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South African Journal of Chemical Engineering 46 (2023) 205–216

Contents lists available at ScienceDirect

South African Journal of Chemical Engineering


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

New design of an electrocoagulation reactor to remove pollutants from


groundwater: Analysis and optimization using response
surface methodology
Forat Yasir AlJaberi *
Chemical Engineering Department, College of Engineering, Al-Muthanna University, Al-Muthanna, Iraq

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

Keywords: Batch electrocoagulation experiments were done using a new design of monopolar-parallel electrodes. The
Groundwater process was conducted to make groundwater suitable for municipal use by removing TDS, TSS, Ca+2, Mg+2, SO–2 4 ,
Finned anode and NO–13 ions. These electrodes were ↱designed as a finned anode made of aluminum and placed concentrically
Tubular cathode
through in ↱a ↱tubular cathode. The new design of the anode has provided a significantly higher ↱active area
TDS
TSS
compared to its wet volume. Response surface methodology (RSM) type central composite design (CCD) was used
RSM for design experiments, analysis, and optimization. The treatment process was studied at room temperature by
OPD examining reaction time (4–30 min), applied current (0.2–2.4 Amp.), and mixing speed (50–250 rpm). As
Optimization observed, all pollutants’ removal was directly proportional to the operating parameters attaining considerable
Thermodynamic study eliminating efficacious for initial concentrations of TDS, TSS, Ca+2, Mg+2, SO–24 , and NO3 ions of 1514, 57.73,
–1

Cost estimation 1744.44, 1308, 180, and 32.6 mg/l, respectively. The optimal values of reaction time of 13 min, 2.3 Amp of
applied current, and 50 rpm of mixing speed provided 81.16% of TDS removal and 85.26% of TSS removal with
low consumption of electrical energy and electrodes (2.4 kWh/m3 and 0.25 g). Moreover, the parameter of the
ohmic potential drop (OPD) was investigated. The obtained results revealed that the present design was less
affected by this essential parameter. As well, the behavior of solution temperature throughout the EC reactor was
studied. The thermodynamic study proves that the present electrocoagulation process was endothermic, spon­
taneous in nature, and randomness of the solution interface. In summary, the core results proved that the new
configuration of electrodes employed in the electrocoagulation reactor was cost-effective, reliable and envi­
ronmentally applicable for the treatment of real groundwater compared to the conventional design of EC
electrodes.

1. Introduction 2021; Changmai et al., 2019; Mojid et al., 2019). These wastewaters
contain significant amounts of the biological oxygen demand (BOD),
Several sources of fresh water are under severe stress due to the carbon oxygen demand (COD), and total organic carbon (TOC), and
continuous growth of the population and the huge requirement for in­ inorganic contaminants such as the hardness, total dissolved solids
dustrial activities all around the world (Shrestha et al., 2017; Benekos (TDS), and total suspended solids ↱↱(TSS), and heavy metals (Ribeiro
et al., 2019). One of the major sources of fresh water is groundwater et al., 2019; AlJaberi, 2020; Omwene et al., 2018; Hansen et al., 2019).
which is found in many areas of the world and differs in its amount from Since groundwater is vulnerable to pollution from different activ­
part to part depending on the geographical nature (Devlin et al., 2019; ities, it ↱should be treated, thereby, using high-performance technolo­
Goren et al., 2020; Si et al., 2018). gies to afford acceptable ↱treated water according to legal requirements
Groundwater is polluted by different sources, such as the raised (Schaep et al., 1998; Prasanth et al., 2012), like biological methods
usage of chemical materials such as agricultural fertilizers and pesti­ (Arellano et al., 2020), precipitations (Nariyan et al., 2018), photo­
cides, as well as uncontrolled discharging of wastewaters from industrial catalysis (Thor et al., 2020), reverse osmosis (Cerva et al., 2019),
activities into rivers and soil and illegal dumping sites (Acharya et al., ion-exchange (Martins et al., 2020), and electrochemical methods such

* Corresponding author.
E-mail address: furatyasir@mu.edu.iq.

https://doi.org/10.1016/j.sajce.2023.08.008
Received 16 October 2022; Received in revised form 31 July 2023; Accepted 14 August 2023
Available online 16 August 2023
1026-9185/© 2023 The Author. Published by Elsevier B.V. on behalf of Institution of Chemical Engineers. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/by/4.0/).
F.Y. AlJaberi South African Journal of Chemical Engineering 46 (2023) 205–216

Table 1 interaction influence of the operating variables on the contaminants’


