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Electrocoagulation in the dual application on the simultaneous removal of

fluoride and nitrate anions through respective adsorption/reduction
processes and modelling of continuous...

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DOI: 10.1016/j.jwpe.2022.102584

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 Journal of Water Process Engineering 46 (2022) 102584

Contents lists available at ScienceDirect

Journal of Water Process Engineering

journal homepage: www.elsevier.com/locate/jwpe

Electrocoagulation in the dual application on the simultaneous removal of

fluoride and nitrate anions through respective adsorption/reduction
processes and modelling of continuous process
H. Tounsi a, b, T. Chaabane b, *, K. Omine c, V. Sivasankar d, *, H. Sano e, M. Hecini a, A. Darchen f
a
Research Center in Semiconductor Technology for Energy (CRTSE), 2 Boulevard Frantz Fanon, BP 140, Alger – 7 Merveilles, 16038 Algiers, Algeria
b
Reaction Engineering Laboratory (LGR) - Faculty of Mechanical and Process Engineering (FGMGP)/Environmental Department, University of Science and Technology
Houari Boumédiène (USTHB), BP 32 El-Alia, 16111, Bab Ezzouar, Algiers, Algeria
c
Department of Civil Engineering, School of Engineering, Nagasaki University, 1-14 Bunkyo-machi, Nagasaki 8528 521, Japan
d
Post Graduate and Research Department of Chemistry, Pachaiyappa's College (Affiliated to University of Madras), Chennai 6000 030, Tamil Nadu, India
e
Division of Chemistry and Materials Science, Department of Civil Engineering, Graduate School of Engineering, Nagasaki University, Nagasaki 8528 521, Japan
f
UMR CNRS n◦ 6226, Institut des Sciences Chimiques de Rennes, ENSCR, 11 Allée de Beaulieu, CS 50837, 35708 Rennes Cedex 7, France.

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

Keywords: Electrocoagulation (EC) is known as an electrochemical process for the efficient removal of various pollutants
Aluminum including fluoride and nitrate anions. Continuous electrocoagulation (CEC) was applied to synthetic aqueous
Continuous process solutions containing mixtures of nitrate and fluoride anions both at initial concentrations of 0.1 g L− 1 for
Dual removal
simulation of effluents arising from the etching process in microelectronic industries. Several parameters such as
Electrocoagulation
Kinetics
electrode material, pH, current density, initial concentration as well as the presence of co-existing ions were
Modelling theory studied. Without addition of an electrolyte, the optimizing conditions were found for aluminum electrodes at pH
= 5.94, current density of 9.09 mA.cm− 2 and distance between electrodes of 18 mm, leading to removal rates of
42.83% and 88.28% for nitrate and fluoride anions, respectively. The isolated electrogenerated solids were
characterized by Energy Dispersion Spectroscopy (EDS) coupled to SEM, FT-IR, XRD, XPS, TGA and Raman
spectroscopy. All the characterizations agree with the removals of nitrate and fluoride anions by reduction and
adsorption, respectively. The anode and the cathode were involved, but the reduction and adsorption processes
were independent of each other. The nitrate reduction was a cathodic reaction leading to hydroxide anions which
were involved in the formation of electrogenerated adsorbents by reaction with the aluminum cations (or metal
cations) arising from the anode oxidation. A modelling kinetic theory for a continuous electrocoagulation process
was developed and applied to the treatment of artificial and real wastewaters. The treatment cost of the real
wastewater was found at 2.3097 USD per m3.

electrocoagulations [9–11]. Improved EC removal technologies have

1. Introduction
Electrocoagulation (EC) is an electrochemical treatment involving
the preparation of coagulant ions thanks to the anodic dissolution of the
corresponding metals. A lot of reviews illustrate the great variety of
applications in pollution treatments. Recent general reviews deal with
the treatment of water and wastewaters [1–4], including the special
cases of defluoridation [5], the depollution of pharmaceutical waste­
waters [6] and industrial wastewaters [7]. The role of electrogenerated
flocs has been analyzed [8]. Various combined processes have been
developed in order to enhance the efficiency of classical
been performed thanks to the hybridization of EC with membrane pro­
cess [12], by coupling with ultrasounds [13,14] or supplementary ad­
sorbents [15,16], photocatalysis [17], electrocatalysis [18],
electrochemical oxidation [19], advanced oxidation [20,21] and bio­
logical treatment [22].
Many academic investigations are performed on the treatment of
single pollutants. However, since industrial wastewaters and drinking
water generally contain more than one pollutant, recent works have
been devoted to the simultaneous removal of several compounds by
using only one method. So, the removal of arsenic and fluoride was
carried out by adsorption [23] and electrocoagulation [24–26].

* Corresponding authors.
E-mail addresses: tchaabane@usthb.dz (T. Chaabane), sivshri.20@gmail.com (V. Sivasankar).

