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Article history: Co-existence of arsenic and fluoride in groundwater has raised severe health issues to living being. Thus,
Received 12 May 2016 the present research has been conducted for simultaneous removal of arsenic and fluoride from synthetic
Received in revised form groundwater by using electrocoagulation process with aluminum electrode. Effects of initial pH, current
16 December 2016
density, run time, inter electrode distance and NaCl concentration over percentage removal of arsenic
Accepted 21 December 2016
and fluoride as well as operating cost have been studied. The optimum experimental conditions are
found to be initial pH: 7, current density: 10 A/m2, run time: 95 min, inter electrode distance: 1 cm, NaCl
concentration: 0.71 g/l for removal of 98.51% arsenic (initial concentration: 550 mg/l) and 88.33% fluoride
Keywords:
Electrocoagulation
(initial concentration: 12 mg/l). The concentration of arsenic and fluoride in treated water are found to be
Synthetic groundwater 8.19 mg/l and 1.4 mg/l, respectively, with an operating cost of 0.357 USD/m3 treated water. Pseudo first
Real groundwater and second order kinetic model of individual and simultaneous arsenic and fluoride removal in elec-
Arsenic removal trocoagulation have also been studied. Produced sludge characterization studies also confirm the pres-
Fluoride removal ence of arsenic in As(III) form, and fluoride in sludge. The present electrocoagulation process is able to
Operating cost reduce the arsenic and fluoride concentration of synthetic as well as real groundwater to below 10 mg/l
and 1.5 mg/l, respectively, which are maximum contaminant level of these elements in drinking water
according to WHO guidelines.
© 2016 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.jenvman.2016.12.053
0301-4797/© 2016 Elsevier Ltd. All rights reserved.
L.S. Thakur, P. Mondal / Journal of Environmental Management 190 (2017) 102e112 103
more toxic than As(V) (Kobya et al., 2011). Very recently in 2015, h i
high arsenic and fluoride concentration has been reported in the AlðOHÞ3ðsÞ þ HAsO2 2
4 / AlðOHÞ3 HAsO4 (4)
s
groundwater of Rajnandgaon district of Chhattisgarh in India (Patel
et al., 2015). Hence, it is an urgent need to find a technology which The mechanism of fluoride removal in electrocoagulation is still
can efficiently remove arsenite and fluoride both from not fully understood. This stems mainly from the fact that at least
groundwater. three mechanisms may compete (Zhu et al., 2007):
From literature it is revealed that many approaches such as
adsorption, chemical coagulation, membrane filtration, electrodi- (a) Adsorption on aluminum hydroxide particles
alysis, oxidation, biological methods etc. are applied for removal of
arsenic and fluoride from contaminated water (Liu et al., 2012; AlðOHÞ3 þ xF /AlðOHÞ3x Fx þ xOH (5)
Mohan and Pittman, 2007; Amor et al., 2001; Castel et al., 2000).
All these technologies mentioned above suffer from various dis-
(b) Coprecipitation
advantages; for examples the adsorption process is pH dependent,
it requires pre-treatment step, high treatment time, and its nAl þ ð3n mÞOH þ mF / Aln Fm ðOHÞ3nm (6)
contamination removal efficiency reduces after each regeneration
cycle (Kobya et al., 2011; Mohan and Pittman, 2007). Coagulation
method requires a large amount of chemical, large area for treat- (c) Fluoride attachment to electrodes.
