Desalination 286 (2012) 200–209

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Desalination
journal homepage: www.elsevier.com/locate/desal

Optimization of baker's yeast wastewater using response surface methodology

by electrocoagulation
Erhan Gengec a, Mehmet Kobya b,⁎, Erhan Demirbas c, Abdurrahman Akyol b, Kadriye Oktor a
a
University of Kocaeli, Department of Environmental Protection, 41275, Izmit, Kocaeli, Turkey
b
Gebze Institute of Technology, Department of Environmental Engineering, 41400, Gebze, Turkey
c
Gebze Institute of Technology, Department of Chemistry, 41400, Gebze, Turkey

a r t i c l e i n f o a b s t r a c t

Article history: In the present paper, electrocoagulation (EC) was employed for removals of color, chemical oxygen demand
Received 20 July 2011 (COD) and total organic carbon (TOC) from baker' s yeast effluents (BYEs) in a batch EC reactor using alumin-
Received in revised form 5 November 2011 ium electrodes. Optimizations of anaerobic (AE) and anaerobic–aerobic effluents (AAE) were carried out by
Accepted 7 November 2011
response surface methodology to describe interactive effects of the three main process independent param-
Available online 2 December 2011
eters (initial pHi, current density and operating time) on removal efficiencies of color, COD and TOC. The re-
Keywords:
sponses were related to maximize color, COD and TOC removal efficiencies and to minimize operating cost in
Electrocoagulation the EC process. The quadratic model fitted very well with the experimental data. R2 correlation coefficients
Baker's yeast wastewater (> 95%) for the removal efficiencies showed a high significance of the model. The maximum color, COD
Response surface methodology and TOC were 88%, 48% and 49% at 80 A/m 2, pHi 4 and 30 min for AE and 86%, 49% and 43% at 12.5 A/m 2,
Optimization pHi 5 and 30 min for AAE, respectively. The operating costs for AE and AAE at the optimized conditions
Operating cost were 0.418 €/m 3 and 0.076 €/m 3.
© 2011 Elsevier B.V. All rights reserved.

1. Introduction Various treatment methods like biological process, viz. anaerobic,

The industrial production of baker's yeast by fermentation that
generally uses molasses as the raw materials includes operations
and processes such as molasses preparation, fermentation, and sepa-
ration and drying of yeast and produces a large quantity of wastewa-
ter [1,2]. There are basically two types of wastewaters; one is high
strength process wastewater that originates from yeast separators
and processes such as centrifuges and rotary vacuum filters, and the
other one is low-medium strength process wastewater that originates
from floor washing and equipment cleaning [3]. The baker's yeast
wastewaters (BYW) are characterized by extremely high chemical
oxygen demand (COD, 80,000–100,000 mg/L) and biochemical oxy-
gen demand (BOD, 40,000–50,000 mg/L), apart from low pH 4–5,
strong odor and a large amount of dark brown color [1,4]. The dark
brown color in these effluents is imparted by the pigment called mel-
anoidins which is refractory in nature to the biological treatment and
resistance to biodegradation, not disappear and can even increase due
to re-polymerization of colorants [5,6]. The dark brown color from
baker's yeast effluents (BYEs) interferes with the absorption of sun-
light which reduces the natural process of photochemical reactions
for self-purification of the surface waters.
⁎ Corresponding author. Tel.: + 90 262 6053214; fax: + 90 262 6538490.
E-mail address: kobya@gyte.edu.tr (M. Kobya).
aerobic, physico-chemical treatment, viz. adsorption, membrane pro-
cess, reverse osmosis, coagulation/flocculation and oxidation processes,
viz. ozone, Fenton have been attempted for the treatment of BYEs. Cur-
rent biological treatment of BYEs involves combinations of anaerobic
digestion and aerobic systems that successfully reduce BOD to accept-
able limits, but does not deal effectively with either the dark color or
the associated COD that remains and limits the reuse/recycling of the
process water [6–8]. Moreover, anaerobic treatment is a slow process
and typically requires long start-up periods. Treatment by oxidation
technologies is generally effective on the color but not COD, membrane
filtration processes are prone to fouling [2,9], and reverse osmosis gen-
erates a high salinity retentate that presents disposal difficulties [10].
Chemical coagulation and adsorption remove color and COD relatively
effectively, but has a number of drawbacks such as requirements for
high amount of inorganic coagulants, regeneration of adsorbent, cost
limitation on a large scale, etc. [11]. Decolorization through chemical
treatment with ozone [12,13], Fenton's reagent [14] and H2O2/UV
[15] leads to temporary color reduction because of transformation of
the chromospheres groups therefore, these are not preferred solutions.
As a result, the above treatment processes are disadvantaged for in-
stance, high equipment and operational cost, less effective decoloriza-
tion rate and simultaneous generation of hazardous secondary
pollutants in treated effluents. For these reasons, the BYEs require an
alternative treatment technologies in terms of relatively simple and ef-
fective in removals of color, COD and total organic carbon (TOC) before
its safe disposal into the environment [7].

