project 3

Environmental Technology & Innovation 24 (2021) 101924
Contents lists available at ScienceDirect
Environmental Technology & Innovation

journal homepage: www.elsevier.com/locate/eti
Synthesis and characterization of magnetic nanoparticles, and

their applications in wastewater treatment: A review
∗ ∗
Saurabh Shukla a ,1 , Ramsha Khan a , ,1 , Achlesh Daverey b ,
a
Faculty of Civil Engineering, Institute of Technology, Shri Ramswaroop Memorial University, Uttar Pradesh, 225003, India
b
School of Environment and Natural Resources, Doon University, Dehradun, Uttarakhand, 248012, India
article info a b s t r a c t
Article history: The sustainable growth of any society is in direct proportion with developing novel
Received 18 April 2021 methods and technologies for the management of its environmental quality. The use
Received in revised form 25 August 2021 of Magnetic Nanoparticles (MNPs) has emerged as an efficient tool for remediation of
Accepted 1 September 2021
wastewater owing to its intrinsic qualities including size, surface effect, quantum effect,
Available online 4 September 2021
etc. These intrinsic properties of MNPs have diversified their application in managing
Keywords: the qualitative stress on water resources. The present review aims to assess the use of
Nanotechnology MNPs in removing organic and inorganic contaminants from wastewater. Insights into
Wastewater remediation various synthesis methods and their effects on contaminant removal are also presented.
Contaminant degradation It is reported that MNPs provide target specificity and cost-effectiveness as compared
Eco-friendly synthesis to conventional treatment methods. Moreover, the biological synthesis of MNPs is
Organic pollutants proven to be eco-friendly and aids in sustainable development. Nearly 100% removal of
Inorganic pollutants
various types of contaminants such as pharmaceuticals and personal care products, dyes,
pesticides, heavy metals, etc. can be achieved through MNPs. Some MNPs have shown
a magnetic saturation reaching up to 70 emu/g, and recycling up to 5 cycles with >95%
removal efficiency. High pollutant removal efficiency (>98%) can also be achieved in a
short time (within 5 min) by MNPs. It is noteworthy that, nanosorption along with the
redox reactions are the most frequently used and efficient mechanisms of contaminant
removal from wastewater samples.
© 2021 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY
license (http://creativecommons.org/licenses/by/4.0/).
Contents
1. Introduction............................................................................................................................................................................................... 2
2. Synthesis of magnetic nanoparticles...................................................................................................................................................... 3
2.1. Physical methods of synthesis ................................................................................................................................................... 3
2.1.1. Mechanical milling ....................................................................................................................................................... 3
2.1.2. Electron beam lithography.......................................................................................................................................... 5
2.1.3. Gas-phase deposition................................................................................................................................................... 5
2.1.4. Vapour deposition and patterning ............................................................................................................................. 5
2.1.5. Electrical explosion of wires ....................................................................................................................................... 5
2.2. Chemical methods of synthesis.................................................................................................................................................. 6
2.2.1. Spray pyrolysis ............................................................................................................................................................. 6
∗ Corresponding authors.
E-mail addresses: saurabh.shukla2020@gmail.com (S. Shukla), ramshaokhan@gmail.com (R. Khan), achlesh.senr@doonuniversity.ac.in
(A. Daverey).
1 Equal contribution.
https://doi.org/10.1016/j.eti.2021.101924
2352-1864/© 2021 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/
licenses/by/4.0/).
S. Shukla, R. Khan and A. Daverey Environmental Technology & Innovation 24 (2021) 101924
2.2.2. Laser pyrolysis .............................................................................................................................................................. 6

