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A review on industrial wastewater treatment via electrocoagulation processes

A.K. Darban, Visiting Professor, A. Shahedi, Ph. D, student, F. Taghipour, Professor,

A. Jamshidi-Zanjani, Assistant Professor

PII: S2451-9103(20)30109-5
DOI: https://doi.org/10.1016/j.coelec.2020.05.009
Reference: COELEC 590

To appear in: Current Opinion in Electrochemistry

Received Date: 18 March 2020

Revised Date: 6 May 2020
Accepted Date: 21 May 2020

Please cite this article as: Darban AK, Shahedi A, Taghipour F, Jamshidi-Zanjani A, A review on
industrial wastewater treatment via electrocoagulation processes, Current Opinion in Electrochemistry,
https://doi.org/10.1016/j.coelec.2020.05.009.

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 A review on industrial wastewater treatment via
electrocoagulation processes
A. K. Darban1 , A. Shahedi2, F. Taghipour3 , A. Jamshidi-Zanjani4
1
. Visiting Professor at Nanyang Environment & Water Research Institute, Singapore, Faculty of
Engineering, Tarbiat Modares University, Chair of Modares Environmental Research Center. Tehran,
Iran, [email protected]
2
. Ph. D. student, Faculty of Engineering, Tarbiat Modares University, Tehran, Iran.
3
. Professor, Department of Chemical and Biological Engineering, University of British Columbia,
Vancouver Canada.

4
. Assistant Professor, Department of Mining, Faculty of Engineering, Tarbiat Modares University,
Tehran, Iran.

Abstract

Every year, a large amount of wastewater is discharged from various industries

into the environment, and various methods are used to treat wastewater in order
to reduce the amount of pollutants. Electrocoagulation (EC) is an
electrochemically-based technique that generates coagulant species in situ from
the electro dissolution of sacrificial anodes, usually made of iron or aluminum
destabilizes suspended, dissolved, or emulsified pollutants by employing an
electric current. It has a potential in removing various kinds of pollutants
including organic and in-organic contaminants for various types of wastewater.
The effectiveness of EC process depends on various parameters including pH,
electrode, operation time, and current density. The goal of this study is to
review the most relevant literatures that published recently. The main
challenges associated with the EC process are electrode passivation and energy
consumption. EC compared with other common methods has advantages such
as reducing energy consumption and reducing operating costs.

Keywords: Heavy metals removal; Wastewater treatment; Electrocoagulation.

1. Introduction
The negative impact through the contaminated water and wastewater and limitation of hydric
sources is nowadays an irrefutable worldwide issue. Thus, water recycling and pollution are

1
considered as the most important environmental problems of the current century [1].
Definition of the industrial wastewater is very wide and different from the domestic one. Due
to the different types of industries and various applied process, the resulting composition and
characterization of the effluent is totally different and very complex. Based on the harm
caused by industrial effluent for environmental contamination is different, than can be
divided into organic pollutants, solid pollutants, toxic pollutants, oil pollutants, acid-base
pollutants, biological contaminants, nutritional pollutants, aerobic pollutants, thermal
pollution, and sensory pollutants. Although, certain types of the contaminants are as same as
to the municipal wastewater, but its numerical value or concentration is usually very different
from urban effluent. The partition of harmful substances existed in industrial wastewater and
their probable sources are presented in Table 1 [2].

Table 1 Main contaminants and probable sources in industrial wastewater [2].

Harmful contaminants The probable sources
Caustic soda, chemical fiber, paper, leather, printing and dyeing, oil
Alkali
re-fineries, and electroplating industry.
Mining, chemical, steel, machinery, electroplating industries and
Acid
non-ferrous metallurgy.
Smelting, metal mining, electroplating, batteries, metal processing,
Cadmium and its compounds
and chemical, etc.
Explosives, mercury refining industry, cholor alkali, mercury
Mercury and its compounds
pesticides, chemicals, instruments, electroplating, etc.
Pharmaceutical, chemical, metallurgical, ore processing, pesticides,
Arsenic and its compounds
paint, fertilizers and other industrial
Hexavalent chromium and its Specialty glass industry, smelting, mining, electroplating, chemical,
compounds metal processing, batteries, etc.
Coal gas, coking, electroplating, acrylic,metal cleaning, synthesis,
Cyanide
the gold industry and acrylonitrile refining industry, etc.
Coal gas, coking, synthetic resins, oil refining, chemicals, dyes,
phenol
pharmaceuticals and other industries
Machinery, oil refining, food processing, natural gas processing and
oil
oil industry
Leather, chemicals, gas, dyeing, coking, oil refining, gas and oil
Sulfide
processing industry, etc.
Pesticides, smelting, lead paint, gasoline explosion, chemicals,
Lead and its compounds
enamel industry.
Organic phosphorus, organic
Chemical industry, pesticides, etc.
chlorine
Free chlorine Textile bleaching, papermaking, chemical industry, etc.
Radioisotope laboratories, nuclear industry, hospitals, and other
Radioactive substances
weapons production
Polychlorinated biphenyls
Plastics, electricity, lubricants and other industrial
(PCBS)

It could be mentioned that water treatment techniques appear as the main important
solution to decrease the pollution effect in aqueous phase and aquatic systems. All
wastewater and water treatment plants try to resolve the above mentioned
environmental problems. Among the treatment methods, physico-chemical methods
are the most prevalent process because these have been applied and known since
centuries to produce potable water for human consumption. However, recently due to
the industrial activities and the technological development the contaminants existed in

