Separation Science and Technology

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The removal of cephalexin antibiotic in aqueous

solutions by ultrasonic waves/hydrogen peroxide/
nickel oxide nanoparticles (US/H2O2/NiO) hybrid
process

Abdolmotaleb Seid-Mohammadi, Ghorban Asgarai, Zeinab Ghorbanian &

Abdollah Dargahi

To cite this article: Abdolmotaleb Seid-Mohammadi, Ghorban Asgarai, Zeinab Ghorbanian &
Abdollah Dargahi (2019): The removal of cephalexin antibiotic in aqueous solutions by ultrasonic
waves/hydrogen peroxide/nickel oxide nanoparticles (US/H2O2/NiO) hybrid process, Separation
Science and Technology, DOI: 10.1080/01496395.2019.1603241

To link to this article: https://doi.org/10.1080/01496395.2019.1603241

Published online: 13 Apr 2019.

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SEPARATION SCIENCE AND TECHNOLOGY
https://doi.org/10.1080/01496395.2019.1603241

The removal of cephalexin antibiotic in aqueous solutions by ultrasonic waves/

hydrogen peroxide/nickel oxide nanoparticles (US/H2O2/NiO) hybrid process
Abdolmotaleb Seid-Mohammadia, Ghorban Asgaraia, Zeinab Ghorbanianb, and Abdollah Dargahib,c
a
Social determinants of health research center (SDHRC), Environmental Health Engineering, School of Public Health, Hamadan University of
Medical Sciences, Hamadan, Iran; bEnvironmental Health Engineering, School of Public Health, Hamadan University of Medical Sciences,
Hamadan, Iran; cStudent Research Committee, Hamadan University of Medical Sciences, Hamadan, Iran

ABSTRACT ARTICLE HISTORY

Antibiotics are non-biodegradable and can remain for a long time at aquatic environments and Received 27 February 2019
they have a big potential bio-accumulation in the environment. The antibiotics are broadly Accepted 1 April 2019
metabolized by humans, animals and plants and they or their metabolites, after metabolization, KEYWORDS
are entered into the aquatic environment. This study aimed to optimize the operational para- Advanced oxidation process;
meters by Taguchi design and to carry out the kinetic studies for removal of cephalexin antibiotic Cephalexin antibiotic;
from aqueous solutions by US/H2O2/NiO hybrid process. This experimental study was performed Kinetic studies; US/H2O2/NiO
on a laboratory scale in a 500 mL pyrex-made reactor. The main operational parameters to process; Taguchi method;
influence the US/H2O2/NiO process were identified as the initial concentration of CEX Aqueous solution
(20–80 mg/L), hydrogen peroxide (H2O2) (10–40 mL/L), NiO nanoparticle (2.5–10 mg/L) and
reaction time (15–90 min) and therefore, the influence of these factors were studied. Under
optimum conditions (pH = 3, reaction time = 90 min, CEX = 40 mg/L, NiO = 7.5 mg/L and H2
O2 = 30 mL/L) and using the US/H2O2/NiO process, the removal efficiencies of CEX, COD and TOC
were 93.86%, 72.46% and 54.55%, respectively. The percentage contribution of each factor was
also determined. Results introduced the solution pH as the most powerful factor, and its percen-
tage contribution value was up to 94% in the studied process. It was also identified that the
removal of CEX antibiotic using the hybrid process obeys the pseudo-first-order kinetics.

Introduction environment.[12,13] The resistant to biodegradation is one

important feature of many types of these pharmaceutical
Today, uncontrolled use of antibiotics and consequently
compounds which may lead to a generation of resistant
the entry of these compounds into the environment have
bacterial strains. The transmission of these resistant bac-
raised global concerns. About 100,000–200,000 tons of
terial strains to the human population may cause serious
antibiotics are annually used in the world.[1] They have
health problems.[2,14] The bio-accumulation of the Fat-
extensive application in medicine, animal husbandry and
soluble pharmaceuticals in the body of aquatic species
agriculture. However, a significant portion of these anti-
such as fish may lead to transferring these medicines
biotics (30–90%) is not entirely metabolized in human or
into the human population during consumption of such
animal bodies and are excreted as active compounds.[2–4]
aquatic animals as a food.[15] Cephalexin (CEX) is a type
Thus, the presence of large amounts of antibiotics in
of semi-synthetic cephalosporin antibiotic, which, due to
medical waste, industrial wastewater, cattle waste and
its broad antibacterial activity, is broadly applied for treat-
sewage effluent and, consequently, in the environment is
ment of infections throughout the body.[16] Figure 1 indi-
not surprising.[5] These are frequently detected in
cates the chemical structure of CEX antibiotic.
groundwater,[6,7] drinking water,[8] surface water[9,10]
The environmental pollution by antibiotics, for example
and agricultural lands.[11] Releasing the wastewaters
CEX has identified as an emerging issue. However, enough
from different resources such as households, hospitals,
attention to this type of pollution has not been paid yet.[17]
veterinary and pharmaceutical industries to the water
Therefore, more studies towards this harmful pollutant are
body is considered as serious problem because there are
required. Accordingly, the methods such as advanced oxi-
a number of pollutants, for example antibiotics in these
dation process (AOPs),[18,19] adsorption,[2,20,21] biological
wastewaters, which is led to sever risks for human and
treatment[22] and sonochemical degradation[23] have been

