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Removal of arsenic from water by electrocoagulation

P. Ratna Kumar a, Sanjeev Chaudhari


, Kartic C. Khilar a, S.P. Mahajan

Department of Chemical Engineering, IIT Bombay, Powai, Mumbai 400076, India

Centre for Environmental Science and Engineering, IIT Bombay, Powai, Mumbai 400076, India

In the present study electrocoagulation (EC) has been evaluated as a treatment technology for arsenite [As(III)] and
arsenate [As(V)] removal from water. Laboratory scale experiments were conducted with three electrode materials
namely, iron, aluminum and titanium to assess their eciency. Arsenic removal obtained was highest with iron electrodes. EC was able to bring down aqueous phase arsenic concentration to less than 10 lg l1 with iron electrodes.
Current density was varied from 0.65 to 1.53 mA cm2 and it was observed that higher current density achieved rapid
arsenic removal. Experimental results at dierent current densities indicated that arsenic removal was normalized with
respect to total charge passed and therefore charge density has been used to compare the results. Eect of pH on arsenic
removal was not signicant in the pH range 68. Comparative evaluation of As(III) and As(V) removal by chemical
coagulation (with ferric chloride) and electrocoagulation has been done. The comparison revealed that EC has better
removal eciency for As(III), whereas As(V) removal by both processes was nearly same. The removal mechanism of
As(III) by EC seems to be oxidation of As(III) to As(V) and subsequent removal by adsorption/complexation with
metal hydroxides generated in the process.

Keywords: Electrocoagulation; Arsenite; Arsenate; Chemical coagulation

1. Introduction
Arsenic in drinking water is a worldwide concern.
Arsenic contamination in ground water of Bangladesh
and West Bengal state of India is well known. More than
100 million people have been reported to be at risk due
to the consumption of arsenic from ground water for
drinking purposes. Arsenic is a carcinogen and its
ingestion may deleteriously aect the gastrointestinal
tract, cardiac, vascular system and central nervous system (Farrell et al., 2001). Due to its high toxic eects on
human health, recently the USEPA has lowered the

maximum contaminant level for arsenic in drinking

water from 50 to 10 lg l1 .
Arsenic contamination of the ground water occurs by
both natural processessuch as weathering of arsenic
containing minerals and anthropogenic activitiessuch
as uncontrolled industrial discharge from mining and
metallurgical industries, and application of organoarsenical pesticides (Krishna et al., 2001). Inorganic
arsenic is predominantly present in natural waters.
Arsenate [As(V)] and arsenite [As(III)] are primary
forms of arsenic in soils and natural waters (Ferguson
and Gavis, 1972). As(III) is more mobile in groundwater
and 2560 times more toxic than As(V). The concentration of arsenic species is mainly dependent on redox
potentials (Masscheleyn et al., 1991) and pH (Hering
et al., 1996). Under low pH and mildly reducing conditions (>100 mV), As(III) is thermodynamically stable
and exists as arsenious acid (H3 AsO03 , H2 AsO
3 , HAsO3