2.2.3. Co-precipitation ............................................................................................................................................................ 6
2.2.4. Thermal decomposition ............................................................................................................................................... 6
2.2.5. Microemulsion .............................................................................................................................................................. 6
2.2.6. Hydrothermal/solvothermal method ......................................................................................................................... 6
2.2.7. Sol-gel method ............................................................................................................................................................. 6
2.2.8. Polyol method............................................................................................................................................................... 6
2.2.9. Non-thermal plasma methods .................................................................................................................................... 7
2.3. Biological methods....................................................................................................................................................................... 7
2.4. Comparison between physical, chemical and biological synthesis approaches ................................................................... 7
3. Key properties and characterization of MNPs ...................................................................................................................................... 7
3.1. Geometry of nanoparticles ......................................................................................................................................................... 8
3.2. Structural properties of nanomaterials ..................................................................................................................................... 9
3.3. Surface charge and thermodynamic properties of nanoparticles .......................................................................................... 9
3.4. Magnetic properties of nanomaterials ...................................................................................................................................... 9
4. Mechanisms of contaminant removal using MNPs .............................................................................................................................. 9
5. Recent applications of MNPs in wastewater treatment ...................................................................................................................... 10
5.1. Removal of organic pollutants using MNPs.............................................................................................................................. 10
5.2. Removal of inorganic pollutants using MNPs .......................................................................................................................... 11
6. Toxicity and legalization of MNPs.......................................................................................................................................................... 12
7. Future research prospects ....................................................................................................................................................................... 13
8. Conclusions................................................................................................................................................................................................ 14
CRediT authorship contribution statement ........................................................................................................................................... 14
Declaration of competing interest.......................................................................................................................................................... 14
Acknowledgements .................................................................................................................................................................................. 14
Appendix A. Supplementary data........................................................................................................................................................... 14
References ................................................................................................................................................................................................. 14
1. Introduction
The rapid pace of urbanization and industrialization has severely affected the availability of potable water across the
globe (Shukla and Saxena, 2020a; Siddeeg et al., 2019). The indiscriminate discharge of domestic sewage and industrial
effluents into the water bodies has created a potential hazard of accumulation of various types of contaminants (Khan
et al., 2020; Shukla et al., 2020). Additionally, the release of partially treated or untreated wastewater has led to severe
deterioration in the water quality of natural water resources (Ali et al., 2019; Shukla and Saxena, 2020b,c). A wide variety
of contaminants including pesticides, antibiotics, inorganic chemicals, heavy metals, textile dyes can affect human health
and lead to various diseases (Mishra and Kumar, 2020). Exposure to these pollutants may also cause several health
issues like kidney failure, respiratory problems, skin cancer, and cardiovascular diseases, etc. (Santhosh et al., 2016).
The maintenance of a healthy aquatic environment is vital for the sustenance of aquatic flora, and fauna population.
The potential risk of lack of clean water for drinking purposes makes the efficient treatment of wastewater even more
relevant. Further, water scarcity and inadequate treatment of wastewater have been identified as a critical threat to the
human population around the world (Mishra et al., 2016; Raj and Shaji, 2017). Hence, studies addressing these issues
associated with water and wastewater treatment technologies have been gaining major attention worldwide (Shukla and
Saxena, 2020d; Tripathi and Shukla, 2018).
The conventional wastewater treatment technologies involving physical, chemical, and biological methods have certain
demerits such as high capital and maintenance costs, toxicity of leachates etc. which are summarized in Fig. S1. To
overcome these challenges, researchers started to look for solutions that can overcome these demerits. Among all the
treatment technologies for water and wastewater, nanotechnology is perceived as one of the best and most promising
technologies. Moreover, the use of magnetic nanomaterials (NMs) in wastewater remediation has been proven to be
advantageous, owing to their distinguished properties which makes them preferable over the conventional treatment
methods. Some of these properties include magnetic, electrical, and optical properties, and characteristics such as catalytic
activities, high reactivity, high mobility, and high adsorption capacities (Peigneux et al., 2020). Moreover, nanotechnology
is the solution to many other issues associated with water purification and treatment such as cost issues, and recycling
potential of the materials used. A word cloud representing an illustrative view of the concept of magnetic NMs, and its
associated areas of influence and applications have been stated in Fig. S2. It can be observed from the word could (Fig. S2)
that these magnetic NMs have been used in remediation for almost all kinds of contamination from water and wastewater.
In the past few decades, the role of magnetic nanoparticles (MNPs) has grown exponentially in various fields such as
chemistry, biology, sensing and detection of pollutants, medicines, and treatment (Masjedi et al., 2020). The chronological
development in the field of nanotechnology is summarized in Fig. 1, which suggests that the significant improvements in
the research have started after the year 2010, and a steep rise was observed in the year 2015 and onwards. For further
estimation of increasing advancements in the use of nanotechnology, two databases, Science Direct and PubMed were
2
Table 1
A comparison of the present review article and some other recent review papers published on magnetics nanoparticles for wastewater treatment.
Reference Various Green/ Characteri- Contaminant Effect of synthesis Effect of synthesis Use of
methods of biological zation removal method on removal of method on removal of nanotechnology
synthesis synthesis mechanism organic contaminant inorganic contaminant and its toxicity
potential
This study ✓ ✓ ✓ ✓ ✓ ✓ ✓
Shan et al. ✓ ✘ ✘ ✘ ✘ ✘ ✘
(2016)
Gupta et al. ✓ ✓ ✘ ✓ ✓ ✓ ✘
(2017)
Adewunmi ✓ ✘ ✘ ✘ ✘ ✘ ✘
et al. (2021)
Mohammed ✓ ✘ ✓ ✓ ✘ ✘ ✘
et al. (2017)
Gutierrez et al. ✘ ✘ ✘ ✓ ✓ ✘ ✘
(2017)
Khan et al. ✓ ✘ ✘ ✓ ✓ ✓ ✘
(2020a,b)
Gao (2019) ✓ ✘ ✓ ✓ ✓ ✓ ✘
Hassan et al. ✓ ✓ ✘ ✓ ✓ ✓ ✓
(2020)
Rocha et al. ✓ ✘ ✘ ✓ ✘ ✓ ✘
(2020)
searched for the literature review with the following keywords ‘‘nanoparticles’’ + ‘‘wastewater treatment’’ + ‘‘magnetic
nanoparticles’’ + ‘‘organic pollutant removal’’ + ‘‘inorganic pollutant removal’’ in March 2021. The year-wise number of
articles published related to these topics is represented in Fig. S3. Researchers around the world have started exploring
the use of nanoparticles in the water purification sector during the late 2000s which is in coherence with the findings of
Fig. 1. The use of MNPs in the waste treatment sector has huge potential towards achieving greater efficiency of filtration
materials, promoting reuse and recycling to a much greater extent. Nano remediation techniques (using magnetic NMs)
can not only be used to reduce the overall costs, but also reduce the treatment time, possibilities of in-situ treatment, and
achieving near 100 percent treatment efficiency. Moreover, the biggest advantage of magnetic NMs and nanotechnology
in general lies in the fact that they may also enhance performance of conventional treatment technologies, e.g., lower
energy requirement in thermal treatment techniques, and better residual management.
Recently, many studies have been conducted concentrating on the removal of various kinds of organic and inorganic
pollutants such as pesticides, dyes, heavy metals (HMs), pharmaceutical and personal care products from wastewater.
These studies have mostly focussed on using different types of magnetic NMs and their varying removal efficiencies.
Very limited literature is available which explores the mechanism of contaminant removal and/or their degradation in
wastewater and its effect on the removal efficiency. The recent review articles published in literature covering various
aspects of nanotechnology and MNPs are compiled in Table 1. The present study attempts to address major critical aspects
of MNPs and compile this necessary information at one place fulfilling the gaps from previous studies. Therefore, the major
objectives of this review are to (1) summarize the various synthesis methods of MNPs, (2) compile the different methods
to characterize nanoparticles and MNPs, and (3) identify the best possible pollutant removal/degradation mechanism of
MNPs.
2. Synthesis of magnetic nanoparticles
Many significant efforts have been dedicated towards the development of novel methods for synthesis of MNPs.
Precision in preparation and surface functionalization of the MNPs is critical as it may affect their physicochemical
properties, stability, their movement, and pollutant removal efficiency (Reddy et al., 2012). In a general and broad sense,
the synthesis of MNPs can be classified into three primary methodologies, viz. (a) physical methods, (b) chemical methods,
and (c) biological or microbial methods (Kudr et al., 2017) . The physical methods are based on the top-down strategy,
i.e., synthesis starts from bulk material and depleting to generate NPs. Whereas, chemical and biological methods follow
a bottom-up approach, where the atoms/molecules are assembled which forms different sizes of NPs (Fig. 2).
2.1. Physical methods of synthesis
2.1.1. Mechanical milling

Mechanical milling is a very convenient, simple, and organized method to synthesize MNP powder. This process is
generally used to produce different types of materials based upon various initiating compounds and is used to develop
metallic granular alloys. The process of milling can be executed through various mills including shaker and planetary
mills (Österle et al., 2013). Various parameters influence the production of MNPs through mechanical milling including
3
Fig. 1. Chronological developments in the field of nanotechnology.
the ratio of ball-to-powder weight, milling time, milling speed, and material of the container. In a study by Bououdina
et al. (2019), nanocrystalline magnesium ferrite was synthesized through ball milling of α -Fe2 O3 and MgO in powdered
4
Fig. 2. Classification of synthesis methods for MNPs and their key features.
form and strengthened at 700–900 ◦ C. It was further reported that ferromagnetic properties were observed for the
magnetic nanopowders, with low coercivity (68.68 Oe), remanence (0.840 emu/g) and saturation magnetization (6.517
emu/g). The synthesized magnetic nanopowders were found to be suitable for removal of heavy metals from wastewater.
In another study, carbonaceous magnetic adsorbents were synthesized through ball milling a combination of activated
carbon and with Fe3 O4 nanoparticles. Authors found that the ball-milled magnetic adsorbents are environmentally friendly
to synthesize, have high efficiency, low cost, and offers convenience in operation.
2.1.2. Electron beam lithography

The electron beam lithography method involves the use of an electron beam (e-beam) for the conversion of iron
particles into iron oxides (Fe3 O4 ). The generation of nanosized iron oxide NPs through the emission of e-beam in a
defined manner across a surface filmed with iron particles. This methodology has been accepted as a low-cost method
that produces stable NPs and offers versatility (Scuderi et al., 2016; Wang et al., 2019).
2.1.3. Gas-phase deposition

