Cleaner Engineering and Technology 4 (2021) 100261

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Cleaner Engineering and Technology

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Hybrid process of electrocoagulation and electrooxidation system for

wastewater treatment: A review
Yemane G. Asfaha a, b, *, Andinet Kebede Tekile b, Feleke Zewge a
a
Africa Center of Excellence for Water Management, Addis Ababa University, Addis Ababa, Ethiopia
b
Adama Science and Technology University, Department of Water Resources Engineering, Adama, Ethiopia

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

Keywords: Water is one of the most essential natural resources required for all living things. Globally, due to various factors,
Electrocoagulation the volume of wastewater generated and contaminant loads are increasing. Therefore, currently, there is high
Electrooxidation interest and concern in developing more effective wastewater treatment technologies. Particularly, the emerging
Hybrid process
electrochemical methods, mainly electrocoagulation (EC), electrooxidation (EO), and the hybrid of both EC and
Wastewater treatment
EO, have recently attracted attention as a potential method for treating wastewater due to its wide application
and environmental compatibility. In the EC process, different metal hydroxide species are formed. The metal
hydroxides (coagulant) aggregate the dispersed particles in the solution, which forms bigger flocs and then is
removed by sedimentation. In most cases, EC is not able to reduce the stable persistent organic compounds to
below the allowable discharge limits. Also, the EO process is an emerging process where contaminants are
removed by oxidizing directly at the surface of the electrode or indirectly by generating oxidants in the solution.
However, the main drawback of the EO method is that it is not applicable or requires a long operation time for
treating water and wastewater with large amounts of suspended solids. Thus, to use the EO treatment system, the
suspended solids of the wastewater have to be removed first by using other techniques. This can be achieved by a
hybrid process of EC and EO. Besides, the hybrid process can enhance the removal of COD, TOC, NH4+-N, ni­
trates, phenol, which is not effectively achieved by using only EC or EO. Therefore, in this particular review,
special emphasis was given to a hybrid of EC and EO processes, in addition to assessing electrocoagulation and
electrooxidation as exceptional electrochemical methods. Even though several studies have covered EC, EO, and
a hybrid process of EC and EO systems separately, to our best knowledge, there is an extremely limited number of
review papers that have been done on the hybrid process of EC and EO. Therefore, this manuscript aims to review
the potential of a hybrid of the EC and EO processes for treating wastewater generated from various sources.

1. Introduction world’s wastewater is discharged into the natural environment without

Along with air, without which man cannot survive for more than a
few minutes, water is one of our most essential natural resources
(Aulenbach, 1968). Since the available amount of water is limited and
not spatially distributed, proper management of this precious resource is
essential to maintain its sustainability.
Globally, the volume of wastewater generated and contaminant
loads are increasing due to population increment, economic develop­
ment, and expansion of urbanization. Moreover, according to the United
Nations World Water Development Report (WWAP (United Nations
World Water Assessment Programme), 2017), more than 80% of the
treatment. Likewise, in developing countries, a large volume of waste­
water generated is directly connected to the nearest drainage line with
very little or without treatment (WWAP (United Nations World Water
Assessment Programme), 2017).
Thus, to achieve the sustainable development goal of 2030, any drop
of water generated from any source has to be carefully managed during
every part of the water cycle. Also, to minimize the negative impacts on
the aquatic environment, every wastewater generated from each source
has to be efficiently treated before being released into receiving bodies.
To remove the pollutants from the wastewater, there are many
treatment techniques such as biological, Physicochemical, and advanced

* Corresponding author. P.O.Box: 1176, Africa Center of Excellence for Water Management, Addis Ababa University, Addis Ababa, Ethiopia. Tel.: +251 911 57 55
75
E-mail address: yemane.gebreselassie@aau.edu.et (Y.G. Asfaha).

