Environ. Eng. Res.

2017; 22(2): 141-148 pISSN 1226-1025

https://doi.org/10.4491/eer.2016.029 eISSN 2005-968X

Assessment of kinetics behavior of electrocoagulation process

for the removal of suspended solids and metals from
synthetic water
Hariraj Singh, Brijesh Kumar Mishra†
Department of Environmental Science and Engineering, Indian Institute of Technology (ISM) Dhanbad, Jharkhand 826004, India

ABSTRACT
Globalization, industrialization, mining, and uncontrolled population growth have fostered a shortage of potable water. Therefore, it has become
imperative to understand an effective and reasonable water purification technique. A renewed interest in electrocoagulation (EC) has been
spurred by the search for reliable, cost-effective, water-treatment processes. This paper has elucidated a technical approach for getting rid of
heavy metals and total suspended solids (TSS) from synthetic water using an aluminum electrode. The effect of operational parameters, such
as current density, inter-electrode distance, operating time, and pH, were studied and evaluated for maximum efficiency. This study corroborates
the correlation between current density and removal efficiency. Neutral pH and a low electrode gap have been found to aid the efficacy of
the EC setup. The outcome indicates that a maximum TSS removal efficiency of 76.6% occurred at a current density of 5.3 mA/cm2 during
a contact time of 30 min. In the case of heavy metals remediation, 40 min of process time exhibited extremely reduced rates of 99%, 59.2%,
and 82.1%, for Cu, Cr, and Zn, respectively. Moreover, kinetic study has also demonstrated that pollutants removal follows first-and second-order
model with current density and EC time being dependent.

Keywords: Current density, Electro-coagulation, Heavy metals, Kinetic, Synthetic water

1. Introduction management strategies. To resolve this problem, technical ap-

proaches such as ion exchange chromatography, ultrafiltration,
reverse osmosis and chemical precipitation have been applied.
The explosive population increase and expansion of urban areas
But each treatment method comes with their respective pros and
have exacerbated adverse impacts on water resources [1, 2].
cons. For example, Ion exchange chromatography is highly effective
Nowadays, Mining and industries have been found to produce
in removing certain charged contaminants, but it requires costly
significant contributions in accelerating extent of contamination
resin regeneration. Ultra filtration and reverse osmosis are clean
in the surroundings. Mine water and Industrial effluents are known
processes, merely they are prohibitively expensive. Chemical pre-
antecedent of heavy metals. Doubtless, it has deteriorated water
cipitation is a simple procedure; it does get a high volume of
quality by incorporating a high absorption of toxic metals. The
sludge.
repercussions of metallic contaminants like Pb, Cr, Zn and Cu
Researchers have explored different innovative approaches to
on the wide application of water have been scrutinized and it
unfold eco-friendly heavy metals remediation. Studies have re-
has been recommended to treat contaminated water before
vealed electrocoagulation (EC) as one of the efficient and cost
discharging. Thus, there is an exigency to develop effective and
effective technique for the removal of heavy metals. This technique
economical water purification technique to curtail its deleterious
relies on the principal of segregating heavy metals in the presence
effects.
of electric current using suitable electrodes [3-5]. In this process,
The right of all people to access suitable water supplies must
Iron is the most widely used electrode followed by aluminum.
thus be seen as a global challenge, the solution of which is depend-
When aluminum is used as anodes, it produces aluminum hydrox-
ent on the formulation and implementation of sustainable water

This is an Open Access article distributed under the terms Received February 18, 2016 Accepted October 17, 2016
of the Creative Commons Attribution Non-Commercial License
†
(http://creativecommons.org/licenses/by-nc/3.0/) which per- Corresponding author
mits unrestricted non-commercial use, distribution, and reproduction in any Email: bkmishra3@rediffmail.com
medium, provided the original work is properly cited. Tel: +91-947-1191704 Fax: +91-326-2296624
Copyright © 2017 Korean Society of Environmental Engineers

