. The mean particle size
was 14  nm. The maximum dye adsorption capacity was
144.79  mg/g. The data followed pseudo-second-order
kinetics and fitted well to the Langmuir-Freundlich
model. The adsorption was spontaneous and endother-
mic in nature. The dye removal was optimized using a 32
factorial design.
Safarik et  al. (2012) magnetically modified spent
coffee grounds and used these for various dye removal,
including malachite green. The pore size of coffee ground
was up to 30 μm. Spent coffee ground was modified by
using water-based magnetic fluid. The equilibrium was
attained in 3 h. The maximum dye removal was 43 mg/g.
Song et  al. (2012) prepared low-cost carbon nano-
spheres from glucose solution by hydrothermal reaction
for malachite green removal. The average pore diameter
was 3.84 nm. These nanospheres were activated by NaOH.
The prepared nanospheres had a very high percentage of
hydroxyl and carboxyl groups. The maximum dye adsorp-
tion capacity was 310 mg/g. The equilibrium was attained
in 20 min. The process was chemisorptions and followed
pseudo-second-order kinetics. The data fitted well to the
Langmuir model.
Xu et  al. (2012) prepared mesoporous poly(acrylic
acid)/SiO2 composite nanofiber membrane using sol-gel
electrospinning process for malachite green removal. The
prepared membranes were modified using triethoxyvinyl-
silane. The pore size was 3.8 nm, with a very high surface
area of 523.84 m2 g−1. The data followed Redlich-Peterson
isotherm and fitted well to pseudo-second-order kinet-
ics. The percentage dye removal was 98.8% in 240  min.
The maximum dye adsorption capacity was 220.49 mg/g.
These membranes were regenerated using alcohol solu-
tion and showed very high efficiency.
Yu et al. (2012) synthesized low-cost magnetic carbon
nanotubes using facile one-pot method. The as-prepared
carbon nanotubes modified using NaClO were well dis-
persed in water, with excellent magnetic properties. The
modified as-prepared carbon nanotubes had high surface
area (186.3 cm2 g−1) and small pore volume (0.53 cm3 g−1).
The adsorption capacity was 94.34 mg/g.
Fan et  al. (2013) prepared a nanocomposite
hydrogel from graphene oxide, sodium alginate, and
poly(acrylamide) for malachite green removal. They used
free radical polymerization for this preparation. They
checked the mechanical properties of the gel. The pre-
pared gel had high compressive and tensile strengths. The
prepared gel was used to remove several dyes and showed
excellent adsorption characteristics.
Pal and Deb (2013) synthesized silver nanoparticle
bead by biological route. The percentage dye removal
was 97% at pH 7.2. The data fitted well to the Freundlich
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model and followed pseudo-second-order kinetics. The
percentage dye removal decreased to 67% after 25 cycles.
Zeng et al. (2013) prepared carbon nanotubes filled with
poly(aniline) for malachite green removal. The maximum
dye adsorption was 13.95  mg/g, which was 15% higher
than the pure poly(aniline). This enhancement was due
to the large surface area and better interactions. The data
followed pseudo-second-order kinetics and fitted well to
the Langmuir model.
Femila et  al. (2014) synthesized silver nanoparticles
from plant extract of Aegle marmelos in a very economical
route in a short reaction time for malachite green removal.
The percentage dye removal was 99.8% in 4  h. Kerkez
and Bayazit (2014) synthesized multiwalled carbon nano-
tubes with magnetite. The particle size was in the range of
30–40 nm. It was used to remove malachite green. The per-
centage dye removal was 94% at pH 6 and 25°C in 80 min.
The maximum adsorption capacity was 55.25  mg/g. The
data followed pseudo-second-order kinetics and fitted
well to the Langmuir model. The adsorption process was
spontaneous and endothermic in nature.
Mohammadi et  al. (2014a) synthesized the super-
paramagentic Fe3O4 nanoparticles for malachite green
removal. These nanoparticles were coated by sodium algi-
nate. The particles were synthesized using coprecipitation
method. The particle sizes were around 12  nm. The data
followed pseudo-second-order kinetics and fitted well to
the Langmuir model. The maximum adsorption capacity
was 47.84 mg/g.
Soni et  al. (2014) synthesized magnetic alginate
microspheres loaded with nano-iron oxide particles for
malachite green removal. The synthesized adsorbent par-
ticles were found to be 26.44% crystalline. Their analysis
showed the presence of hydroxyl and carboxyl groups on
adsorbent surface that were mainly responsible for dye
