Journal of Water Process Engineering 21 (2018) 52–60

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Journal of Water Process Engineering

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Sono-assisted electrocoagulation and cross-flow membrane processes for T

brewery wastewater treatment
⁎
Nadir Dizgea, , Ceyhun Akarsua, Yasin Ozaya, H. Elif Gulsena, Serpil Konen Adiguzelb,
M. Ali Mazmancia
a
Mersin University, Department of Environmental Engineering, 33343 Yenisehir, Mersin, Turkey
b
Mersin University, Department of Biology, 33343 Yenisehir, Mersin, Turkey

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

Keywords: The combinations of treatment processes are one of the hot topics in environmental engineering. Especially, the
Electrocoagulation highly-polluted wastewater can be treated effectively using combined processes. The objective of the present study
Ultrasonication was to investigate the treatment performance of brewery wastewater using electrocoagulation (EC), ultrasonication
Sono-electrocoagulation (US), and sono-electrocoagulation (SEC) processes. A cross-flow membrane system was integrated to succeed con-
Membrane process
tinuous treatment. The effect of electrode combination (Fe and Al), current density (50–100 A/m2), pH (5.0–9.0), and
Brewery wastewater
Genotoxicity
operating time (0–60 min) on the treatment of wastewater were investigated to obtain maximum treatment effi-
ciency. The maximum removal efficiencies of color and chemical oxygen demand (COD) were obtained as 99.2 and
60.5%, respectively, at the electrode combination of Al/Al, current density of 100 A/m2, pH 7.0, and reaction time of
60 min. In order to improve treatment quality, a cross-flow membrane process was integrated to the sono-electro-
coagulation process. Nanofiltration (NF) and reverse osmosis (RO) membranes were tested. The combined sono-
assisted electrocoagulation and membrane system supplied 100% color and 90.8% COD removal efficiency when
supported with RO membrane. The results indicated that the proposed integrated process supplied higher pollutant
removal compared to the alone electrocoagulation and sonication process. Operating cost of the combined process
was calculated as 1.83 $/m3. Moreover, the genotoxic effect of brewery wastewater was also assessed by comet assay
before and after treatment. This process can be used to treat a different kind of wastewater as an efficient technique.

1. Introduction
Wastewater contains various kinds of pollutants such as pharmaceu-
ticals, pesticides, dyes and organic pollutants. Most of these substances
may cause ecological risk to aquatic environment. This ecological risk is
potentially genotoxicity, toxicity, and extinction [1]. Therefore, these
substances must be removed from wastewater before discharge or reuse.
Ecological risk of these pollutants does not only depend on their con-
centrations but also their metabolites and degradation products. Effluents
from wastewater treatment present lower toxicity than the corresponding
influent. Thus, the genotoxicity of water pollutants should be an important
matter of study in the field of wastewater treatment [2]. So, scientists
should increase these studies that contain detecting genotoxic risk of
pollutants in aquatic environment.
Industrial wastewater characteristics can be variable and waste-
water must be treated before being discharged to any receiving en-
vironment [3]. The brewery industry use large quantities of water and
produce huge amounts of wastewater [4]. The typical brewery industry
produces 3–10 L wastewater per liter of beer [5]. It mostly contains
sugars, soluble starch, ethanol, volatile fatty acids, and suspended solids
[6]. Therefore, to make dischargeable of brewery wastewaters has be-
come an important issue to protect environment [7]. So far, conven-
tional treatment methods such as anaerobic packed-bed reactor [8],
anaerobic membrane bioreactor [9], coagulation/flocculation [10],
microalgae [11], microbial fuel cells [12], aerobic granulation [13] and
electrocoagulation [14] have been applied for brewery wastewater
treatment.
Electrocoagulation (EC) is one of the important technology that
combines the advantages of conventional coagulation, flotation, and
adsorption in water and wastewater treatment [15]. Process depends on
dissolution of the anode electrode. Oxidation reactions take place on
anode while reduction reactions occur on cathode [16]. Iron and alu-
minum metals are the most used electrode materials because they are
cheap, effective, and easy to find [17]. Electrocoagulation offers many
advantages over traditional treatment processes, such as easy opera-
tion, simple equipment, low capital-operating costs, and relatively low