https://doi.org/10.1016/j.jwpe.2022.102584
Received 27 October 2021; Received in revised form 12 December 2021; Accepted 16 January 2022
Available online 24 January 2022
2214-7144/© 2022 Published by Elsevier Ltd.
H. Tounsi et al.
Nomenclature
A constant in the modelling of concentrations
[A] concentration of specie A
[A]0 initial concentration of specie A
[A]t a concentration at time t
B constant in the modelling of concentrations
BEC batch electrocoagulation
CA concentration of specie A
CAin concentration of A at the entry of the EC reactor
CAex concentration of A at the exit of the EC reactor
Cads adsorption capacity
C0 initial concentration
CEC continuous electrocoagulation
CEP continuous electrocoagulation process
Cst concentration at the stationary state
C(t) concentration at time t
C(∞) calculated concentration at stationary state
EC electrocoagulation
EGA electrogenerated adsorbent
ELC electrode consumed
Adsorption has been applied to the removal of phosphate and fluoride
[27], the removal of nitrate and fluoride [28] and the removal of nitrate,
fluoride and phosphate anions [29]. Various attempts on simultaneous
removals have been performed by photoelectrocatalysis [30], radical-
induced oxidation [31], and with the use of nanoparticles [32].
EC is generally carried out for the removal of single pollutant. Since
EC works with two electrodes it would be interesting to develop the use
of both electrodes in dual treatments of pollutants. For example, the
dissolution of the anode leading to an electrogenerated coagulant
involved in the removal of one pollutant, coupled to the removal of the
second pollutant thanks to the reduction at the cathode. The present
work is devoted to the simultaneous treatment of fluoride and nitrate
anions. Both anions may be found in drinking water or in industrial
wastewaters arising from surface treatment industries. The simulta­
neous removal of nitrate and fluoride anions has been investigated by
adsorption [28,29,33], ion exchange [34,35], electrodialysis [36,37],
capacitive deionization [38], precipitation [39] and reduction by zero
valence iron [40]. Only rare studies of simultaneous removal of nitrate
and fluoride anions from drinking water were performed by electro­
coagulation [41–43]. The present paper reports the treatment, by a
continuous electrocoagulation, of artificial polluted solutions and in­
dustrial wastewaters arising from the etching process of silicon wafers in
microelectronic industries. For the first time, this paper presents the
modelling of a continuous electrocoagulation.
2. Material and methods
2.1. Chemicals and solutions
All chemicals, which were used in the study, were of analytical grade
and they were purchased from Sigma-Aldrich (France). The synthetic
solutions of fluoride and nitrate ions were made with deionized water.
0.1 M HCl and 0.1 M NaOH solutions were used to adjust the pH of the
solutions.
Real wastewaters arose from the Semiconductor Research Center for
Energy (Algiers, Algeria). They were formed during the etching of sili­
con wafers with a mixture of hydrofluoric acid, nitric acid and acetic
acid, followed by several rinsing operations with distilled water, until
the neutrality of the rinsing water was reached. All the rinsing waste­
waters were put together and the acidity was neutralized with Ca(OH)2.
After filtration of the precipitates, NaCl (1 g L− 1) was added to the
2
Journal of Water Process Engineering 46 (2022) 102584
ENC energy consumption
F Faraday constant (96,485C mol− 1)
KA experimental constant
KB experimental constant
k1 first order rate constant
k2 second order rate constant
MEGA calculated molar mass of the EGA
n number of electrons in the Faraday law
Qads quantity of adsorbed species
QEGA quantity of EGA
Qfr flow rate of a solution
Qin flow rate of a solution at the entry of the EC reactor
Qex flow rate of a solution at the exit of the EC reactor
TC treatment cost
tCEP time of the treatment process
U electric voltage of the EC reactor
V volume of the EC reactor
Vt volume of treated solution out of the EC reactor
τ residence time in the EC reactor
ΔCt abatement
ΔCct concentration variation in the collecting tank
filtrate in order to increase its conductivity for a better electro­
coagulation treatment. Typically, the concentrations of nitrate and
fluoride anions were of 88.2 mg L− 1 and 40.6 mg L− 1, respectively.
Samples of real wastewaters were carried out in polypropylene tanks.
The composition of the investigated real wastewater is given in Sup­
plementary data (Table S1).
2.2. Continuous electrocoagulation process (CEP)
The continuous electrocoagulation treatment was performed with
the equipment which is presented in Fig. 1. The main elements were: (1)
an influent feeding tank of 3 L, (2) a peristaltic pump (Heidolph model
Hei-Flow Value) working at the rate of 8.33 mL min− 1, (3) an electro­
coagulation reactor of 1.5 L equipped with four monopolar electrodes
which were connected to a current generator (7) (Yizhan PS-305D).
Aluminum and iron electrodes of dimensions 10 cm × 10 cm × 0.1 cm
were immersed with an active area of 55 cm2 and arranged with a gap of
10 or 18 mm between two successive electrodes. Before all the elec­
trocoagulation experiments, the electrodes were cleaned, first by abra­
sion with sandpaper followed by a washing in 1 M NaOH or 1 M HCl for
aluminum or iron electrodes, respectively. Then, the electrodes were
rinsed with distilled water and finally dried for 1 h in an oven at 100 ◦ C.
The treated solution left the electrocoagulation reactor at the same rate
which was controlled at the entry by the peristaltic pump. One elec­
trocoagulation experiment needed 3 L of solution and a duration of 3 h.
1.5 L of solution was put in tank (1) and 1.5 L was put in the electro­
coagulation reactor (3). All the analyses, which were done versus the
electrolysis time, were performed on the collected effluent of tank (6).
The effect of coexisting anions was investigated by adding sodium salts
of chloride, sulfate, carbonate and phosphate with a concentration of 1
g L− 1 of these salts.
For the needs of analysis, samples of the solutions were removed
during the electrocoagulation processes, or at their ends, and then they
were filtrated for the separation of the electrogenerated solid material
from the liquid phase. After determining the concentration of fluoride
and nitrate anions, the percentage removal was expressed by Eq. (1)
where [A]0 and [A]t are the initial concentration and concentration at
time t, respectively.
100 ( )
Removal (%) = [A]0 − [A]t (1)
[A]0
H. Tounsi et al. Journal of Water Process Engineering 46 (2022) 102584

Fig. 1. Scheme of the equipment used in the continuous electrocoagulation process (CEP): (1) Feeding tank; (2) Magnetic bar; (3) Magnetic stirrer; (4) Peristaltic
pump; (5) Current generator; (6) Monopolar electrodes; (7) Electrocoagulation reactor; (8) Treated water tank.

