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Journal of Environmental Science


and Health, Part A
Toxic/Hazardous Substances and
Environmental Engineering
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http://www.informaworld.com/smpp/title~content=t713597268

METAL LEACHABILITY FROM SEWAGE


SLUDGE-AMENDED THAI SOILS

Preeda Parkpian a; Katerachada Klankrong b; Ronald DeLaune c; Aroon


Jugsujinda c
a
School of Environmental Resource and Development (SERD), Asian Institute of
Technology (AIT), Klong Luang, Pathumthani, Thailand
b
Water Quality Management Division, Department of Drainage and Sewerage,
Bangkok Metropolitan Administration, Dingdaeng, Bangkok, Thailand
c
Wetland Biogeochemistry Institute, Louisiana State University, Baton Rouge, Louisiana, U.S.A.
Online Publication Date: 14 May 2002
To cite this Article: Parkpian, Preeda, Klankrong, Katerachada, DeLaune, Ronald and Jugsujinda, Aroon (2002) 'METAL
LEACHABILITY FROM SEWAGE SLUDGE-AMENDED THAI SOILS', Journal of Environmental Science and Health, Part
A, 37:5, 765 - 791
To link to this article: DOI: 10.1081/ESE-120003588
URL: http://dx.doi.org/10.1081/ESE-120003588

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J. ENVIRON. SCI. HEALTH, A37(5), 765791 (2002)

METAL LEACHABILITY FROM SEWAGE


SLUDGE-AMENDED THAI SOILS
Preeda Parkpian,1 Katerachada Klankrong,2
Ronald DeLaune,3,* and Aroon Jugsujinda3
1

Urban Environmental Engineering and Management Program,


School of Environmental Resource and Development (SERD),
Asian Institute of Technology (AIT), P.O. Box 4,
Klong Luang, Pathumthani 12120, Thailand
2
Water Quality Management Division, Department of Drainage
and Sewerage, Bangkok Metropolitan Administration,
Dingdaeng, Bangkok 10320, Thailand
3
Wetland Biogeochemistry Institute, Louisiana State University,
Baton Rouge, Louisiana 70803, USA

ABSTRACT
Determining mobility and availability of metals in sewage sludge
amended soil is an environmental concern. Potential leachability and
bioavailability of metals following sludge applied to agricultural soil
was evaluated. Geochemical forms of metal occurring in sludge-amended
soil were subjected to fractionation for understanding heavy metal transformation and remobilization in sludge-amended soil. Metal leachability
was determined using reconstructed soil proles where dewatered sewage
sludge was incorporated into the surface 010 cm of soil. Two-sludge
application rates; 150 and 300 kgN/ha, equivalent to sludge at 4 and 8
ton/ha, were applied to soil columns representing typical agricultural
clay soils of Thailand (Rangsit acid sulfate soil). The soil columns
were leached with 32 l equivalent to 600 mm of surface water using different leachants (distilled water pH 6, distilled water adjusted to pH 3

*Corresponding author. E-mail: rdelaune@aol.com


765
Copyright

2002 by Marcel Dekker, Inc.

www.dekker.com

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PARKPIAN ET AL.

and rainwater pH 5). Among metals measurement, results showed Mn


leachability from sludge-amended Rangsit soil were high at both sludge
application rates (1829% of total Mn applied). The leachability of other
metals was less than 2.5 and 7.2% following application of 150 and
300 kgN/ha of sludge, respectively. Results from the experiments indicated that the leachant at pH 3 had the most eect on potential leachability of Cu, Zn, Cd, and Ni, except Fe and Mn, at low sludge
application rate. Whereas, only the leachability of two metals was inuenced by the lowest pH (pH 3) when sludge applied was increased.
Besides pH of leachant, it appeared that leachability of elements from
the soil column depended on rate of sludge applied, the particular metal,
and metal form or fraction. The soil studied had organic matter, CEC,
pH, clay content, etc., that resulted in high buering capacity, which
favors metal retention. Less than 0.5 and 1.8% of the added Cu and
Zn applied at the 150 and 300 kgN/ha application rates, respectively,
were detected in the leachate. Approximately 100% of the added Cu
and Zn in the sludge remained in the surface 10 cm at each sludge application rate. Sequential extraction of sludge-amended soil following leaching (at the high sludge application rate) revealed that most of the Cu
remained in the surface sludge-amended soil layer (02 cm depth) in the
form of organic and residual Cu fractions that are not easily mobilized.
An exchangeable fraction of Zn increased, approximately representing
60% total Zn applied in sludgesoil layer as compared with its native
soil Zn fractions. These results demonstrate that Zn availability in the soil
would increase as a result of sludge application. However, the total Zn in
the leachate is safe for agricultural use, because it represents an amount
of less than 2% of total Zn applied.
Key Words: Heavy metal; Leaching; Sewage sludge; Linkage form;
Soil column

INTRODUCTION
Like many countries in Southeast Asia, Thailand is regarded as an
agricultural country, and the majority of national income comes from agricultural exports. Most of Thai agricultural soils have been used extensively
for crop production for extended periods of time and are usually low in soil
organic matter (SOM) and essential plant nutrients. Added nutrients (chemical fertilizer) are needed for maintaining and increasing crop production.
As a result, the fertilizer applications have increased substantially.
Chemical fertilizers are most commonly imported, being paid for in foreign
currency equivalent to several thousand millions Baht. To reduce such expenditures for chemical fertilizers, sewage sludge (which is considered an organic
fertilizer) is available from wastewater treatment plants in Bangkok for use as
an alternative source of plant nutrients for crops. Agricultural application of

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METAL LEACHABILITY FROM SEWAGE SLUDGE