⁎
Corresponding author.
E-mail address: nadirdizge@gmail.com (N. Dizge).

https://doi.org/10.1016/j.jwpe.2017.11.016
Received 8 August 2017; Received in revised form 19 November 2017; Accepted 26 November 2017
2214-7144/ © 2017 Elsevier Ltd. All rights reserved.
N. Dizge et al.
amount of sludge generation [18].
Ultrasonication (US) is transmitted to the material by waves that
compress and stretch its molecules. When the negative pressure is large
enough to disrupt the distance between the molecules of the liquid, the
cavitation bubbles are created [19]. The collapse of these bubbles may
generate very high temperatures and pressures and these conditions
will cause the breakdown of the water molecules inside the cavitation
bubbles. These conditions will cause the breakdown of the water mo-
lecules inside the cavitation bubbles. Therefore, the sonolytical clea-
vage of water molecules produces reactive OH%radicals that are non-
selective oxidants for organic pollutants in wastewater [20,21].
The sono-electrochemical (SEC) process consists of ultrasound (US)
and electrochemical (EC) techniques. This process enhances radicals
production from ultrasound, therefore higher reaction rate and pollu-
tant degradation can be achieved [22]. Moreover, ultrasound irritation
affects particle size, solubilization, formation of refractory compounds,
and organic material structure [23].
To set-up continuous treatment process, a cross-flow membrane
system can be integrated with different types of processes. It is well
known that membrane technology has been proved to be an efficient
way to purify wastewater for recycle or reuse [24–29].
The quality of organism’s life is dependent on the environment.
When the large amounts of pollutants are released into the environ-
ment, they may lead to some adverse effects on organisms. Moreover,
the adverse effects may be genotoxic which damages DNA molecule.
Due to presence of genotoxins in the environment, it is important to
evaluate the genotoxic effects on organisms. The aquatic environment
has ecological risk because of genotoxic agents such as chemicals,
pesticides, nanoparticles, factory wastes [30,31]. Several tests are used
to assess genotoxicity in aquatic environment. Micronucleus and comet
assay have been commonly used for the evaluation of DNA damage.
Comet assay shows DNA single and double strand breaks [32,33].
In recent years, integrated processes have been intensively in-
vestigated to increase the efficiency of wastewater treatment [34–37].
The main novelty of this work is to enhance a synergistic effect with
combined sono-electrocoagulation (SEC) process integrated to cross-
flow membrane (CFM) process for further removal of color and COD.
The effects of several operating parameters such as electrode combi-
nation (Fe and Al), current density (50–100 A/m2), pH (5.0–9.0) and
operating time (0–60 min) were tested. The effect of membrane type
(NF and RO) was also investigated. Moreover, the genotoxic effect of
brewery wastewater was assessed by comet assay before and after
brewery wastewater treatment.
Tejedor-Sanz et al. proposed the integration of two electrochemical
techniques as an electrocoagulation (EC) and a microbial electro-
chemical fluidized bed reactor (ME-FBR) to treat brewery effluents. It
was reported that the soluble organic matter was oxidized > 88% of the
COD using a fluidized anode at 25 A/m current density when EC pro-
cess was integrated with ME-FBR [38]. BanI-Melhem and Edward Smith
investigated the performance of an integrated process consisting of an
electro-coagulation (EC) unit and a submerged membrane bioreactor
(SMBR) to treat grey water. It was shown that integrating EC process
with SMBR (EC-SMBR) improved the overall performance of the
