Pedosphere 25(4): 555–568, 2015

ISSN 1002-0160/CN 32-1315/P

c 2015 Soil Science Society of China
Published by Elsevier B.V. and Science Press

Immobilization of Lead and Cadmium in Contaminated Soil

Using Amendments: A Review

Amanullah MAHAR1,2 , WANG Ping1 , LI Ronghua1 and ZHANG Zengqiang1,∗

1 College of Natural Resources and Environment, Northwest A&F University, Yangling, Shannxi 712100 (China)
2 Centre for Environmental Sciences, University of Sindh, Jamshoro 76080 (Pakistan)
(Received September 9, 2014; revised May 4, 2015)

ABSTRACT
Since the inception of industrial revolution, metal refining plants using pyrometallurgical processes have generated the prodigious
emissions of lead (Pb) and cadmium (Cd). As the core target of such pollutants, a large number of soils are nowadays contaminated
over widespread areas, posing a great threat to public health worldwide. Unlike organic pollutants, Pb and Cd do not undergo chemical
or microbial breakdown and stay likely in site for longer duration after their release. Immobilization is an in-situ remediation technique
that uses cost-effective soil amendments to reduce Pb and Cd availability in the contaminated soils. The Pb and Cd contamination in
the soil environment is reviewed with focus on source enrichment, speciation and associated health risks, and immobilization options
using various soil amendments. Commonly applied and emerging cost-effective soil amendments for Pb and Cd immobilization include
phosphate compounds, liming, animal manure, biosolids, metal oxides, and biochar. These immobilizing agents could reduce the
transfer of metal pollutants or residues to food web (plant uptake and leaching to subsurface water) and their long-term sustainability
in heavy metal fixation needs further assessment.
Key Words: bioavailability, biochar, biosolids, heavy metal, public health, remediation, soil extraction

Citation: Mahar A, Wang P, Li R H, Zhang Z Q. 2015. Immobilization of lead and cadmium in contaminated soil using amendments:
A review. Pedosphere. 25(4): 555–568.

INTRODUCTION pends upon the source, dosage, rate, and magnitude

The contamination of land resources is a major
worldwide concern as urban sprawl and industrial units
are continuously rising and leaving negative ecological
footprints on the natural environment (Wong and Li,
2004). Lead (Pb)- and cadmium (Cd)-contaminated
soils are a global environmental concern that results
not only in human health and ecological hazards, but
also in huge economic implications with respect to
reclamation and restoration costs (Semenzin et al.,
2007). Since the last few decades, the distribution and
mobility of heavy metals in various soils have been
documented. While few heavy metals are essential for
living organisms in trace quantities, most are haza-
rdous in high concentrations. Among the later, Cd and
Pb, which are naturally present in soils, can accumu-
late in humans and cause serious health problems (Ok
et al., 2004).
Various unsustainable waste disposal practices
have resulted in significant accumulation of a diverse
range of toxic heavy metals including Cd and Pb.
The contamination of toxic metals in food chain de-
of plant metal uptake, physico-chemical properties of
soil, and the extent of absorption by animals (Adri-
ano, 2001). Worldwide public now becomes vocal on
the detrimental health implications to humans and the
natural environment (Marshall, 2001). On a histori-
cal note in human health, metal toxicity has gained
significant attention as a result of serial poisoning at
a large scale; i.e., a huge number of human poisoning
tragic cases of Minamata disease due to consumption
of contaminated fish by toxic metals were recorded, in
Minamata Bay in Japan in the late 1950s (Knopf and
König, 2010).
Many countries have recorded excessive Pb and Cd
concentrations in their soils. Significant negative effects
of Pb and Cd on human health have been noted in
China, India, and Bangladesh with an alarming large
number of populations at risk from toxic metals (Bhat-
tacharya et al., 2012). Cadmium is a serious concern
for Australia and New Zealand, where it accumulates
in offal of grazing animals and makes it unsuitable for
human usage (Loganathan et al., 2008). Likewise, Pb
in soils resulting from unsustainable use as a compo-

∗ Corresponding author. E-mail: zhangzq58@126.com.

