Professional Documents
Culture Documents
Al Qodah2017
Al Qodah2017
net/publication/319302382
CITATIONS READS
35 2,564
2 authors:
Some of the authors of this publication are also working on these related projects:
At the moment I am a visiting professor in the Chemical Engineering department, Taibah University, Saudi Arabia. View project
All content following this page was uploaded by Mohammad Al-Shannag on 08 November 2017.
To cite this article: Zakaria Al-Qodah & Mohammad Al-Shannag (2017) Heavy metal ions removal
from wastewater using electrocoagulation processes: A comprehensive review, Separation Science
and Technology, 52:17, 2649-2676, DOI: 10.1080/01496395.2017.1373677
Article views: 46
Download by: [Professor Mohammad Al-Shannag] Date: 08 November 2017, At: 10:40
SEPARATION SCIENCE AND TECHNOLOGY
2017, VOL. 52, NO. 17, 2649–2676
https://doi.org/10.1080/01496395.2017.1373677
a
Chemical Engineering Department, Faculty of Engineering Technology Al-Balqa Applied University, Amman, Jordan; bChemical Engineering
Department, School of Engineering, The University of Jordan, Amman, Jordan
the process complexity. This comprehensive review considers the fundamental aspects of EC Electrocoagulation;
processes such as mechanisms, kinetic models, and isotherm models used by different research- electrochemical reduction;
ers. Furthermore, the impact of the main design and process operational parameters on the heavy metal ions removal;
removal efficiency is discussed and analyzed. Many concluding remarks and perspectives are industrial wastewater
stated to give insights for possible future investigations. treatment
CONTACT Zakaria Al-Qodah z_alqodah@hotmail.com; zqudah@taibahu.edu.sa Chemical Engineering Department, Faculty of Engineering
Technology, Al-Balqa Applied University, P. O. Box 340558, Amman, Jordan.
Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/lsst.
© 2017 Taylor & Francis
2650 Z. AL-QODAH AND M. AL-SHANNAG
Table 1. Sources of some heavy metals, their toxic effects, and the maximum contamination limits standards (MCLS).
MCLS (µg/L)
Heavy metal Main sources Major toxic effects WHO USEPA References
Arsenic Combustion of fossil fuel, Bronchitis, bone marrow, skin cancer, depression, pigmentation changes, 10 50 [18]
mining, pesticides neurological disorders, muscular weakness, dermatitis, hepatomegaly
Cadmium Mining, smelting, and plastic Kidney damage, emphysema, weight loss, gastrointestinal disorder, Itai– 3 5 [19]
welding, refining pesticide, Itai disease, bronchitis, hypertension,
fertilizer
Chromium Steel, electroplating, dyes, and Carcinogenic, severe diarrhea, skin rashes, respiratory problems,, kidney 50 100 [20]
textile industry and liver damage, vomiting, weakened immune systems and genetic
material
Copper Electroplating, mining, Neurotoxicity, anemia, hyperactivity, schizophrenia, postpartum 250 1300 [14]
pesticides, batteries, copper psychosis, insomnia, cystic fibrosis. Autism, stuttering, inflammation, and
cooking pots dizziness
Lead Batteries, mining, paint, Anemia, malaise, brain damage, anorexia, liver dysfunction, kidney 10 5 [21]
pigments, explosives, dysfunction, gastrointestinal damage, mental retardation
electroplating
Mercury Mining, paper and paint Damage to kidney and nervous system, protoplasm poisoning, 1 2 [22]
industries, batteries dermatitis, corrosive to skin, eyes, muscles
Nickel Electroplating, porcelain Dermatitis, lung cancer, chronic bronchitis, pulmonary fibrosis, rapid 200 134 [23]
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
processes include bioadsorption,[13,14] biological Table 2. Common methods to remove heavy metals from
treatment,[26] chemical precipitation,[27–29] coagulation, wastewater.
membrane filtration, activated carbon,[33] solvent Process Advantages Disadvantages
extraction,[34] ion exchange,[35] reverse osmosis,[36,37] Adsorption using High efficiency (99%) Costly, no regeneration,
activated carbon performance depends
sedimentation, flotation,[11] electro-dialysis,[38] resin che- on adsorbent
lation, solid–liquid extraction,[29] electrocoagulation Adsorption using Low cost, high efficiency Production, reservation,
industrial by- and regeneration of the
(EC), flocculation, or coagulation, and neutralization.[7] products or adsorbent still cause
Unfortunately, many of these treatment processes are mineral much attention
considered as inefficient and costly, particularly, if the substances
Bioadsorption using Good adsorption Challenges concerning
ion concentrations in wastewater are lower than the modified capacity, selectivity the proper synthetic
range 1–100 mg/L.[17,27,39] Moreover, the complete biopolymers methods and
optimizing the
removal of the metal ions by some processes requires operating conditions
large amounts of reagents and consumes energy[15,29] Chemical Ease sludge settling, Costly, high
coagulation dewatering consumption of
which could lead to new waste disposal problems.[40] chemicals
Moreover, the selection of a sustainable treatment pro- Chemical Ease of operation, cheap Large quantity of
precipitation sludge, sludge disposal
cesses is influenced by several factors including low cost, problems
ease of operation, high efficiency, and low sludge Electrochemical Selectivity for metal ions, High capital and
methods no chemical operational cost,
production.[41,42] Table 2 depicts a summary of the most consumption, most of current density
mentioned treatment processes used for the removal of the metals can be
removed
heavy metal ions in addition to their advantages and Electro-dialysis High selectivity High operation cost
disadvantages.[32,43,44] It is evident from Table 2 that due to membrane
most of the processes suffer from serious technical and fouling and energy
consumption
economical disadvantages. Unlike other processes, EC Ion-exchange Selective for metal ions, Costly, available for less
treatment process seems to offer potential advantages of regeneration of materials number of metal ions
Membrane filtration Low space requirement, High operation cost
the efficient application, ease of operation, reduction of low pressure, high
sludge production, and a cost-effective treatment process separation selectivity
Nano filtration Easy operation, Low anti-compacting
for heavy metal ions.[2,45,46] Accordingly, there have been reliability, high efficiency ability compared with
a numerous number of publications during the last two ultra-filtration
Photo-catalysis Removal of metals and Long time duration,
decades using EC as a promising treatment method.[47] organic pollutant limited applications
For this reason, the main objective of this paper is devoted simultaneously, less
harmful by-products
to review and analyze researches concerning the
SEPARATION SCIENCE AND TECHNOLOGY 2651
application of EC process for the removal of heavy metal stringent environmental regulations regarding the was-
ions from wastewater. The mechanism of EC, the kinetic tewater discharge have led EC technologies to regain
and isotherm models used in the adsorption step, the their importance worldwide.[42,54]
effect of the main design, and operational parameters As mentioned above, electrochemical processes can be
affecting the EC process are analyzed and compared used to remove many different pollutants in wastewaters
between different investigations. expressed as: suspended solids (SS) and total dissolved
solids (TDS),[55] chemical oxygen demand (COD),[41,56]
and biochemical oxygen demand (BOD),[57] lignin and
Background on EC processes
phenol,[57] dyes,[58] phenols from olive mills wastewater,[59]
EC is an electrochemical process that involves the and anionic contaminants.[60] In addition, heavy metals
usage of an in situ direct current to promote oxidation have gained considerable focus to be treated by EC pro-
of a metallic sacrificial anode made of iron (Fe) alu- cesses. Actually, EC is used to treat wastewater containing
minum (Al), or other metals to generate positively organic pollutants or heavy metal ions. However, there are
charged ions.[48] These positively charge ions act as many differences between the constituents of the organics
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
destabilizing agents for the emulsion by neutralizing or metal ions containing wastewater. This suggests some
the repulsive forces that keep the particles suspended differences in the process mechanism and performance in
in the aqueous medium. Then, these ions will act as the two applications. For this reason, this review will focus
magnets that attract the oppositely charged particles on the application of EC process for the removal of heavy
to form relatively big masses or agglomerates.[42,49] metal ions from wastewater.
