Materials Science and Engineering B 272 (2021) 115325

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Materials Science & Engineering B

journal homepage: www.elsevier.com/locate/mseb

Review

Magnetic graphene, synthesis, and applications: A review

Mohammad Jafar Molaei
Faculty of Chemical and Materials Engineering, Shahrood University of Technology, Shahrood 3619995161, Iran

A R T I C L E I N F O A B S T R A C T

Keywords: After the discovery and recent developments of graphene and graphene oxide (GO), magnetic graphene has
Magnetic graphene received research interest during the past years. The exceptional properties of magnetic graphene materials such
Graphene oxide as electron mobility, high surface area, high saturation magnetization, biocompatibility, easy functionalization,
Drug delivery
and water solubility make them potential candidates in different biomedical and environmental applications.
Hyperthermia
Absorption
Magnetic graphene materials can be synthesized through different methods including simple mixing of gra­
Ions removal phene/GO and magnetic nanoparticles, in-situ synthesis of magnetic materials on graphene materials, and co­
valent functionalization. Magnetic graphene foam and magnetic graphene quantum dots are also other advanced
magnetic materials. The magnetic materials have found application in different biomedical areas such as drug
delivery systems, hyperthermia, and combined therapy. The environmental applications of magnetic graphene
materials include the removal of heavy metal ions, removal of radioactive metal ions, removal of pesticides, and
removal of herbicides. Different functionalization and surface modifications have been applied to the graphene
materials to improve their properties such as absorption, biocompatibility, water solubility, etc. In this review,
the properties of the magnetic graphene materials are introduced. Different synthesis and functionalization
methods of magnetic graphene materials that have been used by researchers during recent years are studied.
Recent biomedical and environmental applications of magnetic graphene materials have been addressed.

1. Introduction increases the type of the surface interactions. Reduced GO (rGO) is the
result of the reduction process of the GO. The GO can be synthesized
Graphene has been one of the first discovered and synthesized two- through two steps of oxidant intercalation oxidation and sheet peeling
dimensional (2D) materials with only one atomic layer thick. In the [14]. The Hummers’ method for the synthesis of the GO has been used
last 50 years, severe efforts have been devoted to synthesizing single extensively [15–19]. Marcano et al. have also synthesized GO with the
layers of graphite to achieve the properties of a one atomic layer sp2 aid of less corrosive phosphoric acid, compared to the Hummers’
carbon atoms structure [1]. However, In 2004, Geim and co-workers method [20]. Reduction of GO can also be performed mainly by the aid
first could isolate a single atomic layer from graphite which led to of sodium borohydride as the reducing agent [21,22], alcohol as the
extensive studies on graphene, since it was thought that 2D crystals are reducing agent [23], phenolic reduction method [24], and thermal
thermodynamically unstable at finite temperatures [2]. Graphene can be exfoliation reduction [25].
characterized as a semi-metal or a semiconductor with zero bandgap. Graphene foam is also a 3D network of graphene that which has
Graphene has high opacity and a small absorption ratio of 2.3% of white attracted a lot of interest during recent years. Graphene foam is a porous
light [3]. Graphene possess high electron mobility (250,000 cm2V-1s− 1) structure of graphene that possesses a high surface area. Graphene foam
[4], a resistivity lower than silver (10-6 O-cm) [5], large surface area can be synthesized by the chemical vapor deposition (CVD) method. The
(2630 m2g− 1) [6], high modulus of elasticity (around 1 TPa) [7], high metal-foam-directed CVD is capable of producing graphene foams with
mechanical strength, and environmental stability [8]. high crystalline quality with adjustable pore sizes in the range of 100 nm
There have been numerous researches on the synthesis of graphene to 2 µm [26–31].
and graphene oxide (GO) [9–13]. The main difference between gra­ An array of single-domain magnetic nanoparticles could show
phene and GO is the oxygen functional groups on the GO. The functional magnetic hysteresis. When a magnetic field is applied on a ferromagnet,
groups make GO hydrophilic while graphene is hydrophobic. The GO the magnetization increases by increasing the applied field which is
includes both aliphatic (sp3) domains and aromatic (sp2) which accompanied by the domain walls movements and growth of the

E-mail address: [email protected].

https://doi.org/10.1016/j.mseb.2021.115325
Received 5 March 2021; Accepted 17 June 2021
Available online 28 June 2021
0921-5107/© 2021 Elsevier B.V. All rights reserved.
M.J. Molaei Materials Science & Engineering B 272 (2021) 115325