https://doi.org/10.1016/j.clet.2021.100261
Received 18 September 2020; Received in revised form 18 August 2021; Accepted 20 August 2021
Available online 24 August 2021
2666-7908/© 2021 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Y.G. Asfaha et al.
oxidation processes. Physicochemical treatments have good removal
efficiency. However, their use is limited because of the large volume of
chemicals required during the process and the generation of a large
volume of sludge at the end of the treatment (Kurniawan et al., 2006).
Again, biological systems are not always suitable due to their require­
ment of large physical space, some microorganisms are sensitive to some
chemical complexes, and long treatment processes (Núñez et al., 2019).
Moreover, biological methods are difficult to employ for textile effluent,
as the textile effluent is recalcitrant to biodegradation. The advanced
oxidation process is an alternative method to meet their requirements
for chemical and biological methods (Wang and Xu, 2012).
Recently, due to restricting environmental regulations and laws,
researchers have shown that electrochemical treatment systems are
promising technologies to prevent or reduce pollution problems. Aitbara
et al. (2016) conducted a laboratory-scale continuous electro­
coagulation treatment of dairy wastewater collected from factories in
Algeria using Al electrodes. As a result, 90% of COD and 98% of
Turbidity were able to eliminate at the optimal conditions (current
density 15 mA/cm2, electrodes gap 1 cm, supporting electrolyte KCl 2 ×
10− 2 M, temperature 20 ◦ C, and pH of 7.03) with practical energy
consumption between 2 and 3.5 kWh/m3. On the other hand, Amour
et al. (2016) investigated the performance of continuous electro­
chemical reactors and the effect of operating parameters (initial dye
concentration, initial pH, current density, inlet flow rate, and residence
time) on the removal of color and turbidity. Accordingly, 97% of color
and 90% of turbidity were obtained at optimal operating parameters of
initial concentration less than 300 mg/L, initial pH between 2.3 and 8.8,
current density 300 A/m2, inlet flow rate 15 L/h, and residence time of
35 min. At the same time, the electrical energy consumption per kilo­
gram of dye removed was 19.5 kWh. Furthermore, Demir Delil and
Gören (2019a) also studied to investigate the performance of combined
electrocoagulation and electrooxidation electrochemical methods for
real textile wastewater. Besides, the effect of operating conditions
(different electrode arrangements, electrode types, initial pH, applied
voltage, and electrolysis time) of the process was studied on the removal
efficiency of COD and dye color. Finally, at the end of the electro­
coagulation experiment the color and COD was able to reduce from 395
Pt–Co to 28 Pt–Co and 1040 mg/L to 115 mg/L, respectively. In this
study, the maximum removal of COD and color was achieved at 6 V of
applied voltage and pH of 3 with Fe–Fe electrode combination. Simi­
larly, the performance of EO on color and COD removal was performed
and 93% of COD removal was achieved at 6 V with Pt–Fe electrode
combination. According to this study, EC shows best removal efficiency
of than EO. However, the energy consumption of electrooxidation is
more economical than electrocoagulation on COD removal.
In the last two decades, electrochemical methods like electrodepo­
sition (ED), electrocoagulation (EC), electroflotation (EF), electro­
oxidation (EO), and a hybrid of electrocoagulation-electrooxidation (EC-
EO) processes, have got a great attraction as efficient technology by
researchers (Can, 2014). Indeed, to improve the performance of elec­
trocoagulation, it has been integrated with many other treatment
methods such as biological, electro-Fenton, and photo-catalytic
(Suárez-Escobar et al., 2016). Very recently, scholars (Al-Qodah et al.,
2019) reviewed different research articles focused on the combination of
electrocoagulation with various biological wastewater treatment
methods as it can enhance its performance and removal efficiency. In
this review article, the authors noted that compared to the separate EC
process, the combined process of EC with biological treatment method
increases the removal efficiency of water pollutants by 20%. Another
study by Al-Qodah et al. (2018) reviews research on the performance of
electrocoagulation methods assisted by free-radical, ozone, advanced
oxidation, and ultrasound energy. In this review article the mechanism,
kinetics, and cost of the electrocoagulation process assisted by free
radical were well discussed. The authors observed that the effectiveness
of the combined processes was enhanced, and better removal efficiency
(>95%) was obtained with the electrocoagulation process assisted by
2
Cleaner Engineering and Technology 4 (2021) 100261
ozone. Furthermore, the review articles indicate that the use of ultra­
sound energy reduces the electrode passivation problem of electro­
coagulation and improves the performance of the processes.
Similarly, electrooxidation has been integrated with other treatment
processes such as biological (Katsoni et al., 2014), coagulation (Abdes­
samad et al., 2015), and adsorption (Akrout et al., 2015). Moreover, the
electrochemical method, especially electrooxidation using the
boron-doped diamond (BDD) electrode has got great attention due to its
capacity of removing numerous organic and inorganic pollutants
(Ghazouani et al., 2017). However, the power consumption is very high
and as a result, it increases the overall cost of the process. On the other
hand, Anglada et al. (2010) studied the technical and economic feasi­
bility of EO using BDD based on COD and ammonia (NH4+) concentra­
tion reduction, and energy consumption, respectively from landfill
leachate at a pilot scale. The results were examined and compared with
other methods of advanced oxidation processes. Under the optimum
operating conditions, the concentrations of COD and NH4+ were
removed up to 160 mg/L and 30 mg/L, respectively with maximum
energy consumption of 54 kWh/m3. The pollutants were removed below
the level of discharge limit and low formations of by-products.
In this particular review, special emphasis was given to electro­
coagulation (EC), electrooxidation (EO), and the hybrid process of
electrocoagulation and electrooxidation (EC-EO) system. Even though
several studies have covered EC, EO, and a hybrid process of EC-EO
systems separately, to our best knowledge, no review work has been
done on the hybrid process of EC-EO applied for various pollutant re­
movals from wastewater. Therefore, this paper aims to review the po­
tential of a hybrid of the EC-EO process for the treatment of wastewater
generated from various sources. The review paper tried to include the
most recent publications of 2020 and describes, discussing, and com­
pares the potential of each electrochemical method.
2. Electrocoagulation (EC) method
Electrocoagulation can be defined as a process to remove contami­
nants from wastewater by using electricity and to neutralize the negative
particles by the formation of hydroxide complexes in water to gather the
suspended solid, help bridge, bind and strengthen the floc for sedi­
mentation due to gravity force (Fagnekar Nilesh A., 2015). This process
agglomerate the suspended solid in water without chemical coagulant,
and the coagulation happened when the direct current (DC) is applied to
the aqueous solution. Besides, Electrocoagulation involves the genera­
tion of coagulants in situ by electrical dissolution from the respective
metal electrodes (Al, Fe, Cu, or Stainless steel). The dissolved metal ion
and hydrogen gas are generated at the anode and cathode, respectively
(Linares-Hernández et al., 2010a).
Several factors influence the electrocoagulation process such as the
type of electrode, the surface area of the anode electrode, the gap be­
tween electrodes, the number of electrodes, the size of electrodes, cur­
rent density, charge loading, pH of the sample, operational time, and
addition of supporting electrolyte (Can et al., 2006). The electrodes that
are usually used are iron, aluminum, stainless steel, and copper. Among
these, due to the high coagulation efficiency of Al3+, aluminum plates
are more preferable to use for wastewater treatment in combination
with iron plates (Shen et al., 2003). If the solution has a significant
amount of Ca2+ or Mg2+ ions, it is recommended to use stainless steel
material as a cathode (Chen, 2004). During the EC process cathode is
oxidized (loss of electrons) and the water is reduced (gain electrons)
resulted in treated water and easy to settle floc (Fagnekar Nilesh A.,
2015).
Electrocoagulation Process is an electrolysis process for wastewater
treatment using a pair of electrodes (anode and cathode). Electrodes
used in the EC process can be arranged in mono-polar or bipolar
(Demirci et al., 2015). In the mono-polar electrodes in parallel
connection (MP-P), the sacrificial electrodes are connected to the source
of power (Fig. 1). Moreover, in the bipolar electrodes in parallel
Y.G. Asfaha et al.
Fig. 1. Schematic view of the EC reactors (MP-P): (1) current regulator; (2)
electrodes; (3) electrocoagulator unit/reactor; (4) treated water reservoir
(Ozyonar, 2016).
connections (BP–P), the sacrificial electrodes are switched between two
parallel electrodes without connection to the power source. That is,
there is no interconnection between the sacrificial anodes but the two
outer electrodes are connected to the power source (Demirci et al.,
2015). Likewise, in the mono-polar electrodes in series connection
(MP-S), each pair of sacrificial electrodes are internally connected. Be­
sides, in the bipolar electrodes in series connection (BP–S), the outer
electrodes are connected to the power source without an internal
connection between the inner electrodes (Song et al., 2017).
Despite the majority of EC researches (Dubey and Kumar Prajapati,
2019) which is conducted using a conventional vertical electrode
connection, some studies have been done using a horizontally arranged
electrode connection (Fouad et al., 2009). For instance, Fouad et al.
(2009) obtained 99.8% (from 500 to 6 ppm) of reduction in oil con­
centration from the aqueous solution within 30 min using a horizontally
arranged electrode connection.
A positively charged are attracted to the negatively charged hy­
droxides in the solution (Fig. 2) and they produce ionic hydroxides that
make a strong attraction towards dispersed particles as the counterions
cause coagulation.
According to many reports and Al Aji et al. (2012), the following
three successive stages are the main steps in the EC process:
Fig. 2. Principle of electrocoagulation (An et al., 2017).
3
Cleaner Engineering and Technology 4 (2021) 100261
i. Formation of coagulants by electrolytic oxidation of the electrode.
The main reaction occurring at the metal anode is dissolution:
M(s) → M(aq)n+ + ne− (1)
Additionally, water electrolysis occurs at the cathode and anode:
2H2 O(l) + 2e− →H2 (g) + 2OH − (cathodic ​ reaction) (2)
2H2 O(l) → 4H + (aq) + O2 (g) + 4e− (anodic ​ reaction) (3)
ii. Destabilization of the contaminants, particulate suspension, and
breaking of emulsions. A direct electrochemical reduction of metal
cations (Mn+) may occur at the cathode surface:
M n+ + ne− →nM o (4)
Furthermore, the hydroxide ions formed at the cathode increase the
pH of the wastewater thereby inducing precipitation of metal ions as
corresponding hydroxides and co-precipitation with hydroxides:
M n+ + nOH − →M(OH)n (s) (5)
iii. Aggregation of the destabilized phases to form flocs. Anodic
metal ions and hydroxide ions generated at the electrode surfaces
react in the bulk wastewater to form various hydroxides and
built-up polymers. Furthermore, the following physicochemical
reactions may also take place in the EC cell (Al Aji et al., 2012):
cathodic reduction of impurities present in wastewater, discharge
and coagulation of colloidal particles, electrophoretic migration
of the ions in solution, electro-flotation of the coagulated parti­
cles by oxygen and hydrogen bubbles produced at the electrodes,
reduction of metal ions at the cathode, other electrochemical and
chemical processes.
The electrocoagulation method has attracted great attention for
treating various wastewaters because of its wide application and envi­
ronmental compatible (Azarian et al., 2018). Also, the EC process has
many advantages such as simple equipment requirements, easy opera­
tion, a shortened retention time, no or small chemical additions, and less
formation of sludge. Moreover, the application and advantages of EC are
Y.G. Asfaha et al. Cleaner Engineering and Technology 4 (2021) 100261

