Ind. Eng. Chem. Res.

2006, 45, 8105-8110 8105

SEPARATIONS

Removal of Arsenic in Aqueous Solutions by Adsorption onto Waste Rice Husk

Md. Nurul Amin,*,† Satoshi Kaneco,† Taichi Kitagawa,† Aleya Begum,‡ Hideyuki Katsumata,†
Tohru Suzuki,§ and Kiyohisa Ohta†
Department of Chemistry for Materials, Faculty of Engineering, and EnVironmental PreserVation Center, Mie
UniVersity, Tsu, Mie 514-8507, Japan, and Department of Zoology, UniVersity of Dhaka, Dhaka 1000, Dhaka,
Bangladesh

Rice husk has tremendous potential as a remediation material for the removal of arsenic from groundwater.
The present work investigates the possibility of the use of rice husk adsorption technology without any
pretreatment in the removal of arsenic from aqueous media. Various conditions that affect the adsorption/
desorption of arsenic are investigated. Adsorption column methods show the complete removal of both
As(III) and As(V) under the following conditions: initial As concentration, 100 µg/L; rice husk amount, 6 g;
average particle size, 780 and 510 µm; treatment flow rate, 6.7 and 1.7 mL/min; and pH, 6.5 and 6.0,
respectively. The desorption efficiencies with 1 M of KOH after the treatment of groundwater were in the
range of 71-96%. The present study might provide new avenues to achieve the arsenic concentrations required
for drinking water recommended by Bangladesh and the World Health Organization (WHO).

Introduction As(V).14-19 Therefore, a preoxidation step is usually required

Arsenic contamination is one of the most challenging
environmental problems today. Millions of people worldwide
are exposed to naturally occurring As-contaminated groundwa-
ter, which they use as their only source of drinking water.1
Elevated concentrations of arsenic in groundwater are found in
many countries such as Bangladesh, India, Vietnam, and Chile.2
Increased usage of groundwater for drinking has caused serious
health problems,3,4 because arsenic is known to be highly
detrimental to human beings and animals. They include several
neurological,5 dermatological,6 gastrointestinal,7 and cardiorenal
diseases;8 arsenic also is a suspected carcinogenic.9 Furthermore,
recent research has suggested that As acts as an endocrine
disruptor at extremely low concentrations.10 Recently, because
of its high nuisance value, various regulatory agencies have
revised the maximum contaminant level of arsenic in drinking
water from 50 to 10 µg/L.11,12 This situation will require the
development of simple, low-cost methods for the removal of
As from groundwater for drinking water.
The predominant forms of As in groundwater and surface
water are the inorganic species arsenate [As(V)] and arsenite
[As(III)]. The As(V) species exists as oxyanions (H2AsO4- and
HAsO42-) at neutral pH, whereas the predominant As(III)
species is neutral H3AsO3.13,14 As(III) is more toxic and more
difficult to remove with the conventionally applied physico-
chemical treatment methods than As(V). Because most of the
technologies are inadequate for the removal of As(III) on an
industrial scale, they are mainly applied for the removal of
* To whom correspondence should be addressed. Tel.: 81-59-231-
9427. Fax: 81-59-231-9427. E-mail: nurul34@hotmail.com.
†
Department of Chemistry for Materials, Faculty of Engineering,
Mie University.
‡
University of Dhaka.
§ analytical-grade purity. Potassium arsenite (KAsO2) and potas-
Environmental Preservation Center, Mie University.
to transform the trivalent to the pentavalent form. The oxidation
procedures are performed by the addition of chemical reagents,
such as potassium permanganate, chlorine, ozone, hydrogen
peroxide, or manganese oxide.20,21 Although these reagents are
effective for the oxidation of trivalent arsenic, they can also
cause several secondary problems, arising from the presence
of residual reagents and the formation of side products. This
process can result in a significant increase in operating costs.
Therefore, the simultaneous removal of As(III) and As(V) is
needed for the treatment of groundwater.
Many technologies, including coprecipitation with iron or
alum, adsorption onto coagulated floc, ion-exchange resin,
reverse osmosis, and membrane techniques, have been used to
remove As from aqueous solution.15-19 In these methods,
however, the adsorption techniques are simple and convenient
and have the potential for regeneration and sludge-free operation.
So far, various adsorbents for arsenic removal have been
developed that include such materials as metal-loaded coral
limestone,22,23 hematite and feldspar,24 activated carbon,25,26
activated alumina,27,28 and hydrous zirconium oxide.29 However,
most of these adsorbents entail several problems in terms of
efficiency and cost. Because rice husk (RH) is a byproduct of
the rice milling industry, treatment with RH will become a
promising simple method for the removal of arsenic.
The present work was performed to evaluate the use of waste
rice husk without any pretreatment as an alternate adsorbent
for removing arsenite and arsenate from aqueous mediums.
Moreover, the RH was applied to the removal of arsenic from
Bangladeshi As-contaminated drinking water samples in a
single-step column operation.
Materials and Methods
Reagent. All reagents used throughout this work were of

