Hydrothermal method
Hydrothermal method
https://doi.org/10.1007/s13738-019-01809-w
ORIGINAL PAPER
Abstract
The degradation of ceftriaxone (CTX) by heterogeneous catalytic advanced oxidation processes has been explored using
γ-Fe2O3 NaY zeolites synthesized (γ-Fe2O3@NaY) in the laboratory through hydrothermal and chemical co-precipitation
methods. γ-Fe2O3@NaY zeolite was characterized by scanning electron microscopy, energy-dispersive X-ray spectroscopy
and X-ray diffractometer analyses. The effects of the initial concentration of CTX and catalyst, pH and hydrogen peroxide
(H2O2) dose with the presence UV light on the degradation efficiency of CTX have been studied by conducting experiments
in a batch reactor at room temperature. Experimental results reveal that CTX can be efficiently removed after 90 min at pH
4.0, CTX 20 mg/L, catalyst 1.17 g/L, H2O2 30 mM and presence of UV light. A kinetic and isotherm model was developed
for investigation of the adsorption mechanism, and results show that model and data are in good agreement. The reusability
of γ-Fe2O3@NaY was high as it degrades CTX in the presence of UV light and H2O2 even after five consecutive cycles. Also,
due to having magnetic properties, this composite is easily separated from the solution by magnetism. This work indicates
that bench synthesized γ-Fe2O3 NaY zeolite is a heterogeneous recoverable catalyst that can efficiently remove CTX from
wastewater.
Graphic abstract
Oxidative- Degradation
UVC
H2O2 0OH
e-
+
h
γ-Fe2O3@NaY
Keywords Advanced oxidation processes (AOPs) · Heterogeneous catalysis · γ-Fe2O3 NaY zeolite · Ceftriaxone removal
Introduction
* Maryam Hazrati Niari Wastewater contaminants arising from industrial and domes-
[email protected]; [email protected] tic activities cause environmental concerns when discharged
Extended author information available on the last page of the article to the environment. In past decades, wastewater treatment
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processes have been improved to remove contaminants range of organic pollutants. Hydroxyl radicals are formed
through primary and secondary wastewater treatment pro- by processes and agents such as Fenton reagent, UV irra-
cesses. However, trace contaminants (e.g., pesticides, petro- diation, oxidation with hydrogen peroxide and ozonation
leum constituents, endocrine disruptors, antibiotics and [15, 16]. Klavarioti et al. [17] reviewed the degradation of
pharmaceutical products) present in wastewater effluent have pharmaceuticals from water and wastewater using AOPs,
adverse health effects on human and aquatic lives. Phar- and they found that 32% of AOPs tested for pharmaceutical
maceuticals are widely used to promote improved human compounds was focused on the application of heterogene-
health and to prevent diseases, in addition to also find uses ous catalysis. The advantages of heterogeneous catalysis are
for agricultural purposes and animal care. Antibiotics are a non-toxicity, high stability and a high potential for decom-
wide class of drugs that have applications to prevent bacte- posing organic pollutants [18, 19].
rial infection in humans, animals and plants [1, 2]. About Magnetic nanoparticles (MNPs) such as hematite
30–90% of the antibiotics do not decompose in the human (α-Fe2O3), maghemite (γ-Fe2O3) and magnetite (Fe3O4)
or animal body and ultimately enter the environment through are widely used for magnetization of particles [20]. MNPs
feces and urine as active compounds [3]. Therefore, the main increase the adsorption capacity, stability and reusability of
source of environmental antibiotics is the effluent of munici- composites. Also, the magnetic composite is easily sepa-
pal wastewater treatment plants, as well as effluent of phar- rated from aquatic environments by a magnet. MNPs need a
maceutical manufacturing plants [4]. suitable supporter of high-performance capability [21–23].