2
wastewater are totally different and complex. Therefore, the water treatment methods
have been an important topic of investigation to treatment the emerging pollution [3].
According to the literature, wastewater treatment methods could be classified into
three main categories including physical, chemical, and biological processes (Table
2). A conventional wastewater treatment plant includes a combination of the three
above mentioned processes to eliminate various types of pollutants. Physical
processes usually eliminate contaminants from wastewater with no significant change
in the biological or chemical forms of the aimed pollutants. Chemical methods are
categorized as additive methods, as they need the reactants to eliminate aimed
pollutants. However, the addition of reactants makes these processes unattractive in
comparison with other techniques as they increase the net dissolved substances in
wastewater and make it not reusable in other applications. Biological methods apply
microorganisms for the biodegradation of pollutants in wastewater, and the main goal
of these methods is to decrease the nutrients and organic content in water bodies.
Biological processes are categorized into anaerobic and aerobic according to the
existence of dissolved oxygen in aqueous phase [4].

Table 2 Classification of conventional operations unit in wastewater treatment plants [4].

Treatment Level Treatment Method

Sedimentation
Preliminary Physical/mechanical
Screening

Flotation
Physical/mechanical
Sedimentation
Primary
Chemical
Chemical
Chemical precipitation

Aerated lagoon

Activated sludge

Rotating biological contactors

Secondary Biological Trickling filters

Biological nutrient removal

Anaerobic digestion

Pond stabilisation

Ion exchange

Tertiary or advanced Physical Activated carbon adsorption

Reverse osmosis

3
 Gas stripping

Membrane filtration

Chlorination

Advanced oxidation
Chemical
UV irradiation

Ozonation

Typical wastewaters and natural waters are heterodispersions, having a various types
of solid materials with different particles sizes. Presence of particles in aqueous phase
is generally encountered in a wide range of industrial processes. They can have broud
range of size from millimeters to nanometers that lead to difficulty in elimination
process. A summary of typical particle size ranges, as well as some related
information and relationship of type of separation process for special particle are
presented in Fig. 1. As could be seen, a distinction has been presented between
suspended particles and colloidal, with the former taken as having at least one
dimension with a size less than about 1 μm [5].

Fig. 1 Size distribution of particulate material and conventional treatment method [5].

The purpose of this paper is to investigate the parameters affecting the efficiency of
EC method and the possibility of increasing elimination efficiency by combining with
other methods. The innovation of this article is to evaluate the efficiency of EC

4
method in comparison with common methods in terms of efficiency, power
consumption and operating costs.

2. A review of wastewater treatment methods

Different methods are used to treat industrial effluents. Each of them has its own
advantages and disadvantages. In the following section the main treatment methods
and their advantages and disadvantages will be discussed.

• Precipitation
Precipitation method includes three Precipitation methods such as Chemical
Precipitation, Hydroxide Precipitation and Sulfide Precipitation. In this process, the
added chemicals react with heavy metal ions to reduce their solubility. The solid phase
created is easily separated from the solution by filtration or precipitation. Advantages
of using this method are: Inexpensive, ease of operation, most of the metals can be
removed. Disadvantages of using this method include: Large sludge generation and its
management.

• Ion Exchange
The purification process begins with ion exchange and complexes are formed after
heavy metal ions are absorbed by the surface. At the end, hydration occurs at the
surface of the solution or pores of the adsorbent. In this way, the ions are removed
from the electrolyte solution by the resins and enter the solution in front of the ions
with the same load. Advantages of using this method are: Regeneration of materials,
selective for metal ions. Disadvantages of using this method include: Available for
less number of metal ions, costly.

• Adsorption
The philosophy of adsorption is based on the transfer of mass between the liquid
phase and the adsorbent with the solid phase. Three key steps to absorb contaminants
on the adsorbent are involved: (i) Contamination penetration from the solution to the
adsorbent surface; (ii) adsorption of the pollutant on the adsorbent surface; and (iii)
infiltration into the adsorbent structure. One of the most popular adsorbent is activated
carbon that is widely used. Advantages of using this method are: High performance
and low treatment time. Disadvantages of using this method include: Limited
regeneration, costly, efficiency depends on adsorbent.

• Membrane Filtration Process

One of the easiest ways to purify water is to use a membrane. By passing the solution
containing the contaminants through the physical pores of the membrane with
different sizes, which is done under high pressure, the solution is done by passing the
solution through the pores and leaving the contaminants on the membrane. Membrane
filtration technology includes five major types: reverse osmosis, ultrafiltration,
microfiltration, Nano filtration, and electro dialysis. These processes are basically the
same, but have some major differences in the pore structure (pore size, pore size

5
 distribution, and porosity), membrane permeability, and applied operating pressures.
Advantages of using this method are: High separation selectivity, low pressure, low
space requirement, high efficiency, reliability, easy operation. Disadvantages of using
this method include: High operation cost, low anti-compacting ability.

• Photo catalysis Process

This method uses non-toxic semiconductors that harness light with appropriate
wavelength instead of chemical compounds. It is preferred over chemical processes
because of not using toxic materials as catalysts.
In general, the photo catalytic process takes place in five stages which are:
I. Transfer of contaminants from solution to solid surface
II. Absorption by semiconductor surface
III. Photo catalytic reactions
IV. Product decomposition
V. Transfer products from interface region to solution

Advantages of using this method are: simple design, low-cost operation, high stability,
and high removal efficiency. Disadvantages of using this method include: Limited
applications, long time duration electrochemical treatments.