0011-9164/$ – see front matter © 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.desal.2011.11.023
 E. Gengec et al. / Desalination 286 (2012) 200–209 201

In recent years, electrocoagulation (EC) has the potential to exten- Table 2

sively eliminate the disadvantages of the classical treatment tech- Process factors and their levels for AE.

niques and to achieve a sustainable and economic treatment of agro Factor Variables Range of actual and coded variables
industrial wastewater [16–24]. The EC process is characterized by
−2 −1 0 +1 +2
simple and easy operated equipment, short operation time, no addi-
x1 initial pH 3.32 4.00 5.00 6.00 6.68
tion of chemicals and low sludge production. Moreover, advantages
x2 current density (A/m2) 39.77 50.00 65.00 80.00 90.23
of the EC compared to conventional chemical coagulation include re- x3 operating time (min) 3.18 10.00 20.00 30.00 36.82
duced wastewater acidification and salinity, low dosage of coagulant,
superior coagulant dispersion and intrinsic electroflotation separa-
tion capability. Iron (Fe) or aluminium (Al) is generally employed as
a sacrificial electrode material in the EC process. In an EC process, 3þ þ
Al þ 3H2 O→AlðOHÞ3ðsÞ þ 3H ð6Þ
the coagulating ions are produced in situ involving three successive
stages: (i) formation of coagulants by electrolytic oxidation of the
sacrificial electrode such as Fe or Al, (ii) destabilization of the contam- The concentration of hydrolyzed aluminium species depends on
inants, particulate suspension and breaking of emulsions and (iii) ag- the aluminium concentration and the solution pH. The hydrolysis
gregation of the destabilized phases to form flocs. Fe/Al gets dissolved constants for aluminium cover a very narrower range, and all of the
from the anode generating corresponding metal ions, which almost aluminium deprotonations are ‘squeezed’ into an interval of less
immediately hydrolyze to polymeric iron or aluminium oxyhydrox- than 2 pH unit. Therefore, apart from a narrow pH region approxi-
ides. These polymeric oxyhydroxides are excellent coagulating mately 5–6, the dominant soluble species are Al 3+ and Al(OH) −4 at
agents. When aluminium electrodes in the EC process are used as low pH and high pH, respectively [25].
an anode and a cathode, the main reactions are at the anode as fol- COD and TOC successfully reduced with anaerobic and aerobic
lows: treatment processes from BYW, but there are no considerable remov-
3þ − al efficiencies of color from these effluents. The novelty of this study is
Al→Al þ 3e ð1Þ to use the EC process using Al electrodes for the first time to both
Also, oxygen evolution can compete with aluminium dissolution treat anaerobic (AE) and anaerobic–aerobic (AAE) effluents to
at the anode via following reaction: achieve the higher removal percentage of color as well as COD and
TOC to acceptable discharge limits and optimize using response sur-
þ −
2H2 O→O2ðgÞ þ 4H þ 4e ð2Þ face methodology (RSM). Optimizations of AE and AAE were carried
out by the RSM which was used to develop a mathematical model
At cathode, hydrogen evolution takes place via the following reac- to describe the effects and relationships of the main process indepen-
tion. It helps in floatation of the flocculated particles out of the water dent variables (initial pHi, current density and operating time), to
[19]. maximize color, COD and TOC removal efficiencies and to minimize
− 3 − operating cost in relation to energy and electrode consumptions.
3H 2 O þ 3e → =2 H 2 þ 3OH ð3Þ

2. Materials and methods

At high pH values, OH − generated at the cathode during hydrogen
evolution may attack the cathode by the following reaction [26].
2.1. Characterizations of AE and AAE
− −
2Al þ 6H2 O þ 2OH →2AlðOHÞ4 þ 3H2ðgÞ ð4Þ
A manufacturing factory producing of baker's yeast located in
Al3+ and hydroxyl ions generated by electrode reactions: Eqs. (1) Kocaeli, Turkey has a full scale two-stage anaerobic and aerobic bio-
and (4) to form various monomoric-polymeric species such as Al logical treatment plant. The inlet flow rate of the plant is 1050 m 3/
(OH) 2+, Al(OH)+2, Al(OH) −4, Al2(OH)4+2, Al6(OH)3+15, Al7(OH)4+17, day. The high strength wastewaters are treated initially in the anaer-
Al8(OH)4+20, Al13O4(OH)7+24, and Al13(OH)5+34 transformed initially obic stage and then are combined with the low strength wastewaters
into Al(OH)3(s) and finally polymerized to Aln(OH)3n (Eqs. (5) and to be treated in the aerobic stage. The total COD removals of the two-
(6)) in the solution [16,19,25]: stage treatment plant are in the range 80–90%, but the color removal
efficiency is very low. Two wastewater samples collected from AE and
nAlðOHÞ3 →Aln ðOHÞ3n ð5Þ AAE were characterized (Table 1) and kept in refrigerators at 4 °C be-
fore use.
Table 1
Characterizations of effluents from the treatment plant of the BYW. 2.2. Experimental set-up and procedure
Parameters Anaerobic Anaerobic treated Aerobic treated
treated influent effluent (AE) effluent (AAE) The EC treatment was carried out in a batch electrolytic reactor
pH 5.6 7.2 7.7 made from Plexiglas material with dimensions of
Temperature (°C) 24 30 25 100 mm × 100 mm × 130 mm. Four aluminium electrodes in the reac-
Conductivity (mS/cm) 17.24 17.42 7.46 tor were used as cathodes and anodes with effective dimensions of
TS (g/L) 22.2 15.2 5.1
TVS (g/L) 10.3 4.5 0.72
TSS (g/L) 1.01 5.08 0.04
Alkalinity (mg/L) 750 4130 1050 Table 3
COD (mg/L) 27920 2160 544 Process factors and their levels for AAE.
TOC (mg/L) 6090 919 184
Color (Abs475nm/cm) 2.50 1.91 0.66 Factor Variables Range of actual and coded variables
Absorbance (Abs254nm/cm) 2.92 2.78 2.72 −2 −1 0 +1 +2
TKN (mg/L) 648 421 39
NH3-N (mg/L) 560 297 19 x1 initial pH 4.32 5.00 6.00 7.00 7.68
TP (mg/L) 17.5 12.8 2.05 x2 current density (A/m2) 2.44 5.00 8.75 12.5 15.06
PO4-P (mg/L) 9.75 9.72 1.79 x3 operating time (min) 3.18 10.00 20.00 30.00 36.82
202 E. Gengec et al. / Desalination 286 (2012) 200–209

