Separation and Purification Technology: Pranjal P. Das, Mukesh Sharma, Mihir K. Purkait

Separation and Purification Technology 292 (2022) 121058
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Separation and Purification Technology

journal homepage: www.elsevier.com/locate/seppur
Recent progress on electrocoagulation process for wastewater treatment:

A review
Pranjal P. Das a, Mukesh Sharma b, Mihir K. Purkait a, *
a
Department of Chemical Engineering, Indian Institute of Technology Guwahati, Assam, India
b
CORAL, Indian Institute of Technology Kharagpur, West Bengal, India
A R T I C L E I N F O A B S T R A C T
Keywords: Electrocoagulation (EC) is an established wastewater treatment method that has been widely explored for a
Electrocoagulation broad range of wastewater pollutants due to its ease of operation, versatility, eco-friendly nature and low
Hybrid process footprint. EC as a pretreatment process can significantly reduce the total energy usage, while also improving the
Operating variables
quality of treated water. This review paper provides an in-depth assessment of the various operational param
Wastewater treatment
eters and electrode materials used during the electrocoagulation treatment of wastewater. The recent ad
vancements in EC reactor designs and optimization studies have been reviewed. The effectiveness of combining
the EC process with other water treatment techniques viz. membranes, oxidation, chemical and adsorption
processes have also been validated in this review paper. Different combinations of EC process with micro
filtration (EC-MF), ultrafiltration (EC-UF), nanofiltration (EC-NF), reverse osmosis (EC-RO), ozonation (EC-O3),
peroxi-electrocoagulation (EC-H2O2) and electro-oxidation (EC-EO), have been elaborately discussed and sum
marized. The results are critically analyzed, and modifications have been suggested to improve the performance
efficiency. Moreover, case studies regarding the application of the EC process from three different wastewater
sources have been demonstrated. The economic aspects of the EC process and recommendation for its betterment
is also made. Taken together, this review paper effectively illustrates the progress and current achievements in
both standalone and hybrid EC process towards wastewater pollutant treatment, which can present new insights
on improving the wastewater treatment scenario with promising environmental applications. The critical anal
ysis and suggestions provided in this review paper will greatly enhance the scientific knowledge of the readers.
1. Introduction Secondary treatment includes biological processes viz. biological filter

process and activated sludge process to degrade the complex organic
One of the most important challenge of the 21st century is the molecules into non-toxic compounds. Tertiary treatment consists of
problem of water scarcity. Around 2 billion people in the world lacks chlorination, ultraviolet disinfection and membrane bioreactors for
convenient access to safe drinking water and an average of 7.8 million extensive water purification [2]. The schematic outline of a typical
people die every year due to poor water hygiene and sanitation. More wastewater treatment plant is shown in Fig. 1.
over, drought affects around 55 million people annually, which in turn In general, the water treatment process can be categorised into either
causes more than US$5 billion of economic loss. Since 1980, the annual degradation technique or separation technique. Separation technique
usage of water has increased by 1%, and this trend is expected to transfers the contaminants in water from one phase to another, most
continue until 2050 [1]. The demand for reusable waster is echoed from commonly into the solid phase. The finest illustration of this phenom
various sectors including industrial, agricultural and residential sectors. enon is the adsorption process. However, separation technique like
As such, treatment of wastewater might be a solution to the problem of membrane separation concentrate the contaminants in water phase,
water shortage. Primary treatment, secondary treatment, and tertiary thereby requiring additional treatment. Simultaneously, degradation
treatment are the three main phases of conventional wastewater treat technique (used for the removal of organic contaminants) often leads to
ment process. Primary treatment consists of bar screen and sedimenta the breakdown of contaminants until its complete mineralization is
tion basin to eliminate the suspended solids present in wastewater. achieved [3]. Conventional wastewater treatment includes both
* Corresponding author.
E-mail address: mihir@iitg.ac.in (M.K. Purkait).
https://doi.org/10.1016/j.seppur.2022.121058
Received 11 March 2022; Received in revised form 1 April 2022; Accepted 9 April 2022
Available online 15 April 2022
1383-5866/© 2022 Elsevier B.V. All rights reserved.
P.P. Das et al. Separation and Purification Technology 292 (2022) 121058
biological [4,5] and physico-chemical processes [6,7], as well as [16]. Thus, the EC process has the capacity to remove several types of
emerging techniques such as adsorption [8] and membrane filtration contaminants from both water and wastewater such as total suspended
[9]. Biological processes require strictly regulated conditions, extended solids, total organic carbon, oil emulsions, heavy metals, chemical ox
retention time, larger footprint and generation of undesirable byprod ygen demand, colour and turbidity. The use of EC process for waste
ucts. Chemical processes require substantial addition of chemicals, water treatment along with its benefits have been thoroughly examined
which not only increases the expense of the overall process but also in numerous studies [17–19]. However, sludge disposal from the treated
complicates the downstream operations, with subsequent threat of solution is a major issue in the EC process, which requires an additional
secondary contamination. Also, adsorption and membrane filtration post-treatment process. As such, significant research should be con
alone are ineffective in treating high contaminated wastewater, unless ducted on the integration of electrocoagulation with other existing
they are combined with comprehensive pre-treatment processes. wastewater treatment processes to further improve the performance
Adsorption process significantly depends upon the solution pH and re efficiency of the EC technique as well as to tackle the challenges related
quires a longer treatment period; adsorbents eventually lose its potential to environmental applications. To the best of our knowledge, it is
as the number of cycles increases [10]. Also, adsorbent regeneration envisaged that there is no reported work on the comprehensive compi
necessitates the use of steam or vacuum. Moreover, membrane filtration lation of both standalone and hybrid electrocoagulation systems, along
becomes inefficient overtime, owing to the pore blockage by contami with its varied advances and applications in water and wastewater
nants and subsequent flux loss [11]. Thus, current studies on wastewater treatment.
treatment are considerably focused towards electrochemical processes In this context, the goal is to hybridize the electrocoagulation process
[12]. so that it may be successfully applied for various purposes viz. sustain
Electrocoagulation (EC) process has been reported to be an efficient able water desalination, water and wastewater treatment and water
approach for treating both water and wastewater because it is flexible, reuse by utilising its intrinsic properties to remove both organic and
easy to use, and can handle a variety of contaminants [13]. Due to high inorganic contaminants. During the last decade, hybrid electro
removal rate and zero added chemicals, electrocoagulation is considered coagulation processes have received increased research interest. To
as a viable alternative to chemical coagulation for the treatment of high minimise the consumption of energy and improve the removal effi
contaminated wastewater. As no chemical coagulant is added, electro ciency, the hybridization of electrocoagulation process with other
coagulation does not pose any risk of secondary contaminant generation treatment techniques must be carefully chosen. This review paper
unlike chemical coagulation. Also, formation of gas bubbles during the evaluates the performance of combining electrocoagulation with
EC process assist in the floatation of contaminants on the water surface different treatment techniques viz. microfiltration (EC-MF), ultrafiltra
[14,15]. Moreover, the particle size of flocs produced in electro tion (EC-UF), nanofiltration (EC-NF), reverse osmosis (EC-RO), ozona
coagulation are stable and large and can be easily separated via tion (EC-O3), peroxi-electrocoagulation (EC-H2O2) and electro-
decantation or simple filtration. The flocs contain less water (acid oxidation (EC-EO). These hybrid techniques are extensively discussed
resistant compound), thereby making it easier to remove via filtration. and summarized in the present review paper, with a particular focus on
Since most of the flocs are stirred during electrocoagulation, therefore, wastewater treatment and energy usage, along with various challenges
less volume of sludge is produced as compared to chemical coagulation. and future recommendations. This paper also examines the current ad
This suggests that, electrocoagulation is very efficient in the removal of vances in the evolution of electrocoagulation reactor designs and the
tiniest colloidal particles due to the application of an electric field, process optimization, along with an overview of critical electro
responsible for assisting in coagulation and flotation of contaminants coagulation principles required to comprehend its mechanism and the
Fig. 1. Flowchart of the conventional wastewater treatment plant.
2
effect of operational variables on the removal efficiency of the EC pro to its periodic replacement and reduction in process efficiency due to the
cess. Furthermore, the cost estimation study was evaluated to get a clear occurrence of electrode passivation. Also, the generated floc in the
view of the economic feasibility of the EC process in water and waste treated sample contains high concentration of metal ions which cannot
water treatment. The authors believe that this review article might be be directly discharge into the environment, thereby requiring an addi
helpful to the readers in obtaining a critical understanding of both tional post-treatment method in order to satisfy the environmental
standalone and hybrid electrocoagulation processes, together with the legislations. It is suggested that the combination of EC process with
prevailing drawbacks and possible solutions associated with it. other water treatment techniques can overcome such limitations.
Therefore, the use of electrocoagulation as a pre-treatment process could
2. Overview of electrocoagulation (EC) process promote environmental and economic sustainability for the effective
removal of various wastewater contaminants.
Electrocoagulation is a water treatment technique that has received
significant attention in the field of pollutant degradation from different 3. Mechanism and removal kinetics of electrocoagulation
wastewaters (industrial and domestic). It is a comparatively low-cost
technique that breaks the stable emulsion and suspension in a solution The electrocoagulation process is widely used to destabilize the
using salt polymers or polyelectrolytes. The reduction of cathodic im pollutants present in the form of dissolved or suspended particles in the
purities in water with subsequent electro-flotation, is one of the crucial electrolytic solution through the application of electric current. The
reaction that occurs during electrocoagulation. The hydrogen or oxygen electrocoagulation set up comprises of an electrolytic cell and a series of
bubbles generated by the electrodes assist in lifting the coagulated sacrificial metal electrodes (usually Fe or Al) coupled to a controlled DC
particles via electro-flotation [20]. Fig. 2 represents the schematic power source. The cathodes and anodes used during the process can be
layout of an electrocoagulation reactor. The main operational parame made either from the same or different materials [27]. There are seven
ters which influences the electrocoagulation process are inter-electrode important steps in electrocoagulation mechanism viz. (i) formation of
distance, solution pH, type of electrodes, applied current density and metal cations due to the supply of electric current to the anodes; (ii)
electrode configuration. As a result, in every electrocoagulation study, production of hydroxyl ions due to cathode hydrolysis; (iii) interaction
these operational parameters must be optimised [21]. The electrolysis of metal cations with hydroxyl ions to form metal hydroxides; (iv)
effect is responsible for chemical and physiochemical phenomenon in oxidation of toxic contaminants into harmless intermediate products; (v)
