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Editor: M.J. Balart Murria, pp.
2011 Nova Science Publishers, Inc.
Chapter 3
ABSTRACT
Chemical stabilization is an in situ remediation method that uses
inexpensive amendments to reduce contaminants availability in polluted
soil. Amendments may adsorb, bind or co-precipitate the contaminating
elements. Cadmium (Cd) is known as more mobile and soluble than
many other potentially trace element in soils. Furthermore, it has been
identified as a major toxic element reaching the food chain, directly
through crop uptake or indirectly through animal transfer. Recently there
has been increasing interest in the immobilization of Cd using a range of
inorganic compounds, such as lime and phosphate compounds, or organic
compounds, such as biosolids compost. In this chapter, the feasibility of
E-mail: torri@agro.uba.ar
1. INTRODUCTION
Soil contamination with potentially toxic elements (PTE) is a worldwide
problem. Excessive accumulation of PTE in agricultural soils may not only
result in environmental contamination, but also lead to elevated PTE uptake by
crops, which may affect food quality and safety (McLaughlin and Singh 1999;
Zhu et al, 2008). Among PTE, cadmium (Cd) and lead (Pb) have been
recognized as priority pollutants by the United States Environmental
Protection Agency (USEPA) and other organizations. Cadmium may easily
reach the food chain through common agricultural practices such as
fertilization, irrigation or pesticide application (Mees et al., 2002). Other
anthropogenic activities primarily associated with industrial processes,
atmospheric fallouts, manufacturing and the disposal of domestic and
industrial waste materials may also result in a significant input of soil Cd.
The Pampas Region, Argentina, is one of the largest temperate field
cropland areas of the Southern Hemisphere. At present, the concentrations and
dispersion values of PTE in agricultural or grazed soils in this region are
similar to other non-contaminated soils of the world (Lavado et al., 2004).
However, these soils recently started to receive an increased amount of
phosphate fertilizers. Depending on its provenance, Cd in the phosphate rock
can be present in relatively large amounts, from 0 to 150 mg Cd kg1 (Lpez
Camelo et al, 1997). Hence, there is an increasing local concern for protecting
the environmental quality of croplands of the Pampas Region.
In contrast to agricultural soils, some urban areas of Argentina and its
surroundings are starting to show signs of anthropogenic accumulation of Cd
and other PTE (Wannaz et al, 2006; Lavado, 2006). Anthropogenic sources of
cadmium for urban and peri-urban areas include traffic emission (vehicle
exhaust particles, tire wear particles, brake lining wear particles), industrial
emission (power plants, coal combustion, metallurgical industry, chemical
plants, etc.), domestic emission, weathering of building and pavement surface,
atmospheric deposition and so on (Sindern et al, 2007; Christoforidis, Stamatis
2009; Lu et al, 2009; Morton-Bermea et al, 2009; Wei, Yang 2010). Some
alluvial soils of the Riachuelo River in Buenos Aires province were also
reported to accumulate between 1-5 mg Cd kg-1 due to anthropogenic activity
(Ratto et al, 2004). High concentration of Cd in sediments may lead to Cd
release to water and pose risk to aqueous organisms and human health. Lavado
et al. (1998) reported that concentrations of Cd and other PTE in some urban
and peri-urban soils of Buenos Aires province, were much higher than
thresholds proposed by several international standards and by the Argentine
Hazardous Wastes Law (law 24051). Like most other metals, Cd does not
undergo microbial or chemical degradation and therefore persists in soils for a
long time after its introduction. Cadmium has been identified as a major toxic
trace element reaching the food chain, directly through crop uptake or
indirectly through animal transfer (Adriano 2001). Furthermore, Cd is the only
metal that might pose human or animal health risks at plant tissue
concentrations that are not generally phytotoxic (Peijnenburg et al. 2000).
Once ingested or absorbed by humans, it has a long biological half-life and
causes numerous health concerns (Goyer, 1997).
Due to the growing size of the population of Buenos Aires City,
horticulture in urban areas and its surroundings is a means of employment of
migrants from agricultural areas or inmigrants from neighboring countries
(Schnitzler et al., 1999). According to the United Nations (2001), nearly all of
the expected growth in population in the next two decades (20102030) will
take place in urban areas, with almost no growth in the rural population. As a
result, peri urban environments are conducive to intensive production of
perishable foods (fruits, vegetables, meat and dairy products) to be consumed
by urban inhabitants. Many studies have shown that Cd is readily taken up by
roots crops and translocated to aerial organs where it accumulates to high
levels (Jiang et al, 2010; Perilli et al, 2010). In particular, vegetables are
capable of accumulating relatively high levels of Cd in the edible portion at
concentrations that may exceed food safety limits (McLaughlin et al., 2006,
Peralta-Videa et al., 2009; Yang et al, 2009).
that can interact with a biological target. The chemodynamics of Cd in the soil
environment is controlled by its interactions with both solid and aqueous
phases. Processes such as adsorption/desorption, ion exchange,
precipitation/dissolution, soil and solution phase composition regulate the
toxicity and mobility of Cd through soil profiles (Alloway, 1990; Helmke and
Naidu, 1996). Single extraction and/or sequential extraction procedures are
used to estimate the distribution of PTE associated with particular phases in
soils and sediments. A large number of sequential extraction schemes have
been proposed for soils, generally attempting to identify PTE held in any of
the following fractions: soluble, exchangeable, sulfide/carbonate-bound,
organically bound, oxides-bound, and residual or lattice mineral bound
(Tessier et al, 1979; Sposito et al, 1982; Shuman 1985; Rauret et al, 1999).
