POLL Volume 7 Issue 1 Pages 153-179

Pollution, 7(1): 153-179, Winter 2021 Review Paper
DOI: 10.22059/poll.2020.307069.859
Print ISSN: 2383-451X Online ISSN: 2383-4501
Web Page: https://jpoll.ut.ac.ir, Email: [email protected]
The role of nanoadsorbents and nanocomposite adsorbents in the

removal of heavy metals from wastewater: A review and prospect
Nik-Abdul-Ghani, N. R., Jami, M. S.* and Alam, M. Z.
Department of Biotechnology Engineering, Faculty of Engineering, International

Islamic University Malaysia, Jalan Gombak, 53100 Kuala Lumpur, Malaysia.
Received: 27.07.2020 Revised: 19.10.2020 Accepted: 21.11.2020
ABSTRACT: Significant attention has been given to nanotechnology as an emerging

approach in water/wastewater treatment for heavy metals removal. Numerous research
works on synthesizing, fabrication and upgrading nanoparticles have reported as an
efficient adsorbent in removal of wide range of heavy metals from wastewater. This
review intends to provide researchers with understanding and knowledge regarding the
efficient nanoadsorbents, their adsorption mechanism towards selected heavy metals and
fundamental principles of nanoadsorbent materials synthesis. In addition, further attention
on the modification of nanoadsorbent and development of nanocomposites are
highlighted in this paper as value added products to increase the adsorption capacity and
enhance the heavy metals removal. Possible challenges and direction on utilization of
nanocomposites for heavy metal removal in real wastewater effluent are discussed in
view of their removal capability and cost efficiency. Future research works on
developing a cost-effective way of nanocomposite production and toxicity testing of
nanomaterials in wastewater applications are recommended. Further studies on the
efficiency of the nanoadsorbents in pilot or industrial scale are highly needed to test the
practicality of the nanoadsorbents for selected heavy metals removal from real
wastewater.
Keywords: Nanomaterials; adsorption mechanism; adsorption capacity; wastewater
treatment.
INTRODUCTION industrial usage. Production of wastewater

Water is an important element that is is increased proportionally with the
consumed by human and all living things increasing global population; hence it is
having a key role in our survival. The vital to remove all pollutants from
growing world population, depleting water wastewater in providing adequate water
resources and climate change causing quality for human and environmental needs
prolonged droughts, floods and other (Boretti & Rosa, 2019; Teklehaimanot et
consequences have rendered clean water a al., 2015). A broad range of contaminants
competitive resource worldwide (UN- exist in wastewater such as heavy metals,
Water 2020). Therefore, it is necessary to organic and inorganic compounds that have
have a sustainable and reliable treatment been released from industrial effluent will
technologies to ensure the clean water give harmful effects towards human and
supply continuously either to domestic or ecosystem (Dubey et al., 2016; Hasbullah
et al., 2018). Thus, removal of unsafe
* Corresponding Author, Email: [email protected]
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Nik-Abdul-Ghani, N. R., et al.
pollutants from wastewater especially copper, cadmium, chromium, silver and

heavy metal ions is significant. other hazardous metallic pollutants need to
Over the years, the main cause for the be removed from wastewater effluent in
release of heavy metals into environment is turn to make water safe and consumable to
due to rapid industrialization. Heavy metal is the living things. The major means of
any dense metallic chemical element or heavy metals entering the body is through
metalloid with hazardous properties, and it is drinking water. Though our body needs
naturally occurring element that can be found some heavy metals, excessive exposure of
throughout the earth’s crust. Water with heavy metals will lead human to serious
heavy metals contamination is one of the health problems such as gastrointestinal
major problems that increased dramatically tract, cardiac, vascular and central nervous
which led to the environmental and health system as well as affect mental health
concerns worldwide (Ali et al., 2020; (Krause et al., 2015; Pramanik et al.,
Masindi & Muedi, 2018; Mehdinia et al., 2016). Other possible symptoms because
2020). The main sources of heavy metals are of heavy metals toxicity are depression,
wastewater effluents of modern chemical sleep disorder, aggressive behavior, mood
industries such as metal plating facilities, swings and memory loss (Masindi &
battery manufacturing, fertilizer, mining, Muedi, 2018; Tchounwou et al., 2012).
paper and pesticides, metallurgical, mining, The permissible concentrations limits for
fossil fuel, tannery and plastic production each selected heavy metal and their
(Ali et al., 2020; Ihsanullah et al., 2016). toxicities effect on human are summarized
Heavy metals such as arsenic, lead, in Table 1 below.
Table 1. Standard limit of selected heavy metals in drinking water (WHO, 2017)
EPA maximum
Heavy metals WHO guideline
contamination Effects on human health
contaminant value (mg/L)
level (mg/L)
Damage the fetal brain, diseases of the kidneys, circulatory
Lead 0.015 0.01
system, and nervous system
Chromium 0.1 0.05 Headache, diarrhea, nausea, vomiting, carcinogenic
Cadmium 0.005 0.003 Kidney damage, renal disorder, human carcinogen
Copper 1.3 2 Liver damage, Wilson disease, insomnia
Arsenic 0.01 0.01 Skin manifestations, visceral cancers, vascular disease
Rheumatoid arthritis, and diseases of the kidneys, circulatory
Mercury 0.002 0.006
system, and nervous system
Dermatitis, nausea, chronic asthma, coughing, human
Nickel - 0.07
carcinogen
Zinc 5 3 Depression, lethargy, neurological signs and increased thirst
The common conventional methods that (Burakov et al., 2018; Siddiqui & Chaudhry,
had been utilized to remove heavy metals 2017.) Therefore, adsorption approach is
from wastewater effluents are chemical selected as the best alternative to remove
precipitation, solvent extraction, ion heavy metals from wastewater. It has been
exchange, electrochemical removal, and proved that adsorption is the most preferred
coagulation. However, these methods have method for purification, due to effectiveness,
limitations such as inconvenient, large space convenient stability, utility, low-cost, ease of
needed, incomplete removal, high energy operation and high performance (González et
consumption, low efficiency, generation of al., 2017; İnce & Kaplan İnce, 2017).
toxic sludge, and expensive disposal Adsorption is defined as mass transfer
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Pollution, 7(1): 153-179, Winter 2021
process by which a substance (adsorbate) is adsorbents for wastewater treatment and

transferred from the liquid phase to the water purification applications (Mohd et al.,
surface of solid (adsorbent) and bounded by 2017; Dave & Chopda, 2014; Qu et al.,
physical and/or chemical interactions(Khulbe 2013). Pacheco et al., (2006) also reported
& Matsuura, 2018). Conventional adsorbents the capability of nanoadsorbents that can
including carbon and natural sources showed adsorb the contaminants in terms of
the capability to remove heavy metals from molecular size, hydrophobicity and
wastewater with high removal of rate up to speciation behaviour. Besides that,
99%. The most widely used carbon source is nanoadsorbents are also enable the
activated carbon while natural source manufacturing processes to consume raw
adsorbents are from dead or living biomass materials efficiently without releasing any
such as algae, fungi and some higher plants toxic by-products (Burakov et al., 2018).
(Farooq et al., 2010; Karnib et al., 2014; Utilization of different types of adsorbents
Mqehe-Nedzivhe et al., 2018; Saleem et al., including conventional and nanostructured
2019). Other wastewater treatment for heavy materials in removing heavy metals from
metals removal was also investigated using wastewater has been well reviewed by
microbial fuel cell where the pollutants are different authors (Baruah et al., 2019;
removed by the application of electricity in Burakov et al., 2018; İnce and Kaplan İnce,
the presence of microbes as a biocatalyst 2017). Xu’s group and Yang’s group
(Das et al., 2019). However, lack of contributed significantly to the understanding
specificity, poor recyclability, high energy of nanomaterials and their application (Xu et
consumption, electric current instability, high al., 2018; Yang et al., 2019). These groups
material cost, low adsorption efficiencies and systematically reviewed the wide range of
capacities hindered their application in nanoadsorbents for heavy metals removal
concentrated solutions (Baruah et al., 2019; and their preparation, but few information
Thekkudan et al., 2017). Hence, various cost- was elaborated on the knowledge of the
effective, techno-economical and universal adsorption mechanism which is the
adsorbents especially nanoadsorbents have interaction between nanoadsorbents and
been developed in many water and heavy metals that has been influenced by
wastewater applications especially for heavy parametric effects on adsorption process (Xu
metals removal from wastewater (Ali et al., et al., 2018; Yang et al., 2019; Hasbullah et
2020; Thekkudan et al., 2017). al., 2019). On the basis of utilization of
From many previous findings, nanoadsorbents for heavy metals removal in
nanomaterials have been produced as a novel wastewater treatment, this review aims at
high efficiency adsorbent for heavy metal presenting an overview on the existing
removal from wastewater (Hua et al., 2012; nanoadsorbents and their adsorption
Ray & Shipley, 2015; Wang, 2012; Yang et mechanism that can be exploited for the
al., 2019). The development of well- synthesis of advanced nanoadsorbents. The
designed nanoadsorbents from metal oxides scope of this review will be elucidated on the
and carbon sources have been utilized in basic principle of adsorption process
broad industrial applications including including adsorption mechanism, isotherm
bioprocess, environmental remediation and and kinetic models to provide guidance in
their unique characteristics such as high the designing of ideal nanoadsorbents
reactivity, biocompatibility, high surface to system. Then, categories of current
volume ratio, reversibility, metal binding nanoadsorbents, advanced nanocomposite
capability and comparatively low cost as development are also discussed and
well as high degree of functionalization compared based on their advantages and
make them as potential high efficient limitations. Finally, possible
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recommendations for future researches and will form monolayer or multilayer