Table 4
CCD of the experimental variables for AE.

Variables Removal efficiency Consumptions and costs

x1: pHi x2: CD x3: tEC Re,colour Re,COD Re,TOC ENC ELC OC Wsludge pHf
2 3 3 3 3
(−) (A/m ) (min) (%) (%) (%) (kWh/m ) (kg/m ) (€/m ) (kg/m )

1 6.00 50.0 10.00 42 22 22 0.725 0.099 0.216 1.052 6.24

2 4.00 50.0 30.00 85 44 40 1.665 0.289 0.595 1.602 5.18
3 5.00 90.2 20.00 85 43 43 2.414 0.359 0.766 1.865 5.84
4 4.00 80.0 10.00 78 40 41 1.028 0.161 0.339 1.844 4.91
5 5.00 39.8 20.00 72 35 34 0.788 0.146 0.297 1.194 5.52
6 6.00 80.0 10.00 61 25 22 0.952 0.152 0.319 1.067 6.31
7 5.00 65.0 20.00 80 41 41 1.294 0.251 0.508 1.608 5.70
8 5.00 65.0 20.00 80 38 40 1.372 0.256 0.520 1.394 5.73
9 5.00 65.0 20.00 80 36 37 1.528 0.256 0.532 1.675 5.70
10 5.00 65.0 20.00 79 35 37 1.534 0.261 0.542 1.641 5.68
11 4.00 50.0 10.00 66 34 33 0.677 0.099 0.212 1.027 4.86
12 5.00 65.0 20.00 80 36 37 1.432 0.256 0.526 1.550 5.72
13 5.00 65.0 36.82 82 40 38 3.255 0.480 1.026 2.082 5.99
14 6.68 65.0 20.00 61 24 26 1.326 0.253 0.512 1.445 7.02
15 3.32 65.0 20.00 80 43 43 1.456 0.258 0.531 1.574 4.89
16 6.00 80.0 30.00 78 32 36 3.180 0.459 0.987 2.121 6.64
17 5.00 65.0 3.18 41 20 16 0.297 0.041 0.090 1.123 5.25
18 5.00 65.0 20.00 79 36 35 1.432 0.256 0.526 1.550 5.71
19 6.00 50.0 30.00 68 28 27 1.800 0.319 0.644 1.657 6.54
20 4.00 80.0 30.00 88 48 49 3.600 0.474 1.040 2.359 5.55

80 mm × 50 mm × 3 mm. Total effective areas of electrodes were
240 cm 2. The electrodes were situated 5 mm apart from each other
and connected to monopolar parallel connection mode.
Before each run, the electrodes were dipped into solutions of HCl
(35%) and hexamethylenetetramine (2.8%) to remove the oxide
and/or passivation layers from the electrodes [16]. The electrodes
were placed in the reactor and solutions were mixed at 300 rpm in
the EC reactor. In each run, 0.8 L sample was placed into the EC reac-
tor. The current density (CD) was adjusted by a digital DC power sup-
ply (TDK-Lambda Genesys model; 50V-30A) operated at
galvanostatic mode and the experiment was started. At the end of
the run, the electrodes were washed thoroughly with water to
remove any solid residues on the surfaces, dried and reweighed. All
experiments were performed at 25 °C.
2.3. Analytical method
The samples taken from the EC reactor at different operating times
were filtered using a 1.6 μm Whatman glass microfiber filter. Total
COD and TOC were measured according to standard methods [26].
COD was measured by closed reflux titrimetric method and TOC
levels were determined through combustion of the samples at
680 °C using a non-dispersive IR source (Tekmar Dohrmann Apollo
9000). pH of sample was adjusted with H2SO4 or NaOH and measured

Table 5
CCD of the experimental variables for AAE.

Variables Removal efficiency Consumptions and costs

x1: pHi x2: CD x3: tEC Re,color Re,COD Re,TOC ENC ELC OC Wsludge pHf

(−) (A/m2) (min) (%) (%) (%) (kWh/m3) (kg/m3) (€/m3) (kg/m3)