and AsO3
3 ). Under oxidizing conditions, the predominant species is As(V) which exists as arsenic acid
(H3 AsO4 , H2 AsO
4 , HAsO4 and AsO4 ) (Ferguson and
Gavis, 1972).
Various treatment technologies have been developed
for arsenic removal from drinking water. The commonly
used technologies include coagulation and precipitation
with iron and aluminum salts (Edwards, 1994; Hering
et al., 1996), adsorption onto activated alumina, activated carbon and activated bauxite (Gupta and Chen,
1978), ion exchange and reverse osmosis (Cliord, 1999).
Some recent treatment technologies based on oxidation
and adsorption are green sand ltration (Christen, 2000),
iron oxide coated sand (Joshi and Chaudhuri, 1996),
manganese dioxide coated sand (Bajpai and Chaudhuri,
1999), ferruginous manganese ore (Chakravarty et al.,
2002), ferrihydrite (Jain et al., 1999), clay minerals
(Manning and Goldberg, 1997) and zero-valent iron
(Fendorf et al., 1997; Farrell et al., 2001; Su and Puls,
2001). Coagulation, precipitation and other adsorption
techniques such as, activated alumina, and activated
carbon, have been found to be not as ecient for As(III)
removal as for As(V) removal. Therefore for ecient
arsenic removal oxidation of As(III) to As(V) has been
suggested. The use of external oxidizing agents tends to
bring down the water quality. Despite the fact that a
variety of treatment methods are available, the eciency
of these processes is not completely known (Krishna
et al., 2001). Many of them have been reported to be
capable of removing arsenic to levels lower than 50 lg l1 ,
but with the impending of revision of the permissible
levels to 10 lg l1 or lower, it is necessary to investigate
the treatment approaches that would consistently provide drinking water with arsenic less than 10 lg l1 levels.
Studies on arsenic indicate that hydrous metal oxides, such as ferric hydroxides, ferrihydrite, and goethite
strongly adsorb arsenic (Edwards, 1994; Hering et al.,
1996; Fendorf et al., 1997; Ravene et al., 1998; Jain
et al., 1999). Recently arsenic removal by zero-valent
iron has also been reported (Farrell et al., 2001; Krishna
et al., 2001; Su and Puls, 2001). In this method, iron
oxide produced due to corrosion of iron lings removed
both As(III) and As(V) from the contaminated drinking
water. In view of previous discussion, it is clear that
As(III) removal is favored by oxidation to As(V) followed by adsorption on to adsorbent.
Electrocoagulation is an emerging water treatment
technology that has been applied successfully to treat
various wastewaters. It has been applied for treatment of
potable water (Vik et al., 1984; Holt et al., 2002), urban
wastewater (Pouet and Grasmick, 1995), heavy metal
laden wastewater (Mills, 2000), restaurant wastewater
(Chen et al., 2000), and colored water (Jiang et al.,
2002). Further, electrocoagulation oers possibility of
anodic oxidation and in situ generation of adsorbents
(such as hydrous ferric oxides, hydroxides of aluminum).

It is felt that As(III) might be oxidized to As(V) during

electrocoagulation and gets adsorbed on to the metal
hydroxides generated. Therefore, it is expected that
electrocoagulation would be a better choice for arsenic
removal from water. Previous researchers have mostly
considered current density as an important design variable for EC process. Whereas, as per Faradays law
dissolution of electrode is related to the total charge
passed. Thereby the amount of adsorbent produced in
the electrochemical reactor would be proportional to the
charge density (total charge passed through the solution)
and therefore it might be worthwhile to explore charge
density as design parameter for EC process.
The objective of the present study was to (i) investigate the possible oxidation of As(III) to As(V) during
electrocoagulation; (ii) evaluate the ecacy of As(III)
and As(V) removal by dierent electrode materials; (iii)
evaluate arsenic removal at varying current density in
the pH range 68; (iv) compare electrocoagulation and
chemical coagulation for arsenic removal.

2. Materials and methods

2.1. Preparation of samples
Batch experiments were performed at Centre for
Environmental Science and Engineering laboratory, IIT
Bombay, at ambient temperatures ranging from 26 to 28
C. The chemicals were analytical reagent grade and
were used without any further purication. All glassware were cleaned with water and 1 N H2 SO4 and then
rinsed with distilled water. Stock solutions of arsenite
were prepared by dissolving appropriate quantity of
arsenic trioxide, As2 O3 , (S.D. Fine Chem Ltd, India) in
distilled water containing 1% (w/w) NaOH and the
solution was then diluting up to 1 l with distilled water
before use. The arsenate stock solution was prepared
from the sodium arsenate, Na2 HAsO4 7H2 O (Loba
Chemie, India). The intermediate and secondary standards of arsenic solutions were prepared freshly for each
experiment. The working solutions containing arsenic
were prepared by dissolving appropriate amount of arsenic from stock solutions in tap water. Tap water was
tested for the pH, alkalinity, and the presence of arsenic,
iron and phosphate. It was found that the pH of the
water varied from 7.2 to 7.5, bicarbonate alkalinity was
approximately 4550 mg l1 as CaCO3 , the dissolved
iron, phosphate and arsenic concentration were not
detectable in tap water.
2.2. Procedure
Preliminary experiments were conducted with three
dierent electrode materials (iron, aluminum and titanium). Two electrodes of same material were placed