Main properties of collected real groundwater. removal efficiencies is studied using the ANOVA test to validate the
Parameters Values obtained models (Sahu et al., 2010, 2009; Sahu et al., 2009).
The EC reactor employed in this study focuses on eliminating TDS
TDS (ppm) 1514
TSS (ppm) 57.73 and TSS from brackish groundwater. This reactor has an innovative
Conductivity (µS/cm) 2020 configuration of electrodes arranged in a monopolar-parallel mode. The
pH 8.1 cathode electrode is designed as a plane-cylindrical shape, while the
Nitrates (ppm) 32.6 anode is a finned-cylindrical shape placed centrally ↱within the cathode.
Sulfates (ppm) 180
Calcium (ppm) 1744.74
According to the author’s knowledge, no previous studies have
Magnesium (ppm) 1308 addressed the ↱treatment of real groundwater using the present design
and configuration of the ↱electrodes. This work aims to investigate the
capability of the new design of the EC ↱reactor to remove pollutants
as electrocoagulation (EC), electro-oxidation (EO), electro-flotation from real groundwater under the impact of the operating ↱variables and
(EF), electro-Fenton (EF), and Electrodialysis (ED) (Benekos et al., the effect of the ohmic potential drop (OPD) parameter. Consequently,
2019; Ghanbari et al., 2020; Talaiekhozani et al., 2020; Li et al., 2020; optimization process and validation of the proposed models have been
Zhang et al., 2018; Jiang et al., 2018). studied.
Electrocoagulation process (EC) is categorized as a non-conventional
method that has notable advantages over other treatment methods, and
it is applied to eliminate several pollutants, including organic and
inorganic compounds Benekos et al., 2019; Rosales et al., 2018; Mohora
et al., 2018; Hadi et al., 2021; Jasim and AlJaberi, 2022, 2023b, 2023a). Table 2
EC method is feasible in design and ease operation without adding Experimental design ranges of the operating variables.
chemicals, significantly less electrolysis time, high efficiency, and Coded variables
cost-effective. The applicability of using EC in combined systems with
Real Variables (Xi) − 1.732 − 1 0 +1 1.732
other technologies (Changmai et al., 2019; Kong et al., 2019; Adamović X1: Reaction time (min.) 4 9 17 25 30
et al., 2019) depends on the efficient design and configuration of elec­ X2: Applied current (Amp.) 0.2 0.7 1.3 1.9 2.4
trodes performed in the EC cell, which impacts the performance of this X3: Mixing speed (rpm) 50 92 150 208 250
method (AlJaberi et al., 2020; AlJaberi and Mohammed, 2018). In the
EC process, redox reactions at electrodes play an essential role in the
generation of electro-coagulants in situ which are more available and Table 3
less soluble compared to the chemical coagulants (Eqs. (1) – ((5) for Design of experiments.
aluminum electrodes as an example) where the most common metals Run X1: X2: X3: X1: X1: X2:
used of electrodes are aluminum and iron (AlJaberi, 2020; AlJaberi coded coded coded reaction applied mixing
et al., 2020). value value value time current speed
(min.) (Amp.) (rpm)
Al(S) ⇒Al3+
(aq) +3e

(1) 1 − 1 − 1 − 1 9 0.7 92
2 1 − 1 − 1 25 0.7 92
2H2 O⇒O2 +4H+ +4e− (2) 3 − 1 1 − 1 9 1.9 92
4 1 1 − 1 25 1.9 92
5 − 1 − 1 1 9 0.7 208
2H2 O + 2e− ⇒H2(g) +2OH−(aq) (3)
6 1 − 1 1 25 0.7 208
7 − 1 1 1 9 1.9 208
Al3+ +3OH− ⇔ Al(OH)3 (4) 8 1 1 1 25 1.9 208
9 − 1.732 0 0 4 1.3 150
n Al(OH)3 →Aln (OH)3n (5) 10 1.732 0 0 30 1.3 150
11 0 − 1.732 0 17 0.2 150
In the present work, response surface methodology (RSM) type 12 0 1.732 0 17 2.4 150
13 0 0 − 1.732 17 1.3 50
central composite design (CCD) has been performed as a modeling and
14 0 0 1.732 17 1.3 250
optimization method, as usual (Biswas et al., 2019; Bal et al., 2019; 15 0 0 0 17 1.3 150
Sahoo et al., 2017), for the EC process to eliminate pollutants from real 16 0 0 0 17 1.3 150
groundwater. Moreover, based on the CCD matrix, the respective 17 0 0 0 17 1.3 150

Fig. 1. A schematic of the electrocoagulation reactor and electrodes configuration.

