Current Applied Physics 19 (2019) 114–119

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Current Applied Physics

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

Facile synthesis of silver-decorated magnetic nanospheres used as effective T

and recyclable antibacterial agents
Weijun Fangb,1, Qiuxiang Zhengc,1, Ying Fangb, Huabin Huanga,∗
a
Department of Science and Technology for Inspection, Xiamen Huaxia University, Xiamen, 361024, Fujian, China
b
College of Basic Medicine, Anhui Medical University, Hefei, 230032, Anhui, China
c
Department of Oncology, Longyan First Hospital Affiliated to Fujian Medical University, Longyan, 364000, Fujian, China

ARTICLE INFO ABSTRACT

Keywords: The development of a highly effective and recyclable antibacterial agent is of great interest. In this work,
Silver magnetic Fe3O4/Ag antibacterial nanoagent was successfully fabricated through a facile surface functionaliza-
Fe3O4 tion approach. Utilizing the strong interaction between silver and the amino groups on the surface of Fe3O4
Magnetic nanospheres nanospheres, the nanosized silver particles were tightly bonded on the Fe3O4 nanospheres' surface, improving
Recyclable
silver nanoparticalsʼ antibacterial activity by preventing agglomeration of silver nanoparticles. Our antibacterial
Antibacterial activity
tests showed that the as-synthesized Fe3O4/Ag nanospheres presented high antibacterial performance against
Gram-negative and Gram-positive bacteria. Moreover, these antibacterial nanohybrids can be easily recycled
from water solution by applying an external magnetic field. Overall, taking into consideration the facile pre-
paration method, excellent antibacterial activity and high magnetic recycling property, the as-synthesized
Fe3O4/Ag nanospheres have great potential applications in medicine and water disinfection.

1. Introduction nanocomposites which exhibit outstanding catalytic performances and

Silver nanoparticles have important applications in various areas,
including material sciences, electronics and medicines, due to their
unique optical, electrical and antibacterial properties [1,2]. Currently,
their antibacterial effects are extensively investigated because of a rapid
emergence of antibiotic resistant bacteria [3–6]. Silver nanoparticles
exhibit strong cytotoxicity toward a broad spectrum of bacteria with
little effects on human cells and no drug tolerance during the treatment
[7,8]. Although various silver nanocomposites have been applied in the
antimicrobial field, it is still difficult to separate these nanosized silver
particles from water, which may result in serious secondary pollutions
[9].
To solve the problem, a kind of Fe3O4/Ag nanocomposites were
developed recently [10–23], which can be easily separated from water
by a magnet. However, many published methods for synthesis of the
Fe3O4/Ag nanocomposites are relatively complicated and time-con-
suming, and the inadequate combination of silver and Fe3O4 nano-
particles may lead to a decrease in the stability of the nanocomposites.
For instance, lots of innovative procedures have been developed to
fabricate Ag-deposited polymer/SiO2/TiO2-coated Fe3O4
antibacterial activities, but these approaches are complex and involve
multiple steps [24–36]. Therefore, development of a simple and effec-
tive method for synthesis of Fe3O4/Ag nanocomposites is of great in-
terest.
In this study, we present a facile procedure for fabricate a silver-
decorated magnetic (Fe3O4/Ag) nanospheres. The as-synthesized
Fe3O4/Ag nanocomposites were characterized by different techniques,
including transmission electron microscopy, scanning electron micro-
scopy, X-ray diffraction, superconducting quantum interference device
magnetometer and zeta potential meter. Their antibacterial activity
against Gram-negative Escherichia coli (E. coli BL21) and Gram-positive
Staphylococcus aureus (S. aureus) and magnetic recovery property were
also studied.
2. Experimental section
Materials: Ferric chloride (FeCl3·6H2O), silver nitrate (AgNO3), an-
hydrous sodium acetate (NaOAc), poly(vinylpyrrolidone) (PVP
MW = 30,000), formaldehyde (CH2O, 40%), ethylene glycol (EG) and
polyethylene glycol 600 (EG600) were obtained from Sinopharm

