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Evaluation of an Electrocoagulation Process for
the Treatment of Bagasse-Based Pulp and Paper
Industry Wastewater
K. Thirugnanasambandham, V. Sivakumar, and J. Prakash Maran
Department of Food Technology, Kongu Engineering College, Perundurai, Erode 638052,
Tamil Nadu, India; drvsivakumar@yahoo.com (for correspondence)
Published online 9 June 2014 in Wiley Online Library (wileyonlinelibrary.com). DOI 10.1002/ep.12001

In this study, an attempt was made to investigate the effi-
ciency of continuous electrocoagulation process (CEC) to
treat bagasse-based pulp and paper industry wastewater. Dif-
ferent operating conditions such as initial pH (5–9), current
density (15–35 mA/cm2), electrode distance (4–6 cm) and
flow rate (25–55 ml/min) were varied in order to study the
removal efficicency of chemical oxygen demand (COD) and
total suspended solids (TSS). Electrical enrgy consumption
(EEC) of the process was also investigated. Four factors three
level Box–Behnken response surface design (BBD) was used
to evaluate the effect of process variables on CEC. From the
BBD results, second-order polynomial models were developed
and all the process variables have significant effect on the
removal efficiencies. 3D response surface contour plots were
used to study the interactive effects of the process conditions.
Under the optimum operating conditions COD and TSS
removal efficiencies were found to be 84 and 91% with EEC
of 15.25 Wh. V C 2014 American Institute of Chemical Engi-
neers Environ Prog, 34: 411–419, 2015
Keywords: bagasse wastewater, electrocoagulation, Box–
Behnken design, model development, validation
INTRODUCTION
Bagasse-based pulp and paper industry has been a rap-
idly growing sector of worldwide economy for the past sev-
eral decades and the growth trend of this industry is
expected to continue in the future. This leads to a generation
of a large amount of wastewater, which contains harmful
matters and its discharge into ecosystem without pretreat-
ment, causes negative impact on receiving natural water
resources like rivers and canals [1]. An extensive literature
analysis shows that, there is few information reported regard-
ing the treatment of bagasse-based pulp and paper industry
wastewater such as UASB reactor treatment process [2] and
the treatment with white rot fungus [3]. But these treatment
processes have drawbacks such as long treatment time, start-
up problem, difficulty in maintaining of environmental
conditions and low removal efficiency of toxic matters.
Therefore, there is a crtical need to develop an efficient treat-
ment method to treat bagasse-based pulp and paper industry
wastewater.
Additional Supporting Information may be found in the online ver-
sion of this article.
C 2014 American Institute of Chemical Engineers
V bagasse-based pulp and paper industry wastewater.
Last few decades several wastewater treatment process
such as adsorption, chemical coagulation, electrocoagulation,
electro-Fenton, aerobic, anaerobic, and membrane separation
processes were applied to treat various industry wastewaters
[4]. Among these treatment technologies, electrocoagulation
treatment (EC) method shows the the advantages such as
simple equipment and the easy automation of the process.
Also, it does not require any addition of chemicals, the dos-
ing of coagulant reagents depends on the cell potential
applied [5]. EC is a process that generates metallic hydrox-
ides in situ via electro-dissolution of a soluble sacrificial
anode immersed in the wastewater. The electrochemically
generated metallic ions hydrolyze near the anode to form a
series of metal hydroxides that are able to destabilize dis-
persed particles present in the wastewater to be treated. The
destabilized particles are believed to be responsible for the
aggregation and precipitation of suspended particles, thus
the harmful matters were removed [6]. Other advantages
include the promotion in the flocculation process, caused by
the turbulence generated by the oxygen and the hydrogen
evolution that produces a soft mix, and helps the destabi-
lized particles generate bigger particles. In addition, the
formed oxygen and hydrogen bubbles increase the efficiency
of the separation process through electrofloatation [7].
Because of these advantages, electrocoagulation has been
used to treat different types of wastewater such as cutting
oil–water emulsions, olive mill wastewater, oily bilge water,
solutions containing 4-nitrophenol (4-NP), and the waste-
water from different industries, such as textile, dairy, yeast
production, and mechanical polishing. It also has been uti-
lized in the reduction of different contaminants such as phos-
phate, sulfur compounds, phenolic compounds, fluoride,
and heavy metals [8].
However, from the extensive literature survey, it was
found that there is no research reports are available for the
treatment of bagasse-based pulp and paper industry waste-
water using continuous electrocoagulation process (CEC),
which may solve the effluent treatment problems present in
the bagasse-based pulp and paper industry. Hence, the pri-
mary objective of the present study has been made to inves-
tigate the individual and interactive effect of process
variables, such as initial pH, current density, electrode dis-
tance, and flow rate on the COD and TSS reduction with
respect to electrical energy consumption (EEC) from