556
nent of herbicides and fungicides during urban develop-
ment of horticultural sites is also an increasing concern
there (Pietrzak and Uren, 2011).
Toxic heavy metals do not undertake chemical and
microbial degradation and their total concentrations
usually do not change due to their persistent nature
after being released into the environment (Adriano et
al., 2004). As a result, the scientific community fo-
cuses immensely on the development of soil remedia-
tion technologies as global masses are increasingly vo-
cal on the animal and human health implications re-
sulting from contaminated soils. Soil remediation tech-
nologies are of special attention since conventional soil
reclamation practices, i.e., landfilling and excavation,
are often very expansive and environmentally unfea-
sible, as compared to alternative options. Many soil
amendment based-technologies such as soil immobiliza-
tion/solidification are cost effective and less environ-
mentally disruptive (Mulligan et al., 2001; Kumpiene
et al., 2008).
Unlike organic pollutants which can be destroyed,
heavy metals impair their toxicity and mobility by
triggering the important immobilization process, i.e.,
(ad)sorption, precipitation, complexation, and redox
reactions, in the process of soil remediation (Adriano
et al., 2004). In addition, biological and chemical sta-
bilization of toxic heavy metals using organic (i.e.,
biosolids) and inorganic amendments (i.e., phosphate
compounds and lime) are suitable options to minimize
metal bioavailability (Park et al., 2011a). In the ur-
ban environment, as more localized toxic heavy metals
are found, the process of metal stabilization including
chemical washing and phytoextraction has been ap-
Fig. 1 Illustrative diagram showing the relationship between immobilization, bioavailability and remediation of toxic heavy metals
(Bolan et al., 2014). M = metal.
A. MAHAR et al.
plied for remediation. For safe disposal of toxic metals
from urban soil, phytoextraction process and the sub-
sequent recovery are considered for commercial and re-
search implications (Robinson et al., 2009). However,
when phytoextraction is ineffective, alternate options,
i.e., in-situ immobilization, are considered as impor-
tant part of environmental management (Fig. 1). Both
organic and inorganic soil amendments are components
of remediation techniques applied to manage conta-
minated soils.
The immobilization of Pb and Cd in contaminated
soils depends upon the local availability and financial
implications of soil amendments. Therefore, the main
question to be answered here in this review is that
what types of amendments have been commonly em-
ployed and are emerging as cost-effective technologies
to immobilize Pb and Cd in contaminated soils by sig-
nificantly decreasing bioavailability of these metals.
SOURCES OF ENRICHMENT IN SOIL
Soil functions as a final sink for heavy metal
contamination in terrestrial ecosystems. Both anthro-
pogenic and pedogenic sources contribute to heavy me-
tal loads in the soil environment. Most toxic trace ele-
ments are naturally present in the parent material of
soil, mainly in forms that are not readily bioavailable
for plant absorption or uptake as compared to those
of pedogenic contribution by anthropogenic sources
which have extreme bioavailability (Naidu et al., 1996;
Lamb et al., 2009). Anthropogenic activities such as
manufacturing industrial processes, usage of phospho-
rus (P) fertilizers, and disposal of domestic and indus-
trial wastes are the main sources of toxic heavy metals
SOIL LEAD AND CADMIUM IMMOBILIZATION
in the soil environment (Adriano, 2001; Bolan et al.,
2003a, b, c, d; Gray et al., 2003).
Lead is a natural constituent in the Earth’s crust
and is normally available at trace concentrations in
plants, soils, and water bodies. Metallic Pb is rarely
found in the natural environment (Cheng and Hu,
2010). Galena (PbS) and cerussite (PbCO3 ) are the
important Pb minerals; anglesite (PbSO4 ) and pyro-
morphite (Pb5 (PO4 )3 Cl) also frequently occur but in
less quantities (Crook, 1921). Lead is commonly found
in ores which also contain copper (Cu), zinc (Zn), and
silver (Ag) and extracted as a co-product of these me-
tals. Lead is extremely malleable, ductile, and very
easy to smelt, and its ores are extensive. Lead may e-
xist in the Bronze and Copper ages and is considered as
one of the seven antique metals. In 6 500 BC, the first
Pb object was used and the processing of Pb minerals
upgraded significantly around 6 000 years ago (Nriagu,
1983). Due to anthropogenic activities at a global scale,
Pb has become a widespread toxic metal in the natural
environment across the world. Today, Pb is used exten-
sively in lead-acid batteries, weights, pewters, fusible
alloys, and bullets, lead shots (pellets), solders, and
building construction (Cheng and Hu, 2010).
Atmospheric deposition due to emission of Pb-
based petrol is a main problem in various countries
where there is no restriction on consumption of leaded
gasoline (Fenger, 2009). On the other hand, biosolids
are the main source of toxic metals released in North
America and Europe, and P fertilizers are considered to
be the main source of heavy metals, especially Cd and
Pb, in New Zealand, Australia, and China (McLaugh-
lin et al., 1996; Bolan et al., 2003a; Loganathan et al.,
2008; Haynes et al., 2009). The main sources of Pb
contamination in soil are smelting, mining, industrial,
coal burning, and waste incineration.
Cadmium is odorless, whitish silver in appearance
and has a firm bioaccumulative tendency. It is easily
absorbed into animal, human, and plant tissues due
to its chemical nature similar to Zn (van der Voet et
al., 1994). This is a highly toxic metal and usually
found in the industrial work places, extensively used
in electroplating, industrial paints, sprays, and manu-
facturing of batteries, and results from the waste-water
discharge of stearate Cd factories. Cadmium contami-
nation due to P fertilizers used in agricultural soils is
of specific concern because Cd originates from phos-
phate rocks which are used for P fertilizer manufac-
turing and becomes part of food chain through regular
use of Cd-containing P fertilizers. The safe limits for P
fertilizers have not been set, although various countries
have stipulated threshold levels for Cd in soil due to
557
consumption of municipal biosolids (Wuana and Oki-
eimen, 2011).
SOIL EXTRACTION TECHNIQUES
Bioavailability of Pb and Cd in soil can be inves-
tigated using chemical extraction and bioassay proce-
dures that assess a bioaccessible fraction of these me-
tals. Sequential and single extractions using reagents
are the methods of chemical extraction (Ruby et al.,
1996; Basta and Gradwohl, 2000). Animals, plants,
and microorganisms are the tools for bioassay (Yang
et al., 1991; Domene et al., 2010).
Salt solutions (0.01 mol L−1 CaCl2 ), mineral acids
(1 mol L−1 HCl), chelating agents (diethylene triamine
pentaacetic acid (DTPA)), and buffer solutions (1 mol
L−1 NH4 OAc ) are chemical extractants used in sin-
gle extraction procedure for assessing bioavailability
in Pb- and Cd-contaminated soils (McBride et al.,
2009; Bakircioglu et al., 2011). Chelating agents (0.05
mol L−1 DTPA and 0.05 mol L−1 ethylenediamine
tetraacetic acid (EDTA)) have been documented as
more trustworthy in predicting the Pb and Cd availa-
bility in plants and are more impressive in eliminating
soluble metal-organic complexes (Sims and Johnson,
1991; Zhu et al., 2012).
Sequential extraction schemes are commonly used
to determine the redistribution or partitioning of Pb
and Cd in different chemical forms, i.e., adsorbed (ex-
changeable), soluble, occluded, and precipitated (Ta-
ble I). With each successive step of the scheme, the
bioavailability and solubility of Pb and Cd in soil re-
duces, though the extraction methods differ (Basta and
Gradwohl, 2000; Zakir and Shikazono, 2011). Specific
chemical species measured through chemical extraction
procedures have been successfully linked with plant
metal uptake in assuming the plant availability of me-
tals in soils (Naidu et al., 1997; Abedin et al., 2012).
The relative bioaccessibility leaching procedure
(RBALP), physiologically based extraction test (PB-
ET), gastrointestinal (GI) test, and potentially bio-
available sequential extraction (PBASE) are the physi-
ologically based in vitro chemical extraction proce-
dures for assessing bioavailability of Pb and Cd in soil
(Drexler and Brattin, 2007; Ng et al., 2013). These ad-
vanced schemes predict the bioavailability of Pb and
Cd in sediment and soil when ingested by human and
animals. With reference to the conventional sequential
procedures, the capacity of these schemes to solubilize
Pb and Cd enhances with each following extraction
step. Regardless of the identified non-specific nature of
these chemical extraction procedures, their analytical
simplicity and speed prove them to be most potential
558 A. MAHAR et al.