ment and produces a secondary sludge (Kobya et al., 2011;
Balasubramanian et al., 2009). High membrane and operating Many studies are available on removal of arsenic and fluoride
cost, skilled labour requirement, and concentrated sludge genera- from aqueous solution by applying electrocoagulation process (Ali
tion are major drawbacks associated with the membrane filtration et al., 2012; Flores et al., 2013; Lacasa et al., 2011; Song et al.,
technologies (Balasubramanian et al., 2009; Lacasa et al., 2011). 2014a; Ghosh et al., 2008; Zhu et al., 2007; Zuo et al., 2008; Zhao
Whereas, biological processes, are mainly used for treatment of et al., 2009; Un et al., 2013). All these studies were conducted for
industrial waste water and not for drinking water, as the processes removal of arsenic or fluoride separately. While, Zhao et al. (2011)
require several types of pathogenic and non-pathogenic microor- had designed and used an integrated electro-oxidation and elec-
ganisms like algae, yeast, fungi, bacteria etc. Moreover, their trocoagulation process for simultaneous removal of arsenite and
selectivity depends on type of contaminants which has to be fluoride. Titanium based dimensionally stable anode with different
removed (Veglio and Beolchini, 1997). High treatment time, large combination of Fe and Al electrode were used in their research
land area requirement, less design flexibility are additional draw- work. Cost of any treatment process is a significant factor associated
backs of biological processes (Veglio and Beolchini, 1997; Yadav with their implementation. Since, titanium based electrode was
et al., 2012). used, hence their cost of treatment was high. Although, no cost
In comparison to above conventional treatment methods, elec- estimation study was performed by them. Moreover, initial con-
trocoagulation process has drawn attention of researchers due to its centrations of arsenite and fluoride were 1 mg/l and 4.5 mg/l,
high removal efficiency, easy to operate, cost effectiveness and respectively. However, in real groundwater, the concentration of
possibility of complete automation of process (Rajeshwar et al., arsenic is found less (<500 mg/l) and fluoride concentration is found
1994; Chen, 2004; Mollah et al., 2004; Emamjomeh and higher (>10 mg/l) (Neva rez et al., 2011; Aiuppa et al., 2000; Jadhav
Sivakumar 2009). In electrocoagulation process insitu generated et al., 2015). Patel et al. (2015) also reported the presence of arsenic
metal hydroxides act as coagulant in aqueous solution, which and fluoride in groundwater of Rajnandgaon district of Chhattis-
provides the active sites for adsorption of polluting species. Apart garh, India, in which most of the sample contains arsenic concen-
from adsorption, sweep coagulation, bridge coagulation, copreci- tration <575 mg/l and fluoride concentration >10 mg/l. According to
pitation etc. also play a role for the removal of pollutants in elec- the information available, no study has been performed for
trocoagulation process. The electrochemical reactions using Al as simultaneous removal of arsenic and fluoride in these range by
electrode materials may be summarized as follows (Kobya et al., electrocoagulation along with cost estimation.
2011): In the present study, the lab experiments in batch mode have
Reaction at anode been performed at constant initial arsenic and fluoride concentra-
tion, to investigate the effects of initial pH, current density, run
Al/Al3þ þ 3e (1) time, inter electrode distance and NaCl concentration on percent-
age removal of arsenic and fluoride as well as operating cost of
Reaction at cathode
treatment. Removal of arsenic and fluoride mainly depends on their
initial concentration. Hence, variation of initial concentration on
2H2 O þ 2e /H2 þ 2OH (2)
their removal efficiency has also been studied. Furthermore, the
Reaction in aqueous solution kinetic studies for individual and simultaneous arsenic and fluoride
removal in electrocoagulation have also been performed to eval-
Al3þ þ 3OH /AlðOHÞ3ðsÞ (3) uate the reaction rate constants as well as interactions. To explore
the mechanism of removal of arsenic and fluoride, produced sludge
In electrocoagulation aluminum and hydroxides ion generated characterization has been conducted by Field emission scanning
by reactions (1) and (2), react together and form various species of electron microscopy (FESEM), X-ray diffraction (XRD) and Fourier
monomeric such as AlðOHÞþ 4þ 2þ
2 , Al2 ðOHÞ2 , AlðOHÞ , AlðOHÞ4 and
transform infrared spectroscopy (FTIR).
polymeric species viz. Al6 ðOHÞ3þ 15 , Al7 ðOHÞ 4þ
17 , Al 8 ðOHÞ4þ
20 ,
5þ 7þ
Al13 ðOHÞ34 , Al13 O4 ðOHÞ24 (Ghosh et al., 2008; Rinco n and La
Motta, 2014). This species are further transformed into amor- 2. Materials and methods
phous AlðOHÞ3ðsÞ according to complex precipitation kinetics
(Behbahani et al., 2011). Furthermore, this AlðOHÞ3 complex is 2.1. Materials
believed to adsorb arsenic (Kobya et al., 2011; Flores et al., 2013)
and fluoride (Hu et al., 2003). All chemicals used in the present experiment were of analytical
104 L.S. Thakur, P. Mondal / Journal of Environmental Management 190 (2017) 102e112
grade. Stock solutions of arsenite (As(III)) and fluoride (1000 mg/l) water, while a and b are coefficient for Indian market in year 2015,
were prepared from sodium arsenite (NaAsO2) and sodium fluoride respectively.
