Environmental Science and Pollution Research

https://doi.org/10.1007/s11356-021-16045-0

REVIEW ARTICLE

Carbon and polymer-based magnetic nanocomposites for oil-spill

remediation—a comprehensive review
Ahsan Mehmood 1 & Fahad Saleem Ahmed Khan 1 & Nabisab Mujawar Mubarak 1 & Shaukat Ali Mazari 2 &
Abdul Sattar Jatoi 2 & Mohammad Khalid 3 & Yie Hua Tan 1 & Rama Rao Karri 4 & Rashmi Walvekar 5 &
Ezzat Chan Abdullah 6 & Sabzoi Nizamuddin 7

Received: 29 April 2021 / Accepted: 15 August 2021

# The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2021

Abstract
Oil spills are a major contributor to water contamination, which sets off a significant impact on the environment, biodiversity, and
economy. Efficient removal of oil spills is needed for the protection of marine species as well as the environment. Conventional
approaches are not efficient enough for oil-water separation; therefore, effective strategies and efficient removal techniques (and
materials) must be developed to restore the contaminated marine to its normal ecology. Several research studies have shown that
nanotechnology provides efficient features to clean up these oil spills from the water using magnetic nanomaterials, particularly
carbon/polymer-based magnetic nanocomposites. Surface modification of these nanomaterials via different techniques render
them with salient innovative features. The present review discusses the advantages and limitations of conventional and advanced
techniques for the oil spills removal from wastewater. Furthermore, the synthesis of magnetic nanocomposites, their utilization in
oil-water separation, and adsorption mechanisms are discussed. Finally, the advancement and future perspectives of magnetic
nanocomposites (particularly of carbon and polymer-based magnetic nanocomposites) in environmental remediation are
presented.

Keywords Magnetic . Nanocomposites . Oil adsorption . Oil removal mechanism . Superparamagnetic . Oil spill clean-up .
Magnetic separation

Introduction hazard. International Tanker Owners Pollution Federation

The unintentional discharge of crude oil and its products into
the oceans is referred to as an oil spill or leak (Li et al. 2016). It
is a matter of urgent attention for governments as well as
marine monitoring agencies, as it is a severe environmental
(ITOPF) revealed in their recent report (2018) that crude oil
amounting up to~ 5.7 million tons ended up or was spilled into
sea ecosystem from 1970 to 2017. There have been more than
twenty-five oil-spills since 1940, which have adversely affect-
ed the livelihood of the regions as well as recreational

Responsible Editor: Angeles Blanco

* Nabisab Mujawar Mubarak 4

mubarak.mujawar@curtin.edu.my; mubarak.yaseen@gmail.com
5
1
Department of Chemical and Energy Engineering, Faculty of
Engineering and Science, Curtin University, 98009 Miri, Sarawak,
Malaysia
2 6
Department of Chemical Engineering, Dawood University of
Engineering and Technology, Karachi 74800, Pakistan
3 Malaysia (UTM), Jalan Sultan Yahya Petra, 54100 Kuala
Graphene & Advanced 2D Materials Research Group (GAMRG),
School of Engineering and Technology, Sunway University, No. 5,
7
Jalan University, Bandar Sunway, 47500 Subang Jaya, Selangor,
Malaysia
Petroleum, and Chemical Engineering, Faculty of Engineering,
Universiti Teknologi Brunei, Bandar Seri Begawan, Brunei
Darussalam
School of Energy and Chemical Engineering, Department of
Chemical Engineering, Xiamen University Malaysia, Jalan Sunsuria,
Bandar Sunsuria, 43900 Sepang, Selangor, Malaysia
Department of Chemical Process Engineering, Malaysia-Japan
International Institute of Technology (MJIIT), Universiti Teknologi
Lumpur, Malaysia
School of Engineering, RMIT University, Melbourne 3000,
Australia