TABLE I
Different methods used for extraction of Pb and Cd in soils or sediments from various parts of the world

Soil(s) or sediments Extraction techniquea) Analytical References

methodb)
Sediments from Barcelona Harbour, Spain Modified BCR three-step sequential extraction ICP-MS Guevara-Riba et al., 2004
method
Sediments from Kranji & Pulau Tekong Modified BCR three-step sequential extraction GFAAS Cuong and Obbard, 2006
Harbour, method
Singapore
Sediments from Townsville Harbour, Qu- Modified Tessier extraction method AAS Esslemont, 2000
eensland, Australia
Sediments from Richards Bay Harbour, Tessier extraction method FAAS Wepener and Vermeulen,
South Africa 2005
Sediments from East China Sea BCR three-step sequential extraction method ICP-MS Yuan et al., 2004
Sediments from Norwegian Sea and Baltic Four-step sequential extraction method AAS Pempkowiak et al., 1999
Sea
Sediments from Huelva Estuarine, Spain Three sequential extraction methods AAS Usero et al., 1998
Sediments from Southwest Coast, Spain BCR-sequential extraction method GFAAS Morillo et al., 2004
Urban Soils from Hangzhou City, China Optimized BCR three-step sequential extraction ICP-MS Zhang and Wang, 2003
method
Polluted soils and sediments from Morocco Optimized BCR three-step sequential extraction FAAS Elass et al., 2004
method
Soils affected by accidental spills from Optimized BCR three-step sequential extraction ICP-MS Pueyo et al., 2003
Spain method
Contaminated soils from Iran Na2 -EDTA (0.1 mol L−1 ) extraction AAS Mahvi et al., 2005
Soil from Moscow Region, Russia Kerstner-Forstner sequential extraction scheme ICP-MS Katasonova et al., 2005
Contaminated soil from Southwest of Sar- Sequential extraction with H2 O, 0.1 mol L−1 ICP-MS Garau et al., 2007
dinia, Italy Ca(NO3 )2 , and 0.05 mol L−1 EDTA
Tropical soils from Sao Paulo State, Brazil Ahnstrom and Parker extraction scheme AAS Silveira et al., 2006
Contaminated soils from Carpiano, Milan, DTPA/TEA method ICP-OES Contin et al., 2008
Italy
Contaminated soil from Chungnam, Korea Deionized water and 0.1 mol L−1 Ca(NO3 )2 ex- ICP-MS Lee et al., 2009
traction
Contaminated soil from Arnoldstein, Aus- DTPA, CaCl2 , EDTA, and ammonium acetate AAS Tica et al., 2011
tria extraction scheme
Smelter site soils from Anghang, Seocheon, USEPA TCLP method 1311 ICP-OES Bade et al., 2012
Chungnam, Korea
Contaminated soils from Hadong Coast, Aqua regia extraction ICP-OES Ok et al., 2011
Gyeongnam, Korea
a) BCR = Community Bureau of Reference; EDTA = ethylenediamine tetraacetic acid; DTPA = diethylene triamine pentaacetic acid;
TEA = triethanolamine.
b) ICP-MS = inductively coupled plasma-mass spectrometry; GFAAS = graphite furnace atomic absorption spectrometry; AAS =

atomic absorption spectrophotometry; FAAS = flame absorption atomic spectrometry; ICP-OES = inductively coupled plasma-optical
emission spectrometry; TCLP = toxicity characteristic leaching procedure.