These neutrally charged agglomerates will float or
precipitate depending on its apparent density. For
example, if an aluminum-scarified anode is used, alu-
Electrocoagulation of heavy metal ions from
minum cations (Al+3) will be produced and act as a
wastewater
coagulant like aluminum compound coagulants used
in traditional wastewater treatment systems. The EC In the last two decades, EC process has been applied to
process is usually carried out in an electrochemical remove many heavy metal ions from industrial wastewater.
reactor consisting of an electrolytic cell containing These heavy metals include arsenic,[61] copper,[62,63]
one anode and one cathode. The anode or the sacri- nickel,[62,63] zinc,[62] manganese,[62] chromium,[63–65]
ficial electrode is formed from conductive metallic mercury,[66] cadmium,[19] lead,[67] silver,[68] iron,[69]
plates. The cathode could be made of the same boron,[70] and many others. Table 3 shows part of the
anode material or of different materials.[50] During published results of EC treatment processes for some
the last two decades, the EC has proven as a very toxic heavy metal ions.
effective treatment process for the removal of different It is clear from Table 3 that EC process has been
contaminants from wastewater. This process has many successfully tested to remove the most abundant and
advantages over other treatment processes including toxic heavy metals found in wastewater. Actually, if
the reduced sludge production, ease of operation, and mercury is excluded, the literature has much published
the no need for the addition of chemicals.[46] results about these elements. The removal efficiency in
Electrochemical process had been used for the first these studies is relatively high and above 97% in 70%
time in England in 1889 to treat wastewater.[51] of the mentioned studies. In these results, the waste-
Elmore[52] registered a patent for the use of electrolysis water is completely cleaned and the residual traces of
in mineral beneficiation, whereas a large-scale EC pro- heavy metals in the treated water are within the inter-
cess was performed in the USA in 1946[53] to treat water national standard limits. This indicates that EC is a
for drinking purposes. It seems that the relatively large powerful treatment process for heavy metal ions,
capital and energy cost prevented the commercial appli- which are difficult to be effectively removed by
cation of the EC processes worldwide. In contrast, exten- known other traditional methods. Moreover, Table 3
sive research studies have been conducted in the last 20 shows that Fe–Fe, Al–Al, or Al–Fe are the most used
years in the application of EC processes to treat different pairs of electrodes in the previous investigations. This
effluents of wastewater. These studies have presented could be attributed to the fact that both Fe and Al are
more information about the suitable conditions and cheap, nontoxic, and excellent electricity conducting
enabled a better understanding of the process.[54] Two materials. In addition, it is obvious from Table 3 that
important factors encourage again the use of EC tech- acidic media were used in most EC processes in the
nology for wastewater treatment. First, the ever increas- previous studies, whereas basic EC media were rarely
ing standard of drinking water supply. Second, the used.[47,109]
2652 Z. AL-QODAH AND M. AL-SHANNAG
Table 3. Electrocoagulation treatment processes for the removal of some heavy metal ions.
Ion Concentration (mg/L) Electrodes Current density (A/m2) pH Removal efficiency % References
As (III) 2 Fe–Fe, Al–Al 6.5 to 15.3 6–8 99, 37 [71]
50–500 Fe–Fe 45 7 98 [72]
50 Al–Al 60 7.5 92.2 [73]
1–30 CS–CS 136–208 2.8–4.1 99 [74]
50 Fe–Fe 5.4 4 98.42 [75]
50 Al–Al 5.4 4 85 [76]
Cd (II) 5–500 Al–Al 40 V 10 99.9 [77]
50 Fe–Fe 6.5–35.7 7.2–8.2 80 [78]
1.5 Al–SS 66 [79]
20 Al–Al 97.5 [80]
20 Zn–Zn 97.8 [81]
10–50 Fe–Al 30 7 99.9 [82]
Cu (II) 3 Fe–Fe 31–54 7 91 [83]
50 Al–Al 30–50 5.1 99.8 [84]
50–200 Al–Al 150 7 99.5 [85]
10–50 Fe–Al 30 7 98.9 [82]
75–300 Al–Al 100–400 4–8 97 [86]
250 Fe–Fe 2–25 8.95 96 [87]
Cr (III) 1711, 2235 MS–MS 90.6, 7.4 [88]
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
(iv) Interaction between the positive ion and the and zinc.[127]Accordingly, the following oxidation
hydroxyl ion to form metallic hydroxides of reactions could take place:
good adsorption properties. The metallic
hydroxide molecules lumped up to form larger
structures that sweep in solution. Fe or SS anode system
(v) Pollutants are adsorbed into the hydroxide For iron, Fe or stainless steel, SS electrodes, the fol-
structures to form larger aggregates. lowing cell reactions are involved in basic
(vi) Pollutants could be converted to less toxic conditions:[47,60,128]
forms by possible redox reactions. Anode:
(vii) The aggregates are then removed by flotation by
hydrogen and oxygen bubbles which move FeðsÞ ! Feþ2 ðaqÞ þ 2e (1)
upward in the liquid phase or get precipitated if Cathode:
they have relatively high density compared with
the medium. 2H2 OðlÞ þ 2e ! H2 ðgÞ þ 2OH ðaqÞ (2)
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
Precipitation:
These successive steps could be explained by Fig. 1 which Feþ2 ðaqÞ þ 2HO ðaqÞ ! FeðOHÞ2 ðsÞ # (3)
highlights the complex nature and the interplay between
the steps of the EC process. Figure 1 indicates the complex Overall:
nature of the EC process with a multitude of mechanisms FeðsÞ þ 2H2 OðlÞ ! FeðOHÞ2 ðsÞ # þH2 ðgÞ (4)
operating synergistically to remove contaminants from
In acidic conditions, the following reactions take place
wastewater.[122] It should be noted that there exist a
Anode:
wide variety of perspective views in the literature about
the exact mechanism of the EC processes. For this reason, 4FeðsÞ ! 4Feþ2 ðaqÞ þ 8e (5)
a systematic holistic approach is needed to fully under-
Precipitation:
stand EC mechanism and its controlling parameters. This
will enable the design of an optimum process and a prior 4Feþ2 ðsÞ þ 10H2 OðlÞ þ 10O2 ðgÞ ! 4FeðOHÞ3 ðsÞ
prediction of the treatment of any pollutant.[121] # þ8Hþ ðaqÞ (6)
The oxidation reactions that take place on the
sacrificial electrode depend on the anode material. As Cathode:
shown in Table 3, the majority of researches utilize 8Hþ ðaqÞ þ 8e ðaqÞ ! 4H2 ðgÞ (7)
anodes made of Al or Al alloy,[123] Fe, and stainless
steel (SS). Some researches utilize magnesium[124] or Overall:
magnesium-based alloy anode,[81,125] copper,[126,127] 4FeðsÞ þ 10H2 OðlÞ þ 10O2 ðgÞ ! 4FeðOHÞ3 ðsÞ
# þ4H2 ðgÞ (8)
where (aq) is aqueous, (l) is liquid, and (s) is solid.
Al anode system
The redox reactions in case of aluminum electrode systems
in basic conditions can be summarized as follows:[60]
Anode:
AlðsÞ ! Alþ3 ðaqÞ þ 3e (9)
Cathode:
3H2 OðlÞ þ 3e ! 1:5H2 ðgÞ þ 3OH ðaqÞ (10)
Precipitation:
Alþ3 ðaqÞ þ 3HO ðaqÞ ! AlðOHÞ3 ðsÞ # (11)
Figure 1. (a) Schematic diagram of an EC cell showing the main Overall:
reactions involved in the EC process, possessing a carbonaceous
material cathode.[121] AlðsÞ þ 3H2 OðlÞ ! AlðOHÞ3 ðsÞ # þ1:5H2 ðgÞ (12)
2654 Z. AL-QODAH AND M. AL-SHANNAG
Table 5. Kinetic models used to describe metal ion removal by to a monolayer formation of the adsorbate ions on the
electrocoagulation. adsorbent surface. The general Langmuir model can be
Anode Pollutant Kinetic model References defined as:[152]
Fe Cu2+, Ni2+, and Zn2+ Pseudo-first-order [47]
Mg Pb+2 Second-order [111]
Hg=2, Ni+2, and Pb+2
q m Ka C e
Mg Second-order [81] qe ¼ (34)
Mg Cu+2 Second-order [133] ð1 þ Ka Ce Þ
Mg Cd+2 Second-order [124]
Fe In+ Second-order [143]
Al, Fe As First-order [144] where qm is the maximum adsorption capacity at cer-
SS Ni+2, Zn+2 Pseudo-first-order [145] tain conditions (mg/g), Ka is the Langmuir model con-
Al Mn+2, Co+2 First-order [146]
Al, Fe Pb+2, Ni+2, and Cu+2 Pseudo-first-order [147] stant (L/mg).[82] In addition, Ka is also equal to the
Fe As Pseudo-second-order [148] ratio of adsorption/desorption rates. Linearization of
Eq. (34) gives
EC process. This is attributed to the different properties Ce 1 Ce
of the coagulant ion and the nature of the pollutants in ¼ þ (35)
qe Ka qm qm
addition to the operating parameter. It should be noted
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
that the model constants usually vary with the current A plot of Ce/qe against Ce gives a straight line, with 1/qm
density. For this reason, it is difficult to compare the and 1/Kaqm values being the slope and an intercept, respec-
model constants without referring to the current den- tively. If qm values increase as the temperature increases,
sity applied. this indicates that the adsorption process is favorable and
endothermic in nature. An opposite behavior indicates that
the adsorption process is exothermic.[153]
Isotherm models Among the previous studies, several authors
reported that Freundlich isotherm model fits satisfacto-
Adsorption isotherm models are being applied to pre- rily their results.[47,111] On the other hand, other studies
dict the capacity of adsorbents and to further explore reported that Langmuir isotherm model better fits their
the adsorption mechanism.[14,149] Among the various results.[124,144] Actually, some studies found that both
isotherm models, Freundlich and Langmuir isotherms models were able to fit their results.[83,114,133] It should
are the most popular models used to describe the be noted that the isotherm models constant like qm
adsorption step in the EC process.[81,111] usually vary with the current density. For this reason,
Freundlich model is usually used to describe the it is difficult to compare these constants without refer-
bioadsorption of adsorbate ions onto solid bioadsor- ring to the current density applied.
bent. In this model, it is assumed that the solid surface
is heterogeneous and has non-equivalent binding sites.