domains. However, in an array of single-domain nanoparticles, the by the weak interactions between graphene/GO and magnetic materials.
particles’ moments have interactions with other adjacent nanoparticles However, if a strong binding is formed between graphene/GO and the
and the field to align in the direction of the field [32]. The magnetic magnetic nanoparticles, the resulted nanocomposite is more stable and
nanoparticles can be synthesized from hard [33–39] to soft magnetic graphene/GO sheets cannot easily detach from the conjugated magnetic
materials [40–42]. nanoparticles [52]. The magnetic nanoparticles-decorated graphene/
Iron oxide nanoparticles are a family of magnetic materials that have GO has two drawbacks: (1) the attachment of the magnetic nano­
been used for several magnetic applications. The iron oxide nano­ particles is by the aid of electrostatic interactions or simply physical
particles can become superparamagnetic if their sizes are smaller than a absorption that may result in leaching out of the magnetic nanoparticles
single magnetic domain. Superparamagnetic iron oxide nanoparticles from the graphene/GO sheets during the application is a liquid medium,
(SPIONs) have attractive properties such as superparamagnetism, high and (2) it is challenging to exactly determine the amount of magnetic
magnetic saturation, and high field irreversibility. When the external materials which are loaded on the graphene/GO sheets to obtain specific
field is removed, the SPIONs no longer show magnetic interactions. The properties [56]. Different strategies have been applied to bond Fe3O4
SPIONs consist of magnetite (Fe3O4) and maghemite (γ-Fe2O3). The covalently to GO sheets. In one of the strategies, Fe3O4 nanoparticles
SPIONs can have a coating that acts as a shield for the nanoparticles in were modified with (3-aminopropyl) triethoxysilane (APTES) and tet­
the environments and can be functionalized with different surface raethyl orthosilicate (TEOS) to introduce amino groups on the surface of
groups [43]. The graphene and its derivatives can find magnetic prop­ the nanoparticles. Then the amino groups of the surface-modified Fe3O4
erties with the aid of SPIONs. During recent years, magnetic graphene nanoparticles by the aid of N-hydroxysuccinnimide (NHS) and 1-ethyl-3-
with SPIONs has been widely used in different applications [44–51]. (3-dimethyaminopropyl)carbodiimide (EDC) were reacted with the
carboxylic groups of GO to form GO-Fe3O4 hybrid (Fig. 1a) [56]. In
2. Synthesis methods another report, n-Propyltrimethoxysilane (NPTS) has been used as a
cross-coupling agent of GO and Fe3O4/SiO2 core/shell nanoparticles
Magnetic graphene composites can be synthesized through the (Fig. 1b) [57].
following strategies. In another strategy, graphene sheets were modified by 4-aminophe­
noxyphthalonitrile and SOCl2 to introduce nitrile groups on the surface
2.1. Simple mixing with magnetic particles of the sheets. Subsequently, the nitrile groups on the sheets with the help
of ethylene glycol solvent were reacted with ferric ions on the surface of
In this approach, graphene materials and magnetic particles are Fe3O4 to a graphene-Fe3O4 hybrid (Fig. 1c and d) [58].
synthesized individually. Then, mixing the obtained graphene materials
and magnetic particles will result in a magnetic graphene composite. 3. Applications
The magnetic particles will be physically adsorbed on the graphene
sheets. However, this kind of magnetic composites cannot withstand Magnetic graphene/GO has found several biomedical and environ­
harsh conditions since are not stable enough [52]. For example, Luo mental applications. The magnetic properties of the magnetic graphene/
et al. synthesized Fe3O4@SiO2 microspheres and graphene oxide (GO) GO are advantageous for using these structures in drug delivery systems,
by solvothermal reduction, and Hummers and Offeman methods, hyperthermia, and environmental applications in removing hazardous
respectively. After washing the synthesized GO and microspheres, water species from the water. In the following sections, different applications
and N, N-dimethylformamide (DMF) were added to Fe3O4@SiO2/GO of magnetic graphene/GO are introduced.
dispersive solution and stirred vigorously [53].
3.1. Drug delivery systems
2.2. In-situ synthesize of magnetic materials on graphene materials
GO has found several biomedical applications including utilization in
Magnetic particles can be synthesized on graphene/GO sheets in- drug delivery systems [59–64]. Due to the large surface area, solubility
situ. Co-precipitation of Fe2+/Fe3+ ions with a reducing agent in the in physiological environments, lack of obvious toxicity, oxygen-
presence of graphene materials sheets can result in the formation of containing functional groups, easy functionalization, and good
magnetic particles on the sheets. This in-situ method results in better biocompatibility GO has been used extensively in drug delivery systems
dispersion of the magnetic particles on graphene sheets. Fe3O4/GO [54,65]. Magnetic GO has the advantage of combined therapy and
nanocomposite was synthesized by adding FeCl3⋅6H2O and FeCl2⋅4H2O diagnosis in the human body [65–69]. Magnetic GO has been used for
to the well-dispersed GO suspension. Then by dropwise adding NH4OH drug delivery [70,71], magnetic resonance imaging (MRI) [72,73],
to the solution under inert atmosphere and precipitation of Fe3O4, the fluorescence imaging [74], photothermal therapy [75–77], and photo­
magnetic nanocomposite has been formed [54]. dynamic therapy [78].
In another approach in the in-situ synthesis of magnetic graphene, A recent strategy for the targeting of the GO by an external stimulus
magnetic particles are synthesized in situ by the hydrothermal method is making a nano-hybrid of GO and magnetic particles that could be used
on the graphene sheets. This approach can also result in an excellent for drug delivery nano-vehicle acting by an external magnetic field. One
dispersion of the magnetic particles on the graphene sheets. For the of the most used magnetic materials in the synthesis of magnetic GO for
synthesis of magnetic GO with the aid of CoFe2O4 particles, Fe the drug delivery system is Fe3O4 superparamagnetic nanoparticles. The
(NO3)3⋅9H2O and Co(NO3)2⋅6H2O were added to a GO suspension fol­ Fe3O4 nanoparticles have the advantages of low toxicity, good
lowed by dropwise addition of NaOH for adjusting pH. Then the sus­ biocompatibility, strong superparamagnetism, near-infrared (NIR)
pension was transferred to an autoclave to be treated hydrothermally at absorbance, an easy preparation process. Therefore, Fe3O4 nanoparticles
180 ◦ C for 12 h. The precipitates then were washed and dried to obtain have been widely used in magnetic GO drug delivery systems [79].
magnetic CoFe2O4/graphene nanocomposite [55]. Doxorubicin (DOX) is one of the chemotherapeutic agents in cancer
therapy with an effective cell-killing ability. However, the toxic effects
2.3. Covalent functionalization of this drug make its use limited. Therefore, direct delivery of this drug
to the targeted point in the body is essential to reduce its toxicity in the
The magnetic graphene/GO which is synthesized by simple mixing of human body and increase drug efficacy. Nanosystems with controlled-
graphene/GO and magnetic materials and the magnetic graphene/GO release for drug delivery could have switchable gates that can be
which is synthesized by in-situ formation of magnetic structures on the closed and opened by stimuli. The stimuli that can be applied in drug
graphene/GO sheets are not completely stable. The un-stability is caused delivery systems include pH, temperature, or light [67]. For example,

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M.J. Molaei Materials Science & Engineering B 272 (2021) 115325

