Accepted Manuscript

Title: Electrocoagulation-flocculation as a low-cost process

for pollutants removal from urban wastewater

Author: M. Elazzouzi Kh. Haboubi M.S. Elyoubi

PII: S0263-8762(16)30429-4
DOI: http://dx.doi.org/doi:10.1016/j.cherd.2016.11.011
Reference: CHERD 2482

To appear in:

Received date: 8-8-2016

Revised date: 25-10-2016
Accepted date: 12-11-2016

Please cite this article as: Elazzouzi, M., Haboubi, Kh., Elyoubi, M.S.,
Electrocoagulation-flocculation as a low-cost process for pollutants removal
from urban wastewater.Chemical Engineering Research and Design
http://dx.doi.org/10.1016/j.cherd.2016.11.011

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Electrocoagulation-flocculation as a low-cost process for pollutants
removal from urban wastewater

M.Elazzouzi1,2*, Kh.Haboubi2, M.S.Elyoubi1

1
Laboratory of Electrochemistry and Environmental Materials, Faculty of Sciences, Kenitra, Morocco
2
Group of material sciences, Energy and environnement, ENSAH, Alhoceima, Morocco
*Corresponding author. Tel: +212 676788409
E-mail address: [email protected]

Highlights

 Novel electrocoagulation-flocculation process was designed for wastewater

treatment
 The optimization of ECF conditions permit to achieve promised removal efficiencies
 A removal efficiency of 99% of fecal coliform was achieved at 10 min by ECF
process
 The operating removal conditions in ECF led to reduce specific energy consumption

Abstract

A combined two steps electrocoagulation-flocculation was designed to remove COD,

BOD5, TSS, nitrate (NO3), nitrogen (N), phosphate (P), and Fecal coliform (FC) from urban
wastewater. The possibility of adding a natural flocculant extracted from plant material,
Spineless Prickly Pear, Opuntia ficus Indica, juice (OFIJ), by comparing it with an
industrial grade flocculant as anionic polyacrylamide (APAM), in the process of
electrocoagulation-flocculation (ECF) was performed. The electrocoagulation (EC) reactor
was tested in two different sequences (before and after the flocculation unit).The effect of
several operational parameters, such as: current density, reaction time, flocculant dose,

 
1 
specific amount of dissolved electrodes and initial pH, on the removal efficiency of major
pollutants was determined. The application of ECF process under optimal conditions, such
as: current density (200 A/m2), reaction time (30min), flocculant dose (6ml/l), initial pH
(7.4) and specific amount of dissolved electrodes (0.2 kg/m3) allows to achieve these
promised removal efficiencies: 85%COD, 84%BOD5, 94%TSS, 63%N, 73%NO3 and
99%P. Moreover, it is of interest to note that duration of 10 min is sufficient to remove 99%
of FC from the studied urban wastewater. These operating conditions of ECF led to
reducing specific energy consumption from 6KWh/Kg COD and 0.6KWh/Kg P (EC
process) to 5KWh/Kg COD and 0.5KWh/Kg P, respectively. A comparative operating cost
analysis was also given and it was found that ECF performance requires 0.7 $/ Kg of COD
and 0.3 $/Kg of P removed versus 0.9$/ Kg COD and 0.35 $/Kg P for EC process.

Keywords: Urban wastewater; Electrocoagulation (EC); Electrocoagulation-Flocculation (ECF);

Anionic Polyacrylamide (APAM); Opuntia Ficus Indica, juice (OFIJ).
1. Introduction

The treatment of wastewater before their discharge in the environment is an important

subject; because wastewater contains a wide variety of pollutants as the organic compound,
phosphate, nitrogen, bacteria and others which present in with high concentrations that
should be strongly reduced. The urban wastewater generated can be treated by using
different techniques which should allow either its reuse or direct its disposal in the sewage
system. There are usually treated by the conventional system such as biological oxidation,
chemical coagulation (Chenna et al., 2016). Frequently, biological treatment is not enough
to assure complete treatment or pretreatment and refining technologies should be added to
the treatment process (Cañizares et al., 2006), advanced oxidation process as ozonation, UV
and ozone/UV combined oxidation, ultraviolet radiation (UV), ultrasonic irradiation (US),
UV/H2O2 and US/H2O2 processes (Maleki et al., 2010),  photo-catalysis (UV/TiO2) are not
economically feasible (Shu & Huang 1995). Due to high capital and operating costs of these
methods, as well as stringent legislation, there is an urgent need to develop more efficient
and inexpensive methods which require minimum chemical and energy consumptions. In
recent years, Electrocoagulation has been proposed by several authors as an effective
method for the treatment of various types of wastewater, such as: textile wastewater (Can et