Assessment of metal mobility and bioavailability in soils and sediments using
sequential extraction proceduress assumes that mobility and bioavailability
decrease in the order of extraction. Thus, metals in the exchangeable fractions
are most mobile and bioavailable, whereas metals in residual fraction are
tightly bound and least mobile under natural environmental conditions.
Technologies to minimize the chances of Cd reaching the food chain aim to
reduce the concentration of bioavailable forms by increasing adsorption,
precipitation or entrapment of Cd in crystal lattices (Hamon et al, 2002).
3. REMEDIATION TECHNIQUES
Different remediation techniques have been developed in order to reduce
PTE and, in particular, Cd bioavailability in soils (Chen, Lee 1997; Gray et al.,
2006). Several physicalchemical treatments based on excavation, landfilling,
thermal treatment, acid leaching and electro-reclamation have been proposed.
Unfortunately, these methods are not suitable for practical application, because
of their high cost and low efficiency, limiting its use on vast contaminated
areas (Khan et al, 2005). Moreover, they are often environmentally invasive
and do not permit a natural reshaping of the environment (Lombi et al., 2002).
In contrast, bioremediation is cost-effective and environmentally friendly. Two
bioremediation technologies, phytoremediation and stabilization, have been
widely investigated for the remediation of Cd polluted sites (Dushenkov et al,
1997; Carrillo-Gonzlez et al, 2006).
Phytoremediation of Cd-contaminated soils is a fast-expanding
technology, which uses specific plants species which have an innate ability to
tolerate and accumulate Cd (Blaylock and Huang, 2000; Ghosh, Singh 2005;
(Equation 2)
(Equation 3)
(Helyar et al. 1976). Different phosphate sources may impact the effectiveness
of Cd stabilization. Thawornchaisit and Polprasert (2009) evaluated the
efficiency of three commercial phosphate fertilizers: triple superphosphate,
diammonium phosphate, and phosphate rock as stabilizing agents in Cd-highly
contaminated soils. Addition of all tested phosphate fertilizers induced a shift
of Cd mobile forms towards more stable fractions; however, the shifting
degree occurred at different rates depending on the phosphate fertilizer used,
and followed the sequence: triple superphosphate > diammonium phosphate >
phosphate rock. Consequently, stabilization efficiency appeared to be
correlated with dissolution of phosphate sources.
Other studies have shown that many PTE-phosphates are
thermodynamically stable and relatively insoluble in natural environments
(Santillan-Medrano, Jurinak, 1975; Nriagu, 1984; Vieillard and Tardy, 1984;
Ruby et al., 1994). The possibility of forming cadmium phosphate [Cd3(PO4)2]
upon the addition of soluble phosphate compounds in Cd contaminated soils
has been proposed, without direct evidence (Ma et al., 1993; Cotter-Howells,
Caporn, 1996). In effect, Bolan et al. (2003 a) found no evidence of Cd3(PO4)2
formation in soil samples even at the highest level of KH2PO4 and Cd addition.
Moreover, the solubility of Cd3(PO4)2 has been shown to be too high to control
the concentration of Cd in soil suspensions involving iron and aluminium
hydrous oxides (Kuo, 1986; Soon, 1981). Thus, although the precipitation as
Pb or Zn phosphates has been proved to be one of the main mechanisms for
the immobilization of Pb and Zn in contaminated soils (Hettiarachchi et al.
2000; McGowen et al., 2001) no conclusive evidence was provided up to this
time on the existence of new solid phases of Cd-phosphate compounds upon
addition of phosphates on Cd-contaminated soils.
10
11
carbon are responsible for maintaining low plant availability in biosolidsamended soils. Currently, there is intense debate whether the organic or the
inorganic fraction is responsible for Cd and other PTE immobilization (Li et
al., 2001; Stacey et al., 2001, Bolan et al., 2003 c, Hettiarachchi et al., 2003,
Merrington et al., 2003; Kumpiene et al., 2008).
