Arsenic removal by iron oxide coated sponge: treatment and waste management
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Transcript of Arsenic removal by iron oxide coated sponge: treatment and waste management
Arsenic removal by iron oxide coated sponge: treatment
and waste management
Tien Vinh Nguyen, Abdur Rahman, Saravanamuthu Vigneswaran,
Huu Hao Ngo, Jaya Kandasamy, Duc Tho Nguyen, Tuan Anh Do
and Trung Kien Nguyen
ABSTRACT
Tien Vinh Nguyen
Abdur Rahman
Saravanamuthu Vigneswaran (corresponding
author)
Huu Hao Ngo
Jaya Kandasamy
Faculty of Engineering,
University of Technology, Sydney (UTS),
PO Box 123, Broadway,
Sydney NSW 2007,
Australia
E-mail: [email protected]
Duc Tho Nguyen
Tuan Anh Do
Trung Kien Nguyen
Institute of Environmental Technology,
18 Hoang Quoc Viet Road,
Cau Giay,
Hanoi,
Vietnam
One of the problems in drinking water that raises concern over the world is that millions of people
still have to use arsenic-contaminated water. There is a worldwide need to develop appropriate
technologies to remove arsenic from water for household and community water supply systems.
In this study, a new material namely iron oxide coated sponge (IOCSp) was developed and used to
remove arsenic (As) from contaminated groundwater in Vietnam. The results indicated that IOCSp
has a high capacity in removing both As (V) and As (III). The adsorption capacity of IOCSp was up
to 4.6mg As/g IOCSp, showing better than many other materials. It was observed from a pilot
study that a small quantity of IOCSp (180g) could reduce As concentration of 480mg/L in 1.5m3 of
contaminated natural water to below 40mg/L. In addition, an exhausted IOCSp, containing a large
amount of arsenic (up to 0.42 wt %) could safely be disposed through the solidification/stabilization
with cement. Addition of fly ash also reduced the amount of arsenic in the leachate.
Key words | arsenic, cement, drinking water, iron oxide coated sponge (IOCSp),
solidification/stabilization, water treatment technology
INTRODUCTION
Arsenic is a toxic element that can be fatal to human health.
It can have a significant adverse impact on the environ-
ment. Arsenic exists in several oxidation states (2III, 0,
þ III and þ V) in the environment. However, in natural
water, arsenic is mostly found in inorganic form as
oxyanions of trivalent arsenite [As(III)] or pentavalent
arsenate [As(V)]. The toxicity of arsenite is 25–60 higher
than that of arsenate. Arsenic occurs in extremely high
concentrations in groundwater in Bangladesh and a number
of other countries (Vietnam, India, Nepal, China, America).
In Bangladesh, 1.2 million tube wells (29%) were found
to be contaminated with arsenic. It is estimated that
85 million people are at risk from arsenic contamination
(Hossain 2006).
Different treatment technologies are reported in the
literature for arsenic removal. USEPA suggested ion
exchange, activated alumina, reverse osmosis, modified
coagulation/filtration and modified softening as best avail-
able technologies (BAT) (USEPA 1999). Other technologies
emphasized are: iron based coagulation assisted microfiltra-
tion, iron oxide coated sand, manganese greensand filtration
and granular ferric hydroxide (GFH). Appropriate treat-
ment depends on many factors, for example, concentration
of arsenic, water composition, pH and cost effectiveness.
Polyurethane is a polymer consisting of a chain of
organic units joined by urethane links. Generally, the chara-
cteristics of polyurethane depend on the manufacturing
method and the starting chemicals used. As a result,
polyurethane sponge can be flexible (for example sponge
used in furniture cushions) or rigid (for example sponge
used in construction panels). Flexible polyurethane are
made from polyols of moderately high molecular
doi: 10.2166/wst.2009.477
1489 Q IWA Publishing 2009 Water Science & Technology—WST | 60.6 | 2009
weight and low degree of branching, whereas rigid
polyurethane are prepared from highly branched resins of
low molecular weight (Braun et al. 1985). Other properties
of polyurethane (PU) such as foam density, cell structure,
rate of wetting, and water retention vary depending on the
ratio of polymer to cross - linking agent, foaming tempera-
ture, pH, and the type and amount of additives (Havens &
Rase 1993).
To increase the effectiveness of sponge, many researchers
have incorporated additives into polyurethane sponge.
Brookes et al. (1987), Hu et al. (1994) have put living
microorganisms into polyurethane foam matrices as a
method of immobilization and used these sponges as
biofilter media to remove phenols from wastewater. Other
researchers (Wood et al. 1982; Havens & Rase 1993)
have immobilized active enzymes in the foam and used
such materials in biological waste-gas treatment system.