membrane filtration process and up to 13% reduction in membrane
fouling was achieved by EC-SMBR process [39].
2. Materials and methods
2.1. Brewery wastewater characterization
The brewery wastewater was supplied from Anadolu Efes beer fac-
tory located in Adana, Turkey. The specific characteristics of the
brewery industry are shown in Table 1. H2SO4 (0.1 N) and NaOH
(0.1 N) were used to adjust the pH value. All chemicals were purchased
from Merck and Sigma-Aldrich Company. The solutions were prepared
with deionized water (Millipore Direct-Q3UV).
53
Journal of Water Process Engineering 21 (2018) 52–60
Table 1
Characteristics of the raw brewery wastewater from beer industry.
Parameter Unit Value
COD mg/L 6840 ± 118
pH – 7.04 ± 0.12
Conductivity μS/cm 1704 ± 16
Total suspended solid mg/L 895 ± 21
Color Pt/Co 1840 ± 55
2.2. Membranes
Nanofiltration (NF270) and reverse osmosis (SW30) membranes
were used for further color and COD removal from brewery wastewater.
NF270 and SW30 membranes were provided from Dow FilmTec.
According to the manufacturers, the NF270 and SW30 membranes have
molecular weight cutoffs of approximately ∼200–400 and ∼100 Da,
respectively. Previous studies have provided information regarding the
characterization on these membranes [40,41]. The membranes were
wetted in deionized water overnight and compacted by deionized water
for 3 h at room temperature.
2.3. Continuous reactor setup
The experimental set up scheme for the combined SEC process in-
tegrated with CFM system is shown in Fig. 1. The combined process
consisted of the electrochemical (EC), ultrasonication (US), and cross-
flow membrane (CFM) units. EC experiments were carried out in a
cylindrical reactor made of glass material (10.5 × 14.5 cm (ra-
dius × height)). Fe/Fe, Al/Al, Fe/Al, and Al/Fe were used as the
anode/cathode electrodes. The effective electrode surface area was
6 cm × 7 cm (width × height) and both electrodes had the same di-
mensions with 1 mm thickness. The new electrodes were used for each
experiment and placed with an inter-electrode distance of 2 cm. The
reactor had 1250 mL total capacity and 800 mL wastewater was filled
into the electrochemical reactor. A direct current (DC) power supply
(AATech ADC-3303D) was used. The pH was adjusted with NaOH and
H2SO4 and measured using a pH meter (Hach-Lange HQ40d). For ul-
trasonication experiments, the ultrasonic water bath (ElmasonicS 100H;
550 W; 50/60 Hz) was filled with deionized water. EC system was put
into the ultrasonic water bath to set-up sono-electrocoagulation pro-
cess. A cross-flow membrane unit was integrated to sono-electro-
coagulation setup. The cross-flow filtration system was made of stain-
less steel which had a working volume of 5 L and filtration area of
150 cm2. A previous study can provide detailed operation of the
membrane system [40]. During the experiments, the samples were
collected at every 30 min and centrifuged with Hettich-Zentrufugen
EBA20 (6.000 rpm, 10 min). However, the permeate collected from
membranes was analyzed directly for color and COD removal.
Electrode combination (Fe/Fe, Al/Al, Fe/Al, Al/Fe), current density
(50–100 A/m2), pH (5.0–9.0), and operating time (0–60 min) were
tested to find maximum pollutant removal. Two kinds of commercially
available membranes (NF270 and SW30) were used in the experiments.
The NF and RO membranes were operated at 20 bar and 40 bar pres-
sure, respectively. The concentrate was recycled to the electro-
coagulation reactor.
2.4. Analyses
2.4.1. COD removal
The dichromatic closed reflux method was used to determine the
chemical oxygen demand (COD) of the samples, strictly following the
APHA guidelines [42]. COD removal efficiency was calculated by Eq.
(1):
N. Dizge et al. Journal of Water Process Engineering 21 (2018) 52–60

