Journal of Water Process Engineering 35 (2020) 101201

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Journal of Water Process Engineering

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Evaluating electrocoagulation pretreatment prior to reverse osmosis system T

for simultaneous scaling and colloidal fouling mitigation: Application of
RSM in performance and cost optimization
Paria Sefatjooa, Mohammad Reza Alavi Moghaddama,*, Abdollah Rashidi Mehrabadib
a
Civil and Environmental Engineering Department, Amirkabir University of Technology (Tehran Polytechnic), Hafez Ave., Tehran, 15875-4413, Iran
b
Civil, Water, and Environmental Engineering Department, Shahid Beheshti University (SBU), Tehran, 16765-1719, Iran

ARTICLE INFO ABSTRACT

Keywords: In the present research, electrocoagulation (EC) process was applied as a selected pretreatment to evaluate its
Electrocoagulation effectiveness and operating cost regarding simultaneous calcium and turbidity removal in order to mitigate the
Reverse osmosis scaling and colloidal fouling potential of reverse osmosis (RO) technology. The effects of the main parameters,
Calcium and turbidity removal namely, initial calcium concentration, initial turbidity, time, and current density, on EC process were assessed
Response surface methodology
and optimized by employing response surface methodology (RSM). A reasonable correlation between the ex-
Optimization
perimental and predicted data was found through analysis of variance (ANOVA). The highest calcium and
turbidity removal efficiencies of 36 % and 93.5 %, respectively, and the minimal operating cost of 1.58 US$/m3
were obtained at the optimum time of 35.5 min and current density of 3.85 mA/cm2 with the selected constant
initial calcium concentration of 250 mg/L and initial turbidity of 85 NTU. In the present study, the applicability
of two pretreatments, including hybrid EC-filtration and filtration-only to RO membrane fouling was also
compared. The RO recovery of the hybrid EC-filtration pretreatment improved about 25 % in comparison to that
of the filtration-only pretreatment, which demonstrated the effective capability of the EC process in scaling and
colloidal fouling mitigation.

1. Introduction should be considered. The conventional approaches for reduction of

Reverse osmosis (RO) as a cost-effective membrane process in
comparison to other desalination technologies has faced with the re-
strictive problem of fouling [1–4]. Membrane fouling causes a decline
in permeate flux and an increase in feed pressure. Consequently, it re-
sults in higher operating and maintenance costs due to greater energy
consumption and membrane cleaning/replacement [2,5–7]. Fouling,
which results from the accumulation of inorganic or organic materials
on the surface or in the pores of a membrane, could be categorized into
scaling as well as organic, colloidal, and biological fouling [4,8,9].
The presence of calcium ions in feed water can increase the po-
tential of membrane scaling due to the precipitation of low solubility
salts, especially CaCO3 and CaSO4.2H2O [10]. Colloidal and suspended
matters might also form a cake layer on the membrane surface, which
increases the hydraulic resistance of the membrane [11]. Turbidity
must be less than 1 NTU in RO feed water for prevention of colloidal
fouling [3,8].
To enhance the quality of RO feed water, appropriate pretreatments
scaling and colloidal fouling involve injecting antiscalants, adding acid
(control of calcium carbonate precipitation), softening with ion ex-
change, chemical precipitation (lime and soda ash), and coagulation/
flocculation followed by sedimentation and filtration [9,12–16]. In-
creased risk of RO membrane biofouling (due to phosphate-based an-
tiscalants consumption) [3,13], utilization of high amounts of acids/
salts, generation of brine solutions, and the requirement for disposal of
a large volume of sludge are the demerits of the mentioned treatment
technologies [12,16,17].
Electrocoagulation (EC) as a promising pretreatment has been
proven to be effective in the removal of various types of pollutants to
reduce RO membrane fouling [2,10,13]. Researchers have focused on
EC process due to the absence of chemicals, less sludge production,
versatility, simplicity of operation, compact size, and low investment
and operating costs [10,18–20]. Several studies have investigated the
capability of EC to remove hardness [13,21–24] and turbidity [25–27]
separately. However, on the basis of our literature review, only Zhao
et al. [10] explored EC performance in simultaneous hardness,