∗
Corresponding author.
E-mail address: hhb@hxxy.edu.cn (H. Huang).
URL: https://mail.hxxy.edu.cn/ (H. Huang).
1
These authors contributed equally.

https://doi.org/10.1016/j.cap.2018.11.008
Received 28 June 2018; Received in revised form 27 September 2018; Accepted 12 November 2018
Available online 20 November 2018
1567-1739/ © 2018 Korean Physical Society. Published by Elsevier B.V. All rights reserved.
W. Fang et al.
Scheme 1. Schematic synthetic process of Fe3O4/Ag nanospheres.
Chemical Reagent Co. Ltd. (Shanghai, China). 3-(2-aminoethylamino)
propyltrimethoxysilane (APTMS) was purchased from Alfa Aesar. Milli-
Q water (18.2 M Ω, filtered with filter pore size 0.22 μ M) was from
Millipore. The other reagents were analytical grade and were used as
received without any purification.
Synthesis of Fe3O4 nanospheres: The Fe3O4 nanospheres were pre-
pared by the solvothermal method [23]. Briefly, 1.08 g of FeCl3·6H2O,
1.312 g of NaOAc and 1.0 g of PVP were dissolved in 30 mL of EG,
followed by the addition of 30 mL of EG 600 under stirring. The mixed
solution was transferred in 100 mL Teflon-lined stainless-steel auto-
claves, heated from 30 °C to 180 °C for 2 h, and maintained at 180 °C for
12 h. The nanospheres were collected by magnetic separation, washed
by ethanol and water for several times, and then redispersed in water
(30 mL) for subsequent use.
Surface modification of Fe3O4 nanospheres using APTMS
(Fe3O4eNH2): 150 mg of Fe3O4 nanospheres were redispersed in
180 mL of ethanol/water mixture 5:1 (v/v). After ultrasonication for
10 min, 0.5 mL of 3-(2-aminoethylamino) propyltrimethoxysilane
(APTMS) was added. The mixture solution was stirred at 50 °C for 12 h.
The final Fe3O4eNH2 nanospheres were collected and washed with
ethanol and water.
Preparation of Fe3O4/Ag nanospheres: 30 mg of Fe3O4eNH2 nano-
spheres was mixed with 10 mg of AgNO3 in 60 mL of ultrapure water,
and ultrasonicated for 10 min. Then 2.0 mL of formaldehyde aqueous
solution was added. After 12 h stirring under dark conditions, the re-
sulting Fe3O4/Ag nanospheres were separated with a magnet, washed
with water, and redispersed in water for subsequent use.
Measurements of silver content in Fe3O4/Ag nanospheres by ICP-MS:
1.0 mg of Fe3O4/Ag nanospheres was dissolved in 1.0 mL aqua regia
solution. After digestion for 10 h, the digestion solution was diluted by
ultrapure water, and the concentration of silver in the solution was
tested by an inductively coupled plasma mass spectrometry (ICP-MS).
The ICP–MS used in this study was a Quadrupole Mass Spectrometer
(iCAP Q, Thermo Fisher Scientific). The instrument was fitted with a
concentric nebuliser and a peristaltic pump nebuliser. Operating con-
ditions were as follows: RF power (1100 W); injection rate (1.85 mL/
min); nebuliser pressure (33 psi); cooling gas flow (4.0 L/min). Before
measurement, a series of standards, ranging from 0 to 10 ppm (0, 1, 2.5,
5 and 10 ppm) was assayed to demonstrate linearity.
Antibacterial activity test in LB liquid medium: The antibacterial ac-
tivities of the Fe3O4/Ag nanospheres were tested against Gram-negative
Escherichia coli (E. coli BL21) and Gram-positive Bacillus subtilis (B.
subtilis). These Bacteria were cultured in the LB liquid medium at 37 °C
on a shaker bed at 200 rpm until the logarithmic phase (approximately
109 colony forming units per mL). Then 150 μL of 107 CFU/mL bacterial
suspension containing different concentrations of Fe3O4/Ag nano-
