NanoImpact 3–4 (2016) 22–39

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NanoImpact

journal homepage: www.journals.elsevier.com/nanoimpact

Review article

Nanomaterials-enabled water and wastewater treatment

Yanyang Zhang, Bing Wu, Hui Xu, Hui Liu, Minglu Wang, Yixuan He, Bingcai Pan ⁎
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China

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

Article history: With the fast development of nanomaterials and nanotechnology, environmental nanotechnology has attracted
Received 15 July 2016 increasing concerns in the past decades. In the field of water treatment, nanotechnology exhibited great potential
Received in revised form 17 September 2016 in improving the performance and efficiency of water decontamination as well as providing a sustainable ap-
Accepted 19 September 2016
proach to secure water supply. In this review, the current applications of nanomaterials in water and wastewater
Available online 26 September 2016
treatment were briefly discussed. The synthesis and physiochemical properties of diverse free nanomaterials, in-
Keywords:
cluding carbon based nanomaterial, metal and metal oxides nanoparticles as well as noble metal nanoparticles,
Environmental nanomaterials were focused on, and their performance and mechanisms towards removal of various contaminants were
Nanotechnology discussed. When concerning the large-scale application in water treatment, nanoparticles have to face some in-
Water treatment herent technical bottlenecks such as aggregation, difficult separation, leakage into the contact water, as well as
Nanocomposite potential adverse effect imposed on ecosystem and human health. The emerging nanocomposite materials inte-
grate the merits of functional nanoparticles and varying solid hosts of large size, and exhibit great advantages in
scaled-up application. This review particularly covered the topic of environmental nanocomposites, such as those
of organic and inorganic supports, nanocomposite membranes and magnetic nanocomposites. The advantages
and perspectives of various nanocomposites are briefly discussed.
© 2016 Elsevier B.V. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
2. Brief introduction of water nanotechnology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
2.1. Adsorption & Separation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
2.2. Catalysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
2.3. Disinfection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
2.4. Sensing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
3. Nanomaterials used in water treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
3.1. Carbon based nanomaterials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
3.1.1. Graphene based nanomaterials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
3.1.2. Carbon nanotubes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
3.2. Metal & metal oxides nanoparticles. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
3.2.1. Nanosized zero valent iron . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
3.2.2. Nanosized iron oxides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
3.2.3. Nanosized titanium oxides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29
3.2.4. Other metal oxides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29
3.3. Noble metal nanoparticles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30
4. Nanocomposites in water treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30
4.1. Nanocomposites of organic supports . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30
4.2. Nanocomposites of inorganic supports . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
4.3. Nanocomposite membrane . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33
4.4. Magnetic nanocomposites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34
4.5. Reusability of nanocomposites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34

⁎ Corresponding author.
E-mail address: bcpan@nju.edu.cn (B. Pan).

http://dx.doi.org/10.1016/j.impact.2016.09.004
2452-0748/© 2016 Elsevier B.V. All rights reserved.
 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39
5. Concluding remarks. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
1. Introduction
Our environment is under constant pressure with growing industri-
alization and urbanization. Among the world's top environmental prob-
lems, water scarcity has become the foremost issue facing the human
race. In the coming decades, rapid population growth in developing re-
gion will continue to intensify the clean water demand from domestic,
agriculture, industry and energy perspective (Pendergast and Hoek,
2011). By 2025, it was estimated that 50% of the world's population
will be living in water-stressed areas (WHO, 2014). Until 2015, only
around 20% of global wastewater is properly treated. In developing
countries, approximately 70% of industrial wastewater is discharged
without proper disposal of UN (2016). Current infrastructure for waste-
water treatment, as well as for the production of safe and readily avail-
able water is difficult to keep pace with the increasingly stringent
regulation and growing demand for high quality water, in both devel-
oped and developing country. Hence, water treatment technology fea-
tured with high efficiency and low cost is urgently required.
Recent advances in the manipulation of nanomaterials have facilitat-
ed the application of nanotechnology in water and wastewater treat-
ment. In the past decades, water nanotechnology has received
sufficient attentions as a potential supplement to the traditional treat-
ment methods. Nanomaterials are commonly defined as materials that
at least one dimension is smaller than 100 nm (Tesh and Scott, 2014).
At such scale, materials often exhibit unique physical or chemical prop-
erties over their bulky counterparts. For example, nanomaterials usually
have higher density of active sites per unit mass due to their larger spe-
cific surface area. In addition, nanomaterials exhibit greater surface free
energy, resulting in enhanced surface reactivity. At proper size, some
materials would show superparamagnetism, or even quantum confine-
ment effect (Khin et al., 2012; Alvarez and Li, 2013b). Taken advantage
of these size-dependent effects, the current water and wastewater
treatment process could be greatly improved by introducing
nanomaterials into the system.
Until now, numerous studies have shown that nanomaterials have
vast capability and potential in water and wastewater treatment, in par-
ticular, in the areas of adsorption (Ali, 2012), membrane process
(Pendergast and Hoek, 2011), catalytic oxidation (Ayati et al., 2014),
disinfection and sensing (Das et al., 2015). It is a pity that most of the re-
ported nanomaterials were in the stage of laboratory research or merely
a proof of concept. One of the commercially available nanotechnology is
the use of zero valent iron nanoparticles by injection (Karn et al., 2011;
Tesh and Scott, 2014). This is widely used in America for groundwater
remediation. Since the cost for nanomaterials are decreasing, they
have become more competitive for water and wastewater treatment.
However, there are still inherent disadvantages for direct use of free
nanoparticles in water and wastewater treatment process. Firstly, nano-
particles tend to aggregate in fluidized system or in fixed bed, resulting
in severe activity loss and pressure drop (Lofrano et al., 2016). Secondly,
it is still a challenging task to separate most of the exhausted nanopar-
ticles (except for magnetic nanoparticles) from the treated water for
reuse. Apparently, it would be undesirable in terms of the economical
consideration (Al-Hamadani et al., 2015; Qu et al., 2013c). Thirdly, the
behavior and fate of the nanomaterials in water and wastewater treat-
ment process are not fully understood, and the impact of nanomaterials
on the aquatic environment and human health is a major issue that
could hinder the application of nanotechnology (Dale et al., 2015;
Varma, 2012).
To avoid or mitigate the potentially adverse effect brought by the ap-
plication of nanotechnology, it is desirable to develop a material or a
23
34
35
35
device that could minimize the release or mobilization of the
nanomaterials while maintaining their high reactivity. The develop-
ment of nanocomposite is proved to be an effective and promising ap-
proach. Nanocomposite is commonly fabricated by loading desired
nanoparticles onto various supporting materials, such as polymers or
membranes. It could be defined as a multiphase material which at
least one dimension of the constituent phases is b 100 nm (Tesh and
Scott, 2014). Some of the reported nanocomposites were highly effi-
cient in water decontamination, recyclable, cost-effective and compati-
ble with existing infrastructure (Lofrano et al., 2016; Yin and Deng,
2015).
This review focuses on various nanomaterials used for contaminant
adsorption, separation and catalytic degradation from or in water. Both
free nanoparticles and nanocomposites are involved in this paper, and
some promising nanocomposites will be highlighted in the review.
The fabrication and characteristics of these materials will be summa-
rized, and the performance and mechanism of decontamination by
these nanomaterials will be particularly concerned. In the end, the pros-
pect of these nanomaterials in water treatment will also be briefly
discussed.
2. Brief introduction of water nanotechnology
With the development of nanotechnology, its application in water
and wastewater treatment is becoming imminent. Over the past de-
cades, there are numerous studies available on such topic. In this sec-
tion, we provided a brief review of some typical application of
nanotechnology in water and wastewater treatment, i.e., adsorption
and separation, catalytic oxidation, disinfection and sensing.
2.1. Adsorption & Separation
Adsorbents or membrane based separation process are two most
widely used technology for polishing treatment of water and wastewa-
ter. Conventional adsorbents often face challenges such as low capacity
and selectivity as well as the short adsorption-regeneration cycle, which
significantly reduced the cost effectiveness of the adsorbents.
Nanomaterial based adsorbents, i.e., nanosized metal or metal oxides,
carbon nanotubes (CNTs), graphene and nanocomposites, often feature
large specific area, high reactivity, fast kinetics and specific affinity to
various contaminants. Their adsorptive performance towards certain
contaminants is sometimes several magnitude higher than convention-
al adsorbents (Ali, 2012; Khajeh et al., 2013).
Besides adsorption, membrane separation is also a key module in the
polishing treatment stage, enabling water reclamation from unconven-
tional water sources such as municipal wastewater. Removal of contam-
inants by membrane separation is mainly based on size exclusion.
However, there are still many obstacles to further forward membrane
technology, i.e., the inherent trade-off between membrane selectivity
and permeability, high energy consumption, fouling and operational
complexity. To address these issues, advanced nanocomposite mem-
branes were developed by introducing functional nanoparticles into
the membrane. This new class of membrane showed enhanced physio-
chemical properties such as improved mechanical or thermal stability,
porosity and hydrophilicity. Some exhibited unique properties like en-
hanced permeability, or anti-fouling, antimicrobial, adsorptive or
photocatalysis capabilities (Pendergast and Hoek, 2011; Yin and Deng,
2015). Adsorption and separation nanotechnology were currently the
closest to commercial maturity. More discussion concerning the
24 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39
nanomaterials used in the adsorption and separation of various contam-
inants from water will be available in the following section.
2.2. Catalysis
Catalytic or photocatalytic oxidation is an advanced oxidation pro-
cess for removal of trace contaminants and microbial pathogens from
water. It is a useful pretreatment method in enhancing the
biodegradabiliy for hazardous and non-biodegradable contaminants
(Reddy et al., 2016). Photocatalysis can also be used as a polishing
step to treat recalcitrant organic compounds (Qu et al., 2013a).
Nanocatalysts of high surface-to-volume ratio showed significantly
enhanced catalysis performance over their bulky counterparts. Addi-
tionally, the band gap and crystalline structure of the nanosized semi-
conductors exhibited size-dependent behavior. Their electron hole
redox potential and photo-generated charge distribution varied with
varying sizes (Song et al., 2010; Turki et al., 2015). Furthermore, by im-
mobilization of nanoparticles onto various substrates, the stability of the
nanocatalyst was improved and the resultant nanocomposites were
compatible with existing photo-reactor (Petronella et al., 2016).
2.3. Disinfection
To avoid the spread of waterborne disease, disinfection is the last but
critical step in water treatment. The ideal disinfectant should possess
the following properties: (1) broad antimicrobial spectrum within
short time; (2) no generation of harmful by-products; (3) low toxicity
to health and ecosystems; (4) low energy cost and easy operation; (5)
easy to store and must not be corrosive; and (6) capable of safe disposal.
Recently, several nanomaterials have been proved with strong anti-
microbial properties, including chitosan nanoparticles (Higazy et al.,
2010), nano silver (nAg) (Rai et al., 2009), photocatalytic TiO2
(Hebeish et al., 2013), and carbon based nanomaterials (Martynkova
and Valaskova, 2014). These nanomaterials kill microorganisms by re-
leasing toxic metal ions (e.g., Ag+), damaging cell membrane through
direct contact (e.g., chitosan NPs) or generating reactive oxygen species
(ROS, e.g., TiO2). Unlike conventional chemical disinfectants, these anti-
microbial nanomaterials inactivated microorganisms through more sus-
tainable approaches, which is expected to minimize the formation of
harmful disinfection byproducts (DBPs) (Li et al., 2008b). In addition,
when integrated with proper separation strategies, some nano-disinfec-
tants could be operated continuously with high efficiency and low ener-
gy consumption, which is extremely attractive for de-centralized water
and wastewater treatment.
2.4. Sensing
Today, conventional sensing and monitoring methods are incapable
of detecting extremely low concentration of micro-pollutants in com-
plex water bodies. Rapid and in situ detection of pathogens and highly
toxic pollutants are of great significance in emergency situation (e.g.,
water related accidents). Nanomaterials such as carbon nanotubes,
graphene, quantum dots and noble metals (e.g. Ag or Au) possess
unique electrochemical, optical or magnetic properties. Incorporation
of such nanomaterials into sensors or electrodes could selectively pre-
concentrate trace pollutants for detection. Some nanomaterials could
enhance spectroscopic response (e.g. Raman shift or surface plasmon
resonances) by several magnitude (Das et al., 2015; Pradeep and
Anshup, 2009). Also, next generation nanocomposite sensors were
widely explored for their potential in environmental monitoring and
sensing (Shrivastava et al., 2016).
3. Nanomaterials used in water treatment
The advancement of nanotechnology is highly dependent on the in-
novation of various nanomaterials. In this chapter, a number of
nanomaterials that could be used in water and wastewater remediation
were introduced. Their synthesis, removal of contaminants and the un-
derlying mechanism were discussed.
3.1. Carbon based nanomaterials
3.1.1. Graphene based nanomaterials
Graphene is a single carbon layer of the graphite structure (IUPAC),
presenting an ordered honeycomb network structure. It often exhibits
excellent thermal and electrical conductivity. Graphene oxide (GO) is
a monolayer graphene with a highly oxidative form, which consists of
a variety of oxygen-containing functional groups, such as hydroxyl, car-
boxyl, carbonyl and epoxy groups. Reduced graphene oxide (RGO) is
more defective and less conductive than graphene but is relatively
easy to be modified by other functional groups (Avouris and
Dimitrakopoulos, 2012). Application of graphene based materials has
aroused interests of many fields including environmental remediation.
Graphene has rich π-bonds and GO features abundant oxygen-con-
taining functional groups. Both of them have large surface area. In gen-
eral, there are five possible interactions for the adsorption of graphene-
based nanomaterials, including hydrophobic effect, π-π bonds, hydro-
gen bonds, covalent and electrostatic interactions (Zhu et al., 2010). In
general, graphene based materials are favorable adsorbents for various
contaminants from water. Some relevant studies are listed in Table 1.
GO and modified GO/RGO materials were widely explored for their
capability to remove heavy metals such as Pb(II), Zn(II), Cu(II), Cd(II),
Hg(II) and As(III/V). Wang et al. (2013) studied the effect of pH, adsor-
bent dosage, foreign ions and contact time on the adsorption of Zn(II) on
GO. Results showed that the optimal pH for Zn(II) removal was around
7.0 with short equilibrium time. The maximum adsorption capacity for
Zn(II) was up to 246 mg/g based on Langmuir model fitting. Madadrang
et al. (2012) found GO linked with EDTA would be an ideal adsorbent for
Pb(II) uptake. EDTA modification enhanced the adsorption capacity of
GO because of its chelating ability. The adsorption capacity for Pb(II)
was found to be 479 ± 46 mg/g at pH 6.8, and the process was equili-
brated within 20 min. Yang et al. (2013) prepared RGO/Poly(acryl-
amide) composite and studied its adsorption for Pb(II). The RGO/PAM
displayed adsorption capacity as high as 1000 mg/g for Pb(II). Kumar
et al. (2014b) showed that the hybrids of single-layer GO with manga-
nese ferrite magnetic nanoparticles could be employed for efficient re-
moval of Pb(II), As(III), and As(V) from contaminated water. The
maximum capacity was 673 mg/g for Pb(II), 146 mg/g for As(III) and
207 mg/g for As(V). It was promising for co-removal of multiple heavy
metals or metalloids from aquatic environment because of its high ca-
pacity and ease of magnetic separation.
Besides metal ions, the graphene-based materials have been also ex-
plored to adsorb the anionic contaminants of emerging concern. Li et al.
(2011) found that graphene was an excellent fluoride adsorbent with a
capacity of 35.6 mg/g at pH 7.0 and 25 °C. Fluoride ions are predomi-
nantly captured by surface ligand exchange between fluoride ions in so-
lution and hydroxyl ions on the adsorbent. Vasudevan and Lakshmi
(2012) made a systematic study on graphene adsorption for phosphate.
The experimental results showed that the capacity of graphene was up
to 89.37 mg/g. Zhang et al. (2011) reported a 3D nanostructured
graphene-polypyrrole (Ppy) hybrid for perchlorate (ClO− 4 ) purification.
The graphene-Ppy hybrid exhibited a significantly improved uptake ca-
pacity for ClO−4 compared with Ppy film alone, and can be used for ClO4
−
removal through an electrically switched ion exchange. Hartono et al.
(2009) first reported the application of GO for humic acid (HA) adsorp-
tion in aqueous solution. They found that the GO exhibited much higher
adsorption capacity of HA than graphite. Its maximum adsorption ca-
pacity was 190 mg/g based on Langmuir isotherm, much higher than ac-
tivated carbon. The adsorption of some antibiotics, tetracycline,
oxytetracycline and doxycycline by GO was also investigated, and the
estimated maximum adsorption capacities were 313, 212 and 398 mg/
g for the three contaminants, respectively (Gao et al., 2012). The
 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39 25