The gas-phase deposition method consists of a catalyst-assisted chemical vapour deposition (CVD) process of molecular
precursors, Sn(OBut )4 or {Fe (OBut )3 }2 on substrates made of alumina and covered with gold leading to the creation of a
one-dimensional iron oxide nanostructure (Reddy et al., 2012). Many researchers have made use of gas-phase synthesis
for MNPs efficiently and cost-effectively (Grammatikopoulos et al., 2016; Hammad et al., 2020; Kato et al., 2019).
2.1.4. Vapour deposition and patterning

In this method, the magnetic particles can be generated by developing a continuous film and filling holes in a provided
template. The material which composes the particles is deposited through vapour deposition techniques (laser ablation,
sputtering, and evaporation) and electrodeposition. This method has been proven to produce high quality NPs, reduce
alloying temperatures, and may be employed on large scale (Choi et al., 2016; Shifa et al., 2018).
2.1.5. Electrical explosion of wires

The electrical explosion of wires method is not very common for the synthesis of MNPs and consists of evaporation of
a metal wire under the influence of an intense electric current (Lerner et al., 2016). The metal particles produced through
this method are very pure restricted to the initial purity of metal wire, and perfectly spherically in shape. This method is
a green technique considering that no waste is generated (Lozhkomoev et al., 2019).
5
2.2. Chemical methods of synthesis
2.2.1. Spray pyrolysis

In the spray pyrolysis method, the preparation of a solid is done through the application of a solution onto a series of
reactors for evaporation of the solvent to be undergone by aerosol droplets. The solute is condensed within the droplet
succeeded by the drying and breakdown of molecules of the precipitated particle at high temperature (Majidi et al., 2016).
Studies have reported that properties of MNPs such as magnetization, and photocatalytic degradation capacities have been
enhanced through this method (Kaya et al., 2019; Shatrova et al., 2017).
2.2.2. Laser pyrolysis

The laser pyrolysis method involves the application of heat through a constant CO2 laser on a mixture of gases for
initiation and sustenance of chemical reactions. This technique promotes the localized heating and cooling effect and
is very effective in heating the precursors to influence reactions and nucleation (Alonso et al., 2018). This method also
improves the chemical and morphological characteristics such as high surface area, crystalline matrix, stability, electrical
conductivity, coercivity (Siddiqui et al., 2018), and magnetic saturation reaching up to 70 emu/g (Dumitrache et al., 2015).
2.2.3. Co-precipitation
This method is known to be the most effective and accurate way of synthesizing superparamagnetic iron oxide
nanoparticles (SPIONs) which have a mean diameter <50 nm. It includes chemical reactions occurring in an aqueous
monophasic liquid medium in which coherent iron hydroxide nuclei growth and nucleation have to be regulated (Darwesh
et al., 2019). The annealing temperature also plays an important role in magnetization of the MNPs, and temperature in
the range of 900–1000 ◦ C shows most promising results (Albalah et al., 2020).
2.2.4. Thermal decomposition

The use of thermal decomposition has gained wide acceptance in synthetization of high-quality MNPs. It primarily
includes the decomposition of metal precursors including oleates, acetylacetonates etc. at very high temperatures of
150–300 ◦ C in the presence of high boiling points (250–300 ◦ C) organic solvents including benzyl ether or octadecene
(Anderson et al., 2019).
2.2.5. Microemulsion
The microemulsion method consists of dispersal in the presence of a surfactant with two immiscible phases of water
and oil. Microemulsions are stable colloidal suspensions in which two immiscible liquids coexist in a single phase. This
technique is distinctive due to its unique properties such as large interface area, thermodynamic stability, very low
interfacial tension, and the ability to solubilize various immiscible liquids. Moreover, this technique also enables the
control over properties of NPs such as its geometry, morphology, surface area etc. (Salabat and Mirhoseini, 2018).
2.2.6. Hydrothermal/solvothermal method

The hydrothermal method is used in the synthetization of MNPs in aqueous media in autoclaves at very high pressure
(>13 790 kPa) and temperature greater than 200 ◦ C (Natarajan et al., 2019). The nucleation of newly formed particles is
in a directly proportionate relationship with temperature leading to the formation of small-sized NPs. The two primary
ways for the development of NPs under hydrothermal conditions includes (neutralization of mixed metal hydroxides, and
hydrolysis and oxidation). The hydrothermal method provides better control over the geometry (size, structure etc.) of
the NPs (Sobhani and Salavati-Niasari, 2015).
2.2.7. Sol-gel method

The sol-gel method for the synthesis of nanoparticle generation is one of the most explored and widely used techniques,
as it is a proper wet route for the synthesis of metal oxides. It is based upon the hydroxylation and condensation
of a molecular precursor in an aqueous solution, which initiates a ‘sol’ of nanoparticles (Alagiri et al., 2012). Further
condensation and polymerization lead to a 3-dimensional network of metal oxides (wet gel), which requires some
additional heat treatments to obtain the final crystalline structure. Among the other methods, this technique has
certain advantages such as low working temperatures, more control over reaction kinetics through variation in chemical
constituents etc. (Gudikandula and Charya Maringanti, 2016).
2.2.8. Polyol method

The use of surfactants in the Sol-Gel technique of synthesis has its associated issue of modification of the surface charge
and surface morphology of NPs. Thus, Polyol Method is an alternative method employing polyols including propylene
glycol, polyethylene glycol etc. for regulating the growth of particles, maintaining a high degree of crystallinity in newly
developed NPs and preventing inter-particle accumulation (Vega-Chacón et al., 2016). This method of synthetization has
proven to be very popular especially in the biomedical field (magnetic resonance imaging). The direct procurement of
fine metallic particles through reduction of dissolved metallic salts followed by the precipitation of metals is seen in this
method of synthesis. The polyol method is very effective in the synthesis of bimetallic clusters and nanocrystalline alloys
(Hsu and Tao, 2018).
6
2.2.9. Non-thermal plasma methods

