Journal of Water Process Engineering 20 (2017) 168–172

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Journal of Water Process Engineering

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

Treatment of textile wastewaters by electrocoagulation employing Fe-Al T

composite electrode
Akshaya Kumar Verma
Department of Civil Engineering, Faculty of Engineering and Technology, Siksha ‘O’ Anusandhan University Bhubaneswar, 751030, Odisha, India

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

Keywords: In the present study, electrocoagulation process employing Fe-Al composite electrode was applied for treatment
Textile wastewater of different types of textile wastewaters. Effect of major operating parameters such as pH, reaction time, current
Electrocoagulation density, voltage and inter-electrode distance were investigated for chemical oxygen demand (COD) and colour
COD reduction removal efficiency. The process was found promising and produced more than 90% COD and colour removal
Colour removal
efficiency at optimised operating conditions of pH 8, reaction time 80 min, current density 20 A/m2 with an
inter-electrode distance of 3 cm. Robustness of the process was investigated on real and anaerobically pre-
treated textile wastewater. For real textile effluents, the process produced approximately 99% colour removal
efficiency, creating virtually colourless solution even at a lesser reaction time of 60 min. Electrocoagulation
effectively detoxified the anaerobically pre-treated textile wastewater by eliminating 78% of aromatic amines
within a reaction time of 180 min.

1. Introduction
Textile industry effluents are one of the major sources of environ-
mental contamination and public well-beings, mostly in many urban
regions. These effluents are severely polluted with the complex organic
and inorganic chemicals which are used during various steps of textile
processing. The unused constituents from each step are discharged as
wastewater which possesses strong colour due to the presence of re-
sidual dyes, high organic and inorganic matters, turbidity, pH and toxic
chemicals. Presence of a very small amount of residual dye in water is
highly visible and consequently, affects the receiving environment not
only aesthetically, but also disturbs the aquatic life by hindering the
light penetration and oxygen transfer. The carcinogenic and mutagenic
ability of various azo dyes and their precursors produces detrimental
effects to the environment [1]. Therefore, to protect the environment,
textile wastewater must be treated up to the safe discharge limits as
recommended by legal bodies of different countries. Various physico-
chemical, chemical and biological processes, as well as some of the new
emerging techniques like sonochemical or advanced oxidation pro-
cesses are practiced to treat the textile wastewater [2,3]. Each of them
has some limitations and drawbacks in their application. Biological
treatment by activated sludge offers appreciable efficiencies for COD
removal, but does not effective for the elimination of the colour of the
wastewater and often operational problems such as bulking of sludge
appear. Coagulation/flocculation process has been found to be robust,
cost effective, easy to operate and energy saving treatment options, but
the coagulation process does not work well for all the types of textile
dyes [4]. Advanced oxidation processes such as ultrasonication, ozo-
nation, UV-radiation H2O2, and their combinations have a great in-
terest, but the costs are still very high due to the high doses required
and power consumption [5]. Adsorption and nanofiltration processes
are not always enough to satisfy the discharge limits [6]. In addition,
few electrochemical technologies such as electrochemical oxidation,
electrochemical reduction, indirect electro-oxidation with strong oxi-
dants, emerging photo-assisted electrochemical treatments and elec-
trocoagulation have received considerable attention for treating dye
wastewaters during last decade [7]. Electrocoagulation (EC) process
has been successfully used for the treatment of textile wastewater being
attractive for its versatility, safety, selectivity, amenability to automa-
tion, ease of control and environmental compatibility [8]. These pro-
cesses are popular because of the ease of distribution and moderate
requirement of chemicals [9,10]. It involves the generation of coagulant
in situ by the dissolution of metal ions from the consumable anode with
subsequent formation of hydroxide ions at the cathode [11,12]. In EC,
contaminants are encroached up towards the surface of the EC cell by
small bubbles of hydrogen gas produced from the cathode. Therefore,
as an alternative of chemicals and microorganisms, electrons are the
only working agents in electrochemical cell being responsible for fa-
cilitating wastewater treatment [13]. The most widely used electrode
materials in electrocoagulation process are aluminum and iron. Many
researchers reported appreciable treatment efficiency of electro-
coagulation employing aluminum, iron and copper electrodes for

E-mail addresses: akshaya14001@gmail.com, akshayakumarverma@soauniversity.ac.in.