applications of the nanoadsorbents are adsorption and not very specific.
suggested. Meanwhile, in chemical mode of
adsorption, ionic or covalent bond occurs
Mechanism of metal ions adsorption by and makes the process highly specific. The
nanoadsorbent irreversible chemical interaction will form
Adsorption process involves physical and monolayer adsorption (Hasbullah et al.,
chemical interaction between an adsorbent 2019). There are several types of
and an adsorbate which depends on the adsorption mechanisms that explain the
reacting environment (Cheng et al., 2012; adherence of metal ions adsorbates such as
Hasbullah et al., 2018). Physical surface adsorption, precipitation,
interactions involve a weak van der Waals electrostatic interaction and ion exchange
forces between the adsorbate and adsorbent as illustrated in Fig. 1.
with a reversible process. The interactions
Fig. 1. Various adsorption mechanisms of metal ion adsorbate on nanoadsorbent
The mechanism of heavy metals can adsorb at equilibrium conditions and

adsorption can also be explained in detail by constant temperature. This adsorption
studying the adsorption isotherms, kinetics equilibrium relationship known as an
and thermodynamics. Apparently, the isotherm, allows the adsorption capacity of
adsorption mechanisms on nanoadsorbents the adsorbent to be calculated at any given
depend on the chemical nature and properties liquid-phase adsorbate concentration. The
of the material. Besides that, various equilibrium sorption phase is achieved when
parametric effects such as solution pH, initial the concentration of the adsorbate remains
metal concentration, adsorbent’s dosage, unchanged due to zero net transfer of
contact time and temperature influenced the pollutant that is adsorbed and desorbed from
nature of adsorption phenomenon as well the surface of the adsorbent. This equilibrium
(Batool et al., 2018; Wang et al., 2020). The phenomenon is vital for adsorption
details of each type of adsorption mechanism mechanism pathways optimization, surface
are explained here. properties indication and adsorbents
capacities as they can describe the
Adsorption isotherm relationship of contaminants with the
Adsorption isotherms are used to quantify adsorbents (El-Khaiary, 2008; Kyzas &
the quantity of adsorbate that an adsorbent Matis, 2015). The equilibrium solid-phase
156
adsorbate concentration can be calculated added to bottle (L), and M is mass of

from an experimental data that varies the adsorbent (g). There are four regular
adsorbent dose and/or the initial adsorbate isotherm models that have been utilized
concentration (Kyzas & Matis, 2015). From which are the Langmuir, Brauener-Emmett-
here, the relationship with the equilibrium Teller (BET), Freundlich, and Redlich-
liquid-phase concentration can also be Peterson isotherms. These isotherm models
established. The equilibrium capacity is are important to determine the most
calculated using a mass balance expression correlation between adsorbate and adsorbent
as Equation 1: as well as will provide the basis for the
V
design of ideal adsorption system (Auwal &
qe   Co  Ce  (1) Hossen, 2018; Chen, 2015; Kyzas & Matis,
M
2015). Summary of each of the models and
where qe is capacity of adsorption at their parameters are listed in Table 2.
equilibrium (mg/g), Co is initial Determination of the best fit isotherm model
concentration of adsorbate (mg/L), Ce is is obtained using the correlation of linear
equilibrium concentration of adsorbate regression (R2) to evaluate the data according
(mg/L), V is volume of aqueous solution to their equation.
Table 2. Isotherm Models

Model Equation Parameters and Constants
Q: maximum value of metal ion adsorption per unit
QK L Ce weight of adsorbent (mg/g)
Langmuir qe 
1  K L Ce KL: Langmuir constant (L/mg)
Ce: equilibrium concentration of adsorbate (mg/L)
KF: Freundlich parameters related to the sorption
capacity (mg/g)
Freundlich qe  K F Ce1/ n
n: intensity of the sorbent
ACe
A and B: isotherm constants of Redlich–Peterson (L/mg)
Redlich- qe 
1  BCeβ
β: exponential term which lies between 0 and 1
Peterson
CBET: BET adsorption isotherm (mg/L)
qs CBET Ce Cs: adsorbate monolayer saturation concentration (mg/L)
Bruener- qe 
C  Ce: equilibrium concentration of adsorbate (mg/L)
Emmett-Teller Cs  Ce 1   CBET  1  e 
 Cs  qs: theoretical isotherm saturation capacity (mg/g)
qe: equilibrium adsorption capacity (mg/g)
The Langmuir isotherm model indicates indicates the shape of isotherm (Weber &
that the adsorption of heavy metals occurs by Chakkrovarti, 1974; Kajitvichyanukul &
monolayer adsorption on a homogeneous Ananpattarachai, 2013).
surface where the adsorption sites have equal 1
affinities toward the adsorbate (Azizian et al., RL  (2)
1  K L Co
2018; Chen, 2015). Fig. 2 illustrates the
monolayer adsorption mechanism of heavy The value of RL is calculated and the
metals ion on the surface of nanoadsorbent. type of isotherm can be defined as
The important characteristics of the favourable when 0 < RL < 1, linear when RL
Langmuir isotherm can be expressed by a = 1, unfavourable when RL > 1 and
dimensionless constant known as irreversible when RL= 0.
equilibrium parameter RL as defined in
Equation 2 below where this parameter
157
Fig. 2. Monolayer adsorption mechanism of Langmuir model adapted from Milewska-Duda et al., (2000)
Meanwhile, the Freundlich isotherm obtained from y-intercept of the plotted

model describes that the uptake of metal graph. The 1/n-value indicates the degree
ions occurs on a heterogeneous surface of non-linearity between the concentration
without uniform distribution of adsorption of solution and adsorption and often
heat on the surface (Al-Ghouti et al., describes in the range of 0 < 1/n < 1. The
2019). From the equation of Freundlich higher the 1/n value, more favorable is the
above, KF and n parameters can be adsorption and when the 1/n = 1, it
obtained by linearized Equation 3 below: signifies that the relative adsorption
(adsorption partition) of the chemical was
1
log qe    log Ce  log K F (3) the same across the whole range tested,
n
which is unusual (Alimohammadi et al.,
where 1/n is the intensity of adsorption or 2017; Kyzas et al., 2014; Singh, 2016).
heterogeneity factor from slope value The visual of the Freundlich isotherm is
while KF is the adsorption capacity represents in Fig. 3.
Fig. 3. Visual representation of Freundlich isotherm model adapted from Singh (2016)
The Redlich-Peterson model denotes Ce

ln  β ln Ce  ln A (4)
that the adsorption equilibrium over a qe
broad range of adsorbate concentration.
This model is an empirical isotherm with The determination of Redlich-Peterson
three parameters that integrates elements constants is obtained by plotting a graph of
from both the Langmuir and Freundlich Ce/qe versus Ce where β is slope and A is y-
isotherms models and can be applied either intercept. The β value modifies the curve
in homogeneous or heterogeneous surface of the graph, when the β value increases,
(Ayawei et al., 2017; Kumara et al., 2014). the curvature increases. The calculated
The linear form of the Redlich-Peterson value indicates that when β = 1 the curve is
isotherm can be expressed as in Equation 4 same as Langmuir models and the value of
as follows: β is usually less than 1 for Redlich-
158
Peterson isotherm equation (Wu et al., (Kecili & Hussain, 2018). Many
2010). researchers have utilized BET method to
Another isotherm model of adsorption analyze the surface area of various carbon-
process is Bruener-Emmett-Teller (BET) based adsorbents such as activated carbon
isotherm model which represents the and carbon nanotubes (Kacan, 2016;
multilayer adsorption of the adsorbate to Kumar & Jena, 2016; Maryam et al.,
the surface of adsorbent. From BET 2013). The illustration of multilayer
isotherm model, the surface area and the adsorption of heavy metals ions on
porosity of the materials can be determined nanoadsorbent is displayed in Fig. 4.
Fig. 4. Multilayer adsorption mechanism by BET isotherm model adapted from Lyubchik et al., (2011)
Adsorption kinetics mechanism and rate controlling steps