electrocoagulation. This indicates that electricity is required for the charge neutralization of contaminants due to its reaction with the metal
production of coagulants via anodic dissolution, destabilization of par hydroxides; (vi) adsorption of charge neutralized contaminants on metal
ticulate and pollutant suspension as well as floc formation by aggrega hydroxides, followed by its removal via sweep coagulation and (vii) gas
tion of the destabilised phase [22]. Electrocoagulation process is based formation (H2 gas) at the cathode lifts the generated flocs to the solution
on the phenomenon of electrochemistry, in which oxidation or loss of surface via sweep flotation [28,29]. Thus, the degradation of contami
electron takes place at the cathode whereas reduction or gain of electron nants in EC process is primarily attributed to three phenomena viz.
occurs at the anodic surface [12,23]. As in-situ coagulants are produced adsorption, coagulation, and floatation. The pollutant removal mecha
during the treatment, electrocoagulation process does not necessitate nism via electrocoagulation process is shown in Fig. 3. In-situ coagulants
the use of added chemicals [24–26]. are generated in the electrocoagulation chamber due to anodic disso
Though the EC process has been extensively used for water and lution (Eq. (1)), along with the formation of H2 gas at the cathode (Eq.
wastewater treatment, however, there are few limitations associated (2)) and hydroxyl ions at the anode (Eq. (3)). These electrogenerated
with the process such as rapid consumption of sacrificial anodes, leading coagulants are accountable for the formation of floc encircled by metal
Fig. 2. Schematic diagram of the electrocoagulation process.
3
Fig. 3. Mechanism of pollutant degradation by electrocoagulation process.
hydroxides, which functions as an efficient adsorbent [30]. the process efficiency was observed at higher initial phosphate con
centration. The study inferred that, the kinetic behaviour for phosphate
At anode : M(s) → M3+ + ne −
(1)
aq removal was best described by first order reaction kinetics, with average
activation energy of 5 kCal/min and diffusion being the main reaction
H2 O → 4H+
aq + O2 (g) + 4e
−
(2) driving force.
The kinetic study effectively indicates the mechanism of chemical
n
At cathode : nH2 O + ne− → H2 (g) nOH−aq (3) processes, creates time-dependent prediction regarding the composition
2
of reaction mixtures as well as identifies the rate control phenomenon.
In the last two decades, much investigation has been conducted on However, it is not possible to analyse how the pollutant adsorption on Al
the kinetics of pollutant removal by electrocoagulation process. Singh (OH)3 surface promotes its degradation from the wastewater via kinetic
and Mishra, 2017 determined the kinetic properties of batch electro models. Also, model validation based on a limited set of data may create
coagulation process for the removal of heavy metals and suspended uncertainty between soluble and solid Al(OH)3 coagulants. It is sug
solids from synthetic wastewater [31]. The study reported a removal gested that few crucial factors such as heat and mass transfer limitations
efficiency of 76.5% for total suspended solids (TSS), whereas for heavy (due to rapid occurrence of reactions), surface coverage, gas flotation
metals viz. copper, zinc and chromium, the removal efficiencies were rate and oxidation state of the electrodes needs to be considered while
found to be 99%, 82% and 60% respectively, after a treatment time of applying the reaction kinetic models during the EC process.
30 min and applied current density of 5.3 mA/cm2. Moreover, the first
and second order kinetic models were found to be best suited for the 4. Electrode materials for electrocoagulation
removal of pollutants, which depends upon the treatment time and flow
density. Similarly, Ahmadian et al., 2012 studied the kinetic behaviour 4.1. Aluminium and iron electrode
of batch EC process (using eight electrodes) for the treatment of
slaughterhouse wastewater [32]. It was found that an applied current Aluminium (Al) is commonly employed as an electrode material
density of 25 A/m2 and a treatment time of 50 min resulted in a removal during the EC process. Application of current density leads to the for
efficiency of 93%, 97%, 84% and 81% for COD, BOD, total nitrogen and mation of aluminium cations (Al3+) via dissolution of sacrificial anodes
total suspended solids respectively. Also, the kinetic study showed that [34]. The anodic and cathodic reaction using aluminium electrodes are
the pollutant removal efficiency during the treatment followed the first shown in Eqs. (4)–(6). The metal concentration in the solution increases
order reaction kinetic model. On the other hand, El-Shazly and Daous, due to electro-dissolution and eventually precipitates at the bottom of
2013 used the continuous EC process to evaluate the kinetics of phos EC chamber as metal hydroxides. Al3+ ions undergo a complex equi
phate removal from industrial wastewater [33]. In this study, the in librium with various monomeric and polymeric species viz. Al(OH)3, Al
fluence of different operational parameters on phosphate removal rates (OH)2+, Al (OH)−4 , Al (OH)+ 3+ 4+ 4+
2 , Al6 (OH)15 , Al7 (OH)17 , Al8 (OH)20 , Al13
was carefully examined. It was reported that the phosphate depletion
(OH)5+ 7+
34 and Al13O4 (OH)24 depending upon the solution pH. However,
rate increases with increasing current density, solution temperature and
Al(OH)3 produced via complex precipitation mechanisms is primarily
circulation flow rate, whereas the rate of phosphate depletion decreases
responsible for the formation of flocculates and aggregates [35,12].
with increasing phosphate concentration in the solution. A reduction in
4
At anode surface: Al → Al3+ (aq) + 3e− (4) consist of higher charge valency as compared to Mg and Zn ions, thereby
allowing for an improved coagulation process with low coagulant con
3 centrations. On the other hand, the assessment of other electrochemi
At cathode surface : 3H2 O + 3e− → H2 (g) + OH− (5) cally produced coagulants is based on the coagulant residual
2
concentrations present in the treated water. For example, the United
Overall: Al3+ (aq) + 3H2O → Al(OH)3 + 3H+ (6) States Environmental Protection Agency (USEPA) recommends the
limiting Al concentration to 0.2 mg/L, whereas the limit for Mg is set at
Similarly, utilization of applied potential across the iron (Fe) elec
30 mg/L, to avoid any health related issues [42,15].
trodes leads to the production of in-situ coagulants via electro-
dissolution of sacrificial electrodes. Hydroxyl ions are generated at the Mg → Mg2+ + 2e− (13)
anode vicinity via reduction, whereas H2 bubbles are produced at the
cathode vicinity via oxidation, which assist in driving the generated floc Zn → Zn2+ + 2e− (14)
to the water surface. The anodic and cathodic reaction using Fe elec Mg2+ + 2H2O → Mg(OH)2 (s) + 2H+ (15)
trodes are shown in Eqs. (7)–(9) [36]. At low solution pH and oxygen
ated water, ferrous ions are easily transformed into ferric ions. Zn2+
+ 2H2O → Zn(OH)2(s) + 2H +
(16)
Depending upon the pH, the electrogenerated ferric ions undergoes
Al and Fe electrodes are widely preferred among all the other elec
hydrolysis reaction to form different monomeric and polymeric species
trodes in EC process due to their high pollutant removal efficiency, cost-
in the solution viz. Fe(OH)3, Fe(H2O)5OH2+, Fe (H2 O)3+
6 , Fe(H2O)4 effectiveness and easy availability. The high performance of Al and Fe
4− 2+ 4+
(OH)+2 , Fe(OH) , Fe2(H2O)6 (OH)4 and Fe2(H2O)8 (OH)2 . These Fe electrodes is associated with the reduction in the electrical double layer
complexes have a very strong tendency to polymerize at a pH range of by higher charge valency of Al3+ and Fe3+ ions as compared to copper,
3–7. Moreover, the primary complex formed viz. Fe(OH)3 remains in the zinc and magnesium, thereby assisting even more in the coagulation-
aqueous solution as gelatinous suspension, thereby assisting in the flocculation process. Although the use of Fe electrodes can minimize
removal of wastewater contaminants by either electrostatic attraction or the cost of the EC process as compared to Al electrodes, however, it may
complexation phenomenon with subsequent coagulation [37,15]. develop a reddish-brown tinge to the treated EC samples, which in turn
produces a turbid solution. On the other hand, Al electrode constitutes
At anode surface : Fe(s)→ Fe3+
aq + ne
−
(7)
high strength to weight ratio, corrosion resistant property and high
electrical conductivity. Also, it does not impart any colour to the treated
At cathode surface: 2e- + 2H2O → H2 + 2OH+ (8)
solution and can easily outperform Fe electrode in terms of removal
Overall: 4 + 10H2O + O2(aq) → 4Fe(OH)3(s) + 8H+ (9) efficiency depending upon the wastewater. As such, the selection of
appropriate electrode material based on the targeted pollutants and
cost-benefit analysis is very important. Besides, both Al and Fe elec
trodes undergo electrode passivation, which greatly reduces the overall
4.2. Other miscellaneous electrodes performance of the EC process. Therefore, it is suggested that future
studies should focus on inducting self-cleaning techniques of electrodes
In addition to Al and Fe electrodes, utilization of copper (Cu) as an to overcome the phenomenon of electrode passivation.
electrode material also assist in the removal of various wastewater
pollutants during electrocoagulation. A comparative analysis carried out 5. Operational parameters affecting the removal efficiency
between Al and Cu electrodes reported that, Cu electrodes provide during EC
higher removal efficiency against Al electrodes and uniform corrosion
was observed at the surface of Cu electrodes after the treatment. During 5.1. Current density
the utilization of Cu electrodes in electrocoagulation process, typical H2
formation takes place at the cathode vicinity, while copper cations The operational variables affecting the electrocoagulation mecha
(Cu2+) ions were simultaneously released at the anode. Eqs. (10)–(12) nism and its subsequent process efficiency is shown in Fig. 4. Current
represent the reactions that occur during electrocoagulation process density or current applied per effective electrode surface area is
using Cu electrodes, at which Cu2+ ions and Cu(OH)2 are generated in considered a very significant parameter determining the electro
situ to act as a coagulant in the removal of wastewater contaminants coagulation performance. During the application of EC process, current
[38]. Hydrolysis of Cu2+ and Cu3+ ions lead to the formation of both density regulates the rate of electron release, occurring as a result of
monomeric and polymeric species viz. CuOH2+, Cu (OH)+ metal ion dissociation from the electrodes. The range of applied current
2 , Cu (OH)4 ,
−
2+ density may differ depending upon the types of effluent. This variation
Cu2 (OH)4+ 2 , Cu (H2 O)2 , Cu(H2O)4 (OH)2 and Cu(H2O)5OH . The
+ +
in current density is mostly due to the changes in ionic interaction,
colloidal particles (net negative charge) are adsorbed onto the surface of
caused by the type of contaminants present in the effluent [37,16]. In
Cu(OH)2, which get neutralized and subsequently precipitates due to its
most cases, the applied current density in EC process may typically vary
heavy mass [39,40].
from 0.01 to 880 A m− 2 [43,44]. Despite the fact that, the applied
At anode surface: 2Cu → 2Cu2+ + 4e− (10) current density closely corresponds to the release and dissociation of
metal ions in solution, however, a surplus of current may considerably
−
At cathode surface: 4H2O + 4e → 2H2 + 4OH −
(11) reduce the performance of EC process by allowing in-situ secondary
+
Overall: 2Cu + 4H → 2Cu 2+
+ 2H2 (12) reactions along with the formation of colloidal charge reversal due to
overdosing of coagulants. Such phenomenon has the potential to shorten
Moreover, several studies have also suggested the use of alternate the electrode life span, while lowering the process efficiency. Thus,
anodic materials viz. magnesium (Mg) and zinc (Zn) during electro current density is a crucial parameter in EC process that must be opti
coagulation. The principle is similar as stated formerly for Al, Fe and Cu mized to achieve the desirable treatment performance [12]. Several
electrodes, which consist of anodic dissolution (Eqs. (13) and (14) for studies have investigated the influence of applied current density in
Mg and Zn respectively) followed by coagulation and precipitation. different pollutant containing wastewaters [45–47]. A study conducted
Depending upon the solution pH, the generated ions (Mg2+ and Zn2+) by Rahman et al., 2020 reported that, an applied current density of 25
further lead to the formation of its corresponding hydroxides viz. Mg A/m2 is sufficient in achieving a reduction efficiency of 98.5% COD,
(OH)2 and Zn(OH)2 as shown in Eqs. (15) and (16) [41]. Al and Fe ions
5
investigated the effect of current density on the removal of high COD