removal. They used these particles in fixed-bed adsorp-
tion column. The percentage dye removal was 93.9% at pH
8. The equilibrium time was 60 min. The data fitted well to
the Freundlich model. The adsorption process was endo-
thermic in nature.
Fan et  al. (2015) synthesized magnetic nanoferric
oxide for malachite green dye removal. The particle size
of the adsorbent was about 20  nm. The adsorption data
fitted well to the Langmuir model. The adsorption was
very efficient even after several cycles. Around 90% dye
was removed in 45  min. The adsorption data followed
pseudo-second-order kinetics.
Patil and Shrivastava (2015) synthesized polyani-
line nickel ferrite magnetic nanocomposite for malachite
green removal. They used this composite to adsorb the
malachite green from aqueous solution. The data followed
K. Tewari et al.: Removal of malachite green dye      439
pseudo-second-order kinetics and fitted well to the Lang-
muir model. The optimum pH was 7. The adsorbed dye
was separated easily with the help of external magnet and
the adsorbent was used repeatedly without any signifi-
cant loss of adsorption capacity.
Qiao et al. (2015) prepared the carboxylate function-
alized cellulose nanocrystal for malachite green removal.
The adsorbent was prepared by grafting maleic anhy-
dride on hydroxyl groups of cellulose nanocrystals. The
adsorbent was in nanorod shape having length and width
or 0.1–1 μm and 20–40 μm, respectively. The adsorption
capacity of functionalized cellulose nanocrystals was
extremely higher than that of the raw cellulose due to high
surface area and presence of sulfate ester groups. The data
followed pseudo-second-order kinetics and fitted well to
the Langmuir model. The adsorption was spontaneous
and endothermic in nature.
Wang et al. (2015) prepared magnetic β-cyclodextrin
graphene oxide nanocomposite for malachite green
removal. The adsorption capacity of this adsorbent was
990.10 mg/g at pH 7 and 45°C. The adsorption data fitted
well to the Langmuir model and followed pseudo-second-
order kinetics. The adsorption was spontaneous and
endothermic in nature.
Zheng et al. (2015a) synthesized magnetic litchi peri-
carps for malachite green removal. They optimized the
adsorption conditions using Box-Behnken and response
surface methodology. The maximum removal efficiency
was recorded to be 99.5% in 66.69 min at 25°C, pH 6, and
5.15 g/l loading. The adsorbed dye was removed with
the help of an external magnet, which reduced the set-
tling time by 31  min. The maximum dye adsorption was
70.42 mg/g. The adsorption data followed pseudo-second-
order kinetics and fitted well to the Langmuir model. The
adsorption process was spontaneous and endothermic in
nature.
Angelova et  al. (2016) magnetically modified the
sargassum biomass for malachite green removal. The
maximum dye adsorption capacity was 110.4  mg/g. The
data followed pseudo-second-order kinetics. The process
was exothermic in nature. Lin and Lee (2016) synthesized
magnetic reduced graphene oxide/zeolite imidazolate
framework. The adsorbent particles were in the range of
100–500 nm. The prepared adsorbent was highly efficient
in malachite green dye removal. The maximum adsorption
capacity was 3165 mg/g at 40°C. The adsorption process
was endothermic in nature.
Pourjavadi and Abedin-Moghanaki (2016) syn-
thesized magnetic nanocomposite of functionalized
crosslinked poly(methylacrylate) for malachite green
removal. It was synthesized via radical polymerization
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440      K. Tewari et al.: Removal of malachite green dye
of methyl acrylate. Further, it was functionalized by eth-
ylenediamine and sodium chloroacetate. The adsorption
kinetics was pseudo-second-order and fitted well to the
Langmuir model. The maximum adsorption capacity was
890 mg/g at pH 7.
Yakout and Shaker (2016) synthesized dodecyl sul-
phate functionalized magnetic oxide for malachite green
removal. The maximum dye adsorption capacity was
714.3 mg/g at pH 7 and 25°C. The percentage dye removal
was 98.75%. The adsorbent was used several times
without any significant loss in adsorption capacity. The
kinetic data followed second-order model and fitted well
to the Langmuir model. The adsorption process was spon-
taneous and endothermic in nature.
Zhang et al. (2016b) synthesized magnetic hydroxya-
patite nanopowder with dual functionality for malachite
green dye removal. The adsorbent was regenerated several
times without any significant loss of adsorption capacity.
The data followed pseudo-first-order kinetics and fitted