767

sewage sludge has great potential as a fertilizer source and as a means


for waste management of sludge material.
Bangkok sewage sludge contains a large quantity of organic matter,
nutrients (N, P, and K), and major and minor nutrients (Cu, Zn, Fe, etc.)
that can be of value for maintaining crop production. Not only can sludge be
used as a fertilizer source to maintain crop productivity, but sludge can also
improve physical properties of soil (1), e.g., by increasing soil porosity and
the stability of soil aggregation (2). Sludge application can increase the complexation and adsorption capacity of soil, enhancing the ability of the soil to
retain metals (3).
Sewage sludge can be benecial, but it can also contain potentially
hazardous heavy metals. Sewage sludge, upon mineralization by microorganisms, could possibly release solubilized heavy metals into the soil solution and
move into groundwater (4). Likewise, the accumulation of sludge-borne
heavy metals in soil following repeated sludge application can cause phytotoxic concentration. Heavy metals may persist in the soil environment and
be taken up by agronomic plants, entering the edible parts of vegetable
tissues, and thus, representing a direct pathway for incorporation of heavy
metals into the human food chain.
Thailand has a wide range of soil types. Acid sulfate soils represent a
signicant portion of the soil types used for agricultural production. Acid
sulfate soil is estimated to cover a total of 40% of Thailands agricultural
land area and is used for many of the major cropping systems (5). Acid
sulfate soils support poor agricultural productivity because of acidity. Low
pH of soil greatly inuences the release of metals (6).
At present, the feasibility of using sludge as a soil amendment or fertilizer in Thailand is a concern for consumers and the environment. The consequences of sludge application to agricultural soil, especially acid sulfate
soil, with regard to the long-term bioavailability and movement of heavy
metals into the environment are incompletely understood. The determination
of potential hazards of heavy metals released from sewage sludge applied to
soil requires a knowledge of metal remobilization and bioavailability characteristics that are dependent on chemical and physical forms of the metals in
sludge and reactions with soil (7,8). To provide answers to these concerns, a
series of laboratory experiments (using packed soil columns and leaching
techniques adapted from various standard column-leaching tests) (9) were
conducted to simulate the long-term eect of leaching behavior of heavy
metals from sludge-amended soil. Many researchers applied leaching test
techniques to estimate the potential and actual leachabilities of heavy
metals (4,1012).
Tropical weather conditions (rainfall and temperature eects) inuence
metal transformation in soil dierently than in temperate zones, in terms of
turnover rate and immobilization in various geochemical soil fractions. To
better understand heavy metal mobility down to subsurface soil layers

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768

PARKPIAN ET AL.

following surface application of sewage sludge, selective and sequential


extraction techniques have been employed (1315). Modications of the
procedure, such as strength and pH of leachants and use of rainwater,
have been utilized in evaluating metal movement. Such modications have
been designed to simulate the actual tropical eld conditions utilizing various
sludge liquid ratios equal to rainfall scenarios and sludge application rates.
The objectives of this study were to (i) evaluate the potential leachability, availability, and accumulation of heavy metals in Thai soil following
sludge application at several rates (150 and 300 kgN/ha); (ii) identify the
development and distribution of dierent geochemical forms of metalsludge-amended soil using the sequential extraction procedure; and (iii) formulate recommendations for sludge application in soil that will avoid excess
metal mobility and phytotoxicity to agricultural systems.
MATERIALS AND METHODS
Material Sampling and Characterization
Plough (topsoil) layer (015 cm) with no previous history of sludge
application was utilized in this study. The soil obtained from Khlong 5,
Rangsit, Pathum Thani is classied as acid sulfate soil (Rangsit soil series).
The eld had been abandoned for 2 years prior to sampling. Average annual
rainfall for the site is 1040 mm (600 mm for the rainy season) (Meteorological
Department, Thailand 19911999). Soil was collected at 015 cm depth surface after plant residue or debris was removed. At the experimental site, soil
was air-dried under shade at ambient temperature (2530 C) and crushed by
mortar and by hand and sieved through 2 mm stainless steel screen. Sieved
soil was kept in plastic bags prior to experiments and analyses. Various
characteristics of soil, both physical and chemical properties, which inuence
leaching, adsorption, and decomposition of metals in soil, were analyzed.
Dewatered sewage sludge was obtained from Sri Phraya Wastewater
Treatment Plant and stored at 5 C. Sewage sludge was also chemically and
physically characterized before sludge application.

Soil Column Leaching Experiments


Leaching experiments were conducted at the Asian Institute of
Technology (AIT). Seven soil columns constructed from PVC pipe (60 cm
length and 25.4 cm diameter) were maintained in ambient laboratory
conditions. In each column, as shown in Figure 1, a porous acrylic plate
was installed inside PVC pipe at the height of 20 cm from the bottom, and
a plastic funnel was attached under that plate. The inside PVC pipe wall was
coated with resin to protect it from corrosion. Above the porous acrylic plate,

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METAL LEACHABILITY FROM SEWAGE SLUDGE

Figure 1.

769

A schematic of a soil column.

the column wall was sanded to increase roughness of the wall for minimizing
any edge eect. To facilitate drainage and soil retainage, 3 cm depth of acidwashed gravel was put over the porous plate. A geotextile was then placed on
the top of the gravel to prevent soil loss during leaching. Washed sand was
placed onto the geotextile to inhibit soil clogging in the geotextile. The soil
was packed into the column and initially rewetted by distilled water to avoid
entrapment of air in the soil pore, until bulk density and water content
reached eld conditions at 1.04 g/cm3 and 47%. Soil thickness after soil
saturation was 10 cm. The quantity of sewage sludge applied to the soil
columns was determined according to AIT recommendation (16) for sludge
application rates for agricultural soils. Dewatered sewage sludge under wet
condition was applied and mixed with topsoil (02 cm depth) at an application rate of 150 and 300 kgN/ha as a dry weight basis. The columns were
rested to stabilize for 1 week, while water content was maintained at 70%
eld capacity during stabilization. The soil columns were leached using leachants shown in Table 1.
Eight liters of a leachant, which was equivalent to 150 mm of simulated
rainfall on a monthly basis, was continuously passed downward through the
soil columns. A second leaching was conducted after gravitational ow
ceased 3 days afterward. A total of four leachings (32 l as being equivalent
to 600 mm, representing average annual rainfall statistics in Pathum Thani
provinces during the rainy season for 4 months) was sprayed onto topsoil in
each soil column. Leachate following each leaching episode was collected in
plastic bottles by gravity ow. Volume, pH, and dissolved organic carbon
(DOC) were immediately measured and recorded. One liter of aliquot was
ltered through Whatman no. 5 lter paper and stored in a refrigerator until

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PARKPIAN ET AL.
Table 1.

