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5 authors, including:
Abdullah Luqman Chuah
Robiah Yunus
SEE PROFILE
SEE PROFILE
Gregory Koay
Azni Idris
SEE PROFILE
SEE PROFILE
Department of Chemical and Environmental Engineering, bWater Technology Centre, Faculty of Engineering,
Universiti Putra Malaysia, Serdang 43400, Selangor, Malaysia
Tel. +60 (3) 8946 6288; Fax: +60 (3) 8656 7120; email: chuah@eng.upm.edu.my
Received 9 August 2005; Accepted 28 January 2007
Abstract
Arsenic contamination in water, especially groundwater, has been recognized as a major problem of catastrophic
proportions. The toxicology and health hazard also has been reported for many years. Because of the recognition that
arsenic at low concentrations in drinking water causes severe health effects, the technologies of arsenic removal that
have become increasing important. The current regulation of drinking water standard is become more stringent and
requires arsenic content to be reduced to a few parts per billion. There are several treatment methods capable of this
level of performance membranes, coagulation, anion exchange, disposable iron media, softening etc. Treatment
cost, operational complexity of the technology, skill required to operate the technology and disposal of arsenic
bearing treatment residual are factors should be considered before treatment method selection. This paper aims to
review briefly arsenic toxicology and hazards and also the previous and current available technologies that have been
reported in arsenic removal. Residual generation and disposal after treatment will also be discussed.
Keywords: Arsenic; Toxicology; Membrane; Adsorption; Precipitation; GFH; Residual disposal
1. Introduction
Arsenic is a heavy metal with a name derived
from the Greek word arsenikon, meaning potent.
The elements occur in environment in different
oxidation states and form various species, e.g., As
as As(V), As(III), As(0) and As (-III). In oxidized
*Corresponding author.
0011-9164/07/$ See front matter 2007 Elsevier B.V. All rights reserved
140
Inorganic arsenic generally exists in two predominant oxidation states, arsenite (NaAsO2) and
arsenate (Na 2HAsO4), both of which are toxic to
man and plants. Inorganic arsenic is always
considered a potent human carcinogen, associated
with increased risk for cancer of the skin, lungs,
urinary bladder, liver and kidney [2]. Arsenic
commonly present in water are pH dependant
species of the arsenic (H3AsO4) and arsenous
(H3AsO3) acid systems respectively. These anions
have acidic characteristics, and the stability and
dominance of a specific species depend on the pH
of the solution, as shown in Fig. 1. Arsenates are
stable under aerobic or oxidizing conditions,
while arsenites are stable under anaerobic or
mildly reducing conditions.
The presence of arsenic in natural water is
related to the process of leaching from the arsenic
containing source rocks and sediments [4, 5]. It is
generally associated with the geochemical environments such as basin-fill deposits of alluviallacustrine origin, volcanic deposits, inputs from
geothermal sources, mining wastes and landfills
[6,7]. Arsenic is a constituent of over 300 minerals and is commonly found in non-ferrous ores
such as copper, lead, zinc, gold and uranium.
Arsenic is a primary constituent of certain ores
(for example the copper mineral enargite) and
occurs as a trace impurity in others [8]. Uncontrolled anthropogenic activities such as smelting
of metal ores, use of arsenical pesticides and
wood preservatives agents may also release
arsenic directly to the environment [9].
Presently, arsenic has been used for a variety
of purposes such as treatment of ulcers, tuberculosis, syphilis, and many other ailments. More
recently, arsenic has been used as an insecticide,
fungicide, rodenticide, and wood preservative.
The common application of arsenic are in the
manufacture of pesticides (including wood preservatives), dessicants, glass, alloys, electronic
components (semiconductors), pigments, and
pharmaceuticals [10].
In this work, the aim of this article is to provide general description of the toxicity of arsenic,
health hazards, previous and current literatures on
the techniques in treating or removing arsenic.
Different techniques in removing arsenic viz.
adsorption, ion exchangers, membrane, coagulation and precipitation will be discussed. The US
Environmental Protection Agencys (EPA)
Incineration Research Facility has carried out
some tests in evaluating the potential of incineration as a treatment option for contaminated soils
by arsenic and lead [11]. Due to the volatilization
of arsenic containing compounds emission, the
incineration is not practical for this purpose.