spheres was added in a 96-well microplate and incubated at 37 °C with
continuous agitation (200 rpm). At given time intervals, the bacterial
growth curve was determined by measuring OD at 600 nm.
Antibacterial activity test on agar plates: 100 μL solutions with dif-
ferent concentrations of Fe3O4/Ag nanospheres (0 mg/mL, 1.25 mg/
mL, 2.5 mg/mL and 5.0 mg/mL) was firstly plated on the surface of LB
agar plates and left to dry for 5 min at room temperature. Then, 100 μL
of LB liquid medium containing 103 CFU mL−1 of bacteria (Escherichia
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Current Applied Physics 19 (2019) 114–119
coli BL21) was added and imprinted onto the solidified agar plates and
incubated at 37 °C for 14 h.
Measurements of the antibacterial rate of recycled Fe3O4/Ag nano-
spheres: 2.0 mg of Fe3O4/Ag nanospheres was added to 2.0 mL
∼107 CFU/mL E. coli BL21 suspensions and incubated at 37 °C for 4 h.
The bacterial growth inhibition was determined by measuring OD at
600 nm. This was the original antibacterial rate of the nanospheres.
Then, the nanospheres were collected via magnetic force, washed with
sterile water and recycled. 2 mL of fresh bacterial cell suspension was
added to the tube to incubate with the recycled nanospheres for another
4 h. This step was to get the antibacterial rate of the recycled nano-
spheres for the first cycle. The antibacterial rate of the recycled Fe3O4/
Ag nanospheres from the second to the fourth cycle was obtained by
applying the same procedure.
Characterization: The morphologies of the as-synthesized products
were characterized by a scanning electron microscope (SEM, HITACHI
S-4800) and a transmission electron microscope (TEM, JEOL JEM-
2100) with an acceleration voltage of 200 kV. The compositions of the
products was investigated by powder X-ray diffraction (XRD) using a
PANalytical X'Pert diffractometer with Cu-Kα radiation. The bacterial
optical density (OD) was tested by the Microplate Reader (Tecan
Infinite M200) at 600 nm.
3. Results and discussion
The synthesis procedure for fabrication of Fe3O4/Ag nanospheres is
shown in Scheme 1. We firstly prepared high-dispersed magnetic Fe3O4
nanospheres via the modified method proposed by our group [37].
Then, we coated a thin layer of 3-(2-aminoethylamino) propyl-
trimethoxysilane (APTMS) on the surface of the magnetic Fe3O4 na-
nospheres (Fe3O4eNH2) to attract silver ions through coordination in-
teractions. The amino-functionalized Fe3O4 nanospheres were then
added to AgNO3 solution, followed by adding formaldehyde to yield
Fe3O4/Ag nanospheres.
Fig. 1 shows the SEM images and TEM images of Fe3O4 nanospheres
and Fe3O4/Ag nanospheres. The pure Fe3O4 nanospheres (Fig. 1A and
B) exhibit high dispersion and spherical shape, and the average dia-
meter of Fe3O4 nanospheres is about 350–500 nm. After decorated with
silver particles, lots of silver particles were observed on the surface of
Fe3O4 nanospheres from SEM image (Fig. 1C). From the high-magnifi-
cation TEM image (Fig. 1D), it also can be seen that the small silver
particles were well deposited on the Fe3O4 nanospheres surface with a
wide diameter distribution around 15–40 nm.
The crystal structures of the samples were further investigated by
XRD. As shown in Fig. 2, the diffraction peaks (marked with #) at 30.1°,
35.42°, 43.36°, 53.8°, 57.38°, and 62.82° can be ascribed to Fe3O4
(JCPDS NO.75–1609). After modification with amino groups and dec-