http://dx.doi.org/10.1016/j.jwpe.2017.11.001
Received 31 May 2017; Received in revised form 16 September 2017; Accepted 1 November 2017
Available online 05 November 2017
2214-7144/ © 2017 Elsevier Ltd. All rights reserved.
A.K. Verma
different types of wastewater/textile wastewater [12,14–16]. However,
the researches related to the use of composite electrode made of alu-
minum and iron both, for the treatment of textile wastewater are very
terse [12].
To the best of our knowledge, no study has been reported to eval-
uate the effectiveness of composite electrode (Fe-Al) for the treatment
of textile wastewater containing different category of textile dyes along
with different chemical additives that are normally being used during
different steps of textile processing. An electrocoagulation using the
composite electrode (Fe-Al) was employed with the purpose of a si-
multaneous release of both iron and aluminum ions during electrolysis
reaction and to assess its effect on the treatment efficiency. Therefore,
the present study was focused on investigating, for the first time, the
effectiveness of electrocoagulation process employing iron-aluminum
composite electrode for the decolourisation and COD reduction of
synthetic textile wastewater containing different classes of new gen-
eration dyes along with the various other chemicals. The study was
focused on evaluating the effects of pH, inter-electrode distance, cur-
rent intensity, reaction time, and applied voltage on decolourisation
and COD reduction of synthetic textile wastewater.
2. Materials and methods
2.1. Synthetic textile wastewater
Synthetic textile wastewater was prepared as per the reported
chemical constituents of real textile wastewater [4], with a total dye
concentration of 200 mg/L along with various chemical additives such
as starch, acetic acid, sucrose, sodium carbonate, sodium hydroxide,
sulphuric acid, detergent, and sodium chloride, which are used during
textile processing for various purposes. Three different categories of
commercial dyes, namely, Reactive Black 5 (RB5), Congo Red (CR) and
Disperse Blue 3 (DB3) were procured from Sigma-Aldrich, Germany and
used in an equal ratio for the preparation of textile wastewater. The
characteristic wavelength of simulated dye wastewater was determined
by running a scan of the dye solution on a UV–vis spectrophotometer
(Perkin-Elmeyer, Lambda 25), and the maximum absorbance wave-
lengths (λmax) for RB5, CR and DB3 were found as 591, 502 and
638 nm, respectively. The colour content of the wastewater containing
mixture of dyes was determined by taking the sum of the absorbencies
measured at 591, 502 and 638 nm. The synthetic textile wastewater
was possessing COD = 1970 ± 30 mg/L, pH = 9.5 ± 0.1, Abs (mix-
ture) = Abs(591) + Abs(502) + Abs(638) = 2.4; electrical con-
ductivity = 28 ± 2 mS/cm. The percentage decolourisation efficiency
was determined using the following Eq. (1):
Decolourisation efficiency (%) = [(Ab−At)/Ab] × 100 (1)
where Ab and At are the absorbencies of the solution before treatment
and after treatment of the textile wastewater, respectively. Tap water
was used as a reference.
2.2. Experimental setup
The experimental setup is shown in Fig. 1. A container (electro-
chemical cell) made of brass was used as the cathode having a diameter
of 75 mm, depth of 80 mm, and 1.5 mm thickness with an effective
volume of 350 mL. A 300 mL of solution was placed for electro-
coagulation at a time. Brass made electrochemical cell was used as the
cathode to increase the surface area and facilitate the electrochemical
process. Moreover, in this condition, electrocoagulation was highly
enhanced since the bubbles mainly originated from the cathode were
distributed thoroughly and extensively from the bottom and walls of
the electrochemical cell [12]. The electrochemical cell was subjected to
the magnetic stirrer at constant stirring speed (120 rpm) to provide
proper mixing of the solution throughout. The prepared composite
169
Journal of Water Process Engineering 20 (2017) 168–172
electrodes (Fe-Al) with dimensions of 60 mm × 30 mm × 2 mm were
applied as the anodes simultaneously which were placed at the center of
the cell with a certain distance from each other. A 50 mm of the anodes
were submerged in wastewater providing an effective submerged sur-
face area of 0.0033 m2. The electrodes were connected to a digital dc
power supply (Topward 6306D; 30 V).
2.3. Analytical procedures and chemicals
Colour measurement of the reactor effluents treating textile waste-
water was carried out after filtration of supernatant through Whatman
42 filter paper. Subsequently, the absorbance of the sample was mea-