Table 1
Application of graphene, graphene oxide, reduced graphene oxide and modified graphene as adsorbents.

Adsorbent Target contaminant Conditions Adsorption capacity Mechanism References

EDTA-GO Pb(II) pH 6.8 479 ± 46 mg/g Ion exchange, complexing interaction Madadrang et al. (2012)
GO Au(III), Pd(II), Pt(IV),Zn(II) pH 6.0 108.342 mg/g, 80.775 mg/g, – Liu et al. (2013) and
71.378 mg/g, 246 mg/g Wang et al. (2013)
RGO/PAM Pb(II) 298, 308, 318 K 1000 mg/g – Yang et al. (2013)
PEI-GO Cr(VI) – 539.53 mg/g Electrostatic interaction, π-electrons Chen et al. (2014)
PVP-RGO Cu(II) pH 3.5 1689 mg/g Physisorption, the cation-π interaction Zhang et al. (2014)
GO- MnFe2O4 Pb(II), As(III), As(V) 673 mg/g for Pb(II), Cation exchange reaction, complexing Kumar et al. (2014b)
146 mg/g reaction
for As(III), 207 mg/g for As(V)
GMN Fuchsine at pH 5.5, 25 °C 89.4 mg/g Van der Waals interactions, π-stacking Wang et al. (2011)
interaction
G-CNT Methylene blue – 81.97 mg/g Self-induced π-π interaction Ai and Jiang (2012)
RGO-hydrogels Methylene blue, Rhodamine – 7.85, 29.44 mg/g Strong π-π stacking, anion–cation Tiwari et al. (2013)
B interactions
GO- Fe3O4 methylene blue, neutral red – 167.2, 171.3 mg/g Strong π-π interaction Xie et al. (2012)