Summary of Soil Column Leaching Experiments

Treatment

Leachants

At 150 kgN/ha sludge applied


1. Rangsit soil (Control)
2. Rangsit soil sewage sludge
3. Rangsit soil sewage sludge
4. Rangsit soil sewage sludge
At 300 kgN/ha sludge applied
5. Rangsit soil sewage sludge
6. Rangsit soil sewage sludge
7. Rangsit soil sewage sludge

Distilled water (pH 6)


Distilled water (pH 6)
Distilled water adjusted
to pH 3 with H2SO4
Rainwater* (pH 5)
Distilled water (pH 6)
Distilled water adjusted
to pH 3 with H2SO4
Rainwater* (pH 5)

*Rainwater was collected after 15 min rainfall during the rainy


season.

analyzed. The columns, following a 1-week rest after the last leaching, were
dismantled. The soil core was subsequently removed from the column cut
into ve portions: 02, 24, 46, 68, and 810 cm.
Sample Analysis
All samples were characterized for selected parameters utilizing a specic standard method (Table 2) prior to the leaching experiments. In addition, geochemical forms or metal speciation was conducted from the sludgeamended soil samples after leaching soil columns were completed.

RESULTS AND DISCUSSION


Characteristics of Soil
Physical and chemical properties of Rangsit soil were analyzed to evaluate metal availability, leachability, and distribution in the soil column of the
prole. The soil properties are presented in Table 3. Soil pH was relatively
low with a value of 4.58. Any soil with pH below 6.5 could increase metal
solubility, resulting in phytotoxicity to plants. Rangsit soil contained 53%
clay, which is classied as a clay soil (17). Total nitrogen content of the soil
was 0.05%, which is considered low for plant growth. Nitrogen application
is necessary for supplying sucient nutrients for plant growth in this soil.
Phosphorous content of Rangsit soil was low, because soil from the eld site
had not been amended with P fertilizer for the last 3 years. Exchangeable
cations in Rangsit soil were adequate and were derived mainly from a

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METAL LEACHABILITY FROM SEWAGE SLUDGE


Table 2.
Material
Sludge and soil

Sample Analysis Method

Parameter
Particle size
distribution
pH
Total nitrogen
Total phosphorous
Available phosphorous
Organic carbon
Cation exchange capacity
Exchangeable cations
Water soluble trace metal
Total trace metal
concentrations
Metal speciation

Leachate

771

pH
Dissolved organic carbon
Soluble trace metals

Method
Hydrometer method described by Sheldrick
and Wang (47)
Electrometric method described by
Hendershot, Lalande, and Duquette (47)
Semi-micro kjeldahl method described by
McGill and Figueiredo (47)
HC1O4 acid digestion method described by
OHalloran (47)
Bray II method described by Olsen and
Sommer (48)
Walkley-Black method described by
Rhoades (48)
Ammonia saturation method described by
Rhoades (48)
Ammonium Acetate Method described by
Hendershot, Lalande, and Duquette (48)
Extract by 0.01 M CaCl2
AAs after using CEM MDS-2000 microwave
for digestion
Sequential extraction procedure described by
Tessier et al. (13)
pH meter
Shimadzu 5000A TOC analyzer
Shimadzu AA-6701F atomic absorption
spectrometer

previous application of lime and fertilizer. Soils with high clay content, such
as Rangsit soil, have a high cation exchange capacity (35 meq/100 g). The
water-soluble fraction of heavy metals was low in this soil. Total heavy metal
content of the soil was also relatively low due to no previous history of
receiving metals in the form of sludge application.
Characteristics of Sewage Sludge
Sewage sludge from Bangkok Wastewater Treatment Plant was also
analyzed for selected parameters, which are shown in Table 4. Sludge pH
(6.94) was near neutral using a 1 : 5 sludge-to-water ratio. Total nitrogen
in sewage sludge was approximately 3.60%, with available nitrogen being
approximately 755 mg/kg. Such a nitrogen level is sucient for maintaining plant growth. The sewage sludge used in the study is an excellent
source of many plant nutrients. High amounts of calcium in sludge
resulted from liming in a dewatering process. The Ca could increase the
adsorption of metals by exchanging with cations and coprecipitation as

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PARKPIAN ET AL.
Table 3.

Characteristics of Originating Rangsit Soil

Parameter

Analyzed Value
3

Bulk density (g/cm )*


Soil texture (%)
Sand
Silt
Clay

1.04

Soil pH (1 : 5 sludge : water)


Total N (%)
Total P (mg/kg)
Available P (mg/kg)
Cation exchange capacity (meq/100 g)
Exchangeable cations (mg/kg)
K
Ca
Mg

4.58
0.05
360
7.75
35
109
1419
266

Water-soluble trace metal (mg/kg)


Cd
Cu
Ni
Zn
Fe
Mn

0.23
0.51
2.99
1.03
2.52
0.29

Total trace metal content (mg/kg)


Cd
Cu
Ni
Zn
Fe
Mn

0.72
21
13
23
24 831
15

16
31
53

*From Sirisukhodom (1).

carbonates and oxides/hydroxides-bound metal. The amount of basic


exchangeable cations present in sludge would help serve as a soil conditioner, by neutralizing soil pH and increasing the buering capacity of soil
(18). Copper had the highest solubility among the metals measured in
sewage sludge. Because organic matter in dewatered sewage sludge is
actively degraded, humic substances are present. Those dissolved acidic
humic products could complex with Cu and other metals, resulting in
high solubility of metals. A comparison of the concentrations of heavy
metal in sludge and USEPA standards with High Quality Metal
Concentrations Limits for Land Application (19) showed that all of the
metals were below allowable concentrations, except for Cu concentration
(Table 4). Results suggest Cu should be carefully monitored if this sludge
material is applied to agricultural soils.

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METAL LEACHABILITY FROM SEWAGE SLUDGE


Table 4.

773

Characteristics of Sewage Sludge

Parameter
Sludge pH (1 : 5 sludge : water)
Moisture content (%)
Total N (%)
Available N (mg/kg)*
Total P (mg/kg)
Available P (mg/kg)
Organic matter (%)
Alkalinity (g/cm3)*
Exchangeable cations (mg/kg)
K
Ca
Mg

Analyzed Value
6.94
85
3.60
755
13 536
476
46
750
1307
5387
355

Water-soluble trace metal (mg/kg)


Cd
Cu
Ni
Zn
Fe
Mn

0.19
20.58
14.16
3.94
2.29
12.45

Total trace metal content (mg/kg)


Cd
Cu
Ni
Zn
Fe
Mn

1.89
1437
107
1607
23 852
1841

Total metal in sludge standards


for land application (mg/kg)**
Cd
Cu
Ni
Zn
Fe
Mn

39
1500
420
2800

*Potential leachability of toxic heavy metals in Bangkok sewage sludge (45).