Fig. 1. Schematic illustration of the combined treatment system (1. Wastewater storage tank, 2. Peristaltic pump, 3. DC power supply, 4. Electrocoagulation reactor, 5. Electrodes, 6.
Ultrasonic water bath, 7. Pre-treated wastewater storage tank, 8. High pressure pump, 9. Flowmeter, 10. Valve, 11. Manometer, 12. Membrane unit, 13. Membrane permeate, 14 Balance,
15. Computer).

CODi − CODt ⎞ water throughout the membranes in the determined intervals and cal-
CODremoval efficiency = ⎛ ⎜ × 100 ⎟

⎝ CODi ⎠ (1) culated by Eq. (5):

where (CODi) is the inlet COD value (mg/L) and (CODt) is the COD V
J=
value at any reaction time of t (mg/L). A × Δt (5)

where, J is permeate flux (L/m2/h), V is volume of membrane permeate

2.4.2. Color removal
Color was assayed at 455 nm on a Hach spectrophotometer (DR
6000) and calibrated against platinum-cobalt (Pt/Co) method, the unit
of color being that produced by 1 mg platinum/L in the form of the
chloroplatinate ion [42].
2.4.3. Operating cost of the combined process
Operating cost is an important parameter for industrial wastewater
treatment. High charge loading can be option for desirable effluent
water quality although charge loading effects energy consumption.
Power consumption is the most important part of the operating cost and
its formula is given by Eq. (2):
I × V × t
E total = + EUS
VR
3
where Etotal (kWh/m ) is electrical energy consumption, V is potential
(V), I is applied current (A), t is treatment time (h), VR is the net reactor
volume (wastewater volume in the reactor) (m3), and EUS (kWh/m3) is
energy consumption during the ultrasonic process. The energy con-
sumption for sonication process was calculated by considering the
power used by the device.
According to Faradays’ law, the theoretical maximum dissolved
mass of aluminum during SEC process can be determined by Eq. (3).
I × t × MAl
Celectrode =
z×F×ν
where Celectrode is amount of dissolved anode material (g) in theoreti-
cally, I is applied current (A), t is electrolysis time (s), MAl is specific
molecular weight of anode (aluminum) (26.97 g/mol), z is number of
electron involved in the reaction (zAl = 3), and F is the Faraday’s
constant (96,485C/mol).
The power of pumping water can be calculated by Eq. (4).
Q×ρ×g × h
Ph =
3.6 × 106
where Ph is hydraulic power (kW), Q is flow capacity (m /h), ρ is
(L), A is effective area of the membrane (m2), and Δt is filtration time
(h).
2.5. Genotoxicity study
Two volunteers were chosen as a donor and heparinized blood was
obtained by venous puncture. This lymphocytes culture was supplied
from human blood lymphocytes that were centrifuge with histopaque-
1077. This culture media was set up by adding 0.5 mL lymphocyte
suspension in 4.5 mL of RPMI, fetal calf serum, penicillin-streptomycin,
L glutamine, phytohemagglutinin. Comet assay was used to evaluate
genotoxicity. Cells were incubated at 37 °C for 72 h with brewery
wastewater before and after treatment. Sterile water was used as ne-
(2) gative control. Cells were exposed to hydrogen peroxide as positive
control for 3 h. After exposed, comet assay was performed according to
Tice et al. [33]. All procedures were carried out in dark to prevent DNA
damage. These slides were stained with ethidium bromide and analyzed
with a confocal microscope. According to the length of the tail, the DNA
damage in cells was classified by assigning a score of from 0 to IV. Type
0 corresponds to intact cells, Type I corresponds to cells with low level
damage, Type II is medium level damage, Type III is high level damage,
and Type IV is cells with complete damage [43]. A genetic damage
index (GDI) and the extent of DNA damage were estimated for each
subject [44,45].
(3)
3. Results and discussion
Brewery wastewater treatment experiments were systematically
performed to compare the US and EC processes in a batch and con-
tinuous mode. A cross-flow membrane system was integrated to SEC
processes to obtain continuous treatment system. The obtained results
are discussed below in the relevant sections.
(4)
3.1. Comparison of process efficiency
3

density of fluid (kg/m3), g is gravity (9.81 m/s2), and h is differential In this study, the process efficiency of the US, EC, and SEC were
head (m). tested and compared for the removal percentage of color and COD with
a current density (75 A/m2), pH (7.0), electrode combination (Al/Al),
2.4.4. Permeation flux inter-electrode distance (2 cm), reaction time (60 min), and ultrasonic
The permeation flux (J) was measured by collecting the filtered frequency (37 kHz). The color and COD removals were about 7.7, 96.7,