• Electrochemical
Three major electrochemical treatment technologies including electrocoagulation
(EC), electro flotation (EF) and electrode position. Pollutants such as heavy metal ions
are retained in the wastewater by their surface electrical charges or hydrogen bond.
After introducing the electric field, the electrostatic charges holding the suspended or
emulsified pollutants together are neutralized and they will then be coagulated from
the aqueous phase. Heavy metal particles bond together like small magnets to form a
mass that is called sludge or floc. The flocs produced through EC compared with
those of other techniques are large with less bound water and are more stable. Flocs
are easily removed from the solution at the lowest cost. EF separates pollutants by
floating them to the surface of the liquid phase.
Electro deposition is advantageous because no further reagents are necessary, no
sludge will be produced during the process, and it is highly selective and low-cost as
well. It transforms dissolved metal ions into solid particles by deposition on ionic
conductors (cathode and anode) to protect them from corrosion. Advantages of using
this method are: Most of the metals can be removed, no chemical consumption,
selectivity for metal ions. Disadvantages of using this method include: Current
density, high operational and capital cost [5]. Additional merits and dimerits of
common methods to eliminate heavy metals from wastewater are given in Table 3 [6].
Table 3 Prevalent processes to eliminate heavy metals from wastewater [6].
Process Advantages Disadvantages

Bioadsorption using Selectivity and good adsorption Challenges concerning optimizing the
modified capacity operating conditions and

6
 biopolymers the proper synthetic

methods

Adsorption using Reservation, production, and regeneration

mineral substances of the applied adsorbent
High performance, Low cost
or industrial
byproducts

Limited regeneration, costly,

Adsorption process
High performance (99%) efficiency depends
by activated carbon
on adsorbent

Chemical Large sludge generation and its

Inexpensive, ease of operation
precipitation management

Chemical Ease of sludge dewatering and

High chemicals consumption, costly
coagulation settling

Less

harmful by-products,
Simultaneously elimination of Limited applications, long time duration
Photo-catalysis organic pollutants and

metals

Most of

the metals can be

Electrochemical Current density, high operational and
methods removed, no chemical capital cost

consumption, selectivity for metal

ions

High operation cost

due to energy
Electro-dialysis High selectivity
consumption and membrane

fouling

Regeneration of materials, selective Available for less

Ion-exchange
for metal ions number of metal ions, costly

7
 High

Membrane filtration separation selectivity, low pressure, High operation cost

low space requirement,

High efficiency, reliability, easy Low anti-compacting

Nano filtration
operation ability

3. Theory and history of Electrocoagulation

Although utilizing electricity for water treatment applications return to the nineteen’s
century, when EC was applied for the drinking water treatment in the USA, they were
reported impractical because of the high required electricity and capital cost [7].
During the previous decade, electrochemical wastewater treatment process initiated to
be growth as an environmentally friendly technique that produces minimum footprint
without compromising the quality of the treated water, minimum sludge generation,
and requires no chemical additives. EC is an electrochemical process that uses a low
electrical current to eliminate heavy metals from aqueous phase. EC system is also
useful in elimination of tannins, dissolved metals, dyes, and suspended solids. The
pollutants exists in wastewater are maintained in solution by electrical charges. When
charged particles and ions are neutralized with ions of opposite electrical charges
provided by EC process, they precipitate in a stable form after being destabilized.
Electrochemical methods are fast, simple, cheap, eco-friendly and easily operable.
Moreover, the produced purified water is odorless, colorless, clear, and potable with
low sludge generation. There is also no chance of secondary water pollutants in these
processes [8]. EC has been successfully used to eliminate heavy metals and soluble
ionic contaminants from aqueous phase by various researchers [8, 9]. Similar behavior
to traditional coagulation could be expected during the EC process [10, 11]. This
method applies a low current to dissolve aluminum, iron or other metals as sacrificial
anodes immersed in the contaminated wastewater. The electrodisolution raises an
increase on the ions contents in aqueous phase or their complexed species with OH-
depending on the sacrificial anode used and the pH conditions [12–14]. These species
act as destabilization agents or coagulants; lead to separate contaminants from the
aqueous phase [15]. Overall, the below mentioned mechanisms occur during an EC
process [16–18]:
(1) Reactions occurred near the electrodes that generate metal ions from anodes
electrodissolution, and hydrogen gas at the cathode.
(2) Destabilization of the suspended particulate matter, pollutants, and breaking
emulsions.
(3) Generation of aggregates of the destabilized phases and its coagulation in the
aqueous phase as flocs.
(4) Elimination of coagulated contaminants through electroflotation by evolved H2,
and sedimentation (electroflotation could be applied to scatter the coagulated solids

8
through the produced bubbles of hydrogen gas at the cathode during water
electrolysis, transporting the particles to the top of the reactor).
(5) Chemical and electrochemical reactions raising the cathodic reduction of metal
ions and organic pollutants onto the cathode surface (Fig. 2).