 
2 
al., 2006; Ghanbari et al., 2015). urban wastewater (Pouet et al., 1995; Rodrigo et al., 2010),
almond wastewater (Valero et al., 2011), underground wastewater (Martinez et al., 2009),
olive oil mill wastewater (Inan et al., 2004), restaurant wastewater (Chen et al., 2000),
saline wastewater (Lin et al., 1998), chemical mechanical polishing wastewater (Lai et al.,
2004), drinking water (Vik et al., 1984), hydrofluoric wastewater (Aoudj et al.,2013),
seawater desalination (Zeboudji et al., 2013), semiconductor manufacturing wastewater (
Aoudj et al., 2015).
EC produced by anodic dissolution followed by hydrolysis of aluminum or iron hydroxides
destabilizing the particles in suspensions and adsorb dissolved contaminants. Aluminum
and iron are the most common sacrificial plates used in the electrocoagulation process and
the higher performance of aluminum plates compared to iron plates has been well
documented (Irdemez et al., 2006, Hu et al., 2003). In addition, The EC has significant
advantages like: simple equipment, operation and easy automation, rapid sedimentation
rates, reduction in the amount of sludge produced (Mollah et al., 2001) and it requires less
coagulant ions for the treatment of wastewater (Linares-Hernandez et al., 2007).
Furthermore, the type of pollutants, initial pH and concentration, number and type of
electrodes, floc stability, and the current density are among the factors that can influence the
process of electrocoagulation (Cheballah et al., 2014, Bazrafshan et al., 2007). On the other
hand, EC has some disadvantages such as having dissolved sacrificial electrodes, expense of
electricity and the need of high conductivity (Mollah et al. 2001). Hence, it is necessary to
develop a combined system capable of removing the pollutants from the urban wastewater
as well as reducing the cost of energy consumption.
Flocculation is one of the most used wastewater effluent treatments.  In principle, flocculant
enhances the formation of larger flocs from fine colloidal particles formed during EC. These
larger flocs settle more rapidly and are easily removed.
Since 2003, researchers have been classified flocculants into three main groups (Duan et al.,
2003) : (i) inorganic flocculants such as aluminum sulfate or polyaluminum chloride (PAC);
(ii) synthetic organic polymers such as polyacrylamide or a polyethyleneimine derivatives;
(iii) flocculants of natural origin such as biopolymers (Pan et al., 1999; Guo, 2015;
Zouboulis et al, 2004) or microbial (Kuran et al, 1986; Salehizadeh and Shojo Sadati, 2001).

 
3 
The chemicals flocculants as inorganic flocculants or synthetic organic polymers have some
disadvantages on human health and the ecosystems (Vanhorick and Moens, 1983; Bolto and
Gregory, 2007,). In order to contribute solving this problem, in the last few years, another
kind of natural flocculants of vegetable, animal or micro-organism sources have been used
in the treatment of wastewaters, it has the advantage of being biodegradable and present no
risk to public health. Among these natural flocculants, the Moringa oleifera certainly is the
most studied by the scientific community since these flocculant properties have been
recognized (Yin, 2010). Nevertheless, The chitosan and the xanthan are the only animal
materials studied for the wastewater treatments (Rodrigues et al., 2008, Zemmouri et
al.,2012).

The Flocculation ability of the cactus is highlighted (Diaz et al., 1999, Zhang et al., 2006,),
and the different species of Opuntia, reserved to Habit in human food, medicine have
aroused the interest of researchers in the field of the wastewater treatments.

Recently, (Betatache et al., 2013 ,) have used the juice of cactus to eliminate turbidity in
industrial effluents, they have seen the turbidity of the water decreased from 30 NTU to 2.5
NTU and 100 NTU to 2 NTU respectively. (Barka et al., 2013) have also used the cladodes
of the cactus, Opuntia Ficus Indica, as biosorbant to eliminate the methylene blue from the
waters.

Based on these previous studies, the juice of Spineless prickly pear cactus, available on the
Moroccan territory has been extracted and then used as flocculant. The flocculant
performance has been compared with polyelectrolyte as anionic polyacrylamide. Finally, we
aimed to evaluate the performance of the combined ECF reactor developed for the removal
of COD, BOD5, TSS, N, P, NO3 and the FC under different operational conditions of
current density, reaction time and initial pH. Moreover, we compared the operating cost for
each variant in terms of electrical energy consumption, electrodes and the amount of added
flocculant.