well discussed and reviewed by (Zaied et al., 2020). than 3 gm/L (Szpyrkowicz et al., 1994).
In the EC process different monomeric and polymeric metal hy­ According to Özyurt and Camcıoğlu (2018), the following equations
droxide species are formed through the oxidation of sacrificial elec­ are the main anodic oxidation of organic pollutants and generating in­
trodes. The metal hydroxides (coagulant) aggregate the colloidal direct oxidizing agents during the EO process.
particles in the solution which forms bigger flocs that are removed by
sedimentation (Chen, 2004). In those cases, EC was not able to reduce i. Direct oxidation:
the chemical oxygen demand (COD) level to below the allowable
discharge limits. Therefore, to enhance the performance of EC, it is H2 O + S → S[OH]• + H + + e− (6)
essential to integrate with other methods like electrooxidation, Fenton,
R + S[OH]• → S + RO + H + + e− (7)
photo-Fenton, electro-Fenton, ozonation, photocatalysis, and other
degradation methods (Nidheesh et al., 2020).
H2 O + S + Cl− → S[ClOH]• + H + + 2e− (8)
Another research by Can (2014) conducted a study on COD removal
from fruit juice plant wastewater. And, the objective of this research was
R + S[ClOH]• → S + RO + H + + Cl− (9)
to investigate the removal efficiency of COD from the fruit juice plant
wastewater using three different electrochemical processes; namely H2 O + S[OH]• → S + O2 + 3H + + 3e− (10)
electrocoagulation (EC), electrooxidation (EOx), and electro-Fenton
Processes (EF). Accordingly, The performance of each process was H2 O + S[OH]• → S + H2 O2 + H + + e− (11)
evaluated by comparing it with each technology (Table 4). The sampled
wastewater from fruit juice production had high COD content (20,713 S[OH]• + H2 O2 → S + HO2 • + H2 O (12)
mg/L). During the EC process, Al and Fe electrode materials were used
to remove COD from the solution. Again, to remove COD from the O2 + S[OH]• → S + O3 + H + + e− (13)
wastewater by the EF process, simply H2O2 was added to the EC reactor
by changing the anode and cathode electrodes with iron and titanium, H2 O + S[ClOH]• + Cl− → Cl2 + S + O2 + 3H + + 4e− (14)
respectively. As a result, 52.4 and 64.7% maximum COD removal were
achieved by EOx at 60 min and 360 min, respectively. From the EC H2 O + S[ClOH]• + Cl2 → S + ClO2 + 3H + + 2Cl− + e− (15)
process, 59.1% and 61.3% of COD were removed using aluminum and
an iron anode, respectively. Besides, 84.4% maximum removal of COD ii. indirect oxidation:
by EF was achieved by adding 10 mL of H2O2 at the end of 25 min
electrolysis time. Thus, the results showed that electrocoagulation per­ 2Cl− → Cl2(g) + e− (16)
forms less to remove COD. Moreover, this shows even less performance
than an air bubble column bioreactor, 92.2% COD removal (Kosseva, Cl2 + H2 O→HClO + H + + Cl− (17)
2017). According to the study by Kazem et al. (2012), the highest
removal of COD (95.6%) was achieved using the Al electrode at acidic HClO → H + + ClO− (18)
pH conditions between 2 and 3. Therefore, EC is recommended as a
suitable technology for poultry slaughterhouse wastewater treatment. H2 O + R + ClO− + H + →RO + H3 O+ + Cl− (19)
From this result, it has been observed that electrocoagulation as a
3
separate technology can remove COD to the maximum level from 6ClO− + 3H2 O→2ClO3 − + 4Cl− + 6H + + O2 + 6e− (20)
2
poultry slaughterhouse wastewater. Chen (2004) reviewed more than
300 research outputs focused on the design, development, and appli­ Furthermore, the formation of chloride anions and hydrogen gas at
cation of electrochemical technologies namely electrocoagulation, the cathode both at the acidic and alkaline conditions are stated below
electrodeposition (ED), electroflotation (EF), and electrooxidation (Sirés et al., 2014):
methods for water and wastewater treatments. Accordingly, ED was 2H3 O + 2e− →H2(g) + 2H2 O(at ​ acidic ​ conditions) (21)
found most effective for heavy metal recovery from wastewater.
Comparatively, EF is effective in removing organic pollutants, colloidal 2H2 O + 2e− →H2(g) + 2OH − (at ​ alkaline ​ conditions) (22)
particles as well as oil and grease. Moreover, EF is effective to separate
flocculated sludge from the treated water. Furthermore, Shen et al. ClO− + H2 O + 2e− →Cl− + 2OH − (23)
(2003) presented the removal of fluoride concentration from synthetic
solution using a combined electrocoagulation and electroflotation Where, S, R is the active spot of anodic surface, and the organic
method. As a result, at optimum operating condition of pH 6, charge pollutant, respectivelyscholars (Valero et al., 2014) showed that elec­
loading 4.97 F/m3, and electrolysis time of 20 min the concentrations of trooxidation is an effective technique to destroy various persistent and
fluoride were reduced from 15 to 2 mg/L. recalcitrant organic pollutants using different potential electrodes
(Table 1).
3. Electrooxidation (EO) method According to Chaplin (2014), Tin dioxide (SnO2) has low conduc­
tivity, and to improve its conductivity it must be doped with antimony
The EO process is an emerging process where contaminants are (Sb) which has high conductivity and potential for oxygen progression.
removed by oxidizing directly at the surface of the electrode or indi­ Carbon electrodes and titanium sheets coated with active oxides like
rectly by generating oxidants in the solution (Özyurt and Camcıoğlu, ruthenium dioxide (RuO2), iridium dioxide (IrO2), or SnO2 have been
2018). Moreover, direct electrooxidation occurs through the generation successively used to oxidize both phenol and chlorophenols (Cossu et al.,
of physically adsorbed oxygen species (hydroxyl radicals, •OH) or 1998).
chemisorbed oxygen species (MOx+1) (Comninellis, 1994). Besides, the Furthermore, the major drawback of the EO method is that it per­
performance of the anodic oxidation process mainly depends on the forms less for treating water and wastewater with a high concentration
selection of an anodic electrode. The types of anodic materials and their of suspended solids. Thus, to use the EO treatment system the waste­
performance are clearly described by (Chen, 2004). Moreover, indirect water containing suspended solids has to be removed first by using other
electrooxidation happens by generating chlorine or hypochlorite during techniques. This can be achieved by integrating with other methods like
anodic oxidation. This process is effective to remove organic and inor­ the hybrid process of EC and EO (Chakchouk et al., 2017).
ganic contaminants at a high concentration of chloride, the best greater

