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Procedia - Social and Behavioral Sciences 40 (2012) 673 – 680

Trace Elements in Thai Oxisols on Limestone in Relation to

Rainfall
Worachart Wisawapipata,b , Irb Kheoruenromneb,*, Anchalee Suddhiprakarnb,
Robert J. Gilkesc
a
Faculty of Environment and Resource Studies, Mahidol University, Nakhon Pathom 73170, Thailand
b
Department of Soil Science, Faculty of Agriculture, Kasetsart University, Bangkok 10900, Thailand
c
School of Earth and Environment, Faculty of Natural and Agricultural Sciences, University of Western Australia, Crawley, WA
6009, Australia

Abstract

Trace element concentrations of 7 profiles of Oxisols derived from calcareous sedimentary rocks under tropical
monsoonal and the tropical savanna environments have been investigated using XRD, SXRD, XRF, and ICP–OES
analytical techniques so as to provide baseline values for estimating environmental contamination of soils with heavy
metals. Kaolinite was the dominant mineral of the clay fraction with moderate amounts of goethite and hematite.
Gibbsite was only present in Ak1 profile under more humid conditions contributing to high anion exchange capacity
(AEC). Trace element concentrations in these soils conform to those for worldwide normal soils. However, the
extraordinary high arsenic (As) concentration in Ak1 soil represents a hazardous concentration (313 mg kg-1), which
may have been inherited from the parent rock. Arsenic in this soil is probably not toxic because it is immobile in an
oxidized environment, and is sorbed onto soil constituents particularly sesquioxides. Factor analysis showed that for
soils under various rainfalls were deficient. For the whole soil samples, three main groups of similar geochemical
behavior existed. Different concentrations of elements of the Ca group (Ca, Ni, Cr, Mg, Ba, Be, Gd, Rb, K, Co, Mn,
Zn, La, Cu, V, Ce, P, Cd, Sc, Pb, clay, SSA and CEC) and the Si group (Si and sand), resulted in soils developed
under the tropical monsoonal and the tropical savanna climates being clearly different. The Fe group (Fe, Ti, Al, Mo,
Ge, Se, Sr, Ga, Th, Hf, U, As and Sb) separated the soils developed of under a tropical monsoonal into two groups
based on the very high concentrations of Fe, Al and As in Ak1 profile.

© 2012
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*Corresponding author. Tel.: +66 2 9428104; fax: +66 2 9428106

E–mail: irbs@ku.ac.th( I. Kheoruenromne)
Keywords: Geochemistry, Tropical soils, Factor analysis, Arsenic contamination

1. Introduction

Iron oxides are common constituents of soil and may typically contain metals (including metalloids)
other than iron in their structure. Goethite and hematite are the two most stable forms of iron oxides, and
are considered as secure and long term sequestrating agents for trace metals that are potentially toxic [1].
Sorption, precipitation and substitution of metals are key mechanisms for sequestrating these elements.
Several anions such as molybdate, arsenate, asenite, selenite and phosphate can be strongly sorbed as

1877-0428 © 2012 Published by Elsevier Ltd. Selection and/or peer-review under responsibility of the Asia Pacific Business Innovation and Technology
Management Society Open access under CC BY-NC-ND license.
doi:10.1016/j.sbspro.2012.03.248
674 Worachart Wisawapipat et al. / Procedia - Social and Behavioral Sciences 40 (2012) 673 – 680

inner-sphere complexes on surfaces of minerals especially sesquioxides through a ligand exchange

mechanism [2].
Climatic conditions influence the properties of secondary oxides in soils. In drier and warmer
climates, hematite is more abundant than goethite, whereas goethite is more abundant in wetter and cooler
climates. Specific surface area of soil iron oxides is in the order ferrihydrite > goethite > hematite [3].
Low crystallinity of minerals causes them to have a small crystal size and a large specific surface area
that provides much ion adsorption relative to their contribution to the total amount of minerals in soils.
Oxisols are widespread in the tropics (i.e. 25% of the tropical land area) and comprise an important
economic resource for agriculture and mining industry in several countries including in Thailand. They
are generally acidic and infertile. Kaolinite, goethite, and hematite are the dominant clay constituents [4],
which variously contribute to the variable charge of soil and are major sinks for many trace elements.
Although substantial information on trace elements in tropical soils is available, there is a little of
knowledge on trace metal distributions in Thai Oxisols formed on limestone, which is the subject of this
investigation.