Plasma methods are considered as environmentally friendly modification technologies having various advantages
over chemical and thermal reduction procedures such as they are solvent-free, quick, nontoxic, adaptable, and energy-
efficient. Various species such as radicals, electrons, and ions can be created during the plasma conversion process,
initiating interactions between the materials’ surfaces and functional groups that are generally difficult to achieve during
conventional chemical synthesis (Woodard et al., 2018). However, the gas temperature reaches more than 4000 K, and a
considerable part of this input energy is spent on non-valuable power generation, hence these are regarded as high-energy
consumers (Wang et al., 2020). To overcome this, the non-thermal plasma technique is being explored and used because
of its strong chemical activity/selectivity and high energy conversion efficiency (Wang et al., 2020). They have a lower gas
temperature (3000 K) and higher electron energy (>1 eV) and hence are considered more eco-friendly for the synthesis
of MNPs (Duan et al., 2018).
2.3. Biological methods
There is a constant requirement for developing eco-friendly methods for the synthesis of NPs to overcome the
challenges associated with physical and chemical methods. Hence, the biological synthesis of NPs is increasingly gaining
attention as it is rapid, environment friendly, and it could easily be scaled up for field studies. The reinstatement of
our environment to its natural and pristine state through the application of green nanotechnology has gained rapid
momentum. The biocompatibility between MNPs like zero-valent iron, magnetite, and maghemite has been studied with
foremost interest and scrutiny. Both microbes and plants offer various ways for the synthesis of MNPs primarily owing
to their genetic diversity and presence of enzymes (Dave et al., 2021). In general, microbes produce inorganic products
(intra-/extracellularly), which are often in nano dimensions and have explicit morphological characteristics (Joshi et al.,
2018). Furthermore, the utilization of various parts of plants including extracts, barks, tissues, exudates has emerged as an
effective alternative for synthetization of metal NPs (Majidi et al., 2016; Singh et al., 2016). These methods are beneficial
as they provide higher yield, better reproducibility and scalability, and a higher degree of control over the required size
and properties of resulting NPs (Ahmadi et al., 2021; Sivakami et al., 2020).
2.4. Comparison between physical, chemical and biological synthesis approaches
A comparative representation of all the three basic methods for the synthesis of different types of NPs is presented in
Fig. 3. As compared to physical methods, the chemical methods of synthesis are found to be more suitable as they have a
wider application. However, many adverse impacts of these chemical methods have also been reported, as toxic substances
may get sorbed and desorbed from the surface of NPs prepared from chemical methods during their synthesis (Parashar
et al., 2020). Major drawbacks with these physical and chemical methods includes high cost, use of toxic and hazardous
chemicals which pose certain environmental threats and may cause toxicity in humans. Moreover, due to technological
advancements, these physical and chemical methods are not much used these days, and research work is more focussed
on biological methods which are regarded as ‘green synthesis’ methods. Biological methods are advantageous as they
are more natural, for example, the reducing agent in chemical methods is a synthetic chemical solution, whereas, in
the biological method, this role is naturally played by several enzymes, especially nitrate reductase (Ali et al., 2017).
Moreover, the raw material (plant concentrate, microorganisms) is easily accessible as compared to raw materials used in
chemical methods. Studies have also suggested that fungi are better equipped to produce large quantities of NPs naturally
since they produce NPs extracellularly due to the presence of large secretory parts (Parashar et al., 2020). Hence, it can
be concluded that more work should be conducted to identify greener methods of synthesis, which are proven to be
sustainable, however, the risks and toxicity associated with such methods shall also be explored in detail.
3. Key properties and characterization of MNPs
The physicochemical properties are extensively relevant in discovering the accuracy and efficiency of targeted delivery.
The two unique barriers which MNPs need to overcome to reach their target include physiological and cellular barriers
(Jawad and Al-Alawy, 2020; Mohammed et al., 2017). The broad scope of execution based on the structural, physical,
chemical, magnetic, and electrical characteristics of MNPs enhances their field of application. The reusability, regeneration,
easy separation with lowered operational costs are some benefits associated with MNPs (Saxena et al., 2020). Precise
characterization of MNPs is very critical in the determination of the reproducibility of the results, and the size, shape and
composition also govern the magnetic properties of the MNPs (Punia et al., 2021). For example, size reduction of MNPs
leads to excellent magnetism, whereas the shape of MNPs supports inhomogeneity. Moreover, the reliability and validity
of various characterization techniques are also important in the determination of the most efficient synthesis process,
which may enhance the target-specific capacity of the MNPs (Kouhpanji and Stadler, 2020). Some key properties of MNPs
have been discussed in the following sub-sections.
7
Fig. 3. Physical, chemical and biological methods for the synthesis of different types of MNPs.
Fig. 4. Various mechanisms of contaminant removal using MNPs, (a) Adsorption, (b) Filtration using semi-permeable membranes synthesized through
MNPs, (c) Redox reactions for contaminant degradation, (d) Pollutant removal through photo catalysis. CB: Conduction band; VB: Valence band; e:
electron, h: hole.
3.1. Geometry of nanoparticles
This physiochemical property includes the size and shape of MNPs and helps in imparting stability to the MNPs. The
magnetic moment and response are highly affected by the size of the particles. In a study by Reddy et al. (2012) it was
stated that the saturation magnetization of iron oxide particles decreases with a decrease in size. It was also stated by
the authors that the decrease in size increased surface area which may have affected the non-crystalline characteristics of
8
the MNPs and subsequently their magnetic moments may also have been affected. Although, very small-sized MNPs can
exhibit superparamagnetic properties showing better magnetization in comparison to paramagnetic materials (Löwa et al.,
2019). The field-emission scanning electron microscopy (FeSEM) and high-resolution transmission electron microscopy
(HRTEM) are used for the characterization of size and the shape of nanoparticles. The atomic arrangement in the NPs can
be assessed using these techniques, and interfacial structures of the MNPs can be investigated (Liu et al., 2019a,b).
3.2. Structural properties of nanomaterials
In general, the magnetic properties of MNPs are defined by the degree of crystallinity, and purity of constituent
minerals. The structure of these NPs can be determined through infrared spectroscopy, thermal analysis, and X-ray
diffraction. Many researchers have investigated the structure of composite NPs, and interactions between the core and
molecular structure, using various techniques such as thermogravimetric and differential thermogravimetric analysis
(TGA), differential scanning calorimetry (DSC) etc. (Li et al., 2019a,b; Reddy et al., 2012). This data has been further
collated with methods such as Fourier transform infrared spectroscopy (FTIR), statistic secondary ion mass spectra (SSIMS),
scanning electron microscopy (SEM) etc. (Nordin et al., 2021). Several other techniques such as atomic force microscopy
(AFM) and chemical force microscopy (CFM) are there, which helps in investigating the morphological changes happening
on the surface of MNPs (Najafpoor et al., 2020).
3.3. Surface charge and thermodynamic properties of nanoparticles
In general, a relatively high ionic strength is acquired by the MNPs which along with the magnetic attraction
cause aggregation of NPs. The stability in MNPs is gained when these effects are compensated by other forces such as
electrostatic repulsion, hydrophilic interactions, and steric barrier (Reddy et al., 2012; Wang et al., 2013). Moreover, a
charge is acquired on the surface of NPs when they interact with an aqueous electrolytic solution. It has been reported
that positively charge MNPs may react with non-targeted materials which may bind to the surface of MNPs (Almomani
et al., 2020). Hence, the determination of the surface charge of the MNPs becomes crucial, which can be achieved through
the determination of electrokinetic or zeta potential (Girigoswami et al., 2019).
Similarly, the thermodynamic stability of MNPs needs to be ensured which helps in determining the efficiency of
surface modifications in MNPs with organic or inorganic pollutants in wastewater (Wang et al., 2021, 2017a,b). Moreover,
the importance of the wettability of particles and the procedure associated with interaction between particles in the
aqueous medium determines the ability of MNPs to be in dispersed or aggregated state helping in estimating their ability