2. Electrocoagulation and flocculation process

2.1. Mechanism of electrocoagulation

 
4 
Electrocoagulation is a process that involves the generation coagulants by the dissolution of
metallic ions at the anode and the release of hydrogen gas at the cathode as:
Anode: Al Al3+ + 3e- (1)
Cathode: 3H20 + 3e- 3/2H2 + 3OH- (2)
Al3+(aq) and OH- generated by electrodes reaction (1) and ( 2) react to form various
monomeric species such as Al (OH)2+, Al (OH)2+, Al2(OH)24+, and polymeric species:
Al6(OH)153+, Al7(OH)174+, Al8 (OH)204+, Al13O4(OH)247+ and Al13(OH)345+, which is finally
converted into Al2(OH)3.
The formation of Al2(OH)3 ''sweep floc'' have large specific surface area which is beneficial
for a rapid adsorption of soluble organic compounds and trapping of colloidal particles:
These flocs polymerize as:
nAl(OH)3 Aln(OH)3n ( 3)
The complexes formed are easily removed from the sample by sedimentation and / or
flotation by H2.

2.2. Mechanism of flocculation

Long chain polymers can absorb colloids at many points along the chain and it can happen
that a single polymer molecule becomes attached to more than one particle. In that case, the
particles may be said to be "bridged" by adsorbed polymer and this mechanism is of great
practical importance in a number of applications. This mechanism has occurred, when the
polymer needs to be of a quite high molecular weight and to adsorb in such a way that a
segment portion is not in contact with the particle surface but extend some distance into the
aqueous phase. In addition, the adsorbed amount should not be large, so that a significant
fraction of the contacts can occur between unoccupied areas of a particle surface and
extended segments of chains adsorbed on other particles. Furthermore, When excess
polymer “bridging phenomenon” is prevented because there is insufficient free particle
surface for bridging contacts to occur and the adsorbed layers may also “steric repulsion”.
For this reasons, there is an "optimum dosage" of polymer to obtain good bridging
flocculation (Ruehrwein and Ward, 1952).
Another mechanism called "electrostatic effect patch" whereby the polyelectrolyte adsorbs
on an oppositely charged particle in such a way that there are "patches" of excess charge
 
5 
because of local charge reversal and areas of unoccupied surface still bearing the original
particle charge. This type of adsorption will occur when the charge density of the
polyelectrolyte is much greater than that of the particle surface. Particles with polymer
adsorbed in this "patchwise" manner can interact in such a way that positive and negative
areas of different particles are adjacent, giving strong electrical attraction.
Analysis the juice extracted from cactus by size exclusion chromatography, show that both
polysaccharides with a high molecular weight (10 wt%) and proteins, are responsible for the
agglomeration and adsorption particles (Majdoub et al., 2001). Based on this study, the
polysaccharide-proteins complex of natural flocculant (OFIJ) used for treatment of urban
wastewater contributes to the flocculation of colloids formed during the EC process.
3. Materials and methods
3.1. Characterization of the urban wastewater
In order to carry out this work, the urban wastewater was collected from the wastewater
treatment plant of Al Hoceima area, located in the northeast part of Morocco; its principal
characteristics are listed in Table 1.

3.2. Flocculants preparation

3.2.1. Natural flocculant
The spineless prickly pear cactus was washed with distilled water and it was crushed and
sieved. Thereafter, a filter of 500 micron diameter was used to collect the aqueous phase.
The filtrate obtained is centrifuged at 600 rpm / min for 20 min, the aqueous extract was
diluted to 10% vol., with distilled water and then homogenized by a stirrer for 30 min. The
spinless preakly pear, juice (OFIJ) is a viscous liquid with pH of 5 and a bulk density of
1.007 kg / m3. Indeed, the juice can keep its physicochemical and biological properties for
several weeks in a refrigerator at 4° C.
3.2.2. Industrial flocculant
The anionic polyacrylamide is an industrial grade organic polymer prepared in the
laboratory by dissolving 1 g of salt per 1 liter of distilled water. A series of experiments
were shown that above a concentration of 5 g/l, the solution takes the form of gel. In
addition, it is of interest to note that, the direct addition of the salt has proved inappropriate
for its low solubility in water.
 
6 
3.2.3. Experimental apparatus and procedures
EC experiment was performed in a batch electrochemical reactor made of Plexiglas of 500
ml capacity (Fig.1). EC cell is composed of a parallel rectangular plate of aluminum with a
dimension of 10x5x0.1 cm, the total effective area was 73cm2 and the space between each
electrode was 3 cm. the electrodes were connected to a digital DC power supply (ALR 3002
M) with a voltage of 12.5 V and a current density of (50-200 A/m2). A magnetic stirrer 100
rpm/min was used for mixing the solution during electrolysis. Before each run, the
electrodes were purified by the already described method (Do and Chen, 1994).