2.3. Instrumental characterizations

The concentrations of nitrate anions were determined by UV–visible

spectrophotometry (Hach model Odyssey DR2500) at the wavelength of
λ = 415 nm following reference [44]. The concentration of fluoride
anions was measured by ionometry (Hanna model HI4222) with a
fluoride electrode (HI 4110). The pH was measured with a glass elec­
trode and a pH-meter (Hanna model HI8424). The electrolytic conduc­
tivity was measured with a conductance cell and a conductometer
(Hanna model HI2315-01).
The characterizations of sludges were performed by Scanning Elec­
tron Microscopy after a carbon coating of the samples (SEM; Jeol JSM-
7500 FAM) and Energy Dispersive Spectroscopy (EDS; Jeol EDS JSM-
7500) in order to identify which elements were present. The presence
of crystalline phases has been determined by X-Ray Diffraction (XRD;
Rigaku Mini Flex 600 and phase identification with the software
PDXL2). Attenuated Total Reflection - Fourier Transform Infra-Red Fig. 2. Effect of electrode material combination (anode first) on the removal
(ATR-FTIR; Thermo Nicolet Nexus 670NT), Raman spectroscopy rate of nitrate ions. Experimental conditions: initial pH = 5.87; 1 g L− 1 NaCl
(Jasco NRS-3000) and X-ray Photoelectron Spectroscopy (XPS; Kratos solution; nitrate concentration = 0.1 g L− 1; current density = 12.72 mA cm− 2;
Axis Ultra DLD) have been used in the search of chemical functions. Distance between electrodes = 10 mm.
Complementary chemical composition has been performed by Thermo
Gravimetric Analysis (TGA; Shimadzu TGA-50H equipped with a non- removal process. All the subsequent experiments were performed with
dispersive infrared gas analyzer NDIR Shimadzu CGT-7000). the combination pair of Al anode and Fe cathode.
The effect of the cathode nature was not so clear. For an aluminum
3. Results and discussion anode, the removal rate increased with 5% for an iron cathode when
compared to an aluminum cathode. Whereas, for an iron anode, the
3.1. CEP and optimization studies removal rate decreased in 10% for an iron cathode compared to an
aluminum cathode.
3.1.1. Selection of anode – cathode (cell) combination Results of Fig. 2 disagree with the works of Majlesi et al. [45] and
The removal of nitrate ions was found less efficient than the one of Berkani et al. [46] showing that the best nitrate removal was obtained
fluoride anions, and this is why the search of the best abatement was with two aluminum electrodes. Lacasa et al. [47] observed that the ni­
performed on this reaction. Fig. 2 shows the anode-cathode combination trate removal did not show a difference during the electrocoagulation
for effective removal of nitrate ions in this study. It appears, for the same with aluminum or iron electrodes. Our results agree with those of
cathode material, that the nitrate removal was always more efficient Govindan et al. [48] who found that the use of an anode-cathode com­
with an aluminum anode. For an iron cathode, the removal was 30% bination of aluminum‑iron led to a better nitrate removal when
better when an aluminum anode was used. Analogous conclusion is compared to the use of two aluminum electrodes.
drawn for an aluminum cathode, the removal rate was 17% better when
an aluminum anode was used. These results suggest a possible
involvement of the electrogenerated aluminum hydroxide in the nitrate

3
H. Tounsi et al. Journal of Water Process Engineering 46 (2022) 102584

3.1.2. Effect of the current density on the removal rates of fluoride and
nitrate anions
Fig. 3 presents the effect of the current density on the removal rates
of fluoride and nitrate anions when they are alone or in the same solu­
tion. In all the cases, the removal rates increase and reach a plateau. This
observation can be attributed to a kinetic effect where the formation of
the electrogenerated adsorbent is faster than the fluoride adsorption or
the nitrate reduction. The removal rates of fluoride anion are always
greater than those of nitrate anion, and this is observed despite the
higher molar concentration of fluoride anion. On considering the
removal rates in a solution containing fluoride and nitrate anions, the
presence of one anion (fluoride or nitrate) decreases the removal rate of
the other anion. This type of decrease is more pronounced for the
fluoride adsorption than for the nitrate reduction. An explanation can be
found in the low effect of nitrate as a co-existing anion on the fluoride
removal [49], while the electrocatalytic activity of the iron cathode may
be influenced by the presence of fluoride anions.

3.1.3. pH variation and influence of the solution pH

Fig. 4A presents the pH variation during the removal of fluoride and
nitrate ions by electrocoagulation of individual solutions. As known for
electrocoagulation in the presence of nitrate and chloride ions, the pH
increases and reaches a plateau of about 9.3 and 9.6, respectively [49].
The pH difference between the plateaus is due to a different mechanism
in the pH increases. In the presence of chloride anions, the pH increase is
the result of a substitution reaction of hydroxyl group by chloride in the
electrogenerated alumina. In the presence of nitrate anions, the pH in­
crease is the result of a proton consumption during the reduction of these
ions leading to ammonium cations which have a buffer effect. Fig. 4B
shows the effect of initial pH on the removal rate of nitrate and fluoride
ions alone and in a mixture. Since the pH was not buffered, it is expected
that at the end of the electrocoagulation the pH reached the final values
given in Fig. 4A. Whatever the pH, the fluoride anion removal was al­
ways more efficient than the nitrate removal. In the pH range 4–10 the
defluoridation by the electrogenerated coagulants seems approximately
constant, irrespective of the presence of nitrate ions. This result shows
that at the concentration of 100 mg L− 1 the nitrate anions, and their
reduction products, did not show any negative effect on the adsorption
of the fluoride anions. On the other hand, the presence of fluoride anions
shows a noticeable negative effect of about 17% against the nitrate
removal. This effect can be the result of a negative influence of fluoride
anions on the electrocatalytic activity of the iron cathode in the nitrate
anion reduction.
3.1.4. Influence of initial concentrations of fluoride and nitrate ions
The results of the influence of initial concentrations on the removal
Fig. 4. (A) Variation of the pH during the CEP and (B) influence of the initial
pH on the removal rates of fluoride and nitrate anions, alone or in the same
solution. Experimental common conditions: 1 g L− 1 NaCl solution; concentrations
of fluoride and nitrate anions = 0.1 g L− 1; Distance between electrodes = 18
mm. Specific conditions for (A): current density = 12.72 mA cm− 2; for (B):
current density = 9.09 mA cm− 2.
of nitrate and fluoride ions are shown in Fig 5. The removal rate of ni­
trate anions alone (Fig. 5A) decreased from 47.7% to 25.5% in the
concentration range 0.1–1.0 g L− 1. In the same range, the presence of
0.1 g L− 1 of fluoride anions decreased the removal rate of nitrate ions of
about 5%. On the other hand, the removal rate of fluoride anions alone
(Fig. 5B) decreased from 87% to 46% in the concentration range 0.1–1.0
g L− 1, whereas the presence of 0.1 g L− 1 of nitrate anions gave an
additional decrease of about 3.5% to the removal rate.
3.1.5. Effect of coexisting anions
The effect of coexisting anions has been investigated with the addi­
tion of 1 g L− 1 of sodium salts to the initial solution containing nitrate
and fluoride (0.1 g L− 1) in 1 g L− 1 NaCl solution. The results are pre­
sented in Fig. 6. The addition of NaCl increased the removal rate of ni­
trate and fluoride anions of 3.2 and 4.8%, respectively. Conversely, all
the other investigated anions showed negative effects. The decrease in
the removal rate of nitrate was 4.5%, 11.4% and 9.8% in the presence of
carbonate, sulfate and phosphate anions, respectively. The decrease was
relatively noticeable because the initial removal rate of nitrate anions
was 42.0%. Although the removal rate of fluoride anions was high with
88.7% (without accompanying any other anions), the carbonate, sulfate
and phosphate anions inhibited the fluoride anions removal with the
lessened efficiency of 32.2%, 41.9% and 38.7% respectively. High
negative effect (or inhibition) from these anions is already known in
fluoride removal by adsorption onto electrogenerated adsorbents [50]
and bayerite/boehmite nanocomposites [51].