(NaF) salt, respectively. Desired concentration of arsenite and Coefficient a: Wholesale electrode material price ¼ 1.77 USD/kg
fluoride were made from the dilution of stock solution in distilled Al (Web link 1).
water. Initial pH of solution was adjusted by using 1 N NaOH and Coefficient b: Industrial electricity price ¼ 0.08 USD/kwh1
1 N HCl solution. (Web link 2).
Energy consumption in electrocoagulation process was calcu-
2.2. Experiment setup lated by Eq. (9).
Experiments were carried out in a Perspex made batch reactor kwh voltage current runtime
Energy consumption ¼
having dimension of 0.15 m 0.10 m 0.12 m with working vol- m3 working volume of reactor
ume of 1.4 l (Behbahani et al., 2011). Four Al electrodes (97.4% pu- (9)
rity) were fitted in monopolar mode with total effective surface
area of 512 cm2. DC power supply of range 0e30 V and 0e10 A was Cost of electrode material was considered in term of material
used to conduct electrocoagulation. loss in electrocoagulation process by subtracting the initial weight
and final weight of anode electrode before and after electro-
coagulation process.
2.3. Procedure
To evaluate the removal rate constant, which depends on the
initial arsenic and fluoride concentration, further experiments were
Aluminum electrodes were rubbed with sand paper and then
performed in single and bi-component solution at the optimized
dipped in dilute nitric acid solution and distilled water for surface
conditions. The removal kinetics of arsenic and/or fluoride on the
cleaning. After cleaning, electrodes were dried at 105 C and then
amount of electrochemically dissolved aluminum oxyhydroxides
weighted. Working solution composed of fix concentration of
were described by pseudo-kinetic models. The rate of removal of
550 mg/l arsenite and 12 mg/l fluoride was treated in batch elec-
arsenic and fluoride can be represented by the following nth order
trocoagulation at 500 rpm by using magnetic stirrer. The effects of
mechanism:
initial pH, current density, run time, inter electrode distance and
NaCl concentration were studied at different conditions as listed in
dC
Table 1. At the end of electrocoagulation, the solution was filtered ¼ kCn (10)
dt
through 0.45 m filter and analyzed for arsenic and fluoride detec-
tion. All experiments were performed thrice and the average values where, C represents the arsenic/fluoride concentration, k is the rate
are reported. In addition, after the electrocoagulation experiment constant, n is the order of reaction, and t is the run time. For a
produced sludge was dried at 105 C temperature for sludge pseudo first order reaction, the integration of above Eq. (10) yields;
analysis.
The percentage removal of contaminant was calculated from Eq. Ct
ln ¼ k1 t (11)
(7) Ci
Ci Co A slope of graph of ln CCti versus run time (t) gives the value of
Removal ð%Þ ¼ 100 (7) 1
rate constant k1 (min ). Here, Ci is the initial arsenic/fluoride
Ci
concentration, Ct is the concentration values at run time t.
where, Ci and Co are initial and final concentration of contaminants Furthermore, for the pseudo second order reaction, above Eq. (10)
in solution. becomes;
Visual MINTEQ simulation program was used for single
component speciation of As(III), fluoride and aluminum at different 1 1
¼ k2 t (12)
initial pH (1e14) putting the fixed temperature value of 25 C. Ct Ci
Implementation feasibility of any treatment process in large A slope of graph between C1t versus run time (t) gives the value of
scale depends mainly on cost of treatment process. Operating cost rate constant k2 (l/(mg min)).
of electrocoagulation process includes cost of electrode, chemical,
electricity, sludge disposal, fixed cost etc. In the present study,
electrode material cost and electricity charges were taken in ac- 2.4. Analysis
count for preliminary economic evaluation (Daneshvar et al., 2006)
2.4.1. Inductively coupled plasma mass spectrometry and ion
Operating cost ¼ a CElectrode þ b CEnergy (8) selective electrode
Arsenic analysis was carried out by Inductively Coupled Plasma
where, CElectrode (kg Al/m3) and CEnergy (kwh/m3) are consumption Mass Spectrometer (ICP-MS, Perkin Elmer, model ELAN-DRC-e)
of quantities for the treatment of arsenic and fluoride contaminant according to standard method USEPA 200.8 (Creed et al., 1994).
Table 1
Range of operating parameters for arsenic and fluoride removal by electrocoagulation.