2. Materials and methods

2.1. Materials

Fifty four soil samples from 7 Oxisols under tropical savanna and monsoonal environments on
limestone in the Peninsular and Northeast Plateau Thailand were collected for this study. The climate of
the Peninsular Thailand is a tropical monsoonal climate with an annual rainfall of 1800–2200 mm, where
the Northeast Plateau is tropical savanna with an annual rainfall of 1035 mm. The soils are from the
Pathio (Ptu) and Ao Luk (Ak1, Ak2, Ak3) series under a tropical monsoonal climate, and Pak Chong
series (Pc1, Pc2, Pc3) under a tropical savanna climate.

2.2. Laboratory analysis

2.2.1. Physicochemical analyses

Soil samples were air–dried and gently crushed to pass through a 2 mm sieve before analysis.
Physicochemical analyses were determined by standard procedures [5]. Particle size distribution was
determined by pipette. Specific surface area (SSA) of soils was measured by the N2–BET method with a
Micromeritics Gemini III 2375 surface analyzer. Crystalline, non-crystalline, and organic forms of Fe, Al,
and Mn were extracted by the so–called specific extractants dithionite–citrate–bicarbonate (DCB)
solution (Fed, Ald, Mnd), 0.2M ammonium oxalate solution at pH 3.0 (Feo, Alo, Mno), and sodium
pyrophosphate solution (Fep, Alp, Mnp), respectively. Dissolved Fe, Al, and Mn were measured by
atomic absorption spectrophotometry.

2.2.2. Mineralogical analysis

The mineralogical composition of whole soil samples was determined by synchrotron X–ray
diffraction (SXRD). Powder samples of the soil samples were placed in glass capillaries, and SXRD
patterns were obtained over an angular range of 4–60° 2ș at a wavelength of ~1.0 Å to obtain sufficient
resolution. X–ray diffraction (XRD) analyses of the clay and silt fractions were obtained using CuKĮ
radiation with a Philips PW–3020 diffractometer equipped with a graphite diffracted beam
monochromator. Oriented clay was prepared on ceramic plates and XRD patterns were obtained from 4–
35° 2ș with a step size of 0.02° 2ș and a scan speed of 0.04° second–1 after various pretreatments for
aiding the identification of clay minerals [6].
 Worachart Wisawapipat et al. / Procedia - Social and Behavioral Sciences 40 (2012) 673 – 680 675

2.2.3. Major and trace element analysis

The chemical composition of soils was measured by a combination of X–ray fluorescence

spectrometry (XRF) and aqua regia digestion (HCl and HNO3) followed by inductively coupled plasma–
optical emission spectrometry (ICP–OES). Aluminum, Si, Ti, Fe, Mn, Ca, K, Mg, P and Zr were
determined on fused La–bearing lithium borate glass disks using a Philips PW1480 XRF spectrometer
and the elemental concentrations were checked against analyses of a certified international reference
material (OREAS43P). Sodium, As, Ba, Be, Cd, Ce, Co, Cr, Cu, Ga, Gd, Ge, Hf, La, Mo, Nd, Ni, Pb, Rb,
S, Sb, Sc, Se, Sr, Th, U, V, Y and Zn were determined using a PerkinElmer Optima 5300 DV ICP–OES
on aqua regia digests of finely ground soil and the elemental concentrations were checked against
analyses of reference material STSD–1. This digestion procedure does not completely dissolve some
highly resistant sand size minerals; however, the results for most elements closely approximate the total
element concentration and this method is widely used in environmental geochemical research [7].

