Role of Carbon Materials Biointerface

Review
Volume 12, Issue 2, 2022, 1974 - 1997

https://doi.org/10.33263/BRIAC122.19741997
Role of Carbon Materials in the Removal of Organic

Pollutants: An Abridged Review
Venkata Ratnam Kesamseetty 1,*, RameshSingampalli 2,* , Anil BabuTadiboyina 2 , Venkata Krishna
Prasad Narasipuram 2, Venkata Prasad K. 3, Manjunatha Hanumanthrayappa 1
, Venkata Nadh
Ratnakaram 1, Janardan Sannapaneni 1, Chandra Babu Naidu Kadiyala 2,*
1 Dept. of Chemistry, GITAM Deemed to be University, Bangalore -562163, Karnataka, India
2 Dept. of Physics, GITAM Deemed to be University, Bangalore -562163, Karnataka, India
3 Dept of Physics, Centurion University, Vizianagaram - 530018, Andhra Pradesh, India
* Correspondence: chandrababu954@gmail.com (K.C.B); sramesh664@gmail.com (S.R); vratnam2004@gmail.com
(K.V.R);
Scopus Author ID 56520309700, 57213364736, 17346890900
Received: 9.02.2021; Revised: 15.05.2021; Accepted: 17.05.201; Published: 10.06.2021
Abstract: The unraveling of ill-effects of organic pollutants like pesticides and dyes has been
showcased with various devastating incidents worldwide, which seriously affect aquatic biota. Even
still, it can around 180000 fatalities per year noted in developing countries due to pesticide poisoning.
Besides concomitant organic pollutants, organic dyes like azo dyes are highly persistent, non-
biodegradable, and carcinogenic. On peeping into perils of pesticides and dyes, a birds-eye focused on
different methods for their wiped out from water bodies. In recent times, the adsorbents like carbon
nanotubes and graphene were being used in the adsorption method for their elimination. Additionally,
graphene properties include a ratio of rich surface area and volume, honeycomb structure rich in
aromatic appearing like a large polyaromatic molecule, and good chemical stability induced
metamorphosis into adept nano adsorbents. Furthermore, the methods of adsorption, kinetics, and
mechanism are also reported in this review to elicits the extent of adsorption. However, the purview of
this present review was about graphene materials and their impact in removing dyes and pesticides
through the adsorption method.
Keywords: pesticides; dyes; graphene; carbon nanotubes; nanocomposite; adsorption; and adsorption
capacity.
© 2021 by the authors. This article is an open-access article distributed under the terms and conditions of the Creative
Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
1. Introduction
The industrial revolution has changed the world economy and technological aspects in
the forward direction and concomitantly also an impetus for the rapid environmental
degradation [1]. As the years rolled down, there was still a quest for secluded facts and sources
of aquatic pollution since it reached an alarming condition globally that might adversely
influence public health and the environment if the present situation continues. Despite many
reasons for it, organic pollutants have been grabbed a major share among them [2]. It seems
that water pollutants like organic pollutants might induce havoc on water pollution via oxygen
demanding wastes, synthetic organic compounds, and oil [3]. Every day sewage around twenty
crore tons flows into freshwater bodies and 70% of the household sewage, followed by 33% of
the industrial waste directly released into water, which is a primary cause for the supply of
approximately 90% of contaminated water to cities [4]. A microscopic view on synthetic
https://biointerfaceresearch.com/ 1974
organic compounds like pesticides, synthetic dyes, polyaromatic compounds, and

pharmaceutical compounds entered into water bodies through various sources, particularly
industrial effluents. So it understands that a major threat to freshwater resources, 0.1% in the
form of surface water and 0.6% of groundwater out of 2.7%, prevailed with anthropogenic
activities rather than natural causes [5]. Thereupon pesticides and dyes are considered emerging
contaminants (ECs) since they are unregulated compounds and hazardous to the environment
and living organisms [6]. To reduce ill effects caused by ECs like pesticides, dyes, and their
metabolites, advanced techniques should be considered pivotal [7-8]. Hence, it’s unequivocal
information about different nano adsorbents from graphene materials and their adsorption
studies on dyes and pesticides reported in the last five years.
2. A Pragmatic View on Emerging Contaminants (ECs)
The various types of predominant persistent organic pollutants in aquatic biota belong
to pesticides and dyes majority, so considered as emerging contaminants.
2.1 Pesticides.
Pesticides are majorly synthetic compounds of organic nature that kill harmful
microorganisms, fungi, insects, rodents, weeds (pests). They are substances or combinations of
substances that prevent or reduce the damage due to any kind of pest [9]. To tame the world
food crisis, the conventional agriculture system is stepping towards the modern agriculture
system by neglecting regular crops. During this process, the uncontrollable use of pesticides
leaves their residues or metabolites creeping into the environment and cause significant
contamination of tertiary ecosystems, leading to serious health disorders among living
organisms. The worldwide annual use of pesticides on crops was around five billion kilograms,
showing a serious ill effect on biodiversity. Predominantly, in agriculture, pesticide
formulations used for crops were more than 500 in number. In fact, they are used as
agrochemicals to protect crops from various other organisms and disease-spreading vectors in
the form of insecticides, herbicides, fungicides, and rodenticides [10]. But unknowingly, it
focused on non-targeted organisms like birds, fishes including humans. A pragmatic aspect
about the disperse of pesticide on crops reaches target was estimated less than 0.1%, the left
overreaches to environmental ecosystems. Pesticide’s entry into the environment through
different modes includes leaching, run-offs, volatile methods, and drainage [11]. Once they
leached on the aquatic environment, their persistence affected by chemical stability, the action
of microorganisms, and uptake by living organisms in the aquatic environment lead to
biomagnifications, which finally ended with disruption of the ecosystem using food webs. It
understands that the high-level concentrations of pesticides reach tertiary ecosystems like
humankind through the food chain. Notwithstanding, the pesticides are classified into
organochlorines, organophosphates, carbamates, and pyrethroids. Depending on the chemical
composition and hazard level, pesticide classification as per WHO [12] was shown in Table 1.
Table 1. Pesticide classification based on the hazard level.

Class as per Level of Toxicity LD50 for Rat Example
WHO (mg/kg Body Weight)
Oral Dermal
Ia Extreme Risk <5 <50 Parathion
Ib High Risk 5-50 50-200 Eldrin
II Moderate Risk 50-2000 200-2000 DDT
III Slight Risk >2000 >2000 Malathion
IV Not likely to have severe risk in normal use ≥ 5000 Carbetamide
A noteworthy finding was observed that a detectable trace of pesticides like

organochlorines [11] are in surface water even after 30 years indicates its high persistence level.
Indeed, once pesticide was persistent in mammalian tissue, obliquely producing ROS leads to
oxidative stress and low down the antioxidative level, which in turn reason for long-term health
risks like neuro-degeneration, carcinogenesis, and cardiovascular disease, renal, endocrine
system, and reproductive diseases. Furthermore, in the last two decades, there was strong
evidence notified with the advice of epidemiological studies that an unwanted pesticide residue
induces different types of cancer like non-Hodgkin’s lymphoma, solid tumor, and leukemia
[13-17]. Especially organochlorines acted as endocrine disruptor compounds (EDCs) when
they leached into the soil, poised to health risks to humans via food chains. The conspectus
about most commonly used pesticides in crops [17] was given below Table 2.
Table 2. Classification of pesticides with examples.