⁎
Corresponding author.
E-mail addresses: Psefatjoo@yahoo.com (P. Sefatjoo), alavi@aut.ac.ir (M.R. Alavi Moghaddam), A_Rashidi@sbu.ac.ir (A.R. Mehrabadi).

https://doi.org/10.1016/j.jwpe.2020.101201
Received 20 July 2019; Received in revised form 18 February 2020; Accepted 19 February 2020
2214-7144/ © 2020 Elsevier Ltd. All rights reserved.
P. Sefatjoo, et al. Journal of Water Process Engineering 35 (2020) 101201

turbidity, and COD removal from a specific produced water to enhance was measured using the EDTA titration method [28]. Turbidity mea-
the RO feed water. surement was carried out by a turbidity meter (Hach model 2100 N).
The performance of EC and its operating cost in the treatment of The electrical conductivity value was determined using a conductivity
various solutions containing both hardness and turbidity have not been meter (WTW model 340). The percentage removal of calcium and
investigated so far. Furthermore, in most of the conducted studies, the turbidity was calculated according to Eq. (1)
impact of EC pretreatment on RO fouling was evaluated by comparing
EC pretreated water and the raw water. To the best of our knowledge, Y0 Y
Removal efficiency (%) = × 100
the effects of the hybrid EC-filtration and filtration-only pretreatments Y0 (1)
on RO performance have not been compared. Therefore, the principal where Yo and Y are the initial and final calcium concentration (mg/
aim of this work is to assess the efficiency and operating cost of the EC L)/turbidity (NTU), respectively. Based on the literature review, the
process (as an alternative pretreatment of RO) in simultaneous treat- operating cost of EC is mainly affected by electrical energy and elec-
ment of calcium and turbidity, which are influential components on trode consumption in the form of the following equation [29–31].
scaling and colloidal fouling, respectively, in different waters. To
achieve this goal, response surface methodology (RSM) was utilized to CT = aCenergy+ bCelectrodes (2)
investigate the impact of the main parameters (initial calcium con- 3
where CT is the operating cost of the EC process in US$/m . Cenergy
centration, initial turbidity, time, and current density) on the EC pro-
and Celectrodes are the energy consumed in kWh/m3 and electrode con-
cess as well as to optimize the three responses, namely, calcium and
sumed in kg Al/m3, respectively. The coefficients of a and b are the unit
turbidity removal efficiencies along with operating cost. Moreover, the
prices equivalent to 0.024 US$/kWh and 2.78 US$/kg, respectively, in
effects of the two pretreatments, hybrid EC-filtration and filtration-
Iran in 2017. The electrical energy consumption is expressed as Eq. (3)
only, on RO membrane fouling were investigated.
[32,33].
2. Materials and methods t
E= VIdt
(3)
2.1. Synthetic water samples 0