Additionally, Lupton & Zupanac (1991) used polyurethane
foam containing PAC and immobilized microorganisms
for the treatment of wastewater containing phenol.
Al-Marzouqi et al. (2003) reported that low density poly-
urethane sponge (13 kg/m3) has the highest capacity for
absorbing oil (0.06 m3 oil/kg sponge after one minute)
in cooperation with palm trunk, pin fish fiber, rice bag,
feathers, and PP pad sponge.
Sponge is an ideal material for adsorption because
it is very porous and its large surface area facilitates
arsenic adsorption. In addition, sponge is cost effective so
it can be applied in small communities as well as in
developing countries. To achieve high arsenic adsorption,
sponge should be coated with metal oxide because arsenite
and arsenate are strongly attracted to iron oxide. Once
adsorption of arsenic onto a sponge matrix is exhausted,
sponge can be directly disposed of or regenerated with
chemical solutions in extreme cases. Sponge can easily be
compressed and incorporated into building materials such
as concrete, making its disposal easier.
A new adsorbent material, iron oxide coated sponge
(IOCSp), exhibited a high capacity to remove arsenic due to
its physical characteristics (high internal porosity and
specific surface) as well as its high iron oxide content
(12%) (Nguyen et al. 2006). However, the waste from this
treatment process (exhausted IOCSp) also needs to be
treated properly.
As a consequence of the toxicity of arsenic, traditional
ways of direct dumping of arsenic waste are no longer
acceptable. For this reason, it has become necessary to
develop a cheap and effective method for processing arsenic
waste accumulated during the water treatment process,
especially from household and community water supply
systems. Different treatment processes such as coagulation,
flocculation, adsorption or membrane processes that are
often used to treat arsenic-contaminated water, cannot
destroy arsenic completely, rather all these processes convert
arsenic into different forms or transform it into- insoluble
compounds in combination with other elements, such as
iron. The safe disposal of arsenic wastes is a problem.
Encapsulation of arsenic through solidification/
stabilization (S/S) techniques is the most attractive solution
for dealing with the arsenic waste. Although solidification/
stabilization do not demolish the toxic but this method could
eliminate the effect of the toxic to nearby environment. In
solidification process, waste is encapsulated to form a solid
material whereas chemical reactions in stabilization process
could reduce the leachability of a waste (USEPA 2000).
A number of researchers have investigated arsenic S/S
processes using different solidifying materials: Portland
cement (Akhter et al. 1990; Buchler et al. 1996), Portland
cement and iron (II) and (III) (Taylor & Fuessle 1994),
Portland cement and lime (Dutre & Vandecasteele 1998),
Portland cement, iron and lime (Palfy et al. 1999), Portland
cement and fly ash (Chu et al. 1991; Akhter et al. 1997),
Portland cement and silicates (Chu et al. 1991).
Akhter et al. (1990) studied different methods for the
immobilization of arsenic in contaminated soil with an
arsenic concentration of 12,200 mg/L. They tested mixtures
of type I Portland cement, type F fly ash, blast furnace slag,
lime and silica fume. Their results showed that the
performance of Portland cement alone is much better
than that of other reagent or combination (The ratio of
soil: cement ¼ 1: 0.44). The arsenic compound in the waste
also has a strong effect on the success of the S/S process
(Buchler et al. 1996). By applying the Toxic Characteristic
Leaching Procedure (TCLP), leachate concentrations was
found to vary between 1.7–510 mg/L. The experimental
results showed that S/S was a better treatment process for
wastes containing either sodium arsenate or sodium
arsenite than the one containing arsenilic acid. The arsenic
1490 T. V. Nguyen et al. | Arsenic removal by iron oxide coated sponge Water Science & Technology—WST | 60.6 | 2009
in leachate concentrations was 1.7–2.1 mg/L for sodium
arsenate and arsenite respectively in comparison with
510 mg/L for arsenilic acid.
To increase the effectiveness of S/S, a number of
additives were used in the cementation process. Iron
appears to be the favored selection. The research of Taylor
& Fuessle (1994) showed that oxidation states of iron
and arsenic have strong affected on the S/S process.
Solidification investigation of an industrial waste containing
a large amount of arsenic (23–47% arsenic) with cement
and lime was carried out by Dutre & Vandecasteele (1998).
Solidification with cement and lime was found to be
a suitable technique to reduce the leachability of arsenic
from the waste. This process could reduce 99.9% leachate
concentration (from 5 g/L to only 5 mg/L). Palfy et al. (1999)
found the optimum ratios of Ca:As and Fe:As was 8 and 6
respectively for the stabilization of waste arising from the
carbon dioxide scrubbing. The stabilisation process could
help to reduce the leachate concentration from 6,430 mg/L
to 0.823 mg/L.
