Accepted Manuscript

Review

Nanoparticles in household level water treatment: An overview

Prathna TC, Saroj Kumar Sharma, Maria Kennedy

PII: S1383-5866(17)33252-5
DOI: https://doi.org/10.1016/j.seppur.2018.01.061
Reference: SEPPUR 14355

To appear in: Separation and Purification Technology

Received Date: 5 October 2017

Revised Date: 16 January 2018
Accepted Date: 27 January 2018

Please cite this article as: P. TC, S. Kumar Sharma, M. Kennedy, Nanoparticles in household level water treatment:
An overview, Separation and Purification Technology (2018), doi: https://doi.org/10.1016/j.seppur.2018.01.061

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 Nanoparticles in household level water treatment: An overview

Prathna TC1*, Saroj Kumar Sharma1, Maria Kennedy1,2

1
Environmental Engineering and Water Technology Department, IHE Delft Institute for Water Education, 2601
DA, Delft, The Netherlands
2
Faculty of Civil Engineering, Delft University of Technology, Stevinweg 1, 2628 CN, Delft, The Netherlands
*Corresponding author: Email: [email protected]

Abstract

Providing safe drinking water is a great challenge for both the developing and the developed
world. Increasing demand and source water quality deterioration has led to the exploration of
new technological innovations for better water management. Nanotechnology holds great
promise in ensuring safe drinking water through designing innovative centralised and
decentralised (household-level) water treatment systems. The paper provides an overview of
recent advances in nanotechnologies for (household level) water treatment processes, such as
its use as nanoadsorbents, photocatalysts, microbial disinfectants and in membranes.
Extensive implementation of nanotechnology for water treatment would require overcoming
the high cost of the nanomaterials by enabling their reuse and regeneration. This would also
ensure minimising potential environmental exposure. Potential advances in nanotechnology
must go hand in hand with environmental health to alleviate any undesirable consequences to
humans.

Keywords: Nanoparticles, water treatment, household level

1. Introduction

Safe drinking water is considered a vital indicator of a country`s development and according
to recent reports, about 663 million people around the world do not have access to safe
drinking water (WHO/UNICEF, 2015). Pollution and indiscriminate exploitation of surface
water over the years has led to dependence on groundwater for potable purposes by over 50%
of the global population (Ayoob et al., 2008). However, groundwater is a haven for several
naturally occurring and anthropogenic ions such as fluoride, arsenic, lead, chromium, nitrate,
selenium, chloride, heavy metals as well as radioactive materials which greatly compromise
groundwater quality leading to health problems (Jadhav et al., 2015). In addition, pathogens
such as adenovirus, hepatitis A, rotavirus to name a few, are commonly found in both surface
and groundwater and must be effectively inactivated to provide safe water (Hamza et al.,
2009). Drinking water safety is judged by national standard standards or international
guidelines with WHO guidelines for drinking water quality being among the most significant
one and implemented by many developing countries (WHO, 2011). Reports suggest that over
a billion of the estimated 6.2 billion people relying on improved water sources continue to use
water that is unsafe (Bartram et al., 2014). One of the Sustainable Development Goals of the
United Nations (SDG 6) is to achieve safe and affordable drinking water for all by 2030.
Advances in water treatment techniques can play a role in achieving this goal (United
Nations, 2015).

Drinking water treatment with regard to public water supplies generally consists of a series of
barriers in a treatment train that generally vary according to the requirements of the supply
and the vulnerability of the water source (Fawell and Nieuwenhuijsen, 2003). Among the
various technologies traditionally applied for drinking water treatment, sand (granular media)
filtration is one among the oldest treatment techniques. Sand filtration was initially believed
to work by size exclusion through inter-particle interstices. However, later studied revealed
that slow sand filters (SSF) develop an active biofilm (called Schmutzdecke) around the sand
particles that are rich in bacterial population and thereby improve the filtration power of the
media (Johnson, 1914). One of the challenges with the application of granular media filtration
was its inability to effectively remove chemical contaminants besides its vulnerability to
accidents and changes in flow rate (Mwakabona et al., 2017). Some of the other
conventionally used techniques include chemical oxidation, adsorption, chemical
precipitation/ coagulation, ion exchange to name a few (Chubar, 2011; Behbahani et al.,
2011). The most common chemical oxidant used is chlorine which provides an effective and
robust barrier to pathogens (Fawell and Nieuwenhuijsen, 2003). Chemical precipitation, on
the other hand, works by the addition of counter ions to reduce the solubility of ionic
contaminants (Wang et al., 2006). This is usually followed by flocculation and sedimentation
or filtration (Jadhav et al., 2015). Of all the technologies, adsorption is the most technically
feasible and economically attractive approach for removal of arsenic, fluoride and heavy
metals from water in areas with no access to centralized water treatment approaches
(Petrusevski et al., 2008).

Recent years have witnessed increased interest on the application of nanoparticles as

adsorbents in water treatment. Nanotechnology shows great promise as the best feasible way
to treat persistent as well as emerging contaminants (Brame et al., 2011). Nanomaterial based
adsorbents offer attractive alternatives to conventional adsorbents in view of their higher
aspect ratio, enhanced reactivity which in turn translate to higher adsorption capacity (Das et
al., 2014). In addition, nano-adsorbents offer additional possibilities such as the possibility to
be used at household level in different forms, for example, in powder form, coated onto a
substrate or in a filter etc. The smaller size of the particles also provides the possibility of
constructing compact treatment systems. Recent studies have also shown that nanoparticles
can be engineered to target multiple contaminants at the same time (Qiao et al., 2014) thereby
possibly reducing the treatment cost. However, there are emerging concerns over the safe
disposal of nanomaterials and their potential risk to public health and the ecosystem, opening
up a new field known as nanotoxicology. In addition, other issues like relatively higher
production cost (as compared to commonly used adsorbents), operation and management of
the treatment system may be potential limitations in the application of nanotechnology for
household level water treatment.

Accordingly, this review provides a detailed insight into existing technologies involving the
use of nanoparticles in water treatment. Although, there is considerable research on the use of
nanoparticles in water treatment, there are hardly any comprehensive reviews providing a
critical analysis on the subject. This review attempts to fill this void.