1 4.32 8.8 20.00 75 38 30 0.145 0.030 0.060 0.219 5.02

2 6.00 2.4 20.00 19 4 21 0.030 0.009 0.017 0.144 6.12
3 5.00 12.5 30.00 86 49 43 0.301 0.068 0.134 0.257 5.46
4 7.00 12.5 30.00 55 27 27 0.337 0.069 0.138 0.332 7.30
5 6.00 8.8 3.18 18 1 10 0.026 0.010 0.018 0.066 6.14
6 6.00 8.8 20.00 55 24 23 0.142 0.030 0.060 0.188 6.18
7 7.00 5.0 30.00 22 10 12 0.095 0.030 0.056 0.283 7.39
8 7.00 12.5 10.00 22 4 12 0.095 0.038 0.069 0.145 7.24
9 7.68 8.8 20.00 25 10 10 0.121 0.030 0.057 0.201 7.90
10 6.00 15.1 20.00 75 30 36 0.303 0.064 0.127 0.263 6.21
11 6.00 8.8 20.00 57 21 21 0.137 0.033 0.064 0.214 6.17
12 6.00 8.8 36.82 72 30 26 0.222 0.056 0.109 0.346 6.27
13 6.00 8.8 20.00 61 18 22 0.132 0.033 0.064 0.230 6.16
14 6.00 8.8 20.00 56 21 21 0.137 0.033 0.064 0.214 6.18
15 7.00 5.0 10.00 8 4 5 0.046 0.010 0.021 0.052 7.15
16 5.00 5.0 10.00 50 12 12 0.039 0.011 0.021 0.161 5.27
17 5.00 12.5 10.00 71 29 29 0.103 0.032 0.059 0.215 5.22
18 6.00 8.0 20.00 57 25 25 0.130 0.034 0.065 0.195 6.18
19 6.00 8.8 20.00 53 23 23 0,142 0,034 0,066 0,243 6.17
20 5.00 5.0 30.00 60 28 31 0,096 0,028 0,053 0,273 5.40
 E. Gengec et al. / Desalination 286 (2012) 200–209 203

Table 6
Observed (actual) and predicted values of responses for AE and AAE.

Anaerobic effluent Anaerobic–aerobic effluent

Run Re,color(%) Re,COD(%) Re,TOC(%) Re,colour(%) Re,COD(%) Re,TOC(%)

Pre. Act. Pre. Act. Pre. Act. Pre. Act. Pre. Act. Pre. Act.

1 42.00 42.07 22.00 21.33 22.00 20.82 75.00 80.04 38.00 39.79 30.00 30.97
2 85.00 85.35 44.00 43.61 40.00 39.11 19.00 23.81 4.00 5.52 21.00 18.68
3 85.00 87.27 43.00 42.82 43.00 43.96 86.00 90.59 49.00 50.16 43.00 42.67
4 78.00 74.36 40.00 38.1 41.00 37.81 55.00 60.34 27.00 25.57 27.00 24.60
5 72.00 71.04 35.00 35.23 34.00 33.82 18.00 24.93 1.00 2.47 10.00 7.48
6 61.00 59.72 25.00 25.29 22.00 22.34 55.00 56.50 24.00 21.94 23.00 22.53
7 80.00 79.63 41.00 37.00 41.00 37.81 22.00 26.78 10.00 11.12 12.00 14.51
8 80.00 79.63 38.00 37.00 40.00 37.81 22.00 24.99 4.00 5.41 12.00 14.61
9 80.00 79.63 36.00 37.00 37.00 37.81 25.00 19.93 10.00 10.19 10.00 8.16
10 79.00 79.63 35.00 37.00 37.00 37.81 75.00 70.16 30.00 30.14 36.00 37.45
11 66.00 63.71 34.00 32.65 33.00 32.21 57.00 56.50 21.00 21.94 21.00 22.53
12 80.00 79.63 36.00 37.00 37.00 37.81 72.00 65.04 30.00 30.49 26.00 27.65
13 82.00 79.51 40.00 38.11 38.00 36.13 61.00 56.50 18.00 21.94 22.00 22.53
14 61.00 58.85 24.00 22.37 26.00 24.47 56.00 56.50 21.00 21.94 21.00 22.53
15 80.00 83.46 43.00 44.77 43.00 45.31 8.00 3.44 4.00 1.46 5.00 5.95
16 78.00 79.36 32.00 33.25 36.00 36.24 50.00 44.68 12.00 12.04 12.00 15.01
17 41.00 44.80 20.00 22.11 16.00 18.65 71.00 66.24 29.00 26.50 29.00 27.18
18 79.00 79.63 36.00 37.00 35.00 37.81 57.00 56.50 25.00 21.94 25.00 22.53
19 68.00 70.72 28.00 29.79 27.00 29.72 53.00 56.05 23.00 21.94 23.00 22.53
20 88.00 87.00 48.00 48.57 49.00 49.63 60.00 57.03 28.00 25.20 31.00 29.00

by pH meter (WTW Inolab pH 720). Color contents in the AE and AAE model by least squares technique. RSM makes it possible to represent
were measured using a UV–vis spectrophotometer at 475 nm independent process parameters in quantitative form as:
(Perkin-Elmer 550 SE) [27]. Amount of sludge produced after the EC
process was determined after the sludge was placed in an oven at
y ¼ f ðx1 ; x2 ; x3 ;…; xn Þ  ε ð7Þ
105 °C for 24 h.

