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Arsenic in Drinking Water and Its Removal


Liu Zhenzhong1,2, Deng Huiping2, Zhan Jian1
1. School of Architecture, Nanchang University, Nanchang Jiangxi 330031, China;
2. School of Environment Science and Engineering, Tongji University, Shanghai 200092, China

Abstract: Superfluous arsenic in drinking water can do harm to len and Reimer, 1989).
human health. In this paper, a broad overview of the available The high arsenic groundwater is mainly distributed in
technologies for arsenic removal has been presented on the basis Bangladesh, India, American, German, Japan, Argentina,
of literature survey. The main treatment methods included coagu- Mexico, Brazil, Poland and China (Zhao, 2002). Arsenic
lation-sedimentation, adsorption separation and ion exchange, was classified as a Group A carcinogen by the United
membrane technique, which have both advantages and disadvan- States Environmental Protection Agency. There have been
tages. It concluded that the selection of treatment process should extensive epidemiological studies showing that chronic
be site specific and prevailing conditions and no process can serve ingestion of high levels of inorganic As caused skin cancer
the purpose under diverse conditions as each technology has its (NRC, 1999), at the same time, some documentation of As
own limitations. In order to gain good results, some methods exposure also caused cancers of the nasal cavity, trachea,
should be improved. bronchus, lung, liver, bladder, colon, kidney, prostate, brain,
Key words: arsenic removal, coagulation-sedimentation, adsorp- the lymphatic and hematopoietic tissues as well as the
tion, ion exchange, membrane technique nervous system (Chen and Lin, 1994; Naqvi et al 1994;
Remembrance, 2003). According to a recent report by the
1 Introduction United States National Academy of Science and United
States National Research Council, even at 3 µg/L of As, the
Groundwater in the part of the world has been affected risk of bladder and lung cancer is between four and seven
by the arsenic pollution. The arsenic contamination in wa- deaths per 10,000 people. At 10 µg/L, the risk increases to
ter body was not only caused by the physical geography between 12 and 23 deaths per 10,000 people (NRC, 2001).
chemistry change, such as the soil and rocks containing In addition, As can cause high blood pressure and diabetes.
arsenic weathering, geology variance, the arsenic mine Triggered by the risk concerned, most of countries have
drenching, the dissolved groundrock, but also caused by changed their drinking water standard. The US EPA an-
human activities, such as mining, metallurgy, waste release nounced its ruling in October 2001 to lower the maximum
of china industry, leather process, chemistry process, dye- contaminant level (MCL) from 50 µg/L to 10 µg/L with a
ing industry, use of pesticide and insecticide (Chakravarty compliance date of January 22, 2006 (An et al, 2005; EPA,
et al, 2002; Smedley and Kinniburgh, 2002). 2000a). In China, the new standard of drinking water stan-
Common arsenic species in the environment include ar- dard which was promulgated by National Standard Com-
senate (As(V)), arsenite (As(III)), dimethylarsinic acid mittee and Sanitation Ministry lowered the arsenic level
(DMA), and monomethylarsenic acid (MMA) (Gu et al, from 50 µg/L to 10 µg/L after consulted with the developed
2005). Arsenic (As(V) and As(III)) in the inorganic forms countries standard. The new standard will be implemented
were more toxic than those in the organic forms. Most of in July 2007. The improved drinking water standard posed
arsenic was presented in the inorganic forms in the nature new challenges to water treatment technique.
water. When it was in the oxidizing environment, the main
form was arsenate(As(V)); when it was in the reducing 2 Arsenic removal from water
environment, the main form was arsenite (As(III))(Lien et
al, 2005). As(V) includes H3AsO4, H2AsO4−, HAsO42−, Mainly, arsenic species were presented in natural waters
AsO43−, in which the negatively charged arsenate ac- as As (V), As(III), the As valent has a great impact on the
counted for more; while As(III) includes H3AsO3, H2AsO3−, removal effect and the incidence of endemic (Korte and
in which the uncharged H3AsO3 accounted for more (Cul- Quintus, 1991). The dissociation constants of the two arse-

