Soil Washing For Metal Removal: A Review of Physical/chemical Technologies and Field Applications

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Journal of Hazardous Materials 152 (2008) 1–31
Review
Soil washing for metal removal: A review of physical/chemical

technologies and field applications
G. Dermont ∗ , M. Bergeron, G. Mercier, M. Richer-Laflèche
Institut National de la Recherche Scientifique Eau Terre et Environnement (INRS-ETE), 490 rue de la Couronne, Québec, QC, Canada G1K 9A9
Received 14 June 2007; received in revised form 11 October 2007; accepted 11 October 2007
Available online 22 October 2007
Abstract
Soil washing is one of the few permanent treatment alternatives to remove metal contaminants from soils. This paper reviews the various technol-
ogy types and pilot/full-scale field applications of soil washing applicable to soils highly contaminated with heavy metals. The physical separation
technologies, the chemical extraction processes and the integrated processes that combine both physical and chemical methods are discussed
separately. This paper reviews basic principles, applicability, advantages and limitations, methods of predicting and improving performance of
each physical/chemical technology. The discussion is based on a review of 30 recent laboratory investigations and 37 field applications of soil
washing systems which have been undertaken, mostly in the US, for the period 1990–2007. This paper also examines and compares the status of
soil washing technology for remediation of soils contaminated with metals in the US, in Canada and in Europe.
© 2007 Elsevier B.V. All rights reserved.
Keywords: Heavy metals; Soil washing; Physical separation; Chemical extraction
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Soil washing background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3. Physical separation technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.1. Applicability and limitations of physical separation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
3.2. Hydrodynamic classification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
3.3. Gravity concentration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
3.4. Froth flotation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
3.5. Magnetic separation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
3.6. Electrostatic separation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
3.7. Attrition scrubbing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
3.8. Integrated process train of physical separation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
3.9. Advantages/disadvantages of physical separation technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
4. Chemical extraction technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
4.1. Applicability and limitations of chemical extraction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
4.2. Acid extraction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
4.3. Salt solutions and high-concentration chloride solutions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
4.4. Chelant extraction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
4.5. Surfactant-enhanced solubilization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
4.6. Reducing and oxidizing agents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
4.7. Integrated process train of chemical extraction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
∗ Corresponding author. Tel.: +1 418 654 4677; fax: +1 418 654 2600.
E-mail address: [email protected] (G. Dermont).
0304-3894/$ – see front matter © 2007 Elsevier B.V. All rights reserved.
doi:10.1016/j.jhazmat.2007.10.043
2 G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31
4.8. Advantages/disadvantages of chemical extraction technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26

5. Combination of physical separation and chemical extraction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26
6. Status of soil washing technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26
6.1. Soil washing in Europe . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27
6.2. Soil washing in the USA . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27
6.3. Soil washing in Canada . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27
7. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
1. Introduction first purpose of this review is to present a technical description

of the various technologies: principle, applicability, methods of
In the United States, heavy metals are prevalent at almost predicting and improving performance are discussed. Several
all sites targeted by major remediation programs. For instance, recent laboratory studies involving physical separation (seven
metals are present in 77% of the Superfund sites (National Pri- examples) and chemical extractions (24 examples) are sum-
orities List), in 72% of the Department of Defense (DOD) sites marized. The physical separation technologies, the chemical
and in 55% of the Department of Energy (DOE) sites [1]. The extraction processes and the integrated processes that combine
USEPA estimates that over 50 million cubic meters of soil at both physical and chemical methods will be discussed sepa-
current NPL sites are contaminated with metals [1]. rately. The second purpose of this paper is to provide a review
The remediation of metal-contaminated sites has tradition- of the field applications of soil washing systems involved in the
ally involved excavation of the contaminated soils, followed treatment of the metal contamination. The discussion is based
by the immobilization of metal contaminants by solidifica- on a collection of 37 case studies of pilot/full-scale remediation
tion/stabilization (S/S) technology prior to disposal of the projects performed, mostly in the US, for the period 1990–2007.
materials treated in a permitted landfill site or on-site [2,3]. The third purpose of this paper is to review the implementation
The remedial actions based on S/S technology are no longer degree of soil washing technology relevant to the treatment of
considered a permanent environmental solution because of: (1) metal-contaminated soils, in the US, in Canada and in Europe.
the metals are not removed from contaminated media; (2) the
need for future monitoring of heavy metals on site; (3) ques- 2. Soil washing background
tionable longevity of the solidified/stabilized materials; and (4)
the long-term management of the solidified/stabilized materials Soil washing, as discussed in this paper, refers to ex situ
is based on landfilling and requires soil caps to prevent erosion techniques that employ physical and/or chemical procedures
problems. Hence, there is a great need to promote effective soil to extract metals contaminants from soils. Fig. 1 presents a
treatment technologies that attempts to remove the metals from schematic diagram of typical options used in soil washing pro-
the soils. Soil washing, which uses physical or chemical processes: (1) physical separation; (2) chemical extraction; (3)
cesses, is one of the few permanent treatment alternatives to combination of both. Physical separation (PS) concentrates
separate the metals from soils. metal contaminants into a smaller volume of soil by exploiting
This paper provides a review of the soil washing methods (ex differences in certain physical characteristics between the metal-
situ techniques) for soil contaminated with arsenic (As), cad- bearing particles and soil particles (size, density, magnetism,
mium (Cd), chromium (Cr), copper (Cu), mercury (Hg), nickel and hydrophobic surface properties). Chemical extraction (CE)
(Ni), lead (Pb), and zinc (Zn). Although arsenic is a metalloid, relates to techniques that try to solubilize the metal contami-
the term “metals” will be used to include all the elements under nants from the soil with an extracting aqueous fluid containing
discussion. The discussion focuses on the remediation of soil chemical reagents such as acids or chelating agents.
matrices highly affected by industrial and military activities Soil washing systems are quite flexible in terms of num-
(e.g., soil contaminated by tailings/slags, brownfields, battery ber, type, and order of processes involved and other names
recycling site, and shooting range site). Soil washing processes are used for soil washing technologies: “soil separation”, “soil
related to organic contaminants and radioactive metals are not recycling”, or “volume reduction”. The definition and use of
discussed here. Also, the discussion does not include in situ the terms “soil washing”, “physical separation” and “chemical
treatment (soil flushing). In this review, soil washing includes extraction” can differ according to the authors. The degree to
the following options: (1) physical separation based on min- which chemical agent or physical separation techniques are used
eral processing technologies; (2) chemical extraction based on may affect the nomenclature to describe the washing process. In
leaching or dissolving process; and (3) combination of physical the US and in Europe, soil remediation processes based on min-
separation and chemical extraction. eral processing technologies are often referred as the broad term
This paper is organized in five sections: (1) soil washing “soil washing” [4–6] although the term “physical separation”
background; (2) physical separation; (3) chemical extraction; (4) appears more accurate [7–9]. The term “soil washing” is also
combination of physical separation and chemical extraction; and used in the literature for describing processes that involve chem-
(5) status of soil washing in the US, in Canada and in Europe. The ical extraction processes [10–13]. FRTR [4] distinguishes “soil
G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31 3
Fig. 1. Schematic diagram of typical options used in soil washing processes.
washing” from “chemical extraction”: «soil washing generally project description (location, site name, the matrix type treated,
uses water or water with wash-improving additives and differs and completion date); (2) the basic principle and an exhaustive
from chemical extraction, which uses an extracting chemical». description of the process; (3) the metal concentrations in the
Confusion resulting from these misnomers often contributes initial soil and the cleaned soil; (4) the removal efficiencies of
to the propagation of misconceptions about the soil washing the treated metals; (5) the volume capacity of the process; (6)
technology. the treated volume; and (7) the quantities of the recovered met-
In the present paper, physical separation is primarily consid- als/concentrates, the management of the recovered metals and
ered as a particle separation process while chemical extraction washing residuals, and volume reduction efficiency. These data
can be considered as a metal desorption/solubilization process. are used as support for the overall discussion.
In general, physical separation is primarily applicable when
metal contaminants are under particulate forms (ideally liber- 3. Physical separation technologies
ated particle), while chemical extraction is primarily suitable
for ionic forms adsorbed on soil or non-detrital metals. Spe- The general approach in physical separation is to use tech-
cific comments relating to these aspects are provided in the nologies generally applied in mining and the mineral processing
corresponding sections of each technique. industry to extract the desired metal-bearing particles from min-
The authors collected information on full-scale and sig- eral ores. Mineral processing techniques are well established:
nificant pilot/field demonstrations of soil washing projects implementation is relatively simple; operation is often inexpen-
conducted in the US and Canada for treating metal contaminants. sive; equipments and processes involved are well described in
Also, some pilot projects performed in Europe and Korea are the literature [14,15]. In the context of soil remediation, mineral
gathered. Table 1 recapitulates 37 field application case studies: processing technologies were reviewed particularly to separate
16 projects involved PS technologies, 18 projects involved both metal contaminants from the soil [8,9,16,17]. Table 2 summa-
PS and CE processes, and three projects involved CE procedures. rizes the main classes of technologies according to the separation
About one third of the reported projects have been performed principles used. The operation units involved are: mechanical
since the year 2000. The metals most frequently treated are: Pb screening, hydrodynamic classification, gravity concentration,
(78% of the projects), Cu (43%), Zn (41%), and As (27%). For froth flotation, magnetic separation, electrostatic separation, and
each project, Table 1 summarizes the following data: (1) the attrition scrubbing.
4
Table 1
Field applications of soil washing technologies
# Project description (status, location, M/Fa Typeb Technology description Metal Initialc Finalc REd (%) Cap.e Vol.f Metal recovery/recycling, Ref.
remediation sponsor/vendor, and (␮g/g) (␮g/g) management of the
completion date) processed soil and washing
residuals
1 Pilot-scale demonstration of M PS Screening, gravity concentration, Hg >1000 624 25–50 3 m3 /h 5,000 m3 Hg recycling (1.3 t of Hg [103]
transportable unit at PPG Canada hydrocyclone, froth flotation were recovered)
Inc. site in Beauharnois, QC,
Canada (1992)
2 Pilot-scale demonstration M PS Vibrating screen, magnetic As 27–52 14–21 50–60 300 t/day – – [37]
G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