S.No Name of pesticide Basic Structure Summary Examples
These are highly DDT, BHC, aldrin,
persistent in soil, toxic, endrin, chlordane,
and exhibits relatively toxaphane and
1 Organochlorines
non-soluble, low endosulfan
volatility, and lipophilic
nature
These are less persistent Parathion, malathion,
than organochlorines, diazinon, and
less toxic, and broad- glyphosate
2 Organophosphates
spectrum pesticides. It
is biodegradable with
less soil pollution.
It is more persistent Acaricides,
than organophosphates carbofuran, propoxur
3 Carbamates in soil and broad-
spectrum pesticide.
It exhibits non- Cypermethrin and

persistent and low Permethrin
toxicity and broad-
4 Pyrethroids spectrum toxicants
Amongst farmers from developing countries, pesticide poisoning was jeopardized,

evinced by the rate of fatalities around 180000 per year due to the suffering of 0.3 and 2.5
crores due to serious and mild poisoning [10], respectively. Even though pesticides have been
a boon for the agriculture sector because of crop yield and production, unregulated use leads
to a great menace to the environment [15-16]. So the immediate task after understanding the
perils of pesticides was too conspicuous a method for its control, reduce and removal from the
environment.
2.2. Dyes.
Synthetic dyes have been pinned under emerging contaminants like pesticides owing to
their chronic ill effects on the environment and living organisms [18]. In comparison to other
chemical industries like pharmaceuticals and leather, the dye manufacturing industry was
relatively small. About 8,00,000 tons of dyes are being manufactured per year for various
purposes, but a major share is grabbed by textile manufacturing industries other than paper
printing, food, leather, and others. More than 10000 dyes have been used in the textile
manufacturing industry, and more than 70% belong to class azodyes [19]. A large proportion
of liquid waste has organic and inorganic compounds that are unfixed to fabric material during
the process of dyeing and released into nearest water bodies at a high level of concentrations
as textile effluents. The textile production per day, around twelve to twenty tons, requires
around 1000-3000 m3 of water to be released as effluents after processing [20]. However, the
chemicals and unwanted dye waste in effluents, mostly non-biodegradable, persistent, and
carcinogenic, cause dissonance in the environment lead to health disorders among living
organisms. The following table below has provided information about dyes and their
classification [21-22].
Table 3. Classification of dyes with examples.

S.No Name of Chemical structure Conspectus Examples
the dye
1 Azoic dyes In azodyes, –N=N- bond azo Mordant Red,
linkage has two trans groups of Chrysoidine
A and B, posses electron-
accepting and donating nature,
respectively. The color and
types of azodyes are dependent
on the azo group, chromophores,
and auxochromes. Mostly used
in industries related to paper,
dye, textile, leather, plastic and
printing.
2 Reactive Reactive dyes carry one Reactive blue 19,
dyes sulphonic group to induce Reactive red 15, and
solubility and one or two Reactive blue 74.
reactive groups. It forms
interlocking bonds with
cellulose through bridge-group
like –NH-, -CO- and SO2.
3 Vat dyes Vat dyes mostly possess Vat Blue 5 and Acid Blue
indigoid or anthraquinone 74
structures with five and ten
aromatic rings. They have
colorfast to laundering. Further,
they bind to cellulose molecules
of fiber through hydrogen
bonding and van der Waals
forces. The aftermath was
oxidized for producing water-
insoluble Vat pigment possess
outstanding wash fastness
4 Sulphur In sulfur dyes, sulfur linkages Acid yellow 24 and picric
dyes are present in the form of acid
polysulphide(-Sn-), sulphide (-S-
), disulphide (-S-S-), and
chromophores in an integrated
polymeric system. In
comparison to others, sulfur
dyes were inexpensive with
good lightfastness.
5 Acid dyes Most of the acid dyes are bright Acid blue 25
and show good solubility when
structure have sulfonated groups
as well as show a variable
fastness to washing
6 Disperse Disperse dyes consists of Disperse red 28
dyes chromophore and auxochromes
of azo, anthraquinone, nitro
groups. Most of the dyes are
insoluble in water.
S.No Name of Chemical structure Conspectus Examples
the dye
7 Basic dyes Basic dyes have a positive Basic blue 22
charge, named cationic dyes,
which attract electrostatically
negative charge substrates. Most
of them show low colorfastness,
water soluble used for modified
polyesters, paper,
polyacrylonitrile, and modified
nylons.
8 Direct dyes Direct dyes possess a high Direct red 2
molecular mass relatively and
with groups of azo, stilbene, etc.
as chromophores. As well as
shows high substantivity and
good solubility if they have
sulphonated groups
There have been innumerable ill effects that prevailed with dyes on continuous
exposure, especially most of the azodyes are highly toxic to the ecosystem, and their
metabolites also show chronic effects on living organisms. Particularly azo dyes of
chromophoric systems of 1,4 diamino benzene irritate the skin, exophthalmos, chronic
disorders in the respiratory system, vertigo, acute tubular necrosis supervene, and chemosis
[18]. Besides natural ecological services, the rate of photosynthesis of aquatic living organisms
drops drastically whenever contamination occurs with azo dyes in water bodies, which leads
to the formation of anoxia discordance in ecological cycles of the aquatic ecosystem.
3. Adsorption Studies for the Quest of Good Adsorbents
To reduce organic pollutants in the aquatic ecosystem, impeccable methods are

available based on various principles, yet most of them have limitations that push to the
backyard a little. During searching for efficient and economical methods to remove pollutants,
the use of adsorption techniques was one of the excellent methodical procedures to eliminate
or reduce the different pollutants in aquatic biota [24]. Though the adsorption process is not
obscure to humankind since it has been used for long years, approaching techniques is different
and innovative [25]. Adsorption is a surface phenomenon that takes place between adsorbent
and adsorbate, where the interaction takes place through physical or chemical bonds. The
adsorbate, which is a mixture of multiple components similar to liquid or gas, attracts the
adsorbent of a solid porous medium. In the physisorption process, the physical forces are
pivotal during the interaction and reversible with low enthalpy, whereas chemisorption is based
on high enthalpy and irreversible chemical bonds. Consequently, the isosteric heat was one of
a decisive factor in adsorption studies, deduced from Van’t Hoff equation,
∆Ho / RgT2 = - (δ ln P/∂T) Cµ,

Where
‘∆Ho’ - Differential Molar Enthalpy of adsorption in J/mol,
‘Cµ’ - Maximum Adsorbed Concentration,
‘δ’ - Coefficient of Thermal Expansion of Saturation Concentration.
The information from the above equation recalls that heat released in a kinetic study is
similar to the release of heat due to adsorption. Another parameter in adsorption studies was
adsorption capacity which means the amount (mg) of adsorbed molecules on adsorbent per
gram used to estimate the extent of adsorption. As well as on the consideration of equilibrium
data the adsorption isotherms and properties elicits about mechanistic aspects of pollutants and
adsorbent. Moreover, the exactness of the extent of adsorption takes place is being measured
at constant temperature has been shown in terms of adsorption isotherms [26]. Since then, many
isotherms were proposed based on different parameters, but the best fit models are used to
know about the adsorption process of nano-adsorbents. In continuation of the investigation, the
adsorption kinetic models are also used for characterizing adsorption processes of nano
adsorbents [27], where the results mainly fit intraparticle diffusion, spurious first & second
orders, and Elovich models. Finally, studies on adsorption concluded with the application of
thermodynamic quantities entropy, enthalpy, and Gibbs free energy that evoked the data of
heat released or absorbed and spontaneity during the process of adsorption. Gibbs free energy
can be calculated from the equilibrium constant as follows:
∆𝐺 = −𝑅𝑇𝑙𝑛𝐾𝑐
Enthalpy and entropy are related to each other as:

∆𝑆𝑜 ∆𝐻𝑜
𝑙𝑛𝐾𝑐 = −
𝑅 𝑅𝑇
where ‘Kc’ the equilibrium constant, ‘T’ the temperature, ‘R’ the universal gas constant,
‘ΔH’ the standard enthalpy, and ‘ΔSo’ the standard entropy.
The slope and intercept belong to entropy and enthalpy of the adsorption process at
varied temperatures, respectively. The results of positive ΔH confirm that the reaction goes
through the endothermic process, while the positive ΔG refers to processes of non-spontaneity.
Anyhow, based on ’Gibbs’s free energy, we conclude that it follows the physisorption or
chemisorption process when adsorbate and adsorbent nearby. For the proper understanding of
the adsorption mechanism [26], concomitant with computational modeling, the following
approaches are shown in Table 4 have been extensively used.
Table 4. A gist on modeling methods used in adsorption.