Adsorption kinetics is the adsorption including external mass transport, chemical
uptake measurement with respect to time at reaction kinetics and diffusion models
a constant pressure or concentration. It is (Torrik et al., 2019). Four models of
employed to quantify the diffusion of adsorption kinetics (pseudo-first order,
adsorbate in the adsorbent or membrane pseudo-second order, Elovich and
pores (Saha & Grappe, 2017). The rate of intraparticle diffusion) are the most cited in
retention or release of a solute from an many published works related to the
aqueous solution to solid-phase interface adsorption models of heavy metals because
can be described by adsorption kinetics at they can fit the obtained data (Mercado-
certain experimental condition such as Borrayo et al., 2014; Xu et al., 2018). The
adsorbent dosage, flow rate, temperature linear form equation and parameters
and pH (William Kajjumba et al., 2018). description of the adsorption kinetics
Mathematical modelling of adsorption models are given in Table 3.
kinetics describes the adsorption
Table 3. Adsorption Kinetic Models
Equation Basic
Model Parameters and Constants
and Linear Form
dq
Lagergren, pseudo-  k1  qe  q  qe: Equilibrium adsorption capacity (mg/g)
dt q: Time adsorption capacity (mg/g)
qt  qe 1  e k1t 
first order model
k1: First-order rate coefficient (l/min)
dq
 k2  qe  q 
2
dt qe: Equilibrium adsorption capacity (mg/g)

Ho, pseudo-second
q: Time adsorption capacity (mg/g)
order model t t 1
  k2: Second-order rate coefficient (g/mg min)
q qe k2 qe2
dq
 α exp   βqt  qt: Time adsorption capacity (mg/g)
Elovich equation dt α: Initial adsorption rate (mg/g min)
qt  β ln  αβ   ln  t  β: Desorption constant (g/mg)
qt: Time adsorption capacity (mg/g)
Intra-particle
diffusion qt  ki t1/ 2  C ki: rate constants(mg/g.min1/2)
C: constant that approximates the thickness of the boundary layer (mg/g)
159
The kinetics model can explain the coefficient, k2 and equilibrium adsorption
adsorption mechanism in detail. The capacity (qe) can be calculated from the
Lagergren, pseudo-first order kinetic model intercept and slope from the graph of t/qt
is used based on the adsorptive capacity. versus t, respectively.
The rate constant of k1 is the time scale for The Elovich model helps to envisage the
the process to achieve equilibrium. It is mass/surface diffusion as well as
stated to decrease when increasing the activation/deactivation energy of a system
initial concentration which is indicates that which includes the chemical reactions
a longer time is needed if the initial (Kajjumba et al., 2018). The model
concentration is higher (Tan & Hameed, assumes that the adsorption rate of solute
2017). Some reports have found that k1 is decreases exponentially as the amount of
independent of initial concentration which adsorbed solute increases. The graph of qt
is expected to be affected by other vs t will aid to determine the nature of
experimental conditions of temperature and adsorption on the heterogeneous surface of
pH (Tan & Hameed, 2017; Yousef et al., the adsorbent. For the intraparticle model,
2011). The first order rate constant, k1 and the rate limiting step during adsorption is
adsorption capacity, qe can be determined examined and it is divided by three steps: i)
from the slope and intercept of linear graph liquid film diffusion to the adsorbent
of (qe−qt) versus t, respectively. The surface, ii) pore liquid diffusion and iii)
pseudo-second order model assumes that adsorption and desorption of the adsorbate
the adsorption rate is controlled by electron (Xu et al., 2018; Kajjumba et al., 2018;
sharing and transfer between adsorbate and Yildiz, 2018). The schematic diagram of
adsorbent through chemical adsorption the three consecutive steps for physical
where the rate of adsorption of solute is mechanism of heavy metal ions adsorption
proportional to the available sites on the on the surface of nanoadsorbent is
adsorbent (Xu et al., 2018). By plotting the illustrated in Fig. 5.
linear graph, values of second order rate
Fig. 5. Schematic diagram of adsorption mechanism for intraparticle kinetics model adapted from Yildiz
(2018)
160
Thermodynamics Synthesis of nanoadsorbent

The adsorption thermodynamics can be There are two fundamental approaches to
divided into three parameters which are synthesis nanoadsorbents which are top-
adsorption Gibbs’ free energy, enthalpy down and bottom-up approach to obtain
change and entropy change. Thermodynamic nanomaterials of desired sizes, shapes, and
studies are investigated to identify the effects functionalities(El-sayed, 2020; Singh et al.,
of temperature on the adsorption process. 2018). Top-down approach is the
Three thermodynamics state can be conventional method where the process
determined by each equation as stated in starts from larger particle (macroscopic)
Table 4. and the size reduction to nano-scale is done
by externally- controlled source of energy
Table 4. Thermodynamics state and mathematical applied such as erosion, sputtering, reactive
equations
milling, high energy ball milling and
Thermodynamics
Equation mechanical alloying (Singh et al., 2018;
parameter Soni et al., 2018). However, the main
Gibbs’s free energy
G  RT ln Ko problem faced by top-down method is
(ΔG°)
Enthalpy change associated with the crystallographic and the
G H   T S  surface structure destruction that might be
(ΔH°)
Entropy change(ΔS°) ln Ko  S  / R  H  / RT occurred during particle size reduction (El-
sayed, 2020). Therefore, bottom-up
Thermodynamic calculations basic approach is such a modern and new
principle is based on the adsorption isotherm, technique to synthesize nanoadsorbent
which gives the amount of the metals materials. The bottom-up approach applies
adsorbed in the porous adsorbent structure as physical and chemical processes that
a function of the amount at equilibrium in the operate at the nanoscale to integrate main
solutions (Lyubchik et al., 2011). components into bigger structures. The
Furthermore, thermodynamic studies provide bottom-up approach includes molecular
information on various adsorbent structural self-assembly, sol-gel, supercritical fluid,
characteristics and their effects on metal ions chemical and physical vapor deposition
adsorption. The negative value of where these methods produce
indicates the spontaneous adsorption process nanomaterials with less surface defects,
while positive value of shows the less contamination, homogeneous chemical
adsorption is not spontaneous. In contrast, composition and narrow particle size
value gives information either the distribution (El-sayed, 2020; Khaled-
adsorption process is endothermic or Habiba et al., 2014). Despite the difficulty
exothermic where positive value of is to scale-up production, this bottom-up
an endothermic adsorption process (Kecili & approach is the preferred technology
Hussin 2018). The correlation of because it can produce nanoadsorbent
equilibrium, kinetics and thermodynamics materials with specific properties fitted to
data using theoretical or empirical equations the remediation required (El-sayed, 2020).
can be used for the analysis and prediction of Fig. 6 below shows the route of synthesis
adsorption data. All these mathematical for both top-down and bottom-up
models including linear and non-linear approaches in carbon-based nanomaterials
equations are applicable in describing synthesis.
experimental data of adsorption isotherms.
161
Fig. 6. Bottom-up and the top-down approaches in synthesis of carbon-based nanomaterials (Habiba et al.,
2014)
Type of nanoadsorbent in wastewater extensively in removal of heavy metals