The general Freundlich model can be defined as:[150]
Thermodynamic models
1=
qe ¼ KF Ce n (32) Temperature variation plays an important role in the
where Ce is the metal ion concentration at equilibrium bioadsorption process of metal ions.[13] Consequently,
(mg/L), KF is the Freundlich constant relating to the any change in the solution temperature will influence a
bioadsorption capacity, and n is a constant that mea- change in the adsorbed quantity of the ions by the
sures the bioadsorption intensity and how favorable is adsorbent.[14] Accordingly, the effect of temperature on
the adsorption process. In addition, n varies with the the thermodynamic parameters such as Gibbs free energy
heterogeneity of the adsorbent.[151] The linear form of of activation, ΔG°, enthalpy of activation, ΔH°, and entropy
Freundlich model is of activation, ΔS°, should be determined.[137,154] If Gibbs
free energy, ΔG°, has a negative value, the process will be
1 spontaneous and feasible. In addition, if ΔG° decreases as
log qe ¼ log KF þ log Ce (33)
n the temperature increases, this indicates that the adsorp-
If the data fit this model, then a plot of lnqe versus lnCe tion capacity will increase.[130] On the other hand, if ΔH°
will give a straight line with 1/n as the slope and lnKF as has positive or negative values, the process is endothermic
the intercept. If the values of n > 1, this indicates or exothermic, respectively. Finally, negative ΔS° means
favorable adsorption conditions. that the adsorbed metal ions are stable on the active sites.
On the other hand, Langmuir model assumes that The energy of activation, E (J/mol), of metal ion by
the adsorption active sites are evenly distributed on the an electro-coagulant can be expressed using the second-
adsorbent surface. This finite distribution usually leads order kinetic constant using Arrhenius equation:[114]
SEPARATION SCIENCE AND TECHNOLOGY 2657
where CAe (mg/L) is the amount of adsorbed heavy Despite that, these insoluble electrodes are easily avail-
metal ions at equilibrium, and Ce (mg/L) is the ions able, they are cost-effective and show high oxygen
equilibrium concentration. evolution over-potential and low durability. Actually,
Using Eq. (37), a plot of lnKd versus 1/T will give a the most common used metallic electrode materials are
straight line of a slope equals –ΔH°/R, and an intercept iron in form of mild steel (MS) or stainless steel (SS),
of ΔS°/R. Note that ΔG° can be estimated using:[155] aluminum (Al), zinc (Zn), copper (Cu), and magne-
ΔGo ¼ RT ln Kd (39) sium (Mg). These elements are different in many che-
mical and physical properties such as oxidation
Actually, the researches that have considered the ther- potential, ion size and charge, migration speed in the
modynamic parameters during EC processes are lim- solution, the polarity of the ion–OH bond, and the
ited. Vasudevan et al.[124] found that there was a hydroxide compound structure and size. Since the
temperature enhancement for the adsorption capacity metal hydroxide will play the role of an adsorbent
of the electro-coagulant, Mg(OH)2, toward mercury, coagulant in the EC process, these differences lead to
lead, and nickel during the EC process. They referred differences in the adsorption capabilities of each
this result to the possible enlargement of the pore size hydroxide.[47] In addition, these metals are also differ-
and or the possible thermal activation of the adsorbent ent in their cost, regeneration, and toxicity or impact
surface.[156] Kamaraj et al.[111] calculated the thermo- on the environment. For this reason, it is of primary
dynamic parameters for the adsorption of copper by importance to consider these differences in choice of an
the electro-coagulant, Mg(OH)2, ΔG°, ΔH°, and ΔS° at electrode material to reach an efficient design of the
different temperatures. They reported that ΔG° was electrochemical unit for wastewater treatment by EC.
negative and decreases from −726 to −2903 as the
temperature increases from 313 to 343 K, indicating Electrode spacing
an increase in the adsorption capacity with tempera- Electrode spacing is an important parameter affecting
ture. Subsequently, Kamaraj et al.[133] calculated the the performance of an EC process. It affects the elec-
thermodynamic parameters for the same adsorbent trostatic attraction, the residence time between the
for lead and reported similar results. electrodes, and consequently, the turbulence, mass
transfer, and removal efficiency in the cell.
Accordingly, there is an optimum electrode spacing
Parameters affecting the performance of
at which a maximum pollutant removal efficiency is
electrocoagulation processes
obtained.[159] At very small electrode spacing, the elec-
There are several key parameters that influence the trostatic attraction between the metal hydroxide flocks
performance of any EC process efficiency in removing will be high. This leads to degradation of the flocks
metal ions or other pollutants from wastewater.[138] due to the intensive collision and attrition between
These parameters can be classified into two categories them.[160] Asselin et al.[161] reported that an electrode
including design parameters and operational para- spacing less than 10 mm will reduce the swirling
meters. The most important design parameters are velocity of the solution between the electrodes, and
related to the electrochemical cell material and geome- this will affect the pollutant removal efficiency. As the
try such as electrode material, electrode surface and electrode spacing increases, the electrostatic attraction
2658 Z. AL-QODAH AND M. AL-SHANNAG
decreases, leading to a slower movement of the gen- mercury, lead, and nickel. It is clear that as the distance
erated ions and flocks. This behavior provides more increases, the removal efficiency decreases.
time for the agglomeration of produced metal hydro-
xide to form stable flocks with less degradation, result- Electrode arrangement
ing in an increase in the pollutant removal efficiency A simple electrochemical cell is usually composed of an
from the solution. This increase in the removal effi- anode and a cathode. However, in practical wastewater
ciency continues until reaching the optimum electrode treatment processes, where a huge electrode surface area
spacing. Beyond this value and as the electrode spa- is required, the EC cells contain many anodes and cathodes
cing increases, the electrostatic attraction decreases arranged in different ways as shown in Fig. 3. As shown in
and the travel time of the ions increases leading to Fig. 3, there are three different electrode arrangements in a
less flocks formation and the removal efficiency complex EC cell system. These arrangements are:
decreases.
The Ohmic potential drop or IR drop is the (a) Monopolar-parallel electrodes (MP-P, Fig. 3a). In
difference in potential required to transfer the ions this arrangement, the EC cell consists of cathodes
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
through the solution. This drop which resulted from and anodes connected to each other and to the
the solution resistance usually influences the elec- external DC supply. This configuration results in a
trochemical performance. It can be expressed as:[80] relatively low potential difference since the current
is divided between the electrodes.[138] In this
ID
ηIR ¼ (40) arrangement, each pair of cathode/anode repre-
Ak sents a small electrolytic of the same voltage and
where I is the electrical current (A), D is the distance an additive current.
between electrodes (m); A the active anode surface area (b) Monopolar-series electrodes (MP-S, Fig. 3b). In
(m2); k is the specific conductivity (mS/m). From Eq. this arrangement, each pair of internal sacrificial
(40), it is clear that IR drop increases, as the distance electrodes is just connected to each other resulting
between the electrodes increases. For this reason, the in equal electric current and an additive voltage.
applied voltage should be increased to keep a constant (c) Bipolar-series electrode (BP-S, Fig. 3c). This
current input to the system. Therefore, an optimum arrangement comprises two outer monopolar
distance between the electrodes is recommended to electrodes connected to electric power supply
prevent the increase of IR drop.[162] Figure 2 shows and internal bipolar sacrificial electrode. Each
the effect of inter-electrode distance on the removal of bipolar sacrificial electrode has opposite charges
Figure 2. Effect of inter-electrode distance on the removal of mercury, lead, and nickel. Conditions: solution pH = 7.0; solution
temperature = 305 K; anode, magnesium alloy; cathode, galvanized iron; current density = 0.15 Å/dm2; EC duration = 30 min.[114]
SEPARATION SCIENCE AND TECHNOLOGY 2659
Figure 3. Different electrodes’ arrangement within the electrochemical cell: (a) monopolar electrodes in parallel connections; (b)
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
monopolar electrodes in series connections; and (c) dipolar electrodes in series connections.[163]
on its two sides where metal oxidation takes electrostatic precipitator. They found that punched-
place on the positive side, whereas the negative holes electrodes have discharge current and conse-
side is the place for cathodic reactions.[164] quently higher collection efficiency than the plane
electrode. This behavior can be attributed to the fact
It is clear that the performance of each electrode that the electric field intensity at the edge of
arrangement is different. For example, contrary to punched-holes electrodes is 1.2 times higher than
monopolar electrodes, bipolar electrodes require a that of the plane electrode.
high voltage and a lower current. For this reason, the
choice of the best electrode arrangement is determined
Type of power supply
by the yield, efficiency, and the cost of a particular EC
It has been noticed that most of the published
process. BP-S electrode arrangement is more efficient if
research in the literature dealing with EC cells used
the yield of the process is important rather than the
direct current (DC). It is familiar, however, that DC
cost and efficiency.[165] On the other hand, if the ratio
current causes cathode passivation which means anode
of effectiveness–cost is the important parameter, mono-
oxidation and the formation of an oxide layer on the
polar electrodes are more suitable since it consumes
cathode itself. This phenomenon leads to an increase
relatively low energy and enables a high pollutant
in passive over potential and consequently higher
removal.[166] However, bipolar arrangement needs less
power consumption. For this reason, cathode passiva-
cost for operational maintenance cost forcing a new
tion decreases the current flow in the cell and
cost parameter that should be considered in addition
decreases the EC cell efficiency. Mollah et al.[48,170]
to energy consumption in the selection of the most
reported that AC current increases the electrode life
suitable arrangement.[167]
because cyclic energization decreases the electrode
consumption rate, whereas Eyvaz et al.[171] showed
Electrode shape that the alternating pulsed current (APC) provides
Very limited studies have been performed to test the shorter operation, constant removal efficiency with
effect of electrode shape or orientation on the per- time, and lower cost compared to DC. Vasudevan
formance of the electrochemical cell. In addition, et al.[80] investigated the effect of AC and DC currents
the most common rectangular shape of the electro- on the removal of cadmium from wastewater by EC
des, circular, and cylindrical geometries, punched using Al–Al alloy electrodes. They reported that AC
holes type electrodes are sometimes used. In addi- current reduced the power consumption from 1.002 to
tion, electrodes in few cases are horizontally settled 0.454 kWh/kL, and removal efficiency slightly
in EC cell. It was reported that horizontal electrodes increased from 96.2% to 97.5% for DC and AC cur-
could produce in higher mixing efficiency in batch rent, respectively. Yang et al.[172] reported that the
cells.[168] Kuroda et al.[169] used electrodes with and passivation problem could be reduced in the case of
without punched holes to study the effect of elec- Al or Fe electrodes by the addition of chloride ions to
trode shape on the collector efficiency in an breakdown the oxide layer or by using APC.