Fig. 2 Interactions occurring within an electrocoagulation reactor [18]

EC combined with other treatment methods is an effective and safe way for the
elimination of contaminants. It is considered as an effective method, due to the higher
adsorption of OH- on mineral surface in in-situ compared with pre-precipitated
hydroxides when metal hydroxides are applied as coagulant [19]. Since the produced
flocs by EC are relatively large which are more stable and consist less bound water,
thus, they could be easily separated by filtration. EC can be schemed for wide capacity
range of effluent treatment plant and requires simple equipment’s. Since no chemical
addition is needed in this method, it decreases the generation of secondary
contaminants. It requires low current and hence, can be operated by green processes
including fuel cells, solar, and windmills [20]. It is considered as an environmental
friendly process since it does not require addition of the chemicals/reagents and the
electron is the main reagent. This will eventually remove some of the toxic substances
applied as coagulants in the traditional wastewater treatment methods and reduce the
sludge production to a great extent. EC method can generates lower quantity of sludge
compared to other processes and effectively destabilize small colloidal particles. The
generated sludge from the EC process is less as compared with the chemical
coagulation and also the performance EC is 10 to 15% higher compared with the
chemical coagulation process. Moreover, one of the main advantages of EC method is
that it could be scaled up to pilot and industrial scales [21-23]. Additional
disadvantages and benefits of EC method is presented in Table 4. In general, the
versatility, environmental compatibility, energy efficiency, selectivity, safety, cost-
effective, and amenability to mechanization are the add-on benefits of EC method
[24].

Table 4 benefits and disadvantages of EC method [24]

9
 Advantages Disadvantages

Solar power can be used

Lack of systematic
Low energy requirements
reactor design
Without moving parts

Coagulation and precipitation(results in lower

Electrode passivation
capital costs, combines oxidation

Low sludge production over time

Reduced risk of secondary pollution

Address drinking water and wastewater

Need for maintenance
Nonspecific method

4. Principles of EC process

The main fundamental of EC was derived from electrolysis of water formulated by

Michael Faraday [25]. It happens when direct electric current passing through
electrolyte, leading chemical reactions at electrodes. The mechanisms of
electrochemical phenomena in aqueous phase have been described by Lin et al.
(1998). It is mentioned that three main processes including electrooxidation,
electroflotation, and electrocoagulation are responsible for elimination removal [22].
The electroflotation and electrocoagulation processes are particularly important for the
treatment of water and wastewater. During EC, the main chemical reactions include
the formation of OH- ions and H2 gas at the cathode and the dissolution of metal
cations at the anode (Fig. 3). The anode materials have significant role on the
oxidation reactions that occur on the sacrificial electrode. The majority of researches
apply anodes made of stainless steel (SS), Fe, and Al or Al alloy [23]. Some studies
applied Mn [26] or Mn-based alloy anode [27] Cu [28] and Zn [29]. Hence, the below
oxidation reactions (for irons, Fe or stainless steel (SS) electrodes) could be occurred
[30]:
Anode:
Fe(s) Fe+2(aq) + 2e-

4Fe(s) 4Fe+2(aq) + 8e-

Al(s) Al+3(aq) + 3e-

Cathode:
2H2O(l) + 2e- H2(g) + 2OH-(aq)

8H+(s) + 8e- 4H2(g) 10

 Overall:
Fe (s) + 2H2O (l) Fe(OH)2(s) +H2(g)

3H2O(l) + 3e- 1.5H2(g) + 3OH-(aq)

3H2O(l) + Al(s) 1.5H2(g) + Al(OH)3(s)

4Fe (s) + 10H2O (l) +10O2(g) 4Fe(OH)3(s) +4H2(g)

Fig. 3 Mechanisms of electrocoagulation process [22]

5. Applications of EC

Applications of EC were divided into six main categories (Fig. 4). Heavy metals could
be discharged from various anthropogenic sources and industries are challenging to
treat as they are toxic and non-biodegradable. Heavy metals include arsenic, cadmium,
zinc, nickel, copper, chromium, manganese, lead, mercury, silver, iron, boron and
many others. It is evident that EC technique has been successfully examined to
eliminate the most toxic and abundant heavy metals existed in wastewater (Table 5).
According to the Table 5, it could be declared that the EC process is an effective
treatment technique for heavy metals elimination, which are difficult to be eliminated
by other conventional techniques.

11
 Applications Of Electrocoagulation

Water
textile and Food Paper
containing Refinery Produced
industry industry industry
heavy wastewater water
wastewater wastewater wastewater
metals

Fig. 4 Applications of electrocoagulation [31]

Furthermore, Table 5 presents that Al–Al, Fe–Fe, or Fe–Al are the most used pairs of
electrodes in the previous studies. It could be related to the fact that both Al and Fe
with high electrical conductivity are nontoxic and inexpensive [32]. Moreover,
application of EC treatment method to remove organic pollutants is given in Table 6.

Table 5 Application of EC treatment method for the elimination of some conventional pollutants and
heavy metal ions
Content Current density Removal
Pollutants Electrodes pH References
[mg.l-1] (A/m2) efficiency %

5 98.9%,
zinc, nickel
and - Fe–Fe 30,40,35,43,30 5 96.3% [33]
chromium
7.4 99.8%

Zn2+ 50-2000 Al–Al 8.3 5.3 100

[34]
99.93%,
Zn2+, Cd2+,
- Fe–Fe 15 6.9 97.15%, and
and Mn2+ [35]
85.46%,

Al-air fuel
As 1 308 7 100 [36]
cell

Fe–SS 99.7
Uranium - 70 -
[37]
Al–SS 97.7

Phosphate 100 Al-Al 6 6 99

[38]

chromium 91.7
55.3-3.5 SS – SS 73.5 3.5 [39]
(VI)- pb 91.3

Copper,
Nickel, and 50-250 Fe–Fe 0.186 8-10-7 99-92-99
[40]
Chromium

12
 Mn 360 Al– Al 10v 9 92 [41]

Nitrates 300 Al–Al 1.2 9.8 89.4 [42]

fluoride & 80 85.68

Fe–Al 4.5 5
arsenic [43]
10 100

Cadmium 50 Al –Al 20v 7 90

[44]
thallium (I) 10 Al –Al 10 9 86.4 [45]

