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Nanotechnology based water quality management for wastewater treatment

Article  in  Environmental Chemistry Letters · July 2018

DOI: 10.1007/s10311-018-0778-8

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Environmental Chemistry Letters
https://doi.org/10.1007/s10311-018-0778-8

REVIEW

Nanotechnology‑based water quality management for wastewater

treatment
Lavanya Madhura1 · Shalini Singh1 · Suvardhan Kanchi2 · Myalowenkosi Sabela2 · Krishna Bisetty2 · Inamuddin3,4,5 

Received: 3 July 2018 / Accepted: 5 July 2018

© Springer Nature Switzerland AG 2018

Abstract
Water contamination by pollutants has become one of the most critical health problem worldwide. In the current era, the
supply of high-quality drinking water to the society with cheaper technology is a key requirement for growing the economy.
The foremost challenge is to develop innovative wastewater treatment technologies with low production cost and enhanced
efficiency. Concomitantly, the role of nanotechnology in pollution remediation, drinking, and wastewater treatment has proven
to be promising according to numerous pilot-scale, laboratory, and in situ studies. Remarkable nanoscale features, namely
excellent adsorption properties, enhanced photocatalysis, and high reactivity, have fostered dynamic innovation globally.
This review focuses on the state-of-art of treatment techniques with nano-based materials, for example graphene and carbon
nanotubes, metal nanoparticles such as silver, iron, zinc and magnesium, and metal oxide nanoparticles and magnetic-core
composites including cobalt, nickel, and iron. Furthermore, we compare emerging and conventional technologies in terms
of production cost and performance for both organic and inorganic pollutants. In addition, challenges and future aspects of
engineered nanomaterials to environmental applications in wastewater treatment are also outlined.

Keywords  Nanotechnology · Carbon-based nanomaterials · Nanoadsorbents · Metal/metal oxide engineered

nanomaterials · Nanoparticles · Water and wastewater treatment

Introduction global challenge. Currently, the supply of potable water

Water remains the most precious resource essential to sus-
tain all life on earth. However, in the twenty-first century,
access to reliable and affordable clean water remains a key
* Shalini Singh
shalinis@dut.ac.za
* Inamuddin
inamuddin@rediffmail.com
1
Department of Operations and Quality Management, Durban
University of Technology, Durban 4000, South Africa
2
Department of Chemistry, Durban University of Technology,
Durban 4000, South Africa
3
Chemistry Department, Faculty of Science, King Abdulaziz
University, Jeddah 21589, Saudi Arabia
4
Centre of Excellence for Advanced Materials Research, King
Abdulaziz University, Jeddah 21589, Saudi Arabia
5
Advanced Functional Materials Laboratory, Department
of Applied Chemistry, Faculty of Engineering
and Technology, Aligarh Muslim University,
Aligarh 202 002, India
is under stress due to the lack of availability of freshwa-
ter and poor sanitation services. According to the World
Health Organization, nearly 780 million people still lack
access to clean and sustainable drinking water worldwide
(World Health Organization 2012). This is prevalent mainly
in developing countries, where the wastewater infrastructure
is not well established. Therefore, it is prudent to implement
basic water treatment technologies in the affected areas. In
both industrialized and developing countries, water short-
ages are intensified by pollution mainly due to the human
activities. The increasing number of contaminants in waste-
water has led to a new scrutiny of the emerging water treat-
ment and distribution systems with the emergence of strin-
gent quality standards, particularly in developed countries.
The fast-rising world’s population and the improved living
standard increase the demand for clean water. Moreover, it
is important to introduce new norms in the use of water due
to the increasing pressure on water supplies, irregular supply
of freshwater, and global climate change. All these pres-
sures on water systems drive the need for the use or reuse
of alternative water sources such as seawater, stormwater,

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Vol.:(0123456789)

brackish water, and recycled domestic water in historically
water-stressed areas. Currently, wastewater treatment tech-
nologies and infrastructures are providing low, but adequate
water quality to meet societal needs (World Health Organi-
zation 2012).
Recent innovations in nanotechnology offer a handful
of opportunities to establish cost-effective and sustainable
water supply systems. The multi-functional ability of nano-
material is predicted to provide affordable, high-perfor-
mance water and wastewater treatment solutions that depend
less on large infrastructure wastewater systems (Qu et al.
2013a, b, c). Nanotechnology-related water and wastewater
treatments are found to be promising initiatives, not only to
overcome the main challenges in water treatment, but also to
provide novel treatment abilities that could allow economic
exploitation of alternate water sources to increase the water
supply.
Scarcity of water
The scarcity of water remains to be one of the key threats
to human existence in various areas worldwide. Literature
suggests that parts of the African continent, the state of Cali-
fornia in the USA, the Mediterranean Basin, and semiarid
regions (Bunani et al. 2015; Jhansi and Mishra 2013) are
facing severe drought conditions, with water shortages that
emerged from overuse and extensive extraction of ground-
water (Qadir et al. 2010; Roson and Sartori 2015). Recently,
due to growing environmental awareness in water supplies,
inexpensive methods have been developed for the reuse
and treatment of non-conventional water sources from grey
and wastewater systems (Birks and Hills 2007; Salgot et al.
2006). Even though the desalination of seawater and runoff
waters is real option to address the shortage of water, it is
noted that the reuse of treated domestic wastewater is an
alternate solution to a stable water source. The disposal of
treated domestic wastewater into the environment may not
be harmful; however, it is prudent to monitor the potential
environmental risks associated with wastewater pollution
to resolve water shortage challenges. An aim of emerging
technologies is to uphold sustainable food production with
low-quality wastewaters. It has been mooted that these low-
quality wastewaters have the capability of increasing agri-
cultural yields which can remain consistent and stable for
approximately 25 years. Though treated domestic wastewa-
ter is of a great advantage for agriculture because of its high
nutrient content (Jhansi and Mishra 2013; Rusan et al. 2007;
Velho et al. 2012), these nutrients can lead to a eutrophi-
cation process resulting in the accumulation of nitrogen
species in the groundwater (Chislock et al. 2013; She et al.
2016; Xie et al. 2015). According to Turton (2016) stud-
ies, scarcity of water in South Africa was divided into four
stages based on the years. In 1990, population growth and
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Environmental Chemistry Letters
environmental factors such as severe drought and climate
change were related to water scarcity. On the other hand,
water scarcity could become more serious by 2020, 2050,
and 2070 (Turton 2016). In 2070, the most economically
active portion of South Africa could resemble the Middle
East and North Africa.
Occurrence of pathogens in wastewaters
Several reports investigated water quality and disinfection
aspects of treated domestic wastewater applications. Since
the soil acts as a multilayer filter, surface drip irrigation
is regarded as one of the best options to reduce pathogen
content from surface waters (Ayars et al. 2015; Forslund
et al. 2012). Another possibility of reducing pathogens in
the applied conventional effluent is to detain it in a series
of stabilization reservoirs; this process will increase the
salt concentration (Liran et al. 1994; Walker and Lin 2008).
Efforts have been put forward to reduce pathogen content in
groundwater; however, this activity has made the water qual-
ity worse (Herrero and Pérez-Coveta 2005; Mounzer et al.
2013). In some arid regions, precipitation is the only process
that facilitates soil leaching, compared to the rainy regions.
This result in a reduction in crop yield and in low food pro-
duction due to the accumulation of salts and micropollutants
in the soil (Mounzer et al. 2013; Ternes et al. 2007).
The Silicon Valley Clean Water, a company located in
San Francisco Bay, has designed an effective way of treat-
ing wastewaters to remove 97% of organic materials, solids
wastes, and pathogens (Silicon Valley Clean Water 2017).
It was found that 200,000 people are benefitting from envi-
ronmentally clean and safe water from this treatment plant.
Recently, silica monoliths integrated with composites and
biocomposites have been designed for strategical removal
of organic pollutants from wastewater plants. The schematic
illustration of wastewater treatment plants is represented in
Fig. 1 (Rodrigues et al. 2013).
Nanotechnology for water quality
The quality of the effluent can be improved dramatically by
using a nanotechnological system. These systems include
basic separation processes such as reverse osmosis, micro-
filtration, and nanofiltration to treat effluents more effec-
tively. It is also found that the use of these systems allowed
organizations to generate a sustainable water quality, thus
improving their environmental and economic development
(Drews 2010; Qu et al. 2013c; Smith 2006; Wu et al. 2011).
Among all three processes, reverse osmosis is one of the
effective systems used to remove all micropollutants from
wastewaters (Xue et al. 2010). However, the main draw-
back of this process is in the disposal of the resulting brine
solution into the environment in which wastewater would
Environmental Chemistry Letters
Fig. 1  Strategies for removal of pollutants from wastewater effluents
or prepared solutions, based on silica monoliths: 1.a porous com-
posites (mesopores and or hierarchically macro-/mesopores) able to
promote adsorption of chemical compounds; 1.b titania-loaded com-
posites able to promote adsorption and photodegradation of chemi-
cal compounds; 2.a biocomposites with immobilized organism or
unavoidably combine with domestic waters. Therefore, most
of the reverse osmosis systems are located near the seashore
to enable the disposal of brine solution into the ocean (Garg
and Joshi 2015; Shenvi et al. 2015; Xue et al. 2010; Yuan
and He 2015).
Imminent issues associated with nanotechnology
for water treatment
The fundamental challenges identified for the successful
execution of nanofiltration processes are as follows:
(a) the fouling of the membrane (Drews 2010; She et al.
2016);
biomolecules in beads within silica monolith; 2.b immobilized organ-
ism or biomolecules directly within silica monolith; both biocompos-
ites are to promote adsorption and diffusion of target chemical com-
pounds as well as biodegradation followed by diffusion of degraded
compounds (reproduced with permission of Rodrigues et  al. 2013).
Copyright 2013 Elsevier
(b) more energy is required (Guest et al. 2009; Huang and
Keller 2015), and
(c) the safe and environmentally friendly disposal of brine
solution (Pérez-González et al. 2012).
Nanotechnology‑based water treatment
and reuse processes
The treatment and reuse of domestic water can be performed
with nanotechnology. This technology creates opportunities
to remove concerns related to water quality deterioration
within distribution networks. It also reduces dependency
on major infrastructure and utilizes other water sources
(e.g. recycled new water) for agricultural and portable
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 Environmental Chemistry Letters

applications with subsidized energy consumption. This fore-
sight may be predominantly suitable for developing coun-
tries where there are concerns about the rapid deterioration
of water quality and growing pressure for cleaner water to
meet food safety, public health, and stricter environmental
standards. This situation emphasizes the necessity for inno-
vative and high-performance water treatment technologies.
In developing countries, urban areas are focusing on the
use of nanotechnology treatment systems that target a wide
range of pollutants which are inexpensive and easy to oper-
ate. A sustainable urban water management is an ultimate
goal, which can be achieved by adopting ideal treatment
systems with engineered nanomaterials as shown in Table 1.
The reuse of wastewater with nanotechnology is still far
away from being on industrial-scale applications. However,
researchers have succeeded in laboratory scale testing with
promising outputs resulting in the establishment of pilot-
scale plants (He et al. 2010; Radjenović et al. 2009). Silver
nanoparticles have been used as water filters in domestic
wastewater treatment (Oyanedel-Craver and Smith 2007).
The current nanotechnology-related water treatment research
focuses on four areas: (a) filtration through membranes; (b)
adsorptive elimination of micropollutants; (c) microbial
decontamination; and (d) catalytic degradation (Li et al.
2008a, b).
The oxidative or reductive degradation of pollut-
ants related to agriculture and pharmaceuticals has been
performed using nanomaterials with catalytic and photo-
catalytic properties. Functionalized titanium dioxide- and
fullerenes-based nanocomposites are used as a photo-
catalyst for deactivation and disinfection of bacteria and
viruses effectively in the presence of visible and ultraviolet
light (Dunlop et al. 2002). This method signifies a sub-
stantial enhancement over existing chemical disinfection
methods that produce harmful disinfection by-products.
However, these by-products are not effective to disinfect-
ant-resistant pathogens (e.g. Giardia and Cryptosporid-
ium). This method can also be used to treat pollutants such
as pharmaceuticals, endocrine disruptors, pesticides, and
residual antibiotics from wastewaters (Lee et al. 2009).
The effective dechlorination of organic solvents like
trichloroethylene was performed using palladium modi-
fied gold nanoparticles. In this study, the nanocomposite
acts as a superior catalyst for the treatment of wastewater
(Nutt et al. 2005; Wong et al. 2009). The nano-zerovalent
iron nanoparticles are used as an important reductant to
enhance dechlorination resulting in effective groundwater
remediation.

Table 1  Prospects for engineered nanomaterials in wastewater treatment and reuse

Required engineered nanomaterials properties Engineered nanomaterials-aided technologies Citation

Specific and greater surface area Higher sorbents with great irreversible Mayo et al. (2007)
adsorption ability (useful in the removal of
arsenic and other toxic heavy metals by using
magnetite nanoparticles) and reactants and
reactants
Improved catalytic properties Titanium dioxide- and fullerene-based photo- Hoffmann et al. (1995) and Nutt et al. (2005)
catalysts were used as hyper-catalysts, and
hybrid of palladium/gold was also used in the
reduction process of wastewater treatment for
pesticide residues
Antimicrobial properties Titanium dioxide and fullerenes derivatives Lee et al. (2009) and Yang et al. (2009)
were used as disinfectants without toxic by-
products
Characteristics properties (antibiotic, catalytic, Self-cleaning ability, nanofiltration membranes Zodrow et al. (2009)
etc.) that have unique features in deactivating virus
and terminating organic pollutants
Self-assembly on surfaces This feature will reduce bacterial contact with Nel et al. (2009)
electrode surface, the formation of biofilms,
and corrosion in water storage systems
High conductivity New electrodes for electrosorption (fast deioni- Oren (2008)
zation) and cost-effective, energy-efficient
desalination process
Fluorescence Rapid detection of pathogens and other pollut- Bogue (2009)
ants using sensor technology

13
Environmental Chemistry Letters
Nanomaterials as adsorbents for water
treatment
Nano-adsorbents are particles in the nanoscale range that
have a great attraction to adsorb organic or inorganic
substances from aqueous solutions (Baruah et al. 2016;
Madhura et al. 2018). Due to their small size, high poros-
ity, and an active surface, nano-adsorbents are capable
of adsorbing contaminants with varying molecular size
and speciation behaviour. In the manufacturing process of
nano-adsorbents, raw materials are used efficiently without
the release of harmful by-products (Pacheco et al. 2006).
Nano-adsorbents have a strong binding capacity for pol-
lutants, resulting in the effective removal from wastewaters
(Yang and Xing 2007). These adsorbents are attracting
the attention of researchers due to their unique proper-
ties such as small size, surface area to volume ratio, large
surface area, high reactivity, and catalytic potential at
the nanoscale when compared to conventional materials
(Hristovski et al. 2007). The large surface area of nano-
adsorbent creates more active adsorbing sites, resulting
in the effective interaction of different chemical species
from wastewaters (Khaleel et al. 1999; Li et al. 2006a, b).
Magnetic nano-adsorbents can be effortlessly retained and
separated from the water after the treatment process due
to the high specific surface area of magnetic nanoparti-
cles. Therefore, these nanomaterials are commonly used to
remove radionuclides and heavy metals from wastewaters.
The super-paramagnetic properties of nanomagnetite allow
separation under low magnetic fields to enable recycling
and reuse of magnetite nanomaterials (Mayo et al. 2007).
Sand filter treatment for the removal of heavy metals was
first performed on pilot scale by the Rice University in
Mexico and was ranked as top five nanotechnology break-
throughs in 2006 (ForbesMediaLLC. 2006).
Carbon‑based materials
In an adsorption process, the main characteristic features
of adsorbents are a large surface area, pore volume, and
good functionalities for the adsorbate. Several porous
materials such as activated carbon, polymers, mesoporous
oxides, pillared clays, and metal–organic frameworks are
currently available to remove toxic pollutants from waste-
waters and soils (Adeyemo et al. 2012; Gupta and Bhat-
tacharyya 2012; Kim and Yi 2004; Ngah et al. 2011; Wang
and Peng 2010). Among them, carbon-based adsorbents
including carbon nanotubes, activated carbon, graphene,
and fullerenes generally show high thermal stability
and excellent adsorption capacity (Rao et al. 2007; Ren
et al. 2011; Seymour et al. 2012; Wang et al. 2012a, b,
c). For the removal of organic and inorganic pollutants,
various carbon-based nanomaterials have been explored
as superior adsorbents. Fullerenes and carbon nanotubes
are adopted as effective adsorbents due to their extensive
applications. However, the design of low-cost methods for
effective adsorbents is a great challenge. The hybrid of
magnetic nanomaterials and multi-walled carbon nano-
tubes showed substantial removal efficiency of inorganic
metal ions (Yang et al. 2006).
Carbon nanotubes
A carbon nanotube is an allotrope of carbon. Carbon nano-
tubes are mostly composed of cylindrical shapes rolled up
in a tube-like structure. There are two types of carbon nano-
tubes, namely single-walled carbon nanotubes and multi-
walled carbon nanotubes (Wang et al. 2014a, b, c, d). Carbon
nanotubes composed of a single, rolled-up graphene sheet
are known as single-walled carbon nanotubes while multiple
graphene rolled-up sheets are known as multi-walled carbon
nanotubes as shown in Fig. 2 (Das et al. 2014).
Compared to conventional granular and powdered acti-
vated carbon, carbon nanotubes consist of controlled pore
size distribution and high surface active site to volume
ratio, which results in exceptional sorption efficiency. The
adsorption capacity of carbon nanotubes depends on both
the nature of the sorbate and surface functional groups. For
example, the adsorption of polar compounds onto the sur-
face of carbon nanotubes functionalized with acidic groups
like carboxylic, lactonic, and phenolic groups (Wang et al.
2008a, b). On the other hand, a higher adsorption capac-
ity was observed by non-functionalized carbon nanotubes
towards nonpolar compounds such as polycyclic aromatic
hydrocarbons (Stafiej and Pyrzynska 2008). In carbon
nanotubes, sorption behaviours are mainly due to physical
interaction of nonpolar and chemical interaction of polar
compounds, which are shown in Table 2.
The sorption capacity of carbon nanotubes is effective
mainly over a wide pH, ranging from 7.0 to 10.0. It was
reported that, except in this pH range, ionic species could
occur in the reaction systems, resulting in the lowering of
adsorption capacities. When compared to conventional acti-
vated carbon, carbon nanotubes are more expensive, where
their sorption and desorption cycles are effective in terms
of extraction efficiency.
By using purified carbon nanotubes (single- and multi-
walled carbon nanotubes), the removal of zinc(II) was dis-
cussed by Lu and Chiu (2006). The other study by Lu et al.
(2005) suggests that purified carbon nanotubes are more
effective in the removal of metal residual catalysts than the
amorphous carbon. Large amounts of nanotube bundles with
hollow inner tube diameters were observed with purified
carbon nanotubes. Due to the presence of negative functional
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 Environmental Chemistry Letters