**High-quality metal concentrations limits for land application (19).

Potential Leachability in Sludge-Amended Soil Column


In this study, the leachability of selected metals (Fe, Cd, Cu, Mn, Zn,
and Ni) was also investigated in soil column experiments following two rates
(150 and 300 kgN/ha) of sludge application to determine the amount of metal
released within these treatments. Leachability of metals from soil column
experiments was based on dry material weight of metal applied, as shown
in Table 5.

Zn Cd Ni

Fe

Cu

Zn

Cd

Ni

Fe

Mn

1166 20 455

3425 18 219 000

5333 26 184 250

2400 31 200 250

Mn  Cd>Cu>Ni>Zn>Fe

Mn  Cd>Ni>Zn>Cu>Fe

Mn  Cd>Cu>NiZn>Fe

Mn  Cd>Cu>Zn>Fe>Ni

*Input of metals metals from sludge metals from soil metals from distilled water or rainwater.

9833 13 147 68 182 31 600 32 197 610 Mn  Cd  Ni>Zn>Cu>Fe

4.47 31.42

2.37

9389 16 142 72 093 28 701 65 221 258 Mn  Cd  Ni>Zn>Cu>Fe

3667

4601 25 581

Mn

23 291 892

Fe

8.80 34.36 10 778 18 223 60 465 30 779 63 216 101 Mn  Cd  Ni>Zn>Cu>Fe

2.58 26.28

4133

2393 23 256

Ni

2.37

0.25

150 163 4.4 73 139 600 120 0.55 0.19 0.09

3.63 22.11

3800

Cd

1002 11 905

Zn

The Sequence of
Leachability

9.10 35.18

0.40

150 163 4.3 75 139 600 120 0.62 0.75 0.11

4.36 24.03

2835

Cu

Leachability of Individual Metal


(mg/kg of Individual Metal Applied)

2.21

0.18

81 0.34 0.13 0.05 Trace 3.16 23.76

Mn

150 163 4.3 75 139 600 120 0.57 0.39 0.10

120 130 4.2 72 139 000

Cu

At 300 kgN/ha
180 197 4.3 77 140 060 159 1.69 3.18 0.31
5. Rangsit
soil sludge
leached by
DW (pH  6)
6. Rangsit
180 197 4.3 77 140 060 159 1.94 3.59 0.26
soil sludge
leached by
DW pH 3
7. Rangsit
180 197 4.4 75 140 060 159 1.77 2.59 0.30
soil sludge
leached by rainwater
(pH  5)

At 150 kgN/ha
1. Rangsit soil
(no sludge)
leached by
DW (pH  6)
2. Rangsit
soil sludge
leached by
DW (pH  6)
3. Rangsit
soil sludge
leached by
DW pH 3
4. Rangsit
soil sludge
leached by
rainwater (pH  5)

Treatment

The Total Amount of


Metals in Leachate (mg)

Metal Leachability at 150 and 300 kgN/ha of Sludge Applied (Based on Dry Metal Weight)

Input of Metals (mg)*

Table 5.

5275

8572

5303

3851

4012

3598

3438

DOC in
Leachate
(mg/kg)

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PARKPIAN ET AL.

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METAL LEACHABILITY FROM SEWAGE SLUDGE

775

Leachability of Selected Metals at 150 kgN/ha Sludge Applied


Manganese and Iron
The sequence of metal leachability in the 150 kgN/ha sludge application rates in Rangsit soil indicated that Mn had the highest potential
leachability in each treatment studied. Generally, Mn is present in soil
as oxides and hydroxides in coating layers of soil particles, and its compounds and fractions can be dissolved easily by combined factors such as
soil pH, complexation by organic ligands, and microbial eects (20).
However, microbiological activity in soil is also known to be responsible
for the oxidation and reduction of Mn compounds (21). Therefore,
released Mn ions from microbial activity are further complexed by sulfate
and become more soluble. In general, oxidation of sulfur by oxygen is
very low, but may be catalyzed by autotrophic bacteria, which seem to be
ubiquitous in acid sulfate soil (22); therefore, sulfate could be produced in
high amounts in the Rangsit soil.
Soil pH levels below 6 favor reduction of Mn to the more mobile
and plant available forms, resulting in increased levels of dissolved and
exchangeable Mn (23). From Table 5, Mn leachability in soil columns
leached by DW pH 3 would be expected to be high as compared to other
leachate, but the result did not follow such hypothesis. This could be attributed to MnFe antagonism, which has been previously reported in acidic soil
that contains large amounts of solubilized Mn (24). Higher levels of plant
Mn were found at high Mn/Fe ratios in acid sulfate soil in Thailand (25). It is
suggested that high levels of Fe in the soil solution might exert a negative
eect on the uptake of Mn. In a study under acid sulfate soil, little watersoluble Fe was detected at 250 mV and pH 4.5, around 39 mg/kg (25),
whereas 1831 mg/kg of the added Fe was found in the leachate in this
study. It is possible that the conversion of soluble Fe into insoluble ferric
forms under oxidizing conditions occurred in the wetdry cycle of soil during
the experiment. The content of Fe in the leachate was, therefore, low in
comparison with the other trace metals as well as with total Fe content (6).
The pH variation of leachant in this study apparently had a minimal eect on
Mn and Fe leachability.

Cadmium and Zinc


Generally, Cd mobility at soil pH below 5 is high (26). Results
obtained in this study indicated that Cd was the most mobile element in
the soil columns leached with DW pH 3, followed by soil columns leached
with DW and rainwater, respectively. Under acidic conditions in the
Rangsit soil, portions of sulde and oxide of trace metals might have

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776

PARKPIAN ET AL.