adsorption capacities decreased with the increasing pH or Na+ concen-
tration. The mechanism of micropollutants adsorption was attributed to
π-π interaction and cation-π bonding.
GO and their composites also showed attractive potential for the re-
moval of dyes. The adsorption for ionic dyes mainly relies on electrostat-
ic interaction and covalent bonding. GO presented high adsorption
efficiency of cationic dyes, but low affinity for anionic dyes due to the
strong electrostatic repulsion. On the other hand, graphene and
graphene-based composites are good adsorbents for anionic dyes due
to their ion exchange and covalent bonding capacity (Liu et al.,
2012a). Ai and Jiang (2012) prepared graphene-carbon nanotube hy-
brid (G-GNT) for the removal of methyl blue (MB). The hybrid showed
good performance with a maximum capacity of 81.97 mg/g and the re-
moval efficiency of 97% at the initial MB concentration of 10 mg/L.
Tiwari et al. (2013) reported that RGO-based hydrogels removed MB
and Rhodamine B through strong van der Waals force and π-π interac-
tions. Results showed the excellent removal capabilities for MB
(7.85 mg/g) and Rhodamine B (29.44 mg/g). Meanwhile, RGO also ex-
hibited satisfactory catalytic activity towards peroxymonosulfate
(PMS) to produce sulfate radicals for degradation of aqueous organic
pollutants (Sun et al., 2012).
In many cases, surface modification and hybridization are two effec-
tive pathways to enhance the reusability, separation, and removal effi-
ciency of graphene based materials, rending them to be attractive
options for water decontamination from various pollutants. However,
the high cost still limits their wide application in environmental reme-
diation now. Also, there are still some challenges to be concerned,
such as the reusability, environmental safety, and compatibility with
other units.
2012a; Diederich and Thilgen, 1996; Georgakilas et al., 2012;
Nakamura and Isobe, 2003; Tasis et al., 2006). CNTs surface modification
methods include oxidization, chemical grafting and physical modifica-
tions such as impregnating or coating (Yu et al., 2011). The outermost
surface, inner cavities, interstitial channels, and grooves of CNTs consti-
tute four possible adsorption sites (Kumar et al., 2014a). The adsorption
mechanisms of contaminants by CNTs were quite similar to that of
graphene, including hydrophobic, van der Waals forces, H-bonding, π-
π interation, electrostatic interaction, and covalent bonding (Gupta et
al., 2013). In some cases, adsorption also depends on the physical as-
pects of CNTs, where porous structure plays a significant role (Den et
al., 2006; Zhao et al., 2007). According to the past studies, CNTs also ex-
hibited high capacities for lots of organic compounds include polycyclic
aromatic hydrocarbons (PAHs) (Yang et al., 2006), phenolic compounds
(Hu et al., 2015), endocrine disrupt compounds (Pan et al., 2008) and
antibiotics (Wang et al., 2010b).
CNTs were normally used as a mixture of suspended solids, and it is
also difficult to readily separate them from water. Wei et al. (2013) has
developed a novel granular CNTs/Al2O3 composite of good mechanical
strength, hydrophilicity, heat resistance and good sorption performance
for two pharmaceuticals (diclofenac sodium and carbamazepine). The
adsorbed pharmaceuticals can be decomposed in the regeneration pro-
cess (Wei et al., 2013). This hybridization method inspired the develop-
ment of granular CNTs-based composites.
Table 2 summarized the environmental applications of various CNTs.
It can be figured out that many challenges still remained for the envi-
ronmental application of CNTs, and further study should be started for
novel CNT adsorbents such as new types of CNTs composites. This will
be discussed further in the following sections.

3.1.2. Carbon nanotubes 3.2. Metal & metal oxides nanoparticles

Carbon nanotubes (CNTs) have been one of the most important ma-
terials that helped trigger the rush to nanotechnology research and de-
velopment (Lam et al., 2006). CNTs can be classified into three types:
single-walled CNTs (SWCNTs), multi-walled CNTs (MWCNTs), and
CNTs composites (including functionalized CNTs) (Bahgat et al., 2011;
Ma et al., 2011). Because of the one-dimensional structure, CNTs has
outstanding physical properties such as unique mechanical, thermal
and electrical properties (Thostenson et al., 2001). Diameter, length,
chirality play important roles in the characteristics and functions of
the CNTs.
Similar to GO, CNTs were also used for heavy metal adsorption
(Hirlekar et al., 2009). It was suggested that the metal removal of
CNTs could also be significantly enhanced by surface modification.
CNTs could be conveniently surface-modified by suitable functional
groups to enable favorable accessibility and attachment of various or-
ganic and inorganic contaminants (Allen et al., 2009; Chen et al.,
Nanosized metals and metal oxides have received ever-increasing
attentions because of their high performance and low cost for contami-
nants removal. Nanosized metals and metal oxides mainly include
nanosized zero-valent iron, ferric oxides, aluminum oxides, manganese
oxides, titanium oxides, magnesium oxides and cerium oxides (Hua et
al., 2012). Nanosized magnetic adsorbents have also turned up in recent
years (Mahdavian and Mirrahimi, 2010). A number of studies suggested
that nanosized metals and metal oxides exhibit favorable sorption to-
wards metallic contaminants such as arsenic (Kanel et al., 2006;
Lakshmipathiraj et al., 2006), cadmium (Boparai et al., 2011; Engates
and Shipley, 2011), chromium (Hu et al., 2005; Yu et al., 2014), uranium
(Crane et al., 2011), and other common pollutants such as phosphate
(Wen et al., 2014b) and organics (Fan et al., 2009; Shih and Tai, 2010)
in terms of high capacity and selectivity. Current applications of various
metal and metal oxides were illustrated in Table 3.
 26
Table 2
Removal of organic contaminants by using various types of CNTs.

Removal rate/adsorption
Type of CNTs Modification method Target contaminants optimal pH capacity Mechanism Refs.

SWCNTs – Bisphenol A (BPA) and 3.5–8.5 EE2 (95–98%) Hydrophobic interactions and π-π Joseph et al. (2011)
17α-ethinyl estradiol (EE2) BPA (75–80%) electron donor-acceptor (EDA)
SWCNTs and MWCNTs Carboxylated Oseltamivir (OE) and OE: alkaline OE and OC (N90%) Hydrophobic interaction, Wang et al. (2015)
oseltamivir carboxylate (OC) OC: 6–8 electrostatic interaction, van
der Waals force, and H-bonding
MWCNTs Adhere to the bar to be a Phenols, non-steroidal 3.0–5.0 80%–99% Polar and apolar adsorption Hu et al. (2015)
polyaniline/hydroxyl MWCNTs anti-inflammatory drugs, and

Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39

(PANi/MWCNTs-OH) polychlorinated biphenyls
composite-coated stir bar
Granular CNTs Al2O3 was bonded with g-CNTs Diclofenac sodium (DS) and DS: acid CBA:157.4 μmol/g Hydrophobic interaction, Wei et al. (2013)
carbamazepine (CBZ) CBZ: – DS:106.5 μmol/g electrostatic interaction, van
der Waals force, and H-bonding
MWCNTs – Eriochrome cyanine R (ECR) alkaline 73.18 mg/g Hydrophobic interaction, Ghaedi et al. (2011)
electrostatic interaction, van der
Waals force, and H-bonding
MWCNTs Alkali-activated Magnetic carbon (MO) MO: 2–10 MO:149 mg/g Hydrogen bonding, π-π Ma et al. (2012)
Methylene blue(MB) MB: b4 and N8 MB:399 mg/g electron-donor-acceptor
interactions, electrostatic
interactions, mesopore filling
MWCNTs Oxidized 5-(4-dimethyl amino 6.5–7.5 15.52 mg/g Hydrogen bonding, π-π Ghaedi et al. (2013)
benzylidene)rhodanine electron-donor-acceptor
interactions, electrostatic
interactions, mesopore filling
MWCNTs Grafted with iron oxides and 1-Naphthylamine 7.0–9.0 200 mg/g An internal hydrophobic cavity Hu et al. (2011)
β-cyclodextrin (β-CD) from β-cyclodextrin and common
mechanism of CNTs
MWCNTs Magnetic multi-walled carbon Direct Red 23 3.7 85.5 mg/g Magnetic separation technology Konicki et al. (2012)
nanotubes–Fe3C nanocomposite combined with adsorption process
(M-MWCNT-ICN)
MWCNTs Grafted with polyacrylamide Humic acid (HA) acid 80%–85% PAAM grafting improved the Yang et al. (2011)
(PAAM) hydrophilicity and dispersibility
of the MWCNTs
Table 3
Metal oxides for contaminant removal from water.

Absorbent Shape and size (nm) Surface area (m2/g) Target contaminant Optimal pH Performance Refs.

Goethite (α-FeOOH)
Hematite (α-Fe2O3)
Needle like, length 200, width b 50 50 Cu(II) 6 100% Cu(II) removal at pH 6 Grossl et al. (1994)
Needlelike,1–10 – F 7 Adsorption capacity 59 mg/g Mohapatra et al. (2009)
Particle, 37 31.7 Pb(II), Cd(II), Cu(II), Zn(II) 8 100% Pb adsorbed, 94% Cd Engates and Shipley (2011)
adsorbed, 89% Cu adsorbed,
100% Zn adsorbed at 0.5 g/L

Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39

nanohematite
Maghemite (γ-Fe2O3) Particle, 10 198 Cr(VI), Cu(II), Ni(II) Cr(VI): 2.5, Cu(II): 6.5, Ni(II): 8.5 Hu et al. (2006)
Particle, 10 178 Cr(VI) 2.5 Hu et al. (2005)
Magnetite (Fe3O4) Particle, 10–20 – Se(IV) 2–4 Se reduced to b5 μg-Se/L Wei et al. (2012)
from an initial 100 μg-Se/L
Hydrous ferric oxide (HFO) Particle, − 148 F 3 Maximum adsorption Nur et al. (2014)
capacity 6.71 mg F/g at
pH 6.5; adsorption capacity
in column experiments
3.26 mg F/g HFO
Al2O3 Particle, 62–87 42.62 Pb(II), Cd(II), Cr(III), Co(II), 5.5 Maximum adsorption Afkhami et al. (2010)
Ni(II), Mn(II) capacity of Cr(III), Cd(II) and
Pb(II) in a mixture of six ion
metals were 100.0, 83.33 and
100.0 mg/g, respectively
TiO2 Particle, 8.3 185.5 Pb(II), Cd(II), Cu(II), Ni(II), 8 Pb: 2.0 μmol/L(99.9%), Cd: Engates and Shipley (2011)
Zn(II), dye, micro-pollutants 3.9 μmol/L (96.2%), Zn:
6.3 μmol/L (98.2%) i
ZnO Particle, 26 – Zn(II), Cd(II), Hg(II) 8 Maximum adsorption Sheela et al. (2012)
capacity 357, 387,
714 mg/g for Zn(II),
Cd(II), Hg(II);