3
where E = electrical energy consumption (kWh/m ), V = voltage (V), I
In this study, synthetic water samples were prepared to simulate = current intensity (A), and t = electrolysis time (h).
brackish water containing various calcium and turbidity concentra-
tions. To provide turbidity contaminated water, approximately 5 g of
2.4. Experimental design and model development
kaolin powder passed through No.200 sieve was dissolved in 1 L of tap
water. The kaolin suspension was allowed to settle for 50 min to obtain
Central composite design (CCD) as the most-used design method for
a stable dispersion of the particles. This stock kaolin was diluted to
the generation of second-order response surface model [34] was uti-
prepare water with initial turbidity within the range of 20–150 NTU.
lized to determine the significant parameters, the relationships between
The initial calcium concentration of the prepared turbid water was
the parameters and the responses as well as the optimum operating
adjusted to the range of 100−400 mg/L by adding the required amount
conditions. The parameters were studied at five levels (-2, -1, 0, +1,
of CaCl2. The electrical conductivity of the solution was also increased
+2) equivalent to 100−400 mg/L, 20–150 NTU, 10−60 min, and
using 0.017 M NaCl.
2.2–8.8 mA/cm2 for initial calcium concentration, initial turbidity,
time, and current density, respectively (presented in Table 1). The
2.2. Experimental apparatus and procedure
range of these parameters was determined according to preliminary
experiments and literature review [10,25].
EC experiments were accomplished in a batch cell with a working
Thirty experiments, including 6 center points were designed ac-
volume of 1 L. EC cell was equipped with 10 aluminum plate electrodes
cording to Eq. (4):
(with an effective area of 451 cm2) connected to a DC power supply
(PW4053R model Micro) in galvanostatic mode. The electrodes were N = 2K + 2 K + C 0 (4)
fitted at a space of 1 cm in a monopolar parallel configuration. The EC
where N is the total number of experiments; K is the number of para-
supernatant was used for calcium and turbidity concentration mea-
meters; and C0 is the center point number. The second order polynomial
surements after 30 min of settlement of the suspended matters. The
model of CCD responses is explained based on Eq. (5):
weight loss of the electrodes was measured for operating cost estima-
tion in all the experiments. k k k k
2
The effect of the hybrid EC-filtration pretreatment on RO membrane Y= 0 + i Xi + ii X i + ij Xi Xj +
fouling was compared with that of the filtration-only pretreatment by i= 1 i= 1 i= 1 j= i+1 (5)
analyzing the flux decline trends. For this purpose, approximately 1 L of where Y = responses; 0 , i , ii , and βij = constant coefficients; and Xi ,
each sample (synthetic raw water and the EC pretreated water at op- and Xj = coded variables. Analysis of variance (ANOVA), determina-
timum operating conditions) was filtered using a polypropylene car- tion coefficients, and residual plots were utilized to evaluate the effects
tridge filter of 5 μm. For RO experiments, the commercial flat-sheet of the important parameters, significance and quality of the generated
membrane (TW30-1812-50, DOW) with an active area of 80 cm2 was models [35].
loaded into a cross-flow plate and frame module. The tests were per-
formed in batch mode at the constant operating pressure of 7 bar and Table 1
the initial permeate flux of 22 L/m2h. Before each run, the RO mem- Factors and coded levels selected for EC study.
brane was rinsed with deionized water. The data associated with the
Independent factors Variables Coded levels
collected permeate water was recorded as a function of filtration time
using a digital balance for flux calculation. −2 −1 0 +1 +2

2.3. Analytical methods and cost estimation Initial calcium concentration (mg/L) X1 100 175 250 325 400
Initial turbidity (NTU) X2 20 52.5 85 117.5 150
Time (min) X4 10 22.5 35 47.5 60
Evaluation of EC performance was accomplished by the calculation Current density (mA/cm2) X5 2.2 3.85 5.5 7.15 8.8
of calcium and turbidity removal efficiencies. Calcium concentration

2
P. Sefatjoo, et al. Journal of Water Process Engineering 35 (2020) 101201

Table 2
CCD experimental design in coded values for responses.
Run Initial calcium concentration Initial turbidity Time (X3) Current density Calcium removal Turbidity removal Operating cost (US
(X1) (X2) (X4) efficiency (%) efficiency (%) $/m3)