Fig. 2  Structures of a multi-
walled and b single-walled
carbon nanotubes (Reproduced
with permission of Das et al.
2014). Copyright 2014 Elsevier

Table 2  Heavy metal ions Metal ions Nano-adsorbents Adsorption efficiency Citation

adsorption onto various types of
carbon nanotubes Pb(II) CNTs(HNO3) 49.95 mg g−1 at pH:7.0 Li et al. (2002)
CNTs 1.406 mmol g−1 Anitha et al. (2015)
CNT-OH 2.07 mmol g−1 Anitha et al. (2015)
CNT-CONH2 1.907 mmol g−1 Li et al. (2003b)
CNT-COO− 4.672 mmol g−1
MWCNTs ­(HNO3) 97.08 mg g−1 at pH:5.0
Cd(II) CNTs-COO− 3.325 mmol g−1 Anitha et al. (2015)
CNT-OH 1.513 mmol g−1
CNT-CONH2 1.563 mmol g−1
CNTs 1.291 mmol g−1
Ni(II) MWCNTs 7.53 mg g−1 at pH:7.0 Lu and Liu (2006)
SWCNTs 9.22 mg g−1 at pH:7.0
Cu(II) CNTs 1.219 mmol g−1 Anitha et al. (2015)
CNT-OH 1.342 mmol g−1
CNT-CONH2 1.755 mmol g−1
CNT-COO- 3.565 mmol g−1

groups on the surface of purified carbon nanotubes, the zeta
potentials of purified carbon nanotubes were more nega-
tive than those of un-purified carbon tubes. Hence, it can be
noted that in the pH range of 2.0–12.0, the adsorption of zinc
(II) was found to be maximum. At a lower pH, due to the
competition for adsorption sites between hydrogen and zinc
(II), the adsorption capacity of zinc (II) was lowered. How-
ever, up to pH 8.0, the adsorption of zinc (II) was increased
and beyond pH 8.0, the adsorption remains unchanged.
Therefore, the optimum pH 8.0 was selected for the maxi-
mum adsorption and removal of zinc (II) species. The Lang-
muir model was developed to determine the adsorption
capacity of zinc (II) using single- and multi-walled carbon
nanotubes. It was found that at the initial concentration range
of 10–80 mg L−1, the maximum adsorption of 43.66 and
32.68 mg g−1 of zinc (II) within 60 min was reported.
Gupta et al. (2011) studied the removal of chromium
(III) by using multi-walled carbon nanotubes decorated
with iron oxide nanoparticles. The carbonyl and hydroxyl
group’s functionalization of multi-walled carbon nanotubes
was performed by acid treatment with nitric acid. The avail-
ability of additional adsorption sites created by the oxygen
atoms of iron oxide nanoparticles on the surface of multi-
walled carbon nanotubes established an electrostatic force of

13
Environmental Chemistry Letters
attraction, resulting in the enhanced adsorption capacity of
chromium (III). In the pH range of 3.0–7.0, nanocomposite
was found to be effective for the removal of chromium (III)
due to the formation of Cr(OH)2+ at pH 4.0. However, in the
pH range of 4.0–7.0, maximum adsorption of chromium (III)
from multi-walled carbon nanotube was evident due to the
formation of net negative surface charge on the Cr(OH)2+.
The fixed bed experimental results suggested that the low
flow-rate of the sample solution resulted in the increased
adsorption of chromium (III) due to the increased contact
time between the adsorbent and the analyte. Interestingly, it
was found that the uptake of chromium (III) also increased
with fixed bed thickness, due to the availability of additional
adsorption sites on multi-walled carbon nanotubes. Many
researchers have also designed functionalization of carbon
nanotubes to test the adsorption ability and removal effi-
ciency of toxic substances, compared to non-functionalized
carbon nanotubes (Rao et al. 2007; Ren et al. 2011).
The adsorption performance of Procion Red MX-5B dye
from various industrial effluents, with multi-walled carbon
nanotubes, was evaluated by Wu et al. (2007). At pH 6.5,
kinetic analysis was performed at various temperatures.
It was found that the maximum adsorption (20.93, 22.87,
27.20, and 30.53 mg g−1) was attained within 3 h at differ-
ent temperatures 281, 291, 301, and 321 K, respectively.
The results obtained revealed that temperature played a sig-
nificant role in the adsorption of Procion Red MX-5B onto
the multi-walled carbon nanotubes. The adsorption process
increased with temperature, demonstrating that the move-
ment of dye molecules increased with temperature and con-
firmed that the adsorption process was endothermic. The
Langmuir and Freundlich isotherms were studied based on
the standard deviation and linear correlation coefficients
results. It was suggested that the Langmuir isotherm fitted
well with the experimental results. The kinetic models were
also performed and confirmed that the pseudo-second-order
model was accurate with the adsorption process of Procion
Red MX-5B dye.
Multi-walled carbon nanotubes impregnated with chi-
tosan hydrogel beads were used to study the adsorption effi-
ciency and removal of Congo red from aqueous solutions
(Chatterjee et al. 2010). The impregnation of chitosan hydro-
gel beads onto the multi-walled carbon nanotubes resulted
in the high porosity and thickness of the material. At pH
4.0, the adsorption of Congo red onto the chitosan hydro-
gel beads/multi-walled carbon nanotubes was maximum
(423.1 mg g−1), indicating that the adsorption process is pH
dependent. It was noted that amine groups of chitosan do not
undergo protonation. The formation of beads was performed
in a sodium hydroxide precipitation bath. The decrease in
­H+ concentration was observed with increase in initial pH
from 4.0 to 6.0. Such behaviour was not detected for Congo
red solution at neutral or basic pH, as amine groups did
not undergo protonation at pH 7.0 or 9.0 due to the non-
occurrence of H ­ + ions. The isotherm results revealed that
the Langmuir model better fitted to the experimental data
compared to the Freundlich isotherm model. The adsorption
kinetics were conducted, and it was found that the pseudo-
second-order was accurate and that the intra-particle dif-
fusion model suggested the mass transfer rate gradually
increased by the accumulation of multi-walled carbon nano-
tubes. The maximum adsorption efficiency of multi-walled
carbon nanotubes impregnated with chitosan hydrogen beads
was found to be 450.4 mg g−1.
The single-walled carbon nanotubes were used for
the removal of Reactive Red 120 textile dye from textile
wastewaters as a function of pH change. The optimum pH
was found to be 5.0, below and above this pH, while the
adsorption capacity decreased. At an initial concentration
of 50 mg L−1 and pH 5.0, the single-walled carbon nano-
tubes have an adsorption capacity of 426.49 mg g−1 with a
removal percentage of 85.3%. It was found that the adsorp-
tion capacity of dye increased with an increase in adsorbent
dosage up to 882.83 mg g−1 with an equilibrium contact time
of 180 min (Bazrafshan et al. 2013).
Multi-walled carbon nanotubes treated with acids were
used to monitor the adsorption capacity of resorcinol. In
this study, resorcinol was used as a model phenol and it was
found that adsorption kinetics was fast (Liao et al. 2008). It
was noted that the experiments were performed at pH below
8.0, as resorcinol undergoes oxidation in basic medium. The
uptake of resorcinol increased with a decrease in pH, due
to a decrease in its solubility with the decrease in pH. Fur-
thermore, the decrease in the uptake efficiency of resorcinol
was due to the electrostatic repulsion between the multi-
walled carbon nanotubes treated with acid and the nega-
tively charged resorcinol. Interestingly, it was found that the
carboxylic groups on the multi-walled carbon nanotubes act
as electron-withdrawing groups, localizing electrons from
the π-system of multi-walled carbon nanotubes, resulting
in the weakening of bonds between graphite structure of
multi-walled carbon nanotubes and the aromatic ring of res-
orcinol. The hydroxyl group on meta-position of resorcinol
also influenced the adsorption capacity of the multi-walled
carbon nanotubes (Chen et al. 2011a, b).
Promising results have been achieved in the removal of
natural organic matter from aqueous solutions using multi-
walled carbon nanotubes. Due to the hydrophobicity of
multi-walled carbon nanotubes, natural organic matter can
be easily removed from the aqueous systems (Hyung and
Kim 2008). In pH range of 3.0–9.0, the natural organic mat-
ter is ionic in nature and results in the enhanced adsorp-
tion capacity (2.5–50 mg C ­L−1) of multi-walled carbon
nanotubes for some natural surface- and groundwaters.
In this report, Langmuir and Freundlich isothermal stud-
ies were performed and compared with the adsorption of
13

multi-walled carbon nanotubes. It found that the adsorption
layers of natural organic matter on the surface of multi-
walled carbon nanotubes were formed due to the stable sus-
pension in aqueous solution.
In other reports, coagulation and adsorption processes
were combined for the removal of natural organic matter
from a variety of water samples using multi-walled carbon
nanotubes (Joseph et al. 2012). In the presence of ferric chlo-
ride and alum metal coagulants, single- and multi-walled
carbon nanotubes were used for the removal of natural
organic matter with coagulation process. Different samples
such as brackish water (humic acid), synthetic seawater, syn-
thetic landfill leachates (glucose), and natural river water
were selected to attain a thorough knowledge on the natu-
ral organic matter and its behaviour towards adsorption and
coagulation process. The humic acid present in one of the
natural samples has 40% dissolved organic carbon. It was
found that the Freundlich adsorption isotherm fitted well
into the experimental data. Interestingly, single-walled car-
bon nanotubes (407 m2 ­g−1) showed a greater efficiency of
adsorption compared to the multi-walled carbon nanotubes
(60 m2 ­g−1) due to the higher surface area of the former.
Equivalent quantities of trihalomethanes such as chloro-
form, dichlorobromomethane, dibromochloromethane, and
bromoform were investigated from different water samples
(Lu et al. 2006). The multi-walled carbon nanotubes used in
this study were purified with nitric acid/sulphuric acid and
used as an adsorbent. The kinetic studies performed in this
study were a diffusion-controlled mechanism. It was found
that the adsorption of chloroform onto the multi-walled car-
bon nanotubes was rapid over other dichlorobromomethane,
dibromochloromethane, and bromoform due to smaller size
and could easily penetrate into the inner cavities through
the pores. Additionally, the temperature effect on adsorp-
tion was studied and it was found that the increase in tem-
perature from 5–35 °C decreases the adsorption efficiency.
At 5 °C, the maximum adsorption capacity of chloroform,
dichlorobromomethane, dibromochloromethane, and bromo-
form was found to be 3.158, 2.016, 2.008, and 1.976 mg g−1,
respectively.
Morawski et al. (2000) studied the adsorption of chloro-
form onto the carbon nano-spheres and found that adsorption
capacity of 40% was observed from a standard solution .
In addition, several reports are available on the removal of
aquatic pollutants using carbon nanotubes (Chen et al. 2007;
Lu et al. 2008; Pan and Xing 2008). From the foregoing sec-
tion, carbon nanotubes have proved to be a potential adsor-
bent for the removal of dyes, toxic metals, natural organic
matter, and trihalomethanes from aqueous solution. Their
practical use is restricted due to the cost factor. Thus far, the
toxicity of functionalized carbon nanotubes is not reported in
the literature; however, some degree of toxicity is observed
with raw carbon nanotubes (Chen and Wang 2006).
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Environmental Chemistry Letters
In addition to the removal of toxic metals, carbon nano-
tubes are also used to treat wastewaters for organic pollut-
ants. For example, organic dyes are highly toxic at the lower
concentration levels in water because of their potential car-
cinogenic effect on the aquatic system. For treating organic
pollutants, a wide range of adsorbents such as clays, zeolite,
polymers, and activated carbons were used for an effective
adsorption process. Among all the adsorbents used, carbon
nanotubes are found to be the most promising material to
treat leather, food processing, dyeing, paper, and industrial
effluents due to their unique surface properties (Yang et al.
2008a, b; Yao et al. 2011).
Researchers have investigated the capability of various
carbon nanotubes to remove a wide range of organic pol-
lutants from wastewaters. Their findings are summarized
in Table  3. Even though carbon nanotubes have many
important advantages, their usage is limited to the indus-
trial applications due to cost implications (De Volder et al.
2013). Small quantities of carbon nanotubes are required for
point-of-use applications because of competitiveness. For
example, many carbon nanotubes are used in pharmaceutical
industries to remove highly degradable contaminates (Cong
et al. 2013; Ji et al. 2009; Qu et al. 2013a, b, c). Hence, more
research is necessary to develop reliable and cost-effective
procedures for water treatment using carbon nanotubes.
Graphene‑based materials
Graphene, an allotrope of carbon, has recently been used by
several researchers in developing a cost-effective method of
synthesis of graphene oxide. Since the twentieth century, the
use of graphene and graphene-based materials has increased
drastically due to their unique properties, which have moti-
vated the development of novel and performance-enhanced
environmental applications (Hebbar et al. 2017; Jilani et al.
2018). Further, the development of graphene-based tech-
nologies is important due to their environmental implica-
tions and cost considerations. Moreover, graphene is an ideal
material and substitute for carbon nanotubes in water treat-
ment. When compared to carbon nanotubes, graphene-based
materials act as a promising adsorbent for reliable environ-
mental application in terms of production costs.
Single-layered graphene materials offer two basal planes
for the adsorption of pollutants (Rao et al. 2007; Sitko et al.
2013a, b; Stafiej and Pyrzynska 2007). In contrast, the
adsorbates are not accessible in the inner walls of carbon
nanotubes (Sitko et al. 2013a, b). Through chemical exfo-
liation of graphite, reduced graphene oxide (rGO) and gra-
phene oxide (GO) can be easily synthesized without using
complex apparatus or metallic catalysts as shown in Fig. 3
(Amieva et al. 2016; Balaji Mohana et al. 2018). No further
purification steps are needed, and the resulting graphene
material is free from catalyst residues (Sitko et al. 2013a, b).
Environmental Chemistry Letters

Table 3  Removal of organic pollutants using various types of carbon nanotubes (CNT)

Carbon-based nano-adsorbents Organic pollutants Adsorption efficiency (mg g−1) Citation

Untreated CNTs
SWCNTs Oxytetracycline 554 Ncibi and Sillanpää (2015)
Ciprofloxacin 933.8 Ncibi and Sillanpää (2015)
4-Chloro-2-nitrophenol 1.44 Mehrizad et al. (2012)
Dissolved organic matter (DOM) 26.1–20.8 Lou et al. (2011)
Double-walled carbon nanotubes Oxytetracycline 507 Ncibi and Sillanpää (2015)
Ciprofloxacin 901.2 Ncibi and Sillanpää (2015)
MWCNTs Tetracycline 192.7 Álvarez-Torrellas et al. (2016)
Olaquindox 99.7 (%) Zhang et al. (2011)
Ciprofloxacin 391 Ncibi and Sillanpää (2015)
Oxytetracycline 651.4 Ncibi and Sillanpää (2015)
4-Chloro-2-nitrophenol 4.42 Mehrizad et al. (2012)
Methylene blue 59.7 Wang et al. (2012a, b, c)
Treated CNTs
Alkali-activated MWCNTs Methylene blue 399 Ma et al. (2012)
Oxidized SWCNTS Basic red 46 (BR 46) 49.45 Moradi (2013)
MWCNTs activated with KOH Toluene, ethylbenzene, m-xylene 87.12, 322.05, 247.83 Yu et al. (2012)
Carboxylated multi-walled carbon nanotubes Norfloxacin 90.3 Yang et al. (2012)
Pristine and hydroxylated MWCNTs Sulfamethazine 24.78, 13.31 Yang et al. (2015)
CNTs based nanocomposite
Chitosan/Fe2O3/MWCNTs Methyl orange 66.90 Zhu et al. (2010)
Calcium alginate/MWCNTs Methyl orange 12.5 Zhu et al. (2010)
CNTs-C@Fe-chitosan composite Tetracycline 104 Ma et al. (2015a, b)
MWCNTs/CoFe2O4 Sulfamethoxazole 6.98 Wang et al. (2015)