for regular identification of metal forms and assessment
of Pb and Cd bioavailability in situ although the dis-
persal of given metals among different fractions can
only be measured as a valuation at best because of the
subjectivity of the steps involved.
As microorganisms are more sensitive to metal
(Pb and Cd) stress than plant flora or soil microfau-
na, determining bioavailability and toxicity of metals
in contaminated soils employing microorganisms are
gaining more and more focus nowadays (Zhang et al.,
2010; Anyanwu et al., 2011). The procedures using pro-
tozoa and microflora have showed the capacity to de-
liver an extent of short-term bioavailability of heavy
metals and even enable the assessment of temporal
changes. On the other hand, macrofauna (enchytri-
dae, invertebrates, and earthworms) and mesofauna
(microarthropods) have the ability to demonstrate col-
lective impacts. There are drawbacks in these met-
hods: they are time consuming and can only give an
overall impact of metal bioavailability to the species
tested. In addition, molecular techniques are swiftly
developed and applied, but they are generally rela-
tively expensive; thus, the information given by the
techniques requires to be well explained (Amaro et al.,
2011; Frostegård et al., 2011).
PUBLIC HEALTH RISKS
Soils contaminated with toxic heavy metals not
SOIL LEAD AND CADMIUM IMMOBILIZATION
only possess threats to environmental health but al-
so have huge financial issues, i.e., removal costs and
restoration problems (Semenzin et al., 2007; Chapman
et al., 2013). Lead is susceptible for inhalation or in-
gestion from different sources, i.e., food items, pollu-
ted ambient air, soil, and polluted potable water. A
soil contaminated with Pb mostly enters human body
through inhalation or ingestion and may leave harm-
ful effects on the central nervous system (Needleman
et al., 1990). Human adults are vulnerable to lead poi-
soning, causing problems to central and peripheral ner-
vous system, blood pressure, and kidney (Needleman,
2004). Mild exposures to Pb may cause increased blood
pressure, decreased neurological functions, weakness,
and tingling in the extremities (Jennings, 2013). High
Pb exposures may cause kidney damage, miscarriages,
severe brain impairment, and ultimately, death. Com-
pared to adults, infants and children are more vulne-
rable to Pb poisoning, triggering irreparable impacts
on mental development in their early childhood (God-
win, 2001). Even mild exposures can affect infant’s
neurological and physical development (ATSDR, 2007;
NLM, NIH, 2012). Nowadays, Pb contamination is a
global issue and the focus has shifted from suscepti-
bility of adults to increases of emissions in industrial
areas to a significant number of children populations
being more prone to respiratory allergies and asthma
with lesser contacts (Needleman, 2004). A consensus
analysis showed that Pb is probably a human carcino-
gen and leaves multiple impacts on overall quality of
environmental health (ATSDR, 2007).
Without any inhibition of plant growth, Cd can
accumulate in plant at concentrations harmful to hu-
man or animal consumption (Asami, 1984). Cadmium
is poisonous to all living organisms and can enter in-
to the human body through various different routes.
When a human body absorbs Cd, it may show symp-
toms such as difficulty in breathing, salivation, vomi-
ting, nausea, anemia, abdominal pain, diarrhea, and
kidney failure. Furthermore, inhaling smoke or dust
containing Cd may cause headache, dryness of throat,
coughing, chest pain, bronchial complications, and in-
creased uneasiness. Cadmium may also have harmful
effects on the metabolic systems of living organisms
(Doyle, 1977). Moreover, Cd might cause kidney disor-
der or ultimately death at the concentration of 200 mg
kg−1 in the kidney (Alloway et al., 1990). A total of
64 persons died in the Jintsu Valley of Toyama, Japan
in 1969 due to Itaiitai disease (Friberg, 1984).
IMMOBILIZATION USING SOIL AMENDMENTS
Many efforts have been made in developing reme-
559
diation technologies to minimize or control Pb and
Cd contamination in soil. In general, various reme-
diation methods are needed to eliminate Pb and Cd
from wastes containing exceeding levels of contami-
nants than stipulated safe limits. Various amendments
are being employed to immobilize Pb and Cd in conta-
minated soils. Immobilization of toxic heavy metals
can be achieved mainly through precipitation, com-
plexation and adsorption, reactions which result in the
redistribution of metals from solution phase to solid
phase, thus reducing their transport and bioavailability
in the soil (Bolan et al., 2003a; Porter et al., 2004).
Phosphate compounds
Various studies have reported convincing evidence
for the mitigative value of both water-soluble (diammo-
nium phosphate, DAP) and water-insoluble (apatite
from phosphate rock, PR) phosphate compounds (Ta-
ble II), which can immobilize metals in soils, thus
decreasing their bioavailability for plant and human
uptake, mobility, and transport (Bolan et al., 2003b,
d). Phosphate compounds increase the immobilization
of metals in soils through different processes, i.e., di-
rect metal absorption/substitution by phosphate com-
pounds and precipitation of metals with phosphate so-
lution as metal phosphates.
Through increased phosphate anion-induced metal
adsorption and increased surface charge, soil applica-
tion of phosphate compounds can cause direct adsorp-
tion of metals on these compounds depending upon the
sources. Precipitation as metal phosphates has been
proved one of the main mechanisms for the immobiliza-
tion of Pb and Cd in soils (Bolan et al., 2014). These
fairly stable metal-phosphate compounds have ex-
tremely low solubility over a wide pH range, which
makes phosphate application an attractive technology
for managing Pb- and Cd-contaminated soils, but