Fig. 1. Schematic showing the synthesis of GO-Fe3O4 hybrid by modification of the Fe3O4 with TEOS and APTES. Reprinted with permission from ref. [56] Copyright
2010 Elsevier Ltd. (b) Schematic of the synthesis steps of Fe3O4/SiO2-GO hybrid. Reprinted with permission from ref. [57] Copyright 2019 Elsevier B.V. (c) Chemical
modification of the GO sheets with SOCl2. (d) The schematic that shows the synthesis steps of phthalocyanine covalently bonded graphene-Fe3O4 hybrid. Reprinted
with permission from ref. [58] Copyright 2011 Elsevier Inc.

multi-stimuli-responsive magnetic GO that was functionalized with folic values are due to the increased surface area by conjugation with PEC and
acid (FA) was used as a drug delivery system. The synthesized drug hydrogen bonding interactions between the drug and functional groups
delivery system showed photothermal properties from GO. FA func­ on the PEC [82].
tionalized thiolated chitosan (FA-CS-SH) and thiolated GO (TGO) were
used in a sonochemical method to synthesize the nanosystem. FA-CS-SH
and hydrosulfuryl groups (-SH) of TGO could cross-link under the son­ 3.2. Combined therapy
ication. The disulfide bonds that form by the sonication could be broken
under a reductive trigger. Furthermore, the Fe3O4 nanoparticles that Combination therapy can improve anticancer activity. Treatment of
were modified with oleic acid were encapsulated into the synthesized cancer by chemotherapy includes using cytotoxic anti-neoplastic drugs.
nanosystem to give magnetic targeting ability to the nanosystem. However, the treatment may fail due to the resistance against the drug.
Moreover, the FA gives FA-receptor-mediated targeting ability to the The tumor cells start to reduce the accumulation of the anticancer drug
synthesized drug delivery system [80]. at its intracellular site of action. Therefore, combined therapy of
Graphene has hydrophobic characteristics due to the lack of oxygen- chemotherapy with other therapy methods can overcome the drug
containing hydrophilic groups. GO with oxygen-containing hydrophilic resistance and improve the treatment efficiency [83].
groups and also the existence of the defects is hydrophilic but tends to Functionalized GO has been used for simultaneous combined therapy
aggregate in the presence of salts due to the charge screening effect. and diagnosis. PEG-functionalized superparamagnetic GO-iron oxide
Surface modification can improve the dispersity of graphene and GO in hybrid nanocomposite was loaded with doxorubicin (DOX) which makes
physiological media [81]. Different functionalizations have been a magnetically targeted drug delivery system. The synthesized drug
employed to improve the drug loading and release characteristics, delivery system has a strong optical absorbance in the range of visible to
biocompatibility, water solubility, and stability of the magnetic GO in NIR region which is beneficial for photothermal therapy guided by the
physiological solutions. For example, pectin (PEC)-conjugated magnetic magnetic field. Furthermore, functionalized magnetic GO can be used as
GO (PEC-GO-Fe3O4) has been used for the paclitaxel drug delivery sys­ the T2 contrast agent. The functionalized magnetic GO can reach a drug
tem. The paclitaxel loading on the GO-Fe3O4 and PEC-GO-Fe3O4 occurs loading efficiency of 220%. The drug release in 360 min was 20% and
by the aid of hydrophobic interactions and π–π stackings between aro­ 50% in the pH of 7.4 and 5.0, respectively [73]. In another example of
matic and hydrophobic groups of the paclitaxel and synthesized drug the application of magnetic GO for combined therapy, magnetic GO was
delivery systems. The drug entrapment efficiency percents were 78.28 synthesized by depositing nanoparticles of Fe3O4 on GO sheets through
± 5.25 and 84.83 ± 5.33 for the drug delivery systems of GO-Fe3O4 and the co-precipitation method and was used for combined chemotherapy
PEC-GO-Fe3O4, respectively. The loading capacity percents were 33.35 and photothermal therapy. Cetuximab (CET, an epidermal growth factor
± 3.10 and 36 ± 3.21 for the synthesized drug delivery systems of and receptor (EGFR) monoclonal antibody) and PEG were used to modify the
PEC-GO-Fe3O4, respectively. The high drug entrapment and loading surface of the magnetic GO-Fe3O4 hybrid (MGO-PEG-CET). The EGFR is
expressed on the tumor cell surface which makes the functionalized GO-

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M.J. Molaei Materials Science & Engineering B 272 (2021) 115325

Fe3O4 hybrid efficient for the targeted drug delivery system (Fig. 2a). nanocomposite is due to the partial protonation of the amine and hy­
DOX drug loading capacity of 6.35 mg/mg was achieved for the func­ droxyl groups of DOX that results in higher drug solubility and weak­
tionalized GO-Fe3O4 hybrid. The MGO-PEG-CET was used for combined ening of hydrogen bonds between graphene and DOX. Incubation of
photothermal therapy upon exposure to near-infrared (NIR) light and Hela cells with rGO@Fe3O4/DOX for 4 h and confocal laser scanning
magnetically targeted killing of CT-26. The relative tumor volumes for microscopy studies showed that intracellular fluorescence of DOX was
the tumor-bearing BALB/C mice were 12.1 at day 14 of the control seen for the rGO@Fe3O4 with a magnetic field treatment. However,
(normal saline), 10.1 for the mice treated with DOX, 9.5 for them which weaker fluorescence can be observed for the rGO@Fe3O4 without a
were treated with magnetic GO-PEG-CET/DOX, 5.8 for the group that magnetic field loading. In other words, the internalization of the
received magnetic GO-PEG-CET/DOX + magnet, and 0.42 for the mice rGO@Fe3O4 is promoted by a magnet which shows the magnetic tar­
that had received the treatment with magnetic GO-PEG-CET/DOX + geting ability of the synthesized nanocomposites (Fig. 3([85]. Targeting
magnet + laser (Fig. 2b-d). Therefore, the combined chemotherapy and peptide-modified magnetic graphene-based mesoporous silica has also
photothermal therapy compared to the control group showed a 29-fold been used for combined therapy. The synthesized multifunctional drug
increase in therapeutic efficacy [84]. delivery system shows high DOX loading capacity, NIR photothermal
The Fe3O4-decorated hollow graphene microspheres (rGO@Fe3O4) heating characteristics as well as large T2 relaxation rates (r2), and
were used for combined chemo-photothermal therapy and magnetic facile magnetic separation. The synthesized multifunctional drug de­
targeting. The rGO@Fe3O4 was synthesized by spray drying and livery system has dual-targeting recognition (receptor-mediated active
coprecipitation method. The NIR-triggered photothermal effect of the targeting and magnetic targeting) and can be used for chemo-
synthesized nanocomposite showed a high photothermal conversion photothermal therapy and magnetic resonance imaging. The drug
efficiency. The rGO@Fe3O4 microspheres have a high drug loading ca­ release in the multifunctional drug delivery system is also pH-responsive
pacity of 18.43% with the potential of pH-responsive drug release and heat-stimulated. DOX can be loaded by the π-π stacking interaction
behavior. The pH-sensitive drug release behavior of the synthesized with graphene and by the adsorption of mesoporous silica. The loading