treatment including mercury, lead, copper, nickel,
There are many types of nanoadsorbent that chromium, cadmium and arsenic from
have been utilized in water/wastewater aqueous solutions through adsorption
treatment and the most commonly used process (Li et al., 2005; Rodríguez &
nanomaterials are classified into three Leiva, 2019; Šolic et al., 2020). These
categories depending on their morphology, heavy metals are considered the most
size and chemical properties which are; 1) hazardous due to bioaccumulative, non-
carbon-based nanoadsorbents; 2) metal biodegradable and can extremely be
oxide- based nanoadsorbents and 3) polymer harmful to plants, animals and human. The
based nanoadsorbents. The details and hollow and multilayered structure of CNT
examples on each type of nanoadsorbents are owing to its high surface area characteristic
explained below. can contribute to the high adsorption
efficiency (Baruah et al., 2019). Surface
Carbon-based nanoadsorbents modification of CNTs using strong
Carbon based nanoadsorbents including oxidizing agents such as sulphuric acid and
carbon nanotube (CNT), multiwalled carbon potassium permanganate leads to the
nanotube (MWCNT) and graphene have introduction of hydroxyl and carboxyl
been widely utilized in many adsorption functional groups. Functionalized CNTs
processes for wastewater treatment. Due to have been reported to increase the binding
their unique characteristics of high specific capacity of heavy metal ions through
surface areas, large pore volumes, electrostatic bonding and create the active
nontoxicity, noncorrosive and existences of sites on CNTs for heavy metals adsorption
oxygen-containing surface, these (Fu & Wang, 2011; Mallakpour &
nanoadsorbents exhibit high removal Khadem, 2018).
efficiency of contaminants (i. e heavy Previous findings compared the
metals) from wastewater. efficiency of functionalized MWCNT for
CNT is one dimensional material under heavy metals adsorption at different pH
carbon-based nanoadsorbent class. Various values where the percentage removal and
types of CNTs have been utilized
162
sorption capacity increased when the value characteristics in terms of mechanical,

of pH was increased indicating adsorption electronic and thermal properties.
process is strongly dependent on pH Theoretically, graphene has a large specific
(Elsehly et al., 2016; Rodríguez & Leiva, surface area of 2620 m2/g, the value of
2019; Šolic et al., 2020). The adsorption Young’s modulus is 1 TPa with 130 GPa of
mechanism of functionalized MWCNT intrinsic strength. Due to hydrophobic nature
was mainly of ionic interaction where the and water repellant of graphene, it is not
interactions between metal ions and suitable to be utilized in water applications
carboxyl and hydroxyl groups has occurred (Yoon et al., 2016). Hence, synthesizing of
(Elsehly et al., 2016; Šoli´c et al., 2020). graphene oxide (GO) would be the best
On the other hand, Robati (2013) alternative to overcome this issue due to
investigated the adsorption studies of lead addition of oxygenous functional groups
ions removal by MWCNT and MWCNT- which contribute to the hydrophilicity
COOH and the result exhibited the properties of that nanoparticle (Nair et al.,
adsorption system fitted well with pseudo- 2012; Yu et al., 2020). Graphene oxide (GO)
second order kinetic indicating that the is the oxidized form of graphene which is
expression characteristics of reaction prepared by chemical oxidation of graphite
mechanism at variable concentrations were resulting in extended graphene sheets
excellent in the removal of lead from decorated with epoxy and hydroxyl
aqueous solution (Robati, 2013). Other functional groups in the basal planes and
findings on adsorption mechanism for carboxylic acid groups at the edges (Dreyer
copper removal from MWCNT also et al., 2010). GO is highly utilized in
showed the ion exchange mechanism adsorption process due to existence of
between copper ions and MWCNT with abundant oxygen functionalized groups, easy
high copper removal effectiveness of 93% for large-scale production and high surface
(Gupta et al., 2017). Recent research area (Alam et al., 2018; Mohan et al., 2017).
conducted by Bankole et al., (2019) Previous findings reported that graphene and
reported that functionalized CNT was graphene-based nanomaterials are promising
better in adsorption capacity of several nanoadsorbents and become the forefront
heavy metals compared to purified CNT research in water/wastewater treatment
and the data obtained agreed well with process due to strong mechanical stability,
Temkin model adsorption isotherm hydrophilicity, high negative charge density,
indicating good interaction between ease of fabrication, industry scale production
sorbate and sorbent, which is an evidence and the ability in heavy metal ion adsorption
of an ion-exchange mechanism during the from wastewater (Jayakaran et al., 2019;
adsorption. Therefore, it can be concluded Kyzas et al., 2014; Mkhoyan et al., 2009;
that both pure CNTs and functionalized Mohan et al., 2017; Peng et al., 2017; Yu et
CNTs are promising nanoadsorbents in al., 2020).
heavy metals removal but functionalized Previous findings by Madadrang et al.,
CNTs possesses better adsorption capacity. (2012) reported on the comparison of
Another carbon based nanoadsorbent that nanoadsorbents from GO, GO-EDTA and
is widely utilized in wastewater treatment is reduced GO-EDTA for lead removal.
graphene. Graphene is a unique two- Accordingly, they found that GO-EDTA
dimensional structure consisting of a single displayed enhanced adsorption capacity.
atomic layer of sp2 hybridized carbon atoms The experimental data showed that
and densely packed in a honeycomb crystal adsorption mechanism fitted well with
lattice. Graphene is the strongest, yet lightest Langmuir isotherm model which involved
material known. It has excellent two ion exchange of adsorption processes;
163
i) interaction of lead ions onto the surface adsorption capacities of copper, zinc,
of GO to form the complex and ii) complex cadmium and lead on GO at pH 5 were
formation of EDTA with lead and -COOH 294, 345, 530, 1119 mg g−1, respectively
group for complete removal of lead while the adsorption isotherms and kinetic
(Kumar et al., 2019; Madadrang et al., studies were fitted well with Langmuir
2012). Previous study by Sitko et al., isotherm and pseudo second order kinetic
(2013) investigated the adsorptive models, respectively for all divalent metal
properties of GO towards divalent metal ions (Sitko et al., 2013). The mechanism of
ions such as copper, zinc, cadmium and adsorption between GO and divalent metal
lead. In this work, the maximum ions is illustrated in Fig. 7.
Fig. 7. Schematic diagram of adsorption process of divalent metal ions on GO (Sitko et al., 2013)
The study of Mohan et al. (2017) double-exponential kinetics and Redlich–

synthesized graphene oxide-MgO Peterson isotherm models and this
nanohybrid for removal of lead ions from nanofiber showed high reusability with up
aqueous solution. From the results, lead to fifth cycle of regeneration (Hadi
adsorption by graphene oxide -MgO Najafabadi et al., 2015).
mechanisms are controlled by external The modification on GO by synthesizing
mass transfer and intraparticle diffusion, the magnetic GO (MGO) by Ain et al.,
the Langmuir model also suggested the (2020) for heavy metals removal stated that
monolayer adsorption has occurred. different heavy metals had maximum
Meanwhile, White et al., (2018) sorted out adsorption capacities at different pH
carboxylated graphene oxide for large conditions. The findings reported that the
adsorption of copper on the surface of adsorption mechanism followed Langmuir
graphene oxide-COOH compared to the isotherm and pseudo-second-order kinetics
graphene oxide and both GO and GO- model with spontaneous and endothermic
COOH were fitted well with the Langmuir process (Ain et al., 2019). The advantages of
isotherm. The optimization of adsorption using magnetic nanocomposite could be
conditions of lead removal by GO also easily separated from treated water and
reported to be at pH 7 with initial reduce recontamination. However, in terms
concentration of 100 mg/L, 10 minutes of of separation of pure graphene and GO it
contact time and fitted with Langmuir would be difficult (Khan et al., 2017).
isotherm model (Nik-Abdul-Ghani et al., Several types of carbon-based
2019). Graphene oxide-chitosan nanofibers nanoadsorbents and their optimum
revealed that adsorption kinetics and conditions with adsorption capacity are
equilibrium data for lead were described by summarized in Table 5 below.
164
Table 5. Comparative table on carbon-based nanoadsorbents on optimum parameters and removal

efficiency
Carbon-based Heavy Contact Adsorbent Initial metal Removal efficiency/maximum
pH Reference
nanoadsorbent metals time dosage concentration adsorption capacity
CNT Pb 5 20 min - 30 mg/L 35 mg/g Li et al., 2005
Cu 99%
Co 85% Stafiej &
CNT Zn 9 20 mg/L 82% Pyrzynska,
Mn 58% 2007
Pb 87%
Oxidized MWCNT Pb NA 35 min 0.05 g - 20 mg/g Robati, 2013
Elsehly et al.,
MWCNT Ni 8 0.6 min 0.6 mg 85 %
2016
Gupta et al.,
MWCNT Cu 3 60 min 10 mg 20 mg/L 93 %
2017
Fe 15.92%
Ni 77.95%
Cd 99.34%
Polyhydroxylbutyrate
Pb 98.85% Bankole et al.,
Functionalized Carbon 5.65 10 min 20 mg
Cu 83.08% 2019
Nanotubes
Zn 18.34%
Cr 98.19%
As 99.95%
Madadrang et
GO-EDTA Pb 6.8 20 min - 0.1 g/L 479 mg/g
al., 2012
Cu 60 min 294 mg/g