SW: single-walled, MW: multiwalled

Santosh et al. (2016) cited (Zhao et al. 2011a, b) that
the graphene oxide prepared using acid treatment methods
resulted in a large number of oxygen atoms containing func-
tional groups on the surface of graphene oxide. The gra-
phene oxide obtained exhibited excellent hydrophilic char-
acteristics with greater reactivity towards the wide range of
contaminants (Santhosh et al. 2016).
The significant feature of the graphene oxide is due to
the presence of oxygen atoms containing functional groups
on the sheets of graphene oxide, thus facilitating the elec-
trostatic interactions with organic and inorganic pollutants.
Additionally, due to their electron-rich environment and
large specific surface area, graphene-based materials act as
an efficient adsorbent.
Several studies have been reported on the graphene-based
adsorbents and their applications for the removal of inor-
ganic pollutants from aqueous solutions (Zhao et al. 2011a,
b), which was reported by Santhosh et al. (2016). For the
remediation of metal ions from wastewaters, graphene oxide
was used as a model adsorbent in most of the studies cited
in the literature (Santhosh et al. 2016; Sitko et al. 2013a, b;
Wu et al. 2011; Zhao et al. 2011a, b). Graphene oxide is a
preferred material for the adsorption of metal ions due to
the existence of interaction sites, i.e. oxygen groups on the
surface, compared to the pristine graphene. The significance
of oxygen groups was described by using adsorption process
of lead (II) with oxidized a graphene sheet and pristine gra-
phene (Huang et al. 2011). To design composite materials,
graphene nanosheets (GNs) and graphene oxide can also be
combined with metal oxides. A typical hybrid of graphene
oxide/metal oxide has specific characteristics as an adsor-
bent for the removal of various pollutants from wastewaters.
Toxic metal ions such as lead (II), zinc (II) and cadmium (II)
were known to be removed by using a flower-shaped hybrid
of graphene oxide/titanium dioxide (Lee and Yang 2012). In
the same study at pH 5.6, adsorption efficiencies of lead (II),
zinc (II), and cadmium (II) were found to be 65.6 mg g−1,
88.9 mg g−1, and 72.8 mg g−1, respectively, using a hybrid
of graphene oxide/titanium dioxide. It was noted that higher
adsorption capacities were observed with nanocomposite
of graphene oxide/titanium dioxide, compared to graphene
oxide or titanium dioxide alone. The results obtained are
tabulated in Table 4.
The first time, pristine graphene was synthesised using
a vacuum-promoted low-temperature method followed by
a temperature treatment at 500 and 700 °C (GNS500 and

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 Environmental Chemistry Letters

Fig. 3  Graphene: the basic

structure of all carbon materials
that can be rolled up into a
graphene, b 3-D graphite, and
c zero-dimensional fullerenes
(reproduced with permission
of Balaji Mohana et al. 2018).
Copyright 2018 Elsevier

Table 4  Various graphene- Inorganic pol- Graphene-based nanocomposite Adsorption efficiency Citation

based nanocomposites for the lutants (mg/g)
removal of some heavy metal
ions Cu(II) Graphene oxide (GO)/Fe3O4 18.3 Li et al. (2012a, b)
GO/Fe3O4/sulfanilic acid 50.7 and 56.8 Hur et al. (2015)
GO/Fe3O4 23.1 Hur et al. (2015)
GO/Mn-doped Fe(III)oxide 129.7 Nandi et al. (2013)
Pb(II) GO/silica/Fe3O4 333.3 Wang et al. (2013a, b)
GO-MnFe2O4 673 Kumar et al. (2014)
rGo/COFe2O4 299.4 Ozmen et al. (2010)
GO/Fe3O4 38.5 Hur et al. (2015)
TiO2/GO 65.6 Madadrang et al. (2012)
GO-EDTA 479 Madadrang et al. (2012)
SiO2–GNs 113.6 Hao et al. (2012)
Cd(II) GO/silica/Fe3O4 166.7 Wang et al. (2013b)
GO/Mn-doped Fe(III)oxide 87.2 Nandi et al. (2013)
GO/Fe3O4 4.4 Hur et al. (2015)
Hg(II) MnO2/GNs 10.8 Sreeprasad et al. (2011)

GNS700) to incorporate oxygen groups onto the surface
of graphene oxide sheets. Then, the adsorption capacity
of normal pristine graphene was evaluated and found to be
less when compared to the graphene synthesized at 500 and
700 °C for the removal of lead (II) ions from the wastewa-
ters. This was due to the contribution of oxygen functional
groups in the adsorption mechanism (Huang et al. 2011; Lee
and Yang 2012). Furthermore, graphene-based adsorbents
were also used to remove a wide range of organic pollutants
from the wastewater systems and the results obtained are
summarized in Table 5.
Apart from the adsorption capacity, the toxicity, transfor-
mation, and fate of graphene-based materials have been widely
reviewed in the literature (Bianco 2013; Bussy et al. 2012;

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Environmental Chemistry Letters

Table 5  Adsorption of organic pollutants using graphene-based materials

Organic pollutants Graphene oxide-based nanocomposite Adsorption efficiency Citation
(mg/g)

Methylene blue Polyethersulfone/GO 62.50 Zhang et al. (2013a, b)

Fe3O4/GO hybrids 167.2 Xie et al. (2012)
GO sponge 397 Liu et al. (2012)
Reduced GO/ZnO nanohybrids – Fan et al. (2012), Pant et al.
(2013) and Xie et al. (2012)
Reduced GO/CdS hybrids 94 (%) Wang et al. (2012a, b, c)
Reduced GO–MFe2O4 hybrids 92 (%) Bai et al. (2012)
Fe3O4–GNs 45.3 Yao et al. (2012)
GO 351 Bradder et al. (2010)
GNs 154–204 Bai et al. (2012)
Neutral red Fe3O4/GO hybrids 171.3 Xie et al. (2012)
Rhodamine B Reduced GO–MFe2O4 hybrids 92 (%) Madadrang et al. (2012)
Reduced GO/ZnO nanohybrids – Fan et al. (2012), Pant et al.
(2013) and Xie et al. (2012)
Methylene violet GO sponge 467 Liu et al. (2012)
Methylene orange Reduced GO–TiO2 – Pastrana-Martinez et al. (2012)
Congo red Fe3O4–GNs 33.7 Yao et al. (2012)
Ciprofloxacin Porous graphene hydrogel 235.6 Ma et al. (2015a, b)
KOH-activated graphene 194.6 Yu et al. (2015)
Single layer GO 379 Chen et al. (2015)
Tetracycline TiO2-graphene sponge 1805 Zhao et al. (2015)
GO 381.77 Ghadim et al. (2013)
F–GO with MNPs 39.1 Lin et al. (2013)
GO 313.48 Gao et al. (2012)
Doxycycline F–GO with MNPs 35.5 Lin et al. (2013)
GO 398.40 Gao et al. (2012)
Oxytetracycline GO 212.31 Gao et al. (2012)
F–GO with MNPs 45.0 Lin et al. (2013)
Chlortetracycline F–GO with MNPs 42.6 Lin et al. (2013)

GO: graphene oxide, GN: graphene nanosheets, MNP: metal nanoparticle

Hu and Zhou 2013). Due to the lack of historical data, the
ecotoxicological properties and life cycle of different forms
of graphene-based materials which have a minimal impact on
environmental and health system must be evaluated and identi-
fied urgently. It would be difficult to find out the most reliable
areas of graphene-based material research due to their environ-
mental and economic considerations. On the other hand, it is a
challenging task to reduce graphene oxide to pristine graphene
by restoring its mechanical and electronic properties. On the
large scale, reduction of graphene is one of the cost-effective
methods for the production of graphene oxide.
Metal nanoparticles
Silver nanoparticles
The silver nanoparticles are found to be highly toxic to micro-
organisms resulting in effective microbial defence against
fungi (Krishnaraj et al. 2012), bacteria (Kalhapure et al. 2015),
and viruses (Borrego et al. 2016). Due to this activity, silver
nanoparticles have been extensively used for the disinfection
of water. It was reported that silver nanoparticles interact with
bacterial cell wall and then penetrate the cell resulting in a
change in the cell wall structure and consequently enhancing
permeable capacity (Sondi and Salopek-Sondi 2004). In addi-
tion, free radicals can be formed from the interaction of silver
nanoparticles with bacteria resulting in cell wall damage and
finally cause the death of cells (Danilczuk et al. 2006). Fur-
thermore, silver nanoparticles can interact with phosphorus
and sulphur elements present in DNA and destroy the whole
bacterial cell. Interestingly, it was found that the death of bac-
terial cells by the silver nanoparticles is due to the generation
of antimicrobial silver(I) ions, which can later interact with
the thiol functional group of the enzymes, deactivate them,
and disturb the regular functions of the cells (Dhanalekshmi
and Meena 2016; Prabhu and Poulose 2012). Although these

13

theories have emerged, the antimicrobial mechanism of silver
nanoparticles is still unclear and remains under discussion.
Recent advancements in nanotechnology reveal that silver
nanoparticles have been effectively used in wastewater treat-
ment. However, unmodified silver nanoparticles have a ten-
dency to form clusters in aqueous media and thus this slowly
decreases their antimicrobial ability during long-term use
(Li et al. 2011). The integration of silver nanoparticles with
filtration membranes or filters has been considered useful
for the disinfection of water due to their effective antibacte-
rial abilities and cost-effectiveness (Quang et al. 2013). It
was noted that sheets of silver nanoparticles exhibited effec-
tive antibacterial properties towards Enterococcus faecalis,
Escherichia coli, and deactivated bacteria while filtering
through the sheet.
According to World Health Organization and the Envi-
ronmental Protection Agency, the concentration of silver
ions generated from silver nanoparticles was lower than the
standards of silver ions in the drinking water (Dankovich
and Gray 2011). Thus, the membrane filters prepared with
polyethersulfone and silver nanoparticles could be an effec-
tive tool for the treatment of wastewater contaminated by
bacteria.
It was found that unusual suppression of microorganisms
was observed near the membrane resulting in strong antimi-
crobial activity, thus creating the potential for wastewater
treatment applications (Ferreira et al. 2015). In past dec-
ades, silver nanoparticles were coated on ceramic materi-
als or integrated into membranes. This has drawn consider-
able attention due to the biofouling reduction of household
water treatment and disinfection of waters (Ren and Smith
2013). The simple way of designing an effective treatment
of Escherichia coli from wastewaters was performed by
accumulating silver nanoparticles with ceramic filters man-
ufactured with clay and sawdust. It was found that filters
with higher porosity removed more bacteria than those with
lower porosity filters (Kallman et al. 2010). In addition, sil-
ver nanoparticles integrated with cylindrical ceramic filters
made up of flour, grog, clay-rich soil, and water in various
compositions showed improved filtration performances of
Escherichia coli with a removal percentage of 97.80–100%
(Oyanedel-Craver and Smith 2007). The Derjaguin-Landau-
Verwey-Overbeek (DLVO) approximation methods were
adopted to predict successful incorporation of silver nano-
particles into ceramic membranes (Mikelonis et al. 2016).
Additional studies on silver nanoparticles will endorse their
applications in wastewater treatment.
Iron nanoparticles
Recently, researchers’ attention has been drawn on various
nano-zerovalent metal particles such as nickel, aluminium,
iron, and zinc for the treatment of wastewater.
13
Environmental Chemistry Letters
It was found that nano-zero-valent aluminium has a great
reduction ability and is thermodynamically unstable in an
aqueous medium, resulting in the formation of hydroxides/
oxides on the surface preventing the electron transfer from
the contaminants to the metal surface (Rivero-Huguet and
Marshall 2009).
The reduction ability of nickel is lower than iron due to
the less electronegative standard reduction potential. How-
ever, nano-zero-valent iron or zinc has a moderate standard
reduction potential to exhibit good reduction abilities when
compared to various redox contaminants. The nano-zerov-
alent iron has many advantages over zinc due to a weaker
reduction capacity. This property has allowed researchers
to use nano-zerovalent iron extensively in water treatment
processes, owing to its outstanding adsorption capacity, its
cost-effectiveness, oxidation, and precipitation. Because of
the stronger reduction ability, small size, and large surface
area, iron nanoparticles have been widely used metal nano-
particles in wastewater treatment (Fu et al. 2014; Matheson
and Tratnyek 1994; Wang et al. 2013a, b) (Table 6).
Different separation methods such as precipitation,
adsorption, oxidation, and reduction were adopted by
nano-zerovalent iron particles for the removal of wide
range of pollutants, including radioactive elements (Ling
and Zhang 2015), heavy toxic metals (Arancibia-Miranda
et al. 2016), metalloids (Ling et al. 2015; Muradova et al.
2016), inorganic anions (Markova et al. 2013), organic
dyes (Hoag et al. 2009), aromatic compounds with nitro
group (Xiong et al. 2015), phenols (Wang et al. 2013a),
and halogenated organic molecules (Liang et al. 2014).
The applications of nano-zerovalent iron particles in
wastewater treatment are not limited to laboratory scale
but also used for soil remediation in industrial-/pilot-scale
treatment from contaminated sites (Gueye et  al. 2016;
Zhang 2003). Although nano-zerovalent iron particles
have several advantages, oxidation, aggregation, and sepa-
ration difficulties from the degradation system are some
of the disadvantages associated with these nanoparticles.
To overcome these problems, different coating methods
have been adopted to increase the performance of nano-
zerovalent iron particles in wastewater treatment. The most
familiar coating method includes doping of other metals,
encapsulation in the matrix, surface modification, and
emulsification (Stefaniuk et al. 2016). It was demonstrated
Table 6  Standard reduction Metals Standard reduction
potential of various metals potential ­(Eo/V)
(Bratsch 1989)
Nickel − 0.236
Zinc − 0.762
Iron − 0.440
Aluminium − 1.677
Environmental Chemistry Letters
that the nanoparticles doped with other metals are assumed
to increase the reactivity of nano-zerovalent iron particles
(Liou et al. 2005). Furthermore, conjugation with sup-
port and surface modification can avoid aggregation and
increase the dispersibility of nano-zerovalent iron particles
(Chen et al. 2011a, b; Singh and Misra 2016). On the other
hand, encapsulation of nano-zerovalent iron in the matrix
and conjugation with the substrate provided the effective
separation of nano-zerovalent iron particles from the deg-
radation system (Berge and Ramsburg 2009; Li et al. 2016;
Lv et al. 2014).
Zinc nanoparticles
Though reports on the degradation of pollutants in waste-
water treatment by nano-zerovalent metal nanoparticles had
been focused on iron, zinc is considered as an alternative for
the silver and iron nano-zerovalent particles (Bokare et al.
2013). With an extra negative standard reduction ability (see
Table 5), nano-zerovalent iron particles are a weak reductant
when compared to nano-zerovalent zinc particles. Therefore,
it was noted that the degradation ability of pollutants with
zinc nanoparticles may be faster than that of nano-zerov-
alent zinc particles. Most of the dehalogenation reactions
in wastewater have been focused on the nano-zerovalent
zinc particles and their applications. Recent studies have
specified that the reduction rates of carbon tetrachloride with
nano-zerovalent zinc particles were significantly affected by
physicochemical properties than by the size of the particle
or surface morphology. By evaluating the reactivity of dif-
ferent types of nano-zerovalent iron and zinc, it was found
that nano-zerovalent zinc could degrade carbon tetrachloride
faster than with nano-zerovalent iron under optimal experi-
mental conditions (Tratnyek et al. 2010). In addition, a study
examined the degradation of octachlorodibenzo-p-dioxin in
wastewaters with four distinct zerovalent metal nanoparticles
such as nano-zerovalent nickel, aluminium, iron, and zinc.
Under optimal reaction conditions, maximum degradation
efficiency of octachlorodibenzo-p-dioxin was achieved by
nano-zerovalent zinc with minimal chlorinated congeners.
Therefore, it was found that nano-zerovalent zinc was the
first nanomaterial recorded as suitable for octachlorod-
ibenzo-p-dioxin degradation (Bokare et al. 2013). Though
various reports have validated that degradation of pollut-
ants with nano-zerovalent zinc could be fruitful, the appli-
cations of nano-zerovalent zinc towards the degradation of
organic pollutants are limited only to carbon tetrachloride.
Very few reports have been recorded on the treatment of pol-
luted water with nano-zerovalent zinc. Consequently, in situ
research on the treatment of wastewaters for the degradation
of pollutants with nano-zerovalent zinc has not been com-
pletely accomplished (Tratnyek et al. 2010).
Magnetic‑core composite nano‑/microparticles
The magnetic-core nano-/microparticles consist of magnetic
elements such as cobalt, nickel, iron, and other oxides in
the centre including alloys with superparamagnetic or fer-
romagnetic material such as shells ranging from micro- to
nano-level (Ambashta and Sillanpää 2010; Clark and Keller
2012; Girginova et al. 2010; Huang et al. 2012; Liu et al.
2008; Ngomsik et al. 2005). In addition, silica (Bagheri
et al. 2012; Clark and Keller 2012; Huang and Keller 2013;
Mashhadizadeh and Amoli-Diva 2013; Wang et al. 2008a,
b), alumina (Karimi et al. 2012) or organic molecules such
as surfactants (Afkhami et al. 2010; Faraji et al. 2010) and
polymers (Ashtari et al. 2005; Li et al. 2010) can be used to
make the shells of the nanoparticles. These modifications
can enhance the chemical and thermal stability of the nano-
particle, avoid oxidation processes, and increase the water
solubility of hydrophobic pollutants (Clark and Keller 2012;
Huang and Keller 2013; Wang et al. 2008a, 2011a, b) or
selective uptake of ions (Afkhami et al. 2010; Ashtari et al.
2005; Faraji et al. 2010; Li et al. 2010). It was found that
the magnetic-core shell nanoparticles are favourable for
the quick separation of pollutants when compared to non-
magnetic particles from the wastewater by applying exter-
nal magnetic field due to their superparamagnetic property
(Huang and Keller 2013; Wang et al. 2008a).
Metal oxide nanoparticles
Iron oxide nanoparticles
Recently, several researchers have focussed on the use of
iron oxide nanoparticles for the elimination of toxic heavy
metals due to their unique physicochemical properties
such as large surface area, easy to synthesize, and ability
to act as a superior adsorbent. Several magnetic nanoma-
terials are available; however, maghemite, magnetite, and
non-magnetic haematite are often used as nanoadsorbents.
Mostly, nanoadsorbents are small in size and their recovery
and separation after wastewater treatment are challenging
tasks. Nevertheless, maghemite and magnetite nanoparti-
cles can be easily separated after wastewater treatment. This
is one of the unique features of iron oxide nanoparticles.
Therefore, iron oxide nanoparticles are effectively adopted
as promising nanoadsorbents in the removal of a wide range
of toxic heavy metals from wastewaters (Lei et al. 2014;
Ngomsik et al. 2012; Tan et al. 2014). The functionalization
of iron nanoparticles with various ligands, namely α-thio-
ω-(propionic acid) hepta-(ethylene glycol), mercaptobutyric
acid, ethylenediamine tetraacetic acid, L-glutathione, meso-
2,3-dimercaptosuccinic acid, and polymers, may increase the
adsorption efficiency and avoids inference from the other
metal ions (Ge et al. 2012; Warner et al. 2010). Khaydarov
13