Sb(V) and below 0.1

60-29 Fe–Fe 5 5 [46]
Co(II) mg/L

below 0.1
arsenic & Fe– Fe mg/L
4–600 2.9A 8.6 [47]
silica Al –Al below 100
mg/L

boron 10 Fe–Ni 3.75 8 99 [48]

2226 93
Ammonia,
362 Al–Al 5A 8 93 [49]
Zn& Fe
128 83

26.263 91

Saline(TDS, 8.498 93
Cl-, Br- and Al–Al 2 8 [50]
SO42-) 6 92

6562 90

Selenium 0.3 Fe –Fe 1.68A 5 90 [51]

Mercury 1.02 Fe–Fe 4.93 7 82.72

[52]
Fe–Fe - 100
cyanide 100 12 [53]
Al–Al 100 60

Cu, Ni, Zn, 20

and Cr & Fe– Al 4mA 11 >95% [54]
cyanide 100

Table 6 Application of EC treatment method for organic pollutants

Content Current Removal
Pollutants Electrodes pH Ref
[mg.l-1] density efficiency %

13
 95.1
1019 Cu (anode)
COD, oil and grease -Al 25 6.5 92.5 [55]
200 (cathode)
99

45.7
phenolic, turbidity &
- Al–Al 15A 5.5 99.9 [56]
color
70.4

phenolic compounds -- Al–Al 10V 5 40 [57]

10 Al–Al 15v 4.1 51 [58]

COD

natural organic matter

38.3 Fe –SS 4A 6.61 79 [59]
(NOM)

organic compounds - Fe – Fe 30V 3 87.1 [60]

COD 1250 99.7

SS-MS 0.634 A/dm2 7.26
± 50 [61]
oil and grease 96.43

1,155
Lignin (mg 78.5

COD Phenol/ Fe– Al 10V 5 85

L) [62]
Color 100
657

COD - Fe– SS 22 mA/cm2 7 87 [63]

3400-
COD 3840 91.9
Al – Al 28v -
[64]
Turbidity 728NT 92.3
U

Particulate 40.75

Phosphorus (PP), 33.00

Polyphosphate (PO43-
), carbon 32.83
1A -
electrodes [65]
(P2O5), 25.83

(COD) -87.88

(DO) 34.3

14
 Turbidity 202 99.5

phosphates 4.75 Al – Al 0.2 A 7 96.69 [66]

Organic matter 23 43.57

COD 94.88
5803 Al – Al 10.75 8.7 [67]
Color 78.65

Al – Al 25v 85
COD - [68]
Fe – Fe 20v 45

COD 72
- Al – Al 6v 3
[69]
Color 97

TOC 220-260 42.5

COD 280-295 18.6

Turbidity 15-35 Al–Al 25 mA/cm2 5 83.5 [70]

TSS 34 64.7

Color 436-620 90.3-94.9

COD 25500 95

BOD 15600 steel wool 25A 5 94 [71]

SS 12300 96

COD 1250 55

Total Organic Carbon 600 60

Fe–Al 1 8.79 [72]
Total Nitrogen 41 90

Turbidity 310 100

Turbidity 99.9

Phenolic Compounds - Al–Al 65v 5.5 45.7 [73]

Color 70.4

Cefazolin (ppb) 42.3 94

COD 528 Fe–Al 50v 7 85 [74]

Turbidity (NTU) 269 94

Color 3000 Al - Al 166.7 5.5-6 100 [55]

15
 COD mA/cm2 50

Humic Acid - Fe – Fe 50v 5 [75]

92.69

Norfloxacin antibiotic - Fe – Fe 50v 5 [76]

92.69
perfluorobutane
sulfonate (PFBS) 87.4
perfluorohexane
sulfonate (PFHxS) 95.6
- Al–Zn 12v 7 [77]
perfluorooctane
sulfonate (PFOS) 100
perfluoroalkanesulfoni
100
c acids (PFSAs)

Oil & Grease

- Fe–Al 20 mA/cm2 7.8 98.1 [78]
Polycyclic aromatic
hydrocarbons (PAHs) - Fe – Fe 40 mA/ cm2 7.75 86 [79]

6. Operational parameters affecting the removal of contaminants from effluent

Many parameters affect the efficiency of elimination of pollution by EC method, the

most effective of which can be conductivity of the solution, type of power supply, pH
of the solution, distance between the electrode, electrolysis time, and current density.

• Effect of initial pH
One of the key parameters for removing contaminants in the EC method is pH. By
creating alkaline conditions and changing the pH, metal hydroxides are produced,
which increases the efficiency of removing contaminants.
Bener et al (2019) investigated the effect of the different pH values (5, 8, and 10) of
the TOC removal. The maximum TOC elimination at pH=5 was 65%. Test results
showed that the elimination efficiency decreased with increasing pH. The reason for
this can be attributed to the production of hydrogen gas in the cathode [70].
İrdemez et al (2006) investigated the effect of pH on phosphate removal from effluent
using EC method. The results showed that when there is no control over pH, low pH
is suitable for reducing energy consumption, and when the pH of the system is
controllable, the optimal value is between 6-7 because Fe(OH)2 solubility is minimal
in this range [80].