Type of experiments Initial Current density Run time Inter electrode NaCl Initial As(III) Initial F
pH (A/m2) (min) distance concentration concentration concentration
(cm) (g/l) in mg/l in mg/l
While, fluoride analysis was carried out by Ion meter (Orlab India,
model-OR930) coupled with compatible fluoride ion selective
electrode. To prevent the interference of other ions in fluoride
detection, TISAB buffer was added to each aliquot with the volume
ratio of 1:1. This is a solution containing sodium chloride, acetic
acid, sodium hydroxide and 1,2-cyclohexylene diamine tetra acetic
acid (Thakur and Mondal, 2016).
of X-ray powder diffraction patterns maintained by the Interna- AlðOHÞ 4 , Al6 ðOHÞ 3þ
15 , Al7 ðOHÞ 4þ
17 , Al8 ðOHÞ 4þ
20 , Al 13 ðOHÞ 5þ
34 ,
tional Centre for Diffraction Data (ICDD) as well as published Al13 O4 ðOHÞ7þ24 etc. can be formed in aqueous solution (Rebhun and
literature. Lurie, 1993). These species may further transform into amorphous
AlðOHÞ3ðsÞ according to complex precipitation kinetics (Behbahani
2.4.5. Statistical analysis et al., 2011). Freshly formed amorphous AlðOHÞ3 has minimum
Experimental data were subjected to statistical analysis. solubility and is finally polymerized to Aln ðOHÞ3n , which results
into dense flocs formation (Kobya et al., 2006, 2011; Behbahani
3. Results and discussion et al., 2011). The presence of common ions in the solution may
slightly influence the formation of these intermediates (Mouedhen
The effects of initial pH, current density, run time, inter elec- et al., 2008), thus, further investigation is required for better un-
trode distance, and NaCl concentration on percentage removal of derstanding of the process and to determine the intermediates
arsenic and fluoride as well as operating cost are discussed below. under common ion effects. The dense floc has large surface area,
The standard deviations of experimental data are found in range of which provides entrapment of colloidal arsenic particles and thus,
0 to 1.5. the arsenic removal occurs (Ouaissa et al., 2014). Hence, at initial
acidic pH range, entrapment of arsenic in flocs and elevation in
3.1. Effect of initial pH solution pH are accountable for high arsenic removal. It is ascer-
tained from Fig. 2a that as the pH increases to 7, neutral form of
The pH of a solution is one of the most significant parameter arsenite H3 AsO3 decreases slightly, as well as negatively charged
that governs the removal of arsenic and fluoride in electro- H2 AsO 3 increases. Although, at these pH positive charged AlðOHÞ3
coagulation. To investigate this effect, a series of experiments are moiety (Fig. 2b) dominates in bulk solution, hence removal in-
performed according to the parameters mentioned in Table 1. It is a creases due to charge neutralization and is found maximum at
highlighted fact that pH of the solution increases during electro- initial pH 7. As initial pH increases to above 7, amount of negative
coagulation (Fig. 1) for the formation of OH ions and H2 (Vik et al., charge of arsenite and AlðOHÞ3 increases. Therefore, percentage
1984; Chen et al., 2000) gas at the cathode according to Eq. (2). arsenic removal decreases due to charge repulsion. It is also note-
Fig. 1 shows the effects of initial pH on percentage removal of worthy to mention that for initial pH of 11 the solution pH reduces
arsenic and fluoride as well as also depicts the plot of initial pH and to 9.5 which is attributed to amphoteric aluminum hydroxide
final pH of solution before and after electrocoagulation. Final pH of behavior (Eq. (13)), leading to decline in pH (Song et al., 2014b). Due
solution is found to 8.4 for all the initial pH values (3e11). Arsenic to this reason high As(III) removal is observed even at initial pH
and fluoride removal depends on both initial pH and elevation of of 11.