Corresponding author: Liu Zhenzhong ( liuzz79@126.com)

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nic species and its redox reaction were reported as follows et al, 1994; Sancha, 2000; Scot, et al, 1995). This may be
(Luis, 2005): due to some of the aluminum remaining soluble, and pass-
Dissociation of As(V) ing through filtration steps, while iron salts completely
H 2 AsO 4 ↔ H 2 AsO −4 + H + pK1 = 2.2 (1) form particulate iron hydroxide. Meng et al (2000) studied
H 2 AsO −4 ↔ HAsO 24 − + H + pK 2 = 7.0 (2) the influence of the SiO43−, SO42−, CO32− on the As removal
when the ferric chloride was used. SO42− and CO32− have
HAsO 24 − ↔ AsO 24 − + H + pK3 = 11.5 (3) little impact on As at pH 4–10. While SiO43− has decreased
Dissociation of As(III) the As removal efficiency because of its high competition
HAsO3 ↔ AsO 23 − + H + pK1 = 9.2 (4) on adsorption site and produced the soluble polymer with
Redox reaction the ferric. In addition, Meng et al (2001) removed the arse-
H 3AsO 4 + 2H + + 2e − ↔ H 3AsO 3 + H 2O Eh = +0.56V (5) nic in the well using the ferric chloride and found that
It was not favorable for arsenite sedimentation because PO43− and SiO43− were the main anion to decrease the re-
of its high solubility. Figure 1 demonstrated the moval efficiency.
relationship between arsenic species and Eh-pH. Arsenite Liu et al (2005) investigated the effectiveness and
was more difficult to remove than arsenate because of its mechanism of permanganate enhancing arsenite (As(III))
less negatively charged on the surface. Therefore, it was co-precipitation with ferric chloride. Permanganate sig-
necessary to oxidize arsenite to arsenate. nificantly enhanced As(III) removal for ferric co-precipita-
tion (FCP)process. With Fe(III) dosage increasing from 2
A number of treatment technologies have been reported
mg/L to 8 mg/L, As removal increased from 41.3% to
to the date for arsenate and arsenite removal from waters.
75.4% for FCP process; for permanganate oxidation-ferric
Many technologies such as coagulation and sedimentation,
co-precipitation (POFCP) process, however, corresponsive
sorption and ion exchange, membrane separation were
As removal increased from 61.2% to 99.3%. Yuan et al
applied for arsenic separation.
(2006) adopted the ferrate as coagulation and evaluated the
performance of ferrate for arsenic removal by experiment.
The results showed that the efficiency of As removal can
be achieved by 98%. The Optimum pH was 5.5–7.5. The
oxidative and coagulation time was 10 min and 30 min
respectively. The salinity and hardness did not interfere
with removal arsenic. This method was very easy and ef-
fective comparing with the ferric method and KMnO4-
Ferric method.
Coagulation-sedimentation removing the arsenic
adapted to the large-scale water plant which need not in-
crease the other treatment facilities with less investment
Fig. 1 The relationship of arsenic and Eh-pH and convenient operation. However, the disadvantage of
the method was that the process must follow the clarified
2.1 Coagulation- sedimentation tank to remove the produced colloid arsenic and high de-
Coagulation-sedimentation was a common technique to pendence on the pH. It was not good for the arsenite re-
remove the contamination from water. This process can moval efficiency to depend on the constitute in the water.
capture soluble As, transforming it into insoluble reaction At the same time, large quantity chemicals were supplied
products (Edwards, 1994). As may be converted to an in- and the volume of the sludge was huge, other matters were
soluble form by precipitation, co-precipitation and adsorp- also introduced into the water.
tion onto ferric or aluminum hydroxides as the ferric and
2.2 Membrane technique
alum salts were applied. In general, iron salts were more
effective at removing arsenite than aluminum salts (Cheng, The ordinary membrane separation removing arsenic