10.1021/ie060344j CCC: $33.50 © 2006 American Chemical Society

Published on Web 11/01/2006
8106 Ind. Eng. Chem. Res., Vol. 45, No. 24, 2006
sium arsenate (KH2AsO4) were procured from Wako Pure
Chemical Industries Ltd., Osaka, Japan, and NaOH, KOH, HCl,
HNO3, and H2SO4 were obtained from Nacalai Tesque Inc.,
Kyoto, Japan. Stock solutions (1000 mg/L) of As(III) and
As(V) were prepared in distilled water from solid KAsO2 and
KH2AsO4, respectively. Dilute standard solutions were prepared
daily before use. Pure water was purified with an ultrapure water
system (Advantec MFS, Inc., Tokyo, Japan) resulting in a
resistivity of >18 MΩ cm.
Preparation of Adsorbent. The RH used in the present work
was obtained from a local rice mill in Bangladesh. The chemical
composition of RH has been reported as 49.3 wt % oxygen,
44.6 wt % carbon, and 5.6 wt % hydrogen (by elemental
analysis); 34.4 wt % cellulose, 29.3 wt % hemicellulose, 19.2
wt % lignin, and 17.1 wt % ash (by component analysis); and
59.5 wt % volatiles, 17.1 wt % ash, and 7.9 wt % moisture (by
proximate analysis).30 The collected materials were washed with
pure water several times to remove dust and fines. The washing
process was repeated until the color of the wash water was
transparent. The washed materials were then dried in a hot-air
oven at 60 °C for 24 h. The dried material was sieved into the
following five size fractions: 710-850 µm (avg 780 µm), 600-
710 µm (avg 655 µm), 425-600 µm (avg 510 µm), 355-425
µm (avg 390 µm), and 150-355 µm (avg 250 µm). The
materials were used for the removal of arsenic without further
physical or chemical treatment.
Adsorption and Analytical Procedures. RH was added to
the treatment glass columns (2 × 30 cm). The adsorption
experiments were carried out in columns that were equipped
with a stopper for controlling the column eluate flow rate
(treatment rate). Adsorption factors including the amount of rice
husk (0.5-7 g), average particle size (250-780 µm), treatment
flow rate (0.6-33 mL/min), initial sample concentration (50-
500 µg/L), and pH (2-14) were evaluated. After the pH had
been adjusted to the desired value with HCl and NaOH solutions,
the sample solution (100 mL) was passed through the adsorption
column at a given flow rate. The treatment flow rates of 0.6,
0.8, 1.7, 3.3, 6.7, 20, and 33 mL/min correspond to retention
times of 5.3 min, 4 min, ∼109 s, ∼58 s, ∼29 s, ∼10 s, and ∼6
s, respectively, for 1 g of rice husk. The packing density of the
treatment column was 0.32 g/cm3. A small piece of tissue paper
was inserted into the bottom of the column to prevent the loss
of rice husk during the treatment. The flow rate was kept
constant by controlling the stopper valve. The removal treatment
was performed at ambient temperature. The number of experi-
ments for the removal of As was greater than five. A graphite
furnace atomic absorption spectrometer (GFS97, Thermo Elec-
tron Corp.) was used for the determination of arsenic under the
following conditions: resonance line, 193.7 nm (As hollow
cathode lamp); pyrolysis temperature, 1200 °C (20 s); atomi-
zation temperature, 2600 °C (3 s); and matrix modifier, nickel
nitrate (10 mg/L). The removal (adsorption) efficiency was
calculated using the equation
removal (adsorption) efficiency ) (C0 - Ce)/C0 × 100 (1)
where C0 and Ce are the concentration of As in the sample
solution before and after treatment, respectively.
Results and Discussion
First, the performances of four adsorbents (rice husk, rice
straw, tea leaves, and newspaper) were evaluated for the removal
of As(III) and As(V) from aqueous solutions. Preliminary studies
showed that the complete removal of As(III) and As(V) was
Figure 1. Effect of adsorbent amount on the removal of As(III) and As-
(V) by adsorption onto rice husk (initial As concentration, 100 µg/L). (a)
As(V); avg RH particle size, 510 µm. Treatment flow rate: b, 1.7; O, 6.7
mL/min. (b) As(III); avg RH particle size, 780 µm. Treatment flow rate:
0, 1.7; 4, 6.7 mL/min.
achieved under the following conditions: initial concentration,
100 µg/L; amount of rice husk, 6 g; treatment flow rates, 6.7
and 1.7 mL/min; and average particle sizes, 780 and 510 µm,
respectively. The removal efficiencies with rice straw, tea leaves,
and newspaper were 65%, 57%, and 18%, respectively, for As-
(III) and 75%, 58% and 55%, respectively, for As(V). These
three adsorbents had lower removal efficiencies than rice husk.
Therefore, they were not considered for further investigations.
The rice husk used was an available material in the rice mill,
and its size distribution was as follows: 40% >850 µm, 18%
710-850 µm, 10% 600-710 µm, 13% 425-600 µm, 5% 355-
425 µm, 8% 150-355 µm, and 6% <150 µm. Because the main
component of rice husk is carbon, rice husk has the potential
to be used as an adsorbent. Rice husk was chosen for use as an
adsorbent material because of its granular structure, insolubility
in water, chemical stability, and high mechanical strength.31
Effect of Adsorbent Amount. The effect of the amount of
rice husk on the removal of As(III) and As(V) was investigated.
The results are presented in Figure 1. The removal efficiencies
of both As(III) and As(V) increased gradually with increasing
amount of rice husk. It is readily understood that the adsorption
capacity of rice husk depends on the surface activity, that is,
the specific surface area available for As-surface interactions
that is accessible to the As. Hence, increasing the amount of
rice husk will increase removal capacity of As. Obviously,
removal of As(III) from solution by adsorption onto rice husk
took place more readily than removal of As(V). Whereas the
removal efficiency for As(V) decreased as the treatment flow
rate was increased from 1.7 to 6.7 mL/min, the efficiency of
As(III) removal was independent of the rate in the tested range.
At relatively low treatment flow rates, the complete removal
of both As(III) and As(V) from 0.1 mg/L As concentration
aqueous media could be achieved with 6 g of rice husk. Until
now, various kinds of adsorbents have been studied for the
removal of arsenic. The maximum As(III) removal efficiency
achieved was 99% for iron oxide-coated sand at an adsorbent
dose of 20 g/L with an initial As concentration 100 µg/L in
batch studies.32 The removal efficiencies for As(III) and As(V)