Fig. 2. (a) The schematic showing the synthesis steps

of DOX-loaded MGO-PEG-CET. The Fe3O4 nano­
particles were deposited by the coprecipitation
method. Biotin-PEG N-hydroxysuccinimide (NHS) has
been conjugated to cetuximab (CET) or quantum dots
(QDs) and avidin is covalently bonded to the magnetic
GO. Mixing of biotin-PEG-QDs and biotin-PEG-CET
with avidin-modified magnetic GO will synthesize
magnetic GO-PEG-CET-QDs and MGO-PEG-CET for
simultaneous fluorescent tracking and DOX loading.
(b) Optical images of the tumor-bearing BALB/c mice
on day 0 and 14, the incised tumor and the H&E
staining of the incised tumor on day 14 (scale bar for
all images = 200 μm); (c) The relative tumor volume
and (d) body weight for the mice that have received
different treatments. * p < 0.05 compared with con­
trol, DOX, and MGO-PEG-CET/DOX, # p < 0.05 as
compared with MGO-PEG-CET/DOX + magnet.
Reprinted from ref. [84] Copyright 2018 by the au­
thors. Licensee MDPI, Basel, Switzerland.

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M.J. Molaei Materials Science & Engineering B 272 (2021) 115325

Fig. 3. (a) An schematic showing the synthesis

method of rGO@Fe3O4/DOX microspheres and their
application in chemotherapy and photothermal ther­
apy. (b) Hysteresis loops of the rGO@Fe3O4 compared
to the Fe3O4 (inset on the top is coercive field values
(Hc). The inset at the bottom is also an optical image
of their suspensions before and after exposure to an
external magnet. (c) Temperature changes of rGO@­
Fe3O4 solutions at different concentrations (0.0625,
0.125, 0.25, 0.5, and 1 mg mL− 1). The temperature
changes are recorded after heating with an 808 nm
irradiation at 2 W cm− 2 for 5 min. (d) Temperature
changes of rGO@ Fe3O4 solution with the concentra­
tion of 0.25 mg mL− 1 by exposing to an 808 nm NIR
laser at different powers (1 W cm− 2, 1.5 W cm− 2, 2 W
cm− 2) for 5 min. (e) Infrared thermal images of
rGO@Fe3O4 solution exposed to 808 nm (2 W cm− 2)
for different periods (0, 1, 2, 3, 4, and 5 min). (f)
Temperature changes in rGO@Fe3O4 solution due to
the 808 nm irradiation laser successive on/off cycles
at 2 W cm− 2. Reprinted from ref. [85] Copyright 2020
licensed under a Creative Commons Attribution 4.0
International License.

capacity can reach as high as 0.95 ± 0.08 µg/µg due to the large surface 3.3. Hyperthermia
area and pore volume [86].
While most of the magnetic GO nanocomposites that have been used Magnetic hyperthermia is a localized cancer therapy that can be
for combined therapy are based on Fe3O4 nanoparticles, other iron ox­ performed by magnetic nanoparticles. Considering that compared to
ides such as γ-Fe2O3 nanoparticles have also been used for synthesizing normal cells, cancer cells are more sensitive to heat, the magnetic
magnetic GO in biomedical applications. For example, γ-Fe2O3 nano­ nanoparticles can be introduced in the tumor site and by application of
particles were grown on the GO by laser irradiation of a Fe target in the an external magnetic field heat the cancer cells. The external magnetic
solution containing GO-PEG. Since toxic agents are not used during the field increases the temperature of the magnetic nanoparticles and sub­
synthesis process by laser irradiation in the liquid, the synthesized sequently, the produced heat is conducted to the cancer cell which leads
magnetic GO showed in vitro low cytotoxicity compared to the nano­ to their death [88]. The combination of hyperthermia and chemo­
particles that are synthesized chemically. The synthesized nano- therapy is one of the advanced therapeutic treatments for cancer. Hy­
theranostics were tail vein injected and the tumor could be mapped perthermia can also be applied as a drug delivery trigger signal [89].
with the aid of γ-Fe2O3 via T2-weighted magnetic resonance. Moreover, Different magnetic particles such as Fe3O4 [90], γ-Fe2O3 [91], CeFe2O4
the DOX self-fluorescence and photothermal imaging of graphene can [92], MnFe2O4 [93], ZnFe2O4 [94], NiFe2O4 [95], and etc. have been
also be used for bioimaging. In Fig. 4a stronger fluorescence in the tumor utilized for hyperthermia cancer therapy.
site compared to other organs is seen for the H22 tumor-bearing nude The magnetic graphene-based drug delivery systems are promising
mice that have been treated with GO-PEG-γ-Fe2O3-DOX nanocomposite. for exogenous (AC field)/ endogenous (pH) stimuli-responsive actuators
It can be seen in Fig. 4b-iii that at 2 h post-injection the MRI signal for the combined chemotherapy and hyperthermia in cancer treatment
reached the darkest in the tumor site and returned to initial contrast at [96]. Superparamagnetic iron oxide-reduced graphene oxide (Fe3O4-
24 h post-injection (Fig. 4b-vi). The TEM image in Fig. 4d shows that rGO) nanohybrid was used for simultaneous chemotherapy and hyper­
black dots of the synthesized magnetic GO can be observed in the thermia. The nanohybrid was synthesized by the co-precipitation
cytoplasmic that reveals even after 24 h post-injection still it can be method. The rGO nanosheets showed that they can minimize the
accumulated within the tumor. Fig. 4e shows the tumor site temperature agglomeration of the nanoparticles. DOX was loaded on the nanocarrier
elevation of H22 tumor-bearing nude mice that have been treated with to be examined on the HeLa cells. The drug-loaded magnetic rGO with a
PBS, GO-PEG-γ-Fe2O3, and GO-PEG-γ-Fe2O3-DOX nanocomposite at 24 h concentration of 2 mg mL− 1 for one million cells could show cancer cell
post-injection. The temperature elevation of the tumor site can proliferation prevention up to 90% upon exposure for 35 min to an
reach>50 ◦ C by the NIR laser irradiation (5 min, 808, 2 W/cm− 2) while external AC magnetic field of 335 Oe at a frequency of 265 kHz. The
the temperature elevation for the PBS sample was only about 5 ◦ C [87]. temperature is increased to 43 ◦ C under the magnetic field after 30 min