activities (Cirer-Costa 2015). The formation of thick sludge
on the surface of the ocean is an alarming threat to aquatic
biodiversity. It threatens the growth of the indigenous crea-
tures living in waterbodies, disturbing offshore and onshore
ecosystems. The release of oil spills into the aquatic environ-
ment will increase during the production, exploration, trans-
portation, and storage of highly flammable petroleum. Their
products are always a potential threat to nature (Farrington
2014). The most common petroleum products that are spilled
in water are diesel, kerosene, gasoline, heavy oils, petrol, fuel
oil, etc. The presences of various volatile organic compounds
(VOCs), petroleum hydrocarbons (PHCs), and other flamma-
ble petroleum products can cause severe mental and wellbeing
issues upon getting in contact with water or consuming marine
species. These problems include but not limited to skin dis-
eases, dizziness, asthma, liver damage, inflammation, nervous
effects and cardiovascular disorders (Eykelbosh 2014).
Consequently, an efficient approach is needed to remove
thick layers of oil from the water surface to protect marine life
and the environment. Several techniques have been intro-
duced in the past, which are categorized as physical, chemical,
bioremediation, and thermal. A few examples of categorized
techniques use adsorbents, surfactants, in situ burning, and
bio-remediation (Dave and Ghaly 2011), (Moustafa et al.
2017). However, these techniques are not very efficient and
further create more sludge. Hence, nanotechnology has gained
substantial attention for removal of oil spills (Kharisov et al.
2014), (Mahajan 2011). Magnetic nanomaterials exhibit ex-
ceptional properties like high stability, high adsorption capac-
ity and recyclability, and super paramagnetism, which makes
them able to treat oil-polluted water more efficiently and min-
imize the generation of further sludge (Saber et al. 2015). Both
magnetic nanocomposites and nanoparticles are widely
employed to treat oil contaminated water due to their unique
magnetic features and high efficiency. For instance,
superparamagnetic iron oxide nanoparticles (SPIONs) have
huge potential of cleaning up the oil from the surface of water,
due to their extremely small size (nanoscale), high surface
area, and superparamagnetic behavior that offers the capabil-
ity to attract the hydrocarbons. (Saharan et al. 2014).
Nanomaterials are described as multiphase materials com-
prised of nanoparticles with a solid bulk matrix combination,
for example, gels, colloids, and polymers (Thanikaivelan et al.
2012). They possess unique thermal, electrochemical, me-
chanical, optical, and magnetic characteristics. The term mag-
netic nanocomposites are defined as multicomponent mate-
rials typically composed of nanosized magnetic materials to
respond to external stimuli (such as an alternating magnetic
field or external static) (Behrens and Appel 2016). Hybrid
core-shell multi-component is the most known kind of func-
tional magnetic nanocomposite. These nanocomposites are
vastly employed to recover oil from oil-water emulsions
(Zhu et al. 2010b).
Environ Sci Pollut Res
So far, numerous studies have been carried out that empha-
size the fabrication of novel magnetic nanocomposites, spe-
cifically for oil spill removal. The current review highlights
carbon-based and polymer-based magnetic nanocomposites
used for cleaning up oil from the water surface. The study is
distributed into two sections. The first section focuses on the
fabrication techniques that have been designed for
the development of magnetic nanocomposites (carbon/poly-
mer based). The second section provides insights into the di-
verse applications of the magnetic nanocomposites (carbon/
polymer based) that can be successfully employed in the real
world for treating oil spills.
Magnetic nanocomposites
The term magnetic nanocomposite is defined as the combina-
tion of nanosized magnetic material and a host material such
as carbon, polymers, metals, gels, proteins, and liquids. They
exhibit the characteristic features of nanomaterial and embed-
ded matrix (Zhu et al. 2013). These multiphase components
vary in crystalline morphology and size and largely depend on
the material’s nanoscale. Furthermore, they display high sat-
uration magnetization value, magnetic susceptibility, magnet-
ic moments, and magnetic anisotropy. Due to the strong mag-
netic characteristics of magnetic nanocomposites, these com-
posites are significantly used and studied in numerous sectors,
for instance, biomedical and environment as drug delivery, oil
remediation, heavy metal ions, and dyes removal from differ-
ent water sources (Masotti and Caporali 2013). Magnetic tech-
nology is also getting attention in the food industry such as
pathogenesis removal-related chitinases and proteins from
wine (Mierczynska-Vasilev et al. 2019).
Due to the popularity of magnetic nanocomposites in the
real world, various approaches have been introduced to pro-
duce magnetic nanocomposites such as pyrolysis, thermal cur-
ing, arc discharge, self-assembly, solution blending, melt
blending, and ball milling. In this review, we have focused
only on the approaches; there are cost-effective, practicable,
high scale production, high quality, and convenient operation
(Siddiqui et al. 2018). Fig 1 depicts few well-known synthesis
approaches for the carbon-based and polymer-based magnetic
nanocomposites for a range of applications.
Polymer-based magnetic nanocomposites
Synthesis of inorganic/organic hybrid nanocomposites com-
prised of magnetic and polymer components has been able to
gain attention due to a vast array of applications.
Advancement in polymer science has created the capability
to fabricate a wide range of materials possessing features like
electro-active and better mechanical and thermal properties
(Reiss and Hütten 2005). The polymer properties could be
Environ Sci Pollut Res
Fig 1 Synthesis approaches of magnetic nanocomposites
manipulated in a form of nanocomposite material that includes
optical, thermal, mechanical, toxicity, biodegradability, and
hydrophilic/hydrophobic balance. These properties are con-
trolled to form a desired composite material via selecting the
appropriate polymer. Instead of this renewed attention in the
direction of nanocomposites, scientific society began finding
novel approaches to manipulate materials that were associated
with the desired features of nanoparticles as well as polymers
for the development of nanocomposites. One of the advan-
tages of nanocomposite is to mix various materials and en-
hance the overall characteristics. However, in magnetic poly-
mer nanocomposites, interactions of organic/inorganic nature
add up novel features that could not be attained either in an
individual organic nor inorganic component.
For oil recovery from aqueous applications, magnetic poly-
mer nanocomposites have shown excellent removal efficien-
cy. Therefore, several studies have been conducted to prepare
novel nanocomposites with high removal efficiency. For in-
stance, Mirshahghassemi et al. prepared magnetic polymer
nanocomposite using magnetite nanoparticles and functional-
ized polyvinylpyrrolidone under environmentally relevant
conditions (Mirshahghassemi and Lead 2015). The research
concluded that the prepared nanocomposite could remove the
oil with high removal efficiency over a short period. Yu et al.
also prepared magnetic polymer nanocomposite by coating
polystyrene onto magnetic nanoparticles using the solvent-
thermal approach for oil removal application (Yu et al.
2015). The prepared nanocomposite was capable of adsorbing
diesel as high as 2.5 times its weight. In another study,
Tempesti et al. showed that up to 76% of diesel oil could be
absorbed, when magnetic nanoparticles are reinforced within
polystyrene beads to form magnetic polymer nanocomposites
using the polymerization approach (Tempesti et al. 2014). In
this research, a novel magnetic nanocomposite of polystyrene
and polystyrene was prepared via the solvothermal method
The prepared nanocomposite displayed selectivity for crude
and lubricating oil. It was observed a unique absorbing
capacity in a range of 40 and 37 times more than its weight
for crude and lubrication oil, respectively.
Based on the literature, different challenges have been en-
countered in producing nanocomposites of desired character-
istics (Dobson 2006). The main hindrance in nanocomposite’s
high scale production and commercialization is the unavail-
ability of cost-effective techniques to control the nanoparticle
dispersion in the polymeric host. In general, nanoparticle ag-
gregates eventually avoid its advantages linked with the di-
mension (Balazs et al. 2006). The particles need to be inte-
grated, which leads to isolated, good dispersion of nanoparti-
cle within the matrix. Therefore, there is a necessity for de-
signing a synthesis technique that is efficient on the nanoscale
yet suitable for macroscopic processing. Fabrication with high
homogeneity is undoubtedly an issue for nanocomposites.
Scientific society has designed a range of techniques to syn-
thesize nanocomposites that include microemulsion, plasma
polymerization, suspension polymerization, melt-blending,
dispersion polymerization, solution blending, ball milling,
and layer by layer deposition (Khan et al. 2020). Table 1 lists
the merits and demerits of a few known synthesis techniques
designed for magnetic polymer nanocomposites.
Carbon-based magnetic nanocomposites
Recently, advancements in hybrid nanomaterials have direct-
ed attention to the revived studies in the production of manip-
ulated materials, for instance, carbon-based magnetic nano-
composites. The remarkable application of carbon-based mag-
netic nanocomposites in areas such as bio-sensing devices,
catalysis, adsorption, and super-capacitance. (Siddiqui et al.
2018). These nanocomposites are referred to as extremely
competent magnetically recoverable catalysts that have the
potential to merge with a wide range of complex structures
and active components for immobilization. A study conducted
by Frey and co-workers highlighted the characteristics of
magnetic nanomaterials, which allow them to be a suitable
candidate for biomedical applications, specifically for mag-
netic resonance imaging (Frey et al. 2009). Lin and co-
workers also conducted research using carbon-based magnetic
nanocomposites to eliminate heavy metal ions from wastewa-
ter (Lin et al. 2010). The study concluded that carbon-based
magnetic nanocomposites observed higher adsorption capac-
ity for arsenic ions. In a recent study, Thines et al. proposed
that these nanocomposites are suitable as electrodes in
supercapacitor devices due to their outstanding electrical con-
ductivity and overall capacitance (Thines et al. 2017).
As mentioned above, carbon-based magnetic
nanomaterials are gaining extensive attention in the scientific
society for industrial wastewater treatment as well as oil spill
recovery. The widely employed methods for carbon-based
magnetic nanocomposite synthesis are hydrothermal treat-
ment, chemical co-precipitation, and pyrolysis. Magnetic
 Environ Sci Pollut Res