4
Y.G. Asfaha et al. Cleaner Engineering and Technology 4 (2021) 100261

Table 1
Performance of different EO electrodes (Chen, 2004).
Anode Pollutant Current density CE (%) Removal efficiency (%) Comment Ref.
(A/m2)

Granular Phenol 0.03–0.32 70 70, 50 of 5-month stable operation Awad and Abuzaid
graphite mineralization (1997)
Planar graphite Phenol 10–100 24.6–63.5 6-17 of COD NaOH as electrolyte Kanna et al. (1995)
Pt and Ti/Pt Phenol 300 30 of TOC pH 12, initial concentration 1000 mg/L, in Polcaro et al.
0.25 M Na2SO4 (1999)
Ammonia 8.5 53 95 pH 8.2 using phosphate buffer, poor Marinčić and Leitz
performance for organics (1978)
Glucose 100–900 15–20 30 1 M H2SO4 Bonfatti et al.
(2000)
15 organics 5 Stucki et al. (1991)
PbO2 Aniline I=2A 15–40 >90 (in 1 h) initial concentration 2/7 mM, pH 2, Pulgarin et al.
packed bed of PbO2 (1994)
Phenol I = 1, 2,3 A 46–80 initial concentration 14–56 mM, Chen et al. (1999)
Ti/PbO2 Phenol 300 40 of TOC pH 12, initial concentration 1000 mg/L, in Polcaro et al.
0.25 M Na2SO4 (1999)
Landfill leachate 50–150 30 for COD 10% for 90 for COD, 100 for Grimm et al.
NH4+-N NH4+-N (1998)
Glucose 100–900 30–40 100 1 M H2SO4 Bonfatti et al.
(2000)
2-Chlorophenol 80–160 35–40 80-95 of COD Pb2+ formation, initial COD was 1000 mg/ Kirk et al. (1985)
L, 25 ◦ C
IrO2 Organic 17 (Guo, Li, Chen,
2010)
1, 4- Rupture of rings only Rodgers et al.
Benzoquinone (1999)
Ti/SnO2–Sb2O5 2- hlorophenol 80–160 35–40 80-95 of COD Oxalic acid as intermediates Bonfatti et al.
(2000)
Glucose 100–900 <20 30 1 M H2SO4 Polcaro et al.
(1999)
Phenol 300 100 pH 12, initial concentration 1000 mg/L, in (Guo, Li, Chen,
0.25 M Na2SO4 2010)
500 58 70 ◦ C, 10 mM, similar to PbO2 Kötz et al. (1991)
Landfill leachate similar to PbO2 Grimm et al.
(1998)

Fig. 3. Schematic diagram of the electrocoagulation-electrooxidation treatment process and hypothesized treatment effects for each stage (Heffron et al., 2019).