S.No Type of isotherm Isotherm model Summary
One Parameter Isotherm Henry’s Isotherm The adsorbate concentration and partial pressure are
1 directly proportional, and this model suits low adsorbate
concentration.
Hill-Deboer Model It explains the mobility of adsorption and also lateral
2
interaction between adsorbed molecules
Langmuir Isotherm It is meant for understanding the adsorption of the gas-
solid phase, which also quantifies and contrasts the
capacity of different adsorbents. Desorption is
3
proportional to the fraction of adsorbent surface when
covered, while adsorption has the same property when
open
Freundlich Isotherm Designed to evaluate the processes of adsorption taking
4
place on heterogonous surfaces.
Fowler-Guggenheim It was proposed to predict the lateral interaction of
Two Parameter Isotherm
Isotherm adsorbed molecules, which was based on the fact that
5 adsorption heat vary with loading linearly, and it is
noteworthy, only applicable for surface coverage less
than 0.6
Dubinin-Radushkevich This model was used to determine the Gaussian
Isotherm distribution energy of heterogeneous adsorption and is
6
only fit for adsorbate concentrations of the intermediate
range.
Temkin Isotherm This model considers only the interaction effect of
7 adsorbates on the adsorption process and suits only for ion
concentrations of medium range
S.No Type of isotherm Isotherm model Summary
Flory-Huggins Isotherm. This model describes the extent of adsorbate surface
8 coverage properties related to adsorbent, spontaneity, and
convenience of the adsorption process
Hill Isotherm It explains the binding of various species with pure
9
substrates
Halsey Isotherm It evaluates multilayer adsorption at a comparatively large
10
distance from the surface
Harkin-Jura Isotherm. It predicts the possible multilayer adsorption on the
11 surface of the absorbent with a mixed distribution of
pores
Jovanovic Isotherm It assesses the possible mechanical contacts between
12
adsorbent and adsorbate.
Elovich Isotherm. ’Elovich’s model explains that adsorption sites increase
exponentially with adsorption and are applied to
13
multilayer adsorption. From this, it is possible to describe
the kinetics of chemisorptions of gas onto solids
Kiselev Isotherm It explains localized monomolecular layer model and
14
valid only for surface coverage greater than 0.68
Redlich-Peterson Isotherm It shows linear dependence of concentration and
exponential function in numerator and denominator put
together representing adsorption equilibrium for a large
15 range of adsorbate concentration applicable for
homogenous or heterogeneous systems due to its
adaptability and is a combination of Freundlich and
Langmuir isotherms.
Sips Isotherm A mix of Freundlich and Langmuir isotherms that suits
for predicting adsorption on heterogeneous surfaces
16 hence can avoid the limitation on an increase of adsorbate
concentration generally associated with the Freundlich
model
Toth Isotherm It explains the heterogeneous adsorption system that
17 satisfies low-end and high-end boundaries of adsorbate
Three-Parameter concentration
Isotherms Koble-Carrigan Isotherm It is a three-parameter equation that incorporates
18 Freundlich and Langmuir's isotherms representing data
of equilibrium adsorption
Kahn isotherm This model estimates bi-adsorbate adsorption for pure
19
dilute solutions
Radke-Prausniiz Isotherm It represents an excellent plot for a vast range of
20
adsorbate concentration
Langmuir-Freundlich It gives the knowledge of adsorption on heterogeneous
21 Isotherm surfaces as well as the distribution of adsorption energy
onto the heterogeneous surface of the adsorbent
Jossens Isotherm. This model estimates a basic equation depending on the
distribution of energy between the interaction of
22 adsorbate and adsorbent at adsorption sites. It considers a
heterogeneous surface for adsorbent because of its
interactions with an adsorbate.
Fritz-Schlunder Isotherm. This equation suits a wide range of experimental results
23
due to significant number of isotherm coefficients
Baudu Isotherm This model estimates Langmuir coefficients by
measuring tangents for various equilibrium
24
concentrations indicating they are not broad range
Four-Parameter Isotherms
constants
Weber-Van Vliet Isotherm. A four parameter empirical relation providing data
25
pattern description for big range of adsorption systems.
Marczewski-Jaroniec Based on adsorption energy distribution in active sites of
26
Isotherm the adsorbent and local Langmuir isotherm
4. Carbon Materials in Nutshell
In discourse about adsorbents, the carbon-derived nanomaterials [28] occupied apex