Pharmaceuticals are classified as bio-accumulative com- Zeolites can behave as an appropriate porous supporter.
pounds; therefore, they are known as hazardous chemicals They are comprised of porous aluminosilicate material with
[5, 6]. Ceftriaxone (CTX) is a powerful antibiotic that is a three-dimensional open structure that consists of SiO4 and
used to treat infections caused by gram-positive and gram- AlO4 tetrahedrons. Desirable adsorption ability, excellent
negative bacteria, including bone and joint infections, pneu- ion exchange, high surface area and regular mesoporous
monia, skin infections and urinary tract infections [7]. The (with a diameter of between 20 and 100 Å) are unique fea-
chemical formula of CTX is C18H18 N8O7S3 [8]. Its molecu- tures of zeolites [24–26]. Their efficiency depends on their
lar weight is 554.571 g/mol, and the chemical structure is structure, which can improve their absorption capacity. Zeo-
shown in Fig. 1. lite Y is crystalline and microporous, a pore diameter in its
Conventional treatment systems cannot eliminate drug typical framework being ~ 0.74 nm. The microporosity of
compounds. Nowadays, the focus has switched to develop this zeolite has a major role in its form selectivity. Zeolite
tertiary wastewater treatment technologies such as advanced Y is commercially available or can be synthesized [27–29].
oxidation processes (AOPs) and reverse osmosis (RO) that The objective of this study was to demonstrate a new
are more effective in removing wastewater contaminants and approach in CTX degradation using γ-Fe2O3@ NaY zeo-
environmentally benign. [9–13]. AOPs occur through the lite nanostructure as a recoverable magnetic composite in
reactions of contaminants with highly reactive radical spe- the presence of UV light and H2O2. For this reason, NaY
cies (i.e., hydroxyl radical, superoxide and singlet oxygen) nanozeolite was synthesized by a hydrothermal method.
and have been widely used for destruction of non-biodegrad- Subsequently, this nanozeolite was modified with γ-Fe2O3.
able and biodegradable compounds. The NaY nanozeolite and γ-Fe2O3@NaY were characterized
The most essential advantages of AOPs can be high effi- using SEM–EDX and XRD. The effect of basic parameters
ciency in biodegradation, an enhancement in the potential was investigated, including the pH of the solution, compos-
for the destruction of persistent organics and high minerali- ite dose, CTX initial concentration, H 2O2 dose and reaction
zation capability [14]. Due to the production of hydroxyl time. Furthermore, a possible mechanism for the degrada-
radicals (·OH), AOPs are capable of oxidizing a broad tion of CTX γ-Fe2O3@NaY/UV/H2O2 system is proposed.
HN-N N
N
The chemical reagents used contained water glass (28.0 wt%
S H
O S SiO2, Lanzhou Petro Chemical Co., Petro China Company
N S Ltd.), NaAlO2 (95 wt%, Beijing GuoHua Chemical Material
O NH2
Co.), NaOH (96 wt%, Merck, Darmstadt, Germany), HCl
(37 wt%, Merck company), FeCl3.6H2O (Merck company,
Fig. 1 Chemical structure of ceftriaxone Germany), FeCl2.4H2O (Merck company, Germany), H2O2
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(30%, Chengdu, China), Ethanol (96% wt%, Sigma-Aldrich), solution, 1 g of CTX powder was dissolved in 1000 mL of
NH3 (32 wt%, Merck company), acetonitrile (99% wt%, deionized water.
Sigma-Aldrich) and ceftriaxone (Jalinous pharmaceutical The batch experiments were conducted at different exper-
company. Iran) and was used without additional purification. imental parameters such as pH of the solution, reaction time,
During the experiments, deionized water was used. CTX initial concentration (20–60 mg/L), H2O2 concentra-
tion (5–50 mM) and composite dose (0.34–1.17 g/L). The
Synthesis of NaY nanozeolite solution pH was adjusted to 2.0–10.0 using 1.0 Mol/L HCl
or NaOH solution. The mixture of CTX and composite
NaY nanozeolite was synthesized using the hydrothermal was continuously stirred for 120 min, and adsorption was
method. The aluminosilicate gel was prepared in the molar performed with time intervals 10, 30, 60, 90 and 120 min.
ratio of 1 0Na2O:1.0Al2O3:15SiO2:300H2O. The precursor During experiments, the composite was separated from the
was made by combining aluminum isopropoxide, sodium solution using the magnet and filtered by a 0.45-μm mem-
hydroxide, silicate solutions and deionized water. The beaker brane filter. The residual concentration of CTX in the aliquot
containing the gel was continuously stirred at room tem- was detected using high-performance liquid chromatogra-
perature for 24 h, and a completely uniform solution was phy (HPLC). During all experiments, the temperature was
obtained. The heat was the driving force of the crystalliza- 25 ± 1 °C. The experiments were conducted in triplicate.
tion process; thus, to have hydrothermal crystallization, the
homogeneous gel was stirred with a rotation rate of 250 rpm
Analytical method and performance indices
at 60° C for 4 days. Then, the solid product was washed with
deionized water and dried at 90° C for 8 h [30].