5
Y.G. Asfaha et al. Cleaner Engineering and Technology 4 (2021) 100261

4. Hybrid of electrocoagulation and electrooxidation (EC and Therefore, to increase the removal of COD, a hybrid of EC and EO was
EO) method implemented which reduced the COD level by about 60% at 21 min. The
removal efficiency of the three electrochemical treatment technologies
Among the electrochemical treatment systems, EC and EO are the applied to reduce pollutants from dairy industry effluent is summarized
most promising techniques due to no or small chemical requirements in Table 2.
and the easiness of operation (Yılmaz Nayır and Kara, 2018). As it has Also, Yılmaz Nayır and Kara (2018) demonstrated the treatment of
been clearly stated by Bhagawan et al. (2016), electrocoagulation is a container washing wastewater (CWW) using a hybrid of EC-EO. They
fast but ineffective process. Relatively, electrooxidation is an effective were focused on the removal efficiency of soluble chemical oxygen de­
but slow method, and a hybrid of the two processes gives a practical and mand (sCOD) and color. The experiment was performed first by EC using
promising result (Özyurt et al., 2017). Al and Fe electrodes. Thus, at the optimum operating conditions (current
In recent years, a hybrid process of EC and EO on sequential or density of 25 mA/cm2, pH of 5, and electrolysis time of 120 min)
simultaneous arrangement has been used for the treatment of waste­ maximum sCOD removal of 82% was attained. Similarly, color removal
water sampled from container washing (Yılmaz Nayır and Kara, 2018), of 95, 95, and 98% were achieved using the Fe electrode at 436, 525, and
soft drink industry (Linares Hernández et al., 2017), fruit juice pro­ 620 nm, respectively. However, EC shows less performance to remove
duction plant (Can, 2014), Agro-food industry (Ghazouani et al., sCOD. Therefore, a hybrid process of EC and EO was implemented in
2019a), gelatin production plant (Lakshmi Kruthika et al., 2013), textile which EO was processed as a post-treatment of EC using a boron-doped
synthetic (Raju et al., 2008), textile real (Demir Delil and Gören, 2019b), diamond electrode (BDD). Accordingly, the removal of sCOD was
soluble coffee (Ibarra-Taquez et al., 2017a), petroleum refinery (Bha­ improved to 89% at 420 min, but the removal efficiency of color was
gawan et al., 2016), landfill leachate (Ghanbari et al., 2020), canola-oil decreased to 72, 64, 71% using the same optimum current density and
refinery (Sharma and Simsek, 2019), decolorization and removal of an wavelength, respectively. From this, it is possible to conclude that, due
indigo carmine textile dye (Stergiopoulos et al., 2014), pulp and paper to the colloidal particles found in the aqueous solution, EO alone re­
mill (Özyurt et al., 2017), dairy production (Chakchouk et al., 2017), quires a relatively long electrolysis time (not practical) which is also in
COD removal and recovery of tannery industry wastewater (Ghasem line with (Chakchouk et al., 2017). On the other hand, Linare­
et al., 2017), mitigation of virus in drinking water (Heffron et al., 2019), s-Hernández et al. (2010b) also conducted a study on a hybrid of EC-EO
ultrafiltration membrane fouling (Sun et al., 2018a), pre-treatment on treatment for industrial wastewater. This study aims to investigate the
the fungal treatment of pistachio processing (Isik et al., 2020), and in­ performance of EC and EO separately and in a hybrid process using the
dustrial wastewater (Linares-Hernández et al., 2010b). The treatment real wastewater collected from the outlet of the biological wastewater
flow diagram of the electrocoagulation-electrooxidation process applied treatment plant. As a result, EC was very effective in removing colloidal
for dairy wastewater treatment is shown in (Fig. 3). and suspended particles at an operation time of 30 min (a very quick
Indeed, the different pollutants produced from various sources have process). However, it was less effective to remove COD, in which almost
been removed using batch and a continuous system of EC and EO hybrid only half of it was able to reduce from the wastewater. Relatively, EO
processes (Heffron et al., 2019). Batch reactors are more suitable for alone was very effective in removing organic compounds such as COD
laboratory and pilot-scale studies with less working volume of the and BOD5 but it requires a long operation time which is not practical.
reactor, while the continuous modes of reactors are suitable for indus­ During the application of the hybrid process, the colloidal and sus­
trial wastewater treatment studies with a large volume of flow. Besides, pended solid particles, as well as many charged species were removed
because it is easy to control and manage the operations, the continuous quickly by EC and then EO oxidizes the remaining pollutants. Therefore,
mode/or system is preferred to the batch mode/or system. During the the hybrid system is very effective to remove all color, turbidity, and
hybrid process of EC and EO processes encompassing both batch and coliforms, BOD5, and COD to the allowable limit within the practical
continuous mode, most of the time, a batch system is used to investigate electrolysis time.
the optimum operating parameters of the treatment method, and then Furthermore, Linares Hernández et al. (2017) conducted a study on a
only the effect of the initial concentration of the targeted pollutant and monopolar hybrid process of EC-EO for soft drink wastewater treatment.
flow rate will be evaluated through the continuous mode of operation Copper (Cu) was used as an anode and cathode material for the EC
(Naje et al., 2017). method. To achieve this objective the current density was varied with
Even though several types of research have been done using the 17, 51, and 68 mA/cm2. During the EC process, only 37.67% of COD and
batch-type reactor (Yılmaz Nayır and Kara, 2018), however, the 27% of TOC were able to remove at 20 min operating time and pH of 8.
research work on the comparison of both Batch- and continuous-type To enhance the removal efficiency of the system EO was performed as a
reactor especially on the hybrid method of electrocoagulation and post-treatment of EC. The EO process was performed using BDD as anode
electrooxidation processes are few. This includes the performance and Cu as a cathode at an optimum current density of 30 A/m2. As a
evaluation of a continuous flow reactor and batch reactor for electro­ result, the removal efficiency was enhanced to 75 and 85% for COD and
coagulation and electrooxidation processes (Ardhan et al., 2015).
Lakshmi Kruthika et al. (2013) performed a hybrid process of EC and EO
Table 2
systems with continuous and batch systems of a reactor, respectively. So, Physicochemical characteristics of hybrid EC and EO treatment for dairy
the maximum removal was achieved in the range of 38–54%, and 80% of wastewater (Chakchouk et al., 2017).
total organic carbon (TOC) using continuous and batch systems of a
Parameters Raw EC EO Hybrid process of EC-
reactor, respectively. On the other hand, Linares Hernández et al. (2017) sample EO
researched soft drink wastewater treatment by a hybrid of consecutive
COD (mg/L) 3850 2079 2503 1390
electrocoagulation and electrooxidation processes in a batch-type
BOD5 (mg/L) 2800 1100 1900 1000
reactor. Accordingly, only 27 and 85% of TOC could be removed Suspended matter (mg/ 831 140 180 30
using EC and EO, respectively at pH 8. L)
The physicochemical characteristics of diary effluent are mainly Fatty Matter (mg/L) 230 16 20 6.6
composed of total solids and dissolved solids resulting in a high con­ pH 6.62 6.94 7.03 7.04
Conductivity (mS/cm) 4.08 3.98 4 3.69
centration of COD and BOD5 (Chakchouk et al., 2017). Thus, to remove PT 21 2.6 20.4 0.7
these pollutants, EC, EO, and hybrid of EC and EO were performed. The NTK (mg/L) 140 100 133 79
results showed that EC was very effective and quick (6 min) to remove Cl− (mg/L) 460 426 358 341
colloidal and suspended particles, but ineffective to remove COD. Na+ (mg/L) 352 340 345 322
K+ (mg/L) 56 17 19 12.6
Similarly, EO alone was able to reduce COD by about 40% at 30 min.