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included nanofiltration (NF) and reverse osmosis (RO). 2.3.1 Activated alumina (AA)
The large diameter ions including SO42−, Cl− and Na+ can
Because AA was a common, commercially produced
be removed by NF which was a process of relatively low
adsorbent material for water treatment, there was more
pressure. While all the ions can be removed by reverse
literature on the use of the AA for As removal relative to
osmosis which was a process of higher pressure such as
other adsorbents. Activated alumina can remove the arsenic
seawater desaltation. Compared with the coagulation- effectively in the drinking water at pH 5.5. The principle
sedimentation, membrane separation had a higher effi- was that the soluble arsenic (AsO43− and AsO33−) in the
ciency to remove arsenic. water can be adsorbed on the surface of the
A number of studies have been performed to examine AA[am-Al(OH)3] and occupied the aluminous octahedron
the removal of arsenic by NF membranes (Chang, 1994; crystal lattice sites (Xiao et al, 2001). This kind of adsorp-
Urase et al, 1998). The results showed that NF processes tion action can further increase the instability of the AA
were effective for the removal of arsenic. Removal, how- uncrystalloid and be favorable to adsorb more As ion to
ever, depended upon operating parameters, membrane decease the soluble As in the water.
properties and the characteristics of the source water. Re- Compared with other metal oxides such as hydrogen
verse osmosis was an effective arsenic removal technology iron oxide, the kinetic sorption of AA was slower than that
proven through bench and pilot scale studies according to a of hydrogen iron oxide. The former spent two days to reach
report prepared for the US EPA (2000). Various pilot stud- half equilibrium but the latter just used a few hours to be-
ies reported arsenic removal ranging between 40%–99% come equilibrium (Clifford, 1990). The optimum pH to
without specifying the arsenic species removed. Ning adsorb As(III) and As(V) was respectively 5.5 and nearly
(2002) reported As(III) reduction at 73%. Bench-scale neutral, and the big adsorption capability was respectively
studies with RO membranes showed As(V) reductions at 15 mg/L and 3.5 mg/L (Jiang, 2001; Manning et al, 1998).
88%–96%. In addition, some interrupting ions such as SO42−, Cl−,
Generally, the membrane process was highly effective PO43− and F− can decrease the arsenic removal. This
for arsenic removal. Membrane also provided an effective method can be used in the concentrating supply water
barrier to suspended solids, all inorganic pollutants, organic plants and in the family purify equipment. However, com-
micropollutants, pesticides and so on. In another word, it mon AA with low sorption capability adapted to thin pH
range and acidic water, As(III) need be oxidated to As(V).
removed all the ions presented in the water, though some
After a period of the operation, regeneration can lose
minerals were essential for proper growth, remineralization
10%–50% sorption capability. At the same time, aluminum
was required after the treatment. In order to prevent mem-
quantity would increase in the treated water because of the
brane contaminant, some pretreatment was necessary. The
losing of the aluminum. It was known to all that the persis-
water should be acidic and pH need be corrected. The
tent adsorbed aluminum caused the diseases such as aged-
process was expensive compared to other methods.
ness imbecile.
2.3 Adsorption 2.3.2 Metal (hydrogen) oxide
Some materials with big specific surface area and high Iron oxide with high surface energy and surface area has
surface energy which have strong adsorption ability can strong adsorption capability with respect to many inorganic
separate and remove the contaminant to purify water in the ions and organic matters. Lots of literatures have reported
process of adsorption. This adsorption action may be that heavy metal ions and organic contaminate can be re-
chemistry effect such as surface chemistry coordination or moved by iron (hydrogen) oxide. Several iron oxides re-
complex or physical effect such as staticelectric attraction. moved arsenic effectively such as amorphous hydrous fer-
Adsorption was one of the most effective methods to re- ric oxide, crystalline hydrous ferric oxide (ferrihydrite),
move the arsenic in the water; the common adsorbents α-FeOOH, hematite, magnetitie and goethite (Goldberg,
included activated alumina, activated carbon, function resin 2002; Jackson and Miller, 2000; Jain and Loeppert, 2000;
and metal oxide, etc. Manning et al 1998; Raven et al, 1998). The iron hydroxide