2660 Z. AL-QODAH AND M. AL-SHANNAG
EC reactor mode of operation where the EC process is carried out by controlled and/
The modes of operation of an EC reactor can be classi- or varied applied cell voltage. It could vary as a function
fied based on three major distinctions:[173] of amount of coagulant desired to be released in EC
Whether the EC reactor operates in a batch-wise or a reactor. The second mode is often used in electro-
continuous mode. In a batch system, there is a constant oxidation and electro-reduction processes, where there
reactor working volume of wastewater per treatment are no sacrificial electrodes.[176] It should be noted that
cycle with no feed or product stream, as shown in very high current values could enhance secondary reac-
Fig. 4a. On the other hand, in a continuous process tions and consequently negatively affect the EC effi-
there is a continuous stream wastewater feeding to the ciency. In addition, these secondary reactions could
EC cell and continuous output stream of the treated out reverse the colloids charge leading to re-disperse
of the reactor as shown in Fig. 4a.[174] The second them. This process could decrease the coagulant effi-
distinction is whether the feed flow is horizontal or ciency and reduce the electrode lifetime. Harif and
upward.[175] Adin[177] suggested the model shown in Fig. 5, which
The third distinction is whether the aggregated pol- describes how applied electrical current influences the
lutants is separated in situ using flotation or sedimenta-
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
Figure 4. Experimental setup for batch (a), and continuous experiments (b) EC. 1, Power supply; 2, anode; 3, cathode; 4, reactor; 5,
pump; 6, valve; 7, inlet stream; 8, outlet stream; 9, wastewater reservoir tank; 10, filtration tank.[174]
SEPARATION SCIENCE AND TECHNOLOGY 2661
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
Figure 5. Conceptual model predicting flock evolution rate and structure with α as collision efficiency and β as collision
frequency.[177]
Figure 6. Effect of current density on the arsenic removal efficiency (initial arsenic concentration: 50 mg/L, initial pH: 4, and stirring
speed: 150 rpm.[75]
Figure 7. Effect of pH of the solution on the removal of (a) Hg, Ni, and Pb, initial concentration 0.1 mg/L; solution temperature, 305
K; anode, magnesium alloy; cathode, galvanized iron; current density, 0.15 mA/cm2; duration, 30 min.[78] (b) Zn, Cu, Ni, Cr, Cd, and
Co, initial concentration 50 mg/L each; current density, 1.35 mA/cm2; duration, 22.2 min.[114]
Cr(VI) from synthetic solution by EC and conducted process. The used a range of temperature was from
several experiments at different pH values. They 293 to 333 K. They reported that as the temperature
reported that the optimum pH value was 4 (see increased from 293 to 333 K, the boron removal effi-
Fig. 7c). In addition, they noticed that the pH value of ciency increased from 84% to 96%. In addition, Chou
the medium increased with time as a result of hydroxyl and Huang[143] studied the effect of temperature on the
ion (OH–) generation in the medium. removal efficiency indium ion different temperatures of
288, 298, 308, and 318 K (see Fig. 8).
Temperature It is clear in Fig. 8 that the removal efficiency of
In spite the importance of temperature on the perfor- indium ion increases as the time of electrolysis
mance of physiochemical processes such as EC, the increases. Moreover, the removal efficiency after 50
effect of this operational parameter on the removal of min of electrolysis, reached 80.9%, 90.4%, 92.7%, and
metal ions pollutants by EC process has rarely been 94.1% at temperatures of 288, 298, 308, and 318 K,
studied.[143,183] Yilmaz et al.[184] investigated the effect respectively. Chou and Huang[143] analyzed the pro-
of medium temperature on boron removal by EC cess by considering both the indium removal
SEPARATION SCIENCE AND TECHNOLOGY 2663
Agitation
Medium agitation is usually applied in order to
Figure 8. Effect of temperature on the removal efficiency of
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
Initial concentration
Several studies were performed to investigate the effect
of initial ions concentration on the efficiency of the EC
processes.[143,191–193] Thella et al.[191] studied the effect
of arsenic initial concentration on its ion removal effi-
ciency. The results are shown in Fig. 11.
It is evident from Fig. 11 that the removal effi-
ciency is higher at lower initial concentration values.
For example, the removal efficiency of As(III)
decreased from 100% to 43.12% as C0 increases
from 10 to 100 mg/L in a time of 30 min. In addition,
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
voltage = 20 V, temperature = 25°C, electrodes spacing = 2 cm, ior to conventional technologies such as chemical
dosage of NaCl = 100 mg/L, agitation speed = 300 rpm.[143] precipitation. Espinoza-Quiñones et al.[198] applied EC
process to treat tannery effluents and they concluded
that EC is more cost-effective than conventional methods
effluent to dilute the raw wastewater can solve the with relatively high removal efficiencies. Subsequently,
problem and enhances the removal efficiency. Kobya et al.[199] employed a response surface methodol-
Chou and Huang[143] obtained similar results when ogy (RSM) to optimize and evaluate interactions of
they treated a synthetic wastewater containing indium important operational parameters on the treatment effi-
(III) of C0 in the range of 20–100 mg/L. Their results ciency of metal cutting wastewater (MCW). They
shown in Fig. 12 confirm those of Thella et al.[191] and reported that RSM was suitable approach to optimize
they indicate that when indium (III) ion concentration the operating conditions and maximize the removal effi-
increases from 20 to 100 mg/L, the removal efficiency ciencies while keeping minimum operating costs. Similar
after 90 min of electrolysis decreases from 78.3% results were obtained by Bayramoglu et al.[165] who per-
to 49.8%. formed a comparative study between EC and traditional
Dermentzis et al.[193] conducted similar experiments chemical coagulation (CC) processes to determine the
to demonstrate the effect of metal ions concentration rate of electrode consumption and the rate of sludge
using initial concentrations of 100, 200, and 300 mg/L production. They reported that the rate of EC process
of nickel ions and a constant current density of 3 A/m2. was faster and more cost-effective than CC process. In
Contrary to Thella et al.,[191] they concluded that there addition, they found that the EC and CC costs at the
is no direct correlation between metal ion concentra- optimum operating conditions were 0.25 and 0.80 $/m3,
tion and the removal efficiency. This contradiction may respectively. This means that the operating cost for EC
be is referred to the large difference of the concentra- was only around 30% of that CC process.
tion range between the two studies. In addition, they In two successive studies, Kobya et al.[200,201]
reported that the EC process of high ions concentration assessed the efficiency of EC process in the removal of
is more efficient at the beginning than at the end. arsenic from groundwater using Fe ball and plate
anodes and a real dye house wastewater effluent using
Al and Fe, respectively. Kobya et al.[200] reported that
Cost analysis
the removal efficiency and operating cost at the opti-
The operating cost is a fundamental parameter that mum conditions for Fe ball and plate anodes were of
should be considered in any treatment process as it deci- 99.3% and 1.55 $/m3 and 96.9% and 0.10 $/m3, respec-
des the large-scale applicability of that process.[12,47,194] tively. Accordingly, Fe plate anodes in EC process was
Having many alternative treatment processes for the able to provide the WHO limit value. Indeed, it was
removal of heavy metal ions from wastewater, EC is over three times more economical than Fe ball anodes.
necessary to be a cost-effective process to be applied.[195] In another study, Kobya et al.[201] reported that the
Actually, the worldwide unstable energy prices and the operating costs for both Fe and Al electrodes at the
use of electric current as an operating parameter could optimum operating conditions were calculated as 1.562
represent a serious drawback that could discourage the $/m3 for Fe electrode and 1.851 $/m3 for Al electrode.
