Water Air Soil Pollut (2018) 229:184

https://doi.org/10.1007/s11270-018-3813-2

Removal of a Persistent Dye in Aqueous Solutions

by Electrocoagulation Process: Modeling and Optimization
Through Response Surface Methodology
Alain Stéphane Assémian & Konan Edmond Kouassi &
Patrick Drogui & Kopoin Adouby & David Boa

Received: 3 January 2018 / Accepted: 23 April 2018

# Springer International Publishing AG, part of Springer Nature 2018

Abstract This study is related to a laboratory study on
the performance of electrocoagulation process using Fe
and Al electrodes to treat bio-recalcitrant synthetic dye in
a batch mode operation. The performance of the electro-
lytic cell resulted from its capability of generating in situ
coagulants to remove methylene blue from aqueous so-
lution. A factorial experimental design was firstly used to
determine the effects of each parameter on methylene
Research Highlights
• RSM is a helpful method to study MB removal from water using
EC process
• Time and MB concentration were the main parameters
influencing MB removal
• The effect of these two main factors is around 66.9 % on the
investigated response.
• MB could be optimally removed (89% of MB removal) for 0.32
US$/m3
A. Assémian : K. E. Kouassi : K. Adouby
Laboratoire des Procédés Industriels, de Synthèse de
l’Environnement et des Energies Nouvelles (LAPISEN), Institut
National Polytechnique Houphouët-Boigny, BP
1313 Yamoussoukro, Côte d’Ivoire
K. E. Kouassi : D. Boa
Laboratoire de Thermodynamique et de Physico-Chimie du
Milieu (LTPCM), UFR-SFA, Université Nangui-Abrogoua, 02 BP
801 Abidjan 01, Côte d’Ivoire
P. Drogui (*)
Institut National de la Recherche Scientifique (INRS Eau Terre et
Environnement), Université du Québec, 490 rue de la Couronne,
Québec City, Canada
e-mail: patrick.drogui@ete.inrs.ca
blue (MB) removal. The MB concentration, current in-
tensity, electrolysis time, and electrode type were the
main influent parameters on the response studied. The
respective contributions of the main factors on the per-
centage of MB removal were 38.37, 18.41, 28.49, and
9.35%. Result analyses show that MB concentration had
a negative effect, whereas current intensity and electrol-
ysis time had positive effect on the efficiency. Using a 24
factorial matrix, the best performance for MB (89% of
MB removed) was obtained by selecting Fe anode oper-
ated at a current intensity of 3.0 A during 40 min of
treatment time in the presence of 20 mg/L of MB. A
central composite design (CCD) methodology was sub-
sequently used for optimization of EC process in treating
MB. Under the optimal conditions determined by this
method, EC can economically be applied to remove MB
(89% of MB removal for a total cost of 0.32 US$/ m3)
while using Fe anode operated at a current intensity of
1.44 A during 34 min of treatment time in the presence of
11.2 mg/L of MB.
Keywords Methylene blue . Electrocoagulation .
Factorial design . Central composite optimization
Abbreviations
EC Electrocoagulation
MB Methylene blue
FD Factorial design
CCD Central composite design
RSM Response surface methodology
ANOVA Analysis of variance
184 Page 2 of 13
1 Introduction
The use of synthetic dyes is today extensively wide-
spread in numerous industries as those of textile,
printing, food, cosmetic, clinical, paper, leather, phar-
maceutical, and food industries (Mansour et al. 2011;
Brillas and Martínez-Huitle 2015; Robinson et al.
2001). Among these industries, textile industry is
recognized like the most important consumer of water
and dyes in particular during dyeing, printing stages
where dyestuffs are abundantly used to color different
types of textile fibers (nylon, cotton, wool, silk, poly-
amide, polyester, cellulose, and acrylic) (Sala and
Gutiérrez-Bouzán 2012). According to the US EPA,
40 l of water is required averagely for dyeing 1 kg of
cloth, changing according to the textile material and
dyeing process (Arslan et al. 2016). Unfortunately,
not 100% of the dyes are fixed to the fiber during
the dyeing process. For example, reactive dyes show
the minimum range with 20–50% to cotton. A com-
plex molecular structure, high molecular weight
which makes them more stable and difficult to be
biodegraded (Forgacs et al. 2004; Gupta and Suhas
2009). The presence of these pollutants in waters can
change their appearance, e.g., 1 mg dm−3 of a dye is
likely to cause visible colorization (strong color) of
the water or alter the clarity (Martínez-Huitle and
Brillas 2009).
So, due to their color content, dye bath effluents are
not only esthetic undesirable pollutants, but may also
interfere with light penetration in the receiving bodies of
water (impede photosynthesis), thereby driven to deple-
tion of the dissolved oxygen and upset the biological
metabolism processes (Joshi et al. 2004). Accordingly,
dye effluent may contain chemicals that are toxic, car-
cinogenic, mutagenic, or teratogenic to various fish
species (Verma et al. 2012).
A general awareness of authorities in charge of envi-
ronmental protection on textile wastewater threaten drove
to the raising of more and more stringent legislation and
guidelines to protect environment (Alinsafi et al. 2005).
Electrocoagulation (EC) is an emerging technology for
water and wastewater treatment, as it combines the benefits
of coagulation, flotation, and electrochemistry. The mech-
anism behind coagulation/flocculation (CF) and
electrocoagulation (EC) is quite the same (Moussa et al.
2017; Garcia-Segura et al. 2017; Khandegar and Saroha
2013; Merzouk et al. 2010). During electrocoagulation, the
most important chemical reactions involve the dissolution
Water Air Soil Pollut (2018) 229:184
of metal cations at the anode and formation of hydroxyl
ions and hydrogen gas at the cathode (Mollah et al. 2004):
M →M nþ þ ne− ð1Þ
2H 2 Oðl Þ þ 2e− →2OH − þ H 2 ðg Þ ð2Þ
The current passes through a metal electrode, oxidiz-
ing the metal (M) to its cation (Mn+Mn+). Simultaneously,