Figure 2. Effect of particle size on the removal of As(III) and As(V) by
adsorption onto rice husk (initial As concentration, 100 µg/L). b: As(V);
RH, 2 g; treatment flow rate, 1.7 mL/min. O: As(V); RH, 1 g; treatment
flow rate, 6.7 mL/min. 4: As(III); RH, 1 g; treatment flow rate, 1.7 mL/
min.
Figure 3. Effect of treatment flow rate on the removal of As(III) and
As(V) by adsorption onto rice husk (initial As concentration, 100 µg/L).
b: As(V); RH, 2 g; avg particle size, 510 µm. O: As(V); RH, 1 g; avg
particle size, 510 µm. 4: As(III); RH, 1 g; avg particle size, 780 µm.
from an aqueous solution (100 µg/L, 100 mL) by 0.1 g of
modified fungal biomass were 75% and 95%, respectively, after
a 12-h batch treatment.33 When an aqueous As(III) solution of
10 mg/L concentration was stirred in the presence of both 1.0
g/L TiO2 and 1.0 g/L activated alumina under sunlight irradia-
tion, the arsenic removal increased with time and reached 89%
after 24 h.34 Although the removal efficiencies in the proposed
system were similar to those obtained with the other adsorbents,
the treatment time was very short because of the flow method
(column system).
Effect of Particle Size. Column adsorption experiments were
carried out for the removal of arsenic from aqueous solution
using five different particle sizes (average diameters of 250,
390, 510, 655, and 780 µm). The results are shown in Figure 2.
With decreasing particle size, the removal increased from 53%
to 61% for As(III) and from 55% to 80% for As(V). Munaf
and Zein reported that, when the size of the rice husk particles
increased, the adsorption of metal ions decreased.35 Similar
trends have been reported by Wong et al.36 These phenomena
might be due to the fact that the smaller particles offer
comparatively larger surface areas and greater numbers of
adsorption sites.
Effect of Flow Rate. The effect of the treatment flow rate
on the removal of As(III) and As(V) is illustrated in Figure 3.
The removal efficiency for As(III) increased gradually with
decreasing treatment rate down to 6.7 mL/min (linear velocity
2.1 cm/min), and then the efficiency remained almost constant.
The As(V) removal efficiency was nearly constant until the flow
rate decreased to 3.3 mL/min (linear velocity 1.1 cm/min), and
then the efficiency increased sharply. The complete removal of
As(V) with 2 g of rice husk was observed at 0.6 mL/min (linear
velocity 0.2 cm/min).
Effect of Initial Concentration. The removal efficiency is
highly dependent on the initial concentrations of As(III) and
Ind. Eng. Chem. Res., Vol. 45, No. 24, 2006 8107
Figure 4. Effect of initial adsorbate concentration on the removal of
As(III) and As(V) by adsorption onto rice husk. b, O: As(V); RH, 2 g;
avg particle size, 510 µm; treatment flow rate, 1.7 mL/min. 4, 0: As(III);
RH, 1 g; avg particle size, 780 µm; treatment flow rate, 6.7 mL/min.
Figure 5. Effect of pH on the removal of As(III) and As(V) by adsorption
onto rice husk (initial As concentration, 100 µg/L). b: As(V); RH, 2 g;
avg particle size, 510 µm; treatment flow rate, 1.7 mL/min. 4: As(III);
RH, 1 g; avg particle size, 780 µm; treatment flow rate, 6.7 mL/min.
As(V) in the sample solution. The effect of the initial sample
concentration on the removal of arsenic with RH was investi-
gated. The initial concentration was evaluated in the range of
0.05-0.5 mg/L, and the results are illustrated in Figure 4. The
removal efficiency decreased with increasing adsorbate con-
centration in the solution. On the other hand, the amount of As
adsorbed increased with increasing initial sample concentration.