well to the Langmuir model. The maximum adsorption
capacity was 526 mg/g. The adsorption process was spon-
taneous and exothermic in nature.
Zhang et  al. (2016c) synthesized water-soluble mag-
netic graphene nanocomposite by solvothermal and
coprecipitation methods for malachite green removal. The
particle size was between 5 and 20 nm. The dye removal
was very fast and 98.2% dye was removed in 20 min. The
used adsorbent was collected by external magnet and
reused. The adsorbent removal efficiency was constant in
15 consecutive cycles.
Zhang et al. (2016d) synthesized coal fly ash/CoFe2O4
magnetic composites using facile hydrothermal method
for malachite green removal. The adsorbent particles
were irregular spheres in the range of 30 nm. The surface
area was 58.16 m2 g−1, which was many times higher than
that of pure coal fly ash, i.e. 13  m2 g−1. The dye removal
was 92% at pH 7. The maximum dye adsorption capacity
was 89.3  mg/g. The adsorption data followed the Freun-
dlich and Dubinin Kaganer Radushkevich models. The
adsorption process was physical and dominated by van
der Waals forces.
13 Liquid-liquid extraction
Ali and Muthuraman (2015) used orthochloro benzoic acid
to remove malachite green from wastewater. Orthochloro
benzoic acid was used to extract the dye using liquid-
liquid extraction. Orthochloro benzoic acid concentra-
tion was maintained at 0.15 M, which gave 98.67% dye
extraction at pH 11.5 and 80°C. The 99.04% extracted
dye was recovered using 6.5 M acetic acid. This process
is environmentally friendly because it does not create the
problem of secondary waste disposal. In another work,
Soniya and Muthuraman (2015) used 2-nitrobenzoic acid
to extract malachite green. The percentage dye removal
was 98.95% at pH 7. They used 10 M acetic acid to recover
the dye.
14 Other hybrid adsorbents
Kannan et  al. (2008) prepared tetrahedral silica using
silica and alumina for malachite green removal. The silica
gel and alumina were activated at 150°C for 3 h in hot air
oven. The required amount of adsorbent was taken from
this activated adsorbent. In case of silica, the percentage
dye removal was 99% at pH 5–7 due to the development
of a high negative charge on the silica surface. In case of
alumina, the maximum dye adsorption was at pH 6 and
60°C. The data followed pseudo-second-order kinetics.
Recovery of malachite green by silica and alumina were
52 and 3.5  mg/g, respectively. The poor desorption of
malachite green from silica proved that it adsorbed more
strongly and stably than alumina.
Bai et al. (2013) used fenton reaction catalyst as adsor-
bent for malachite green removal. The percentage dye
removal was 97.94% at pH 3–5 for 50 mg/l concentration of
dye. In this study, [Fe(III)-salen]cl complex fenton system
was established for decolorization of malachite green,
and it is a newly developed process. Rong et  al. (2014)
prepared a water-soluble adsorbent for malachite green
removal from wastewater. The adsorbent was prepared
from maleic anhydride and melamine. The data followed
pseudo-second-order kinetics and fitted well to the Lang-
muir model. The adsorption efficiency was 95.08% at pH
9. The adsorption process was spontaneous and endother-
mic in nature. The dye adsorption was due to electrostatic
interaction between dye molecules, as well as carboxyl
and acylamino functional groups present on the adsor-
bent molecule.
El-Zahhar and Awwad (2016) modified the hydroxya-
patite with ethylhexadecyldimethyl ammonium bromide
for malachite green removal. The exchange reaction
was used in the modification. The maximum adsorption
capacity was 188.18 mg/g at 30°C and pH 7. The data fol-
lowed the Langmuir model. Robati et al. (2016) used gra-
phene oxide and a reduced form of it to remove malachite
green. The maximum dye removal was at pH 3 in 100 min.
The adsorption process was endothermic in nature.
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15 Adsorption mechanism
The adsorption mechanism depends on the nature of
dye and the adsorbent. Malachite green is a cationic dye
having two amine groups and positive charge on the nitro-
gen atom present in it. Adsorption occurs by physical
adsorption in the form of monolayer formation followed
by multilayer (Azad et  al. 2015, Banu and Maheswaran
2015, Geetha et  al. 2015). Macropores and mesopores of
the adsorbent having heterogeneous surface provide the
large surface area. The monolayer formation is a fast step,
which is followed by a slow step generally termed as intra-
particle diffusion (Geetha et al. 2015). If the intraparticle
