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DOI 10.1007/s00521-012-1031-1
ORIGINAL ARTICLE
Şahset İrdemez
Received: 12 January 2012 / Accepted: 21 June 2012 / Published online: 6 July 2012
Ó Springer-Verlag London Limited 2012
Abstract In this investigation, firstly, Taguchi method was Keywords Taguchi-neural method Optimization
applied to determine the optimum specific energy consump- Energy consumption Electrocoagulation
tion (SEC) for dye removal from aqueous solution by elec-
trocoagulation using aluminum electrodes. An orthogonal
array (OA16) experimental design that allows to investigate 1 Introduction
the simultaneous variations of five parameters (Initial dye
concentration, Initial pH of the solution, Supporting electro- Wastewaters resulted from industries such as textile, dying,
lyte concentration, Supporting electrolyte type and Current printing cosmetics, food coloring, papermaking, etc. are the
density) having four levels was employed to evaluate the major source of colored effluents [1]. However, textile
effects of experimental parameters with two replicates. industries consume large amount of water and different
According to Taguchi-neural method, while the optimum type of dyes delivering color to wastewater. The dyes and
conditions that dye removal efficiency equals to 62.71 % were colors are toxic, and their adverse effects on fauna, flora,
found to be initial dye concentration 600 mg/L, initial pH of and human beings are well known [2]. The extensive use of
the solution 6, supporting electrolyte concentration 7.0 mM, dyes often causes pollution problems in the form of colored
supporting electrolyte type NaCl, and current density wastewater discharge into receiving environments. Even
0.10 mA/cm2. Under these optimum conditions, energy con- small quantities of dyes can color large water bodies,
sumption is 0.38 kW h/m3. Alternatively, it can be said that which not only affects from an esthetic point of view but
optimum conditions can be modified as follows supporting also reduces light penetration and photosynthesis. In
electrolyte concentration of 10.0 mM and supporting elec- addition, some dyes are either toxic or mutagenic and
trolyte type CaCl2, for 600 mg/L, initial dye concentration carcinogenic [2].
initial pH of the solution 6, and current density 0.10 mA/cm2. The conventional treatment techniques of wastewater
Under these optimum conditions, SEC and dye removal effi- including dyes involve biological oxidation, chemical
ciency are 0.45 kW h/m3 and 69.18 %, respectively. coagulation, advanced oxidation, and adsorption. Biologi-
cal treatment of colored wastewater is cheaper than other
methods, but it is less efficient for decolorization because
Y. Ş. Yildiz (&) of the toxicity of the wastewater and the need for an aer-
Department of Environmental Engineering, ation system [3].
Erciyes University, 38039 Kayseri, Turkey Various physical–chemical techniques are also available
e-mail: yyildiz@erciyes.edu.tr
for the removal of dyes from aqueous streams chemical
E. Şenyiğit coagulation followed by sedimentation and adsorption is
Department of Industrial Engineering, the widely used ones, but other advanced techniques are
Erciyes University, 38039 Kayseri, Turkey often applied, such as UV ozonation, ultrasonic decom-
position, or advanced oxidation processes [4–8].
Ş. İrdemez
Department of Environmental Engineering, Electrocoagulation used as an electrochemical water and
Atatürk University, 25240 Erzurum, Turkey wastewater treatment technology in its simplest form uses
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1062 Neural Comput & Applic (2013) 23:1061–1069
an electrochemical cell where a DC voltage is applied to predicted at a given input. In parameter design application,
the electrodes, usually made of iron or aluminum, and the some studies have combined the neural network technique
electrolyte is water or wastewater. EC involves the gen- with the Taguchi method to successfully solve some of the
eration of coagulant in situ by the dissolution of metal from problems traditionally associated with the Taguchi method,
the anode with simultaneous formation of hydroxyl ions specifying the failure to obtain the real optimum [17, 18].