2. Application of nanoparticles in water treatment

The development and use of novel nanomaterials for environmental protection and water
treatment in particular, has received widespread attention in recent years in view of their
larger surface area to volume ratio and smaller particle size (Zhong et al., 2007; Prathna et al.,
2017). An extensive search on the database (Google Scholar) for nanoparticle application for
drinking water treatment reveals 47,200 entries till date with ~7000 entries in 2017 alone. The
search terms for the database were “nanoparticles” and “drinking water treatment”. This
clearly shows the increased interest in exploring application of nanoparticles for water
treatment. It is worth to mention that silver and iron oxide nanoparticles contribute to the
majority of publications as regard to their application in water treatment. Figure 1 shows the
number of publications in the last five years on the application of silver and iron oxide
nanoparticles in drinking water treatment. The keywords for the search were “iron oxide
nanoparticles”, “silver nanoparticles” and “drinking water treatment”. It was found that
silver nanoparticles were mainly used in studies as disinfection agents for drinking water
treatment whereas the major role of iron oxide nanoparticles were for the removal of arsenic
and other hazardous contaminants in drinking water. The four major areas of application of
nanomaterials in water treatment are (a) adsorptive removal, (b) catalytic degradation, (c)
disinfection, and (d) membrane filtration (Li et al., 2008). Among these, adsorptive removal
of contaminants and disinfection using nanomaterials contribute to the bulk of publications.
Nanotechnology enabled water treatment practices promise to overcome major challenges
currently facing existing technologies and also provide new treatment strategies for economic
utilization of water resources (Qu et al., 2013).

9000
8000 Silver Iron Oxide
Number of Publications

7000
6000
5000
4000
3000
2000
1000
0
2017 2016 2015 2014 2013
Year

Figure 1: Number of publications on silver and iron oxide nanoparticles in drinking

water treatment included in Google Scholar (2013-2017)
2.1. Adsorptive removal

Different classes of nanoparticles have been used for adsorptive removal studies, namely, iron
based nanoparticles for arsenic removal, carbon and aluminium based nanomaterials for
fluoride removal etc. (Jadhav et al., 2015). In this review commonly used nano-adsorbents in
various Point of Use (POU) drinking water treatment systems have been described in detail.

2.1.1. Batch adsorption studies

Carbon nanotubes are an interesting group of nanomaterials which have been widely studied
in view of their high mechanical strength and electrical conductivity. Carbon nanotubes have
been extensively employed in combination with other nanomaterials for the removal of
fluoride from water (Li et al., 2001; Li et al., 2003). Recently modified multi-walled carbon
nanotubes have been used extensively for the removal of a number of heavy metals from
water (Wang et al., 2007; Wang et al., 2012; Zhang et al., 2012; Li et al., 2011). Graphene
based nanomaterials have been used to remediate Pb (II) ions from water (Zhao et al., 2011).
Other nanomaterials such as alumina are used extensively for the removal of fluoride while
magnetic nanomaterials are used for the removal of arsenic from water (Jadhav et al., 2015).
Studies have been carried out to effectively remove organic contaminants using
semiconductor ZnS and TiO2 nanomaterials (Linsebigler et al., 1995; Hu et al., 2005) while
zero-valent iron and bimetallic Fe (0) nanoparticles have been used to remediate both organic
and inorganic contaminants (Zhang et al., 2005; Bang et al., 2005).

Furthermore , significant work is being done on the development of suitable nano-adsorbent

for the simultaneous removal of multiple contaminants. 3D flower like iron oxide
nanostructures have been developed for the simultaneous removal of As (V), Cr (VI) and azo
dye Orange II (Zhong et al., 2006). In another related study, ceria 3D flower like
nanostructures were used for the effective removal of As (V) and Cr (VI) from contaminated
waters (Zhong et al., 2007). Simultaneous removal of the most toxic contaminants in drinking
water, namely arsenic and fluoride has been studied by Li et al. (2011) using mesoporous
alumina.

2.1.1.1.Characterization of nano-adsorbents

The preparation and characterization of nano-adsorbents used in water treatment is the first
step which determines its eventual applicability. Some of the commonly used techniques for
the synthesis of nanomaterials for adsorption are physical methods like laser ablation, spray
pyrolysis, inert gas condensation and chemical methods like reduction, co-precipitation as
well as biological methods such as using microbes and plant extracts etc as reductants (Palkar,
1999; Kornak et al., 2005). The synthesized nanomaterials are commonly characterized using
UV visible spectroscopy, X ray diffraction, particle size analysis, Electron Microscopy among
others (Prathna et al., 2011; Ali et al., 2012). Figure 2 shows the flowchart denoting the
various characterization techniques of nanoparticles. Majority of the characterization
techniques can be grouped into three classes namely (i) preliminary characterization (ii)
surface analytical techniques and (iii) particle size determining techniques while
concentration of nanoparticles can be determined using concentration analysis. Some of the
techniques used for characterization of nanoparticles are mentioned below.

2.1.1.1.1. Preliminary characterization

UV visible spectroscopy is a commonly used technique based on Beer Lambert law for
detection of noble metal nanoparticles in particular. The position of the Surface Plasmon
Resonant (SPR) peak and its absorption maxima depends on the size and shape of the
nanoparticle (Mulvaney, 1996). For example, when the shape of gold nanoparticles changes to
the form of nanorods, the SPR mode shifts from 517 nm to 850 nm (Bhattacharya and
Srivastava, 2003).

X ray diffraction is another technique that is used to confirm the type of nanoparticles. Each
class of nanoparticles produces its specific diffraction pattern and can be used for
identification. For example, silver nanoparticles show the presence of five peaks
corresponding to five different facets of silver namely (111), (200), (220), (311) and (222)
(Prathna et al., 2011).

2.1.1.1.2. Surface analytical techniques

Fourier Transform Infra Red Spectroscopy is a commonly used technique to determine the
surface functional groups on the particle. This spectroscopy is associated with vibrational
energy of atoms or group of atoms in a material and the IR spectra can be called the
“fingerprint” of a molecule. The IR spectra of nanoparticles differ considerably from their
bulk counterpart in view of the higher surface area to volume ratio of the former (Eastman et
al., 1993).

The surface potential of nanoparticles in a solution can be measured using zeta potential
analysis. For any solution to be stable, the zeta potential should be above +20 mV or below -
20 mV (Savage and Hieftje, 1979). Zeta potential measurements are usually carried out by
suspending a dilute solution containing nanoparticles in potassium nitrate or chloride solution.