water is reduced to hydrogen gas and the hydroxyl ion
(OH−OH−). The cations (Al3+, Fe2+Al3+, Fe2+, etc.) de-
stabilize colloidal particles by neutralizing charges. They
also produce monomeric and polymeric hydroxide com-
plex species (M (OH)n (S))M(OH)n(s)) as coagulants (An
et al. 2017; Drogui et al. 2007; Sahu et al. 2014).
Electrocoagulation (EC) is characterized by sim-
ple equipment (compactness of facilities), brief reten-
tion times, and easy operation that contribute to re-
ducing the operating cost in large-scale applications
(Moussa et al. 2017; Mollah et al. 2001; Emamjomeh
and Sivakumar 2009). EC is gaining in popularity
and causes the interest of researchers and engineers
whose efforts are focused on development of new
technologies, for wastewater treatment. EC is consid-
ered as simple, fast, effective, efficient, and eco-
friendly process compared to the conventional
methods (biological, chemical, physical) that present
some drawbacks and prove to be sometimes little
efficient, time-consuming, and inappropriate
(Robinson et al. 2001). During EC process, several
chemical reactions (complexation, precipitation, oxi-
dation, reduction) and physical reactions (flotation,
electrostatic attraction, flocs sedimentation, adsorp-
tion onto metal hydroxides) occur simultaneously
within the electrolytic cell. Therefore, it is not easy
to develop a model able to describe entirely the
process. Besides, with the classic method that con-
sists in making vary only one factor at a time (OFAT:
One Factor At a Time) all in maintaining the other
factors constant modeling is imperfect, and the re-
search of the optimal conditions is approximate and
time-consuming. From that point of view, using sta-
tistical methodology approach appears advantageous
for various reasons. RSM not only allows to get a
maximum of information with a minimum of experi-
ences but, especially to establish a mathematical
equation permitting to predict with precision and
reliability the studied answers (Goupy 2006).
Water Air Soil Pollut (2018) 229:184
RSM is a collection of mathematical and statisti-
cal techniques useful for designing experiments, de-
veloping, improving, and optimizing the process.
Indeed, RSM can be used to evaluate the influence
of several independent variables affecting a process
while taking in account all possible interactions
disregarded in classic methods of one factor at a
time (Kobya et al. 2003; Zaviska et al. 2011). EC
has been widely used to treat textile wastewater all
over the world (Körbahti and Tanyolaç 2008; Golder
et al. 2005; Kobya et al. 2003; Daneshvar et al.
2006; Asghari et al. 2012). The overall objective
of this study is to evaluate the performance of
electrocoagulation (EC) process to treat simulated
textile wastewater enriched by a synthetic dye
(Methylene Blue, MB) chosen as model pollutant.
Thus, an experimental design methodology was used
to investigate the influence of the principal experi-
mental parameters (MB concentration, current inten-
sity, electrolysis time, and electrode type). In this
optic, the specific objectives of this work are the
followings: (i) quantify the effect of factors selected
and their interactions in the experimental field using
a factorial design (FD), (ii) optimize the mathemat-
ical model developed from a central composite de-
sign (CCD) in order to find the best combination of
operational factors that led to the best conditions for
decolourization while taking in account energy
consumption.
2 Material and Methods
2.1 Preparation of the Synthetic Solution
All solutions used for electrolysis tests were prepared
from analytical grade chemical reagents with distilled
water. Methylene blue [3,7-bis (dimethylamino)
phenazathionium chloride trihydrate] was used as
model pollutant. Synthetic solutions of methylene
blue dye (Basic Blue 9; CI: 52015, purity 99%,
Merck) was prepared. A fixed amount of sodium
sulfate 0.2 g L−1 Na2SO4 (Prolabo, purity 99%) was
added as supporting electrolyte to increase the con-
ductivity. At the end of each assay, the treated effluent
was subjected to settling in a 2-L cylinder for 24 h.
Then, the supernatant was carefully collected and
filtered using a glass microfiber filter Whatman™
(1.5-μm rated pore diameter) under vacuum. A sub-
Page 3 of 13 184
sample (20 mL) was also withdrawn to measure the
residual MB concentrations. The removal efficiency
R (%) was calculated using the following equation:
C 0 −C f
Dye removal rate; Rð%Þ ¼ ∗ 100 ð3Þ
C0
where C0 and Cf represent, respectively, the initial and
final dye concentration.
2.2 Experimental Unit
EC runs were carried out in a discontinuous electrolytic
cell made of acrylic material with a dimension of
12.5 cm (width) × 12.5 cm (length)× 20 cm (depth).
Inside the electrolytic cell, anode followed cathode with
an inter-electrode gap of 10 mm. The electrode sets were
composed of ten parallel pieces of metal plates (10 cm
(width) × 11 cm (high)), each having a surface area of
110 cm2. Entirely submerged in the raw effluent, the
electrodes were installed on a perforated acrylic plate
placed at 20 mm from the bottom of the cell (Fig. 1). To
assure constant homogeneity of the solution in the reac-
tor during EC treatment, a magnetic stirrer (Heidolph
Drehzahl, Germany) continuously mixes the effluent to
the same speed (700 rpm). For all tests, a working
volume of 1.7 L of textile effluent was used. Before
each test, electrolytic cell (including the electrodes) was
cleaned with hydrochloric acid (HCl 0.1 M) solution for
at least 15 min to remove greases from electrodes sur-
face, then rubbed with a sponge and rinsed with tap
water. The anode and cathode sets were connected,
1)
2) 3)
4)
5)
6)
Fig. 1 Schematic diagram of EC experimental set-up. (1) DC
power supply; (2) anode material (+); (3) cathode material (−);
(4) EC cell; (5) magnetic bar; (6) magnetic stirrer
184 Page 4 of 13 Water Air Soil Pollut (2018) 229:184