3.2. Characterization of electrogenerated sludges

Fig. 3. Effect of current density on the removal rates of nitrate and fluoride 3.2.1. Scanning electron microscopic study with EDS analysis
anions alone or in the same solution. Experimental conditions: initial pH = 5.83; The EDS diagrams of sludge samples are gathered together in Fig. 7.
1 g L− 1 NaCl solution; initial concentrations of fluoride and nitrate anions = 0.1 All the samples show the signals of Al and O as expected for electro-
g L− 1; Distance between electrodes = 18 mm. generated aluminas. Several samples contain Si compounds which

4
H. Tounsi et al. Journal of Water Process Engineering 46 (2022) 102584

Fig. 5. Effect of the concentration of nitrate (A) and fluoride (B) anions on their removal rates. Experimental conditions: initial pH = 5.88; 1 g L− 1 NaCl solution; the
concentrations of the removed ions, nitrate (A) or fluoride (B) anions, alone or in a mixture, are given under the horizontal axis; in mixtures, the concentration of the
other one was always of 100 mg L− 1; Distance between electrodes = 18 mm; current density = 9.09 mA cm− 2.

Fig. 6. Effect of coexisting anions on the removal rates of nitrate and fluoride
anions. Experimental conditions: initial pH = 5.94; 1 g L− 1 NaCl solution; con­
centrations of fluoride and nitrate anions = 0.1 g L− 1; concentrations of coex­
isting sodium salts = 1 g L− 1; Distance between electrodes = 18 mm; current
density = 9.09 mA cm− 2.

probably arise from a contamination. Several samples also contain Fe

whose origin is the corrosion of the iron cathode of the CEP process.
Fluoride was observed for samples (C), (D) and (E) which were sludges
isolated after the treatment of synthetic fluoride solution, synthetic
fluoride-nitrate solution and real wastewater, respectively. Sample (A)
arising from CEP of NaCl solution shows the signal of Cl at 2.6 keV but
with the absence of Na. As already published [49], these observations
prove the substitution of hydroxyl by chloride anions in the electro-
generated aluminas and this reaction explains the pH increase during
the CEP process. All the treated solutions contained NaCl but the pres­ Fig. 7. EDS analyses of the electro-generated sludges isolated after CEP of so­
ence of Cl element was not observed for all the analyzed samples. It lutions: (A) 1.0 g L− 1 NaCl solution; (B) synthetic nitrate solution at 0.1 g. L− 1;
seems that the presence of coexisting nitrate ions inhibits the chloride (C) synthetic fluoride solution at 0.1 g L− 1; (D) synthetic fluoride – nitrate so­
substitution. Calcium was clearly detected in the sludge (E) arising from lution at 0.1 g. L− 1; (E) real wastewater effluent.
the CEP treatment of the real wastewater effluent which was previously
treated by Ca(OH)2. 3.2.2. X–ray diffraction study and thermal studies
XRD diagrams of the isolated sludges are presented in Fig. 8a. These
patterns reveal only the crystallized phases. Sludge (A) arising from CEP