sured using a UV–vis spectrophotometer (Perkin-Elmeyer, Lambda 25).
COD was analysed as per the closed reflux colourimetric method after
digestion of the samples in a COD reactor (Model DRB 200, HACH,
USA), and then absorbance measurement was carried out by COD
spectrophotometer (Model DR 2800, HACH, USA) at 600 nm 1.0 M
H2SO4 and 1.0 M NaOH were used to adjust the desired pH. High
Performance Liquid Chromatography (HPLC) was used for the analysis
of aromatic amines from anaerobically pre-treated and electro-
chemically treated textile wastewater. Aromatic amines were also
quantified colourimetrically as per the method suggested by Oren et al.
[17]. For the HPLC analysis of aromatic amines, an aliquot of respective
wastewater were centrifuged at 4000 rpm for 15 min. The supernatants
were transferred into a petri-dish which subsequently kept into the
freeze dryer (Christ, ALPHA 1–2 LD plus) for the evaporation to its
dryness. The residues were dissolved in methanol. Samples were fil-
tered through a 0.22 μm nylon filter paper and eluted isocratically
using a C18 column. The mobile phase used was a mixture of filtered
methanol (HPLC grade) and Millipore water in 7:3 (v/v) ratio with a
flow of 0.7 mL/min.
3. Results and discussion
3.1. Effect of initial pH
In wastewater treatment using electrocoagulation, pH plays a very
important role in determining treatment efficiency. Therefore, experi-
ments were designed to determine the optimum pH of synthetic textile
wastewater that allowed for maximum decolourisation and COD re-
duction. The effect of pH on the treatment efficiency was examined by
altering the initial pH from 2 to 11 and keeping all other parameters
(Fe-Al, current density = 15 A/m2 and reaction time = 60 min) con-
stant. Decolourisation and COD reduction efficiency increased with
increasing pH up to pH 8 and then decreased afterward. Results showed
that at pH 8, up to 79% COD, and 86% colour removal efficiencies were
achieved (Fig. 2). A small increase in the overall pH was noted in the
acidic solutions (pH 2–6). In the electrochemical process, an increase in
the overall pH may be linked to the increase of the bulk concentrations
of hydroxide ion formed in the solution due to the reduction of water at
the cathode.
During electrocoagulation, composite electrode (Fe-Al) produces
iron and aluminium hydroxides which start coagulating the impurities
present in the solution. It can also be observed from Fig. 2 that deco-
lourisation and COD reduction followed the same trend and the effi-
ciency of electrocoagulation was low either at low pH or at high pH.
This behavior may be attributed to the amphoteric nature of aluminum
hydroxide which does not precipitate at very low pH and starts dis-
solving at increasing pHs [18]. At low pH, cationic monomeric species
Al3+ and Al(OH)2+ prevail. When pH is between 4 and 9, various
monomeric species such as Al(OH)2+, Al(OH)22+, and polymeric spe-
cies such as Al6(OH)153+, Al7(OH)174+, Al13(OH)345+ transform into
insoluble amorphous Al(OH)3(s) flocs through complex polymerization
and/or precipitation mechanism. When pH is higher than 8, the
monomeric Al(OH)4− concentration increases, decreasing the sig-
nificance of insoluble amorphous Al(OH)3(s) flocs [19]. In contrast, the
A.K. Verma
Fig. 2. Effect of initial pH on removal efficiency (Current density = 15 A/m2; Reaction
time = 60 min).
formation of Fe2+ (aq) ions and subsequently their oxidation to Fe3+
(aq) cause the precipitation of Fe(OH)3 which remove impurities
mainly by adsorption and charge neutralization during coagulation
[20].
3.2. Effect of reaction time
Reaction time (time of electrolysis) determines the charge loading
and thereby affects the performance of electrocoagulation. The effect of
electrolysis time on colour and COD removal efficiency was in-
vestigated maintaining the optimum pH of 8 and keeping constant
current density of 15 A/m2. It can be observed from Fig. 3, that colour
and COD removal efficiency is increasing with increase in the reaction
time up to 80 min and then become constant and no further increase is
observed. This could be related to decreasing extent of cathodic re-
duction and generation of nascent electro-coagulant flocs [21].
Fig. 3. Effect of reaction time on removal efficiency (Current density = 15 A/m2;
pH = 8).
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Journal of Water Process Engineering 20 (2017) 168–172
Fig. 1. Schematic view of experimental setup: 1) cathode (brass
container), 2) anode (Al), 3) anode (Fe), 4) magnetic stirrer, and 5)
DC power supply.
Therefore 80 min is designated as optimal reaction time at which COD
and colour removal efficiency of 90% and 94%, respectively are ob-