large-scale application of EC processes.[138] For this rea- Zeboudji et al.[202] reported that they achieved a
son, optimization of the EC process is a vital step to prove removal efficiency of 96% of boron concentration of
2666 Z. AL-QODAH AND M. AL-SHANNAG
0.4 mg/L at a current density of 6 mA/cm2 and pH = 8 Table 6. Removal efficiencies, amounts of electrodes dissolved,
using aluminum electrodes. They carried out a compar- and electrical energy consumptions at different current densi-
ison between monopolar electrocoagulation (MEC) and ties and EC time with solution volume = 600 mL, pH = 9.6, and
electrical conductivity = 8.9 mS/cm.[47]
bipolar electrocoagulation (BEC) using both aluminum
ηexp (%)
and iron electrodes. They found that the BEC process
CD (mA/m2) t (min) E (kWh/m3) mFe (kg/m3) Cr3+ Cu2+ Ni2+ Zn2+
was able to reduce the applied current density com- 2 45 1.57 0.653 52 49 60 55
pared with MEC process. In addition, MEC achieved a 2 60 2.08 0.870 54 52 61 56
3 45 3.52 0.979 75 74 82 80
high level of boron removal to acceptable levels at low 3 60 4.68 1.306 77 75 83 79
cost in a short reaction time. The results presented in 4 45 6.25 1.306 100 96 97 96
4 60 8.33 1.741 100 99 98 99
this study and that of Cheballah et al.[203] revealed that
the EC process can be effectively used for the removal
of color, COD, TOC, and turbidity from textile
wastewater. Finally, the cost of treatment processes is dependent
Al-Shannag et al.[47] reported that at optimum operating on the energy or electricity prices. The use of a sustain-
conditions the energy consumption and amount of dis-
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
simulation, although there are some local discrepancies with those obtained from the lab scale with a maximum
between them near the entrance portion of the EC cell. removal efficiency of 98.4% indicating that the large
These discrepancies could be explained by the fact that scale of EC process is technologically feasible.[124]
the inlet at each turn of cell does not form a complete Finally, Lin et al.[196] designed a pilot-scale process to
flow channel and the EC process is active only in the reclaim domestic grey water, at 28 m3/day, to meet the
region between the electrodes. In addition, the discre- human noncontact usage general guidelines. They
pancies decrease toward the latter parts of the cell.[204] reported that the cost was US $ 0.27/m3 when the treat-
Zolotukhin[207] scaled up an electrocoagulation–flota- ment unit had 8 m2 electrode surface area.
tion system from lab scale to industrial size. They chose
some dimensionless quantities as a scale-up parameters
to ensure correct sizing and proportioning of the indus- Concluding remarks and perspectives
trial reactors. These dimensionless quantities are
Reynolds number (Re), the Froude number (Fr), and In this review, EC process has been demonstrated as a
Weber criteria (We), while the reactor geometry and practical cost-effective technology for heavy metal ions
gas saturation were kept similar. removal from wastewater. The following are the main
Vasudevan et al.[124] designed, fabricated, and oper- concluding remarks and perspectives that could benefit
ated a pilot-plant-scale EC based on lab-scale results researchers in their future work:
previously obtained for the removal of cadmium ions
from wastewater. A solution of 9 L was used for each (1) Advantages of EC processes include the ease of
experiment as the electrolyte. The results were consistent operation, no addition of chemicals, easy
2668 Z. AL-QODAH AND M. AL-SHANNAG
Table 7. Reactor dimensions and operating parameters for management is considered. Therefore, a sustain-
laboratory- and pilot-scale electrocoagulation studies.[204] able end-use of sludge management is essential
Parameter Laboratory scale Pilot scale especially if toxic ions are produced from the
Reactor interior dimension 320 × 180 × 200 100 × 500 × 600 anode such as Cu+2 and Zn+2 to eliminate any
(L × W × H) (mm)
Working electrode dimension 180 × 140 450 × 400 negative impact of this sludge on the environ-
(W × H) (mm) ment. In addition, the sludge management and
–3
Working volume (m3) 8.0 × 10 0.18
Applied current (A) 0.5–2.5 15–25 reuse have become an attractive research area in
Volumetric flow rate (m3/day) 0.12–0.37 1.0–4.0 the last few years, since sludge sometimes con-
Hydraulic retention time (min) 30–100 65–260
Number of channels, min/max 6/14 10/20 tains economically valuable compounds such as
metallic hydroxides.[47]
(4) Most of the performed studies used synthetic
rather than real wastewater. For this reason,
most of the results are ideal since the interfer-
ence of real mater matrix in the results is
excluded. For this reason, research extension
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
systems. These combinations include electrocoa- biosorbents–a review of the recent literature.
gulation–ozone,[209,210] electrocoagulation– Bioresource Technology, 101: 5043–5053.
adsorption processes,[211,212] electrocoagulation- [10] Costa, M. (1997) Toxicity and carcinogenicity of Cr (VI) in
animal models and humans. Critical Reviews in Toxicology,
ultrasound processes,[213] and electrocoagula- 27: 431–442.
tion–pulsed processes.[214,215] [11] Garcia-Reyes, R.B.; Rangel-Mendez, J.R. (2010) Adsorption
(9) Additional reviews are required to discuss and kinetics of chromium (III) ions on agro-waste materials.
compare the performance of EC process on the Bioresource Technology, 101: 8099–8108.
removal of organic pollutants such as [12] Bazrafshan, E.; Mohammadi, L.; Ansari-Moghaddam, A.;
Mahvi, A.H. (2015) Heavy metals removal from aqueous
COD,[203] pesticides,[216] Azo dye,[217] anions
environments by electrocoagulation process–a systema-
such as fluoride,[218,219] and the effect of elec- tic review. Journal of Environmental Health Science and
tric fields on the microorganisms present in Engineering, 13: 1.
various wastewater effluent.[220] This will lead [13] Al-Qodah, Z. (2006) Biosorption of heavy metal ions from
to an overall comparison between the perfor- aqueous solutions by activated sludge. Desalination, 196:
mances of EC process for the treatment of 164–176.
[14] Zalloum, H.M.; Al-Qodah, Z.; Mubarak, M.S. (2008) Copper
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
different types of pollutants including metallic, adsorption on chitosan-derived Schiff bases. Journal of
non-metallic, or organic compounds. Macromolecular Science, Part A, 46: 46–57.
[15] Abdel-Ghani, N.; Hegazy, A.K.; El-Chaghaby, G.; Lima, E.C.
(2009) Factorial experimental design for biosorption of
iron and zinc using Typha domingensis phytomass.
Desalination, 249: 343–347.
ORCID [16] Bernardo, G.-R.-R.; Rene, R.-M.J. (2009) Chromium (III)
uptake by agro-waste biosorbents: chemical characteriza-
Mohammad Al-Shannag http://orcid.org/0000-0003-0085-
tion, sorption–desorption studies, and mechanism.
2089
Journal of Hazardous Materials, 170: 845–854.
[17] Kelly-Vargas, K.; Cerro-Lopez, M.; Reyna-Tellez, S.;
Bandala, E.R.; Sanchez-Salas, J.L. (2012) Biosorption of
heavy metals in polluted water, using different waste
References
fruit cortex. Physics and Chemistry of the Earth, Parts A/
[1] Brillas, E.; Sirés, I.; Oturan, M.A. (2009) Electro-Fenton B/C, 37: 26–29.
process and related electrochemical technologies based [18] Granados-Correa, F.; Serrano-Gómez, J. (2009) CrO4 2− ions
on Fenton’s reaction chemistry. Chemical Reviews, 109: adsorption by Fe-modified pozzolane. Separation Science
6570–6631. and Technology, 44: 924–936.
[2] Jin, W.; Du, H.; Zheng, S.; Zhang, Y. (2016) [19] Singh, K.; Singh, A.; Hasan, S. (2006) Low cost bio-sorbent
Electrochemical processes for the environmental reme- ‘wheat bran’for the removal of cadmium from waste-
diation of toxic Cr (VI): A review. Electrochimica Acta, 191: water: kinetic and equilibrium studies. Bioresource
1044–1055. Technology, 97: 994–1001.
[3] Al-Qodah, Z. (1998) Adsorption of methylene blue with [20] Gadd, G.M. (2010) Metals, minerals and microbes: geo-
diatomite. Journal of Engineering Technology, 17: 128–137. microbiology and bioremediation. Microbiology, 156:
[4] Al-Qodah, Z.; Al-Shannag, M.; Amro, A.; Assiri, E.; Mustafa, 609–643.
B.; Bani-Melhem, K.; Kasrawi, M.A. (2017) Impact of sur- [21] Edokpayi, J.N.; Odiyo, J.O.; Msagati, T.A.; Popoola, E.O.
face modification of green algal biomass by phosphory- (2015) A Novel Approach for the removal of lead (II)
lation on the removal of copper (II) ions from water. ion from wastewater using mucilaginous leaves of dicer-
Turkish Journal of Chemistry, 41: 190–208. iocaryum eriocarpum plant. Sustainability, 7: 14026–
[5] Fu, F.; Wang, Q. (2011) Removal of heavy metal ions from 14041.
wastewaters: a review. Journal of Environmental [22] Öztürk, A. (2007) Removal of nickel from aqueous solu-
Management, 92: 407–418. tion by the bacterium Bacillus thuringiensis. Journal of
[6] Abia, A.; Asuquo, E. (2006) Lead (II) and nickel (II) adsorp- Hazardous Materials, 147: 518–523.
tion kinetics from aqueous metal solutions using chemi- [23] Singh, H.; Rattan, V. (2011) Adsorption of nickel from
cally modified and unmodified agricultural adsorbents. aqueous solutions using low cost biowaste adsorbents.