diffusion graph passes from the origin, then the intra-
particle diffusion is the rate controlling step (Saygili and
Guzel 2015). The presence of intercept in the intraparticle
diffusion plot shows that intraparticle diffusion process
is not the only controlling mechanism of the adsorption
process (Banu and Maheswaran 2015, Saygili and Guzel
2015). Abou-Gamra and Ahmed (2015) found that the mon-
olayer film diffusion also controls the adsorption mecha-
nism. The presence of a large value of the intercept shows
that surface sorption is the rate controlling step (Agarwal
et  al. 2016a). The adsorption process can also be simul-
taneously controlled by film mass transfer, intraparticle
diffusion, and chemical reaction (Song et al. 2015).
If the mean sorption energy comes out to be between
8 and 16 kJ mol−1, then ion exchange mechanism controls
the adsorption process. If the value is less than 8 kJ mol−1,
then physical adsorption will be the controlling mecha-
nism (Patel and Hota 2014, Gautam et  al. 2015). If the
value is greater than 16  kJ mol−1, then the particle diffu-
sion would be the controlling mechanism (Patel and Hota
2014). If the value is between 20.9 and 418.4 kJ mol−1, then
chemical sorption will be the controlling mechanism.
16 C
 onclusions and future scope
of research
This review article presented a wide range of adsorbents
such as various industrial wastes, agricultural wastes,
activated carbon, biomass activated carbon, clay miner-
als, polymeric adsorbents, nanomaterials, membranes,
and magnetic adsorbents for the removal of malachite
green from aqueous solutions. Inexpensive, locally avail-
able, and effective raw and treated material could be used
in place of expensive material. A large number of pub-
lished literature has been reviewed here. It is observed
that adsorption depends upon the chemical nature of the
K. Tewari et al.: Removal of malachite green dye      441
material, such as pH, adsorbent dose, initial composition
of dye, and temperature. Therefore, these factors are to be
taken into account while evaluating the adsorption capac-
ity of different adsorbents. The summary of the references
reviewed in this work is given in Table 1. This table will be
very useful for a quick reference to the readers and will
help them to select the right adsorbent for further studies
and modifications. A few conclusions and recommenda-
tions are as follows:
–– Some of the biological materials like conch shell do
not require any treatment and have high adsorption
capacities (Chowdhury et  al. 2011a, Chowdhury and
Das 2011). These types of adsorbents can be explored
further.
–– A very few biological adsorbent are being used to
treat the industrial effluent (Patra et al. 2015). A lot of
research work is required to develop the process and
adsorbent to treat the industrial waste on a continu-
ous scale.
–– The only study reported in the field of continuous
treatment of malachite green waste is using pineap-
ple leaf power (Das et al. 2016).
–– So far, only two animal waste materials, hen feath-
ers and eggshells, have been used for dye malachite
green removal, resulting in poor removal efficiency
(Mittal 2006, Chowdhury and Das 2012).
–– Only a few clay-based adsorbents have been used for
malachite green removal. (Castellini et al. 2008, Gong
et  al. 2009, Chaudhuri et  al. 2016, Kaya et  al. 2016,
Tian et al. 2016). Si-MCM-41-β cyclodextrin clay gave
the maximum adsorption of 561.45 mg/g (Chaudhuri
et al. 2016). Other more efficient clays may be explored
in the future.
–– A few studies are reported dealing with ultrasonic
waves/irradiation enhanced adsorption and regen-
eration (Behnajady et al. 2008, Han et al. 2010, Azad
et al. 2015, Sadegh et al. 2015, Jothirani et al. 2016).
–– Several polymer-based adsorbents have shown
remarkably high adsorption capacities (Bildik et  al.
2014, Patel and Hota 2014, Pourjavadi et  al. 2014,
Sarkar et al. 2014, Zheng et al. 2014, 2015b). The gran-
ular composite hydrogel has the maximum adsorp-
tion capacity of 2433 mg/g (Zheng et al. 2014).
–– Very limited studies are being done on the actual
industrial waste (El-Bouraie 2015). More focus is
required to use the existing methods and materials to
treat the real industrial effluents.
–– Very little work has been done in the field of mala-
chite green removal using membrane adsorption
(Sayılkan et  al. 2007, Yin et  al. 2016). Coal-based
membranes completely adsorbed malachite green
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 Table 1: Various adsorbents and their maximum adsorption capacity.