et al. (2010) designed a flexible shell integrated with wide
range of functional groups to safeguard the properties of
iron oxide nanoparticles from any damage . In addition, the
polymer shell was designed to prevent the aggregation of
iron oxide nanoparticles and to improve their monodisper-
sion (Ge et al. 2012). Nanohaematite has been used as a cost-
effective and promising material in environmental applica-
tions, catalysis, and sensors (Liang et al. 2014). Moreover,
nanohaematite has proved to be a powerful adsorbent for
the elimination of heavy metal ions from spiked water sam-
ples (Shipley et al. 2013). Liang and Wang synthesized
self-assembled 3-D flower-like iron oxide nanoparticles for
the water remediation purpose. The flower-like iron oxide
nanoparticles efficiently avoid the aggregation of nanopar-
ticles and improve their surface area with active spaces and
pores, resulting in greater adsorption of pollutants. It found
excellent adsorption of arsenic (V) and chromium (VI) onto
the surface of 3-D flower-like iron oxide, when compared to
that of other nanomaterials (Liang et al. 2014).
The easy existence of iron and its facile synthesis methods
make ferric oxide a cost-effective material for the adsorp-
tion and removal of toxic metals. Moreover, iron oxides are
environmentally friendly and can be used effectively to treat
wastewaters with minimal production of toxic secondary
contaminations (Li et al. 2006a, b).
Different experimental factors such as temperature, incu-
bation time, pH, and adsorbent dosage were optimized to
increase the removal efficiency of iron oxide nanoparticles
(Tyagi et al. 2017). In addition, the adsorption capacity
of iron oxide nanoparticles was evident by modifying the
surface with 3-aminopropyltrimethoxysilane (Ozmen et al.
2010; Palimi et al. 2014). It was observed that after the sur-
face modification of iron oxide nanoparticles, the adsorption
of various heavy metals such as arsenic (III), lead (II), cop-
per (II), cobalt (II), chromium (III), nickel (II), and cadmium
(II) was drastically enhanced from wastewaters (Tyagi et al.
2017).
Zinc oxide nanoparticles
Recent literature has suggested that zinc oxide nanoparticles
have been developed as an effective and promising photo-
catalytic material when compared to titanium dioxide in the
treatment of wastewaters. Due to their unique properties
such as direct and broader band gap in the near-ultraviolet
region, greater oxidation capacity, and excellent photocata-
lytic property, zinc oxide nanoparticles were found to be
excellent materials (Chen et al. 1998; Janotti and Van de
Walle 2009; Reynolds et al. 1999). Moreover, zinc oxide
nanoparticles are eco-friendly as they are coherent with
organisms, thus making them appropriate for the treatment
of wastewaters (Schmidt-Mende and MacManus-Driscoll
2007). Further, the photocatalytic ability of zinc oxide
13
Environmental Chemistry Letters
nanoparticles is comparable to titanium dioxide, in light of
the fact that their band-gap energies are nearly the same
(Daneshvar et al. 2004). Zinc oxide nanoparticles are cost-
effective (Daneshvar et al. 2004), adsorb solar light from
a wider spectrum, and have more light quanta, compared
to those of other semiconducting metal oxides (Behnajady
et al. 2006). It was found that the absorption of light by
zinc oxide nanoparticles is limited in the ultraviolet region
similar to titanium dioxide nanoparticles due to their wide
band-gap energies. Moreover, the applications of zinc oxide
nanoparticles are hindered by photocorrosion, resulting in
the quick rearrangement of photo-generated charges, thus
lowering of photocatalytic ability (Gomez-Solís et al. 2015).
The doping of metals into zinc oxide nanoparticles is one
of the common approaches to enhance the photocatalytic
capacity. It was noted that different dopants, namely cati-
onic, anionic, co-dopants, and rare-earth dopants have been
examined to test the photocatalytic efficiency of zinc oxide
nanoparticles (Lee et al. 2016). Furthermore, several reports
have suggested that the modification of zinc oxide nanopar-
ticles with other semiconducting materials such as graphene
oxide (Dai et al. 2014), tin(IV) oxide (Uddin et al. 2012),
cadmium oxide (Samadi et al. 2014), titanium dioxide (Pant
et al. 2012), and cerium (IV) oxide (Dai et al. 2014) is a
practical approach to increase the photodegradation ability
of zinc oxide nanoparticles.
Manganese oxide nanoparticles
Manganese oxide nanoparticles exhibit excellent adsorption
capacity due to their high Brunauer–Emmett–Teller surface
(Luo et al. 2010) and are extensively used for the removal
of arsenic from wastewaters (Wang et al. 2011a, b). Further-
more, commonly used modified manganese oxide nanopar-
ticles include hydrous manganese oxide and nanotunnel or
nanoporous manganese oxides (Tyagi et al. 2017). In another
report, hydrous manganese oxide was synthesized by add-
ing manganese sulphate dihydrate into sodium hypochlorite
solution (Zaman et al. 2009). The fabricated hydrous man-
ganese oxide has Brunauer–Emmett–Teller surface area of
about 100.5 m2 ­g−1. Gupta and co-workers developed a novel
hydrous manganese oxide for the removal of zinc (II), cad-
mium (II), and lead (II) effectively due to the ion-exchange
process (Tyagi et al. 2017). The adsorption mechanism of
divalent metal ions takes place in two steps. Initially, adsorp-
tion of metal ions onto the external surface of hydrous man-
ganese oxides occurs, followed by the intra-particle diffusion
(Parida et al. 1981).
Magnesium oxide nanoparticles
Magnesium oxide is utilized for the elimination of various
types of toxic heavy metals from wastewaters. Magnesium
Environmental Chemistry Letters
nanospheres are novel and used to enhance the adsorption
efficiency for the removal of heavy metals (Tyagi et  al.
2017). To enhance the adsorption ability of magnesium
oxide, various fabrication methods were performed in
nanoparticles morphology. These are comprised of nano-
cubes (Li et al. 2002), nanobelts (Zhu et al. 2001), nanorods
(Engates and Shipley 2011), nanotubes (Yin et al. 2002),
and three-dimensional structures (Klug and Dravid 2002).
It demonstrated that the efficient adsorption of lead(II) and
cadmium(II) was performed with mesoporous flower-like
magnesium oxide (Li et al. 2003a, b, c, d).
Nanomaterial‑enabled wastewater
techniques for organic pollutants
Literature suggests that carbon-based nanomaterials were
used as excellent adsorbents on laboratory-scale experiments
for the removal of organic compounds (Bikshapathi et al.
2011; Cheng et al. 2005; Ji et al. 2012; Ma et al. 2011; Peng
et al. 2003a, b; Velzeboer et al. 2014; Wang et al. 2014a,
b, c, d). Recently, 3-D sponge-like carbon nanotube frame-
works were designed by Camilli and co-workers. They found
that the adsorption capacity of dichlorobenzene was 3.5-fold
greater when compared to carbon nanotubes and it was easy
to recover them from the aqueous solutions (Camilli et al.
2014). It was demonstrated that carbon nanotubes and gra-
phene oxide interacted strongly with chlorobenzene, due to
the presence of chlorine groups. Therefore, these materials
are highly suitable for the adsorption and the removal of
chlorobenzene. However, graphene oxide showed stronger
interaction with chlorobenzene, resulting in a higher adsorp-
tion ability than single-walled carbon nanotubes (Balamuru-
gan and Subramanian 2013). Like existing methods, metal or
metal oxide engineered nanomaterials-based photodegrada-
tion is one of the main methods for the treatment of organic
pollutants. Due to their specific and large surface area to
volume ratio, these materials provide a greater reactivity
compared to the current bulk catalyst. It was found that pure
(Ba-Abbad et al. 2012a, b; Oyama et al. 2011; Peiro et al.
2001; Shengyong et al. 2013) and doped forms of titanium
dioxide (Jung and Park 2000; Park and Lee 2014; Shchukin
et al. 2004), as well as other selected nanomaterials (Botía
et al. 2012; Kamat et al. 2002), have been considered as
excellent photocatalysts for the wide range of organic pollut-
ants. It was concluded that dehalogenation and photodegrad-
ation processes are found to be suitable for a variety of water
treatment applications (Ba-Abbad et al. 2012a, b; Barakat
et al. 2014; Botía et al. 2012; Oyama et al. 2011; Peiro et al.
2001; Suryaman and Hasegawa 2010) in laboratory-scale
experiments, as well as in pilot-scale reactors (Oyama et al.
2011; Peiro et al. 2001).
Furthermore, organochlorine pesticides, organic dyes,
polychlorinated biphenyls, and other chlorinated organic
solvents were degraded effectively using nano-zerovalent
iron particles (Cho and Choi 2010; Liu et al. 2007; Ma et al.
2013; Zhang 2003). Kim et al. (2012) developed a novel
method for the degradation of polybrominated diphenyl
ethers and their degradation products using a sequential
nano-bio-treatment process with nano-zerovalent iron par-
ticles. Li et al. (2008a, b) prepared cetyltrimethylammonium
bromide-modified iron oxide nanoparticles for the adsorp-
tion and removal of a variety of chlorophenols from the
wastewaters. Likewise, Wang et al. (2008a, b) used a mag-
netic permanently confined micelle array for the removal of
organochlorinated pesticides from water and soil samples. It
demonstrated that a magnetic permanently confined micelle
array was effective for the removal of organochlorinated
pesticides and can be easily regenerated after the treatment
process (Wang et al. 2008a).
Performance and cost evaluation between existing
methods and nanomaterial‑based methods
Based on the adsorption and removal efficiency of chlo-
rinated organic pollutants, activated carbon is found to be
a cost-effective and promising material in the wastewater
treatment process. Though metal or metal oxide engineered
nanomaterials have the highest removal ability of pollut-
ants (per weight up to 500 mg g−1 of nanoparticles), in the
case of P25 titanium dioxide nanoparticles-based photoca-
talysis, similar cost implications were found in the treat-
ment of organic pollutants. It was found that treatment of
wastewater for chlorophenols (per gram) cost US$ 0.51 with
titanium dioxide. But with activated carbon and coir pith,
the estimated cost was found to be US$0.14 and US$ 0.03
for chlorophenols-associated wastewater treatment process
(Adeleye et al. 2016).
Magnetic permanently confined micelle array tech-
niques are considered as effective methods for the removal
of 80 mg g−1 of chlorophenols with an approximate cost
of US$0.05 per gram, which is comparable to the existing
conventional methods. Though magnetic permanently con-
fined micelle arrays are highly expensive, it has the ability
for multiple uses. Photocatalysis by metal/metal oxide engi-
neered nanomaterials removes the extra costs allied with
the management and storage of huge quantities of polluted
sorbent. Accordingly, these existing methods for the treat-
ment of chlorinated pollutants are practical and expensive,
compared to the other methods.
Carbon-based engineered nanomaterials are considered
to have excellent adsorption ability for variety of organic
pollutants such as volatile organic compounds, polyaro-
matic hydrocarbons, industrial dyes, and herbicides in both
natural and spiked water samples (Farghali et al. 2013a,
13

b; Hou et al. 2013; Hüffer et al. 2013; Liu et al. 2011a, b;
Moradi et al. 2012; Wang et al. 2014a, b, c, d). The adsorp-
tion of water-insoluble organic pollutants is circuitously
associated with the degree of oxidation of carbon-based
nanoadsorbents (WangChen et al. 2014, WangHuang et al.
2014). On the other hand, carbon-based nanoadsorbents
were also used as filters for the separation and removal of
water/emulsified oil mixtures (Shi et al. 2013). The inte-
gration of graphene oxide and carbon nanotubes has been
adopted to fabricate membranes/filters that recollect pol-
lutants based on size exclusion and have also been inserted
into existing membranes such as polyamide, polyether-
sulfone, and ceramics for enhanced performance. It was
found that fewer nanocomposite membranes have revealed
a reasonable to a greater removal percent of industrial
dyes from wastewaters (Hou et al. 2013). A recent report
suggested that the carbon nanotube-based hollow fibre
membrane showed 100% removal of Rhodamine B from
wastewater samples (Wei et  al. 2014). The most com-
monly used water treatment processes such as adsorption,
non-photoactive oxidation/reduction, and photodegrada-
tion with metal/metal oxide engineered nanomaterials are
reported in the literature for the removal of organic pollut-
ants. Titanium dioxide nanoparticles-based photodegrada-
tion is a widely used technique for its enhanced perfor-
mance after doping (Bouras et al. 2007a, b; Georgekutty
et al. 2008; Nagaveni et al. 2004; Yang et al. 2002, 2013)
and (Barakat et al. 2014; Kim and Kwak 2007; Kominami
et al. 2002; Peiro et al. 2001; Zhan et al. 2006) with other
semiconducting metals oxides. Besides titanium dioxide,
several other materials such as zinc oxide/zinc-aluminate
(Cho et al. 2012; Lam et al. 2013; Ullah and Dutta 2008),
nickel oxide (Suo et al. 2013), silver/silver oxide (Lam
et al. 2013; Xiong et al. 2010), cuprous oxide (Aazam
and Mohamed 2013), and russellite (Zhang et al. 2009)
were used as photocatalysts. In the literature, only a few
reports are available on the metal/metal oxide engineered
nanomaterials as adsorbents and oxidizing agent for the
removal of organic materials (Chen and He 2008; Wu et al.
2014). Chen and He (2008) used manganese oxide nano-
particles for the removal of methylene blue (Chen and He
2008), whereas others have proposed manganese oxides
as an oxidizing agent for organic impurities (Behnam
et al. 2013; Ding et al. 2005; Saputra et al. 2013a, b).
In addition, dioxoruthenium (Muhammad et  al. 2012),
cobalt oxide (Saputra et al. 2013a, b), magnesium oxide,
and aluminium oxide (Behnam et al. 2013) were used as
oxidizing agents; however, in the early studies mentioned
above, peroxymonosulphate was used to generate sulphate
radicals for oxidation to occur. Various experimental con-
ditions such as high dosage of nano-zerovalent iron, high
reaction temperature, and low initial pH were studied to
13
Environmental Chemistry Letters
enhance the adsorption capacity of dye wastewaters (Fan
et al. 2009; Shu et al. 2010, 2007a, b).
Magnetic nanoparticles are extensively used for the removal
of polyaromatic hydrocarbons (Liu et al. 2009; Wang et al.
2008a; Zhang et al. 2010) and natural organic matter (Wang
et al. 2011b) from wastewaters. Liu et al. (2009) developed
­C18-functionalized iron oxide microspheres for the extraction
of 16 polyaromatic hydrocarbons from tap water based on the
hydrophobic interactions.
In another study, octadecyl-functionalized iron oxide nano-
particles were used to prepare hydrophilic alginate polymers
to increase the solubility and dispersibility of analytes in aque-
ous solutions (Zhang et al. 2010). The alginate polymer-based
nanomaterials were used for selective extraction of polyaro-
matic hydrocarbons due to the blockage of humic acid via size
exclusion and electrostatic force of repulsion. Zhao and co-
worker designed cetyltrimethylammonium bromide-modified
iron oxide engineered of 4-n-nonylphenol and 4-tert-octylphe-
nol (Zhao et al. 2008a, b).
Performance and cost evaluation of existing
methods and nanomaterial‑based methods
In the case of organic pollutants treatment, the adsorption
process was found to be the more effective method in terms
of both cost and removal efficiency. The treatment cost of
polyaromatic hydrocarbons is comparable to the existing and
nanotechnology-based methods. However, magnetic nanopar-
ticles are cheaper and can be used to treat naphthalene polluted
wastewater at an estimated cost of US$ 4 per gram of pollut-
ant, compared to the current methods with removal efficiency
greater than 95%.
It was found that some of the existing methods such as
microfiltration, ion-exchange, ultrasound degradation, oxida-
tion, and activated sludge have shown that complete removal
of pollutants occurs from hours to months based on the ana-
lyte and treatment process. Interestingly, it was shown that
the magnetic permanently confined micelle arrays have the
greater adsorption and removal efficiency and a relatively low
cost compared to existing methods. It can be concluded that
carbon-based nanomaterials have demonstrated higher adsorp-
tion and removal ability in a wide variety of organic pollutants.
Additionally, the operational cost is reasonable compared to
current methods, making them a perfect choice, since the price
of the carbon-based nanomaterials is expected to reduce con-
tinuously with time. Literature survey results were created in
the form of database and are presented in Table 7.
 Table 7  Performance and cost for various treatment technologies for organic compounds
Contaminants Engineered nanomaterials-based methods Merit of figures Citation
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