respectively, to the positive and negative outlets of a DC
power source, (ELC-AL781D: 0-5A; 0-30V, France) in
monopolar parallel (MPP) configuration. All EC tests
were carried out in a batch reactor under potentiostatic
regime. Likewise, an ammeter (ALDA DT-830-D) was
used to follow current intensity changes during
electrolysis.
2.3 Response Surface Methodology
Response surface methodology (RSM) helps to develop
a statistical model describing complex phenomenon by
performing minimum number of experiments and to
determine optimal combination of variables which lead
to expected responses (Goupy 2006; Myers and
Montgomery 2002). To the difference of the classic
method (one-factor-at-time) where interactions are
disregarded, effects of several variables influencing the
responses in RSM are studied by varying them simulta-
neously. So, full factorial design (FD) was firstly
employed to investigate the effects of the main factors
and their eventual interactions on textile wastewater
treatment (assays 1 to 16). Secondly, a central composite
design (CCD) was employed to describe and optimize
textile wastewater treatment using electrocoagulation
process (assays 17 to 28 and 29 to 40). Four independent
variables were used in this study: MB concentration
(X1), current intensity (X2), electrolysis time (X3), and
type of electrode (X4) (Table 1). A four-factorial design
at two levels (2k=4) completed by a central composite
design, with six replicates at the center of the experi-
mental region, led to a total number of 40 experiments
employed for response surface modeling (see Tables 2
and 3). The experimental range and levels of indepen-
dent variables investigated with the coded values are
shown in Table 1. Variable values and their variation
limits were selected based on exploratory tests. All
model coefficients were calculated using the least
squares method. Analysis of variance (ANOVA) was
carried out to determine the significant effects of process
variable (model terms) and goodness of fit. Statistical
software NEMROD-W (Version 9901 Française,
LPRAI-Marseille Inc., France) was used for regression
and graphical analyses of experimental data obtained.
The second-order response (Y (%)) surface model is
given by the following equation:
k k k
Y ð%Þ ¼ b0 þ ∑ bi X i þ ∑ bii X 2i þ ∑ ∑ bijX i X j
i¼1 i¼1 j≠i i¼1
þ ei ð4Þ
where Xi, Xj, are the coded independent variables. b0, bi,
bii, and bi j are the regression coefficient for intercept,
linear, quadratic, and interaction terms, respectively.
2.4 Economic Aspect
The economic study included the consideration of chem-
ical and energy consumption. The electric cost was esti-
mated to be approximately 0.059 US$ kW h−1. The unit
cost of the electrolyte (Na2SO4 industrial grade) was 3.6
US$ kg−1 and 0.173 US$ kg−1 of Fe. The total cost was
evaluated in terms of US dollars spent per cubic meter of
treated solution (US$ m−3). The total operating cost was
determined using the following eq. (5):
Operating cost US =m3 Þ ¼ aCenergy þ bCelectrode þ cCchemicals
ð5Þ
In this equation, Cenergy represents the energy con-
sumption in terms of kWh/m3, Celectrode represents the
electrode consumption (kg (Fe)/m3) calculated by Fara-
day’s law, whereas Cchemicals represents the chemical
consumption (kg (Na2SO4)/m3). a, b, and c given repre-
sent the unitary prices mentioned above.