oration with silver particles, the emergence of diffraction peaks
(marked with *) at 38.12°, 44.36° and 64.52° are assigned to the (111),
(200) and (220) crystal planes of silver (JCPDS NO.04–0783). These
results confirmed that the silver-decorated Fe3O4 nanospheres (Fe3O4/
Ag) were successfully fabricated through our amino-functionalized
approach.
The pure Fe3O4 nanospheres without amino functionalization were
W. Fang et al.
Fig. 1. SEM (A,C) and TEM (B,D) images of Fe3O4 nanospheres (A and B) and Fe3O4/Ag nanospheres (C and D).
Fig. 2. XRD patterns of Fe3O4 nanospheres (bottom curve) and Fe3O4/Ag na-
nospheres (top curve).
also used to generate Fe3O4/Ag nanospheres for the control experiment.
After formaldehyde-reduction process, we found out that only a few
silver particles were bonded on the surface of Fe3O4 spheres (Fig. S2). It
means that the surface amino-functionalized process is an essential step
to fabricate Fe3O4/Ag nanospheres. This may be due to the coordina-
tion interactions between amino groups and silver ions [37–40], which
is helpful for the nucleation and growth of silver on the Fe3O4eNH2
nanospheres surface under the reduction with formaldehyde. To date,
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Current Applied Physics 19 (2019) 114–119
several groups have developed various methods to synthesize such
Fe3O4/Ag composites (Table 1) [11,14,24,25,41–52]. Generally, three-
step reactions are designed for preparation of the magnetic composites,
where Fe3O4 particles is synthesized first, then an intermediate layer for
the supporting of Ag particles is coated on the Fe3O4 particles, finally
Ag particles are grown on the surface of nanocomposites. Compared
with the above three-step procedures, our amino-functionalized ap-
proach is more convenient and simple.
To further examine the thermal stability of the Fe3O4/Ag nanos-
tructure, TG analysis was carried out. As shown by the TG analysis
performed under nitrogen flow (Fig. 3), the first weight loss of 7.3% at
the range of 40–430 °C corresponds to the removal of high boiling point
solvents and guest molecules. Then the second weight loss (5.4%) at the
range of 430 °C ∼ 800 °C is ascribed to the decomposition of the che-
mically bound aminosilanes on the Fe3O4 nanospheres surface. From
the SEM and TEM images (Fig. S3) of the nanocomposites by heating
stepwise from 30 to 500 °C under nitrogen flow, such Fe3O4/Ag na-
nostructures were mostly destroyed and a few large Ag particles were
observed on the surface of Fe3O4 nanospheres. These data demonstrated
that the Fe3O4/Ag nanostructures are not stable in the presence of high
temperature.
It is well known that the antibacterial ability and the reactive ac-
tivity of silver nanoparticles are mainly dependent on their size and
shape. Usually, smaller Ag particles exhibit higher bactericidal ability
than larger ones. However, the smaller particles are easier to aggregate,
leading to a decrease in the antibacterial activity. Therefore, it is vital to
fabricate a stable nanosystem in material science. In our Fe3O4/Ag
nanostructures, the nanosized silver particles, which are well-dispersed
on the surface of the Fe3O4 nanospheres, may exhibit high antibacterial
activity due to the stabilization by the amino groups grafted on the
Fe3O4 surface. To detect the antibacterial effect of the Fe3O4/Ag na-
nospheres, the growth curves of Escherichia coli BL21(E. coli BL21) and
W. Fang et al. Current Applied Physics 19 (2019) 114–119