content (29,000 mg/L) from poultry slaughterhouse wastewater [51].
As the current density was increased from 20-150 A/m2, the maximum
oil and COD removal efficiencies of 98% and 94% were reported within
25 min via Al and Fe electrodes, respectively. Similarly, Eryuruk et al.,
2018 carried out an electrocoagulation treatment of poultry slaughter
house effluent contaminated with high COD concentration (9000 mg/L)
[52]. The study evaluated the process performance as a function of
current density variation (30–50 mA/cm2). At an optimum current
density of 50 mA/cm2, the highest COD removal efficiency of 96% was
observed within 40 min of treatment time. It was concluded that the EC
process could effectively treat high COD contaminated wastewaters via
optimization of the current density.
It is well established that an increase in the current density results in
higher pollutant removal efficiency. However, the formation of in-situ
secondary reactions and colloidal charge reversal may be seen due to
the supply of excess current density. This may cause faster electrode
depletion and formation of a thin film layer on the electrode surface,
which considerably lowers the process efficiency. Thus, the current
density should be suitably optimized based on the targeted effluents.
Also, the use of larger electrode surface area at lower or optimized
current density can overcome the aforementioned challenges.
5.2. Inter-electrode distance
In EC process, the inter-electrode distance is considered to be a very

crucial parameter, as it governs the electrostatic field between the
cathodes and anodes. A decrease in the inter-electrode distance even
tually increases the electrostatic field. Thus, the metal hydroxides which
assist in the formation of flocs to promote coagulation deteriorates due
to the intense collisions caused by the high electrostatic attraction.
Consequently, at a shorter inter-electrode distance, the efficiency of the
EC process significantly increases [19]. Besides, larger inter-electrode
distance delays the subsequent production of metal hydroxide based
flocs due to low electrostatic forces. Excessive electrode distance also
lowers the process efficiency, thereby resulting in high power con
sumption to compensate for the slower release of metal ions between the
Fig. 4. Parameters affecting the mechanism of electrocoagulation process. cathodes and anodes. As such, it is very important to operate the EC
process at an optimal inter-electrode distance [53]. Several studies have
98% turbidity, 92% TOC and 100% decolorization from peat water [34]. predicted the optimum range of inter-electrode distance to be 0.5–1 cm
However, a substantial decrease in the pollutant reduction efficiency for different wastewaters [54,39,55]. Rahman et al., 2020 reported that,
was observed at lower current density of 5.99 A/m2. The reason may be a shorter inter-electrode distance of 0.5 cm significantly assists in
due to the formation of high Al(OH)3 content at an increased current improving the efficiency of the EC process [36]. The study showed a
density of 25 A/m2, thereby improving the coagulation and flocculation removal efficiency of 93.7% turbidity, 85.5% color and 26% of TOC
process. Higher current density is also beneficial as it reduces the bubble from peat water via utilization of galvanized Fe electrodes. In another
size, which eventually assist in the faster removal of pollutants via study, Rahman et al., 2020 showed that Al electrodes also require a
hydrogen floatation. Similarly, Bener et al., 2019 also examined the lower inter-electrode distance for improving the process performance
effect of varying current density on the TOC reduction efficiency from [34]. The high removal efficiency of 93.3% turbidity, 88.2% TOC,
real textile wastewater [48]. It was found that, the maximum TOC 89.9% COD, and complete decolorization was observed for Al electrodes
reduction was obtained at an applied current density of 100 mA/cm2. In with 1 cm inter-electrode spacing. Thus, both studies concluded that a
contrast, a lower current density of 12.5 mA/cm2 corresponds to a sig lower inter-electrode distance of 0.5–1 cm was best suited for achieving
nificant decrease in the reduction efficiency. The study concluded that, the maximum pollutant removal efficiency. On the other hand, at higher
an increase in current density from 12.5 to 100 mA/cm2 resulted in an inter-electrode spacing, the interaction between the hydroxides and
improved TOC reduction efficiency from 10% to 22.5% after 2 h of pollutants decreases due to poor mass transfer rate from the electrode
treatment time. Furthermore, Mousazadeh et al., 2021 reviewed the surface to the bulk solution, resulting in lower pollutant removal effi
effect of operating parameters on the EC removal efficiency of high COD ciency. Both Akarsu et al., 2016 [56] and Aswathy et al., 2016 [57]
contaminated wastewater [49]. It was shown that higher values of investigated the effect of inter-electrode distance during the treatment
current density are anticipated to improve the COD removal efficiency. of bilge wastewater. Akarsu et al., 2016 observed a COD removal effi
An increase in applied current density on the electrode surface leads to a ciency of 52% within 90 min of treatment time as compared to 89.9%
higher coagulant generation rate and increased formation of bubbles, removal in 120 min by Aswathy et al., 2016. The treatment time and
resulting in destabilization of the contaminant molecule. For instance, inter-electrode distance were reported to be the major determining
an increase in current intensity from 1 to 25A considerably improved the factors for both the studies. The huge difference in the removal effi
EC removal efficiency of high COD contaminated (25,000 mg/L) palm ciency is mainly due to the variation in inter-electrode distance. Aswa
oil mill effluent (POME). At an optimum current intensity of 25 A, the EC thy et al., 2016 utilized an inter-electrode spacing of 1 cm, whereas
process significantly removed 96% COD, 94% BOD, and 95% SS within Akarsu et al., 2016 employed a spacing of 8 cm between the electrodes.
50 min of treatment time [50]. In another study, Bayramoglu et al., 2006 Although the removal of high COD content (>1000 mg/L) from different
6
effluents was found to be satisfactory, however, the release of COD-rich cathode vicinity. In another study, Irdemez et al., 2006 examined the
wastewater (>10,000 mg/L) can pose a significant challenge during its effect of varying pH on phosphate removal from synthetic wastewater
treatment. Mousazadeh et al., 2021 studied the treatment of COD-rich via Fe electrodes [64]. It was reported that, a considerable reduction in
wastewater using the EC process [58]. It has been shown that lower the energy consumption of EC process was observed at a lower pH of
inter-electrode spacing significantly improves the process efficiency. 3–4. Also, the optimum pH value for highest phosphate removal effi
However, ohmic loss in relation to the cathode and the anode over ciency (93%) was found to be in the range of 6–7, as the solubility of Fe
voltage increases at higher inter-electrode spacing, resulting in slow (OH)2 is lowest within this range. On the other hand, Demirbas and
formation of coagulants. For instance, Maha Lakshmi and Siva Kobya, 2017 investigated the use of both Fe-Fe and Al-Al electrodes at
shanmugam, (2013) evaluated the effect of inter-electrode spacing on varied pH conditions in metalworking fluid wastewater [47]. It was
the removal of high COD content (25,000 mg/L) from oil tanning found that, Fe electrode provides best result at pH 7.5, while Al electrode
wastewater [59]. The removal efficiency of COD was improved when the performs better at pH 6.5. The study concluded that, the variation in
inter-electrode spacing was maintained between 10 and 15 mm. The solution pH had a very significant effect on the optimum performance
study concluded that an inter-electrode spacing of 15 mm was optimal efficiency of both the electrodes when tested for the same wastewater.
for achieving the highest COD removal efficiency of >90% within 15 The solution pH greatly controls the release and formation of co
min. In another study, Prajapati et al., 2016 investigated the removal of agulants during the EC process. The evolution of H2 at the cathode vi
colour and COD from rice grain-based distillery wastewater [40]. The cinity and the formation of OH− ions considerably increases the solution
initial COD content of the wastewater was found to be 11,500 mg/L. It pH. However, inappropriate pH conditions may alter the double layer,
was reported that the maximum COD and colour removal efficiency of which in turn may decrease the coagulant formation. Also, the mono
90% and 86%, respectively, were achieved at an optimum inter- meric and polymeric species formed at highly alkaline condition shows
electrode distance of 10 mm and a current density of 178.5 A/m2. As very low adsorption capacity. As such, the variation in pH should be
such, it can be inferred that, the inter-electrode distance plays a very effectively maintained to improve the pollutant adsorption capacity of
important role in improving the overall pollutant removal efficiency of the coagulant species throughout the EC process.
the EC process.
The variation of inter-electrode distance plays a major role in 5.4. Electrode configuration
determining the performance of the EC process. However, an increase in
the electrode spacing leads to higher resistance to mass transfer and slow The electrode configuration mode not only affects the pollutant
charge transfer. Also, the formation of metal hydroxide based coagulants removal efficiency but also the operational cost and energy consumption
slows down due to low electrostatic forces. Thus, it may require high of the EC process. The most commonly used electrode arrangements are
power consumption to overcome the slower release of coagulants, bipolar electrodes in serial connection (BP-S) and monopolar electrodes
thereby increasing the overall cost of operation. Therefore, smaller in serial (MP-S) and parallel connection (MP-P) [65]. The arrangement
inter-electrode spacing can be preferred to significantly improve the of various electrode connection modes in an EC reactor is shown in
process efficiency and optimize the economic aspects of the EC process. Fig. 5. Depending on the electrical polarity, each electrode in a
monopolar configuration mode functions as either cathode or anode in
the electrochemical cell. In case of MP-P connection, the sacrificial an
5.3. Solution pH odes are interlinked directly with one another in the EC cell; besides the
cathodes are also connected in a similar configuration. Meanwhile, in
The solution pH plays a very significant role in determining the MP-S connection, each set of electrode (anode-cathode) is connected
performance of EC process. The effect of pH is directly associated with internally; however, they are not linked to the outer electrodes. How
the formation of coagulants in solution, which exhibits several species in ever, in BP-S connection, the electrodes which are monopolar (except
equilibrium viz. metal ionic complexes and monomeric/polymeric the outer electrodes) exhibit different polarity at each of the electrode
hydroxide-complexes. The variety and quantity of such complexes are vicinity, based on the charges of previous electrodes. The bipolar elec
important since they all exhibit different interactions with wastewater trodes are always connected in series configuration. It is worth noting
contaminants, thereby providing different coagulant performances. For that, series connection necessitates the use of higher potential differ
instance, the species formed at highly alkaline conditions for Fe and Al ence, while the same current is spread across all electrodes [66,67,39].
electrodes viz. Fe (OH)−4 and Al (OH)−4 respectively performs very poorly Besides, the electric current in parallel connection is distributed among
with regards to adsorption efficiency [60]. On the other hand, Fe (OH)−3 all the electrode interconnection as a function of its resistance. Never
and Al (OH)−3 formed under neutral and slightly alkaline/acidic condi theless, parallel connection mode provides significant benefits in terms
tions significantly enhance the adsorption capacity of the coagulants. of energy consumption [65,15]. Also, the BP-S connection mode aids in
Thus, the solution pH has a considerably influence on the physi high pollutant removal, whereas use of MP-P connection provides low
ochemical characteristics of coagulants viz. (i) particle size of coagulant cost of operation [68]. In a study conducted by Ghosh et al., 2008, the
species and (ii) solubility and electrical conductivity of metal hydroxides performance of both bipolar and monopolar electrode configuration was
[61,62]. Moreover, the net charges and electrostatic interactions of the investigated for the removal of fluoride from drinking water [24]. It was
pollutants are directly influenced by the protonation/deprotonation reported that, high fluoride removal efficiency (85%) and less treatment
(based on pKa values) of its functional groups. As such, the double layer time (45 min) were observed for bipolar connection mode as compared
gets altered which in turn affects the coagulant formation. Therefore, the to monopolar connection. On the other hand, electrode corrosion and
solution pH needs to be optimized according to different physico- sludge formation were found to be higher for bipolar connection, which
chemical nature of the targeted pollutants and the effluent characteris in turn increases the operational cost of the process. It was inferred that
tics [63]. Bener et al., 2019 investigated the effect of three different pH monopolar connection mode is more cost-effective, while bipolar
conditions (5, 8 and 10) on TOC removal efficiency from real textile connection provides better pollutant removal efficiency. Kobya et al.,
wastewater via Al electrodes [48]. The maximum TOC removal (65%) 2007 used two different electrode materials (Al and Fe) in connection
was obtained at a solution pH of 5. It was further observed that the with MP-P, MP-S and BP-S configuration for the treatment of textile
removal efficiency decreases with an increase in the solution pH up to wastewater [65]. It was reported that Fe electrode with MP-P connection
10. The reason behind the decrease in EC removal efficiency at pH 10 exhibits higher performance at low current density, while all the three
may be attributed to two factors: (a) the species formed at highly alka configurations performed equally well at high current density. However,