position owing to high flexibility, low cost, a big area of the surface, and high adsorption
capacity. Consequently, the factors that are the size and shape of nano adsorbents as well as
temperature, pH, and reaction time can influence the adsorption capacity.
4.1. The uniqueness of graphene and its derivatives.
The quirky behavior of graphene was found on account of its structure, properties, and
a myriad of applications in different fields. Undoubtedly, graphene has been lured by
researchers in surface science predominantly [29-31], whereas the fundamental points about it
are as follows. Firstly the structure of graphene is a two-dimensional nanosheet comprise of
sp2 bonded carbon atoms arranged honeycomb model and appeared as large polycyclic
aromatic molecules. The terminating edges of graphene were the basal plane and the edge.
Anyhow the graphene-based nanomaterials are classified in terms of their dimensions towards
z-axes and the x-y axes. Based on the z-axis, the graphene nanomaterials categorize as a single
layer with zero band gaps, double layer with zero bandgaps in the native state but on the
application of electric field axially toward the bilayer, few-layer with metallic nature, and
graphene platelets with 3-30nm thick that resembles with HOPG. Further, in orientation
towards x-y-z axes, the graphene nanomaterials exist in the form of nanoribbons that are
considered carbon nanotubes (CNTs). Secondly, as mentioned earlier, the properties of
graphene are pivotal, which are high capacitance, outstanding carrier mobility, and fast electron
transfer rate, as well as high surface area (2630 m2g-1), includes a rich surface to volume ratio,
greater mechanical strength, superior electrical conductivity.
Interestingly such properties can be modified by operating synthetic conditions, doping,
and the number of layers. Thirdly the application of graphene was made by surface
functionalization method, either covalent or non-covalent modifications. Especially the
delocalized pi bonds in graphene molecule provide an extended conjugation that carries high
surface area leads to binding of metal nanoparticles or other special groups. Hence
nanomaterials with graphene base are the main impetus for novel adsorbents in removing
organic pollutants [32-34]. Despite several methods used in the synthesis of graphene [35],
which include different exfoliation methods, the oxidative exfoliation of graphite was forefront
named Hummers’ method, and later on, the same method was improved by adding specific
changes called modified Hummers’ method. The approach of the two methods is shown below
Fig. 1.
Hummers method Modified Hummers method
In this method exfoliation done with Here 9:1mixture of H2SO4/H3PO4 was used
KMnO4 and NaNO3 initially and with by increasing concentration of
hydrazine was used in reduction of KMnO4 by exclude of NaNO3.
gaphene oxide to graphene at the
end.
Reductioon of emsissions of toxic
gases as well as this method well
It was more advantageous than Brodies suited for the preparation of graphene
method but toxic gases like NO2 and oxide .
N2O4 which stops the removal of the
impurites such as Na+ and NO-3
Figure 1. Strategic approaches in the synthesis of graphene.
The other two graphene derivatives [36-37] were graphene oxide and reduced graphene
oxide. In between, graphene oxide (GO) is an oxidized product of graphite with a chemical
composition C+x (OH)-y (H2O)2. GO is a monolayer where the oxygen content is high with the
ratio of C:O less than 3:1 and usually closer to 2:1. It has also been proven as a good adsorbent
when the basal and edge plane sites of graphene oxide were modified with a special group like
carboxyl, hydroxyl, and epoxy. The other one in the carbon family is reduced graphene oxide
(rGO), which also shows good electrical conductivity and can be produced from the exfoliation
of graphite to graphene oxide followed by apply of reduction using different routes like
thermal, electrochemical, and chemical (TRGO, ERGO, CRGO) methods [38-39]. On account
of its excellent chemical stability and a huge area on the surface, rGO was well suited as an
adsorbent in the removal of organic pollutants like dyes and pesticides [40-41].
4.2. Graphene materials as dye adsorbents.
The aforementioned properties of graphene and its confidants understand that they are
well suited as nano adsorbents. Specifically, in removing organic dyes [42-43], graphene and
its derivatives (Table 5) play a significant role.
Wang and his coworkers [44] prepared a magnetic nanocomposite adsorbent of
CoFe2O4/graphene oxide (GO) through the hydrothermal method and used it to remove
methylene blue (MB) rhodamine B (RhB), and methyl orange (MO) from wastewater. The
order of adsorption capacity noted as MB > RhB > MO as well as by reason of the magnetic
nature of the nanocomposite was easily separated. Jana et al. [45] studied the removal of
organic pollutants like rhodamine B dye, phenol using ZG30, and methyl orange, a hierarchical
hollow microsphere of ZnO- chemically converted graphene nanocomposites prepared through
a low-temperature solution method. The ZG30 acts as a successful reusable adsorbent for
pollutants (organic type). In simulated wastewater, the malachite green (MG) dye was removed
using reduced graphene oxide reported by Khatri et al. [46], where a mechanism occurs
between negatively charged oxygen of reduced graphene and cationic center of aromatic rings
of MG dye. This was possible due to the high surface area (931 m².gm⁻¹) of rGO, which
effectively removes the cationic dye like MG. Besides, Zhang and his group [47] synthesized
a 3D-3D Bi2WO6/graphene hydrogel (BWO/GH) by a one-step hydrothermal method, which
was used as an adsorbent and photocatalyst for methylene blue (MB) and 2,4 –dichlorophenol.
In another study, Chen et al. [48] showed that Fe3O4-graphene@mesoporous SiO2
nanocomposites (MG@m-SiO2) adsorb firmly the organic pollutant of common dye,
methylene blue (MB), which is endothermic, spontaneous reaction and method was low cost
and highly facile. Interestingly, Chen and his group [49] prepared magnetic β-cyclodextrin-
graphene oxide nanocomposites (MCG) that acts as nano adsorbent which removes an organic
pollutant like p-phenylenediamines (PPD), and results revealed that MCG was a good
adsorbent to remove organic pollutant about 98%. Zhang et al. [50] continued studies with β
cyclodextrin grafted graphene oxide (GO-β-CD) that show good adsorption capacities for
organic dyes like fuchsin acid methylene blue, methyl orange. Meanwhile, Ag/ZnO/graphene
oxide (GO) composite materials were synthesized by the Yang group, [51] acts as adsorbent
and degradation heterostructure for an organic dye, rhodamine B (RhB). It is a promising
material for the removal of organic dyes. Furthermore, the studies of Copello et al. [52] proven
that chitin/graphene oxide (Chi:nGO) hybrid gels were used to remove organic dyes like
RB,NR (Remazol Black, Neutral Red) as acid and basic dyes, hence Chi:nGO acts as
biosorbent.
Table 5. Adsorption studies on organic dyes using graphene and its derivatives.
S.No Adsorbent Adsorbate/ organic dye Isotherm models and Adsorption Capacity of Ref.
studies adsorption
Methylene blue (MB), MB = 355.9 mg.g⁻¹
CoFe2O4/graphene Nitrogen adsorption /desorption at
1 rhodamine B (RhB) and and RhB = 284.9 [44]
oxide (GO) 77 K and Langmuir model
methyl orange (MO) mg.g⁻¹
Brunauer-Emmet-Teller (BET)
ZnO-chemically nitrogen adsorption and desorption
converted graphene Rhodamine B dye, Methyl isotherms measurements at liquid