The total surface area of nanoparticles can be effectively measured using Brunauer-Emmett-
Teller (BET) analysis (Prathna et al., 2017). Since many useful properties of nanoparticles
arise due to their smaller size, it is essential to be able to determine their surface area.
However, BET analysis has few shortcomings when compared to techniques like Nuclear
Magnetic Resonance (NMR) spectroscopy. BET analysis can only be done on dry powders
and the technique is time consuming since adsorption of gas molecules takes time.

Surface Enhanced Raman Scattering (SERS) Spectroscopy is a linear Raman technique

carried out on metallic nanoparticles (Vanhecke et al., 2014). It offers many advantages such
as high sensitivity, fingerprinting ability, minimal sample preparation, resistance to
photobleaching and ease of operation. Recent studies have demonstrated that it is possible to
correlate SERS signal with concentration of nanoparticles labelled with Raman reporters
(Sirimuthu et al., 2010).

2.1.1.1.3. Particle size determining techniques

The primary and secondary particle size of nanoparticles can be determined using electron
microscopic techniques (Scanning (SEM) and Transmission Electron Microscopy (TEM)),
Atomic Force Microscopy (AFM) and using a Particle Size Analyzer. AFM provides
information about size, morphology, surface roughness of particles ranging from 1 nm to 8
µm and need not be operated under vacuum conditions. TEM provides an unmatched
resolution of 1 nm and can be used to determine aggregation state and size of particles
(Vanhecke et al., 2014). The particle size of nanoparticles in solution can be determined using
a Particle Size Analyzer which is based on Dynamic Light Scattering (DLS). The particle size
in solution is generally increased due to various forces of attraction such as van der Waals
force of attraction. Figure 3 shows various microscopic techniques used for the analysis of
nanoparticles used in water treatment.

2.1.1.1.4. Concentration analysis

The elements of nanoparticles and their concentrations can be effectively determined using
Inductively Coupled Plasma (ICP) techniques including ICP-MS (Mass Spectroscopy) or
Optical Emission Spectrometer (OES)) (Vanhecke et al., 2014). These techniques are hard
ionization source elemental spectroscopies and are powerful tools for detecting and analysing
trace and ultra-trace elements in the solution (with a detection limit of <1 µg/L). The
nanoparticle containing solutions are first digested with concentrated acid and then diluted
prior to analysis. ICP-OES systems have been determined to have 2-3 orders of magnitude
higher detection limits than ICP-MS (Olesik, 1991). Atomic Absorption Spectroscopy (AAS)
and ICP-AES (Atomic Emission Spectroscopy) are other similar techniques used for
concentration analysis of nanoparticles (Prathna et al., 2014).
Figure 2: Flowchart showing different characterization techniques for nano-adsorbents
Figure 3: Commonly used microscopic techniques for nano-adsorbents used in water
treatment. (a) AFM microscopy of alumina nanoparticles (b) SEM micrograph of iron
oxide nanoparticles (c) FE-SEM micrograph of alumina nanoparticles (d) HR-TEM
micrograph of iron oxide based nanomaterials

The adsorption mechanism of the contaminant onto the nanomaterial can often be explained
by various models such as Langmuir, Freundlich, interparticle diffusion, Lagergren to name a
few (Ali et al., 2012). Table 1 gives a summary of application of various nanoparticles used in
drinking water treatment by adsorption.

Table 1: Summary of nanoparticles used for contaminant removal for drinking water
treatment

Nanoparticles Contaminant Adsorption Reference

capacity (mg/g)
MgO F 21.1 Oladoja et al.
(2016)
Fe-Al-Ce F 2.22 Chen et al. (2009)
Fe3O4 As (III), As 46.06 - As (III) Feng et al. (2012)
(V) 16.56 - As (V)
Jute fiber Fe2O3 composite As (V) 48.06 Sahu et al. (2017)
SO4 doped Fe3O4/Al2O3 F 70.4 Chai et al. (2013)
GO Pb (II) 1119 Sitko et al. (2013)
CNT dendrimer Pb (II) 4870 Hayati et al.
(2017)
PGMA coated Fe3O4 Cd (II) 48.53 Hasanzadeh et al.
(2017)
Chitosan bound Fe3O4 Cu (II) 21.5 Chang et al.
(2005)
SDS coated Fe3O4 Cu (II), Ni (II), 24.3 - Cu (II) Adeli et al. (2017)
Zn (II) 41.2 - Ni (II)
59.2 – Zn (II)
Fe3O4 Hg (II) 125.0 Song et al. (2011)
Maghemite Cr (VI) 19.20 Hu et al. (2005)
rGO-Co3O4 Cr (VI) 208.8 Al Nafiey et al.
(2017)
Magnetic chitosan Co (II) 27.5 Chang et al.
(2006)
Ferrite coated apatite Eu (III) 157.14 Moussa et al.,
magnetic nanomaterial (2013)
Zn-Fe2O4 Congo red 16.58 Rahimi et al.
(2011)
Al2O3 Orange G 93.3 Banerjee et al.
(2017)
Halloysite nanotubes Malachite 99.6 Kiani et al. (2011)
green
Anatase Pb (II), Cu (II), 31.25 – Pb (II) Atakli and Yurum
As (III) 23.74 – Cu (II) (2013)
16.98 – As (III)
Titania embedded on E.coli, - Wang et al.
silver nanoparticles S.aureus (2017)
Lanthanum based oxides E.coli, - Dedkova et al.
S.aureus, (2017)
P.aeruginosa
ZnO- Al2O3 E.coli - Sahin et al.
(2017)

Though there are numerous laboratory-scale studies on the adsorptive removal of

contaminants using nanoparticles, there is a dearth in research and implementation with
regard to their real time application in household level water treatment systems.