pH during electrocoagulation. In aqueous solution arsenite (As(III))
species are present in the form of H3 AsO3 , H2 AsO 2
3 , HAsO3 , while AlðOHÞ3 ðsÞ þ ðOHÞ ðaqÞ/AlðOHÞ
4 ðaqÞ (13)
fluoride is present in HF and F form. Speciation of arsenic and
fluoride changes with pH of solution and redox potential. Similarly, The FTIR spectra (Fig. 8e) also confirms the presence of As(III) in
the aluminum ion speciation also changes with the solution pH. the produced sludge. In case of fluoride, percentage removal is
Thus, in electrocoagulation process arsenic and fluoride removal found maximum (95.83%) at initial pH 3 and then decreases
changes with solution pH. continuously with increase in pH. It is revealed from Fig. 2c that
It is evident from Fig. 1 that percentage arsenic removal in- negative charge fluoride and positive charge AlðOHÞ3 are domi-
creases from 93.61% at acidic initial pH 3 to 98.43% at neutral initial nated at pH 3. Hence, maximum removal of fluoride is observed
106 L.S. Thakur, P. Mondal / Journal of Environmental Management 190 (2017) 102e112
Fig. 2. Distribution of species as a function of pH, a) Arsenite, b) Aluminum, c) Fluoride in solution simulated by Visual MINTEQ version 3.1. (Song et al., 2014b).
due to charge neutralization. The drop in percentage removal of current I (A) passed for a period of time t (s), M is molecular mass of
fluoride occurs with the increment in initial pH, it is attributed due Al (26.98 g/mol), Z is number of electron transferred (Z ¼ 3 for Al), F
to reduction in positive charged AlðOHÞ3 colloidal particles. As is Faradays constant (96,485 C/mol), V is volume (m3). It is ascer-
initial pH increases to above 8, the removal decreases further due to tained from Eq. (14) that as more current passes through process,
presence of negative charge fluoride and AlðOHÞ 4 species in solu- more amount of coagulant and bubble generate, which increase
tion. No significant effect of pH is observed on operating cost, as for mixing intensity inside electrocoagulation process. Thus, increasing
cost calculations only anode mass loss and electricity consumption current density would accelerate the liberation rate of Al3þ and
were considered (Eq. (8)). FTIR and XRD spectra (Fig. 8e and f) also OH ions, which further help to accelerate the removal efficiency.
prove the presence of fluoride in the produced sludge. To understand the effect of current density on operating cost,
percentage removal of arsenic and fluoride, several lab experiments
have been performed at different current densities in the range of
3.2. Effect of current density 10e60 A/m2. Fig. 3 represents the effect of current density on
operating cost and percentage removal of arsenic and fluoride. It
Current density plays an important role for removal of arsenic could be seen from Fig. 3 that at current density 10 A/m2 operating
and fluoride in electrocoagulation process, as it determines rate of cost, percentage removal of arsenic and fluoride are found
coagulant dosage, bubble production, size and growth of flocs, 0.269 USD, 96.11% and 83.33%, respectively. Incremental increased
which influence the removal efficiency of electrocoagulation. Cur- in operating cost, percentage removal of arsenic and fluoride are
rent density is a measure of amount of current passed through unit observed with increased in current density. At current density 40 A/
cross section area. According to Faraday law (Eq. (14)), loss in m2 and above the residual concentration of arsenic and fluoride
weight of material is proportional to quantity of electricity passed reduce to 10 mg/l and 1.5 mg/l, respectively, which comes under
in solution during electrocoagulation. the safe drinking water according to WHO guidelines. Maximum
percentage removal of arsenic (99.47%) and fluoride (91.66%) are
MIt
Celec thero ¼ (14) found at current density 60 A/m2. It is mainly attributed due to the
ZFV generation of high amount of Al3þ and OH ions at anode and
where Celect is theoretical amount of aluminum produced by cathode, respectively, and combination of these to form AlðOHÞ3 ,
thero
L.S. Thakur, P. Mondal / Journal of Environmental Management 190 (2017) 102e112 107
Fig. 4. Effect of run time on removal of arsenic and fluoride, operating cost (Initial As Fig. 5. Effect of inter electrode distance on removal of arsenic and fluoride, operating
concentration: 550 mg/l, F concentration: 12 mg/l, NaCl concentration: 0.71 g/l, initial cost (Initial As concentration: 550 mg/l, F concentration: 12 mg/l, NaCl concentration:
pH: 7, current density: 10 A/m2, inter electrode distance: 1 cm). 0.71 g/l, initial pH: 7, current density: 10 A/m2).
108 L.S. Thakur, P. Mondal / Journal of Environmental Management 190 (2017) 102e112
3.6. Effect of variation of initial arsenic and fluoride concentration Fig. 7. Effect on removal of a) arsenic in presence of fluoride. b) fluoride in presence of
on their removal arsenic (Initial As concentration: 300e1250 mg/l, F concentration: 5e20 mg/l, NaCl
concentration: 0.71 g/l, initial pH: 7, current density: 10 A/m2, inter electrode distance:
1 cm).