Liming of contaminated soils is the most widely used remediation
treatment to reduce the bioavailability of Cd (Bolan et al. 2003 b; Tlusto et
al., 2006; Hong et al, 2009). Alkaline amendments increase soil pH (McBride
et al., 1997 and Filius et al., 1998) and facilitate the formation of oxides,
metal-carbonate precipitates and complexes that decrease metal solubility
(Mench et al., 1994). Biosolids compost can therefore be combined with
alkaline materials to complement Cd sequestering ability on compost
components (Mench et al., 1994 and Chlopecka and Adriano, 1996). Recent
studies have shown that alkaline-stabilized biosolid compost that are low in
total and/or bioavailable metal content can be used as an effective sink for
reducing the bioavailability of Cd in contaminated soils (Brown et al., 2000; Li
et al., 2000; Basta et al., 2001; Clemente et al., 2005). Numerous
investigations have been carried out for biosolids compost as potential
contamination sources of heavy metals. Conversely, limited work has been
done regarding the capacity of biosolids compost obtained at different stages
of the composting process, lime and a mixture of mature compost and lime to
immobilize Cd on an artificially Cd contaminated soil of the Pampas Region,
Argentina. These aspects are further discussed.
12
Table 1. Selected properties of the soil and the organic amendments used
in the study
pH
EC
(dS
m-1)
0.7
%C
Conta5.72
2.02
minated soil
Compost 1
7.5
2.10 13.42
Compost 2
7.6
2.08 11.08
Compost 3
7.6
2.62 4.05
1
EC: Electrical Conductivity.
2
CEC: Cation Exchange Capacity.
Soluble
C
%C
0.24
0.06
0.031
CEC2
Texture (%)
Clay
(%)
30.3
Silt
(%)
53.6
Sand
(%)
16.1
(cmol
kg-1)
24.5
Total
Cd
(mg kg
MS-1)
10.94
24
18.13
14.3
<4
<4
<4
Biosolids
Biosolids from Buenos Aires City was provided by the local water
operator Agua y Saneamientos Argentinos S.A. (AySA). The aerobically
stabilized biosolids used in these experiments was previously dried in holding
pools in the biosolids treatment plant. Biosolids was thoroughly mixed with
pine sawdust (1:1, V:V) and composted in piles. Composite samples were
taken at three different stages of the composting process: i) a day after
composting started (compost 1); ii) at the end of the thermophilic stage, 10
days after the process started (compost 2); iii) mature compost, after 90 days
composting started (compost 3).
Incubation Experiments
Artificially soil contaminated samples were amended at proportions
equivalent to a field application rate of i) 50 Mg ha-1 of compost 1 (C1); ii) 50
Mg ha-1 of compost 2 (C2); iii) 50 Mg ha-1 of compost 3 (C3); iv) 50 Mg ha-1
of compost 3 + 20 Mg ha-1 lime (LC3); v) 20 Mg ha-1 lime (L). A control
(artificially contaminated soil CS) with no amendment was also included.
Deionized water was regularly added to keep amended and control soils to
moisture contents of 60% to ensure minimum denitrification (Rowell, 1994).
Soils were incubated in glass flasks (360 ml) in darkness in a temperaturecontrolled incubator at 24 C to achieve stable soil conditions. Sampling was
managed by removing three pots per treatment at 0, 14, 28 and 42 days.
The sequential extraction procedure of McGrath and Cegarra (1992) was
used to investigate the mechanism of action of the amendments. Briefly, soil
was sequentially extracted with 0.1 M CaCl2 for 16 h (exchangeable fraction,
13
C1
C2
C3
C3+L
3
L
14
28
1
0
0
42
days
14
pH
5,72
5,66
5,83
6,00
7,75
7,93
0,05
0,07
0,05
0,04
0,03
0,01
day 28
a
a
a
a
b
b
5,54
5,55
5,66
5,62
7,72
7,98
0,01
0,10
0,06
0,13
0,13
0,09
day 42
a
a
a
a
b
b
5,54
5,47
5,48
5,54
7,74
7,95
0,13
0,14
0,10
0,01
0,12
0,31
a
a
a
a
b
b
15
16
17
CS
C1
ab
ab
C2
ab
C3
C3+L
3
L
b
2
1
0
0
14
28
42
days
CS
C1
C2
C3
4
a
C3+L
2
1
b
28
42
0
0
14
days
18
4. CONCLUSION
Remediation of Cd-contaminates soils can be achieved by adding
phosphate compounds or biosolids compost. Both amendments can enhance
Cd immobilization by redistribution of Cd to less available fractions.Phosphate
addition was found to decrease Cd availability, although the mechanisms of
Cd fixation is not fully known. Alternatively, the addition of alkaline biosolid
compost decreased the concentration of the soluble and exchangeable Cd
fraction, and increased the concentration of organic and, to a lesser extent,
inorganic-bound Cd fractions.
The environmental factor more likely to have the largest effect on Cd
availability is soil acidification. Consequently, if in situ remediation materials
exert their effect through changes in soil pH, then reacidification of soil would
return Cd to the original toxic level. Therefore, there may be a need to manage
soil pH in perpetuity if toxicity is to be avoided. Nevertheless, one of the
major inherent problems associated with these immobilization techniques is
that, although Cd becomes less bioavailable, total Cd concentration in soils
remains unchanged. In the long-term the immobilized element may become
more mobile and bioavailable through natural weathering processes.
19
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