0.5 cm apart in a 1.5 l beaker and 1 l of arsenic containing water was added. The total submerged surface
area of each electrode was 36 cm2 . Before each experiment, the electrodes were abraded with sand paper to
remove scale and then cleaned with successive rinses of
water and 1 N H2 SO4 .
A direct current by stabilized power supply (015 V,
2 A) was applied to the terminal electrodes in which
electrical current was controlled by a variable transformer. Since most of the arsenic contaminated ground
waters have the pH in the range of 68, the experiments
were conducted in this pH range only. The pH of the
solution was adjusted by adding either dilute HCl or
NaOH. Duplicate runs were carried out for each
experiment. Experiments were also conducted for conventional coagulation methods for arsenic removal.
Ferric chloride (FeCl3 ) was used as a coagulant. The
chemical coagulation experiments were conducted using
jar test apparatus as specied in the literature (Edwards,
1994; Hering et al., 1996). The summary of experimental
conditions employed is presented in Tables 1 and 2.
2.3. Analytical methods
The residual arsenic in water sample was determined
using molybdenum blue complex method (Johnson and
Pilson, 1972). The method was used to estimate As(III)
and As(V) concentrations in treated water samples to
assess the eciency of the oxidation step and the subsequent removal of arsenic. Spectrophotometric measurements were made at a wavelength of 865 nm using
absorbance cells of 5 cm path length for arsenic determination. Calibration curve for total arsenic was prepared using solutions containing As(III) or As(V)
dissolved in distilled water. Total iron analysis was
performed by 1,10, phenanthroline method as described
in standard methods (APHA, 1985).

Table 1





run no.

Arsenic type/
electrode material

Current density pH
(mA cm2 )

1, 2
3, 4
5, 6
7, 8
9, 10
11, 12
13, 14
15, 16
17, 18
20, 21



6 0.20
7 0.15
8 0.25
6 0.20
7 0.20
8 0.20
6 0.15
7 0.20
8 0.20
7 0.25
7 0.20

Table 2
Experimental conditions employed in chemical coagulation
run no.


Range of FeCl3
dose as Fe (mg l1 )





6 0.20
7 0.20
8 0.20
6 0.20
7 0.20
8 0.20


3. Results and discussion

3.1. Comparison of electrode materials
In any electrochemical process, electrode material
has signicant eect on the treatment eciency. Therefore, appropriate selection of the material is important.
The electrode material for drinking water treatment
should also be non-toxic to human health. Hence iron,
aluminum and titanium were chosen as electrode material as these are non-toxic and readily available.
3.1.1. Iron electrode
Fig. 1(a) presents the results of experimental run no.
3 and 4. The gure shows the variation of total As
[As(III) + As(V)], As(V), and total As removal with
charge passed in solution. It can be seen from the gure
that arsenic removal was greater than 99% and the
residual arsenic concentrations obtained were less than
10 lg l1 after 100 coulombs per liter (C l1 ) was passed.
As(V) concentrations increased initially at the beginning
of the process and decreased later as the total arsenic
removal increased. A possible reason for the behavior
may be that at the beginning of the EC process (i.e., lag
stage), the rate of As(III) oxidation to As(V) is more
than the rate of adsorption of As(V) onto hydrous ferric
oxides, as initially hydrous ferric oxides would be quite
less. However, as the time proceeds sucient hydrous
ferric oxides are generated and arsenic adsorbs on it.
3.1.2. Aluminum
Fig. 1(b) shows the variation of total As, As(V) and
total As removal with charge passed in solution for
experimental run no. 19. It can be observed from the
gure that As(V) concentration at the start of the
experiment was 0.2 mg l1 and reduced to 0.053 mg l1
with charge passed. The arsenic removal obtained was
37%, which is lower as compared to the removal obtained with iron electrode. The plausible reason for less
arsenic removal by aluminum in comparison to iron
could be that the adsorption capacity of hydrous aluminum oxide for As(III) is much lower in comparison
to hydrous ferric oxides (Hering et al., 1996).

