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and its polymer with high adsorption and fast kinetic which respectively 163–184 BV and 149–165 BV (Joshi and
have the biggest capability of adsorption were the most Chaudhuri, 1996). The iron oxide coated sands has low
effective. However, some shortcomings with iron hydrox- saturation capacity of arsenite and arsenate. When the
ide still existed, for example, some anions have an adverse coated iron oxide quantity was 0.1%–0.2% or 1%–2%, the
influence on the arsenic removal such as SO42−, Cl−, F−, saturation quantity was respectively 0.041 mg/L and 0.043
PO43− and SiO3−. The latter two have relatively stronger mg/L (Thirunavukkarasu, 2003).
impact than the former three. In addition, the arsenic re- The shortcoming of the process was that the granular
moval was influenced by pH markedly. The removal effi- size must be large enough to reduce the stream resistance
ciency decreased quickly as pH was over 8.5. Arsenate which decreased the sorption capacity of the unit volume
removal was much better than arsenite by iron hydroxide. and quality. The larger volume sorption unit and frequently
On the other hand, the robustness and mechanical strength regeneration operation was needed because of the low ad-
of the granular iron hydroxide was not very good and sorption capacity. Because sands belonged to the silicon
needed improvement, the headloss pressure was produced oxide, which combined with the iron oxide and hydroxide
quickly with time and became more significant after back- less strongly, the iron oxide was subject to break off.
washing, the larger the particles, the less adsorption capac-
ity. While the regeneration of granular iron hydroxide
2.3.4 Activated carbon
seemed feasible, it generates an alkaline solution with high Activated carbon, either granular or powered, was
levels of arsenate, which requires further treatment and widely used as an adsorbent for water and advanced
disposal (Gu et al, 2005; Selvin et al, 2000). wastewater treatment. It was capable of adsorbing a wide
As far as iron hydroxide had poor adsorption to arsenite, of organic contaminants and heavy metals and was desig-
Lakshmipathiraj et al (2006) combined the advantages of nated as the best available technology by the US ( Gu et al,
Mn and Fe, synthesize a suitable adsorbent, Mn-substituted 2005; James, 1985). Arsenic adsorption onto virgin acti-
iron oxyhydroxide (MIOH), which could remove both ar- vated carbon was minimal and regeneration was difficult,
senite and arsenate from aqueous solutions with consider- so it cannot be directly applied for arsenic treatment (Daus
able efficiency. Mn-substituted iron oxyhydroxide (MIOH) et al, 2004; Deng et al, 2005). Literature has, however,
efficacy was studied for the removal of arsenite and arse- shown that the adsorption on activated carbon can be sig-
nate from aqueous solutions. The maximum uptake of ar- nificantly increased by treatment with various metal com-
senite and arsenate was found to be 4.58 and 5.72 mg/g pounds (Huang and Vane, 1989; Reed et al, 2000). Some
respectively. Adsorption was best described by Langmuir
iron compounds were impregnated into activated carbon,
isotherm and activation energies as calculated from a
resulting in enhanced As sorption (Gu et al, 2005; Huang
model-free isoconversional method were found to be on the
and Vane, 1989). Enhanced arsenic adsorption was simi-
order of 15–24 and 45–67 kJ mol−1 for arsenate and ar-
larly observed with copper-treated and zirconium-treated
senite, respectively.
activated carbon (Birgit et al, 2004; Manju et al, 1998).
2.3.3 Iron oxide coated sands Birgit (2004) adopted Zr treated activated carbon to
remove arsenic in the wastewater, and the efficiency was
In light of the deficiency of granular iron hydroxide,
high, but it was not suitable for drinking water because of
some iron oxide was coated on the sands to remove the
its toxic. Then Birgit coated Cu and Fe to the carbon, both
contamination in the water. It was low cost operation for
of arsenite and arsenate removal effect were improved
iron oxide coated sands beds and it adapted to the small
markedly. Huang et al (1989) reported that activated car-
equipment and family usage. In the trial, the iron oxide
bon traited ferrous salts improved the arsenate removal
coated sands volume was 50 mL, diameter was 11 mm,
efficiency because of the producing ferrous arsenate com-
velocity was 1 cm/m, detention time was 50 min, the initial
plex. Gu et al (2005) posed that ferrous ion can impenetrate
concentration was 1 000 µg/L, according to WHO drinking
into activated carbon inner holes and be oxided to ferric ion
sanitary standard, the arsenic goal level was 10 µg/L. The
by oxidants. Then ferric ion can combine multifunction
equipment operated for ten times, the penetrating volume
of the iron oxide coated sands for arsenite and arsenate was group to enhance the sorption capacity of arsenic (Fig. 2).