The concentration of CTX was measured by an HPLC
instrument (Eclipse plus C18 column; 3.5 lm, 4.6 × 100 mm)
Synthesis and characterization of γ‑Fe2O3@NaY equipped with a UV detector at a wavelength of 190 nm.
A mixture of acetonitrile and phosphate buffer (pH = 4.8)
In this study, both γ-Fe2O3@NaY and MNPs were synthe-
was used as the mobile phase that was injected at 1 mL/min
sized using a chemical co-precipitation method. To syn-
[34]. The CTX removal efficiency was calculated according
thesize MNPs in an aqueous solution of 150 mL, 2.02 g
to Eq. [1]:
FeCl3·6H2O and 0.75 g F eCl2·4H2O were mixed and soni-
cated at 70° C for 20 min. This mixture was stirred at 80 °C CTX0 − CTXt
CTX removal efficiency (%) = × 100 (1)
for 1 h. Afterward, 15 mL of NH3 solution was slowly added CTX0
to the upper mixture and its color changed from brown to
black. The produced material was washed with deionized where CTX0 and CTXt represent CTX concentration before
water followed by ethanol and then was dried in an oven at and after the reaction, respectively.
100 °C for 3 h [31]. Also, the γ-Fe2O3@NaY composite was
prepared using the above method. Also, before adding NH3
solution, 3 g of NaY nanozeolite was added to a ferrous/ Results and discussion
ferric solution.
The morphology of the catalyst surface was detected by Characterization of catalysts
scanning electron microscopy (SEM, Mira 3, Czech Repub-
lic). The chemical elements of the catalyst were also deter- SEM images of γ-Fe2O3@NaY and the NaY nanozeolite
mined using energy-dispersive X-ray spectroscopy (EDX, are shown in Fig. 2 to reveal their surface morphology
Carl Zeiss, Germany) coupled with SEM. The crystalline characteristics. According to Fig. 2a, b, external surfaces
characteristics of composites were identified by X-ray dif- of the γ-Fe2O3@NaY composite are rougher than then NaY
fraction (XRD, Quantachrome, NOVA 2000) with Cu Kα nanozeolite, which can be due to the filling of composite
radiation (λ = 0.15406 nm) at 50 kV and 200 mA, and the 2θ pores with MNPs. Therefore, the non-uniform surfaces of
range was scanned between 4° and 80° [32, 33]. the synthesized composite can be attributed to the aggre-
gation of MNPs on NaY nanozeolite surfaces, indicating
Catalytic oxidation experiments methodology that composite synthesis has been successfully performed
and MNPs have been placed on the NaY nanozeolite sur-
In this study, catalytic oxidation experiments were carried faces. The analysis of γ-Fe2O3@NaY and NaY nanozeolite
out in a 250-mL glass reactor equipped with a mechanical elements was performed by the EDX technique (Fig. 3).
mixer (at an agitation speed of 200 rpm). To perform the According to Fig. 3a, the weight percent of the NaY nanoze-
oxidation reaction, a UV-C lamp (6 W PHILIPS) was placed olite elements was 55.39% oxygen, 27.72% silicon, 11.66%
along the reactor (a distance of 3 cm). To prepare the stoke aluminum and 5.23% sodium. Also, in the γ-Fe2O3@NaY
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Fig. 2 SEM images of γ-Fe2O3@NaY (a) and the NaY nanozeolite (b)
composite, the presence of both iron and oxygen elements removal efficiency was close at pH 2.0 and 4.0 (p value
indicates that they are the main elements of the magnetiza- 0.004), the pH value of 4.0 was chosen as the optimum pH.
tion process (Fig. 3b). As there was an absence of impurity Similar results have been reported in the literature that the
peaks in the EDX spectrum, the product was of high purity. efficiency of removing CTX and tetracycline (TC) increased
The XRD patterns of MNPs, the NaY nanozeolite and in more acidic conditions [2, 29]. It was well known that
γ-Fe2O3@NaY are presented in Fig. 4. In XRD patterns of the solubility of iron is high in low pH and ultimately CTX
the NaY nanozeolite, sharp diffraction peaks at 2θ values of decomposes by the action of the catalyst better [35–37].