S. no.   Name of adsorbent   Maximum adsorption capacity (mg g−1)  References

1   Octahedral ZnO/ZnFe2O4   4983  Liu et al. 2016b

2   Magnetic reduced graphene oxide/zeolite imidazolate framework   3165  Lin and Lee 2016
3   Zinc oxide nanoparticles   2963  Zhang et al. 2016a
4   Granular composite hydrogel (acrylic acid-itaconic acid-attapulgite, 5%)   2433  Zheng et al. 2014
5   N-doped carbon nanotubes stabilized Cu2O   1495.46  Li et al. 2016
6   Tunable porous carbon nanospheres   1455  Chang et al. 2013
7   Large pore carbon nanoparticle   1390  Tripathi et al. 2016
8   Gelatin grafted granular composite hydrogel of poly(acrylic acid)   1370  Zheng et al. 2015b
9   Carboxylate functionalized poly(acrylonitrile)(PAN/NaOH/NaHCO3) nanofibers   1038  Patel and Hota 2014
10   Effect of ultrasonic   1000  Zhou et al. 2013
11   Magnetic β-cyclodextin graphene oxide nanocomposite   990.10  Wang et al. 2015
12   HP-3 de-inking paper sludge HP-3   982  Mendez et al. 2010
13   Magnetic nanocomposite based on functionalized crosslinked poly(methylacrylate)  890  Pourjavadi and Abedin-Moghanaki 2016
14   Kappa-carrageenan grafted poly(acrylic acid)   833.33  Pourjavadi et al. 2014
15   Dodecyl sulphate functionalized magnetic graphene oxide   714.3  Yakout and Shaker 2016
442      K. Tewari et al.: Removal of malachite green dye

16   Triethylamine modified sawdust   697.8  Song et al. 2015

17   Mesoporous carbon from industrial grape waste   667  Saygili and Guzel 2015
18   Kappa-carrageenan grafted poly(acrylic acid)/TiO2-NH2 hydrogel nanocomposite   666.66  Pourjavadi et al. 2014
19   Tyre derived activated carbon   648  Song et al. 2013
20   Melamine/maleic anhydride (S-Me/Ma)   641.03  Rong et al. 2014
21   Mesoporous carbon CMK-3   625  Dong et al. 2012
22   Sulfonic acid group modified metal organic framework   596  Luo et al. 2017
23   Si-MCM-41-β cylcodextrin   561.45  Chaudhuri et al. 2016
24   Iron nanoparticles loaded on ash from Rosa canina L.   500  Agarwal et al. 2016b
25   Acid treated neem bark   500  Sharma et al. 2014
26   Ultrasonic modified corn pith   488.3  Jothirani et al. 2016
27   Iron functionalized metal organic framework   485  Huo and Yan 2012
28   Mesoporous carbon   476.1  Anbia and Ghaffari 2011
29   Durian seed   476  Ahmad et al. 2014
30   Crosslinked poly(styrene) based quaternary ethyl piperazine resin   450  Bildik et al. 2014
31   Chitosan coated bentonite beads   435.00  Ngah et al. 2010
32   RT-3 organic sludge RT-3   435  Mendez et al. 2010
33   CCB beads   435.0  Khan et al. 2013
34   Copper nanowires loaded activated carbon   434.8  Ghaedi et al. 2015b
35   Rambutan peel   388  Ahmad and Alrozi 2011
36   Graphene oxide   384  Nuengmatcha et al. 2014
37   Poly(vinyl alcohol)/chitosan foam   381  Li et al. 2012
38   Maleic anhydride modified cellulose   370  Zhou et al. 2015

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39   Ordered mesoporous carbon   354  Tian et al. 2011b
 Table 1 (continued)