(1) DC power supply, (2) magnetic bar stirrer, (3) digital magnetic stirrer, (4) Reactor
electrochemical, (5) flocculation reactor.

In a typical run, conducted at constant temperature 25 °C and a volume of 500 dm3 was
placed into the electrolytic cell. When the electrolysis was completed, the solution was
discharged from the bottom of the EC cell into the flocculation reactor. Either OFIJ or
APAM flocculant was added, mixed for 15 min and final settling step lasted 30 min.
Table 2 shows the variation of the COD and turbidity as a function of the EC time, amount
of aluminum released from the electrodes and the flocculant volume (APAM or OFIJ). The
effective reduction in the turbidity obtained in 10 minutes is 98% for both flocculants and
COD removal efficiency was 82% and 80 % for (APAM) and (OFIJ), respectively. with a
flocculant volume of 4 ml/l which correspond to 0.08 kg/m3 of aluminum released in the
treated solution, note that the best removal rate is achieved at 30 min of EC time, flocculant
volume of 6 ml/l, 0.20kg/m3 of Al supplied and no significant increase in the COD and
turbidity removal is observed when the EC time were increased up 30 min.

3.3. Analytical methods

The physicochemical and biochemical parameters such as pH, Conductivity, Turbidity,
BOD5, COD, TSS, P, N and Fecal Coliforms were characterized by standard methods
(APHA, 2005). BOD5 was analyzed by the monomeric method with a respirometer system
OxyTop. COD, P and N samples were analyzed by Spectrocoquant PHAR 300 MERK
spectrophotometer. TSS was quantified by filters 47 mm diameter, the turbidity was

 
7 
measured by 2100Q marquee HACH, both pH and conductivity were measured by
pH/ion/Cond 750 WTW inolab.
4. Results and Discussion
4.1. Current density effect
The current density is the most important parameter for controlling the reaction rate within
the electrochemical reactor. It is expected to exhibit a strong effect on EC, especially on the
kinetics of removal, shortening the treatment. This is ascribed to the fact that at high current
density, the extent of anodic dissolution of aluminum increases, resulting in a greater
amount of precipitate for the removal of pollutants. Moreover, bubble generation rate
increases with increasing current density. These effects are both beneficial for high
pollutant removal. To investigate the effect of the current density, a series of experiments
were performed with the urban wastewater solution containing 400 mg/l of initial COD at
pHi = 7.4 and current density varying from 50 to 200 A/m2 (Fig.2). For a current density of
200 A/m2 and 30 min of operating time, the removal efficiency of COD, BOD5 and TSS,
increased rapidly up to 80%, 74% and 86%, respectively. Moreover, when the current
density was increased from 50 to 200 A/m2, the percent removal of COD in the EC unit was
increased. These results have to be related to the increase of the amount of Al3+ cations
released by the anode and hence the increase of Al(OH)3 particles. For the experimental
conditions, the optimal current density was found to be equal 200A/m2.

4.2. Effect of initial PH

It has been established that pH is an important operating factor influencing the performance
of electrocoagulation process (chen et al., 2000). Generally, the pH of the medium changes
during the process, as observed also by other investigators (Rodrigo et al., 2010; Bleek et
al., 2015, Cheballah et al., 2015). This change depends on the type of electrode material and
on initial pH. (fig.3) shows that, pH increases from 7.4 to 8.1 in the end of EC process.
Furthermore, for Aluminum, the final pH is always higher than initial pH. This is mainly
due to a large amount of ion OH- released by the electrochemical reaction of the hydrolysis
of water at the cathode. In order to investigate the effect of the initial pH on the combined
 
8 
ECF process, laboratory scale experiments were carried out by adjusting the effluent at
desired pH of wastewater. Even to know the influence of initial pH of urban wastewater on
COD removal efficiency in the case of ECF, a series of experiments was carried out and
comparative results are given in (fig.4). For an acid pHi=5 the percentage reduction was
70% and 85% for (OFIJ) and (APAM), respectively. Then, at pHi = 6.5 even 77% of COD
removal efficiency was achieved for both flocculants, and at pHi = 7.4 we found that the
percentage reduction was 83% and 75% for (OFIJ) and (APAM), respectively. Based on
these results, it is clear that the anionic Polyacrylamide requires an initial pH adjustment by
adding H2SO4. It was very interesting to note that the pH adjustment by H2SO4 was
excellent that provides more clear solution and compact sludge as compared to hydrochloric
acid. It might be due to strong oxidizing behaviour of sulphuric acid. Additionally, there are
several authors have found some results (Sarika et al., 2005; Can et al., 2006; Irfan et al,
2015.). While, for natural flocculant (OFIJ), the optimum result was obtained at an original
pHi = 7.4. This result is promising because the addition of natural flocculant (OFIJ) does
not require an adjustment of the initial pH of the urban wastewater.