Table 1
Different silver-based magnetic nanocomposites for antimicrobial applications.
Nanocomposites Preparation Method Antibacterial Property(AE/MIC/MBC/DIZ) Ref

Ag/Fe3O4 One-step method: Core-shell Ag/Fe3O4 nanocomposites were prepared by co- precipitation route E.coli: 2.5 mM (silver concentration) [41]
followed by hydrothermal treatment in one-pot synthesis under various (Ag(NH3)2)+ ions DIZ = 4.2 mm
concentrations without adding any reducing agents. 10 mM (silver concentration) DIZ = 6.3 mm
25 mM (silver concentration) DIZ = 7.6 mm
Fe3O4@Ag Two-step method: Fe3O4@Ag nanoparticles were prepared by reducing silver nitrate on the E.coli: MIC ≥ 70 μg/mL [43]
surface of Fe3O4 nanoparticles using the water-in -oil microemulsion method S.epidermidis MIC ≥ 60 μg/mL
B.subtilis
MIC ≥ 70 μg/mL
Ag@Fe2O3-Glu Two-step method: In the first step, the yolk–shell Ag@Fe2O3 nanoparticles were prepared by the E.coli O157:H7: MIC = 15.2 μg/mL [46]
Kirkendall effect. These Ag@Fe2O3 nanoparticles were then modified with glucose molecules. B. subtilis: MIC = 21.8 μg/mL
GO-Fe3O4eAg Two-step method: Fe3O4 NPs anchored GO (GO-IONP) was synthesized first. For the further E.coli.: MIC = 14.4 μg/mL [14]
growth of AgNPs, GO-IONP solution was mixed with silver nitrate dissolved in deionized (DI) S.aureus.: MIC = 14.4 μg/mL
water under stirring in oil bath. Sodium citrate was then added into the boiling aqueous solution
to produce AgNPs.
rGO–Fe3O4–Au–Ag–Au Three-step method: rGO-COOH was exfoliated in deionized water by sonication. Fe3+/Fe2+ E.coli. O157:H7: 100 μg/mL, AE = 40% [44]
solution was added in the above mixture. The adsorbed Fe3+/Fe2+ cations on the surface of the (without NIR irradiation)
GO-COOH material facilitated the in situ formation of tiny magnetic Fe3O4 nuclei nanoparticles. 50 μg/mL, AB = 100% （with NIR 10-min
Then, PEI was modified on the surface of rGOeCOOHeFe3O4. Finally, the positive irradiation）
rGOeCOOHeFe3O4 NPs mixed with PSS-coated Au–Ag–Au nanorods to produce
rGO–Fe3O4–Au–Ag–Au nanocomposites.
Ag@rGO-Fe3O4-PEI Three-step method: Fe3O4-NPs were firstly decorated onto GO in the presence of Fe3+/Fe2+ in E.coli. O157:H7: 0.067 μg/mL, AE = 45% [24]
an alkaline medium. The rGO-Fe3O4 composite was then modified by PEI to provide a positive (without NIR irradiation)
charge and facilitate the capture of negatively charged bacteria. Ag-NPs were finally grown in situ 0.067 μg/mL, AE = 100%(with 15-min NIR
on the rGO-Fe3O4-PEI composite with AA as a reducing agent. irradiation)
Fe3O4@ECS/PAA-Ag Three-step method: Fe3O4 NPs were prepared through a chemical coprecipitation method. Next, E.coli.: 10 mg/mL, AE = 99.3% (30 min) [25]
immobilization of CS coating onto Fe3O4 NPs was achieved with the aid of polymerization of S.aureus.: 10 mg/mL, AE = 98.9% (30 min)
acrylic acid. Finally, the Ag NPs were deposited onto the magnetic nanoparticles by in situ
reduction of [Ag(NH3)2]+ with poly(vinyl pyrrolidone) as reductant and stabilizer in the presence
of ECS/PAA polymer coating as template.
Fe3O4@SiO2eAg Three-step method: Fe3O4 nanoparticles were synthesized by using a solvothermal method, and E. coli.: MBC = 10 mg/mL [11]
then, a thin layer of SiO2 shell was coated on the surface of Fe3O4 nanoparticles to produce
Fe3O4@SiO2. Then, Ag(NH3)2+ was well-dispersed on the surface of the Fe3O4@SiO2 magnetic
composite, which was then reduced by the Ag mirror reaction.
Fe3O4@Ag@ TiO2 Three-step method: Bimetallic Fe@Ag nanoparticles with a raspberry structure were firstly E.coli: 1.43 mg/mL, AE = 99.3% [45]
prepared from chemical reduction of ferrous sulfate in water with presence of sodium borohydride
as a reducing agent, followed then by redox transmetalation with addition of silver nitrate
solution at room temperature. Finally, the Fe@Ag particles were grafted with reagent-grade 2-
mercaptoethanol molecules on the surface for preparing the Fe3O4@Ag@TiO2 nanocomposites.