phosphate is also a fossil source and high phosphate ap-
plication rates cause eutrophication of water resources.
In typical arable soils, precipitation of Pb and Cd is un-
likely, but in modest Pb- and Cd-contaminated soils,
this process can play a major role in the immobilization
of such metals.
The potential of apatite to immobilize Pb in conta-
minated soils or solution by Pb-phosphate precipita-
tion has been well reported (Chrysochoou et al., 2007).
The precipitants are usually termed as chloropyromo
rphite or hydroxypyromorphite. Two methods have
been recommended for the reaction of dissolved Pb
with apatite. Firstly, Pb(II) in apatite can be a substi-
tute for Ca(II). Thereby, through adsorption of Pb or
dissolution of hydroxyapatite (Ca10 (PO4 )6 (OH)2 ), (Ca,
TABLE II
Promising soil amendments in the immobilization of Pb and Cd in contaminated soils 560
Soil amendment(s) Target Immobilization result(s) Reference
metal(s)
Liming material(s)
Ca(OH)2 Cd Transforming to less mobile fractions, reduced phytoavailability Bolan et al., 2003c
Lime Cd No reduction in uptake, transferring to the kernels of sunflower Li et al., 1996
Lime Cd Reduced uptake by lettuce Lehoczky et al., 2000
Lime Pb, Cd Decreased Cd uptake, little influence on Pb uptake by radish Han and Lee, 1996
Ca(OH)2 , CaCO3 Cd Phytotoxicity prevented by Ca(OH)2 , but not by CaCO3 Chaney et al., 1977
Lime Cd Reduced uptake of Cd Brallier et al., 1996
Red mud, natural zeolite, lime Pb, Cd Reduced solubility of Pb and Cd, changes in microbial communities Garau et al., 2007
Zeolite, compost, calcium hydroxide Pb, Cd Increased residual fraction of metals in soils, decreased metal uptake by Castaldi et al., 2005
white lupin
Lime, red mud Cd, Pb Reduced metal concentrations in grass Gray et al., 2006
Cyclonic ash, lime Cd Reduced Cd accumulation in plant and concentration in soil pore water Ruttens et al., 2010
Portland cement Cd, Pb Different combinations with cement instead of cement alone as fixing agents Jang and Kim, 2000
Phosphate compound(s)
KH2 PO4 Cd Enhanced immobilization, decreased plant availability Bolan et al., 2003b
Apatite, zeolite, Fe oxide Cd, Pb Reduced mobility and plant uptake Chlopecka and Adriano, 1997
KH2 PO4 Pb, Cd, Zn Reduced Pb level, but not Zn and Cd levels in earthworms Pearson et al., 2000
Phosphate Pb Decreased Pb uptake with increasing phosphate supply, decreased phosphate Wang et al., 2002
concentration in the root with increasing Pb supply
Phosphate Pb, As Increased plant uptake of soil As, but no effect on soil Pb phytoavailability Creger and Peryea, 1994
H3 PO4 , Ca(H2 PO4 )2 , phosphate rock Pb Increased residual fraction, reduced translocation from root to shoot of plant Cao et al., 2003
Phosphate rock, diammonium phosphate Cd, Pb Reduced metal elution Basta and McGowen, 2004
Bonemeal (finely ground, poorly crystalline apatite) Pb Reduced concentration in the leachate and availability in soils Hodson et al., 2000
Hydroxyapatite, phosphate rock, triple superpho- Cd, Pb Reduced plant uptake Chen et al., 2007
sphate, diammonium phosphate
Metal oxide
Hydrous Mn oxide Cd, Pb Reduced mobility and ryegrass uptake Mench et al., 1994
Mn oxide Pb Reduced bioavailable fractions Hettiarachchi et al., 2000
Fe-rich waste (Fe (hydro)oxides) with redox cycles Cd, Pb, Reduced exchangeable fractions Contin et al., 2007
Mn oxide Cd, Pb Reduced exchangeable fraction and Chinese cabbage uptake Cheng and Hseu, 2002
Fe oxide waste byproduct Cd, Pb Reduced uptake by maize and barley Chlopecka and Adriano, 1996
Organic matter
Biosolid Cd Reduced bioavailability Bolan et al., 2003a
Papermill sludge, sewage sludge Cd Increased uptake Merrington and Madden, 2000
Biosolid Cd Reduced plant availability Brown et al., 1998
Biosolid Cd Increased phytoavailability in biosolid-amended soil by chloro-complexa- Weggler-Beaton et al., 2000
tion of Cd
Cow manure Cd No reduction in rice Kashem and Singh, 2001
Chicken manure compost Cd Reduced soluble/exchangeable fractions and phytotoxicity Liu et al., 2009
Compost Cd, Pb Decreased Cd leaching, but increased Pb leaching Ruttens et al., 2006
Coal fly ash, peat Pb Reduced leaching in the field lysimeters Kumpiene et al., 2007
Humus, compost Cd Reduced uptake by rice Ok et al., 2011
Biosolid, wood ash, K2 SO4 Pb, Cd Alleviated phytotoxicity of Pb and Cd and reduced bioavailability of Pb DeVolder et al., 2003
Hard wood biochar Cd Immobilization due to enhanced pH by biochar Beesley et al., 2010
Chicken manure- and green waste-derived biochars Cd, Pb Immobilization due to partitioning from the exchangeable to organic- Park et al., 2011c
bound fraction
Oak wood biochar Pb Sorption due to increases in soil pH Ahmad et al., 2012
A. MAHAR et al.
SOIL LEAD AND CADMIUM IMMOBILIZATION
Pb) apatites could be formed, followed by co-precipi-
tation of mixed apatites. Secondly, by precipitation of
pure hydroxypyromorphite (Pb10 (PO4 )6 (OH)2 ), Pb2+
can react with apatite through hydroxyapatite disso-
lution.
A substitute process, which happens to be signifi-
cant in temperate soils, involves metal-ligand com-
plexation in solution and followed reductions in cation
charge, which most likely decreases adsorption (Har-
ter and Naidu, 1995). The formation of soluble Cd-
phosphate complexes reduces Cd(II) sorption onto soils
in the presence of phosphate (Krishnamurti et al.,
1996). The activity of free Cd(II), rather than total
dissolved Cd(II), is a regulatory factor in Cd(II) sorp-
tion (O’Connor et al., 1984). The efficacy of phosphate-
induced metal immobilization can be improved by
enhancing solubility of phosphate compounds in the
soil. The combination of rock phosphate and phos-
phoric acid has the potential to immobilize Pb (Cao
et al., 2003). To enhance Pb immobilization in soil,
phosphate-solubilizing bacteria (PSB) were used to
slowly release phosphate from insoluble phosphate
rock (Park et al., 2011a, b) (Fig. 2). There are some