Environmental Progress & Sustainable Energy (Vol.34, No.2) DOI 10.1002/ep March 2015 411
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Electrical energy consumption ðWhÞ 5
(2)
volts ðV Þ 3 amperes ðAÞ 3 retention time ðhÞ

Retention time of the CEC was calculated by the following

equation [12]:

Retention time ðminÞ 5 volume of the reactor ðmLÞ=

volumetric flow rate ðmL=minÞ (3)

Figure 1. Schematic diagram of continuous electrocoagula-

tion reactor. BBD Response Surface Design
In this present study, four factors three level Box–
Behnken response surface experimental design (BBD) was
Moreover, response surface methodology (RSM) coupled employed to investigate the individual and interactive effects
with fours factor three level Box–Behnken response surface of process variables such initial pH (5–9), current density
design (BBD) was used to develop mathematical models [9] (15–35 mA/cm2), electrode distance (4–6 cm) and flow rate
in order to predict the response values under the experimen- (25–55 mL/min) on the COD and TSS removal with respect
tal range used in this study. to electrical energy consumption (EEC) via Design-Expert
8.0.7.1 (State-Ease, Minneapolis, MN) statistical package. For
statistical calculations, the process variables were coded at
MATERIALS AND METHODS three levels (21, 0, and 11) and the coding was done by
the following equation [13].
Raw Wastewater and Chemicals
The wastewater used in this study was collected from Xi 2Xz
bagasse-based pulp and paper industry near Erode, Tamil- xi 5 i51; 2; 3 . . . . . . . . . k (4)
DXi
Nadu, India and was stored at 4 C prior to the experiments.
The characteristics of wastewater was found to be: initial pH where xi is the dimensionless value of an independent vari-
of 7.5, COD of 6500 mg/L and TSS of 1368 mg/L, respec- able; Xi, the real value of an independent variable; Xz, the
tively. All the chemicals (HCl and NaOH) used in this study real value of an independent variable at the centre point;
were anlaytical grade and purchased from local suppliers and DXi, step change of the real value of the variable i. The
from Erode, Tamil Nadu. range of independent variables and their levels are presented
in Table 1; 29 experiments were designed with five replica-
Experimental Method tions using the following equation (Table 2),
A working volume of 3 L tank (Acrylic made) was fabri-
cated and used to conduct the continuous electrocoagulation N 52K ðK 21Þ1C0 (5)
(CEC) experiments. Stainless steel plates of 33 cm 3 6 cm 3
0.2 cm were used as electrode and the entire electrode where K is number of factors and C0 is the number of central
assembly was fitted on nonconducting wedges and hanged point [14]. The relationship between the response and four
from the top of the electrocoagulation tank. The effective independent variables were evaluated by developing the
surface area of each electrode was 108 cm2. The assembly second-order polynomial mathematical models and the gen-
was connected to DC power supply equipment and it was eralized form of equation was given below [15].
used to adjust the desired current density. In each run, 1.6 L
of wastewater was placed into the reactor and all the runs X
k X
k XX
k
were performed at constant stirring speed of 250 rpm and l Y 5b0 1 bj Xj 1 bjj Xj2 1 bij Xi Xj 1ei (6)
g/L of NaCl. Peristaltic pump was used to vary the inlet flow j51 j51 i <j52
rate of the wastewater. After the CEC treatment process
(steady state), supernatant wastewater was collected and it where Y is the response; Xi and Xj are variables (i and j
was used for determination of and COD and TSS. Schematic range from 1 to k); b0 is the model intercept coefficient; bj,
diagram of continuous electrocoagulation reactor is shown in bjj, and bij are interaction coefficients of linear, quadratic,
Figure 1. and the second-order terms, respectively; k is the number of
independent parameters (k 5 4 in this study); and ei is the
error. Adequcy of developed mathematical models were
Analytical Method investigated by the pareto analysis of variance (ANOVA) and
The COD and TSS analysis were carried out by methods developed models was used to plot the response surface
described by American Public Health Association (APHA).
The removal efficiency (RE) of COD and TSS was calculated
by using the following equation [10]
Table 1. Ranges of independent variables and their levels
 
c0 2ce
RE5 3100 (1) Factors Level
c0
Variable (unit) X 21 0 1
where c0 and ce is the initial and final concentrations of Initial pH A 5 7 9
COD and TSS respectively. Meanwhile, the following Current density (mA/cm2) B 15 25 35
equation was to used to calculate the electrical energy con- Electrode distance (cm) C 4 5 6
sumption (EEC) during continuous electrocoagulation Flow rate (mL/min) D 25 40 55
process [11],