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F.Y. AlJaberi South African Journal of Chemical Engineering 46 (2023) 205–216

Table 4
Results of the studied variables.
Run X1: (min.) X1: (Amp.) X2: (rpm) Actual Predicted Actual Predicted κ (µS/cm) OPD
YTDS% YTDS% YTSS% YTSS% ohm

1 9 0.7 92 61.69 58.80 50.29 48.18 773.33 1.97


2 25 0.7 92 45.71 43.87 62.31 66.30 1096 1.39
3 9 1.9 92 71.73 70.29 69.51 73.29 570.67 7.24
4 25 1.9 92 58.39 57.99 80.08 76.62 840 4.92
5 9 0.7 208 63.54 61.89 61.20 64.24 736 2.07
6 25 0.7 208 54.56 53.95 72.80 68.59 917.33 1.66
7 9 1.9 208 52.25 52.04 62.84 58.42 964 4.28
8 25 1.9 208 45.90 46.74 46.30 47.90 1092 3.78
9 4 1.3 150 51.12 53.96 62.24 61.86 986.67 2.86
10 30 1.3 150 37.25 37.52 67.09 68.11 1266.67 2.23
11 17 0.2 150 50.66 53.46 59.29 58.69 996 0.44
12 17 2.4 150 57.73 57.38 61.72 62.82 853.33 6.11
13 17 1.3 50 68.23 71.05 69.69 68.20 641.33 4.41
14 17 1.3 250 64.07 64.01 55.31 57.37 725.33 3.90
15 17 1.3 150 65.79 65.82 67.61 67.60 690.67 4.09
16 17 1.3 150 65.46 65.82 67.78 67.60 697.33 4.05
17 17 1.3 150 66.31 65.82 67.43 67.60 680 4.16

2. Materials and methods

2.1. Characterization of real groundwater

All experiments were done using real groundwater obtained from a


farm well located in Al-Khidher (South of Iraq) of which the main
characterizations are listed in Table 1. The collected samples were
characterized as brackish groundwater due to the high values of con­
ductivity (2020 µS/cm) and TDS (1514 ppm). The analytical measure­
ment of different ions and other parameters was conducted according to
the standard procedures. The values of conductivity and pH were
determined using an electronic conductivity meter, Model (CCP, China),
and an electronic pH meter, Model (ATC company, China), respectively.
The studied response of TDS and TSS removal efficiencies were
conducted using the following equation (Eq. (6)):
C0 − Cf
Y% = × 100 (6)
C0
Where the initial and final concentrations of contaminants are
designated as C0 and Cf in mg/L respectively.
Since, the consumption of the electrical energy (EEC) and electrodes
(TEC) is a real challenge in any new design of EC reactors. These pa­
rameters were evaluated using Eqs. (7) and (8) as follows:
UIt
EEC = (7)
V

ItM
TEC = (8)
ZF

Where U is the operating voltage in volts, I is the applied current in


Amps., t is the reaction time in hours, V is the volume of the sample in
m3, M is the molecular weight of aluminum electrodes in g/mol, Z is the
number of electrons (equals 3 for aluminum), and F is Faraday’s con­
stant (96,485.34 C/mol).
The ohmic potential drop between the electrodes (Eq. (9)) is an
extremely important parameter that impacts the performance of elec­
trochemical reactors that should be taken into consideration in this field
of treatment technology (AlJaberi, 2019):
OPD = (j ∗ d)/k (9)

Where: OPD is the ohmic potential drop (ohm), j is the current density in
(mA/cm2), d is the distance between electrodes (cm), and κ is the elec­
trical conductivity (mS/cm).

Fig. 2. Observed and predicted values for (a) TDS removal %, (b) TSS removal
%, (c) OPD responses.