AE = Antibacterial Efficiency, MIC = Minimum Inhibitory Concentration, MBC = Minimum Bactericidal Concentration, DIZ = Diameter of Inhibition Zone.

Staphylococcus aureus (S. aureus) in LB liquid medium were studied. As

Fig. 3. TG curve of Fe3O4/Ag nanospheres.
shown in Fig. 4 (4A and 4B), the Fe3O4/Ag nanospheres (Ag content,
6.5% by weight, ICP-MS testing) showed an antibacterial effect toward
both bacteria in a concentration-dependent manner. The growth of
bacteria can be completely suppressed within 24 h, when the con-
centration of the Fe3O4/Ag nanospheres reached 0.8 mg/mL (Ag con-
tent is 52 μg/mL, Table S1) for E. coli BL21, and 1.0 mg/mL (Ag content
is 65 μg/mL, Table S1) for S. aureus. Fig. 4C and F shows the number of
E. coli BL21 colonies grown on LB agar plates with different con-
centrations of the Fe3O4/Ag nanospheres after 14 h cultivation at 37 °C.
It could be clearly observed that the number of bacterial colonies de-
creased with the increase of Fe3O4/Ag nanospheres dosage. By in-
creasing the concentration of the Fe3O4/Ag nanospheres to 5.0 mg/mL,
the proliferation of E. coli was completely inhibited.
Finally, the magnetic property of the Fe3O4/Ag nanospheres was
tested by superconducting quantum interference device (SQUID). The
magnetic hysteresis loop (Fig. 5) indicated that the as-prepared nano-
composites are superparamagnetic with a saturation magnetism of 61
emu/g. The high saturation magnetism maintained in the Fe3O4/Ag
nanospheres makes them very promising for magnetic separation and
recycling applications.

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W. Fang et al. Current Applied Physics 19 (2019) 114–119

Fig. 4. Growth curves of E. coli BL21

(A) and S. aureus (B) in LB liquid
medium at different concentrations of
Fe3O4/Ag nanospheres; Photographs of
E. coli BL21 colonies grew on LB agar
plates after incubation with different
concentrations of Fe3O4/Ag nano-
spheres for 14 h: (C) 0.0 mg/mL, (D)
1.25 mg/mL, (E) 2.5 mg/mL and (F)
5.0 mg/mL, respectively.

Fig. 5. Magnetic hysteresis loop of Fe3O4/Ag nanospheres. Fig. 6. Antibacterial activity of Fe3O4/Ag nanospheres against E. coli BL21 with
four antibacterial recycles.

Therefore, we further studied the recycling property of the Fe3O4/

Ag nanospheres, as illustrated in Fig. 6. The as-prepared nanocompo- Acknowledgements
sites can be successfully recycled and reused for four times with 52%
inhibition rate, indicating that the Fe3O4/Ag nanospheres possessed a We thank the Fund of State key laboratory of loess and quaternary
good recycling performance. geology (SKLLQG1607), China, the China Postdoctoral Science
Foundation (2016M590559), China, the Key projects of Anhui province
university outstanding youth talent support program
4. Conclusions (gxyqZD2018021), China and the National Training Programs of
Innovation and Entrepreneurship for Undergraduates (201610366034),
In summary, Fe3O4/Ag nanospheres were successfully synthesized China for the financial support.
through a sample surface amino-functionalized approach. Due to the
present nanosized silver particles with high dispersity and stability, the
Fe3O4/Ag nanospheres showed excellent antibacterial effects toward Appendix A. Supplementary data
Gram-positive Escherichia coli BL21 and Gram-negative Staphylococcus
aureus. Moreover, the as-synthesized Fe3O4/Ag nanospheres possessed Supplementary data to this article can be found online at https://
high saturation magnetization, and they were magnetically recyclable. doi.org/10.1016/j.cap.2018.11.008.