line conditions for Al electrodes viz. Al (OH)−4 performs poorly with Fe electrode with BP-S, MP-P and MP-S connection requires longer
regards to adsorption efficiency; and (b) the generation of H2 gas at the treatment time to reach steady removal efficiency as compared to Al
7
Fig. 5. Different electrode configurations in an electrochemical cell. (a) monopolar-parallel connection, (b) monopolar-series connection and (c) bipolar-
series connection.
electrodes. The study concluded that Fe electrode connected in MP-S select and optimize the electrode configurations to minimize the energy
mode performs better at neutral pH, whereas Al electrode showed consumption and achieve the desired treatment performance.
higher efficiency with BP-S connection under acidic condition.
Amongst the electrode connection modes, two electrochemical cells 6. Advancement in electrocoagulation process
act together in a bipolar electrode configuration, resulting in a higher
surface area compared to monopolar configuration. This adequately 6.1. Reactor design and operational control
favours the anodic oxidation in bipolar mode which in turn improves the
efficiency of the EC process. On the other hand, the efficiency of Several studies have been carried out for the improvement of elec
monopolar electrode configuration is considerably lower with the same trochemical reactor design in order to increase the process performance
applied current density for both configurations due to the less available for wastewater treatment. Fig. 6 represents the different type of reactor
surface area. However, low operating cost can be observed during the designs used in EC process. Fouad et al., 2009 investigated the efficiency
monopolar electrode connection. Therefore, it is necessary to adequately of both vertical and horizontal electrode design for the separation of oil
Fig. 6. Types of electrocoagulation reactor design.
8
and grease in EC process [69]. An array of separated horizontal Al cyl D-optimal design (an experimental unit of RSM) for separation of oil
inders served as the anode cell. The horizontal cell design was found to from oil-in-water emulsion [75]. The reduction in turbidity and COD
be more effective compared to the conventional vertical parallel plate content were measured to estimate the oil separation. It was observed
cell. The efficiency of rotating cylindrical electrodes in EC process was that, highest removal efficiencies of 90% COD and 99% turbidity were
also investigated for the demulsification of crude oil emulsions [70]. A obtained under an optimum current density and treatment time of 22
decrease in anode passivation tendency was observed due to an mA/cm2 and 22 min respectively. In another study, the EC process was
increased mass transfer rate between the solution and the anode. The optimized for the treatment of bilge wastewater by Ulucan et al., 2014
turbulence produced at the rotating cylindrical electrode also contrib [76]. The RSM study showed that, a maximum oil and grease (O&G)
uted to the favourable mixing conditions in bulk solution, which in turn removal efficiency of 81.7% was observed at the optimal inlet temper
intensifies the process efficiency. Moreover, separation of oil and grease ature and current density of 29 ◦ C and 9.87 mA/cm2 respectively. A Box-
in an electrochemical cell can also be achieved by the development of Behnken design (an experimental unit of RSM) was used by Chavalparit
high-porosity fixed-bed sacrificial anodes. It provides numerous ad and Ongwandee, 2009 for the removal of COD and oil content from
vantages over the conventional electrode design (horizontal or vertical biodiesel wastewater in EC process [77]. It was found that the optimi
anodes) such as low space footprint, high rate of removal and prolonged zation of process parameters effectively reduces the COD and oil content
treatment time between electrode replacements. During the separation by 55.5% and 98.5% respectively. Integration and design of EC process
of crude oil emulsion, the use of Al wire gauze anode was also investi with other treatment methods necessitates comprehensive understand
gated in a batch electrochemical cell [71,72]. Another reactor design for ing of the process. Several attempts have been made for modelling the
the treatment of oil-in-water emulsion is the use of dimensionally stable process performance under different experimental conditions. Carmona
electrodes (anodes). The underlying mechanism consist of electro et al., 2006 developed a simulation model to estimate the separation of
chemical oxidation, which is not present in EC process. Furthermore, hydrocarbon fractions from oily wastewater via use of Al electrodes
taking into account the dynamics of EC process, the operational control [78]. This model was used to simulate the adsorption of organic content
of process parameters has also gained significant technological on the surface of Al(OH)3 particles. The experimental datas obtained
advancement in recent years. During the separation of oil emulsion in EC from lab-scale electrochemical reactor were successfully interpreted by
process, the effect of pulse electric voltage on energy usage was evalu the simulated model. Khemis et al., 2006 established a simulation model
ated by Genc and Bakirci, 2015 [73]. It was reported that the application for indicating the reduction in COD content via particle complexation by
of pulse electric voltage can considerably prevent the overuse of energy Al3+ ions, while taking into consideration the experimentally observed
consumption rate. The study concluded that, a high energy saving effi latency period [79]. The simulation models were mostly based on batch
ciency of 48% was observed during the use of continuous operation reactors, however, few preliminary works have also been conducted on
mode. Maha Lakshmi and Sivashanmugam, 2013 utilized a hybrid sono- plug-flow reactors. A synthetic emulsion consisting of hexane extract
electrocoagulation process for the treatment of oil tanning wastewater able compounds was used in a series of electrochemical studies. It was
[59]. It was observed that the cavitation bubbles were easily broken or reported that, the first-order kinetic model was found to be best suited
coalesced during ultrasonication. It also inhibited the phenomenon of for electrocoagulation of hexane extractable compounds via dispersion
floc formation. As such, it was inferred that the continuous use of son and tanks-in-series (TIS) models. Also, TIS model suggested that each of
ication negatively affected the EC process. However, modifying the the electrochemical cell acted as a discrete continuous-stirred batch
operational control via use of intermittent ultrasonic impingement can reactor.
significantly overcome the problem of passivation. The RSM studies have shown satisfactory results during the optimi
The reactor designs such as high porosity fixed-bed, rotating cylin zation and analyses of the EC process. Design of experiments viz. central
ders, vertical and horizontal plates have gained considerable attention composite design (CCD), Box-Behnken design (BBD), fractional factorial
in the recent years for the removal of wastewater contaminants. Several design (FFD) and several other designs have been implemented to better
factors viz. electrode material, operation mode (batch or continuous), understand and optimize the responses based on the changes in oper
reactor volume, total effective area, depth to width ratio and power ating variables. Even so, there are few limitations associated with these
supply significantly influences the operations of the aforementioned experimental designs. In CCD design, the squared terms of the model
reactors. As such, these parameters need to be optimized for effective may not be orthogonal to each other and there may be difficulty in
performance of the EC process. Also, during the operational control of estimating the individual interaction terms (quadratic by quadratic or
EC process, the phenomenon of electrode passivation in direct current linear by quadratic). Also, FFD requires several experimental runs for
mode may result in the blockage of electrode’s active sites, which in turn the same amount of resources or time available and also the design space
lowers the process efficiency. However, this limitation can be overcome is highly constrained. However, the use of D-optimal design may be
by the application of alternating current or pulse electric field to the considered to overcome such problems. These factors should be taken
solution. into consideration while implementing the RSM study for obtaining a
better performance efficiency of the EC process.
6.2. Optimization and modelling of EC process
7. Integration of EC with other treatment methods
In the field of environmental engineering, optimization of process
parameter has gained significant attention in recent years. The experi 7.1. Hybrid electrocoagulation – membrane processes
mental design tools assist in the anticipation of combined variable ef
fects, which result in achieving the desired optimization. Response Membrane filtration process exhibits high recovery rate, small
surface methodology (RSM) is a set of statistical and mathematical footprint, and low sludge volume. It is considered as one of the most
system, utilized for the optimization and modelling of experimental widely utilized methods for desalination and wastewater treatment.
problems. RSM can be suitably used to investigate and optimize the Microfiltration (MF), nano filtration (NF), ultrafiltration (UF) and
relevant parameters in EC process [28]. In a study conducted by Zhao reverse osmosis (RO) are some of the different types of membrane dis
et al., 2014, the RSM study was used to optimize the EC process for the cussed in this section. Table 1 shows the treatment of different waste
pre-treatment of synthetic water in a hybrid EC-RO system [74]. It was waters via hybrid EC-membrane process. Depending up on the types of
reported that, a current density of 5.90 mA/cm2, solution pH of 7.35 and membrane used and the feed water quality, the membrane separation
treatment time of 31 min were found to be optimal with corresponding processes are considered superior, exhibiting a high recovery rate.
pollutant removal efficiency of 85.8% hardness, 93.8% turbidity and Fouling of membranes and the elevated operational cost are the major
66.5% COD. Tir and Moulai-Mostefa, 2008 optimized the EC process via drawbacks of membrane technologies [1]. As such, EC can be used as a
9
Table 1
Wastewater treatment by hybrid EC-membrane process.
Hybrid Types of Pollutants Operating conditions Removal efficiency of EC Improvement in process References
processes wastewater process performance via hybrid process
EC Membrane
(EC-membrane)
EC-MF Steel Magnesium, Current density = TMP = The removal efficiency for Mg After filtration, the treated [94]
industry Manganese, 10–50 A/m2, Electrode 103–196 kPa, and Ca were 73% and 90% sample followed the surface
wastewater Iron, Calcium, distance = 0.005–0.02 Treatment respectively. Fe and Mn were water discharge limit with
Turbidity and m, Electrolysis time = time = 25 min found to be completely turbidity and TDS value of 0.1
TDS 20 min removed from the treated NTU and 1890 mg/L
pH = 7.0, Electrode effluent. respectively. The permeate flux
connection = BP-S varied from 1146 to 648 L/m2.h.
Drinking Fluoride, Current density = 5–15 TMP = A fluoride removal efficiency The filtered water quality [95]
water Turbidity, TDS A/m2, Electrode 196–509 kPa, of 91.7% was obtained. The obeyed the drinking water
and dissolved distance = 0.005 m, Treatment values of Turbidity, TDS and specification with turbidity
oxygen (DO) Electrolysis time = 20 time = 25 min DO were found in the range of value of 0.8 NTU, TDS of 600
min, pH = 7.9, 12–7.6 NTU, 1310–500 mg/L, mg/L and DO values of 14.3 mg/
Electrode connection and 26.1–12.3 mg/L L. The flux obtained was varied
= BP-S respectively. from 19.19 to 8.16 × 10− 5 m3/
m2.s.
EC-UF Poultry COD, BOD and Current density = 3 TMP = 70 The removal efficiency for An increased removal efficiency [85]
processing TSS mA/cm2, Electrode kPa, COD, BOD and TSS were 59%, of 92% COD, 98% BOD and
wastewater distance = 0.9 cm, Treatment 87% and 84% respectively. 100% TSS were achieved. The
Electrolysis time = 5 time = 7 days water volume recovery was
min, pH = 6.7, enhanced by 30%. The permeate
Electrode connection flux was found to be 52 L/m2.h.
= BP-S
Synthetic Sulfonated Current density = 4–10 TMP = 1–4.5 The removal of SHA from the A high SHA removal efficiency of [96]
wastewater humic acid mA/cm2, Electrode bar, synthetic wastewater was 96.5–98% was obtained. A small
(SHA) distance = 1.5 cm, Treatment observed as 84.3% decrease in the retentate flow
Electrolysis time = 7 time = 5 h rate from 21 to 18 L/h was
min, pH = 5, Electrode observed with an increase in the
connection = MP-P feed concentration from 80 to
160 mg/L respectively.
EC-NF Textile Colour, COD and Current density = 40 TMP = 2–12 The removal efficiency for A complete decolourization was [97]
industry TDS mA/cm2, Electrode bar, turbidity, colour and COD were achieved. The removal of COD
wastewater distance = 20 mm, Treatment found to be 80%, 95% and 50% and turbidity were increased up
Electrolysis time = 60 time = 3 h respectively. to 95% and 99.9% respectively.
min, pH = 13 The average value of membrane
permeability was 14.2 L/h.m2.
bar. The permeate flux was
found to be 22.5 L/m2. h.
Synthetic Amoxicillin Current intensity = TMP = Amoxicillin concentration was The removal efficiency for [98]
wastewater 0.1–1 A, Electrode 0.1–0.5 MPa, reduced up to 52.7% amoxicillin was increased to
distance = 1 cm, Treatment 99%. The hydraulic permeability
Electrolysis time = 60 time = 5 h was found to be 2.21 × 10− 1 m/s
min, .Pa. A reduction of ̴ 30% was
pH = 2.5 and 10 observed in the electrical
consumption of the overall
process.
EC-RO Oil emulsion COD, TDS and Current density = 1.85 TMP = 0.7–3 The removal efficiency for A removal efficiency of 100% [99]
wastewater turbidity mA/cm2, Electrode MPa, turbidity, colour and COD were COD, 99.9% turbidity, 98.9%
distance = 1 cm, Treatment 99.5%, 96% and 92% TDS, and 99.6% Al ions were
Electrolysis time = 6 Time = 2 h respectively achieved. The permeate flux was
min, pH = 4–9, found to be 20 L/m2. h.
Electrode connection
= MP-S
Brackish Silica and Current density = 3.47 TMP = 500 A silica removal efficiency of The turbidity was completed [100]
water turbidity mA/cm2, Electrode kPa, 80% and turbidity of 99% were removed and a feed flux of 82
distance = 4 cm, Treatment obtained. m3/m2.day was obtained. The
Electrolysis time = 30 time = 3.5 h normalized flux was found to be ̴
min, pH = 7, Electrode 0.8. The flux decline was