African Journal of Biotechnology, 5. Water Quality Research Journal of Canada, 46: 239–249.
[7] Malkoc, E.; Nuhoglu, Y. (2006) Removal of Ni (II) ions from [24] Bhattacharya, A.; Mandal, S.; Das, S. (2006) Adsorption of
aqueous solutions using waste of tea factory: adsorption Zn (II) from aqueous solution by using different adsor-
on a fixed-bed column. Journal of Hazardous Materials, bents. Chemical Engineering Journal, 123: 43–51.
135: 328–336. [25] Hussein, H.; Ibrahim, S.F.; Kandeel, K.; Moawad, H. (2004)
[8] Demirbas, A. (2008) Heavy metal adsorption onto agro- Biosorption of heavy metals from waste water using
based waste materials: a review. Journal of Hazardous Pseudomonas sp. Electronic Journal of Biotechnology, 7:
Materials, 157: 220–229. 30–37.
[9] Farooq, U.; Kozinski, J.A.; Khan, M.A.; Athar, M. (2010) [26] Sarı, A.; Tuzen, M. (2009) Biosorption of As (III) and As (V)
Biosorption of heavy metal ions using wheat based from aqueous solution by macrofungus (Inonotus
2670 Z. AL-QODAH AND M. AL-SHANNAG
hispidus) biomass: equilibrium and kinetic studies. influent using electrocoagulation technique. Separation
Journal of Hazardous Materials, 164: 1372–1378. Science and Technology, 48: 673–680.
[27] Pehlivan, E.; Altun, T.; Parlayıcı, S. (2009) Utilization of [42] Al-Shannag, M.; Al-Qodah, Z.; Alananbeh, K.; Bouqellah,
barley straws as biosorbents for Cu 2+ and Pb 2+ ions. N.; Assirey, E.; Bani-Melhem, K. (2014) COD reduction of
Journal of Hazardous Materials, 164: 982–986. baker’s yeast wastewater using batch electrocoagulation.
[28] Opeolu, B.O.; Bamgbose, O.; Arowolo, T.; Adetunji, M. Environmental Engineering and Management Journal, 13:
(2010) Utilization of biomaterials as adsorbents for 3153–3160.
heavy metals removal from aqueous matrices. Scientific [43] Nguyen, T.; Ngo, H.; Guo, W.; Zhang, J.; Liang, S.; Yue, Q.;
Research and Essays, 5: 1780–1787. Li, Q.; Nguyen, T. (2013) Applicability of agricultural
[29] Cerino-Córdova, F.D.J.; García-León, A.; Soto-Regalado, E.; waste and by-products for adsorptive removal of heavy
Sánchez-González, M.; Lozano-Ramírez, T.; García-Avalos, metals from wastewater. Bioresource Technology, 148:
B.; Loredo-Medrano, J. (2012) Experimental design for the 574–585.
optimization of copper biosorption from aqueous solution [44] Salman, M.; Athar, M.; Farooq, U. (2015) Biosorption of
by Aspergillus terreus. Journal of Environmental heavy metals from aqueous solutions using indigenous
Management, 95: S77–S82. and modified lignocellulosic materials. Reviews in
[30] Egila, J.; Dauda, B.; Iyaka, Y.; Jimoh, T. (2011) Agricultural Environmental Science and Bio/Technology, 14: 211–228.
waste as a low cost adsorbent for heavy metal removal [45] Emamjomeh, M.M.; Sivakumar, M. (2009) Review of
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
[57] Uğurlu, M.; Gürses, A.; Doğar, Ç.; Yalçın, M. (2008) The [72] Ucar, C.; Baskan, M.B.; Pala, A. (2013) Arsenic removal
removal of lignin and phenol from paper mill effluents by from drinking water by electrocoagulation using iron
electrocoagulation. Journal of Environmental electrodes. Korean Journal of Chemical Engineering, 30:
Management, 87: 420–428. 1889–1895.
[58] Daneshvar, N.; Oladegaragoze, A.; Djafarzadeh, N. (2006) [73] Flores, J.; Nava, J.L.; Carreño, G. (2014) Arsenic removal
Decolorization of basic dye solutions by electrocoagula- from groundwater by electrocoagulation process in a fil-
tion: an investigation of the effect of operational para- ter-press-type FM01-LC reactor. International Journal
meters. Journal of Hazardous Materials, 129: 116–122. Electrochemical Sciences, 9: 6658.
[59] Esfandyari, Y.; Mahdavi, Y.; Seyedsalehi, M.; Hoseini, M.; [74] Parga, J.; Valenzuela, J.; Vazquez, V.; Rodriguez, M.;
Safari, G.H.; Ghozikali, M.G.; Kamani, H.; Jaafari, J. (2015) Munive, G. (2014) Thermodynamic study for arsenic
Degradation and biodegradability improvement of the removal from freshwater by using electrocoagulation
olive mill wastewater by peroxi-electrocoagulation/elec- process. Advances in Chemical Engineering and Science,
trooxidation-electroflotation process with bipolar alumi- 4: 548.
num electrodes. Environmental Science and Pollution [75] Can, B.Z.; Boncukcuoglu, R.; Yilmaz, A.E.; Fil, B.A. (2014)
Research, 22: 6288–6297. Effect of some operational parameters on the arsenic
[60] Pulkka, S.; Martikainen, M.; Bhatnagar, A.; Sillanpää, M. removal by electrocoagulation using iron electrodes.
(2014) Electrochemical methods for the removal of anio- Journal of Environmental Health Science and Engineering,
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
[87] Vasudevan, S.; Lakshmi, J.; Sozhan, G. (2012) [103] Keshmirizadeh, E.; Yousefi, S.; Rofouei, M.K. (2011) An
Electrocoagulation studies on the removal of copper investigation on the new operational parameter effective
from water using mild steel electrode. Water in Cr (VI) removal efficiency: A study on electrocoagula-
Environment Research, 84: 209–219. tion by alternating pulse current. Journal of Hazardous
[88] Golder, A.; Samanta, A.; Ray, S. (2007) Removal of triva- Materials, 190: 119–124.
lent chromium by electrocoagulation. Separation and [104] Vasudevan, S.; Lakshmi, J.; Sozhan, G. (2011) Studies on
Purification Technology, 53: 33–41. the Al–Zn–In-alloy as anode material for the removal of
[89] Golder, A.K.; Samanta, A.N.; Ray, S. (2007) Trivalent chro- chromium from drinking water in electrocoagulation pro-
mium removal by electrocoagulation and characteriza- cess. Desalination, 275: 260–268.
tion of the process sludge. Journal of Chemical [105] Martínez-Delgadillo, S.; Mendoza-Escamilla, V.; Mollinedo-
Technology and Biotechnology, 82: 496–503. Ponce, H.; Puebla, H.; Méndez-Contreras, J. (2010) Effect
[90] Akbal, F.; Camcı, S. (2012) Treatment of metal plating of the ultrasonic irradiation on the Cr (VI) electroreduc-
wastewater by electrocoagulation. Environmental tion process in a tubular electrochemical flow reactor.
Progress & Sustainable Energy, 31: 340–350. Industrial & Engineering Chemistry Research, 50: 2501–
[91] Shahriari, T.; Bidhendi, G.N.; Mehrdadi, N.; Torabian, A. 2508.
(2014) Removal of chromium (III) from wastewater by [106] Barrera-Díaz, C.; Lugo-Lugo, V.; Roa-Morales, G.;
electrocoagulation method. KSCE Journal of Civil Natividad, R.; Martínez-Delgadillo, S. (2011) Enhancing
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
[118] Nouri, J.; Mahvi, A.; Bazrafshan, E. (2010) Application of [133] Kamaraj, R.; Ganesan, P.; Lakshmi, J.; Vasudevan, S. (2013)
electrocoagulation process in removal of zinc and copper Removal of copper from water by electrocoagulation pro-
from aqueous solutions by aluminum electrodes. cess—effect of alternating current (AC) and direct current
International Journal of Environmental Research, 4: 201– (DC). Environmental Science and Pollution Research, 20:
208. 399–412.
[119] Fernandes, A.; Pacheco, M.; Ciríaco, L.; Lopes, A. (2015) [134] Lagergren, S. (1898) Zur Theorie Der Sogenannten
Review on the electrochemical processes for the treat- Absorption Gelöster Stoffe. PA Norstedt & söner:
ment of sanitary landfill leachates: present and future. Stockholm, Sweden.
Applied Catalysis B: Environmental, 176: 183–200. [135] Marín, A.P.; Ortuno, J.; Aguilar, M.; Meseguer, V.; Saez, J.;
[120] Cañizares, P.; Louhichi, B.; Gadri, A.; Nasr, B.; Paz, R.; Lloréns, M. (2010) Use of chemical modification to deter-
Rodrigo, M.; Saez, C. (2007) Electrochemical treatment mine the binding of Cd (II), Zn (II) and Cr (III) ions by
of the pollutants generated in an ink-manufacturing orange waste. Biochemical Engineering Journal, 53: 2–6.
process. Journal of Hazardous Materials, 146: 552–557. [136] Al-Shawabkah, R.; Al-Qodah, Z.; Al-Bsoul, A. (2015) Bio-
[121] Holt, P.K. (2002) Electrocoagulation: unravelling and adsorption of triadimenol pesticide from aqueous solu-
synthesising the mechanisms behind a water treatment tions using activated sludge of dairy plants. Desalination
process. PhD thesis, The University of Sydney. and Water Treatment, 53: 2555–2564.