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F.Y. AlJaberi South African Journal of Chemical Engineering 46 (2023) 205–216

2.3. Experimental design

In the present work, the experimental design of the batch electro­


coagulation experiments, the analysis of the obtained results, and the
optimization process were conducted using the statistical method of
response surface methodology (RSM) based on central composite design
(CCD) and the statistical software Minitab program.
RSM technique overcomes traditional experiential design limita­
tions. The conventional methods examine how one factor affects the
result, disregarding interactions with other factors, and keeping them
constant. Whereas, RSM takes these interactions into consideration
(Biswas et al., 2019).
The mathematical models relate the investigated responses to the
operating parameters were conducted based on the second-order mul­
tiple regression (Eq. (10)) as follows (AlJaberi, 2018; Mohammed and
Al-Zuheri, 2018):
q
∑ q
∑ ∑∑
Y = B0 + Bi Xi + Bii Xi2 Bij Xi Xj (10)
i=1 i=1 i j

where Y is referred to the studied responses, i.e. YTDS% and YTSS% for TDS
and TSS removal efficiencies respectively; q is the total number of the
operating variables; X1, X2, to Xq are the operational parameters; and Bo,
Bii, and Bij are designated as the regression coefficients.
The influences of the reaction time (X1: 4–30 min), applied current
(X2: 0.2–2.4 Amp.) which is equivalent to (0.44 – 5.22 mA/cm2), and the
mixing speed (X3: 50–250 rpm) were investigated.
Subsequently, the selection of the operating variables and their
ranges of 17 experiments with 8 factorial, 6 axial and 3-fold repetition of
center points, were designed to optimize the TDS and TSS responses
observed (Tables 2 and 3). Each run was repeated with three repetitions
and the average mean value was reported.
The real conditions of the operating parameters (XReal) were deter­
mined using Eq. (11) as follows:
XReal − XCenter
XCoded = XCenter − Xmin (11)
√̅̅̅
q

and the rotatability [α = (2q)0.25] equals +1.732.

3. Results and discussion

For the groundwater samples treated, three factors with three levels
of RSM-CCD matrix of actual and predicted values of TDS and TSS
Fig. 3. Interaction plots among the operating variables for (a) TDS removal %, removal efficiencies, as well as the electrical conductivity and the ohmic
(b) TSS removal %, (c) OPD responses. potential drop for each experiment, are given in Table 4. The observed
findings of the TDS%, TSS%, and OPD responses varied between
2.2. Electrocoagulation reactor 37.25%− 71.73%, 47.30%− 80.08%, and 0.44 ohm to 7.24 ohm,
respectively, which are in good agreement with their predicted values of
The batch EC experiments were conducted at room temperature in a 37.52%− 70.29%, 47.90%− 76.62%, and 0.41 ohm – 6.68 ohm, respec­
one-liter cylindrical reactor (Fig. 1). The volume of groundwater in each tively, as explained clearly in Fig. 2(a–c). The graphs plotted in Fig. 2(a-
run was 0.5 l; an aluminum tube (6 cm × 4.4 cm) contains 39 fins (2 cm c) related the observed values to predicted values in order to estimate
× 4.4 cm) with a total area of 460 cm2 was employed as anode where the the error analysis. As revealed in Fig. 2(a-c), the closeness of all points
active area of anode is the new challenge, and it is significantly higher in listed in these graphs, around the diagonal line, proposed low differ­
comparison to its wet volume (68 cm3). A tubular cathode (8 cm × 9 cm) ences in observed and predicted values.
with a total area of 96 cm2 made of aluminum was arranged around the The low values of ohmic potential drop observed in all experiments
anode. These electrodes were connected to a power supply (model were obtained due to the higher values of the solution conductivity and
SYADGONG, China) in a monopolar-parallel manner. An electromag­ the lower values of current density performed in each run. Furthermore,
netic stirrer (model ALFA: HS-860; 0–1000 rpm) was used to provide a sulphate ions present in the solution will enhance the pitting corrosion
complete mix according to the designed value. After each experiment, of the anode which consequently assessed the pollutants removal at a
the electrodes were rubbed using sandpaper and washed with distilled low reaction time (AlJaberi et al., 2020). The core results indicate the
water to remove the passivation layer, and then dried and weighed. significant performance of the present design of the electrocoagulation
reactor. Table 4 shows the values of the solution conductivity and ohmic
potential drop for each experiment done.

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F.Y. AlJaberi South African Journal of Chemical Engineering 46 (2023) 205–216

3.1. Mathematical models of the studied responses 3.3. Mutual effect of the operating variables on TDS removal

The mathematical models of predicting TDS%, TSS%, and OPD Eqs. From Fig. 4(a), it can be noted that at 4 min and 0.2 Amp, low TDS
(12) – ((14)) were estimated based on the findings presented in Table 4 removal was achieved due to the degradation of Al(OH)3 flocs caused by
in terms of real variables. As shown, the high values of the regression the collision effect, as well as the satisfactory mass transfer was not
coefficients of R2 and adjusted R2 confirmed the suitability of the ob­ reached. As the reaction time increased and sufficient electro-coagulants
tained models and enhanced the validation of these models: formed, the TDS removal efficacy increased. When the applied current