been transformed to water-soluble forms, which combined with Cd,


resulting in dissolved Cd (27). In general, Cd exhibits higher mobility
than Zn under acidic soil systems. When compared to total Zn applied,
the leachability of Zn was restricted and accounted for less than 1%
(0.10.45%). Soil column leached by DW pH 3 also had the highest leachability of Zn.
Copper
Copper is a metal that has a high anity for binding with electrondonating groups, such as carboxylate and amide groups, in dissolved
organic carbon (DOC) (3,28). DOC is an important component of solutions in terrestrial and aquatic ecosystems through its inuence on acidity,
nutrient availability, toxicity, and transport of metals and contaminants.
Generally, DOC is a major product of the decomposition process, molecular structures ranging from simple to complex fulvic acids (FA) (29).
Fulvic acids, due to high contents of oxygen-containing functional groups,
are the most active components of organic matter in complexing
metals (30). Fulvic acids contained in sludge-amended soil in the column
should, thus, serve as a good available carrier of metal mobility in soil
solution.
The stability of the metal fulvic acid complexes decreased in the
order Cu>Fe>Ni>Pb>Co>Ca>Zn>Mn>Mg was reported (31).
Therefore, Cu could form stable complexes with fulvic acids. Because
sewage sludge from Sri Phraya WWTP had not stabilized, microorganisms
were still actively degrading and producing DOC that was detected in
leachate from the soil column (Table 5). It should be noticed here that
organic matter in sewage sludge could be decomposed within 24 h (32).
This is attributed to the high water content and initially relative oxidized
nature of the sludge, resulting in a faster rate of microbial degradation
(33). Based upon this phenomenon, a large portion of the DOC would be
removed with Cu complexes and transported further down the soil column
or prole. Ion-selective electrode measurement was the method that conrmed that a large fraction of soluble Cu was organically complexed,
existing in mobile forms (34). The high concentration of DOC observed
in the leachate seemed to indicate that bacterial activity still functioned
actively in this experiment. Results from this experiment indicated that Cu
combined with DOC in columns leached by DW pH 3 had the highest
leachability. This was supported with high total DOC concentration
(4012 mg/kg), which was detected in the leachate (Table 5). Leachability
of DOC from sludge-amended soil was a function of pH (9). At low pH,
DOC was released in soil solution, because it was replaced by H ions for
adsorption sites.

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777

Nickel
In addition to Cu, Ni is another transition metal that tends to form
covalent bonds with organic ligands (35), but the bond is not as strong as Cu.
In general, Ni is controlled with pH-dependent solubility and complexation
with soluble carbon (28). However, under acid sulfate soil such as Rangsit
soil, the form of Ni is mainly in Ni-sulfate in soil solution. As pH of leachant
was increased, Ni leachability was decreased. This was because H ions
in low pH leachant are strongly attracted to the soil surface (negative
charges), and they have the power to replace Ni. The sequence of metal
leachability in soil column leached with DW pH 3 showed that Ni mobility
was dierent from the other sludge-amended soil leachates. This was because
Ni solubility was aected by the low pH (pH 3). Low pH metal binding
competed with H ions, resulting in fewer sites available for binding (30).
Therefore, under acid soil Ni, with water solubility (2.99 mg/kg) higher
than Cu (0.51 mg/kg), had more leachability than Cu in the soil column
leached by DW pH 3.

Leachability of Selected Metals at 300 kgN/ha Sludge Applied


Most metals, except Mn, showed increasing leachability in accordance
with a high sludge application rate (300 kgN/ha) (Table 5). This indicated
that the sludge application rate aected metal leachability. The sequences of
metal leachability in soil columns at a high sludge application rate were in the
same sequence or order, except Cu and Ni were altered. Cu leachability was
far below Ni leachability. This was possibly because Ni possessed intermediate chemical behavior, being inuenced both by pH dependency and by
the ability to form organic complexes with DOC (28). Another factor that
resulted in less Cu leaching out from soil than Ni was that Cu fractions
developed and were present in the soil after the sludge was applied. Table
8 indicated that more than 50% of the least soluble fraction (residual fraction) predominated after a high sludge application rate, which was not easily
soluble. Zn was greater than Cu at the higher rate of application. This
diered from that of Zn at a low sludge application rate, where Cu was
more easily solubilized than Zn. Results from sequential extraction procedure
(Table 8) showed that Zns forms were transformed to an exchangeable
fraction (approximately 60% of total Zn applied in topsoil), which was
expected to become available after the sludge-applied rate was increased.
Therefore, under acid soil, Zn (1.03 mg/kg), which has a higher solubility
than Cu (0.51 mg/kg), would be found in more soluble forms in Rangsit soil.
Soil pH in the leachate at both sludge application rates increased from 5
to 5.5 after the rst leaching and remained constant at pH around 7 after the
third leaching (Figure 2). This was possibly due to the presence of exchange-

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778

PARKPIAN ET AL.

Figure 2. pH in the leachate of sludge-amended soil after receiving dierent amounts of


leachant: (a) pH in the leachate at sludge rate 150 kgN/ha; (b) pH in the leachate at sludge
rate 300 kgN/ha.

able cations, especially calcium associated with previous lime application,


and the Ca leached increased the pH of the leachate. Because of the near
neutral pH in the leachate, precipitation of metals in the leachate would have
occurred. Therefore, metals became less solubilized instead of remaining
dissolved in the leachate. However, leachate pH at a high sludge application
rate (300 kgN/ha) was lower than that at a low sludge application rate, likely
as a result of the production of organic acids from degradable organic materials in sludge (soluble forms) that could lower pH of the leachate.
Recovery Leachability of Selected Metals from Sewage Sludge
Under the same conditions, the amount of metals leached from sludgeamended soil column by DW was subtracted from the amount of leachable
metals in the control column in order to quantify metals leached as a result of

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METAL LEACHABILITY FROM SEWAGE SLUDGE


Table 6.

779

Metal Leachability of Sewage Sludge


Leachability of Individual Metal (mg/kg)

Treatment

Cu

Zn

Cd

Ni

Fe

Mn

At 150 kgN/ha
1. No sludge leached by DW
2. Sludge leached by DW
3. Leachability of
sewage sludge (3) (2)  (1)

2835
3800
955

1002
2393
1391

11 905
23 256
11 351

Trace
2400
2400

23
31
8

291 892
200 250

At 300 kgN/ha
4. Sludge leached by DW
5. Leachability of
sewage sludge (5) (4)  (1)

9389
6554

16 142
15 140

72 093
60 188

28 701
28 701

65
42

221 258

sewage sludge addition or metal recovery determination. The results shown in


Table 6 indicated that Cd was most readily leached from sewage sludge followed by Ni, Zn, Cu, Fe, and Mn. Apparently, Mn, which became more
soluble in sludge-amended soil, was not from the sewage sludge but from
Mn content in the native soil material. Cd and Ni were the rst two metals
that were released from sludge into solution. However, their concentrations in
the sludge were below EPA standard levels, reported to not be harmful to the
environment. Cu and Zn leachability from sludge were not as high as Cd and
Ni. Nevertheless, Cu and Zn have been selected to identify geochemical forms
in this study. This was likely because Cu concentration in sewage sludge
(1437 mg/kg) was near EPA regulatory standards (1500 mg/kg) allowing for
sludge application to agricultural lands (19). The Zn forms in the sewage
sludge were mainly transformed into an exchangeable form, which was readily
available, following sludge application (Table 8). As a result, these two metals
should be closely monitored if sludge is applied to Thai soil.
Potential Environmental Pollution from Sludge-Amended Soil
The concentrations of metals released into the leachate from soil column
leached with rainwater (natural condition) at low and high sludge application
rates were compared to the groundwater quality standard of Thailand
reported in Table 7. Metal concentrations in the leachate, except Cd concentration (at high application rate) and Mn concentration (at both application
rates), were below the maximum permissible levels for groundwater. These
allowable concentrations for the metals were saved, despite some Cd and
Mn that moved below 10-cm depth in the soil surface prole. However, Cd
and Mn concentrations as a result of the metal re-adsorption process would
not expect to move down the soil prole and reach the water table depths
(2030 m depth).