and hydrogen gas at the cathode. This process produces the In this paper, Taguchi-neural method was applied to
corresponding aluminum or iron hydroxides and/or poly- determine the optimum Specific Energy Consumption
hydroxides. The generated gas also helps to float the floc- (SEC) by electrocoagulation using aluminum electrodes. In
culated particles at the water surface [9]. the Taguchi method, according to the control factors and
Electrocoagulation occurs via serial steps such as elec- their number of levels, the proper orthogonal arrays are
trolytic reactions at electrode surfaces, formation of coag- selected and the signal-to-noise ratios (SNRs) of the
ulants in aqueous phase, adsorption of soluble or colloidal experiment results are obtained to identify the relationship
pollutants on coagulants, which are removed by sedimen- between the parameters and the responses and to obtain the
tation or flotation. The metal ions generation takes place at primary optimums of the operating parameters. Further-
the anode hydrogen gas is released from the cathode. The more, each row in the orthogonal array, together with its
hydrogen gas would also help to float the flocculated par- relative responses, comprised a set of training patterns
ticles out of the water. The main reactions occurring at the (input/target pair) to the neural network. The trained neural
electrode are as follows: network can be used to determine the optimum specific
electric consumption (SEC) for the process of electroco-
Anode: Al(s) ! Al3þ ðaq) þ 3e ð1Þ
agulation for dye removal from aqueous solution.
Cathode: 3H2 O(l) þ 3e ! 3=2H2 ðg) þ 3OH ðaqÞ ð2Þ
Al3? and OH- ions generated by electrode reactions (1)
and (2) react to form various monomeric species such 2 Materials and methods
as Al(OH)2?, Al(OH)2?, Al2(OH)24?, Al(OH)4- and
polymeric species such as Al6(OH)153?, Al7(OH)174?, 2.1 Materials
Al8(OH)204?, Al13O4(OH)247?, Al13(OH)345?, which
transform finally into Al(OH)3(s) according to complex Bomaplex Red CR-L dye used in this study was supplied
precipitation kinetics [1, 10–12]. from a textile mill in Turkey (dye textile industry company
Gaziantep, Turkey), and the chemical structure of the dye
AlðaqÞ 3þ þ 3H2 OðlÞ ! Al(OH)3ðsÞ þ 3HðaqÞ þ ð3Þ was shown in Fig. 1.
Dye solutions were prepared by dissolving desired
On the other hand, the Taguchi method has attracted amounts of dye in 1 L of distilled water and used. All
increased attention. The Taguchi method, a leading opti- chemicals used were analytical grade and used without any
mization technique reducing the experimental cost, enables further treatment. Distilled water was used in all experi-
us to minimize the variability around the target when ments. Solutions were prepared from NaCl (Merck, 99.5 %
bringing the performance value to the target value. Another
advantage is that optimal working conditions determined
from the experimental work can also be reproduced in real
applications [13]. The parameter design used in Taguchi
method is the robust parameter design that integrates tra-
ditional engineering with statistics. It reduces the influence
of variations in environmental conditions and reduces
variations caused by product aging. However, the param-
eter levels selected to form the orthogonal array in the
Taguchi method are discrete, and thus the real optimum
can be only obtained from the available parameter levels.
The Taguchi method significantly reduces experimental
time and cost while simultaneously yielding reliable results
and products [13–16].
Artificial neural network (ANN), with its high learning
and nonlinear mapping ability, can precisely represent the
complex relationship between the input and output spaces.
In the trained neural model, the output can be accurately Fig. 1 Chemical structure of the Bomaplex Red CR-L dye
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Neural Comput & Applic (2013) 23:1061–1069 1063
Fig. 2 Schematic diagram of the experimental setup. 1 Water Artificial neural networks (ANNs) are systems that are
circulator. 2 Digital D.C. power supply. 3 Digital ampermeter.
4 Digital voltmeter. 5 Electrochemical reactor. 6 Digital magnetic
deliberately constructed to make use of some organiza-
stirrer tional principles resembling those of the human brain.