YTDS% = 17.3 + 2.664X1 +44.79 X2 +0.049 X3 − 0.119 X21 − 8.60 X22 +0.0002 X23 +0.137 X1 X2
(12)
+0.004X1 X3 − 0.153X2 X3

raises, an increment of TDS removal was attained, especially at the range


R2 (Adjusted) = 0.933; R2 = 0.971 of 0.5 Amp to 2.2 Amp. Consequently, TDS removal tends to decrease

YTSS% = − 34.9 + 2.880X1 +63.0X2 +0.505X3 − 0.016X21 − 5.66X22 − 0.0005X23 − 0.770X1 X2 − 0.007X1
(13)
X3 − 0.222X2 X3

due to the increase of OPD because the OPD parameter is related directly
R2 (Adjusted) = 0.774; R2 = 0.901 to the applied current (Eq. (9)). The same behavior of the latter status, i.

YOPD = − 3.83 + 0.232 X1 +7.51 X2 +0.002 X3 − 0.009 X21 − 0.627 X22 − 0.0001 X23 − 0.048 X1 X2
(14)
+0.0005 X1 X3 − 0.016 X2 X3

e. the continuous minimizing of TDS removal, was observed when the


R2 (Adjusted) = 0.952; R2 = 0.979 reaction time increased beyond the mean value especially at the
maximum range due to the huge amount of gas bubbles among the an­
3.2. Analysis of variance (ANOVA) ode’s fins. Moreover, the passivation effect on the cathode may impact
the formation of Al(OH)3 compounds (AlJaberi et al., 2020; Hadi et al.,
To validate the adequacy of the mathematical models established, 2022). The mutual effect of the reaction time and the mixing speed is
ANOVA was performed to analyze these models and fitting them to the revealed in Fig. 4(b). At 4 min and (140 – 250) rpm, the TDS removal
data in order to evaluate the misleading results that may affect the ac­ was attained less than 45% due to high turbulence occurred between
curacy of the developed mathematical models (AlJaberi et al., 2020; each pair fins of the anode that may prevent the interaction between
AlJaberi and Mohammed, 2018; Bal et al., 2019). As revealed that the ions released from the anode and that released at the cathode to form
F-value (TDS%; 25.59, TSS%; 7.10, and OPD; 36.18) and p-value (TDS electro-coagulants (Arellano et al., 2020; Nariyan et al., 2018; Jasim and
%; <0.0001, TSS%; <0.001, and OPD; <0.0001) for the developed AlJaberi, 2023). The same behavior of TDS% decreasing was observed
models indicated obviously the suitability of these models. Based on the when the reaction time exceeded 21 min to the final range of the reac­
ANOVA test, the electrocoagulation method can be performed to elim­ tion time and for all values of the mixing speed. This observation
inate pollutants containing real groundwater. revealed that the present design of electrodes does not require high
Fig. 3(a–c) explain the interaction among the operating parameters periods to achieve higher removal of TDS. As seen in Fig. 4(b), the
of the studied responses of TDS and TSS removal efficiencies, as well as highest values of TDS removal efficiency were attained at the low range
the OPD response where the strong interaction is presented when there of mixing speed, i.e., less than 80 rpm, and around the mean value of the
is a large deviation between the two non-parallel curves. As shown in reaction time, i.e., 16 min.
Fig. 3(a) for TDS ↱removal response, the reaction time was interacting
well with the values of other variables (0.2 Amp and 2.4 Amp of applied 3.4. Mutual effect of the operating variables on TSS removal
current) and (50 – 250 rpm of mixing speed). While for TSS removal
response, the reaction time has interacted with all the ranges of other As presented in Fig. 5, the minimum values of TSS removal were
operational variables as revealed in Fig. 3(b). But for the OPD response, obtained at the lowest and highest ranges of the operational variables.
the reaction time has interacted only with the range of the stirring speed From Fig. 5(a), the TSS removal was directly increased with both the
variable. reaction time and the applied current at 150 rpm of mixing speed. When
The mutual influence of the operating variables on the studied re­ the treatment process attained 15 min at 2.6 Amp or 30 min at 1.6 Amp,
sponses of TDS removal %, TSS removal %, OPD responses were inves­ the TDS removal tends to be minimized to less than 45 percent. This
tigated as follows. observation could be interpreted as the rule of insufficient attendance of
mass transfer effect and the negative influence of the collision that
degraded the formation of flocs required for the electrocoagulation

209
F.Y. AlJaberi South African Journal of Chemical Engineering 46 (2023) 205–216

Fig. 4. Mutual interaction of the reaction time, for TDS removal %, with (a) Applied current at 150 rpm of mixing speed, (b) Mixing speed at 1.3 Amp of
applied current.