to remove various contaminants from water and wastewater samples (Sahu et al., 2018).
3.4. Magnetic properties of nanomaterials
Assessment of magnetic properties of nanomaterials is very important in estimating their stability, efficiency, sepa-
ration, recovery and recyclability (Liu et al., 2019a,b). MNPs which exhibit permanent magnetization even after being
removed from a magnetic field are referred to as ferromagnetic particles, whereas when paramagnetic particles are
removed from a magnetic field, no permanent magnetization is observed (Kouhpanji and Stadler, 2020). Magnetism or
magnetic properties of NPs depend primarily upon two factors, (i) magnetic induction (B), and (ii) strength of magnetic
field (H). In general, there exist a linear relationship between B and H, which is governed by the magnetic permeability (µ)
of NPs. The MNPs will exhibit paramagnetic properties if µ > 1, and diamagnetic properties if µ < 1 (Reddy et al., 2012).
The magnetic properties also help in limiting the need to separate the catalyst by centrifugation, filtering, or extraction
processes. Moreover, the surface of magnetic nanoparticles significantly reduces dispersion and hence product purity
(Khan et al., 2020).
4. Mechanisms of contaminant removal using MNPs
Rapid industrialization and increasing population is the major reason behind the release of various contaminants in
wastewater including both organic and inorganic pollutants such as dyes, pesticides, personal care products, heavy metals
etc. (Boretti and Rosa, 2019; Soni et al., 2020). The biggest challenge comes from the partial or un-treated wastewater
directly getting discharged into the surface water bodies causing severe environmental risk, endangering aquatic species,
affecting the food chain and subsequently affect human health through bioaccumulation and biomagnification. For
efficient remediation and removal of these contaminants, eco-friendly nanomaterials have been developed over years and
the research is continually expanding. Various types of MNPs have been synthesized and used for remediation purposes,
with varying sizes, chemical properties, and morphologies. These MNPs act through four major removal/degradation
mechanisms viz., (a) adsorption, (b) filtration, (c) transformation, and (d) catalysis (Li et al., 2019b).
Adsorption is a surface phenomenon that involves the binding of pollutants on the surface of the adsorbent mediated
through physical or chemical interactions (Fig. 4a). Broadly, the adsorption process for contaminant removal/wastewater
treatment occurs in three steps, (i) movement of the contaminant to the surface of the adsorbent, (ii) binding at the
adsorbent surface, and (iii) movement within the adsorbent. In general, the MNPs have higher specific surface areas, hence,
9
they can be easily functionalized towards a target contaminant. Moreover, the nano-sized pores present on the surface of
MNPs help in the adsorption of contaminants (Das et al., 2020). Furthermore, the magnetic properties of nanomaterials
enhance their ability to be separated from the contaminant and regenerated to improve reusability.
In water and wastewater treatment, filtration plays a significant role, including both media filtration and membrane
filtration techniques (Fig. 4b). Nanofiltration using MNPs can be easily defined as a membrane separation technique (acting
under pressure), which has been gaining a lot of attention due to its high rate of permeation (Ali et al., 2019). Various
other factors like lower pressure requirements (7–30 atm) as compared to reverse osmosis (20–100 atm), a fixed surface
charge which helps in providing selectivity towards a target contaminant makes it unique.
Various anthropogenic activities lead to the accumulation of various contaminants in the ambient environment. The
process of transformation through oxidation and/or reduction has been proved to be an effective technique for the removal
of both organic and inorganic pollutants from water and wastewater (Fig. 4c). These redox reactions lead to speciation
of metals present in wastewater and hence reduce the metal toxicity (Kumar et al., 2018). Moreover, the occurrence of
these redox reactions towards reaching a stable oxidation state may also lead to reduced toxicity (Samsonu et al., 2018).
Catalysis technology is an inexpensive method for contaminant removal from water and wastewater using MNPs. The
preparation of an efficient catalyst can be achieved through cheap and easily available raw materials. In this context,
photocatalysis accelerates the photodegradation of organic and inorganic contaminants. The photocatalysis technique for
contaminant removal uses a light active catalyst medium made of MNPs that degrades several types of pollutants present
in wastewater. In a photocatalysis system where a semiconductor material is used as a catalyst medium, an electron–hole
(e–h) pair is created upon absorption of light energy higher than its bandgap energy (Fig. 4d). These e–h pair produce
highly reactive oxidizing and/or reducing agents and radicals in wastewater (OH− , O2 − etc.), which degrades the organic
and/or inorganic contaminants present in the wastewater (Shaheen et al., 2016). The photo-generated electron and holes
(e–h pairs) are readily available at the surface of these magnetic nano-photocatalysts due to their higher surface-volume
ratio as compared to the traditional photo-catalysts. Hence, the nanostructured semiconductor materials are much more
suitable for wastewater treatment compared to their traditional counterparts (Das et al., 2020).
5. Recent applications of MNPs in wastewater treatment
5.1. Removal of organic pollutants using MNPs
The presence of various organic contaminants such as dyes, pesticides, personal care products, phenols etc. in
wastewater has become a major source of pollution. These pollutants adversely affect aquatic life and human health as
well. These organic pollutants are extremely difficult to remove using conventional wastewater treatment technologies.
Their degradation is achieved mostly through methods such as acidic decomposition, heating, or employing biological
treatment methods. Hence, the identification of a suitable method becomes important for wastewater treatment. Many
studies have made use of nanomaterials for wastewater treatment through nanosorption, photocatalytic degradation
mechanisms, and membrane filtration (Yu et al., 2019; Zeng et al., 2018).
Highly stable and very efficient Fe-MNPs were prepared via a novel oxidative precipitation-combined iono-thermal
synthesis for degradation of organic contaminants with H2 O2 (Chen et al., 2017). It was reported that these MNPs were
magnetically recoverable and have high degree of recyclability and good catalytic activity. Poly(ethylenimine) (PEI) coated
MNPs have been proven to remove variety of wastewater contaminants. Lakshmanan et al. (2014) synthesized PEI-iron
oxide MNPs using a chemical co-precipitation method which were stabilized with trisodium citrate. The MNPs were able
to remove 50% of the total organic carbon (TOC) within 60 min from 0.5 L wastewater sample. Turbidity, colour, total
nitrogen and microbial content were also reduced by 89%, 86%, 24% and 90%, respectively. The PEI-MNPs reduced the
processing time, complexity, sludge production and requirement of additional chemicals for the treatment process. In
another study, a sustainable and eco-friendly method for the preparation of copper-doped Fe3 O4 MNPs (Fe3−x Cux O4 ) was
achieved, which enhanced the H2 O2 activation ability of these MNPs (Huang et al., 2018). The results suggested a much
faster decomposition of H2 O2 on Cu-doped MNPs as compared to undoped MNPs. The environmental application of the
enhanced activation ability of H2 O2 was described through the removal of ‘rhodamine B’ (RhB) from textile wastewater,
and removal efficiency of >97% was achieved.
Removal of coloured wastewater has been reported as a critical research problem, as dyes are stable organic compounds
that can remain in the environment for very long periods and affect the photosynthesis process. In a study, it was reported
that Kaolinite-supported nanoscale zero-valent iron (K–nZVI) can be successfully used to remove more than 97% of crystal
violet (Chen et al., 2013). Moreover, the authors reported after evaluating various adsorption and reduction kinetics,
isotherms, and thermodynamic parameters that a removal efficiency of more than 99.9% can be achieved for wastewater
treatment using K–nZVI MNPs. Similarly, a study reported that degradation of methylene blue (MB) dye was achieved
through betaine-modified magnetic iron oxide nanoparticles (BMNPs) synthesized by facile method (Wang et al., 2017a,b).
The BMNPs exhibited excellent super-magnetic properties implying greater recyclability (∼73% up to 5 cycles). The
maximum adsorption capacity of MB dye was calculated as 136 mg/g at room temperature and the adsorption data fitted
closely with Langmuir adsorption isotherm model. Fe3 O4 MNPs produced by co-precipitation method using glutaraldehyde
were studied for the removal of direct green azo dyes, reactive red azo dyes, and a mixture of both green and red dyes
by Darwesh et al. (2019). These MNPs were reported to be stable even after 90 days and maintained maximum activity
10
upon recycling for 100 cycles. It was also reported that complete decolouration of red and green azo dyes was achieved
after 4 h, whereas the mixture of both dyes disappeared after 6 h from the textile wastewater samples. In another study,