1 0 0 0 0 41.6 91.5 2.1

2 0 −2 0 0 36 67.5 1.55
3 −1 −1 −1 −1 36 85.7 0.87
4 +1 +1 −1 +1 34.8 89.2 1.82
5 0 0 0 0 42 91.2 1.77
6 +1 +1 +1 +1 40 89.8 3.16
7 0 0 −2 0 18 85.2 1.25
8 0 +2 0 0 35.6 87.5 2.18
9 −1 +1 +1 −1 38.3 96.9 2.44
10 −1 +1 +1 +1 50.8 86.8 3
11 0 0 0 0 36 89 2.3
12 0 0 0 −2 28 90.2 0.69
13 +1 −1 +1 +1 34.5 63.8 3.02
14 −1 +1 −1 +1 42.3 93.4 2.17
15 +1 +1 +1 −1 31.4 88.6 2.27
16 +2 0 0 0 28.2 80.7 1.81
17 0 0 0 0 37.6 89.2 1.86
18 +1 −1 −1 −1 23.1 77.7 0.87
19 0 0 0 +2 44 83.2 2.84
20 −1 −1 −1 +1 43.4 83.6 1.8
21 −2 0 0 0 60 91.8 1.93
22 −1 +1 −1 −1 31.4 93 0.98
23 +1 −1 −1 +1 29.3 72.2 1.57
24 0 0 0 0 39.2 90.3 2.16
25 0 0 0 0 38.4 85.2 2.32
26 +1 +1 −1 −1 26.1 95.3 0.59
27 +1 −1 +1 −1 36 93.4 1.69
28 −1 −1 +1 +1 63.4 76.6 3.04
29 −1 −1 +1 −1 46.5 89.9 2.08
30 0 0 +2 0 42.8 85.9 3.34

3. Results and discussion
3.1. Fitting the models and data analysis of the EC process
According to the 30 conducted experiments, the CCD matrix of
calcium and turbidity removal efficiencies along with operating cost is
demonstrated in Table 2. The fitted models for calcium removal effi-
ciency, turbidity removal efficiency, and operating cost in coded values
were obtained as Eqs. (6) to (8), respectively:
Y1 = 39.13 – 6.69 X1 – 0.75 X2 + 5.17 X3 + 4.24 X 4
+ 2.24 X1X2 – 1.08X1X3– 1.61 X1X 4 –1.42 X2X3 + 0.73 X2 X 4
+ 0.21 X3X 4 + 1.47 X12 –0.60 X22 – 1.95 X32 – 0.55 X24
Y2 = 90.24 – 3.69 X1 + 5.31 X2 – 0.66 X3 – 2.68 X 4 + 1.18 X1X2 – 0.39 X1X3
+ 1.43 X2X 4 –2.57 X3X 4 –0.98 X12 – 3.17 X22 – 1.16 X32 – 0.87 X24
Y3 = 2.09 – 0.068 X1 + 0.11 X2 + 0.62 X3 + 0.50 X 4 + 0.034 X1X3
+ 0.032 X1X 4 + 0.037 X2X3 –0.019 X3X 4 – 0.045 X12 – 0.046 X22
+ 0.022 X23 – 0.071 X24 (8)
The ANOVA reports shown in Table 3 confirmed the significance of
the presented models (p ≤ 0.0001). The results also indicated that
initial calcium concentration, time, and current density were significant
at 95 % confidence level (p-values < 0.05) for calcium removal effi-
ciency. Furthermore, the most influential parameters for turbidity re-
moval efficiency were found to be initial calcium concentration, initial
turbidity, and current density. Operating cost was also affected by in-
itial turbidity, time, and current density (data not presented).
(6) Based on Table 3, the lack of fit for calcium removal efficiency (p-
value of 0.2578), turbidity removal efficiency (p-value of 0.1266), and
operating cost (p-value of 0.7670) were not significant, which indicated
that the models were fitted appropriately to the experimental data.
(7) High values of R2 (close to 1) demonstrate a satisfactory agreement

Table 3
ANOVA output for calcium removal efficiency, turbidity removal efficiency, and operating cost.
Source Sum of squares df Mean square F value p-value Prob > F