33.07, 47.27 and 58.57 were observed, consistent with the
XRD pattern of the γ-Fe2O3@NaY composite. In XRD pat- The influence of γ‑Fe2O3@NaY dose
terns of MNPs, sharp peaks positioned at 2θ of 15.92, 20.62,
23.87, 27.28, 31.62 and 34.32 are obvious, aligning well The effect of different γ-Fe2O3@NaY doses (0.34–1.17 g/L)
with the pure maghemite according to the JCPDS (1-37- on the degradation of CTX was investigated in the presence
1309). The diffraction peaks of NaY nanozeolite and MNPs of UV light and H 2O2. As shown in Fig. 5b, the efficiency
in the XRD patterns of γ-Fe2O3@NaY composite indicate of CTX degradation increased as a function of catalyst dose
that synthesis has been successfully performed. from 0.34 to 1.17 g/L. Based on the results, the percentage
of CTX removal increased from 83 to 99% by increasing
Effect of experimental factors the adsorbent dose from 0.34 to 1.17 g/L, respectively. By
increasing the amount of catalyst, excess active sites become
Effect of solution pH available, which consequently increases the adsorption of
pollutants [38, 39]. Thus, the γ-Fe2O3@NaY surface area
One of the main parameters affecting the catalyst proper- is enhanced with higher catalyst doses, meaning that the
ties and the ionization degree of pollutants is the pH of the efficiency of CTX removal increases.
solution. To remove CTX, the influence of solution pH was
studied by the γ-Fe2O3@NaY/UV/H2O2 system at a cata- The influence of initial concentration
lyst dose of 0.5 g/L, CTX initial concentration of 20 mg/L,
H2O2 dose of 30 mM and pH range of 2.0–10.0 at differ- The influence of CTX initial concentration on the removal
ent contact times. According to Fig. 5a, the efficiency of efficiency by γ-Fe2O3@NaY/UV/H2O2 system was evalu-
CTX removal increased at highly acidic conditions with the ated in 20–60 mg/L range. According to Fig. 5c, by increas-
highest efficiency was achieved at pH = 2.0. Because CTX ing CTX initial concentration (from 20 to 60 mg/L), the
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Intensity (Counts)
Na 5.23 4.45
O Kα
6000
Al 11.66 8.46
5000
AlKα Si 27.72 19.32
4000
3000
2000
NaKα
1000
0 keV
0 5 10
Energy (KeV)
b 4000
SiKα
Elt W% A%
3500
O 39.77 59.29
3000
Na 2.26 2.35
2500 ClK α
O Kα Al 5.65 4.99
Intensity (Counts)
2000
Si 16.78 14.25
1500 AlKα
Cl 16.06 10.80
FeLα
1000
Fe 19.48 8.32 FeKα
500 NaK α
ClK β
FeKβ
keV
0
0 5 10
Energy (KeV)
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a
120
100 c
100
80
80
CTX Re (%)
CTX Re (%)
60
60
pH=2.0 20 mg/L
40 pH=4.0 30 mg/L
40
pH=6.0 40 mg/L
20
50 mg/L
pH=8.0 20
60 mg/L
pH=10.0
0 0
0 20 40 60 80 100 120 0 20 40 60 80 100 120
Reaction time (min) Reaction time (min)
d 100
b
100
80
80
50 mM
CTX Re (%)
60
CTX Re (%)
60 0.34 g/L 5 mM
0.5 g/L 40 10 Mm
40
0.84 g/L 15 mM
20 1.17 g/L 20
30 mM
0 0
0 20 40 60 80 100 120 0 20 40 60 80 100 120
Fig. 5 Characteristics of CTX removal using γ-Fe2O3@NaY/UV/ CTX initial concentration (pH 4.0, catalyst dose: 1.17 g/L), d H2O2
H2O2 system: a initial solution pH (catalyst dose: 0.5 g/L, initial con- dose (pH 4.0, C0: 20 mg/L, catalyst dose: 1.17 g/L)
centration (C0): 20 mg/L), b adsorbent dose (pH 4.0, C0: 20 mg/L), c
60
to 50 mM). This can be described that excess H 2O2 amount 41
act as a scavenger of hydroxyl radicals to produce per 40
H2 O2 +⋅ OH → H2 O + HO2⋅ (2)
HO2⋅ +⋅ OH → H2 O + O2 (3)
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nanozeolite. Also, the efficiency of CTX removal in iron- The results showed that the model of pseudo-second-order
rich systems was higher than the non-iron systems, because (R2 = 0.999) and isotherm of Langmuir (R2 = 0.987) had
MNPs increase the area of the composite surface [43, 44]. better correlation than pseudo-first-order (R2 = 0.947) and
The modeling and behavior of CTX adsorption on isotherm of Freundlich (R2 = 0.983). These results were
γ-Fe2O3@NaY were evaluated by isotherm and kinetic stud- matched with studies of Azari et al. [34, 45].