3. Results and discussions

3.1. Soil properties

All soils were Oxisols derived from calcareous rock. They are very deep, well drained having red
color. These soils were clayey throughout the profile except for the surface horizon of Ptu, which had a
sandy clay loam texture. They were strongly acidic with low organic matter, low total N, low available P
and very low available K. However, most surface soils were relatively fertile due to the influences of
liming and fertilization. Cation exchange capacity (CEC) ranged from low to high and is consistent with
the clay content and specific surface area (SSA).

Table 1 Range, mean and standard deviation values for physicochemical properties of Thai Oxisols on limestone under different
climatic conditions

Oxisols on limestone under Oxisols on limestone under

Properties
a tropical monsoonal climate (n = 29) a tropical savanna climate (n = 25)
Range Median ± SD Range Median ± SD
pH (H2O) 5.1 –6.5 5.5 ±0.27 4.4–7.6 5.0±1.0
pH (KCl) 3.5 –5.6 4.0 ±0.64 3.7–7.1 3.9±1.2
pH (NaF) 8.5 –9.4 8.9 ±0.26 8.9–9.3 9.0±0.13
-1
OM (g kg ) 1.3 –25 4.3 ±5.6 2.1–41 5.5±12
-1
Total N (g kg ) 0.070 –1.1 0.30 ±0.22 nd–2.1 0.50±0.52
Avail. P (mg kg-1) 0.1 –131 0.45 ±24 0.45–22 1.6±5.3
Avail. K (mg kg-1) 2.8 –33 10 ±7.7 7.1–678 26±132
CEC (cmol kg-1) 3.2 –13 7.8 ±2.2 10–20 12±2.9
Sand (%) 4.2 –55 12 ±13 0.30–11 3.0±2.4
Silt (%) 1.7 –28 7.8 ±5 0.20–49 4.5±10
Clay (%) 26 –92 82 ±15 40–97 93±12
SSA (m2 g-1) 15 –47 39 ±6.7 33–68 52±9.2
Fed (g kg–1) 39 –138 79 ±31 61–107 84±12
Ald (g kg–1) 4.4 –27 7.2 ±8.9 2.8–8.9 4.9±1.9
Mnd (g kg–1) 0.35 –1.7 0.8 ±0.35 0.4–2.7 0.63±0.60
Feo (g kg–1) 1.3 –4.3 2.0 ±0.62 1.4–3.2 2.1±0.51
–1
Alo (g kg ) 1.8 –18 9.2 ±3.7 3.0–17.2 3.9±3.9
–1
Mno (g kg ) 0.0076 –1.3 0.23 ±0.32 0.024–2.0 0.13±0.56
Fep (g kg–1) 0.049 –3.2 0.13 ±0.58 0.036–0.46 0.13±0.092
Alp (g kg–1) 0.68 –5.9 2.1 ±1.1 0.55–4.6 3.0±0.89
Mnp (g kg–1) 0.0 –0.5 0.038 ±0.11 0.0078–0.59 0.036±0.14
nd = non detectable.
676 Worachart Wisawapipat et al. / Procedia - Social and Behavioral Sciences 40 (2012) 673 – 680

Kaolinite was the dominant mineral of the clay fraction with moderate amounts of goethite and
hematite. Various amounts of accessory minerals including quartz, hydroxyl–Al interlayer vermiculite
(HIV), gibbsite, boehmite and anatase were present in the soils. Goethite dominated over hematite in the
soils under more humid conditions except for Ak2 and Ak3 profiles, where hematite was more abundant.
Gibbsite and boehmite were only present in a soil derived from limestone (Ak1) formed under a high
rainfall condition (Fig. 1).