Calcium removal efficiency

Model 2545.57 14 181.83 21.48 < 0.0001
Lack of fit 99.95 10 9.99 1.85 0.2578
R2 = 95.25%, Adjusted R2 = 90.82%, Predicted R2 = 77%, C.V. = 7.69%, Adequate precision = 19.047
Turbidity removal efficiency
Model 1575.91 12 131.33 38.67 < 0.0001
Lack of fit 39.02 9 4.34 3.38 0.1266
2 2 2
R = 97.27%, AdjustedR = 94.76%, Predicted R = 85.27%, C.V. = 2.16%, Adequate precision = 22.474
Operating cost
Model 14.89 12 1.24 32.81 < 0.0001
Lack of fit 0.35 11 0.032 0.62 0.7670
R2 = 96.09%, Adjusted R2 = 93.17%, Predicted R2 = 88.29%, C.V. = 9.69%, Adequate precision = 21.642

3
P. Sefatjoo, et al.
Fig. 1. Normal probability plots of residuals for (a) calcium removal efficiency; (b) turbidity removal efficiency; (c) operating cost.
between the obtained and predicted results [36]. Also, a coefficient of
variance (C.V.) ≤10 % and an adequate precision ≥4 indicate a rea-
sonable fit of the results to the model [37,38]. In this research, high R2
coefficient values were obtained 95.25 %, 97.27 %, and 96.09 % for
calcium removal efficiency, turbidity removal efficiency, and operating
cost, respectively. In addition, the predicted R2 and adjusted R2 values,
differing with less than 0.2, were in reasonable agreement. The C.V. and
adequate precision were calculated as 7.69 % and 19.047, 2.16 % and
22.474 as well as 9.69 % and 21.642 for calcium removal efficiency,
turbidity removal efficiency, and operating cost, respectively. Normal
probability plots of residuals for all three responses follow a straight
line (displayed in Fig. 1(a–c)). All these obtained reports indicate the
adequacy of the models as well as a desirable relationship between the
experimental and predicted results.
3.2. Effects of the operating parameters on the EC process
3.2.1. Initial calcium concentration/turbidity
Initial calcium concentration had a significant influence on calcium
and turbidity removal efficiencies. As shown in Fig. 2(a), by increasing
the initial calcium concentration at various times, the calcium removal
efficiency decreased. For example, a noticeable decrease of about 28 %
was obtained for calcium removal efficiency at the time of 35 min (the
average of the considered time range) when the initial calcium con-
centration increased from 175 mg/L to 325 mg/L. Initial calcium con-
centration also had a negative effect on turbidity removal efficiency
(Fig. 3(a)). According to Fig. 3(a), turbidity removal percentage de-
clined from about 86 % to 76 % and 94 % to 89 % at the constant initial
turbidity values of 52.5 NTU and 117.5 NTU, respectively, by changing
the initial calcium concentration from 175 mg/L to 325 mg/L. The
decrease in removal rates of calcium and turbidity could be due to the
insufficiency of complexion sites compared with aqueous calcium.
The effect of initial turbidity on calcium and turbidity removal ef-
ficiencies as well as operating cost is shown in Figs. 2(b), 3 (a) and (b),
as well as 4(a), respectively. Fig. 2(b) reveals that an increase of initial
4
Journal of Water Process Engineering 35 (2020) 101201
turbidity resulted in a gradual decrease of calcium removal rate. Max-
imum decrease of about 8% was attained at the constant current density
of 3.85 mA/cm2, when the initial turbidity increased from 52.5 NTU to
117.5 NTU. A higher turbidity removal efficiency was obtained with
higher initial turbidity (Fig. 3(a) and (b)). Fig. 3(a) shows that at
constant initial calcium concentrations of 175 mg/L and 325 mg/L, by
increasing the initial turbidity from 52.5 NTU to 117.5 NTU, turbidity
removal efficiency improved approximately 10 % and 17 %, respec-
tively. This result is probably due to the higher amount of aluminum
hydroxides as coagulants. Thus, the additional coagulants may produce