Table 1 Data for optimization operation: experimental range and levels of independent process variables

Variables coded Factors (Ui) Description Experimental field U i,0 ΔU i,0

(Xi) Min Valeur (− 1) Max Valeur (+ 1)

X1 U1 Concentration (mg/L) 20 50 35 15
X2 U2 Intensity (A) 1 3 2 2
X3 U3 Time (min) 20 40 30 10
X4 U4 Electrode type Fe Al – –
Water Air Soil Pollut (2018) 229:184 Page 5 of 13 184

Table 2 Experimental factorial matrix and decolorization rate

Runs Experiment design Experiment plan Decolorization yield

X1 X2 X3 X4 U1 U2 U3 U4 Y (%)

1 −1 −1 −1 −1 20 1 20 Fe 69.79
2 1 −1 −1 −1 50 1 20 Fe 56.05
3 −1 1 −1 −1 20 3 20 Fe 70.69
4 1 1 −1 −1 50 3 20 Fe 62.76
5 −1 −1 1 −1 20 1 40 Fe 76.29
6 1 −1 1 −1 50 1 40 Fe 60.76
7 −1 1 1 −1 20 3 40 Fe 89.44
8 1 1 1 −1 50 3 40 Fe 78.04
9 −1 −1 −1 1 20 1 20 Al 62.57
10 1 −1 −1 1 50 1 20 Al 49.76
11 −1 1 −1 1 20 3 20 Al 67.16
12 1 1 −1 1 50 3 20 Al 56.47
13 −1 −1 1 1 20 1 40 Al 72.19
14 1 −1 1 1 50 1 40 Al 56.39
15 −1 1 1 1 20 3 40 Al 81.29
16 1 1 1 1 50 3 40 Al 68.03

3 Results and Discussion coded as − 1 (low), 0 (central point), and + 1 (high). A

3.1 Effect of the Experiment Parameters on MB
Removal Using a Factorial Design
The percentage of MB removal (Y1) was considered as
dependent factor (response). The factor levels were
total of 16 trials were carried out for the factorial design
(FD). The conditions in each experiment were modified
using different combinations of the two selected levels.
The experimental response associated to a 24 factorial
design is represented by a linear polynomial model with
interaction (Eq. 7):