Table 1 Synthesis approaches of polymer-based magnetic nanocomposites

Synthesis Merits Demerits References

/approach

Thermal • Simple approach, especially for thermosetting polymer • Re-modeling is a difficult task Advani and Hsiao
curing • Difficult to reuse (2012)
Melt blending • Potential to synthesize different nanocomposites • With high filler contents, the Rane et al. (2018)
• Well-recommended approach, especially for industrial applications approach demonstrates
• Cost-effective approach unsatisfactory dispersion
• Wide spectrum of materials can be employed • High temperature is essential
• Best for mass-scale production
• Environmentally friendly approach
Solution • Suitable for film or membrane formation • Higher capital cost Barnes et al. (1989),
blending • Show suitable dispersion and exfoliation of filler • Compatibility issues between Cheremisinoff
• Mostly suggested if the polymer show degradation polymer and solvent (2018)
• Re-assemble of polymer chains have
been observed during evaporating
Microemulsion • Time-saving • Difficult to remove residual of Mahdieh et al.
• One-step approach surfactants (2017)
• Higher molecular weight nanocomposites can be obtained • Considerable chain transfer to the
polymer may occur
Ball milling • A suitable approach for mass production • Low efficiency Bai et al. (2000)
• Environmentally friendly approach • Loading of the rotational ball is
• Supports modifying the fillers’ structure which eventually upgrades difficult
the fillers’ compatibility with polymer bends, in addition, offers • Producing thinner material is difficult
appropriate grafting reactions • Cause noise pollution
• Suitable for all grades of hardness • Higher consumption of electricity
Dispersion • Produce high yield • Prolonged operation Gupta and Kumar
polymeriza- • Potential to synthesize nanocomposites of various sizes • It cannot operate without a suitable (2008)
tion • Provide good control of polymer composition as well as molecular polymer stabilizer
mass
Layer by layer • Cost-effective • Prolonged operation Soler (2018)
deposition • Operate at room temperature • Further additional procedures are
• The film growth layer can be controlled at the nanoscale must for purification
Suspension • Ease and effective approach • Polymer purification is required Suganya and
polymeriza- • The range of polymers are applicable • Polymer size is difficult to control Anuradha (2017)
tion • No surfactant is required
• Cost-effective
Plasma • Time-saving • Low deposition rates Thiry et al. (2016)
polymeriza- • Operate at ambient atmosphere • Higher cost
tion • Environmentally friendly approach • Low abrasion resistance
• Handle varying nanocomposites' thickness
• Nanocomposites produced via this approach is very coherent,
adherent, and pin-hole free

carbon nanotube-based nanocomposites could be synthesized a magnetic carbon-based nanocomposite consisting of a

by filling carbon nanotubes (CNTs) with magnetic
ferrofluids or grafting or attaching magnetic nanoparticles
on carbon nanotubes (Gómez-Pastora et al. 2014).
Similarly, magnetic graphene oxide was developed by
using ferrous and ferric salts and graphene oxide as pre-
cursors. The adjustment of temperature between 80 and 90
°C and pH at 9–11 helped in forming magnetic nanopar-
ticles and deposition on GO (Zhu and Diao 2011b).
Similarly, Fe3O4/C core-shell nanocomposite was devel-
oped by the one-pot hydrothermal method by employing
glucose and FeCl3 as carbon and iron sources, respectively
(Xuan et al. 2007b). Pyrolysis is also found many appli-
cations and found to be a promising method. For example,
core-shell structure was synthesized by coating magnetic
nanoparticles with carbon precursors and followed by car-
bonization (Pang et al. 2019). The sol-gel method was
employed to prepare Fe2O3/multi-walled carbon nanotubes
nanocomposites (Kim et al. 2010). The common carbon-
based magnetic nanocomposite includes carbon nanotube-
based magnetic nanocomposite, graphene oxide-based
magnetic nanocomposites, biochar-based magnetic nano-
composite, and nanodiamond-based magnetic nanocompos-
ites (Pang et al. 2019). Lately, immense research and de-
velopment have been made using carbon-based magnetic
nanocomposites, especially for spilled oil recovery and
wastewater treatment. Gui et al prepared carbon nanotubes
Environ Sci Pollut Res
(CNTs)-based magnetic nanomaterial for diesel oil recov-
ery (Gui et al. 2013). The study concluded that the nano-
composites maintain their original structure and shown an
adsorption capacity of 56 g/g. In another study, magnetic
multi-walled carbon nanotubes (MWCNTs) embedded with
silicon oxide (SiO2) were prepared by Moustafa et al.
(Moustafa et al. 2017). The study revealed a high separa-
tion rate of 92.8% and was proposed as an effective nano-
composite for oil-water separation. In a similar study,
magnetic nanocomposites (Fe 3 O 4 /carbon nanotubes/
polyaniline) were prepared using an in situ approach and
had shown high removal capacity of 99.7% for diesel oil
recovery from seawater within first 10 min (Chu and Pan
2012). Fig 2 shows the graphical illustration of oil-water
separation using CNT-based magnetic nanocomposites.
Apart from CNTs, several other carbon-based materials
like activated carbon are also used for spilled oil recovery
in the research study done by Zhu et al.; activated carbon
was embedded in Fe3O4 via thermal decomposition ap-
proach (Zhu et al. 2010a). The results indicated that lubri-
cating oil can have absorbed as high as 3.8 times more
than its own weight and repelling most of the water.
Production of carbon-based magnetic nanocomposites
using the appropriate approach will dictate its efficiency.
Several studies have been carried out by the scientific
society to introduce efficient synthesis pathways to
achieve extremely stable, shape-controlled, and finest
well-defined magnetic carbon hybrid nanocomposites.
Few of the known synthesis approaches include hydro-
thermal, template-based, filling, pyrolysis, sol-gel,
microemulsion, and self-assembly. Table 2 shows the
merits and demerits of the synthesis methods of carbon-
based magnetic nanocomposites like hydrothermal, fill-
ing, sol-gel, self-assembly, arc-discharge, pyrolysis,
sono-chemical, chemical vapor deposition, detonation-
induced reaction, template-based, capillary action, and
pulse laser irradiation.
Fig 2 Schematic illustration of oil
removal using CNT-based mag-
netic nanocomposites
Application of magnetic-based
nanocomposites
Nanocomposites are synthesized for multiple applications
(Weldegebrieal 2020). A few of the well-known applications
of nanocomposites are illustrated in Fig 3. Applications across
various fields of study are due to the characteristics like mor-
phology, nanosize, unique magnetic features, and higher effi-
ciency. However, in this work, environmental applications of
nanocomposites are particularly focused for oil spill removal.
Conventional and advanced techniques of oil spill
remediation
Petroleum is produced and consumed in large volumes to
sustain the needs of a rapidly growing world. Release of oil
spills into the aquatic environment can takes place at various
operation stages like exploration, production, and transporta-
tion, as well as due to accidents and lack of compliance to
standards in drilling and production operations (Fard et al.
2016). According to the recent report, oil spills worldwide
are estimated to be at 700 metric tons (since 1970).
Furthermore, these oil spills have adverse environmental im-
pacts, which are directly accountable for the devastation of
marine species as consequent interaction between lipophilic
hydrocarbons and layers of lipid of flora and fauna results in
the intoxication that may even lead to death. The oil reduces
the contact area between the atmosphere and water that con-
sequently affects the biological oxygen demand (BOD) and
chemical oxygen demand (COD); thus, respiration of aerobic
organisms and photosynthesis by aquatic plants is disturbed
(Kingston 2002). Eventually, oil spills adversely impact the
food and tourism industry and thus show major impact on the
country’s economy. Table 3 provides a brief overview of oil
spill incidents along with their root causes, impact, conse-
quences, responses, and action taken by the authorities.
 Environ Sci Pollut Res