Q
Gi
K = Kaolinite
Q B = Boehmite
Gi = Gibbsite
Q = Quartz
Go = Goethite
H = Hematite
A = Anatase

Gi

Gi
K
K
Go
A
K B
B H
Ak
Pc

3 3.5 4 4.5 5 5.5 6 6.5 7 7.5 8 d spacing (ǖ) 

Fig. 1. Synchrotron XRD patterns of random powder of whole soil samples

All soils showed variable charge behavior but the amounts of charge and the rate of change in surface
charge with pH varied between the soils [8]. The values of positive charge (Anion exchange capacity,
AEC) of soils formed under more humid conditions (Ptu, Ak) were greater than for the soils occurring
under drier conditions (Pc). This difference was partly attributed to the Ak and Ptu profiles containing
more sesquioxides, mostly goethite, with hematite dominating in Pc profiles. The Ak1 profile had high
positive charge, which is partly due to gibbsite and boehmite in its clay fraction contributing to anion
adsorption. The surface soil of Pc1 profile showed a strong variable negative charge behavior due to the
abundant organic matter in this soil.

3.2. Soil geochemistry

The complete chemical analyses of the soils are not given here due to the large data set; however the
range, median and standard deviation of elemental concentrations are provided in Table 2. Silicon, Al, Fe
and Ti were the major elements in these soils. Calcium, Mg, Mn, K and Na were present at minor
concentrations. Trace element concentrations varied greatly between the soils, which is probably due to
differences in parent rocks and environmental conditions.
Concentrations of most trace elements in Thai Oxisols were comparable to those for worldwide
normal soils (i.e. within the range of published values) [9]. However, the concentrations of As, Cd, Cr,
Cu and Ni were above values for normal worldwide soils (Table 2), and As and Cr were present at
hazardous concentrations. These elements are relatively immobile in an oxidized soil environment as they
can be sorbed and/or incorporated into soil constituents such as clay minerals and sesquioxides. The
mechanism of arsenate sorption resembles phosphate sorption. The more goethitic and gibbsitic soils had
higher values of P sorption capacity than did hematitic soils [10].
 Worachart Wisawapipat et al. / Procedia - Social and Behavioral Sciences 40 (2012) 673 – 680 677

