Journal of Applied Science and Engineering, Vol. 18, No. 4, pp. 323-330 (2015)
DOI: 10.6180/jase.2015.18.4.02
Arsenic of Adsorption Characteristics in Taiwan Soils
Shui-Wen Chang Chien1, Shou-Hung Chen2* and Kun-Jie Huang1
1
Department of Environmental Engineering and Management, Chaoyang University of Technology,
Taichung, Taiwan 413, R.O.C.
2
Department of Geography, Chinese Culture University,
Taipei, Taiwan 111, R.O.C.
Abstract
In soil environment, various forms of solid-phase arsenic of total amount of arsenic and the
aqueous form of arsenic in soil solution make a thermodynamic equilibrium system. The uptake of
aqueous arsenic by crop roots results in the shift of this equilibrium system. The purpose of this
research was thus to investigate the adsorption characteristics of aqueous As (III) and As (V) in Taiwan
soils. The results from the adsorption batch experiment showed that the adsorption capability of the
soils increased with increasing amounts of Fe, Mn and Al oxides. In addition, the adsorption of As (V)
was higher than As (III) by the same soil. Because of the competition between phosphate and arsenite/
arsenate anions for the adsorption sites on the soils, the samples with high amount of bound phosphate
were less capable to adsorb aqueous arsenic. The desorption of arsenic occurred within 2-3 hr when
the soils were submerged in water. This contributed to the increase of concentration of aqueous arsenic
in the reaction systems. In the batch experiment, the kinetics analyses of the adsorption of As (III) and
As (V) by the soils showed that the main reaction was of zero order in 0 to 24 hr and of the 3rd order in
some few reaction periods.
Key Words: Arsenic, Aqueous Form, Adsorption, Desorption, Kinetics
1. Introduction
Naturally arsenic exists in rocks and minerals. Due
to weathering, erosion and volcanic emissions, arsenic
contacted the groundwater and develops pollutant [1].
Arsenic is one of the most harmful and toxic element
found in nature. It was a slowly poisoning element which
severely affected the human health and other living organisms [2]. Arsenic is among the inorganic contaminants
that have become of evolving environmental concern
lately because it is a toxic substance to both animals and
plants. Its geochemical dispersion into the environment
naturally occurred through weathering processes and this
could be enhanced by mining activities which might lead
to important local and regional pollution of soil and water. In industry, arsenic was mainly used as the wood pre*Corresponding author. E-mail: [email protected]
servative, hence it was used in dyes, paints and pigmenting substances. It was also used in glass-making, electronics manufacturing and leather tanning industries. A
small amount of arsenic was used in both human and animal medications and care products, and it was present in
many food supplement products also [1]. The actual distribution, mobility, bioavailability, toxicity, bioaccumulation, and biodegradability of arsenic depended not only
on its total concentration but also on its chemical form in
the sample [1]. Arsenic can exist in inorganic form, organic form and gaseous state. Organic arsenic species are
less harmful and readily eliminated by the body. However, the inorganic form of arsenic is highly toxic compared to organic arsenic. Inorganic arsenate and arsenite
referred to a pentavalent As (V) and trivalent As (III), respectively, were most common in natural waters [3]. As
(III) was 60 times more toxic than As (V) because of its
greater cellular uptake [3].
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Shui-Wen Chang Chien et al.
Arsenic normally derived from surface water or groundwater, depending on local availability, which are very
variable in their arsenic contents, although the highest
concentrations were often found in groundwater [4]. The
arsenic contamination of soils and water represented a
great threat to human health because of its high potential
to enter into the food chain [5]. Long-term exposure to
inorganic arsenic compounds could lead to various diseases such as conjunctivitis, hyperkeratosis, hyper pigmentation, cardiovascular diseases, disorders of the central nervous system and peripheral vascular system, skin
cancer and gangrene of the limbs [5-7]. Additionally, arsenic poisoning also led to death from multisystem organ
failure by allosteric inhibition of sulfhydryl containing
essential metabolic enzymes. It also interfered with some
biochemical processes involving phosphorous owing to
the similar chemical properties [5-7].
According to World Health Organization (WHO) and
United States Environmental Protection Agency (US
EPA), the maximum allowed concentration of arsenic in
drinking water is 10 mg L-1 [8]. However, the arsenic concentrations about 100 times more than the permissible
limit were found in many areas around the world [1,4].