These results indicate that, provided that batch methods are
applied, the removal efficiencies can be better compared with
those obtained in the present work. At an initial arsenic
concentration of 0.5 mg/L, the adsorption amounts were 16 and
13 µg of As/g of RH for As(III) and As(V), respectively.
Effect of pH. pH is one of the most important parameters
controlling the metal ion sorption process.37,38 Figure 5 depicts
the effect of pH on As(III) and As(V) removal with RH. The
removal efficiency of As(V) increased slightly with increasing
pH, was nearly constant above pH 8, and decreased markedly
at pH >12. For the removal of As(III), the efficiency curve
was essentially a plateau in the pH range of 4-10, and then,
the efficiency tended to decrease with increasing pH. The poor
As removal efficiencies at high pH can be attributed to the
following factors: First, both chemical species for As(III) and
As(V) in this pH region are oxyanions. Next, hydroxyl groups
are more plentiful on the surface of RH with increasing pH.
The maximum removal efficiencies for As(III) and As(V) were
8108 Ind. Eng. Chem. Res., Vol. 45, No. 24, 2006
Figure 6. Breakthrough curves for the removal of As(III) and As(V) by
adsorption onto rice husk (initial As concentration, 100 µg/L). b: As(V);
RH, 6 g; avg particle size, 510 µm; treatment flow rate, 1.7 mL/min. 0:
As(III); RH, 6 g; avg particle size, 780 µm; treatment flow rate, 6.7 mL/
min.
observed in comparatively neutral regions (at pH 6.5 and pH
8.0, respectively). These results should be of great advantage
for the practical implementation of arsenic removal from
groundwater.
Breakthrough Curves. Breakthrough curves were investi-
gated for the removal of As(III) and As(V) at an initial
concentration of 100 µg/mL by adsorption onto rice husk using
the optimized conditions, as illustrated in Figure 6. In the
experimental process, the As sample solution was continuously
fed into the RH-packed column, and at a given treatment time
(volume), 3 mL of treated solution was sampled and subjected
to GFAAS analysis. The breakthrough volumes for As(III) and
As(V) can be relatively small (approximately 100 mL). Because
the exhaustion volumes were comparatively large, the total
amount of each solute removed from the sample upon saturation
of the adsorbent, which is equal to the amount of solute that
the adsorbent phase contains, was calculated by the integration
of the area above the breakthrough curve. The amounts adsorbed
under the specified removal conditions were 20 and 7 µg of
As/g of RH for As(III) and As(V), respectively.
Adsorption Mechanism. Arsenic removal by adsorption onto
RH can be supposed to occur mainly through two routes: (i)
affinity adsorption and (ii) anion exchange between the arsenic
in the water and the carbon surface of the rice husk. Affinity
adsorption is related to the surface behavior of RH, whereas
anion exchange relates to the existing forms of the arsenic
species. OH groups are created on the carbon surface during
the activation process.39,40 The mechanism of adsorption of metal
anions onto activated carbon is generally well explained by
electrochemical theory: Carbon in contact with water reduces
oxygen to a hydroxyl group41
O2 + 2H2O + 2e- f H2O2 + 2OH- (2)
and thus, the carbon loses electrons and become positively
charged. Electrical neutrality is maintained with hydroxyl ions,
resulting in their adsorption. Although the rice husk used in
the present work was not subjected to any chemical or physical
activation treatment, a large number of OH groups will remain
on the surface of the RH after the drying process. When a metal-