[122] Malkin, V. (2003) Electrolytic effluent treatment. Chemical [137] Das, N.; Vimala, R.; Karthika, P. (2008) Biosorption of
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
and Petroleum Engineering, 39: 46–50. heavy metals-An overview. Indian Journal of
[123] Fekete, É.; Lengyel, B.; Cserfalvi, T.; Pajkossy, T. (2016) Biotechnology, 7: 159–169.
Electrochemical dissolution of aluminium in electrocoa- [138] Moussa, D.T.; El-Naas, M.H.; Nasser, M.; Al-Marri, M.J.
gulation experiments. Journal of Solid State (2016) A Comprehensive Review of Electrocoagulation for
Electrochemistry, 20: 3107–3114. Water Treatment: Potentials and Challenges. Journal of
[124] Vasudevan, S.; Lakshmi, J.; Packiyam, M. (2010) environmental management, 186: 24–41.
Electrocoagulation studies on removal of cadmium [139] Zeldowitsch, J. (1934) Über den mechanismus der kata-
using magnesium electrode. Journal of Applied lytischen oxydation von CO an MnO2. Acta Physicochim.
Electrochemistry, 40: 2023–2032. URSS, 1: 364–449.
[125] Oumar, D.; Patrick, D.; Gerardo, B.; Rino, D.; Ihsen, B.S. [140] Chien, S.; Clayton, W. (1980) Application of Elovich equa-
(2016) Coupling biofiltration process and electrocoagula- tion to the kinetics of phosphate release and sorption in
tion using magnesium-based anode for the treatment of soils. Soil Science Society of America Journal, 44: 265–268.
landfill leachate. Journal of Environmental Management, [141] Yılmaz, A.E.; Boncukcuoğlu, R.; Kocaker, M.M.;
181: 477–483. Kocadağistan, E. (2008) An empirical model for kinetics
[126] Prajapati, A.K.; Chaudhari, P.K.; Pal, D.; Chandrakar, A.; of boron removal from boroncontaining wastewaters by
Choudhary, R. (2016) Electrocoagulation treatment of the electrocoagulation method in a batch reactor.
rice grain based distillery effluent using copper electrode. Desalination, 230: 288–297.
Journal of Water Process Engineering, 11: 1–7. [142] Xi, Y.; Luo, Y.; Luo, J.; Luo, X. (2015) Removal of Cadmium
[127] Ali, I.; Asim, M.; Khan, T. (2013) Arsenite removal from (II) from Wastewater Using Novel Cadmium Ion-
water by electro-coagulation on zinc–zinc and copper– Imprinted Polymers. Journal of Chemical & Engineering
copper electrodes. International Journal of Environmental Data, 60: 3253–3261.
Science and Technology, 10: 377–384. [143] Chou, W.-L.; Huang, Y.-H. (2009) Electrochemical removal
[128] Al-Shannag, M.; Lafi, W.; Bani-Melhem, K.; Gharagheer, F.; of indium ions from aqueous solution using iron electro-
Dhaimat, O. (2012) Reduction of COD and TSS from paper des. Journal of Hazardous Materials, 172: 46–53.
industries wastewater using electro-coagulation and che- [144] Balasubramanian, N.; Kojima, T.; Srinivasakannan, C. (2009)
mical coagulation. Separation Science and Technology, 47: Arsenic removal through electrocoagulation: Kinetic and
700–708. statistical modeling. Chemical Engineering Journal, 155:
[129] Al-Shannag, M.; Al-Qodah, Z.; Nawasreh, M.; Al- 76–82.
Hamamreh, Z.; Bani-Melhem, K.; Alkasrawi, M. (2017) On [145] Kabdaşlı, I.; Arslan, T.; Ölmez-Hancı, T.; Arslan-Alaton, I.;
the performance of Ballota Undulata biomass for the Tünay, O. (2009) Complexing agent and heavy metal
removal of cadmium (II) ions from water. Desalination removals from metal plating effluent by electrocoagula-
and Water Treatment, 67: 223–230. tion with stainless steel electrodes. Journal of Hazardous
[130] Al-Qodah, Z.; Shawaqfeh, A.; Lafi, W. (2007) Two-resis- Materials, 165: 838–845.
tance mass transfer model for the adsorption of the [146] Shafaei, A.; Rezaie, M.; Nikazar, M. (2011) Evaluation of
pesticide deltamethrin using acid treated oil shale ash. Mn 2+ and Co 2+ removal by electrocoagulation: A case
Adsorption, 13: 73–82. study. Chemical Engineering and Processing: Process
[131] Al-Qodah, Z.; Al-Shannag, M.; Bani-Melhem, K.; Assirey, E.; Intensification, 50: 1115–1121.
Alananbeh, K.; Bouqellah, N. (2015) Biodegradation of [147] Rehman, A.; Kimb, M.; Reverberic, A.; Fabianoa, B. (2015)
olive mills wastewater using thermophilic bacteria. Operational parameter influence on heavy metal removal
Desalination and Water Treatment, 56: 1908–1917. from metal plating wastewater by electrocoagulation
[132] Gupta, V.K.; Jain, C.; Ali, I.; Sharma, M.; Saini, V. (2003) process, 43: 2283–9216.
Removal of cadmium and nickel from wastewater using [148] Kobya, M.; Demirbas, E.; Ulu, F. (2016) Evaluation of
bagasse fly ash—a sugar industry waste. Water Research, operating parameters with respect to charge loading on
37: 4038–4044. the removal efficiency of arsenic from potable water by
2674 Z. AL-QODAH AND M. AL-SHANNAG
electrocoagulation. Journal of Environmental Chemical [166] Naje, A.S.; Abbas, S.A. (2013) Combination of electro-
Engineering, 4: 1484–1494. coagulation and electro-oxidation processes of textile
[149] Argun, M.E.; Dursun, S. (2006) Removal of heavy metal waste waters treatment. Civ Environment Research, 3:
ions using chemically modified adsorbents. Journal 63–73.
International Environment Applications Sciences, 1: 27–40. [167] Kobya, M.; Can, O.T.; Bayramoglu, M. (2003) Treatment of
[150] Freundlich, H. (1906) Over the adsorption in solution. textile wastewaters by electrocoagulation using iron and
Journal Physical Chemical, 57: 1100–1107. aluminum electrodes. Journal of Hazardous Materials,
[151] Wang, J.; Chen, C. (2009) Biosorbents for heavy metals 100: 163–178.
removal and their future. Biotechnology Advances, 27: [168] Fouad, Y.; Konsowa, A.; Farag, H.; Sedahmed, G. (2009)
195–226. Performance of an electrocoagulation cell with horizon-
[152] Langmuir, I. (1916) The constitution and fundamental tally oriented electrodes in oil separation compared to a
properties of solids and liquids. Part I. Solids. Journal of cell with vertical electrodes. Chemical Engineering Journal,
the American Chemical Society, 38: 2221–2295. 145: 436–440.
[153] Tong, K.; Kassim, M.J.; Azraa, A. (2011) Adsorption of copper [169] Kuroda, Y.; Kawada, Y.; Takahashi, T.; Ehara, Y.; Ito, T.;
ion from its aqueous solution by a novel biosorbent Uncaria Zukeran, A.; Kono, Y.; Yasumoto, K. (2003) Effect of elec-
gambir: Equilibrium, kinetics, and thermodynamic studies. trode shape on discharge current and performance with
Chemical Engineering Journal, 170: 145–153. barrier discharge type electrostatic precipitator. Journal
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
[154] Al-Qodah, Z.; Lafi, W. (2003) Adsorption of reactive dyes of Electrostatics, 57: 407–415.
using shale oil ash in fixed beds. Journal of Water Supply: [170] Mollah, M.Y.; Morkovsky, P.; Gomes, J.A.; Kesmez, M.;
Research and Technology-AQUA, 52: 189–198. Parga, J.; Cocke, D.L. (2004) Fundamentals, present and
[155] Gupta, V.K.; Ali, I. (2001) Removal of DDD and DDE from future perspectives of electrocoagulation. Journal of
wastewater using bagasse fly ash, a sugar industry waste. Hazardous Materials, 114: 199–210.
Water Research, 35: 33–40. [171] Eyvaz, M.; Kirlaroglu, M.; Aktas, T.S.; Yuksel, E. (2009) The
[156] Vasudevan, S.; Lakshmi, J.; Sozhan, G. (2010) Studies on effects of alternating current electrocoagulation on dye
the removal of arsenate by electrochemical coagulation removal from aqueous solutions. Chemical Engineering
using aluminum alloy anode. Clean–Soil, Air, Water, 38: Journal, 153: 16–22.
506–515. [172] Yang, Z.-H.; Xu, H.-Y.; Zeng, G.-M.; Luo, Y.-L.; Yang, X.;
[157] Hakizimana, J.N.; Gourich, B.; Chafi, M.; Stiriba, Y.; Vial, C.; Huang, J.; Wang, L.-K.; Song, P.-P. (2015) The behavior of
Drogui, P.; Naja, J. (2017) Electrocoagulation process in dissolution/passivation and the transformation of passive
water treatment: A review of electrocoagulation model- films during electrocoagulation: influences of initial pH,
ing approaches. Desalination, 404: 1–21. Cr (VI) concentration, and alternating pulsed current.