Zn 30 min 345 mg/g Sitko et al.,
GO 5 -
Cd 60 min 530 mg/g 2013
Pb 60 min 1119 mg/g
GO 97%; 277.77 mg/g White et al.,
Cu 6 60 min - 50 mg/L
GO-COOH 99.4; 357.14 mg/g 2018
Mohan et al.,
GO-MgO nanohybrid Pb 6.5 30 min - 0.4 g/L 190 mg/g
2017
Nik-Abdul-
GO Pb 7 10 min 0.1 mg 100 mg/L 99%; 500 mg/g Ghani et al.,
2019
5 25 min 200 mg/g
Pb 6 35 min 0.014 g/L 24.330mg/g
Magnetic GO Cr Cu 6 25 min - 62.893 mg/g Ain et al., 2020
Zn Ni 7 35 min 0.016 g/L 63.694 mg/g
8 25 min 51.020 mg/g
Briefly, carbon-based nanoadsorbents properties of GO and GO–COOH were

that had been utilized in the adsorption for also reported that copper removal
heavy metals have different adsorption efficiency only reduced by 4.50% and
mechanisms in aqueous solutions based on 3.96%, respectively after five cycles of
the physical, chemical and electrostatic adsorption/desorption process (White et al.,
interaction. Mainly, adsorption process on 2018). The reusability of magnetic-GO was
GO and CNTs are dominated by ion evaluated, and the results showed that the
exchange mechanism due to presence of total adsorption capacity of MGO for
surface functional groups that allow heavy metals ions remained in the range of
interaction and provide high adsorption 87.51 % - 78.12 % after four successive
sites to heavy metals (Khan et al., 2017). adsorption/desorption cycles (Ain et al.
Many findings estimated the reusability of 2019). These findings supported that GO-
the carbon-based nanoadsorbents by based nanoadsorbents possess good
adsorption/desorption process. The reusability and regeneration properties
reusability of graphene oxide-chitosan (White et al., 2018; Ain et al., 2019).
nanofibers is reported by Hadi-Najafabadi Despite all the exceptional properties of
et al., (2015) which is up to fifth cycles of the carbon-based nanoadsorbents, the
regeneration process. The regeneration applications of CNTs in wastewater are
165
limited due to low volume of production ions on the external surface and secondly
and high cost. Besides, CNTs cannot be by the rate limiting intraparticle diffusion
used alone without any supporting or along the micropore (Koeppenkastrop &
matrix to form structural components and Decarlo, 1993; Trivedi & Axe, 2000;
the effective techniques for regeneration or Wang et al., 2020).
reuse of CNTs have not been elucidated yet
(Ihsanullah et al., 2016; H. Lu et al., 2016). Nickel oxide
In addition, some limitations of utilization The adsorption study of nickel oxide in
of GO are high water absorption and poor nanopowder form is reported for the
performance of the solid–liquid separation, removal of lead and zinc with enhanced
thus GO might remain in the filtered water catalytic activity and high adsorption
and will cause a risk of exposure to capacity with 50.5 mg/g and 63.7 mg/g
humans, animals, and other aquatic respectively (Abd El fatah & Ossman,
organisms (Pérez-Ramírez et al., 2016). 2014). The authors reported that lead
Moreover, these nanomaterials of CNTs removal by nickel oxide fitted well with
and GO also have limitations when used in Langmuir isotherm and pseudo second
the packed bed column process due to high order kinetic models while zinc removal
pressure drop when the small particles followed Freundlich isotherm and pseudo
were tightly packed and leading to the low first order kinetic model (Abd El fatah &
adsorption rates because of loss of active Ossman, 2014). Mahmoud et al., (2015)
adsorption sites (Zhang et al., 2019). reported that nickel oxide prepared by
organic solvent is capable of lead removal
Metal oxide-based nanoadsorbent and the equilibrium was achieved at 2-
Metal oxides nanoparticles provide high hour, and the adsorption mechanism fitted
removal capacity, high surface area and to Langmuir model and pseudo-first order
specific affinity towards heavy metal reaction. The green synthesis of nickel
adsorption and become a great potential as oxide from lemon juice extract also
nanoadsorbent for wastewater treatment showed the capability to remove
applications (Hua et al., 2012; Yang et al., chromium, copper and nickel from aqueous
2019). Metal oxides-based nanoparticles solution. The results obtained showed that
are nanosized materials (in range 1-100 the adsorption was highly pH dependent
nm) including manganese oxide, zinc and well defined with Langmuir isotherm
oxide, nickel oxides, iron oxides, and pseudo second order kinetic models
aluminium oxides, titanium oxide, (Panji et al., 2016). Recent finding by
magnesium oxides and zirconium oxides. Krishna et al., (2018) reported that
These metal oxide-based nanoparticles are chromium doped nickel oxide nanoparticle
the promising nanoadsorbents to remove offers a great potential for heavy metals
heavy metals from aqueous system due to removal including lead, cadmium and
their high adsorption capacity and large copper. The cation removal and high
surface areas (Hua et al., 2012; Taman, adsorption capacity in aqueous solution by
2015; Yang et al., 2019). All of these chromium doped nickel oxide is due to the
nanosized metal oxides have been utilized formation of hydroxide on the surface
in various heavy metals removal from nanoparticle with the adsorption kinetic
wastewater. The adsorption mechanisms of and isotherm models were well fitted using
metal oxides were governed by pseudo-second-order kinetic and
complexation between dissolved metals Freundlich isotherm model, respectively
and the oxygen in metal oxides with two (Krishna et al., 2018).
step process; firstly the adsorption of metal
166
Copper oxide cost and extraordinary removal capacity

Previous findings using copper oxide as (Ghiloufi et al., 2016; Khan et al., 2019; Le
nanoadsorbent showed high removal of et al., 2019). A study conducted by
heavy metals including iron and cadmium Ghiloufi et al., (2016) compared the
with adsorption capacity of 94.34 mg/g and adsorption capacities of doped gallium-
131.33 mg/g, respectively (Taman et al., zinc oxide nanopowders in different
2015). Moreover, Hassan et al., (2017) concentrations for cadmium and chromium
reported that copper oxide also has high removal from aqueous solution. The results
capability to remove other heavy metals showed high percentage removal of heavy
such as cadmium and nickel with respect to metal ions was at 1wt% of doped gallium
64.935 mg/g and 322.50 mg/g of zinc oxide compared to the bare zinc oxide
adsorption capacity, respectively. indicated that the incorporation of gallium
in zinc oxide nanoparticles could improve
Titanium oxide the uptake effect of these heavy metals.
Titanium oxides had been well studied for Green synthesis of zinc oxide also
the removal of heavy metals from aqueous exhibited maximum removal efficiencies
solution (Gebru & Das, 2017; Y. Lu et al., up to 93% of lead ion at pH 5 and
2016; Moon et al., 2014; Youssef & Langmuir isotherm fits with the adsorption
Malhat, 2014). Gebru and Das (2017) data indicated the favourable surface
reported that highest removal capacities of adsorption on the metal ions (Azizi et al.,
lead and copper were obtained by 2017). Le et al., (2019) also reported that
electrospun cellulose acetate/titanium zinc oxide nanoparticles can removed
oxide nanoadsorbent which were at effectively various heavy metals including
maximum removal efficiency of 99.7% and Cu (II), Ag(I) and Pb (II) ions with
98.9%, with adsorption capacity of 25 removal efficiency more than 85%.
mg/g and 23 mg/g, respectively as
compared to pure cellulose acetate. The Iron oxide
adsorption mechanism process was well Iron oxide nanoparticle has been extensively
fitted with the Langmuir isotherm model studied and reviewed as nanoadsorbent for
and pseudo-second order kinetic model for heavy metals removal due to their high
both lead and copper ions (Gebru & Das, surface area, small size, superior adsorption
2017). Other finding from Li et al., (2014) capacity, easiness of isolation method and
stated that titanium oxide was used for magnetic property (Dave & Chopda, 2014;
chromium removal using magnetic Nizamuddin et al., 2019; Vélez et al., 2016).
mesoporous titanium dioxide–graphene Baalousha, (2009) had studied the
oxide. The study showed that the aggregation properties of iron oxide at
adsorption process followed Freundlich different parameters including particle
isotherm and pseudo second order kinetic concentration and pH. Arsenic adsorption by
models with maximum adsorption Magnetic γ-Fe2O3 biochar exhibited
capability of 117.4 mg/g (Li et al., 2014). Langmuir isotherm and pseudo-first order
Thus, it demonstrated that titanium oxide is kinetic models adsorption mechanism with
a potential nanoadsorbent for wastewater the maximum adsorption capacity 3.147
application. mg/g (M. Zhang et al., 2013). Lin and Chen,
(2014) also reported that carbonized
Zinc oxide Fe3O4/phenol–formaldehyde resins were
In addition, zinc oxide is a nanoparticle capable for the maximum adsorption of
that has been synthesized and applied arsenic at 216.9 mg/g. Furthermore, iron
widely in heavy metals removal due to its oxide nanoparticles i.e. Fe3O4 and γ-Fe2O3
characteristics of high surface area, low
167
were successfully synthesized and removed Nizamuddin et al.; 2019). Therefore,