Methods of arsenic wastes residual disposal after
treatment will also be discussed.
141
contaminant level (MCL), but the revised compliance levels that reduced this to 10 ppb MCL
represented a big change.
The Malaysia Environmental Quality Act
(1974) has stated that limit of sewage and industrial effluents for arsenic ranged between 0.05
0.1 mg/L. However, an overview of groundwater
contamination in Malaysia has been reported by
Suratman [24]. The Department of Environment,
Malaysia, monitors a programme at areas that are
potentially exposed to contamination that include
industrial, animal burial, rural, urban/suburban,
and agricultural area, golf courses and landfills,
and has found that in general mercury, arsenic,
phenolic compounds and nitrate exceeded benchmark values for agricultural, landfill and industrial sites.
Jain and Ali [25] reported comprehensively on
the occurrence and toxicity of arsenic. The toxicology of arsenic is a complex phenomenon and
generally classified into acute and sub-acute
types. The acute arsenic poisoning requiring
prompt medical attention usually occurs through
ingestion of contaminated food or drink. The
major early manifestation due to acute arsenic
poisoning includes burning and dryness of the
mouth and throat, dysphasia, colicky abnormal
pain, projectile vomiting, profuse diarrhea, and
hematuria. The muscular cramps, facial edema
and cardiac abnormalities, shock can develop
rapidly as a result of dehydration [26].
In general, there are four recognized stages of
arsenicosis, or chronic arsenic poisoning [23,27]:
C Preclinical: the patient shows no symptoms,
but arsenic can be detected in urine or body
tissue samples.
C Clinical: various effects can be seen on the
skin at this stage. Darkening of the skin (melanosis) is the most common symptom, often
observed on the palms. Dark spots on the
chest, back, limbs or gums have also been
reported. Oedema (swelling of hands and feet)
is often seen. A more serious symptom is
142
Table 1
Concentration of arsenic in urine, hair and nails of the
affected people in different arsenic contaminated water
ingestion episodes [32]
Location
Conc. in
urine
(mg/l)
Conc. in
hair
(mg/kg)
Conc.
in nails
(mg/kg)
Fairbanks, AL
0.1783
1.0
4.0
Millard County,
UT
Antofagasta,
Chile
Lassen County,
CA
Taiwan
West Bengal,
India
Bangladesha
0.025-0.66
0.104.7
0.025-0.77
4.083.4
0.012.0
0.03660.259
0.032.0
1.81
31.05
0.059.42
1.1
19.84
1.47
52.03
1.3
33.98
143
Table 2
Distribution of arsenic drinking water concentrations from historical and recent arsenic measurement data for Utah
communities in the study area [35]
Town
Number Median
Mean
Minimum arsenic
conc., ppb
Maximum arsenic
conc., ppb
Standard
deviation
Hinckley
Deseret
Abraham
Sugarville
Oasis
Sutherland
Delta
21
37
15
6
7
19
46
164.4
190.7
134.2
94.5
91.3
33.9
18.1
80
30
5.5
79
34
8.2
3.5
285
620
310
120
205
135
125
48.1
106.6
67.2
15.3
57.8
31.8
17.7
166
160
116
92
71
21
14
144
Fig. 2. (a) SEM micrographs of akaganite particles and (b) SEM micrographs of akaganite particles after As(V) sorption
[89].
145
The effect of the presence of sulfate, competition with other anions, is an important factor
to ion exchanger treatment of arsenic. Sulfate
levers can limit the applicability of ion-exchanger
as arsenic treatment. Jackson and Miller [49]
reported that sulfate was reported not to influence
As(V) sorption by ferrihydrite but resulted in a
considerable decrease in As(III) sorption below
pH 7, with the largest decrease at the lowest pH.
Sorbed As(V) by ettringite [Ca6Al2(SO4)3(OH)12
26H2O] was also not desorbable in the presence
of concentrated sulfate and high ionic strength
solutions [50]. On the contrary, sulfate was found
to decrease both As(V) and As(III) sorption on
hydrous ferric oxide in the pH range of 47 [51].