2.4. Experimental design and data analysis
The Design Expert 8.0.4 software (trial version) was used for the
statistical design of experiments and data analysis. The three most
important operating variables: initial wastewater pH (x1), current
density (x2) and operating time (x3) were optimized for both waste-
waters. Their range and levels were shown in Tables 2 and 3 for AE
and AAE, respectively. The independent variables' ranges and levels
were determined from preliminary experiments [28–30].
RSM is a collection of mathematical and statistical techniques,
commonly used for improving and optimizing processes. It can be
used to evaluate the relative significance of several affecting factors
in the presence of complex interactions [29–33]. RSM uses an exper-
imental design such as the Central Composite Design (CCD) to fit a
where y is the response (yield), f is the response function, ε is the ex-
perimental error and x1, x2, x3,….,xn are independent parameters. By
plotting the expected response of y, a surface known as the response
surface is obtained. A higher order polynomial such as the quadratic
model (Eq. (8)) was used in this study. Analysis of variance
(ANOVA) was used to obtain the interaction between the process var-
iables and the responses. The quality of the fit polynomial model was
expressed by R 2, and its statistical significance was checked by the
Fisher F-test in the same program. Model terms were evaluated by
the P value (probability) with 95% confidence level.
2 2 2
y ¼ β0 þ β1 x1 þ β2 x2 þ β3 x3 þ β11 x1 þ β22 x2 þ β33 x3 þ β12 x1 x2
þ β13 x1 x3 þ β23 x2 x3 ð8Þ

Table 7
Coefficients of the response functions.

Responses β0 β1 β2 β3 β11 β22 β33 β12 β13 β23

Anaerobic effluent (AE)

Re,Colour (%) 79.63 − 7.32 4.82 10.32 − 3.00 − 0.17 − 6.18 1.75 1.75 − 2.25
Re,COD (%) 37.00 − 6.66 2.23 4.73 − 1.21 0.73 − 2.45 − 0.37 − 0.62 − 0.12
Re,TOC (%) 37.81 − 6.19 3.01 5.20 − 1.03 0.38 − 3.68 − 1.00 0.50 1.25
ENC (kWh/m3) 1.43 − 0.039 0.49 0.87 0.0077 0.082 0.14 − 0.085 − 0.032 0.34
ELC (kg/m3) 0.26 − 5.86 × 10− 4 0.059 0.13 – – – − 6.10− 3 0.0023 0.027
OC (€/m ) 3
0.53 − 3.74 × 10− 3 0.13 0.27 − 8 × 10− 5 3.48 × 10− 3 0.013 − 0.016 1.46 × 10− 3 0.07
Wsludge (kg/m3) 1.57 − 0.085 0.23 0.32 – – – − 0.14 0.071 0.049
Anaerobic–aerobic effluent (AAE)
Re,Colour (%) 56.50 − 17.87 13.78 11.92 − 2.30 − 3.36 − 4.07 0.001 2.75 3.00
Re,COD (%) 21.94 − 8.79 7.23 8.33 1.07 − 1.40 − 1.93 − 2.62 − 0.87 2.63
Re,TOC (%) 22.52 − 6.78 5.58 6 − 1.05 1.96 − 1.75 − 0.87 − 1.37 0.38
ENC (kWh/m ) 3
0.14 − 6.19 × 10− 4 0.075 0.064 − 0.0018 0.01 0.0049 2.78 × 10− 3 4.44 × 10− 3 0.042
ELC (kg/m3) 0.033 5.09 × 10− 4 0.016 0.013 − 5.49 × 10− 4 1.79 × 10− 3 6.6 × 10− 4 6.72 × 10− 4 − 3.28 × 10− 4 3.9 × 10− 3
OC (€/m3) 0.064 7.9 × 10− 4 0.032 0.027 − 1.04 × 10− 3 3.68 × 10− 3 7.5 × 10− 4 1.3 × 10− 3 − 2.2 × 10− 4 9.4 × 10− 3
Wsludge (kg/m3) 0.21 − 9.1 × 10− 3 0.028 0.076 – – – 0.013 0.033 − 0.014
204 E. Gengec et al. / Desalination 286 (2012) 200–209