Y 1ð%Þ ¼ 67:36−6:323X 1 þ 4:380X 2 þ 5:448X 3 −3:122X 4 þ 0:9118X 1 X 2 −

ð7Þ
0:6769X 1 X 3 −0:2467X 1 X 4 þ 2:015X 2 X 3 −0:3746X 2 X 4 −0:2063X 3 X 4

The levels of the four variables studied for each
experimental system and results are shown in Tables 1
and 2. The coefficients of the polynomial model were
calculated by means of NEMROD-W program soft-
ware. It is worth underlining that the recorded responses
are well fitted to the polynomial model with a regression
coefficient R2 of 0.992. Besides, the low relative value
of standard deviation of the response recorded (1.632)
indicated that the linear polynomial model described by
Eq. (7) is satisfactory. Equation (7) shows that the re-
moval of MB is mainly influenced by the initial MB
concentration, which has negative effect (b1 = −6.323).
While increasing the MB concentration of 20 to 50 mg/
L, the dye removal rate is reduced on average of
12.65%. The electrolysis time is the second most impor-
tant factor which also has positive effect (b3 = +5.448)
on the studied response. The percentage of MB removal
increases on average of 10.90% when the electrolysis
time goes from 20 to 40 min. The third most important
factor on MB removal is the current intensity with a
positive effect (b2 = +4.380). The increase of current
intensity contributes to improve the removal rate of MB.
So, the percentage of MB removal increases on average
of 8.76% when the current density goes from 1 to 3 A.
The fourth parameter which influences the response
studied is according to the mathematical equation
184 Page 6 of 13 Water Air Soil Pollut (2018) 229:184

Table 3 Central composite matrix and experimental results

Runs Experimental design Experimental plan Decolorization yield (%) Energy (kWh/m3)

X1 X2 X3 U1 (mg/L) U2 (A) U3 (min)

Fe electrode

17 − 1.682 0 0 9.755 2 30 82.86 7.06

18 1.682 0 0 60.245 2 30 66.49 7.06
19 0 − 1.682 0 35 0.317 30 43.33 0.18
20 0 1.682 0 35 3.683 30 90.00 23.03
21 0 0 − 1.682 35 2 13.17 65.00 3.083
22 0 0 1.682 35 2 46.83 82.50 11.02
23 0 0 0 35 2 30 65.83 7.06
24 0 0 0 35 2 30 64.17 7.06
25 0 0 0 35 2 30 62.5 6.14
26 0 0 0 35 2 30 63.33 7.06
27 0 0 0 35 2 30 65.83 6.78
28 0 0 0 35 2 30 66.67 6.88
Al electrode
29 − 1.682 0 0 9.755 2 30 51.43 5.33
30 1.682 0 0 60.245 2 30 56.02 4.91
31 0 − 1.682 0 35 0.317 30 40.83 0.18
32 0 1.682 0 35 3.683 30 70.83 21.64
33 0 0 − 1.682 35 2 13.17 52.50 2.79
34 0 0 1.682 35 2 46.83 73.33 7.99
35 0 0 0 35 2 30 42.53 5.89
36 0 0 0 35 2 30 48.33 5.54
37 0 0 0 35 2 30 43.33 6.28
38 0 0 0 35 2 30 46.67 5.29
39 0 0 0 35 2 30 41.67 4.94
40 0 0 0 35 2 30 43.33 6.35