4.3. Effect of electrolysis time on COD, BDO5 and TSS removal

Figs.5, 6 and 7; showed the effect of electrocoagulation time on the reduction of COD,
BOD5 and TSS. Theoretically, based explicitly on Faraday's law, the amount of coagulants
released from aluminum electrodes tends to increase with time of electrocoagulation
(Drouiche et al., 2009). Furthermore, as seen in (Fig.5) more than 50% of quality
wastewater parameters were removed in the first minute only (10 min), COD removal
efficiency for EC is 70%. (Chen et al., 2000) observed that the removal of the organic
matter (COD) is rather low (61%), a fact that could be attributed to the presence of
carbohydrates, coupled with some dissolved organic compounds. As observed previously by
(Tchamango et al., 2010) in their study of a restaurant wastewater with aluminum
electrodes, only 72% COD removal effeciency was reached; these authors attributed to this
low yield of the insufficient efficiency of the EC process applied to the elimination of
dissolved organic compounds. In the other study, (Cheballah et al., 2015) showed that the
value of COD decreased with increasing operating time and 98% of COD removal
efficiency were achieved from industrial wastewater by EC. Nevertheless, this increasing of
 
9 
COD removal can be explained by the adsorption of organic matter on the Fe(OH)3 flocks
formed in situ.
The results shown in (fig.5) indicate that in 10 min of operation time, the efficiency of ECF
was 80% of COD removed from wastewater (vs. 70% for EC). It is therefore concluded
that, adding a flocculant to the EC units correspond to decrease of operating time and
increase in removal efficiency. This is mainly due to the role of organic flocculant (APAM)
or natural flocculant (OFIJ) in accelerating the flocculation of the formed coagulants during
EC and improves their density to rapidly promote settling.
Furthermore, as seen in (Fig.6) for an operating time of 50 min, BOD5 removal efficiency is
83% for EC. (Barrera-Díaz et al., 2008) were used electrochemical method to remove BOD5
from a highly complex industrial wastewater by aluminum and iron electrodes assisted with
hydrogen peroxide (H2O2), they found that treatment reduced biochemical oxygen demand
(BOD5) by 89%. In accord with the results of this study, it can be concluded that Adding a
flocculant to EC process, the efficiency increased up 84% and 86% and the
electocoagulation time decreased (30 min) vs. (50 min for EC). In addition, as shown in
(Fig.7), the TSS removal from urban wastewater using either electrocoagulation or ECF
processes was determined. At 10 min and 30 min of operation time, the TSS removal
efficiency by EC process was 77% and 90% and the efficiency increased up 87% and 95%
for ECF.

4.4. Phosphate, nitrate and nitrogen removal

Nitrate, phosphate and nitrogen are undesirable substances in wastewater because they are
responsible for the eutrophication of receiving waters, so it is necessary to reduce their
concentration before their releases.
As mentioned in (Figs.8, 9 and 10), the efficiency of the EC and ECF process for phosphate,
nitrate and nitrogen removal was tested under different operating time. Fig. 8 depicts the
removal efficiency of phosphate at different operating times with an influent phosphate
concentration of 15 mg/l and a current density of 200A/m2. The maximum efficiency of the
EC for phosphate removal was observed at 50 min, and the removal efficiency reduced
when the operating time was decreased. For example, with an operating time of 50 min, a
maximum removal efficiency of 97% was observed and the efficiency decreased to 94%
 