CONTACT Abdollah Dargahi a.dargahi29@yahoo.com Environmental Health Engineering, School of Public Health, Hamadan University of Medical
Sciences, Hamadan, Iran
Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/lsst.
© 2019 Taylor & Francis Group, LLC
2 A. SEID-MOHAMMADI ET AL.
Figure 1. Chemical structures of Cephalexin (CEX).
executed to remove the antibiotics. However, the advanced
oxidation processes (AOPs) are of the methods that have
recently found as the superb methods to eliminate the
antibiotics. The production of ●OH radicals, which have
an admirable potential to degrade a broad range of organic
compounds, is the main features of these techniques.[24,25]
The basis of these methods are the combination of oxidiz-
ing agents (i.e. O3, H2O2) and/or catalysts (e.g. Fe, Mn and
TiO2) and/or ultrasound and their performance may also
enhance by UV light and/or electricity.[26–31] H2O2 is one
of the strongest oxidants, which is stronger than chlorine,
chlorine dioxide and potassium permanganate. The mole-
cular structure of this material consists of an oxygen bridge,
which connects each of these oxygen atoms to a hydrogen
atom. It can directly or indirectly react with organic matter
in water. Studies have shown that the decomposition and
oxidation rate of the material is greater at the presence of
the higher number of hydroxyl radicals. Considering the
fact that the number of ●OH radicals produced by the
combined system is greater than the separate ultrasonic
system; therefore, the oxidation rate of the combination is
greater than that of the system a separate ultrasonic.[32]
Hydrogen peroxide can participate in processes such as
US/H2O2, O3/H2O2 or Fenton processes.[33] Ultrasonic
waves, by stimulation of cavitations in chemical com-
pounds, are led to the formation of strong and active
radicals such as OH°, H° and H2O2. The produced radicals
may react with collapsing bubbles and produce new mole-
cular structures or may be transformed into a situation that
the inner liquid becomes active. In water, the hydroxyl and
hydrogen active radicals are produced through the
sonolysis.[34] The methods that apply the ultrasonic waves
have been found to be effective in removing the chemicals
and toxic contamination. Nowadays, the combination of
ultrasonic waves with other methods such as advanced
oxidation process has extensively applied in studies to
remove the pollutants.[35] The combined use of the ultra-
sonic wave and H2O2 leads to producing the hydroxyl
radicals through the cavitation; these radicals have a high
oxidation potential and are capable to directly degrade the
organic pollutants. But, the lifetime of hydroxyl radicals is
very short and they incline to combine with each other and
to form H2O2. The reactions occurred under ultrasonic
irradiation in the presence of H2O2 are as follows.[35,36] In
general, in the US/H2O2 process, the ultrasonic is used to
decompose the O-O bond in hydrogen peroxide and pro-
duce hydroxyl radicals. The reaction processes of US/H2O2
are as follows (Equations1–5).[37]

H2 O2 þ US ! 2OH (1)
 
H2 O2 þ OH ! HO2 þ H2 O (2)
 
H2 O2 þ HO2 ! OH þ H2 O þ O2 (3)

2OH ! H2 O2 (4)

2HO2 ! H2 O2 þ O2 (5)
The benefits of this process include the lack of produc-
tion of any kind of carcinogen, lack of odour and taste
problems, the lack of need for the use and storage of
hazardous chemicals, and the need for small space to
deploy an ultrasonic unit.[38]
Hence, considering the hazards of CEX, the pre-
sent study aims to determine the efficiency of
Ultrasonic waves/Hydrogen peroxide/Nickel oxide
nanoparticles (US/H2O2/NiO), as a hybrid process
in removing CEX from aqueous solutions. In this
study, the initial CEX concentration, pH of the initial
solution, H2O2 concentration, reaction time and NiO
nanoparticle are the parameters influencing the
hybrid process. Thus, optimization of the studied
system is necessary; for this purpose, the estimation
and determination of the optimum values of the
studied parameters for obtaining high CEX removal
using the mentioned system were carried by Taguchi
design approach. An orthogonal array experiment
design (L16) with five factors having four levels
each was employed. ANOM and ANOVA, the opti-
mal conditions and the percentage contribution of
each parameter were determined using the S/N
ratio. Furthermore, under optimal conditions, the
kinetics of CEX removal using the US/H2O2/NiO
system was studied.