S. no.   Name of adsorbent   Maximum adsorption capacity (mg g−1)  References

40   Amylopectin/poly(acrylic acid)   352.11  Sarkar et al. 2014

41   Biodegradable grafted copolymer derived from amylopectin and poly(acrylic acid)   352.11  Sarkar et al. 2014
42   Rarasaponin bentonite   339  Kurniawan et al. 2012
43   Mesoporous carbon   335  Tian et al. 2011a
44   Aminopropyl functionalized magnesium phyllosilicate   335  Lee et al. 2011
45   Zinc oxide nanoparticle-loaded activated carbon   322.58  Ghaedi et al. 2014
46   Colliodal carbon nanospheres   310  Song et al. 2012
47   Activated carbon from used stevia leaf having sodium hydroxide 1:2 weight ratios   288.67  Mullick and Neogi 2016
48   Activated carbon from used stevia leaf having sodium hydroxide 1:1 weight ratios   284.45  Mullick and Neogi 2016
49   Sawdust functionalized with oxalic acid   280  Wang et al. 2014
50   Magnetic amino functionalized metal organic framework   274  Liu et al. 2016a
51   Bamboo   263.58  Hameed and El-Khaiary 2008b
52   Fibrous sodium titanate   261.38  Huang et al. 2015
53   Spent tea leaves   256.4  Akar et al. 2013
54   Graphite oxide   248  Bradder et al. 2011
55   Wheat bran Fomes sclerodermeus   240  Papinutti et al. 2006
56   Garlic root   232.56  Ren et al. 2016
57   Poly(acrylic acid)/SiO2 nanofiber membrane   220.49  Xu et al. 2012
58   Coconut derived activated carbon   214  Bello and Ahmad 2012
59   sawdust with monosodium glucamate   196.08  Gong et al. 2009
60   Cattail   196  Shi et al. 2010
61   Organically modified hydroxyapatite   188.18  El-Zahhar and Awwad 2016
62   Macrophyte alligator weed   185.5  Wang 2010
63   Poly(ethyleneimine) functionalized coal fly ash   174.83  Dash et al. 2016
64   Gold nanoparticles loaded on activated carbon   172.20  Roosta et al. 2014
65   Au-NP-activated carbon   165  Roosta et al. 2014
66   Biosorbent Yarrowia lipolytica ISF7   155.098  Asfaram et al. 2016
67   Zinc oxide nanoparticle loaded on activated carbon   153.85  Ghaedi et al. 2014
68   Oil palm trunk fiber   149.35  Hameed and El-Khaiary 2008a
69   Lignite activated carbon   149.0  Kiani et al. 2011
70   Metal-organic framework MIL-100(Fe)   146  Huo and Yan 2012
71   N-benzyl-O-carboxymethylchitosan magnetic nanoparticles   144.79  Debrassi et al. 2012
72   Plasma treated sepiolite   143  Kaya et al. 2016
73   Tin oxide nanoparticle-loaded activated carbon   142.87  Shamsizadeh et al. 2014
74   Functionalized multiwalled carbon nanotubes   142.85  Shirmardi et al. 2013
75   Ultrathin NiO nanoflakes   142.08  Wei et al. 2014
76   Aluminum and amino functionalized metal organic framework   141  Li et al. 2015a
77   Cuprous iodide-cupric oxide nanocomposite loaded on activated carbon   136.57  Nekouei et al. 2016
78   Modified cellulose (CMGT)   131.93  Zhou et al. 2014

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79   Aminopropyl functionalized magnesium phyllosilicate   130.64  Lee et al. 2011
K. Tewari et al.: Removal of malachite green dye      443
 Table 1 (continued)

S. no.   Name of adsorbent   Maximum adsorption capacity (mg g−1)  References

80   Modified Sphagnum peat moss   121.9  Hemmati et al. 2016

81   Nanocrystalline embedded activated carbon   121.1  Banu and Maheswaran 2015
82   Phthalic anhydride modified cellulose   111  Zhou et al. 2015
83   Acid treated potato peels   111  Sharma et al. 2014
84   Halloysite nanotubes   99.6  Kiani et al. 2011
85   Lignin sulfonate based mesoporous material   97  Tang et al. 2016
86   Citric acid modified rice straw   94.34  Gong et al. 2006
87   Magnetic as-prepared carbon nanotubes (MAPCNTs)   94.34  Yu et al. 2012
88   Conch shell powder   92.25  Chowdhury and Das 2011
89   Amino functionalized graphenes   91.48  Guo et al. 2015
90   Walnut shell   90.80  Dahri et al. 2014
91   Coal fly ash/CoFe2O4   89.3  Zhang et al. 2016d
92   Activated carbon/CoFe2O4 composite   89.29  Ai et al. 2010
93   Copper oxide nanoparticles loaded activated carbon   87.72  Dil et al. 2017
94   Biologically active poly(urea)   84.60  Hasnain et al. 2012
444      K. Tewari et al.: Removal of malachite green dye

95   Treated ginger waste   84  Ahmad and Kumar 2010

96   Ashoka leaf powder   83.30  Gupta et al. 2012
97   Bivalve shell and Zea mays L. husk leaf   81.50  Jalil et al. 2012
98   Cadmium hydroxide nanowires loaded activated carbon   80.6  Ghaedi and Mosallanejad 2014
99   Wood apple shell   80.6  Sartape et al. 2014
100   Lignin based poly(urethane)   80  Kumari et al. 2016
101   Clayey soil   78.57  Saha et al. 2010a
102   Nickel hydroxide nanoplate modified activated carbon   76.92  Agarwal et al. 2016a
103   Brown marine macroalga Sargassum swartzii   76.92  Jerold and Sivasubramanian 2016
104   Rice husk   76.92  Rahman et al. 2005
105   Sawdust carbon   74.1  Khattri and Singh 2009
106   Magnetic litchi pericarps   70.42  Zheng et al. 2015a
107   Lignin sulfonate polymer   70.07  Tang et al. 2015
108   Graphite oxide/poly(urethane)   68.82  Qin et al. 2014
109   Rice husk bio char   67.6  Leng et al. 2015
110   Zinc oxide nanoroad loaded activated carbon   66.68  Ghaedi et al. 2016
111   Aerobic granules   66.6  Sun et al. 2008
112   Turbinaria   66.6  Kannan et al. 2010
113   Rotten sawdust   64  Hameed and El-Khaiary 2008c
114   ZnO nanorod-loaded activated carbon   59.17  Azad et al. 2015
115   p-Tert-butyl thiacalix(4)arene imbedded flexible poly(urethane)   58.82  Mohammadi et al. 2014b
116   Oxidized multi-walled carbon nanotubes   57.60  Ghaedi et al. 2015a
117   Rice husk (NCP)   57.14  Rahman et al. 2005