Blackfoot disease is an endemic peripheral vascular disease found among the inhabitants of a limited area on
the southwest coast of Taiwan, where artesian well water
with a high concentration of arsenic has been used for
more than eighty years [9,10]. The rapid expansion of industry and commerce development in Taiwan had caused
the difficulties in land acquisition. As a result, industrial
zones built around agricultural areas had caused pollution problems. To increase the agricultural output, farmers
used pesticides and fertilizer excessively which were another arsenic pollution source. Adsorption was one of the
most commonly reported, and it would occur possibly the
initial reaction when arsenic interacted with soils [11].
There were many factors which affected the arsenic adsorption in soil. Arsenic was known to strongly adsorb by
inorganic constituents in soils such as clay minerals, iron
(Fe) and aluminium (Al) oxides/hydroxides. Both As (V)
and As (III) had the strong affinities for Fe and Al oxides
[11,12], and even the soil organic matter content exhibited the most important influence on arsenic adsorption
[13]. From adsorption research performed on 18 soils with
varying soil properties, Burns et al. (2006) reported that
arsenic adsorption was highly correlated with the soil pH
and iron oxide content [14]. In addition, X-ray spectroscopy studies demonstrated the formation of strong innersphere complexes between adsorbed arsenic and the adsorbent surfaces that were mainly composed of Fe/Al
oxides [11,12]. The concentration of phosphate (PO4)
was also a main factor which affected the As adsorption
negatively, because PO4 had a competition for adsorption
sites with As (V) [15]. Understanding of the As (V) and
As (III) adsorption processes in Taiwan soils was poor.
Therefore, the objectives of this research were to examine the As (V) and As (III) adsorption behavior with soils
samples collected around Taiwan. This fundamental research would be helpful for further application in the
treatment of arsenic contaminated Taiwan soils.
2. Materials and Methods
2.1 Soil Sample Collection
Two alluvial soil samples with low arsenic concentration were collected from cultivated land at Xihu Township in Changhua and Gueiren District in Tainan, one red
soil was collected from Pingzhen District in Taoyuan.
All samples were used for the batch of adsorbability test
for inorganic arsenic.
Each sample consisted of ten random sub-samples,
and each sampling point ncluded surface soil (0~15 cm)
and bottom soil (15~30 cm). The soil samples for the
batch of adsorbability test were collected from surface
soil (0~15 cm). Individual sub-samples were mixed, air
dried, grinded, and stored in plastic bottles after 2 mm
sieving.
2.2 Analysis of Soil Characteristics
Soil pH was measured in soil suspension at 1:1 (w/v)
soil solution ratio using glass electrode [16]. Electrical
conductivity (EC) was measured with electric conductor
using the soil suspension prepared as described above
[17]. Organic carbon was determined by dry heating method [18]. Soil texture was tested with the hydrometer
method [19]. Cation exchange capacity of the soil was
evaluated with the ammonium saturation method [20].
Valid phosphorous was determined with Bray NO. 1 method [21]. Crystallized manganese, iron and aluminum
oxides were determined using the methods of Mehra and
Arsenic of Adsorption Characteristics in Taiwan Soils
Jackson (1960) [22]. Citrate-bicarbonate-dithionite (CBD)
reagent solution was used to dissolve oxidized manganese, oxidized iron and oxidized aluminum in the soil
and then the concentration of manganese, iron and aluminum in suspension was analyzed using Inductively
Coupled Plasma-Optical Emission Spectrometer (ICPOES) to calculate the concentration of manganese, iron
and aluminum in soil. Irregular iron, manganese and aluminum oxides extracted by ammonium oxalate were analyzed by Schwertmann (1964) method [23], using 0.2
M of ammonium oxalate at pH 3.0 for extraction.
2.3 Batch Experiments on the Adsorbability of
Arsenic Based on Soil Compositions
Each 10 g surface soil sample collected from Pingzhen District (red soil), Xihu township (alluvial soil), and
Gueiren District (alluvial soil) was added with 100 mL of
HAsO42- or AsO 2- solution whose As concentration was
6 mg L-1 to mix into suspension with soil and solution
ratio at 1:10 (w/v). Then the samples were oscillated for
1 h, 2 h, 4 h, 8 h, 12 h, 16 h and 24 h, and centrifuged
(33,000 g), the supernatant was filtered (No. 42) and measured the residue concentration of arsenic by inductively
coupled plasma atomic emission spectrometry (ICP-OES,
IRIS Intrepid II XSP, Thermo Scientific).