10 
and 90% at 30 min and 10 min, respectively. On the other hand, in the case of coupled
technique (ECF), by adding natural or organic flocculants, 99% of the phosphate was
removed when the operating time was 30 min and no change in removal efficiency was
observed afterward. Additionally, the combined treatment (ECF) was observed to be an
adequate alternative to treat the phosphate of urban wastewater at its natural pH for (OFIJ)
and acidic pH for (APAM) using relatively shorter operating time in comparison with the
treatment using EC alone. In the literature, (Mahvi et al., 2011) were tested the performance
of a continuous bipolar electrocoagulation/electrooxidation–electroflotation (ECEO–EF) for
the elimination of phosphate from wastewater effluent under the optimum operational
conditions (pH of 7, current density of 3A, and detention time of 60 min). It was found that
the reactor was able to decrease the phosphate concentration by 98% (effluent concentration
of 0.96 mg/l).
Scare studies on phosphate removal mechanism by aluminum compound are available in
literature. However, one pathway has been reported by (Bektaş et al., 2004 ), which
involves phosphate interaction with aluminum as shown in the equations 4 and 5:
Al(aq)3+ +3H20→ Al(OH)3 + 3H+ (4)
Al(aq) 3+ + PO4 3− → AlPO4                              (5) 
The products of Eqs. (4) and (5) participate in phosphate removal. Figs. 9 and 10; illustrates
the effect of operating time on the efficiency of the ECF process for nitrogen and nitrate
removal with an influent concentration of 89 mg/l and 1.2 mg/l, respectively; under optimal
current density and pH aforementioned. In contrast to phosphate, the average removal
efficiency for nitrogen and nitrate was as low as slightly below 40% and 50%, respectively;
with an operating time of 10 min, while it significantly increased to over 60% at 60 min for
nitrogen and 67% at 50min for nitrate and remains almost unchanged afterward. This
indicates that nitrogen and nitrate need, respectively, 50 min and 60 min to be removed vs.
just 10 min for phosphate. Thus, it has been reported in the literature that nitrates can be
removed from wastewater via their adsorption onto the surfaces of hydroxide precipitates,
which are generated from metals and released by the electrodes.
(Hu et al., 2003) adapted (Eqs. (5)-(7)) to describe the reactions in the electrochemical cell
when NO3− ions are in the solution:
3NO3− + 3H2O + 2Al → 2Al3+ + 3NO2− + 6OH (6)
 
11 
6NO3− + 18H2O + 10Al → 10Al3+ + 3N2 + 36OH− (7)
3NO3− + 18H2O + 8Al → 8Al3+ + 3NH3 + 27OH− (8)
The removal of phosphate, nitrogen and nitrate is governed by two phenomena: the
electroreduction and/or adsorption. Moreover, the nitrate removal by electroreduction
requires a high current density and a short time, while adsorption requires only a low
current density but more time to remove nitrate (Lacasa et al, 2011;. Emamjomeh and
Sivakumar, 2009). In addition, the analysis of the solid phase (sludge) show the existence of
the total nitrogen (Yehya al., 2014), and the presence of a large amount of phosphate at the
end of electrocoagulation (Kuokkanen et al., 2015). nevertheless, the phosphate present in
the wastewater is removed by adsorption with aluminum hydroxide ions (Vasudevan et al.,
2009) and phosphate precipitation was mainly due to the formation of AlPO4 (İrdemez et
al.,2006).
As previously discussed, the nitrate turns into nitrogen and ammonia by electroreduction
that is readily adsorbed by the coagulants formed during EC process, while nitrogen and
phosphate are removed by direct adsorption followed by precipitation.

4.5. Fecal coliforms removal

Several authors have explained theoretically, the influence of the electric field generated by
electrocautery on the degradation of many microorganisms such as bacteria (Diao et al.,
2004) and viruses (Zhu et al., 2005). Furthermore, (Fig.8) shows the effect of
electrocoagulation on the reduction of fecal coliforms. In both cases either EC or the ECF,
the percentage reduction of fecal coliforms at first time (<10min) is estimated at more than
99%. To better understand The mechanism that controls this phenomenon, the application
of an electric current creates a potential difference on both ends of the cell membrane,
microscopic observation reveals an increase the distance between the outside and inside the
cell membrane when the polarization causing their breakdown and inactivation of
microorganisms increases with the increase of applied electric current. A biological cell
comprises a cytoplasm surrounded by a membrane, the cytoplasm can be considered as an
electrical conductor having opposite charges in its two sides. A charge accumulation is
observed during electrocoagulation thereby producing increased transmembrane potential
followed by the formation of ruptures in the membrane. In addition, the membrane consists
 
12 
of a phospholipid bilayer, which protects the vital center of the bacterial cell; the proteins
existing inside the membrane allow the ion exchange with the cellular environment. A
phospholipid membrane is not easily oxidized, while proteins are easily destroyed by the
effect of an electric field (Weaver and Chizmadzhev 1996). Furthermore, (Zimmerman et
al., 1973) found in the electron microscope observation, the increase of the distance
between the inside and outside of the cell membrane of fecal coliforms during the
polarization, which causes the rupture of the membrane and therefore the death of the
bacterium.

4.6. Operating cost Analysis

Generally, the cost estimation analysis during the wastewater treatment processes includes
the cost of electricity, chemical reagent, cost of sludge disposal, labor, maintenance, and
equipment. In the hybrid electrochemical process, the most important parameters that affect
operating cost are the cost of electrode material and consumed electrical energy. Thus, the
operating cost based on electrode material, electrical energy, and chemical consumed was
calculated using the following equation:

Operating cost= a Cenergy + b Celectrode + c Cflocculant (4)

Were Cenergy, Celectrode and Cflocculant are experimental consumption quantities per Kg of
wastewater treated. Coefficient (a) was given by national office for water and electricity of
Morocco. While, (b) and (c) are obtained by the international market (2016), are as follows;
(a) electrical enegy price 0.6 US$ / KWh, (b) cost of aluminum electrodes 1.5 US $ / kg and
(c) is the cost of flocculants; 0.8 US $ / Kg for anionic polyacrylamide, 0.5 US $ / Kg for
natural flocculant and 0.40 $/kg for H2SO4 for adjustment of a desired pH of the wastewater.
On the other hand, Cenergy and Celectrode respectively were calculated from Eqs. (5) - (6):
(Kobya et al., 2016).