141
Hariraj Singh and Brijesh Kumar Mishra

ide, Al(OH)3, upon oxidation in an electrolytic system [6]. with reference to energy requirement and percentage removal has
Table 1 shows the values of EC parameters chosen by some not yet been studied in detail. The aim of the present study was
authors [4, 7-10] for the removal of heavy metal using aluminum to understand the various factors affecting removal efficiency of
or iron electrodes. The parameters, whose values will be compared metals and TSS by EC process with reference to energy requirement
with this work (Table 1), are: Conductivity and electrolyte composi- to understand the feasibility of EC process.
tion; initial pH; number of metals present in the medium and
initial metal concentrations; the volume of the solution inves-
tigated; number of electrodes used; total electrode surface area 2. Materials and Methods
and distance between electrodes; current density; operating time.
As indicated in Table 1, EC is usually taken using high electrolyte 2.1. Reagents and Solutions
conductivity (from 1.5 to 20 mS/cm). High conductivity can be
Reagents were prepared using distilled demineralized water from
obtained with the addition of salts like NaCl, NaNO3 and Na2SO4
the Mili-Q water system. Titrisol Merck standard solutions of 1,000
[7, 8]. The role of salt addition is to lower the electrolysis potential
mg/L of copper, chromium, and zinc were used and solutions
and, in the case of chloride ions, to enhance anodic dissolution
of different concentrations were obtained by adequate dilutions.
of the electrodes.
The pH of the solution was adjusted by 0.1 N HCl and 0.1 N
Metals and total suspended solids (TSS) removal through the
NaOH solutions prepared from AR grade Merck chemicals.
EC process is well known, but optimization of the EC process

Table 1. Comparisons of Treatment Performances of Different Wastewater with Process Conditions and Variables in the EC Process
This study
Reference [7] [8] [9] [4] [10]
conditions
Metal plating Grenhole ground
Kind of water Synth. Water Synth. Water Synth. Water Synth. Water
wastewater water
Conductivity
20 1.7-2.9 2 1.47 0.35 0.62 (21.3°C)
(mS/cm)
3.2
Initial pH 4.5-7.5 4.9 3 3; 5.68; 8.95 7.7 (7 after addition of
NaOH)
Cu2+ 50-250
Cu2+ 50-250
Zn2+ 50-5000 Cu2+ 59 2+ Cu2+ 12 Cu2+ 10
Metal concentration Cu 45 Cr(VI) 44.5 Zn2+ 50-250
Ni2+ 50-250 Zn2+ 67 Zn2+ 20 Cr6+ 10
(ppm) Ni2+ 394 Ni2+ 50-250
Cr(VI) 10-50 Ni2+ 67 Ni2+ 20 Zn2+ 10
Mn2+ 50-250
Ag+ 5-50
Treated volume (L) 1.2 0.9 0.65 0.5 15 7
Number of electrode
4 2 6 6 4 2
used
Electrode material Al Al Al or Fe Fe Al or Fe Al
Interelectrode
5 40 10 3 15 30
Distance d (mm)
Anodic surface
300 54 200 100 720 113
area S (cm2)
Ratio d/S
0.002 0.074 0.005 0.003 0.002 0.017
cm-1
Current I (A) 0.3-3 0.27-1.08 0.5-2 0.2-2.5 0.5-1 0.15-0.6
Current density
16-98 50-200 25-100 20-250 7-14 13-53
(A/m2)
Voltage U (V) - 7- 22 - 11.75 4-10.5 6.3-16.6
Treatment time t
0-140 0-80 0-60 0-50 0-180 0-40
(min)
45 0.6 and 0.59
(calculated 2 49 (at I = 1A and 0.459
Energy consumption
- from the data at (at I = 1A and (at I = 2.5 A and t = 60 min with (at I = 0.450 A and
U.I.T/V (kW h m-3)
I = 1 A and t = 15 min) t = 50 min) Fe respectively time 30 min)
t = 60 min) Al electrodes)

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 Environmental Engineering Research 22(2) 141-148