connection = BP-S reduced significantly due to the
pre-treatment step by EC
process.
pre-treatment process for the effective removal of different wastewater In general, a high cross-flow velocity can be used to lift the particles and
pollutants, while also reducing the overall operating cost of the com keep the pores of the membrane free, thereby preventing fouling. High
bined process. cross-flow velocity causes spiral-wound polymeric membranes to tele
scope, henceforth, anti-telescoping devices are used in most of the sys
7.1.1. Electrocoagulation – microfiltration (EC-MF) tems to keep the membrane in place. At the retentate side, a larger cross-
Microfiltration (MF) is a sieving procedure for particles exhibiting flow velocity (5–7 m/s) is provided by elevating the retentate recircu
pore sizes of 0.1 µm or greater. Both the ceramic and polymeric MF lation pump rate to minimize the fouling on ceramic MF membrane. This
membranes have been implemented widely for the industrial scale creates high wall shear stress, which removes the foulants off the
treatment units over the last few decades. MF membranes foul more membrane surface [80]. On the other hand, electrocoagulation is a
readily than other types of membrane because of their higher pore size. viable and cost-effective technology that can be adapted as a pre-
10
treatment process to remove the suspended particles and organic con involving the UF membranes. As such, EC assisted UF filtration process
taminants, which in turn assist in preventing the membrane fouling. In a may prove to be a very useful approach for reducing the membrane
study conducted by Ben-Sasson et al., 2013, natural organic matter fouling by reducing the suspended particles and organic pollutants.
(NOM) from simulated wastewater was removed using a hybrid EC-MF Besides, decreasing the pollutant concentration in the feed water for UF
system [81]. It was observed that pre-treatment with both Fe and Al process may significantly improve the overall water quality of the hybrid
electrode-based EC process enhances the MF filtering of NOM- process [1]. During the application of EC as a pre-treatment process,
containing solutions in several ways: (1) it can significantly reduce the Sardari et al., 2018 used 5 Al electrodes having an inter-electrode
fouling caused due to the presence of NOM and hence decreases the spacing of 0.9 cm and a current density of 3 mA/cm2 for the removal
energy consumption during the filtration process, and (2) it can also of COD, BOD and TSS from poultry wastewater [85]. The electrode
improve the overall ability of the combined process to remove NOM configuration was arranged in BP-S mode. Pre-treatment with EC pro
content from the simulated wastewater. The influence of EC on filtering cess, resulted in a removal efficiency of 84% for TSS, 59% for COD and
performance is greatly dependent on the solution pH, anodic material, 87% for BOD. The energy consumption of the process was found to be
treatment period, and the type and concentration of NOM. Also, Fe- very low (0.15 kW h/m3). Due to prior degradation of the aforemen
based EC showed better results than the Al-based EC at pH values of tioned impurities, the initial permeate flux increases, while the flux
≥7 in terms of fouling mitigation and NOM degradation. When declination rate decreases at the time of UF process. The UF process
compared to 100 kDa ultrafiltration alone, the EC-MF hybrid process consisted of regenerated cellulose (RC) separator with 1.2 L/min as the
showed a 36-fold reduction in the filtration time and an improvement of flow rate and 70 kPa as the applied pressure. The initial flow rate was
20% in NOM removal rates under ideal operating conditions. Several determined to be 97 L/m2 h with permeate volume of 500 mL, however,
advantages including the capacity to support high permeate flux, low it gets reduced to 55 L/m2 h (43% reduction) over the course of time. At
fouling and high removal rates illustrates the potential of adopting a the end of the hybrid (EC-UF) process, high water permeate quality was
hybrid EC-MF method as an alternate treatment to UF for the removal of obtained with TSS, COD and BOD removal efficiency of 100%, 92% and
NOM [82,83]. Changmai et al., 2019 incorporated a batch EC-MF pro 98% respectively. However, in a study conducted by Yahiaoui et al.,
cess for the treatment of oily wastewater emulsions comprising of oil and 2011, the UF process was utilised prior to EC for the treatment of COD in
grease along with metals viz. Na, Cr, Cu, Ni, and Pb [46]. The operating olive mill effluents [86]. As a pre-treatment process, an UF system with a
parameters such as electrode distance (0.005–0.2 m), initial pH ceraver membrane was used. The degradation of COD via the UF
(3.6–8.7) and current density (20–80 A/m2) were altered during the pre- membrane was very successful, as the process reduced the COD con
treatment process to study its effect on the pollutant removal efficiency. centration from 28 g dm3 to 1.1 g dm3, thereby obtaining a removal
It was reported that the application of voltage difference across the efficiency of 96%. Even after the UF process, the discharge regulation for
electrode surface led to the formation of high amounts of flocs. These surface water was not met. As a result, the permeate with an average
generated flocs are mainly responsible for reducing the oil and grease COD value of 1.1 g dm3 was treated in an electrochemical reactor
concentrations from 35 to 10.2 mg/L, along with the removal of un equipped with iron electrodes. The influence of operational parameters
wanted metal ions from the effluent solution. The MF technique was viz. solution pH, current density, NaCl content, and surface electrode/
then utilized to remove the flocculants from the treated water and reactor volume ratio on the COD removal efficiency was studied. It was
further reduce the pollutant concentration. It was observed that with the reported that, the highest COD removal efficiency was achieved at an
increment in the sintering temperatures from 700 to 1000 ◦ C, the optimum current density of 93.3 A/m2 and solution pH of 4.5–6.5. The
permeate flow increased from 264 to 423 L/h m2 at a pressure of 98 kPa. EC process significantly reduced the COD concentration from 1.1 g dm3
Besides, an increase in the operating pressure also increases the to 78 mg dm3 at the optimum operating conditions, thereby permitting
permeate flux, which may be attributed to the high driving force. It was the direct release of olive mill effluents into the environment. Therefore,
concluded that, the hybrid EC-MF process further reduced the oil and the hybrid EC process can be considered a very effective approach in
grease content below its respective permissible limit (0.2 mg/L). removing the wastewater pollutants due to its cost-effectiveness and
The selective transport of species based on the pore sizes highly sustainability.
determines the membrane performances. As such, pretreatment of the The UF membrane having a pore size of 20 nm− 0.1 µm can be
feed becomes essential to enhance the process performance. This shows effectively used to resolve the limitations of the MF process. The hybrid
the relevance of combining the EC process with different membranes for EC-UF process showed significant improvement in the rejection rate of
effective wastewater treatment. The MF membrane coupled with EC heavy metals, humic acids and bacteria, along with a reduction in
showed high removal efficiency for various wastewaters contaminated membrane fouling, and transmembrane pressure. Even so, there are few
with heavy metal ions viz. As, Cu, Pb, Zn, and Cd. However, the larger limitations associated with the UF membrane such as low salt rejection
pore size (0.1–5 µm) of MF increases the possibility of smaller solutes, capacity and inability to separate low molecular weight species. Also, it
colloids and macromolecules to permeate across the membrane, thereby is highly sensitive to oxidative chemicals. These factors should be taken
lowering the permeate water quality. The use of smaller pore size into consideration and proper solution needs to be developed for further
membranes viz. UF, NF and RO can effectively eliminate the pollutants improving the performance of hybrid EC-UF process. However, the use
that permeates through the MF pores. Besides, more efficient approaches of NF and RO membranes can efficiently reject the salts and low mo
for overcoming such issues should be addressed to improve the perfor lecular weight species that permeates through the UF membranes.
mance of the EC-MF process.
7.1.3. Electrocoagulation – nanofiltration (EC-NF)
7.1.2. Electrocoagulation – ultrafiltration (EC-UF) A nanofiltration (NF) membrane is categorized as a pressure-driven
Ultrafiltration (UF) is basically a low pressure and cost-effective membrane technology, having a pore size between ultrafiltration (UF)
membrane based treatment process. It is a type of filtration process and reverse osmosis (RO) membranes. The pore size ranges from 0.2 to
which utilizes hydrostatic pressure to allow the transportation of water 2 nm, with a variation in the molecular weight cut-off (MWCO) between
molecules via a selective semi-permeable separator while retaining the 150 and 2000 Dalton (Da). In general, the membrane surface is nega
suspended solids and high molecular weight solutes. Parameters tively charged to improve the dissolved ion separation efficiency. The
affecting the process performance viz. membrane fouling leads to a NF membrane is defined by the following characteristics: (1) passage of
considerable reduction in water recovery efficiency due to particle a significant amount of monovalent ions (>30%) across the membrane,
accumulation at the surface of the membrane and across the membrane (2) pore diameters of less than 2 nm, (3) molecular weight cut-off
pores [84]. Suspended solids along with the organic pollutants are (MWCO) ranges between 150 and 2000 Da, (4) significant rejection of
considered as the crucial foulants in the membrane separation process multivalent ions (>90%), and (5) rejection of positive and neutral
11
species based on their shape and size [87]. Due to high permeability and fouling of RO membranes. The use of EC process prior to RO has been
low energy consumption, NF membranes have found considerable proven to reduce the organic matter content, responsible for causing
application in the field of water softening, wastewater treatment as well organic and biofouling. During the treatment of synthetic water, Zhao
as food and pharmaceutical industries. However, membrane fouling is et al., 2014 utilized the EC process prior to RO to minimize the limita
the most serious operational drawback of NF process, since it causes an tions of membrane fouling [74]. A total of 6 electrodes were used con
abrupt decline in the permeate flux and an increase in the operating cost sisting of graphite cathodes and iron anodes. The electrodes were
[88]. To prevent the issue of membrane fouling, NF membranes can be connected in MP-P configuration and an electrode spacing of 1.5 cm was
effectively combined with a proper pre-treatment process, particularly kept. The effectiveness of the EC process was determined by examining
for wastewaters having high pollutant concentrations. The EC process the removal rates of turbidity, COD and hardness. The removal effi
can be successfully used as a pre-treatment step to improve the quality of ciencies of turbidity, COD and hardness were found to be 93.8%, 66.5%,
feed water and minimize the membrane fouling. The EC process has and 85.8%, respectively. The electrocoagulated samples were further
been selected due to its low chemical usage, effective pollutant removal treated by RO process at an applied pressure and flow rate of 2 MPa and
efficiency and low operational cost. Tavangar et al., 2019 treated textile 0.8 L/min respectively. An abrupt decline was observed in the water flux
industry wastewater by both separate and combined EC and NF pro after 60 min of operating time due to the high concentration of scaling
cesses [89]. It was reported that, the combined EC-NF process can ions and organic compounds in the feed water. After 90 min, the water
entirely degrade the high colour content and other remaining pollutants flux decreases to 26 L/m2 h and 4 L/m2 h for pre-treated and raw water
from the treated EC solution, while also improving the overall process respectively. Also, the permeate flux was decreased to 22 L/m2 h after
performance. When compared to standalone EC and NF processes, the 200 min of operating time. The use of EC as a pre-treatment process led
colour reduction was improved by around 2% and 8%, respectively. to an increase in the permissible filtration period by 55%. Besides, the
Also, the use of EC with Al electrodes prior to NF process increases the hybrid EC-RO process exhibited a very high removal efficiency for all the
flux by 76%, as compared to Fe and Ti electrodes. The use of Al elec pollutants viz. oil (>99%), COD (95.5%), turbidity (99.1%) and hard
trodes in EC process considerably improves the flux recovery ratio value ness (99.5%). Sadeddin et al., 2011 also reported similar results during
and alters the fouling mechanism from irreversible to reversible. Be the treatment of well water via hybrid EC-RO process [92]. The EC
sides, Gönder et al., 2020 treated the carwash wastewater via EC-NF reactor consisted of 2 stainless steel electrodes connected to a DC power
process in order to effectively reuse the treated wastewater as rinsing source. The removal efficiencies of TSS and turbidity were found to be
water [90]. The EC process with Fe electrode was used for the pre- 99% and 98% respectively. The pre-treated sample (feed water) was
treatment of carwash wastewater at different operating temperatures then subjected to RO process, which operated for a period of 6 months.
(25–45 ◦ C), stirring speeds (150–350 rpm) and electrode connection The feed water contains very low silt density index (3%/min), which is
modes (monopolar and bipolar). The best performance for EC in terms of considered suitable for the RO plants. The study concluded that, EC as a
pollutant removal and energy consumption was attained at an optimum pre-treatment process significantly improves the RO system in term of
condition of 25 ◦ C, 250 rpm, and MP-P configuration. The electro water flow, silt density index and pressure drop. Besides, the RO process
coagulated samples were again treated by NF process by using Desal 5DL was successful in completely removing the dissolved solids, while the
and NF 270 membranes. The oil and COD content of the carwash hybrid EC-RO process exhibited higher potential in the degradation of