27
28 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39
3.2.1. Nanosized zero valent iron
Zero valent iron (ZVI) is an effective tool for water remediation. Its
reactivity has been largely improved by the development of nanoscale
zero valent iron (nZVI). nZVI possesses many specific positive features
such as a high reactivity towards a broad range of contaminants due
to their large specific areas (Tosco et al., 2014), diminutive sizes that
help to promote effective subsurface dispersion (Li et al., 2006) and in-
jection (Tosco et al., 2014) in aqueous slurries for remediation of con-
taminated areas. Studies showed that by manipulating the size of ZVI
from micron to nanoscale, the rate constant for As(V) removal could
be improved by 1–3 orders of magnitude (Kanel et al., 2006). This out-
standing reactivity of nZVI was presumed to result from its significantly
increased surface area and active sites, compared to bulky ZVI. Besides,
nZVI was featured with high surface modifiability, excellent magnetic
properties and great biocompatibility (Xu et al., 2012). nZVI usually pre-
sents as a core-shell structure with the outer layer of iron oxides and the
inner layer of Fe0. The Fe0 core could be oxidized to form iron oxides upon
reactions with water, and then transforms to a series of corrosion prod-
ucts, including goethite (α-FeOOH), akaganeite (β-FeOOH), lepidocrocite
(γ-FeOOH), magnetite (Fe3O4), maghemite (γ-Fe2O3), green rusts, sider-
ite (FeCO3). The corrosion products also presented powerful adsorption
ability towards large amounts of contaminants (Liu et al., 2014).
nZVI was widely applied as adsorbent for contaminants removal.
The iron (oxy)hydroxide layer surrounding Fe0 core was proved to be
a strong adsorbent. Kanel et al. (2006) found that 100% As(V) was re-
moved by 0.1, 0.2, and 0.4 g/L nZVI for three different kinds of real
wastewater, respectively. Laser light scattering indicated that As(V) ad-
sorption onto nZVI occurred via an inner-sphere surface complexation
(Kanel et al., 2006). Wen et al. (2014b) found that phosphate adsorption
onto nZVI were mainly through adsorption and co-precipitation pro-
cess, with the maximum capacity of 245.65 mg/g. Many other pollutants
such as cadmium (Boparai et al., 2011), chromium (Yu et al., 2014) cap-
tured by nZVI were also found to form inner-sphere complexes with the
iron oxides layer surrounding nZVI core.
Some contaminants such as As(III/V), U(VI), Se(VI) could be reduced
to lower oxidation states upon immobilization onto the nZVI surface.
Crane et al. (2011) suggested that U(VI) could be removed by nZVI to
10 μg/L (N 98% removal) within 2 h, and U(VI) was partially reduced to
U(IV) concurrent with Fe oxidation. Li et al. (2014) demonstrated that
the average removal capacity of Cu(II) by nZVI was 343 mg/g. Cu(II)
was reduced to metallic copper or cuprite (Cu2O) after adsorption.
Ramos et al. (2009) found that As(V) or As(III) was partially reduced
to As(0) after reacting with nZVI, demonstrating that reduction to ele-
mental arsenic by nZVI was an important process for arsenic immobili-
zation. Furthermore, As(III) ended in the form of As(0), As(III) and
As(V) on the nZVI surface after reaction, indicating both reduction and
oxidation of As(III) occurred when reacting with nZVI. The dual redox
functions of nZVI are enabled by its core-shell structure, that is, the
inner core was metallic iron with a strong reducing characteristic, the
outer layer containing thin amorphous iron (oxy)hydroxides promoted
coordination and oxidation.
Apart from the aforementioned contaminants, nZVI was also capable
of removing other contaminants such as nitrate (Ryu et al., 2011), dyes
(Fan et al., 2009), environmental persistent toxic contaminants (Shih
and Tai, 2010) and antibiotics (Fang et al., 2011) through adsorption,
oxidation, reduction and co-precipitation. To sum up, nZVI is proved
to be a highly reactive, cost-effective, environment-friendly material
and exhibits multifaceted removal pathways for wastewater treatment.
3.2.2. Nanosized iron oxides
The growing interest in the use of nanosized iron oxides for waste-
water treatment resulted from their strong sorption capability, opera-
tional simplicity and resourcefulness. The phases of iron oxides
discussed in this article, are the non-magnetic goethite (α-FeOOH)
and hematite (α-Fe2O3), magnetic magnetitie (Fe3O4) and maghemite
(γ-Fe2O3) and hydrous ferric oxides (HFO). Goethite and hematite
incorporate a range of geo-chemically and environmentally important
oxyanions and cations in their complex matrixes. They have been con-
sidered as efficient and low-cost absorbents for the mitigation of various
contaminants.
Nanosized goethite exhibited a high adsorption capacity of 59 mg/g
for fluoride, successfully bringing down fluoride from 10.25 to 0.5 mg/L
(Mohapatra et al., 2009). FT-IR characterization of As(V) on the goethite
surface suggested the presence of both As\\O\\Fe and As\\O bonds, in-
dicating the formation of surface complexes (Lakshmipathiraj et al.,
2006). Kinetics and mechanisms of Cu2+ adsorption on goethite was in-
vestigated by Grossl et al. (1994) using the pressure-jump relaxation
technique. They found that a monodentate inner-sphere Cu2+/goethite
complex was formed on the goethite surface. The adsorption rate of di-
valent metal cations on goethite was directly related to the removal rate
of a water molecule from the primary hydration sphere of a specific di-
valent metal cation (Grossl et al., 1994).
Another non-magnetic iron oxides, hematite, is also highly reactive
and has been widely examined. Compared with nanosized goethite
(149.25 Cu(II) mg/g), the maximum Cu(II) capacity of nanosized hema-
tite (84.46 mg/g) was lower, although both showed similar adsorption
kinetics and mechanisms (Chen and Li, 2010). Adsorption of metal
ions (Pb(II), Cd(II), Cu(II), Zn(II)) onto nanosized hematite was exam-
ined as a function of sorbent concentration, pH, temperature (Shipley
et al., 2013). Results indicated that 100% Pb, 94% Cd, 89% Cu and 100%
Zn species were adsorbed with 0.5 g/L nanosized hematite. The effect
of temperature on adsorption demonstrated that Pb(II), Cu(II), and
Cd(II) underwent an endothermic reaction, while Zn(II) underwent an
exothermic reaction. Both nanosized goethite and nanosized hematite
are effective materials that could be employed in various environmental
remediation.
Separating and recovering nanomaterials from water after reaction
has long been a technical bottleneck to overcome. Magnetic nanosized
iron oxide sorbents offered a viable and convenient solution by utilizing
an external magnetic field (Hua et al., 2012). There have been numerous
reports on the use of nanosized maghemite and magnetite for adsorbing
heavy metals including arsenic, chromium (Hu et al., 2005), selenium
(Wei et al., 2012), copper, lead, and nickel (Hu et al., 2006) from syn-
thetic solutions and natural water systems. Maghemite nanoparticles
of 10 nm with a surface area of 178 m2/g were synthesized using a
sol-gel method. The adsorption of Cr(VI) reached equilibrium within
15 min. Competition from common coexisting ions such as Na+, Ca2+,
Mg2+, Cu2+, Ni2+, NO3−, and Cl− was negligible, implying the selective
adsorption of Cr(VI) from wastewater. The maghemite nanoparticles
retained the original metal removal capacity after six successive adsorp-
tion-desorption processes (Hu et al., 2005). Further studies on the ad-
sorption of heavy metals (Cr(VI), Cu(II), and Ni(II)) also verified the
fast kinetics, high selectivity and satisfactory reusability towards target
contaminants. The adsorption of Cr(VI) and Cu(II) was mainly attribut-
ed to electrostatic attraction and ion exchange, whereas the adsorption
of Ni(II) resulted from electrostatic attraction only (Hu et al., 2006).
Another important magnetic adsorbent is nanosized magnetite con-
sidering its low cost, simple manipulation and environment-friendly
properties. Nanosized magnetite has been used to remove various con-
taminants such as heavy metals Cr(VI) (Hu et al., 2004), Cu(II), Zn(II),
and As(III/V), Se(IV) (Wei et al., 2012), methylene blue (Mak and
Chen, 2004), as well as dichlorophenol (Cumbal and SenGupta, 2005b)
from aqueous solutions. Magnetite nanoparticles of 10 nm with a sur-
face area of 198 m2/g were synthesized using the same sol-gel method
with nanosized maghemite (Hu et al., 2004). Wei et al. (2012) success-
fully achieved a final Se concentration of b5 μg/L using nanosized mag-
netite with an initial Se concentration of 100 μg/L. Nanosized magnetite
exhibited high selectivity towards Se in the presence of common anions
and high removal capacity at low pH. (Wei et al., 2012).
Nanosized maghemite and magnetite could be produced in large
quantity using the relatively easy sol-gel method. Their large surface
area and highly active surface sites impetus the high adsorption capacity
 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39
towards a wide range of contaminants. The uptake process of contami-
nants occurred mainly via external adsorption, resulting in a very short
adsorption time. Furthermore, the separation of metal-loaded magnetic
adsorbent from treated water can be easily achieved via a simple mag-
netic field (Hu et al., 2005).
At oversaturated concentrations, hydrolyzed iron species precipitate
and aggregate into amorphous structures with high porosity known as
hydrous ferric oxide (HFO) (Mercer and Tobiason, 2008). A comparison
of the influence of oxide structure on the removal performance showed
that amorphous oxides such as HFO, have larger sorption capacities for
metal contaminants than crystalline oxides such as goethite (Trivedi
and Axe, 2001). Although both are composed of chains of octahedral
units of FeO6, HFO or ferrihydrite has short-range order and a discontin-
uous layered structure, contributing to its high surface area and sorption
capacity (Spadini et al., 1994). HFO provides active sites for sorption of
dissolved species mainly by surface complexation or ligand exchange
(Anderson et al., 1985; Dzombak and Morel, 1990; Stumm, 1992).
Swallow et al. (1980) found that adsorption of Cu(II) or Pb(II) on amor-
phous HFO was independent on aging of the solid over several days, or
variations in ionic strength from 0.005 to 0.5. The sorption process can
be approximately described as a simple mass action law by systematic
variations in metal and HFO concentrations. The corresponding adsorp-
tion constant increasing with pH with a slope of ca. 1.5 (pK vs. pH) ap-
peared applicable over a wide range of pH. Also, the high capacity of the
iron oxide for metals suggested an open, permeable structure for the
HFO (Swallow et al., 1980).
3.2.3. Nanosized titanium oxides
As a classic semiconductor, TiO2 was of the most widely studied
photocatalyst. TiO2 photocatalysis involves the formation of highly reac-
tive species like hydroxyl (OH) radicals, superoxide anions (O− 2 ) and,
peroxides (O2− 2 ) that can decompose organic compounds in the pres-
ence of UV, visible light, or solar light. TiO2 possesses sound photocata-
lytic efficiency, biological and chemical inertness and high oxidative
potential. In order to achieve high photocatalytic activity of TiO2, various
TiO2 inorganic nanomaterials of highly porous network were synthe-
sized through template based sol-gel method. The morphological struc-
ture, crystal phase, defect structure impurities, band gap energy and
hydrophilicity could be tuned by adjusting the type, chain length and
concentration of surfactant template (Choi et al., 2010). Nanosized
TiO2 was also widely applied in the removal of micro-pollutants like en-
docrine disrupting compounds, cyanotoxins, antibiotics (Fagan et al.,
2016). Moreover, photocatalysis using nanosized TiO2 under both
solar and artificial light has been extensively studied and applied to-
wards the decomposition and mineralization of various organic pollut-
ants such as pesticides (Ahmed et al., 2011), dyes (Comparelli et al.,
2005), polymers, phenolic contaminants in wastewater (Ahmed et al.,
2011), persistent organic pollutants (such as aldrin, polychlorinated bi-
phenyls, etc.) (Arabatzis et al., 2002), as well as for general water puri-
fication (Gelover et al., 2004).
3.2.4. Other metal oxides
Besides the extensive study and widespread use of nZVI and nano-
scale iron oxides adsorbents, some other metal oxides also have high
surface areas, microporous structure, and high affinity for various con-
taminants. Those widely used nanoscale metal oxides include alumi-
num oxides, zinc oxides, magnesium oxides, cerium oxides, etc.
Alumina is a classical adsorbent and the form of γ-alumina is antic-
ipated to be more adsorptive than α-alumina (Hiraide et al., 1995; Li et
al., 2008a). Nanosized γ-Al2O3 is a promising adsorbent because of its
large specific surface area, high adsorption capacity, and satisfactory
mechanical strength (Sharma et al., 2008; Türker, 2007; Zhang et al.,
2008a). Nanosized alumina could be developed by the sol-gel method
and were used for the removal of Ni(II) from aqueous solutions