Table 2 Synthesis approach of carbon-based magnetic nanocomposites

Synthesis Merits Demerits References

Approach

Hydrothermal • Size of the nanostructure can be maintained • Needs high temperature and pressure for operation ~ Xuan et al. (2007a)
• Generate a phase, crystalline in nature that is not >200 °C and > 2000 psi)
steady at the melting point
Filling • Cost-effective • Prolonged process Zhu and Diao (2011a)
• Easy availability of raw material • Reusability and quality are not up to standard
• Used in many commercial applications such as • The mass ratio of magnetic and carbon precursors is
memory devices challenging
Sol-gel • The product quality could be managed • Unsatisfactory bonding Graf et al. (2003)
• High potential for the development of magnetic • High permeability
carbon hybrid materials • Cost of raw material is not cheap
Self-assembly • Properties of nanocomposites can be manageable • Nanocomposites’ uniformity is difficult Stoffelbach et al.
(2005)
Arc-discharge • Cost-effective • Inert condition is mandatory Qiu et al. (2004)
• Easy approach • Prolonged process
• Known for developing a product of the desired size • Difficult to attain the product from arc-chamber walls
Pyrolysis • Appropriate for mass production • Develop carbon black, which is an unwanted product Shen et al. (2010)
• Demonstrate good mechanical as well as magnetic • Inert condition must stop oxidation
strength
• Display ferromagnetic properties at ambient condition
Sono-chemical • Easy approach • High temperature is mandatory Samadishadlou et al.
• Known for developing a product of the desired size (2018)
• Potential to employ for the production of metal oxides
as well
Chemical vapor • Suitable for mass-production • Required high consumption of energy Holmberg and
deposition • Convenient procedure • Equipment is complex Matthews (2009)
• Nanostructure can be controlled
Detonation-induced • Yield production is satisfactory • Massive detonation could be dangerous Ning et al. (2009)
reaction • Develop a range of nanocomposites, i.e., 10 to 50 nm • Not recommended in terms of process safety
• Required complex facility
Template-based • Known for a high-quality product • The quality of the product is dependent on the template Dong et al. (2007)
• Shape and size could be managed structure.
• Multi-stages are required to develop the desired product
Capillary action • Suitable for a range of applications such as 3-D • Not valid if the substrate’s thickness is less than 100nm Komarneni (1992)
nanodevices
Pulse laser • Demonstrate satisfactory mechanical strength • Metallocene’s of different types are mandatory Park et al. (2008)
irradiation • Known approach for nanocomposites development • Prolonged process
• Cost-effective
• Convenient operation

Conventional oil spill removal technologies

Conventional methods of oil cleaning can be categorized into

four main classes, namely chemical treatment using disper-
sants, bioremediation, in situ burning, and mechanical tech-
niques using skimmers and booms (Jiang et al. 2010; Orbell
et al. 1997). However, numerous materials have been
employed for remediation of oil, such as adsorbents, disper-
sants, detergents, and solidifiers. These methods have many
disadvantages like creating secondary pollution in the form of
sludge, inefficient in the adsorption of thin oil layers, time-
consuming, and cost-intensive method. Table 4 shows the
conventional technologies used for oil spill removal. In the
research report released by the World Wide Fund (WWF) in
2009, highlighted those 20 years were still not sufficient to
restore the havoc caused by major oil spills. Yet, it is hard to
estimate any period to clean oil spill entirely from the water
Fig 3 Nanocomposite applications
Table 3 A brief overview of oil spill incidents along with their root causes, impact, consequences, responses, and action taken by the authorities

Incident Date and Spilled oil Area affected Spill Spillage causes Impact and consequences Response Actions References
location type quantity
(tonnes)
Environ Sci Pollut Res

WWII oil Waters of Crude 176,120 km2, 50 484,200 Cargo ship and No long-term impacts. While Torpedoing, burning, an General inquiry of the Campbell et al.
spillage Eastern petrole- miles of the ship tanker the short-term impact on action to change the incident, reported by (1977)
American um, American sinking Marine species and diving beach’s outlook the Department of
Coasts, along coastline birds Ocean Engineering,
Carolina, with its MIT
USA, products
1942
An oil spill Seven stones Crude oil 700 km2, around 119,328 Shipwrecking Thousands of seabirds died, Cleaning operation by the A marine organization Wells (2017)
of reef, 80 km of the threatened the livelihood of Ministry of Defence, is constituted by the
Torrey England, French locals, pollution in excessive usage of joint cooperation of
Canyon 18 coastline southwest England, polluted cleansing agents and governments
Marc- harbors, and beaches in the dispersants, weathering
h 1967 Brittany and Channel process, burning by aerial
Islands bombardment
An oil spill Brittany Heavy and 320 km of the 223,000 Ship breakage Millions of benthic More than 3000 tonnes of Inquiries by ITOPF (2017)
of Coast, light coastline of invertebrates died, sea dispersant were used, Franco-American by
Amoco France, 16 crude oil Brittany mollusks, sea urchins, and shores clean-up, pressure different agencies
Cadiz Marc- around 20,000 diving birds washing such as NOAA,
h 1978 died ERL, and CNEXO
An oil Caribbean Crude oil A most 287,000 An accident Twenty-seven people died, The fire burnt off all the oil, No investigation. (Horn and Neal
spillage Sea, West enormous, between large impact on zooplankton, Dispersant spray (1981)
of 1979 Indies, reported slick crude carriers brown shrimp, amphipods,
The Island of 25 miles, 10 consequently infant turtles, and redfish,
of miles off the resulted in an extensive impact on
Tobago, coast of explosion environment and
19 Tobago and biodiversity
July 1979 Trinidad
The oil North West Volatile 64 km off the 160,000 Drifting and Oiled feathered birds, offshore 230 m3 dispersants were used - ITOPF (2017)
spill of Cape To- crude oil Table Bay breaking of the breaking and drifting, oiling and sprayed at slick edges,
Castillo wn, SA, 6 burning vessel of 1500 gannets affected and booms were used
de August marine planktons
Bellver 1983
oil
The oil Nova Scotia Crude oil 700 nautical 132,000 The explosion Fish and other sea creatures Natural An amount of 86.7 ITOPF (2017)
spill of Canada 10 (North miles away resulted in the died dissipation/dispersion of million was spent; a
Odyssey November Sea) from Canadian shipwreck, oil, no action, sprayed dis- committee on marine
1988 Coast. firing persants pollution was set up
by Sea Council
An oil Prince Crude oil 28,000 km2, a 37,000 Exxon Valdez oil 35,000 dead birds were Recovery and containment, An amount of US 2 ITOPF (2017)
spillage William coastline tanker collected, 250,000 seabirds skimmers, booms, HP hot billion dollars was
of Sound, 800 km long, grounding died, high mortality water washing, spent, Oil pollution
Exxon USA was affected afterward of certain species bioremediation trials on a Act 1990, NOAA
Valdez large scale was formed
Table 3 (continued)

Incident Date and Spilled oil Area affected Spill Spillage causes Impact and consequences Response Actions References
location type quantity
(tonnes)