6
Y.G. Asfaha et al.
TOC, respectively. Accordingly, the hybrid system of EC-EO was effec­
tive to remove pollutants from soft drink wastewater and it also reduced
the operation time and operating cost which contributes to the sus­
tainable reuse of industrial liquid effluent. Similarly, Ghazouani et al.
(2019a) conducted a comparative study of electrochemical hybrid sys­
tems for the treatment of real wastewaters from agri-food activities. This
study aimed to investigate the efficiencies of two electrochemical
treatment processes (electrochemical oxidation/reduction (EOR) and
electrocoagulation) set through two scenarios (first combination: 3 h of
EOR followed by 1 h of EC, and second combination: 1 h of EC followed
by 3 h of EOR) for the treatment of two different industrial effluents;
namely poultry slaughterhouse wastewater (SHWW) and dairy waste­
water (DWW). Besides, the removal efficiency of these systems was
evaluated in terms of COD, nitrates, ammonium/ammonia, and phos­
phates as well as electric energy consumption. Also, the performance of
EOR was evaluated on a bipolar electrode arrangement with
boron-doped diamond supported on silicon electrodes. The EC treatment
system was performed with mild steel electrodes connected in parallel.
Accordingly, the results for both scenarios (3 h of EOR followed by 1 h of
EC and 1 h of EC followed by 3 h of EOR) are summarized in Table 3.
The results showed that the EOR treatment system had the highest
removal efficiency of the pollutants from the two sources except for the
phosphates which were fully removed by the EC process. Generally, the
second scenario showed a better removal rate when the EC system was
used as a pre-treatment.
Also, Lakshmi Kruthika et al. (2013) studied the efficacy of electro­
coagulation and electrooxidation methods for wastewater treatment
generated from the gelatin production plant. As the wastewater gener­
ated from the gelatin factories is very complex and difficult to treat by
conventional techniques, electrochemical methods were implemented
in this study. The result showed that around 60% of TOC removal was
achieved by electrocoagulation alone using the Al electrode as anode.
However, the performance was highly affected especially due to the
scaling of the anodes. To minimize this problem and improve the per­
formance, bicarbonate was used to precipitate calcium as calcium car­
bonates (CaCO3). Since the removal efficiency of the EC process was
limited, EO was implemented along with EC using the IrO2–Ta2O5
coated Ti electrode and TiO2 nanotubes grown on the Ti sheet (TiO2
nanotubes) as electrodes. As a result, 80% TOC removal was observed by
the TiO2 nanotubes (NT) electrode. Heffron et al. (2019) also conducted
a study on sequential electrocoagulation for virus mitigation in drinking
water. The main objective of this study was to evaluate EC as a pre­
treatment for the disinfection of water-born viruses by EO using iron and
BDD electrodes, respectively. It is novel research to investigate a
sequential EC-EO system for virus mitigation. To achieve the objective of
the research bench scale-batch reactors were implemented. The
collected wastewater from the surface and groundwater was first treated
by electrocoagulation and then by sequential EC-EO. The two bacte­
riophages (MS2 & ФX174) were inhibited from the surface water and
groundwater model. The results indicate that EC alone showed better
performance than the hybrid of the EC-EO system for groundwater.
Likewise, the hybrid of the EC-EO system showed better performance
only in the surface water models (Zinicovscaia and Cepoi, 2016). In
Table 3
Removal efficiency of EOR and EC for pollutants from SHWW and DWW.
Pollutants (mg Concentrations First combination: 3 h of EOR followed by
L− 1) 1 h of EC
Initial SHWW Treated SHWW
COD 2366 71.7
N–NO3- 0.45 1.9
P-PO43- 19.2 0 100
Initial DWW Treated DWW
COD 3350 254.9
N–NO3- 471 38.8
P-PO43- 12.4 0 100
Cleaner Engineering and Technology 4 (2021) 100261
general, electrooxidation improves virus reduction beyond electro­
coagulation alone. Moreover, Ibarra-Taquez et al. (2017a) investigated
the performance of sequential EC and EO processes for the treatment of
soluble coffee effluent using aluminum and graphite electrodes,
respectively. They were focused on the degradation of color, COD, and
TOC of the effluent as well as optimization of operation time analysis. In
the individual electrooxidation process, maximum color removal of
about 100%, COD removal of 74%, and TOC removal of 63.5% were
achieved. Then, the integrated process was performed and able to
reduced COD and TOC by about 89% and 72%, respectively. Finally, the
authors concluded that the hybrid of the EC-EO system is an efficient
alternative for the treatment of soluble coffee wastewater.
In addition, Bhagawan et al. (2016) conduct a study on the hybrid of
the electrochemical method for petroleum refinery wastewater treat­
ment. The purpose of this research was to evaluate the performance of
EC and electrochemical hybrid processes on phenol, COD, TOC, oil, and
grease removal. The hybrid process of electrochemical processes namely
electrocoagulation and electrooxidation (EC and EO),
ultrasono-electrocoagulation at 25 (ECS25) and 33 kHz (ECS33), ECEO
plus ultra-sonication at 33 kHz (ECEO + US33) were performed,
respectively. Results showed that, applying hydrogen peroxide to
enhance the oxidative process of the ECEO process followed by
ultra-sonication at 33 Khz (ECEO + US33) accomplished the maximum
removal efficiency of 98, 92, 92, 92% of phenols, COD, TOC, oil, and
grease, respectively. Therefore, it is possible to conclude that, the hybrid
process of electrochemical is a promising and reliable technique for
petroleum refinery wastewater (PRW) treatment.
In general, several investigations have been done on the treatment of
various water and wastewater treatments, and reducing membrane
fouling in membrane filtration by the hybrid system is shown in Table 4.
On the other hand, different potential electrodes have been applied
for the hybrid of EC-EO (Table 4). However, the selection of electrode
material is very important as it influences the removal efficiency of the
system. Therefore, to achieve maximum removal efficiency, the elec­
trode material must have properties such as high electrical conductivity,
resistance to water corrosion, high stability as well as low cost to life
ratio.
Recently, Boron-doped diamond (BDD) and titanium-based boron-
doped diamond film (Ti/BDD) electrodes are commonly used in EO
research due to their high resistance to chemical and thermal degrada­
tion and low tendency to react with solvents as well as it shows high
performance and gives reasonable stability (Macpherson, 2015). More­
over, BDD in EO is capable of removing pollutants including pathogens
through either the production of reactive oxygen species from electro­
chemical water decomposition or free chlorine and chlorine dioxide
produced from the oxidation of chloride (He et al., 2019). In the absence
of chloride, hydroxyl radicals at the surface of the electrodes are the
primary oxidant species and the oxidation process relies on the electrode
surface (Bruguera-Casamada et al., 2017). In general, the efficiency of
the Boron-doped diamond-electrooxidation method increases with the
concentration of chloride in the water matrix (Rajab et al., 2015).
Removal efficiency second combination: 1 h of EC followed by 3 Removal efficiency
(%) h of EOR (%)
Treated SHWW
97 31.7 67
− 322 3.1 101
0 100
Treated DWW
92 113.9 − 23
92 5.7 94
0 100
7
Y.G. Asfaha et al. Cleaner Engineering and Technology 4 (2021) 100261

Table 4
Hybrid process, EC-EO or EC and EO for water and wastewater treatment.
Anode Pollutant Current Techno-logy Removal efficiency Comment Ref.
density (%)
(mA/cm2)