412 March 2015 Environmental Progress & Sustainable Energy (Vol.34, No.2) DOI 10.1002/ep
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Table 2. BBD and their experimental results

Run Initial pH Current density Electrode distance Flow rate COD removal TSS removal EEC
1 9 35 5 40 65.04 67.35 25.19
2 5 35 5 40 45.28 41.58 24.55
3 7 35 5 25 85.46 91.56 35.45
4 5 25 6 40 30.48 31.58 17.76
5 7 25 5 40 83.28 90.58 15.85
6 7 35 5 55 65.28 66.58 16.63
7 7 25 5 40 83.28 90.58 15.85
8 7 25 4 55 50.32 53.28 10.94
9 7 15 6 40 45.38 46.28 7.55
10 5 15 5 40 30.28 31.58 8.16
11 7 35 4 40 85.68 84.62 23.61
12 7 15 5 55 45.38 45.38 6.66
13 7 35 6 40 45.62 42.58 19.2
14 7 25 5 40 83.28 90.58 15.85
15 9 15 5 40 50.24 51.28 10.11
16 7 25 6 55 40.68 41.28 12.64
17 9 25 5 55 50.84 52.28 13.23
18 9 25 4 40 65.84 63.58 17.08
19 9 25 6 40 32.54 33.28 17.98
20 7 15 4 40 44.22 45.28 7.28
21 7 25 4 25 75.36 76.26 21.48
22 7 25 5 40 83.28 90.58 15.85
23 5 25 4 40 31.52 32.58 14.5
24 7 15 5 25 65.28 66.58 13.09
25 9 25 5 25 55.42 56.28 25.81
26 7 25 6 25 60.04 61.28 22.98
27 5 25 5 25 55.84 55.68 26.65
28 5 25 5 55 18.64 19.37 12.3
29 7 25 5 40 83.28 90.58 15.85

contour graphes [16]. After verifying the effect of process var-

iables on the responses, optimization of operating conditions
was carried out by Derringer’s desired function methodol-
ogy. After optimization, competence of the model equation
for predicting the optimum response values was validated
under the optimal operating conditions.
TSS removal ð%Þ 5 90:58 1 9:31A 1 8:99B2 8:28C
2 10:79D 1 1:52AB 2 7:33AC 1 8:08AD 210:76BC
(8)
2 0:95BD 1 95:75CD 2 30:63A2 2 12:60B2 2 21:20C2
2 11:95D2

RESULTS AND DISCUSSIONS
Mathematical Model Development
The BBD experimental design with response values are
investigated by two different analysis namely the sequential
model sum of squares and model summary statistics in order
to select effective mathematical model to describe the contin-
uous electrocoagulation process (CEC) and the results are
shown in Supporting Information (S1). From the Supporting
Information S1, it is observed that, quadratic model shows
high R2, adjusted R2, predicted R2, F value and low P value,
when compared with other models [linear and interactive
(2FI)]. Cubic model was found to be aliased [17]. Therefore,
the quadratic model is selected to represent the effects of
process variables on the CEC. To understand the interactive
relationship between the responses and process variables
three empirical models were developed from the BBD exper-
imental data and the final developed mathematical models
obtained in terms of coded factors are given below:
COD removal ð%Þ 5 83:28 1 8:99A 1 9:30B
2 8:18C 2 10:52D 20:050AB 28:07AC 1 8:16AD 210:31BC
20:070BD 1 070:42CD 2 26:84A2 2 9:19B2 217:37C2
2 9:77D2
(7)
EEC ðWhÞ 5 15:85 1 0:46A 1 7:65B 1 0:27C 2 6:09D
20:33AB 2 0:59AC 1 0:44AD 21:17BC 2 3:10BD (9)
2 2 2 2
1 0:050CD 1 1:62A 20:36B 2 0:92C 1 2:19D
Adequacy of Developed Models
Then the adequacy of developed mathematical models to
represent the CEC process was evaluated by constructing
diagnostic plots such as predicted versus actual plot (Figure
2) and normal % probability graphs (Supporting Information
S2). The data points lies very close to the diagonal line for
both the graphs and it depicts a good relationship between
experimental and predicted data [18]. Moreover, pareto analy-
sis of variance (ANOVA) was used to analyze the experimental
data and significance of the developed model equations were
evaluated by their corresponding F value and P values (Table
3). The higher model F values and lower P values, AP and
CV% values of the responses demonstrated that the developed
model was highly significant and effective. From the results, it
is concluded that, the developed mathematical models has the
ability to describe the CEC process very robustly [19].
Effect of Process Variables on Responses
It is very important that study of effects of process varia-
bles on the responses, which helps to understand the