2 - [45]
(CCG) orange and Phenol nitrogen temperature / Multipoint
nanocomposite BET nitrogen adsorption-desorption
isotherms of ZG30
Reduced Graphene Malachite green Langmuier and Frendlisch
3 476.2 mg.g⁻¹ [46]
Oxide (MG) dye adsorptiobn method
3D-3D porous
Methylene blue (MB) and 2, Adsorption and photocatalytic
4 Bi2WO6/graphene [47]
4-dichlorophenol process
hydrogel composite
Fe3O4-
graphene@mesopor Langmuir isotherm model/ UV 178.49 mg/ g−1 at [48]
5 Methylene Blue (MB)
ous SiO2 visible method 313K.
nanocomposites
β-cyclodextrin-
Langmuir adsorption model and
6 graphene oxide p-Phenylenediamine 1102.58 mg/g [49]
UV–Vis spectrophotometer
nanocomposites
β-Cyclodextrin
Methyl Orange, methylene
7 functionalized UV absorption method - [50]
blue, Fuchsin acid
graphene oxide:
Ag/ZnO/graphene Adsorption and photocatalytic
8 Rhodamine B - [51]
oxide process
RB and NR were
Chitin/graphene RB, NR(Remazol Black,
Elovich and Modified Freundlich 9.3 × 10−2 mmol/g
9 oxide hybrid Neutral Red) as acid and [52]
models/ UV absorption method and
composite base dye models
57 × 10−2 mmol/g
4.3. Graphene materials as pesticide adsorbents.
The pesticides like organochlorines and organophosphates were crawled into aquatic
environments majorly from industries, textiles, and agriculture that induce pesticide pollution.
Sometimes, the mode of entry of pesticides into the air using dust particles in the atmosphere
leads to travel and reaches the nearest water bodies, soil, and sediments. Amongst all two
pesticides, malathion and lindane are commonly used in India, which are highly toxic. So their
predominant levels in polluted water were reduced by low-cost adsorbents like graphene,
graphene oxide, and reduced graphene oxide.
Tamara et al. [53] used three graphene-based materials like GO,IG,GNP (graphene
oxide, industrial quality graphene, and graphene nanoplatelets) for adsorption of dimethoate
(DMT) and chlorpyrifos (CPF) belongs to a class of organochlorine pesticides. It was found
that DMT strongly adsorbs hydrophilic oxidized graphene surfaces while CPF prefers to adsorb
on the base surface of graphene having high order of structure and maintained π electron
system. Casa and his group [54] worked on a persistent organic pollutant like chlordane. Its
removal is possible by reduced graphene oxide- silver nanoparticles that are efficient green
adsorbent and allow the degradation of pesticides. Afterward, Wang et al. [55] reported that
novel Zr-based MOF/GO hybrid nanocomposite (UiO-67/GO) shows a strong affinity towards
organic phosphate pesticides like glyphosate from wastewater. Here the sequestration of
glyphosate was done due to the availability of a large GO surface where Zr-OH groups exhibit
a strong affinity towards glyphosate. Pang and his coworkers [56] have introduced fast,
economical, easy, effective, rough, and safe adsorbent of magnetic graphene to determine the
26 types of organochlorine left out pesticide in tobacco. Besides this, to remove triazine
pesticides, Ma et al. [57] introduced a novel, highly efficient novel sorbent cellulose/graphene
composite (CGC) where the rough and wrinkled surfaces with a lamellar structure provide a
high adsorption rate. Graphene-modified TiO2 arrays were prepared using the electrodeposition
method by Zhou et al. [58], which acts as an adsorbent for diethofencarb, isoprocarb carbaryl,
and metolcarb, which are carbamate pesticides. In other studies using the solvothermal method,
Wang et al. [59] prepared a novel nano adsorbent of phenyl-modified magnetic
graphene/mesoporous silica (MG-MS-Ph) to remove toxic pesticides efficiently from
wastewater. For quick removal of noxious pesticide, oxamyl using GQD (graphene quantum
dots) was synthesized through a hydrothermal route assisted by microwave by Gupta et al.,
[60] that adsorption did through ionic interactions and electrostatic interactions between
oxamyl cation and GQDs. Sazlinda et al. [61] have synthesized a novel super hydrophilic
graphene oxide/electrospun cellulose nanofibre (GO/CNF) as an adsorbent to remove
organophosphates like ethoprophos, methyl parathion, chlorpyrifos, and sulfotepp in food and
water samples. Das et al. [62] used magnetic Fe3O4/reduced graphene oxide nanocomposite to
remove triazine pesticides like ametryn, prometryn, simazine, simeton, and atrazine. In turn,
there was a strong electrostatic, hydrophobic and π-π interaction between the aromatic rings of
nanocomposite and triazine pesticides, leads to strong adsorption for their elimination. Pradeep
and his coworkers [63] introduced the dehalogenation process for lowering the toxicity of
pesticides using reduced graphene oxide-silver nanocomposite for dehalogenation, reducing
the toxicity and removal of persistent organochlorine pesticide, lindane where it was converted
to different isomers of trichloro benzene. The same group [64] continued their studies belongs
to alkyl halide groups like endosulfan, chlorpyrifos, dichlorodiphenyldichloroethylene, and
fluorocarbons using reduced graphene oxide–silver nanocomposite (rGO@Ag) where
adsorption mechanism reduces the pesticides. Xu et al. [65] fabricated a novel Fe4O3–graphene
oxide (GO)–β-cyclodextrin (β-CD) nanocomposite that was used for removal of neonicotinoid
insecticide pollutants from wastewater. GO-Fe3O4 (graphene oxide-iron oxide )
nanocomposite magnetic nanoparticles were synthesized by Shrivas et al. [66] for
stereoselective removal of isomeric pesticides like endrin and dieldrin with high adsorption
rates and capacity. A remarkable observation was found here as the endo-positioned O2 atom
in endrin favor strong interaction with GO-MNP leads to high adsorption but in dieldrin such
interaction possible by exo position of oxygen. Subsequently, organophosphate pesticides were
removed by using ACCE/G(sieve-like cellulose/ graphene oxide composites) and GO-based
SiO2 with Fe3O4 nanocomposites functionalized with 2-phenylethylamine as adsorbents also
reported by Ji et al. [67] and Ndungu and his group [68], respectively. Interestingly there is a
report by Sonal and coworkers [69] that exclusively Graphene oxide (GO) acts as an adsorbent
to remove organophosphorus pesticides, and the rate of adsorption was calculated and
confirmed with density functional theory (DFT) studies. The following Table6 has various
nanocomposites and their role in the removal of pesticides through adsorption.
4.4. Carbon nanotubes (CNTs)-A capstone among carbon nanomaterial.
In most carbon-based materials, carbon nanotubes attained the greatest interest because
of outstanding thermal, electrical and mechanical [70-75] properties. These carbon nanotubes
are folded with graphene layers and have the sp2 combined hexagonal clusters of C (carbon)
atoms. The properties of CNTs depend on the radius and rolling angle of the tubes. The tube
ends are covered with half fullerene molecules. The carbon nanotubes are dimension systems
anticipated, just similar to the single sheets of graphite [76-78]. Now, it is a fact that the carbon
nanotubes are classified based on the graphene layers existing on the CNTs. They are classified
as SWCNT and MWCNT (single-walled, multi-walled) carbon nanotubes. They are rolled up
with single hexagonal carbon nanotubes of about 0.4 to 3 nm (or less than 1 nanometer).
Moreover, the MWCNTs with a diameter of 1.4 to 100nm (or more than 100nm) contain one
inner tube and outer tube as reported [79] and their properties are discussed in Table7.
Table 6. Adsorption studies on pesticides using graphene and its derivatives.