a low cost and selective adsorbent was prepared by grafting poly(ionic liquid) (PIL) onto the silicon coated Fe3 O4 NPs via
polymerization method (Yang et al., 2019). The synthesized MNPs were tested for the removal of various dyes, including
alizarin red (AR), thionin acetate (TA), malachite green (MG) and acid orange II (AO). The adsorbent demonstrated ultrafast
adsorption process reaching a maximum adsorption capacity up to 510.2 mg/g for AR. In a recent study, a novel three-
dimensional (3D) magnetic bacterial cellulose nanofiber/graphene oxide polymer aerogel (MBCNF/GOPA) was synthesized
and analysed for removal of malachite green (MG) dye from wastewater solution (Arabkhani and Asfaram, 2020). The
results suggested that the adsorption of MG dye was an endothermic and spontaneous process with 93% removal. The
MNPs demonstrated superparamagnetic behaviour (at room temperature), lightweight, large specific surface area, and
had simple and eco-friendly synthesis.
With the advent in science and technology, the use of pharmaceutical and personal care products (PPCPs) has also
increased drastically. Waste generated from these products, especially the pharmaceutically active compounds (PhACs)
such as antibiotics, hormones, etc. has been a concern for researchers due to their impact on human health and
environment (Freyria et al., 2018; Wang and Chu, 2016). In a study, 2-D graphene oxide (GO) and graphite carbon
nitride (g-C3 N4 ) were used along with Fe3 O4 MNPs to prepare a novel adsorbent for the treatment of wastewater (Sahoo
et al., 2020). Authors reported that toxic tetracycline (TC) antibiotic and methylene blue (MB) dye can be simultaneously
removed from the wastewater due to π -π and hydrogen bonding interaction, and the adsorbed TC and MB can be
recovered and reused up to 5 cycles. In another study, an efficient amino-modified magnetic nano adsorbent (Fe3 O4 @SiO2 -
NH2 ) was prepared for the removal of methylparaben (MeP) from wastewater samples (Mohammadi et al., 2018). The
optimum conditions for 98% removal of MeP was achieved at an adsorbent dosage of 1.1 g/L and reaction time of 120
min, with the maximum adsorption of 75 mg/g. In a study by Arabkhani et al. (2021), a novel magnetic nanocomposite
(NC) was prepared through a combination of solvothermal and solid-state dispersion methods. The magnetic NCs were
found successful in removal of diclofenac sodium (pharmaceutical drug). The NCs showed a good removal efficiency even
after five cycles of regeneration.
The nanotechnology has been proven as a cost-efficient and the MNPs have shown increased stability, targeted
contaminant removal, and high rate of potential reusability, as seen through the studies presented earlier. Various other
bench-scale and field studies have been conducted for removal of various types of organic pollutants from wastewater.
A summary for the research papers published since the year 2020 is compiled in Table 2. It can be concluded that the
efficiency of contaminant removal from wastewater using MNPs is very high. Based upon the mechanisms of removal, it
can be said that magnetic nanosorption is the most suitable mechanism for the pollutant removal from wastewater. The
photocatalytic degradation using MNPs is another efficient mechanism for the contaminant removal and degradation.
5.2. Removal of inorganic pollutants using MNPs
The use of MNPs is not just limited to the removal of organic pollutants. Several heavy metals such as copper, mercury,
chromium, etc., which are present as toxic inorganic contaminants in the environment, can also be removed efficiently
from the wastewater using MNPs. Moreover, the MNPs can also be implemented for nutrient recovery and removal
from wastewater. In recent times, various MNPs have been used to prepare colorimetric sensors for the detection and
subsequent removal of heavy metals, which has proven to be a simple and cost-effective approach (Das et al., 2018; Jiang
et al., 2019)
A low-cost, environment-friendly, novel magnetic nanoparticles (γ -Fe2 O3 ), was used as an adsorbent for ultrasound-
assisted removal of Pb2+ ion from wastewater (Dil et al., 2017). A maximum adsorption capacity of 163.57 mg/g was
reported within 4 min of ultrasound time, with the adsorption kinetics represented by Langmuir isotherm model. In
another study, a novel and environmentally friendly synthesis process was adopted to prepare Fe3 O4 /porous graphene
NCs for the removal of heavy metal ions from wastewater (Bharath et al., 2017). The study reported ultrahigh adsorption of
Pb2+ , Cu2+ and Cd2+ ions using the Fe3 O4 /graphene nanocomposites. These magnetic NCs demonstrated high adsorption
capacity, easy separation and reusability due to the high surface area of graphene, and magnetic properties of Fe3 O4 .
Lingamdinne et al. (2017) used a biogenic synthesis method to prepare magnetic inverse spinel iron oxide nanoparticles
(MISFNPs) using extract of Cnidiummonnieri (L.) Cuss (CLC) as a precursor. The batch adsorption studies revealed that
Pb(II) and Cr(III) can be efficiently adsorbed on the surface of MISFNPs, and it was observed that these MISFNPs can
be reused and recycled as well. Rajput et al. (2017) successfully synthesized superparamagnetic maghemite (γ -Fe2 O3 )
nanoparticles of controllable morphology using flame spray pyrolysis (FSP) technique. The maximum adsorption capacities
were reported as 68.9 mg/g for Pb2+ and 34.0 mg/g for Cu2+ . The equilibrium data for Pb2+ was best represented by
Freundlich isotherm equations, whereas the Langmuir isotherm equations best fit the equilibrium data for Cu2+ . In a recent
study, novel iron-oxide filled multi-walled carbon nanotubes (m-MWCNTs) were successfully synthesized and studied for
simultaneous removal of heavy metals and cyanate from wastewater samples (Ranjan et al., 2019). The authors reported
that the removal efficiencies of 39.31%, 35.53%, 34.48%, 29.63%, and ≥84% for chromium, iron, lead, copper, and cyanate,
respectively from a synthetic wastewater sample. The m-MWCNTs were reported to retain >94% of their initial activity
after 10 cycles of bio-catalytic activity.
Apart from heavy metals, the nutrient load in wastewater effluents has also been a concern for researchers around
the world. Vegetation, atmospheric deposition, and fertilizers are the primary source of nutrient load, especially in urban
11
Table 2
Remediation of various types of organic pollutants from wastewater by MNPs and their removal mechanism.
No. Name of MNP Contaminant removed Removal Contact Removal Reusability of NM Reference
mechanism time efficiency
1. Humic acid Carcinogenic malachite Adsorption 35 min 97% Up to five cycles for Gautam and
functionalized Fe3 O4 green dye 85% removal Tiwari (2020)
2. Combination of Fe3 O4 Bromophenol blue dye Photocatalytic 60 min 98% Up to three cycles Fatimah et al.
and Fe2 O3 degradation for 95% removal (2020)
3. Silica coated Emulsified oil Transformation 05 min 98% Up to five cycles for Lü et al. (2020)
ferro-ferric oxide 95% removal
(Fe3 O4 @SiO2 )
4. Magnetic activated Pharmaceutical Adsorption 06 min 99.97% Up to five cycles for D’Cruz et al.
carbon-Fe3 O4 substance 99% removal (2020)
(AC-Fe3 O4 )
5. JC-Fe3 O4 and CT-Fe3 O4 Organic dyes Adsorption 120 min 99% Not studied Das et al. (2020)
NPs
6. Nano porous E. faecalis Disinfection 05 min 100% Not studied Abou Hammad
Co2 O3 /Cu2 O3 : et al. (2020)
Al2 O3 :SiO2
7. Magnetic Janus Cooking oil and crude Phase- 15 min 96% Up to five cycles for He et al. (2020)
nanoparticles (M-Janus oil separation 90% removal
NPs)
8. FeNi3@SiO2@TiO2 Humic acid (HA) Photocatalytic 30 min 100% Not studied Khodadadi et al.
degradation (2020)
9. Chitosan-coated Bio-refinery Adsorption 90 min 46.2% Up to five cycles for Kumar et al.
magnetic nanoparticles wastewater containing 20% of initial (2020)
(cMNPs), phenol removal efficiency
10. Moringa extract Colour Coagulation 07 min 89% Up to two cycles for Triques et al.
modified MNP 80% removal (2020)
11. Copper-doped ZrO2 Methyl orange dye Photocatalytic 100 min 98% Up to four cycles Reddy et al. (2020)
MNPs degradation for 90% removal
12. MOM-Fe3 O4 Pharmaceutical Adsorption 720 min 93.9% Not studied Cusioli et al.
substance (2020)
13. Novel MNP-alum Adsorption cum Natural organic 30 min 98.7% Up to five cycles Kumari and Gupta
conjugate enhanced coagulation– matter with ∼91% removal (2020)
flocculation
14. MCPEI Black 5 dye Adsorption 180 min 100% Up to five cycles for Nordin et al.
(polyethyleneimine and 48% removal (2021)
magnetic nanoparticle)
15. Magnetic silica-based Pharmaceutical Adsorption 200 min 80% Up to eight cycles Peralta et al.
nanoadsorbents substance for 100% removal (2021)
areas. The nitrogen loading can also be increased through natural nitrogen cycle. Hence, cost-effective methods with high
removal efficiency are required for nutrient removal from wastewater, and nanotechnology plays a key role for the same.
In a study, aluminium doped MNPs were synthesized through co-precipitation method studied for removal of phosphorus
from wastewater samples (Xu et al., 2017) suggesting high adsorption capacity by the MNPs. In another study, novel
magnetic nano-composites (Fe3 O4 @EPS) were synthesized via co-precipitation method (Govarthanan et al., 2020). These
Fe3 O4 @EPS MNPs were found to be highly magnetic in nature (5.0 emu/g). It was found that under optimum conditions,