bearing solution contains anions that exhibit a higher affinity
toward carbon than the hydroxyl groups, the latter are ex-
changed, as shown in the case of As(V)
carbon-(OH)2 + HAsO42- f carbon-HAsO4 + 2OH-
(3)
In the present study, the removal of uncharged As(III) species
from the solution by adsorption onto RH took place more readily
Table 1. Influence of the Eluent on the Desorption of As(III) and
As(V)a
desorption (%)b
desorption agent standing time (h) As(III) As(V)
KOH (2 M) 8 65 81
12 65 80
18 67 80
24 69 82
36 71 83
KOH (1 M) 8 65 77
16 65
20 68
NaOH (1 M) 8 51 75
HCl (1 M) 8 3 0.6
HNO3 (1 M) 8 3 1.4
H2SO4 (1 M) 8 2 0.5
a Adsorption process: initial As concentration, 100 µg/L; RH, 4 g;
average particle size, 780 µm for As(III) and 510 µm for As(V); treatment
flow rate, 6.7 mL/min for As(III) and 1.7 mL/min for As(V); efficiency,
89% for As(III) and 87% for As(V). b Volume of desorption agent, 50 mL.
than the removal of charged As(V) species. At pH values of
less than 9, neutral H3AsO3 is predominantly present as As(III)
species. The As(III) removal efficiency from solution by
adsorption onto rice husk was found to be much better than
that of As(V) in the neutral pH range. These results can be
attributed to the lack of electrostatic repulsion between the
surface and the neutral As(III) species. The physical adsorption
and interaction between the H3AsO3 species and the rice husk
surface might be partly responsible for the removal of As(III).
From the information in the literature, it is not clear which
process is predominant for the adsorption of As onto rice husk.
These mechanisms are still being examined.
Desorption. Recovery of the adsorbed material and regenera-
tion of the adsorbent are also important aspects of wastewater
treatment. Attempts were made to desorb both As(III) and
As(V) from the RH surface with various eluents, such as
hydrochloric, sulfuric, and nitric acid solutions and base
solutions containing sodium hydroxide and potassium hydroxide.
This desorption process was performed using the batch method.
For each experiment, 50 mL of desorption solution was added
to the column and held there for a fixed period of time. After
the standing time, the solution was passed through the column.
The results are presented in Table 1. Although the achievement
of arsenic elution using strong acidic or alkaline solutions has
been reported in the literature,42 the present work showed that
effective desorption was obtained with alkaline solutions. These
phenomena are consistent with the results observed for the effect
of pH. In general, the desorption efficiency of arsenic tended
to increase with increasing desorption time. Consequently,
potassium hydroxide solution was useful for the desorption of
arsenic from the surface of RH.
Application of the Developed Treatment System. The
utility of the waste RH was evaluated for the treatment of As-
contaminated Bangladeshi groundwater samples. The concentra-
tions of total arsenic in the samples were 270 and 595 µg/L. It
has been reported that the total arsenic concentration in the
tubewell water is in the range 0.25-1 mg/L, with 60-90% of
the arsenic present as As(III) species.43 Because the pH of these
groundwater samples was around 7, the arsenic species might
be HAsO42- for As(V) and H3AsO3 for As(III).13,14,44 The
treatment results are presented in Table 2. Although 12 g of
adsorbent was applied in the treatment, the concentrations of
arsenic in the treated sample water could be lowered to 10 and
26 µg/L. The desorption efficiencies with 100 mL of 1 M KOH
were 71% and 96%. From the present results, the arsenic was