Table 8 showed for both of wastewaters in these tables. The effects of x1, x2
ANOVA results for the EC process applied to AE. and x3 investigated on color, COD, TOC removal efficiencies and
Response R2 Adj. R2 SD CV PRESS F-value Prob > F AP amounts of ENC, ELC, OC and Wsludge were determined using approx-
imating functions. Observed (actual) and predicted values of re-
Re,color (%) 0.98 0.96 2.74 3.74 562 47.81 b0.0001 23.3
Re,COD (%) 0.96 0.92 2.22 6.36 230 25 b0.0001 17.3 sponses, and coefficients of the response functions for AE and AA
Re,TOC (%) 0.95 0.91 2.56 7.34 356 21 b0.0001 17.1 were shown in Tables 6 and 7. The R 2 coefficient gave the proportion
ENC (kWh/m3) 0.99 0.99 0.10 6.37 0.55 162 b0.0001 43.9 of the total variation in the response variable accounted for the pre-
ELC (kg/m3) 0.99 0.99 b 0.01 2.28 b 0.10 1369 b0.0001 126.2
dictors (x's) included in the model. A high R 2 value, close to 1, was de-
Wsludge (kg/m3) 0.95 0.92 0.10 6.64 0.55 37 b0.0001 20.9
sirable and a reasonable agreement with the quadratic model to the
SD: Standard Deviation, CV: Coefficient of Variance, PRESS: Predicted Residual Error experimental data (Tables 4 and 5).
sum of squares, AP: Adequate Precision, P: Probability of Error.
The RSM was used for analyzing the relationship of three variables
(initial pH, current density and operating time) and process re-
sponses such as color, COD, and TOC removal efficiencies, amounts
The predicted response (y) is therefore correlated to the set of re- of electrode (ELC) and energy (ENC) consumptions, and amount of
gression coefficients (β): the intercept (β0), linear β1, β2, β3), interac- sludge (Wsludge). Adequacy of the RSM was justified through ANOVA
tion (β12, β13, β23) and quadratic coefficients (β11, β22, β33). and the results were shown in Tables 8 and 9.
The F-statistics values were higher and its values for AAE and AE
2.5. Operating cost were 27–48 for colour, 48–25 for COD and 28–21 for TOC removals,
respectively. The large F-values indicated that most of the variation
The operating cost (OC) of the EC process includes material, main- in the response could be explained by the regression model. The
ly electrodes and electrical energy costs, as well as labour, mainte- Prob > F values for the AAE and the AE from the ANOVA was less
nance, sludge dewatering and disposal, and fixed costs. The latter than 0.05 showed that the model was considered to be statistically
cost items are largely independent of the type of the electrode mate- significant. In this study, values of Prob > F were b0.0001 for both of
rial [34,35]. In this study, energy and electrode material costs were the models. The coefficient of variance (CV) as the ratio of the stan-
taken into account as major cost items in the calculation of the OC dard error of estimate to the mean value of the observed response
(€/m 3): (as a percentage) was a measure of reproducibility of the model. CV
was considered to be reproducible when it is not greater than 10%.
OC ¼ aENC þ bELC þ cCC ð9Þ As shown in Tables 8 and 9, values of CV for AE and AAE were 3.4–
12.6% for color, 6.4–12.8% for COD and 7.3–11.9% for TOC removals.
where ENC is energy consumption (kWh/m 3) and ELC is electrode The adequate precision (AP) measures the signal to noise ratio and
consumption (kg/m 3). Prices provided in the Turkish market in June AP was compared for the range of the predicted values at the design
2011 for a and b were 0.072 €/kWh for electrical energy and 1.65 €/ points to the average prediction error. The AP values greater than 4
kg for Al electrode material. c stands for chemical consumption (CC, indicated an adequate signal for all responses of AAE and AE
kg/m 3) such as NaOH (0.73 €/kg) and H2SO4 (0.29 €/kg) for adjust- (Tables 8 and 9). Therefore, the quadratic model could be used to nav-
ment of a desired pH. Costs for electrical energy (kWh/m 3) in igate the design space. A higher value of R 2 (>0.95 for all responses in
Eq. (10) and electrode consumptions (kg/m 3) were calculated from AE and AAE) showed that the model could explain the response suc-
Faraday's Law in Eq. (11): cessfully (Fig. 1).
Actual values were the measured response data for a particular
U  i  t EC
ENC ¼ ð10Þ run, and the predicted values were evaluated from the model and
v
generated by using the approximating functions. It was seen in
i  t EC  Mw Fig. 1 that the data points lay close to the diagonal line and the devel-
ELC ¼ ð11Þ oped model was adequate for the prediction of each response.
zF v