ies. The rate of adsorption of CTX on adsorbent was rapidly As shown in Fig. 6, the percentage of CTX removal in
performed during the first 90 min, but then no consider- the γ-Fe2O3@NaY/UV/H2O2 system was greater than the
able variation was seen after that time. Therefore, the time other systems in this study. According to Fig. 7, free radicals
of 90 min in this experiment is selected as the equilibrium of OH were produced by decomposing hydrogen peroxide
time. The correlation coefficient of kinetic models and equi- during the UV irradiation (Eq. 4) [46–48].
librium isotherms of CTX adsorption is shown in Table 1.
H2 O2 + hv → 2⋅ OH (4)
Table 1 Constants of studied Models Nonlinear equation Linear equation Parameters Value
kinetic and isotherm models
for CTX removal through Kinetics
adsorption on γ-Fe2O3@NaY
Pseudo-first-order dqt/dt = K1(qe − qt) ln(qe − qt) = lnqe − k1t qe, cal 2.656
k1 0.236
R2 0.947
Pseudo-second-order dqt/dt = k2(q2 − qt)2 t/qt = t/qe + 1/k2q2e qe,cal 19.120
K2 0.582
R2 0.999
qe, exp 19.076
Equilibrium Adsorbent dose (g/L)
Isotherms 1.17
Langmuir qe = (qmKLCe)/(1 + KLCe) Ce/qe = Ce/qm + 1/KLqm KL 0.58
qm 39.5
R2 0.987
Freundlich qe = KF(Ce)1/n lnqe = lnKF + n−1lnCe n 2.62
KF = qm/C1/n
0 qm 46.9
R2 0.983
H2O2 0OH e- H2 O2
H2O 0OH
e-
0OH
e- e-
CB
Ze/NaY
Fe2O3
Oxidative- Degradation
h+ h+
VB
UVC
+
e- h
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100 Conclusions
99
80 94 91 88
81 In this study, a γ-Fe 2O 3@NaY composite was synthe-
CTX Re (%)
H2 O2 + e− →⋅ OH + OH− (7) Acknowledgements This paper was financially supported by the Envi-
ronmental Technologies Research Center, Ahvaz Jundishapur Univer-
sity of Medical Sciences (Grant No. 98s48).
OH + CTX → Oxidative − Degradation (8)
⋅
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7. X. Guo, J. Wan, X. Yu, Y. Lin, Study on preparation of SnO2-TiO2/ wastewater by adsorption, Fenton, UV-Fenton and US-Fenton
nano-graphite composite anode and electro-catalytic degradation using magnetic nanoparticles-functionalized carbon (MNPs@
of ceftriaxone sodium. Chemosphere 164, 421–429 (2016) C). J. Ind. Eng. Chem. 56, 163–174 (2017)
8. C.-C. Zhang, T.-C. Weng, B.-A. Su, C.-C. Lai, Y.-C. Chuang, 24. C.F. Cogswell, T.P. Nigl, A. Stavola, A. Wolek, Y. Wang, J.
W.-C. Ko et al., Salvage therapy with intravenous fosfomycin plus Zummo et al., Generation and use of a pure titanium pillared
ceftriaxone for necrotizing fasciitis caused by penicillin-nonsus- MCM-36 structure as a high efficiency carbon dioxide cap-
ceptible Streptococcus pneumoniae. J. Microbiol Immunol. Infect. ture platform and amine loaded solid adsorbent. Microporous
51, 573 (2018) Mesoporous Mater. 280, 151–156 (2019)
9. M. Malakootian, M. Yaseri, M. Faraji, Removal of antibiotics 25. N. Suárez, J. Pérez-Pariente, F. Mondragón, A. Moreno, Gen-
from aqueous solutions by nanoparticles: a systematic review and eration of hierarchical porosity in beta zeolite by post-synthesis
meta-analysis. Environ. Sci. Pollut. Res. 26, 8444–8458 (2019) treatment with the cetyltrimethylammonium cationic surfactant
10. A. Takdastan, B. Kakavandi, M. Azizi, M. Golshan, Efficient acti- under alkaline conditions. Microporous Mesoporous Mater. 280,
vation of peroxymonosulfate by using ferroferric oxide supported 144–150 (2019)
on carbon/UV/US system: a new approach into catalytic degrada- 26. L.M. Henning, D.D. Cubas, M.G. Colmenares, J. Schmidt, M.F.