(Environment Canada program) of separation, attrition scrubbing, Cu 115–366 100–347 <25
Tallon’s physical separation unit at froth flotation Pb 248–336 188–327 <25
Dickson site, Montreal, QC,
Canada (1993)
3 Full-scale application performed by M PS Wet screening, hydrocyclones, Cr 500–5500 73 >90 30 t/h 19,200 t 85% of soil was [6,104]
Alternative Remediation attrition scrubbing, froth flotation Cu 800–8500 110 >90 re-deposited on site;
Technologies (ART) at King of Ni 300–3500 25 >90 revegetation; sludge cake
Prussia Superfund site, NJ (1993) (2000–6000 ␮g/g of metals)
was disposed off-site
4 SITE demonstration of BESCORP F PS Wet screening, attrition Pb 5600 200 65–85 20 t/h 56,000 t Disposal; Pb recycling (Pb [105]
(Brice Environmental Service) scrubbing, density separator smelter)
plant system at the Alaskan Battery
Enterprises site, Fairbanks, AK
(1993)
5 SITE demonstration of physical F PS Crushing, screening, attrition Hg 780–1080 17 98 4–20 t/h 63 t Hg recovery: thermal [106]
separation coupled with thermal scrubbing, hydroclassification desorption
desorption system (Harbauer (vacuum-distillation)
GmbH & Co. KG, Berlin) for
remediation of soils from
Marktredwitz site, Germany (1996)
6 Field application performed by M PS Size and density separation Pb >20,000 14–92 >90 – 1,500 t Pb recycling (10 t of [21]
Metcalf & Eddy for remediation of recovered bullet); 70 t of
Naval Weapons Station Earle Pistol clay fines required recycling
Range, NJ (1996) at an asphalt batch plant
7 Full-scale application performed by F PS Screening, hydrocyclones, froth Cu 200–10,000 – – 30 t/h 22,300 t Some site soils, which were [6,107]
ART and CINTEC for remediation flotation Pb 700–3000 not feasible for treatment
of soils from seven brownfields in Zn 1000–5000 by soil washing, were
Montreal, Qc, Canada (1996) disposed directly at the
Cintec landfill
8 Pilot-scale demonstration of the F PS Screening, fluidized-bed Cu 675–950 321–419 52–56 – 10 t Soil fraction <6 mm was [22]
physical separation process (INRS separation, gravity separators Pb 466–994 399–466 26–60 treated; the cleaned soil
and Dragage Verreault Inc.) for (jigs, spiral conc., MGS-Mosley), Zn 1869–2293 1483–1793 21–22 fraction was 85% of initial
remediation of brownfield soils froth flotation soil
from Montreal, QC, Canada (2000)
9 Several full-scale applications of – PS Gravity separator (KMS Cu – – – – – [108]
Kuryluk Mineral Separator (KMS) concentrator) Pb
concentrator (Phase Remediation Zn
Inc.) in Europe (2000)
10 Full-scale application of M PS Grizzly, vibrating wet screen, Pb 5300–38,000 396 93 – 3,600 t Recovering spent bullets [109,110]
BESCORP’s Particle Separation hydrocyclone, gravity separation and Pb recycling (21 t of
System, performed on by jig Pb 95% purity) for
Pb-contaminated soils from the Pb-smelter; 100% of soil
SAFR site at range 24, Fort Dix, NJ suitable for reuse

(1999)
11 Full-scale application of M PS Screening, hydrocyclone, gravity Pb >4820 <TCLP 98 – 6,200 t Pb recycling (50 t of spent [109,110]
BESCORP’s Particle Separation separation by jig bullet) for manufacturing
System, performed on soils from batteries; 601 t of residual
the SAFR site at Massachusetts soil was stabilized; 90%
Military Reservation (MMR), Cape of soil suitable for reuse;
Cod, MA (1999) revegetation
12 Full-scale application of M PS Screening, hydrocyclone, gravity Pb 20,000 1600 89 250 t/day 12,000 t Pb recycling (240 t of Pb [109,110]
BESCORP’s Particle Separation separation by jig 94% purity); 100% of soil
System at the SAFR complex of suitable for reuse
Marine Corps Air Ground Combat
Center, 29 Palms, CA (1998)
13 Full-scale application of ART’s M PS Vibrating wet screen, Pb – – – 100 t/h 30,000 m3 Pb shot recovered (90% [107]
Process at Former Skeet Shooting hydrocyclones, gravity separation purity) was treated in
Range Site (soil and sediment), jig off-site facility for Pb
Lordship Point in Stratford, CT recycling; revegetation
(2000)
14 NATO/CCMS Pilot test on F PS Hydrocyclone, wet gravity Hg 100–10,0000 <10 – – 2t Hg recycling [111]
decontamination of separation
mercury-polluted site (267–445 t of
Hg in 222.740 m3 of soil) in Ústı́
nad Labem, Czech Republic (2000)
15 Pilot-scale demonstration of M PS Grizzly, vibrating wet screen, Pb 2000 227 95 400 t/day 400 t Metal recycling [109,110]
BESCORP’s Particle Separation hydrocyclone, gravity separation Cu – <100
System at the SAFR site, Fort Ord, by jig
CA (period 2001–2005)
16 Full-scale application of ART’s M PS Screening, gravity separation by As – <400 ∼90 50 t/h 23,800 t Pb recycling (110 t of [107]
Process at Former Bend Trap Club jig Pb upgraded Pb shot); 90%
Skeet Range, Bend, OR (2007) of soil was disposed
on-site
5
6
Table 1 (Continued )
completion date) processed soil and
washing residuals
17 SITE demonstration of Toronto F PS/CE (1) PS: screening, hydrocyclones, Cu 1223 169 86 50 t/h 820 t Metal recovery in metallic [112]
Harbour Commissioners attrition scrubbing, density Ni 469 84 82 forms by electrowinning
(THC)/Bergmann USA for the separation; (2) CE: solubilization Pb 1687 211 87
remediation of the contaminated by acid leaching followed by ion Zn 3072 211 93
fine particles of soil from a former exchange chelating resin
auto/metal salvage site, Port