2-Chlorophenol Fenton ­processa 90/6 min Kwon et al. (1999)

Photo-Fenton 97/30 min Kavitha and Palanivelu (2003), Perez-Moya
et al. (2007) and Poulopoulos et al. (2008)
Environmental Chemistry Letters

Ultrasound coupled to Fenton p­ rocessa 99/90 min Lin and Ma (2000)

Electrochemical-based ­oxidationa 50/360 min Polcaro et al. (1999)
Adsorption using activated ­carbona < 0.0001 80/7 d 140–270 Aktaş and Çeçen (2007)
Carbon-based ­adsorptiona < 0.00003 99/20 min 4–17 Namasivayam and Kavitha (2003)
Reverse ­osmosisa > 99/7.5 h Williams et al. (1999)
Degradation by aerobic–anaerobic p­ rocessa 95/26 h 17 Atuanya et al. (2000)
Hybrid of titanium dioxide/In2O3b 26/1.5 h 58 Shchukin et al. (2004)
Titanium dioxide (P25)b 0.0005 68/2 h 248 Peiro et al. (2001)
Titanium dioxide ­nanoparticlesb 99/1.5 h 50 Ba-Abbad et al. (2012a, b)
Titanium dioxide nanoparticles(P25) coupled 100/2 h 64.3 Suryaman and Hasegawa (2010)
to ­bioreactorb
Titanium dioxide nanoparticles (P25) cou- 100 80 Oyama et al. (2011)
pled to ozonation ­processb
Magnetic permanently confined micelle ~ 0.00005 80/24 h Huang and Keller (2013)
­arraysb
Zinc oxide/zinc sulphide functionalized with 89/ 50 Anjum et al. (2017)
­polyanilineb
Chlorobenzene Photolysisa 90/4 min Legrini et al. (1993)
Ultraviolet coupled to hydrogen peroxide > 98/30 min Legrini et al. (1993)
­methoda
Biodegradation ­processa > 99/90 d Field and Sierra-Alvarez (2008)
Fenton ­processa > 99/1 h Casero et al. (1997)
Magnetic permanently confined micelle 0.000096 41.692 Huang and Keller (2013)
­arraysb
Titanium dioxide modified with bentonite > 99/10 min 0.2 Mishra et al. (2017)
­nanocompositeb
1,1,1-Trichloroethane Pristine multi-walled carbon ­nanotubesb 36.1 0.35 Ma et al. (2011)
Biochar-supported hybrid of nickel/iron 99.3 20 Li et al. (2017)
bimetallic ­nanoparticlesb

13


Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation

13
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

1,2-Dichlorobenzene Pristine carbon ­nanotubesb 5.26 30.8 Peng et al. (2003a, b)

Graphitized carbon ­nanotubesb 5.66 28.7 Peng et al. (2003a, b)
Carbon nanotubes ­frameworkb 100 Camilli et al. (2014)
Zinc sulphide@ indium(III) sulphide core@ 49/8 h Liu et al. (2017)
shell ­compositeb
Magnetite nanoparticles @titanium dioxide 95/90 min Salamat et al. (2017)
­nanocompositeb
1,3,5-Trichlorobenzene Pristine multi-walled carbon ­nanotubesa 9.77 1.29 Ma et al. (2011)
Thermally treated multi-walled carbon 6.24 2.01 Ma et al. (2011)
­nanotubesb
2,2′-Dichlorobenzene Membrane integrated with iron/palladiumb 100/1 h 7.36 Xu and Bhattacharyya (2005)
2,4,6-Trichlorophenol Adsorption using activated ­carbona 2.17–6.33 > 92/25 h 169–716 Hameed et al. (2008, 2009) and Tan et al.
(2009)
Adsorption using c­ laya > 90/100 min 14–79 Hameed (2007)
Ultraviolet process coupled to titanium 80/15 min Benitez et al. (1999)
­dioxideb
Natural haematite modified with chloride of 96/180 100 Benbachir et al. (2017)
zirconium ­oxideb
2,4-Dichlorophenol Biodegradation ­processa 90/21 d Wang et al. (2000a, b)
Biodegradation process coupled to 82/21 d Contreras et al. (2003)
­ozonationa
Biodegradation process coupled to Fenton 90/400 min Chamarro et al. (2001)
­processa
Adsorption using activated c­ arbona 98/21 min 0.38–1.90c Akhtar et al. (2006) and Sathishkumar et al.
(2007)
Electrochemical ­oxidationa > 90/360 min Brillas et al. (2000)
Photo-Fenton ­processa > 99/1 h Pupo Nogueira et al. (2002)
Ultraviolet ­processa 19.5/2 h Yang et al. (2008a, b)
Titanium dioxide ­nanoparticlesb 248 99/2 h Ba-Abbad et al. (2012a, b)
Titanium dioxide nanoparticles(P25) coupled 50 100/2 h Suryaman and Hasegawa (2010)
to ­bioreactorb
Titanium dioxide nanoparticles(P25) coupled 313 100/0.67 h Peller et al. (2003)
to ­sonolysisb
Cobalt-doped titanium dioxide n­ anoparticlesb 96.62/120 min 40 Benbachir et al. (2017)
Magnetic spinel iron cobaltite n­ anoparticlesb 95.8/90 min Hoseini et al. (2017)
Environmental Chemistry Letters
 Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

2,4,5- Trichlorophenol Photoelectron-associated ­Fentona > 98/360 min Boye et al. (2003a, b)

Ultraviolet ­processa > 95/360 min Boye et al. (2003a, b)
Biodegradation ­processa 97/6 d Kilbane et al. (1982)
Environmental Chemistry Letters

Titanium dioxide nanoparticles(P25) coupled 50 100/2 h Suryaman and Hasegawa (2010)

to ­bioreactorb
Hexachlorobenzene Hydrogen peroxide-based oxidation p­ rocessa >90/4 h Watts et al. (1994)
Hydrogen peroxide-based ultraviolet oxida- 50/1 h Legrini et al. (1993)
tion ­processa
Titanium dioxide thin ­filma Lu et al. (2013)
Phencyclidine Electrochemical oxidation p­ rocessa 95/11 h Hanna et al. (2005)
Photo-Fenton ­processa > 90/5 min Engwall et al. (1999)
Biodegradation-based anaerobic ­processa 66 Mikesell and Boyd (1986)
Titanium dioxide nanoparticles(P25) coupled 100/2 h 50 Suryaman and Hasegawa (2010)
to ­bioreactorb
Trichloroethylene Adsorption using c­ laya > 95 Zhao and Vance (1998)
Photocatalysisa 100/2 h Pruden and Ollis (1983)
Biodegradation by cometabolic ­processa 98/312 d McCarty et al. (1998)
Adsorption using activated c­ arbona 0.28–1.46 83/2 wk < 12 Karanfil and Dastgheib (2004), Wilmanski and
Van Breemen (1990)
Ozone oxidation ­processa 0.38–1.4a > 95/7.5 min Peyton et al. (1982)
Ultraviolet process coupled to ozone > 95/53 s Peyton et al. (1982)
­oxidationa
Biodegradation coupled to activated c­ arbona > 0.006 82.5/48 h 3.2 Nakano et al. (2000)
Pristine multi-walled carbon n­ anotubesb 23 0.55 Ma et al. (2011)
Thermally treated multi-walled carbon 16 0.77 Ma et al. (2011)
­nanotubesb
Membranes integrated with hybrid of nickel/ 100/2 h 100 Xu and Bhattacharyya (2005)
ironb
Fenton-like degradation by hydrogen perox- 98.9/30 min 0.94 Yan et al. (2017)
ide activated with nanoscale zerovalent iron
loaded on b­ iocharb

13


Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation

13
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

Decabromodiphenyl ether Degradation using ­anaerobica 97/240 d Gerecke et al. (2006, 2005)
Ultraviolet ­processa 88/60 min Hua et al. (2003) and Shih and Wang (2009)
Nano-zerovalent iron p­ articlesb 0.1 0.1 Shih and Tai (2010)
Biochar-supported nickel/iron bimetallic 91.29/10 min 0.1 Yi et al. (2017)
­nanoparticlesb
Hexachlorocyclohexanes Degradation by anaerobic ­processa 94/102 d Quintero et al. (2005)
Adsorption using c­ arbona 1.4–3.8 98/60 min Gupta et al. (2010)
Activated ­sludgea 90/8 d Buser and Mueller (1995) and Nyholm et al.
(1992)
Reverse ­osmosisa 1.9–3.4 99/< 1 h Chian et al. (1975)
Biosorptiona 43/1 h Mac Rae (1985)
Nano-zerovalent iron p­ articlesb 0.39 0.23 Li et al. (2007)
Magnetic permanently confined micelle 70/24 h 70 Hua et al. (2003)
­arraysb
Hexachlorobenzene Hydrogen peroxide-based o­ xidationa 80/30 min Watts et al. (1994)
Silver-doped nano-zerovalent iron p­ articlesb 0.11 0.8 Xu and Zhang (2000)
Xylenes Reverse ­osmosisa 0.48–4.86c 99/< 4 h Agenson and Urase (2007)
Photocatalysisa > 90 Bahnemann (2004)
Photo-Fenton ­processa > 90 Andreozzi et al. (1999)
Degradation by anaerobic p­ rocessa > 90/10 d de Nardi et al. (2005) and Edwards et al.
(1992)
Adsorption by activated c­ arbona 0.37–5.43c > 90/200 h Voice et al. (1992)
Adsorption by ­carbona > 75/500 h Banerjee et al. (1997), Janks and Cadena
(1992) and Ranck et al. (2005)
Activated ­sludgea 0.000003–0.00003c 99/20 d Tellez et al. (2002)
Ultrafiltrationa 0.48–4.68c 54 Bilstad and Espedal (1996)
Magnetic permanently confined micelle 0.000267 15/24 h 15 Huang and Keller (2013)
­arraysb
Environmental Chemistry Letters
 Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

Rhodamine B Adsorption by ­carbona 100/5 h Gupta et al. (2004) and Jain et al. (2007)
Adsorption by activated c­ arbona 93/5 h 6–16 Jain et al. (2007) and Kadirvelu et al. (2005)
Ultrasound ­processa 76/30 min Sivakumar and Pandit (2001)
Environmental Chemistry Letters

Biosorption by anaerobic s­ ludgea 52/2 h Wang et al. (2006)

Hydrogen peroxide coupled to ultraviolet < 51/10 min Daneshvar et al. (2008)
­oxidationa
Reduced graphene oxide modified with mag- 91/2 h 13 Sun et al. (2011)
netite ­nanocompositeb
Carbon nanotubes hollow fibre ­membraneb 100 Wei et al. (2014)
Hybrid of praseodymium Pr/Titanium diox- 95/5 h 6.0 Wang et al. (2000a, b)
ide ­nanocompositeb
Hybrid of gold nanoparticles/grapheneb 100/3.5 h 40.3 Xiong et al. (2010)
Nickel oxide n­ anoparticlesb 100/1 h 2.5 Suo et al. (2013)
Hybrid of silicon dioxide/titanium dioxide 100/2.7 h 300 Ma et al. (2013)
­fibresb
Reduced graphene oxide-supported 90.0/20 min 87.72 Shi et al. (2017)
nanoscale zerovalent ­Ironb
Rhodamine 6G Fenton-like ­degradationa 52/2 h Dükkanci et al. (2010a, b)
Catalytic ­oxidationa 59/2 h Dükkanci et al. (2010a, b)
Photocatalysisa > 90/3 h Kansal et al. (2007)
Adsorption by ­carbona 0.00000077 90.5/500 min 32.6 Senturk et al. (2010)
Silver-doped zinc oxide ­nanoparticlesb 100/4 min 2.0 Georgekutty et al. (2008)
Rhodamine WT Graphene oxide nanosheet fi ­ ltersb 95 (% rejection) HouZhu et al. (2013)
a
Ethylbenzene Ultraviolet ­irradiation > 98/30 min Legrini et al. (1993)
Adsorptiona 0.55–2.04c 99/1 h Akhtar et al. (2007), Gallup et al. (1996),
Ranck et al. (2005) and Zhu et al. (1998)
Precipitation by dissolved ­aira 70/5 h Thoma et al. (1999)
Anaerobic process coupled to ­bioreactora 97/189 d Gusmão et al. (2007) and Gusmão et al. (2006)
Activated ­sludgea 4.41–11.77 99/20 d Tellez et al. (2002)
Trickle bed air ­biofiltera > 99/14 d Sorial et al. (1997)
Biodegradationa 100/14 d Morgan et al. (1993)
Magnetic permanently confined micelle 0.000058 68.1/24 h 68.1 Huang and Keller (2013)
­arraysb
Acenaphthene Magnetic permanently confined micelle 79.9/24 h Clark and Keller (2012)
­arraysb

13


Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation

13
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

Toluene Adsorption by activated c­ arbona 0.02–0.06c < 250 Wibowo et al. (2007)

Degradation-based sonolytic ­processa 55/3 h Thoma et al. (1998)
Ultraviolet-based ­photocatalysisa 100/7 h Luo and Ollis (1996)
Trickle bed b­ iofiltera 99/12 min Serial et al. (1995)
Adsorptiona <0.000004 30/4 d < 30 Ghiaci et al. (2004) and Huttenloch et al.
(2001)
Biodegradationa 92 Morgan et al. (1993) and Zeyer et al. (1986)
Magnetic permanently confined micelle 0.000076 52.6/24 h 52.6 Huang and Keller (2013)
­arraysb
Catechol Ultraviolet coupled to ozone-based oxidation > 70/1 h Li et al. (2003a, b, c, d)
­processa
Ultraviolet coupled to hydrogen peroxide 95/1 h Mandal et al. (2004)
­oxidationa
Titanium dioxide(P25) 0.001 40/2 h 29.4 Peiro et al. (2001)
p-Nitrophenol Adsorption by activated c­ arbona 0.00001–0.00002c 98.5/1 wk 500 Haydar et al. (2003)
Single-walled carbon ­nanotubesb 1.07 151.77 Moradi et al. (2011)
Single-walled carbon nanotubes-functional- 1.12 144.83 Moradi et al. (2011)
ized carboxylic g­ roupsb
Resorcinol Adsorption by activated c­ arbona > 95/24 h Kumar et al. (2003)
Electrochemical ­oxidationa 94 Rajkumar et al. (2001)
Hybrid of silver oxide/zinc oxide 100/5 h 20 Lam et al. (2013)
­nanocompositeb
Phenol Electrochemical ­oxidationa 90/8 h Comninellis and Pulgarin (1993)
Photo-Fenton ­processa 96/2 h Kavitha and Palanivelu (2004)
Ultraviolet coupled to Fenton p­ rocessa 97/2 h Kavitha and Palanivelu (2004)
Oxidationa 99/30 min Cooper and Nicell (1996)
Adsorption by ­carbona 0.00002–0.00003c 98/8 h 18.3 Mukherjee et al. (2007) and Rengaraj et al.
(2002)
Bioreactora > 90/15 h González et al. (2001)
Biodegradation by aerobic p­ rocessa 98/< 200 d Vázquez et al. (2006)
Titanium dioxide(P25)b 0.0008 60/2 h 37.6 Peiro et al. (2001)
Manganese oxide + peroxymonosulphate 100/0.33 h 62.5 Saputra et al. (2013a, b)
nanocomposite
Ruthenium oxide + peroxymonosulphate 100/0.33 h 125 Muhammad et al. (2012)
nanocomposite
Environmental Chemistry Letters
 Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