concerns related to the usage of phosphate compounds
for metal immobilization. The leaching of phosphate
induced after the phosphate treatment must be consi-
dered. A mixture of soil with phosphate addition in
the molar ratio of H3 PO4 :hydroxyapatite of 0.75:1 is
suggested to be optimum to reduce phosphorus (P)
leaching (Zupančič et al., 2012). Furthermore, bacte-
ria affect the stability of pyromorphite. It is assumed
that the microbes enhance the dissolution of mineral P,
promoting its transformation into pyromorphite. The
controversy of the method stems from the need of in-
troducing a living, extraneous strain of bacteria into an
uncontrolled environment, although the long-term ef-
fect of such a treatment is unknown. Park et al. (2011a,
c) showed that PSB can affect the stability of pyro-
morphite and the effectiveness of the process depend-
s on the availability of dissolved phosphates in solu-
tion. However, the interaction between microbes and
minerals are complex and some aspects of the potential
involvement of PSB in remediation treatments remain
unclear. There is some evidence that various organic
compounds, microbial metabolites, and plant activity
may increase the dissolution of pyromorphite and cause
a secondary Pb release (Sayer et al., 1997; Fomina et
al., 2004; Manecki and Maurice, 2008; Debela et al.,
2010, 2013; Topolska et al., 2013).
Lime treatment
Lime is basically used to ameliorate soil acidity but
561
Fig. 2 Immobilization of Pb by phosphate amendments with or
without phosphate solubilizing bacteria (PSB) as measured by
the Pb concentration in soil extracted with ammonium nitrate
(NH4 NO3 ) (Park et al., 2011b; Bolan et al., 2014). The soils
tested, a naturally Pb-contaminated soil collected from a shoo-
ting range and a Pb-spiked soil collected from an uncontamina-
ted site, are a sandy loam with a pH of 5.8, water-holding capaci-
ty of 38.5%, electrical conductivity of 34.5 μS cm−1 , and organic
matter of 7 g kg−1 and a silt loam with a pH of 5.23, water-
holding capacity of 73%, electrical conductivity of 66.9 μS cm−1 ,
and organic matter of 109 g kg−1 , respectively. CK = control
without phosphate amendment; TP = tricalcium phosphate; HA
= hydroxyapatite; PR = phosphate rock.
at the same time it is getting wide acceptance as a
potential option among scientific community to reduce
metal poisoning in soil (Fig. 3). Liming materials are
in a diverse range with differences in their potential
to neutralize the acidity (Table II). Over the years, li-
ming has been employed as a regular traditional prac-
tice to decrease levels of Cd and Pb in edible parts
of agricultural crops. Liming increases sorption of me-
tals through decreasing the H+ concentration and en-
hancing negatively charged ions. Addition of alkaline
materials such as lime and red mud increases the con-
centrations of residual fractions of Cd and Pb in conta-
minated soil. The pH increases in red mud and lime
result in the heavy metal precipitation (Garau et al.,
2007).
The competition between Ca(II) and metal ions
and the reduced mobility in soils by precipitation and
adsorption result in reduced metal uptake by plants
with liming on the root surface (Gray et al., 2006). An
in-situ field trial of heavy metal remediation in conta-
minated soil proved that combing red mud and lime en-
hances soil pH and reduces metal bioavailability, thus
forming vegetative cover in soil contaminated by Pb
and Cd.
Lime can be employed in combination with other
amendments to decrease metal availability. When lime
is mixed with biosolids, it decreases electrical conduc-
tivity (EC) and enhances pH, precipitating soluble ions
562
Fig. 3 Immobilization of Cd and Pb by eggshell, oyster shell
and calcium carbonate treatments as measured by the Cd and
Pb concentrations in soil extracted with 1 mol L−1 calcium chlo-
ride (CaCl2 ) after treatments (Ok et al., 2011; Ahmad et al.,
2012). The soil tested is a sandy loam with a pH of 6.21, ele-
ctrical conductivity of 0.22 dS m−1 , organic matter of 38.69 g
kg−1 , total N of 1.49 g kg−1 , and cation exchange capacity of
15.11 cmol(+) kg−1 . CK = untreated control; CC10 = calci-
um carbonate at 10 g kg−1 ; CC50 = calcium carbonate at 50 g
kg−1 ; ES10 = eggshell at 10 g kg−1 ; ES50 = eggshell at 50 g
kg−1 ; OS10 = oyster shell at 10 g kg−1 ; OS50 = oyster shell at
50 g kg−1 .
(Fang and Wong, 1999). Composting with lime addi-
tion also effectively increases pH and decreases leaching
and bioavailability of metals (Singh and Kalamdhad,
2013).
Cement-based solidification/stabilization
Soil contaminated with Cd and Pb usually needs
solidification/stabilization, aiming to lower the leac-
hing rate and bioavailability. Cement is the most adap-
table binder currently available for the immobilization
of Cd and Pb. The selection of cements and operating
parameters depends upon an understanding of che-
mistry of the system (Chen et al., 2009).
Cement-based stabilization/solidification techno-
logy is an attractive option for the management of soil
polluted with Cd and Pb to facilitate land use and
reduce the release of contaminants into the environ-
ment. The efficacy of cement-based solidification/sta-
bilization can be improved by modifying cement phase
compositions and controlling temperature, water/solid
ratios, particle size, and other factors that affect set-
ting and strength development and long-term durabili-
ty of solidified waste forms. The potentially deleterious
Cd and Pb may adversely affect the cementing matrix;
pretreatment to render such substances harmless, e.g.,
by adsorbent addition, is necessary in some cases (Jang
and Kim, 2000).
Portland cement (15%, weight/weight) was used
A. MAHAR et al.
for solidification/stabilization of Cd- and Pb-contami-
nated soils from a former industrial site (Voglar and
Leštan, 2010a). Soils formed solid monoliths with ce-