Nano-based adsorbents exhibit higher efficiency and faster rates in the removal of pollutants
from contaminated water when compared with traditional adsorbents (Bushra et al., 2017).
For example, most of the low cost adsorbents are microparticles and require considerable time
to achieve maximum removal of pollutants in view of their small surface contact area (Tan et
al., 2015). However, the same adsorption models are used to describe the mechanism of
adsorption for nano-based adsorbents as compared to conventionally used adsorbents.
Langmuir, Freundlich, Lagergren, Temkin, Dubinin-Radushkevich model, BET isotherm and
intraparticle diffusion are some of the commonly used models used to explain results of
adsorption studies (Bushra et al., 2017). It is important to note that in some cases, adsorption
may not be the only mechanism of removal and can be intertwined with other mechanisms
such as chemical interactions, reduction, biodegradation etc.

2.1.2. Point of use system

2.1.2.1. Removal of heavy metals

The presence of heavy metals in water sources is a global menace and some are known to be
toxic and carcinogenic (Ali, 2012). Heavy metal ions like lead, arsenic, cadmium, chromium,
selenium, mercury and cobalt are known to compromise water quality and are known to be
toxic above the permissible limits (Zhu et al., 2007; Marin et al., 2007). Adsorption is a
common technology applied for the removal of heavy metals and is more attractive for
household level water treatment in view of it being a robust technique, its low cost and
effectiveness (Jadhav et al., 2015). Iron based nanoparticles are the most common nano-
adsorbents utilized for heavy metal removal. Among the various heavy metals, arsenic
contamination is reported to affect about 150 million people worldwide in about 70 different
countries (Brammer and Ravenscroft, 2009). Preliminary studies undertaken by researchers at
the Massachusetts Institute of Technology (USA) determined the efficacy of magnetite
nanoparticles to develop a low cost sustainable water filter for the removal of As (V) and Pb
(II). Magnetite nanoparticles were synthesized very cheaply utilizing household materials and
were later used to develop filter prototypes to effectively remove upto 100 ppb As (V) and Pb
(II) meeting USEPA standards. The magnetite nanoparticles were further modified with
silica- combined silver coating to check for its microbe removal potential. However, the
authors did not observe consistent results and proposed the use of a slow sand filter for
microbe removal. The prototype was designed using a Pasteur pipette, the bottom of which
was filled with glass wool. Sand was added to the next layer, followed by layer of
nanoparticles and topped off with a sand layer (D`Couto, 2008).

Hematite nanoparticles incorporated into polypropylene cartridge filters were effectively used
for the removal of arsenic. Preliminary tests demonstrated the efficiency of the filter material
in treating spring water with moderate arsenic concentrations (30-40 ppb). On an average, 100
mg hematite nanoparticles was required to treat each litre of spring water (Tomaszewska et
al., 2016).
The idea of a tea bag model as a POU system for the removal of arsenic was proposed by
Gillman (2006) using hydrotalcite. It was proposed that this technology could be used at
household level by the distribution of sachets containing adsorbent combined with collection
for central processing of the used sachets. Further exploring the technology, Prabhu et al.
(2016) developed a POU drinking water treatment system with a lanthanum iminodiacetic
acid and chitosan composite for the effective removal of fluoride using the tea bag
technology. Reusability of the adsorbent was also tested to make the process cost effective.
The same technology can also be further explored using nano-adsorbents for the removal of
heavy metals/ contaminants. In this case, the release of ions from the nanomaterial need to be
taken into account while developing the technology. Another challenge associated with its
implementation would be to ensure retention of the nanoparticles inside the tea bag. This may
possibly involve immobilizing nanoparticles onto a suitable substrate such as chitosan beads
etc (Malwal and Gopinath, 2017) before packing into tea bags.

2.1.2.2. Removal of pesticides

Even though the major role of silver nanoparticles is in the field of disinfection, they have
also been utilized for the removal of halogenated pesticides and organics and the technology
has been patented for drinking water purification by researchers from the Indian Institute of
Technology, Madras (Pradeep and Nair, 2006). Silver nanoparticles embedded on activated
alumina incorporated in a cartridge was commercialized in India under the name Aquaguard
Gold Nova for the effective removal of halogenated organics and pesticides (Pradeep and
Anshup, 2009). The removal of pesticides was achieved by the novel chemical reactions
between the nanoparticle surface and the pesticides. Majority of the pesticides are either
halocarbons or molecules with sulfur. The halocarbons for example were degraded to metal
halides and amorphous carbon at room temperature upon interaction with the noble
nanoparticles. It was observed that pesticide free water could be obtained when water spiked
with pesticides (50 ppb concentration) was passed through the filter (Nair et al., 2007). The
cartridge life was 6000 litres and the price of the unit was 50 US$ (Pradeep and Anshup,
2009). Since silver nanoparticles have been known for their antibacterial properties, the filter
is also likely to be effective for disinfection purposes. The product, however, is currently not
available in the market.

2.1.2.3. Microbial load reduction

Prolonged use of commercial disinfectants has led to development of resistance by some
pathogens such as Giardia and Cryptosporidia. Hence, there is a need to re-evaluate
conventional disinfection methods and consider innovative approaches (Li et al., 2008). The
major antimicrobial mechanisms of nanoparticles is by interrupting transmembrane electron
transfer, disrupting electron transfer, oxidising cell components, generating secondary
products like Reactive Oxygen Species (ROS) which can further cause damage. Unlike
commercial disinfectants, nanoparticles do not generate harmful disinfection by products
since they are not strong oxidants and are relatively inert (Li et al., 2008).

The most commercialized application of silver nanoparticles is its utilization in various

products that utilize its antibacterial properties and hence this section discusses in detail,
application of silver nanoparticles for pathogen load reduction (Pradeep and Anshup, 2009).
Synthetic granular nanocomposites composed of aluminium oxyhydroxides reinforced with
chitosan and further embedded with silver nanoparticles were used by Sankar et al. (2013) to
develop a point of use (POU) water purification system. The chemical and microbe filter
component of the system was separate and the microbe filter was constructed using silver
nanoparticles embedded in a cage made of aluminium and chitosan. The cage also functions
to protect the nanoparticles from sediments. The nanoparticles were functionalized to be
specific for arsenic and iron. The system could deliver pure drinking water at US$ 2.5/year
per family. The nanocomposite used was tested for its antibacterial and antiviral activity and
placed as a cartridge. The major advantage of the filter as claimed by the authors was that
synthesis and assembly of the filter component was a ‘green synthesis’, room temperature
process. The authors further demonstrated that depending on the region of use, the cartridge
could be packed with unique composites to remove harmful chemical contaminants like
pesticides, mercury etc. in addition to microbial load.