Table 2. Removal and Desorption of As from the Contaminated
Groundwater of Bangladesh
sample 1 sample 2
pH 7.8 7.6
initial As concentration (µg/L) 270 595
final concentration (µg/L) 10 26
removala (%) 96 96
desorptionb (%) 96 71
a Removal: RH, 12 g; average particle size, 780 µm; flow rate, 0.8 mL/
min. b Desorption: 1 M KOH, 100 mL; standing time, 8 h.
successfully removed from practical As-contaminated ground-
water, and the adsorbed As could be recovered from the surface
of RH. On the basis of the present treatment system, purification
of 10 L of As-contaminated groundwater will be achievable
with 1.2 kg of rice husk in a treatment time of 125 min.
Conclusions
The proposed column treatment systems are appropriate and
suitable homemade approaches to arsenic removal in local areas,
because of their simplicity and easy operation and handling.
The present method is effective for a wide range of concentra-
tions (i.e., 50-500 µg/L), which were quite similar to those
observed in contaminated Bangladeshi groundwater. No second-
ary-pollution problem will occur, because desorption of the
arsenic is possible. Direct removal of both arsenite and arsenate
can be achieved without first oxidizing arsenite to arsenate,
whereas the traditional methods require the oxidation process.
Because rice husks are abundant agricultural wastes, they are
readily available. Moreover, after the desorption process, RH
can be used as a fuel source because it does not contain any
harmful substances.
Acknowledgment
This work was supported by the Ministry of Education,
Culture, Sports, Science and Technology of Japan and the Grant-
in-Aid for the Japan Society for the Promotion of Science (JSPS)
Fellows 16‚04403.
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ReceiVed for reView March 22, 2006
ReVised manuscript receiVed September 25, 2006
Accepted September 25, 2006
IE060344J