24 affected bald eagles and

Marc- otters
h 1989
An oil 1500 lm Heavy Oil slick of 80 260,000 Explosion, Fire Five-member of the ship were Minimal effect on the Investigated by various ITOPF (2017)
spillage from the crude oil km2 killed, the beaches were environment, oil agencies
of ABT coast of closed due to floating dead vaporized naturally, clean
Summer Angola, fishes, eutrophication, fishes up manually by workers
Oil Afric- tainted with oil, disturbing
a,11991 food chain
An oil spill The Persian Crude oil 101 ×42 miles 1,500,000 Resultant of action 600 oil wells were blown, fire, Oil penetrated sediments as Five hundred forty Bejarano and
of the Gulf, area affected, a against US explosion, sea marine no shore clean-up was million dollars spent Michel (2010)
Gulf January slick of 5 marines during organisms affected by performed to clean Saudi
War 1991 inches thick the Gulf War chemical pollutants, air coastline,
was formed pollution, birds, fish, otters Investigated by US
Gulf Environmental
Technical Support
An oil spill Northern Heavy fuel A shoreline of 77,000 Ship damage A sector of fishing and tourism A heavy clean-up operation Dues of €451.69 Acosta-González
of Spain, 13 oil 1900 km was was affected, rocky was performed, estuaries million in Galicia et al. (2015)
Prestige November affected shoreline contaminated booming and habitat sen- and €737.18 million
2002 heavily sitivity for all over Spain
An oil spill The Crude oil 8 km off the 11,000 Barrage hit An adverse impact on seabirds, Floating oil cleaning by A collective effort by Yang (2017)
of Hebei Republic coastline benthic species, affected sorbents, skimmers, the Korean coast
Spirit of South sandy beaches and rocky dispersants sprayed by guard, Korean navy,
Korea, 7 shores helicopters, manual KOEM
December cleaning by more than 100
2007 vessels and 1500 fishing
boats
An oil spill Gulf of Crude oils An area between 627000 The leakage Death of eleven people, Controlled burning of crude US coast guard, Beyer et al.
on Mexico, 6500 to consequently destruction of wildlife oil, 1.84 million gallons of National Response (2016)
Deepw- Mississip- 176,00 km resulted in an habitat, marine life, corals, dispersant sprayed, Team, EPA
ater pi, USA square was explosion of the birds, pelagic, and an skimmer ships used,
Horizon 20 April affected rig, blowout, adversely affected tourism manually removed in
2010 and leakage of and fishing industry Louisiana
oil for 87 days
Environ Sci Pollut Res
Table 4 A brief overview of conventional oil spill removal technologies along with their advantages and limitations

Technology Methods Advantages Conditions Limitations References

for oil spill
response
Types Mechanism Cost Environmental
Environ Sci Pollut Res

effect

Physical Skimmers Oleophilic Mechanical Expensive No adverse Removal of an oil spill, highly Thick slick, Only effective in calm weather, Kleinguetl et al.
surface removal effect efficient terrestrial oil structural constraints, access to (2020)
Suction/vacuum spills, calm the spill site, no useable in iced
Elevating weather water
Submerged conditions,
Weir floating oils
Booms Fence Mechanical Expensive Eco-friendly, no Large scale removal, treatment Small oil spills, the Cannot be employed in bad Song et al.
Fire resistant removal effect over large areas, sensitive thick layer of oil weather and high tides, rough (2014)
Curtain areas are protected by over a water sea conditions time-consuming,
diverting oil from them, surface, a stable requires manual labor,
remove emulsified oils environment submerged in high currents
Manual removal Use of bailers, Costly Not effected Very little waste generated, Storage and A slow process, intensive labor Robertson et al.
trowels, immediate action transportation required, unable to recover light (1997)
drums, used to clean oil, time-consuming
buckets, and heavy spills at
rakes the shoreline
Adsorbent Synthetic Adsorption Cost-effective In comparison, Possess high capacity of Only for small Sorbents are difficult to remove, Singh et al.
Natural organic natural removal spills, mostly non-useable in open waters and (2020a)
Natural sorbents are employed on viscous oils; more time is re-
inorganic eco-friendlier shorelines and quired
offshores,
floating oil
Chemical Solidifiers Gelling agents Cheap Not effected Quick solidification of oil, oil is Spills of lesser Produces wastes, solidifies are Motta et al.
consequently prevented from spreading by volume, light to required in large amounts, (2018)
solidify oil immobilization, can be heavy oils cannot be applied on oils
applied easily consisting of volatile
hydrocarbons
Dispersants Solvents Chemicals Expensive Harmfulness of Surface oil is removed, treats Open water, fresh Ineffective in a calm sea, impact on Harvey et al.
Stabilizers break down environment large area, and oil spills, viscous marine life is dangerous, (1990)
oil into has an impact biodegradation is enhanced oils are of low low-efficiency on emulsified or
smaller on marine medium heavily weathered oils
drops
Emulsifiers Demulsification Economical No harmful Separation of oil-water at a Fuel lubricants and Toxic to marine organisms Roulia et al.
impact higher rate, dispersion is oils, seashore (2003)
promoted, efficient collec- effectiveness for
tion of oil, low concentra- crude oils
tions
Thermal In situ burning Burning Cheap Method causes It can be applied in cold water, Remotely open sea Can affect marine biodiversity, Fritt-Rasmussen
pollution and no waste is generated, a area, normal inapplicable near coastal areas, et al. (2015)
large volume of oil is weather secondary pollution, another
removed conditions, the compound like CO, PAHs, SO2
thick oil layer is
required
Biological Microorganisms Microbial No cost, free Eco-friendly No manpower required, highly Weathered oil, thin Favorable pH and temperature Lin et al. (2010)
bioremedia- degradation effective, no requirement of oil layers, any requirements for microbial
tion machinery and equipment, size of the spill growth, dependent on nutrients,
natural incomplete oil removal, long
process