Industrial District, Toronto, ON,
Canada (1992)
18 Field demonstration of physical – PS/CE (1) PS: screening, hydrocyclone, Pb 100,000 – >90 – – Pb concentrate can be sent [8]
separation techniques for gravity concentration (jig, spirals to Pb smelter; No data
remediation of soils from SAFR, conc., Bartles-Mozley table); (2) about % of cleaned soil
conducted by US Bureau of Mines CE: heap acid leaching
(1993)
19 Field demonstration of physical – PS/CE (1) PS: vibrating screen, gravity Hg(s)g 15,370 10 80–99 – – RE are given for PS and [8]
separation to remove Hg from concentration (Neffco Hg(c)g 920 33 30–96 CE, respectively; Hg
soils, conducted by MRSDI for concentrator and spirals); (2) CE: recycling (600 g of Hg
Energy and Environmental acid leaching element was recovered)
Research Center (EERC) (1994)
20 Field-scale application of M PS/CE (1) PS: BESCORP process Pb 380–86,000 <200 >75 15 t/h 400 t PS process reduced the Pb [113]
BESCORP and COGNIS systems (trommel and wet classifier, load to the CE process by
at Twin Cities Army Ammunition density separation by jigs); (2) 39% to 63%; Pb
Plant, Site F in New Brighton, MI CE: COGNIS Terramet® (acid) concentrates from jigs
(1994) leaching process for fine particles and CE processes were
transported to Pb smelter
21 Pilot plant demonstration F PS/CE (1) PS: density separation, Cu 117–7533 34–402 48–98 – 45 t Potential for reuse of [114]
(Environment Canada and MCEBR magnetism separation and froth Cd 1020 <5 99 processed soil or
program) of a metal-separation flotation; (2) CE or bioleaching Pb 1202–2595 591–877 51–69 sediments; potential for
process developed by Alex-Sol Inc. Zn 1521–22,800 333–791 68–99 recovery of extracted
and INRS for remediation of soils metals
and sediments from Quebec city,
Montreal, and Trois-rivieres,
Canada (1995)
22 Field demonstration of M PS/CE (1) PS: attrition, size screening, Pb 4117 165 90 6 t/h 835 t 67% and 32% of soil [41]
BESCORP’s soil washing process hydrocyclones, density Cu – – 97 suitable for reuse after PS
at Joint Small-Arms Range 5, Fort separation by jig; (2) CE: acid Zn – – 89 and CE, respectively; Pb
Polk, Leesville, LO (1996) leaching (HCl) recycling (9 t) by
Pb-smelting
23 Field demonstration of ContraCon M PS/CE (1) PS: attrition, size screening, Pb 2828 122–1443 93 3 t/h 263 t The processed soil was [41]
Northwest’s soil washing process at hydrocyclones, density Cu – – 93 unsuitable for return to
Joint Small-Arms Range 5, Fort separation by jig; (2) CE: acetic Zn – – 77 the site (due to inadequate
Polk, Leesville, LO (1996) acid leaching neutralization and failed
TCLP) and was sent to a
landfill
24 Pilot-scale demonstration of soil M PS/CE (1) PS: size/density separation; As 97–227 7–142 34–93 – 200 t – [115]

washing performed by Metcalf & (2) CE: acid leaching Pb 3500–6300 10–306 95–99
Eddy at explosives manufacturing,
location unknown (1996)
25 Full-scale application of soil M PS/CE (1) PS: screening, gravity and Pb 11,800 max <1000 93 600 t/day 150,000 t 95% of processed soil [100,116]
washing system of Tallon Metal magnetic separation; (2) CE: suitable for reuse;
Technologies Inc. at the Longue hydrometallurgical extraction and potential recycling of Pb
Pointe site in Montreal, QC, VitrokeleTM adsorption concentrates
Canada (reported in 1998)
26 Pilot-scale demonstration of soil M PS/CE (1) PS: screening, gravity and Cd 4 <1 90 600 t/day 35 t Potential recycling for [100,116]
washing system of Tallon Metal magnetic separation; (2) CE: Cu 950 290 70 recovered metal; 85% of
Technologies at the Ataratiri site in hydrometallurgical extraction and Pb 2112 898 57 soil was recovered for
Toronto, ON, Canada (reported in VitrokeleTM adsorption Zn 2535 286 67 reuse
1998)
27 Field demonstration of the soil – PS/CE (1) PS: fluidized bed separation; Cu, Cr Pb, Zn – – – – – – [117]
washing system at Hunter’s Point (2) CE: acid leaching
Shipyard, San Fransisco, CA
(1998)
28 Full-scale application (results of 0– PS/CE (1) Washing with high pressure As 12.3 7.8 36 30 m3 /h 200,000 m3 /year Potential reuse of [118]
pilot demonstration) of biogenesis water and surfactants/chelating Cd 3.1 1.2 61 decontaminated sediment;
sediment washing technology for agents (metal separation) in Pb 157 68 57 further treatment of
remediation of dredged materials collision chamber; (2) Zn 279 131 53 washing solution (metal
(90% silt/clay) from the New hydrocyclone and wet screen Hg 3.9 0.3 92 precipitation)
York/New Jersey Harbor
(1999–2001)h
29 Pilot soil washing/leaching test for M PS/CE (1) PS: size separation, density PS:Pbi 750 87–117 84–88 – 40 t 85% and 5% of soil was [70]
remediation of soils from separation by jig; (2) CE: CE:Pbi 2300 84 96 cleaned with PS and CE,
battery-breaking site in Fairbanks, leaching with chloride solution respectively (VR = 90%);
AK (2001) (NaCl, 2 M; HCl, pH 2) and jig concentrate was 2.7 t;
oxidant (NaOCl) metal recovery by PbS
precipitation; PbS cake
can be sent to smelter
7
8
completion date) processed soil and
washing residuals
30 Pilot soil washing/leaching test for M PS/CE (1) PS: size separation, density PS:Pbi 5721 139–342 94–98 – 13 t29% and 62% of soil was [70]
remediation of soils from SAFR separation by jig; (2) CE: CE:Pbi 830 81 90 cleaned with PS and CE,
site, DE (2001) leaching with chloride solution respectively (VR = 91%);

(NaCl, 2 M; HCl, pH 2) and jig concentrate was 1.2 t;
oxidant (NaOCl) metal recovery by PbS
precipitation; PbS cake
can be sent to smelter
31 Pilot-scale demonstration of the F PS/CE (1) Washing with high pressure As 16–73 6–15 6–85 15 m3 /h 330 m3 Precipitation of metals [119]
BioGenesis sediment water and surfactants/chelating Cd 6–41 1–9 0–83 from washing solution;
decontamination process for agents in collision chamber; (2) Cu 95–375 17–39 60–91 Fine fraction of treated
remediation of dredged materials hydrocyclone and wet screen Pb 40–531 27–138 0–74 sediment, which has
from the lagoon of Venice, Italy Zn 115–531 84–630 0–72 higher metal
(2005)h Hg 3–10 0.5–2 75–93 concentrations, was
disposed to a landfill site
32 Pilot-scale study for remediation of M PS/CE (1) Attrition scrubbing As 43 10–15 63–75 Batch 0.5 t VR = 51–98% (vary [45]
contaminated soils from mining chemically enhanced by acid Ni 340 140–145 59–60 (40 kg) according to particle size
area, Seoul, Korea (2006) leaching (HCl, H2 SO4 , or Zn 68 50–55 38–45 fraction); the fine soil
H3 PO4 ) in drum-type scrubber; fraction (highly
(2) separation of fine contaminated) requires
soil + wastewater and sand soil further treatment
33 Pilot plant demonstration for M PS/CE (1) PS: size separation (screening, Cu 202–350 40–234 44 – 30 t The process produced [101]
remediation of urban contaminated spiral, hydrocyclone); (2) CE: Pb 2030–2200 69–848 60 91% of a
soil from Québec city, Canada acid leaching (HCl, pH 2–3) Zn 870–960 111–941 52 non-contaminated soil
(2007) and 9% of metallic
residue and heavily
contaminated soil
34 Full-scale application of the ART’s F PS/CE (1) PS: size screening, As 20–5000 <20 – 70 t/h 350,000 t Off-site disposal for filter [107,120]
process at Vineland Chemical hydrocycloning; (2) CE: leaching cake residue containing
(Pesticide manufacturing) and precipitation high concentrations of As
Superfund site, NJ (project in
progress)
35 Full-scale project of soil washing M CE Batch washing process using As 2–6200 <1 99 – 10,000 m3 Chemical treatment of [121]
coupled with chemical treatment sodium metaphosphate to lower Cr 4–6200 627 90 leachate: reduction of
(chromium reduction) at Palmetto pH to 2.0 and extract the Cr(VI) to precipitate in
Wood Preserving, SC (1989) chromium from the soil Cr(III) form; disposal of
soil and sludges residual
Three aspects about physical separation for remediation of
[116]
[96]
metal-contaminated soils will be separately discussed: (1) the
–: not available; SAFR: small arms firing range; SITE: Superfund Innovative Technology Evaluation of USEPA; MCEBR: Montreal Centre of Excellence in Brownfields Rehabilitation; VR: volume reduction.
a form potentially suitable
applicability of physical separation technologies according to
metals are concentrated in
levels; metal recovery by

RE is most lower for As;
forms of metal contamination and characteristics of soil matrix;