where U is cell voltage (V), i is current (A), tEC is operating time (s) 3.2. Effect of variables on the color, COD and TOC removals
and v is volume (m 3) of the wastewater, Mw is molecular mass of al-
uminium (26.98 g/mol), zAl is number of electron transferred The effects of x1, x2 and x3 were investigated on color, COD, TOC
(zAl = 3,) and F is Faraday's constant (96487 C/mol). removal efficiencies and amounts of OC were determined using ap-
proximating functions. A quadratic model (Eq. (8)) fitted very well
3. Results and discussion with the experimental data and estimated coefficients of functions
are given in Table 7 for AE and for AAE.
3.1. Statistical analysis 3D surface plots for AE and AAE in Figs. 2 and 3 were shown to vi-
sualize the effects of experimental factors on removal efficiencies of
The actual designs of this work for AE and AAE were presented in color and COD responses. As seen from Figs. 2 and 3 and Tables 4
Tables 4 and 5. The CCD in the form of a 2 3 full factorial design with and 5, color, COD and TOC removal efficiencies showed the similar re-
six additional experimental trials as replicates of the central point moval trends with experiments results. The maximum removal of
colour, COD and TOC were presented in Tables 4 and 5 as 88%, 48%
and 49% at 80 A/m 2, pHi 4 and 30 min for AE and 86%, 49% and 43%
Table 9 at 12.5 A/m 2, pHi 5 and 30 min for AAE, respectively. It is well-
ANOVA results for the EC process applied to AAE. known that current density and operation time not only determine
Response R2 Adj. R2 SD CV PRESS F-value Prob > F AP the coagulant rate but also the bubble production rate, size and the
flocs growth which can influence the treatment efficiency and operat-
Re,color (%) 0.96 0.92 6.26 12.56 2796 27 b 0.0001 19.7
Re,COD (%) 0.98 0.96 2.62 12.79 352 48 b 0.0001 26.4 ing cost of the EC process. The effect of current density shown in
Re,TOC (%) 0.96 0.93 2.61 11.91 481 28 b 0.0001 19.9 Figs. 2–4 was studied in the range 39.8–90.2 A/m 2 for AE and 2.4–
ENC (kWh/m3) 0.99 0.98 0.01 9.19 0.01 101 b 0.0001 34.6 15.1 A/m 2 for AAE, respectively. The maximum color, COD and TOC
ELC (kg/m3) 0.99 0.99 b 0.01 6.08 b0.01 159 b 0.0001 40.9 removal efficiencies were obtained at 80 A/m 2 for AE (run 20) and
Wsludge (kg/m3) 0.97 0.95 0.02 7.96 b0.01 60 b 0.0001 30.7
12.5 A/m 2 for AAE (run 3). On the other hand, increasing of the
 E. Gengec et al. / Desalination 286 (2012) 200–209
Fig. 1. Comparisons of predicted and experimental values for AE (a–c) and AAE (d–f).
operation time showed also the same trend. When all factors held
constant (runs 7, 13 and 17) in Table 4 expect for the operating
time, the color removal efficiencies for AE were 41%, 80% and 82%
for 3.2, 20.0 and 36.8 min of the operation time and runs 5, 6 and 12
in Table 5 showed the removal efficiencies of color for AAE as 18%,
55% and 72% for 3.18, 20 and 36.82 min of the operation time, respec-
tively. The high current density and operation time led to increase in
color, COD and TOC removal efficiencies because the high current den-
sity and the operating time in the EC process increased the amount of
metal species formed by dissolution of the anode calculated from Fara-
day's law (Eq. (11)). Higher removal efficiency was realized by a great-
er amount of dissolved Al3 + during the EC process. ENC was closely
related to over potential and time as described in Eq. (10). Perturbation
plots of ELC and ENC showed that there was no significant effect of ini-
tial pH on energy and electrode consumptions (Fig. 4).
When compared to traditional chemical treatments, the EC has
some advantages since less coagulant is required and less sludge is
formed. Nevertheless amount of sludge produced during the EC pro-
cess is an environmental problem of solid waste generation and an
economical problem due to the high disposal costs. In the EC process,
amount of sludge production depended on removal efficiency of pol-
lutants and metal ions dissolution at electrode and its species in solu-
tion. Generally sludge was separated by gas bubbles formed at
electrode (sludge flotation) and by sedimentation. Amount of sludge
production was affected by initial pH, current density and operation
time for AE and AAE. As seen in Table 4, amount of sludge produced
during the EC process was determined in runs 3, 5 and 7 and runs
17, 12 and 13 as 1.865, 1.608 and 1.194 kg/m 3 for current densities
of 90.2, 65.0 and 39.8, and 1.123, 1550 and 2.082 kg/m 3 for operating
time of 3.2, 20.0 and 36.8 min, respectively. As mentioned the above,
205
a greater amount of coagulant and removal efficiency of pollutants
resulted in a greater amount of sludge with respect to high current
density, operation time and low pH.
Removal of dissolved organic compounds with different functional
groups in the AE and AAE can occur at initial pHi 4–6 where the max-
imum removals were obtained for color, COD and TOC (final pH was
5–6 after the treatment). Initial pHi and final pHf are the most impor-
tant parameter due to solution affected for production of polymeric
Al-species and hydroxyl ions by the EC reactions and chemical struc-
ture of wastewaters. Final pHf affected the removal rate of pollutants
in the BYEs. Dissolved organic molecules such as melanoidins in the
BYEs are acidic, polymeric and highly dispersed colloids which are
negatively charged due to the dissociation of carboxylic, hydroxyl
and phenolic groups [36–40]. The most active functional groups are
carboxyl and phenolic hydroxyl groups, and dissociation of H + relates
to the pH of the solution. When enough amount of coagulant electro-
chemically produced at anode and increased the final pHf in the solu-
tion, coagulant was consequently interacted with negatively charge
fragment(s) of melanoidins. This pH dependent phenomenon was re-
lated to deprotonation (―COO) of acidic organic functional groups
such as carboxylic acid (―COOH) in melanoidins [36–40]. The main
components of dissolved organic carbon in the BYEs were hydropho-
bic acids, hydrophilic bases and hydrophilic acids which contributed
to 31.2%, 26.3% and 26.1% of the dissolved organic materials, respec-
tively. Color from BYEs was mainly caused by hydrophobic acids
(85.7%) which were long-chain fatty acids and esters, and not soluble
in water, leading to their hydrophobic characteristics [37]. Liang et al.
[38–40] proposed the insoluble organic fraction with larger molecular
size and hence larger molecular weight was more readily removed by
chemical coagulation. Our results also confirmed these observations.
206 E. Gengec et al. / Desalination 286 (2012) 200–209

Fig. 2. Effects of the variables on color, COD and TOC removal efficiencies for AE.

Thus, color removal efficiency was relatively higher than COD and
TOC removal efficiencies as compared to each other.
Co-precipitation, adsorption and sweep flocculation were three
major interaction mechanisms considered during the EC process.
Each of the mechanism was applicable in different pH ranges. At
low pH values, metal species like Al 3 + generated at anode bind to
the anionic species, thus neutralizing their charge and reducing
their solubility. This process of removal was termed as precipitation.
Adsorption mechanism operates at a higher pH range (>6.0) and in-
volves adsorption of organic substances on amorphous metal hydrox-
ide precipitates. Under the optimum conditions, at final pH 4–6, the
initially formed colloidal precipitate was positively charged and col-
loidally stable which suggested that co-precipitation played a vital
role in the EC process for AE and AAE. At pH higher than 6, formed
amorphous Al(OH)3(s) (sweep flocs) flocs with the minimum solubil-
ity within the pH range 6.5–7.8 had a large specific surface area that
can absorb some soluble organic compounds such as melanoidins
onto its surface. The EC in the pH range 4–6 was explained as co-
precipitation. Therefore, an effective color removal of BYW was real-
ized between these pH ranges as the case in our study. This was in a
good agreement with the optimum pH 5–6 reported in the literature
for BYEs in the EC and chemical coagulation process using Al elec-
trode and Al salts [16–18,38–40].
3.3. Optimization results
When operating variables were in range, the removal efficiencies
of color, COD and TOC was maximized and the operating cost was
 E. Gengec et al. / Desalination 286 (2012) 200–209 207