(Sharma et al., 2008). The maximum removal was found to be 96.6%
at 25 mg/L Ni(II). Zhang et al. (2008a) indicated that nanosized Al2O3
29
was an effective adsorbent for Tl(III) from aqueous solutions with a
nearly 100% removal at pH 4.5. Sometimes, nanosized alumina exhibit-
ed poor affinity towards some heavy metals. To overcome this problem,
chemical or physical modification of the surface γ-Al2O3 nanoparticles
was performed with functional groups containing donor atoms such
as oxygen, nitrogen, sulfur and phosphorus (Dadfarnia et al., 2002;
Ghaedi et al., 2008; Hiraide et al., 1994; Manzoori et al., 1998; Shabani
et al., 2009). For instance, 2,4-dinitrophenylhydrazine (DNPH)
immobilized on sodium dodecyl sulfate coated nano-alumina was de-
veloped for removal of metal cations, and the maximum adsorption ca-
pacity for Cr(III), Cd(II) and Pb(II) ions was 100.0, 83.33 and 100.0 mg/g
respectively (Afkhami et al., 2010). When a modifier is immobilized at
the surface of alumina, the contaminants are removed by dual functions
from both the added functional groups and the alumina.
Nanosized manganese oxides (NMnOs) exhibited superior adsorp-
tive performance towards certain contaminants than other metal oxides
because of its polymorphic structures and higher specific area (Tripathy
et al., 2006). In the past decades, NMnOs have been exploited for sorp-
tion of cationic or anionic pollutants from natural waters, such as heavy
metal ions (Mishra et al., 2004), arsenate (Takamatsu et al., 1985), and
phosphate (Kawashima et al., 1986). It was effective in the removal of
contaminants from aqueous solutions. Also, it was low-cost and readily
available in the environment (Tripathy et al., 2006). Hydrous manga-
nese oxide (HMO) was the most widely studied one among manganese
oxides. Mishra et al. (2004) found that HMO was effective in the remov-
al of Hg(II) from aqueous solutions. A higher percentage of Hg(II) up-
take by HMO was favored by an increase in concentration (10−8–
10−2 M), temperature (298–328 K), and pH (2.0–10.5) of adsorptive so-
lution. In addition, HMO was found to be fairly radiation-stable towards
the 11.1-GBq (Ra\\Be) neutron source with a nominal γ-dose of ca. 1.72
Gyh− 1. Tripathy et al. (2006) found that HMO adsorption towards
Cd(II) increased with the increasing pH with the optimum one of 6.05.
The adsorption of Cd(II) can be modeled either by the formation of
the SOCd+-type complex or as a combination of SOCd+ and SOCdOH-
type complexes, depending upon the nature of the electrolyte medium
(Tripathy et al., 2006). Heavy metal was adsorbed onto NMnOs via the
inner-sphere complex formation (Mishra, 2007). Sorption to NMnOs
could be described as a two-step process similar to HFO, i.e., a rapid
and reversible adsorption reaction to the external surface including
the macropores, followed by a slow surface diffusion along the micro-
pore walls of the oxides (Trivedi and Axe, 1999).
As an environmental friendly material, ZnO is a promising candidate
for catalysts (Lu et al., 2008), gas sensors (Jing and Zhan, 2008), solar
cells (Chou et al., 2007). As an adsorbent, ZnO was mostly applied to
eliminate H2S (Flytzani-Stephanopoulos et al., 2006). Recently,
nanosized ZnO was found to be capable of removing various contami-
nants with high performance and selectivity. Nanosized porous ZnO
plates with a pore diameter of 5–20 nm and a high specific surface
area (147 m2/g) were produced by Wang et al. (2010a,b). It showed
strong and selective adsorption towards cationic contaminants includ-
ing various toxic metals. It showed an unsaturated adsorption capacity
of N 1600 mg/g for Cu(II). Such strong, structurally enhanced adsorption
resulted from a large number of polar sites on the walls of pores within
the nanoplates. The adsorbed hydrated Cu(II) could partially hydrolyze,
leading to the formation of Cu\\O\\Cu on the pore walls and hence
multiply its adsorption capacity, thus exhibiting a Freundlich-type ad-
sorptive behavior (Wang et al., 2010a). Nanosized ZnO could also effi-
ciently remove other various contaminants. The maximum capacity of
nanosized ZnO at 303 K were 387 and 714 mg/g for Cd(II) and Hg(II)
ions, respectively (Sheela et al., 2012). It was suggested that the initial
adsorption rate was controlled by the film diffusion followed by the
pore diffusion (Sheela et al., 2012). Surface hydroxyl groups of
nanosized ZnO was proved to play a major role in adsorbing various
heavy metals as mentioned above (Ma et al., 2010).
MnOx and ZnO nanoparticle could also serve as catalyst for ad-
vanced oxidation process. Dong et al. (2009) synthesized β-MnO2
30 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39
nanowires for ozonation catalysis through a simple hydrothermal pro-
cess. The resultant β-MnO2 nanowires showed sound catalytic degrada-
tion of phenol. A series of flower-like ZnO nanotructures were
fabricated via bio-mediation using natural substances (Sharma, 2016).
The synthesized ZnO featured small crystallite size, abundant surface
defects, wide band gap and capability to hinder electron-hole pair re-
combination. It also exhibited significant photo-catalytic and antibacte-
rial activity. Another study suggested that the natural dye-sensitized
ZnO nanoparticles could effectively utilize solar light to degrade bacteria
and their organic contents (Zyoud et al., 2016). Furthermore, some
studies pointed out that, by doping N, Cu, Zr or Ce into nanosized
metal oxides, the photocatalytic activity and stability of similar metal
oxides nanoparticles could be significantly enhanced (Chen and Burda,
2008; Forouzani et al., 2015; Li et al., 2013).
3.3. Noble metal nanoparticles
Noble metals were commonly referred to certain transition metals
like Gold (Au), Silver (Ag), Platinum (Pt) and Palladium (Pd). They usu-
ally have high ionization energy owing to their small atom size, hence
low oxidation potential (Pradeep and Anshup, 2009). However, at
nanoscale, their ionization energy and oxidation potential changed sub-
stantially, allowing many novel reactions with noble metal feasible
(Schmid, 1992). The synthesis method of noble metal nanoparticles
was commonly through reduction of the corresponding metal salts
and controlled nanocrystal nucleation and growth with a stabilizing
agent. In many cases, polymers and surfactants were employed to en-
hance the stability of noble metal nanoparticles (Pradeep and Anshup,
2009).
Au and Ag nanoparticles have been extensively utilized for detection
of trace level of organic contaminants due to their unique optical prop-
erties (Sajanlal and Pradeep, 2008). It was reported that significant
Raman signal enhancement was observed in the presence of silver
nanostructures (Alula and Yang, 2014). Also, a clear correlation was
found between the shift in plasmon resonance wavelength and pesti-
cide concentration (Rajan et al., 2007). By modifying gold nanoparticle
surface with indoxyl groups, the signature of the functional groups
under the presence of pesticides was altered, with the detection limit
even reaching ppt level. Till now, various Ag/Pt, Au/Pt or Ag/Au bimetal-
lic nanoparticles based electrodes were studied for trace contaminants
sensing, monitoring and photocatalysis (Kumari et al., 2015; Tan et al.,
2015; Zhang et al., 2016a).
Besides contaminant monitoring, noble metal nanoparticles could
also been applied to adsorb the contaminants and to inactivate bacteri-
um. Au nanoparticles could effectively adsorb Hg by forming AuHg,
Au3Hg and AuHg3, with the capacity of 4.065 g/g Au (Sumesh et al.,
2011). The biocidal activity of silver nanoparticles was exploited for
water disinfection, water borne micro-organisms such as E. coli could
be inactivated in contact with Ag nanoparicles (Xiu et al., 2011). It was
suggested that Ag nanoparticles could cause damage to the cellular
membrane through direct contact, and their anti-bacterial activity was
dependent upon particle size and crystal shape. Higher atom density,
better anti-bacterial activity (Morones et al., 2005; Pal et al., 2007). Ag
nanoparticles were now widely used as disinfectant for surgical
masks, textile fibers and even mouthwash.
Noble metal nanoparticles were also being employed for photo-cat-
alytic degradation of various water contaminants such as pesticides,
dyes and halogenated organics. Noble metals could act like electron
sinks, inhibiting the photo-generated e −/h + recombination, while
promoting the surface charge separation (Pradeep and Anshup, 2009).
A various of noble metal based nanocomposites, e.g. Ag/ZnO and Pt/
ZnO nanocomposites (Munoz-Fernandez et al., 2016), Au\\CuS\\TiO2
nanobelts (Chen et al., 2016), Ag/AgBr/graphene-oxide nanocomposites
(Esmaeili and Entezari, 2016), were fabricated, and they all showed en-
hanced photocatalytic performance against certain organic contami-
nants. Some Ag, Pt and Pb based nanocatalyst could also be utilized for
catalytic energy conversion (Lang et al., 2012; Quan et al., 2015; Wen
et al., 2014a), which will not be detailed here.
4. Nanocomposites in water treatment
Most of the nanomaterials mentioned above are present as nanopar-
ticles. When concerning the large-scale application of nanoparticles in
water treatment, they have to face some inherent technical bottlenecks,
such as aggregation, difficult separation, leakage into the contact water,
potential adverse effect imposed on ecosystem and human health. One
promising approach to forward the application of nano-particulate ma-
terials is to develop nanocomposite materials that take advantages of
both the hosts and impregnated nanoparticles. In addition, nanocom-
posites could mitigate the release of nanoparticles into the environ-
ment, and improve the compatibility of nanotechnology with existing
infrastructures. Nanocomposite is essentially multiphase solid material,
including porous media, colloids, gels and copolymers in a broad sense.
The selection of hosts for nanocomposites is of great significance, and
even dominates the performance of the resultant nanocomposites.
Compared with free nanomaterials, the performance and usability of
nanocomposites were significantly improved, in terms of nanoparticle
dispersion, stability and recyclability. Hence, nanocomposite materials
could bridge the gap between nanoscopic and mesoscopic scale. Till
now, nanocomposites were believed to be the most promising way to
forward water nanotechnology from lab study to large scale application.
In this chapter, nanocomposites of inorganic and organic supports,
along with nanocomposite membranes and magnetic nanocomposites
of multi-functionality were discussed. Table 4 summarizes the advan-
tages and potential applications of various nanocomposites. Fig. 1 illus-
trated the structure of some typical nanocomposites and their
properties and unique functions.
4.1. Nanocomposites of organic supports
Polymers are unique supports for nanomaterials as they usually pos-
sess tunable porous structures, excellent mechanical properties and
chemically bounded functional groups. Polymer-based nanocomposites
(PNCs) are prospecting materials for their sound performance in water
and wastewater treatment. PNCs often incorporate the inherent advan-
tages of both the nanoparticles and the polymeric matrix (Pan et al.,
2014b; Zhao et al., 2011). PNCs could be fabricated by grafting NPs
into polymer structures, or by anchoring polymers to NPs (Mandavian
and Mirrahimi, 2010). Direct compounding and in situ synthesis are
two main strategies used for the fabrication of various PNCs (Lofrano
et al., 2016; Zhao et al., 2011). In particular, for direct compounding,
functional nanoparticles were directly introduced and grafted into the
polymers. Or, precursors of nanoparticles were first saturated inside
the pores of polymeric hosts, and then subjected to synthesis through
in-situ precipitation and nucleation by some specific initiators. Another
in-situ synthesis method was to add functional nanoparticles during the
polymerization of monomers (Fig. 2).
Some of the widely used polymeric hosts were alginate (Chen et al.,
2007; Chiew et al., 2016), macromolecule (polypyrrole) (Baig et al.,
2015; Chen et al., 2015a), polyaniline (Bushra et al., 2015; Khan et al.,
2014), porous resins (Chen et al., 2015b; Katsoyiannis and Zouboulis,
2002; Wang et al., 2011) and ion-exchangers (Blaney et al., 2007;
Cumbal and Sengupta, 2005a; Pan et al., 2007; Su et al., 2009; Zhang
et al., 2008b). Among them, one of the commonly used support was
cross-linked polystyrene ion-exchanger. This support featured unique
porous 3D structure. Its surface was amenable to modification with
functional groups (\\SO2− 3 and\\CH2N+(CH3)3), the positively or neg-
atively charged functional groups facilitating permeation and dispersion
of nanoparticle precursors (such as Zr4+ or FeCl4−) inside its pores. In
addition, the nano-confinement effect could promote in situ nucleation
and precipitation of nanoparticles (Pan et al., 2010; Zhang et al., 2013b).
Li et al. (2016) and Wang et al. (2011) found that by increasing the
 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39 31