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Fig. 2 An illustrative model for preparation of As-GAC and arsenic adsorption

The sorption capacity increased after activated carbon bind with a transition metal such as copper and iron, and (b)
was traited. However, some shortcomings existed when metal ions that was immobilized to the functional groups of
metal-impregnated activated carbon was used. The metal the hosting resin. While sharing many common features
ion was subjected to leak from the media in the process of with standard ion exchangers, a ligand exchanger employs
backwashing, then the second contamination of water transition metal ions as its terminal functional groups. As a
source was caused and the sorption capacity decreased. In result, ligand exchange involves concurrent Lewis
order to improve the combination ability with metal ions, acid-base (LAB) interactions (metal-ligand complexation)
activated carbon was substituted with the ion exchange and electrostatic interactions between the fixed metal ions
resin and fiber, to remove arsenic in water. and target anionic ligands. While conventional anion ex-
changer selectivity for various anions was governed by
2.3.5 Ion exchange resin and fiber electrostatic interactions, the affinity of a PLE was pre-
Ion exchanged resin has many kinds according to the dominated by both the ligand strength and ionic charge of
material, making method and purpose. As far as the func- the ligands (An et al, 2005).
tion group was concerned, there were strong (weak) acid In the 1980s, Chanda et al (1988) impregnated iron to
canion exchanged resin, strong (weak) base anion ex- weak base macroporus chelating resin to remove As (III)
change resin, redox resin, heat regeneration resin and che- and As (V), the results showed that As (III) and As (V)
lating resin (Shao, 1989). Ion exchange technique was re- were prior to other anions reacting with the resin at a low
garded as one of the best available technology for arsenic level of As. When equilibrium level reached, As (III)was
removal (EPA, 2000a). Current commercial ion exchanger lower than As (V) for one order of magnitude. Chanda also
was prone to be saturated because of its poor selective to studied the sorption principle of iron impregnated chelating
arsenic and suffered from competing with other anions. resin and thought iron was not toxic metal, and the adsorp-
Due to the lack of As-selectivity, current ion exchange re- tion activity was prior to other metal ions such as copper
quired frequent regeneration and lots of regeneration brine and nickel ion. In order to effectively select anions, the
was used, which in turn resulted in a large quantity of hosting resin must have positive charge, which was anion
volumes wastewater containing arsenic (Clifford, 1999). exchanger. Such polymers have high affinity to metal ions
Generally, a polymeric ligand exchanger (PLE) was and prevented to strip off from the hosting resin. An (2005)
composed of (a) a cross-linked hosting resin that can firmly prepared a polymeric ligand exchanger (PLE) by loading