5
H. Tounsi et al.
Fig. 8. XRD (a) and TG-DTA (b) studies of the electro-generated sludges isolated after CEP of solutions: (A) 1.0 g L− 1 NaCl solution; (B) synthetic nitrate solution at
0.1 g L− 1; (C) synthetic fluoride solution at 0.1 g L− 1; (D) synthetic fluoride – nitrate solution at 0.1 g L− 1; (E) real wastewater effluent.
of NaCl solution (A) shows the presence of bayerite Al(OH)3 and
boehmite AlO(OH) characterized by sharp and broad reflections,
respectively. The simultaneous presence of nitrate anions and chloride
anions in solution (B) seems leading mainly to crystallized bayerite,
whereas all other solutions (C), (D) and (E), which contained fluoride
anions led to boehmite. The formation of crystallized bayerite was not
observed for sludges (D) and (E). The pattern of (E) which arose from
CEP of the real wastewater effluent shows the presence of calcite CaCO3
which was identified thanks to its reflections at 2θ of 23.0◦ , 29.4◦ , 35.9◦ ,
39.4◦ , 43.1◦ and 47.1◦ [52]. The formation of calcite is not surprising
since the real wastewater contained calcium ions and the increase of pH
during the CEP allows the formation of Ca(OH)2 and then CaCO3 after
absorption of atmospheric CO2. Additional reflections were observed at
2θ of 28.27◦ and 47.01◦ . They were attributed to CaF2 which was formed
during the acid neutralization of the real wastewater. The presence of
this compound is due to the difficulties in the separation of CaF2 after its
precipitation in real wastewater [53].
The TG-DTA studies of the isolated sludges are presented in Fig. 8b.
Sludge (B) shows a great mass change, at about 280 ◦ C, which can be
attributed to the dehydration of bayerite leading to Al2O3 which pre­
sents a mass change at 300 ◦ C [54]. All other sludges show a first mass
change before 100 ◦ C which can be attributed to the loss of adsorbed
water. Sludges (A), (C), (D) and (E) present three mass changes: before
100 ◦ C, and at about 265 ◦ C and 400 ◦ C. The first mass loss corresponds
to a water desorption and agrees with the thermal behavior of boehmite
[55]. The second and third mass changes are due to the dehydration of
bayerite and boehmite, even when crystalized bayerite is not observed
in the XRD pattern (Fig. 8a). These mass changes occur at temperatures
in agreement with the literature, for the dehydration of bayerite [54]
and boehmite [55]. Sludge (E) shows at 680 ◦ C a mass change which
must be attributed to the thermal behavior of the calcite observed in the
XRD diagram (Fig. 8a).
The mass changes between 150 ◦ C and 600 ◦ C for sludges (B) and (D)
were 29% and 20%, respectively. The theoretical mass changes for a
dehydration of bayerite and boehmite are of 34.6% and 15.0%,
respectively. The calculation process of the experimental mass changes
leads to 80% of Al(OH)3 and 20% of AlO(OH) for sludge (B), and 37% of
6
Journal of Water Process Engineering 46 (2022) 102584
Al(OH)3 and 63% of AlO(OH) for sludge D. So, the thermogravimetry
analysis reveals the presence of amorphous boehmite in the electro­
generated sludge. As shown by their similar shapes, the thermograms of
sludges (A), (C) and (E) confirm the simultaneous presence of bayerite
and boehmite.
3.2.3. FTIR and Raman spectroscopy
FTIR and Raman spectra patterns (Fig. S1) did not give much in­
formation about the structures of the electrogenerated sludges. The most
important point is the absence of vibrations at 1384 cm− 1 which would
be expected for adsorbed nitrate anions.
3.2.4. X–ray photoelectron spectroscopy (XPS)
XPS spectra of all sludges are gathered together in Fig. 9 confirming
the chemical composition given by SDS (Fig. 7). Regarding the adsorbed
fluoride anions, F1s is observed with a binding energy of 685 eV for
sludges (C), (D) and (E). Cl is observed at 199 eV for sludge (A). N is not
observed for sludges (B), (D) and (E), in agreement with the absence of
adsorbed nitrate anions or their reduction products. A desorption of
nitrate anions by fluoride anions is involved, as already observed by
FTIR and XPS [51]. For sludge (B), analogous explanation could be given
by a possible desorption of nitrate anions by chloride anions.
3.3. Adsorption kinetics theory in a continuous process for a first order
kinetics
Batch experiments of electrocoagulation (BEC) are always treated as
batch experiment of adsorption, with the notable difference that the
adsorbent is continuously added as soon as it is formed by dissolution of
the anode. The decrease of the sorbent concentration allows the deter­
mination of adsorption capacities, adsorption rate constants and the
choice of the best model of isotherm adsorption. All these characteristics
are important, but BEC does help for a continuous application. A
continuous electrocoagulation (CEC), or a continuous electro­
coagulation process (CEP), is a better treatment from an engineering
point of view.
A CEP is easy to perform with the successive assembling of a feeding
H. Tounsi et al. Journal of Water Process Engineering 46 (2022) 102584

Fig. 9. XPS study of the electro-generated sludge after CEP of: (A) 1 g L− 1 NaCl solution; (B) synthetic nitrate solution at 0.1 g. L− 1; (C) synthetic fluoride solution at
0.1 g. L− 1; (D) synthetic fluoride – nitrate solution at 0.1 g. L− 1; (E) real wastewater effluent.

tank, a pump, an EC reactor and finally a collecting tank for the ( )

continuously treated solution [56–62]. Such experiments can be seen as Qfr .CAin = CAex k1 .V + Qfr (5)
the pilot of industrial equipment. The aim of a CEC is to work at a sta­
Qfr .CAin CAin
tionary state or steady-state operation conditions. So, the behavior of a CAex = =( ) (6)
k1 .V + Qfr
CEC treatment cannot be modelled as a BEC [63]. Depending upon the 1 + kQ1 .V
experimental conditions, the stationary state is reached more or less
fr

quickly, and this creates two situations with different modelling V

treatments.
3.3.1. At steady-state operation conditions
The electrocoagulation experiments were carried out in a perfectly
stirred open reactor. In this situation, the use of differential form of the
rate cannot be used because the adsorption of the substrates is not alone
involved in the variation of the concentrations. Considering A the sor­
bent, the balance relationship can be written for a stationary state by Eq.
(2) where Qin is the flow rate at the entry of the EC reactor, CAin is the
concentration at the entry of the EC reactor, V is the volume of the EC
reactor, [A] is the concentration of A in the EC reactor, Qex is the solution
flow at the exit of the EC reactor, and CAex is the concentration of A at the
exit of the reactor.
d[A]
Qin CAin + V. − Qex CAex = 0
dt
Since the EC reactor is perfectly stirred, there is an egality among
concentrations [A] = CAex = CA, and flow rates Qin = Qex = Qfr.
Considering a first order kinetics for the adsorption of A as shown in Eq.
(3) where k1 is the first order rate constant of the reaction and the bal­
ance relationship for Eq. (2) can be written by Eq. (4). Then, further
rearrangement leads to Eq. (5) and finally the concentration of A at the
exit of the EC reactor is given by Eq. (6).
is the residence time of compound A in the EC reactor. It is written as
Qfr
τ. For given experimental conditions and rate constant k1, the targeted
concentration at the exit can be calculated with Eq. (7) and the rate
constant k1 is given by Eq. (8). A relation equivalent to Eq. (7) can be
found for a first order kinetics in a perfectly mixed flow reactor [64].
CAin
CAex = (7)
(1 + k1 .τ)
(CAin − CAex )
k1 = (8)
(CAex .τ)
3.3.2. Determination of adsorption capacity at steady-state conditions
At a stationary state, the difference between concentrations of
influent and effluent of the EC reactor is the result of the treatment by
(2) the EC current. It may be assumed that the electro-generated adsorbent
already present in the reactor is not involved in the removal process in
accordance with the following theory. For a given ΔV volume of flowing
solution during a given time Δt, the quantity of adsorbed species Qads is
calculated by Eq. (9) where C0 and Cst are the initial concentration and
the concentration at the stationary state, respectively, and where ΔV is
(Qfr × Δt) with Qfr the flow of the solution during time Δt.
Qads = (C0 − Cst ).ΔV orΔCt .ΔV (9)

d[A] The quantity of EGA (QEGA in g) produced for a given time Δt is

= − k1 .CA (3)
dt calculated by Faraday law (Eq. (10) where i (A) is the current intensity, n
is the number of electrons involved in the anodic dissolution of
Qin CAin − k1 .V.CAex − Qex CAex = 0 (4) aluminum (n = 3), F is the Faraday constant (F = 96,485C mol− 1) and
MEGA is the molar mass of the EGA (MEGA is calculated as 66.66 g mol− 1