established by the electrode type. The negative value (b4
= − 3.122) means that the choice of iron electrodes
encourages a better decolorization. The average rate of
MB removal in solution decreased 6.24% when the Al
electrode was used. Concerning the interaction terms,
X 2X 3 (current intensity and electrolysis time) and
X2X4(current intensity and electrode type) have been
studied. Interaction X2X3 has positive effect (b23 = +
2.015) whereas X2X4 show negative effect (b24 =
−0.3746). The importance of the factors and interactions
was studied using graphical Pareto analysis [28]. The
contributions of the principal effects (X1, X2, X3, X4) on
the percentage of MB removal are, respectively, 38.37,
18.41, 28.49, and 9.35% (Fig. 2). The contribution of
the different interactions (X1X2, X1X3, X1X4, X2X3, X2X4
and X3X4) on the percentage of MB removal were 0.8,
0.44, 0.06, 3.9, 0.14, and 0.04%, respectively (Fig. 2).
As one can note, all interactions have a negligible effect
(less than 1%) on the process except interaction X2X3
(current intensity-electrolysis time) with a contribution
of 3.9%. In this way, Figs. 3 and 4 help us to better
understand the interactions. Interactions studied are
X2X3 and X2X4: current intensity and electrolysis time
(Fig. 3) and current intensity and electrode type (Fig. 4).
For example, in Fig. 3, the corner at the top (at the left)
of this figure corresponds to electrolysis time of 20 min
and current intensity of 3 A imposed. The value of
64.27% is obtained by calculating the average of the
experimental results from the assays carried out with
electrolysis time of 20 min at a current intensity of 3 A.
When the electrolysis time (X3) is fixed at 20 min, the
current intensity (X2) had a significant influence on the
Water Air Soil Pollut (2018) 229:184 Page 7 of 13 184

Fig. 2 Graphical Pareto analysis 50

of the effect of MB concentration,
current intensity, time, and type of 38.37
40

Contribution (%)
electrode
28.49
30

18.41
20
9.35
10
3.9
0.8 0.44 0.06 0.14 0.04
0

Intensity-Electrode
Concentration-Electrode

Intensity-Time
Time

Time-Electrode
Intensity

Concentration-Intensity
Electrode

Concentration-Time
Concentration

response. In this case, the average rate of the MB re-
moval passed from 59.54 to 64.27%. When the electrol-
ysis time is fixed at 40 min, the current intensity had
always an influence on the response, but it is more
important than the first case while imposing 40 min as
electrolysis time. The average rate of MB removal
passed from 66.41 to 79.20%. Consequently, it can
be noticed that the effect of current intensity de-
pends on the electrolysis time. For X2X4 interaction,
the same approach can be used to understand this
interaction (Fig. 4). When Fe is used as electrode
material (X4), the current intensity (X2) has a signif-
icant influence on the response, the average rate of
MB removal increased from 65.72 to 75.23%. Oth-
erwise, when Al is used as electrode material, the
current intensity has in the same way a notable
effect on the response. The average rate of MB
removal passed from 66.41 to 79.20%. The effect
of the current intensity was not constant at all, and it
was a factor that greatly influenced the rate of MB
removal during electrocoagulation process. The Pa-
reto analysis shows that the influence of current
intensity directly depends on the type of electrode
used. A factorial design is a powerful tool to deter-
mine the interactions affecting the response and
indicates if the lowest or the highest levels of the
factors are favorable or not. The results are reliable
based on the tendency of the response, which are
greatly influenced by the factors having a significant
effect. Nevertheless, FD model is mainly used to
quantify effect of factors and their interactions can-
not be used for prediction or to determine the opti-
mization conditions. In view of determining the
optimal operating conditions for MB removal, a

Fig. 3 Interaction b23 between

current intensity (A) and electrol- X2 Intensity (A)
ysis time (min) 64.27% 3 79.20%

X3
20 40
Time
(min)