325
observed that the presence of PO43- greatly decreased As
(V) sorption by soils containing low amounts of Fe oxides
but had little effect on the amount of As (V) adsorbed by
soils with high Fe content [24]. Chen et al. (2010) found
that there was no competitive effect of the presence of
equimolar As (III) or As (V) adsorption [25]. Our results
Figure 1. The adsorption tendency of aqueous As (III) and As
(V) on Pingzhen soil at room temperature.
3. Results and Discussion
The adsorption tendency of soil samples in this research were shown in Figures 1-3. The adsorption follows in the order: Pingzhen > Gueiren > Xihu soil. It was
interesting to note that Pingzhen soil contain the higher
content of oxides as well as lower content of phosphorous (P) as compared with Xihu and Gueiren soil series
(Table 1). In this research, the contents of P in soil samples collected from Pingzhen, Gueiren and Xihu were
7.62 mg kg-1 and 42.1 mg kg-1 and 212 mg kg-1, respectively, thus Pingzhen and Gueiren soil provided less valid
adsorptive positions for P than Xihu soil. These results
indicated that the tested soils could provide valid adsorptive positions to P and As (Figures 1-3, Table 1). Violante and Pigna (2002) studied the competitive sorption
of PO43- and As(V) on selected clay minerals [15]. They
found that PO43- could inhibit As (V) sorption on clay
minerals such as gibbsite and kaolinite. Smith et al. (2002)
Figure 2. The adsorption tendency of aqueous As (III) and As
(V) on Xihu soil at room temperature.
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Shui-Wen Chang Chien et al.
were in agreement with these previous reports that the P
content negatively correlated with arsenic adsorption.
As seen in Figures 1-3 and Table 2, the concentration of As (III) and As (V) in water soluble form of surface soil collected from Pingzhen and Gueiren decreased
rapidly in 0-1 h. In particular, the concentration of As
(V) decreased from 6.01 mg kg-1 to 0.10 mg kg-1 and 0.57
mg kg-1, respectively. During the same period, the content of As (III) decreased in Pingzhen and Gueiren soils
from 5.65 mg kg-1 to 2.01 mg kg-1 and 4.02 mg kg-1, respectively. These results indicated that as soon as arsenic
entered into the soil, it was adsorbed by iron, aluminum
and manganese oxides in soil, and this led to a rapid drop
in concentration of As (III) and As (V) in solution (Table
2). In addition, the data also indicated that the concentration of As (V) in Pingzhen and Gueiren soils remained
nearly stable from 1 h to 24 h, while the same for As (III)
from 1 h to 16 h because of the occupation of valid adsorption positions by As (III) and As (V) within 0-1 h,
and the slowdown of adsorption. Previously, it was reported that the adsorption of As (V) from aqueous solution was rapid in the initial stages of contact and reached
a maximum in the range of 35-60 min for soil [26]. In
this research, within 0-1 h the residual concentration of
Figure 3. The adsorption tendency of aqueous As (III) and As
(V) on Gueiren soil at room temperature.
Table 1. Physical and chemical properties of the soils for the adsorption of batch experiments
Sampling
Texture pH
site
EC
CEC
-1
Pingzhen
Xihu
Gueiren
C
LS
L
Org-C
-1
mS cm cmol kg
4.52 0.210
7.16
6.79 0.209
4.87
5.09 0.651
7.89
%
0.62
0.42
0.72
Total
As
-1
mg kg
10.51
08.0
08.3
Citrate-bicarbonateBray-I P dithionite extractable
Fe
Al
Mn
-1
mg kg
7.62
212
42.1
-1
%
3.83
0.60
0.71
% mg kg
0.61
187
0.05
192
0.09
120
Oxalate extractable
Fe
%
0.30
0.27
0.45
Al
Mn
% mg kg-1
0.25
2.8
0.05
7.2
0.08
5.4
Table 2. The remaining concentrations of As (III) and As (V) after the absorption of aqueous Arsenic in surface soils at
various reaction periods
Pingzhen
Reaction period
hour
0
1
2
4
8
12
16
24
a
a
Xihu
Gueiren
As (III)
As (V)
As (III)
As (V)
As (III)
-1
-1
-1
-1
-1
mg kg
5.65 ± 0.01a
2.01 ± 0.02
2.15 ± 0.01
1.61 ± 0.05
1.61 ± 0.06
0.93 ± 0.00
1.42 ± 0.01
0.05 ± 0.01
mg kg
6.01 ± 0.02
0.10 ± 0.01
0.08 ± 0.00
0.05 ± 0.01
0.03 ± 0.00
0.03 ± 0.00
0.03 ± 0.00
NDb
Standard deviation of the mean. b Not detectable.