54
N. Dizge et al.
Fig. 2. Comparison of sonication, electrocoagulation, and sono-electrocoagulation pro-
cess on color (A) and COD (B) removal efficiency (Experimental conditions: current
density, 75 A/m2; pH, 7.0; COD concentration, 6840 mg/L; electrode combination, Al/Al;
inter-electrode distance, 2 cm; ultrasound frequency, 37 kHz; and reaction time, 60 min).
98.2% (Fig. 2a) and 2.7, 46.5, 53.7% (Fig. 2b) for the US, EC, and SEC
processes, respectively. It can be concluded from the results that the
individual US process did not supply reasonable removal of color and
COD. The individual EC process supplied high color removal but
moderate COD removal. The main reason of efficiency increasing for
SEC process may be due to regeneration of new electrode surface by
dynamic cavitation and/or micro-streaming effect during the sonication
process [28]. The other reason was probably enhancing bridge between
coagulants and pollutants by increasing the mixing efficiency to support
collisions frequency [28,29]. As a result, COD removal efficiency was
improved by SEC combined process compared with individual US and
EC process.
3.2. Optimization of operating parameters for the SEC process at batch
mode
3.2.1. Effect of electrode combination
The chemical reactions observed in the EC process for aluminum
and iron electrodes are as follow [46,47]:
For aluminum electrodes:
55
Journal of Water Process Engineering 21 (2018) 52–60
Al (s) ↔ Al (+aq3 ) + 3e− (anode )
−
3H2 O + 3e− ↔ 3/2H2(g ) + 3OHaq (cathode )
2Al (s) + 6H2 O ↔ 2Al (OH )3(s) + 3H2(g ) (overall reaction)
For iron electrodes:
4Fe (s) ↔ 4Fe (+aq2) + 8e− (anode )
+2 +
4Feaq + 10H2 O + 2O2(g ) ↔ 4Fe (OH )3(s) + 8Haq (anode )
4H2 O + 2e− ↔ 4OH(−aq) + 2H2(g ) (cathode )
4Fe (s ) + 10H2 O + O2(g ) ↔ 4Fe (OH )3(s ) + 4H2(g ) (overall reaction)
In this study, different Fe and Al electrode arrangements were studied
and the results are presented in Fig. 3. The anode/cathode materials
had an evident impact on the color and COD removal. The color and
COD removals were about 92.4, 93.7, 96.7, 98.2% (Fig. 3a) and 42.0,
46.1, 50.8, 53.7% (Fig. 3b) by the anode/cathode electrode arrange-
ments of Fe/Al, Al/Fe, Fe/Fe, and Al/Al, respectively. The sacrificial
Al/Al electrode combination supplied the highest pollutant removal.
For this reason, all the SEC experiments were conducted using the Al/Al
electrode.
3.2.2. Effect of pH
It is well known that the pH has a remarkable influence on the
performance of EC and SEC process. The effect of pH on the removal
efficiencies of color and COD was investigated with the pH values in the
range of 5.0–9.0 using aluminum electrodes. Constant current density
and electrode distance were 75 A/m2 and 2 cm, respectively. The re-
sults of color and COD removal efficiencies as a function of pH is de-
monstrated in Fig. 4. It can be noticed that pH of the wastewater af-
fected removal efficiencies. The color and COD removal efficiencies
increased from 83.1 to 98.2% (Fig. 4a) and from 29.1 to 53.7%
(Fig. 4b), respectively, when pH increased from 5.0 to 7.0. The highest
color and COD removal efficiencies were obtained in neutral media (pH
7.0) with Al electrodes. However, the color and COD removal effi-
ciencies decreased from 98.2 to 95.4% and from 53.7 to 45.3%, re-
spectively, when pH increased from 7.0 to 9.0. It could be seen that
coagulation decreased at lower and higher pH values. Aluminum ions
produced by EC process can form monomeric and polymeric aluminum
hydroxide complex depending on pH scale [48]. The monomeric and
polymeric aluminum complexes such as Al(OH)3, Al(OH)2+,
Al2(OH)24+, Al6(OH)153+, Al7(OH)174+, Al8(OH)204+ and
5+
Al13(OH)34 are effective coagulants between pH 5.0 and 8.5 [49]. At
higher pH values, both cathode and anode may be chemically attacked
by OH− ions and the solubility of Al(OH)3 will increase to form Al
(OH)4− which is ineffective in wastewater treatment [26,50]. However,
the previous studies showed that the treatment efficiency was higher for
aluminum electrode when pH was below 8.0 [51,52].