surface (Chen et al. 2013). The devastation caused by oil spill
events such as Campos/Brazil (2011), Gulf Mexico (2010),
and in Dalian/China (2010) consequently shows that novel
approaches of remediation need to be continuously explored
(Oliveira et al. 2012; Souza Jr et al. 2012).
Wastewater discharged from oil and gas industries consists
of lubricant mixture, cutting oils, heavy metals, oil fluids,
grease, heavy and light hydrocarbons, lubricants, and other
hazardous contaminants (Srinivasan and Viraraghavan
2008). Oily wastewater is discharged from different textile,
vegetable oil, food, domestic sewage, leather industries, vehi-
cles, kitchens, and metal (Santander et al. 2011). The oil con-
centration in wastewater released from industrial activities
may reach 40,000 mg/L (Arcadio 2000). It is simply released
to the environment without employing any effort on purifica-
tion or treatment that causes catastrophic environmental and
health issues, consequently disturbs the ecosystem.
Magnetic nanocomposites for the remediation of oil
spill
Magnetic nanomaterials are fabricated as nanoparticles em-
bedding magnetic nature of other materials (Ni, Mn,
maghemite, Co, mixed ferrites, Fe, etc.), hybrid nanostruc-
tures with hybrid magnetic characteristics. They also fabricat-
ed as molecular magnets such as magnetic nanofluids,
nanothreads, nano-beads, multilayer or single-layer films,
core-shell configurations, magnetic fluids, NP clusters or ag-
glomerates, ferrofluids, magnetic nanocomposites, magnetic
foams, and nano-beads. The nanoparticles fabricated by vari-
ous fabrication methods are biofunctionalized or surface
engineered with appropriate specific molecular species to gain
similar properties and structure (Lu et al. 2007). Fig 4 displays
some of the essential features of carbon/polymer-based mag-
netic nanocomposites. Further, they have an external response
to magnetic field in action, making them more beneficial in
the applications. In nanomaterials selection, several aspects
Fig 4 Few important features of carbon/polymer-based magnetic
nanocomposites
Environ Sci Pollut Res
are considered, such as superparamagnetic nature, oleophilic
dispersity, magnetic recoverability, hydrophobicity, crystal-
linity, properties such as surface wetting, the capacity of large
adsorption, and recyclability (Zhu et al. 2018).
So far, diverse kind of nanomaterials of magnetic charac-
teristics has been fabricated, for example, mono-component
materials (alloys, metals oxides, metallic nanomaterials, etc.),
multicomponent materials (functionalization of nanoparticles
is done with any functional group or entity), and
heterostructures (shell core, nanostructures, CNTs with mag-
netic nanoparticles, core-shell, core, shell-core nanostruc-
tures). Furthermore, hybrid structures maintain the key com-
ponent functionality and also contain synergic characteristics
(thermal, improved catalytic, magnetic, optical characteristics)
developing from functionalization (Kudr et al. 2017). In the
past few decades, more emphasis has been kept to develop
adsorbents based on nanoparticles of iron oxide through var-
ious synthesis methods to achieve desired properties and char-
acteristics. Such methods include microemulsion (Vidal-Vidal
et al. 2006), sol-gel process (Laurent et al. 2008), co-
precipitation of iron salts (Bee et al. 1995), organometallic
precursors compounds thermal decomposition (Hyeon et al.
2001), and hydrothermal gels.
The common magnetic nanocomposites are composed of
magnetic material of nanosized and host matrix material such
as gels, metals, silica, micelles, proteins, organic polymers,
carbon, liquids, ceramics, and liposomes (Zhu et al. 2013).
Thus, the resultant material possesses characteristic features
of both nanomaterial and incorporated matrices. The differ-
ence in crystalline structure and size of multiphase material is
due to nano-dimensions of the material. Furthermore, they
possess large magnetic moments, high magnetic anisotropy,
large saturation values, and high magnetic susceptibility
(Behrens and Appel 2016). Table 5 provides an overview of
nanocomposites’ utilization for oil-water separation at labora-
tory and industrial scale.
Advantages and mechanisms of carbon-based
magnetic nanocomposites
The emergence of a variety of magnetic nanocomposites in
recent times results from unique features such as novel mech-
anisms, eco-friendly, and innovative ways to extract oil from
wastewater. Innovative materials with super oleophilicity and
hydrophilicity are synthesized and combined with magnetic
nanocomposites to develop oil sorbents (Singh et al. 2020b).
The oleophilic nature of ferromagnetic particles, after mixing
in oil, produces magnetic oil, and the oil can be extracted from
nanocomposites with the help of an external magnet. Hence
magnetic nanocomposites possess the distant characteristics
attributed to ideal oil sorbents. The characteristics attributed
to magnetic nanocomposites are possessing better surface
Table 5 An overview of nanocomposites’ utilization for oil-water separation at laboratory and industrial scale.

Magnetic Fabrication method Size range Characteristics Equilibrium Absorption Oil removal Model Remarks Ref
nanomaterial time capacity application

NiFe2O4/sawdust and Hydrothermal method 32 nm Initially, oil absorption was 30 min 18.171 g/g Simple oil Blanchard kinetic Can be produced at Houshangi et al.
Environ Sci Pollut Res

CoFe2O4 magnetic fast due to empty actives equation large scale, (2020)
nanocomposites sites, as the sites filled up (second-order economical,
absorption process slows kinetic equation) highly selective
down hydrophilic,
inexpensive,
environment
friendly
MAC/Bi2O3 and Green 447.1 and Cost-effective, Short Separation Egyptian crude Quadratic polynomial The factors Abdel-Salam et al.
MAC/SiO2 microwave-assisted 445.1 nm, environment-friendly, operating rate of oil equation considered are (2020)
pyrolysis of sawdust 140.5 nm hydrophilic and time 99.4% at initial oil
and integration of advanced material, high 1 g/L concentration,
nanomaterials by sorption capacity, after even water salinity,
co-precipitation hydrophobic, high 5 cycles eater salinity,
method recovery efficiency, pH and amount
short operating time of nanomaterial,
high affinity to
oil
A sugar-based Through co-assembly of Nanocomposites eventually - Tenfold Crude oil - Ability to be Dong et al. (2020)
magnetic hybrid magnetic iron oxide break down into their their controlled
material nanoparticles constituents and elevate original remotely,
PEG-b-PGC[(EPC− the production and weight reused, resource
MPA)−co−(EPC− persistence of efficiency, lower
DOPA)]−b− micropollutants economic and
PGC(EC) energy costs
ZFHA (ZnFe2O4 Precipitation method Nanocomposite depicted 48 min 3500 mg/L Egyptian crude Thomas and Has the potential El-Maghrabi et al.
hydroxyapatite reusability for three oil Yoon-Nelson for production at (2019)
core-shell cycles, high magnetic model a large scale, the
nanocomposites) properties effect of
temperature, bed
height, and the
flow rate were
observed
Fe3O4/chitosan Co-precipitation method Adsorption process follows 75 min 157.739 Petroleum-based Pseudo-second-order Optimization was Singh et al. (2019)
superparamagnetic pseudo-second-order mg/g diesel kinetics, Langmuir carried out on
nanocomposite kinetics, Langmuir isotherm four factors,
(SPIONS) isotherm, showed namely stirring
monolayer speed, pH,
chemisorption process, adsorption time
nanocomposite and adsorbent
recyclability for five dose,
cycles eco-friendly
Hydrothermal 1.677,3.422nm Results were analyzed 50 min 1135mg/h Diesel, petrol, Langmuir isotherm The absorbent Sharma et al. (2019)
Polydimethylsilox- through and kerosene model, showed an
ane@zinc oxide, pseudo-first-order, pseudo-first-order-- adsorption
which states that kinetics
Table 5 (continued)

Magnetic Fabrication method Size range Characteristics Equilibrium Absorption Oil removal Model Remarks Ref
nanomaterial time capacity application

tetrapod@iron proportionality of capacity of 96%

oxide unoccupied sites with at 1135 mg/g.
adsorption rate,
superoleophobic, and
superhydrophobic
characteristics have
WCA of 157°. Showed
reusability for six cycles
Polycaprolactone Electrospinning method 10 nm 1 % by weight silica 18 min 28.4 g/g Light mineral oil - Can be used Barroso-Solares
(PCL) and Poly nanoparticles in 50/50 efficiently for et al. (2018)
(methyl PCL/PMMA fibers emulsions with
methacrylate) achieved best-optimized oil content
(PMMA) results, homogeneous between 10 and
nanocomposites and compact membranes 80 v%,
single-step
fabrication
method, a wide
range of
application
range
PVP-Fe - 20 to 30 nm Fe particles completely 10 min Thirty times Cooking oil - Oil recovery Zahari et al. (2018)
nanocomposites coated with PVP its capacity up to
volume 80%, ability to
be scaled up
Fe3O4 nanoparticles Co-precipitation 18 nm Highly dispersed, - Heavy crude oil The efficiency of Atta et al. (2015)
coated with rosin hydrophobic, covalent oil removal
amidoximes bonding of magnetite increased to
derivatives with amidoximes form a 80% of capped
core-shell nanostructure magnetite as
compared to
uncoated
magnetite with
only 45%
Magnetite Facile green method 9nm Spherical geometry, super 5 min 3.3 g/g Crude oil and - High efficiency of Atta et al. (2017)
nanoparticles oleophilic and seawater oil adsorption
capped with hydrophilic, cubic spinel (90%) even at
1-allyl-3-- magnetite Fe3O4 with a low magnetite
methylimidazolium small size distribution, content
porous, monodispersed,
extremely small size,
superparamagnetic, high
adsorption rate, high
reusability, highly
selective
Magnetic Fe2O3 Co-precipitation method 565 nm Nanoparticle surfaces have 1:10 ratio by Heavy crude oil - Up to 90% oil Abdullah et al.
stabilized and Wander Walls forces of weight removal (2018)
Environ Sci Pollut Res
Table 5 (continued)