Arsenic removal (%)



Arsenic removal (%)












Arsenic removal (%)

Arsenic conc. (mg l-1)

Arsenic conc. (mg l-1)

Arsenic conc. (mg l-1)


Fig. 2. Eect of current density on arsenic removal (experimental run no. 3, 4, 9, 10), where, symbols indicate (d) total
arsenic concentration (1.53 mA cm2 ), ( ) As(V) concentration
(1.53 mA cm2 ), (j) total arsenic concentration (0.65
mA cm2 ), () As(V) concentration (0.65 mA cm2 ).










Charge density (C l-1)

Fig. 1. Arsenic removal with (a) iron electrodes (experimental

run no. 3, 4), (b) aluminum electrodes (experimental run no.
19), (c) titanium (experimental run no. 20 and 21), where,
symbols indicate (d) total arsenic removal, ( ) total arsenic
concentration, (j) As(V) concentration.

3.1.3. Titanium
The EC experiment with titanium electrodes was
conducted with As(III) containing water. The results
obtained from experimental run no. 20 and 21 have been
presented in Fig. 1(c). Arsenic removal was up to 58%
with titanium electrodes after 180 C l1 was passed. It
can be observed that variation of As(V) concentration
was in the range of 0.1640.278 mg l1 . Bissen et al.
(2001) have reported that As(V) adsorption on TiO2 was
more in comparison to As(III). Therefore it is speculated
that partial oxidation of As(III) might be occurring and
the oxidized As(V) might be getting adsorbed on to
hydroxides of titanium. However, the aqueous phase
arsenic concentration was about 0.75 mg l1 at the end
of experiment, which is much higher than the drinking
water guideline value for arsenic.
3.2. Eect of current processing time
The time dependence of arsenic removal by EC
process at pH 7 is shown in Fig. 2. It can be seen from
the gure that up to 5060% of the initial concentration

decreased within 5 min of the process and the residual

arsenic concentration in water was less than 10 lg l1 ,
which is the recent guideline value of WHO. At the
beginning of process the arsenic removal is rapid and
later it decreased gradually over almost the entire process examined. Arsenic ions are more abundant at the
beginning of the EC process, and the generated iron
hydroxides due to corrosion of the anode at that time
will form complexes with arsenic and therefore rapid
removal of arsenic was observed. However, as the
experiment proceeds the aqueous phase arsenic concentration goes on reducing and simultaneously hydrous
ferric oxides concentration increases, thereby abundance
of hydrous ferric oxides occur at the end of the process,
so the curves are nearly the same at the end of experiment.
3.3. Eect of current density
Some investigators have reported that in electrocoagulation, current density can inuence the treatment
eciency (Pouet and Grasmick, 1995), while others
have reported that current density has no signicant
eect on pollutant removal (Chen et al., 2000).
Therefore, it remains unclear that whether the current
density aects the treatment eciency or not. Fig. 2
shows the aqueous phase arsenic concentration as a
function of time for current densities 0.65 and 1.53
mA cm2 . It can be seen from the gure that a steep
decrease in arsenic concentration just at the beginning


of the process for both current densities occurred.

Current density has no signicant eect on the nal
total arsenic removal, but removal was rapid with high
current density. This indicates that it is not the current
density, but may be the charge density that really affects the treatment eciency. The above conclusion
does not rule out the advantage of using high current
density for reducing the water retention time (Chen
et al., 2000).
3.4. Eect of charge density
The results obtained at dierent current densities
were converted to charge passed per liter of water. The
results are presented in Fig. 3. It is clear from the gure
that current density is not an appropriate parameter for
assessing arsenic removal from water but charge passed
per liter seems to be an appropriate parameter for
assessing arsenic removal. It has been reported that arsenic removal increases with increasing iron dosages in
chemical coagulation (Edwards, 1994; Hering et al.,
1996). Thereby it may be expected that in electrocoagulation, arsenic removal would be governed by the formation of hydrous ferric oxides in solution. According
to Faradays law, the charge passed to the solution is
directly proportional to amount of iron dissolved (Vik
et al., 1984). This implies that the arsenic removal by
electrocoagulation may be governed by the formation of
arsenic-hydrous ferric oxide complexes. It is observed
from Fig. 3 that arsenic removal is dependant on the
total charge passed through the solution. Therefore
charge density seems to be an appropriate parameter for
comparison of dierent experimental results and it may