59.54% 1 66.41%
184 Page 8 of 13
Fig. 4 Interaction b24 between
current intensity (A) and type of
electrode 75.23%
Fe
65.72%
surface response methodology (central composite
design) was used.
3.2 Optimization Conditions for MB Removal Using
Central Composite Design
The response can be described by a second-order model
for predicting the response in all experimental regions.
Considering MB decolorization rate (Y1) and energy
consumption (Y2), the regression model in terms of
Y 2ð%Þ ¼ 6:738 þ 0:057X 1 þ 8:601X 2 þ 1:292X 3 þ 0:686X 21 þ 2:293X 22 þ 0:683X 23 þ
0:195X 1 X 2 þ 0:062X 1 X 3 −0:010X 2 X 3
Table 4 shows the analysis of variance (ANOVA) of
regression parameters of the predicted response surface
quadratic model for MB removal and energy consumed.
As it can be seen from this table, the model F-value of
88.8054 and a low probability value ((Pr > F) << 0.01)
indicate that the model is very significant for decolori-
zation. The value of the correlation coefficient (R2 =
0.876; R2adj ¼ 0:765) means that only 12.4% of the total
variation could not be explained by the empirical model.
The regression model explained well the
electrocoagulation process. R2 should be at least 0.80
for a good fit of a model (Joglekar and May 1987).
Furthermore, the lack of fit F-value of 21.6013 and the
probability value ((Pr > F) << 0.01) indicate that the lack
of fit of the model is not significant.
The energy consumption is calculated from the
followed equation:
Water Air Soil Pollut (2018) 229:184
Intensity (A)
X2
3 68.24 %
X4
Al
Electrode
1 60.23%
coded variables can be explained by the following
second-order polynomial equation:
For decolorization:
Y 1ð%Þ ¼ 64:775−5:575X 1 þ 8:533X 2 þ 3:172X 3 þ 0:341X 1 2
þ 0:341X 2 2 þ 2:845X 23 þ 1:243X 1 X 2 −0:657X 1 X 3 ð8Þ
þ 2:853X 2 X 3
For energy consumption.
ð9Þ
U *I *T
E¼ ð10Þ
V
where BE^ is the energy consumption in kWh m−3, BI^
the current intensity (A), BU^ the electrical potential
(V), BT^ the treatment time (h), and BV^ the volume
of treated water (m−3).
The analysis of variance (ANOVA) of the regression
parameters of the predicted response surface quadratic
model for energy consumption shows that the model is
significant (F-value of 968.1096 and a low probability
value ((Pr > F) << 0.01). As it can be seen, the model is
significant, with a p value below 0.01. Indeed, when
using a significance level of 0.05, a model is considered
significant if its p value is below 0.05. The value of the
correlation coefficient (R2 = 0.941; R2adj ¼ 0:888) indi-
cates that only 5.9% of the total variation could not be
explained by the empirical model (Table 4). According
Water Air Soil Pollut (2018) 229:184 Page 9 of 13 184

Table 4 Analysis of variance results for response surface quadratic model for MB removal energy consumption

Source Sum of square Degree of freedom Mean square F-value Pr > F

Decolorization: Y1
Model 2.14673 × 103 9 2.38526 × 102 88.8054 ***
2
Residual 3.03528 × 10 10 3.03528 × 10
Lack of fit 2.90099 × 102 5 5.80198 × 10 21.6013 **
Pure error 1.34296 × 10 5 2.68594
Total 2.45026 × 103 19
Energy consumption: Y2
Model 1.11491 × 103 9 1.23879 × 102 968.1096 ***
Residual 6.95607 × 10 10 6.95607
Lack of fit 6.89209 × 10 5 1.37841 × 10 107.7226 ***
−1
Pure error 6.39800 × 10 5 1.27960 × 10
Total 1.18447 × 103 19

**< 1%; ***< 0.1%

R2 = 0.876; R2adj ¼ 0:765; for decolorization
R2 = 0.941; R2adj ¼ 0:888 for energy consumption

to Joglekar and May, R2 should be at least 0.80 for a
good fit of a model. Moreover, the lack of fit F-value of
107.7226 and the probability value ((Pr > F) << 0.01)
indicate that the lack of fit of the model is not significant.
The comparison of actual (experimental values) and
predicted values of MB removal and energy consump-
tion is presented in Figs. 5 and 6. As one can note it,
curves of theoretical and experimental values are very
close. The agreement between the actual and predicted
values for MB removal and energy consumption is
satisfactory and in accordance with the statistical signif-
icance of the quadratic model presented in Table 4.
Besides, these graphs clearly illustrate that the gap be-
tween the experimental values and theoretical is weak
showing the quality of the statistical model.
The effect of MB concentration and current intensity
on the dye removal is illustrated in Fig. 7. When current
intensity and MB concentration were kept constant at
2 A and 60 mg/L, respectively (at the center of the
experimental region investigated), an increase MB con-
centration decreases the removal rate of the pollutant
while an increase of current rather increases the re-
sponse. As seen from the contour plot, illustrated by
Fig. 8, the energy consumption evolves in the same way

Fig. 5 Comparison of actual and 100

predicted MB removal values by
RSM Y3(%) Théo
90
Y3(%) Exp
Decolorization (%)

80

70

60

50

40
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20
Runs
184 Page 10 of 13 Water Air Soil Pollut (2018) 229:184