Magnetic Fabrication method Size range Characteristics Equilibrium Absorption Oil removal Model Remarks Ref
nanomaterial time capacity application

capped with interactions, stable,

Environ Sci Pollut Res

Anthemis hydrophobic,
pseudocotula environment-friendly,
extracts high agglomeration,
improved dispersion,
efficient auto five cycle
SPION and In situ synthesis, facile 15 nm Multi-pollutant removal, 30 min 7.2 g/g Malachite green, Pseudo-second-order Can be applied Kumar et al. (2015)
β-cyclodextrin precipitation method crystalline structure, Seven times biphenol a kinetics with confidence
SPION/ β-CD efficient recycling, by weight belonging to in catalysis
photocatalytic-- crude oil, assignment
compatible particle lubricating oil
agglomeration,
eco-friendly
Superparamagnetic Addition in dropwise 10.8 nm Efficient wetting - 22.5 g of Crude oil and - Oil collection Abdullah et al.
iron oxide manner of SAS and characteristics, irregular crude oil water mixture facility of 90% (2016)
nanoparticles ammonium solution spherical shape, strong
coated with spontaneously to the magnetic properties,
sulfonated reaction mixture spinel crystal lattice
asphaltene containing Na2SO3 structure, nano-chain
and Fe.Cl3.H2O cluster
Magnetic NPs Co-precipitation 66 nm Surface interactions among 5 min Sample from - Oil absorption of Ko et al. (2017)
functionalized with surface-modified water and oil 99.9 %
amine magnetic nanoparticles from oil and
and oil drops gas production
(1) Magnetic (1) Acidified (1) 190.6 nm Uniform spherical 2 to30 min 2157g/kg Petroleum and (1) MNP has an oil removal capacity of Debs et al. (2019)
nanoparticles precipitation of Iron (2) 970 nm structures, 2841 g/kg motor oil 55% for 55 and
(MNP) (II) and Iron (III) salts superparamagnetic 89% for motor
(2) YB-MNP with addition in nature, the hydrophobic oil
dropwise manner of character (2) The oil removal
NH4OH solution efficiency of
(2) The above suspension YB-MNPs is
was heated with MNP 69.1%
and yeast biomass in
an 8:1 ratio
Fe3O4 coated with Solvothermal technique 250 nm Up to seven recycling 30 sec - Emulsified oil - Oil removal Lü et al. (2017)
chitosan cycles, Easy magnetic capacity of 90%
separation, good
demulsification property
Fe3O4 based carbon Thermal decomposition 36 nm Superoleophilic, efficient, - 3.8 times Lubrication oil - Stability for a long Zhu et al. (2010a)
core-shell eco-friendly, good their time in a
nanoparticles structural stability, weight corrosive
polysiloxane coated highly hydrophobic and environment
selective, reusable, high
adsorption, thermally
stable
Co-precipitation 62–90 nm - - Engine oil - Zhu et al. (2012)
Table 5 (continued)

Magnetic Fabrication method Size range Characteristics Equilibrium Absorption Oil removal Model Remarks Ref
nanomaterial time capacity application

Fe3O4 at sodium Superhydrophobic, fast and Has a broad

oleate efficient oil removal, application for
water-repelling wastewater
treatment
SPIONs-Collagen Collagen is derived from 10 nm The ability of magnetic - 2g/g Motor oil - Environmental Thanikaivelan et al.
nanocomposites leather and magnetic tracking, environment sustainability (2012)
nanoparticles by stability, high selectivity conversion of oil
molecular interactions for oils, inexpensive, adsorbed
stable, scalable nanocomposites
into
bi-functional
graphitic
nanocarbon
Fe3O4/PS The solvent, thermal 250 nm Superoleophilic, high - 2.492 times Vegetable oil, - Oil absorption Yu et al. (2015)
nanocomposites method, and ultrasonic efficiency, oil removal at its weight oil-water capacity of 92.5
dispersion large scale, mixtures, %
superhydrophobic, good diesel oil
dispersion, selective
renewable, reusable up
to 10 times
Co-Fe2O3 magnetic The solvent, thermal 5–10 nm Superparamagnetic - - Crude oil - Oil removal of Saber et al. (2015)
nanocomposite method under critical behavior, hydrophobic 97%
pressure, and character, adsorption,
temperature efficient, high specific
surface area, high
physical adsorption,
nature-friendly,
regeneration of
nanoparticles
SiO2-Fe3O4-MPS Co-precipitation and 75 nm Large surface area, - 4.84 g/g Kerosene, crude - An efficiency of Kamgar et al.
shell/core Sober method biocompatibility, high oil, and 100% for crude (2018)
nanocomposites efficiency, non-volatile, gasoline oil
highly hydrophobic,
high saturation
magnetization, increased
stability, non-toxic,
superparamagnetic
Magnetic polyaniline Emulsion polymerization 17–55 nm Oil removal is spontaneous - 60.3 g/g Diesel oil Pseudo-second-order Oil absorption Abdelwahab and
nanocomposite and chemical and endothermic, and kinetic model efficiency of Abd El-Ghaffar
oxidation the oil removal process 96% (2016)
followed the
pseudo-second-order
model, reusable up to ten
cycles, tunable
conductivity
32 nm 5 min 3.24 mg/mg Lubricating oil - Yaacob et al. (2018)
Environ Sci Pollut Res
Table 5 (continued)

Magnetic Fabrication method Size range Characteristics Equilibrium Absorption Oil removal Model Remarks Ref
nanomaterial time capacity application

Magnetic-material Co-precipitation of Fe2+ Reusable, MNPs embedded High selectivity for