Materials and methods
Chemicals and reagents
Cephalexin antibiotic ((CEX), the chemical formula of C16
H17N3O4S and the purity of 98%) was purchased from
Sigma Aldrich (St. Louis, MO, USA). Nickel oxide nano-
particles (NiO) (Sigma Aldrich, St. Louis, MO, USA) and
Hydrogen peroxide (H2O2) 30% w/w were supplied from
Sigma-Aldrich. Double distilled water was utilized to pre-
pare the solutions. 0.1 M Hydrochloric acid (HCl) and
0.1 M sodium hydroxide (NaOH) were applied to regulate
the pH of the solutions. All the chemicals used in the
experiments were of analytical grade and were applied
without further purification.
US/H2O2/NiO process reactor
This experimental study was performed on laboratory scale
in a 500 mL pyrex-made reactor, equipped with a turbulent
reservoir, a pH meter and an ultrasonic wave generator.
The ultrasonic device used in this study is a model of
the LUC-405 model, Stainless steel and manufactured
in South Korea. Its other properties include: Time
range: 0–99 min, Voltage: 100-240v-AC, 50/60Hz,

Temperature range: 0–40 C, Frequency: 40 KHZ,
Capacity dimensions: 300 × 55 × 150 mm and Main
dimensions: 300 × 285 × 255 mm. The schematic
design of the reactor is presented in Figure 2.
Analytical procedure
After conducting the related experiments, the sam-
ples were collected at predetermined time intervals
Figure 2. Schematic of studied reactor. (1) Mixer, (2) ultrasonic wave chamber, (3) reaction chamber and (4) pH meter.
SEPARATION SCIENCE AND TECHNOLOGY 3
and were filtered through 0.45 µm membrane filter,
and the concentration of CEX was measured using
a high-performance liquid chromatography (HPLC)
at a wavelength of 262 nm. HPLC Agilent 1260
infinity (Agilent Technologies Co. Ltd., USA)
equipped with a Shimadzu LC-20 AB pump:
140 mm×260 mm×420 mm, operating temperature
range: 4–35°C, power requirements: 100 VAC,
150 VA, 50/60 Hz, maximum discharge pressure:
40 MPa, flow-rate setting range: 0.0001–10 mL/min,
solvent delivery method: parallel-type double plunger,
plunger capacity: 10 μL), A C18 column (250 mm ×
4.6 mm, with 5 μm particle size, pore size: 12 nm,
surface area: 410 m2/g, carbon loading: 20%, pore
volume: 1.25 mL/g, pH range: 2–7.5, bonding type:
monomeric) was used as the stationary phase, and
a UV-Vis spectrophotometer (Shimadzu UV-1600
(Japan), dimensions: 380 mm (200 mm at closing
LCD unit)×550 mm×470 mm, power consumption:
160 VA, frequency: 50/60 Hz, wavelength range: 190–
1,100 nm, wavelength accuracy: ±0.5 nm, wavelength
repeatability: ±0.1 nm, photometric range: absor-
bance: −0.5 to +3.999 Abs, photometric accuracy (at
0.5 Abs): ±0.002 Abs, photometric repeatability (at
0.5 Abs): ±0.001 Abs). The mobile phase was a mix-
ture of water and methanol (40:60 v/v, HPLC grade,
Merck) with a flow rate of 1 mL/min at 25°C. The
injection of 20 μL of CEX antibiotic solution into the
column was done and its concentration was deter-
mined at a wavelength of 262 nm. Furthermore, the
determination of chemical oxygen demand (COD)
was carried out using COD ampoules (HACH
Chemical) using a spectrophotometer (DR 6000,
4 A. SEID-MOHAMMADI ET AL.

HACH, USA). TOC analyser (Elementar, Germany) ½CEX 0  ½CEX t

ARE ð%Þ ¼  100 (6)
was used to measure the total organic carbon (TOC) ½CEX 0
content of the CEX antibiotic.