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780
Table 7.

PARKPIAN ET AL.
Metal Concentrations in the Leachate from Soil Column Leached by Rainwater

Control1

1501

3002

Maximum Level
Groundwater
Quality Standard3

0.012
0.005
0.002
Trace
0.114
0.861

0.017
0.006
0.008
0.008
0.081
0.821

0.056
0.083
0.029
0.076
0.143
1.004

1.5
15.0
0.01

1.0
0.5

Metal Concentrations (mg/L)


Element
Cu
Zn
Cd
Ni
Fe
Mn
1

Soil with no sludge applied.


Sludge applied at 150 kgN/ha.
3
Sludge applied at 300 kgN/ha.
4
Groundwater for consumption by pollution control department, Thailand (46).
2

Under acid sulfate soil (clay soil) in these leachate studies, Mn showed
the highest concentration in the leachate. Whereas in other studies, Zn concentration from sewage sludge applied to sandy loam soil and silty clay loam
soil was the highest concentration in the leachate (36,37). The dierence of
those metal concentrations or movement in the soil prole was associated
with dierence in soil type and background metal contents in sludge.
Copper and Zinc Mobility in Sludge-Amended Soil
The concentrations of Cu and Zn remain in a sludge-amended soil
prole after leaching soil columns were analyzed to quantify depth metals
penetrated following sludge application. Mobility of Cu and Zn within
soil depth is present in Figures 3 and 4. At the 150 kgN/ha application rate
to the Rangsit soil, there was no evidence of Cu movement from sludgesoil
layer (02 cm depth) with depth into the soil column. As mentioned previously, microbial oxidation of organic components in sewage sludge is an
important aspect governing the movement of sludge in soil. When organic
material is degraded, both fulvic (soluble) and humic (insoluble) acids
are produced. Insoluble organic material eectively inhibits uptake of
metal cations such as Cu, which binds strongly with organic material, preventing plant uptake. Conversely, soluble organics increased the carrying
capacity of soil solution for Cu (38). Therefore, DOC containing fulvic
acids resulting from the origin sludge application could signicantly inuence
the mobility of Cu. However, Cu movement was restricted to surface 4 cm
below sludgesoil layer. Beyond 4-cm depth, Cu concentration was still in
line with native Rangsit soil Cu (21 mg/kg) concentration. When sludge
application was doubled (300 kgN/ha), two soil columns leached with DW

Soil Depth (cm)

0-2
4-6

20.81

8-10

19.64

20

40

Soil Depth (cm)

0-2

80

68.59

43.94
18.52
17.75

4-6

19.72
18.16

8-10
0

20

40
Cu Conc (mg/kg)

Sludge Applied at 150 kgN/ha

Soil Depth (cm)

60

Cu Conc (mg/kg)

(b)

60

80

Sludge Applied at 300 kgN/ha

58.28

0-2

45.98
23.8
20.78

4-6

20.12
18.71

8-10
0

10

20

(c)

30

40

50

60

70

Cu Conc (mg/kg)
Sludge Applied at 150 kgN/ha

Sludge Applied at 300 kgN/ha

71.69

0-2

39.14

4-6

21.44
19.76

8-10

21.42
20.94

0
(d)

781

22.87

(a)

Soil Depth (cm)

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METAL LEACHABILITY FROM SEWAGE SLUDGE

20

40

60

80

Cu Conc (mg/kg)
Sludge Applied at 150 kgN/ha

Sludge Applied at 300 kgN/ha

Figure 3. Cu mobility in Rangsit soil as inuenced by dierent leachants: (a) No sludge


amended soil leached by DW pH 6; (b) Sludge amended soil leached by DW pH 6; (c)
Sludge amended soil leached by DW pH 3; (d) Sludge amended soil leached by rainwater
pH 5. Background total Cu in soil 21 mg/kg.

Soil Depth (cm)

PARKPIAN ET AL.

0-2

22.78

4-6

21.57

8-10

21.86

20

40

Soil Depth (cm)

46.22
35.92

4-6

24.89
27.05

8-10

15.55

20

40
Zn Conc (mg/kg)

Sludge Applied at 150 kgN/ha

Soil Depth (cm)

80

67.78

0-2

(b)

60

80

Sludge Applied at 300 kgN/ha

68.94

0-2

49.04
25.54
21.53

4-6

29

8-10

16.84

(c)

20

40
Zn Conc (mg/kg)

Sludge Applied at 150 kgN/ha

60

80

Sludge Applied at 300 kgN/ha


68.42

0-2

52.71
32.45

4-6

24.52
29.84

8-10

15.31

0
(d)

60

Zn Conc (mg/kg)

(a)

Soil Depth (cm)

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782

20

40
Zn Conc (mg/kg)

Sludge Applied at 150 kgN/ha

60

80

Sludge Applied at 300 kgN/ha

Figure 4. Zn mobility in Rangsit soil as inuenced by dierent leachants: (a) No sludge


amended soil leached by DW pH 6; (b) Sludge amended soil leached by DW pH 6; (c)
Sludge amended soil leached by DW pH 3; d) Sludge amended soil leached by rainwater
pH 5. Background total Zn in soil 23 mg/kg.