In this research, detailed experiments were conducted
to evaluate the capacity and effectiveness of the new coated
material IOCSp in removing different forms of arsenic
(As(III) and As(V)) from arsenic-contaminated synthetic
water in the laboratory and natural groundwater in
Vietnam. The encapsulation of exhausted IOCSp through
the S/S technique was also carried out.
EXPERIMENT
Experimental materials
Water
In this study, two kinds of water were used. In the batch
experiments, synthetic water (tap water spiked with the
required concentrations of As(III) and As(V)) was used. In
order to evaluate the effectiveness of IOCSp in practice,
actual groundwater samples from Hanoi, Vietnam were also
employed. The characteristics of the synthetic water and
groundwater used are presented in Table 1. Arsenic
concentration was determined by hydride generation
atomic absorption spectroscopy (HGAAS).
Standards and reagents
All chemicals used in this study were reagent grade, and
were used without any purify cation.
Iron oxide-coated sponge (IOCSp)
Commercial polyurethane (PU) sponge was coated with
iron oxide (IOCSp contains 12% of iron oxide). The method
of preparation is explained elsewhere (Nguyen et al. 2006).
Cement
Common cements, including Type I Portland cement and
Type F fly-ash were used for solidification.
Experimental study
Batch equilibrium study
Equilibrium studies were conducted at a pH of 7 using
IOCSp and synthetic water with As(III) and As(V)
concentrations of 5 mg/L. Equilibrium studies were con-
ducted at the room temperature of 228C. In these
experiments, different amounts of adsorbent (0.018 g
to 1.296 g) was placed into 250 mL Erlenmeyer flasks
containing 100 mL of the arsenic sample, and the samples
were shaken at 130 rpm for 20 hours. After 20 hours of
contact time, samples from each flask were decanted and
analyzed for the residual arsenic in the solution.
Table 1 | Characteristics of the synthetic water and groundwater used in experiments
Parameters Synthetic water Hanoi groundwater
As(III) & As(V) 0.26–5 0.480
pH 7 6.5–7.3
Iron 0.016–0.09 3.6
Manganese 0.004–0.02 0.9
Nitrate 0.74–2 N/A
Copper 0.001–0.049 0.05
Zinc ,0.005 0.01
Phosphate 0.004 1.8
Silicate 0.8 17
Note: All parameters are in mg/L, except pH, N/A: Not available.
1491 T. V. Nguyen et al. | Arsenic removal by iron oxide coated sponge Water Science & Technology—WST | 60.6 | 2009
Pilot study
Pilot scale experiments were conducted to study the
removal of arsenic from groundwater in Hanoi, Vietnam.
A bucket of 200 mm in diameter and 350 mm in height
was used in the study. The bucket was packed with 180 g
of IOCSp. The test was conducted at a normal pH of
water of between 6.5–7.3. The water was allowed to
flow through the packed bucket at a filtration velocity
of 50 mL/min (which corresponds to 0.1 m/h).
Solidification
The exhausted IOCSp was obtained by mixing IOCSp with
synthetic water for 20 hours. The amount of As(III) and
As(V) in the exhausted IOCSp were calculated by following
equation:
Q ¼ ðCo 2 C1Þ*V =M
in which: Co: initial As(III) and As(V) concentrations of
synthetic water, C1: As(III) and As(V) concentration of
synthetic water after 20 hours contact with IOCSp, V:
Volume of synthetic water, M: Amount of IOCSp.
The exhausted IOCSp were solidified in different
concrete samples with different ratios of cement: sand:
binders and cured for various times. Leachate tests were
conducted by agitating 10 g of the concrete with 100 mL of
aceticacid (10%) for24 h.Hereexhausted IOCSprefers to the
IOCSp which has attained maximum adsorption of arsenic.
RESULTS AND DISCUSSION
Equilibrium adsorption experiments
Adsorption equilibrium experiments were conducted
to evaluate the adsorption capacity of IOCSp. The
equilibrium results were then fitted with Langmuir,
Freundlich, and Sips isotherm equations. The adsorption
curves simulated by all of these models fitted well with
the observed values. The simulated and the experimental
Figure 1 | Prediction of equilibrium adsorption of As by different adsorption models (contact time ¼ 20 hours, mixing rate ¼ 130 rpm, temperature ¼ 228C).