wastewater were reduced by 90% and 88% respectively, while the en multiple pollutants at high removal efficiency. However, during the
ergy usage was calculated as 2.7 kWh/m3. Also, Desal 5DL membrane investigation of EC as a pre-treatment process for seawater desalination,
showed better removal efficiency for total hardness (90%), conductivity Hakizimana et al., 2016 reported that the EC process was ineffective in
(80%) and chloride (92%), compared to NF 270 membrane. Therefore, it the degradation of scaling ions (Ca2+ and SO2− 4 ) due to the low removal
was concluded that the hybrid EC-NF process played a significant role in rate of hardness [93]. The performance of EC process was evaluated
recycling of wastewater. Although EC as a pre-treatment process is very based on the degradation rate of the organic matters viz. absorbance,
effective at reducing the NF membrane fouling and increasing the hardness and dissolved organic carbon (DOC). The energy consumption
permeate flux, however the types of electrode used typically determines of the process was 0.17 kW h/m3. Although the removal rates of
the effectiveness of the hybrid process. absorbance (81%) and DOC (59%) were found to be satisfactory, the
The use of NF membrane (0.2–2 nm) can provide a better alternative hardness was only removed up to 10%. As a result, the scaling ions were
as the process shows much higher flux and better salt rejection charac not properly removed during the pre-treatment process. Except for
teristics compared to UF membrane. The NF membrane process can also hardness, the removal rate of other pollutants was increased with a
effectively retain multivalent salts and smaller solutes. However, the decrease in the inter-electrode spacing and the solution pH. Besides, the
membrane fouling is a crucial problem in NF processes which may affect study concluded that the degradation rate of aromatic compounds was
the quality of the permeate water. Also, the NF membrane process re higher as compared to aliphatic compounds.
quires high energy consumption compared to both MF and UF mem The RO membrane with extremely small pores (0.0002–0.0005 µm)
branes. Factors such as controlling the inorganic salt solubility, is highly capable of rejecting all types of pollutants. The process is
increasing the feed water temperature and the use of a suitable disin relatively insensitive to total dissolved solids and is very effective for the
fectant can assist in reducing the challenges of fouling. In addition, it is desalination of water. Nevertheless, factors such as acidic pH of the
suggested that the NF separators must be used in conjunction with a treated solution, production of permeate water between 20 and 25% of
suitable pre-treatment process to further reduce the membrane fouling the utilized feed and high capital and operating cost needs to be properly
and the overall energy usage of the treatment technique. addressed to support the future adoptability of the hybrid EC-RO pro
cess. Also, the maintenance of the RO membrane is highly complex.
7.1.4. Electrocoagulation – reverse osmosis (EC-RO) Thus, certain conditions viz. reduction in the normalized flux to
Reverse osmosis (RO) is frequently used in combination with other 10–15%, increment in the normalized permeate salt content to 10% and
water treatment techniques to improve the process efficiency and pre reduction in the pressure gradient to 15% should to be strictly followed
vent the limitations of membrane fouling. The membrane fouling prior to the cleaning of RO systems.
considerably affects the RO process, including organic and biofouling.
Accumulation of humic acids, proteins, polysaccharides, oils and lipids
on the surface of RO membrane is mainly responsible for organic 7.2. Hybrid electrocoagulation – oxidation processes
fouling. On the other hand, biofouling is caused due to the adherence
and accumulation of fungus, bacteria and yeast on the membrane sur The oxidation process is mostly utilized in the tertiary stage of
face [91]. Thus, a pre-treatment technique is required to overcome the wastewater treatment. The reason may be attributed to the high
12
degradation rates of heavy metals and organic compounds. Also, no of the saline water was reported to be 11.82. The EC reactor consisted of
toxic substances are introduced into the treated water as a result of the 11 Al/Fe electrodes and are connected in BP-S configuration. A colour
oxidation process. Table 2 shows the treatment of different wastewaters removal rate of 85% was achieved after 10 min of electrolysis time.
via hybrid EC-oxidation process. However, the major drawback of However, the treatment time did not have any significant effect on the
oxidation process is the low degradation rate of pollutants with high rate of removal due to the very high solution pH. A semi-batch stirred
molecular weights, longer operational time as well as high energy reactor of 1L capacity was used for further treating the electro
consumption especially for highly concentrated pollutant enriched coagulated samples. The concentration and the flow rate of ozone was
wastewaters [1]. As a result, the use of EC process as a pre-treatment maintained at 42 mg/L and 40 L/h respectively. The O3 process obtained
step to oxidation may prove to be effective in minimizing the a colour removal efficiency of 92% and energy consumption of 56.3 kW
pollutant concentration at a lower cost and shorter time period. h/m3 after 50 min of treatment time. However, the hybrid EC-O3 process
resulted in the overall decolourization of 98% at the end of 10 min. The
7.2.1. Electrocoagulation – ozonation (EC-O3) study concluded that the use of EC process prior to O3 significantly
Ozonation (O3) is a very effective process that utilizes ozone as a lowered the ozonation time from 50 min to 10 min, thereby lowering the
powerful oxidant to degrade a variety of wastewater pollutants, ozonation period by 80% and consequently saving 5 times the amount of
including dyes. The phenomenon of ozone oxidation occurs either by a ozone dosage. Hernández-Ortega et al., 2010 studied the use of EC in
direct ozone attack (Eq. (17)) through electrophiles or by an indirectly combination with O3 process for the treatment of industrial effluent and
generated in-situ hydroxyl radical attack (Eqs. (18)–(22)) [107]. An observed that the hybrid EC-O3 process was very effective compared to
increase in the O3 dosage enhances the oxidation rate of the pollutants. the standalone O3 process [109]. A current density and electrolysis time
However, O3 cannot remove the pollutants having high molecular of 3 mA/cm2 and 15 min respectively were reported as the optimum
weights, therefore, EC as a pre-treatment process may considerably operating conditions for the EC process. On the other hand, an O3 con
assist in improving the overall process efficiency. Bilińska et al., 2019 centration of 0.052 g/L and flow rate of 13.8 L/h acted as the optimum
determined the efficiency of hybrid EC-O3 process for the removal of condition for the O3 process. During the O3 process, the removal rate of
high colour concentration from saline water [108]. The initial pH value COD, colour and turbidity were found to be 23%, 40.8% and 37.5%
Table 2
Wastewater treatment by hybrid EC-oxidation process.
Hybrid Types of Pollutants Operating conditions Removal efficiency of EC Improvement in process References
processes wastewater process performance via hybrid
EC Oxidation
process (EC-oxidation)
EC-O3 Steel industry Cyanide, COD Current density = Ozone generation The removal efficiency for An improved removal rate [101]
wastewater and BOD 50–150 A/m2, rates = 1–1.33 mg/ cyanide, COD and BOD were of 99.8% cyanide, 94.7%
Electrode distance = s, Treatment time 62%, 60% and 61% COD and 95% BOD were
0.005 m, Electrolysis = 40 min respectively achieved. The operating
time = 30 min, pH = cost of the overall process
7.7, Electrode was 5.801 US$/m3.
connection = BP-S
Grey water COD,TOC and Current density = Ozone A COD removal efficiency of The removal rates of COD [102]
Escherichia coli 5–20 mA/cm2, concentration = 77% and TOC of 64.5% were and TOC were found to be
(E.coli) Electrode distance = 22.3–56 mg/L, obtained. 86% and 70.2%
2 cm, Electrolysis Treatment time = respectively. The E. coli
time = 60 min, pH = 60 min content was reduced up to
7 86%. Also, the total cost of
the process was 1.9 US
$/m3.
Peroxi-EC Pharmaceutical COD Current density = H2O2 The removal of COD from the The removal efficiency was [103]
wastewater 1.7–1.9 mA/cm2, concentration = treated wastewater was increased to ̴ 58% (residual
Electrode distance = 300 mg/L observed as 34.2% 205 mg/L). The
2.5 cm, Electrolysis consumption of energy was
time = 60 min, pH = reduced by 50.6%.
7, Electrode
connection = BP-S
Industrial park COD, Colour Current density = Amount of H2O2 A COD removal efficiency of The removal rates of COD, [104]
treatment plant and Total 14.2 mA/cm2, added = 40 mL/ 56% was obtained. colour and total coliform
coliform count Electrode distance = 0.6 L count were found to be
2.5 cm, Electrolysis 78%, 97% and 99.9%
time = 30 min, pH = respectively.
2.8, Electrode
connection = MP-P
EC-EO Groundwater Nitrate and Current density = 40 Current density = The removal efficiency of The concentration of NH+4 -N
[105]
Ammonium mA/cm2, Electrode 75 mA/cm2, nitrate content varied between ion in the solution was
ion (NH+4 -N) distance = 0.3 cm, Hydraulic 90 and 100% over a 60 min of completely removed
Electrolysis time = retention time = treatment time. Also, an (100%) at a volumetric flow
60 min, pH = 7.8 25–50 min, increase in the NH+4 -N ion rate of 4 mL/min. No toxic
Volumetric flow content up to 6.7 mg/L was by-products were formed.
rate = 4–8 mL/min seen.
Synthetic deep Trace organic Current density = Current density = The removal rates of An improved removal [106]
aquifer compounds 5.55 mA/cm2, 14.8 mA/cm2, trimethoprim (TMP) and efficiency of ̴ 87% TMP and̴
(TrOCs) Electrode distance = Treatment time = benzyldimethyl- 70% BAC-C10 were
1 cm, Electrolysis 20 min, pH = 7.5 decylammonium chloride obtained. The electrical
time = 5 min, pH = 6, (BAC-C10) were̴ 10% and̴ 5% energy per order
Electrode connection respectively. (EEO) was found to be
= MP-P around 10–75 kWh/m3.
13
respectively. However, the use of EC process consisting of 8 Fe elec Overall, the addition of H2O2 to the EC process resulted in the complete
trodes as a pre-treatment step greatly assisted in improving the overall decolourization of distillery effluents along with a total COD reduction
performance of the hybrid process. It was reported that the hybrid EC-O3 of 86% and energy consumption of 1.1 kW h/m3. Farhadi et al., 2012
process led to a significant improvement in the removal rates of COD evaluated the performance of peroxi-EC process for the removal of high
(67.3%), colour (>98%) and turbidity (>98%). Due to the presence of Fe concentrations of COD from pharmaceutical effluent [103]. In the EC
species in the treated electrocoagulated solution, the activation of hy process, 4 Fe electrodes were used having an inter-electrode distance of
droxyl radical-assisted mechanism can substantially improve the yield of 2.5 cm between them and is connected to a DC power source. A current
O3 process. The Fe species generated via EC process act as a catalyst for density of 1.9 mA/cm2, electrolysis time of 60 min and initial pH of 7
the breakdown of hydrogen peroxide into hydroxyl radicals. This im were taken as the optimum operating parameters for the EC process. At
proves the production of hydroxyl radicals in solution, which in turn the optimal conditions, the energy consumption and the COD removal
increases the process efficiency [110]. As such, the rate of pollutant efficiency were found to be 65.1 kW h/kg and 34.5% respectively.
removal was much higher for the hybrid EC-O3 process compared to the However, the addition of H2O2 (300 mg/L) to the EC process substan
standalone O3 process. tially increases the rate of removal to 57.7%. Besides, the energy con
sumption was lowered to 32.2 kW h/kg, thus showing>50% reduction
O3 + 2H+ + 2e– → O2 + H2O (17) from the previous value. Similarly, Yüksel et al., 2009 also investigated
O3 + H2O → 2HO• + O2 (18) the efficiency of peroxi-EC process for the treatment of sodium dodecyl
sulfate (SDS) contaminated wastewater [114]. A total of 4 Fe electrodes
O3 + OH → −
O⋅−2 + HO⋅2 (19) with 2.5 cm spacing between them were placed vertically inside the EC
cell. The electrodes were arranged in BP-S connection mode. At an initial
O3 + HO⋅ → O2 + HO⋅2 ⇄2O⋅−2 + H+ (20) surfactant concentration of 60 mg/L, the hybrid process resulted in the
SDS removal efficiency of 81.5% (residual 11.04 mg/L). Also, the
O3 + HO⋅2 →2O2 + HO⋅ (21)
average energy consumption was found to be 1.63 kW h/kg SDS. It was
concluded that the use of peroxi-EC process showed better pollutant
2HO⋅2 → O2 + H2 O2 (22)
degradation efficiency, when compared to separate H2O2 and EC pro
During the oxidation process, the generation of hydroxyl radical cesses. Moreover, the net energy consumption was significantly reduced
plays a very crucial role in determining the pollutant removal efficiency. in the peroxi-EC process.
Although the hybrid EC-O3 process showed significant results in the
Fe2+ + H2 O2 → Fe3+ + OH + OH⋅− (23)
removal of different wastewater pollutants, however, there are few
drawbacks associated with it. The ozonation process produces acidic
Fe3+ + H2 O2 →Fe2+ + HO⋅2 + H+ (24)
water along with the formation of toxic intermediates at high ozone
concentration. The energy consumption and the operational cost of the The peroxide process is a dosage dependent approach, so that
ozonation process is very high. Besides, complete mineralization of appropriate amount of HO radicals are formed to obtain the required
•
complex contaminants may not be possible. However, addition of a pre/ removal efficiency. However, the addition of excess amount of H2O2 to
post-treatment step can substantially maintain the solution pH and the solution may cause reverse effect and decrease the process effi
lower the required ozone concentration in the solution. Thus, proper ciency. Also, the presence of residual H2O2 in the treated solution may
mineralization of the complex species in the final treated solution and be harmful. As such, the addition of an optimized amount of H2O2 to the
reduction in the energy consumption of the hybrid process can be suc EC process may be helpful in improving the biodegradation of the target
cessfully achieved. effluent and lowering the H2O2 dosage in the solution.
7.2.2. Peroxi-electrocoagulation (EC-H2O2) 7.2.3. Electrocoagulation electrooxidation (EC-EO)