tained.
During electrocoagulation, negatively charged colloidal particles
are neutralised by collisions with iron and aluminium counter ions
[22,23]. Slightly higher degree of colour removal as compared to COD
reduction may be linked to the presence of residual soluble impurities
in the wastewater, which cannot be removed effectively [24].
3.3. Effect of current density
It is well known that current density determines the coagulant
production rate, regulates bubble production, and therefore affects the
growth of flocs and therefore is one of the most important parameter for
controlling the reaction rate in the electrocoagulator [25]. To in-
vestigate the effect of current density on the removal efficiency, elec-
trocoagulation process was performed at increasing current densities
from 5 to 25 A/m2 and maintaining constant pH of 8 and reaction time
of 80 min (Fig. 4). It can be observed that COD and colour removal
efficiencies increases with increase in the current density, however, a
very small increase of 2% is observed from 20 to 25 A/m2. The higher
removal efficiency of impurities with increased current density might
be related to the higher amount of ions produced on the electrodes that
promote destabilisation of the pollutant molecules and, finally, the
agglomeration of the induced flocs, with increase in the hydrogen
evolution [20]. In addition to the current density, effect of applied
voltage on treatment efficiency of electrocoagulation was also in-
vestigated by varying voltage from 6 to 12 V at the current density of
20 A/m2. Both colour and COD removal efficiency followed the same
increasing trends with increase in the applied voltage and a maximum
removal efficiency of 96% and 94%, respectively was attained at an
extreme voltage of 12 V.
Fig. 4. Effect of current density on removal efficiency (Reaction time = 80 min; pH = 8).
A.K. Verma
3.4. Effect of inter-electrode distance
Inter-electrode distance is an important variable with regards to
operational costs. In the case of high values of the conductivity (as in
present study) of the effluent, it is recommended that, when the con-
ductivity of the effluent is relatively high, greater inter-electrode dis-
tance be used [20]. To assess the effect of inter-electrode distance on
electrocoagulation efficiency, Fe-Al electrode (anode) was adjusted in-
side the brass container at variable distances.
Since cathode is fixed and therefore increasing the distance between
anodes leads to the decrease of distance between each anode and
cathode. Fig. 5 depicts that colour and COD removal efficiency is im-
proved by decreasing the distance between the anodes and cathode
(i.e., increasing the distance between two anodes). This can be attrib-
uted to the increase of electrical current associated with reducing the
inter-electrode distance resulting in higher collisions of the ions that
enhance the coagulation [20]. Maximum decolourisation and COD re-
duction efficiency of 90% and 94%, respectively was attained with a
distance of 3 cm between the two anodes. No significant improvement
in the treatment efficiency was observed beyond a distance of 3 cm.
3.5. Energy and electrode consumption
Consumption of energy and electrode during the electrocoagulation
treatment play an important role which affect the economic feasibility
of the process. In this regard, energy and electrode consumption was
determined as per the following equations (Eqs. (2) and (3)) suggested
by Şengil and Özacar [26].
V × I × t × 103
(
Energy consumption kWh kgofdye = )
60(Co − Ct ) × v
M×I×t
Electrode consumption ⎛ kgofelectrode kgofdye ⎞ =
⎝ ⎠ n× F× v × (Co − Ct )
where V is the applied voltage (Volt), I is the applied current (A), t is the
time (sec) and v is working volume (L). M is the molar mass of iron/
aluminium (gMol−1), n is the number of moles of electron involved in
the reaction (Fe = 2, Al = 3), F is the Faraday constant
(F = 96,487C Mol−1), Co is the initial concentration of the dye and Ct is
the concentration at time t. At the optimised conditions for colour re-
moval, energy consumption was determined to be 0.018 kWh/kg of dye
removed. Combined electrode consumption of 0.72 ± 0.001 kg/kg of
dye (0.18 kg Fe/kg of dye and 0.55 kg Al/kg of dye) was observed at the
optimised conditions. The observed electrode consumption can ratio-
naly be corelated to the theorectical electrode consumption as per Eq.
(2). Similar findings related to energy and elecrode consumption during
wastewater treatment were also observed by Sakthisharmila et al. [27]
and Chelliapan et al. [9].
Journal of Water Process Engineering 20 (2017) 168–172
Fig. 5. Effect of Inter-electrode distance on removal efficiency (Reaction