ment. Concentrations of Cd and Pb in the water ex-
tracts and the toxicity characteristic leaching proce-
dure (TCLP) extracts were lower in the solidified/sta-
bilized soils than the original soils.
Formulations of 15% (weight/weight) ordinary
Portland cement (OPC), calcium aluminate cement
(CAC), and pozzolanic cement (PC) and additives
including plasticizers cementol delta ekstra (PCDE)
and cementol antikorodin (PCA), polypropylene fibers
(PPF), polyoxyethylene-sorbitan monooleate (Tween
80) and aqueous acrylic polymer dispersion (Akrimal)
were used for solidification/stabilization of soils from
an industrial brownfield contaminated with up to 157
and 32 mg kg−1 Cd and Pb, respectively (Voglar and
Leštan, 2010b). Based on the model calculation, the
most efficient formulation was CAC + Akrimal, which
greatly reduced the leachability of soil Cd and Pb into
deionized water below the limit of quantification and
into TCLP solution and the mass transfer of the ele-
ments from soil monoliths.
There are several areas ripe for further investiga-
tions in the field of cement-based solidification/stabi-
lization of Cd and Pb in contaminated soils, for exa-
mple, the phase development of cement pastes in the
presence of Cd and Pb, the dissolution and precipita-
tion of stoichiometric phases and solid solutions, and
surface phenomena controlling Cd and Pb immobiliza-
tion (Akhter et al., 1990).
Animal manure and biosolids
Animal manures and biosolids are the signifi-
cant sources of organic composts. Biosolids are consi-
dered traditionally as one of the key sources of metal
contamination in the soil. Advances in the industrial
wastewater and sewage treatment technologies are suc-
cessfully decreasing metal contamination in biosolids.
Moreover, alkaline materials are used for stabilizing
metals in biosolids. Zeolites are also valuable as a metal
scavenger in the metal-contaminated biosolids. Natu-
ral zeolites stabilize Cd and Pb through transforming
them in the exchangeable and carbonate to residual
fractions (Zorpas et al., 2000).
Cattle, poultry, swine, and dairy are key sources
of animal manure byproducts worldwide. The majori-
ty of the manure products are less contaminated with
metals except As in poultry and Zn and Cu in swine
manure. However, recent developments in the manure
byproduct treatment have brought reduction in the
bioavailability of metals. For example, treatment of
SOIL LEAD AND CADMIUM IMMOBILIZATION
poultry manure with alum (Al2 (SO4 )3 ) reduced the
concentration of water-soluble Cd. Manure byproducts
lowly contaminated with metals can be employed in
stabilizing metals in soil (Bolan et al., 2014).
Various studies have assessed the role of biosolids
in the heavy metal contamination in the soil; howe-
ver, only few have documented the advantageous im-
pact of organic amendments as a sink for stabilization
of toxic metals in the soil (Li et al., 2000; Brown et
al., 2003). Alkaline-stabilized biosolids, known as de-
signer sludge with exceptional quality of being low in
metal bioavailability, can be employed as a potential
sink for decreasing metal bioavailability in sediment
and soil (Table II). Complexation, redox reaction, and
adsorption are the immobilization processes accom-
plished through such amendments.
Metals form both soluble and insoluble complexes
with organic constituents in soil; the mechanisms spe-
cially depend on the type of the organic matter. The
organic constituents in soil have a great affiliation to
metal cations due to the existence of functional groups
or ligands which can form chelates with metals. The
alcoholic, phenolic, carbonyl, and carboxyl functional
groups dissociate due to increasing pH, thus enhancing
ligand ion affinity towards metal cations. Through pre-
vention of sulfide oxidation/hydrolysis, the decreases
in the metal concentration can be credited to an in-
crease in soil pH (Hartley et al., 2004). Likewise, com-
post amendment increased the growth of white lupin
and decreased uptake of Pb through reducing metal
bioavailability in the soils (Castaldi et al., 2005). High
fulvic and humic acid concentrations of compost are
credited for the high metal-binding capacities of com-
post (Perminova and Hatfield, 2005; O’Dell et al.,
2007).
Oxides of metals
Oxides of metals such as iron (Fe), aluminum (Al),
and manganese (Mn) play an important role in metal
geochemistry in soils. Atmospheric nature and highly
active surface area make them potential for immobi-
lization and sorption of diverse soil pollutants (Table I-
I). Co-precipitation, formation of inner-surface comple-
xes, and specific sorption result in a strong metal bin-
ding by metal oxides. Synthesized, industrial bypro-
ducts and naturally occurring oxides have been docu-
mented in their potentiality to be employed for soil
remediation objectives (Kumpiene, 2010). Recent de-
velopments in the application of metal oxides and their
precursors for chemical immobilization of metals in
contaminated soils have been studied well (Komárek
et al., 2013).
563
Oxides of Mn (birnessite and phyllomanganates
group of minerals), oxyhydroxides (goethite, ferrihy-
drite, lepidocrocite, feroxyhite, and akaganeite), and
oxides of Fe (magnetite, hematite, and maghemite)
mostly occur in soil. Arsenat (AsO3− 4 ) and Pb(II)
form inner-sphere surface complexes with hydrous fer-
ric oxides and Pb and Cd form mononuclear comple-
xes on goethite and ferrihydrite surfaces (Knox et al.,
2001). The surfaces of Fe hydrous oxides play a signifi-
cant role in metal retention; Pb and Cd were immo-
bilized with amalgamation of Fe(II) and (III) sulfates
(Hartley et al., 2004). The re-use of Fe oxide-based
drinking water treatment residuals may be a beneficial
retention of heavy metals and suitable soil amendment
for various cations and anions (Impellitteri and Schec-
kel, 2006).
Manganese oxide minerals such as cryptomelane,