Fe sCOD 25 EC 82 (Yılmaz Nayır and

Color 25 EC 85, 95, 98 at 436, 525, 620 nm, respectively and pH 5, 120-min Kara, 2018)
BDD sCOD 25 EO 89 EO was post treatment process
Color 25 EO 72, 64,71 at 436, 525, 620 nm, respectively and pH 3, 300-min
Cu COD 17, 51 EC 37.67 pH 8, 20 min Linares Hernández
TOC 17,51 EC 27 hybrid process et al. (2017)
BDD COD 3 EC-EO 85
TOC 3 EC-EO 75
Graphite COD 20 EO 52.4, 64.7 at 60 and 360 min, respectively Can (2014)
Al COD 20 EC 59.1 At 25 min, pH 3.5, EO was performed before and
continued with EC
Fe COD 20 EC 61.3
Fe COD 20 EF 84.4 At 25 min, pH 3.5, 10 mL of H2O2
BDD COD (SHWW, DWW) 35.7 EOR 97, 88 BDD supported on silicon electrodes, 6 h electrolysis time Ghazouani et al.
nitrates (SHWW, EOR 99 (2019a)
DWW)
Mild steel COD (SHWW, DWW) 5 EC 89, 74
Nitrates (SHWW) EC 100 after 30 min of treatment
nitrates (DWW) EC 88.6 at the end of treatment
BDD-Mild COD (SHWW, DWW) EOR-EC 97, 92 EOR followed by the EC process
steel nitrates (DWW) EOR-EC 92 EOR followed by the EC process
Mild steel- COD (SHWW, DWW) EC-EOR 98.7, 96.6 EC followed by the EOR process, the EC treatment was
BDD carried out on mild steel electrodes for 1 h followed by 3 h
of treatment with BDD
Al TOC EC 60 Lakshmi Kruthika
TiO2 NT TOC 12.5 EO 80 better oxidation was observed with Titanium oxide et al. (2013)
nanotube electrode
Ti/ TOC 12.5 EO 58
IrO2–Ta2O5
Al suspended solids (SS) 12, 18, 24 EC 99 Al-98% purity, EC was conducted first to remove SS Raju et al. (2008)
Al COD 30 EC 62 Al was more effective than Mild steel
RuO2/IrO2/ COD EO 16 COD removal was high with graphite electrode
TaO2
Graphite COD EO 97 EO was conducted using the filtrate water from EC
Fe virus inactivation EC removed to an sequential EC-EO treatment was adopted than Heffron et al.
(MS2 & ФX174) acceptable range simultaneous EC-EO (2019)
BDD virus inactivation EO EO improves virus reduction beyond EC alone
(MS2 & ФX174)
Al COD EC 74 Al purity of >99%, Ibarra-Taquez
Graphite TOC EO 63.5 EC-12 grade of graphite, sequential EC-EO treatment et al. (2017a)
Al, graphite COD, TOC EC-EO 89, 72 coupled EC-EO process is efficient than EO alone
Al for EC, SS phenols, COD, TOC, ECEO + 98, 92, 92, 92 EC-EO followed by ultra-sonication at 33 KHz, H2O2 Bhagawan et al.
for EO oil, and grease US33 (2016)
Al Humic acid (HA) UF 57.78 ± 1.13 indicating severe membrane fouling (This was due to the Sun et al. (2018b)
fractions/membrane blockage of membrane
fouling
HA molecules into membrane pore directly through the
breaking up of HA molecules
Ti–Ru HA fractions/ ECMR 77.33 ± 1.76 Coagulation and sedimentation happened before reached
membrane fouling membrane filtration
Ti–Ru HA fractions/ EOMR 73.70 ± 4.27 surface porosity is 15.30%, 13.73%, 16.73% for ECMR,
membrane fouling EOMR, ECOMR, respectively
Al/Ti–Ru HA fractions/ ECOMR 86.90 ± 4.0 EOMR>ECMR>EOMR>UF, & all measurement is based
membrane fouling on normalized water flux
Fe indigo carmine dye 5 and 10 EC 100 in 35 and 20 min process, coagulation increases with Stergiopoulos et al.
increasing current density (2014)
Ti/Pt indigo carmine dye 5 and 10 EO 100 in 20 min process
Graphite indigo carmine dye 5 and 10 EO 100 in 35 min process
Fe indigo carmine dye 5 and 10 electro- 100 the electro-Fenton process with Fe electrode and H2O2 in
Fenton acidic solution was the fastest
Al COD, NH3–N 40 EC 49.8, 9.8 30 min rxn time Ilhan et al. (2007)
Fe COD, NH3–N 40 EC 7.4 of NH3–N At the end of 30 min, the removal of COD is higher by EC
than the EO process.
Ti/Pt COD, NH3–N 40 EO 39.6 & 52.8 of COD, at 120 and 360 min, respectively
34.5 & 74.2 of
NH3–N
Ti/RuO2 COD, NH3–N 40 EO 12.6 &41.7 of COD, at 120, and 360 min, respectively
34.5 & 83.9 of
NH3–N
Al COD, phenol 5–30 EC 15–47.6 & at current density 2.5–30 mA/cm2, EC as a pretreatment Isik et al. (2020)
28.9–67.9 before fungal treatment
Fe COD, phenol 5–30 EC at current density 2.5–30 mA/cm2
(continued on next page)

8
Y.G. Asfaha et al. Cleaner Engineering and Technology 4 (2021) 100261

Table 4 (continued )
Anode Pollutant Current Techno-logy Removal efficiency Comment Ref.
density (%)
(mA/cm2)

10.3–36.2 &
22.1–39.4
SS COD, phenol 5–30 EC 14.0–48.9 & at current density 2.5–30 mA/cm2
28.1–58.9
BDD COD, phenol 5–30 EO 54.3–69.9 & at current density 2.5–30 mA/cm2, EC as a pretreatment
27.8–60.0 before fungal treatment
COD, phenol EO-fungal 90.1, 88.7 The EO-assisted fungal treatment process
treatment
Al Color, COD EC 92, 88 at pH 6.9 and 10 V Demir Delil and
Fe Color, COD EC 93, 89 at pH 3 and 6 V Gören (2019a)
Pt Color, COD EO 93 of COD at 6 V
Al & Graphite turbidity, color, COD EC-EOx 99, 100, 90 Özyurt et al.
(2017)
Al COD, color 6–24 EC 19.6–53, 87.52 less performed for COD removal Chakchouk et al.
platinized Turbidity, color, 18 EO 91.61, 59.46, & 42 after 60 min (2017)
titanium COD
COD EC-EO 63.8
PbO2 COD, color 42 EO 98.3, 99.1 The removal of both COD and color is higher than the Ghasem et al.
separate process. (2017)
Al COD, color 17 EC 82.2, 68.3
COD, color 17/42 EC/EO 99.9, 99.9