Table 2 Range, median and standard deviation for concentrations of 39 elements in soil samples for Thai Oxisols (n = 54), and
mean values for normal surface soils worldwide
Oxisols on limestone under the Oxisols on limestone under the Range for normal Critical soil
Element
tropical monsoonal climate (n=29) tropical savanna climate (n=25) surface soils worldwide A concentration B
Range Median ± SD Range Median± SD
Major element (g kg−1)
Si 116– 391 260± 83 219– 244 226± 6.7 250–410
Al 53– 265 165± 63 155– 194 185± 11 10–300
Fe 37– 158 78± 40 98– 108 102± 3.0 2–550
Ti 4.2– 14 8.7± 3.2 7.9– 14 10± 1.7 2.3–26
Zr 0.38– 0.80 0.45± 0.092 0.25– 0.47 0.33± 0.058 140–305
Ca 0.083– 1.4 0.31± 0.27 0.12– 4.1 0.71± 1.3 0.7–500
Mg 0.28– 0.81 0.39± 0.14 0.33– 1.1 0.71± 0.22 0.4–9.0
Mn 0.32– 1.5 0.72± 0.30 0.38– 2.4 0.54± 0.51 0.20–0.53 1.5–3
K 0.10– 0.30 0.18± 0.054 0.16– 1.4 0.44± 0.28 0.08–37
Na nd– 0.17 0.0091± 0.042 nd– 0.032 0.0080± 0.0070 0.15–25
Trace element (mg kg−1)
As 30– 313 105± 103 45– 68 53± 6.6 4.4–9.3 20–50
Ba 4.4– 27 7.4± 5.7 11– 49 18± 11 84–960
Be 0.18– 0.61 0.32± 0.12 0.95– 1.7 1.3± 0.22 0.35–3.5
Bi nd– 2.7 0.81± 0.82 nd– 2.2 0.63± 0.7 0.2
Cd 0.047– 0.72 0.25± 0.21 0.2– 1.7 0.30± 0.37 0.37–0.78 3–8
Ce 33– 75 55± 13 52– 106 69± 12 21–146
Co 4.0– 18 9.1± 3.3 8.8– 37 13± 7.4 0.1–70 25–50
Cr 51– 246 123± 52 334– 586 465± 59 15–221 75–100
Cu 8.0– 28 16± 6.5 28– 43 36± 4.9 6–35 60–125
Ga 13– 65 30± 13 23– 40 31± 4.3 11–29
Gd 1.6– 6.9 4.6± 1.5 8.6– 12 11± 0.91 6
Ge 0.24– 2.0 0.81± 0.41 0.50– 1.6 0.83± 0.25 0.8–1.6
Hf nd– 2.3 0.49± 0.70 0.10– 0.60 0.39± 0.14 5–21
La 12– 52 27± 10 56– 85 62± 5.8 1.4–55
Mo 0.72– 21 2.0± 8.6 4.4– 12 10± 2.7 0.013–17
Nd 4.8– 31 18± 6.9 29– 40 35± 2.7 1–57
Ni 17– 43 23± 7.0 60– 107 82± 13 4–92 100
P 85– 529 114± 107 145– 483 217± 81 35–5300
Pb 15– 49 21± 12 25– 48 34± 6.8 10–67 100–400
Rb 1.8– 16 3.3± 4.7 5.2– 41 17± 11 33–270
S 47– 647 184± 218 nd– 327 68± 90 30–1600
Sb 3.7– 28 13± 8.0 1.4– 4.0 2.9± 0.68 0.19–1.8
Sc 6.4– 18 11± 3.5 14– 18 16± 1.0 5–10
Se 1.5– 21 5.6± 4.6 3.7– 11 7.1± 2.0 0.13–1.3
Sr 1.3– 31 3.5± 11 4.1– 15 6.1± 2.9 87–210
Th 17– 65 35± 15 33– 41 37± 2.1 3.4–13.4
U nd– 27 3.8± 8.6 nd– 2.6 nd± 0.92 0.79–11
V 94– 329 189± 72 304– 458 380± 47 18–115 50–100
Y 0.8– 22 7.1± 6.2 57– 95 72± 8.7 16–33
Zn 10– 44 20± 12 45– 152 72± 34 17–236 70–400
nd = non detectable.
A
Mean of total concentrations of elements in the surface horizon of normal worldwide soils, normal means that the data excluded
contaminated or mineralized soils. Data are from [9].
B
Higher concentrations may be toxic to plants depending on speciation [15]

Some researchers consider that retention of arsenate (As5+) by soils is closely related to the contents of
oxalate-extractable Al and DCB-extractable Fe. This reflects that microcrystalline Al oxides and
crystalline Fe oxides retain arsenic.
The depth distribution for concentration of some heavy metals (As, Cd, Cr, Cu, Ni, Zn) in these soils
is quite uniform, and is probably inherited from the parent rock (Fig. 2). However, surface horizons of
the Pc1 profile that have elevated values of Cd, which may be resulted from anthropic activity possibly
from P fertilizer application. The concentration of As is high throughout the Ak1 profiles indicating that
As was inherited from the parent materials rather than being of anthropic origin.
678 Worachart Wisawapipat et al. / Procedia - Social and Behavioral Sciences 40 (2012) 673 – 680

As (ppm) Cd (ppm) Cr (ppm)

0 100 200 300 400 0.00 0.50 1.00 1.50 2.00 0 200 400 600
0 0 0

30 30 30

60 60 60
Depth (cm)

Ptu
90 90 Ak1 90

Ak2
120 120 120
Ak3
150 150 Pc1 150
Pc2
180 180 PC3 180

210 210 210

Cu (ppm) Ni (ppm) Zn (ppm)

0 10 20 30 40 50 0 30 60 90 120 0 50 100 150 200
0 0 0

30 30 30

60 60 60
Depth (cm)