Cenergy (KWh/Kg COD or P) = (U x I x tEc) / (v x Ci x Re) (5)

Celectrode (Kg/Kg COD or P) = (I x tEc x Mw x ɸAL ) / (z x F x v x Ci, x Re) (6)

 
13 
where U is cell voltage (V), i is current (A), tEC is operating time (hour), v is volume (m3) of
the wastewater, Ci (kg/m3) is COD or P concentration of wastewater in the inlet stream, and
Re is COD or P removal efficiency, Mw is molecular mass of electrode (Mw,Al = 0.02698
kg/ mol), tEC is operating time (s), z is number of electrons transferred (zAl = 3), and F is
Faraday’s constant (96.487 C/mol). ɸ is the faradic yield (ɸAl = Δmexp/Δmth) of the
electrode.
Figs. 12 and 13; showed that energy consumption per Kg of COD or P removed ,in the case
of ECF process by adding either APAM or OFIJ, increases with increasing of the
electrolysis time. For example; When operating time increased from 10 to 60 min,
respectively, the energy consumption increases from 2 KWh/Kg COD to 10 KWh/Kg COD
and 0.2 KWh/Kg P to 1 KWh/Kg P.  Therefore, the energy consumptions at 30 min were 5
KWh/ Kg for COD and 0.5 KWh/Kg for phosphate. According to these results, phosphate
removal from wastewater by ECF process was more efficient in term of Energy
consumption compared to that consumed in the case of COD removal.
Figs. 14 and 15; illustrate operating cost for ECF process as a function of time. Values of
the operating cost for both flocculants were 0.3 US$/kg COD and 0.1 US$/kg P for 10 min,
and increases to 0.7 US$/kg COD and 0.3 US$/kg P for 30 min. As seen in fig 14, Up to 50
min of electrolysis time, the operating cost ($/Kg COD removed) of ECF, tends to increase
more than EC process. Contrariwise, Fig 15 shows that below 30 min of operating time;
nearly the same operating cost ($/Kg phosphate removed) is obtained with EC and ECF and
monotonically increasing trend with increasing of electrolysis time for chemical flocculant
(APAM).

5. Conclusion

The method of EC used in this study to reduce the organic pollution of urban wastewater is
effective for the removal of colloids and suspended solids as well as charged particles, but it
requires more time that influences the cost energy. Coupling this technique with a natural
flocculant (OFIJ), showed that the process of EC accelerates the removal of colloids and
suspended solids and increases the treatment efficiency. Furthermore, the effect of operating
parameters (current density, reaction time, flocculant dose and initial pH) by the ECF

 
14 
process on COD, BOD5, TSS, N, NO3, P and FC removal efficiencies have been
investigated. The optimum operating conditions were determined to be as following,
operating time of 30 min, initial pH of 7.4 and a current density of 200 A/m2 for Al
electrodes. The obtained values of COD, BOD5, TSS, N, NO3, P and FC after the treatment
under optimum operating conditions reduced to 240 mg/L, 100 mg/L and 20mg/L, 30 mg/L,
0.7 mg/L, 0.3 mg/L and 750 NPP/100ml, respectively; and the latter values are in the range
of permissible limit to discharge into the sewage. In addition, (OFIJ) has the advantage of
being biodegradable and presents no risk to public health. In contrast, APAM presents some
disadvantages for human health and the ecosystems, because it is not biodegradable and
carcinogenic. Furthermore, The operating conditions for COD and P removal in ECF
process, led to reduce specific energy consumption from 6KWh/Kg COD and 0.6KWh/Kg
P (EC process) to 5KWh/Kg COD and 0.5KWh/Kg P, respectively; which can be expressed
by operating costs as 0.7 $/ Kg for COD and 0.3 $/Kg for P (ECF process) versus 0.9$/ Kg
COD and 0.35 $/Kg P for (EC process). According to these results, the process of ECF has
shown efficiency in the treatment of urban wastewater and economically feasible, which
permits to ECF by adding natural flocculant (OFIJ) process, to be a good alternative to the
industrial scale.