mercury from water with 87 % removal researchers suggested that functionalization
efficiency (Vélez et al., 2016). of metal oxides based nanoadsorbent could
However, metal oxides nanoadsorbent be implemented to overcome these
such as titanium oxides, zinc oxides and iron limitations and enhance their adsorption
oxides have several disadvantages when they properties. For example, addition of ligands
are used in the suspension especially in such as ethylenediamine tetraacetic acid, L-
wastewater treatment (Lu et al., 2016; glutathione and mercaptobutyric acid or
Nizamuddin et al., 2019). These addition of copolymers might increase the
nanoparticles are difficult to recover from the adsorption capacity of metal oxides (Ge et
treated water due to small size, complicated al., 2012; Lu et al., 2016; Warner et al.,
production procedure of metal oxides and 2010). The summary of metal oxide-based
production cost would hinder the upscaling nanoadsorbents and its optimum operating
process for water application (Lu et al., 2016; parameters are shown in Table 6.
Table 6. Comparative table on metal-oxides nanoadsorbent and their optimum operational parameters
Heavy Contact Adsorbent Initial metal
Metal oxide pH Reference
metals time dosage concentration
Independent of
Nickel oxide Pb 6 Abd El fatah &
120 min NA initial
nanopowder Zn 9 Ossman, 2014
concentration
Nickel oxide nano Mahmoud et al.,
Pb 5.8 120 min 0.2 g 5 mg/L
catalyst 2015
Cr 3 10 min 25 mg
Nickel oxide Ni 7 5 min 10 mg NA Panji et al., 2016
Cu 7 10 min 6 mg
Cd
Chromium doped Krishna et al.,
Pb 9 45 min 0.15 mg NA
nickel oxide 2018
Cu
Fe 0.3 mg
Copper oxide 6 20 min NA Taman et al. 2015
Cd 0.4 mg
Cd Hassan et al.,
Copper oxide 6 30 min 0.1 15
Ni 2017
Cellulose
Pb 5.2 300 min Gebru & Das,
acetate/titanium 2.5 wt.% NA
Cu 5.8 300 min 2017
oxide
Magnetic
mesoporous
Cr 2 40 min NA NA Li et al., 2014
titanium dioxide–
graphene oxide
TiO2 and γ-Al2O3 Shirzadeh et al.,
Cd 8 NA NA 80 mg/L
nanoparticles 2020
Doped gallium- Cd 5 10 min Ghiloufi et al.,
1 wt.% NA
zinc oxide Cr 3 760 min 2016
Zinc oxide-green
Pb 5 60 min 0.1 g 25 ppm Azizi et al., 2017
synthesis
Magnetic γ-Fe2O3
As NA 240 min NA 10 ppm Zhang et al., 2013
biochar
Iron oxide Hg NA 24 min 8 mg/L NA Vélez et al., 2016
Tabatabaei et al.,
Granule iron oxide As 5 49.9 min 8 mg/L 30 ppm
2020
NA: not available
168
Polymer based nanoadsorbent potential to remove various kinds of heavy

Conventional adsorbents have limitations metal ions from wastewaters and aqueous
such as lack of specificity, lower adsorption solutions (Samiey et al., 2014; Wadhawan
capacity and poor recyclability (Burakov et et al., 2020; Zare et al., 2018; Zhao et al.,
al., 2018; Siddiqui & Chaudhry, 2017). 2018). The study of Dubey et al., (2016)
Therefore, numerous organic-inorganic investigated the role of chitosan-alginate
hybrid polymers with stronger adsorption nanoparticle in removal of mercury. This
capacity, greater thermal stability and higher study showed that maximum adsorption
recyclability have been developed to capacity of 217.39 mg/g is achieved at
overcome the issues of conventional optimum conditions of pH 5 at 90 minutes
adsorbents (Lofrano et al., 2016). Polymeric contact time with 4 mg/L of initial ion
based nanoadsorbents having high specific concentration. Chitin nanofibrils, a
surface area, porous structure, and presence derivative of chitosan was fabricated by
of functional groups on the surface are Liu et al., (2013) to remove wide range of
identified to have the capability of binding metal ions such as cadmium, nickel,
efficiently towards organic dyes and heavy copper, zinc, lead and chromium.
metal ions including lead, arsenic, cadmium Dendrimers are another organic polymer
and zinc from wastewater (Lofrano et al., based nanoadsorbents with highly
2016; Baruah et al., 2019). branched and star shaped macromolecules
Different types of polymers which are in nanometer scale dimension. They
categorized based on materials used (i.e:; consist of three components which are a
chitosan, dendrimers, cellulose), methods central core, an interior dendritic structure
of preparation of a good nanoadsorbent, (the branches), and an exterior surface with
adsorption process and mechanism have functional surface groups (Vunain et al.,
been reviewed and demonstrated that the 2016) (Fig. 8).
polymer-based absorbents are good
Fig. 8. Structure of dendrimers (Vunain et al., 2016)
169
Mainly, the functional groups on Nanocomposite adsorbents