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ARTICLES

Cu2+ to a commercially available chelating ion exchange surface area than gel resin which can adsorb more iron
resin. Results from batch and column experiments indi- inside. Strong base anion resin with positive charge re-
cated that the PLE offered unusually high selectivity for moved more arsenic than strong acid canion. Compared the
arsenate over other ubiquitous anions such as sulfate, bi- iron-loaded resin with granular ferric hydroxide, Cumber
carbonate and chloride. Because of the enhanced arsenate found the former removed more arsenic than the latter, but
selectivity, the PLE was able to treat ten times more bed the sorption kenetic was slow. Diffusion inside the granular
volumes (BVs) of water than commonly used SBA resins. maybe velocity limited process.
Lenoble et al (2004) loaded manganese dioxide on a Because the adsorption velocity of ion exchange resin
polystyrene matrix anionic commercial resin in chloride was low, ion exchange fiber was used to remove arsenic.
form, called R-MnO2, which was tested for As(V) retention Ion exchange fiber, a kind of surface adsorption and sepa-
and for As(III) simultaneous oxidation and removal. Equi- ration material in fiber type, was 20–300 µm in diameter
librium was reached in 2 h and isotherms showed that which composed of lots of single silk. Compared with tra-
R-MnO2 maximal capacities towards As(III) and As(V) ditional ion exchange resin, ion exchange fiber has high
were, respectively, 0.7 and 0.3 mmol/g. Various mecha- stable chemistry, short distance of transfer, fast adsorption
nisms involved in As(III) and As(V) as follows (Fig. 3). and disadsorption, comprehensive purifying, good washing
and regeneration capacity, low energy consumption and
small fluid resistance (Xu et al, 2005).
Liu et al (2002) prepared a new type of ion exchange
fiber to remove arsenate from water. The batch sorption
experiments showed that fibrous sorbent had high sorption
capacity and good kinetic property for arsenate ion. The
sorption kinetic data can be described by Lagergren
pseudo-second order rate equation very well. Greenleaf
(2006) loaded nanoparticle hydrated iron oxide (HFO) on
Fig. 3 Various mechanisms involved in As(III) retention by R-
ion exchange fiber to sorb arsenic. Compared with the cor-
MnO2
responding resin, the efficiency was higher, sorption and
desorption velocity was more fast. Other anions have less
Luis (2005) loaded nanoparticle iron hydroxide on the influence on it. While the marked shortcoming of ion ex-
polymer resin producing four polymers (HCIX-M, HCIX-G, change fiber was its high cost.
HAIX-M,HAIX-G) to remove arsenic. Lewis acid-type
functional groups existed between iron hydroxide and hy- 3 Conclusion
brid polymeric sorbents. Lewis acid-base LAB, electric-
static action and complexation combined two matters to- The literature survey has indicated that each of the dis-
gether. Luis proposed the main reason and process to ad- cussed techniques can remove arsenic under specified con-
sorb arsenic by iron hydrogen as follows ditions. Different techniques have different advantages and
= FeOH −2 ↔ H + + = FeOH pK1 (5) disadvantages. Specific technique can be selected accord-
= FeOH ↔ H + + = FeO − pK 2 (6) ing to specific conditions. The existing methods should be
EL + LAB
perfected to gain the best effect.
(≡ FeOH +2 )(CI − ) + H 2 AsO −4 ⎯⎯⎯⎯

(7)
(≡ FeO +2 )(H 2 AsO −4 ) + CI − References
(≡ FeOH +2 ) + H 2 AsO 2 ⎯⎯⎯
LAB
→ ( ≡ FeOH)(HAsO 2 ) + H + (8) 1. An B R, Steinwinder T R, Zhao D Y, 2005. Selective re-
Luis found the removal effect of macroporous resin was moval of arsenate from drinking water using a polymeric
better than gel resin. Perhaps macroporous resin has more ligand exchanger. Water Research, 39: 4993–5004

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