In another study, pathogenic bacteria in groundwater namely Escherichia coli, Salmonella

typhimurium and Shigella dysenterae were effectively removed using silver nanoparticles
deposited on cation resin substrates. Results from the study indicated 100% removal of all the
pathogenic bacteria. Prototype studies were performed in South Africa and it was observed
that the filtered water had a microbial load below the limit set by South African guidelines
(Monyatsi et al., 2012). E.coli and B. subtilis have also been effectively removed using silver
nanoparticle coated polyurethane foams (Phong et al., 2009). In a similar study, 100% E. coli
removal was established after 6.5 h of filtration using a custom made pilot plant with silver
nanoparticles decorated on a porous polypropylene filter (Heidarpour et al., 2011).
Nano silver coated ceramic candle filter was developed by ARCI, India and later
manufactured and commercialized by SBQ Aqua Tech Ltd in India under the name Puritech.
The coated ceramic candle was a cheaper option costing around 4 US$ and was effective in
providing disinfected water. The typical filter consisted of two containers and the nanosilver
coated ceramic candle filter was screwed into the base of the top container and filtered water
passing through the candles drips into the lower container. Candle filters on an average have a
flow rate of 1-2 L/hour per candle. The scientists behind the product claim that even though
bare ceramic candle filters bacteria due to electrostatic force of attraction, they may however
lead to biofilm formation. The presence of nano silver will prevent biofilm formation in
addition to filtering bacteria. They further claimed that leaching of silver ions was within the
permissible limits (ARCI, 2008) and was equally effective against virus and protozoa.
However, questions like how often the candles need to be replaced and whether there is an
alarm system or indicator to know if the lifetime of the candle is over, need to be answered.

Similarly, silver nanoparticles impregnated in ceramic filters have also been successfully
developed as a POU drinking water treatment system and implemented in parts of South
Africa under the name PureMadi (http://www.puremadi.org/science-overview/). The filters
were manufactured using fired clay and later treated with a dilute solution of silver
nanoparticles. The filters were then placed in a 20 L plastic receptacle and water poured into
the filter. It was ensured that the flow rate was in between 1-2 L/hour. Physical filtration and
silver disinfection gradually removes the turbidity and provides bacteria free water. The filters
were an effective disinfectant against pathogens like Vibrio cholerae and pathogenic strains of
E coli. The price of the system ranges between 5 to15 US$ and has a filter life time of 2-3
years. However, the filter needs to be cleaned periodically with a brush to maintain the typical
flow rate. There is also no data available on the long term performance of the filter (Craver
and Smith, 2008). Another less common method of incorporating silver nanoparticles into
ceramic pots is to mix the nanoparticles with the raw materials prior to firing, called “firing
in”. It is postulated that this method would be more effective rather than painting or
submersion techniques as the silver does not wash off, oxidise or react with chlorine in the
treated water. It is currently used to develop POU ceramic pots by the company FilterPure
under the name AguaPure in the Dominican Republic with a filter lifespan of 5 years
(Ballantine and Hawkins, 2009). However, it is of crucial importance to ensure that strict
quality control is maintained in the manufacturing process to ensure similar activity within
batches.
Tata Swach Silver Boost is another POU system using silver nanotechnology currently
marketed in India. The system consists of a micro mesh to effectively remove visible
impurities. The water then comes in contact with a bulb with silver nanoparticles to
effectively remove bacteria and virus. The water is later passed through a micro filtration
membrane to remove cysts. The price of the system is approximately 40 US$ and has a
filtration capacity 3000 litres and has an auto shut off mechanism. However, it is not clear
what support material is used for the silver nanoparticles (http://www.tataswach.com/tata-
swach-silver-boost).

An interconnected carbon nanotube mesh under the name Waterstick has been used for the
effective removal of pathogenic microbes. It was originally designed for use by NASA
astronauts and the technology developed by Seldon Laboratories Ltd. The device cleans 5
gallons of water/min and requires a simple filter change after every 73 gallons. It is currently
sold as a standalone device through which water is poured and tests show that it can remove
99 % bacteria, virus and pathogens like Giardia and Cryptosporidia in addition to arsenic,
copper, herbicides and mercury. There are no details on the actual cost of the device,
however, the operation of the device requires no skilled labour and is easy to use (Cummings,
2008).

Paper based filters coated with nanoparticles are easy to produce and distribute to remote
locations and do not require energy inputs for water treatment. A POU water treatment system
consisting of bactericidal paper impregnated with silver nanoparticles to deactivate
pathogenic bacteria was developed by Dankovich and Gray (2011). The silver loss from the
nanoparticle impregnated sheets was minimal and had the potential to be an effective
emergency water treatment system. The same group have also developed POU paper filters
with copper nanoparticles effective against E.coli with a log reduction of 8.8 when a
concentration of 65 mg Cu/g was used. The authors reported that the amount of copper in
each paper amounts to less than a cent and can be potentially used in emergency response and
disaster relief, rural household filters and as backpacking filters. However, studies are still
ongoing regarding the volume of water that can be treated using a single filter paper
(Dankovich and Smith, 2014).

Systematic studies need to be carried out testing the efficacy of commercial nanotechnology
based filters in the market. In a related study, Mwabi et al. (2011) evaluated the design and
working of four household water treatment devices, namely a biosand filter, a bucket filter,
ceramic candle filter and silver impregnated porous pot filter. The performance was evaluated
in terms of flow rate, physico-chemical contaminant and microbial contaminant removals.
The silver coated ceramic pot demonstrated the highest bacterial reduction compared to other
filters. However, a cost comparison study was not performed. A challenge associated with the
use of nano-adsorbents is the likely release of metal ions from the nanoparticles into the
treated water. For example, Stumm and Wollast (1990) observed the dissolution of Al3+ ions
from alumina nanoparticles to be a two- step process; the first step involved the interaction of
the nanoparticle surface with the matrix followed by detachment of metal ions from Al-O
complex. Aluminium ions have been observed to cause neurological and gastro intestinal
toxicity (Krewski et al., 2007), though the WHO has not established a firm limit on
aluminium ion toxicity due to inadequate data. Similarly, WHO states that the known risk of
silver ingestion is a condition called argryia which discolours skin and hair. To prevent this,
WHO recommends that silver concentrations of 0.1 mg/L can be tolerated for 70 years
without any health risk (WHO, 2011). Hence, studies should also focus on the potential
release of metal ions from the nanoparticles when used for water treatment. The study
conducted by Mellor et al. (2015) observed that water treated by nano silver coated ceramic
pots had silver concentrations less than the WHO permissible limits over a period of 12
months as compared to using conventional treatment involving chlorination where over
chlorination was observed in 20% of the households tested. The WHO limit for chlorine is 5
mg/L and elevated levels can increase the risk of bladder cancer (WHO, 2006). More studies
in this direction can be helpful in determining the long-term performance of filters and can be
used to provide recommendations to small communities for household level treatment of
drinking water.