As and Cd > targeted (2) a review of each technology class; and (3) integrated pro-
precipitation/ion
cesses of physical separation. The discussion focuses first and
foremost on gravity concentration and froth flotation technolo-
for recovery
exchange
gies because they are the most important separation methods
used in a soil remediation context. The arguments are often based
on the assessment of the field-scale applications (Table 1) and
recent laboratory investigations (Table 3).
–
h The description does not include the remediation process of the organic contaminants, which were destroyed by cavitation/oxidation after separation with surfactants.
3.1. Applicability and limitations of physical separation
Physical separation techniques are primarily applicable to

10–100 kg/h
particulate forms of metals: discrete particles or metal-bearing

5–10 t/h
particles. Physical separation is generally not appropriate for

treating the sorbed forms of metals although attrition scrubbing
c Metal concentration: mean value or range, which may vary according to the tested samples or the particle size fractions that have been treated.
can significantly improve metal desorption in chemical leaching

process. The knowledge of the degree of liberation of the miner-
50–95
50–70
alogical phase containing heavy metals is significant to predict

the applicability of physical particle separation methods [16,18].
The liberation degree depends on the mineralogical aspects of
1000–22,500 <Dutch B
Variable
metal contaminant particles (shape, morphology, and miner-

levels
alogical association). Liberation degree refers to the release

availability of the “metal phase” according to various associ-
ations with the “carrying phase” or the soil particles. The term
Variable
“metal phase” refers to the mineral form under which the metal
d Removal efficiency of metal (the value is calculated from the concentrations or the recovered metal mass).
is present. The term “carrying phase” refers to another min-

a M: mobile system suitable for remediation on-site; F: the project has been performed in fixed facilities.
eral phase (Fe-oxides, carbonates, silicates, etc.) with which

Zn, Pb,
Cr, Cu,
As, Cd
Cd, As
Pb, Zn
Cr, Cu
the “metal phase” can be associated. Fig. 2 summarizes some

examples of various potential states of the metal phase (par-
e Capacity in tonnes metric per hour (t/h) or per day (t/day), cubic meters per hour (m3 /h).
ticulate forms): (a) included in the volume, (b) associated, (c)

weakly bounded on surface, and (d) liberated or free. Libera-
(oxidants, complexing agents,
Mild leaching and extraction
tion degree and applicability of particle separation, by gravity

Acid leaching (HCl, pH < 2)
concentration and froth flotation, are briefly discussed for each

b Basic principle of process: PS: physical separation; CE: chemical extraction.
state of metal phase (Fig. 2). The mineralogical aspects and

and organic acids)
i The study distinguishes the performances of the PS and CE processes.
solid phase speciation of metal-bearing particles can be inves-

g The study distinguishes the treated soil fractions (s: sand, c: clay).
tigated by microscopy and spectroscopy technologies such as

scanning electron microscope coupled with energy-dispersive
X-ray analysis (SEM–EDX).
The efficiency of physical separation depends on several
soil characteristics such as particle size distribution, particulate
CE
CE
shape, clay content, moisture content, humic content, hetero-

geneity of soil matrix, difference in density between soil matrix
F
and metal contaminants, magnetic properties, and hydrophobic

CACITOXTM process to remediate
for Hazardous Materials Research
properties of particle surface [8,9]. The treatment is difficult or

for remediation of four soils from
content, United Kingdom (1998)

SITE demonstration (bench- and
pilot-scale) performed by Center
NATO/CCMS Pilot test of the
unfeasible for the following cases: (1) the metal contaminants

soils with high clay and silt
US Superfund Sites (1995)
are strongly bound on soil particles; (2) the difference in density

or surface properties between metal-bearing particles and soil
matrix are not significant; (3) high variability of chemical forms
f The treated volume.
of metals; (4) the metals are present in all particle size fractions
of contaminated soil; (5) the soil contains silt/clay content in
excess of 30–50%; (6) the soil contains high humic content; and
(7) the soil contains organic compounds with high viscosity.
Particle size of feed material is one of the most significant
36
37
parameters that affect applicability of physical separation tech-

Table 2
Summary of physical separation types
Operation unit Basic principle Description and main objectives Comments Typical technologies
implemented
Mechanical screening Separation based on particle Mechanical screening uses size Widely used. Fine screens Vibrating grizzly; barrel
size exclusion through a physical barrier are fragile trommel; vibrating or
to provide suitable dimensions for gyratory screens
treatment
Hydrodynamic classification Separation based on settling Hydrodynamic classification Widely used. Difficult Hydrocyclones, elutriators,
velocity separates the particles by difference when clay and humic mechanical classifiers (screw
of settling velocity or by centrifugal soils are present classifier)
force into a water flow. These
methods are often used for size
separation
Gravity concentration Separation based on density The gravity concentration Widely used. Difficult Spiral concentrator, shaking
of particles technologies separate high density when clay and humic table, jig, MGS-Mozley,
from low density minerals or soils are present dense media separation
particles in a slurry of water and soil (DMS)
(relatively high solid content)
Froth flotation Separation based on The differences in hydrophobic Widely used. Chemical Flotation in cell or in column
hydrophobic properties of the properties of particle surfaces are additives are required (agitation or nonagitation
surface of particles exploited to separate certain minerals system)
from soil by attachment to air bubbles
injected in a pulp (low solid content)
Magnetic separation Separation based on magnetic Mineral particles are separated Moderately used. High Dry or wet separators using
properties of particles according to their different magnetic capital and operating high intensity (HIMS) or low
susceptibilities costs intensity (LIMS)
Electrostatic separation Separation based on electrical The separation is based on the Rarely used. Materials Electrostatic and
conductivity properties of difference in the surface electrical must be completely dry electrodynamic separators
particles conductivity of the particles to be
separated
Attrition scrubbing Mechanical Attrition scrubbing uses high energy Widely used. Various types of scrubbers
particle-to-particle scrubbing agitation of soil slurry (high solid Pre-treatment that
content) to remove coating of particle improves separation
surface and to disperse soil process
aggregates
nologies because the contaminated soils usually contain a wide natural/anthropogenic landfills. On the other hand, physical sep-
range of particle sizes, and the technology performance is often aration techniques are not appropriate for treating the “natural”
restricted to a specific particle size range (Fig. 3). Usually, most soils or agricultural soils affected by a diffuse contamination
of the hydroclassifiers and gravity concentrators have a good because: (1) the metals are mostly present in sorbed forms; (2)
applicability for the sand fraction (63–2000 ␮m). The standard the metal concentration levels are relatively low; and (3) these
gravity concentrators (jig, shaking table, and spiral) are usu- soils typically have a high content of silt/clay and organic mat-
ally not suitable for fine particles (<63 ␮m). Depending upon ter. Since metals present in soils are mostly in sorbed forms
the technology, there is a point at which the percentage of fine as opposed to discrete particles, physical separation is often
particles will be a limiting factor. Physical separation is mainly associated with chemical procedures to enhance metal removal.
appropriate and more cost effective for soils with sand content
in excess of 50–70% [19,20]. However, a process combining 3.2. Hydrodynamic classification
attrition scrubbing (which can be enhanced by chemical addi-
tives) and wet screening or hydrocyclones may be used for the Hydrodynamic classification, also called “hydroclassifica-
remediation of fine-grained matrices such as sediments [10]. tion”, involves separation of particles based upon the velocity
Likewise, froth flotation may be effective for treating relatively with which particles fall through water flow (involving sedimen-
fine particles (20–63 ␮m). tation, elutriation, and fluidization) or separation by centrifugal
The selection of the physical separation technologies strongly force into water flow (hydrocyclone) [8,16]. The main goal
depends on the soil and site types to be treated. These is separation by size particle. Hydrodynamic classification
techniques are primarily applicable to “anthropogenic” soils technologies principally include three technology classes: (1)
located in urban or industrial areas (e.g., brownfields, mine technologies based on centrifugation such as hydrocyclones;
spoils/tailings/slags from mining/smelting sites, and shoot- (2) technologies based on elutriation such as elutriation col-
ing range site) (Table 1). These soils are greatly affected by umn and fluidized-bed classifier; (3) mechanical classifiers such
human activity (industrial artifacts, disposal, landfills, etc.) as screw classifier. Hydrocyclones were widely implemented
and are typically composed of mixture of toxic wastes and in soil washing process to separate the fine soil from larger
Table 3
Laboratory investigations of physical separation technologies
Examples of studies Study objective Technologies (treated soil fractions) Metal Conc. (␮g/g) RE%a (technology or operating conditions) VR%b Ref.
Magnetic separation (HIMS) on six Use of magnetic separation as High intensity magnetic separation Cu 126 83 87–93 [35]
soils in the Netherlands (results stand-alone remediation (HIMS) with dry and wet separators Cr 244 77
with soil “L”) technique (63–2000 ␮m) Pb 121 46
Zn 598 79
Attrition scrubbing in conjunction Improvement of density Wemco attrition scrubber, Wifley Pb 40,000 96 80 [43]
with a shaking table on a soil separation (shaking table) by the shaking table
from an Army small arms use of attrition scrubbing