90 90 90

120 120 120

150 150 150

180 180 180

210 210 210

Fig. 2. Trend with depth for concentration of some heavy metals (As, Cd, Cr, Cu. Ni, Zn) in Thai Oxisols

3.3. Multivariate analysis on element distributions in soils

Two factors represented 66 percent of variation in the data for these soils (Fig. 3). Elements can be
divided into three main groups of similar geochemical behavior. The first group included clay, SSA,
CEC, Ca, Ni, Cr, Mg, Ba, Be, Gd, Rb, K, Co, Mn, Zn, La, Cu, V, Ce, P, Cd, Sc and Pb. These elements
can be incorporated into octahedral cation sites in the structures of kaolinite, gibbsite, hematite, and
goethite, and consequently are related to clay, SSA and CEC [11]. Several monovalent (Rb, K) and
divalent (e.g. Ca, Ba, Mg, Zn Mn) cations in this group persist in the soils developed under dry conditions
and were not fully removed during weathering. Cerium, La, Th, Nd and P occur in monazite which was a
highly resistant mineral but under extreme weathering, monazite is dissolved and thorianite (ThO2) may
precipitate [12]. Therefore, Th did not occur in this affinity group but is in the second group of elements
that are more abundant in soils that have experienced more extreme weathering.
The second group included Fe, Ti, Al, Mo, Ge, Se, Sr, Ga, Th, Hf, U, As and Sb. Titanium and Al are
commonly classed as residual elements in soils as they are highly resistant to removal by weathering.
Arsenic belongs to the group as it strongly adsorbed on Al and Fe oxides [13]. High concentrations of
arsenic (30-313 mg kg-1 As) in these Oxisols (Ak, Pc, Ptu), were inherited from their parent rocks. The
dominant form of As in oxidic soils is As(V), which is less toxic, less soluble and less mobile than As(III)
[14]. The third group of elements is the Si group which is particularly abundant in the Ptu profile, which
has more sand content than do the other soils.
 Worachart Wisawapipat et al. / Procedia - Social and Behavioral Sciences 40 (2012) 673 – 680 679

10
1.0 (a) Oxisols derived from limestone (b)
8
Si under tropical monsoonal environment
6 Oxisols derived from limestone
Group1 under tropical savanna environment
Group3 4
0.5 Mg
Ni CEC
Be YRbBa 2
Sand
Gd NdK Ca
Factor 2 : 30.03%

Factor 2: 30.03%
Cr 0
Co
La Na
Zn
SSA Mn -2
0.0 Cu
Silt
Bi -4
V Zr
Clay
CePCd -6

-8
-0.5 Sc Group2 Ptu
Pb
Ge Gibbsite rich Ak1
-10
Ti Se Ak2
Sb -12 Ak3
Al
FeMo Sr Ga Pc1
S U As
Th -14 Pc2
-1.0 Hf
Pc3
-16
-1.0 -0.5 0.0 0.5 1.0 -15 -10 -5 0 5 10 15
Factor 1 : 36.07% Factor 1: 36.07%

Fig. 3. Factor analysis for standardized element concentrations in whole soil samples of Oxisols derived from limestone (a elements,
b soils)

4. Conclusions
As soil is an important constituent in ecosystems so its quality must be addressed and integrated into
the environmental monitoring agenda. The concentrations of metals were low in these soils, except for
As, which represented a significant concentration in some soils. Therefore, management of these As-rich
soils should consider redox conditions as these strongly govern concentrations of toxic forms of As.
These As-rich soils should be reserved and restricted for forestry, perennial plants or energy crop, their
use for crops especially rice should be prohibited. Lower parts of these areas may have a high risk of As
ground water contamination which may affect human health.
Acknowledgments
The authors are grateful to the Royal Golden Jubilee Ph.D. Program under the Thailand Research
Fund for financial support. We thank the laboratory staff at the School of Earth and Environment, UWA
for their support particularly Mr. Michael Smirk for assistance with chemical analyses. We acknowledge
the Australian Synchrotron for providing beam time.

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