7
H. Tounsi et al. Journal of Water Process Engineering 46 (2022) 102584

for a mixture of 37% of Al(OH)3 and 63% of AlOOH)). absence of analysis of the treated solution, the adsorbed quantity in the
treated solution was calculated by a numerical integration (Eq. (15))
i.Δt.MEGA
QEGA = (10) where ΔV is the integration step.
nF
∑
The adsorption capacity Cads is calculated by Eq. (11) leading to Eq. Vt .ΔCct = ΔC.ΔV (15)
(12) as following:
A set of results is given in Fig. 11 for the removal of fluoride,
Qads ( ) nF assuming that these removals follow a first order kinetics as already
Cads = = ΔCt .Qfr .Δt × (11)
QEGA i.Δt.MEGA published for fluoride adsorption [65–67].
The kinetics of the nitrate reduction is also known to follow a first
Cads = KA .ΔCt where KA is equal to
Qfr .nF
(12) order [68–70]. But in our hands, the nitrate ion abatement was lower
i.MEGA than the fluoride ion and it did not give a good modelling, so these re­
The adsorption capacity is proportional to the experimental abate­ sults could not be kinetically treated.
ment ΔCt and to the experimental constant KA. A targeted abatement ΔCt Fig. 11 shows a slight decrease of the fluoride adsorption capacity
can be calculated by Eq. (13) and reached thanks to the control of cur­ during the course of the CEP. In the literature, the fluoride adsorption
rent i and solution flow Qfr. capacity is not a physical constant. It greatly varies with the alumina
nature or the electrochemical parameters. The present results agree with
ΔCt =
Cads .i.MEGA
= KB .
i
(13) the sedimentation investigation during electrocoagulation experiments
Qfr .nF Qfr which showed variations in the behavior of electro-generated alumina
Experimental results in the papers of Betancor-Abreu et al. and Mena [71].
et al. [56,57] confirm for a CEC that the fluoride anion removal in­ Fig. 12 shows the decrease of fluoride anion concentration during
creases with an increase of the electrolysis current. As expected from Eq. CEP for various current electrolysis. The concentrations followed
(13), the fluoride removal in a CEC [59] shows an increase of the decreasing exponential equations. Since stationary states were not
abatement ΔCt when the current increases and when the flow rate reached during the experiments, the results were used in a mathematical
decreases. modelling leading to Eq. (16) (see Appendix A1 in Supplementary Ma­
The results of the real wastewater treatment (Fig. 10) corroborated terials) where A and B are constants, C(t) and C(∞) are concentration at
that the fluoride removal reached a stationary state. From the observed time t and time = infinity, respectively.
abatement of 39.72 mg L− 1 for a current intensity of 0.5 A and a solution C(t) = A exp( − Bt) + C(∞) (16)
flow of 0.138 10− 3 L s− 1, an adsorption capacity of 47.87 mg g− 1 of EGA
was calculated. The present adsorption capacity of EGA may be The modelling concentrations at the infinity are equal to the con­
considered in good agreement with the capacity of 56.8 mg g− 1 obtained centrations at stationary state. With these results, adsorption capacities
by Jia et al. [51] for a bayerite/boehmite nano composite. were calculated leading to values gathered in Table 1. These calculated
adsorption capacities are lower than the values gathered in Fig. 11. All
3.3.3. Determination of adsorption capacity before reaching the steady- the calculated values which are in Table 1 and in Fig. 11 provide the
state same order of magnitude of literature values. The simulated concen­
At the time t, the quantity of adsorbed fluoride (Qads) is the sum (Eq. tration at stationary state allows the calculation of kinetic constants. For
(14)) of the amounts adsorbed in the EC reactor and that in the treated a first order kinetics, the adsorption constants k1 were calculated with
solution Vt (at the exit of the reactor). Eq. (8) leading to results which are gathered together in Table 2. The
adsorption constant is not a strong physicochemical characteristic of an
Qads = ΔCecr .V + Vt .ΔCct (14) adsorption process. In BEC predicted rate constants have been estab­
lished in the ranges 0.05–0.25 min− 1 [67] and 0.02–0.06 min− 1 [65].
ΔCecr = (C0 − Ct)ecr is the concentration variation in the EC reactor, V is
These rate constants depend on experimental parameters such as pH,
the reactor volume, Vt is the volume of the treated solution, and ΔCct = electrolysis current, initial fluoride concentration, distance between the
(C0 − Ct)ct is the concentration variation in the collecting tank. In the
electrodes, conductivity and temperature. Considering a possible
involvement of these parameters, the first order kinetic constants of

Fig. 10. Variation of residual concentrations of fluoride, nitrate anions and pH Fig. 11. Effect of the electrocoagulation current on the variation of the fluoride
during the CEP treatment of the real wastewater. Experimental conditions: cur­ anion adsorption capacities. Experimental conditions: nitrate concentration 0.1 g.
rent density = 9.09 mA cm− 2, Distance between electrodes = 18 mm, 1 g L− 1 L− 1; fluoride concentration 0.1 g. L− 1; initial pH = 5.83; Distance between
NaCl, [F‾] = 40.57 mg L− 1, [NO3‾] = 88.22 mg L− 1. electrodes = 18 mm; 1 g L− 1 NaCl.

8
H. Tounsi et al. Journal of Water Process Engineering 46 (2022) 102584

d[A]
= − k2 CA2 (17)
dt
The rate constant can be calculated from Eq. (2) which can be
rearranged in Eqs. (18)–(20) leading finally to the second order constant
k2 (Eq. (21)).