• Electrolysis time

The next parameter to eliminate contamination and increase efficiency is to eliminate

electrolysis time. By increasing the electrolysis time, the efficiency of removal is

16
increased to a maximum and then led to a constant rate. The number of generated
metal hydroxide increases with an increase in the electrolysis time.
In this regard Esfandiari et al. (2019) used EC process to remove cefazolin and COD
from hospital wastewater. The tests were performed in three specific voltage (15, 30,
50 v) and time periods (10, 30, 50 min). Result showed that the maximum efficiency
of contamination removal in 50 minutes was more than 92% [74].
Bazrafshan et al (2012) Used EC to remove COD, TSS, and BOD5 from dairy
effluent. This research was conducted at different times (15-60 min) and voltages (10,
20, 30,40,50,60 v). The results showed that the highest removal efficiency of COD,
TSS and BOD5 at 60 minutes and 60 volts were obtained at 98.84, 97.75 and 97.95%,
respectively [81].

• Current density
The next effective parameter in EC process is current density as it determines the
coagulant dosage rate, bubble production rate, size and growth of the flocs, which can
affect the efficiency of the EC. As the current density increases, the dissolution of the
anode, along with the metal hydroxide flocs, increases, resulting in increased
efficiency in removing contaminants from the effluent.
In this regard Bener et al (2019) investigated the effect of current density (12.5, 100
mA/cm2) on the TOC removal efficiency. The maximum efficiency of elimination of
these pollutants was obtained in the flow density of 100 mA/cm2. In contrast, the
lowest efficiency of pollution elimination was related to density at 12.5 mA/cm2.
They showed a doubling of current density, removal efficiency improved from 10 to
22.5% after 120min. When the current density increased from 50 to 100 mA/cm2, the
results showed that the efficiency of TOC removal increased from 28.5% to 34.42%.
Also, First and second order kinetic models were investigated on the
electrocoagulation. With the increasing current density reaction rate increasing for
both models the second-order kinetic model was found more suitable with the R2
values between 0.962–0.986 [82].
Nasrullah et al (2014) Used high Current densities (605, 908, 1211, 1513 and 1816
A/m2) in electrocoagulation process to treat sewage wastewater. The test results
showed that at the highest current density and pH=7, the removal efficiency of COD,
BOD and SS was 98.07, 98.07 and 97.64, respectively [83].

• Distance between the electrodes

The distance between the electrodes and their surface area are important parameters,
the optimization of which directly affects the operating costs.
When the effluent has a high electrical conductivity and a constant current density is
used to reduce energy consumption, the distance between the electrodes must be
increased. Conversely, when the effluent has a weak electrical conductivity, the
distance between the electrodes must be reduced to reduce the power consumption.
Attour et al (2014) investigated the effect of electrode distance to remove phosphate
from wastewater using electrocoagulation. They used aluminum electrodes at different
distances in the effluent with a specific electrical conductivity. The results showed

17
optimal operating conditions are an electrodes gap of 5 mm, an initial pH of 3 and a
conductivity of 3.2 mS [84].

• Effect of applied voltage on metal removal

The voltage applied, like other parameters, directly affects the elimination efficiency
and costs.
In this regard, Bhagawan et al (2014) examined the effect of the amount of voltage (4
and 8 V) used on the efficiency of heavy metal removal using electrocoagulation
method. Result showed At 8 V, the maximum removal of metals was found to be 96,
96.4, 99.9, 98, and 99.5 % for Cr, Ni, Zn, Cu, and Pb respectively [85].

7. Comparison with other treatment methods

In recent years, many researchers have conducted to compare the EC method with
other treatment techniques. Akyol et al (2013) compared the two methods of EC and
electro Fenton (EF) to treat effluents from liquid organic fertilizer plant.
Under optimal operating conditions for the electrocoagulation method (50 A/m2, 45
min and pH= 6), the removal efficiencies of 79% for TOC, 83% for COD, 73% for
total phosphate and 95% for color was obtained, while under the optimal conditions
for the electro Fenton method (50 A/m2, 45 min, 25 mM H2O2 and pH= 3), the
removal efficiencies 87% for TOC, 91% for COD, 96% for total phosphate and 99%
for color was obtained, respectively.
In addition, operating costs were calculated for methods, which were obtained for EC
and EF methods, 0.74 and 1.23 €/m3, respectively. They concluded that, the EF
method was more efficient than the EC method in terms of efficiency in removing
contaminants, while the EC method was less expensive than the EF method [86].
Al-Shannag et al (2015) used EC method to remove heavy metal ions from metal
plating effluent. The results showed that with increasing current density and residence
time, elimination efficiency increases. So that more than 97% of heavy metal ions are
removed at current density of 4 mA/cm2, pH of 9.56 and treatment time of 45 minutes.
While under these conditions specific energy consumption and specific amount of
dissolved electrodes were about 6.25 kWh/m3 and 1.31 kg/m3, respectively [87].
Manikandan et Al (2017) compared the two methods of EC and photo Assisted
Chemical Oxidation (PACO) to eliminate reactive blue dye. The results showed that
the removal efficiency of both methods was more than 99%. Operating costs for EC
and PACO process are calculated at 0.5937 $ and 0.016 US$, respectively. But in
terms of electrical energy consumption as well as the overall operating cost EC
process compete (0.0481 US$ and 0.6418 US$) with the PACO process (1.0267 US$
and 1.04337 US$) [88].
Eskibalci et Al (2018) compared the coagulation and electrocoagulation methods for
dewatering of coal preparation plant. The results show that when aluminum electrodes
are used, the removal efficiency is the same for both methods. In addition, the use of
the EC method has reduced operating costs to 22.2% compared to the coagulation
method [89].
Kumar Sandhwar et al (2018) compared the three methods electrocoagulation, peroxi-
electrocoagulation and peroxi-coagulation processes for treatment of simulated