mg kg
5.65 ± 0.01
5.74 ± 0.02
5.57 ± 0.02
4.78 ± 0.06
4.81 ± 0.14
3.75 ± 0.03
4.02 ± 0.08
0.28 ± 0.01
mg kg
6.21 ± 0.03
6.18 ± 0.10
5.28 ± 0.14
4.65 ± 0.01
4.28 ± 0.07
4.02 ± 0.03
3.82 ± 0.01
3.31 ± 0.03
mg kg
5.65 ± 0.01
4.02 ± 0.03
4.56 ± 0.02
3.75 ± 0.05
3.40 ± 0.08
3.29 ± 0.10
3.23 ± 0.06
00.16 ± 0.015
As (V)
mg kg-1
6.01 ± 0.03
0.57 ± 0.02
0.76 ± 0.03
0.30 ± 0.02
0.35 ± 0.00
0.31 ± 0.00
0.30 ± 0.00
0.21 ± 0.02
Arsenic of Adsorption Characteristics in Taiwan Soils
As (V) in solution was lower than As (III) (Table 2).
Therefore, the adsorption of As (V) was higher than that
of As (III) and the results were in agreement with the results reported earlier [27,28]. The high adsorption of Arsenic had been a global problem, challenges for Safe
Water Production reported that adsorption of As (V) was
higher than that of As (III) when the molar ratio of As
(III)/As (V) equaled 5:1 and 10:1 [28]. Jain and Loeppert
(2000) found that in the dual-anion system at equimolar
As concentrations of £ 156 mg L-1 each, As (V) influenced
the retention of As (III) in the pH range of 4 to 10 more
pronouncedly than As (III) influenced the retention of
As (V) [29]. The oxidation state of As depended primarily on pH and redox conditions, with As (V) being the
most stable form under aerobic conditions as the pH-dependent deprotonated oxyanions of arsenic acid (H2AsO4and HAsO42-) and As (III) the chemically dominant forms
in reducing environment as a neutral species (i.e., pKa1
= 9.2) at natural pH. Therefore, the As (III) was more difficult to remove from water at neutral pH by means of
adsorption and coprecipitation because of the lack of
electrostatic attraction [30]. However, most As-enriched
groundwater was generally dominated by As (III), up
to 96% of total As [31]. McGeehan and Naylor (1994)
reported that the Fe and Mn oxides were restored and
dissolved by the release of adsorbed arsenic to the solution [32]. Barrachina et al. (1996) observed that 80% of
the total amount of As (III) adsorbed was sorbed by Spanish soil in the first 30 min [31]. O’Reilly et al. (2001)
discovered that As (V) sorption on goethite was initially
rapid, with over 93% As (V) adsorption within 24 h
[32]. In this research, the concentration of As (III) in
Pingzhen and Gueiren soils decreased rapidly from 16 h
to 24 h. The reason was considered that the saturated soil
in anaerobic state reduced Fe and Mn, hence the reduction of Mn increased the As (III) adsorption and As (III)
was oxidized into As (V). In addition, the concentration
of As (III) in Pingzhen soil, As (III) and As (V) in Gueiren
soil might increase after two hours immersed because of
the arsenic desorption (Figures 1 and 3). Further studies
were required to examine the kinetics of both As (III)
and As (V) adsorption in the same soil system. This information was essential because both As (III) (predominantly in the reduced condition) and As (V) (predominantly in the oxidized condition) were often discovered in
327
either redox environments because of the relatively slow
redox transformation of As [33].
The adsorption of As (III) and As (V) by Xihu soil
during the period of 0-16 h was lower (Figure 2) than
Gueiren soil (Figures 1 and 3). These results might possibly be derived from the relationship between the factors of valid adsorption position and oxide content. Another explanation was the relationship between pH and
pE. The pH of Xihu soil was 7.21 and increased when the
soil immersed in water, while the pE drops noticeably.