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METAL LEACHABILITY FROM SEWAGE SLUDGE

783

and rainwater showed that Cu still accumulated only in such layer (04 cm),
the same as the 150 kgN/ha application rate. However, soil columns leached
with DW pH 3, which had the highest amount of DOC (4012 mg/kg) Cu
reached down to the 6-cm depth of a 10 cm depth packed soil column.
Mobility of Zn in Rangsit (Figure 4) after receiving sludge at a low rate
(150 kgN/ha) seemed to be restricted to the surface 08 cm layer. Beyond
8-cm depth in the soil column, Zn concentration of sludge-treated soil was
similar to values found for background Zn concentration (23 mg/kg) in soil.
When sludge application rate was increased (300 kgN/ha), Zn concentration
below 8-cm depth in all soil columns increased above background levels.
Increase in the sludge application rate inuenced Zn mobility more than
Cu mobility under acid sulfate soil. This was due mainly to the linkage form
of Zn that is favorable to remobilization, whereas Cu was mainly accumulated in the topsoil as predominated by less mobilizable forms. However, Cu
and Zn concentrations were recovered close to 100% within 10-cm soil depth
because re-adsorption and precipitation of metals occurred during their
movement from the sludgesoil layer.
Other reported research observed similar results, which showed that the
majority of sludge applied accumulated in the soil surface. As a result, the
movement of metals from the application site was typically minimal.
Following are a few examples of such observations; no sludge-borne metals
were detected below the 15-cm depth in the soil columns, even on the
Plaineld sand with a pH of 4.9 (39). Over 90% of the deposited heavy
metals (Cd, Cr, Ni, Pb, and Zn) were found in the 015 cm soil depth,
where sludge was incorporated, and no statistically signicant increase in
heavy metal content of the soil was detected below the surface 30 cm of the
soil prole after 6 years of continued annual sludge application in coarse and
loamy soil (40). Similar to the work in California that found that the metals
include Cd, Cu, Zn, and Hg, which had concentrations in sludge that were
markedly greater than those in the untreated soil that had moved in small
amounts into the 2530 cm depth over the 9-year period (41). Metals transported from soil surface in grassland soil treated with sewage sludge also did
not go below 10 cm. Most of the 7 metals (Cd, Cr, Cu, Mo, Ni, Pb, and Zn)
(60100%, mean 87%) remained in the upper 5 cm of soil (42). These earlier
studies showed soil below the topsoil layer (015 cm depth) had no signicant
enrichment in heavy metals following sludge application. Less than 1% of the
metal applied had moved below the topsoil layer.
Soil pH at 02 cm depth in sludge-amended Rangsit soil increased over
background topsoil pH (Figure 5). Generally, sewage sludge is treated with
lime to control odor at wastewater treatment plants during sludge processing.
Corresponding organic biodegradation under the acidic condition takes
place, and no acidic products are produced to further decrease soil pH.
The increased soil pH resulted from calcium content of sludge, as such,
would alleviate metal leaching in the soil prole, helping to neutralize soil

Soil Depth (cm)

PARKPIAN ET AL.

0-2

4.48

4-6

4.51

8-10

4.59

4.4

4.5

4.6

4.7

Soil Depth (cm)

(a)

4.9

4.97

0-2

4.61
4.78

4-6

4.57

8-10

4.57

4.64

4.4

4.5

4.6

Sludge Applied at 150 kN/ha

Soil Depth (cm)

4.8

Soil pH

(b)

4.7
Soil pH

4.8

4.9

Sludge Applied at 300 kgN/ha

4.48
4.48

0-2

4.52
4.5

4-6

4.52
4.54

8-10
4.4

4.5

4.6

(c)

4.7

4.8

4.9

Soil pH
Sludge Applied at 150 kgN/ha

Soil Depth (cm)

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784

Sludge Applied at 300 kgN/ha

4.74
4.72

0-2

4.69
4.68

4-6

4.67

8-10

4.56

4.4

4.5

4.6

(d)

4.7

4.8

4.9

Soil pH
Sludge Applied at 150 kgN/ha

Sludge Applied at 300 kgN/ha

Figure 5. Soil pH distribution as inuenced by dierent leachants: (a) No sludge amended


soil leached by DW pH 6; (b) Sludge amended soil leached by DW pH 6; (c) Sludge
amended soil leached by DW pH 3; and (d) Sludge amended soil leached by rainwater
pH 5.

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METAL LEACHABILITY FROM SEWAGE SLUDGE

785

pH. Except for pH of soil column leached with DW pH 3, pH did not


increase over background soil pH (4.58). Soil pH at a high sludge application
rate was slightly greater than that at the low rate, because the greater decomposition rates produced higher NH
4 levels and organic acids.

Copper and Zinc Speciation in Sludge-Amended Soil


The speciation or metal form in soil following the application of sewage
sludge to agricultural land is likely to be more important than the total
concentration of metals, because metal forms determine the availability of
metals for plant uptake and the potential for further contamination of
groundwater. The observed inuence of total metal concentrations and
sludge characteristics on metal speciation emphasized the necessity for consideration of all ve fractions, including exchangeable, carbonates, Fe and
Mn oxides, organic bound, and residues. This investigation using sequential
extraction procedure developed (13) to identify and quantify the dierent
chemical forms in which Cu and Zn were present in sewage sludge and
Table 8. Sequential Extraction of Sludge-Amended Soil on the Distribution of Cu and Zn
at Sludge High Application Rate (300 kgN/ha)
Material

Treatment

Soil Depth
(cm)

(a) Copper
Sewage

sludge
Rangsit soil No sludge leached
by DW (pH 6) (control)
With sludge leached
by DW (pH 6)
With sludge leached
by DW3
With sludge leached
by rainwater (pH 5)

Carb

Ox

Org

Res

Copper (% of Total Cu Applied)

11.98

10.40

12.18

59.35

6.09

02
810
02
810
02
810
02
810

10.77
16.74
10.14
16.13
14.28
14.60
12.18
11.20

13.48
11.09
7.73
10.08
7.60
11.24
7.47
8.14

9.49
10.37
9.97
9.84
11.83
13.53
15.16
12.60

12.49
9.04
14.67
11.3
15.72
15.46
12.78
13.37

53.77
52.75
57.49
52.64
50.57
45.17
52.40
54.69

11.71

24.95

52.98

6.12

4.25

02
810
02
810
02
810
02
810

7.94
13.17
62.36
20.16
59.63
19.89
54.99
13.99

4.14
6.05
7.76
3.91
4.69
2.54
4.61
4.61

8.10
11.08
11.60
12.01
15.45
10.68
20.83
13.99

7.00
10.40
6.16
6.23
4.88
9.75
4.71
4.28

72.82
59.30
12.12
57.68
15.35
57.14
14.86
63.12

(b) Zinc

Sewage
sludge
Rangsit soil No sludge leached
by DW (pH 6) (control)
With sludge leached
by DW (pH 6)
With sludge leached
by DW3
With sludge leached
by rainwater (pH 5)