Environmental Progress & Sustainable Energy (Vol.34, No.2) DOI 10.1002/ep March 2015 413

Figure 2. Predicted versus actual plot for responses.
individual and interactive effects of process variables on the
continuous electrocoagulation process. So that, from the
developed mathematical models, response surface contour
plots [20] were constructed to evaluate the effects of the
independent variables on the responses and it is shown in
Figures 3–6.
Effect of Initial pH
The initial pH is one of the important parameter, which
influences the performance of the continuous electrocoagula-
tion process significantly. To examine its effect, the experi-
ments were carried out at different initial pH (5–9) and the
results are exhibited in Figure 3. From the Figure 3a–c, it is
found that, the removal efficiencies of COD and TSS are
increased with increasing pH upto 8. This can explained by the
fact that, the formation effective polymeric species [21] takes
place at pH of 5–8, which could increased the removal effi-
ciency of COD and TSS. Thereafter, there is a drastic decrease
in removal efficiencies of COD and TSS. Although effect of pH
shows negligible effect on electrical energy consumption,
which depicts the key role of pH in electrocoagulation process.
Effect of Current Density
The process of electrocoagulation and performance of
electrochemical reactions are highly affected by current
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19447450, 2015, 2, Downloaded from https://aiche.onlinelibrary.wiley.com/doi/10.1002/ep.12001 by INASP/HINARI - PAKISTAN, Wiley Online Library on [12/02/2023]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
density. In order to investigate the effect of current density
in electrocoagulation process, experiments were performed
at different current densities (15–35 mA/cm2) and the obser-
vation is depicted in Figure 4. From Figure 4a–c, it was
observed that the percentage of COD and TSS removals are
increased with increasing current density upto 30 mA/cm2,
due to the formation of large amount of metal hydroxides
[22]. This particles contains strong affinity for the dispersed
particles present in the wastewater and results in coagulation
thus increased the removal efficiency of COD and TSS.
Beyond that, there is no significant effect on removal effi-
ciencies. But, current density shows strong effect on electri-
cal energy consumption that is to say EEC linearly increases
with increasing current density throughout the experiment.
Effect of Electrode Distance
The electrode distance is a key factor to determine the
pertantage removal of COD and TSS in bagasse-based pulp
and paper industry wastewater using electrocoagulation pro-
cess. In order to evaluate its effect, experiments were per-
formed at various electrode distance (4–6 cm) and the results
are illustrated in Figure 5a–c. From the results, it is found
that, the removal efficiencies of COD and TSS are increases
with increasing electrode distance upto 5 cm. Thereafter,
there is a drastic decrease in removal efficiencies of COD
 19447450, 2015, 2, Downloaded from https://aiche.onlinelibrary.wiley.com/doi/10.1002/ep.12001 by INASP/HINARI - PAKISTAN, Wiley Online Library on [12/02/2023]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Table 3. ANOVA table for responses

COD removal TSS removal EEC

Source F value P value F value P value F value P value
Model 128.85 <0.0001 80.47 <0.0001 63.20 <0.0001
A 161.07 <0.0001 89.64 <0.0001 1.76 0.2058
B 172.31 <0.0001 83.66 <0.0001 493.89 <0.0001
C 133.46 <0.0001 70.90 <0.0001 0.61 0.4486
D 220.63 <0.0001 120.48 <0.0001 312.96 <0.0001
AB 0.00 0.9681 0.79 0.3878 0.30 0.5914
AC 43.21 <0.0001 18.51 0.0007 0.98 0.3391
AD 44.18 <0.0001 22.51 0.0003 0.55 0.4702
BC 70.54 <0.0001 39.94 <0.0001 3.85 0.0699
A2 775.99 <0.0001 524.81 <0.0001 12.01 0.0038
B2 91.01 <0.0001 88.81 <0.0001 0.58 0.4572
C2 325.18 <0.0001 251.34 <0.0001 3.85 0.0701
D2 102.76 <0.0001 79.95 <0.0001 21.88 0.0004
CV% 4.29 5.77 7.04
PRESS 485.56 934.98 292.40
AP 37.11 28.89 33.91
R2 0.9923 0.9877 0.9844
Adj-R2 0.9846 0.9755 0.9688
Pre-R2 0.9556 0.9293 0.9103

Figure 3. Effect of initial pH on responses.