Acknowledgements

The authors would kindly thanks Dr. Achraf El Kasmi from Faculty of Sciences and
Techniques (Tangier) for his insightful contributions and discussions and also Dr. Abdellah
Aouaaram from ONEEP (Al Hoceima) for his technical support.

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 Figure.1: Schematic diagram of experimental setup

Figure.2: Effect of current density on COD,BOD5 and TSS removal. Applied by (pHi= 7.4; initial
COD = 1490 mg/l; initial BOD5 = 700mg/l; initial TSS = 400 mg/l and V = 500 dm3)

 
23 
Figure 3: Effect of electrolysis time on pH evolution during EC time. applied by (pHi= 7.4 and
current density 200 A/m2)

Figure 4: Effect of initial PH on COD removal. Applied by (initial pH (OFIJ) = 7.4; initial pH (APAM) =
5.5; current density = 200 A/m2 and V = 500 dm3)

 
24 
Figure 5: Effect of electrocoagulation time on COD removal. Applied by (initial pH (OFIJ) =7.4;
initial pH (APAM) = 5.5; initial COD=1490 mg/l; current density=200 A/m2 and V=500 dm3)

Figure 6: Effect of electrocoagulation time on BOD5 removal. Applied by (initial pH (OFIJ) =7, 4;
initial pH (APAM) = 5.5; initial BOD5=700 mg/l; current density=200 A/m2 and V=500 dm3)

 
25 
Figure 7: Effect of electrocoagulation time on TSS removal. Applied by (initial pH (OFIJ) =7, 4; initial
pH (APAM)= 5.5; initial TSS=400 mg/l; current density=200 A/m2 and V=500 dm3)

Figure 8: Effect of electrocoagulation time on phosphate removal. Applied by (initial pH (OFIJ) = 7.4;
initial pH (APAM) =5.5; initial P=12mg/l; current density=200 A/m2 and V=500 dm3)

 
26 
Figure 9: Effect of electrocoagulation time on nitogen removal. Applied by (initial pH (OFIJ) = 7.4;
initial pH (APAM) = 5.5; initial N=89 mg/l; current density=200 A/m2 and V = 500 dm3)

Figure 10: Effect of electrocoagulation time on nitrate removal. Applied by (pH (OFIJ) =7.4; initial pH
2 3
(APAM) = 5.5; initial NO3=1.2 mg/l; current density=200 A/m and V=500 dm )

 
27 
Figure.11: Effect of electrocoagulation time on FC removal. Applied by (initial pH (OFIJ) = 7.4; pH
7 2 3
(APAM) = 5.5; initial FC=5x10 NPP/100ml; current density=200 A/m and V = 500 dm )

Figure 12: Effect of electrocoagulation time on energy consumption for COD removal. Applied by
(initial pH (OFIJ)= 7.4; initial pH (APAM) = 5.5; current density=200 A/m2 and V = 500 dm3)

 
28 
Figure 13: Effect of electrocoagulation time on energy consumption for phosphate removal.
Applied by (initial pH (OFIJ) = 7.4; initial pH (APAM) = 5.5; current density=200 A/m2 and V = 500 dm3)

Figure 14: Effect of electrocoagulation time on operating cost for COD removal. Applied by (initial
pH (OFIJ) = 7.4; initial pH (APAM) = 5.5; current density=200 A/m2 and V = 500 dm3)

 
29 
Figure 15: Effect of electrocoagulation time on operating cost for phosphate removal. Applied by
(initial pH (OFIJ) = 7.4; initial pH (APAM) = 5.5; current density=200 A/m2 and V = 500 dm3)

 
30 
 Table1: Characteristics of the urban wastewater used in this study
Parameters Units values
COD mg/l 1460
BOD5 mg/l 700
TSS mg/l 400
P mg/l 12
N mg/l 89
NO3 mg/l 1.2
FC NPP/100ml 5x107
Conductivity µs/cm 3240
Turbidity NTU 300
pH pH 7.4
 

Table 2: Flocculant optimisation by measuring COD and turbidity parameters

EC time           Optimal flocculants          Al supplied                            APAM                                               OFIJ 
(min)                (ml/l)                                (Kg/m3)         COD (mg/l)     Turbidity (NTU)       COD(mg/l)     Turbidity(NTU) 

  0     0   0                     1460        300                     1460                  300 

 10   4   0.08                         260                   7.15                     280                  12.5 
 20   5  0.12                          220                   5.6                       250                  9.3 
30  6  0.20                          200                  2                          220                  3.5 
40  7  0.30                          200                  2                          220                  3.5 
50  8                                0.34                          200                  2                          220                  3.5 
 60   9                                0.42                          200                  2                          220                  3.5 
 

 
31