91% of PO4 3− and 85% of NH4 + was found to effectively removed from the wastewater samples.
Various studies conducted since 2020 for evaluating the effects of MNPs on removal of inorganic pollutants from
wastewater are summarized in Table 3. It can be seen here that most of the studies for the removal of inorganic pollutants
from wastewater have been performed on batch scale studies on synthetic wastewater solutions. However, it is important
to note that the use of MNPs makes it possible to target more than one pollutant and enhance the removal efficiency. It
can also be inferred through these studies that adsorption along with redox reactions remains the mostly used mechanism
of contaminant removal for inorganic pollutants. High removal efficiency, more surface area, easy and spontaneous
separation, and low cost are some of the success factors behind the use of MNPs in wastewater remediation.
6. Toxicity and legalization of MNPs
Every invention brings a lot of excitement and uncertainties with it and causes a scientific debate with respect to
its societal, economical, ethical, and environmental aspects. It can be expected that nanomaterials including MNPs and
their use in wastewater remediation will have certain repercussions as well. Some of these negative aspects may be
anticipated, and some of these may well not be. Although some researchers have started focussing on the negative impacts
of nanotechnology, they are mostly focused on the technological aspects. Hence, more studies must be conducted keeping
in mind the societal, ethical, and economical aspects as well (Mohmood et al., 2013).
The use of MNPs in wastewater treatment also leaves a possibility of these magnetic NMs remaining in water due to
their small size, subsequently entering the human body and causing toxicity. Moreover, many of these NMs may cause
12
Table 3
Remediation of various types of inorganic pollutants from wastewater using MNPs and their removal mechanism.
No. Name of MNP Contaminant removed Removal Contact Removal Reusability of NM Reference
mechanism time efficiency
1. Fe3 O4 @Ag@MESNa Hg(II) Adsorption 30 s 100% Up to two cycles Vicente-Martínez
for 100% removal et al. (2020)
2. Magnetic eggshell lead Adsorption 48 h 95% reusable Peigneux et al.
membrane (MESM) (2020)
3. Fe3 O4 @EPS PO4 2− Adsorption 13 h 91% Not studied Govarthanan et al.
(2020)
NH4 + 85%
4. Magnetic tubular carbon Cu(II) Adsorption 10 min 99.9 ± 0.1% Up to six cycles Ahmad et al.
nanofibers (MTCFs) for 85% removal (2020)
2+ 2+
5. JC-Fe3 O4 and CT-Fe3 O4 Co and Cu Adsorption 120 min 513.7 mg/g for Not studied Das et al. (2020)
NPs Co2+ and
463.23 mg/g
for Cu2+
6. Hyperbranched Ni, Cu and Al Adsorption 130 min 94% Up to nine cycles Almomani et al.
polyglycerol HPG-MNPs for 90% removal (2020)
2+
7. Maghemite nanoparticles Cd ions Adsorption 01 h 84% reusable Devatha and
coated Bacillus subtilis Shivani (2020)
8. Chitosan-coated magnetic Bio-refinery Adsorption 90 min Cu (42.2%), Cr Up to five cycles Kumar et al.
nanoparticles (cMNPs), wastewater (18.7%), and As for 20% of initial (2020)
containing heavy (2.44%) removal efficiency
metals
9. Superparamagnetic Pb2+ and Cd2+ Adsorption 55 min Pb2+ : 93.5 Up to five cycles Masjedi et al.
Fe3 O4 @SiO2 @GLYMO(S)-en mg/g for 90% removal (2020)
Cd2+ : 80.64
mg/g
10. Eucalyptus leaf extracts PO4 2− Adsorption 30 min 99.8% Not studied Xu et al. (2020)
(EL-MNP@zeolite)
+
NH4 43.3%
11. MNP@SiO2 –PEI-DTPA Pb2+ and Cd2+ Adsorption 72 h >90% Up to five cycles Zhu et al. (2020)
for 80% removal
12. Nanochitosan coated Pb(II), Cu(II) and Adsorption 10– 57.6%–95.5% Up to three cycles Hosain et al.
MNPs Cd(II) 30 min for 96% removal (2020)
13. Epoxy-Triazinetrione- Malachite green (MG) Adsorption 15 min 95% Up to six cycles Nejad and
Functionalized and Pb(II) for 61% removal Mohammadi
MNPs (2020)
14. DES/GO-Fe3 O4 nanohybrid Pb(II) Adsorption 20 min 80% Not studied Mehrabi et al.
(2020)
15. Magnetic nanoparticles Cr(VI) Adsorption 60 min 99.4% Not studied Saravanan et al.
coated mixed fungal (2021)
biomass (MNP-FB)
environmental toxicity which consequently may affect human health as well. The use of MNPs in clothes as antimicrobials,
personal care products, and cosmeceuticals has increased a lot in recent years (Fytianos et al., 2020). Since clinical trials
are not required for these, many other negative impacts like reactivity of smaller particles, toxicity etc. is not explored
in detail (Kaul et al., 2018). MNPs have also been reported to affect the circulatory system, digestive system, endocrine
system, nervous system, and immunity in humans (Ayubi et al., 2019; Jiang et al., 2019).
It can be concluded that most of the acute toxic effects caused due to exposure to various types of magnetic
NMs include, generation of reactive species, denaturation of protein structure, effect on mitochondria, asthmatic and
carcinogenic effects, possible organ enlargement, retention in the body, and elimination from the body (Malhotra
et al., 2020). Hence, certain legal aspects must be brought in to address the common global concerns over the use of
nanomaterials. The human health and environmental safety related to use of these MNPs may be reduced through certain
practices such as, collection of reliable scientific data, establishment of prudent practices and punishments, increasing the
awareness with respect to nanomaterial toxicity, enforcing an international consensus and obligations. A balance must
be ensured between technological development and hazard prevention. It has also been found that same MNPs may have
varying levels of toxicity in different study models, hence studies focussed on accurate assessment of the toxicity caused
by these MNPs. However, it is noteworthy that compared to other NMs, MNPs can be easily recovered and reused, which
somewhat reduces the possibility of their discharge in to the environment.
7. Future research prospects
Rapid advancements in science and technology, and breakthrough in the applications of MNPs in wastewater re-
mediation have made rapid steps in the field of nanotechnology. Especially in recent years, the economic impacts of
nanotechnology research works have increased significantly. Since, a large number of studies have been conducted
13
on synthetic wastewater solutions, there is a need for more field studies which must be conducted to address some
possible issues like, (a) performance evaluation of MNPs on large-scale plants and industrial applications, (b) assessment
of simultaneous removal of multiple contaminants and evaluate the removal efficiencies of magnetic nanocomposites, (c)
eco-toxicity and behavioural toxicity assessment of MNPs, (d) proper disposal of MNPs after their saturation (post their
regeneration cycles), (e) life cycle analysis of MNPs and their impact assessment in different ecosystems. Since, most of
the studies have reported a recycling of MNPs up to five cycles of reuse, hence, more studies are required to search for
stable and recyclable materials for commercial applications.
8. Conclusions
Several studies have been published concerning the utilization of MNPs for wastewater treatment and contaminant
removal/degradation. The literature present in this review paper demonstrated that various types of organic and inorganic
pollutants can be successfully removed from wastewater using MNPs. These methods have been proven to be cost-
effective, highly efficient and provide rapid results, as studies have reported that >95% removal efficiency can be achieved
within 5 min. However, it is worth noting that the removal efficiencies increased in case of magnetic nanocomposites as
compared to other types of MNPs. Moreover, photocatalytic degradation, adsorption and transformation through redox
reactions have been the most successful mechanisms for the contaminant removal and offers better sustainability. It has
been found that various MNPs have very high magnetic saturation which reaches up to 70 emu/g. MNPs have been proven
to be more stable, shown capabilities to target specific contaminants, offer easy separation, and have a high degree of
reusability and regeneration capacity. Results also suggested that removal efficiency is not affected even up to recycling
for 5 cycles retaining >95% removal efficiency. It can also be concluded that the use of MNPs, especially for biosynthesized
MNPs, is more cost-efficient as compared to most of the traditionally used methods such as activated carbon, activated
sludge process, membrane filtration etc in case of wastewater treatment. However, more studies on economics and toxicity
of using magnetic nanomaterials for wastewater treatment must be conducted.
CRediT authorship contribution statement
Saurabh Shukla: Visualization, Conceptualization, Writing – Original Draft . Ramsha Khan: Methodology, Writing –
Original Draft, Writing – Review & Editing. Achlesh Daverey: Conceptualization, Writing – Review & Editing, Supervision.
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgements
SS and RK are thankful to Prof. (Dr.) A. K. Singh, Vice-Chancellor, Shri Ramswaroop Memorial University for support in
conduction of this study. The support of our families during the compilation of this paper is to be highly acknowledged.
All authors read and approved the manuscript.
Appendix A. Supplementary data
Supplementary material related to this article can be found online at https://doi.org/10.1016/j.eti.2021.101924.
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Environmental Technology & Innovation 24 (2021) 101924