tion of bisphenol A. Chem. Eng. J. 331, 729–743 (2018) Bekheet, B.R. Pauw et al., High specific surface area ordered
11. A.D. Shiraz, A. Takdastan, S.M. Borghei, Photo-Fenton like deg- mesoporous silica COK-12 with tailored pore size. Microporous
radation of catechol using persulfate activated by UV and ferrous Mesoporous Mater. 280, 133–143 (2019)
ions: influencing operational parameters and feasibility studies. J. 27. X. Liu, N. Yan, L. Wang, C. Ma, P. Guo, P. Tian et al., Land-
Mol. Liq. 249, 463–469 (2018) scape of AlPO-based structures and compositions in the data-
12. Z. Noorimotlagh, I. Kazeminezhad, N. Jaafarzadeh, M. Ahmadi, base of zeolite structures. Microporous Mesoporous Mater. 280,
Z. Ramezani, S.S. Martinez, The visible-light photodegradation 105–115 (2019)
of nonylphenol in the presence of carbon-doped TiO2 with rutile/ 28. D.J. Moon, W.T. Lim, K. Seff, Crystal structure of a hydrogen
anatase ratio coated on GAC: effect of parameters and degradation sulfide sorption complex of anhydrous Mn2+-exchanged zeolite
mechanism. J. Hazard. Mater. 350, 108–120 (2018) Y (FAU, Si/Al = 1.56). Microporous Mesoporous Mater. 279,
13. Z. Noorimotlagh, S.A. Mirzaee, S.S. Martinez, S. Alavi, M. 432–438 (2019)
Ahmadi, N. Jaafarzadeh, Adsorption of textile dye in activated 29. T.-H. Pham, K.-M. Lee, M.S. Kim, J. Seo, C. Lee, La-modified
carbons prepared from DVD and CD wastes modified with multi- ZSM-5 zeolite beads for enhancement in removal and recov-
wall carbon nanotubes: equilibrium isotherms, kinetics and ther- ery of phosphate. Microporous Mesoporous Mater. 279, 37–44
modynamic study. Chem. Eng. Res. Des. 141, 290–301 (2019) (2019)
14. M. Mousavi, A. Habibi-Yangjeh, S.R. Pouran, Review on magneti- 30. Y. Zhao, Z. Liu, W. Li, Y. Zhao, H. Pan, Y. Liu et al., Synthe-
cally separable graphitic carbon nitride-based nanocomposites as sis, characterization, and catalytic performance of high-silica Y
promising visible-light-driven photocatalysts. J. Mater. Sci. Mater. zeolites with different crystallite size. Microporous Mesoporous
Electron. 29(3), 1719–1747 (2018) Mater. 167, 102–108 (2013)
15. M. Ahmadi, S. Samarbaf, M. Golshan, S. Jorfi, B. Ramavandi, 31. M. Ahmadi, M.H. Niari, B. Kakavandi, Development of maghe-
Data on photo-catalytic degradation of 4-chlorophenol from aque- mite nanoparticles supported on cross-linked chitosan (γ-Fe2O3@
ous solution using UV/ZnO/persulfate. Data Brief 20, 582–586 CS) as a recoverable mesoporous magnetic composite for effective
(2018) heavy metals removal. J. Mol. Liq. 248, 184–196 (2017)
16. S.A. Mirzaee, N. Jaafarzadeh, S. Jorfi, H.T. Gomes, M. Ahmadi, 32. M. Moosavifar, A. Alemi, M.R. Marefat, N. Nouruzi, H.