It is revealed from Fig. 7a that removal of arsenic (initial con-
centration: 550 mg/l) decreases from 99.05, 98.65, 95.39 and 94.15%
with the increase in initial fluoride concentration from 5, 10, 15 and
20 mg/l, respectively. Similarly, removal of fluoride (initial con- 3.7. Real groundwater study
centration: 15 mg/l) also decreases from 87.33, 85.33, 84.66 and
84% with the increase in initial arsenic concentration from 300, The performance of electrocoagulation process was also evalu-
550, 900, 1250 mg/l. Similar trends of decrease in percentage ated for the removal of arsenic and fluoride from real groundwater
removal are also observed with the other initial arsenic and fluoride sample collected from Kaudikasa village, Rajnandgaon district,
concentration as shown in Fig. 7a and b. It is due to the preferential Chhattisgarh, India. The initial characteristics of groundwater was
adsorption of high amount of available ions in the solution as pH: 6.8, D.O.: 4 mg/l, turbidity: 17 NTU. Other parameters are
compared to less amount ion as the dose of coagulant remains same mentioned in Table 2. At optimum conditions (Initial pH: 7, current
in electrocoagulation. It is also evident from Fig. 7a and b, that density: 10 A/m2, run time: 95 min), electrocoagulation process
removal of both arsenic and fluoride is responsive to alteration of successfully reduced the arsenic and fluoride concentration to
their initial concentration. below maximum contaminant level according to WHO drinking
water guidelines (removal As: 98.41%, F: 96.69%) along with
reduction of nitrate, iron, phosphate and total hardness as shown in
Table 2.
Evaluation of present process with some reported literature on
the removal of arsenic and fluoride individually or simultaneously
from water through electrocoagulation process are listed in Table 3.
There is only one literature for the simultaneous removal of As and
F through electrocoagulation in which no economic evaluation is
reported. Further, the precise comparison of the performance and
operating cost of present process with the other are difficult, since
the initial concentration, electrode material, operating conditions
etc. are not similar in these studies. From Table 3 it seems that the
operating cost of the present process with F concentration 12 mg/l
and As(III) concentration 550 mg/l, is lower than the operating cost
of the process reported by Ghosh et al., 2008 with 10 mg/l F con-
centration. Most of the studies have not provided cost comparison.
Fig. 6. Effect of NaCl concentration on removal of arsenic and fluoride, operating cost From this it is evident that the present process is highly competitive
(Initial As concentration: 550 mg/l, F concentration: 12 mg/l, initial pH: 7, current
to others.
density: 10 A/m2, inter electrode distance: 1 cm).
L.S. Thakur, P. Mondal / Journal of Environmental Management 190 (2017) 102e112 109
Table 2 Table 4
Initial characteristics of real groundwater and their removal. Kinetic rate constants with pseudo first order and pseudo second order models for
arsenic and/or fluoride removal.
Initial concentration (mg/l) Removal (%)
Pseudo first order model Pseudo second order model
As 512a 98.41
F 6.3 96.69 k1 (min1) R2 K2 ((l/(mg min)) R2
Iron 3.5 97.14
Individual
Nitrate 42 30.95
As 0.064 0.899 4.747 0.949
Phosphate 3 82.12
F 0.018 0.887 0.014 0.981
Total hardness 105 73.33
Simultaneous
a
mg/l. As 0.046 0.948 1.004 0.922
F 0.009 0.895 0.006 0.958
Table 3
Evaluation of the performance of some electrocoagulation processes along with operating cost for the individual and simultaneous removal of arsenic and fluoride (Thakur and
Mondal, 2016).