Table 2 | Isotherm equations for arsenic removal using IOCSp (for synthetic water
spiked with arsenic)
Arsenic species
Parameters As(III) As(V)
Langmuir qm 3.85 4.5
b 0.95 0.7
r 0.966 0.974
Equation qe ¼ 3.66C/(1 þ 0.95C)
qe ¼ 3.15C/(1 þ 0.7C)
Freudlich kF 1.97 1.9
n 3.5 2.8
r 0.985 0.990
Equation qe ¼ 1.97C 0.29 qe ¼ 1.9C 0.36
Sips qm 4.2 4.6
b 0.91 0.74
n 1.27 1.22
r 0.965 0.972
Equation qe ¼ 4.18 (0.91C)0.79/(1 þ (0.91C)0.79)
qe ¼ 4.6 (0.74C )0.82/(1 þ (0.74C )0.82)
1492 T. V. Nguyen et al. | Arsenic removal by iron oxide coated sponge Water Science & Technology—WST | 60.6 | 2009
concentrations of the remaining As(III) and As(V) are
shown in Figure 1. The model equations and the isotherm
parameters are shown in Table 2.
Where Ce: the equilibrium concentration (mg/L),
Langmuir model qe ¼ ðqmbCe=1 þ bCeÞ, b: Langmuir
constant related to the binding energy of adsorption
(L/mg), qm: the saturated maximum monolayer adsorption
capacity (mg/g), Freundlich isotherm qe ¼ KF·C1=ne , KF:
a Freundlich constant indicative of the adsorption
capacity of the adsorbent, n: an experimental constant
indicative of the adsorption intensity of the adsorbent,
Sips model qe ¼ qmðbCeÞ1=n=1 þ ðbCeÞ
1=n has the features
of both the Langmuir and Freundlich isotherm models.
It can be seen that the Langmuir and Sips models
yielded the same values for arsenic adsorption capacity
(qm). The values were 3.85–4.2 mg As(III)/g IOCSp and
4.5–4.6 mg/g IOCSp respectively. The values of b for
both models were almost same. It was in the range of
0.91–0.95 for As(III) and 0.7–0.74 for As(V). This predic-
tion shows that there is not much difference between these
two models in describing the adsorption of a single
component system. The low value of 1/n (,0.36) in the
Freundlich isotherm suggests that any large change in the
equilibrium concentration of soluble arsenic would not
result in a significant change in the amount of arsenic
sorbed by the IOCSp. The correlation coefficient (r) for all
the isotherms ranged from 0.965 to 0.99, representing a
good fit of the observed data.
In this study, the value of the adsorption capacity of
IOCSp (qm) is much higher than that with a number of
other adsorbents (Table 3). This indicates that IOCSp has
a superior arsenic adsorption capacity.
Pilot experiments
Following the success of the IOCSp system in removing
arsenic at the University of Technology, Sydney (UTS),
Australia, the IOCSp pilot system was tested with ground-
water contaminated with arsenic in Vietnam. To evaluate
the effectiveness of IOCSp under actual conditions,
pilot experiments were carried out using groundwater
with an arsenic concentration of 480mg/L from a well
in Hanoi, Vietnam. The filter was run at a filtration rate
of 0.1 m/h. The column (bucket) was packed with 180 g
of IOCSp. These experiments were conducted using
a small bucket of 200 mm in diameter and 350 mm in
height (Table 4).
During the initial stage of the experiment, the effluent
arsenic concentration was less than 10mg/L (up to a
throughput volume of 330 L). After this, the arsenic in the
effluent increased slowly but the effluent concentration was
Table 3 | Comparison of arsenic adsorption capacity of IOCSp with other adsorbents
Name of adsorbent Adsorption capacity (mg/g) References
Iron oxide coated sand 0.029 Gupta et al. (2005)
Granular ferric hydroxide 0.11 Thirunavukkarasu et al. (2003)
Activated alumina 0.180 Singh & Pant (2004)
Red mud 0.66 Altundogan et al. (2000)
Ferruginous manganese ore 0.680 Chakravarty et al. (2002)
Iron oxide impregnated activated alumina 0.734 Kuriakose et al. (2004)
Activated red mud 0.87 Altundogan et al. (2002)
Nanoscale zero valent iron 3.5 Kanel et al. (2005)
Iron oxide coated sponge 3.85–4.6 This study
Table 4 | Arsenic removal from groundwater by IOCSp bucket
No Throughput volume (L) Effluent conc. (mg /L) Bed volume
1 75 4 11
2 330 10 47
3 1,120 20 160
4 1,410 31 201
5 1,550 40 222
1493 T. V. Nguyen et al. | Arsenic removal by iron oxide coated sponge Water Science & Technology—WST | 60.6 | 2009
still lower than 40mg/L even when the bed volume was
about 222 (which correspond to a throughput volume of
about 1,550 L).