Environmental Progress & Sustainable Energy (Vol.34, No.2) DOI 10.1002/ep March 2015 415

Figure 4. Effect of current density on responses.
and TSS. This can explained by the fact that, electrical con-
ductivity is directly proportional to the distance between the
two electrodes. As the distance between the anode and the
cathode (g) increases, resistance (R) offered by the cell
increases by the following relation [23]
g to the effective contact between metal hydroxides produced
R5 (10)
KA
where K is the cell specific conductance and A is electrode
surface area. And, therefore, the current in the cell decreases
at constant voltage by the relation: current 5 voltage/resist-
ance. Thus production of metal hydroxides is decreased,
which reduce the removal efficiencies of COD and TSS sig-
nificantly. Whereas electrical enrgy consumption is linearly
increased with increasing electrode distance from 4 to 6 cm.
Effect of Flow Rate
In the electrocoagulation process, the flow rate is an
important factor which can influences the overall removal
416 March 2015 Environmental Progress & Sustainable Energy (Vol.34, No.2) DOI 10.1002/ep
19447450, 2015, 2, Downloaded from https://aiche.onlinelibrary.wiley.com/doi/10.1002/ep.12001 by INASP/HINARI - PAKISTAN, Wiley Online Library on [12/02/2023]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
efficiencies of COD and TSS in bagasse wastewater treat-
ment. To determine the effective of flow rate, experiments
were done at different flow rates (25–55 mL/min) and results
are shown in graphically Figure 6a–c. The obtained results
indicate that, the percentage removal of COD and TSS were
constant in the range of flow rate from 25 to 45 mL/min, due
[24] from electrodes and counter ions in the wastewater.
Thereafter, there is a decrease in removal efficiencies of
COD and TSS, due to the ineffective contact between metal
hydroxides and counter ions. Meanwhile, electrical energy
consumption is decreased with increasing flow rate.
Optimization and Validation
Derringer’s desired function methodology is used to opti-
mize the operating variables based BBD results and it was
found to be: initial pH of 7, current density of 25 mA/cm2,
electrode distance of 4.5 cm and flow rate of 40 mL/min.
Under these conditions, the removal efficiency of COD and

Figure 5. Effect of electrode distance on responses.
TSS were 84, 91% respectively with respect to EEC of 15.25
Wh. In order to validate the optimum operating conditions,
triplicate experiments were performed under the optimized
conditions and the results are close agreement with pre-
dicted values from developed mathematical models. This
results demonstrated the validation of the optimized condi-
tions of CEC treatment process to treat bagasse-based paper
and pulp industry effluent using SS electrodes.
Comparison with Existing Literatures
Chinnaraj and Venkoba Rao [2] reported the anaerobic
treatment of bagasse-based pulp and paper industry effluent
and concluded that COD removal of 80% was achieved in
HRT of 20 h. Srinivasan and Murthy [3] studied the treatment
of bagasse-based pulp mill effluent using a white rot fungus
Environmental Progress & Sustainable Energy (Vol.34, No.2) DOI 10.1002/ep
19447450, 2015, 2, Downloaded from https://aiche.onlinelibrary.wiley.com/doi/10.1002/ep.12001 by INASP/HINARI - PAKISTAN, Wiley Online Library on [12/02/2023]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
and concluded that the maximum colour removal efficiency
of 82.5% was obtained with an optimal glucose and ammo-
nium chloride concentrations of 15 and 0.5 g/L, respectively
in the pH range of 4.5. But in this present study shows that
the COD removal of 84% and TSS removal of 91% which
indicates the higher treatment efficiency of CEC over the
treatment methods reported in literature.
CONCLUSIONS
In this present study, removal efficiencies of chemical
oxygen demand (COD) and TSS with electrical energy con-
sumption (EEC) from bagasse-based pulp and paper industry
wastewater was examined under different process conditions
such as initial pH (5–9), current density (15–35 mA/cm2),
electrode distance (4–6 cm), and flow rate (25–55 mL/min)
March 2015 417

Figure 6. Effect of flow rate on responses.
using continuous electrocoagulation process (CEC). Mathe-
matical modeling of the present study was done by response
surface methodlogy (RSM) coupled Box–Behnken response
surface design (BBD) with four factors at three levels.
Second-order polynomial models were developed from the
experimental data in order to predict the responses with
high correlation coefficient values. This results exhibited that,
CEC is found to be a suitable treatment method (>80%
removal of COD and TSS) to treat bagasse-based pulp and
paper industry wastewater in terms of high removal effi-
ciency as well as easy automation.
ACKNOWLEDGMENTS
The authors are thankful to University Grant Commission,
Government of India, for financial support (F.No:39-853/
2010) to fabricate and use the experimental setup.
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