18
purified terephthalic acid wastewater. Wastewater containing major toxic components
of purified terephthalic acid wastewater: benzoic acid, terephthalic acid, para-toluic
acid and phthalic acid.
Process variables included pH (4-12), current density (45.72-228.60 A/m2), electrolyte
concentration (0.04-0.08 mol/L), electrode gap (1-3 cm), H2O2 concentration (600-
1,000 mg/L) and reaction time (20-100 min). The maximum COD removal of EC,
PEC and PC treatments was 60.76%, 73.91%, 66.68%, respectively. In addition, the
energy consumption of each method was 95.81, 49.58, 69.26 (kWh/kg COD
removed), respectively. Because the PEC method has the lowest energy consumption
and the highest removal efficiency, it is the most effective removal method [90].
Maitlo et al (2018) Used air metal fuel cell electrocoagulation techniques to remove
arsenic in water. The results showed that using this method continuously eliminates
more than 99.5% of arsenate in water for 4 hours with maximum power density 5.9 W
m-2.Also, in batch mode; more than 99.9% of arsenate was removed from the water in
6 hours with maximum power density of 1.99 W m-2[36].
Gaied et al (2019) compared Tertiary treatment of wastewater by electro-coagulation,
electro-Fenton and advanced electro-oxidation processes. After 180 min, the removal
efficiency of BOD5 and COD was 56% and 14%, respectively, while the EC method
destroyed a large number of germs. At the same time, this elimination rate increases to
75% and 52%, respectively, when the EF process is used, and the germs are
completely destroyed.
Using the AEO method, the removal efficiency of BOD5 and COD was obtained, 92%
and 57%, respectively, and all germs are eliminated. The economic study showed that
the EF process is technically and economically the best of these alternatives for
treatment of this wastewater.
The treatment cost of 1 m3 of wastewater was estimated at 13.8, 17.3 and 21.8 €/m3
for ECiron, EFiron and AEOPt processes respectively. Reactor cost and total capital
investment (without anode, for flow rate 1 m3.d-1) (in €) were 19518.3 € and 111059.1
€ respectively for both ECiron and EFiron. However, estimates for AEOPt were 6022.9€
for reactor cost and 34270.5€ for total capital investment [91].
Ramprasad et al (2019) compared two methods of coagulation and electrocoagulation
to eliminate Landfill Leachate. These tests, which were performed in Batch mode,
showed that the efficiency of removing the two methods was almost the same (more
than 74%). In addition, the efficiency of eliminating pollution in
coagulation/flocculation process has been higher than EC method. In EC method, the
removal efficiency of turbidity, COD, chloride, alkali and soluble solids were 98%,
78.1%, 84.5%, 77.9% and 75.8%, respectively. While for the coagulation/flocculation
process, the efficiency of removing the expressed contaminants was 97%, 74%, 83%,
74% and 71% respectively [92].
Arturi et al (2019) compared electrocoagulation and chemical coagulation (CC)
method in order to the treatment of gelatin production plant wastewater. Results
indicated that the composition of the precipitates at different operation conditions,
such as pH, show that EC has increased efficiency of COD removal, compared to CC
with the same dose of aluminum (Al+3) as coagulant. The efficiency of COD removal
was 73.6% with EC and 55.6% with CC. The in-situ formation of zeolites in the EC

19
process explains the high efficiency of this treatment compared to the CC process
[93].
Ghanbari et al (2020) investigated efficient treatment for landfill leachate through
sequential electrocoagulation, electro oxidation and peroxymonosulfate
(PMS/UV/CuFe2O4) process. Result showed that COD removal efficiencies were up
to 60.0, 50.0 and 77.9% for EC, EO and SR-AOP, respectively. Removal efficiencies
for the sequential process were 95.6, 90.5, 91.6 and 99.8% for COD, TOC, BOD and
ammonia (NH4-N) respectively [94].
Padmaja et al (2020) compared efficiency of chemical coagulation and
electrocoagulation methods in the treatment of pharmaceutical effluent. The results
showed that though chemical coagulation has brought a considerable decrease in
percentage of COD, suspended solids and chlorides, but the extent of decrease in the
Total Dissolved Solids is only 14.05 % using Alum and 26.3 % with FeCl3. Whereas
electrocoagulation method which has reduced both COD and TDS to 92.3 % and
91.5% proved more efficient with Fe-Al assembly using a lowest current of 0.04 A at
a time interval of 15 min. The coagulant consumption is also less in electro
coagulation compared to chemical coagulation rendering it as a cost effective
technology [95].

8. The kinetics of removal by EC method

In recent years, researches have been performed on the kinetics of effluent removal
using the EC method. For example, Ahmadian et al (2012) studied the kinetic
treatment of slaughterhouse effluent by electrocoagulation method. In this study, the
effect of various parameters such as electrode number (4, 6, 8), operating time (10-
60min) and current density (5, 10,15,20,25 A/m2) were investigated. The results
showed that increasing the time and number of electrodes had a positive effect on
increasing the elimination efficiency, so that a large number of electrodes must be
used to achieve a certain efficiency in a short time. The highest removal efficiency
BOD5, COD, TSS, total nitrogen using eight electrodes in 50 minutes and current
density 25 A/m2 was 97, 93, 81 and 84%, respectively. The test results showed that
the BOD5, COD, TSS and TN deletion kinetics follow the first-order kinetic model
[96].
El-Shazly et al (2013) examined the kinetics of phosphate removal from industrial
effluents using the continuous EC method and the effect of several variables on
phosphate removal rates. Results showed that the rate of phosphate depletion increases
with increasing solution circulation flow rate, current density, and the temperature of
the solution, while the rate of depletion decreases with increasing concentration of
phosphate ions.
The kinetics of phosphate removal by this method was described by the first-order rate
equation.
-v ( ) = KAC
Where V is the solution volume, Co and Ct are phosphate ions initial concentration and
concentration at any time t, respectively, while K is the mass transfer coefficient and
A is the anode surface area [97].