turbidity and consequently cause a slight drop in turbidity removal rate
at lower initial turbidity. Merzouk et al. [26] investigated the effect of
initial turbidity concentration ranged from 100−800 mg/L as silica gel
on turbidity removal rate. It was found that low initial turbidity con-
centrations (100−300 mg/L as silica gel) had no significant effect on
removal efficiency, while a significant reduction in removal rate oc-
curred for higher concentrations. A gradual increase in operating cost
from about 1.9 US$/m3 to 2.1 US$/m3 at the time of 35 min also oc-
curred by increasing initial turbidity (Fig. 4(a)).
3.2.2. Time/current density
The effect of time on calcium removal efficiency, turbidity removal
efficiency, and operating cost is seen in Figs. 2(a) and (c), 3 (c) as well
as 4 (a) and (b). According to Fig. 2(a) and (c), increasing the time from
22.5 min to 47.5 min had a positive impact on calcium removal effi-
ciency. Calcium removal efficiency steadily improved from approxi-
mately 39%–52% and 28%–36%, when the values of initial calcium
concentration were 175 mg/L and 325 mg/L, respectively (Fig. 2(a)).
Extending the treatment time could enhance the calcium removal effi-
ciency due to greater generation of metal hydroxide flocs, according to
Faradays law (Eq. (9)). The influence of time on turbidity removal ef-
ficiency follows an unsteady approach involving slight changes
(Fig. 3(c)). As shown in Fig. 3(c), at lower current density (3.85 mA/
cm2), turbidity removal efficiency showed a minimal improvement of
about 4% with the increase of time from 22.5 min to 47.5 min;
P. Sefatjoo, et al.
Fig. 2. 3D surface plots for calcium removal efficiency in terms of (a) initial calcium concentration and time (initial turbidity = 85 NTU, current density =5.5 mA/
cm2); (b) initial turbidity and current density (initial calcium concentration = 250 mg/L, time =35 min); (c) time and current density (initial calcium concentration
= 250 mg/L, initial turbidity = 85 NTU).
conversely, it experienced a reducing trend of nearly 7% at higher
current density (7.15 mA/cm2). Bukhari [27] also demonstrated that
increasing time up to 20 min resulted in higher turbidity removal ef-
ficiency. However, the decrease of removal rate was obtained at a
higher time.
The increasing rate of operating cost due to increasing time is illu-
strated in Fig. 4(a) and (b). As time increased with the average constant
current density of 5.5 mA/cm2, operating cost raised dramatically from
about 1.5 US$/m3 to 2.7 US$/m3 (Fig. 4(b)). Increasing time could
induce an increase in operating cost associated with electrical energy
and electrode consumption based on Eqs. (3) and (9), respectively.
ItM
X=
zF
where X: the coagulants generated by anodic dissolution (g), I: current
(A), t: treatment time (s), M: atomic mass (MAl = 26.98 g/mol), z:
electron number (zAl = 3, and F: Faradays constant 96,485 C/mol
[30,33,39].
Current density had a considerable effect on all the responses (cal-
cium removal efficiency, turbidity removal efficiency, and operating
cost). Greater removal of calcium occurred with higher current density
Journal of Water Process Engineering 35 (2020) 101201
(shown in Fig. 2(b) and (c)). For instance, according to Fig. 2(c), the
maximum calcium removal efficiency of 46 % was obtained at the
current density of 7.15 mA/cm2. Several research groups stated that the
significant improvement in pollutant removal efficiency at higher cur-
rent density was due to the increase in the production rate of coagulants
(Faradays law) and hydrogen bubble as well as the decrease in bubble
size [18,26,30,31].
Current density had a reverse influence on the turbidity removal
rate (Fig. 3(b) and (c)). As seen in Fig. 3(b), by increasing the current
density from 3.85 mA/cm2 to 7.15 mA/cm2, slight reductions of about