training range, USA
Evaluation of physical separation Study of various physical Wet magnetic separator Cu 7,458 52 (jig)/89 (shaking table) NA [18]
technologies for remediation of separation technologies for an (63–2000 ␮m), Attrition scrubbing, Pb 4,893 61 (jig)/67 (shaking table)
six browndfield soils (polluted integrated soil washing process gravity concentration: shaking table Zn 3,535 58 (jig)/54 (shaking table)
by landfilling of various wastes (63–850 ␮m); jig (850–2000 ␮m)
in Quebec City, QC, Canada
(results with soil “A1”, 90% of
sand)
Gravity separation to remediate Study of applicability of gravity Shaking table, heavy liquid Cu 113,000 73 (DMS)/85 (DMS + shaking table) 80–90 [122]
two shooting range soils separation to remove bullet separation (DMS) Pb 24,000 88 (DMS)/91 (DMS + shaking table)
contaminated by Pb-containing fragments
shotgun pellets in Finland
(results with Utti soil)
Evaluation and analysis of soil Evaluation of gravity separators Shaking table (74–840 ␮m); jig Pb 500–2,195 22–93c (jig + shaking table) NA [51]
washing for seven in an integrated soil washing (840–4760 ␮m)
Pb-contaminated soils from process
Netherlands
Froth flotation as a remediation Evaluation of froth flotation as Denver laboratory cell (grain size: Cd 13 60 at pH 8 80 [25,26]
technique for heavily polluted stand-alone remediation 70% <50 ␮m) Cr 267 48
sediment in Belgium technique. The influence of the Cu 128 53
particle size distribution and Pb 721 60
metal speciation on the froth Zn 3,200 60
flotation efficiency
Froth flotation on a soil in Tienen, Improvement of froth flotation by Sulfidisation with Na2 S, Denver Cd 8 25 (without sulfi.)/47 (with sulfi.) 70–80 [28]
Belgium sulfidisation pre-treatment laboratory cell (0–2000 ␮m) Cu 68 30 (without sulfi.)/45 (with suldi.)
Pb 142 30 (without sulfi.)/42 (with suldi.)
Zn 357 30 (without sulfi.)/42 (with suldi.)
a Removal efficiency.
b Volume reduction of contaminated soil.
c Range value, according to soil types.
11
Fig. 2. Applicability of physical separation according to liberation degree of the metal phase for the particulate forms.
sand particles. The centrifugal force is more powerful than the the separation process [8]. For this reason, it is necessary to
force due to gravity; thereby, the operating time to achieve sep- classify by size the soil to be treated before performing grav-
aration is significantly reduced [16]. Hydrocyclones have low ity concentration. If the density difference between the soil
capital and operational costs compared to other classification and contaminant particles is significant, the gravity concen-
equipment [9]. Screw classifiers and hydroclassifiers based on tration technologies should be particularly suitable for particle
elutriation can also be implemented in a soil remediation con- separation. The volume capacities of gravity concentrators are
text [16,21,22]. Moreover, new more efficient technologies of 100–500, 25, 4, and 5 t/h for dense media separation (DMS),
fluidized-bed separator such as the CrossFlow classifier and mineral jig, spiral, shaking table, and MGS-Mozley, respec-
the HydroFloat separator have recently been developed for the tively [14,16]. The particle size range conditions are reported
mineral processing industry [23]. on Fig. 3.
The most common gravity concentrators, used for soil treat-
3.3. Gravity concentration ment at large scale, are jigs, shaking tables and spirals (Table 1).
Mineral jigs are commonly used to treat coarse sand frac-
Theses techniques exploit the difference in gravity of parti- tions (800–2000 ␮m) or gravel fractions (2000–6000 ␮m) while
cles in slurry to separate the metal-bearing particles from soil shaking tables and spirals are more suitable to treat fine to
matrix. Settling is due to density, size, shape and weigh of par- medium/coarse sand fractions (63–2000 ␮m) (Table 3). Silt/clay
ticle; however, density is the key factor. Gravity separation is (<63 ␮m) and very fine sand (63–125 ␮m) fractions can be pro-
inefficient when used to treat particles that have either a wide cessed with MGS-Mozley. Bergeron [22] reported the following
size distribution or a narrow density distribution [9]. Gosselin results for long-term trials in remediation project of brownfield
et al. [16] report that density difference must be greater than soils from Montreal, Canada: (1) 75% of Cu removal efficiency
1 g/cm3 for sufficient separation. The effectiveness of density (823 ␮g/g of Cu in initial soil) obtained with the use of two
separation can be estimated by the “concentration criterion” jigs (in series) from the 1700–6400 ␮m fraction; (2) 54% of Cu
from Taggart [8,14]. The gravity concentrators such as jig, shak- removal efficiency (1025 ␮g/g of Cu in initial soil) obtained with
ing table and spirals can be affected by particle size effect during the spiral method from the 106–1700 ␮m fraction; and (3) 47%
Fig. 3. Feed particle size range for application of physical separation techniques. Adapted from [9,14–16,126].
of Cu removal efficiency (924 ␮g/g of Cu in initial soil) obtained is widely used in the mineral industry, and metal sulfides are
with MGS-Mozley from the <106 ␮m fraction. easier to separate than carbonates and oxides [14]. There are
Since Pb is a dense element, gravity concentration may be different types of flotation systems including flotation cells and
used for remediation of soils contaminated with particulate a flotation column.
forms of Pb (e.g., Pb-based old paint debris, battery- Froth flotation has been successfully used to remove met-
manufacturing/recycling sites, and smelting/mining sites). als (primarily Cd, Cu, Pb, and Zn) from sediments and soils
Density separation with jigs is a well-established method to [24–31]. Some examples of metal removal efficiency obtained
remove Pb from small arms firing ranges (SAFR) where Pb with flotation systems are described in Table 3. However, the
is mostly present in the form of spent bullets (Table 1, projects use of froth flotation as a remediation technique is still less used
#10–13, 15, 16, 20–23, 29, and 30). than other soil washing technologies. Froth flotation appears to
be a relevant technique for treating fine-grained matrices, espe-
3.4. Froth flotation cially anoxic dredged sediments (best separation efficiency in
the 20–50 ␮m range) where heavy metals are mostly present
Froth flotation is a physico-chemical technique that exploits under sulfide forms [25,26].
difference of hydrophobic properties to separate metal-bearing In soil remediation context, major factors influencing the
particles from the soil matrix. The separation principle is based floatability of metal-bearing particles are: (1) the heterogene-
on the affinity of a particle’s hydrophobic surfaces for air bub- ity of the metal compounds; (2) the metal distribution over the
bles injected in the slurry of soil. The separation process involves different particle size fractions; (3) the presence of high contents
three steps: (1) attachment of the desired metal-bearing particles of organic matter; and (4) the proportion of the very fine particles
to the air bubbles; (2) the bubbles are gathered in a foam portion; <10 ␮m [26,29]. Since sulfide minerals are more floatable than
and (3) the foam fraction, which floats up slurry, is removed. The carbonates or oxides, chemical pre-treatment by sulfidisation
surface of metals-bearing particles is often rendered hydropho- has been investigated (Table 3) [24,30]. The efficiency of flota-
bic by the use of a surfactant agent (collector). The froth flotation tion columns is usually much higher than that of flotation cells
in the finer portion of the grain size range [16,27]. The selective 3.7. Attrition scrubbing
flotation of metal-bearing particles from the particle size frac-
tion <10 ␮m is problematic in most mechanical flotation cells Typical attrition scrubbers use an intense opposing flow gen-
because of various phenomena of entrainment and entrapment erated by twin impellers in soil slurry with a very high solid
of the fine hydrophilic undesirable gangue particles [31,32]. The content (70–80%) to provide mechanical particle-to-particle
dissolved air flotation (DAF) system, which can produce very scrubbing in order to accomplish two main effects: scouring
small bubbles, is promising to improve the selective flotation and breaking [9,40]. The scouring effect involves the removal
for the fine particles range [29]. The conventional flotation sys- of coating or film from individual grains. The breaking effect
tems are less effective in floating large particles (>200–300 ␮m) involves the dispersion/separation of silt and clay bonded to sand
due to the inability of bubbles to carry coarse and heavy parti- and gravel particles, and the disintegration of soil agglomerates.
cles [14]. Compared to conventional flotation technologies, the Soil scrubbing is accomplished mostly by particle-to-particle
separation in froth (SIF) technology is more suitable for separa- attrition, but also by the interaction between the paddles and the
tion in the coarser particle size range [14]. Attrition scrubbing is particles [41].
often used prior to the flotation process in order to disaggregate Williford et al. [42] showed that preconditioning by attri-
the small particles bound on coarse particles and to remove the tion scrubbing enhanced size hydroclassification. Marino et al.
coating of a particle’s surface. Also, power ultrasound can be [43] showed that mechanical attrition increases the removal effi-
used instead of attrition conditioning [33]. ciency of metal on the Wilfley table (gravity concentration).
In full-scale application, flotation was mostly combined with Scrubbing effect produces fresh and clean grain surfaces (by
hydroclassification, and gravity concentration (Table 1). In the removing oxidized coating), and thus can enhance subsequent
1980s, Dutch companies like Jaartsveld, Mosmans and Heidemij froth flotation processes [14]. Attrition scrubbers can also be
pioneered the flotation technique for soil cleaning with Metso used to improve the chemical extraction of superficially bound
(Swedish company) as a major equipment supplier [34]. The contaminants (adsorbed metal cations) from solid particles [44].
most significant example of full-scale froth flotation use in the Ko et al. [45] have used a drum-type scrubber (pilot-scale) chem-
US, for metal removal from contaminated soils, is the project ically enhanced by acid leaching to extract metals (As, Ni, and
performed at King of Prussia Superfund site in 1993 (Table 1, Zn) from soils (Table 1, project #32).
project #3).
3.8. Integrated process train of physical separation
3.5. Magnetic separation
Table 1 shows that most of the large-scale applications of
Particles present in soil have magnetic susceptibilities which PS process trains (16 projects reported) primarily exploit the
vary from negative (organic), intermediate (paramagnetic min- differences in particle size (hydroclassification) and density
erals and organometallics) to largely positive ferromagnetic (gravity concentration). Froth flotation is moderately used. Attri-
minerals [35]. Ferromagnetic material can be attracted by a low tion scrubbing is often employed as a pre-treatment to improve
intensity magnetic field, while separation of paramagnetic mate- the separation process. Magnetism and electrostatic separators
rial requires a high intensity magnetic field [18]. Low intensity are not often used. In field applications, typical treatment train of
magnetism separation (LIMS) has been used to recover spent physical separation process includes: (1) a preliminary size clas-
munitions debris at military sites [36] or ferrous/metallic debris sification step using mechanical screening to isolate oversized
material containing high heavy metals concentrations in brown- material; (2) a hydroclassification step preceded or followed by
fields [37]. The magnetic separation of heavy metals from the attrition scrubbing to provide suitable particle size range for fur-
soil matrix is based on the fact that metal contaminants are asso- ther treatments; (3) the treatment of the sand fraction by gravity
ciated with the ferromagnetic materials. Rikers et al. [35] showed concentration or froth flotation; (4) the treatment of the fine
that wet high intensity magnetism separation (WHIMS) is suit- fraction; and (5) the management of the generated residuals.
able for removing Cr, Cu, Ni, Pb, and Zn from several soils. If the Many physical separation processes were based on simple
heavy metals are not associated with a ferromagnetic phase, sep- particle size separation because the fine fraction (clay and silt) is
aration is not efficient. When the soil matrix is heterogeneous, often considered as contaminated and the coarse fraction (sand)
as in the case of brownfields, magnetic separation is not signif- is considered as uncontaminated. However, metal contamination
icantly efficient to remove metal contaminants from soils [17]. can be distributed throughout the various particle size fractions
of soils and concentrations can be high in sand fraction, espe-
3.6. Electrostatic separation cially for urban or industrial soils polluted by heterogeneous
waste disposal [46–48]. If metal contamination is of particulate
The use of electrostatic separation for soil remediation nature and is abundant in all particle size fractions, separation
appears limited and is rarely used. One example of an elec- only based on size cannot accomplish a sufficient separation of
trostatic separation application at full-scale is the PMET’s metal contaminants. In this case, the separation based on den-
lead-base paint chip separation and recovery technology sity or floatability must be investigated. The physical separation
[38]. This process uses a final step of electrostatic separation treatment train can require crushing, desliming, dewatering, and
after size classification, ferromagnetic separation, and gravity water treatment. Physical separation can be used as a stand-
separation steps [39]. alone volume reduction process or as pre-treatment prior to metal
recovery (Table 1). In certain cases, Pb and Hg may be recovered The use of high-concentrations chloride salt solutions at low
under a saleable form. In remediation projects of shooting range pH conditions combines the acid leaching action and the
soil, the Pb concentrates were usually sent to smelter for metal formation of metal chloro-complexes to extract metals from
recycling (Table 1). soils. Chelating agents solubilize metals through complexation.
Surfactants target desorption of metals from soil interface.
3.9. Advantages/disadvantages of physical separation The redox manipulation aims to enhance metal solubilization
technologies through a valence change. The choice of the extracting reagent
depends on the metal type, metal concentration, metal frac-
This section provides general comments for the integrated tionation/speciation, and soil characteristics (Table 4). Strong
processes, specially large-scale applications. The advantages acids such as hydrochloric acid (HCl) and chelating agents
and disadvantages for each technology type were specifically such as ethylenediaminetetraacetic acid (EDTA) are commonly
discussed in the preceding paragraphs. Physical separation investigated to extract heavy metals from soils.
presents many advantages: (1) this technology can treat both
organic and metal contaminants in the same treatment system; 4.1. Applicability and limitations of chemical extraction
(2) the volume of soil to be further treated (for metal recovery) or
to be disposed of off-site are considerably reduced; (3) the soil Metal removal efficiency by the chemical extraction pro-
processed can be returned to the site at low cost; (4) the metal cess depends on the soil geochemistry (e.g., soil texture, cation
recovered may be recycled in certain cases (e.g., sent to smelt- exchange capacity, buffering capacity, and organic matter con-
ing facility); (5) the treatment train systems are easily modular tent); metal contamination characteristics (type, concentration,
and some mobile unit systems are available at full-scale for on fractionation, and speciation of metals); dosage and chemistry
site remediation; and (6) the technologies are well established of extracting agent; and processing conditions (solution pH,
in the mineral processing industry and the operational costs are residence time, number of successive extraction steps, mode
usually low. of reagent addition, liquid/solid ratio, etc.) (Table 4). Several
On the large-scale applications, the soil treatment by phys- experimental results of metal removal efficiency according to
ical separation presents some disadvantages: (1) this treatment the leaching methods, the reagent types (EDTA, HCl, and salts
system requires a large equipments and large spaces for soil solutions) and the soil characteristics are reported in Table 5.
treatment; (2) the volume of soils to be treated must be large The speciation (distribution of chemical species) and frac-
to be cost effective (>5000 t for treatment on site); (3) wash- tionation (fractions according to bonding with specific soil
water treatment and off-site disposal of residual solids may be substrates) of metals in soils are important parameters for deter-
required, thus significantly increases the cost [8,20]. mining the metal removal efficiency by chemical treatment.
The metal speciation analysis can be complicated (especially
4. Chemical extraction technologies when the soil is contaminated with a complex mixture of metal
compounds) and the metal fractionation according to soil sub-
Chemical extraction uses an extracting fluid containing a strates is often applied. The partitioning of metals according to
chemical reagent (acids/bases, surfactants, chelating agents, their association with the soil substrates is usually determined
salts, or redox agent) to transfer the metals from the soils into an by the sequential extraction procedure [47,48]. The analytical
aqueous solution. In extractive metallurgy, the chemical extrac- protocols used generally involve five fractions: (F1) exchange-
tion procedures, referred to by the term “hydrometallurgy”, are able, (F2) acid soluble/carbonate bound; (F3) reducible/Fe–Mn
extensively employed for recovery of the metals from ores, bound; (F4) oxidizable/organic matter and sulfide bound; (F5)
concentrates, and recycled or residual materials [49]. In the residual [50] (Table 4). Van Benschoten et al. [51] have studied
soil remediation context, solubility enhancement can be accom- metal partitioning for up to 10 fractions.
plished by leaching solutions in which the metal contaminants The fractions most amenable to metal removal by chemical
are dissolved; or by converting the metal compounds into forms leaching are: (1) exchangeable; (2) associated with carbonates;
that are more soluble (e.g., conversion to soluble metal salts by and (3) associated with reducible Fe–Mn oxides of soils [52]
valence change). In this review, the use of five leaching solu- (Table 4). However, extraction of metal bound to exchangeable
tion types will be separately discussed: (1) acids; (2) salts and and carbonate fractions was faster compared to extraction of
high-concentration chloride solutions; (3) chelating agents; (4) metal bound to Fe–Mn oxides [53,54]. In describing leaching
surfactants; and (5) reducing or oxidizing (redox) agents. with EDTA and HCl, Van Benschoten et al. [51] reported that
Table 4 summarizes the soil types, the treated metals (initial non-detrital Pb (i.e., associated with water soluble, carbonates
concentrations), the leaching methods, the studied factors in and organic) was removed from soils, while Pb bound to the Fe-
leaching process, the overall results and conclusions of 24 oxides, sulfide and residual fractions was not removed. Organi-
laboratory investigations (18 studies involved EDTA; three cally bound metals can be extracted along with the target organic
studies compared EDTA vs. other chelating agents; seven contaminants by the solvent extraction method [4]. The removal
studies compared EDTA vs. acids; six studies involved the efficiency of metals from the distinct fractions depends on the
chloride salt solutions, four studies compared several acids). extracting reagents used (Table 4). For instance, due to dissolu-
Generally, acids rely on ion exchange and dissolution of tion effects, certain acid leaching processes may partially remove
soil components/discrete metal compounds to extract metals. metals from the crystalline lattice [55]. Nevertheless, the metal
16
Table 4
Laboratory investigations of chemical extraction technologies
Soil type Metals (␮g/g) Leaching Reagent Studied factors in leaching process Overall results and conclusions Leachate treatment Ref.
method
Calcareous soils Cd (20–130) Batch EDTA Test with seven different soil samples; Pb RE varied for the different samples – [65]
polluted by mining Pb (500–34,800) successive steps (1–2) with Na4 -EDTA vs. (50–98%). Cd and Zn RE was <50%. Best