Environ Sci Pollut Res

sporopollenin and Fe3+ salts with sporopollenin, oil, effective in

ammonium solution superparamagnetic, oil pH 7 solution
addition in a dropwise adsorbent, can be
manner regenerated, large
surface area,
environment friendly,
recyclability for 5 cycles
Fe2O3 nanoparticles CNTs coated with iron 24 nm Fast de-oiling, the 20 min 7g/g Gasoline oil Freundlich isotherm, Removal efficiency Fard et al. (2016)
doped carbon oxide NPs, Wet enhanced adsorption pseudo-second-- of 100%
nanotubes impregnation capacity of oil, chemical order kinetic model
adsorbents inertness, high
hydrophobicity,
pseudo-second-order
Magnetic porous A hydrothermal method, 190 nm Stable dispersion, excellent - 8 to 25 of its Pump oil, - High separation Bu et al. (2017)
MWCNTs/graphe- PS microspheres, water robust mechanical weight heptane, efficiency can
ne beads capillary microfluidic properties, and hexane, colza be recycled
device resistance, abundant oil, silicone through a simple
porosity, long-term oil, toluene method of
recyclability, easy distillation and
operation, uniformity, combustion
abundant porosity
Fe2O3 and doped Wet impregnation 24 nm Crystalline structure, 20 min 7g/g Gasoline oil Freundlich isotherm, Maximum oil Fard et al. (2016)
carbon nanotubes technique thermally stable, large pseudo-second-- capacity
surface area order equation
Magnetic Simple chemical 8 nm Fast kinetics, efficient, 30 min 12.93 g/g for Motor oil and Pseudo-second-order Superior sorption Raj and Joy (2015)
nanocomposite methods porous, low cost, high premium premium equation capacity
coconut shell oil retention capacity, oil, 7.65 motor oil
activated carbon good adsorbing power, g/g for
and magnetite large surface area, easily used oil
available
Polystyrene beads of Mini emulsion 58–113 nm Magnetic nanoparticles - - The emulsion - An oil absorption Tempesti et al.
magnetic polymerization polystyrene beads consisting of capacity of (2014)
nanocomposites embedded diesel-water 76.3%
Maghemite, γ−ferric Disaggregation-colloidal 14 nm Low aggregation, tuned - It can absorb Castor oil - Higher degree of Gomes de Souza Jr
oxide- biopolymer sol preparation composition, easy 8 times its attraction et al. (2010)
material synthesis, spherical weight between
morphology of magnetic
nanoparticles, high composites and
superparamagnetic magnet
force, eco-friendly,
biodegradable
Epoxidized natural 30 m High absorption capacity, 7 g/g Gasoline oil - Stale immersion Venkatanarasimhan
rubber magnetite biodegradable even after days, and
nanocomposites magnetically, low cost, high stability for Raghavachari
petrol (2013)
Table 5 (continued)

Magnetic Fabrication method Size range Characteristics Equilibrium Absorption Oil removal Model Remarks Ref
nanomaterial time capacity application

high stability,
eco-friendly, reusable
Poly (vinyl Co-precipitation of iron 20–30 nm hydrophobic interactions 10 min - Peanut oil, - Oil removal Zahari et al. (2018)
pyrrolidinone) iron salts between hydrocarbon oil sesame oil, efficiency of
magnetic chains and PVP, high and palm olein 80%
nanocomposites surface area, uniform
spherical shape
Magnetic Fe3O4 Hydrothermal method 400–500 nm Floating characteristics due - Can three N100 lubricating - Can clean large Chen et al. (2013)
polymer to superoleophobicity times oil spill areas, high
nanocomposites and hydrophobicity, weight selectivity for
wrapped with PS thermally stable, no lubricating oil
agglomeration, excellent
recyclability, good
dispersion, eco-friendly
Magnetic sponges Polymerization induced Cross-linked networks, 9.9 g/g for Engine oil, crude - Sponges have good Wu et al. (2017)
phase separation high yields, pore crude to oil, and other recovery for oil
presence, the water 20.33 g/g organic
contact angle of 140°, for compounds
oleophilic, engine oil
hydrophobicity
SPIONs decorated Thermal chemical vapor 14.5 nm Reusability, magnetically - Minutes to Water diesel Langmuir model, Oil removal Wang et al. (2013)
multiwalled carbon deposition separated, Langmuir 1.5h emulsion pseudo-second-- efficiency of
nanotubes model is followed, order 80%
Magnetic microporous Chemical vapor - Large sorption capacity, - 49 g/g for Gasoline and - Absorption Gui et al. (2013)
carbon nanotubes deposition recyclability, rich iron gas; 56 diesel from capacity of 99%,
sponges encapsulation, oleophilic g/g for produced recyclability
and hydrophobic, highly diesel water more than 1000
selective, accessible times
collection, porous, stable
eco-friendly
Environ Sci Pollut Res
Environ Sci Pollut Res
properties, non-sinking property, large sorption capacity, low
surface energy, biodegradability, reusability, simple recovery,
and eco-friendly nature (Doshi et al. 2018). The salient fea-
tures that stand out are super oleophilicity and hydrophobicity,
which helps nanocomposites to attract oil and repel water.
Another feature, wettability is measured as an angle at the
liquid-solid interface, which ordinarily is known as the contact
angle (Manukyan and Schneider 2016). An angle greater than
90° is considered as high hydrophilicity of material. The hy-
drophobicity and oleophilicity of material could be achieved
by increasing the contact angle from 0 to 150°. Other valuable
characteristics of magnetic nanocomposite are recyclability
and reusability; with the application of an external magnet,
nanocomposite could be extracted, which in turn produces
an easily recoverable and cost-effective sorbent (Singh et al.
2020b).
Future perspective
Remarkable progress has been made in functional carbon-
based and polymer-based magnetic nanocomposite fabrica-
tion and applications. Following are the recommendations
for further developments and applications of functional
carbon-based and polymer-based magnetic nanocomposite
for spilled oil recovery:
& First and foremost, there is a need for a wide range of
experimentation to determine the true capability and char-
acteristics of nanocomposites so that they could be imple-
mented commercially with confidence.
& The manufacturing cost at the lab scale is high; however,
the mass synthesis may reduce the overall cost.
Furthermore, financial studies with cost analysis need to
be carried out at pilot scale and industrial scale.
& The regeneration of nanocomposites and enhancing their
features should be investigated in detailed rather than
studying few cycles at lab scale, as they could help in
further reducing cost with high reusability.
& Furthermore, oil adsorption should be included in studies
combined with oil biodegradation as a support mechanism
for the microorganisms to perform the degradation of oil
into constituent elements.
Conclusions
The present review compiles a brief history of oil spill inci-
dents, various conventional methods devised for oil removal,
and the application of magnetic nanocomposites for oil spill
removal. The history section highlights the oil spill incidents
and their catastrophic effect on aquatic life and the
environment in general. The second section highlights that
all the conventional techniques have limitations; most are ex-
pensive and cannot remove oil significantly, so there is im-
mense need for new efficient oil removal technologies. The
review on magnetic nanocomposite highlights significant fea-
tures and characteristics of nanocomposites synthesized for
the sole purpose of oil removal. Analysis of studies highlight
the higher adsorption capacity, reusability with easy regener-
ation, cost-effective and straightforward synthesis technique,
and fast oil recovery using magnetic nanocomposites. Hence,
they could be utilized commercially to remove oil spills from
water with further testing and analyses.
Acknowledgements The authors gratefully acknowledged Curtin
University for constantly providing research support through the Curtin
Malaysia Graduate School and Research and Development Office.
Availability of data and materials This section is not applicable
Author contribution Ahsan Mehmood, Fahad Saleem Ahmed Khan, and
Nabisab Mujawar Mubarak collected data and prepared the first draft.
Shaukat Ali Mazari, Abdul Sattar Jatoi, Mohammad Khalid, Yie Hua
Tan, Rama Rao Karri, Rashmi Walvekar, Ezzat Chan Abdullah, and
Sabzoi Nizamuddin check the first draft and improve the scientific dis-
cussion. All authors contributed to writing a review paper.
Declarations
Competing interests The authors declare no competing interests.
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