time = 80 min; pH = 8; Current density = 20 A/m2).
3.6. Effectiveness of optimised electrocoagulation parameters for treatment
of real textile effluents
Efficacy of the optimised electrocoagulation parameters (Reaction
time = 80 min; pH = 8; Current density = 20 A/m2; inter-electrode
distance = 3 cm, and Voltage = 12 V) were assessed for COD and
colour removal of real textile effluents collected from a local textile
hand mill situated in Khurda district (20.1660° N, 85.6660° E) of
Odisha, India. The effluents obtained from the textile hand mill contain
intense brown colour, pH 10.2 ± 0.5, COD (mg/L) 1950 ± 150, and
electrical conductivity (mS/cm) 20.1 ± 2. The average value of λmax
was found to be 540 nm. It was investigated during the course of
treatment that almost all the colour of real textile effluents get vanished
producing a virtually colourless solution (colour removal effi-
ciency ∼ 99%). COD removal efficiency was also appeared to be pro-
mising (95%) under the mentioned operating conditions. Further, the
treatment efficiency was also assessed at different decreased reaction
durations. It was observed that a 60 min of reaction was sufficient for
effective treatment of textile effluent producing colour and COD re-
moval efficiency of 98.5% and 94%, respectively.
3.7. Electrocoagulation as a post-treatment for removal of total aromatic
amines from anaerobically pre-treated textile wastewater
In our previous study, a significant concentration of carcinogenic
aromatic amines (6.92 mg/L) was produced during the treatment of
synthetic textile wastewater using an integrated process [28]. A number
of methods such as coagulation [29], ultrasonication [30], and che-
mical assisted ultrasound [31] have been tried to reduce the con-
(2)
centration of generated aromatic amines but none found suitable.
Electrocoagulation was also applied to assess the efficiency of the
process for removal of total aromatic amines (TAAs). HPLC was used to
determine the presence of these aromatic compounds in the samples.
Researchers investigated that RB5 and CR produce sulphanilic acid and
(3) benzidine like compounds, respectively after their reductive cleavage
under the anaerobic environment [32]. HPLC grade sulphanilic acid
and benzidine served as a reference to obtain the information about the
appearance of respective peaks. It can be seen from Fig. 6a that a
continuous decrease in the aromatic amines concentration was ob-
served with increasing reaction time producing a removal efficiency of
78% within 3 h. Further, the treated effluents were analysed using
HPLC to observe the presence of residual aromatic amines (Fig. 6b).
Sulphanilic standard with a concentration of 100 mg/L was injected
into the C18 column (curve I). Specific peak was obtained for sulpha-
nilic acid standard at a retention time of 2.74 min. Chromatogram of
anaerobically pre-treated textile effluent indicates the presence of sul-
phanilic acid (curve II), where similar peak was also observed at a re-
tention time of 2.75 min. The intensity of observed peak was sig-
nificantly reduced after the electrocoagulation of aerobically pre-
171
A.K. Verma
Fig. 6. Effect of electrocoagulation on aromatic amines removal (Initial TAAs = 6.92 mg/L, pH = 8; current density = 20 A/m2; inter-electrode distance = 3 cm, voltage = 12 V).
treated textile effluents (curve III), indicating the physico-chemical
removal of aromatic compounds through their coagulating mechan-
isms.
4. Conclusions
The results of the study showed that electrocoagulation is an effi-
cient way to treat industrial textile wastewaters containing a variety of
textile dyes and complex chemicals. The electrolysis time, current
density, pH and inter-electrode distance come out to be the major op-
erating variables which regulate the treatment efficiency of the elec-
trocoagulation process. The investigations revealed that virtually
complete colour and 90% COD removal efficiency was achieved in
electrocoagulation process employing Fe-Al as composite electrode at
its optimised operating conditions. The optimised operational condi-
tions of electrocoagulation were also applicable for assessing the
treatment efficiency for real textile effluents, and for effectively elim-
inating toxic aromatic amines from anaerobically pre-treated textile
wastewater, thus showing the robustness of the process for various
types of contaminants. Based on the investigations made, the composite
electrode electrocoagulation process appears to be an efficient process
for producing direct dischargeable or recyclable quality wastewater
from textile wastewater.
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