and smelting Zn (700–20,200) EDTA dosage (0.2–1 M), i.e.,
Na2 -EDTA; results were obtained with two steps, high
activities in EDTA/ Me molar ratio (1–23); S/L conc. ofNa2 -EDTA (0.25 M, i.e.,
Lavrion, Greece (10–36%); study of EDTA/Ca vs. EDTA/Me EDTA/ Me molar ratio was >20) and low
molar ratio S/L ratio (10%). EDTA may contribute to the
co-dissolution of CaCO3
Calcereous soil from Pb (24,600) Batch EDTA EDTA dosage (0–0.2 M); pH (4–8); Removal of Cu/Cd/Ni/Zn was less effective Nano-filtration for [54]
the battery site, Cd (27) extraction kinetic; extraction mechanism than removal of Pb. RE of Pb was 99% with Pb-EDTA complex
Canada Zn (241) (two-reaction models); MF (6 fractions) high EDTA dosage (0.2 M) and within 12 h recovery (98%)a
Cu (43) of the leaching. Extraction of Pb bound to
Ni (120) carbonates and exchangeable fractions was
faster compared to extraction of Pb bound to
oxides
Artificially Cu (1230) Batch EDTA EDTA/Cu molar ratio (1–12.5); L/S ratio Cu RE = 80–90% within 5 h of the leaching. – [64]
contaminated sandy (5–25); pH (4.8–6.56); extraction time Cu RE strongly depended on L/S ratio and
soil (0–25 h); extraction mechanism of Ca2+ , EDTA/Cu ratio. Best results were obtained
Fe3+ and Cu2+ with L/S = 12.5 and EDTA/Cu = 12.5
Four soils from Pb (1136–4424) Batch/heap EDTA EDTA dosage (0.00375–0.06 M); pH Increasing EDTA conc. did not produce a – [63]
mining and Zn (288–5489) (4.5–9); Successive steps (1–10); proportional gain in RE. Multi-steps using
smelting site in interference of major cations (Ca, Fe) with low EDTA dosage gave best results
Slovenia Pb/Zn-EDTA complexation; laboratory compared to single-step mode. Fe3+
simulation of soil heap leaching interfered more strongly with Pb/Zn
(time = 0–72 h) EDTA-complexation when single step mode
was used. The interference of Ca2+ was less
important
Soil from Pb-smelting Pb (1243) Batch/heap EDTA Small-scale heap leaching; Successive steps Multi-step using low EDTA dosage gave Degradation of EDTA [78]
site in Mezica Zn (1190) (1–6) with EDTA/Pb molar ratio (0.42–6.67) best results compared to single-step mode. by ozone/UV
Valley, Slovenia and EDTA/Zn molar ratio (0.14–2.2); EDTA extracted more Pb than Zn (Zn bound treatment and
extraction time (0–96 h); MF study (six to the residual soil fraction) absorption of metals
fractions)
Four soils (mining Cd (49–380) Batch/column EDTA = 5): EDTA dosage
(1) Batch tests (L/S (1) Batch tests: EDTA extracted the metals – [56]
activity) in UK and Cu (42–1350) (0.01 M); EDTA/ Me ratio for initial/final similarly. (2) column tests: EDTA extracted
France Pb (265–9430) soil; (2) column tests: effect of the mode of the metals differently. The results showed
Zn (1920–30,260) EDTA addition (continuous and pulse that metal removal occurs differently in
mode); EDTA dosage (0.01–0.025 M); (3) batch and column leaching
MF study (five fractions) before and after
treatment