Electrochemical advanced oxidation processes (EAOPs) are ecologi Electrooxidation (EO) is a water treatment technique that utilizes the
cally sustainable wastewater treatment techniques for the degradation phenomenon of oxidation to effectively remove the organic compounds
of harmful and persistent contaminants. The introduction of EAOPs to from different wastewaters, especially from industrial effluents. The EO
wastewater treatment has the potential to avoid and remediate the process deals with the use of hydroxyl radicals to attack the pollutants
pollution issues generated by the clean electron reagent. Even so, some present in wastewaters [26]. In a direct EO process, the oxidation re
limitations associated to the EAOPs have been identified viz. chemically action takes place once the pollutants reach the surface of the electrode
generated sludge, high acid consumption for lowering the solution pH and gets adsorbed in it. The major benefits associated with EO process
and high sulphate and chloride ion concentrations in the treated includes complete reduction and disposal of biological sludge, reduced
wastewater samples. The chemical reactions involved in the oxidation maintenance cost, easy operation and simple equipment design. Some of
process are used to describe the benefits of peroxi-EC process. The the most commonly used electrodes in EO process are platinum, carbon,
oxidation process is highly dependent on the presence of H2O2 and a lead dioxide and boron-doped diamond electrodes. However, longer
ferrous ion source (Eq. (23)). H2O2 is added externally during the peroxi- treatment time and relatively high operating costs limits the applica
EC process, while sacrificial Fe anodes are utilized as the Fe2+ source. bility of the process, particularly in the presence of colloidal particles.
Moreover, Fe2+ ions can be regenerated continuously based on the The EC process can be effectively used as a pre-treatment step to lower
reduction of Fe3+ species (Eq. (24)) [111,112]. In a study conducted by the operating time and minimize the colloidal particles. The EC process
Asaithambi et al., 2016, the electrochemically-induced oxidation pro rapidly coagulates and removes the suspended and colloidal particles,
cess was used for the treatment of distillery effluents [113]. The EC thereby allowing the remaining organic pollutants to be oxidized by the
reactor consisted of 2 Fe electrodes with 3 cm spacing between them and EO process [115]. Linares-Hernández et al., 2010 investigated the
is connected in a BP-S configuration. Two additional Fe electrodes were benefits of adopting the EC process prior to electrooxidation for the
kept between the cathode and the anode for further improving the treatment of industrial effluents [116]. During the pre-treatment step,
pollutant removal efficiency. At the start of the EC process, H2O2 was the EC process consisted of 2 Fe electrodes connected to a DC power
added into the solution, which led to an improvement in the COD source. At an optimum current density and treatment time of 80 mA/
removal efficiency of EC by 13%. Also, the energy consumption of the cm2 and 30 min respectively, the removal efficiency of 85.5% COD,
process was reduced by 15%. It was reported that an optimum H2O2 46.5% BOD, 52.2% colour and 99% total coliform count were obtained.
concentration of 234 mg/L, current density of 1.3 mA/cm2 and elec On the other hand, the EO process consisted of a boron-doped diamond
trolysis time of 240 min were used to produce the best possible results.
14
(BDD) electrode at the anode and a Fe electrode at the cathode. The spacing of 1 cm, and a treatment time of 4 h, respectively for the hybrid
current density was kept similar, while the treatment time for the USEC process. On the other hand, the standalone US process removed
removal of pollutants was 90 min. It was observed that the COD con 4.9% colour and 90% COD, whereas 2.5% colour and 76% COD removal
centration was completely removed within 90 min of electrolysis time, were obtained in the EC process, respectively. Thus, it was concluded
thereby saving around 15% of the total time required for the thorough that the hybrid USEC process led to a significant improvement in the
removal of COD via standalone EO process. Also, the hybrid EC-EO removal efficiency of both COD and colour. Chu et al., 2012 studied the
process resulted in >99% removal of total coliform count, COD and effect of the hybrid USEC process on the reduction of COD and turbidity
BOD along with complete decolourization of the effluent. In another from car washing wastewater [120]. The removal efficiency of the
study, Yılmaz Nayır and Kara, 2018 evaluated the treatment of container hybrid process was determined as a function of time. The pollutant
washing wastewater (CWW) via hybrid EC-EO process [117]. The study degradation occurs primarily within the first 20 min of operation. Pa
mainly focused on the removal of colour and COD content. During the rameters such as current density, inter-electrode spacing, and reaction
EC process, both Al and Fe electrodes were used. A current density of 25 time were varied to evaluate their effect on the process performance. It
mA/cm2, pH of 5 and treatment time of 120 min were taken as the was reported that the operating conditions of 1.2 A current, 1.5 cm inter-
optimal operating parameters. At the optimum conditions, the use of Fe electrode spacing, and 20 min reaction time were found to be optimum
electrodes resulted in the maximum colour and COD removal efficiency for achieving the highest pollutant removal efficiency. At the optimum
of 98% (620 nm wavelength) and 80% respectively. However, the EC conditions, the hybrid USEC process exhibited COD and turbidity
process showed less performance in the removal of COD content. As removal efficiencies of 80% and 96.3%, respectively. The study
such, the EO process was implemented as a post-treatment step to EC. concluded that the final reduced values of both COD and turbidity met
The use of BDD electrodes in the EO process significantly improved the the surface water reuse criteria. Özyonar et al., 2020 investigated the
COD removal efficiency to around 90% within 420 min of treatment removal of colour and COD from aqueous solutions containing reactive
time, whereas at the same wavelength and current density, the decol red and disperse blue dyes via US, EC and USEC processes [121]. The EC
ourization efficiency decreases to 71%. It was concluded that, although process obtained a maximum colour and COD removal of 90% and 80%
the EO process required a relatively longer treatment period for respectively, whereas the US method was able to remove only 50%
achieving high pollutant removal efficiency, the use of hybrid EC-EO colour and 36% COD. However, the hybrid USEC process showed a COD
process can effectively overcome such limitation without hindering removal efficiency of 99% with complete decolourization. These find
the process performance. ings confirmed that the hybrid USEC process outperformed both the
The EO process may produce some disinfection by-products viz. standalone EC and US processes in terms of colour ad COD removal ef
bromates, perchlorates and chloramines depending upon the pollutants ficiency. The reason behind the high pollutant removal by the hybrid
present in the wastewater. Also, the use of BDD and platinum electrodes USEC process may be attributed to the formation of cavitation and/or
for longer period of time may increase the operational cost of the pro micro-streaming effect via US irradiation, leading to the renewal of
cess. The finding of an effective and stable yet economical electrode additional electrode surface.
material would greatly assist in overcoming such limitations. Also, the The integration of ultrasound with the EC process not only improves
integration of EO with other water treatment processes may greatly the rate of dissolution of Fe and Al electrodes, but also significantly
assist in reducing the overall cost of operation. For future sustainability increases the gas bubble structure in the electrodes. During US irradia
of the hybrid EO process, new approaches are needed to reduce the tion, free radicals are generated beyond two HO radicals, which interact
•
production of disinfection by-products and the loss of process perfor to form H2O2, thereby improving the flocculation of the contaminants. It
mance caused by mass transfer limitations. Nevertheless, the use of flow- is worth noting that US irradiation has a substantial influence in the size,
through and channel flow configurations in electrochemical reactors dissipation and amount of gas bubbles produced in the EC process,
may be considered to overcome the limitations of mass transfer in EO which favours the wastewater treatment, resulting in higher pollutant
process. removal efficiency. Although the hybrid EC-US process exhibited
excellent results, however, there are few drawbacks associated with it.
7.2.4. Electrocoagulation – ultrasound (EC-US) The availability of large-scale US reactors is a challenge. For specific
The energy generated from ultrasound (US) irradiation is predicted usage, the US reactors have to be custom made, which considerably
to improve both the kinetics and pollutant removal efficiency of the EC increases its implementation cost in industries. Also, the energy con
process. Also, US irradiation significantly enhanced the removal effec sumption of the process can be very high and the solution turbidity may
tiveness of iron hydroxides. The reason can be attributed to the decrease increase during the process. Besides, direct contact between the ultra
in electrode passivation by reducing the electrical double layer thickness sonic horn and the target liquid can sometimes possess a challenge.
and destroying the solid layer deposited at the electrode surface. US However, this could be overcome by utilizing a flow through the US
stimulates both the electrodes and the ions present in the reaction zone reactor with short residence time and developing non-contact reactors.
of the electrodes by causing flaws on their surface. Moreover, US in Also, optimization of the process parameters viz. power density, fre
creases the friction between the electrode surface and the liquid, quency, irradiation time and addition of a pre/post-treatment method
resulting in local amplification. The energy produced by US substan can considerably assist in reducing the overall energy consumption of
tially improves the production of free radicals, viz. HO⋅2 , H , and OH . the process.
• •
However, one or two such radicals may easily recombine. These radi
cals, on the other hand, are accountable for the breakdown of organic
contaminants. Therefore, the combination of US irradiation with EC 7.3. Hybrid electrocoagulation – biological processes
process has emerged as a promising hybrid technique for the removal of
different toxic pollutants [118]. Asaithambi et al., 2017 employed EC, The hybrid EC-biological process has emerged as a viable option for
US, and hybrid USEC methods for the treatment of paper and pulp in treating highly contaminated industrial effluent and producing high-
dustrial effluent [119]. The study investigated the effect of various quality treated water. Biological treatments are often considered
operational parameters, viz. current density (1–5 A/dm2), inter- economical, simple, and easy to implement for removing different types
electrode spacing (1–3 cm), effluent pH (3–11), and electrode combi of organic constituents present in industrial effluents. However, most
nation (Al and Fe) on the COD and colour removal efficiency of all the industrial effluents consist of hazardous and nonbiodegradable con
three processes. The highest COD and colour removal efficiencies of 95% taminants, in addition to significant amounts of suspended solids and
and 100% were observed at an optimum electrode combination of Fe/ colloidal matter. The presence of such pollutants at high concentration
Fe, an effluent pH of 7, a current density of 4 A/dm2, an inter-electrode may affect or severely diminish the efficiency of the biological treatment
15
process [122]. Moreover, the characteristics of wastewater treated by a membrane fouling and clogging, and high operational cost may signif
single traditional biological process may not meet the new and stringent icantly affect the process performance of the MBR reactors. Several
national and international environmental criteria. These factors have operational parameters in the MBR reactor such as solid retention time,
incited a growing and continuous urge to create a cost-effective, high- transmembrane pressure, mix liquor suspended solid, flux, hydraulic
performance, and sustainable integrated wastewater treatment solution. retention time and food to microorganism ratio needs to be optimized to
The primary reasons for using EC as a pretreatment step are as follows (i) achieve improved effluent quality and lower the effect of membrane
wastewater detoxification by eliminating biotreatment step inhibitors; fouling. Also, chemical cleaning and physical cleaning viz. backwashing,
(ii) removal of the majority of COD or dissolved constituents that might membrane relaxing and/or an amalgamation of both can be used to
result in membrane bioreactor fouling and; (iii) improvement in the mitigate the clogging of membranes. Besides, modification in the
microorganism activity. This combination provides an innovative and membrane bioreactor by using activated carbon as a biofouling reducer
promising application with improved performance and degradation ef and addition of a pre/post-treatment method can considerably assist in
ficiency. There are limited literatures on the hybrid EC-biological prolonging the membrane life and lowering the operational cost of the
treatment system; nevertheless, enhanced performance and higher overall process.
degradation efficiencies of the hybrid process were attained in all in
vestigations, particularly when aluminium electrodes were used, 8. Case studies on electrocoagulation of wastewater treatment
resulting in >95% degradation efficiency [123]. Dia et al., 2018 inves
tigated the possibility of treating landfill leachate using a hybrid EC- Case Study I: Removal of manganese and iron from the effluent of
biofiltration (BF) treatment process [124]. A new design was San Rafael mine in Antauta, Perú [127].
employed in the EC treatment process by concentrically arranging the The San Rafael Mine is situated in the Antauta district (Melgar
electrodes via a cylindrical hollow rod as a cathode and a complete province) of Perú. The major contaminants detected in the mining
cylindrical rod as an anode. Besides, an aerated BF column consisting of effluent are iron (Fe), manganese (Mn) and total suspended solids. Be
formerly acclimated biomass on landfill leachate was used to conduct sides, copper, cadmium and zinc are also present in considerable
the biofiltration treatment process. Additionally, a combination of wood amount. The effluent is collected at the end of tin concentration process,
chips and peat was used to fill the BF column. The study reported that followed by decantation into an 80 feet wide thickener before being
the use of EC as a pre-treatment process removed approximately 37% of discharged into the Antauta river. Acrylic sheet was used for the fabri
the total COD content. It was observed that the COD removed was cation of EC reactor. The reactor consists of seven vertically oriented Fe
mainly composed of humic acid and insoluble organic constituents. electrodes with 0.03 m inter-electrode spacing, 5 L volume capacity and
Furthermore, the removal efficiency of phosphorous, colour, turbidity a dimension of 0.224 m × 0.133 m. A total of three anodes (0.179 m2)
and zinc in the pre-treatment step was found to be 82%, 65%, 82% and and four cathodes (0.238 m2) were utilized in the reactor. The optimum
95% respectively. On the other hand, 45% of the dissolved COD content operating conditions for effective removal of pollutants were 22.3 A/m2
and >99% of the initial ammonium ions were removed during the (current density), 7 V (electric voltage) and 45 min (treatment time).
biofiltration treatment process. The findings confirm that the hybrid EC- During the EC process, the pH was maintained within the range of 6.5–8.
BF treatment process is able to remove both organic and inorganic After the treatment, the solution pH increased for acidic influent;
contaminants from a wide range of refractory wastewaters, including whereas it decreased for alkaline influent at the optimum current den
municipal, industrial and mature landfill leachates. Another reason for sity of 22.3 A/m2. Due to the formation of ferric and ferrous hydroxides,
performing EC as a pre-treatment step during the biological process is to the colour of the formed precipitate became greenish-black. The
prevent membrane fouling in the submerged membrane bioreactors removal efficiency of manganese and iron were reported to be 99.7%
(SMBRs). SMBRs are often utilized in municipal wastewater treatment and 99.2% respectively within the first 15 min of EC process. Besides, a
systems. The performance of the hybrid EC-SMBR process was investi TSS removal efficiency of 98% was achieved at an applied current
gated by Keerthi et al., 2013 [125]. They studied the effectiveness of the density of 22.3 A/m2, however, as the current density was increased to
hybrid membrane bioreactor (HMBR) that included microfiltration, EC, 66 A/m2, the removal efficiency significantly decreased to 91.5%. All
and biological (activated sludge) treatment to remove colour and COD the other contaminants viz. cadmium (Cd), zinc (Zn) and copper (Co)
from tannery effluent. It was reported that the hybrid process signifi were also removed below their respective permissible limits.
cantly improved the treated effluent quality with 90% and 93% removal Case Study II: Removal of COD and turbidity from the effluent of
for colour and COD, respectively, in the HMBR system compared to 73% industrial waste management pond in Befesa, Perú [127].
and 76% in a standalone MBR system. The integration of EC with the The effluent to be treated originated from the industrial ponds of
MBR system causes a substantial reduction in the thickness of the cake waste disposal unit. The industrial pond is 10,000 m2 in diameter and
layer formed across the membrane, resulting in high removal efficiency possess a capacity of receiving 250,000 m3 of industrial waste. The
of the combined process. In another study, Vijayakumar and Keerthi, primary concern of industrial waste disposal ponds is the presence of
(2015) evaluated the efficiency of a combined EC-SMBR system for the high turbidity and COD content. A reactor of 0.004 m3 volume was
treatment of heavy metal contaminated wastewater [126]. This study fabricated with the help of acrylic sheets. Five Fe electrodes having a
was the first to investigate the effect of a hybrid treatment system that dimension of 0.134 m × 0.134 m × 0.0016 m, including 3 cathodes
combined the EC process with membrane bioreactor (EMBR) on the (0.054 m2) and 2 anodes (0.036 m2) were arranged vertically inside the