also serve as a design parameter for electrocoagulation

3.5. Eect of pH
In electrocoagulation, a slight increase in the pH was
observed with time during the process and it was within
the regulatory drinking water standards. Vik et al.
(1984) observed the same eect during the EC process
and also reported that electrocoagulation can act as pH
neutralization step. The pH increase in electrocoagulation is attributed to the formation of hydrogen gas at the
cathode (Vik et al., 1984; Chen et al., 2000). Also a slight
increase in pH may be expected because of sorption
reactions of As(V) and As(III), which release OH
groups from sorbents as a result of ligand exchange
(Arienzo et al., 2002).
The importance of pH in regard to coagulation is
well documented. As(III) and As(V) removals by iron
oxides normally behave dierently at dierent pH (Edwards, 1994; Hering et al., 1996; Bose and Sharma,
2002). Su and Puls (2001) have reported that As(III)
shows greater removal than As(V), and mixture of As(V)
and As(III) showed intermediate removal by iron oxides.
It has been reported that pH is an important operating
factor inuencing the performance of electrocoagulation
process (Chen et al., 2000).
To study the eect of pH a series of experiments were
performed under controlled pH conditions. The pH was
kept nearly constant throughout the experiments by
adding HCl or NaOH. As(III) and As(V) removal eciencies obtained in the pH range 68 are shown in
Table 3. It can be seen from the table that there is no
signicant eect of pH on arsenic removal and, As(III)
and As(V) removal up to 9799% were obtained over
almost the entire pH range examined. The observed
behavior can be explained by considering speciation of
both arsenic and hydrous ferric oxides. The speciation
was determined from MINEQL equilibrium speciation
software and it is observed from the results that in pH
range 68, almost all iron present in the soluble phase is
Table 3
Summary of experimental results for electrocoagulation


Coagulant dose as Fe (mg l1 )






Arsenic removal (%)

Fig. 3. Eect of charge density on arsenic removal (experimental run no. 3, 4, 9, 10) where symbols indicate (d) total
arsenic removal (%) [1.53 mA cm2 ], ( ) As(V) concentration
[1.53 mA cm2 ], (j) total arsenic removal (%) [0.65 mA cm2 ],
() As(V) concentration [0.65 mA cm2 ].




















Many researchers have studied arsenic removal by

conventional coagulation methods using iron salts (e.g.
ferric chloride, ferrous sulfate) and aluminum salts (e.g.
alum) (Cheng et al., 1994; Edwards, 1994; Hering et al.,
1996). They reported that removal achieved was up to
99% for As(V) and the removal was only up to 4050%
for As(III). Therefore, oxidation of As(III) to As(V) has
been suggested for eective arsenic removal. The comparison of EC and CC has been done on the basis of iron
dose. In electrocoagulation, the amount of iron dissolved was calculated theoretically by using Faradays
law. The validity of Faradays law was also ascertained
experimentally. Tables 3 and 4 show the performance of
EC and CC for As(III) and As(V) at dierent pH (6, 7
and 8). It is observed from Tables 3 and 4 that in both
methods arsenic removal increased with increasing iron
dosage and As(V) removal was always higher than
As(III) removal. In electrocoagulation, removal of both
As(III) and As(V) achieved was greater than 99%.
Whereas, in chemical coagulation up to 9799% removal
was achieved for As(V), but only 9093% of As(III)
removal was obtained even for iron dose of 51.60 mg l1 .
Experimental observations of less removal of As(III) in
comparison to As(V) by conventional coagulation are in
agreement with the earlier research work (Cheng et al.,
1994; Edwards, 1994; Hering et al., 1996). Based on the
results, it is clear that As(V) removal by CC and EC
seem to be the same, but As(III) removal eciencies
of EC are much higher than CC.
Table 4
Summary of experimental results for chemical coagulation