Experimental design–Taguchi orthogonal array
The effect of main operational parameters such as the
initial concentration of CEX (20–80 mg/L), hydrogen
peroxide (H2O2) (10–40 mL/L), NiO nanoparticle
(2.5–10 mg/L) and reaction time (15–90 min) on the
US/H2O2/NiO process was studied. In this study,
Taguchi (L16) orthogonal array experimental design
containing five factors with four levels was employed
and was presented in Table 1. The design suggested 16
experiments conducted for the chosen factors with their
corresponding levels along with the experimental
results observed, as presented in Table 2. All of the
experiments were accomplished in duplicate and inte-
grated into the model and analysed by the model.
Minitab16 software was applied to the design of experi-
ments, to analyse the variance and to optimize the
process.
The efficiency of US/H2O2/NiO process in removing
antibiotic CEX was calculated using Equation (6) and
the removal efficiency of chemical oxygen demand
(COD) by this process was determined using
Equation (7).
Table 1. The experimental factors and their levels for CEX
removal by US/H2O2/NiO process.
Factors Level 1 Level 2 Level 3 Level 4
A: pH 3 5
B: CEX concentration (mg/L) 20 40
C: H2O2 (mL/L) concentration(mg/L) 10 20
D: NiO nanoparticle (mg/L) 2.5 5 7.5
E: reaction time (min) 15 30
½COD0  ½CODt
COD removal ð%Þ ¼  100 (7)
½COD0
Where Antibiotic removal efficiency (ARE) (%) shows
CEX removal efficiency, [CEX]0 and [CEX]t represent
the initial concentration of CEX at the time 0 and the
concentration of CEX at time t, respectively. [COD]0
and [COD]t is related to the COD before and after
treatment, respectively. The COD evolution was deter-
mined at the start of the treatment (0 min) and after
90 min (the end of the treatment).
In the Taguchi method, the accurate analysis of the
results was carried out by a converted response func-
tion, defined as the ratio of the sign of each effect (S) to
the effects caused by the error (N). In this study, ARE
was considered as response. The S/N ratio is calculated
using the Equation (Equation 8).[39,40] The n denotes
the number of replication of the experiment and ARE
shows the results of the experiments. The average S/
N ratio for degradation of CEX antibiotic by US/H2O2
/NiO process was shown in Table 3.
" #
1 X  1 2
S= ¼ 10log (8)
N 10
n AREi
In this study, the determination of the optimal condi-
7 9 tions was carried out using the analysis of means
60 80
30 40 (ANOM). At first, the average S/N ratio of each factor
10 was calculated at a certain level. For example, the
60 90

Table 3. Results of ANOM Analysis for determination of the

Table 2. The condition for Taguchi design experiments (L16) optimal conditions for US/H2O2/NiO process.
and the results obtained for each experiment and their related Factor/level j=1 j=2 j=3 j=4 M
S/N values in US/H2O2/NiO process. pH/1 34.37 34.86 36.55 35.54 35.33
Factor ARE (%) pH/2 29.91 30.91 31.20 32.20 31.05
pH/3 29.57 28.64 28.01 26.12 28.08
Tests A B C D E ARE1 ARE1 S/N pH/4 25 22.93 25.90 25.62 24.86
1 3 20 10 2.5 15 51.70 53.00 34.37 H2O2/1 34.37 29.91 29.57 25 29.71
2 3 40 20 5.0 30 54.60 56.10 34.86 H2O2/2 34.86 30.91 28.64 22.93 29.33
3 3 60 30 7.5 60 67.70 66.80 36.55 H2O2/3 36.55 32.20 28.01 25.90 30.66
4 3 80 40 10.0 90 60.10 59.60 35.54 H2O2/4 35.54 32.20 26.12 25.62 29.87
5 5 80 10 5.0 60 31.10 31.50 29.91 NiO nanoparticle/1 34.37 30.91 28.01 25.62 29.72
6 5 60 20 2.5 90 35.10 35.20 30.91 NiO nanoparticle/2 34.86 29.91 26.12 25.90 29.19
7 5 40 30 10.0 15 36.20 36.50 31.20 NiO nanoparticle/3 36.55 32.20 29.57 22.93 30.31
8 5 20 40 7.5 30 40.50 41.00 32.20 NiO nanoparticle/4 35.54 31.20 28.64 25 30.09
9 7 40 10 7.5 90 30.20 30.00 29.57 CEX concentration/1 34.37 32.20 28.64 25.90 30.27
10 7 20 20 10.0 60 27.10 27.00 28.64 CEX concentration/2 34.86 31.20 29.57 25.62 30.31
11 7 80 30 2.5 30 25.11 25.23 28.01 CEX concentration/3 36.55 30.91 26.12 25 29.64
12 7 60 40 5.0 15 20.20 20.30 26.12 CEX concentration/4 35.54 29.91 28.01 22.93 29.09
13 11 60 10 10.0 30 17.60 18.00 25.00 Reaction time/1 34.37 31.20 26.12 22.93 28.65
14 11 80 20 7.5 15 11.40 20.10 22.93 Reaction time/2 34.86 31.20 29.57 25 30.15
15 11 20 30 5.0 90 19.50 20.00 25.90 Reaction time/3 36.55 29.91 28.64 25.62 30.18
16 11 40 40 2.5 60 19.00 19.20 25.62 Reaction time/4 35.54 30.91 29.57 25.90 30.48
 SEPARATION SCIENCE AND TECHNOLOGY 5