20
El-Shazly et al (2013) examined the performance of the EC method in batch mode to
remove nitrate and phosphate ions from effluent. Experimental results showed that
with increasing current density and pH, the removal efficiency of nitrate and
phosphate increased, while with increasing concentration of these ions, the removal
efficiency decreased. Also, experimental results showed that to eliminate these ions
using the EC method, the first rate order equation can be used to describe the kinetic.
In addition, the activation energy of this reaction is 5 kCal/mol and the reaction is
controlled by diffusion [98].
Attour et al. (2014) investigated the effect of electrode distance to remove phosphate
from wastewater using electrocoagulation. The results showed optimal operating
conditions are an electrodes gap of 5 mm, an initial pH of 3 and a conductivity of 3.2
mS, in these conditions the phosphate is totally removed with a rapid kinetic rate.
[75].
Singh et al (2017) evaluated the kinetic behavior of the EC process in order to remove
suspended solids and metals from artificial effluent. In this study, the relationship
between elimination efficiency and flow density was evaluated. The results showed
that the removal efficiency of TSS was 76.6% in 30 minutes and the current density
was 5.3 mA/cm2 and for heavy metals such as chromium, zinc and copper was 59.2,
82.1 and 99%, respectively. Kinetic study showed that the pollution elimination model
follows the first and second order equations, which depend on the flow density and
EC time [99].
Bener et al (2019) investigated kinetic for TOC removal at various current densities
(12.5–100 mA/cm2). The first and second kinetic models were used for the EC
method. The results showed that with increasing reaction rate, the efficiency of
removal eliminates up to the maximum and as the current density increases, the
reaction rate for the kinetic model increases for the second time, and R2 was suitable
for this equation [82].

9. Economical aspects

The economical aspect is one of the main parameters that affect the wastewater
treatment process. In the EC method, the costs include the cost of external chemical,
cost of dissolved electrode, and energy consumption. The operating cost during the
EC method could be calculated through the following equation [100].
Consumption of electrode (Cel, kg/m3: kg of electrode dissolved/m3 of wastewater):
C electrode= M × I×RT /V × F × n

Consumption of electrical energy (Cen, kW h/m3):

C energy= RT × U × I / V

Consumption of chemical (Cchem, kg of chemical/m3):

(Cchem = Chemicals used /m3 of wastewater)

Total cost (cost/m3 ) = a C electrode +b C energy +c C chemicals

where RT = reaction time of treatment (s), U = voltage (V), I = electrical current (A),
Z = amount of electron moles (3 for Al, 2 for Fe), M = molecular mass of Fe (55.84
g/mol) and Al (26.98 g/mol), V = volume of wastewater (L), F = Faraday’s constant

21
(96,500 c/mol), c = cost of chemicals which can be added (US$/kg), b = electricity
costs (US$/kWh), and a = cost of aluminum or iron (US$/kg). AlJaberi found the
relation between the value of operating cost in one hand and the effect of electrodes
geometry and their consumption as well as energy consumption on the other hand
[101]. Kobya et al. applied EC technique to remove Cd, Ni, and CN from
electroplating rinse water. The elimination efficiencies were reported 90%, 93%, and
95% for Cd, Ni, and CN, respectively. The remediation cost was calculated around
2.45 US$/m3 and 1.85 US$/m3 for Ni and Cd at optimum conditions, respectively.
[102].

10. Conclusion and perspectives

Various parameters such as pollutants types, their toxicity and concentration, volume of
wastewater are affected the selection of effluent treatment method. Among the different
technique, EC has been applied for effective elimination of a wide range of contaminants
from aqueous phase. It revealed a better efficiency in comparison with some other
conventional treatment technique. EC recognized as a simple technique, which has less
remediation time and adequate cost. Electrocoagulation is effective process for heavy metals
removal for industrial wastewater however, its efficiency depend electrode type and other
operation parameters such as initial concentration, pH and electrolyte concentration. The
mechanism of removal is due to AlO(OH) generation in the sludge sample through the Al
electrode, and FeO(OH) and Fe3O4 generation in the sludge samples using Fe electrodes.
Heavy metals were also co-precipitated during the formation of iron oxides. It is
characterized by high settle-ability and low sludge production. Moreover, it could be
combined with some other treatment techniques such as advanced oxidation and UV-LED, to
have better performance which could be a new area of investigation [103]. This coupled
system may apply for disinfection water for drinking. Use of three dimensional electrode,
porous electrode, Nano electrode are also new areas of investigation which has not been
discussed here. Overall, the EC process is considered as capable treatment technology to
overcome lots of drawbacks for heavy metals removal from industrial wastewater.

Conflict of interest statement

Nothing declared.

Acknowledgement

This work was supported by Modares Environmental Research Institute (MERI), Tehran, Iran
and Nanyang Environment and Water Research Institute (NEWRI) Singapore.

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30
Declaration of interests

The authors declare that they have no known competing financial interests or personal relationships
that could have appeared to influence the work reported in this paper.

☐The authors declare the following financial interests/personal relationships which may be considered
as potential competing interests:

The authors declare that they have no known competing financial interests or personal relationships that
could have appeared to influence the work reported in this paper.