CuSO4･5H2O, K2Cr2O7, and ZnO were used in the present study The current values were selected from 150 mA to 600 mA corre-
for preparing of Cu, Cr and Zn based synthetic water. A measured sponding to a current density from 1.3 mA/cm2 to 5.3 mA/cm2 using
quantity of 1 L of freshly prepared synthetic solution of Cu, Cr a precision DC power supply (Microtech agencies Dhanbad, India)
and Zn using tap water was taken in EC process. characterized by the ranges 0-2 A for current and 0-30 V for voltage.
Before each experiment, the electrodes were polished with abrasive
2.2. Experimental Setup and Procedure paper to get rid of any oxide film and then thoroughly rinsed.
A Perspex made reactor (Table 2) having specific dimension 250 To pursue the progress during treatment, 10 mL samples were
mm × 250 mm × 300 mm was used to carry out remediation periodically taken from the container at predetermined time inter-
of heavy metals as a batch type to conduct the experiments. Good vals (10 to 40 min) and were filtered using Whatman filter paper
quality metal sheets of aluminum used as electrodes of 150 mm of grade 42 (GE Healthcare UK Limited) to sort out the sludge
× 250 mm × 2 mm size for EC. The sufficient gap between the from the solution to be dissected. The residual concentrations
anode and cathode was varied as per requirement. The reactor of metal ions were determined using an atomic absorption spec-
is constructed in such a style; it could be adjusted horizontally trophotometer (FAAS-GBC Avanta, Australia) according to APHA
as well as vertically as needed. standard 2012 [11]. The pH was continuously measured in the
The experimental setup is shown in Fig. 1 for the EC experiments, 18-L container and was not adjusted during the treatment. All
Aluminum (Al) plates with 2 mm thickness were used, and the experiments were performed at room temperature.
surface area in contact with the electrolyte was in each case 113
cm2 per side. In each experiment, two plates were used in the 2.3. Calculations
electrochemical reactor and the distance (d) between plates was The amount of electrical energy used is an important economical
varied from 2-4 cm. The electrodes were placed using a monopolar parameter in the EC process [10]. This parameter is computed
configuration with a total anodic or cathodic surface area (S) of by Eq. (1):
450 cm2.

  (1)
Table 2. Reactor and Electrodes Characteristics 
Reactor Characteristics Specification
E is the electrical energy used (in kWh/m3), U is the voltage
Material Plexiglass
applied (in V), I is the current (in A), T is the coagulation time
Size 250 mm × 250 mm × 300 mm in hours. V is the volumes in liters. The amount of sacrificed
Reactor mode Batch electrode use is determined by measuring the initial and eventual
Reactor Volume 18 L weight of the electrodes.
Working volume 7 L The percentage removal efficiency of EC process was computed
DC power supply as a function of operating time by Eq. (2):
Voltage range (V) 0-30 Removal efficiency, %
Current range (A) 0-2
  
Electrode    × (2)

Material Aluminum
Size 300 mm × 150 mm × 2 mm Where C0 and Ct are heavy metal concentrations for each heavy
Anode surface area 113 m2 metal and TSS at times 0 and t.
Connection arrangement Parallel type For kinetic study, first order and second order kinetic model
were considered to describe for the removal rate [12]. The EC
batch process, the mass conservation of pollutants ion is:


    (3)


Where (  ) is the removal rate in ppm/min and t is EC time

in min. With the first-order model (     ), the integration of
Eq. (3) at the initial concentration C(0) = C0, gives

  
    (4)

Where  is the first-order rate constant in min−1. For the second

order model (       ), the time-dependent concentration is
Fig. 1. Schematic diagram of electro chemical cell for removal of metals obtained as:
and TSS.

143
Hariraj Singh and Brijesh Kumar Mishra

 
     (5)
 

Where  is the second-order rate constant in ppm−1min−1.

3. Results and Discussion

3.1. Establishment of Metals Concentration and Other Water
Characteristics
To evaluate the EC performance, synthetic water was prepared
with initial concentration of TSS and heavy metals concentration
which imparted a sufficient electrical conductivity, total dissolved Fig. 2. Removal of TSS along with contact time at different current
solids (TDS), turbidity in water samples. The pH of the synthetic density and at pH 7, electrode distance 2 cm.
water drops down, which again adjusted as per experimental re-
quirement during the establishment of physiochemical character-
istics (Table 3). The pH of the solution was adjusted by adding
either 0.1 N NaOH or 0.1 N HCl solution.