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M.J. Molaei Materials Science & Engineering B 272 (2021) 115325

Fig. 4. Multimodal imaging of H22 tumor-bearing nude mice that have been treated with GO-PEG-γ-Fe2O3-DOX nanocomposite at different post-injection times (a)
fluorescence and (b) MRI imaging; (c) Temporal T2 signal from region-of-interest (ROI) analysis of tumor site. (d) TEM images of tumor cells from mice treated with
GO-PEG-γ-Fe2O3-DOX nanocomposite (24 h post-injection). aggregated nanoparticles are shown by arrows. (e) Photothermal images of tumor-bearing mice that have
been treated with PBS, GO-PEG-γ-Fe2O3, and GO-PEG-γ-Fe2O3-DOX nanocomposite after NIR laser irradiation (5 min, 808, 2 W/cm− 2) at 24 h post-injection.
Reprinted from ref. [87] Copyright 2018 Elsevier B.V.

[97]. functionalized magnetic graphene with a high loading capacity of 91%

The water solubility and biocompatibility of the graphene materials (w/w, representing 910 μg mg− 1) of DOX has a high heating efficiency
in the body environment are the key factors in designing the drug de­ upon exposure to the alternating (AC) magnetic field. The drug delivery
livery systems for the simultaneous hyperthermia effect. Furthermore, it system under an AC magnetic field in 30 min can release 46% of the
is important to functionalize the drug delivery systems to prevent the loaded drug at acidic tumor pH while the drug is released only 7% at
agglomeration of the nanocarriers in the body. For example, the water- physiological pH [96].
soluble and biocompatible copolymer pluronic F-127 has been used for The heating of the nanosystems can occur by simultaneous magnetic
the functionalization of hydrophilic magnetic graphene. The heating using an external alternating magnetic field and also the heating

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M.J. Molaei Materials Science & Engineering B 272 (2021) 115325