3% and 9% were obtained for turbidity removal efficiency with the
initial turbidity of 117.5 NTU and 52.5 NTU, respectively. These de-
clining removal rates are likely related to the excess production of
(9)
aluminum hydroxides, which subsequently increases the turbidity of
the aqueous solution. Similar results were reported by Merzouk et al.
[26], which demonstrated that increasing current density (from 11.55
mA/cm2 to 91.5 mA/cm2) led to a decrease in turbidity removal effi-
ciency. Conversely, a study evaluated the effectiveness of EC process in
turbidity removal and showed the positive effect of increasing current
density (from 16.3 mA/cm2 to 57.5 mA/cm2) on turbidity removal rate
[40]. In another research, an enhancement trend of turbidity removal
5
P. Sefatjoo, et al.
Fig. 3. 3D surface plots for turbidity removal efficiency in terms of (a) initial calcium concentration and initial turbidity (time =35 min, current density =5.5 mA/
cm2); (b) initial turbidity and current density (initial calcium concentration = 250 mg/L, time =35 min); (c) time and current density (initial calcium concentration
= 250 mg/L, initial turbidity = 85 NTU).
efficiency was achieved by increasing current density up to 5.56 mA/
cm2 followed by a declining rate with further increase in current den-
sity [10]. Also, Aoudj et al. [41] revealed that turbidity removal effi-
ciency was not significantly influenced by current.
The influence of current density on operating cost is shown in
Fig. 4(b). As an example, with the assumption of the constant time of 35
min, an increase in current density from 3.85 mA/cm2 to 7.15 mA/cm2
caused an enormous rise of approximately 66 % in operating cost (from
1.5 US$/m3 to 2.5 US$/m3). In many studies, the similar pattern of
operating cost as a function of current density was exhibited regarding
the removal of different pollutants, such as nitrate [18], algae [31], and
fluoride [33].
3.3. Performance of EC on RO fouling under optimum conditions
The ultimate objective of this study is the evaluation of the EC
performance on RO fouling at optimum conditions. For this purpose,
the effects of 4 main parameters including initial calcium concentra-
tion, initial turbidity, time, and current density on three responses
(calcium removal efficiency, turbidity removal efficiency, and
6
Journal of Water Process Engineering 35 (2020) 101201
operating costs) were optimized through CCD. The optimum conditions
were determined with the aim of achieving maximum calcium removal
efficiency, maximum turbidity removal efficiency and minimum oper-
ating cost. In addition, calcium concentration and turbidity were con-
sidered the constant values of 250 mg/L and 85 NTU (the average of the
selected range), respectively. According to these conditions, calcium
and turbidity removal efficiencies as well as operating cost were
achieved 36 %, 93.5 %, and 1.58 US$/m3, respectively at the optimum
conditions predicted by CCD (time: 35.5 min and current density: 3.85
mA/cm2). The experimental and predicted responses were in good
agreement, confirming the validity of the models.
To investigate whether EC pretreatment could efficiently reduce
membrane fouling, RO experiments were performed to compare the
synthetic raw water containing the calcium concentration of 250 mg/L
and turbidity of 85 NTU with hybrid EC-filtration and filtration-only
pretreatments under the optimum conditions. As shown in Table 4, the
residual calcium and turbidity of the EC pretreated water were 160 mg/
L and 5.5 NTU, corresponding to 36 % and 93.5 % removal efficiency,
respectively. The residual turbidity of the EC pretreated water after
filtration reduced to 0.2 NTU. However, the residual turbidity of the RO
P. Sefatjoo, et al. Journal of Water Process Engineering 35 (2020) 101201