3.2. TSS Removal

The relationship between the TSS removal efficiency and contact
time for pH 7 at 30 min operating time of EC process is depicted
in Fig. 3 in which maximum removal occurred at 2 cm electrode
distance. The synthetic water of the initial value of TSS is 135
mg/L is used for experiments The Fig. 2 depicts that as the contact
time increased from 10 min to 40 min removal efficiency increased
Fig. 3. The relationship between TSS removal efficiency and current
from 62.1% to 76.6%. The removal efficiency, increased up to
density at pH 7, different electrode distances, contact time 30 min.
30 min of contact time and beyond that no further significant
increased was observed. Bukhari [13] also demonstrated same ob-
the electrode surface, due to the passivation, has a rough surface,
servation at current 0.2 A which has supported removal of TSS
which provides larger adhering forces to bubbles than smooth
was significantly consistent after 30 min of process time [14].
surfaces, thus decreasing their generation.
The maximum removal of suspended solids removed in first 10
min after that suspended solids removed in smaller ratios are
3.3. Effect of pH
indicated in the Fig. 2, which was also reported by Aji et al.
[4], for first 15 min after that removal was consistent and also According to literature study, it was found that at neutral pH
similar results has been also reported by Chou et al. [15] for colour of 7, all the metals demonstrated optimal and consistent removal
removal efficiency in 20 min of process time (at least 80%) and efficiency [18], so pH 7 was established in this study for
53-99% of the initial concentration of zinc and copper decreased experimentation. Duration of the process was 40 min and after
within 15-30 min of processing reported by Bazrafshan et al. [16]. every 10 min pH of the solution has been checked using a digital
The maximum removal efficiency of TSS was observed (> 76%) pH meter was found that pH changes from its initial value as
after 40 min of operating time at current density 5.3 mA/cm2 indicated in Fig. 4. At the end of the process pH has been reached
from synthetic water in this study. The efficiency of TSS removal to a value of 7.34, 7.77 and 7.88, respectively, for different interelec-
was increased with an increase in current density from 46.6% trode distances (2-4 cm). In EC where the Al electrode is used,
at 1.3 mA/cm2 till it reaches 76.6% at 5.3 mA/cm2. Beyond 5.3 it has been observed that at passably basic ambience, Al(OH)3
mA/cm2 no further TSS removal was observed. Such lower removal precipitation occurs and the sweep-flock mechanism dominates
efficiency for suspended solids was bubble formation mechanism [19]. Maximum variation was observed at a lower interelectrode
in the reactor [17] investigated that the bubbles formed by EC distance (2 cm) while at another distance pH of water had less variation.
were not sufficient for a high removal efficiency of suspended Chen et al. [15] advocated that in the presence of anions such as
solids. The reason that affects bubble size and generation is that chloride or sulphate, aluminum hydroxide can exchange with these

Table 3. Physiochemical Characteristics of Synthetic Water Used

Electrical conductivity Salinity TDS Turbidity TSS Metal Conc.
Initial pH Colour
(μS/cm) (ppt) (ppm) (NTU) (mg/L) (mg/L)
3.2 1,055 592 748 33 135 Yellowish 10

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 Environmental Engineering Research 22(2) 141-148