Artificially Pb (1399) Batch EDTA Extraction time (0.5–4 h); EDTA/Pb ratio Optimal conditions for EDTA leaching were: – [77]
contaminated soil Zn (752) and EDTA/Zn ratio (1–2); pH (5–9); Initial extraction time = 2 h; EDTA/Pb ratio = 2 and
Pb and Zn conc. in soil; study of competition pH 7 for Pb; EDTA/Zn ratio = 1 and pH 9 for
between Zn and Pb Zn. Metals RE increased with an increases of
initial metals conc. (with a fixed EDTA/Me
ratio). There is competition between Zn and
Pb under different EDTA dosage. Pb RE was
higher than Zn RE with low EDTA dosage
Artificially Cd (269) Batch EDTA L/S ratio = 20; EDTA dosage Optimum condition for metals RE depends EDTA regeneration [73]
contaminated soil Pb (2510) (0.001–0.01 M), i.e., EDTA/ Me ratio on soil geochemistry and MF. The order of (84%) and metal
Ni (605) (0.8–8); pH (4.7–8); extraction times RE was Cd > Pb > Ni. EDTA appeared phosphates
(15–240 min); tests with fresh EDTA and capable for extracting the Cd/Pb/Ni bound to precipitation
recycled EDTA; MF study (five fractions) the exchangeable, acid soluble, reducible (89–95%)a
and part of the oxidizable fractions
Soil contaminated by Cd (56) Batch EDTA + surfact. Tests with EDTA (0.002 M), The use of surfactants improved EDTA EDTA regeneration [76]
metals and PCB in Cr (436) EDTA + surfactant (anionic and non-anionic) leaching. RE with EDTA + surfactant and metal
Montreal, Canada Cu (2726) with various ultrasonication times (3, 5, 10, (non-anionic) was effective for Pb (73%) and precipitation by
Ni (364) 30 min); tests with fresh and recycled EDTA. moderately effective for Cu (49%), Cd addition of Ca(OH)2
Pb (17,944) Study of Fe, Mg, and Fe removal (36%) and Zn (44%). RE was ineffective for and Mg0 (73–96%)a
Zn (8940) Cr and Ni (mainly associated with residual
soil fraction)
Artificially Cd (603) Batch/column EDTA + red. (1) Batch tests: EDTA (0.01 and 0.1 M) RE depended on the dissolution of – [11]
contaminated soil Cr (1231) and/or reducing agent Na2 S2 O5 (0,1 M); L/S metal–mineral bond, and the dispersion of
Pb (742) ratio (5,12.5,25); pH (3.9–6.3); extraction metal in the washing solution. RE of Cr was
Zn (624) time (2–90 h); (2) column tests: EDTA low compared to RE of Cd, Pb, Zn. The use
(0.01 M) and/or Na2 S2 O5 (0.1 M) of reducing agent improved the EDTA
leaching. L/S ratio had less effect. Column
tests resulted better metal RE rather than
batch tests
17
18
method
Two metal-polluted Cd (197–280) Batch EDTA EDTA (1 M) vs. oxalate (1 M) (time = 24 h); MF was a major factor. EDTA was efficient – [53]
soils from Pb (812–210,000) Oxalate pH (3–10); study of Fe-oxides removal; MF to extract metal associated with non-detrital
Indianapolis, IN Zn (521–2700) (five fractions) and organic fractions. EDTA was less