Fig. 5. Mutual interaction of the reaction time, for TSS removal %, with (a) Applied current at 150 rpm of mixing speed, (b) Mixing speed at 1.3 Amp of
applied current.

process (Acharya et al., 2021; Jasim and AlJaberi, 2023). But at the agitation speed due to the beneficial assistant of soft mixing provided by
highest ranges of these variables, the excessive supply of electric current multi eddies formed between fins and that provided by hydrogen and
for a long time will increase the OPD between the electrodes, which will oxygen bubbles formed at electrodes (Hadi et al., 2021; AlJaberi et al.,
affect the performance of the electrochemical cell (AlJaberi et al., 2020; 2020). Based on the core findings shown in Fig. 5(b), the highest TSS
AlJaberi, 2019). Therefore, and as observed in Fig. 5(a), the best per­ removal was conducted at the ranges of the reaction time, i.e. 25 – 30
formance of TSS removal was achieved at a low applied current (<1.0 min, and 50 – 90 rpm of the mixing speed.
Amp) within 27 – 30 min of the reaction time. The behavior of TSS
removal under the mutual effect of the reaction time and mixing speed at
1.3 Amp of applied current was conducted in Fig. 5(b), which was 3.5. Mutual effect of the operating variables on OPD response
similar to that observed in Fig. 5(a). While, the TSS removal efficiency
was increased as the operating conditions moved toward the highest According to the mathematical equation (Eq. (9)) that was used to
range of time and lowest range of mixing speed. This observation proves estimate the ohmic potential drop, Fig. 6(a) proved the direct relation
that the efficient removal of TSS could be achieved at the lowest value of between OPD with the applied current, therefore, the highest values of
OPD were observed at the range of 2.2 – 2.4 Amp and 4 – 18 min of the

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F.Y. AlJaberi South African Journal of Chemical Engineering 46 (2023) 205–216

Fig. 6. Mutual interaction of the reaction time, for OPD response, with (a) Applied current at 150 rpm of mixing speed, (b) Mixing speed at 1.3 Amp of
applied current.

reaction time. The desired values of OPD could be attained when the min, 2.3 Amps, and 50 rpm, respectively, which produce 81.16% and
applied current decreases for all values of the reaction time, especially 85.26% of TDS and TSS removal efficiencies, respectively, as shown in
the lowest and the highest ranges as explained clearly in Fig. 6(a). While Fig. 8. The composite desirability (D) equals one, which refers to the
in Fig. 6(b), the desired values of OPD were established at 4 min and the high accuracy of the obtained results. OPD value at the optimal condi­
highest range of mixing speed, as well as the highest range of the re­ tions equals 8.9 ohm due to the high value of the applied current
action time at all conditions of the stirring speed. The interpretation of parameter.
this behavior could be referred to the continuous variation of conduc­ The core results observed in the present study prove the high per­
tivity parameter value along the period of the experiment depending on formance of the new electrocoagulation reactor that could be employed
the continuous releasing of different ions from electrodes and the per­ to eliminate pollutants from real groundwater.
formance of removing solids ions that affect strongly on the conductivity A comparative table providing the main findings attained in the
value and, consequently, the OPD value. The OPD values change present work with those obtained by other works is listed below
because of the decreased or increased interaction of different ions and (Table 5):
the production of gas bubbles, which can influence the value of the As observed in Table 5 that the core results achieved were compa­
conductivity in each zone throughout the reactor (Omwene et al., 2018; rable with previous studies. In the present design, contaminants were
Hadi et al., 2022). eliminated at low reaction time, lowest mixing speed and minimal
consumption of energy compared to other previous results. The core
3.6. Consumption of electrodes and electrical energy findings of Table 5 reveal the ability of the present EC reactor to treat
real groundwater with high performance.
Fig. 7(a–c) explains in 3D graphs the influence of the operating
variables on the consumption of electrical energy (EEC) and the theo­ 3.8. Temperature response
retical consumption of electrodes (TEC). Based on Eqs. (7) and 8, EEC
and TEC responses are directly related to the applied current and the The behavior of solution temperature should be investigated for all
reaction time of the batch electrocoagulation experiments done (Schaep experiments to have a model that could relate the temperature to the
et al., 1998; Jiang et al., 2018), as revealed clearly in Fig. 7(a and b). operating variables of the reaction time, applied current and the stirring
Therefore, the amount of consumption for both EEC and TEC responses speed. The findings obtained for this object are shown in Table 6 for each
was increased with the continuous increment of the reaction time and experiment designed as explained before:
the applied current at the mean values of other variables. While, the The Mathematical model of temperature response relating to the
behavior of EEC and TEC responses with the mixing speed encourages operating parameters is listed clearly in Eq. (15):
the employment of the present design of finned-anode and tubular
cathode, the significantly low consumption of the electrical energy and YTemp. = 20.64− 0.041X1 +0.11X2 − 0.0008X3 +0.003X21 +0.867X22 +0.0001X23
electrodes was obtained at all values of mixing speed and mean values of +0.052X1 X2 + 0.0001X1 X3 − 0.014 X2 X3
other operating variables. (15)
2
R = 0.912
3.7. Statistical optimization of operating variables The behavior of the temperature response against each of the oper­
ating variables is revealed clearly in Fig. 9. As shown that the temper­
The statistical optimization process of the operating variables was ature increased in similar behavior with all ranges of the reaction time at
conducted using Minitab statistical software program. The optimum mean values of other variables. While, the temperature raises as the
values of the reaction time, applied current, and mixing speed were 13 applied current increases along the period of the experiment. This