− k2 .V.C2 A − Qfr .CA + Qfr .CAin = 0 (18)

k2 .V.C2 A = Qfr .CAin − Qfr .CA (19)

Qfr
k2 = (CAin − CA ) (20)
V.C2 A

CAin − CA
k2 = (21)
τ CA2
The resolution of the second order Eq. (18) allows the determination
of the concentration inside the EC reactor or in the effluent (CAex).
Taking the positive root of Eq. (18), the concentration of the effluent is
calculated by Eq. (22). This concentration depends upon the rate con­
Fig. 12. Effect of EC current on the concentration of fluoride anion. Experi­ stant k2, the solution flow Qfr, the initial concentration of the solution
mental conditions: nitrate concentration 0.1 g. L− 1; fluoride concentration 0.1 g. CAin and the reactor volume V. For a targeted concentration of the
L− 1; initial pH = 5.83; Distance between electrodes = 18 mm; 1 g L− 1 NaCl.
effluent with known rate constant (k2) value, the experimental condi­
tions can be calculated by Eq. (22).
Table 1
( ( )1/2
− Qfr − Qfr 2 + 4k2 VQfr CAin
Adsorption capacities calculated from Eq. (11) with simulated stationary
CA = (22)
concentrations. 2k2 V
I (A) C0 (mg L− 1) ΔC (mg L− 1) Cads (mg g− 1) A set of results of rate constant is given in Table 2 for the removal of
0.3 100 (a) 82.0 163.7 fluoride, assuming that these removals follow a second order kinetics.
0.5 100 (a) 78.4 93.9 Results are in the range 0.94–2.29 L g− 1 min− 1. For BEC, few papers
0.5 40.5 (b) 39.2 46.9 reported the rate constants calculated with the same unity [72,73]. The
0.7 100 (a) 80.3 68.7
removal of fluoride anions, alone and in the presence of arsenic, follows
1.0 100 (a) 85.5 51.2
a pseudo-second order model with rate constants of 0.014 and 0.006 L
(a) synthetic solution; (b) real wastewater. mg− 1 min− 1 (or 14 and 6 L g− 1 min− 1) respectively [72]. The removal of
fluoride from synthetic ground water gives decreasing rate constants in
the range 62.9–5.3 L g− 1 min− 1 when the fluoride anion concentration
Table 2
increases from 3 to 12 mg L− 1 [71]. In these cited papers [72,73] models
Kinetic constants calculated from simulated stationary concentrations C/Aex.
of pseudo-first order and pseudo-second order were applied, and the
Current 5.45 9.09 12.72 18.08
second order model was found with better correlation coefficients R2.
density
(mA cm− 2) The results of the present study can be considered in the same order of
magnitude of literature values. But, the kinetic study of the CEP cannot
C/Aex 0.018 ± 0.022 ± 0.019 ± 0.015 ±
(g L− 1) 0.006 0.006 0.006 0.006
give a clear conclusion about the best occurrence of the kinetic order.
k1a 0.0250 ± 0.0200 ± 0.0230 ± 0.0330 ±
(min− 1) 0.0004 0.0004 0.0001 0.0003
k2b 1.410 ± 0.940 ± 1.170 ± 2.290 ± 3.5. Mechanism discussion of separate removal of fluoride and nitrate
(L g− 1 0.007 0.003 0.002 0.008 ions
min− 1)
a
First order kinetic constants were calculated using Eq. (8). 3.5.1. Fluoride anions removal by adsorption
b
Second order kinetic constants were calculated using Eq. (21). All the papers dealing with fluoride anions removal agree with an
adsorption process. There is no unanimity in the kinetics of fluoride
Table 2 are in the same order of magnitude of literature values. anions removal by adsorption onto the electro-generated aluminas.
Several papers dealing with a removal by BEC (Batch Electro Coagula­
3.4. Theory for a second order kinetics tion) have shown that the reaction followed a first order [65–67] or a
second order kinetics [74,75]. Adsorption onto five aluminas [76] and a
For a second order kinetics at steady-state operation conditions Eq. sludge resulting after the electrocoagulation [77] showed a second order
(2) can be written with the rate relation Eq. (17): kinetics.
d[A]
Qin CAin + V − Qex CAex = 0 (2) 3.5.2. Nitrate anions removal by adsorption or reduction
dt
All the papers reporting the treatment of nitrate anions by EC agree
With the following relations: with a removal, but there is no unanimity about the involved mecha­
Qin = Qex = Qfr nism. Few papers concluded that an adsorption occurred without giving
proof of such reactions [78,79]. In few papers, the nitrate removal was
[A] = CAex = CA reported due to the occurrence of adsorption and reduction [46–48,80].
For other authors, the nitrate removal was due to a reduction leading to
ammonium cation, ammonia and gaseous nitrogen compounds [68,69].
In the present paper, no proof for nitrate or ammonia adsorption was