Table 4
Different hosts for fabrication of environmental nanocomposites.

Hosts Advantages Properties

Graphene Laminar structures; high selectivity and transport rate towards water Adsorption, separation, antimicrobial
molecules; good mechanical strength
CNT Nano-channel for ultra-fast molecular transport; superb mechanical strength Adsorption, sensing
Activated carbon Low cost; high porosity; good compatibility Adsorption
Silica Remarkable mechanical strength; good chemical stabilities; tunable structure Adsorption, electrode materials, (photo)catalysis
Polymer Cross-linked structure for stable immobilization; excellent mechanical Adsorption, sensing, (photo)catalysis,
strength, chemical stability and compatibility; tunable structure; charged antimicrobial
surface promote dispersion of nanoparticles and contaminants; ease of separation
Bio-polymer Abundant and readily availlable resource; moderately flexible molecule; Adsorption, antimicrobial
hydrophilicity, chirality and eco-friendly
Minerals Low cost; chemical stability; heat resistance; eco-friendly; unique structure Adsorption, in-situ remediation
providing functional groups
Membranes Porous structure; tunable surface properties; chemical, thermal and mechanical Adsorption, separation, antimicrobial,
stability; stable nanoparticle incorporation; high compatibility (photo)catalysis
Magnetic substrate Ease of surface modification; easy to separate; fast kinetics Adsorption, (photo)catalysis, coagulation

cross-linking density of the polystyrene structure, the immobilized
nanoparticles of smaller size could be obtained through pore size effect,
and thereby enhance their activities. Furthermore, Pan et al. (2014a)
and Nie et al. (2013) revealed that the surface chemistry of the
nanosized hydrous manganese oxides (HMO) confined in polymeric
hosts were quite different from its bulky counterparts, where its pHpzc
shifted from 10.5 to 6.2, while the confined nanosized hydrous iron ox-
ides (HFO) exhibited a decreased pHpzc from 8.2 to 6.3.
These above-mentioned nanocomposites are of great potential for
contaminants removal. The impregnated nanoparticles, such as HFO
(Pan et al., 2009), ZrP (Zhang et al., 2008b), ZrO2 (Chen et al., 2015b),
PEI (Chen et al., 2010) and La(OH)n (Zhang et al., 2016c), often provided
specific bindings to target pollutants, including heavy metals (Cu, Pb,
Cr(III), Ni), As, F, and P. The contaminants were often removed through
multiple mechanisms including surface complexation, electrostatic at-
traction and co-precipitation (Pan et al., 2013). Also, the charged sup-
ports could facilitate pre-concentration and diffusion of certain
contaminants inside the pores of the nanocomposites (Jiang et al.,
2011). More importantly, the stability of the immobilized nanoparticles
was significantly enhanced. It was suggested that the cross-linked poly-
mer could protect the confined nanoparticles by so-called shielding ef-
fect. Cai et al. (2016) impregnated Li/Al LDH inside a polystyrene
anion exchanger, and the resultant nanocomposites showed enhanced
stability in the pH range of 3–12, while the bare LDH could only exist
stably at pH 4–10. Zhang et al. (2016c) fabricated a novel nanocompos-
ites La-201 by loading La into cross-linked polystyrene network. They

Fig. 1. Illustration of typical environmental nanocomposites and nano-enabled properties.