3.2.3. Effect of current density
Current density is another important parameter which affects pro-
cess rate, coagulant dosage, bubble properties of flocks in the EC and
SEC process [53]. The color and COD removal efficiencies were in-
creased in the range of 96.7–99.2% (Fig. 5a) and 37.2–60.5% (Fig. 5b)
at current density of 50–100 A/m2 (Fig. 5). The current density was
selected as 100 A/m2. It was reported that the removal efficiency of
organic pollutant increased as the current density increased [54]. Ac-
cording to Faraday’s Law, the amount of dissolved electrode increases
with the increasing current density in the EC process. This provides
increasing of aluminum solubility rate and more Al(OH)3 reacts with
further pollutant amount. In addition, US process might induce the
formation of hydroxyl radicals which increased color and COD removal
[55,56].
N. Dizge et al.
Fig. 3. Effect of electrode combination on color (A) and COD (B) removal efficiency
(Experimental conditions: current density, 75 A/m2; pH, 7.0; COD concentration,
6840 mg/L; inter-electrode distance, 2 cm; ultrasound frequency, 37 kHz; and reaction
time, 60 min).
3.3. Continuous mode treatment studies
The continuous treatment studies were carried out after de-
termining of the optimum conditions in batch studies. Optimum con-
ditions were determined as current density of 100 A/m2, initial pH of
7.0, electrode distance of 2 cm, ultrasound frequency of 37 kHz, and
reaction time of 60 min. The average removal efficiency for color and
COD at these conditions were found as 99.2 and 60.5% for Al–Al
electrode in batch reactor, respectively. The SEC batch process was
integrated to CFM process to obtain continuous treatment. NF and RO
membranes were used in the membrane system. The color and COD
were analyzed by taking samples at 30 min intervals. During the con-
tinuous treatment studies, brewery wastewater was fed to SEC reactor
with a flow rate of 800 mL/h. The permeate flux was calculated at
5 min internals.
3.3.1. Change of color and COD during continuous studies
The change of color and COD removal efficiencies in continuous
operation is shown in Fig. 6. Membrane system was operated 24 h and
color and COD were measured in membrane permeate. It was de-
termined that total color removal efficiency by membranes was 99.7%
for NF270 membrane and 100% for SW30 membrane in continuous
56
Journal of Water Process Engineering 21 (2018) 52–60
Fig. 4. Effect of pH on color (A) and COD (B) removal efficiency (Experimental condi-
tions: current density, 75 A/m2; COD concentration, 6840 mg/L; electrode combination,
Al/Al; inter-electrode distance, 2 cm; ultrasound frequency, 37 kHz; and reaction time,
60 min).
mode (Fig. 6a). It should be remembered that the color removal effi-
ciency was 99.2% in batch mode of SEC process.
The COD concentration of raw wastewater was 6840 mg/L. The
COD concentration of membrane permeate was measured as 2560 mg/L
and 630 mg/L for NF270 and SW30 membranes at the end of the op-
erating time, respectively. Accordingly, it was determined that total
COD removal efficiency by membranes was 62.6% for NF270 mem-
brane and 90.8% for SW30 membrane in continuous mode (Fig. 6b). It
should be remembered that the COD removal efficiency was 60.5% in
batch mode of SEC process. It can be seen that removal efficiency by
nanofiltration appeared to be close to SEC process. The results showed
that the size of dissolved organic molecules was smaller than NF270
membrane pore size (∼200–400 Da). However, SW30 membrane
showed better performance than NF270 in terms of COD removal effi-
ciency. It can be said that the size of most dissolved organic molecules
in brewery wastewater was in the range of 100–400 Da for this study.
Moreover, flux analyses were performed to determine the relationship
between untreated organic molecules during the SEC process and
membrane fouling.
3.3.2. Change of flux during continuous studies
The wastewater pretreated with SEC process was filtered using
N. Dizge et al. Journal of Water Process Engineering 21 (2018) 52–60