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References [24] W. Ning, H. Bo, C.M. Li, W.J. Hua, Nanotechnology 26 (2015) 195703.
[25] C. Yong, X. Chen, Q. Xiang, Q. Li, X. Xing, Bioact. Mater. 3 (2018) 80.
[26] A. Maleki, H. Movahed, P. Ravaghi, Carbohydr. Polym. 156 (2017) 259.
[1] S. Eckhardt, P.S. Brunetto, J. Gagnon, M. Priebe, B. Giese, K.M. Fromm, Chem. Rev. [27] A. Maleki, T. Kari, M. Aghaei, J. Porous Mater. 24 (2017) 1481.
113 (2013) 4708. [28] A. Maleki, Helv. Chim. Acta 97 (2014) 587.
[2] M. Rycenga, C.M. Cobley, J. Zeng, W. Li, C.H. Moran, Q. Zhang, D. Qin, Y. Xia, [29] A. Maleki, S. Azadegan, Inorg. Nano-Metal Chem. 47 (2017) 917.
Chem. Rev. 111 (2011) 3669. [30] A. Maleki, M. Ghassemi, R. Firouzi-Haji, Pure Appl. Chem. (2018) 387.
[3] S. Chernousova, M. Epple, Angew. Chem. Int. Ed. 52 (2013) 1636. [31] A. Maleki, R. Firouzi-Haji, Z. Hajizadeh, Int. J. Biol. Macromol. 116 (2018) 320.
[4] B. Le Ouay, F. Stellacci, Nano Today 10 (2015) 339. [32] A. Maleki, M. Aghaei, N. Ghamari, Appl. Organomet. Chem. 30 (2016) 939.
[5] J.C. Jin, X.J. Wu, J. Xu, B.B. Wang, F.L. Jiang, Y. Liu, Biomater. Sci. 5 (2017) 247. [33] A. Maleki, E. Akhlaghi, R. Paydar, Appl. Organomet. Chem. 30 (2016) 382.
[6] W.J. Fang, C.F. Xu, J. Zheng, G.J. Chen, K. Jiang, RSC Adv. 5 (2015) 39612. [34] A. Maleki, Ultrason. Sonochem. 40 (2018) 460.
[7] R.Y. Pelgrift, A.J. Friedman, Adv. Drug Deliv. Rev. 65 (2013) 1803. [35] A. Maleki, P. Ravaghi, H. Movahed, Micro & Nano Lett. 5 (2018) 591.
[8] N.F. Adegboyega, V.K. Sharma, K.M. Siskova, R. Vecerova, M. Kolar, R. Zbořil, J.L., [36] A. Maleki, H. Movahed, P. Ravaghi, T. Kari, RSC Adv. 6 (2016) 98777.
Environ. Sci. Technol. 48 (2014) 3228. [37] W.J. Fang, C. Han, H.B. Zhang, W.M. Wei, R. Liu, Y.X. Shen, RSC Adv. 6 (2016)
[9] C. Marambio-Jones, E.M.V. Hoek, J. Nanoparticle Res. 12 (2010) 1531. 67875.
[10] M. Mahmoudi, V. Serpooshan, ACS Nano 6 (2012) 2656. [38] Y. Tian, J. Qi, W. Zhang, Q. Cai, X. Jiang, Facile, ACS Appl. Mater. Interfaces 6
[11] X. Wang, Y. Dai, J.L. Zou, L.Y. Meng, S. Ishikawa, S. Li, M. Abuobeidah, H.G. Fu, (2014) 12038.
RSC Adv. 3 (2013) 11751. [39] W. Wei, A. Li, S. Pi, Q. Wang, L. Zhou, J. Yang, F. Ma, B.J. Ni, ACS Sustain. Chem.
[12] D.C. Riccardo, P. Domenico, M. Roberto, S. Marco, C.R. Susana, R.G. Pilar, P.W.J., Eng. 6 (2018) 749.