32 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39
Fig. 2. Illustration of synthesis methods for polymeric nano-composites.
found that La-201 was quite resistant to the influence of high concentra-
tion of humic acid. These PNCs could avoid problematic issues such as
nanoparticle dissolution, which was common when using free nanopar-
ticles (Zhao et al., 2011). Some of the nanocomposites were also amena-
ble to regeneration and reuse without significant capacity loss, which is
crucial from economical perspective. Because of the large size of the
PNCs, they could be easily separated from treated water, or packed in
columns without excessive pressure drop. However, till now, only a
handful studies were available to test the viability of polymeric nano-
composites in real wastewater treatment scenario. Commercial prod-
ucts such as ArsenXnp and HFO-201 were actually widely used
(Lofrano et al., 2016). Hua et al. (2013) recently scaled up the applica-
tion of HFO-201 nanocomposites for phosphate removal. The perfor-
mance of HFO-201 was stable and could effectively process ~1500 BV
real wastewater containing phosphorus. Furthermore, polymer sup-
ported nZVI was also applied for oxidative or reductive removal of con-
taminants such as As(III) and nitrate (Du et al., 2013; Jiang et al., 2011).
Other types of polymeric hosts are mainly bio-polymers such as chi-
tosan and cellulose. They are abundant in nature and relatively eco-
friendly. Cellulose is affluent worldwide (O'Connell et al., 2008). Bio-
polymers could suffer a serious problem in long-term application be-
cause they are biodegradable (Guibal, 2004). However, cellulose exhib-
ited good chemical stability and mechanical strength, due to its densely
and orderly aligned, hydrogen bonded molecules, which also granted it
sound swelling resistance (Sionkowska et al., 2002). It also exhibited
characteristics such as hydrophilicity and chirality (Klemm et al.,
2002). Cellulose-based NCs also possess adsorptive or ion exchange ca-
pability. They were usually resistant to microbiological attack and ex-
hibited sound thermal stability (O'Connell et al., 2008). Some
approaches were adopted to fabricate cellulose-based NCs. One is
quite similar with that of polymeric nanocomposites (O'Connell et al.,
2008). Wei et al. (2015) prepared gold nanoparticle/bacterial cellulose
(AuNP/BC) nanocomposites by citrate mediated in situ reduction of
Au3+ in the presence of a BC hydrogel at 303 K. They found that sorption
not only occurred on the top surface of AuNP/BC nanocomposite, but
also within the nanocomposite matrix. In addition, agitation could in-
tensify the surface enhanced Raman spectroscopy (SERS) response by
four times. Khan et al. (2013) immobilized ZrO2 on cellulose matrix
and obtained cellulose/ZrO2 nanohybrid particles, with an average size
of 50 nm. The nanohybrid showed high selectivity to Ni2+, with the ad-
sorption capacity at 79 mg/g. The adsorption process was mainly mono-
layer on homogeneous adsorbent surfaces. A nano-ZnO-cellulose fiber
was synthesized by Varaprasad et al. (2016) by adding ZnO nanoparti-
cles into solution containing cellulose fibers via sodium alginate matrix.
It was considered a good antibacterial agent.
Chitosan is the second most naturally abundant polysaccharide after
cellulose (Vunain et al., 2016). Chitosan has unique characteristics such
as high reactivity, excellent chelation behavior and chemical stability
(Vunain et al., 2016). The amino and hydroxyl groups of chitosan
serve as active sites for water pollutants (Vunain et al., 2016). Generally,
cross-linked chitosan was insoluble even at low pHs, so that they could
be used over a broad pH range (Bhatnagar and Sillanpaa, 2009). The en-
hanced adsorption of chitosan-based NCs towards various pollutants
were extensively documented (Babel and Kurniawan, 2003; Bhatnagar
and Sillanpaa, 2009; Chen et al., 2014; Crini, 2005; Jaiswal et al., 2012;
Ouyang et al., 2015). Liu et al. (2012b) synthesized chitosan/graphene
oxide (CSGO) composite with three different amounts of GO (5 wt%,
10 wt% and 15 wt%), and investigated the optimum condition for the ad-
sorption of Au(III) and Pd(II) at pH 3.0–4.0. Chitosan with 5 wt%
graphene oxide (CSGO5) composite possessed the highest capacity of
1077 mg/g for Au(III) and 217 mg/g for Pd(II). Djerahov et al. (2016)
prepared a stable CS-AgNPs colloid by dispersing the AgNPs sol in chito-
san solution, and further used it to obtain a cast film with high stability
under storage and good mechanical strength for handling. It showed ef-
ficient separation and extraction of Al(III), Cd(II), Cu(II), Co(II), Fe(III),
Ni(II), Pb(II) and Zn(II). Approximately 95% removal for most studied el-
ements and around 16% for Mn(II). Ouyang et al. (2015) synthesized
spherical chitosan-CNT composite beads via freeze casting by dropping
a mixed solution into liquid nitrogen, and the resulting highly porous
composite beads contain radially oriented channels with hybrid chito-
san–CNT channel walls. The composite beads exhibited hierarchical
open-porous structure and mesopores from the exposed CNTs, and
showed high adsorption towards bilirubin (43.6 mg/g) within 2 h.
Jaiswal et al. (2012) applied copper-coated chitosan nanocomposite
(CuCH) to remove malathion, a organophosphorous pesticides, from ag-
ricultural runoff. The maximum capacity reached 322.6 ± 3.5 mg/g at an
optimum pH of 2.0. Furthermore, Mansur et al. (2014) developed a ZnS
quantum dots/chitosan nanocomposite to serve as high-performance
heterogeneous photocatalyst. The material was synthesized based on
colloidal chemical method at room temperature. Under UV irradiation,
methylene blue and methyl orange dyes were effectively degraded
through oxidation in 120 min.
4.2. Nanocomposites of inorganic supports
Inorganic supports for nanocomposites mainly include activated car-
bon, CNTs, as well as natural minerals such as zeolite, biochar and clay.
Activated carbon (AC) is a classic adsorbent widely applied in water
and wastewater treatment facilities. AC is a highly porous adsorbent of
sufficient micropores (specific surface area 100–2000 m2/g) and hydro-
phobic surface, which could serve as an excellent support for nanopar-
ticles (Foo and Hameed, 2010). Arcibar-Orozco et al. (2012)
immobilized iron oxyhydroxide nanoparticles onto granular AC via
forced hydrolysis of FeCl3, and found that the size of loaded iron nano-
particles could be significantly reduced by addition of phosphate. The
resultant AC-iron nanocomposites showed a 40% increase on As(V) ad-
sorption capacity (PO4/Fe = 1.5) over the virgin sample. Nano-ZnO was
loaded to granular activated carbon to enhance its removal capability
 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39
for Pb(II) with a capacity of 76.7 mg/g (Kikuchi et al., 2006). The surface
functional groups responsible for Pb(II) adsorption were considered to
be hydroxyl groups formed on the oxides. AC nanocomposites embed-
ded with magnetite (Fe3O4) showed remarkable performance in remov-
ing aromatic pollutants. The saturated adsorbent could be recycled by
using ethanol as back-wash agent (Furlan and Melcer, 2014). Further-
more, a Fe/Pb bimetallic nanoparticle impregnated AC was developed
by reductive deposition using NaBH4. The immobilized Fe/Pb nano-
alloy was well dispersed and stable. 90% of 2-chlorobiphenyl were re-
duced by the as-synthesized AC nanocomposite in 48 h, and the residual
2-chlorobiphenyl and the dechlorination products were simultaneously
adsorbed (Choi et al., 2008).
CNT-nanocomposites (CNT-NCs) refer to materials that contain two
or more ingredients prepared to form a composite mixture with CNTs as
the primary host (Upadhyayula and Gadhamshetty, 2010). Nabid et al.
(2014) synthesized the poly 1,8–diaminonaphthalene/MWCNTs-
COOH hybrid material which could be used as an effective sorbents for
the separation and preconcentration of Cd(II) and Pb(II) at trace levels.
The bounded extractive sites on polymers/MWCNTs-COOH exhibited
high affinity to heavy metals. The maximum capacity for Cd(II) and
Pb(II) were 101.2 and 175.2 mg/g and the detection limits of this meth-
od for the two heavy metals are 0.09 and 0.7 ng/mL, respectively. Shao
et al. (2011) examined the adsorption of 4,4′-DCB by using MWCNTs
grafted with methyl methacrylate (MMA). Konicki et al. (2012) used
M-MWCNT–Fe3C nanocomposite (M-MWCNT-ICN) to remove red 23
from aqueous solution with a maximum capacity of 85.5 mg/g.
Zeolite generally consists of silicon-oxygen tetrahedron and alumi-
num-oxygen tetrahedron. Zeolite is widely used as adsorbents, ion-ex-
change materials and catalysts due to the low cost and the unique
internal structure, which provides abundant binding sites. Mthombo
et al. (2011) studied the adsorption behavior of Cu(II), Pb(II), and
Co(II) onto ethylene vinyl acetate-clinoptilolite nanocomposites. The
results showed that nanocomposites filled with HCl-activated particles
demonstrated a high capacity for the three metals. Khatamian and
Alaji (2012) prepared ZnO/HZSM-5 nanocomposites for the adsorption
of 4-nitrophenol (4-NPh). They observed that about 91% of 4-NPh
(20 mg/L initially) was removed within 90 min at pH = 5. Chong et
al. (2015) synthesized TiO2-zeolite nanocomposites for the advanced
treatment of industrial dyes. The results indicated that the nanocom-
posite followed an adsorption-oriented photocatalytic degradation,
which is particularly effective for removing trace dye compounds.
Biochar is a carbon-rich material produced from biomass pyrolysis in
anaerobic environment (Sohi, 2012). It is widely available and of low
cost. Development of biochar-based nanocomposites could achieve in-
tegrated objectives such as water pollution control, waste disposal and
carbon sequestration. Biochar nanocomposites were usually designed
through two different pathways, pre-enriching biomass using nanopar-
ticle precursors or direct impregnation of nanoparticles after pyrolysis
(Tan et al., 2016). γ-Fe2O3/biochar nanocomposites could be directly
synthesized by thermal pyrolysis of FeCl3 pretreated biomass, which ex-
hibited good adsorption towards As(V) (Zhang et al., 2013a). Inyang et
al. (2014) fabricated CNTs coated biochar composites with a large spe-
cific surface area of 359 m2/g. The material showed sound adsorption
towards dye pollutants. Biochar/MgO nanocomposites fabricated by
Zhang et al. (2012) exhibited extremely high phosphate adsorption of
835 mg/g. The adsorption was usually realized by multiple mechanism
such as ion-exchange, π-cation interaction, surface complexation, and
co-precipitation. Additionally, a novel graphitic C3N4 biochar nanocom-
posite was applied to remove dyes through simultaneous adsorption
and catalytic degradation (Beesley et al., 2011; Tan et al., 2016). Most
mineral based nanocomposites were powder-like and was suitable for
in-situ remediation. Currently, more attentions were drawn to magnetic
nanocomposites because it facilitated readily separation and collection
(Faghihian et al., 2013).
Clay-based polymeric nanocomposites (CPNs) are a blend of poly-
mer and inorganic clay minerals, which take advantages of both organic
33
and inorganic hosts. CPNs showed dramatically enhanced mechanical
and chemical stability, heat resistance, high surface area, and decreased
gas permeability. Various CPNs were widely applied for the removal of
inorganic and organic micro-pollutants such as Co(II), Zn(II), Se(IV)
and atrazine (Scocchi et al., 2007; Unuabonah and Taubert, 2014). A
Cu/polyethylene/montmorillonite CPN were observed to show strong
anti-microbial activity to E. coli (Bruna et al., 2012). A sepiolite-
PDADMAC (polydiallydiamethylammonium) CPNs were employed for
wastewater pre-treatment, resulting in an efficient treatment of a win-
ery effluent with 1610 mg/L TSS through coaguflocculation in b 2 min
(Rytwo, 2012). In general, CPNs are promising sustainable materials
for pollutants removal.
4.3. Nanocomposite membrane