averages S/N ratio of factor I at level i is calculated conditions were presented in Table 3 depict. The highest
using the equation (9). values of M for each factor denote the optimal situation of
"  # the agent. Table 3 revealed that the optimum conditions for
1 X nIi
S Level¼i US/H2O2/NiO hybrid process were as following: (1) pH
MNS ¼ MFactor¼I¼ S ¼
Leveli
(9)
N nIi j¼1 N Factor¼I level 1 (pH: 3), (2) reaction time level 4 (Reaction time:
j
90 min), (3) initial concentration of CEX antibiotic level 2
Where nIi is the number of conditions for the factor (C0: 40 mg/L); (4) H2O2 concentration level 3 (H2O2 con-
I and level i in thehexperiment,
Level¼i i which was 2 in the centration: 30 mL/L) and (5) NiO nanoparticle level 3 (NiO:
present study. Also, NS Factor¼I is the S/N ratio of the 7.5 mg/L). The experiment was carried out on the basis of
j
experiments with the condition of factor I and level i. these conditions with two repetitions and the results were
Similarly, this ratio is calculated for all factors and represented in Table 4; considering this Table, the optimum
average levels. Finally, an experiment is carried out conditions for Taguchi analysis were greater than S/N. The
using the optimal conditions to prove the method confirmation experiment was accomplished based on the
used. In this study, the assessment of the effect of abovementioned optimum conditions, the ARE of US/H2
each factor on the rate of CEX antibiotic removal was O2/NiO hybrid process registered, and the S/N ratio calcu-
implemented using the analysis of variance (ANOVA). lated (Table 2). The value of the S/N ratio under optimum
The percentage of the effect of the studied factors was conditions (39.42) was somewhat greater than its value
determined by equation (10). observed in Test 3 (36.55), and the average ARE under
SSF  ðDOFF  VER Þ optimum conditions (93.98%) was higher than that of
RF ¼  100 (10) obtained in Test 3 (66.80%). Considering the results, the
SST
rank order of the percentage contributions of each factor
In this equation, DOFF reveals the degree of freedom of for US/H2O2/NiO hybrid process is: (1) the pH of solution
each factor (one unit less than the number of levels of (94%), (2) H2O2 concentration (2.7%), (3) the CEX initial
the target factor, which is 5 in this research). The total concentration (1.7%), (4) NiO nanoparticle (1.2%) and (5)
sum of squares (SST) and the sum of the factorial reaction time (0.4%) (Table 5). According to the results,
squares (SSF) are calculated using equation (11) and among four studied factors, the pH was the most influential
equation 12, respectively. factor in the studied process.
!
Xm X n  2
SST ¼ AREi  mn ARET
2
(11)
j¼1 j¼1 Effect of effective factors in US/H2O2/NiO hybrid
process