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F.Y. AlJaberi South African Journal of Chemical Engineering 46 (2023) 205–216

Fig. 7. Electrical energy consumption (EEC) and theoretical electrodes consumption (TEC) vs. the operating variables in the electrocoagulation treatment of
groundwater. (a) vs. reaction time at 1.3 Amp and 150 rpm, (b) vs. applied current at 30 min and 150 rpm, (c) vs. mixing speed at 30 min and 1.3 Amp.

behavior means that the higher the temperature, the higher the value of equation.
the applied current. But the temperature was decreased when the speed As presented in Table 7, the negative value of ΔG refers to the
of mixing increased, which did not assist the endothermic process. spontaneous nature of electrocoagulation. The positive values of the
Therefore, the lowest range of the stirring speed was more beneficial entropy change (ΔS) reveal the increment in the randomness of the
than the highest values to provide the heating required. solution interface through the electrocoagulation removal of TDS on the
electro-coagulants formed. The positive value of (ΔH) refers to the
endothermic nature of the present electrocoagulation process.
3.9. Thermodynamic parameters

The deduction of thermodynamic parameters of Enthalpy change 3.10. Cost estimation


(ΔH), Gibbs free energy (ΔG), and Entropy (ΔS) is important in
informing their effects on the performance of the present reactor. The Operating cost measurement is important to assess the ability of
value of ΔH (J/mol) could be estimated from the slope of the linear electrocoagulation technology in water treatment. Electrodes and elec­
relation of Van’t Hoff equation (Eq. (16)) and Fig. 10, as follows: trical energy consumption are the main topics that must be taken into
ΔH consideration in operating cost estimation. The values of electrode and
logKd = logK0 − (16) energy consumption at the optimal values of the operating variables
2.303 RT
were 0.25 g and 2.4 kWh/m3, respectively. The total cost of that two
where Kd is the equilibrium constant and K0 is the constant of this types of consumption at the optimal conditions was 0.0218 $ per cubic

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Fig. 8. The optimum values of the operating parameters and the studied responses of TDS and TSS removal efficiencies for the treatment of real groundwater.

Table 5
A comparative table of the present EC findings to other cited works used for groundwater treatment.
Ref. Pollutants Electrodes EC time Current Stirring speed (rpm) Removal efficiency EEC
Anode Cathode (min) % kWh/m3 or (kWh/
L)*

(Omwene et al., 2018) P Flat Flat 80 20 A/m2 300 99 3.40


(Hansen et al., 2019) Se Flat Flat 360 153.4 A/ Air stirring 90 120*
m2
(Nariyan et al., 2018) SO2-
4 Flat Flat 120 25 mA/cm2 98 150*
(Jiang et al., 2018) Zn Flat Flat 120 15 mA/cm2 Air stirring 99 14.80
(Martín-Domínguez et al., Cr tubular tubular 360 – 600 99 –
2018)
(Doggaz et al., 2018) Fe Flat Flat 60 2.5 mA/ 200 97 0.30
cm2
(Khemila et al., 2018) Turbidity Flat Flat 60 400 A/m2 Pumping feed caused 99 16
mixing
(Lin et al., 2019) B Flat Flat 15 – 150 27 –
(C.J. and V.D., 2019) TDS; Flat Flat 20 40 A/cm2 – 50; 2.30
Turbidity 94
The present study TDS;TSS Finned tubular 22 2.3 A 50 81; 2.40
85