Solidification experiments
The safe disposal of IOCSp after the adsorption process
is very important to prevent the spreading of toxicants
into the environment. In this study, the fully exhausted
IOCSp (containing up to 0.42% of arsenic) were solidified
in different concrete samples with different ratios of
cement: sand: binders and cured for various times. The
As(III) and As(V) concentrations in the effluent after
leaching test are presented in Table 5.
The results showed that arsenic concentration in the
leachate of the concrete samples was very low, from 1 to
35mg/L. The percentage of arsenic leached in term of
quantitative was only from 0.1 to 1.1%. The low leachability
of arsenic in the samples is attributed to the high affinity of
arsenic to the iron oxide coated in sponge. The arsenic
concentration in the leachate increases with decreasing
ratios of cement. However, this decrease was very small.
The results also showed that fly ash can help in reducing
arsenic concentration in the leachate, especially with As(V)
through the formation of insoluble fly ash–arsenic com-
pound in the leachate. Arsenic concentration in the
leachate of samples added by fly ash was at least three
times lower than the samples without adding fly ash
(Table 5). The addition of lime also increased the capture
of arsenic but the effect of lime addition was smaller than
that of fly ash.
The batch extraction results indicate that the exhausted
IOCSp have no adverse effect on the environment if it is
properly encapsulated in cement. Only a small amount of
arsenic is released from the concrete. The concrete can be
used as road base or safely disposed directly in the landfill.
The ratio of cement: sand in the first 3 samples were based
on the Vietnamese standard for concrete. If the ratio of
cement: sand and cement: IOCSp increased (more than 3.5
and 50 respectively), the hardness of concrete decreases
significantly although arsenic is still captured in the
concrete. In this case, the concrete should be disposed
directly to landfill as it is not suitable for road base.
CONCLUSIONS
IOCSp exhibited a high arsenic removal capacity in both
batch and column experiments. The high removal capacity
of IOCSp was due to its physical characteristics (high
internal porosity and specific surface) as well as its high iron
oxide content (12%). The IOCSp adsorption equilibrium
results with synthetic water were successfully simulated by
Langmuir, and Sips models. The adsorption capacity of
IOCSp (up to 4.2 and 4.6 mg of As(III) and As(V) per gram
of IOCSp respectively) was much higher than that of a
number of adsorbents such as ferruginous manganese
ore (0.680 mg/g), iron oxide coated sand (0.029 mg/g),
activated alumina (0.180 mg/g), red mud (0.66 mg/g), iron
oxide impregnated activated alumina (0.734 mg/g),
and activated red mud (0.87 mg/g) (Altundogan et al.
2000, 2002; Chakravarty et al. 2002; Kuriakose et al. 2004;
Table 5 | Effect of additives on leachate concentration
Weight of additives per 2g of exhausted IOCSp material (g) Leachate concentration (mg/L)
No Cement Sand Lime Fly ash
1 day 1 week 1 month
As(III) As(V) As(III) As(V) As(III) As(V)
1 150 230 0 0 24 21 23 18 16 14
2 150 320 0 0 27 28 26 23 21 15
3 150 320 75 0 16 9 17 12 13 6
4 50 125 0 0 32 19 35 25 27 22
5 50 190 0 10 20 12 5 2 13 1
6 100 350 0 50 12 6 3 3 8 2
7 150 525 0 75 5 3 2 2 8 1
1494 T. V. Nguyen et al. | Arsenic removal by iron oxide coated sponge Water Science & Technology—WST | 60.6 | 2009
Singh & Pant 2004). The IOCSp filter yielded consistent
arsenic removal efficiency for a long period. A bucket
(20 cm diameter and 35 cm height) packed with 180 g of
IOCSp reduced As from 480mg/L to less than 40mg/L. The
bed volume was 222. Once adsorption of arsenic onto a
sponge matrix is exhausted, IOCSp can easily be com-
pressed and incorporated into building materials such as
concrete, making its disposal easier. The results showed that
solidification process with cement is suitable to encapsulate
arsenic into the cement. This simple method can help in
managing the disposal of waste in an inexpensive and safe
way. This simple method can be applied in small commu-
nities as well as in developing countries.
ACKNOWLEDGEMENTS
This research was funded by the Australian Research
Council (ARC) Discovery Grant (DP0450037: Healthier
Water: Innovative Processes for Arsenic Removal and
Sludge Management) and ARC International Linkage
Grant (LX0345566: A better way to remove arsenic from
drinking water).
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