generated by the NIR absorption. Magnetic graphene using cobalt as the environment and makes the resulted nanocomposite suitable for dye
magnetizing agent was functionalized with PEG to be used for anti­ removal applications. The graphene quantum dots have been integrated
bacterial activity and theranostics application. The synthesized mag­ with magnetic GO for dye removal. The as-synthesized filler has been
netic graphene was used for hyperthermia by the heat generated from incorporated within PEG-1500 induced macroporous polyvinyl alcohol/
the cobalt nanoparticles in an external field, as well as the heat gener­ carboxymethyl cellulose hydrogel beads. The resulted hydrogel has a
ated by NIR absorption by the reduced GO. The PEGylated rGO/Co swelling behavior sensitive to pH. This hydrogel has been used for the
nanocomposite can also exhibit antibacterial activity toward E. coli removal of cationic pollutants of MB/RhB [114].
bacteria of about 100% under AC magnetic field for 15 min [98]. Magnetic graphene foam has also been used for adsorption proper­
ties. 3D graphene foam/Fe3O4 nanocomposite has been used for
3.4. Removal of heavy metal ions adsorption of Cr(IV) from an aqueous solution. Graphene foam was
synthesized with the aid of nickel foam. Subsequently, the graphene
For the removal of heavy metals ion, some of the methods including foam was functionalized with Fe3O4 nanoparticles. The magnetic gra­
ion-exchange [99], reverse osmosis [100], electrochemical processes phene foam with a high saturation magnetization of 40.2 emu/g, a high
[101], coagulation [102], and chemical precipitation [103] have been surface area of 574.2 m2/g, and a maximum absorption capacity of
used. Most of the mentioned methods have limitations that hinder their 258.6 mg/g for Cr(IV) ions is promising for the absorption of heavy
development. For example, alkaline conditions are needed for chemical metal ions. The absorption process rapidly performs during the first 5
precipitation which is provided by the addition of lime. This, in turn, min and the process reaches equilibrium after 20 min. The fast ab­
produces sludge and leads to secondary pollution. Being susceptible to sorption of heavy metal ions has been attributed to the interconnected
sedimentation on the membrane by solids and organics is the drawback porous structure of the graphene foam with a large specific surface area
of the membrane method and being limited to low concentrations of the which is advantageous for the diffusion of metal ions to the adsorption
metal solution is the drawback of the Ion-exchange method. However, sites. The adsorption performance is better in lower pH values of 1–2 and
an alternative cost-effective method is absorption technology. Among decreases by increasing pH value [115].
the several absorbents that have been used for heavy metal ions Different functionalization and surface modifications have been
removal, graphene-based materials have shown to be promising absor­ applied to improve the absorption properties of the magnetic graphene
bents due to their exceptional mechanical and electrical properties materials including dithiocarbamate (DTC) [116,117], ethyl­
[104]. enediaminetetraacetic acid (EDTA) [118,119], polyethylenimine (PEI)
Graphene is hydrophobic which is not suitable for the removal of [120], polymaleicamide dendrimer [121], poly(acrylamide) [122], etc.
some substances such as dye pollutants in aqueous environments. GO For example, the functionalization of 3D graphene with chitosan leads to
with the carboxyl, carbonyl, epoxide, and hydroxyl groups on it can be an increment in the surface area due to the decrease in the restacking
easily dispersed in the aqueous solutions and form a stable suspension. effects of graphene sheets as spacers. Furthermore, the absorption ca­
Therefore, GO has the potential to be utilized in the removal of dyes and pacity of the heavy metals ions improves, and the functionalization re­
heavy metal ions. Since the separation of the carbonaceous adsorbents is sults in overcoming the chitosan limitations such as low thermal
not easy, magnetic nanoparticles have been used for absorbent mate­ stability, weak acid stability, and low mechanical strength [123]. Cyclic
rials. Magnetic GO as an excellent absorbent can also easily be separated oligosaccharide of b-Cyclodextrin (b-CD) with the hydrophilic exterior
from the solutions [105]. The high absorption capacity of the magnetic and hydrophobic lining of the central cavity has been used for the
GO has been attributed to the thin nanosheets, high dispersibility, and functionalization of the magnetic GO. The macrocyclic structure of the
O-containing functional groups on the surface of the sheets [106]. b-CD is advantageous since it can encapsulate hydrophobic molecules
Magnetic graphene/GO with high surface active sites, high specific and entrap them inside their cavities. Poly(b-cyclodextrin)-conjugated
surface area, tunable shape and size, high chemical stability, easy magnetic GO was successfully used for the removal of organic pollut­
functionalization, multi-functional properties, and magnetic separation ants and heavy metal ions. By the functionalized GO, the heavy metal
capability are adsorbents adsorbent for the removal of organic dyes, ion of Cd2+ is removed by the complexation and electrostatic in­
radionuclides, and heavy metal ions from wastewaters [107]. For teractions mechanism while the sulfamethazine (SMT) is removed by
example, magnetic GO was used for the adsorption of heavy metal ions host–guest supramolecular, hydrogen bonding, and π–π interactions
such as Pb+2, Cr+3, Cu+2, Zn+2 and Ni+2 in different pH, temperature, [124]. Table 1 compares different magnetic graphene/GO with versatile
adsorbent dose, and contact time. It was observed that the adsorption is functionalizations that have been used for the removal of heavy metal
endothermic and spontaneous. The maximum adsorption capacities at ions and other species.
pH 8 for Ni (II), pH 7 for Zn (II), pH 6 for Cu (II), pH 6 for Cr (III), and pH
5.0 for Pb (II) were 51.020, 63.694, 62.893, 24.330, and 200 mg/g, 3.5. Removal of pigments & dyes
respectively [108]. In another study, In another study,
polyvinylpyrrolidone-functionalized magnetic GO has been used for the There are several industries including paint, paper, plastics, textile,
removal of the Pb(II) ions from the water with an adsorption capacity of and leather that use dye compounds and upon the plant operation, toxic
793.65 mg/g. The functionalized nanocomposite has selective absorp­ colored effluents are released into the ground and/or surface water.
tion toward Pb(II). This nanocomposite can remove 99.74% of Pb(II) in a Dyes are chemical reagents that can cause cancer and are toxic to
solution that contains other ions such as Mg(II), Mn (II), Na(I), K(I), Cd aquatic organisms. Therefore, it is necessary to remove them from the
(II), Zn(II), Cr(III), and Cu(II). The Pb(II) adsorption mechanism is wastewater of such plants [136]. The complicated chemical structures of
chemical absorption between Pb(II) and the PVP group and electrostatic the dyes that are used in industries make them resistant to biodegra­
interaction between –COOH of Fe3O4/GO and Pb(II). The nano­ dation. The common dyes that are mostly used in the industries include
composite can decrease the Pb(II) content of the river water down to methylene orange [137], methylene blue [138], Congo red [139],
~0.4 ppb [109]. malachite green [140], acid orange 8 [141], Persian orange [142],
Graphene quantum dots and carbon quantum dots are quantum dots reactive orange 12 [143], Azo acid red 14 [144], acid yellow 99 [145],
mostly with fluorescence properties with a typical size of<10 nm. The BR-12 [146], amido black 10B [147], and a few more. There have been
graphene quantum dots are small fragments of the graphene sheet, while several physicochemical methods that are used for the removal of
carbon quantum dots are synthesized from different carbon-containing colored compounds from effluent wastewater including separation by
sources. The graphene quantum dots and carbon quantum dots have the membrane [148], photocatalytic degradation [149], electrolysis
large surface areas [110–113]. The large surface area of the graphene [150], adsorption [148], liquid–liquid extraction [151], and coagula­
quantum dots with layered graphene enhances their sensitivity to the tion process [107]. Some of the developed methods for the removal of

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Table 1
Magnetic graphene/GO with different functionalizations and corresponding studied ions/species removal.
Type of graphene derivative Conjugated Functionalization Saturation Ions/species removal Absorption capacity Refs.
magnetic magnetization (emu/ (mg g− 1)
material g)