Guaiacol Photo-Fenton ­processa 60/6 h Amat et al. (2005)

Electrochemical ­oxidationa 82 Samet et al. (2006)
Titanium dioxide(P25)b 49.7 60/2 h 49.7 Peiro et al. (2001)
Environmental Chemistry Letters

Naphthalene Degradation by ultrasound ­processa 63/14 d El-Hadj et al. (2007)

Adsorption by ­carbona 0.21–19a 99/4 d <450 Ania et al. (2007), Huttenloch et al. (2001) and
Zhu et al. (1998)
Microfiltrationa 0.03–0.21a 61/12 h Campos et al. (2002)
Activated ­sludgea 61/6 h De Wever et al. (2007)
Electrochemical ­oxidationa 40 Panizza et al. (2000)
Membrane-based ­bioreactora 80 De Wever et al. (2007)
Electro-Fenton ­processa 87 Panizza and Cerisola (2001)
Ion exchange-based r­ esina 0.03–0.21a 87/7 d 20 Long et al. (2008)
Ozone ­oxidationa 0.28–1.9a 75/< 12 h Legube et al. (1986)
Single-walled carbon ­nanotubesb 2 8 Moradi et al. (2012)
Single-walled carbon nanotubes-functional- 0.81 200 Moradi et al. (2012)
ized with carboxylic ­groupsb
Magnetic permanently confined micelle 0.0048 0.82 Wang et al. (2008a)
­arraysb
Phenanthrene Adsorption by ­claya 99/30 min Ma and Zhu (2006)
Biological (wetlands)a 99.9/< 7 d Machate et al. (1997)
Ozone-based ­oxidationa 0.96–4.62c 95/4 h Masten and Davies (1997)
Degradation by anaerobic p­ rocessa 63/40 d Bernal-Martinez et al. (2007)
Magnetic permanently confined micelle 70/24 h Clark and Keller (2012)
­arraysb
Pyrene Biodegradationa 78/7 d Lei et al. (2007)
Degradation by ultrasonic ­processa 34/20 d Benabdallah El-Hadj et al. (2007)
Ozone-based oxidation p­ rocessa 1.68–36.00c 91/40 min 2–40 Corless et al. (1990) and Masten and Davies
(1997)
Magnetic permanently confined micelle 64/24 h Clark and Keller (2012)
­arraysb
Biphenyl Magnetic permanently confined micelle 0.0034 97/24 h 1.191 Legrini et al. (1993)
­arraysb

13


Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation

13
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

Methyl orange Adsorptiona > 90/400 min 47–180 Mittal et al. (2007) and Ni et al. (2007)
Electrochemical ­oxidationa 100/1 h Ma et al. (2007)
Reverse ­osmosisa > 99 Al-Bastaki (2004)
Activated ­carbona <0.0006 > 99/300 min 350–44 Chen et al. (2010)
Photocatalysis coupled to ­biodegradationa > 90/90 min Chun and Yizhong (1999)
Electro-Fenton ­processa > 80/21 h Rosales et al. (2009)
Photo-Fenton ­processa 75/1 h Devi et al. (2009)
Hybrid of titanium dioxide/tin oxide 95/12 min 38 YangLi et al. (2002)
­nanocompositeb
Hybrid of silver/Titanium dioxide 90/0.8 h 135 Yang et al. (2013)
­nanoparticlesb
Magnetic permanently confined micelle 0.00004 98/30 min 100 Huang and Keller (2013)
­arraysb
Azo dye black 24 Degradation of anaerobic ­processa 84/228 d O’Neill et al. (2000)
Degradation of aerobic/anaerobic p­ rocessesa 98/228 d O’Neill et al. (2000) and Seshadri et al. (1994)
Coagulation coupled to carbon ­adsorptiona 99.9/6 h Papić et al. (2004)
Adsorptiona 79/80 min Gupta et al. (2006)
Nano-zerovalent iron n­ anoparticlesb 0.0003 299 Shu et al. (2007a, b)
Environmental Chemistry Letters
 Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

Methylene blue Adsorptiona < 0.0033 > 99/2 h 7.5–714 Kadirvelu et al. (2003), Mohan et al. (2002),
Otero et al. (2003), Rafatullah et al. (2010)
and Yang et al. (2011)
Environmental Chemistry Letters

Electrochemical ­oxidationa > 99/2 h Panizza et al. (2007)

Activated ­carbona > 99/35 m Garg et al. (2004) and Kannan and Sundaram
(2001)
Adsorption by c­ laya 0.066 > 99.9 300 Ghosh and Bhattacharyya (2002)
Fenton ­processa 99/2 h 7.5–20.5 Dutta et al. (2001)
Electrocoagulationa 97/15 m Golder et al. (2005)
Ultrafiltrationa 94/30 m Bielska and Szymanowski (2006)
Graphene oxide ­spongeb 99/0.03 h 390 Liu et al. (2012)
Graphene oxide ­filtersb 44–46 (% rejection) Hou et al. (2013)
Amorphous ­carbonb 194 Ai and Li (2013)
Hybrid of graphene oxide/iron oxide Deng et al. (2013)
­nanocompositeb
Graphene oxide/β-cyclodextrin–chitosan/ 84 Fan et al. (2013a, b)
magnetite ­nanocompositeb
Titanium dioxide ­nanoparticlesb 100/0.75 h 50 Kim and Kwak (2007)
Titanium dioxide ­nanotubesb 87/0.67 h 174 Zhan et al. (2006)
Manganese oxide ­nanoparticlesb 90/0.08 h 68 Chen and He (2008)
Silver-doped titanium dioxide n­ anoparticlesb 90/0.67 h 135 Yang et al. (2013)
Methyl green Adsorption by polymeric ­resina 95/150 min dos Reis et al. (2011)
Multi-walled carbon nanotubes/cobalt ferrite 91.7 Farghali et al. (2013a, b)
nanoparticles functionalized with amine
groups
Multi-walled carbon nanotubes/transition 173 Farghali et al. (2013a, b)
metal-substituted cobalt ferrite nanoparti-
cles functionalized with amine groups
Methyl violet Adsorption by activated c­ arbona 99% 400 Chen et al. (2010)
Graphene oxide ­spongeb 99/0.03 h 386 Liu et al. (2011a, b)
Titanium dioxide/platinum and titanium 95, 78/20 min 0.5, 2.5 Saeed et al. (2017)
dioxide/palladium photocatalysts

13


Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation

13
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

Procion red Adsorptiona < 0.0000034 99/8 h 35–70 Calvete et al. (2009)

Photocatalysisa > 90/80 min So et al. (2002)
Degradation by anaerobic ­processa 80/3 h O’Neill et al. (2000)
Fenton ­processa 95/11.5 h Rodrigues et al. (2009)
Ultraviolet coupled to Fenton p­ rocessa > 79/20 min Ince and Tezcanh (1999) and Núñez et al.
(2007)
Fenton process coupled to b­ ioreactora 99.8/11.5 h García-Montaño et al. (2006) and Rodrigues
et al. (2009)
Wet peroxide o­ xidationa 84/15 min 310 Chen et al. (1999)
Silver-doped titanium dioxide n­ anoparticlesb 100/0.25 h 150 Yang et al. (2013)
Activated carbon–Magnetite particles com- 94/50 min 278 Hariani et al. (2018)
posite
Malachite green Adsorption by activated c­ arbona 95/2 h 92.3 Bulut et al. (2008)
Reduced graphene oxide/magnetite 94/2 h 22 Sun et al. (2011)
­nanoparticlesb
Magnetic cobalt ferrite nano-adsorbent 85/30 min 22 Vergis et al. (2018)
Orange II Coagulationa 99/30 min Xiong et al. (2001)
Electrocoagulationa > 98/360 min Daneshvar et al. (2003) and Mollah et al.
(2004)
Hydrogen peroxide-based o­ xidationa 80/60 min Peralta-Hernández et al. (2008)
Photo-Fenton ­processa 80/< 27 h Fernandez et al. (1999)
Zinc/aluminium/gold ­nanoparticlesb 100/2 h 35 Cho et al. (2012)
Direct Blue Coagulationa 80 Shi et al. (2007)
Activated ­carbona 0.00059 98/180 min 33.8 Nemr et al. (2009)
Hydrogen peroxide-based o­ xidationa 97/60 min Malik and Saha (2003)
Copper oxide ­nanoparticlesb 100/1 h 75 Aazam and Mohamed (2013)
Diuron Adsorption by ­claya < 4 Bouras et al. (2007a, b)
Biodegradation by Photo-Fenton p­ rocessa >99/2 d Farré et al. (2006)
Ozone-based ­oxidationa 0.2c 75 Ormad et al. (2008)
Chlorine-based ­oxidationa 0.07c 100 Ormad et al. (2008)
Activated ­carbona 0.14–0.21c 65 Ormad et al. (2008)
Ultraviolet ­photolysisa >99/200 min Malato et al. (2003)
Magnetic permanently confined micelle 0.0035 90/24 h 1.142 Wang et al. (2008a)
­arraysb
Environmental Chemistry Letters
 Table 7  (continued)
Contaminants Engineered nanomaterials-based methods Merit of figures Citation
Cost associated with Removal efficiency (%/time) Removal
removal efficiency ($ ability
­mg−1) (mg g−1)

Atrazine Ozone-based ­oxidationa 6.00–18.00c 99/2 h Acero et al. (2000), Hua et al. (2006), Majew-
ska-Nowak et al. (2002), Snyder et al. (2006)
and Westerhoff et al. (2005)
Environmental Chemistry Letters

Electrochemical ­oxidationa > 99.9/2 h Malpass et al. (2006)

Photo-Fenton ­processa > 98/2 h Huston and Pignatello (1999)
Adsorption by ­carbona 4.33–19.00c > 90/20 min Brown et al. (2004)
Ozonation/hydrogen ­peroxidea 99 Esplugas et al. (2007)
Fenton ­processa 75 Esplugas et al. (2007)
Ultrafiltrationa 5.67–17.00c 80 Majewska-Nowak et al. (2002)
Magnetic permanently confined micelle 0.0037 76/24 h 1.1 Wang et al. (2008a)
­arraysb
Polyethylenimine copper nanoparticles 85.94/60 min 24.8756 Kalidhasan et al. (2017)
deposited onto montmorillonite and sand
a
 Existing methods
b
 Nanotechnology-based methods
c
 Based on the cost calculations performed by the literature report (Adeleye et al. 2016)

13

Pharmaceuticals, personal care products
and endocrine‑disrupting chemicals
Literature survey on the laboratory-scale reports has dem-
onstrated that the carbon-based engineered nanomateri-
als have excellent adsorption capacity for emerging pol-
lutants such as pharmaceuticals, personal care products,
and endocrine-disrupting chemicals from natural and
spiked wastewaters (Bohdziewicz and Kamińska 2013;
Gao et al. 2012; Joseph et al. 2011a, b, 2012; Liu et al.
2014). Recently, Joseph and co-workers have designed
a combined technique, coagulation–adsorption for the
removal of endocrine-disrupting compounds using single-
walled carbon nanotubes, multi-walled carbon nanotubes,
and powdered activated carbon. It demonstrated that the
results obtained were similar to the adsorption process
alone (Joseph et al. 2013). Pharmaceuticals and personal
care products such as ibuprofen (Cho et al. 2011), car-
bamazepine (Cai and Larese-Casanova 2014), bisphenol
A (Bohdziewicz and Kamińska 2013; Joseph et al. 2013;
Joseph et al. 2011a, b), ciprofloxacin (Liu et al. 2014),
doxycycline hydrochloride (Gao et al. 2012), triclosan
(Cho et  al. 2011), tetrabromobisphenol A (Zhou et  al.
2012), oxytetracycline (Gao et al. 2012; Oleszczuk et al.
2009), and norfloxacin(Yang et al. 2012) were removed
using carbon-based engineered nanomaterials from syn-
thetic and natural wastewaters (Joseph et al. 2011b; Kumar
and Mohan 2012). The adsorption process using carbon-
based engineered nanomaterials is mainly dependent on
the physicochemical properties such as water–octanol par-
titioning (Heo et al. 2012; Joseph et al. 2011a), aromaticity
(Gao et al. 2012), natural organic matter (Cho et al. 2011;
Joseph et al. 2011a, b), and adsorbate concentration for
the removal of endocrine-disrupting compounds. In the
literature, very few reports are available on the evalua-
tion of metal/metal oxide engineered nanomaterials as a
remediation method for the removal of pharmaceuticals,
personal care products, and endocrine-disrupting com-
pounds. Nevertheless, even though nano-zerovalent iron
has not been extensively used for the removal of pharma-
ceuticals and personal care products, some studies have
demonstrated the oxidation ability of this nanomaterial for
metronidazole (Fang et al. 2010), amoxicillin, ampicillin
(Ghauch et al. 2009), and ibuprofen (Machado et al. 2013)
from industrial wastewaters. The generation of hydrogen
and electron species from nano-zerovalent iron could be
accountable for the degradation of pharmaceuticals and
personal care products (FangQiu et al. 2010). It was found
that pharmaceuticals and personal care products are very
difficult to undergo degradation. Therefore, it is desirable
to use two methods concurrently, for example, biodegrada-
tion by a functional microorganism (Bokare et al. 2010)
13
Environmental Chemistry Letters
and Fenton chemistry with nano-zerovalent iron/hydrogen
peroxide (Shirazi et al. 2013) for the removal of pollutants.
In another study, pharmaceuticals and personal care prod-
ucts such as succinic acid, gemfibrozil, sulfamethoxazole,
L-3, 4-dihydroxyphenylalanine, D-gluconic, and ateno-
lol were removed by using magnetic permanently con-
fined micelle arrays (Huang and Keller 2013; Wang et al.
2008b). The adsorption and removal mechanism included
hydrogen bonding, hydrophobic and electrostatic forces of
interactions. Additionally, cetyltrimethylammonium bro-
mide modified with iron oxide engineered nanomaterials
has also demonstrated excellent adsorption properties for
bisphenol A (Zhao et al. 2008b).
Performance and cost evaluation between existing
methods and nanomaterial‑based methods
The most commonly used technologies are reverse osmosis
and ozonation for the removal of some of the persistent and
emerging contaminants which are discussed in Table 3. It
was found that 70–99% removal efficiency of emerging con-
taminants was observed with these two technologies; how-
ever, more than 90% removal efficiency was achieved with
Fenton/hydrogen peroxide method. The current technolo-
gies such as membrane bioreactor, UV radiation, activated
sludge, biological treatment, and solid-phase extraction sor-
bents have demonstrated that some effect on the removal
efficiency was obtained within reasonable cost. Surprisingly,
it was found that carbon-based engineered nanomaterials
and magnetic permanently confined micelle arrays are the
most extensively used methods for the treatment of emerg-
ing pollutants with maximum removal capacity compared
to the existing methods. By using carbon-based engineered
nanomaterials, it was found that more than 300 mg g−1 of
doxycycline and tetracycline was removed from the waste-
waters. Finally, it was concluded that carbon-based engi-
neered nanomaterials are cost-effective for the removal of
pharmaceuticals and personal care products and endocrine-
disrupting compounds.
Nanomaterial‑enabled wastewater
techniques for inorganic pollutants
Several reports are available on the adsorption of heavy
metals with carbon-based engineered nanomaterials (Gong
et al. 2011; Gupta et al. 2010; Rao et al. 2007; Tofighy and
Mohammadi 2011; Wang et al. 2013a, b; Xiao et al. 2012).
It was found that the adsorption ability of pristine carbon
nanotubes for metals is low; however, it may be enhanced
significantly by functionalization (Hadavifar et al. 2014; Li
et al. 2003a, b, c, d; Yu et al. 2013). After functionalization
of carbon nanotubes, a greater number of nitrogen, oxygen,
Environmental Chemistry Letters
or other groups are observed on the surface, resulting in
the enhanced dispersibility of nanomaterials, thus leading
to a higher surface area (Adeleye and Keller 2014; Li et al.
2002). Recent advancement in designing carbon-based nano-
composites has led to the hybridization of other metals into
the nanocomposites that have desired features. For example,
incorporation of iron oxide nanoparticles onto carbon-based
nanocomposites has facilitated an easy and cost-effective
method for the removal of metal ions through an applied
external magnetic field (Deng et al. 2013; Tang et al. 2012;
Zheng et al. 2012). Doping of organic molecules or metals
into carbon-based engineered nanomaterials could enhance
the selective adsorption ability for specific metallic contami-
nants (Chandra et al. 2010; Fan et al. 2013a, b; Zhou et al.
2014). On the other hand, graphene sheet-based membranes
have also been used as a filtration tool for metal ions to
some extent (Sun et al. 2012). In general, adsorption is the
only method that can be used frequently using metal/metal
oxide nanomaterials in the treatment of organic and inor-
ganic pollutants. For example, modification of zirconium
oxide engineered nanomaterials with commercially available
cation exchange resin (D-001) resulted in a 13-fold increase
in the adsorption and selectivity for cadmium (II) and lead
(II) from mining acidic effluent, compared to the unmodi-
fied resin (Hua et al. 2013). These nanocomposite resins
can also be easily recovered and reused after the wastewater
treatment process.
In another report, granular activated carbon was modified
with iron oxide and manganese oxide for the removal of cad-
mium (II) from wastewaters, resulting in a slight enhance-
ment in the adsorption ability; however, the result obtained
was similar. In this study, the granular activated carbon was
prepared from rice hulls or areca nuts (Lee et al. 2013).
Interestingly, it was noted that at low pH, nano-zerovalent
iron gains a positively charged surface which is facilitated
in the removal of dichromate ions (YangFu et al. 2013),
whereas at high pH, it contributes to the removal of heavy
metals (Boparai et al. 2013; Su et al. 2014) due to nega-
tively charged surface. After adsorption, metals with stand-
ard potentials (Eo) such as nickel (II), copper (II), lead (II),
and silver (I) undergo reduction, due to their more positivity
than iron (Li and Zhang 2007). The nano-zerovalent iron has
high removal ability for metal ions with minimal generation
of solid waste; therefore, this material is environmentally
friendly and an ideal contender for the wastewater treatment.
Apart from these materials, various other metal/metal oxide
engineered nanomaterials have been reported in the litera-
ture for removal of metal ions from aqueous solutions (Lee
et al. 2012; Maliyekkal et al. 2010; Zhu et al. 2007).
Recent studies have suggested that magnetic nanoparti-
cles have been used for the removal of cadmium (II) (Ghe-
bremeskel and Bose 2002), mercury (II) (Hadavifar et al.
2014; Pacheco et al. 2006), and some other toxic metal ions
(Bhaumik et al. 2011; Bystrzejewski et al. 2009; Chen et al.
2011b; Faulconer et al. 2012; Ghebremeskel and Bose 2002;
Huang et al. 2012; Larraza et al. 2012; Liu et al. 2011b;
Sprynskyy et al. 2012; Towler et al. 1996) from wastewaters.
Functionalization of magnetic nanoparticles with dithiocar-
bamates has been applied to eliminate mercury (II) from
wastewaters (Girginova et al. 2010). It demonstrated that
selective and sensitive removal of arsenic (III) was per-
formed with magnetite nanoparticles coated with manganese
oxide (Silva et al. 2012). The resultant magnetic adsorbent
exhibited excellent chemical and physical stability over the
pH range of 3.0 to 9.0. The lead (II) and copper (II) ions
are removed from the wastewaters, and porous manganese
ferrospinel was used as a reusable, effective, and selective
material (Ren et al. 2012; Su et al. 2014). The regeneration
process was performed by using 0.2 M hydrochloric acid as
an eluent. The magnetic nanoparticles functionalized with
ethylenediaminetetraacetic acid were used to remove a wide
range of metallic ions such as lead (II) and cadmium (II)
from aqueous solutions (Huang and Keller 2015).
Performance and cost evaluation of existing
methods and nanomaterial‑based methods
The conventional methods such as sulphide precipitation,
ion-exchange, pH alteration, and coagulation are commonly
used for the removal of heavy toxic metals from wastewaters.
Coagulation, sulphide precipitation, and pH adjustment
are frequently used methods in the treatment of industrial
wastewater due to their reasonable operational cost, although
the ion-exchange method was applied to treat drinking water
effectively with a higher estimated cost. The generation of a
large quantity of heavy metal solid waste after the wastewa-
ter treatment process from these methods resulted in addi-
tional cost implications and was one of the main drawbacks.
Furthermore, nanomaterials such as magnetic, metal/metal
oxide engineered, and nano-zerovalent iron nanomaterials
can produce less solid waste due to higher adsorption capaci-
ties. The nano-zerovalent iron and their derivatives includ-
ing magnetic particles have gained significant attention and
exhibited viability for the treatment of toxic heavy metals in
different aquatic systems and soil samples.
It was concluded that the effect of interference is greatly
minimized in the case of real sample analysis by using nano-
zerovalent iron. Based on the literature results presented
in Table 8, nano-zerovalent iron becomes a cost-effective
nanoadsorbent to treat wastewaters for heavy metals in
the future. The estimated operational cost of carbon-based
engineered nanomaterials is less with greater adsorption
abilities compared to other nanomaterials and conventional
techniques.
Adsorption process was adopted to remove fluo-
ride ions (Gupta et  al. 2009; Li et  al. 2003a, b, c, d;
13