Fig. 4. Change in pH value during experiments at various electrode

distances. Fig. 5. Variation of percentage removal efficiencies of heavy metals
with current density after 40 min of EC process time of 7 L
ions thus releasing hydroxyl ions and raising pH. The fact behind synthetic water (Inter electrode distance 3 cm, and pH 7).
this mechanism that the generated metal hydroxides which act as
the flocs and remove the pollutant by sedimentation get degraded density. Both of these trends are benign in terms of high pollutant
by collision with each other due to high electrostatic attraction [20]. removal efficiency by H2 flotation [9]. By observing the impact
of EC operating time on the removal efficiency of metals from
3.4. Effect of Current Density the waste synthetic water, it was observed that removal efficiency
In all EC processes, current density is the most important parameter increases with the increase of electrolysis time, which is in accord-
for controlling the reaction rate within the electrochemical reactor ance with the results of other authors [8, 27]. According to this
and adjusts bubble production and its size and distribution. It work, the highest chromium removal efficiency (> 59%) was ob-
has been found that as current density increases the removal rate tained after 40 min under the condition of 4 mA/cm2 of current
of pollutants also increases [17, 21]. Higher metal removal efficiency density (Fig. 5). Some authors found that the pH of the solution
accomplished by using electrocoagulation-flotation (ECF) with iron has a significant effect on the Cr(VI) removal efficiency [28-30].
electrodes results from its capability of simultaneously inducing The findings show that ions of chromium(VI) change into Cr3+
several processes (metal deposition on the cathode, precipitation, during the reaction that occurs around the cathode, and then the
and co-precipitation of metals) and, more importantly, from the ions of Cr3+ are combined with the OH- resulted from water hydrol-
high sorption capacity of polymeric iron hydroxides generated ysis and Cr(OH)3 is produced. When pH is kept between 3 and
by the anodic dissolution [14, 22]. The current density is expected 7, cations of Al3+ around the anode produce polymeric species
to exhibit a strong effect on the removal efficiency [23-25] especially such as Al13O4(OH)247+ that leads to the effective removal of ions
on the kinetics of heavy metals removal: the higher the current, of Cr3+ via a sweep coagulation process [29]. Zewail and Yousef
the more efficient the ECF treatment. An increase in current density [31] demonstrated the effect of pH on % removal of Cr3+ & Cr6+
from 1.3 to 5.3 mA/cm2 yields an increase in the efficiency of and found maximum % removal of Cr3+ occurs at pH 8, whereas
chromium, copper and zinc removal for aluminum electrode. At the maximum % removal of Cr6+ occurs at pH 4.5. The copper
a high current density, the extent of anodic dissolution of aluminum removal efficiency (> 99%) was obtained after 40 min by using
increases, resulting in a greater amount of precipitate and removal an interelectrode distance of 3 cm and current density of 4 mA/cm2.
of copper, zinc and nickel [26]. In the case of zinc, the removal efficiency (> 82%) at 5.3 mA/cm2
In this study it has likewise been noticed during a process for 3 cm was achieved after 40 min (Fig. 5). A shorter interelectrode
that hydrogen bubble production was more and small in size that distance is desirable, because the electrical resistance (IR drop)
helps to accumulate the pollutants at upper surface at high current increases with the interelectrode distance increase [32]. By increas-
density. Flocs deposited on the surface of the water easily removed ing the interelectrode distance, less interaction of heavy metals
and sludge generated was less in quantity at the bottom of reactor with hydroxide polymers of aluminum is expected [33]. According
as such condition. to the Cu-Pourbaix diagram, copper is solid in the form of Cu(OH)2
at pH approximately > 4.5 until pH 14. The Zn-Pourbaix diagram
3.5. Heavy Metals Removed shows that zinc is solid as ZnO at pH between 7 and 14 [4]. Removal
In this study the experiments conducted for 40 min contact time of copper and zinc has been investigated higher as per Pourbaix
at different current density and electrode distances. Here chro- diagrams indicates pH 7 suitable for such higher removal, but
mium, copper and zinc removal percentages at different time and zinc pourbaix diagrams indicate stability of oxide of zinc due which
current density have been studied. Chromium, Copper and zinc zinc found in stable passive phase at temperature range reported
initial concentration in water were 10 mg/L before the experiment. in revised pourbaix diagrams of zinc [34].
The more current density was applied, the more Al3+ and OH− The results can be explained by the flotation of hydrogen bubbles
were dosed into the ECF system and the faster the metal produced at the cathode, which produce more stable flocks when
concentrations decreased. In addition, the rate of bubble generation the interelectrode distance was 3.0 cm. The lowest interelectrode
increases and the bubble size decreases with the increase of current distances obstruct the adequate mass transport in the ECF cell, thus

145
Hariraj Singh and Brijesh Kumar Mishra

Table 4. Predicted Parameters of First- and Second-order Removal Rates of Heavy Metal Ions at Different Current Densities with Solution Volume
= 7,000 mL, and pH = 7
Second order kinetic,
Current density First order kinetic, Coeff. of Determination Coeff. of Determination
Pollutants 2 2 − dC/dt = k2 C2, k2
(mA/cm ) −1
dC/dt = k1C, K1(min ) (R ) −1 −1 (R2)
(ppm min )
1.3 0.015 0.7802 0.0022 0.6748
2.6 0.016 0.8606 0.0022 0.0001
Cr
4 0.022 0.8491 0.0036 0.8260
5.3 0.015 0.8528 0.0021 0.8301
1.3 0.08 0.7724 0.0632 0.3267
2.6 0.081 0.1488 0.063 0.8253
Cu
4 0.115 0.6740 0.247 0.6435
5.3 0.115 0.7456 0.247 0.1089
1.3 0.009 0.5538 0.0011 0.5400
2.6 0.017 0.7684 0.0017 0.8813
Zn
4 0.031 0.3768 0.0063 0.1255
5.3 0.043 0.8824 0.0114 0.3218
1.3 0.0156 0.2909 0.00016 0.0076
2.6 0.019 0.7529 0.00021 0.6112
TSS
4 0.033 0.8869 0.00053 0.0751
5.3 0.036 0.9560 0.00059 0.9998