Fig. 4. 3D surface plots for operating cost in terms of (a) initial turbidity and time (initial calcium concentration = 250 mg/L, current density =5.5 mA/cm2); (b)
time and current density (initial calcium concentration = 250 mg/L, initial turbidity = 85 NTU).

feed water with filtration-only pretreatment was 5 NTU. These results

indicate that filtration and EC pretreatments are alone inefficient to
achieve the desirable residual turbidity (less than 1 NTU).
In order to evaluate the effects of the two pretreatments (hybrid EC-
filtration and filtration-only) on RO fouling, the normalized flux is
presented as a function of filtration time (Fig. 5). As seen in Fig. 5, both
pretreatments experienced an initial rapid drop around 40 min and a
milder reduction rate up to 180 min. This initial decrease is related to
the pore plugging of the membrane probably caused by the formation of
calcium carbonate precipitation. The normalized flux decline for the
hybrid EC-filtration pretreatment was lesser than that of the filtration-
only pretreatment. After a duration of 180 min, the normalized flux
reached 0.71 and 0.57 for the hybrid EC-filtration and filtration-only
pretreatments, respectively, equivalent to an improvement of 25 % in
RO recovery.
Fig. 5. RO flux trends for hybrid EC-filtration and filtration-only pretreatments.
4. Conclusions
calcium removal efficiency increased by the decrease of initial calcium
In the present study, EC was applied as a pretreatment of RO system
concentration and initial turbidity as well as increase of time and cur-
for simultaneous calcium and turbidity removal to reduce membrane
rent density. The percentage removal of turbidity was enhanced as in-
scaling and fouling. The effective parameters, including initial calcium
itial turbidity increased, whereas initial calcium concentration and
concentration, initial turbidity, time, and current density on EC per-
current density had a negative influence on the removal rate. In addi-
formance and its operating cost were investigated using RSM. Based on
tion, time had a positive effect on turbidity removal efficiency at lower
the ANOVA reports, high values of R2 were achieved 95.25 %, 97.27 %,
current density and a negative influence at higher current density. The
and 96.09 % for calcium removal efficiency, turbidity removal effi-
EC operating cost dramatically increased by the increase of initial tur-
ciency, and operating cost, respectively. In addition, the values of C.V.
bidity, time, and current density. The maximum calcium and turbidity
and adequate precision were obtained ≤10 % and ≥4, respectively.
removal efficiencies and minimum operating cost were 36 %, 93.5 %,
These results indicate that the experimental data was satisfactorily
and 1.58 US$/m3, respectively, at the optimum time of 35.5 min and
fitted to the empirical model. The 3D surface plots demonstrated that

Table 4
Efficiency of the RO pretreatments on calcium and turbidity removal.
Pollutant RO pretreatments

Filtration-only Hybrid EC-filtration

Residual (mg/L/NTU) Removal efficiency (%) EC Filtration

Residual (mg/L/NTU) Removal efficiency (%) Residual (mg/L/NTU) Removal efficiency (%)

Calcium 250 0 160 36 160 36

Turbidity 5 94.1 5.5 93.5 0.2 99.7

7
P. Sefatjoo, et al.
the current density of 3.85 mA/cm2 considering the constant initial
calcium concentration of 250 mg/L and the initial turbidity of 85 NTU.
The effects of the two pretreatments (hybrid EC-filtration and filtration-
only) on RO fouling were examined by analyzing the normalized flux as
a function of filtration time. The RO recovery associated with the hy-
brid EC-filtration was enhanced 25 % compared with that of the fil-
tration-only pretreatment, which indicated that EC could efficiently
reduce scaling and fouling.
Declaration of Competing Interest
There are no conflicts of interest to declare.
Acknowledgments
The authors acknowledge Amirkabir University of Technology for
financial support. Moreover, authors appreciate the insightful sugges-
tions from Mr. Nematollah Bakhshi (Staff of Amirkabir University of
Technology Environmental Engineering Laboratory), Mr. Mehdi
Hashemi Shahraki (PhD candidate of Shahid Beheshti University), Ms.
Elnaz Karamati-Niaragh (Former M.Sc student of Amirkabir University
of Technology), and Mr. Hossein Shams (PhD candidate of Amirkabir
University of Technology).
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