Table 8  Performance and cost for various treatment technologies for heavy metals
Contaminants Engineered nanomaterials/methods Merit of figures Citation
−1

13
Cost associated with Removal Removal ability (mg g­ )
removal efficiency ($ efficiency (%/
­mg−1) time)

Chromium Fly ash–lime p­ recipitationa 99/10 min Chen et al. (2009a, b)

Biosorption (various biomass sources)a 2–230 Singh et al. (2011)
Ultrafiltrationa 0.0001–0.34a < 100 Fu and Wang (2011) and Kurniawan et al. (2006)
Ion ­exchangea 0.00002–0.04a 100 10–40 Kurniawan et al. (2006)
Activated carbon ­adsorbentsa 0.0001–0.38a 150–170 Kurniawan et al. (2006)
Chemically modified plant a­ dsorbentsa 1.7–28 Wan Ngah and Hanafiah (2008)
Chemical ­precipitationa > 99 Fu and Wang (2011)
Graphene oxide/polypyrroleb 500 Li et al. (2012a, b)
Cerium oxide c­ ompositeb 60/5 h 5.9 Zhong et al. (2007)
Nano-zerovalent ­ironb 73–110 Li et al. (2007)
Polypyrrole-coated magnetite p­ articlesb 170 Bhaumik et al. (2011)
Zinc Fly ash–Lime ­precipitationa 97/10 min Chen et al. (2009a, b)
Biosorption (various biomass sources)a 0.2–641 Singh et al. (2011)
Chemical ­precipitationa 99.7 45 Fu and Wang (2011) and Kurniawan et al. (2006)
Coagulation ­flocculationa 99.9 45 Kurniawan et al. (2006)
Reverse ­osmosisa 0.0002–0.003c 99 Fu and Wang (2011) and Kurniawan et al. (2006)
Ion ­exchangea 0.00002–0.0003c 100 10–40 Fu and Wang (2011) and Kurniawan et al. (2006)
Activated carbon ­adsorptiona 0.0001–0.003c 63.2–103 Kurniawan et al. (2006)
Chemically modified plant a­ dsorbentsa 0.18–83.3 Wan Ngah and Hanafiah (2008)
Ultrafiltrationa 0.0002–0.003c 99 Fu and Wang (2011)
Nano-zerovalent ­ironb 0.000229 393 Yan et al. (2010a, b)
Environmental Chemistry Letters
 Table 8  (continued)
Contaminants Engineered nanomaterials/methods Merit of figures Citation
−1
Cost associated with Removal Removal ability (mg g­ )
removal efficiency ($ efficiency (%/
­mg−1) time)

Lead Recycled alum sludge c­ oagulationa 98 166–300 Chu (1999)

Cetyltrimethylammonium bromide carbon 98/180 min 6–9 Nadeem et al. (2006)
­adsorbenta
Environmental Chemistry Letters

Fly ash–lime p­ recipitationa 98/10 min Chen et al. (2009a, b)

Biosorption (various biomass sources)a 2–770 Singh et al. (2011)
Chemically modified plant a­ dsorbentsa 4.5–310 Wan Ngah and Hanafiah (2008)
Chemical ­precipitationa 99.6 Fu and Wang (2011)
Ion exchange ­resina 0.001–0.02a > 55 0.21–1.4 Fu and Wang (2011)
a
Ultrafiltration 0.001–0.17a > 99 Fu and Wang (2011)
b
Multi-walled carbon nanotubes/magnetite p­ articles 42 Hu et al. (2011) and Ji et al. (2012)
Multi-walled carbon nanotubes/magnetite particles 75 Ji et al. (2012)
functionalized with amine ­groupb
Multi-walled carbon nanotubes/cobalt ferrite func- 66 Zhou et al. (2014)
tionalized with amine g­ roupb
Multi-walled carbon nanotubes/cobalt ferrite func- 140 Zhou et al. (2014)
tionalized with amine group/chitosanb
Graphene oxide/chitosan/magnetiteb 77 Fan et al. (2013a)
Manganese spinel ferrite n­ anoparticlesb 69 Ren et al. (2012)
Mag-ligandb > 98/15 min 100 Huang and Keller (2015)
Zirconium oxide ­nanoparticlesb 25/1.7 h 320 Hua et al. (2013)
Nano-zerovalent ­ironb 0.00005 1667 Zhang et al. (2013a, b)
a
Cobalt Biosorption (various biomass sources) 2.4–156 Singh et al. (2011)
Ion exchange ­resina 100 60–75 Rengaraj and Moon (2002)
Ultrafiltrationa 100 Kurniawan et al. (2006)
Bentonite/iron oxide magnetic c­ ompositesb 22.73 ChenHuang et al. (2011)
Nano-zerovalent ­ironb 172 Uzum et al. (2008)

13


Table 8  (continued)
Contaminants Engineered nanomaterials/methods Merit of figures Citation
−1

13
Cost associated with Removal Removal ability (mg g­ )
removal efficiency ($ efficiency (%/
­mg−1) time)

Cadmium Biosorption (various biomass sources)a 3.4–220 Singh et al. (2011)

Chemical ­precipitationa 99.6/24 h 15 Kurniawan et al. (2006)
Coagulation ­flocculationa 99.7 15 Kurniawan et al. (2006)
Reverse ­osmosisa 0.002–0.85a 99 Kurniawan et al. (2006)
Ion ­exchangea 0.0003–0.1a 100 10–40 Fu and Wang (2011) and Kurniawan et al. (2006)
Activated ­carbona 0.002–0.95a 146 Kurniawan et al. (2006)
Chemically modified plant waste ­adsorbentsa 4.5–310 Wan Ngah and Hanafiah (2008)
Ultrafiltrationa 0.002–0.85a 99 Fu and Wang (2011)
Oxygen-functionalized multi-walled carbon 0.57 22 Vuković et al. (2010)
­nanotubesb
Multi-walled carbon nanotubes–ethylenediamineb 22 Vuković et al. (2010)
Graphene oxide/iron ­oxideb 91 Deng et al. (2013)
Zirconium dioxide n­ anoparticlesb 30/1.7 h 215 Hua et al. (2013)
Nano-zerovalent ­ironb 0.0014 67 Zhang et al. (2014a, b, c)
ZEAa 85 Sprynskyy et al. (2012)
Mag-ligandb > 98/2 h 79 Huang and Keller (2015)
Zinc oxide ­nanoparticlesb 90/30 min 217.4 Khezamia et al. (2017)
Nickel Biosorption (various biomass sources)a 0.8–30 Singh et al. (2011)
Chemical ­precipitationa 71/1 h Kurniawan et al. (2006)
Reverse ­osmosisa 0.0002–0.17c 100 Fu and Wang (2011) and Kurniawan et al. (2006)
Ion ­exchangea 0.00002–0.02c 100 10–40 Kurniawan et al. (2006)
Activated carbon ­adsorbentsa 0.0001–0.19c 80.9–160 Kurniawan et al. (2006)
Chemically modified plant waste ­adsorbentsa 3.37–62.5 Fu and Wang (2011) and Wan Ngah and Hanafiah
(2008)
Ultrafiltrationa 0.0002–0.17c 100 Kurniawan et al. (2006)
ZEAa 67.35  Sprynskyy et al. (2012)
Nano-zerovalent ­ironb 80 Efecan et al. (2009)
Environmental Chemistry Letters
 Table 8  (continued)
Contaminants Engineered nanomaterials/methods Merit of figures Citation
−1
Cost associated with Removal Removal ability (mg g­ )
removal efficiency ($ efficiency (%/
­mg−1) time)

Copper Fly ash–lime p­ recipitationa 99/10 min Chen et al. (2009a, b)

Biosorption (various biomass sources)a 0.4–380 Singh et al. (2011)
Chemical ­precipitationa 100/24 h Fu and Wang (2011) and Kurniawan et al. (2006)
Environmental Chemistry Letters

Coagulation ­flocculationa 99.6 0.8–4 Kurniawan et al. (2006)

Reverse ­osmosisa 0.001–0.03a 100 Kurniawan et al. (2006)
Ion ­exchangea 0.0001–0.004a 100 10–40 Kurniawan et al. (2006)
Activated carbon ­adsorbentsa 0.0005–0.04a 83–150 Kurniawan et al. (2006)
Chemically modified plant waste ­adsorbentsa 0.15–140 Wan Ngah and Hanafiah (2008)
Ultrafiltrationa 0.001–0.03a 99.7 Fu and Wang (2011)
Multi-walled carbon nanotubes Magnetite p­ articlesb 39 Hao et al. (2012) and Hu et al. (2011)
Nano-zerovalent ­ironb 0.00026 340 Zhang et al. (2014a, b, c)
Manganese spinel ferrite n­ anoparticlesb 61 Ren et al. (2012)
ZEAa 96 120 Sprynskyy et al. (2012)
Mercury Biosorption (various biomass sources)a 290 Singh et al. (2011)
Chemically modified plant waste ­adsorbentsa 150 Wan Ngah and Hanafiah (2008)
Chemical ­precipitationa > 99.9 Fu and Wang (2011)
Magnetite/silicon dioxide p­ articlesb 50 17 Girginova et al. (2010)
Magnetite/silicon dioxide particles functionalized 74 25 Girginova et al. (2010)
with amine and sodium salt of carbon ­disulphideb
Nano-zerovalent ­ironb 80 Yan et al. (2010a, b)

13


Table 8  (continued)
Contaminants Engineered nanomaterials/methods Merit of figures Citation
−1

13
Cost associated with Removal Removal ability (mg g­ )
removal efficiency ($ efficiency (%/
­mg−1) time)

Arsenic Chemical ­oxidationa < 80 Ning (2002)

Alum ­coagulationa 95/< 2 min 1.8–10 Kang et al. (2003) and Kartinen Jr and Martin (1995)
Iron ­coagulationa 99/20 min 17–50 Baskan and Pala (2009), Hering et al. (1997),
Kartinen Jr and Martin (1995), Song et al. (2006)
Ion exchange ­resina 0.001–0.07a 98/12 h 66–2500 An et al. (2005), Kartinen Jr and Martin (1995) and
Ruixia et al. (2002)
Reverse ­osmosisa 0.001–0.57a > 95 Gholami et al. (2006), Kartinen Jr and Martin (1995),
Shih (2005), Van der Bruggen and Vandecasteele
(2003)
Alum ­precipitationa > 90 10 Kartinen Jr and Martin (1995)
Ozone ­oxidationa 0.001–0.6a 96/4 min 15 Kim and Nriagu (2000)
Multi-walled carbon nanotubes/magnetite p­ articlesb As(III) = 1.7, As(V) = 0.2 Addo Ntim and Mitra (2011)
Grafting of multi-walled carbon nanotubes with As(V) = 18 Veličković et al. (2012)
ethylenediamine and iron (II) p­ articlesb
Grafting of multi-walled carbon nanotubes with As(V) = 11 Velickovic et al. (2012)
ethylenediamine and iron (III) p­ articlesb
Multi-walled carbon nanotubes/zirconium dioxide As(III) = 3, As(V) = 5 Ntim and Mitra (2012)
­nanocompositeb
Reduced graphene oxide/magnetite ­nanocompositeb As (III) = 13, As(V) = 5.8 Chandra et al. (2010)
Graphene oxide/zirconia dioxide ­nanocompositeb As(III) = 95, As(V) = 85 LuoWang et al. (2013a, b)
Reduced graphene oxide/nano-zerovalent ­ironb As(III) = 36, As(V) = 29 Wang et al. (2014a, b, c, d)
Cerium oxide n­ anoparticlesb 100/1.2 h 14 Zhong et al. (2007)
Mixed manganese/aluminium oxide ­nanocompositeb 65/5 h 140 Wu et al. (2012)
Nano-zerovalent iron with air and carbon d­ ioxideb 0.00078 130 Tanboonchuy et al. (2011)
Sulphate Anaerobic biological ­removala < 99/8 d Genschow et al. (1996), Pol et al. (1998) and Silva
et al. (2002)
Activated ­carbona < 0.000003c 99/140 h Zhao et al. (2008a, b)
Ion exchange ­resina < 0.0000003c > 99/150 m 100 mg/ml Haghsheno et al. (2009)
Magnetic permanently confined micelle ­arraysb 75.7 Clark and Keller (2012)
Environmental Chemistry Letters
 Table 8  (continued)
Contaminants Engineered nanomaterials/methods Merit of figures Citation
−1
Cost associated with Removal Removal ability (mg g­ )
removal efficiency ($ efficiency (%/
­mg−1) time)