Table 5. Consumption of Electrical Energy during Experiments at Different Time Conditions

Electrical energy consumption (kW h/m3)
Voltage, (Volt) Current, (Amp)
10 min 20 min 30 min 40 min
6.3 0.150 0.0216 0.0445 0.067 0.089
8.6 0.300 0.058 0.121 0.184 0.243
14.3 0.450 0.141 0.303 0.459 0.606
16.6 0.600 0.227 0.469 0.711 0.939

reducing removal efficiency rates. This behavior indicates the propor- Only first-order kinetic model can describe the removal rate of
tional importance of water movement and turbulence along the han- chromium ions (Cr3+) at lower current density. The copper and
dling time and their great dependence on the interelectrode space. zinc ions were the only heavy metal ions that their removal rate
can be modeled by first- and second-order kinetics since the corre-
3.6. Effect on Electrical Conductivity sponding R2 value at a lower current density was close to unity.
Electrical conductivity is the ability of the solution to conduct In case of total suspended solids only for both kinetics modeled
electrical current between two electrodes. This electrical con- corresponding coefficient of determination, R2 were close to unity
ductivity seems to affect more directly the voltage or the current at higher current density i.e. 5.3 mA/cm2.
intensity. During the EC process, it has been observed that the
electrical conductivity of the solution in the reactor fluctuated 3.8. Electrical Energy Consumption
in decreasing order due which TDS also changed. It had fluctuated The amount of energy consumed is an important economic parameter
5-6% of its initial value. Decreasing the conductivity of the solution in the EC process. The majority of operating costs is also related
resulted in enhance of the cell voltage. to the amount of electrical energy used. Also in this study the amount
of energy used for metals and TSS removal was evaluated as a function
3.7. Effect of EC Time and Kinetic Study of time in different current densities and potential. When the current
In this work, the kinetic study for the removal of pollutants was density increases from 1.3 mA/cm2 to 5.3 mA/cm2 (0.150-600 A),
considered for various current densities at the ambient temperature the energy consumption increased slightly. Results showed that in-
and constant synthetic water volume. The squared-correlation co- crease in current leads to increase in energy consumption due to
efficient, R2, was used to measure the goodness of the kinetic polarization and increase in the number of aluminum compounds,
model. The kinetic parameters of both first- and second-order which elevate the efficiency of metals and TSS removal as well.
models together with the R2 values are given in Table 4. At current Therefore, in order to reach an optimum current density, it’s
density of 5.3 mA/cm2, the R2 values that correspond to both kinetic necessary to evaluate both the removal percent and the amount
models were found close to unity for all heavy metals and TSS. of electrical energy used [7, 8, 21, 26, 33] as depicted in Table 5.

146
 Environmental Engineering Research 22(2) 141-148

The electrical energy, 0.459 kWh/m3 has been consumed to m Amount of electrode (anode) metal dissociate in reactor, g
achieve 99%, 59.2% and 71.6% removal of Cu, Cr and Zn re- M Molar mass, g/mol
spectively for 30 min process time. Moreover, beyond 4.0 mA/cm2 RE Removal efficiency (%)
current density (0.450 A current) no significant removal was ob- S Anode surface area (cm2)
served as shown in Fig. 3 and Fig. 5. T Time of EC process (h)
U Cell voltage (V)
V Volume of water in reactor (m3)
4. Conclusions Al Electrode with aluminum anode/cathode
Fe Electrode with iron anode/cathode
In this work, EC treatment using aluminum sacrificial electrodes EC Electro-coagulation
for a synthetic water containing Cu, Cr, and Zn heavy metals ECF Electrocoagulation-Flotation
were investigated. Effects of current density, operating time, and TSS Total suspended solids, mg/L
initial pH on the removal efficiency were examined in a parallel TDS Total dissolved solids, mg/L
plate electrochemical reactor.
This study has concluded that experimentally as well as kinetic
modeling has given high removal rate for all metals and TSS at References
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