Nanocomposites membranes can be roughly classified into three
categories: 1) conventional nanocomposite membrane, 2) thin-film
nanocomposite and 3) surface coated nanocomposite membrane. The
first one was usually synthesized by phase inversion method, where
the nanoparticles were loaded onto the pores and substrate of the mem-
brane. For the thin-film nanocomposite, an ultra-thin film was coated
on the substrate as a barrier layer, as widely used in the RO/NF mem-
brane. Nanomaterials were loaded into the thin-film during the phase
inversion and interfacial polymerization process. For the third category,
functional nanomaterials could be coated to membrane surface through
self-assembly, in-situ deposition, adsorption or chemical grafting (Goh
et al., 2016; Lau et al., 2015; Yin and Deng, 2015).
Nanocomposite membrane coated with functional nanoparticles
like nano-TiO2 (Yang et al., 2012) exhibited hyper-catalytic or photo-re-
activity properties (Yin and Deng, 2015). Under UV irradiation, TiO2 im-
bedded PES membrane showed enhanced antifouling capability
(Athanasekou et al., 2015). Liu et al. (2016) reported a novel anatase/
tetanate nanocomposite membrane that could simultaneously remove
Cr(VI) and 4-chlorophenol through adsorption and photocatalytic oxi-
dation. Photo-catalysis self-cleaning was achieved by nano-ZnO/PVDF
membrane and TiO2 thin film nanocomposite, which facilitated the re-
covery of water flux through the membrane (Banerjee et al., 2015;
Hong and He, 2014). Yan et al. (2005) immobilized alumina nanoparti-
cles during phase inversion of PVDF for the production of a mixed ma-
trix UF membrane. This process dramatically enhanced hydrophilicity,
water permeability, fouling resistance, flux recovery, and mechanical
stability, while pore density and size remained unchanged. Such mem-
brane combines the good mechanical strength of polymeric membrane
and high reactivity or specific functionality of inorganic nanoparticles.
Enhanced water permeability was also found in membrane embedded
with ZrO2 nanoparticles (Arsuaga et al., 2013). Impregnation of silver
nanoparticles (AgNp) into the membrane would allow the membrane
to be antibacterial. Instead of loading Ag into organic phase during inter-
facial polymerization process, Yin et al. (2013) coated AgNp onto the
thin-film surface of the membrane, resulting in the inhibited dissolution
of AgNp and Ag+ into the environment. The fabricated thin-film nano-
composite showed excellent antibacterial performance along with en-
hanced water flux.
A CNT embedded membrane was reported by Chen et al. (2012b).
The membrane was fabricated by depositing CNT onto ceramic mem-
brane through chemical vapor. It integrated the function of ceramic
pore channels and the grown CNTs in the pores. The optimized CNT-ce-
ramic membrane featured 100% rejection rate to oil and a flux rate of 36
L/h m2/bar. It also showed certain resistance to organic fouling. In addi-
tion, graphene-based nanocomposites exhibited huge potential in
membrane based water purification, minimizing the transport resis-
tance and simultaneously maximizing the permeate flux (Cao et al.,
2014; Liu et al., 2015; Mahmoud et al., 2015). Cao et al. (2014) fabricat-
ed a graphene-based nanocomposites through combining graphene
oxide (GO) with sodium alginate. The resultant composite showed
high selectivity and transport rate towards water molecules. This
34 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39
property should be ascribed to the presence of oxygen-containing
groups, structural defects, edge-to-edge slits and non-oxides regions
of GO nanosheets, which could provide abundant water channels.
When GO concentration reached 1.6 wt%, an optimum permeation
flux of 1699 g/(m2 h) was achieved. Furthermore, they claimed that
the smaller nanosheet size, more structural defects and fewer oxygen-
containing groups of GO could construct more water channels. A thin
film nanocomposite (TFN) membrane was fabricated by incorporating
GO of different quantity (ranging from 0 to 0.5 wt%) into polysulfone
(PSf) microporous substrate. As to pure water flux, TFN membrane
made of 0.3 wt% GO exhibited the highest water permeability with re-
jections for Na2SO4, MgSO4, MgCl2 and NaCl recorded at 95.2%, 91.1%,
62.1% and 59.5%, respectively (Lai et al., 2016). Apart from promoting
molecular transport through membranes, graphene-based nanocom-
posite membranes also possess anti-biofouling properties (Liu et al.,
2015). Such satisfactory properties could also be attributed to the pres-
ence of oxygen-containing groups, resulting in an increased surface hy-
drophilicity and enhanced negative zeta potential, which could repel
microorganism through electro-repulsion and impede the surface at-
tachment of the microorganism. In conclusion, the development of
nanocomposite membranes have broadened and enhanced the applica-
tion of membrane technology drastically. Considering the commercial
maturity of membrane technology, nanomaterial-enabled membranes
hold great potential for large-scale application.
4.4. Magnetic nanocomposites
Magnetic nanocomposites are a class of unique nanomaterials. They
usually feature a core-shell nanostructure that could be easily and swift-
ly recovered with an external magnetic field. Functional nanoparticles
or functional groups could be grafted or immobilized onto Fe3O4 nano-
particles through chemical bounding or direct deposition (Gómez-
Pastora et al., 2016). The materials to be coated include Ag, TiO2, CNTs,
GO, Pd and SiO2, and so on. SiO2 coating could provide high surface
area and sound porosity, while protecting the magnetic core from corro-
sion. After coating, the resultant magnetic nanocomposites often exhib-
ited enhanced adsorption or photocatalytic capability with fast kinetics
towards contaminants such as heavy metals, dyes, phenolic compounds
or microbial (An et al., 2014; Colmenares et al., 2016; Ferroudj et al.,
2013; Mahmood et al., 2014; Sharma et al., 2015).
In recent years, Cui et al. (2013, 2014a, b) synthesized a series of po-
rous Mn-based magnetic nanowires to remove heavy metals, As(III) and
some organic pollutants. A simple one-step solvothermal method was
also suggested to fabricate magnetic carbon hollow spheres, which
was highly efficient for heavy metal removal (Cui et al., 2014b). In addi-
tion, a maghemite/silica nanocomposite was synthesized and used as
heterogeneous Fenton catalyst. It could efficiently degrade pollutants
like PNP and MB (Ferroudj et al., 2013). Long-term usage witnessed
negligible Fe leaching. Jin et al. (2014) suggested magnetic nanoparti-
cles modified with amino acid could capture N 94% of bacterial cells
over a pH range of 4–10 within 20 min. Shan et al. (2015) found
poly(1-vinylimidazole)-grafted Fe3O4@SiO2 nanocomposite could ef-
fectively adsorb Hg(II) at pH 7, with the capacity of 346 mg/g. The
exhausted adsorbent could be generated with 0.50 M HCl in merely
10 min. Another particular interesting magnetic nanoparticle of multi-
functionality was developed by Zhang et al. (2016b), where a
polyethylenimine-derived corona was coated around the magnetic
core. The resultant nanomaterial could inactivate bacterial through
cell membrane penetration, while capturing heavy metal through che-
lation and adsorbing anions by electrostatic attraction. The nanocom-
posite could be regenerated and reused by EDTA and NaOH. In
addition, magnetic nanocomposites were also used to accelerate the co-
agulation of sewage (Booker et al., 1991), and some polymer-coated
magnetic nanoparticles were tested for in-situ oil spill remediation
(Gu et al., 2014; Orbell et al., 1997).
Generally speaking, magnetic nanocomposites are diverse materials
of great potential for real water remediation. However, the cost for syn-
thesis and its compatibility with current infrastructure should be con-
sidered in further study.
4.5. Reusability of nanocomposites
The regeneration of the exhausted nanocomposites is of great im-
portance to improve their sustainability. Usually, acidic and basic solu-
tions were used to rinse the nanocomposites, dependent upon their
structure, the nature of the captured contaminants as well as the remov-
al mechanism. The common desorption reagents included HCl, HNO3,
NaCl, CH3COONa, NaOH, NaCO3 and NaHCO3 (Anirudhan and
Suchithra, 2010). Another option is solvent (organic) extraction, and
the solvent selection and its cost effectiveness should be particularly
considered (Unuabonah and Taubert, 2014). Furthermore, mixture of
organic solvent and aqueous solution may reach a rewarding effect in
some cases (Unuabonah and Taubert, 2014). Advanced oxidative ap-
proaches using Fenton reagents, thermal (re)activation, or photocata-
lytic approaches were also viable for both material regeneration and
brine disposal. However, they were not suitable for the regeneration
of nanocomposites of organic supports, as oxidation would likely
cause the hosts to break down (Unuabonah and Taubert, 2014). Devel-
opment of new regeneration methods for the nanocomposite materials
would make them more attractive and sustainable in industrial
application.
5. Concluding remarks
Nanomaterials are widely explored as highly efficient adsorbents,
(photo)catalyst and disinfectant for water treatment. Generally, they
exhibited various merits, such as high capacity, fast kinetics, specific af-
finity towards targeted contaminants, enhanced photocatalytic re-
sponse for a broad light spectrum, and strong anti-bacterial activity.
They are arguably the most promising candidate for the development
of next generation water treatment technology. Of particular note is
that, there are still many obstacles to overcome for engineering applica-
tion of nanomaterials. Firstly, nanomaterials are usually unstable, tend
to agglomerate due to the presence of van der Waals forces and other
interactions. Secondly, it is still challenging to recycle nanomaterials
from treated water except for magnetic nanoparticles, render the use
of nanomaterial uneconomic or sometimes unfeasible. Last but not the
least, the long-term fate, transformation and toxicity of nanoparticles
are not clearly understood.
One promising approach to forward the application of
nanomaterials is to develop nanocomposite materials that take advan-
tages of both the hosts and the impregnated functional nanoparticles.
Hosts like polymers, bio-polymers, minerals, activated carbons or mem-
branes could facilitate the dispersion and stability of the loaded nano-
particles. They could also promote the transfer or diffusion of
contaminants in the hosts, further enhancing the interfacial interaction.
Nanocomposites could also effectively mitigate the release of nanopar-
ticles into the receiving water. Moreover, nanocomposites could im-
prove the compatibility of nanotechnology with existing infrastructure
like fixed-bed column or fluidized bed. We believe that nanocomposites
enabled water nanotechnology could considerably alter the current
water treatment modes. Future work should forward the understanding
of interactions between immobilized nanoparticles and hosts, develop-
ing techniques for host structure and nanoparticle manipulation, and
guiding the design of more rationale nanomaterials of multi-
functionality.
Meanwhile, the impacts and risks of the environmental
nanomaterials should be further focused on, and their synthesis via
green chemistry to diminish their environmental impact should also
be pursued in parallel. Protocols and guidelines should be established
to regulate the use of nanomaterials to minimize their impact to
 Y. Zhang et al. / NanoImpact 3–4 (2016) 22–39
human health and aquatic environment. These protocols, standards and
guidelines are expected to be built based on our deep understanding on
the nano impact.
Acknowledgement
This study was financially supported by National Key Research and
Development Program of China (Grant No. 2016YFA0203104) and
NSFC (Grant 51578024 and 51378249).
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