dendrimers in polymer based nanoadsorbent As mentioned above, every nanoadsorbent
are chelating functional groups (Wadhawan has its own disadvantages. Hence, to
et al., 2020). Previous report stated chelating overcome all these problems it is an effective
agents such as 3-aminobenzoic acid 1, 2- strategy to fabricate novel nanocomposites
diaminoethane or 1, 3-diaminopropane were for water and wastewater treatment. New
used for modification of poly (styrene-alt- strategy in nanoadsorbent modification by
maleic anhydride) and the percentage incorporating nanoparticles with
removal efficiency of heavy metals were polymer/metal/carbon based has been
reported in the descending order of Fe introduced to produce various types of
(II)>Cu (II)>Zn (II)>Pb (II) (Hasanzadeh et nanocomposites. Recently, there are several
al., 2012). Polyacrylonitrile is selected as types of nanocomposite that have been
base polymer to prepare three ion selective developed which are inorganic-polymer,
nanofibers modification with chelating organic-polymer and magnetic
groups of ethylenediamine (EDA), nanocomposites that take advantages from
ethyleneglycol (EG) or diethylenetriamine different nanomaterials (Yang et al., 2019).
(DTA) by (Martín et al., 2018). In this study, These nanocomposites would improve the
obtained values of adsorption capacity for Cu adsorption performance and provide more
(II), Pb (II) and Zn (II) are 6.1, 8.8 and 7.2 specific interaction with the targeted
mmol/g, respectively which are higher than contaminants, thus, better adsorption
other materials due to large surface area and capacity and high efficiency removal of
high degree of surface functionalization as a heavy metals from wastewater would be
results of greater number of chelating groups achieved (Yang et al., 2019; Zhao et al.,
accessible for metal adsorption (Martin et al., 2018). Nanocomposites have many
2018). advantages in terms of low cost, stability,
Biopolymer based nanoadsorbents such better mechanical properties, low energy
as cellulose had been studied for uptake of consumption, susceptible to high temperature
heavy metal ions. Previous finding by and harsh chemical environments (Barak et
Mautner et al., (2016) stated that cellulose al., 2018). Moreover, the development of
nanofibrils with phosphate groups adsorbed hybrid nanocomposite adsorbents also
Cu (II) ions efficiently from aqueous provides amazing advantages in terms of
solution due to existence of functional physiochemical stabilities and magnetic
groups on the surface of the nanopapers. characteristics for wastewater treatment
Other cellulose based nanoadsorbents such applications (Nizamuddin et al., 2019).
as cellulose gels, cellulose composites and Several works on nanocomposites, their
derivatives as well as nanocrystalline adsorption mechanisms and remarkable
cellulose had been reviewed by Jamshaid et discoveries are summarized in Table 7
al., (2017) and results exhibited the below. The reusability and longevity of the
adsorption capacity of heavy metals were nanocomposite adsorbents also had been
enhanced successfully. Furthermore, other reported by several findings that the
polymer based nanoadsorbents such as nanocomposite adsorbents possess a very
chitosan, polyaniline, polypyrrole, poly(1- good regeneration properties as the key
amino-5-chloroanthraquinone) have been factor for the cost-effective strategy of heavy
fabricated for heavy metals removal and the metals removal from wastewater
adsorption studies and mechanism have (Ahmaruzzaman, 2019; Ge et al., 2012;
been reported (Dubey et al., 2016; Huang et Hadi-Najafabadi et al., 2015; Mahmoudi et
al., 2016; Mahmud et al., 2017; Piri et al., al., 2019; Nasir et al., 2019; Razzaz et al.,
2016). 2016).
170
Table 7. Summary of efficacy for various nanocomposite adsorbents for heavy metals removal
Heavy Parametric
Nanocomposite Results/Findings Remarks Reference
metals conditions
Magnetic iron oxide pH 5.5
modified with 30 minutes of contact Adsorption capacities for cadmium,
Cd The metal ion adsorption capacity remained
copolymers (acrylic time zinc, lead and copper were 29.6, 43.4,
Zn constant for 4 cycles, indicates no irreversible
acid and crotonic acid) initial concentration of 166.1 and 126.9 mg/g, respectively. Ge et al., 2012
Pb sites on the surface of Fe3O4@APS@AA-co-
and 3- metal ions, 20–450 Langmuir isotherm
Cu CA MNPs
aminopropyltriethoxys mg/L Pseudo-second order kinetics
ilane T = 298 K
Superior adsorption capacity property is due
pH = 5 for Pb(II) Langmuir isotherm to the combination of the unique layered
Graphene oxide–
Pb pH = 4 for As(V) Pseudo-second order nature (allowing maximum surface area) of Kumar et al.,
MnFe2O4 magnetic
As pH = 6.5 for Surface complex formation theory the hybrid system and the good adsorption 2014
nano-hybrids
As(III) -spontaneous and endothermic capabilities of both the GO and NP.
Magnetic separation
Contact time: 20 Maximum adsorption capacities were X-ray photoelectron spectroscopy analysis
Hydrous minutes 62.33 and 41.31 mg/g for As(III) and indicated that the major chemical state of
cerium oxide– As Maximum adsorption As(V) cerium (Ce) element in the adsorbent was Yu et al., 2015
graphene composite at pH 4.0 (As (III)) and Langmuir isotherm +IV and the hydroxyl group might be
pH 7.0 (As (V)) Pseudo-second order involved in the adsorption process.
The sorption process occurs in two steps:
Double-exponential kinetic model
Contact time 6 h, i) external diffusion (transport of the metal
D–R isotherm model indicated that the
U temperature 45 °C, ion to the external surface of the adsorbent)
Electrospun PVA/ZnO mechanism of U(VI), Cu(II) and Ni(II) Hallaji et al.,
Cu adsorbent which is a rapid phase, ii) the pore diffusion
nanofiber sorption on the nanofiber adsorbent 2015
Ni concentration 1 g/L and (sorption of the metal ion on the interior
was physisorption
pH 5 surface of the adsorbent) which is a slow
Endothermic and spontaneous
phase
The composite with absorbed Pb(II) can be
pH=7.0 with the initial
Reduced GO-Fe3O4 Adsorption capacity was 30.68 mg/g easily collected by magnetic separation from
Pb concentration of Pb(II) Cao et al., 2015
composite Langmuir isotherm wastewater because of the excellent
ions of 80 mg/L
magnetism of Fe3O4
Adsorption capacity of Pb2+, Cu2+and
Cr6+ metal ions using chitosan/GO
Reusability studies indicated chitosan/GO
Cu Equilibrium time of 30 nanofibers was found to be 461.3, Hadi-
nanofibers could be reused frequently
Chitosan-GO Pb min and temperature of 423.8 and 310.4 mg/g Najafabadi et
without any significant loss in adsorption
Cr 45 °C Redlich–Peterson isotherm models al., 2015
performance
Double-exponential kinetic
Endothermic and spontaneous reaction
Adsorption capacity of M-GO and
MrGO for As(III) and As(V) were 85
As (III) adsorption at Electrostatic interaction between the
mg/g (M-GO for As(III)), 38 mg/g (M-
Magnetite–graphene pH 7 positively charged surface of Fe3O4–
GO for As(V)), 57 mg/g (M-rGO for
oxide and magnetite- As (III) As (V) adsorption at graphene-based adsorbents and anionic Yoon et al.,
As(III)), and 12 mg/g (MrGO for
reduced graphene As(V) pH 4 As(V) 2016
As(V))
oxide composite temperature = 25 ◦C, -adsorption mechanism of As(III) was
Freundlich isotherm
adsorption time = 12 h strongly affected by a surface complexation,
Pseudo-first order
Surface complexation
The maximum adsorption capacities of
Cu and Pb ions were 710.3, 579.1 and The selectivity of metal sorption using
Equilibrium time of 30
Cu 526.5, 475.5 mg/g chitosan/TiO2 nanofibrous adsorbent was in Razzaz et al.,
Chitosan/TiO2 min
Pb pseudo-first order and Redlich– order of Cu > Pb. 2016
Temperature= 45 °C,
Peterson isotherm models Five cycles of adsoprtion/desorption
endhothermic/spontaneous
Hydrated manganese pH 6.7 High adsorption capacity >50 mg/g
GO offered the preconcentration of Pb for
oxide (HMO) on GO sorbent Freundlich isotherm Wan et al.,
Pb enhanced sequestration through the Donnan
nanocomposite dose = 0.2 g/L Pseudo-second order 2016
membrane effect
(HMO@GO) Temperature = 298 K Intraparticle diffusion
Adsorption capacities of 56.43, 24.43
α-FeOOH decorated Arsenic interact with α-FeOOH@GCA to
and 102.11mg/g1 for As(V)
graphene Maximum As form inner-sphere complexes which could be
As Langmuir isotherm Fu et al., 2017
oxide-carbon adsorption at pH 9.5 interpreted through ligand exchange
Pseudo-second order
nanotubes aerogel mechanism
Endothermic reaction
Adsorbent dose:
0.4 g/L Langmuir, and D-R isotherm model
The lead adsorption was governed by the
graphene oxide-MgO 30 min of equilibrium Spontaneous and endothermic Mohan et al.,
Pb external mass transfer which was followed
nanohybrid time Pseudo-second-order kinetic (2017)
by intraparticle diffusion
temperature: 30 °C, pH Intraparticle diffusion
6.5
Adsorption capacity was found to be
Optimum pH 2
Polyaniline/ZnO 346.18 mg/g -Langmuir Electrostatic adsorption coupled reduction of Ahmad &
Cr optimum temperature
nanocomposite Pseudo-second order adsorption mechanism Hasan, 2017
60 °C
endothermic and spontaneous
GO-blended Maximum rejection of 98% was GO and NMP in obtaining a highly porous
Ravishankar et
Polysulfone (PSf) Lead concentration = achieved membrane that provides improved flux and
Pb al., 2018
ultrafiltration 50 mg/L and pH = 5.5 -high flux of 43.62 L/m2 h, higher enhanced rejection of lead ions
membrane porosity membrane
pH: 9
Maximum adsorption was 168 mg/g Green synthesis of pure mesoporous KCC-1
Adsorbent dose =
Functionalised Langmuir and pseudo-second-order was prepared through the facile
20 mg, contact time = Zarei et al.,
mesoporous KCC-1 Pb models were found to be the best fit hydrothermal-assisted sol-gel process in a
100 min, initial 2019
and chitosan-oleic acid models to predict isotherms and Teflon-lined stainless steel
concentration:
kinetics of adsorption, respectively. autoclave at 393 K
100 mg/L
None of nanocrystal aggregation, poor
Polydopamine/metal
Cd 0.01 % of metal the removal rate was in the range of stability and large MOF loss when a MOF is
organic framework
Ni organic framework 94% to 99.2% for Ni2+, Cd2+, and Pb2+ , applied to membrane separation He et al., 2020
thin film
Pb concentration respectively new application of nanocrystals in heavy
nanocomposite
metals removal
171
Limitations and future perspective conducted and developed on fabrication of