meter of the treated groundwater according to the local price. 85.26% of TDS and TSS removal efficiencies, respectively, as well as 8.9
ohm of the ohmic potential drop (OPD). The solution temperature was
4. Conclusion directly proportional with all ranges of the reaction time and applied
current and was largely raised with the lowest range of the stirring
The treatment of real groundwater using an innovative electro­ speed, which is more fitted with the optimal value of this variable. The
coagulation reactor was conducted in the present work under the in­ present EC process was endothermic, spontaneous in nature, and the
fluences of several operating variables. Optimal values in terms of the randomness of the solution interface. Low consumption of the electrical
reaction time, applied current and mixing speed were attained to be 13 energy and electrodes was observed due to the reliability of the new
min, 2.3 Amp of, and 50 rpm, respectively, producing 81.16% and design of finned-anode and tubular-cathode that may assist the

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Table 6
Results of the temperature response.
Run X1: (min.) X1: (Amp.) X2: (rpm) YTemp. Run X1: (min.) X1: (Amp.) X2: (rpm) YTemp.
(◦ C) (◦ C)

1 9 0.7 92 21 10 30 1.3 150 24


2 25 0.7 92 23 11 17 0.2 150 22
3 9 1.9 92 23 12 17 2.4 150 24
4 25 1.9 92 26 13 17 1.3 50 22
5 9 0.7 208 21 14 17 1.3 250 23
6 25 0.7 208 23 15 17 1.3 150 22
7 9 1.9 208 21 16 17 1.3 150 22
8 25 1.9 208 24 17 17 1.3 150 22
9 4 1.3 150 21

Fig. 9. Interaction plots among the operating variables for temperature response.

Fig. 10. Estimation of enthalpy change (ΔH) at 30 min of reaction time, 1.3 Amp of applied current, and 150 rpm of mixing speed.

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Table 7 Goren, A.Y., Kobya, M., Oncel, M.S., 2020. Arsenite removal from groundwater by
Thermodynamic parameters for electrocoagulation of TDS. aerated electrocoagulation reactor with Al ball electrodes: human health risk
assessment. Chemosphere 251. https://doi.org/10.1016/j.
Temp. (K) Kd ΔH (kJ/mol) ΔG (J/mol) ΔS (J/mol.K) chemosphere.2020.126363. Article 126363.
Hadi, D.R., Ajjam, S.K., AlJaberi, F.Y., 2022. Assessment of electrocoagulation treatment
277.84 209.363 131.326 − 12,344.6 254.8949 of textile wastewater using constant voltage and constant current modes: a
284.155 43.867 − 8932.86 237.2235 comparative study. In: AIP Conference Proceedings, 2398, 040045. https://doi.org/
292.16 14.614 − 6514.64 222.4467 10.1063/5.0095300.
298.72 3.349 − 3001.78 205.802 Hadi, D.R., AlJaberi, F.Y., Ajjam, S.K., 2021. Removal of reactive blue dye from
simulated wastewater by electrocoagulation using bipolar connection mode.
J. Phys.: Conf. Series 1999 (1). https://doi.org/10.1088/1742-6596/1999/1/
performance of the electrocoagulation to be more desirable in ground­ 012007. Article 012007.
Hansen, H.K., Peña, S.F., Gutiérrez, C., Lazo, A., Ottosen, L.M., 2019. Selenium removal
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Declaration of Competing Interest Jasim, M.A., AlJaberi, F.Y., 2022. Treatment of oily wastewater by electrocoagulation
technology: a general review (2018-2022): review paper. J. Electrochem. Sci. Eng.
13 (2), 361–372. https://doi.org/10.5599/jese.1472.
The authors declare that they have no known competing financial Jasim, M.A., AlJaberi, F.Y., 2023a. Removal of COD from real oily wastewater by
interests or personal relationships that could have appeared to influence electrocoagulation using a new configuration of electrodes. Environ. Monit. Assess.
195 (651), 1–7. https://doi.org/10.1007/s10661-023-11257-y.
the work reported in this paper. Jasim, M.A., AlJaberi, F.Y., 2023b. Investigation of oil content removal performance in
real oily wastewater treatment by electrocoagulation technology: RSM design
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