Enhanced degradation of Bisphenol A from high saline polycar- Mahmoodi, The effect of synthesis method and post-synthesis
bonate plant wastewater using wet air oxidation. Process Saf. treatment on the formation of neutral Mn(II) complex into ani-
Environ. Prot. 120, 321–330 (2018) onic zeolite structure and investigation of its catalytic activity in
17. M. Klavarioti, D. Mantzavinos, D. Kassinos, Removal of residual the epoxidation of alkenes. J. Iran. Chem. Soc. 11(6), 1561–1567
pharmaceuticals from aqueous systems by advanced oxidation (2014)
processes. Environ. Int. 35(2), 402–417 (2009) 33. R. Ghahremanzadeh, Z. Rashid, A.-H. Zarnani, H. Naeimi, Highly
18. M. Pirhashemi, A. Habibi-Yangjeh, S.R. Pouran, Review on the active magnetically separable CuFe 2 O 4 nanocatalyst: an effi-
criteria anticipated for the fabrication of highly efficient ZnO- cient catalyst for the green synthesis of tetrahydrofuro [3,4-b] qui-
based visible-light-driven photocatalysts. J. Ind. Eng. Chem. 62, noline-1, 8 (3H, 4H) dione derivatives. J. Iran. Chem. Soc. 11(5),
1–25 (2018) 1407–1419 (2014)
19. M. Shekofteh-Gohari, A. Habibi-Yangjeh, M. Abitorabi, A. Rouhi, 34. M.Y. Badi, A. Azari, H. Pasalari, A. Esrafili, M. Farzadkia, Modi-
Magnetically separable nanocomposites based on ZnO and their fication of activated carbon with magnetic Fe3O4 nanoparticle
applications in photocatalytic processes: a review. Crit. Rev. Envi- composite for removal of ceftriaxone from aquatic solutions. J.
ron. Sci. Technol. 48(10–12), 806–857 (2018) Mol. Liq. 261, 146–154 (2018)
20. M. Ahmadi, H. Rahmani, A. Takdastan, N. Jaafarzadeh, A. Mos- 35. M. Hayasi, N. Saadatjoo, Preparation of magnetic nanoparticles
toufi, A novel catalytic process for degradation of bisphenol A functionalized with poly (styrene-2-acrylamido-2-methyl pro-
from aqueous solutions: a synergistic effect of nano-Fe3O4@ Alg- panesulfonic acid) as novel adsorbents for removal of pharma-
Fe on O3/H2O2. Process Saf. Environ. Prot. 104, 413–421 (2016) ceuticals from aqueous solutions. Adv. Polym. Technol. 37(6),
21. M. Ahmadi, B. Kakavandi, N. Jaafarzadeh, A.A. Babaei, Catalytic 1941–1953 (2018)
ozonation of high saline petrochemical wastewater using PAC@ 36. F.-F. Liu, J. Zhao, S. Wang, P. Du, B. Xing, Effects of solution
FeIIFe2IIIO4: optimization, mechanisms and biodegradability chemistry on adsorption of selected pharmaceuticals and personal
studies. Sep. Purif. Technol. 177, 293–303 (2017) care products (PPCPs) by graphenes and carbon nanotubes. Envi-
22. A.A. Babaei, Z. Baboli, N. Jaafarzadeh, G. Goudarzi, M. Bahrami, ron. Sci. Technol. 48(22), 13197–13206 (2014)
M. Ahmadi, Synthesis, performance, and nonlinear modeling of 37. S. Miralles-Cuevas, F. Audino, I. Oller, R. Sánchez-Moreno, J.S.
modified nano-sized magnetite for removal of Cr(VI) from aque- Pérez, S. Malato, Pharmaceuticals removal from natural water by
ous solutions. Desalin. Water Treat. 53(3), 768–777 (2015) nanofiltration combined with advanced tertiary treatments (solar
23. A.A. Babaei, B. Kakavandi, M. Rafiee, F. Kalantarhormizi, I. photo-Fenton, photo-Fenton-like Fe(III)–EDDS complex and ozo-
Purkaram, E. Ahmadi et al., Comparative treatment of textile nation). Sep. Purif. Technol. 122, 515–522 (2014)
13
Journal of the Iranian Chemical Society
38. I.-G. Yi, J.-K. Kang, S.-C. Lee, C.-G. Lee, S.-B. Kim, Synthesis copper ferrite nanoparticles/ozone: a novel combination of
of an oxidized mesoporous carbon-based magnetic composite and advanced oxidation processes. Chem. Eng. J. 320, 436–447 (2017)
its application for heavy metal removal from aqueous solutions. 45. S.K. Maeng, K. Cho, B. Jeong, J. Lee, Y. Lee, C. Lee et al., Sub-
Microporous Mesoporous Mater. 279, 45–52 (2019) strate-immobilized electrospun TiO2 nanofibers for photocatalytic