m  2 Effect of pH of solution
mn X F The pH of the environment has been identified as an
SSF ¼ AREk  ARET (12)
L k¼1 important factor affecting the speed of chemical reac-
F tions, and it, directly and indirectly, influences the
AREk shows the mean of the measured values of the oxidation of organic matter. In advanced oxidation
desired factor in the level of k. The error variance of processes, pH changes affect the oxidation of organic
VER is calculated using the equation 13. matter through the production of various radicals.[41]
P
SST  EF¼A SSF
VER ¼ (13)
mðn  1Þ Table 4. The optimum conditions for CEX antibiotic removal by
US/H2O2/NiO process.
Factor A B C D E ARE1 ARE2 S/N
Test 3 for CEX 3 60 30 7.5 60 67.70 66.80 36.55
Results and discussion Optimization condition for 3 40 30 7.5 90 94.75 93.98 39.49
CEX
Optimum conditions and percentage of
contribution
Table 5. Analysis of variance (ANOVA) of effective parameters
Table 2 depicts the results and the values of S/N obtained on CEX antibiotic removal by US/H2O2/NiO process.
for each of the related experiments. As is observed, the Factors DF Sum Sq Mean Sq P value RF (%)
highest and lowest S/N values were obtained from the A: pH 3 1246.6 3739.81 0.001 94
experiments 3 and 14, respectively and the highest value B: CEX concentration (mg/L) 3 22.45 67.35 0.001 1.7
C: H2O2 (mL/L) 3 35.64 106.93 0.173 2.7
related to in Test 3 should be compared with the optimal D: NiO nanoparticle (mg/L) 3 14.81 44.43 0.06 1.2
mode. In addition, the average analysis values for optimal E: reaction time (min) 3 22.45 67.35 0.107 0.4
6 A. SEID-MOHAMMADI ET AL.
Due to a direct effect of pH on the production of
hydroxyl radicals and, its effect on the efficiency of
the oxidation process, the pH is the first parameter
that is examined by the process. In the present study,
in order to evaluate the effect of this parameter, the
experiments were conducted at pH range between 3
and 9, and the results based on S/N were represented
in Figure 3a. According to results, the highest CEX
removal in US/H2O2/NiO hybrid process was attained
at pH = 3 with S/N ratio of 35.33. At higher pH values
(pH = 9), the process efficiency was reduced; so that,
the S/N ratio was 24.86 at pH = 9. Seid-Mohammadi
et al. used the US/H2O2/Fe2+ and US/S2O82-/Fe2+ pro-
cesses to remove the colourful wastewater and found
that acidic pH (pH = 3) is best to obtain the highest
removal efficiency.[36]
Figure 3. (a) The effect of pH, (b) the effect of reaction time, (c) the effect of CEX antibiotic concentration, (d) the effect of H2O2 and
(e) the effect of NiO nanoparticle on the S/N ratio in the removal of CEX antibiotic by US/H2O2/NiO hybrid process. Circles on figures
indicate optimum electrolysis time for US/H2O2/NiO hybrid process.
Effect of reaction time
Optimization of time in removal reactions is lead to sav-
ing the costs of operation and the consumption of energy.
In the present study, in order to determine the effect of
reaction time on the removal of CEX antibiotics by the
US/H2O2/NiO process, the experiments were carried out
at different reaction times of 15–90 min. The results based
on S/N are shown in Figure 3b. The results showed that
the reaction time is directly related to the removal effi-
ciency of CEX antibiotics, so that the antibiotic removal
rate was increased by increasing the reaction time.
According to the results, with an increase in reaction
time of 15–90 min, the S/N rate was increased from
28.65 to 30.48. Because, with increasing electrolysis time,
the radical hydroxyl content produced is greater and, as
a result, the efficiency of CEX removal is increased by the