GO Fe3O4 EDTA and Chitosan Magnetic GO = 44, Cationic dye, Rhodamine 1085.3 [125]
GO-EDTA = 20, GO- B (RhB)
Chitosan = 18
GO Fe3O4 Diethylenetriaminepentaacetic acid – tetracycline and Tetracycline ~ 250, [126]
ciprofloxacin Ciprofloxacin > 100
(600 min)
GO Fe3O4 SiO2/molecularly imprinted polymer Magnetic GO = 22, Bisphenol A (BPA),4-tert- BPA = 16.81, 4-tert- [127]
(MIP) magnetic GO@SiO2 octylphenol (4-tert-OP) OP = 35.97, and 4-
=4 and 4-nonylphenol (4- NP = 61.73
NP) in water
α-Fe2O3 impregnated rGO α-Fe2O3 – 4.4 Eriochrome Black T 210.53 [128]
GO Fe3O4 – 27.4 Cu2+/ Methylene blue Cu2+=18.1, [129]
(MB) Methylene blue =
23.2
Magnetic GO, magnetic Fe3O4 – Magnetic GO = 33.0, Phenanthrene Magnetic GO = 13.65, [130]
chemically-reduced MCRG = 53.9, MARG = 26.18
graphene(MCRG) and MARG = 70.7
magnetic annealing-
reduced graphene (MARG)
GO Fe3O4 Magnetic copper-based Fe3O4-GO = 51.32, Triazole pesticides >3μg/mg [131]
metal–organic framework M− MOF− 199 = (concentrations of
(M− MOF− 199) 11.16 5000 μg/L)
GO Fe3O4 and – 5.02 MB and p-tert- MB = 390.25, PTBP [132]
γ-Fe2O3 butylphenol (PTBP) = 59.18
Fe3O4@CuO/GO Fe3O4 CuO 30 As(III) and As(V) As(III) = 70.36, As(V) [133]
= 62.60
Fe3O4@GO Fe3O4 – 30.81 MB, rhodamine B (RhB), MB = 131.1, RhB = [134]
and Methyl orange (MO) 34.5, and MO = 39.95
GO MnFe2O4 Tetraethylenepentamine (TEPA) 44.39 Pb2+ 263.2 at pH of 5.5 [135]

dye and pigments are not suitable due to the high cost, energy-intensive, 3.6. Removal of radioactive metal ions
and production of a large amount of carcinogenic and toxic byproducts
[152]. Several adsorbents such as wheat shells [153], silica [154], The release of the radioactive waste of the mining and nuclear energy
zeolite [155], almond shells [156], orange peel [157], natural polymeric activities into the water sources has been one of the long-term threats to
materials, etc have been used in the adsorption method [152]. the environment. The leakage of radionuclides such as 235U, 137Cs, 129I,
In the last couple of years, different magnetic nanoparticles have and 90Sr, which are the products of fission, can cause entering them into
been used for the adsorption of metal ions and organic pollutants. GO the water sources and food chain. The mobile water with radioactive
has been used for the removal of dye and pigments due to its high contamination can be absorbed by plants by permeating into soils that
removal capacity which is a result of large surface area and surface finally can reach human beings and animals [107]. Magnetic GO
oxygenated functional groups [107]. Moreover, GO has chemical sta­ nanoribbons that are synthesized by a hydrothermal method were used
bility and can be functionalized for better adsorption of different dye for thorium adsorption. It was observed that the absorption of thorium
molecules. The GO can be converted to magnetic GO for easy collection by magnetic GO nanoribbons is endothermic, pH-dependent, and
in the adsorption process of the dyes from wastewaters. spontaneous. The removal of Th(IV) by magnetic GO nanoribbons is also
Surface modification of the magnetic GO can make it capable of the influenced by temperature, contact time, adsorbent dosage, and initial
removal of both cationic and anionic dyes. For example, Magnetic concentration [160].
nanoparticles were used to be integrated with GO for the removal of Uranium contamination in the wastewaters is a serious concern in
methyl violet and acid red 88 in different conditions. The GO was the process of uranium mining. Uranium as heavy metal has radiological
modified with metformin to introduce polyamine functionality. The and chemical toxicities. If the radioactive wastewater of the uranium
results showed that adsorption is performed according to the Langmuir mines is not effectively remediated, radioactive species may migrate in
isotherm with an adsorption capacity of 243 mg g− 1 and 303 mg g− 1 for the water and soil and finally reach the food chain. Therefore, it is
methyl violet and acid red 88, respectively. It was shown that modified necessary to remove radioactive species to keep the food chain safe.
magnetic GO is promising for application as an adsorbent for the Magnetic GO can properly remove radioactive species from the water
removal of both anionic and cationic dyes [158]. [161]. Magnetic GO supported on carboxymethyl cellulose synthesized
For enhancement of the adsorption capacities of the magnetic GO by a low-temperature plasma was used for removal of U(VI). The
different synthetic or natural polymers such as alginate, b-cyclodextrin, maximum capacity of the magnetic GO nanocomposite was 7.94 × 10-4
ethylenediaminetetraacetic acid, cellulose, chitosan, etc. have been mol/g at 301 K and pH 5.5. The U(VI) ions can interact with the syn­
utilized in conjugate with magnetic GO. For example, chitosan has been thesized magnetic GO nanocomposite in the entire range of pH values by
used with magnetic GO for the removal of blue 19 (RB19) and Ni(II) inner-sphere surface complexation [162]. The polyamidoxime/poly­
ions. The maximum adsorption capacities for the removal of blue 19 ethyleneimine magnetic GO has also been used for the removal of U(VI)
(RB19) and Ni(II) ions were 102.06 mg/g and 80.48 mg/g, respectively. from radioactive wastewater of the mine. The synthesized modified
The chitosan/magnetic GO nanocomposites were made as magnetic magnetic GO had a maximum adsorption capacity of 606.06 mg/g at pH
beads. The mechanical stability of the beads is enhanced by the 6.0 and 298 K toward U(VI). The removal occurs as monolayer chemi­
hydrogen bonds between oxygen-containing groups on the GO surface sorption by the synthesized functionalized magnetic GO which is
and amine groups on the chitosan (Fig. 5) [159]. endothermic and spontaneous. The residual U(VI) concentration in
wastewater after removal by the synthesized magnetic GO is 6.37 μg/L

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M.J. Molaei Materials Science & Engineering B 272 (2021) 115325