todorokite, hausmannite, and birnessite exist in soil
(Hettiarachchi et al., 2000). Birnessites exhibit the
highest adsorption capacity of Cd and Pb among these
Mn oxide minerals. The sequence of birnessite sorption
capacity is Pb(II) > Cd(II) and the maximum adsorp-
tion of metals by birnessite is attributed to hydroly-
sis which shows metal adsorption through Mn oxides
present primarily in the form of hydroxylation cations
(Feng et al., 2007). Oxides of Mn(IV) are well known to
precisely adsorb Pb. Cryptomelane is representative of
Mn oxides and was employed to decrease Pb bioavaila-
bility.
Fungi and bacteria enzymatically oxidize Mn(II),
produce insoluble oxides of Mn(III, IV), and form bio-
genic Mn oxides, which have a great sorption poten-
tial for metals including oxidation of metals (Miyata
et al., 2007). Sorption of metals by manganese oxides
is through complexation above or below the structural
vacancies and at structural sheet edges, and incorpo-
ration into the vacancies by isomorphical substitution
for Pb oxidation by biogenic Mn oxide produced by
bacteria.
Nanosized metal oxides such as Mn oxides, ferric
oxides, titanium oxides, aluminum oxides, cerium o-
xides, and magnesium oxides are referred to as poten-
tial adsorbents for metal remediation due to their high
activities and surface areas (Hua et al., 2012). Am-
monium acetate fuel has been used for the synthesis of
nanosized alumina and is effective in the Pb adsorption
in soil, but there are limited available studies which
employed metal oxides in soil environment (Rahmani
et al., 2010).
Biochar
Recent research development has proved that bio-
564
char has the capacity to adsorb metals in contaminated
soil and serves as a green environmental sorbent. Vari-
ous parameters are involved in assessing the main
role of biochar for environmental protection. Feedstock
types and pyrolysis conditions are the important fac-
tors affecting the sorption capacity of biochars (Joseph
et al., 2010; Kookana et al., 2011). However, research
studies have documented the reduction of Cd and Pb
in contaminated soils amended with biochar (Table
II). Therefore, the assessment of the biochar efficien-
cy in immobilization of contaminants in multi-metal-
contaminated soils should be conducted including the
metal immobilization mechanism of biochar to examine
the long-term efficacy.
Hardwood-derived biochar is effective in immobi-
lizing Cd in contaminated soils. Cadmium solubility
decreases at alkaline pH induced by biochar (Beesley et
al., 2010). However, biochar produced at low pyrolysis
temperature regimes immobilizes Pb (Uchimiya et al.,
2011). Remarkable Pb immobilization by biochar pro-
duced at low temperature results in the augmented re-
lease of available Ca, K, and P in the soil environment.
Biochar derived from dairy manure having a great
quantity of available P stabilizes Pb through making
insoluble hydroxypyromorphite (Pb5 (PO4 )3 (OH)) in
soil (Cao et al., 2011). The cotton seed hull-derived
biochar produced at 350 ◦ C contains a high oxygen
concentration, resulting in high uptake of Pb and Cd
due to the role of oxygen-containing functional groups
on biochar surfaces in metal binding (Uchimiya et al.,
2011).
CONCLUSIONS
Unlike organic contaminants, Pb and Cd do not
undergo microbial or chemical degradation and persist
for a long time after their introduction. Bioavailability
of Pb and Cd plays a vital role in the remediation of
contaminated soils. This paper reviews the remedia-
tion of Pb- and Cd-contaminated soils through ma-
nipulating their bioavailability using a range of soil a-
mendments. Metal-immobilizing amendments such as
precipitating agents and sorbent materials decrease
the bioavailability of Pb and Cd. Immobilizing agents
can be used to reduce the transfer of Pb and Cd to
food chain via plant uptake and leaching to groundwa-
ter. One of the major limitations of the immobilization
technique is the long-term stability of the immobilized
Pb and Cd that needs to be monitored.
In the current review, the immobilization options
with regards to engineering the bioavailability Pb
and Cd and following the remediation of polluted
A. MAHAR et al.
soil are summarized. More research studies are de-
sirable on the influence of immobilizing agents on
the physiological processes of the plant, i.e., photo-
synthetic activity, hydrolysis, plant nutrient uptake,
tropism, development of plant hormones including
their functions, nastic movement, photomorphogene-
sis, circadian rhythms, photoperiodism, plant response
to environmental stress, seed dormancy, germination,
osmotic pressure, turgor potential and stomata func-
tion in relation to plant-water nexus. Further studies
are required on the chelate-assisted phytoremediation
and the root-soil interface. Further phytotoxicity re-
search is required with focus on the effects of Pb- and
Cd-contaminated soils amended with solidifying agents
on the crop plants in both field and laboratory condi-
tions and the activity of enzymes required for photo-
synthesis, cell division and respiration, water absorp-
tion and transpiration, and chlorophyll, carotenoid,
and adenosine triphosphate (ATP) synthesis. More in
situ studies are needed to validate the significance of
a diverse range of immobilizing soil amendments to
restore contaminated soils. These kinds of field-based
experiments are essential to assess the effects of soil
amendments on co-contaminants. There is a dire need
to develop procedures to determine immobilization ef-
ficacy that could be used to assess the in-situ short and
long-term environmental stability of metal immobiliza-
tion. Additional in-situ studies should be conducted
to determine phyto-poisoning, ecological receptor end-
points, and human biomagnification to demonstrate
the heavy metal risk management efficiency resulting
from soil amendments.
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