Contents lists available at ScienceDirect

Environmental Technology & Innovation

Synthesis and characterization of magnetic nanoparticles, and

2.2.2. Laser pyrolysis .............................................................................................................................................................. 6

2. Synthesis of magnetic nanoparticles

2.1. Physical methods of synthesis

2.1.1. Mechanical milling

Fig. 1. Chronological developments in the field of nanotechnology.

2.1.2. Electron beam lithography

2.1.3. Gas-phase deposition

2.1.4. Vapour deposition and patterning

2.1.5. Electrical explosion of wires

2.2. Chemical methods of synthesis

2.2.1. Spray pyrolysis

2.2.2. Laser pyrolysis

2.2.4. Thermal decomposition

2.2.6. Hydrothermal/solvothermal method

2.2.7. Sol-gel method

2.2.8. Polyol method

2.2.9. Non-thermal plasma methods

2.3. Biological methods

2.4. Comparison between physical, chemical and biological synthesis approaches

3. Key properties and characterization of MNPs

3.1. Geometry of nanoparticles

3.2. Structural properties of nanomaterials

3.3. Surface charge and thermodynamic properties of nanoparticles

3.4. Magnetic properties of nanomaterials

4. Mechanisms of contaminant removal using MNPs

5. Recent applications of MNPs in wastewater treatment

5.1. Removal of organic pollutants using MNPs

5.2. Removal of inorganic pollutants using MNPs

6. Toxicity and legalization of MNPs

7. Future research prospects

CRediT authorship contribution statement

Declaration of competing interest

Appendix A. Supplementary data

Supplementary material related to this article can be found online at https://doi.org/10.1016/j.eti.2021.101924.

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