hybrid process of US/H2O2/NiO. This is consistent with
the results of Seid-Mohammadi et al.[42]
Effect of CEX antibiotic initial concentration
Another parameter that influences the amount of CEX
antibiotic removal by the hybrid process of US/H2O2
/NiO, is the various concentrations of antibiotic CEX.
Accordingly, antibiotic concentrations in the range of
20–80 mg/L were investigated. The effect of this para-
meter on the removal rate based on S/N is shown in
Figure 3c.
The results showed that the combined process of
US/H2O2/NiO has an indirect relationship with anti-
biotic concentration. As the concentration of antibiotic
CEX increases in each hybrid process, the elimination
efficiency decreases. As the antibiotic concentration
increased from 20 to 80 mg/L, S/N decreases from
29.09 to 30.27. At low concentrations of antibiotics,
hydroxyl radicals can easily eliminate a high percentage
of contaminants in the reaction reactor; but, by increas-
ing the concentration of contaminants, the amount of
hydroxyl ions produced is not sufficient for the com-
plete elimination of antibiotics.[36]
The effect of H2O2 concentration
The type and concentration of the used oxidizing agent
are the factors affecting the performance of the
AOPs.[43] The estimation of the effect of initial
Hydrogen peroxide (H2O2) concentration on the CEX
removal efficiency was performed at H2O2 concentra-
tions of 10–40 mL/L. Figure 3d reveals the effects of
initial concentration of H2O2 on the CEX removal rate
based on S/N.
The results related to the effect of H2O2 on the
removal of CEX in the process of US/H2O2/NiO show
that the removal process is dependent on the initial
concentration of H2O2; so that, with increasing the
initial concentration of H2O2, the removal efficiency is
partially increased and then reduced (Figure 3d).
According to this figure, with an increase in H2O2 up
to the concentration of 30 mL/L, due to increasing the
hydroxyl radical production, the removal efficiency is
increased.[44] However, with a further increase in the
initial concentration of H2O2, the removal of CEX was
decreased. Decreasing the removal efficiency can be due
to the fact that, at higher concentrations of H2O2, H2O2
itself acts as an effective hydroxyl radical receptor and
reduces the hydroxyl radical in the environment, which
is led to reducing the removal efficiency.[45] In fact, at
higher concentrations of H2O2, OH radicals are prob-
ably produced by other reactions through other reac-
tions, such as the radical receptivity effect of H2O2 and
SEPARATION SCIENCE AND TECHNOLOGY 7
the recombination of the radicals of OH, according to
the following reactions(Equations 1–5).[46]
Therefore, the time of complete removal of CEX at
a higher concentration of H2O2 will be longer, and control
of H2O2 level in the removal of CEX has a great impor-
tance, which is consistent with the results of the study by
Gharbani et al (2016)[47] and Malani et al. (2014).[48]
Malani et al., in their study, concluded that increasing
H2O2 concentration up to a certain extent would increase
the percentage removal of benzaldehyde and, subse-
quently, it leads to decreasing the removal percentage.
Also, the results of Babuponnusami et al. (2012)[49]
showed that, by increasing H2O2 concentration, phenol
removal efficiency was initially increased, but, with
further increase of H2O2, the decrease in efficiency was
observed, which, based on the results of this study, it is
due to the excessive production of hydroxyl radical.
The effect of NiO nanoparticle
The effect of NiO nanoparticle on the CEX antibiotic
removal efficiency using US/H2O2/NiO hybrid process
was studied at the NiO nanoparticle in the range of
2.5–10 mg/L. Generally, by increasing NiO concentra-
tion, the removal efficiency was initially increased and
then decreased. The results based on S/N are shown in
Figure 3e. As shown in Figure 3e, by an increase in NiO
concentration from 2.5 to 7.5, the ratio of S/N was
increased, but this ratio was decreased at the NiO con-
centration from 7.5 to 10. The lowest and highest levels
of S/N were related to the NiO concentration of 5 and
7.5 mg/L, respectively.
The increase in the removal efficiency may be attrib-
uted to the fact that increasing the NiO nanoparticle
concentration is led to increasing the adsorbent surface
for CEX molecules. This is valid for a particular value
of nanoparticle concentration and, after this value, the
removal efficiency is reduced by increasing the nano-
particle concentration; it can be due to lessening the
effective surface area which is consistent with the
results of Panji et al. (2016).[50]
Kinetics of CEX removal by the US/H2O2/NiO
process
Chemical kinetics is utilized to evaluate the rate of che-
mical reactions. The rate of a reaction could be inter-
preted by reducing the concentration of a reactant in
a unit of time or increasing the concentration of
a product per unit time. The calculation of the reaction
rate of gases and liquids is carried out by concentration in
a unit time, which the change in concentration, in other
words, the change of mole in a unit time in a chemical
reaction is a factor for the progress of a reaction.[1]
8 A. SEID-MOHAMMADI ET AL.

Figure 4. Kinetics of CEX antibiotic removal at the optimum conditions (CEX initial concentration = 40 mg/L, H2O2 = 40 mL/L,
pH = 3, NiO concentration = 7.5 mg/L). (a) Pseudo-first-order model and (b) pseudo-second-order model.