Table 2 shows some examples of the current applications of antimicrobial nanoparticles

Table 2: Mechanism of action and specificity of various antimicrobial nanoparticles

Nanoparticle Mechanism of action Active against Reference

Ag Membrane damage, inhibition E. coli, S. aureus, E. Duran et al. (2016)
of DNA replication faecalis, Proteus sp.,
Klebsiella sp
Pd Membrane damage, inhibition E. coli, S. aureus, P. Sharmila et al. (2017)
 of respiration, disruption of aeruginosa, B. subtilis
transport process
TiO2 Reactive Oxygen Species MS2, polio virus, Liga et al. (2011)
coliform bacteria
Lanthanum Reactive Oxygen Species E. coli, S. aureus, P. Dedkova et al. (2017)
oxides aeruginosa, E. faecalis
Fe3O4 Reactive Oxygen Species, P. aeruginosa Irshad et al. (2017)
membrane damage
ZnO Membrane damage, B. subtilis, E. coli El Saeed et al. (2015)
production of H2O2
C60 Reactive Oxygen Species B. subtilis, E. coli, Lyon et al. (2006);
independent oxidation Salmonella sp. Brunet et al. (2009);
Kang et al. (2007);
Dizaj et al. (2015)
Carbon Membrane damage, oxidative E. coli, S. enterica Kang et al. (2007);
nanotubes stress Dizaj et al. (2015)
Cu Membrane damage, E. coli Santo et al. (2011);
destabilize cells Dankovich and Smith
(2014)

On an average, 842,000 deaths every year are caused due to insufficient water, sanitation and
hygiene, of which 48 % occur in children under the age of five (Pruss-Ustun et al., 2014).
Diarrhoea has been identified as the fourth leading cause of death in children (WHO, 2015). It
is thus worth to mention that, out of the many household level drinking water treatment
systems currently available in the market, the majority of them target microbial load reduction
as compared to removal of hazardous chemical contaminants.

2.2. Membrane based filtration

The use of membranes for drinking water treatment is a rapidly growing field (Goh et al.,
2016). Membranes provide a physical barrier for undesirable constituents in water (Qu et al.,
2013). However, membrane fouling is one of the greatest barriers for its efficient application
and significantly decreases its lifetime and increase operational costs through increased
cleaning, energy and replacement costs.
 2.2.1. Nano-enabled filtration membranes

Nanotechnology is being utilised in developing innovative polymeric and ceramic membranes

to improve the performance of membrane filtration systems (Pendergast and Hoek, 2011). In
theory, incorporation of nanoparticles in membranes provides fouling resistance as well as
additional benefits of disinfection and contaminant degradation, depending on the
nanomaterial used (Li et al., 2008).

2.2.1.1. Removal of fluoride

Nanofiltration membranes such as NF90 and NF400 have been used to remove fluoride from
groundwaters with F removal of 98% at a pressure of 10 bar (Tahaikt et al., 2007; Elazhar et
al., 2009). Commercially available NF membranes have also been modified using
polyelectrolyte thin films to improve selectivity of the membranes (Malaisamy et al., 2011).

2.2.1.2. Removal of pathogens

Silver nanoparticles have also been impregnated onto nitrocellulose membranes and used for
the removal of bacterial pathogens such as E. coli, P. aeruginosa and E. faecalis (Fernandez
et al., 2016). Water purification systems for households such as Aquapure, Kinetico and QSI
Nano use membranes impregnated with silver nanoparticles and demonstrate 99.9% removal
of bacteria, virus and protozoa (Maynard, 2007).

Hydrophilic metal oxide nanoparticles are usually added to membranes to reduce fouling by
increasing hydrophilicity (Qu et al., 2013). For example, alumina, titania, silica and zeolite
nanoparticles have been added to polymeric ultrafiltration membranes (Maximous et al.,
2010; Bae and Tak, 2005). Lab-scale studies have been carried out to determine the potential
of carbon nanotube membranes in water treatment. These nanotube membranes have been
studied to be effective against bacteria, virus, turbidity and also towards the removal of
organic contaminants. The membranes were identified as promising for desalination and as an
alternative to reverse osmosis membranes since these filters require less energy due to their
high permeability. Carbon nanotube membranes in addition are expected to be more durable
and easier to clean and reuse (Srivastava et al., 2004). The cost of carbon nanotube adsorbents
currently ranges between US$ 25-38/Kg. Large-scale commercial production could possibly
bring down the cost considerably to US$ 10 (Dalton et al., 2003).

NanoH2O (now LG NanoH2O Inc.) introduced porous nanoparticles to membranes to

increase their efficiency. They hypothesized that since it increased permeability, it increased
water throughput for the same pressure. This eventually could reduce energy requirements by
20% or increase water productivity by 70% for the same cost
(https://www.technologyreview.com/s/410909/purifying-water-with-nano-particles/).
However, most of the nano-impregnated membranes have not been tested for their long term
effectiveness and therefore cannot be demonstrated as long term solution with the current data
available.

2.3.Catalytic degradation

The commonly used nanomaterials for photocatalytic degradation are titania, ceria and carbon
nanotubes. Among these, titania nanoparticles are being widely explored in water treatment in
view of its stability, being non- toxic by ingestion and low cost. Titania nanoparticles produce
free radicals in the presence of water, UV irradiation and oxygen which later decompose into
lesser toxic carbon compounds. Titania can either be used as a slurry, coated as a thin film or
in membranes (Kwak et al., 2001). Photocatalytic degradation of organic contaminants by
titania nanoparticles has been used commercially in industrial-scale water purification
systems, Purifics (Li et al., 2008). The Purifics Photo-Cat system has been studied to treat as
high as 2 million gallons of water/ day and remove organics without producing waste streams
(Westerhoff et al., 2009). However, there are a few technical challenges that need to be
addressed for large-scale application of nanoparticles in photocatalytic degradation: (1)
efficient photocatalytic reactor design and (2) optimization of catalyst to utilize visible light
(Qu et al., 2013).