removal efficiency of heavy metal ions. It was observed that the removal EC reactor. A spacing of 0.03 m was maintained between all the elec
efficiencies of heavy metals in both EMBR and MBR treatment processes trodes. At current densities of 100 and 110 A/m2, the turbidity removal
were in the sequence Cr > Cu > Zn. The hybrid EMBR system showed a efficiencies were found to be 96.1 and 98.3%, respectively, after 30 min
removal of 96.1% COD, 98.6% Cr, 97.5% Cu, and 93.5% Zn. On the of treatment time. However, an increase in current density to 130 A/m2
other hand, the removal efficiencies obtained in a standalone MBR led to a significant reduction in the removal efficiency of turbidity
process were 89% COD, 60.9% Cr, 53.2% Cu, and 48.2% Zn. These (83%). Water becomes turbid or coloured due to the presence of par
findings exhibited the high process performance of the combined EC- ticulate substances viz. silts, clays, algae and organic compounds,
MBR treatment system for a mixture of heavy metals concentration. thereby giving rise to a high COD concentration. Apart from current
Membrane bioreactors not only can handle high volumetric loads, density, the solution pH also has a substantial effect on the removal
but also provides improved pollutant degradation rate, resulting in high efficiency of turbidity and consequently on TSS. An increase in the so
treated water quality. Even though the hybrid EC-bio process demon lution pH of 0.44, 0.54 and 0.68 were observed at current densities of
strated high process efficiency in the treatment of different industrial 100, 110 and 130 A/m2 respectively. Under alkaline condition, the pH
and municipal effluents, however, limitations associated with aeration, did not change much with regards to the reported current densities (100,
16
110 and 130 A/m2). The reason could be due to the exhibition of buff 9. Cost estimation of electrocoagulation process
ering capacity by EC process, which prevents any noticeable change in
the solution pH. As such the pollutant removal efficiency decreases. The practical implementation of the EC process in water and
Furthermore, at applied current densities of 100 and 110 A/m2, an in wastewater treatment depends not only on its technical aspects, but also,
crease in response was detected during the removal of COD. A maximum and perhaps more crucially, on its economic feasibility. Thus, the cost
COD removal efficiency of 38.9% was obtained at 110 A/m2 along with estimation study is critical in establishing the sustainability of the EC
an increase in the solution pH from 8 to 8.5. It was reported that, the process. However, the existing literature lacks the evaluation and opti
increase in current density up to 110 A/m2 did not have any significant mization of the EC operating cost, since only few articles are available
effect on the removal of COD. However, at a current density higher than with detailed cost estimation study for the EC process. Bayramoglu et al.,
200 A/m2, the EC process showed a maximum COD removal efficiency 2007 carried out a cost-benefit analysis for the electrocoagulation
of 61.5%. treatment of textile effluent [129]. The overall operational cost
Case Study III: Removal of turbidity, colour and COD from the including electrode materials, sludge disposal, energy usage, labour,
effluent of textile industry in Béjaia, Algeria [128]. maintenance and depreciation expenses for a chemical plant having a
The wastewater used was collected from the manufacturing section treatment capacity of 1000 m3/day of wastewater was determined for
of a textile industry situated in Béjaia, Algeria. The textile industry different electrode connections (MP-P, MP-S and BP-S), treatment time,
produces around 5000 m3 of wastewater daily. The major contaminants current density, pH and electrode materials (Al and Fe). An operating
detected in the concentrator plant effluent are COD, BOD, turbidity, condition of MP-P connection mode with Fe electrodes at current density
colour and total suspended solids. An electrochemical reactor of 1.5 L and treatment time of 30 A/m2 and 15 min, respectively, was found to be
capacity was fabricated in which a combination of electrocoagulation the most economical option for obtaining a minimum operational cost of
(EC)-electrofloatation (EF) process was carried out. Two rectangular Al 0.25 $/m3 of effluent. The study also reported that the cost of electro
electrodes having a dimension of 27 mm × 17 mm × 1 mm and surface coagulation process was 3.2 times lower than that of chemical coagu
area of 4.59 cm2 were arranged horizontally in the middle of the EC lation for treating the same effluent. During the treatment of cadmium
reactor. The turbidity and TSS removal efficiency in the textile waste containing wastewater, Khaled et al., 2019 studied the effect of different
water were found to be 76.2% and 85.5% respectively. The inter- reactor design parameters on the operating cost and efficiency of EC
electrode distance and current density varied between 1 and 3 cm and process [130]. In this study, the operating cost calculation mainly
11.5–91.5 mA/cm2 respectively. It was reported that the turbidity considered the price of electrical energy, electrode materials and
removal efficiency decreases after 10 min of treatment time as the chemicals used for pH correction. It was reported that the optimum
current density of the process was increased from 11.5 to 91.5 mA/cm2. conditions of 13.5 S/V ratio, 0.5 cm inter-electrode spacing, 300 rpm
Besides, the COD and BOD concentration were also removed up to stirring speed and MP-P electrode connection mode were sufficient for
79.7% and 88.9%, respectively. This significant reduction in COD and the complete removal of cadmium with a minimum operating cost of
BOD could be due to the fact that the hybrid EC-EF process impart 0.116 Tunisian National Dinar (1 TND ≈ 0.06 USD). The study
positive effects on the presence of non-biodegradable organic com concluded that the electrocoagulation process was much more cost-
pounds in textile wastewater. Also, the hybrid EC-EF process can effective than chemical coagulation (4.36 TND ≈ 2.1USD) for treating
considerably improve the effluent biodegradability by converting the the same wastewater. In another study, a techno-economic analysis of
non-biodegradable organics into more biodegradable compounds. Apart chemical coagulation and electrocoagulation was conducted by Rodri
from the aforementioned contaminants, a decolourization efficiency of guez et al., 2007 to treat metallurgical wastewater [131]. For the same
>93% was obtained, indicating that the hybrid EC-EF process is highly flow rate of 110 m3/y, it was observed that the cost of energy con
effective for wastewater clarification. Table 3 shows the operational sumption was 220 £/y ≈ 246.4 USD for the electrocoagulation process.
parameters and removal efficiency of the EC process for the selected case In contrast, the chemical coagulation process showed a much lower
studies. energy consumption cost of 106 £/y ≈ 118.7 USD. However, the mate
rial cost of the chemical coagulation process (1100 £/y ≈ 1232 USD) was
higher than that of electrocoagulation (440 £/y ≈ 492.8 USD). The
comparative analysis suggested that the overall operating cost of the
Table 3
Operational characteristics of the electrocoagulation process for the treatment of three selected case studies.
Effluents Initial pollutant Reactor Design Optimum operating condition Removal Efficiency (%)
concentration
San Rafael mine Fe = 25.1 mg/l Electrode material = Fe electrodes (7 Nos); Current density = 22.3 A/m2; Manganese and iron were removed up to 99.7% and
effluent (Antauta, Mn = 8.3 mg/l 3 anodes = 0.179 m2; 4 cathodes = 0.238 Inter-electrode spacing = 99.2% respectively. Also, TSS removal efficiency of
Perú) TSS = 547 mg/l m2; Reactor volume = 5 L; Dimension = 0.03 m; 98% was achieved. Other pollutants such as
Zn = 0.13 mg/l 0.224 m × 0.133 Electric voltage = 7 V; cadmium, zinc and copper were all removed up to
Co = 0.11 mg/l Treatment time = 45 min, pH 99.9%.
Cd = 0.005 mg/l = 6.5
Waste management COD = 8500 mg/l Electrode material = Fe electrodes (5 Nos); Current density = 110 A/m2; The turbidity content was reduced up to 98.3%
pond effluent Turbidity = 470 2 anodes = 0.036 m2; 3 cathodes = 0.054 Inter-electrode spacing = while only 39% of COD content was removed.
(Befesa, Perú) NTU m2; Reactor volume = 0.004 m3; 0.03 m; However, at a higher current density of 200 A/m2,
Dimension = 0.134 m × 0.134 m × 0.0016 Electric voltage = 4 V; the COD removal efficiency increases to 61.5%. The
m Treatment time = 30 min, pH energy consumption and operating cost of the
=8 process was found to be 4.1 kwh/m3 and 0.36 $ /m3
respectively.
Textile industry COD = 340 mg/l Electrode material = Al electrodes (2 Nos); Current density = 11.55 mA/ The turbidity and TSS removal efficiency were
effluent (Béjaia, BOD = 210 mg/l Surface area of single anode and cathode = cm2; Inter-electrode spacing found to be 76.2% and 85.5% respectively. The
Algeria) Turbidity = 130 4.6 cm2; Reactor volume = 1.5 L; = 1 cm; Treatment time = 10 COD and BOD concentration were also removed up
NTU; TSS = 300 Dimension = 27 mm × 17 mm × 1 mm min, pH = 7.6 to 79.7% & 88.9%, respectively. A decolourization
mg/l efficiency of >93% was obtained.
Colour = >200 Pt-
Co
17
electrocoagulation process (660 £/y ≈ 739 USD) was significantly lower efficiency of EC process. In addition, combining the EC process with
than that of chemical coagulation (1206 £/y ≈ 1350.8 USD). Further other water treatment techniques further lead to an improvement in its
more, during the treatment of can manufacturing wastewater, Kobya pollutant removal efficiency. It was also observed that, the hybrid EC
and Demirbas, 2015 investigated the effect of different experimental process considerably reduces the overall energy consumption and
variables on the operating cost and efficiency of the electrocoagulation operational cost of the treatment. This review investigates the perfor
process [132]. The operating cost calculation mainly included the price mance of different water treatment processes viz. membrane filtration,
of electrode materials and energy consumption. A minimum operating oxidation, adsorption and chemical processes in combination with the
cost of 0.411 $/m3 of wastewater was determined under the optimum EC process. Amongst the several hybrid techniques evaluated, the
working conditions of 20 A/m2 current density, 40 min treatment time combination of membrane filtration with EC process have been found to
and MP-P electrode connection mode. On the other hand, Lin et al., 2005 be quite promising for both water and wastewater treatment, due to its
evaluated the capital and operational cost of pilot-scale electro environmental sustainability, low footprint requirement and easy
coagulation set up with 28 m3/day capacity to recycle residential operational handling. It was concluded that, the use of EC as a pre-
greywater onsite for non-contact usage [133]. The cost calculation treatment process provides many advantages such as mitigation of
mainly considered the price of electrode materials, energy usage, sludge membrane fouling, improvement in permeate water quality as well as
treatment, and chemicals for pH adjustment. The capital and operational reduction in the overall treatment cost of the hybrid process.
costs were determined to be 0.08 $/m3 and 0.19 $/m3, respectively. Few challenges still exist that needs to be solved before the hybrid EC
Thus, the overall cost of the electrocoagulation treatment was reported process can be effectively commercialized. Though the combination of
to be 0.27 $/m3 of wastewater. The study concluded that the total cost of EC with other techniques resulted in high process performance, yet
EC set up and the required surface area (8 m2) are much lower than that factors like non-uniform coagulant dosing and electrode passivation
reported in the existing literature. continue to restrict its industrial application. However, this can be
The operating cost of EC process was found to be economical when resolved by the use of alternate current and regular electrode cleaning.
compared to other water treatment processes. Optimization of the cur Further studies must be conducted to reduce the electrode consumption
rent density and treatment time and selection of appropriate electrode and increase the pollutant reduction efficiency of the process. This might
material and configuration greatly reduces the operating cost of the EC be achieved by evaluating the performance of dielectrophilic improved
process. However, there are few other factors which may increase the electrodes, which are projected to minimize the electrode consumption
process operating cost and needs careful evaluation. Apart from the while also improving the water quality of permeates. Such knowledge
aforementioned parameters, the operating cost may drastically vary would assist in understanding the fouling control and pollutant removal
with electrode passivation and electrode thickness. The reduction in mechanism by the EC process along with future reactor design of the
electrode thickness due to high current density causing rapid anode combined techniques. Besides, the energy consumption rate of different
dissolution may result in frequent replacement of electrodes which in hybrid EC processes must be carried out in order to obtain a sustainable
turn can significantly increase the operating cost of EC process. Also, and energy efficient process. It is highly suggested to conduct extensive
electrode passivation has a potential role in increasing the operating cost research on continuous EC process at pilot scale to replicate the com
as it substantially restricts the flow of electrons throughout the EC mercial scenario. The conventional EC process can be effectively
process. This phenomenon may result in the use of more current and replaced by the use of aeration system. As such, further studies should be
treatment time for the effective removal of pollutants. Another param conducted on aerated EC process to improve the quality of treated water.
eter that may affect the cost estimation is the treatment of produced Degradation process viz. electro-Fenton requires oxygen for proper
sludge. It involves the use of additional sludge disposal system, which functioning. Thus, integration of aerated EC process with electro-Fenton
may eventually increase the overall treatment cost. These aforemen may prove to be beneficial. More studies need to be carried out
tioned factors should be strictly taken into consideration while per regarding the optimization of process parameters, reactor designs,
forming the cost calculation analysis and reactor design for the EC simulated models and cost-effectiveness of hybrid EC processes to
process. However, periodically reversing the electrode polarity via evaluate its potential in achieving industrial scale implementation.
switching the current direction intermittently, and auto cleaning of Although there exist several case-specific process optimization studies,
electrodes via modification with highly hydrophobic and conductive however, a more generic approach is needed to anticipate the reaction
nanocomposites as well as the application of a post-treatment method mechanism and improve the overall pollutant reduction efficiency. It is
may further bring down the operating cost of the EC process. also necessary to evaluate the trade-off between different competing
factors in both modelling and optimization study. Significant impor
10. Conclusion and future prospective tance should be given to the development of simulation and modelling
approach such as artificial neural network (ANN) and Taguchi models
The validity of EC process for the removal of wastewater pollutants for the prediction of pollutant removal efficiency in complex wastewa
at both lab and pilot scale plants has been widely demonstrated by ters. The use of machine learning tools viz. AutoCAD and Python is
various available literatures. However, more studies need to be con another emerging area which could be explored for designing the pro
ducted in order to justify the operating parameters used for scaling up cess reactor and operational control of the EC system. Furthermore, it is
the process, especially when these parameters vary based on the type of highly recommended to develop a sustainable approach for the utiliza
effluents. Even though, the mechanism for the removal of wastewater tion of generated H2 gas and proper disposal of sludge formed during the
pollutant depends strongly on its physico-chemical properties, yet the EC process. This can significantly make the process more efficient, eco-
EC process can be considered highly efficient over other conventional friendly and cost-effective apart from providing a feasible alternative for
techniques. The use of either Al or Fe electrodes results in higher the degradation of different wastewater contaminants.
pollutant removal efficiency, however, it does not always attain com
plete removal. Besides, the use of alternate electrodes viz. Zn and Cu as CRediT authorship contribution statement
sacrificial anodes in EC process has also been reported. The efficiency of
EC process is primarily based on several operating parameters viz. cur Pranjal P. Das: Writing – original draft, Conceptualization, Meth
rent density, type of electrodes, solution pH, electrolysis time, sup odology, Data curation. Mukesh Sharma: Software, Methodology.
porting electrolyte and inter-electrode distance. The use of different Mihir K. Purkait: Supervision.
electrode connection modes, optimal reactor designs and simulation
models along with the development of advanced electrode materials
may altogether play a significant role in enhancing the treatment
18
Declaration of Competing Interest Environ. Prot. 146 (2021) 169–189, https://doi.org/10.1016/j.

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Separation and Purification Technology: Pranjal P. Das, Mukesh Sharma, Mihir K. Purkait

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Separation and Purification Technology 292 (2022) 121058

Contents lists available at ScienceDirect

Separation and Purification Technology

Recent progress on electrocoagulation process for wastewater treatment:

1. Introduction Secondary treatment includes biological processes viz. biological filter

Fig. 1. Flowchart of the conventional wastewater treatment plant.

Fig. 2. Schematic diagram of the electrocoagulation process.

Fig. 3. Mechanism of pollutant degradation by electrocoagulation process.

investigated the effect of current density on the removal of high COD

5.2. Inter-electrode distance

In EC process, the inter-electrode distance is considered to be a very

Fig. 6. Types of electrocoagulation reactor design.

7.2.2. Peroxi-electrocoagulation (EC-H2O2) 7.2.3. Electrocoagulation electrooxidation (EC-EO)

Declaration of Competing Interest Environ. Prot. 146 (2021) 169–189, https://doi.org/10.1016/j.

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