9
H. Tounsi et al.
obtained by FTIR and XPS analysis of the sludge (Fig. S1, Fig. 7), and
ammonium was detected as a reduction product. The first order kinetics
of the nitrate removal is compatible with an exponential decrease of an
electro active substrate in an electrochemical reaction [81].
3.6. Treatment of the real wastewater
3.6.1. Compositions of the real wastewater before and after CEP
The treatment of wastewaters arising from semiconductor industries
has been carried out with BEC using aluminum or iron electrodes
[82–86] or with a CEP [87]. These wastewaters generally contain high
concentration of fluoride anions, silicate, calcium and CaF2 micropar­
ticles. The compositions of the real wastewater, before and after the CEP,
are given in Supplementary Materials (Table S1).
The variations of the concentrations of fluoride and nitrate anions
during a CEP are presented in Fig. 10. After this experiment, the con­
centrations of main elements are gathered in Table S1. As expected for
an EC treatment, all the heavy metals were quantitatively removed. In
addition, the other elements such as Ca, Mg and Si are also removed by
EC and show great abatements. The removal efficiency of nitrate and
fluoride anions was 53.1% and 97.9%, respectively, after 180 min of
CEP.
3.6.2. CEP treatment
At the end of the CEP, the residual concentrations of fluoride and
nitrate anions were lower than the regulated concentrations for this kind
of wastewater. Assuming that stationary states could be reached, it
would be possible to use Eq. (13) and fluoride adsorption capacity of
47.87 mg g− 1 to choose the EC current i and the solution flow Q for a
given concentration of the effluent. Since the fluoride adsorption ca­
pacity decreases when the current increases, according to Eq. (13), a
targeted concentration abatement ΔCt can be reached only with a
decrease of solution flux Qfr.
The effluent discharge regulations for the fluoride and nitrate anions
are 10 mg L− 1 [86] and 10 mg N L− 1 (or 44.28 mg NO3‾ L− 1) [89],
respectively. Based on the obtained results from Fig. 10, the regulated
concentrations of fluoride and nitrate were achieved after 30 min and
150 min respectively. It was the nitrate abatement which controlled the
wastewater treatment. Fig. 3 shows that an increase of the CEP current
does not improve the removal rate of nitrate anions. So, the experi­
mental conditions of the CEP are almost optimized for the used reactor
with a solution flow rate of 0.138 mL s− 1 and a current density of 9.09
mA cm− 2.
3.7. Efficiency, energy consumption and cost evaluation
The EC reactor is almost optimized. The energy and efficiency must
be calculated for the CEP current which allowed the obtaining of a
depolluted effluent. In the CEP, the energy consumption (ENC) is
calculated as a function of the volume of the effluent to be treated and it
is given by Eq. (23) where U is the electric voltage of the EC reactor (V), I
is the current (A), tCEP is the time of the treatment process (h) and V is the
volume of effluent to be treated (m3). The treatment for 3 h of 1.5 L with
a current of 0.5 A was performed with a voltage of 4.9 V or 9.4 V for a
synthetic solution or the real wastewater, and it gave ENC values of 4.9
kWh m− 3 or 9.4 kWh m− 3 for a synthetic solution or the real wastewater,
respectively.
(
kWh
)
UItCEP
ENC = (23)
m3 V
In the same conditions, the amount of electrode consumed (ELC) was
0.34 kg m− 3 on the basis of calculation by Faraday's law using Eq. (24)
where I (A) is the EC current, t (s) is the duration of the EC, M is the
molecular weight of Al, n (= 3) the electron number, F the Faraday
constant and V (m3) the volume of treated solution.
10
Journal of Water Process Engineering 46 (2022) 102584
( ) 3
kg I.t.M.10−
ELC = (24)
m3 n.F.V
The treatment cost (TC) of the CEP must include the costs of all
consumed electricity (in the EC reactor and for the pumping of solution),
electrode material (Al) and the consumed chemicals (excluding the costs
of sodium fluoride and sodium nitrate), and the cost of the sludge sep­
aration and treatment.
The treatment cost (TC) for the synthetic and real wastewaters is
calculated in Appendix 2, only with known terms of electricity
consumed in the EC reactor, 130% of the electrode material calculated
with the Faraday law, and the consumed sodium chloride and sodium
hydroxide. The consumed electrode material is always greater than the
calculated value. TC of 2.1792 USD per m3 and 2.3097 USD per m3 were
found for the synthetic solution and the real wastewater, respectively.
The most important costs are the aluminum material and the sodium
hydroxide used in the pH control. There is only a slight effect of the
voltage on TC. An improvement of TC could be obtained thanks to the
change of sodium hydroxide by a cheaper base.
In the present CEP treatment, it was not possible to reach the regu­
lated concentrations [88] of both fluoride and nitrate anions. The
treatment of the real wastewater showed that the removal of nitrate
anions was the determining step of the process, and it was observed after
160 min of EC which correspond to 1.33 L of treated solution. But this
does not involve a modification of the calculated ENC and ELC.
Thakur et al. [90] and Mena et al. [57] performed similar type of
continuous process at low cost (less than 0.4 USD) per m3 and achieved
the removal efficiency of 87–94% but using synthetic fluoride solutions
between 9 mg L− 1 and 12 mg L− 1, respectively. In the present work, the
cost was greater for more concentrated solutions. Moreover, it was the
removal of nitrate anions which needed a more expensive treatment.
Remarkably, the present contribution extended the practicability of CEP
in the treatment of a real wastewater which contained 80.22 mg L− 1 of
nitrate anions and 40.57 mg L− 1 of fluoride anions. Moreover, as shown
by the concentrations in Table S1, the EC treatment is efficient in the
removal of Si, Na, Mg, K, Cr, Cu, Al, Pb, Mn, Fe, Ni, P and Zn ions present
in real wastewater.
4. Conclusions
In the present research contribution, the simultaneous removal of
fluoride and nitrate anions was investigated by using a CEP. The EDS
analysis, XPS spectra and XRD patterns confirmed that fluoride anions
were adsorbed onto the electro-generated aluminas, and that nitrate
anions were reduced during the process.
The CEP was applied to a real wastewater which contained high
concentrations of fluoride and nitrate anions. The recommended
discharge regulation of fluoride was reached faster than the one of ni­
trate anions. The application of this treatment in a microelectronic in­
dustry would need a change in the electrocoagulation reactor, such as a
greater cathode than anode, or by using another cathode nature in order
to improve the nitrate anion removal by reduction.
From an engineering point of view, the theoretical behavior of CEP
which was developed in the present paper would need to be extended to
other pollutants with various changes in the reactor structure.
CRediT authorship contribution statement
H. Tounsi – Investigation.
T. Chaabane – Conceptualization and methodology & Supervision.
K. Omine – Supervision.
V. Sivasankar – Writing – Review and Editing.
H. Sano – Resources.
M. Hecini – Resources.
A. Darchen – Writing Original Draft & Writing – Review and Editing.
H. Tounsi et al.
Uncited reference
[88]
Declaration of competing interest
The authors declare that they have no known competing interests or
personal relationships that could have appeared to influence the work
reported in this paper.
Acknowledgements
We would like to thank the heads of the collaborating institute,
namely Research Center in Semiconductor Technology for Energy
(CRTSE, Algiers, Algeria), P.G. and Research Department of Chemistry
of Pachaiyappa's College (Chennai, India), Nagasaki University (Japan),
USTHB (Algiers, Algeria), CNRS and National College of Chemistry
(ENSCR, Rennes, France). Ms. H. Tounsi deeply thanks the Director of
CRTSE for giving her the opportunity to carry out research at Geo-
technological Laboratory, Nagasaki University, Japan under the super­
vision of Prof. Kiyoshi Omine and the Ministry of Higher Education and
Scientific Research (MESRS, Algeria) for the financing of her internship.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jwpe.2022.102584.
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