S.No Adsorbent Adsorbate/ Pesticide Isotherm models and Adsorption Capacity of Ref.
studies adsorption
1 Graphene-based Dimethoate (DMT) and Langmuier and Freundlich isotherm/ [53]
materials Chlorpyrifos (CPF) UPLC method
2 Reduced graphene Chlordane GC analysis [54]
oxide−silver
nanocomposite
3 Metal-Organic Glyphosate Langmuir and Freundlich models and 482.69 mg. g-1 [55]
framework/grapheme UV-Vis method
oxide hybrid
nanocomposite (UiO-
67/GO)
4 Magnetic graphene Organochlorine BET isotherm and GC-MS method [56]
pesticide (OCPs)
5 Cellulose/graphene Triazine Pesticides, Langmuir and Freundlich models, 30 mg. g-1 [57]
composite (CGC) Simeton, Simazine, GC analysis
Atrazine, Cyprazine,
Ametryn, and
Prometryn.
6 Graphene-modified Carbamate pesticides, HPLC analysis [58]
TiO2 nanotube Metolcarb, Carbaryl,
Isoprocarb, and
Diethofencarb
7 Phenyl-modified Avermectin, Langmuir and Freundlich model. [59]
magnetic Imidacloprid, UV absorption method
graphene/mesoporous Pyridaben, Dichlorvos,
silica (MG-MS-Ph) Acetamiprid, Dursban,
composites Isocarbophos, and
Phoxim
8 Graphene quantum Carbamate pesticide Langmuir and Freundlich model. 0.6g [60]
dots,GQD oxamyl GC analysis
9 Superhydrophilic Organophosphorus Langmuir and Freundlich isotherm Ethoprophos, [61]
graphene oxide/ pesticides, Methyl models Sulfotepp,
electrospun cellulose parathion, Ethoprophos, UPLC–UV methods Chlorpyrifos and
nanofibre sulfotepp, and Methyl parathion
chlorpyrifos were 0.421, 0.243,
0.258 and 0.228
mg g−1
10 Fe3O4/graphene Triazine pesticides, Langmuir and Freundlich isotherm 54.8 mg g−1 [62]
nanocomposite Ametryn, models/
Prometryn, Simazine, UV -Vis method
simeton and Atrazine
11 reduced graphene Chlorpyrifos (CP), GC analysis 1534 mg/g [63]
oxide–silver Endosulfan (ES),
nanocomposite Dichlorodiphenyl
(rGO@Ag) dichloroethylene (DDE)
12 Fe4O3–graphene oxide Neonicotinoid Langmuir and the Freundlich model. Thiamethoxam, [64]
(GO)–β-cyclodextrin insecticides HPLC-MS-MS Imidacloprid,
(β-CD) Acetamiprid,
nanocomposite Nitenpyram,
Dinotefuran,
Clothianidin, and
Thiacloprid at 100
mg/L were 2.88,
3.11, 2.96, 2.56,
1.77, and 2.88 mg/g,
respectively
13 Reduced graphene Lindane GC analysis 827 mg/g [65]
oxide-silver
composites
(rGO@Ag)
S.No Adsorbent Adsorbate/ Pesticide Isotherm models and Adsorption Capacity of Ref.
studies adsorption
14 Graphene oxide (GO) Endrin and Dieldrin Langmuir adsorption isotherm model 99 mg g−1 for [66]
and iron oxide (Fe3O4) endrin and 28 mg
magnetic L−1 for dieldrin
nanoparticles (MNPs)
15 Sieve-like cellulose/ Chloropyrifos Langmuir and Freundlich adsorption 152.5 mg g-1 [67]
graphene oxide isotherm model, GC analysis
composites (ACCE/G)
16 Fe3O4@SiO2@GO Chlorpyrifos, Parathion, Langmuir, Freundlich, Temkin, Chlorpyrifos -11.1 [68]
functionalized with 2- and Malathion Dubinin–Radushkevich (D-R), Sips, mg/g, Malathion -
phenylethylamine Redlich and Peterson Isotherms and 10.6 mg/g and
(PEA) Nitrogen adsorption /desorption at 77 Parathion10.9 mg/g
K, and a Vibrating Sample
Magnetometer (VSM)
17 Graphene Oxide Chlorpyrifos, Malathion Freundlich isotherm and Langmuir [69]
isotherm
UV-Vis absorption spectra
Table 7. Comparison between SWCNT and MWCNTS.