Disagreement in the literatures on the effects of
sulfate on As(V) and As(III) sorption may have
derived from different experimental conditions.
Scattered research has already been conducted
on a wide variety of sorbents. Some of the
reported sorbents include zeolites, goethite, clay,
kaolinites, activated carbon, chitosan beads, coconut husk, coal, fly ash, ferrous iron, alumina,
zirconium oxide, red mud, petroleum residues,
rice husk, human hair, sawdust, manganese
greensand, orange juice residues, akaganitenanocrystal and chome waste.
Activated carbon is also commonly used as the
material in arsenic treatment [5254]. Eguez and
Cho [55] measured the adsorption of As (III) and
As (V) using activated carbon at various pH
values. From the effect of temperature on adsorption, they could determine the isoteric heat of
adsorption. Other researchers [53,56] impregnated carbon with various metal ions such as iron
oxide in order to improve arsenic adsorption. The
iron oxide impregnated activated carbon has
shown higher As(III) and As(V) removals compared with the non-impregnated carbon.
Rajakovic [57] found that carbon pretreated
with Ag+ or Cu2+ ions improved As(III) adsorption but reduced As(V) adsorption. Evdokimov et
al. [58] reported that arsenic adsorption can be
146
147
148
149
150
Table 3
Treatment option for various arsenic bearing sources water characteristics [136]
Source water
Treatment option
Possible treatment
Filtration alone
Characteristic
As speciation
As(III)
As (V)
As size distribution
Dissolved
Particulate
Co-occurrence
NOM
Inorganic
RO
NF
UF
MFa
Preoxidationb
R
R
PE
R
NR
PE
NR
NR
R
NR
R
NR
PE
NR
NR
PE
NR
PE
NR
NR
PE
R
PE
PE
NR
NR
NR
NR
NR
NR
151
152
153
Table 4
Summary of arsenic precipitation processes [123]
Parameters
Alum
Iron
Lime softening
Chemicals
Cl2
Acid
Allum
NaOH
Cl2
Cl2
Fe2(SO4)3 Lime
Acid
pH
Removal, %
with Cl2
w/o Cl2
Initial arsenic conc., g/L
<6.5
6-8
>10.5
Cl2
FeCl3 a
SO2 a
KMnO4 a
Polymeric aluminium silicate sulfate (PASS)a
Organic polymer
7+
90
20
300
90
60
300
90
80
400
40-90
<100
Chemical may/may not be needed depending on water chemistry and process employed.
154
Table 5
Performances and limitations of arsenic oxidants.
Oxidants
Ozone (O3)
Ozone may be the most satisfactory for pre-oxidation to convert As (III) to As(V) in water
with the requirement to reduce disinfectant byproducts. Limitations are probably fewer on the
use of ozone as a pre-oxidant for arsenic than when O3 is used after filtration as a primary
disinfectant. Assimilable Organic Carbon (AOC) formation is ameliorated by
coagulation/filtration treatment downstream, and oxidation of bromide, though still possible,
is much less likely during pre-oxidation because the development of a significant ozone
residual is not necessarily required. Ozone pre-oxidation before nanofiltration could present a
problem if the AOC that is formed has a low molecular weight and passes through the
membrane.
Hydrogen peroxide oxidation was effective but limited by reactions with calcium hydroxide.
After oxidation, the resulting arsenate waste was effectively stabilized using ferric sulfate.
Chlorine is a good oxidant for As(III), but application must come early in the treatment train
when disinfectant byproduct precursor concentration is high and there is a danger of
producing large concentrations of disinfectant byproducts.
Permanganate may work better than chlorine, however, no sufficient information on the
permanganate demand for arsenic oxidation relative to the demand exerted by other
substances.
Hydrogen peroxide
(H2O2)
Chlorine (Cl)
Permanganate
the oxidation rate. The half-life for As(III) oxidation by ozone was very short, only 4 min. The
half-life for pure oxygen ranged from 2 days to 5
days, and for air a half-life of 9 days. Their
findings showed that ozone can be used to
remove arsenic from groundwater through oxidation, coprecipitation and adsorption reactions
effectively. A comparison of the relative performance between ozone and other oxidants e.g.
hydrogen peroxide and chlorine with respect to
oxidation of As is shown in Table 5.