2.4. Cost- benefit analysis

Although there are a number of studies reporting the effectiveness of nanotechnology enabled
water treatment techniques, information regarding the cost is scarcely available in view of
their limited commercialization (Adeleye et al., 2016).

The long-term effectiveness of nano silver painted ceramic pots were compared to a
conventional method using sodium hypochlorite. No significant difference in the water
quality was observed between the two methods and the researchers reported that the average
cost of maintenance of the silver painted ceramic pot ranged around US$ 6.06/ year for a
family of 5 consuming 10 L/ day while other conventional method required re-chlorination
once every 6 months costing US$ 3.14 (Mellor et al., 2015).
Ahmedna et al. (2004) evaluated the use of granulated activated carbon from nutshells in a
POU water filter (Envirofilter) for the removal of Cu, Pb and Zn ions and compared it with
commercial POU systems (BRITA, Omni Filter, PUR and Teledyne Water Pik). The
researchers observed that the Envirofilter removed nearly 100% of lead, 90-95% copper and
80-90% zinc when the initial concentration of Pb2+, Cu2+ and Zn2+ were 0.15 mg/L, 3 mg/L
and 10 mg/L at pH 7 respectively and estimated that the production cost of the Envirofilter
would be around US$ 8.71/ kg cost of carbon (assuming that there are 9 pitcher filters/ kg of
carbon). Studies have indicated that it is possible to reduce the production cost of carbon
nanotubes to US$ 10/ kg (Dalton et al., 2003). One among the many advantages of using
nanotechnology related water treatment options are lower sludge generation and faster
treatment (Adeleye et al., 2016). The overall production cost of using carbon nanotubes in
cartridges can considerably be brought down assuming that the quantity of nanotubes used/
cartridge would be significantly lower compared to bulk material.

The effectiveness of nanosilver-aluminium-oxyhydroxide chitosan granular composites for

the removal of pathogens in a water purification device was investigated by Sankar et al.
(2013). It was observed that by using 120 g of the adsorbent in cartridge form, safe drinking
water could be provided to a family of five for 1 year (assuming a daily drinking water
consumption of 10 L). This translated to an annual expense of US$ 2 per family (taking into
account cost of media, sediment prefilter, plastic assembly and cartridge packing).

Even though there is limited information on long term cost-benefit analysis of

commercialized POU systems with nano-adsorbents, it can be observed from the given
examples that the system is cost-effective and affordable. Retention/ Regeneration of
nanoparticles post adsorption in water treatment is one of the crucial aspects as it determines
the feasibility of the system and controls the economy of the technology. It is also extremely
important to recover the toxic heavy metals from the spent adsorbent for safe disposal (Saha
and Sarkar, 2012). Few workers have attempted the regeneration of nanoparticles for
recycling. Retention of nanomaterials in the system may be achieved by immobilization in the
system or by using a separation device (Qu et al., 2013). Materials such as resins, bio-
polymers may be used to immobilize the nanomaterials (Sankar et al., 2013).

Regeneration of the nanomaterials is usually done by treating with acid/ alkali to reuse the
material and improve the efficiency of the system. Titania nanoparticles were effectively
regenerated using 0.1 M NaOH for further uptake of selenium ions from aqueous solution
(Zhang et al., 2009). In another study, ferric oxide nanoparticles were regenerated with NaOH
and NaCl solutions with the removal of phosphate. The authors reported no loss of
performance after 10 regeneration cycles (Martin et al., 2009). In many cases, the adsorption
capacity of metal oxide nanoparticles is maintained after regeneration cycles. However, there
are few reports on the loss of activity post-regeneration (Deliyanni et al., 2003). However,
there are very few studies describing the regeneration of nanoparticles when used in a POU
system. More detailed research is required to determine the feasibility of regenerating the
nano-adsorbents when used in the form of cartridge or a filter. Another challenge would be to
devise strategies to treat the waste streams which would be loaded with sodium hydroxide. In
an interesting study, Sankar et al. (2013) reported a simple innovative technique for the
reactivation of metal oxy hydroxide nanocomposites used in cartridge form in a POU system.
The saturated nano-adsorbents were incubated in water at 70-100 ˚C for 3-4 hrs to enable
reactivation. Furthermore, application of dilute lemon juice was suggested as an alternative
reactivation technique thereby avoiding use of harsh alkali/acid treatment (Sankar et al.,
2013).

Immobilization of the nanomaterial may significantly decrease its release into the
environment. Management of the used nanoparticles and recovered pollutants is of utmost
importance but there are hardly studies describing their management (Ali, 2012). Table 3
gives some examples of nanotechnology enabled water treatment devices in the market.

Table 3: Examples of few nanotechnology enabled drinking water treatment systems in

the market (compiled from multiple sources on the web)

Product Nanoparticle Effective against

used
MARATHON Ag Bacteria
Aquapure Ag Bacteria
Tata Swach Ag Bacteria/virus
AguaPure Ag Bacteria
PureMadi Ag Bacteria
Aquaguard Gold Nova Ag/Al2O3 Pesticides, halogenated organics
ArsenX Fe2O3 As, Va, Cr, U
AMRIT Fe oxyhydroxide- As
chitosan
Seldon Water stick C nanotubes Bacteria/virus, As, Cu, herbicides
 3. Long term evaluation of nano-enabled POU water treatment systems
Even though there are currently many nanotechnology enabled household level water
treatment systems in the market and many in pipeline, it is of utmost importance to have data
on the long term performance of the filters. Mellor et al. (2015) studied the long term
application of silver coated ceramic water filters in Guatemala over a period of 12 months and
observed a decrease in the log reduction of total coliform bacteria at the end of six months.
Similarly, in another related study, the long term evaluation of candle ceramic filter coated
with colloidal silver and carbon (marketed under the name Stefani) was carried out in
Colombia. The study was carried out for a period of 14 months and a high reduction in the
filtration rate was observed during use (72% in the first year). There is also an increased risk
of biofilm formation in the storage container. However, there was no decrease in the
disinfection efficiency over the period studied (Perez-Vidal et al., 2016).