In this study, the kinetics of the CEX antibiotic Table 7. The kinetics for the removal of CEX antibiotic by US/H2O2
removal was studied in optimal conditions and using /NiO process (time: 90 min, pH: 3, H2O2: 30 mL/L, [CEX]0 = 40 mg/L
first and second order kinetics models and the results and NiO = 7.5 mg/L).
Kinetics k (min−1) R2 t1/2 (min)
were presented in Figure 4 and Table 5, Table 6.
Pseudo-first-order model 0.0295 0.9975 23.49
Considering the results, the regression coefficients Pseudo-second-order model 0.0077 0.9488 90
(R2) of the kinetic model for the first order and
the second order were obtained to be 0.9975 and
0.9488, respectively. Where C0 and Ce are the initial and final concentrations
The obtained results of kinetic studies represent that the of CEX antibiotic, respectively, and k is a constant of
pseudo-first-order model, with a considerable coefficient of removal value; k value is equal to the slope of the plot
correlation (R2), was the superior model to fit the data of of Ln(C0/Ce) versus time t. In addition, the half-life
CEX removal than the second-order kinetics model. These (t1/2) was calculated using equation 16.
results are proved by the results of the studies conducted by 0:693
Zarei et al. (2018)[51] and Rocha et al. (2017).[19] t1=2 ¼ (16)
k
The rate constant (k) obtained for CEX antibiotic
removal using the US/H2O2/NiO hybrid process was
0.0295 min−1. Furthermore, the half-life (t1/2) of anti- Performance of US/H2O2/NiO process in removal of
biotic removal using the hybrid process was 23.49 min CEX, TOC and of COD
(Table 6), Table7.
In this study, the pseudo-first-order and the pseudo- In this study, the COD/TOC ratio parameter was eval-
second-order models were used for CEX removal and uated to determine the biodegradability potential of
were calculated using equations 14 and 15. CEX antibiotic in US/H2O2/NiO process. The results
  showed that COD/TOC ratio was decreased from 2.35
C0
Ln ¼ kt (14) to 1.43; this indicates the biodegradability potential of
Ce the CEX antibiotic by the US/H2O2/NiO process, which
is consistent with the study by Ferrag-Siagh et al. in
their study, the electro-Fenton process was used as pre-
1 1 treatment for the biological process to treat the Tylosin
 ¼ Kt (15)
Ce C0 tartrate, and the results revealed that the COD/TOC
ratio was decreased which it is indicative of the biode-
gradability of the process so that the COD/TOC ratio
Table 6. Kinetics of CEX antibiotic removal at the optimum condi-
tions (CEX initial concentration = 40 mg/L, H2O2 was decreased from 2.32 to 0.73.[52]
concentration = 30 mL/L, pH = 3, NiO concentration = 7.5 mg/L). In this study, the capability of the US/H2O2/NiO
Time (min) Ct (mg/L) 1/C C/C0 -Ln(C/C0) Removal (%) hybrid process in removal of CEX, TOC, and COD
0 40 0 1 0 0 was studied under optimum conditions, that is pH of 3,
15 24 0.083 0.6 0.51 40
30 15.2 0.131 0.38 0.96 62
H2O2 of 30 mL/L, NiO of 7.5 mg/L, CEX initial con-
60 6 0.33 0.15 1.89 85 centration of 40 mg/L and reaction time of 90 min
90 2.8 0.71 0.07 2.65 93
(Figure 5). Considering the results obtained from this

100
90
80
70
Removal (%)
60
50
40
30
20
10
0
CEX
Figure 5. Performance of US/H2O2/NiO process in the removal of CEX antibiotic, COD and TOC at the optimum conditions (pH: 3,
Reaction time: 90 min, H2O2: 30 mL/L, NiO: 7.5 mg/L, CEX concentration: 40 mg/L, COD0 = 53.4 mg/L, TOC0 = 22.7 mg/L).
section, the studied system was able to remove 93.86%
of CEX, 54.55% of TOC and 72.46% of COD. As can be
observed, this system can provide a considerable CEX
antibiotic removal efficiency; obtained results are con-
firmed by Rocha et al (2017). Based on their reports,
the cephalexin removal using the advanced oxidation
processes studied was achieved to be 83%.[19]
Conclusion
The optimal conditions for the US/H2O2/NiO hybrid pro-
cess were investigated in the CEX antibiotic removal based
on Taguchi statistical analysis. The results showed that,
using this design method, the determination of the optimal
conditions for the removal of CEX antibiotics is possible.
Accordingly, optimum laboratory conditions for the
hybrid process of US/H2O2/NiO were obtained at the pH
of 3, reaction time of 90 min, initial CEX antibiotic con-
centration of 40 mg/L, H2O2 concentration of 30 mL/L and
NiO nanoparticle of 7.5 mg/L; in this situation, the process
efficiency for CEX removal was 93.98%. Moreover, accord-
ing to the results obtained from the model and the con-
firmatory tests, it can be concluded that this statistical
model can be used as an efficient method, so that it can
reduce the time and cost needed to conduct the tests. Based
on the percentage contribution of each factor, the pH and
reaction time were the factors that had the highest and
lowest effect on the removal of CEX antibiotic using US/H2
O2/NiO hybrid process (94% and 0.4%, respectively).
Moreover, under optimum conditions, the COD and
TOC removal efficiency were achieved to be 72.46% and
54.55%, respectively. It is also observed that Taguchi design
is a proper method in optimizing the parameters. The
obtained results of kinetic studies revealed introduced the
SEPARATION SCIENCE AND TECHNOLOGY 9
COD TOC
pseudo-first order kinetic, with highest values of R2, as
a most suitable model to fit the data of CEX antibiotic
removal compared to pseudo-second-order kinetic.
Acknowledgments
This study was extracted from the research project with No:
9605032770 the Hamadan University of Medical Sciences. So
we acknowledge research and technology deputy of the
University for Financial Aids providing the financial support.
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