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1064 Neural Comput & Applic (2013) 23:1061–1069
Many different neural network models have been proposed There are four runs in each trial of the factor combi-
since the 1980s. ANNs, with their excellent learning and nation, namely y1 and y2, which can be treated as targets in
nonlinear mapping ability, can precisely represent the the ANN, and has a set of the different factors, which is a
complex relationships between the input and output spaces. set of five inputs in the ANN. Each row in the orthogonal
In ANNs, the Levenberg–Marquardt back propagation array has a set of five inputs and two targets, so there are
(LMBP) algorithm, with its high efficiency, high precision two input/target pairs. Overall, a total of 32 input/target
and ease of convergence, is applied in this study. The pairs in 16 trials are obtained. The 32 input/target pairs
details of LMBP can be found in the literature [19–22]. were divided into three subsets, including training, vali-
The number of hidden neurons will affect neural net- dation, and testing sets. Functionally, the input/target pairs
work performance. A large number of hidden neurons of 60 and 20 % were randomly selected for the training and
offers excessive flexibility and results in over fitting, but the validation sets, respectively, while the remaining 20 %
too few hidden neurons can constrain network learning served as the testing set. The required network can be
capability and limit its ability to approximate arbitrary acquired by using the neural network package software
accuracy. Therefore, in neural network design, the optimal Neurosolution.
number of hidden neurons is generally determined by In the Taguchi method, the number of the factorial level
comparing trained networks in different numbers of hidden in the L16 (24) orthogonal array used in this paper is four
neurons [21, 22]. This study applied the early stopping levels. It can be obtain which level at each factor is opti-
method to improve neural network generalization as Wu mum, but the actual optimum cannot be certain it may be
et al. [21, 22]. among the four levels. The Taguchi-neural method can
Table 2 Experimental variables, their levels, specific energy consumptions (SEC) dye removal efficiency results of conducted experiments
corresponding to L16 experimental plan
Exp. No Variables and their levels Specific energy consumption (kW h/m3) Dye removal efficiency (%)
(A) (B) (C) (D) (E) First Second Average Average
series series
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then construct relationships between the operating factors conductivity of the wastewater. It can be clearly seen that
and responses, so the intervals between the factorial levels SEC values for Exp. 1 are higher than that of Exp. 15 (See
can be divided into more desired levels, and which level is Table 2). The main difference of these experimental con-
the actual optimum can be determined precisely. The ditions is average applied potential values, which equal to
Taguchi approach is used to perform the experiments 4.93 and 1.22 V Exp. No 1 and 15, respectively.
according to the orthogonal array selected in this paper. It In Fig. 4a, effect of initial dye concentration on SEC has
uses the orthogonal array for experimental design and been presented. It can clearly be seen that as initial dye
signal-to-noise ratios (S/N) for the robust parameter design, concentration increases, SEC values decreases and it
and can optimize the output response and minimize the should be kept in mind that performance criteria—namely
variance of the output response. From Table 2, the experi- SEC—has been evaluated according to ‘‘Smaller is better’’
mental results can be acquired, and 32 input/target pairs thus for either this parameter or the others, optimum con-
can be organized to the ANN. In the ANN, all input/target ditions can be provided when S/N value calculated by
pairs presented can be utilized to train the network and get Eq. (4) equals to maximum. So, it can be concluded that
the outputs of the corresponding network. optimum condition for initial dye concentration is level 4
for which equals to 600 mg/L for this parameter.
Effect of the initial pH of the dye solution (pHi) on SEC
3 Results and discussions has been shown in Fig. 4b. When Fig. 4b examined, it can
be said that optimum condition for initial pH of the dye
3.1 Statistical analysis solution is fourth or third level of the parameter, which pHi
value equals to 6 and 5, respectively. For pHi, value of
Variation of Specific energy consumption (SEC) with time contribution to optimum SEC is highly close to each other.
can be seen in Fig. 3. Figure 3 was plotted using the data These contributions are -6.77 and -6.73 for pHi values 5
obtained from experiments 1 and 15. SEC was selected as and 6, respectively. Consequently, optimum condition for
performance criteria and calculated according to Eq. (6). initial pH is level 4, which equals to 6.