Fig. 5. Schematic showing the synthesis steps of the magnetic GO/chitosan nanocomposite, (b) The synthesized spherical beads, (c) The interaction of the chitosan
chains and magnetic GO nanosheets, (d) Mechanical stability of the beads, and (e) the magnetic properties of the beads which gives them the ability to be recovered
by using an external magnetic field. Reprinted from ref. [159] Copyright 2019 Taylor & Francis Group, LLC.

that is lower than the permissible concentration of 30 μg/L for drink functionalized calix[4]arene was used for the removal of pesticides of
water. Therefore, the synthesized functionalized magnetic GO is a chlorpyrifos and hexaconazole from the water with high adsorption
promising adsorbent for the removal of radioactive U(VI) from waste­ capacities of 93.46 mg g− 1 and 78.74 mg g− 1 for hexaconazole and
waters [163]. chlorpyrifos, respectively. The maximum adsorption capacity of the
synthesized magnetic GO is comparatively high as compared to acti­
3.7. Removal of pesticides vated carbon fiber, activated carbon, calixarene/magnetic sporopol­
lenin, nanomembranes, and bio-adsorbent (activated sludge). The high
A pesticide is a substance or mixture of substances that are produced absorption capacity for the synthesized magnetic GO has been attributed
synthetically or are derived naturally to be used for deteriorating the life to the establishment of proper interactive forces of π-π, H-bonding, and
cycle of the pest. Pesticides include fungicides, insecticides, herbicides, electrostatic bonding between selected pesticides and synthesized
and bactericides [164]. Plant cultivation, like vegetables, rice, maize, magnetic GO [165].
and fruits may pollute the environment by agricultural discharges due to The adsorptive removal efficiency of pesticides is influenced by the
the excessive usage of pesticides and/or insecticides. Accumulation of type of raw material, preparation method, and treatment conditions.
pesticides and/or insecticides over time can result in the contamination Most of the graphene family materials are stable in varying pH ranges.
of environmental waters, soil, vegetables, and crops [107]. A nano­ However, the maximum removal efficiency of graphene materials for
composite of GO, Fe3O4 nanoparticles, and N-methyl-D-glucamine different insecticides and pesticides is achieved in different pH ranges

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M.J. Molaei Materials Science & Engineering B 272 (2021) 115325

[164]. organic solvents and water [171]. The graphene is suitable for the ab­
GO has high electron mobility and can be effective in reducing the sorption of the organic compounds with the benzene ring due to its
recombination rate by acting as an electron sink in the photocatalysts delocalized π electron system. It is difficult to use graphene alone for
that are used for the removal of the Pesticides. For example, amine- removing the pollutants since removing the graphene in a suspended
functionalized Fe3O4 wrapped with GO was used for supporting MIL- form from the water is not easy and also the graphene sheets agglom­
101(Fe) (MIL refers to Material of Institute Lavoisier and Fe-based erate [168].
MILs are candidates in the field of photocatalysis). The obtained nano­ Magnetic graphene grafted with thermosensitive polymer and den­
composite was used for the degradation of atrazine and diazinon pesti­ drimer (methyl methacrylate and ethylenediamine) showed efficient
cides. The nanocomposite reached 81 ± 1% and 100 ± 1% degradation adsorption ability for the removal of butachlor [BUT] in 45 min, at a pH
efficiency for atrazine and diazinon by irradiation of visible light for value of 5, and 1 mg L–1 concentration of the pollutant with a dose of 3 g
105 min. It is suggested that there is a fast electron transfer through L–1 of the adsorbent. The adsorption process has a negative value of ΔG◦
interlayers of GO in the nanocomposite and also an enhanced conversion which indicates that the process is feasible and spontaneous [172]. In
between Fe2+/Fe3+ can be realized (Fig. 6) [166]. another study, magnetic TiO2-graphene was used for photocatalytic
removal of typical herbicide 2,4-dichlorophenoxyacetic acid (2,4-D)
3.8. Removal of herbicides from water with almost 100% efficiency. The Fe3O4-based magnetic
nanocomposite showed a saturation magnetization of 13 emu/g [170].
The herbicides (weed killers) in agriculture refer to the materials that
can leave the main crop undamaged while controlling the growth of a 3.9. Challenges and prospective
certain weed [107]. Magnetic graphene has found applications in the
nanocomposites that are used for removing herbicides [167–170]. The In this review, magnetic graphene materials were introduced.
magnetic nanoparticle adsorbents have the benefit of the synergistic Different synthesis methods and the applications of magnetic materials
effect of easy separation of the adsorbent with an external magnet, high in various areas including drug delivery systems, hyperthermia, com­
adsorption capacity, reduced consumption of solvents, reduced extrac­ bined therapy, removal of heavy metal ions, removal of radioactive
tion time, use of a small amount of adsorbent, and reusability of the metal ions, removal of pesticides, and removal of herbicides were dis­
adsorbent. However, agglomeration of the magnetic nanoparticles is a cussed. The magnetic graphene materials have novel characteristics
disadvantage which results in decreasing the total surface area of the such as high surface area, enhanced absorption properties, water solu­
nanoparticles. Therefore, surface modification agents are used to over­ bility, biocompatibility, electron transfer, and high saturation magne­
come this drawback. GO can also be used for the modification of the tization which make them superior candidates in biomedical and
magnetic nanoparticles for the removal of herbicides. The oxygen environmental applications. The magnetic graphene materials are easy
functional groups on the GO such as carbonyl, hydroxyl, and epoxy to be synthesized and functionalized to give them specific characteristics
groups alter the interaction between the GO layers. The oxygen func­ for each of the applications. Despite the outstanding researches on
tional groups on the GO surface also enhance the GO solubility in magnetic graphene materials, their applications in different

Fig. 6. (a) The synthesis method of the amine-functionalized Fe3O4 wrapped with GO as a supporter for MIL-101(Fe). The photocatalytic degradation efficiency of
(b) diazinon and (c) atrazine with various photocatalysts. Reprinted from ref. [166] Copyright 2020 Elsevier Ltd.

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