SWCNT MWCNT
It contains a single layer of graphene It contains multiple layers of graphene
The diameter ranges between 0.4 to 3nm The diameter ranges between 1.4 to 100nm
The structure forms six atom carbon rings in hexagonal It consists of concentric layers in a cylindrical
shape, similar to that of graphite shape.
For the synthesis SWCNTs, a catalyst is required These are produced without catalyst
Bulk synthesis is very difficult due to proper control of its Bulk synthesis is very easy
growth and atmospheric condition
The purity of the SWCNT is poor Purity of the MWCNT high
During functionalization, the possibility of defect is high Possibility of defect is less while functionalization
but difficult to correct if once occurred
Less accumulation in the body More accumulation in the body
Easy evaluation and characterization Tough evaluation and characterization because of
structure complexity
Easily flexible and twisted It cannot be easily twisted
These are used in electronics, water filtration, hydrogen Very less application compared to SWCNT
storage, oil spill removal, etc.
There are different methods to prepare carbon nanotubes. Sol-Gel, Laser Ablation, Arc
Discharge, and Chemical Vapor Deposition methods are the most extensively used methods
[80]. Also, arc discharge and laser ablation methods limit scale creation of produced CNTs,
and they are cleaned further due to a large number of impurities like amorphous carbon and
non-tubular fullerene structures joined in adding with the catalyst. CVD method (chemical
vapor deposition) is an appropriate technique for the enormous creation of CNTs with very low
impurities [81].
CNT’s exhibit high thermo-mechanical and electrical properties due to their high aspect
ratio and rare structure. , The ideal course of action between carbon covalent bonds along with
hub of nanotubes makes them exceptionally solid with brilliant solidarity to weight proportion.
They show exceptionally huge elasticity, roughly about 50–500GPa, which is much more than
good-quality small-scale measured carbon fibers. They additionally have an extremely low
thickness of ≈1.3 g/cm3. This makes them more grounded, less weight than steel, high ’Young’s
modulus ≈1500 GPa [82-84] possessing thermal conductivity approximating to 3500W m−1
K−1 and steady up to 2800◦C in vacuum [85,86]. Depending on their geometry, they may be
semiconducting or metallic dependent [87-89].
Removal of organic and inorganic pollutants from wastewater and dyes gained wide
focus during recent years in research perspective since carbon nanomaterials act as major
adsorbents for this purpose [90, 91]. An increase of waste in CNT’s encourages adsorption
because of their specific morphological and structural properties like big surface-to-volume
ratio, very small size, porous structure, and highly hollow [92, 93]. Dyes are of many types that
include direct, basic, reactive acid, and disperse, which show very high toxic levels at less
concentration. Adsorbents like clay, zeolites, polymers, and activated carbon can be used to
treat organic dye pollutants. Among the actual adsorbents, the functionalized carbon nanotube
is one of the important adsorbents that can remove dye contaminants from wastewater.
Carbon nanotubes have been used in many fields in science and engineering due to their
exceptional properties. At present, in the area of environmental monitoring, the properties of
the carbon nanotubes have greater chances in the wide application as detection and remediation
of various contaminants and wastewater treatment. The pesticides are given more concentration
due to their wide usage to save plants from weeds, disease, and insect damage. The MWCNTs
have a well-defined structure, functional groups, and surface area; due to this, these are well-
absorbent materials that possess a good performance of adsorption. Therefore these materials
are the removal of pesticides from the aqueous solutions [94].
Multi-walled carbon nanotubes are used to remove different types of dyes; the
concentration of dyes mainly affects pH, a dose of adsorbent, and contact time. Many
experiments indicate UV-spectrophotometer was used to study the initial and final
concentration of dyes.
The dye removal rate (R) in percentage and adsorption capacity (qe) mg/g at
equilibrium is given below [95].
R= [(Co –Ct)/Co] x100%
qe = [(Co –Ce)/m]V
Where ‘Co’ the initial concentration, ‘Ct’ the reaction process concentration, and ‘Ce’the equilibrium concentration
of the dye, ‘V’ the volume of the dye solution in liters and ‘m’ the mass of the carbon nanotube.
To calculate the adsorption performance at the different hydrodynamics is:
Remixing = ρNd2m/µ
Where ‘ρ’ the density, ‘µ’ the viscosity, ‘N’ the rotating frequency, and ‘d’ the diameter for the adsorption process.
4.5. Carbon nanotubes materials as dye adsorbents.
Based on the properties defined and discussed on the carbon nanotubes, it knows that
these are suitable for removing dyes; the CNTs and theirderivative (Table8) play a vital role.
Mona A. Shouman and his coworker [96] synthesized (CX/MWCNTs) with various loadings.
SEM, TEM, and N2 adsorption and FTIR are used to study the physical and chemical properties
of the resulting samples.The samples' adsorption capacity and catalytic activity are known
during the elimination of the Rhodamine dye from the solution. The specific surface area was
increased, and these materials are known to be microporous materials. The synthesized
nanohybrids have shown an appreciably high absorption capacity of 154-256mg/g, and these
nanohybrids will remove RB dye completely removed in the presence of H2O2 and visible light
at 60min. Later on, Sachin G.S. et al. [97] prepared C, N, S, and NiCNSZrO2/MWCNT’s
nanocomposites are in the homogeneous co-precipitation method. The largest photocatalytic
activity on the carmine anionic dye indicates by 1% Ni, C, N, s doped ZrO2/MWCNTs are
confined to the low bandgap energy and low recombination. Asadollah M et al. [98]
synthesized (MWCNTs/Gly/β-CD) as a novel absorbent and advanced for the removal of dyes.
The results show that the highest capacities MB, AB113, MO, and DR1 onto MWCNTs/Gly/β-
CD were 90.90 mg g−1, 172.41 mg g−1, 96.15 mg g−1, and 500 mg g−1, respectively. From the
results, it is understood that MWCNTs/Gly/β-CD has an absorbing capacity to remove MB,
AB113, MO, and DR1 from the aqueous solutions. Ola A.Shabaan et al. [99] explained that
adsorption parameters like PH value dye concentration, contact time, and a dose of adsorbent
affect dye removal using MWNTs, which act as an effective adsorbent for removing various
dyes from wastewater. Further, Tian Yao et al. [100] developed HPGCB of mechanically
strong and more efficient absorbent. The adsorption studies observed that the HPGCB reached
a maximum adsorption capacity of 521.5mg/mL for the methylene blue (MB). The prepared
HPGCB has the great ability to remove organic pollutants or Dyes from the wastewater.
Moreover, Seyed M. S. A. et al. [101] investigated that the ZnO nanoparticles filled on
MWCNTs to remove Congo red dye from the aqueous solutions. They got parameters with a
high removal rate of about 99.8%. Zichao Li et al. [102] reported studies on adsorption of
rhodamine B, crystal violet dyes on functionalized multi-walled carbon nanotubes, confirming
single and binary adsorption of these dyes to be endothermic and physical based. It is reported
from the literature [103] that related to adsorption methods, MWCNTs exhibit better
performance than SWCNTs because of their structural composition. The porous nature of
MWCNTs is due to inner hollow cavities of small diameter formed from the interaction
between single CNTs resulted from van der Waals forces. Similarly, adsorption efficiency in
MWCNTs might be due to structural defects on a large scale, potentially active sites for
adsorption. Especially, the adsorption of a large number of biological contaminants is due to
aggregated pores. Laifu et al. [104] reported that the amorphous carbon nanotubes (ACNTs)
adsorbent and the hollow structures exhibited a distinguished adsorption capacity
(467.96mg/g) for CR dye due to their large specific area of about 877.09m2/g. and to the pore
diameter. It is also observed that the rigorous adsorption of CR was not due to the pH values
but is due to a lot of various pH-dependent adsorbents. Machado et al. [105] developed
activated carbon powder and MWCNTs as adsorbents to remove textile dye (Reactive Red M-
2BE )from the aqueous solution indicated a maximum capacity of 335.7mg g-1. Vahid and his
coworker [106] fabricated MWCNTs with TETA as an organic nanofiller showed flux recovery
ratio reached from 62.2% to 76.1%. The addition of 0.25% TETA with MWCNTs was the best
to achieve water flux, BSA solution flux, and dye rejection. Tirandai et al. [107] reported that
Ru nanoparticles supported on the SWCNTs have been observed to have a higher % dye
degradation at low initial dye concentration due to the increase in the Ru nanoparticles on the
SWCNTs. Yun et al. [108] prepared SWCNTs, and some of the nanometer iron oxide particles
are anchored to it. The AO-Fe-SWCNTs' adsorption of MB and MO has reached equilibrium
within 10min, and maximum adsorption capacity was observed to be 256.69 mg g−1 and 93.58
mg g−1, respectively. Mohamed et al. [109] synthesized zinc oxide nanocrystallites with various
weight ratios are integrated into the carbon nanotubes (ZnO/CNTs) by ultrasonication/
hydrothermal methods. These with 70 wt% of ZnO (ZnO(70)/CNT) s showed considerable
visible light photocatalytic activity enhancement for MB degradation up to 99% compared to
other nanohybrids. Guang et al. [110] explained that carbon nanotubes with a smaller size,
large π conjugation system, and high specific surface area were used to remove dyes and
environmental pollutants from the wastewater. The functionalized CNT@IL has more
adsorption capacity than the normal CNT for removing CR from the stock solutions. The
adsorption capacity of CNT@IL reached a maximum of 175.98mg g-1 at 298K for a while of
56min. Tansir, et al. [111] developed amino-functionalized multi-walled carbon nanotubes
(NH2-MWCNTs), and magnetic nanoparticles were embedded into them. These fabricated
NH2-MWCNTs @Fe3O4 are used to remove toxic methylene blue dye (MB) from the aqueous
solution, and the maximum adsorption capacity was observed to be 178.5 mg g−1. Isiaka et al.
[112] studied the removal of phenol and crystal violet dye by using the CNTs modified with
eutectic solvent (DES) was prepared and studied using NMR. The CNT-DES has enhanced the
adsorption capacity of 298 and 394 mg g-1 for PHE and CRV. Further, Janaína et al. [113]
developed chitosan hydrogel scaffold absorbent changed carbon nanotubes for removing food
dye in binary and single aqueous systems resulting in high adsorption capacities of 955 mg g-
1
and 902 mgg-1 for binary system and 1508 mg g-1 and 1480mg g-1 for a single system. The
observed thermodynamic parameters show a favorable, spontaneous, and exothermic
adsorption process.
Table 8. Adsorption studies on dyes using Carbon nanotubes (SWCNTs & MWCNTs) and their derivatives.
S.No Adsorbent Adsorbate or Method Capacity of Ref.
Organic dye adsorption (mg/g)
1. CX/MWCNTs Rhodamine B (RB) Langmuir, Freundlich, Flory- 154–256
[96]
nanohybrids Huggins, Halsey and Elovich
2. Ni, C, N, S and MWCNT indigo carmine Spectrophotometric method [97]
3. (MWCNTs/Gly/β-CD) MB, AB 113, MO and Langmuir isotherm method 90.90, 172.41,
[98]
DR 1 96.15, and 500
4. Multi-walled carbon Acid Scarlet 3R
[99]
nanotubes (MWCNTs)
5. Highly porous Methylene blue (MB) Langmuir 521.5
[100]
graphene/CNTs hybrid
6. ZnO/MWCNTs Congo red (CR) Pseudo first and second-order 249.51
[101]
model
7. MWCNs Crystal violet (CV) Physical modeling 0.59 to 0.88 mmol/g
and rhodamine B and (for CV) and
[102]
(RhB) 0.77 to 0.9 mmol/g
(for RhB)
8. Multiwall carbon Textile Pseudo-second order model
[103]
nanotubes (CNTs)
9. Amorphous carbon Congo red and Methyl Langmuir model 467.97 & 253.26
[104]
nanotubes (ACNTs) orange
10. MWCNTs Reactive Red M-2BE 335.7 [105]
11. TETA-MWCNTs Lanasol blue 3R Phase inversion method [106]
12. SWNT-Ru Congo red [107]
13. SWCNTs Methyl blue (MB) Pseudo-first-order and 256.69
& Methyl orange Pseudo-second-order kinetic & [108]
(MO) models 93.58
14. ZnO/CNT and ZnO/GO Methylene blue dye First-order model
[109]
(MB)
15. CNT@IL (carbon Congo Red (CR) Adsorption kinetic models 178
[110]
nanotube ionic liquid) and Isotherm models
16. Amino functionalized Methylene blue (MB) Langmuir isotherm 178.5
multi-walled carbon
[111]
nanotubes (NH2-
MWCNTs)
17. CNT–DES (Deep Phenol (PHE) and Pseudo-second-order 298 (PHE) &
Eutectic Solvent) Crystal violet dye 394(CRV) [112]
(CRV)
18. Chitosan hydrogel food red 17 (FdR17) Langmuir model 1508 & 1480
scaffold modified with & food blue 1 (FdB1) [113]
CNTs
4.6. Carbon nanotubes materials as pesticide adsorbents.
Considering the extensive usage of carbon nanotubes and their applications in several
fields, it does not surprise their usage in pesticide analysis. Pesticides are widely used in
agriculture against pests damaging the crops, thereby preventing the loss and raising the yield
in crops, vegetables, and fruits[114,115]. An organophosphorus insecticide named diazinon
was widely used to control the pest in animal husbandry and agriculture activities. As per the
assumption of WHO, diazinon insecticide refers to have a medium risk with acute oral toxicity
300mg/kg [116]. Reports indicate that 0.5-0.1µg/L amount of pesticide is permitted in water
[117]. These pesticides severely harm human health in terms of disorder in the central nervous
system leading to severe disorders in the intestines, chest, vision, neuro, hypotension, coma,
etc., [118-120]. Some methods for removing organophosphorus pesticides include oxidation,
adsorption, decomposition (biochemical& electrochemical), photocatalysis, and membrane
separation. An interesting method to remove pesticides from aqueous solutions is adsorption
because of its performance efficiency, simplicity, and eco-friendliness [121-124]. Silica
particles and magnetic materials include various types of adsorbents [125].
The diazinon removal efficiency using multi-walled carbon nanotubes was given by
RE = [(Ci –Ct)/Ci] x100%