ðv I tÞ Figure 4c illustrates the effect of supporting electrolyte
SECðkW h=m3 Þ ¼ ð6Þ concentration on SEC. It can be seen from the figure, as
V
supporting electrolyte concentration rises, it provides more
where v is the applied potential, I is the current passing favorable results for energy consumption. As it would be
through the circuit, t is the reaction time, and V is the expected, optimum condition for SEC is the fourth level of
volume of the electrocoagulator. the parameter (CSE = 10.0 mM, See Table 1). Because
As it would be expected, calculated SEC values increase increasing supporting electrolyte concentration causes the
with reaction time, but all evaluations were conducted rising electrical conductivity of the wastewater. For
based on SEC values calculated according to reaction time example, when supporting electrolyte concentration has
of 60 min. Thus, average SEC values in Table 2 were been arranged in ascending order for NaCl, in Table 2 exp.
strongly influenced by two parameters namely Current numbers 1, 12, 14 and 7 have been obtained. In these
Density (CD) and applied potential. Current passing experimental conditions, values of average electrical conduc-
through the circuit—of course current density—is a func- tivity equal to 370.80, 690.20, 1,063.50 and 1,348.20 ls/cm,
tion of applied potential, which is related to electrical respectively.
Investigation of supporting electrolyte type has been
1.8 conducted using NaCl, NaNO3, Na2SO4, CaCl2 as seen in
1.6 Exp. No Table 1. Essentially, function of the supporting electrolyte
1.4 1 is increasing the electrical conductivity of the wastewater.
Not only in electrocoagulation but also in any other elec-
SEC (kW h/m 3)
1.2 15
trochemical process, the electrolysis voltage is one of
1.0
the most important operation variables. And it strongly
0.8
depends on the conductivity of water/wastewater, current
0.6
density, inter-electrode distance, and surface state of the
0.4 electrodes. Electrical conductivity is easily controllable
0.2 factor among the parameters mentioned above; using sup-
0.0 porting electrolyte, it can be said that NaCl and CaCl2
0 10 20 30 40 50 60 70
provide the highest contributions, which equal to -6.75
t (min.)
and -5.47, respectively, on SEC from the Fig. 4d, thus it
Fig. 3 Variation of SEC values as a function of reaction time can be concluded that real optimum supporting electrolyte
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Fig. 4 a Effect of initial dye concentration level parameter on level parameter on optimization criteria. d Effect of supporting
optimization criteria. b Effect of initial pH level parameter on electrolyte type level parameter on optimization criteria. e Effect of
optimization criteria. c Effect of supporting electrolyte concentration current density level parameter on optimization criteria
type is NaCl, whereas according to Fig. 4d, optimum real concentration), A (Initial dye concentration), and D (sup-
optimum supporting electrolyte type should be CaCl2. porting electrolyte type) are the significant parameters that
Figure 4e demonstrates the effect of current density on affect the quality characteristic (SEC). When evaluated the
SEC. According to Fig. 4e, optimum condition for current ANOVA table, initial dye concentration is one of the least
density is the first level (0.25 mA/cm2). In all electro- significant parameter on SEC. Because it strongly related
chemical processes, current passing through the circuit—of production process, it cannot be controlled. While the other
course current density—is highly effective parameter, parameters such as supporting electrolyte type, supporting
based on removal efficiency because it determines the electrolyte concentration, current density, and initial pH
amount of coagulant released to the reactor in electroco- can be easily controlled. For this reason, current density,
agulation process. Additionally, it is one of the two com- supporting electrolyte concentration, and supporting elec-
ponents for SEC together with applied potential. trolyte type have been taken into account in this study.
Using ANOVA results as shown in Table 3, the control Figures 5 and 6 show the relationship among the current
factors E (Current Density), C (supporting electrolyte density, supporting electrolyte concentration, supporting
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1a 4 600 4 6 b
7 1 NaCl b
0.1 0.38 0.487 0–2.562
b
2 4 600 4 6 4 10 4 CaCl2 0.1 0.45 0.660 0–2.735
a
Optimum conditions
b
Interval desired levels according to Taguchi-neural method
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