During this time, As (V) might undergo reduction and
transformed into As (III) in the reaction system. For another, the researchers studied the adsorption of As on the
soil minerals (oxides, hydroxides, or clays) and found
that adsorption decreased with increasing pH [28]. Desorption of As (III) and As (V) occurred after oscillation
for 1 h (Figure 2). In 16-24 h of reaction time, the concentration of As (III) in Xihu soil dropped to near zero
(Figure 2), perhaps the Xihu alluvial soil contained relatively large amounts of carbonate. Sadiq (1997) pointed
out that arsenic in alkaline soil was adsorbed by carbonate, and the sediment of calcium arsenate formed by calcium ions might lead to decrease the As (III) [34]. Previous reports about pH influence on As adsorption suggested that As (III) sorption was maximum at around pH
7 [35,36], whereas As (V) sorption reached to maximum
sorption around pH 4-7 and then decreased with increasing pH [36,37]. However, further studies required to
know the reason for the concentration of As (V) was not
decreased within 16-24 h.
The evaluation on the As (III) and As (V) adsorbabilities of surface soil collected from Pingzhen, Gueiren
and Xihu were calculated with the following dynamics
equation according to different reaction level simulated
at different time blocks.
(1)
where C, t, k, and n were represents the concentration,
reaction time, rate constant and reaction order, respectively. The equations of zero and third degree were as
follows:
C = C0 - kt
(2)
328
Shui-Wen Chang Chien et al.
(3)
where C0 was the initial concentration.
Generally, within two adjacent test times, sample
with rapid change in concentration was treated as 0 order
reactions to calculate its rate constant. In consecutive
times, the trend of concentration change was simulated
from order 0 to 3, and the highest reaction order was selected to simulate the optimal order. The results were
shown in Table 3.
In 0-24 h, Pingzhen soil was of 0 order reaction to
As (III) and As (V). The rate constant of As (V) adsorption was higher than that of As (III) during 0-1 h, but the
constant of As (III) was higher than As (V) (Figure 1 and
Table 3) because of the oxidization of As (V) from As
(III). In Xihu soil system, the rate constant of As (V) in
0-4 h was five times larger than that in 4-24 h; the reason might be As (V) not yet transformed into As (III)
during the response time. In 4-24 h, As (V) gradually
transformed into As (III) caused the reaction rate decrease. As (III), in 16-24 h, increased four times because
As (III) and calcium arsenate produced by calcium ion
was settled (Figure 2 and Table 3). As (III) adsorption
into Gueiren soil showed the 3rd order reaction in 0-16
Table 3. The kinetic analyses of aqueous As (III) and As
(V) absorbed by various soils
Sampling
site
As(III)
Pingzhen
Xihu
Gueiren
As(V)
Pingzhen
Xihu
Gueiren
a,b
Correlation Rate
Reaction Reaction
coefficient constant
period (h) order
(R)
(k)
00-01
01-24
00-16
16-24
00-16
16-24
0
0
0
0
3
0
1.000
0.921
0.880
1.000
0.901
1.000
3.628a
0.073a
0.122a
0.480a
0.002b
0.379a
00-01
01-24
00-04
04-24
00-01
01-24
0
0
0
0
0
3
1.000
0.994
0.933
0.990
1.000
0.895
5.890a
0.002a
0.382a
0.063a
5.443a
0.414b
The units for the rate constants indicated are mg L-1 h-1
and [(mg L-1)2]-1h-1, respectively.
h, and 0 order reaction in 16-24 h. As (V) adsorption
showed level 0 reaction in 0-1 h, and the 3rd order reaction in 1-24 h (Figure 3 and Table 3). The reason for
direct proportional reaction between reaction speed and
concentration in 0-16 h and 1-24 h was yet to be studied.
As seen in Table 3, most soil samples showed 0 order reaction to As (III) or As (V). Thus, the adsorption reaction
rate had no correlation with arsenic concentration. Any
reaction over order 0 should be caused by different compositions of soil.
4. Conclusions
1. The main link for arsenic in soil was based on iron,
aluminum and manganese oxides and hydrated oxides.
Thus, in the batch adsorbability test, soil with high
content of oxides had high arsenic adsorbability. However, results of Pingzhen soil showed that adsorptive
positions, such as phosphate of high adsorbability could
compete for adsorptive position with arsenic and result in reduction in arsenic adsorbability. The arsenic
adsorbability of three soil series showed that As (V)
adsorbability was higher than As (III), and desorption
at the initial stage of soil immersed in water could
cause increase of arsenic concentration in solution.
2. For the adsorptive dynamics of As (III) and As (V) in
0-24 hr in batch adsorbability test, only As (III) adsorbability in 0-16 hr and As (V) adsorbability in 1-24
hr of Gueiren soil were of the 3rd order and the arsenic
adsorbability of reaction system was of the 0 order.
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Manuscript Received: May 27, 2015
Accepted: Sep. 30, 2015