Fig. 3. Effects of the variables on color, COD and TOC removal efficiencies for AAE.

minimized in the RSM model with desirability of 0.757 and 0.623 for
AE and AAE, respectively (Table 10). Optimization results for the max-
imum removal efficiencies of color, COD and TOC as 82%, 41% and 39%
at 50 A/m 2, pH 4 and 22 min for AE and 77%, 36% and 32% at 11 A/m 2,
pH 5 and 18 min for AAE in the EC process were obtained for the sys-
tem. It is clear that 1128 mg/L of COD for AE and 266 mg/L of COD for
AAE satisfied the national legislation's constrain which was 1200 mg/L
of COD. The operating costs of the model at the optimised conditions
were 0.418 €/m 3 for AE and 0.076 €/m 3 for AAE. Effluents from the
EC process can satisfy effluent limits for color, COD and TOC removals.
Based on the above results, the EC process may be applied to AAE.
There were a couple of studies related to costs of COD and color re-
movals from BYEs reported in the literature [41,42]. 86% of COD and
95% of color removal efficiencies with a cost of 1.58 €/m 3 and 71%
of COD and 96% of color removal efficiencies with a cost of 1.33 €/
m 3 were obtained for treated BYW with ozone and Fenton processes,
respectively when properties of BYEs were in range of 529–2006 mg/
L of COD, 0.25–2.4 of Abs/cm and pH 7.9–8.2 [41]. When lime was
used for the treatment of BYEs contained 10,000–30,000 mg/L of
COD and pH 6.0–6.5, 84.3% of color removal efficiency and 0.84 €/
m 3 of operational cost were obtained [42].
4. Conclusions
In this study, the EC process was applied to removals of color, COD
and TOC from the anaerobic and the anaerobic–aerobic effluents of
BYW. The process variables were initial pH, current density and oper-
ation time which was designed and analyzed by the RSM. Quadratic
208 E. Gengec et al. / Desalination 286 (2012) 200–209

Fig. 4. Perturbation plots of ELC, ENC and OC for AE (a–c) and AAE (d–f).

models were developed for the responses to obtain removal efficien-
cies of color, COD and TOC for AE and AAE. In the results of runs, the
maximum color, COD and TOC removal efficiencies and minimized
the operating cost were determined from the model. The proposed
quadratic model fitted very well with the experimental data with
R 2 > 0.95 for all responses in anaerobic and anaerobic–aerobic efflu-
ents. The optimum process conditions for removal efficiencies of
color, COD and TOC were 82%, 41% and 39% at pH 4, 50 A/m 2,
22 min for AE and 77%, 36% and 32% at pH 5, 11 A/m 2, 18 min for
AAE, respectively. In addition, ENC, ELC, OC and Wsludge at the opti-
mum conditions were 1.082 kWh/m 3, 0.208 kgAl/m 3, 0.418 €/m 3
and 1.319 kg/m 3 for AE and 0.169 kWh/m 3, 0.039 kg/m 3, 0.076 €/
m 3 and 0.225 kg/m 3 for AAE. Under the optimum conditions, co-
precipitation was the predominant EC mechanism since the maxi-
mum decolorization was obtained in pH 4–6. These results showed
that RSM was a suitable method to optimize the operating conditions
and maximize the color, COD and TOC removal efficiencies for Al elec-
trode while keeping the operating costs to minimal and the EC pro-
cess was an appropriate process to treat of BYEs. This study
provided for removal of higher percentage of colors (>88%) from
both AE and AAE in the EC process, but the biological treatment pro-
cess did not give the same or a better removal rate. Therefore, the EC
has more advantages for both removals of color from these wastewa-
ters and COD and TOC as well.

Table 10
Optimization's constraints and results.

Name Goal Anaerobic effluent Anaerobic–aerobic effluent

Lower limit Upper limit Optimization results Lower limit Upper limit Optimization results

x1:pH in range 4 6 4 5 7 5
x2:CD (A/m2) in range 50 80 50 5.0 12.5 11.0
x3:time (min) in range 10.0 30.0 22 10.0 30.0 18
Re,color (%) max. 41 88 82 8 86 77
Re,COD (%) max. 20 48 41 1 49 36
Re,TOC (%) max. 16 49 39 5 43 32
ENC (kWh/m3) in range 0.297 3.600 1.082 0.026 0.337 0.169
ELC (kgAl/m3) in range 0.041 0.480 0.208 0.009 0.069 0.039
OC (€/m3) min. 0.090 1.040 0.418 0.017 0.138 0.076
Wsludge (kg/m3) min. 1.027 2.359 1.319 0.052 0.346 0.225
Desirability max. 0 1 0.757 0 1 0.623
 E. Gengec et al. / Desalination 286 (2012) 200–209
Acknowledgements
The authors thank to University of Kocaeli for their financial sup-
port of this project under contract of BAP 2009/049.
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