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118   Organically modified montmorillonite   56.82  Arellano-Cardenas et al. 2013
 Table 1 (continued)

S. no.   Name of adsorbent   Maximum adsorption capacity (mg g−1)  References

119   Eggshells   56.76  Chowdhury and Das 2012

120   Degreased coffee bean   55.3  Baek et al. 2010
121   Fe2O4 decorated multiwalled carbon nanotubes   55.25  Kerkez and Bayazit 2014
122   Oxalic acid modified rice husk   54.02  Zou et al. 2011
123   Hydrothermally carbonized pine needles   52.91  Hammud et al. 2015
124   Carrot leaves powder   52.6  Kushwaha et al. 2014
125   Tetrahedral silica   52  Kannan et al. 2008
126   Rice husk   50  Sharma 2011
127   Carboxylate functionalized multiwalled carbon nanotubes   49.45  Sadegh et al. 2015
128   Activated carbon derived from Borassus aethiopum   48.48  Nethaji et al. 2010
129   Palm flower activated carbon   48.48  Santhi et al. 2010
130   Bamboo leaves   48.3  Chen et al. 2014a
131   Poly(urethane) – attapulgite porous material   47.985  Dong et al. 2013
132   Mango seed husks   47.9  Franca et al. 2010
133   Sodium alginate coated Fe3O4 nanoparticles   47.84  Mohammadi et al. 2014a
134   Carrot stem powder   43.4  Kushwaha et al. 2014
135   Magnetically modified spent coffee grounds   43  Safarik et al. 2012
136   Pine wood decayed by fungi Poria cocos   42.6  Zhang et al. 2011
137   Brown rotten pine wood   42.43  Zhang et al. 2011
138   Sea shell powder   42.33  Chowdhury and Saha 2010b
139   Chlorella vulgaris biomass   42.33  Kousha et al. 2013
140   Onto Pithophora sp., a freshwater algae   42.2  Kumar et al. 2006
141   Copper nanowire loaded activated carbon   34  Roosta et al. 2015
142   Scenedesmus quadricauda biomass   33.76  Kousha et al. 2013
143   Pleurotus ostreatus   32.33  Chen et al. 2014b
144   Graphene oxide caged in cellulose microbeads   30.09  Zhang et al. 2015
145   Ricinus communis   27.78  Santhi et al. 2010
146   Activated carbon from coconut coir   27.44  Uma et al. 2013
147   Coconut coir activated carbon   27.44  Banerjee et al. 2016
148   Chitin hydrogels   26.833  Tang et al. 2012
149   Banana pseudo stem fiber   26.50  Gupta et al. 2011
150   Invasive marine alga Caulerpa racemosa   25.67  Bekçi et al. 2009
151   Natural zeolite   23.94  Han et al. 2010
152   Diatomite   23.65  Tian et al. 2016
153   Degreased coffee beans   23.00  Baek et al. 2010
154   Bimetallic Fe-Zn nanoparticles   21.74  Gautam et al. 2015
155   Palm flower based activated carbon   20.5  Nethaji et al. 2010
156   Cell suspension cultures of Blumea malcolmii Hook   20  Kagalkar et al. 2011
157   Cadmium hydroxide nanowires loaded on activated carbon   19.0  Setareh Derakhshan and Moradi 2014

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158   Chlorella based biomass   18.4  Tsai and Chen 2010
K. Tewari et al.: Removal of malachite green dye      445
 Table 1 (continued)

S. no.   Name of adsorbent   Maximum adsorption capacity (mg g−1)  References

159   Citric acid treated pea shells   17.2  Khan et al. 2014
160   Poly(urethane)/chitosan foam   16.67  Li et al. 2015b
161   Degreased coffee bean   16  Baek et al. 2010
162   Chemically modified rice husk   15.49  Chowdhury et al. 2011b
163   Pea shells   14.96  Khan et al. 2014
164   Graphene oxide caged in cellulose microbeads   14.06  Zhang et al. 2015
165   Carbon nanotubes/poly(aniline) composite   13.95  Zeng et al. 2013
166   Poly glycidyl methacrylate/divinyl benzene   13.6  Husaain et al. 2015
167   Carboxylate group functionalized multi-walled carbon nanotubes   11.73  Rajabi et al. 2016
168   Bagasse fly-ash   9.97  Mall et al. 2005
169   Deinococcus radiodurans R1   7.63  Lv et al. 2013
170   Titania nanoparticles   6.3  Abou-Gamra and Ahmed 2015
171   Pisum sativum   6.17  Khan et al. 2014
172   Activated carbon prepared from the epicarp of Ricinus communis   5.33  Santhi et al. 2010
173   Intensification of sonochemical degradation of malachite green by bromide ion   5  Moumeni and Hamdaoui 2012
446      K. Tewari et al.: Removal of malachite green dye