39. S. Jorfi, S. Pourfadakari, B. Kakavandi, A new approach in sono- degradation of pharmaceuticals: the effects of pH and dissolved
photocatalytic degradation of recalcitrant textile wastewater using organic matter characteristics. Water Res. 86, 25–34 (2015)
MgO@ Zeolite nanostructure under UVA irradiation. Chem. Eng. 46. F. Ghanbari, M. Moradi, F. Gohari, Degradation of 2,4,6-trichlo-
J. 343, 95–107 (2018) rophenol in aqueous solutions using peroxymonosulfate/activated
40. B. Kakavandi, A. Raofi, S.M. Peyghambarzadeh, B. Ramavandi, carbon/UV process via sulfate and hydroxyl radicals. J. Water
M.H. Niri, M. Ahmadi, Efficient adsorption of cobalt on chemi- Process Eng. 9, 22–28 (2016)
cal modified activated carbon: characterization, optimization and 47. J.C. Carlson, M.I. Stefan, J.M. Parnis, C.D. Metcalfe, Direct UV
modeling studies. Desalin. Water Treat. 111, 310–321 (2018) photolysis of selected pharmaceuticals, personal care products and
41. S. Ba, J.P. Jones, H. Cabana, Hybrid bioreactor (HBR) of hollow endocrine disruptors in aqueous solution. Water Res. 84, 350–361
fiber microfilter membrane and cross-linked laccase aggregates (2015)
eliminate aromatic pharmaceuticals in wastewaters. J. Hazard. 48. H. Mansouri, R.J. Carmona, A. Gomis-Berenguer, S. Souissi-
Mater. 280, 662–670 (2014) Najar, A. Ouederni, C.O. Ania, Competitive adsorption of ibupro-
42. L. Ai, C. Zhang, L. Li, J. Jiang, Iron terephthalate metal–organic fen and amoxicillin mixtures from aqueous solution on activated
framework: revealing the effective activation of hydrogen peroxide carbons. J. Colloid Interface Sci. 449, 252–260 (2015)
for the degradation of organic dye under visible light irradiation. 49. M. Moradi, F. Ghanbari, M. Manshouri, K.A. Angali, Photocata-
Appl. Catal. B 148, 191–200 (2014) lytic degradation of azo dye using nano-ZrO 2/UV/Persulfate:
43. B. Kakavandi, A. Takdastan, S. Pourfadakari, M. Ahmadmoaz- response surface modeling and optimization. Korean J. Chem.
zam, S. Jorfi, Heterogeneous catalytic degradation of organic com- Eng. 33(2), 539–546 (2016)
pounds using nanoscale zero-valent iron supported on kaolinite: 50. M. Ahmadi, F. Ghanbari, A. Alvarez, S.S. Martinez, UV-LEDs
mechanism, kinetic and feasibility studies. J. Taiwan Inst. Chem. assisted peroxymonosulfate/Fe2+ for oxidative removal of car-
Eng. 96, 329–340 (2019) moisine: the effect of chloride ion. Korean J. Chem. Eng. 34(8),
44. N. Jaafarzadeh, F. Ghanbari, M. Ahmadi, Efficient degradation of 2154–2161 (2017)
2,4-dichlorophenoxyacetic acid by peroxymonosulfate/magnetic
Affiliations
Afshin Takdastan2,3 · Hadi Sadeghi4 · Sina Dobaradaran5,6,7 · Lin Ma8 · Armin Sorooshian8 · Maryam Ravanbakhsh1,2 ·
Maryam Hazrati Niari1,2
1 5
Student Research Committee, Ahvaz Jundishapur University Systems Environmental Health and Energy Research Center,
of Medical Sciences, Ahvaz, Iran The Persian Gulf Biomedical Sciences Research Institute,
2 Bushehr University of Medical Sciences, Bushehr, Iran
Department of Environmental Health Engineering, School
6
of Health, Ahvaz Jundishapur University of Medical Department of Environmental Health Engineering, Faculty
Sciences, Ahvaz, Iran of Health, Bushehr University of Medical Sciences, Bushehr,
3 Iran
Environmental Technologies Research Center, Ahvaz
7
Jundishapur University of Medical Sciences, Ahvaz, Iran The Persian Gulf Marine Biotechnology Research Center,
4 The Persian Gulf Biomedical Sciences Research Institute,
Department of Environmental Health Engineering, School
Bushehr University of Medical Sciences, Bushehr, Iran
of Health, Ardabil University of Medical Sciences, Ardabil,
8
Iran Department of Chemical and Environmental Engineering,
The University of Arizona, Tucson, AZ, USA
13