Recently, several nanotechnology products nanocomposite throughout the world. Thus,
have been applied in water purification as the necessary procedure and proper
well as wastewater treatment. There are management are important prior to large-
differences in opinions of several researchers scale nanocomposite for water and
regarding the use of nanomaterial for wastewater treatment. It is very crucial to
wastewater treatments. Although all types of design the devices that curb the
nanoadsorbent exhibited extremely large nanomaterials from leached out and can
specific areas and promising adsorption regenerate after a period time of usage. The
capacity towards heavy metals from previous studies on existence of
wastewater, there are some limitations that nanoadsorbent regarding the adsorption
need to be addressed for improving their mechanism might be utilized and applied in
properties to make them more suitable in real the real wastewater effluent from industries
wastewater applications. Moreover, the related with the heavy metals production.
nanoparticles utilized in the waste The present and latest nanocomposite
management process are expected to have an systems for wastewater treatment can be
adverse effect towards human and living improved further by improving and
things. Exposure to the risk of toxicity might enhancing the effectiveness of the material
be happened in a long-term exploitation due used as well as the applicability of
to leaching out of nanoparticles. Yet the risk nanocomposites towards wide range of
and the response of nanoparticles towards heavy metals and other pollutants species.
human health are still unclear because only Considering all the features stated above, it is
few reports are available on this matter. very promising that nanocomposite
Therefore, assessing the risk of the adsorbent can be opted as one of the leading
nanomaterials in the environment is nanotechnologies for various applications
necessary to understand the mobility, especially for heavy metals removal from
reactivity persistency and toxicity of the wastewater.
nanomaterials. In addition, the cost analysis
on the preparation of nanoadsorbent CONCLUSIONS
materials should be addressed before the Challenges in the global water situation
application in the real wastewater. Therefore, resulting from population growth, climate
the adsorption capacity of each change, rapid urbanization and
nanoadsorbent should be considered along industrialization require an innovative
with the cost aspect because a good water purification technology to overcome
nanoadsorbent not only satisfies the cost water scarcity and meet the demand of
aspect but should also provide a competitive drinking water to people. Recent
adsorption capacity. Besides that, one of the engineering knowledge has led to the
crucial factors to develop a cost-effective recognition of nanotechnology application
nanoadsorbents is reusability of the to sustain and preserve the environment.
nanoadsorbent where good regeneration To date, this work presented a brief review
properties of nanoadsorbents still give a high of a wide range of nanoadsorbents had
efficiency of heavy metals removal after been successfully utilized for heavy metals
recycles for many times. adsorption from wastewater with
Further work needs to be done to clarify excellence and high removal. However, the
whether nanocomposite adsorbents have reports on the nanoadsorbents utilization
more advantages compared to single use of on the real wastewater are insufficient and
polymer, carbon-based and metal based highly in need of further investigations on
nanoadsorbent. Numerous studies have been pilot and industrial-scale studies. Thus,
172
much more investigation is required to Disinfection. J. Water Process. Eng., 33, 101044, 1-
show that, the optimization of 12.
nanoadsorbents considering the removal Alam, J., Shukla, A. K., Alhoshan, M.,
capability, reusability, their synthesis, cost Arockiasamy Dass, L., Muthumareeswaran, M. R.,
Khan, A. and Ahmed Ali, F. A. (2018). Graphene
and appropriate strategies are required to
oxide, an effective nanoadditive for a development
improve the efficiency and practicability of of hollow fiber nanocomposite membrane with
the nanoadsorbents in real wastewater antifouling properties. Adv. Polym. Technol., 2017,
treatment. 1–12.
Ali, M. E., Hoque, M. E., Safdar Hossain, S. K. and
ACKNOWLEDGEMENT Biswas, M. C. (2020). Nanoadsorbents for
The authors express their gratitude to wastewater treatment: next generation
Ministry of Education (MOE) Malaysia for biotechnological solution. In Int. J. Environ. Sci.
granting a Fundamental Research Grant Technol. (Issue 0123456789). Springer Berlin
Heidelberg.
Scheme (FRGS), project no. FRGS-19-
194-0803, and to International Islamic Alimohammadi, M., Saeedi, Z., Akbarpour, B.,
University Malaysia for the financial Rasoulzadeh, H., Yetilmezsoy, K., Al-Ghouti, M.
A., Khraisheh, M. and McKay, G. (2017).
support. Adsorptive Removal of Arsenic and Mercury from
Aqueous Solutions by Eucalyptus Leaves. Water
CONFLICT OF INTEREST Air Soil Pollut., 228(11), 1-27.
The authors declare that there is no conflict
Auwal, A. and Hossen, J. (2018). Removal of
of interests, regarding the publication of Phenol From Aqueous Solution Using Tamarind
this manuscript. The authors declare that Seed Powder As Adsorbent. IOSR J. Environ. Sci.
there is not any conflict of interests Toxic. Food Technol. vf 12(3), 41–48.
regarding the publication of this Ayawei, N., Ebelegi, A. N. and Wankasi, D. (2017).
manuscript. In addition, the ethical issues, Modelling and Interpretation of Adsorption
including plagiarism, informed consent, Isotherms. J. Chem., 2017(3039817), 1-11.
misconduct, data fabrication and/ or Azizi, S., Shahri, M. M. and Mohamad, R. (2017).
falsification, double publication and/or Green synthesis of zinc oxide nanoparticles for
submission, and redundancy have been enhanced adsorption of lead Ions from aqueous
completely observed by the authors. solutions: Equilibrium, kinetic and thermodynamic
studies. Molecules., 22(6), 1-14.
LIFE SCIENCE REPORTING Azizian, S., Eris, S. and Wilson, L. D. (2018). Re-
No life science threat was practiced in this evaluation of the century-old Langmuir isotherm for
research. modeling adsorption phenomena in solution. Chem.
Phys., 513, 99–104.
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Pollution, 7(1): 153-179, Winter 2021 Review Paper

The role of nanoadsorbents and nanocomposite adsorbents in the

Department of Biotechnology Engineering, Faculty of Engineering, International

Received: 27.07.2020 Revised: 19.10.2020 Accepted: 21.11.2020

ABSTRACT: Significant attention has been given to nanotechnology as an emerging

INTRODUCTION industrial usage. Production of wastewater

pollutants from wastewater especially copper, cadmium, chromium, silver and

process by which a substance (adsorbate) is adsorbents for wastewater treatment and

recommendations for future researches and will form monolayer or multilayer

Fig. 1. Various adsorption mechanisms of metal ion adsorbate on nanoadsorbent

The mechanism of heavy metals can adsorb at equilibrium conditions and

adsorbate concentration can be calculated added to bottle (L), and M is mass of

Table 2. Isotherm Models

Meanwhile, the Freundlich isotherm obtained from y-intercept of the plotted

The Redlich-Peterson model denotes Ce

Adsorption kinetics mechanism and rate controlling steps

dt qe: Equilibrium adsorption capacity (mg/g)

Thermodynamics Synthesis of nanoadsorbent

Type of nanoadsorbent in wastewater extensively in removal of heavy metals

sorption capacity increased when the value characteristics in terms of mechanical,

The study of Mohan et al. (2017) double-exponential kinetics and Redlich–

Table 5. Comparative table on carbon-based nanoadsorbents on optimum parameters and removal

Cu 60 min 294 mg/g

Briefly, carbon-based nanoadsorbents properties of GO and GO–COOH were

Copper oxide cost and extraordinary removal capacity

were successfully synthesized and removed Nizamuddin et al.; 2019). Therefore,

Polymer based nanoadsorbent potential to remove various kinds of heavy

Fig. 8. Structure of dendrimers (Vunain et al., 2016)

Mainly, the functional groups on Nanocomposite adsorbents

Limitations and future perspective conducted and developed on fabrication of

poly (styrene-alt-maleic anhydride) networks as a Treatment. Int. J. Chem. Eng., 2019(9872502), 1-

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