174   Sugarcane dust   4.88  Franca et al. 2010

175   Neem sawdust   4.35  Khattri and Singh 2009
176   Gum zanthan/psyllium nanocomposite   3.21  Kaith et al. 2016
177   Hen feathers   2.93  Mittal 2006
178   Nano-iron oxide loaded alginate microspheres   2.3  Soni et al. 2014
179   Tamarind fruit shell   1.951  Saha et al. 2010b
180   Gum rosin alcohol-poly(acrylamide)   1.4  Kaith et al. 2015
181   Unsaturated polyester phosphate   1.01  Khan et al. 2013
182   By polyethylene glycol micelles in cloud point   1  Chen et al. 2009
183   Thermal power plant (bottom ash)   0.71  Gupta et al. 2004

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(Yin et al. 2016). This type of membrane may be tried
in continuous operation and industrial plants. New
material can be invented with filtration and adsorp-
tion characteristics.
–– The nanomaterials have shown tremendously high
adsorption capacity. The adsorption capacity of octa-
hedral zinc oxide/ZnFe2O4 was reported as 4983 mg/g
(Liu et al. 2016b). This adsorbent can be explored fur-
ther to minimize the cost.
–– Metal organic frame work has shown very high
adsorption capacity, i.e. 596  mg/g (Luo et  al. 2017).
Further work can be done to improve the adsorption
capacity and regeneration capability.
–– It is easy to collect the adsorbed dye with the help of
external magnet. Magnetic reduced graphene oxide/
zeolite imidazolate framework has shown as excellent
adsorption capacity of 3165 mg/g (Lin and Lee 2016).
Other magnetic materials can be explored in near
future.
Acknowledgments: The authors are very thankful to Dr.
Barun Kumar Nandy, assistant professor, Department of
Fuel and Mineral Engineering IIT (ISM) Dhanbad, India,
for arranging the literature. The authors are highly grate-
ful to Dr. Sanjeev Ahuja, assistant professor, Chemical
Engineering Department, Thapar University, Patiala, and
Ms. Jyoti Sharma, PhD scholar, School of Chemistry and
Biochemistry, Thapar University, Patiala, for manuscript
reading. The authors are also very thankful to the authori-
ties of JUET Guna, M.P., for being encouraging to complete
this review on time.
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Bionotes
Kshitij Tewari
Department of Chemical Engineering, Jaypee
University of Engineering & Technology,
Guna, A. B. Road, Raghogarh, Guna 473226,
M. P., India
Kshitij Tewari completed his bachelor of technology degree in
chemical engineering in 2015 at Jaypee University of Engineering
and Technology, Guna, India. He worked at the Indian Institute of
Technology, Kanpur. He has published three research articles in
scientific journals and presented papers at five conferences.
Gaurav Singhal
Department of Chemical Engineering, Jaypee
University of Engineering & Technology,
Guna, A. B. Road, Raghogarh, Guna 473226,
M. P., India
Gaurav Singhal completed his bachelor of technology degree in
chemical engineering in 2015 at Jaypee University of Engineering
and Technology, Guna, India. Currently, he is working as a chemical
engineer at Nirma Ltd, India.
Raj Kumar Arya
Department of Chemical Engineering, Thapar
University, Patiala, Patiala 147004, Punjab,
India,
rajarya@thapar.edu, rajaryache@gmail.com,
http://orcid.org/0000-0003-1210-108X
Raj Kumar Arya completed his PhD in chemical engineering at IIT
Bombay, India, in 2010. He did his MTech in chemical engineering
at IIT Delhi, India, in 2002 and his BTech in chemical engineering at
HBTI Kanpur, UP, India in 2001. At present, he is working as an assis-
tant professor of chemical engineering at Thapar University, Patiala,
Punjab, India. Prior to that, he worked as a faculty member at Jaypee
University of Engineering and Technology, Guna, M.P., India, and
BITS–Pilani, Goa Campus, India. He is an active researcher in the
fields of polymeric thin film coating, and modeling and simulation.
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