Nitrate Electrocoagulationa > 0.00000012 > 90/150 min Koparal and Öğütveren (2002)

Chemical ­denitrificationa < 100 Bhatnagar and Sillanpää (2011)
Biological ­denitrificationa 0.000003–0.02a > 99/3.5 h Bhatnagar and Sillanpää (2011), Reyes-Avila et al.
Environmental Chemistry Letters

(2004) and Schoeman and Steyn (2003)

Ion exchange ­resina 0.0000001–0.001a 100/12 h 14–82 Bhatnagar and Sillanpää (2011), Clifford and Liu
(1993) and Schoeman and Steyn (2003)
Reverse ­osmosisa 0.000001–0.01a > 95 Bhatnagar and Sillanpää (2011), Bohdziewicz et al.
(1999) and Phenrat et al. (2010)
Carbon ­adsorptiona 0.000001–0.01a 97/45 min 1–100 Bhatnagar and Sillanpää (2011) and Öztürk and
Bektaş (2004)
Carbon ­nanosheetsb 0.088 140 Tofighy and Mohammadi (2012)
Magnetic permanently confined micelle ­arraysb 100 Clark and Keller (2012)
Perchlorate Biological ­treatmenta 0.0000263 > 87/35 h Coates et al. (1999), Gu et al. (2007), Hatzinger
(2005), Matos et al. (2006), Srinivasan and Sorial
(2009) and Wallace et al. (1996)
Ion exchange ­resina < 0.00001c > 99/8.3 h
b
Magnetic permanently confined micelle ­arrays 98.8 Clark and Keller (2012)
Phosphate Ion exchange ­resina 0.0000039–0.0000044a 99/5 min Ruixia et al. (2002) and Zhao and Sengupta (1998)
a
Carbon ­adsorption 0.00003–0.00004a > 99 2.5–1150 Sakadevan and Bavor (1998)
a
Biological ­removal > 68/360 min Chen et al. (2004)
Electrocoagulationa > 80/20 min Bektaş et al. (2004)
Activated ­sludgea 94/65 d De Kreuk et al.( 2005)
Magnetic permanently confined micelle ­arraysb 95.7 Clark and Keller (2012)
Mixed manganese/aluminium oxide ­nanocompositeb 100/5 h 60 WuLiu et al. (2014)
Zirconium dioxide/graphene oxide ­nanocompositeb 18 Zong et al. (2013)
Zirconium-modified magnesium–aluminium lay- 60/2 d 30 Chitrakar et al. (2010)
ered double ­hydroxideb
a
 Existing methods
b
 Nanotechnology-based methods
c
 Based on the cost calculations performed by the literature report (Adeleye et al. 2016)

13

Ramamurthy et  al. 2011) and other nutrients such as
ammonium and nitrates (Moradi et al. 2012; Tofighy and
Mohammadi 2012) from different water systems using
graphene oxide, carbon nanotubes, and web-like cellu-
lose nanofibres. It was found that the adsorption capacity
of carbon nanotubes sheets for nitrates was higher with
shorter equilibrium time and improved regeneration abil-
ity compared to commercially available activated carbon
(Tofighy and Mohammadi 2012). If the estimated operat-
ing cost of the carbon-based nanomaterials reduces sig-
nificantly, this technology could be considered as prom-
ising to minimize the nutrient content of industrial and
agricultural wastewaters. In addition, carbon-based engi-
neered nanomaterials have shown to be a good adsorbent
for the removal of arsenic from wastewaters (Luo et al.
2013). Studies have been performed on the simultaneous
adsorption of arsenic (0), arsenic (II), and arsenic (V)
on to the surface of nano-zerovalent iron, indicating that
along with adsorption, both reduction and oxidation of
arsenic occurred through nano-zerovalent iron treatment
(Mauricio 2010; Ramos et  al. 2009). Additionally, by
considering the stability of arsenic (III), arsenic (V), and
complexes of iron oxide, nano-zerovalent iron can be con-
sidered as an effective nanomaterial for in situ removal of
arsenic from polluted sites.
Though nano-zerovalent iron has been considered as
an in situ method for the removal of nitrates (Jiang et al.
2011; Kassaee et al. 2011; Ryu et al. 2011; Sohn et al.
2006), the production of ammonium as a by-product indi-
cated that additional treatment is necessary to complete
remediation process (Ryu et al. 2011; Sohn et al. 2006).
Different literature reports have examined the signifi-
cance of various metal/metal oxide engineered nanoma-
terials such as zirconium oxide-modified graphite oxide
(Zong et  al. 2013), zirconium-coated magnesium-iron
double-layered hydroxide carbonates (Chitrakar et  al.
2010), and manganese-doped aluminium-based bimetal-
lic oxides (Wu et al. 2014) for the removal of phosphates
and other nonmetals from aquatic systems. The removal
of arsenic (III) (Silva et al. 2012), boron (Tural 2010), and
phosphate (Sarkar et al. 2010) was successfully achieved
by using magnetic nanoparticles. Most of the common
oxyanions were removed effectively with magnetic
permanently confined micelle arrays from wastewaters
(Clark and Keller 2012). It demonstrated that high free
energy was found with magnetic permanently confined
micelle arrays during adsorption of sulphates and phos-
phates, nitrates, and perchlorates (Clark and Keller 2012).
Interestingly, the competitive investigation revealed that
sulphates and phosphates, nitrates, and perchlorates did
not target for similar binding sites, suggesting different
interaction mechanisms.
13
Environmental Chemistry Letters
Performance and cost evaluation of existing
methods and nanomaterial‑based methods
Several engineered nanomaterials-based technologies have
been used effectively to treat wastewater for phosphatase
and arsenic. For example, carbon-based engineered nano-
materials and metal/metal oxide engineered nanomaterials
were used for the removal of arsenic. Magnetic nanoparticles
and metal/metal oxide engineered nanomaterials were suc-
cessfully used for the effective removal of phosphate from
wastewater.
Literature suggests that conventional treatment meth-
ods are available and found to be effective up to 99% in
terms of adsorption efficiency and estimated operational
cost. Furthermore, metal oxide nanomaterials seem to be
the alternate technology for the removal of phosphatase and
arsenic. However, the treatment time to a comparable per-
centage removal is generally longer than for conventional
technologies. It should be noted that the removal percentages
vary extensively by treatment technology, which makes them
difficult to compare over other treatment methods. In the
case of carbon-based engineered nanomaterials, the removal
abilities vary widely, suggesting their superiority and suit-
ability in wastewater treatment over conventional methods.
Though nanomaterials offer an effective substitute for the
treatment of inorganic nonmetals, the selection of nanoma-
terials should be done carefully depending on the type of
pollutants. Literature survey results were created in the form
of database and are presented in Table 8.
Overview of performance and cost
of nanotechnology methods
For the treatment of several contaminants, nanotechnol-
ogy-based methods are found to be a reliable and practical
option. These technologies are effective compared to con-
ventional methods due to their unique features such as low
sludge generation, quicker treatment, or processes associated
with a broader range of interaction mechanisms. It was found
that metal and metal oxide nanoparticles are considered to
be effective for the removal of halogenated, non-halogenated
organic pollutants and comparable to the existing technol-
ogy (activated carbon-based adsorption). The estimation of
operational costs of the technologies varies, depending on
the treatment process, analytes, and nanomaterials. But in
some cases, the costs can be comparable. For example, costs
related to the removal of chromium, cadmium, zinc and tolu-
ene, xylene with nano-zerovalent iron, and magnetic perma-
nently confined micelle arrays, respectively, are comparable
with existing technologies, whereas in some cases, current
nanotechnology-related methods for the removal of chlo-
ramphenicol, arsenic, lindane, trichloroethylene, lead and
Environmental Chemistry Letters
methyl orange, gemfibrozil, 2-chlorophenol, ethylbenzene,
naphthalene, atrazine, atenolol, diuron with nano-zerovalent
iron, and magnetic permanently confined micelle arrays,
respectively, are less expensive compared to the existing
technologies.
In the literature, current technologies such as reverse
osmosis and ozonation are found to be more expensive than
existing nanotechnology techniques (magnetic nanoparticles
and carbon-based engineered nanomaterials) for emerging
contaminants in terms of removal efficiency.
Furthermore, magnetic permanently confined micelle
arrays and nano-zerovalent iron technologies are less expen-
sive, compared to those of current methods in treating waste-
waters for chloramphenicol, atenolol, and gemfibrozil. In the
treatment of heavy metals with current technologies (metal
oxide nanoparticles and nano-zerovalent iron), the produc-
tion of a significant amount of solid waste increases opera-
tional cost compared to the other nanotechnology-related
methods (see Table 4). Depending on the concentration of
metal ions present in the water samples, the operational cost
of the nanotechnology becomes cheaper to treat wastewaters
for zinc (II), lead (II), and copper (II).
Moreover, the treatment of inorganic nonmetals is feasi-
ble using different existing nanotechnologies. Though very
few reports are available on the nano-based treatments with
major conclusions, effectiveness of the method depends on
the analyte.
Interestingly, it was found that nano-zerovalent iron for
arsenic seems to be less expensive than the most existing
methods, but in the case of nitrates, current methods are
highly economical compared to the carbon-based nanomate-
rials. The overall cost of current treatments mainly depends
on the chemicals costs, initial capital costs, operations and
maintenance costs. For example, adsorption based on the
granular activated carbon appears to be the most commonly
used option and greatly relies on the source of carbon, cost,
and frequency of regeneration (Behnam et al. 2013; Cai
and Larese-Casanova 2014; Gupta et al. 2009). It should
be noted that based on the type of pollutants removed, the
activated carbon treatment method may not be a cost-effec-
tive choice compared to other methods. Depending on the
extent of oxidation required, it is also an expensive method
of treating a wide range of pollutants ranging from organic
compounds to inorganic metals and nonmetals. Though a
biological treatment method is not effective for all contami-
nants, it was found to be less expensive and requires very
low operational costs with minimal maintenance. Depending
on the size of the wastewater treatment plant, the estimated
investment cost for existing methods was found to be US$90/
m3 and US$2800/m3 per day for 3000 and 5 m3 treatment
plant, respectively. From this study, it was demonstrated
that the larger treatment plants have lower operational costs
(Legrini et al. 1993; Martinez-Huitle and Ferro 2006).
The price of carbon-based engineered nanomaterials
differs broadly depending on the type of nanomaterials
(graphene, carbon nanotubes, amorphous carbon nanoma-
terials), grade and level of purity (wt%), and functionali-
zation of nanomaterials. The price of single-walled carbon
nanotubes, multi-walled carbon nanotubes, and graphene-
based derivatives is found to be ranging from US$25–300/g,
US$0.10–25/g, and US$2.50–1000/g, respectively (Cheap-
TubesInc. 2017).
For example, the adsorption and removal of lead (II) from
wastewaters by single-walled carbon nanotubes could cost
roughly US$2.2/g-Pb with an average adsorption ability of
75 mg lead (II)/g-single-walled carbon nanotube. In this
study, the cost of single-walled carbon nanotubes is only
considered. Furthermore, the overall estimated cost of the
treatment process may be decreased by various features
since carbon-based engineered nanomaterials may be eas-
ily recoverable and reusable over many cycles (Bandaru
et al. 2013; Hadavifar et al. 2014; Zhang et al. 2014a, b,
c). In general, carbon nanotubes are comparatively more
expensive than most of the other nanomaterials for waste-
water treatment. However, high stability and easy recovery
of carbon nanotubes are some of the advantages compared
to other nanomaterials (Qu et al. 2013a; b, c; Zhang et al.
2014a, b, c). It is necessary to consider the toxicity of engi-
neered nanomaterials in future work. For example, nano-
zerovalent iron is highly reactive in laboratory tests; how-
ever, larger amounts of nano-zerovalent iron are required to
treat natural waters due to the presence of other unwanted
components. Additionally, the estimated production cost
of nano-zerovalent iron is relatively more expensive due to
the use of borohydride (reducing agent) to reduce iron to
nano-zerovalent iron. It is found that the manufacturing of
borohydride is highly expensive compared to that of other
reagents or reducing agents.
The advancement in nanotechnology resulted in the
reduction of production cost; however, it was found to be
US$0.05–0.10/g (Crane and Scott 2012). Some metal/metal
oxide engineering nanomaterials are commercially produced
and highly useful in wastewater treatment plants; however,
titanium dioxide has distinguished properties with limited
applications. It is found that the production cost of some
nanomaterials/techniques is not accessible in the literature
as most remain largely at the patenting stage. Due to the
wide range of applications, the estimated production cost
of titanium dioxide nanoparticles ranges from US$0.16/g to
1.21/g (Lu et al. 2011), whereas the approximate wastewater
treatment cost per gram of pollutant ranges from US$0.50
to US$1.00/g (Sigma–Aldrich 2018; US Research Nanoma-
terials 2018).
Titanium is an inexpensive element and is most abun-
dantly available in the earth’s crust (Barksdale 1949).
Despite the adequate investment on some metal/metal
13

oxide engineered nanomaterials, it may not reach the esti-
mated production cost, similar to that of titanium dioxide
nanoparticles (Yang et al. 2002). It is noted that titanium
dioxide nanoparticles do not produce oxidizing radicals dur-
ing photodegradation; hence, they have really been listed
under quickly regenerated and reused materials. Therefore,
the overall treatment cost decreases with using metal/metal
oxide engineered nanomaterials. As the technology and pro-
duction of magnetic core increases, the actual cost of these
nanoparticles has been gradually reducing. Interestingly, it
was found that there was a huge cost difference between
laboratory- and industrial-scale production of magnetic per-
manently confined micelle arrays. For example, manufac-
turing of magnetic permanently confined micelle arrays in
a laboratory scale costs approximately US$70/kg, whereas
US$4/kg to produce industrially (Huang and Keller 2013).
This material is easy to regenerate and reuse after treatment,
resulting in the decrease of additional cost associated with
the technique (Clark and Keller 2012; Wang et al. 2008a,
2011b).
Conclusion
Presently, there is a reasonable need to establish innova-
tive water treatment technologies to remove biological and
chemical contaminants from wastewater and to safeguard
high water quality. In this aspect, nanotechnology is one
of the perfect options for nanomaterials-based wastewater
treatment processes. Most of the conventional water treat-
ment methods are not cost-effective for the removal of com-
mon contaminants at low concentrations. It is noteworthy
that many of these methods have some limitations and may
be incapable of meeting the growing rigorous water qual-
ity standards. Additionally, traditional treatment methods
are frequently consuming higher amounts of energy while
emitting huge amounts of solid and toxic waste into the
environment.
With the increase in opportunities in wastewater treat-
ment, it is highly necessary to have specialized methods
where nanotechnology can fill in the gaps when traditional
methods are either slightly effective or non-realistic. The
effectiveness of several nanomaterial-based technologies can
be increased through the modification of nanoparticles in
contrast to conventional methods. Hence, their cost may be
decreased by bulk scale production. The most extensively
reported metal/metal oxide engineered nanomaterials are
emphasized in this review, along with their applications in
wastewater treatment. In view of the recent research and
development in nanotechnology, nanomaterials seem to be
a perfect tool to meet the present and rising clean water
demands worldwide.
13
Environmental Chemistry Letters
On the other hand, researchers should focus more on
addressing the challenges associated with nanomaterials.
Presently, very few nanomaterials have materialized com-
mercially. Since the production cost is one of the crucial
parameters, future research should be dedicated to designing
cost-effective and highly efficient nanomaterials. For exam-
ple, the synthesis of nanomaterials from various waste mate-
rials by greener routes results in low-cost nanomaterials.
Applications of these eco-friendly nanomaterials will reduce
the overall production cost of the treatment process with a
lower environmental footprint. Furthermore, some of these
methods have an added advantage of the regeneration and
reuse of engineered nanomaterials to enhance the adsorption
efficiency and further decrease the production cost which
may be important for developing countries. Moreover, with
growing interest in the application of nanomaterials in water
and wastewater treatment, there is increasing consternation
on their potential toxicity to the human health and environ-
ment. It is concluded that nanotechnology is developing as a
promising tool to the conventional techniques of wastewater
treatment.
Acknowledgements  Authors are grateful to Durban University of
Technology and National Research Foundation of South Africa for
their financial support in the form of NRF-DST Innovation Doctoral
Scholarship (UID: 107643) to carry out this work.
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