Where ‘Ci’the initial concentration and ‘Ct’ the final concentration at time t.
It is reported by Mohammad et al. [127] that multi-walled carbon nanotubes (MWCNT)

are most adequately used to take out nearly 100% of malathion from water at the optimized
conditions of initial pesticide concentration of 6 mg/L, initial multi-walled carbon nanotubes
of concentration, 0.5 g/L, contact time, 30 min; neutral pH; and ambient temperature (24 ± 2
C). Considering the reports of the research, it is concluded that the MWCNTs have a larger
potential for the elimination of malathion from water. It also discussed that MWCNT is
considered because of low cost and action in correlation with conventional methods eliminating
cent percent of diazinon from water sources within 15minutes time of contact, adsorbent dose
of 0.1g/L, and initial concentration of 0.3 mg/L diazinon at a surrounding temperature of 25 ±
1°C. In common, the MWCNTs have a greater possibility of eliminating organophosphorus
pesticides, such as diazinon, from water [128]. Further, Jing et al. [129] developed the UAE-
DES pretreatment method merged with MSPE by HPLC for the detailed study of seven
pesticides in fruit and vegetable samples. This method was the best-proposed method to
determine pesticides. Adsorption studies on pesticides on to MWCNTs are listed in Table9.
Table 9. Adsorption studies on pesticides on carbon nanotubes (SWCNTs & MWCNTs) and their derivatives.
Adsorbent/ Aqueous PH CT IC AD OT SS MRE Ref.
Material solution (Contact (Initial pesticide (adsorbent (operating (Stirring (Maximum
type time) concentration) dose) (g/L) time) time) removal efficiency)
(mg/L)
(ZnO/MW Synthetic Neutral 2-30 6 & 10 0.1 to 0.5 24 Almost 100 for [127]
CNTs-OH water Range pesticide malathion
MWCNTs 4&7 15 0.1 100 [128]
MMWCNT Eutectic 8 50 [129]
solvent
(DES)
5. Conclusions
An expository analysis of carbon nano-adsorbents of graphene, graphene oxide,

reduced graphene oxide, and carbon nanotubes has shown high potential for removing dyes
and pesticides, which was one of phenomenal in environmental remediation. The use of
functionalization methods to fabricate carbon materials like graphene, graphene oxide, and
reduced graphene oxide with metal and metal oxide nanoparticles remarkably shows high
adsorption capacity towards organic pollutants. Notwithstanding the toxicity of carbon nano
adsorbents, their strong affinity towards dyes and pesticides leads to their removal even at low
concentrations (µg-1). SEM, TEM images have characterized the prepared functionalized
materials, and their adsorption studies were evaluated by UV-Visible absorption studies, IR
studies, and adsorption-desorption by nitrogen methods. The adsorption mechanism is mainly
based on the interaction between adsorbate and adsorbent hydrophobic, hydrogen bonding, π-
π interactions, electrostatic, covalent, etc. Especially there was strong binding was possible
when an aromatic ring was present in pesticides and dyes due to π-π interactions. Anyhow
graphene-based materials exhibit high adsorption capacity than others towards pesticides and
dyes. As well as polymer nanocomposites also play a predominant role in their removal. An
interesting finding was also noticed with magnetic nanoparticles, which were easily separated
from the organic pollutants after adsorption using an external magnetic field. The
functionalization of carbon nano-adsorbents imparts some specific properties like high surface
area, and functional groups are having oxygen atoms, porosity, and hydrophilicity. To treat
wastewater and agricultural waste, applying carbon nanomaterial adsorbents is highly
economical and yields good results. To reduce the leaching process of agro-waste into soil or
aquifers, treatment with carbon nano adsorbents is one of the best approaches in comparison to
others. But to explore their potential, it was required further studies at a large/pilot scale with
industrial operating conditions are mandatory. As well as another challenge will be its
application towards the treatment of pharma waste and medical waste in a practical way.
Finally, this review mainly focused on various nanocomposites with carbon materials using
graphene, graphene oxide, reduced graphene oxide, and carbon nanotubes in the removal of
dyes like methylene blue (MB), rhodamine B (RhB), methyl orange (MO), Malachite green
(MG) dye, etc. and pesticides like organochlorines, organophosphates, carbamates,
pyrethroids, etc.
Funding
This research received no external funding.
Acknowledgments
We are thankful to GITAM, Bengaluru management, for supporting research.
Conflicts of Interest
The authors declare no conflict of interest.
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Role of Carbon Materials Biointerface

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Review

Volume 12, Issue 2, 2022, 1974 - 1997

Role of Carbon Materials in the Removal of Organic

organic compounds like pesticides, synthetic dyes, polyaromatic compounds, and

2. A Pragmatic View on Emerging Contaminants (ECs)

Table 1. Pesticide classification based on the hazard level.

A noteworthy finding was observed that a detectable trace of pesticides like

Table 2. Classification of pesticides with examples.

It exhibits non- Cypermethrin and

Amongst farmers from developing countries, pesticide poisoning was jeopardized,

Table 3. Classification of dyes with examples.

3. Adsorption Studies for the Quest of Good Adsorbents

To reduce organic pollutants in the aquatic ecosystem, impeccable methods are

∆Ho / RgT2 = - (δ ln P/∂T) Cµ,

Enthalpy and entropy are related to each other as:

Table 4. A gist on modeling methods used in adsorption.

4. Carbon Materials in Nutshell

In discourse about adsorbents, the carbon-derived nanomaterials [28] occupied apex

4.1. The uniqueness of graphene and its derivatives.

Hummers method Modified Hummers method

Figure 1. Strategic approaches in the synthesis of graphene.

4.2. Graphene materials as dye adsorbents.

4.3. Graphene materials as pesticide adsorbents.

4.4. Carbon nanotubes (CNTs)-A capstone among carbon nanomaterial.

Table 6. Adsorption studies on pesticides using graphene and its derivatives.

Table 7. Comparison between SWCNT and MWCNTS.

To calculate the adsorption performance at the different hydrodynamics is:

4.5. Carbon nanotubes materials as dye adsorbents.

4.6. Carbon nanotubes materials as pesticide adsorbents.

RE = [(Ci –Ct)/Ci] x100%

It is reported by Mohammad et al. [127] that multi-walled carbon nanotubes (MWCNT)

An expository analysis of carbon nano-adsorbents of graphene, graphene oxide,

This research received no external funding.

We are thankful to GITAM, Bengaluru management, for supporting research.

The authors declare no conflict of interest.

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