Fig. 5. Effect of current density on color (A) and COD (B) removal efficiency Fig. 6. Color (A) and COD (B) removal efficiency in continuous operation (Experimental
(Experimental conditions: pH, 7.0; COD concentration, 6840 mg/L; electrode combina- conditions: current density, 100 A/m2; pH, 7.0; COD concentration, 6840 mg/L; electrode
tion, Al/Al; inter-electrode distance, 2 cm; ultrasound frequency, 37 kHz; and reaction combination, Al/Al; inter-electrode distance, 2 cm; ultrasound frequency, 37 kHz; ΔP,
time, 60 min). 20 bar for NF270; ΔP, 40 bar for SW30).

NF270 and SW30 membranes and permeate flux was calculated. Initial
drop occurred in the permeate flux within first 60 min with NF270
(Fig. 7). The initial flux was 115 L/m2/h and the flux reached a pseudo
steady-state condition after 60 min. Steady-state permeate flux value
was 22 L/m2/h. However, the initial flux was 33 L/m2/h when SW30
membrane was combined to the system. The flux reached a pseudo
steady-state condition within 30 min and steady-state permeate flux
was 13 L/m2/h. The membranes were chemically cleaned with NaOH
(0.1 N) every 6 h. The flux results showed that the NF270 membrane
lost its flux seriously and organic or inorganic fouling blocked more
rapidly than the BW30 membrane. Dissolved aluminum ions or alu-
minum hydroxide incoming from the SEC process might have caused
the inorganic fouling or scaling.

3.4. Genotoxicity of brewery wastewater

In fact, many components (i.e. sugars, soluble starch, ethanol, vo- Fig. 7. Flux changes during continuous operation (Experimental conditions: current
latile fatty acids, and suspended solids) in aquatic environment may be density, 100 A/m2; pH, 7.0; COD concentration, 2700 mg/L; electrode combination, Al/
toxic or genotoxic on livings depending of the concentration and nature Al; interelectrode distance, 2 cm; ultrasound frequency, 37 kHz; ΔP, 20 bar for NF270;
of the components. Ethanol is a major ingredient of alcoholic drinks and ΔP, 40 bar for SW30).