[158] Burns, S.; Yiacoumi, S.; Tsouris, C. (1997) Microbubble Electrochimica Acta, 153: 149–158.
generation for environmental and industrial separations. [173] Holt, P.K.; Barton, G.W.; Mitchell, C.A. (2005) The future
Separation and Purification Technology, 11: 221–232. for electrocoagulation as a localised water treatment
[159] Khandegar, V.; Saroha, A.K. (2013) Electrocoagulation for technology. Chemosphere, 59: 355–367.
the treatment of textile industry effluent–A review. [174] Petsriprasit, C.; Namboonmee, J.; Hunsom, M. (2010)
Journal of Environmental Management, 128: 949–963. Application of the electrocoagulation technique for treat-
[160] Daneshvar, N.; Sorkhabi, H.A.; Kasiri, M. (2004) ing heavy metals containing wastewater from the pick-
Decolorization of dye solution containing Acid Red 14 ling process of a billet plant. Korean Journal of Chemical
by electrocoagulation with a comparative investigation Engineering, 27: 854–861.
of different electrode connections. Journal of Hazardous [175] Jiang, J.-Q.; Graham, N.; André, C.; Kelsall, G.H.; Brandon,
Materials, 112: 55–62. N. (2002) Laboratory study of electro-coagulation–flota-
[161] Asselin, M.; Drogui, P.; Benmoussa, H.; Blais, J.-F. (2008) tion for water treatment. Water Research, 36: 4064–4078.
Effectiveness of electrocoagulation process in removing [176] Ruotolo, L.; Gubulin, J. (2011) A mathematical model to
organic compounds from slaughterhouse wastewater predict the electrode potential profile inside a polyani-
using monopolar and bipolar electrolytic cells. line-modified reticulate vitreous carbon electrode operat-
Chemosphere, 72: 1727–1733. ing in the potentiostatic reduction of Cr (VI). Chemical
[162] Nasrullaha, M.; Singh, L.; Zularisam, A.W. (2012) Engineering Journal, 171: 1170–1177.
Treatment of sewage by electrocoagulation and the [177] Harif, T.; Adin, A. (2011) Size and structure evolution of
effect of high current density. Energy Environment kaolin–Al (OH) 3 flocs in the electroflocculation process: a
Engine Journal, 1: 27–31. study using static light scattering. Water Research, 45: 6195–
[163] Pretorius, W.; Johannes, W.; Lempert, G. (1991) 6206.
Electrolytic iron flocculant production with a bipolar [178] Basha, C.A.; Bhadrinarayana, N.; Anantharaman, N.;
electrode in series arrangement. Water S. A., 17: 133–138. Begum, K.M.S. (2008) Heavy metal removal from copper
[164] Demirci, Y.; Pekel, L.C.; Alpbaz, M. (2015) Investigation of smelting effluent using electrochemical cylindrical flow
Different Electrode Connections in Electrocoagulation of reactor. Journal of Hazardous Materials, 152: 71–78.
Textile Wastewater Treatment. International Journal [179] Khosa, M.K.; Jamal, M.A.; Hussain, A.; Muneer, M.; Zia, K.
Electrochemical Sciences, 10: 2685–2693. M.; Hafeez, S. (2013) Efficiency of Aluminum and Iron
[165] Bayramoglu, M.; Eyvaz, M.; Kobya, M. (2007) Treatment of Electrodes for the Removal of heavy metals [(Ni (II), Pb
the textile wastewater by electrocoagulation: economical (II), Cd (II)] by Electrocoagulation Method. Journal of the
evaluation. Chemical Engineering Journal, 128: 155–161. Korean Chemical Society, 57: 316–321.
SEPARATION SCIENCE AND TECHNOLOGY 2675
[180] Ihou, M.; Abida, F.; Hatim, Z.; Kheribech, A. (2016) Removal [196] Lin, C.-J.; Lo, S.-L.; Kuo, C.-Y.; Wu, C.-H. (2005) Pilot-scale
of heavy metals from synthetic solution by electrocoagu- electrocoagulation with bipolar aluminum electrodes for
lation. Mediterranean Journal of Chemistry, 5: 521–527. on-site domestic greywater reuse. Journal of
[181] ASLa, D.M.K.; Moshtaghi, M.; Hassani, D. (2014) Efficiency Environmental Engineering, 131: 491–495.
evaluation of electrocoagulation process for removal of chro- [197] Rodriguez, J.; Stopić, S.; Krause, G.; Friedrich, B. (2007)
mium (heavy metal) from municipal and industrial waste- Feasibility assessment of electrocoagulation towards a
water. Indian Journal of Sciences Research, 7: 1258–1268. new sustainable wastewater treatment. Environmental
[182] Moreno-Casillas, H.A.; Cocke, D.L.; Gomes, J.A.; Science and Pollution Research-International, 14: 477–482.
Morkovsky, P.; Parga, J.; Peterson, E. (2007) [198] Espinoza-Quiñones, F.R.; Fornari, M.M.; Módenes, A.N.;
Electrocoagulation mechanism for COD removal. Palácio, S.M.; Da Silva, F.G.; Szymanski, N.; Kroumov, A.
Separation and Purification Technology, 56: 204–211. D.; Trigueros, D.E. (2009) Pollutant removal from tannery
[183] Naje, A.S.; Chelliapan, S.; Zakaria, Z.; Ajeel, M.A.; Alaba, P.A. A effluent by electrocoagulation. Chemical Engineering
review of electrocoagulation technology for the treatment Journal, 151: 59–65.
of textile wastewater. Reviews in Chemical Engineering, 33: [199] Kobya, M.; Demirbas, E.; Bayramoglu, M.; Sensoy, M.
263–292. (2011) Optimization of electrocoagulation process for
[184] Yilmaz, A.E.; Boncukcuoğlu, R.; Kocakerim, M.M.; Yilmaz, the treatment of metal cutting wastewaters with
M.T.; Paluluoğlu, C. (2008) Boron removal from geother- response surface methodology. Water, Air, & Soil
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
[210] García-Orozco, V.; Barrera-Díaz, C.; Roa-Morales, G.; Dye Wastewater Treatment, in: advanced Materials
Linares-Hernández, I. (2016) A Comparative Research. Transactions Technical Publication, 233: 444–451.
Electrochemical-Ozone Treatment for Removal of [216] Behloul, M.; Grib, H.; Drouiche, N.; Abdi, N.; Lounici,
Phenolphthalein. Journal of Chemistry, 1: 1–9. H.; Mameri, N. (2013) Removal of malathion pesticide
[211] Ouaissa, Y.A.; Chabani, M.; Amrane, A.; Bensmaili, A. from polluted solutions by electrocoagulation: model-
(2013) Removal of Cr (VI) from model solutions by a ing of experimental results using response surface
combined electrocoagulation sorption process. Chemical methodology. Separation Science and Technology, 48:
Engineering Technology, 36: 147–155. 664–672.
[212] Bellebia, S.; Kacha, S.; Bouyakoub, A.Z. (2012) [217] Lemlikchi, W.; Khaldi, S.; Mecherri, M.; Lounici, H.;
Experimental investigation of chemical oxygen demand Drouiche, N. (2012) Degradation of disperse red 167
and turbidity removal from cardboard paper mill efflu- azo dye by bipolar electrocoagulation. Separation
ents using combined electrocoagulation and adsorption Science and Technology, 47: 1682–1688.
processes. Environmental Progress & Sustainable Energy, [218] Aoudj, S.; Khelifa, A.; Drouiche, N.; Hecini, M. (2013) HF
31: 361–370. wastewater remediation by electrocoagulation process.
[213] Asaithambi, P.; Aziz, A.R.A.; Sajjadi, B.; Daud, W.M.A.B.W. Desalination and Water Treatment, 51: 1596–1602.
(2016) Sono assisted electrocoagulation process for the [219] Palahouane, B.; Drouiche, N.; Aoudj, S.; Bensadok, K.
removal of pollutant from pulp and paper industry efflu- (2015) Cost-effective electrocoagulation process for the
Downloaded by [Professor Mohammad Al-Shannag] at 10:40 08 November 2017
ent. Environmental Science and Pollution Research, 24: remediation of fluoride from pretreated photovoltaic
5168–5178. wastewater. Journal of Industrial and Engineering
[214] Ren, M.; Song, Y.; Xiao, S.; Zeng, P.; Peng, J. (2011) Chemistry, 22: 127–131.
Treatment of berberine hydrochloride wastewater by [220] Boudjema, N.; Drouiche, N.; Abdi, N.; Grib, H.; Lounici, H.;
using pulse electro-coagulation process with Fe elec- Pauss, A.; Mameri, N. (2014) Treatment of Oued El
trode. Chemical Engineering Journal, 169: 84–90. Harrach river water by electrocoagulation noting the
[215] Chen, Y.M.; Zhou, B.X.; Li, L.H.; Song, Y.H.; Li, J.H.; Liu, Y.B.; effect of the electric field on microorganisms. Journal of
Cai, W.M. (2011) Application of Pulse Electrocoagulation to the Taiwan Institute of Chemical Engineers, 45: 1564–1570.