4.1. Process parameters of the hybrid process of EC and EO
Researches have shown that initial pH has a significant influence on
the efficiency of the EC and EO or hybrid of both processes. Ghazouani
et al. (2019b) studied a comparative performance of EC and anodic
oxidation for diazo dye degradation. The authors reported that the
removal efficiency was favored in the acidic pH of the anodic oxidation
process for color and COD removal. Therefore, the initial pH plays a
remarkable role in the formation of electro-generated active chlorine
which is the most oxidizing species. Furthermore, Ghasem et al. (2017)
studied the removal of COD, TSS, oil, and grease from poultry slaugh­
terhouse effluent by EC using aluminum and iron electrodes. Conse­
quently, the highest COD removal was achieved in an acidic condition
and decreased with an increase in pH. At pH 2, the maximum COD
removal was 93 and 85% for aluminum (Al) and iron (Fe) electrodes,
respectively. Moreover, compared to the Al electrode, the Fe electrode
was not affected by the initial pH between 2 and 8. Similarly, Can (2014)
demonstrated the effect of initial pH (within the range of 4–12) by
keeping the other factors constant (200 A/m2 of current density and 60
min operating time) on COD removal from fruit juice production efflu­
ents with EO, which showed a serious effect on the process efficiency.
Accordingly, the minimum removal efficiency was observed at pH 4 and
between pH of 8–10. However, the maximum removal of COD (52%)
was achieved at a pH of 6.
Likewise, Can (2014) in their other study investigated the effect of
supporting electrolyte concentration with NaCl in the range of
500–4000 mg/L on COD removal. The results showed that the highest
COD removal efficiency (52%) was reached by adding a 500 mg/L
concentration of NaCl. Due to adding supporting electrolyte, the con­
centration of chloride in the aqueous solution was increased, and the cell
voltage was decreased from 12.5 to 7.8 V. As a result, energy con­
sumption was decreased.
Furthermore, Linares-Hernández et al. (2010b) also investigated and
compared the effects of operating time on the COD reduction by the
hybrid of EC and EO processes. Accordingly, 90 min of operating time
was taken to completely remove COD, which is less than 10% of the time
needed by EO alone. On the other hand, Aquino et al. (2014) demon­
strated electrochemical degradation of real textile effluent by EO. The
authors reported that 100% of color and 86% of COD could be removed
at 180 min. Additionally, Chakchouk et al. (2017) compared the impact
of operating parameters on color, turbidity, and COD reduction by
electrocoagulation, electrooxidation, and the hybrid of both methods.
Finally, 100% of turbidity, 90% of color, and 66.4% of COD removal
were achieved by the hybrid processes (Table 2). Similarly, the influence
of applied current intensity on color, turbidity, and COD removal has
been investigated. The results indicated that increasing current density
led to the decrease of color, turbidity, and COD (Chakchouk et al.,
2017).
4.2. Reactor design of the hybrid process of EC and EO
Reactor/cell design is one of the important parameters of electro­
chemical technology that could govern the effectiveness of the pro­
cesses. The design effect on the performance of the hybrid of EC and EO
processes is the accumulation result of EC and EO design separately.
Therefore, during the cell design, it is quite important to take the types/
geometry of the electrodes (two and three-dimensional electrodes), size
of the electrodes, the surface area of the electrodes, reactor configura­
tion, electrode arrangements, operating conditions, flow rate, electrode
material, etc into consideration. For example, reactor configuration is
important to keep and allow the maximum mass transfer during the
electrolysis period. Besides, bipolar and monopolar electrode arrange­
ments in series or parallel connections are most commonly used in
hybrid processes of EC and EO. Furthermore, the reactor design for EC
has been discussed well by Mollah et al. (2004) and can be used as a
good input for this issue.
4.3. Energy consumption of the hybrid process of EC and EO
Compared to the separate processes of EC and EO, research studies
(Nawarkar and Salkar, 2019) indicated that the hybrid of EC and EO
highly reduce energy consumption and increase the removal efficiency.
For example, Ghasem et al. (2017) reported that even though the con­
sumption of energy by EC is 12 times less than that of EO, the residual
COD in the effluents was 17 times higher than the EO process. Therefore,
to reduce the consumption of energy and enhance the efficiency of the
process, it is recommended to combine the two processes. Ilhan et al.
(2007) conducted a comparative performance study of EC and EO pro­
cesses in removing COD from leachate. In all their experiments, a con­
stant current density of 40 mA/cm2 was applied. Accordingly, EC was
able to remove the COD value by 49.8% at the end of 30 min using the Al
electrode. Similarly, EO was able to remove the COD value only by 39.6
and 52.8% at the end of 120 and 360 min, respectively using Ti/Pt-SS
electrodes. The overall experimental study showed that the energy

9
Y.G. Asfaha et al.
consumptions by EC were 3.09 kWh/kg of COD removed and 11.16
kWh/kg of NH3–N removed within 30 min of electrolysis time. Besides,
the consumptions of energy by EO were also 33.16 kWh/kg of COD
removed and 135.73 kWh/kg of NH3–N removed within 360 min of
electrolysis time. In the study, it has been observed that the operational
time and energy consumption of EO are higher than EC. The authors
concluded their study that the combination of EC and EO processes
greatly reduces the overall energy consumption.
4.4. Electrode consumption and sludge production of the hybrid process of
EC and EO
For this case, Daghrir et al. (2012) conducted a study on restaurant
wastewater treatment by EC and the hybrid process of EC-EO, consid­
ering the consumption of electrode and sludge production. Accordingly,
0.30 kg/m3 and 4.30 kg/m3 consumption of electrode and sludge pro­
duction was recorded, respectively by EC. Likewise, they also observed
that only 0.17 kg/m3 and 2.98 kg/m3 of electrode consumption and
sludge production, respectively. Furthermore, Ibarra-Taquez et al.
(2017b) studied the total operation cost of the sequential EC-EO for the
treatment of soluble coffee wastewater. For the cost determination, they
have considered the energy consumption for both electrocoagulation
(EEC) and electrooxidation (EEO), anode material consumption (AMC),
and amount of sludge production. The calculation of AMC was linearly
increased with EC operation time (tEC). As of Faraday’s Law, anode
material consumption was linearly proportional to the applied current
and the experimental results were fitted (Eqn. (24)) (Ibarra-Taquez
et al., 2017b).
( )
/ 2211–2217. https://doi.org/10.2166/wst.2010.130.
AMC kg m3 = 0.0138 × tEC (24)
Similarly, the amount of sludge production was large and increased
with the operational time of EC (tEC).
5. Conclusion
In general, it has been shown by various researchers that the elec­
trochemical method is an efficient technology for removing numerous
pollutants. Among the different electrochemical techniques, EC, EO, and
hybrid processes of EC and EO attracted the attention of most scholars.
In the electrochemical process, EC is comparatively very effective in
removing colloidal and suspended particles in a very short time. How­
ever, it is less effective in removing stable persistent organic compounds
like COD, TOC, and BOD5 to below the allowable discharge limits. EO
alone is effective in removing even the stable persistent organic com­
pounds but it requires a long operation time, which is practically diffi­
cult to implement when colloidal and suspended materials are present.
Therefore, it can be concluded that EO, as a separate method, is not
applicable for treating water and wastewater with large amounts of
suspended solids. In the hybrid process of EC and EO, EC quickly co­
agulates and removes the colloidal and suspended solids particles and
many charged species then EO oxidizes the remaining pollutants.
Therefore, the hybrid method can remove both the suspended and
colloidal as well as stable persistent organic compounds to the allowable
limit in a practical time. In this review, it was assessed that a hybrid of
EC-EO/or EC and EO has the potential of removing various pollutants
such as COD, TOC, NH4+-N, nitrates, phenol, virus mitigation/inacti­
vation, and also preventing membrane fouling. In those cases, EC or EO
alone showed less performance than the hybrid process. Moreover, from
the majority of the studies on hybrid processes, it has been proofed that
electrocoagulation as a pretreatment of electrooxidation is more effec­
tive to remove both colloidal particles and persistent organic com­
pounds than a separate operation.
10
Cleaner Engineering and Technology 4 (2021) 100261
Acknowledgements
The authors acknowledge all technical and financial support from
the Africa Center of Excellence for Water Management (ACEWM), Addis
Ababa University.
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