Type of electrode Parameters Initial concentration Removal (%) Operating cost (USD/m3) Reference
Simultaneous
Al pH: 7, Current density: 10 A/m2, run time: 95 min, As(III): 550 mg/l As: 98.51 0.357 This study
Electrode distance: 1 cm F: 12 mg/l F: 88.33
DSAa pH: 7, Current density: 40 A/m2, run time: 40 min, As(III): 1000 mg/l As: 99 e Zhao et al. (2011)
Fe Electrode distance: 0.02 cm F: 4.5 mg/l F: 77.7
Al
Individual
AleFe pH: 4, Current density: 300 A/m2, run time: 60 min, As(III): 13,400 mg/l As: >99.6 e Gomes et al., 2007
Electrode distance: 3 cm
AleAl pH: 4, Current density: 300 A/m2, run time: 60 min, As(III): 13,400 mg/l As: 97.8 e Gomes et al., 2007
Electrode distance: 3 cm
FeeFe pH: 2.4, Current density: 300 A/m2, run time: 60 min, As(III): 13,400 mg/l As: 97.2 e Gomes et al., 2007
Electrode distance: 3 cm
Fe pH: 6.5, Current density: 2.5 A/m2, run time: 12.5 min, As(III): 150 mg/l As: 93.5 0.022 Kobya et al., 2011
Electrode distance: 1.3 cm
Al pH: 7, Current density: 2.5 A/m2, run time: 15 min, As(III): 150 mg/l As: 95.7 0.019 Kobya et al., 2011
Electrode distance: 1.3 cm
Al pH: 8, Current density: 625 A/m2, run time: 45 min, F: 10 mg/l F: >90 For monopolar connection- 0.38 Ghosh et al., 2008
Electrode distance: 5 cm For bipolar connection- 0.62
a
DSA- Dimensionally stable electrode.
110 L.S. Thakur, P. Mondal / Journal of Environmental Management 190 (2017) 102e112
Fig. 8. a) SEM image b) existence of arsenic c) existence of fluoride d) EDX image e) FTIR spectra f) XRD pattern of produced sludge.
at 2q ¼ 67, 76 and 81 (ICDD data base). The FTIR and XRD analysis of pH: 7, current density: 10 A/m2, run time: 95 min, inter electrode
sludge confirm once again that arsenic and fluoride are linked with distance: 1 cm, NaCl concentration: 0.71 g/l at initial arsenic and
aluminum hydroxide complexes. fluoride concentration 550 mg/l and 12 mg/l, respectively. Under the
optimized condition, the concentration of arsenic and fluoride in
4. Conclusion treated water are found to be 8.19 mg/l (% removal: 98.51%) and
1.4 mg/l (% removal: 88.33%), respectively, with an operating cost of
Arsenic and fluoride contaminated groundwater can be effec- 0.357 USD/m3 treated water. Removal of both arsenic and fluoride is
tively treated by using electrocoagulation process. The optimum found responsive to the alteration of their initial concentration.
condition for arsenic and fluoride removal are found to be initial Reaction rate of individual arsenic and fluoride removal in
L.S. Thakur, P. Mondal / Journal of Environmental Management 190 (2017) 102e112 111
electrocoagulation follows pseudo second order kinetic model. Gomes, J.A.G., Daida, P., Kesmez, M., Weir, M., Moreno, H., Parga, J.R., Irwin, G.,
McWhinney, H., Grady, T., Peterson, E., Cocke, D.L., 2007. Arsenic removal by
Although, in simultaneous arsenic and fluoride removal, arsenic
electrocoagulation using combined AleFe electrode system and characteriza-
follows both pseudo first and pseudo second order kinetics; fluo- tion of products. J. Hazard. Mater. 139, 220e231.
ride follows pseudo second order kinetics. Analyzing the charac- Gomez, M.L., Blarasin, M.T., Martínez, D.E., 2009. Arsenic and fluoride in a loess
teristics of the sludge it seems that some amount of arsenic is aquifer in the central area of Argentina. Environ. Geol. 57, 143e155.
Gross, U., Rudiger, S., Mukhopadhyay, S., Kemnitz, E., Bailey, C., Brzezinka, K.,
removed as As(III), and the entrapment of As(III) in the aluminum Wander, A., Harrison, N., 2007. Vibrational analysis study of aluminum tri-
oxides floc (sweep coagulation) is a possible mechanism for As(III) fluoride phases. J. Phys. Chem. A 111, 5813e5819.
removal along with other phenomena like bridge coagulation He, J., Ma, T., Deng, Y., Yang, H., Wang, Y., 2009. Environmental geochemistry of high
arsenic groundwater at western Hetao plain, Inner Mongolia. Front. Earth Sci.
(adsorption), co-precipitation etc. Real groundwater sample China 3, 63e72.
collected from Kaudikasa village, Rajnandgaon district, Chhattis- Hu, C.Y., Lo, S.L., Kuan, W.H., 2003. Effects of co-existing anions on fluoride removal
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