Coagulant dose as Fe (mg l1 )






Arsenic removal (%)





















mg As adsorbed / mg Fe

3.6. Electrocoagulation (EC) vs chemical coagulation


3.6.1. Adsorption of arsenic on hydrous ferric oxides

Adsorption of both As(III) and As(V) on amFe(OH)3 has been studied at various pH by Moore and
Pierce (1982). They reported that As(III) and As(V)
normally behave dierently in terms of pH on the
adsorption on hydrous ferric oxides. Some investigators
have reported that favorable adsorption of As(V) on
to hydrous ferric oxides at pH < 7 (Farrell et al., 2001;
Su and Puls, 2001), while others have reported more
favorable adsorption of As(III) at pH > 7 (Jain et al.,
1999) and equal amounts of As(V) and As(III) adsorption below pH 7 (Su and Puls, 2001). Therefore the
adsorption capacities of As(III) and As(V) in electrocoagulation and chemical coagulation were investigated.
Fig. 4 shows the variation of sorption capacity of As(III)
and As(V) with equilibrium arsenic concentration for
electrocoagulation and chemical coagulation experiments at pH 6. It is evident from the gure that electrocoagulation is more eective for As(III) removal than
chemical coagulation. Whereas, As(V) removal by both
the processes is nearly the same. The higher As(III)
sorptive capacity observed in EC in comparison to CC
may be attributed to possible oxidation of As(III) to
As(V) during the EC process.





mg As adsorbed / mg Fe

of Fe3 species, which is in equilibrium with Fe(OH)3 (s).

Whereas, As(III) exists as H3 AsO03 and As(V) forms
H2 AsO
4 , HAsO4 . As the speciation in the pH range
remains nearly the same therefore it is likely that the
eect of pH would not be signicant on arsenic removal.
Similar results have been reported in previous studies
(Arienzo et al., 2002).










As concentration (mg l )

Fig. 4. Sorption isotherms obtained for (a) As(III) and (b)

As(V), where, symbols indicate (d) electrocoagulation ( )
chemical coagulation.


3.7. Mechanisms of arsenic removal by EC

Since As(III) is more mobile and more toxic than
As(V), it is advantageous to convert As(III) to As(V).
Also due to poor As(III) removal from water by many
conventional processes, oxidation of As(III) to As(V) as
the rst step is recommended and then subsequent removal of As(V). But in electrocoagulation, it seems that
oxidation of As(III) to As(V) occurs as observed from
the increase in As(V) concentration with time. The same
trend is also supported by higher sorptive capacity obtained for As(III) in EC (Fig. 4). The As(V) concentration increased with time initially (Figs. 2 and 3), later it
decreased gradually as the total arsenic concentration
decreased. This decrease in both As(III) and As(V)
concentrations might be due to the adsorption on to the
freshly generated iron hydroxides in the reactor. EC
experiment was conducted with water containing no arsenic, and hydrous ferric oxide was produced. Hydrous
ferric oxide, so produced was then tested for its As(III)
removal capacity. It was found that As(III) removal by
the hydrous ferric oxides were quite less, which further
supports that oxidizing conditions in EC cell have signicant role in As(III) removal. Thereby, it seems that
the removal mechanism for As(III) is oxidation to As(V)
and subsequent adsorption on to hydrous ferric oxides.

4. Conclusions
In electrocoagulation process, arsenic removal eciencies with dierent electrode materials follow the sequence: iron > titanium > aluminum. The process was
able to remove more than 99% of arsenic from an Ascontaminated water and met the drinking water standard of 10 lg l1 with iron electrode. Arsenic removal is
rapid at higher current densities but when the results
of dierent current density were converted into charge
density, arsenic removal correlated well with charge
density and thereby charge density is a suggested as a
design parameter for the process. The aqueous phase pH
did not have signicant eect on both As(III) and As(V)
removal in the pH range 68. As(III) was more eciently removed in electrocoagulation than chemical
coagulation, whereas, As(V) removal performance of
both EC and CC was nearly same. As(III) removal
mechanism in electrocoagulation seems to be oxidation
of As(III) to As(V) and surface complexation with iron
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