Nanoparticle coated POU filters may need to be cleaned on a regular basis (similar to systems
using chlorination) using soft bristle brushes to improve the filtration rate. However, care
must be taken to ensure that cleaning is not rigorous so as to cause dislodging of nanoparticles
from the filter. The effectiveness of the POU system will ultimately depend on the degree of
training received by the end user in the community. Hence, communities as a whole need to
be trained regarding operational issues and maintenance to ensure success and sustainability
of the POU system. There is a definite lack of critical data regarding the long term evaluation
of the filters and future studies need to be focussed in this direction.

4. Safe disposal of nanoparticles- Environmental implications

Nanoparticle based POU systems have immense advantages in the field of drinking water
treatment. The effect of a nanomaterial needs to be evaluated not only in terms of its
application but also from the standpoint of its potential toxicity effects when released into the
environment. Few studies indicate that the effects of specific nanomaterial properties and the
toxicity limit depend on the type and size of the nanoparticle (Tiede et al., 2009; Kuang et al.,
2016; Lei et al., 2016). Also the behaviour of the nanoparticle in the environment depends on
many factors such as pH, surrounding medium, ionic concentration, surface capping agent,
particle size etc. (Prathna et al., 2011). A number of studies have been carried out on the
toxicity of different nanoparticles to various organisms. However, very few studies have been
carried out at environmentally relevant low concentration of nanoparticles (Pakrashi et al.,
2013). The available information is insufficient to determine the maximum permissible
concentration of a particular nanomaterial in drinking water (Li et al., 2008).

Although there are a number of tools to assess the nanostructures, nanotoxicology still
requires precise determination of biological systems and nanomaterials at the nano scale.
Hence, careful control and strict guidelines over the release of nanoparticles is of utmost
importance. However, there are no specific guidelines to deal with nanotoxicity though safety
measures have been suggested (Ali, 2012). Metal ion dissolution from the nanomaterials is
another major issue and detecting their release is a challenge for which sophisticated,
expensive techniques, and analytical methods with ultra-low levels of detection, are required
(Qu et al., 2013).

Until more clear guidelines on the release of nanomaterials are developed by environmental
agencies, the best way of disposal management is recycling of nanoparticles. Used
nanoparticles may be applied for the manufacture of bricks or filled in steel cylinders and
disposed deep in the earth as landfills. Regenerated metal ions may also be used for the
synthesis of other materials (Ali, 2012). Diale et al. (2011) studied the sequestration of heavy
metals from spent waste using natural zeolites. The same approach may be further explored
for the sludge of spent nano-adsorbents. Researchers have also explored various ways to
solidify and stabilize the spent heavy metal waste in the form of cement, in bricks, in
polymeric matrices to be disposed in landfills ultimately. Dhoble et al. (2017) studied the use
of spent magnetic binary oxide particles laden with arsenic waste to be used as concrete. The
authors carried out toxicity leaching tests to determine if the leachate concentration was
considered hazardous. Similarly, in a recent study, stabilization of arsenic and fluoride
bearing spent adsorbent was explored using clay bricks. The leachate concentration of As and
F were 510 μg/L and 2.1 mg/L respectively (Rathore and Mondal, 2017) which was below the
permissible limits of USEPA. A leachate concentration of <5 mg/L arsenic and 48 mg/L
fluoride is considered to be non-hazardous (Dou et al., 2011; USEPA, 1992).

5. Summary and Conclusions

1. As water becomes scarcer and more contaminated, advanced technology is needed to

provide cleaner water for the world. Nanotechnology has the potential to address this need in
an inexpensive and efficient way. Several research papers have shown that nanotechnology
based systems can be efficient and effective in removal of arsenic, fluoride and other metals
as well as pathogens from water at different scales.

2. Some nanotechnology based water treatment systems already available on the market
targeting different contaminants and many more are in the pipeline. However, long-term
evaluation of these systems is required as most of them have been tested and marketed based
on laboratory-scale studies only. The maximum long-term evaluation data available for nano-
coated ceramic filters is for a period of 14 months.

3. More options of using nanoparticles in POU systems like sandwich filters, coated on a
substrate, tea bag model, coffee filter etc. should be explored further. Large-scale commercial
production of nanoparticles would considerably bring down the production cost.

4. Extensive application of nanomaterials in water treatment systems would also depend on

cost effectiveness in addition to performance. Cost effectiveness may be achieved by ensuring
the retention and reuse of the nanomaterials. More collaboration between governments,
research institutions and the industry will be required for better implementation of
nanotechnology based POU water treatment systems. Furthermore, dissemination of POU
technologies in various forms such as production of cartridges, sachets, water filter devices
etc. can contribute to large-scale employment opportunities as well as contribute to the local
economy.

5. More in depth studies are needed to address the management of recovered pollutants and
the exhausted nanoparticles. Currently, potential disposal methods for pollutant saturated
nanoparticles are solidification and stabilization of the waste in the form of cement, bricks etc.

6. There are potential environmental concerns regarding the release of nanoparticles into the
environment and exposure to the human body. However, recent studies have also indicated
that nanomaterial based toxicity depends on a number of factors like size and type of
nanoparticle, surrounding environmental matrix, pH of solution to name a few. Hence, there is
a need to consider each on a case by case basis. Of utmost importance, is to ensure early
assessment and mitigation of potential environmental impacts of nanomaterials for long-term
safe supply of drinking water.

Acknowledgements
The research leading to these results was funded by the People Programme (Marie Curie
Actions) of the European Union's Seventh Framework Programme (FP7/2007-2013) under
REA grant agreement no PCOFUND-GA-2013-606838.

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Web Sources
http://www.puremadi.org/science-overview/
http://www.tataswach.com/tata-swach-silver-boost
https://www.technologyreview.com/s/410909/purifying-water-with-nano-particles/
Highlights
 Progress in application of nanoparticles for drinking water treatment are presented
 Real time application at household level are reviewed
 Potential environmental impact of spent nano-adsorbent is discussed
 Future prospects of nanoparticles for household level water treatment are discussed
Graphical abstract