Fig. 6 Comparison of actual and 30

predicted values for energy
consumption by RSM Y3(%) Théo
25
Y3(%) Exp

Energy (kWh/m3)
20

15

10

0
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20
Runs

as current intensity and electrolysis time. An increase of
each or both parameters drives obviously to an increase
of energy consumed.
In order to rigorously determine the optimal condi-
tions for MB removal in terms of cost/effectiveness, the
energy consumption during electrolysis has to be taken
into account. The criteria selected for the optimization
condition for this electrocoagulation process are the
removal of MB that has to be maximized (1/1 weighting
factor) whereas the energy consumption has to be
minimized with equal importance (1/1 weighting factor)
in order to reduce the treatment cost related to energy
consumption. Based on these criteria imposed, the
NemrodW Program Software proposed interesting so-
lution, their corresponding value of desirability
(Table 5). On one hand, the desirability is a value
varying from zero to one and it gives information about
the adequacy between the solution and the criteria im-
posed. If the value is closer to one, it means that the
solution is very close from what we want and the

Fig. 7 Contour plots of MB removal obtained from RSM using Nemrod-W Software
Water Air Soil Pollut (2018) 229:184 Page 11 of 13 184

Fig. 8 Contour plots of energy consumption obtained from RSM using Nemrod-W Software

software has done few compromises to satisfy the im-
posed criteria. On the other hand, if the desirability is
close to zero, it means that it is very difficult to satisfy
the criteria without making a lot of compromise (García-
Gómez et al. 2014). The best solution for MB removal
in terms of energy consumption/effectiveness has been
found imposing a current intensity of 1.44 during
33.93 min of electrolysis to remove 11.20 mg/L MB in
solution. Under these conditions, the MB removal
should be nearly 80.43% for a corresponding energy
consumption of 5.04 kWh m−3. Once the appropriate
values of the optimal parameters were determined, the
optimal conditions using Fe electrode (the best optimal
solution proposed in terms of MB removal and energy
consumption) were carried out in triplicate to verify the
reproducibility of the results (Fig. 8). After the series of
experiments to validate the model, the removal rate
obtained for MB removal was superior to the predicted
response (88.59%), whereas the energy consumption is
finally lower than the expected value (3.59 kWh m−3).
These results are globally close to those proposed by the
model. It is also interesting to note that the value of
desirability (79.11%) is relatively close to 1 as presented
in Table 5.
3.3 Economic Analysis
The economic study included the cost of chemical re-
agents used to increase conductivity, electrodes con-
sumption, and energy consumption. So, at a cost of
US$ 0.0593/kWh, US$ 0.173/kg Fe, and US$ 3.6/kg

Table 5 Determination of optimal condition in terms of cost/effectiveness proposed by NemrodW Program Software

Factors Theoretical results Experimental results Desirability

U1 (mg/L) U2 (A) U3 (min) U4 − Decolorization Energy Decolorization Energy

(%) consumption (%) consumption
(kWh m−3). (kWh m−3)

11.20 1.44 33.93 Fe 80.43 5.04 88.59 3.59 0.791

184 Page 12 of 13
Na2SO4, EC process involved a total cost of 0.322 US$/
m3 of textile effluent treated.
4 Conclusion
This study investigated batch treatment of simulated
textile effluent containing MB by electrocoagulation
process. An experimental design methodology was ap-
plied to model and determine the optimal experimental
conditions. The factorial design demonstrated that all
the main factors (MB concentration, current intensity,
electrolysis time, and electrode type) are influent param-
eters on the percentage of MB removal. In particular,
MB concentration had a negative effect while current
intensity and electrolysis time had positive effects on the
efficiency of MB removal. The contributions of the
main factors on the percentage of MB removal are,
respectively, 38.37, 18.41, 28.49, and 9.35%.
Concerning interaction effect, they were almost negligi-
ble (less than 1%). Subsequently, a central composite
design was employed to determine the optimal operat-
ing conditions for MB removal while taking into ac-
count energy consumption. Under these conditions, a
removal rate of 88.59% was reached for an energy
consumption of 3.59 kWh m−3. These values are close
to those predicted by the mathematical model
established. These results recorded at laboratory scale
could open interesting perspectives for practical appli-
cations of the treatment of real textile wastewaters.
Acknowledgments Sincere thanks are extended to the Associa-
tion of Universities and Colleges of Canada and International
Development Research Centre for their financial support.
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