P. Teresa, Small 8 (2012) 2731. [40] B. Ramalingam, M.M.R. Khan, B. Mondal, A.B. Mandal, S.K. Das, ACS Sustain.
[13] S. Singh, D. Bahadur, Colloids Surfaces B Biointerfaces 133 (2015) 58. Chem. Eng. 3 (2015) 2291.
[14] T. Tian, X. Shi, L. Cheng, Y. Luo, Z. Dong, H. Gong, L. Xu, Z. Zhong, R. Peng, Z. Liu, [41] A. Amarjargal, L.D. Tijing, I.T. Im, C.S. Kim, Chem. Eng. J. 226 (2013) 243.
ACS Appl. Mater. Interfaces 6 (2014) 8542. [42] W.J. Fang, J. Zheng, C. Chen, H. Zhang, Y. Lu, L. Ma, G. Chen, J. Magn. Magn.
[15] P.Y. Furlan, A.J. Fisher, M.E. Melcer, A.Y. Furlan, J.B. Warren, J. Chem. Educ. 94 Mater. 357 (2014) 1.
(2017) 488. [43] G. Ping, L. Huimin, H. Xiaoxiao, W. Kemin, H. Jianbing, T. Weihong, Z. Shouchun,
[16] W.J. Fang, H.Y. Zhang, X. Wang, W.M. Wei, Y.J. Shen, J.S. Yu, J.X. Liang, J. Zheng, Y. Xiaohai, Nanotechnology 18 (2007) 285604.
Y.X. Shen, New J. Chem. 41 (2017) 10155. [44] B. Hu, N. Wang, L. Han, M.L. Chen, J.H. Wang, Chem. A Eur J. 21 (2015) 6582.
[17] M. Maham, M. Nasrollahzadeh, S.M. Sajadi, M. Nekoei, J. Colloid Interface Sci. 497 [45] W.J. Tseng, Y.C. Chuang, Y.A. Chen, Adv. Powder Technol. 29 (2018) 664.
(2017) 33. [46] Z. Wei, Z. Zhou, M. Yang, C. Lin, Z. Zhao, D. Huang, Z. Chen, J. Gao, J. Mater.
[18] X.X. Zhou, Y.J. Li, J.F. Liu, ACS Sustain. Chem. Eng. 5 (2017) 5468. Chem. 21 (2011) 16344.
[19] L. Jing, Y. Xu, S. Huang, M. Xie, M. He, H. Xu, H. Li, Q. Zhang, Appl. Catal. B [47] A. Maleki, Z. Hajizadeh, R. Firouzi-Haji, Microporous Mesoporous Mater. 259
Environ. 199 (2016) 11. (2018) 46.
[20] W.J. Fang, J. Zheng, C. Chen, H.B. Zhang, Y.X. Lu, L. Ma, G. Chen, J. Magn. Magn. [48] A. Maleki, Tetrahedron 68 (2012) 7827.
Mater. 357 (2014) 1. [49] A. Maleki, RSC Adv. 4 (2014) 64169.
[21] A. Maleki, H. Movahed, R. Paydar, RSC Adv. 6 (2016) 13657. [50] A. Maleki, R. Paydar, RSC Adv. 5 (2015) 33177.
[22] V.K. Sharma, T.J. McDonald, H. Kim, V.K. Garg, Adv. Colloid Interface Sci. 225 [51] A. Maleki, P. Zand, Z. Mohseni, RSC Adv. 6 (2016) 110928.
(2015) 229. [52] A. Maleki, P. Ravaghi, M. Aghaei, H. Movahed, Res. Chem. Intermed. 43 (2017)
[23] T. Wang, B. Ma, A. Jin, X. Li, X. Zhang, W. Wang, Y. Cai, J. Hazard. Mater. 342 5485.
(2018) 392.

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