3.7. Biological remediation and other biological
treatments
Biological treatment has been demonstrated to
be a useful alternative to conventional treatment
systems for the removal of toxic metals from
dilute aqueous solution. However, the bioprocesses for treating toxic effluents must compete
with existing methods in terms of efficiency and
economy. To its advantages, the biotechnological
155
2H+ + 2e! 6 H2
As(III) + 3e! 6 As(0)
As(0) +3e! + 3H+ 6 AsH3
Anode:
H2O!2e! 6 O2 + 2H+
156
157
water. Two general types of residuals are potentially generated from media adsorption: spent
media and regeneration solutions. Spent media
will be generated from systems that use the media
on a one-time throw-away basis, or from systems
where the media has become exhausted and can
no longer be regenerated, or is no longer effective. In some cases, depending on manufacturer
policy, spent media may be sent back to the
vendor for reactivation, recovery, or disposal.
No details were provided for regeneration. It
is generally assumed that the same steps as for
ion exchange will be utilized: backwash, regeneration, and rinse. Each of these steps will generate
an aqueous residual which will likely be combined. Some of the new adsorption media have
such large arsenic removal capacities that periodic backwashing (with regeneration) is required
to remove the particulate material that is filtered
out during its treatment operation. This backwash
water will likely contain some arsenic that is
attached to the particulate material or any very
fine adsorption media that is removed by the
backwashing process. The waste stream is a
residual that may be disposed of immediately at
the time of backwashing or it may be held and
disposed with the regeneration waste water.
Depending on the concentration of arsenic in the
influent and other factors, the disposal of the
regeneration waste and the backwash water may
be subject to the disposal requirements [175].
4.4. Iron/manganese removal methods
Iron/manganese removal processes, both the
oxidation/filtration and the potassium permanganate greensand techniques, produce a liquid
residual from the filter backwashing step (Fig. 7).
Occasionally, the filter media or greensand needs
to be replaced and this material also becomes a
residual product that must be disposed. Similar to
the backwash and regenerant solution from the
ion exchange and activated alumina processes,
the filter backwash water will contain arsenic, the
158
Table 6
Residual generation and disposal for the various arsenic treatment methods [175]
Treatment method for arsenic
Form of residual
Residual generation
Disposal
Ion exchange
Liquid
Regeneration streams
Spent backwash
Spent regenerant
Spent rinse stream
Spent resins
Sanitary sewer
Discharge
Evaporation ponds/lagoon
Solid
Activated alumina
Liquid
Solid
Adsorption
Liquid
Liquid
Membrane processes
Regeneration streams
Spent backwash
Spent regenerant (caustic)
Spent neutralization (acid)
Spent rinse
Liquid filtrate (when brine
streams are precipitated)
Spent alumina
Sludge (when brine streams
are precipitated)
Regeneration streams
Spent backwash
Spent regenerant
Spent rinse stream
Filter backwash
Solid
Liquid
Landfill
Hazardous waste landfill
Return to vendor
Sanitary sewer
Direct discharge
Evaporation ponds/lagoon
Landfill
Hazardous waste landfill
Land application
Sanitary sewer
Direct discharge
Evaporation ponds/lagoon
Direct discharge
Sanitary sewer
Evaporation ponds/lagoons
Sanitary sewer
Land application
Landfill
Landfill
Hazardous waste landfill
Direct discharge
Sanitary sewer
Deep well injection
Evaporation ponds/lagoon
5. Conclusion
To remove arsenic from wastewaters, the most
commonly used technologies are adsorption onto
activated alumina, and precipitation or adsorption
by metals oxides, predominantly Fe(III) and
membranes. These technologies for removal of
arsenic from wastewaters are most suited to dealing with relatively low concentrations of arsenic,
i.e. the low g/l level. However, the technique of
precipitation, generally using Fe (III) or lime
softening is suited to higher concentrations,
normally at the low mg/l levels. Adsorption is a
method that has been an important method used
in arsenic removal. Most studies are focused on
159
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