Exch

Zinc (% of Total Zn Applied)

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786

PARKPIAN ET AL.

sludge-amended soil. From Table 8, the major forms of Cu extracted in


sewage sludge were in the order: organic bound  oxides>exchangeable>
carbonates>residue. The order of Zn speciation was oxides>carbonates>
exchangeable>organic bound>residue. An organic complex of Cu was predominated in sewage sludge, because most sludge was abundant with organic
material (bacteria cells) and the binding capacity of organic matter was
greatest for Cu (3), whereas the most adsorption of Zn in sewage sludge
was oxide fraction.
Following sludge application at 300 kgN/ha and being leached with
various leachants, control soil columns (no sludge) and soil columns leached with DW, DW pH 3, and rainwater were fractionated to determine Cu
and Zn speciation. Comparing Rangsit soil column leached with DW with
control columns showed that organic bound and residual fractions of Cu in
sludgesoil layer (02 cm depth) increased slightly from 12.49 and 53.77%
to 14.67% and 57.49%, respectively. Only the carbonate fraction decreased.
The other fractions remained the same as the fractions in the control. At
the lowest section of the soil column (810 cm), no signicant change
occurred in all Cu fractions, suggesting that most Cu in sewage sludge
accumulated and remained at the origin of level of application to the surface soil.
More than 70% of Zn was found in the residual forms as surface soil
layer (02 cm depth) of Rangsit soil, however, the exchangeable fraction of
Zn (62.36%) signicantly increased in soil treated with sludge that was
leached with DW. The explanation for such increase of exchangeable fraction
was that under acid sulfate soil, H ions replaced organic and inorganic
ligands easily from Zn, and thus, Zn formed soluble zinc sulfate. When the
Zn concentration in soil solution increased, Zn was attracted by the negative
charge of exchangeable sites (43). Such an eect suggested that the application of sewage sludge at 300 kgN/ha to Rangsit soil provided more labile Zn
that might potentially become bioavailable than in nonamended soil (44).
At 810 cm depth of soil column, an exchangeable fraction of Zn (20.16%)
previously leached by DW was also increased higher than its control soil of
the same depth (13.17%), as a result, Zn became more easily mobilized than
Cu.
In the surface soil layer (02 cm) of soil column leached with DW pH 3,
Cu occurred in organic fraction slightly higher than in a column leached with
DW and rainwater. This is because organic matter decomposed was
restricted due to extremely low pH of soil. At 810 cm depth section, Cu in
residual fraction (45.17%) of column leached with DW pH 3 became dissolved and re-adsorbed by other fractions including carbonates (11.24%),
oxides (13.53%), and organics (15.46%). Comparing soil columns leached
with DW, DW pH 3, and rainwater, Zn in exchangeable fraction of those
columns increased more than 55% (5562%) in the surface soil (02 cm
depth) after sludge was applied. However, regardless of pH of the leachants,

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METAL LEACHABILITY FROM SEWAGE SLUDGE

787

Zn was predominated in the exchangeable soil fraction. Based on this nding,


leaching of sludge-amended soil induced Zn remobilization as indicated by
the higher level of its exchangeable fraction.
Recommendations for Sludge Reuse in Agriculture
Sewage sludge application to Thai soils should be further treated following the dewatering process to remove organic matter. Humic substances
such as humic and fulvic acids could be produced if sludge has not stabilized. Those acid products could complex with metals, especially Cu,
increasing solubility. Although almost 100% of metals were restricted to
the surface 10-cm soil depth in this study, plants could possibly assimilate
those soluble metals and translocate them to plant parts and into the food
chain. Metals in the sludge could be transformed into exchangeable forms,
which were easily bioavailable. This study found that most metals applied
from sewage sludge under acid sulfate soil remained in the topsoil (010 cm
depth), with the major concentration at the 02 cm surface layer. This was
attributed to the fact that the soil had higher CEC due as a result of lime
application. This phenomenon helps alleviate metal mobility. Further study
showed that when the sludge application rate was increased, potential
leachability also increased. This could be of concern in no lime-amended
soil with low soil pH. Therefore, caution should be taken in not applying
more than the recommended rate of 150 kgN/ha recommended by AIT (16).
Metal leachability should not have any signicant impact on groundwater
contamination, but because of potential increases in bioavailability fractions in the surface, caution should be taken regarding plant uptake and
toxicity. Therefore, phytotoxicity might be expected in plant species sensitive to Zn toxicity.

CONCLUSIONS
The leachability of metal from the soil prole depended on pH of leachant, rate of sludge applied, chemical nature of metal and metal species, and
fraction. Properties such as organic matter, CEC, soil pH, and minerals in
soil increased the buering capacity of soils, favoring higher metal retention
in the surface layer. Results of this study showed that for Cu and Zn, less
than 0.5% of the two metals applied at 150 kgN/ha and less than 1.8% of
each metal applied at 300 kgN/ha were detected in the leachate. Whereas,
close to 100% of the added metals from sludge were recovered within 10 cm
of the soil column from both sludge application rates. Sequential extraction
of sludge-amended soil after leaching at a high application rate revealed that
Cu was associated with organic and residual fractions, which are not easily

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788

PARKPIAN ET AL.

remobilized. Exchangeable fraction of Zn increased predominately (around


60% of total Zn applied) in the Rangsit soil, as compared to original fractions found in soil receiving no sludge. This could lead to the conclusion that
availability of Zn could be expected from sludge application. However, the
total Zn in the leachate detected was far less than that in the regulatory
guideline and, thus, is safe for agricultural use. Because soil used in this
study was clay texture with high CEC and organic matter content, the
amount of metal binding sites in the soil was, therefore, far higher than
soils from other areas. In terms of potential leachability, results obtained
from this study also conrmed that this soil had a high capacity for retaining
metals following sludge application.

ACKNOWLEDGMENTS
The author would like to thank Mr. Somchai Sornwanee, Ms. Jarirat
Srinatpat, and Ms. Noppawan Jantavee for their excellent technical support
and assistance on sample analyses throughout the experiment at the Department of Drainage and Sewerage, Bangkok Metropolitan Administration
(BMA). The Royal Thai Government provided the nancial support for
this research.

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