ability of ethanol to damage DNA was exhibited in different studies and

tissues [57]. Additionally, fatty acids can alter leukocytes (neutrophils,

57
N. Dizge et al. Journal of Water Process Engineering 21 (2018) 52–60

eosinophils, basophils, lymphocytes, and monocytes) function and

higher concentrations of certain acids like volatile fatty acids can cause
cell death via apoptosis or necrosis [58]. Moreover, it is possible that
main component or degradation products provoke genetic alterations
concerning fertilization. The DNA of the cells may be damaged due to
genotoxic stress. The damaged DNA migrates at a different rate than
undamaged DNA in the electric field (gel electrophoresis). If the cells
have the DNA strand break, the strand breaks migrate away from the
undamaged DNA-containing nucleoid body. The DNA strand breaks
lead to tail formation. The percentage of DNA in the tail shows mag-
nitude of damaged. Consequently, the DNA strand breaks caused by an
agent can be evaluated and compared with negative control (known as
non-genotoxic) and positive control (known as genotoxic). For this
reason, genotoxic effect of the brewery wastewater was evaluated be-
fore and after treatment process.
Our results showed that brewery wastewater did not exhibit geno-
toxic effect after treatment. If the livings in aquatic environment expose
to pollutants for long time, they may fall with different hazards such as
extinction and genetic alterations for fertilization. Cell incubated with
treated brewery wastewater, did not show an increase in the DNA da-
mage compared to other exposed cells (Table 2). Except for positive
control, the results obtained from all tested concentrations are similar Fig. 8. Comet views in damaged DNA in peripheral blood lymphocytes treated with the
to the results of the negative control (Fig. 8). Consequently, our pro- brewery wastewater.
posed treatment system effectively reduces the water genotoxicity from
the brewery wastewater. Table 3
Consumption of energy and electrode material for optimum conditions.
3.5. Operating cost of the combined process
EC process SEC process SEC-CFM
process
For the optimum operating conditions, consumption of electrode
and energy are given in Table 3. Energy consumption values are esti- Cenergy (kWh/m3) 6.750 7.020 8.120
mated by considering the conditions in Table 4. The energy costs for the Celectrode (kg/m3) 0.063 0.063 0.063
Energy cost ($/m3) 0.945 0.983 1.137
EC and SEC process were 0.945 and 0.983 $/m3, respectively. However,
(1 kWh = 0.14$ according to Turkey
the energy costs for the SEC integrated with CFM process was 1.137 Electricity Distribution Company)
$/m3. The total costs for the EC, SEC, and SEC-CFM combined process Material cost ($/m3) 0.049 0.049 0.049
were as 0.994, 1.032 and 1.830 $/m3, respectively. (1 kg Al = 0.77$) 0.644
It can be clearly seen that high recovery efficiency is achieved even (1 cm2 membrane = 0.0043$)
Total Cost ($/m3) 0.994 1.032 1.830
after 20 min (Fig. 6). It is known that the reaction time will reduce the
operating cost. However, extension of SEC period promoted further
COD removal. For this reason, the relationship between soluble organic results were obtained from this study:
matter and membrane fouling needs to be investigated more deeply and
the optimum retention time should be determined to save energy
consumption in real application.
• The SEC process supplied further color and COD removal from
brewery wastewater as compared to the individual US and EC pro-
cesses.
4. Conclusion • The combined SEC process ensured 99.2% color and 60.5% COD
removal efficiency at pH 7.0, current density of 100 A/m2, electrode
The present study proposes a continuous treatment process in- combination of Al/Al, and reaction time of 60 min.
cluding combined process to treat brewery wastewater. The following

Table 2
Analysis of DNA damage for raw and treated brewery wastewater.

Treatment groups Proportion of damaged nuclei (%)a Damaged Cells (%)b GDIc

Type 0 Type I Type II Type III Type IV

Negative control 80.75 8.25 5.00 2.50 3.50 11.00 ± 5.47 0.39 ± 0.19
Positive control 37.50 21.75 6.75 14.00 20.00 40.75 ± 7.67 1.57 ± 0.16*
Raw brewery wastewater 70.25 10.50 5.00 4.25 10.00 19.25 ± 5.90 0.73 ± 0.18
Treated wastewater 80.00 9.25 3.50 3.50 3.75 10.75 ± 7.13 0.41 ± 0.21

Type 0 :Undamaged.
Type I :Low damage.
Type II :Medium damage.
Type III :High damage.
Type IV :Complete damage.
a
0–IV indicate grades of DNA damage [39].
b
Percentage of damaged cells = Type II + III+ IV [41].
c
Genetic Damage Index (GDI) = (Type I +2 Type II + 3 Type III + 4 Type IV)/(Type 0 + I + II + III + IV) [40].
* P < 0.001.

58
N. Dizge et al. Journal of Water Process Engineering 21 (2018) 52–60

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• Genotoxicity results showed that brewery wastewater did not ex-
hibit genotoxic effect after treatment.
• The proposed combined process can also be used for the treatment
of other wastewater containing COD and color.
Acknowledgment
This research was supported by department of scientific research
projects of Mersin University (Project number: 2015-AP4-1368).
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