and Palmerton, PA efficient to extract metals bound to oxide
fraction. Oxalate was efficient to extract
metals associated with oxide fraction
Two urban soils in Cd (1–6) Batch EDTA HCl (0.001 M) vs. EDTA (0.00274 M) Acid washing with low HCl conc. was Anion exchange resin [60]
Montreal, Canada Cu (130–700) HCl (time = 24 h); successive steps (1–12) with ineffective because the soils had high for EDTA–metal
Pb (269–800) EDTA; EDTA dosage (0.00684–0.0274 M); buffering capacity. EDTA was more complex recovery
Zn (360–2650) pH (4 and 8.5) effective. RE depended on EDTA dosage (90–99%)a
(best result with high conc.). High silt/clay
content affected metal RE
Artificially Pb (5000) Column EDTA Tests with 10 Pb-compounds (adsorbed Best results of acid leaching is obtained at – [12]
contaminated soil HNO3 Pb2+ , carbonate, sulfate, oxide, dioxide, pH 2. RE of adsorbed, carbonate, sulfate,
sulfide, elemental forms of Pb, Pb-compound oxide forms was effective and RE of sulfide,
from paint); tests with HNO3 at various pH dioxide, Pb from paint, and elemental forms
(1–6); tests with EDTA (0.0003 and 0.001 M, was ineffective. RE with EDTA (EDTA/Pb
i.e., EDTA/Pb ratio = 1 and 3) at pH 6 ratio = 3) was effective for adsorbed,
carbonate, sulfate, oxide, dioxide forms,
while was ineffective for other tested forms
of Pb
Seven Pb (1394–11,933) Batch EDTA Acids vs. EDTA (0.01 M) at pH (1,2,3); HCl was effective for Pb RE at low pH. RE – [51]
Pb-contaminated HCL temperature (25, 50 ◦ C); L/S ratio (5, 10, and kinetic mainly depended on pH. The use
sandy soils in the HCLO4 H2 SO4 20); the use of reducing agent NH2 OH–HCl of EDTA (0.1 M) improved Pb RE at pH 3
US Red. (0.4 M); extraction kinetic; MF study (10 and not at pH 1. L/S ratio and temperature
fractions) had less effect. Pb not removed by
acids/EDTA leaching was associated with
Fe-oxides, sulfide and residual. The use of
reducing agent improved removal of Pb
bound to Fe-oxides
Soil polluted by Pb (65,200) Batch EDTA HCl (0.1–1 M) vs. chelatants The order of Pb RE: Metal hydroxides [55]
battery recycling ADA (0.0225–0.075 M); extraction time (1–5 h); EDTA > ADA > PDA > HCl. The order of Cd precipitation by
and Pb-smelting PDA successive steps (1–3); MF study (five RE: HCl > ADA ≈ PDA ≈ EDTA. RE addition of Ca2+ and
operation, IN HCL fractions) depended on EDTA dosage. Three-step NaOH (72–93%)a
leaching (1 h) improved RE. Cd was removed
from the crystalline lattice by HCl leaching
Soil polluted with As (7540) Batch EDTA Tests with HCl (1, 2, 3, 6 M), H2 SO4 (6 M), RE highly depended on the metal forms. HCl – [67]
slags and sulfur Cu (4100) HCl HNO3 (6 M), Na2 -EDTA (0.1 M); study of resulted best RE compared to other acids. RE

compounds in Pb (64,195) HNO3 extraction kinetic for HCl (1 M) and was improved with increasing HCL dosage
Lavrion, Greece Zn (5590) H2 SO4 Na2 -EDTA (0.1 M) leaching; mineral and at long extraction time (4 h). EDTA was
analysis by XRD of metal compounds more effective at low leaching time (<1 h).
HCl 1 M (4 h leaching) presented better RE
compared to EDTA 0.1 M (1 h leaching).
HCL 1 M strongly affected soil matrix. RE
of As was ineffective with EDTA
Artificially Cd (49) Batch EDTA Single-step at pH 7; extraction time The order of Pb RE: – [74]
contaminated soil Pb (294) NTA (15–300 min); tests with EDTA/NTA/DTPA EDTA ≈ NTA ≈ DTPA > HNO3 > CaCl2 .
Cr (270) DTPA (0.001–0.01 M); comparison of The order of Cd RE:
HNO3 EDTA/NTA/DTPA (0.005 M), HNO3 (pH EDTA > NTA > DTPA > HNO3 > CaCl2 .
CaCl2 2–3), and CaCl2 (0.5 M); MF study (five Chelating agents were ineffective in
fractions) removing Cr (mainly associated with
oxidizable and residual fraction)
Soil from mining area As (41) Batch HCl Tests with HCl, H3 PO4 , H2 SO4 at pH 2–3; Acids with oxyanions (H3 PO4 , H2 SO4 ) was – [57]
located in Korea Ni (88) H3 PO4 study of RE vs. particle size fractions effective for removing As and Zn. HCl was
Zn (335) H2 SO4 (0.841–2, 0.420–0.250, <0.074 mm); less effective in As removal. Acid leaching
extraction time (10 to 25 min) and MF (four of Ni was less efficient (residual fraction).
fractions) Acid leaching caused a loss of OM (50%)
and an increase of acidity (7.6–3.3) of the
treated soil
Two contaminated Cd (4) Batch HCl + CaCl2 Study of the relation of soil suspension pH The use of CaCl2 increased RE in diluted – [66]
rice soils in Taiwan Cr (720) with the amount of H+ added and the loss of HCl (<0.01 M) for Cd removal. Fe–Al oxides
Cu (800) H+ from solution; Study of the dissolution of are attacked by HCl with dosage >0.01 M
Ni (850) Fe and Al oxides by HCl; Effect of CaCl2
Pb (1849) dosage (0–0.1 M) and HCl dosage
Zn (1222) (0.001–0.01 M) in RE of Cd with
HCL + CaCl2 solution at various pH (1–7)
19
20
method
Three artificially Pb (995–1078) Batch HCl + CaCl2 Three soil types: kaolinitic, smectitic and The successive batch washing with HCL – [62]
contaminated soils allophonic soil; successive steps (1–10) (1 M) + CaCl2 (0.1 M) was effective in
using HCl (1 M) followed by CaCl2 (0.1 M) removing Pb. RE depended on soil
washing; study of Pb bioaccessibility after properties (buffering capacity, CEC, humic
the soil washing; MF study (three fractions) substance content, and clay mineral content)
Two soils from Pb (14,400–67,400) Batch NaCl Tests with seven chloride solution types Best results (RE = 97%) were obtained with – [69]
abandoned HCl NaCl, CaCl2 , HCl, MgCl2 , NH4 Cl, KCl, successive two-step extraction (L/S = 7,

Pb-battery EDTA LiCl (Cl− = 4.3 M); successive steps (1–6, time = 1 h) using acidified (pH 4) NaCl
recycling sites, TX time = 30 min) using HCl (0.3 M) + NaCl solution (4.3 M to saturated 6 M). Kinetic
and FA (4.3 M); L/S ratio (5–50); tests with HCl study suggested that Pb removal mechanism
(0.2 M) + NaCl (4.3 M) vs. EDTA (EDTA/Pb is composed of three stages: (1) extraction of
ratio: 4.6–40) and pH (2–10); tests with HCl free-Pb precipitates (quick process: <1 min);
(0.1–4.3 M) vs. acidified NaCl (4.3 M) (2) cation exchange of Pb located on soil
solutions; mineral analysis (Pb species) by surface (30 s to 5 min); (3) removal of Pb
XRD; kinetic and mechanism extraction located within soil structure (slow process
Pb after 5 min)
Soil from Pb (2730) Batch NaCl + HCl NaCl dosage (0–6 M); pH (2–4); soil pulp Pb RE (65–75%) was more effective with Electrochemical [123]
Pointe-aux-Lievres, density (5–30%); extraction times (0–1 h) high Cl− conc. (5.5 M), pH 2 and at 30% soil reduction/coagulation
Canada pulp density. Pb RE was independent of acid for Pb recovery
type, but depended on the pH (best result at (95%)a
low pH)
Calcereous soil from Pb (2730) Batch NaCl + HCl NaCl (8 M); successive steps (1–6); study of Six steps with NaCl (8 M) was effective Regeneration of Cl− [71]
the battery site in Ca removal; extraction kinetic; MF study (RE = 93%); RE increases with extraction and metal
St-Jean-sur- (five fractions) time (RE > 80% after 90 h). Extraction precipitation with
Richelieu, appeared to be controlled by a first-order rate addition of NaCO3 ,
Canada (Pb extraction from carbonate and CaCO3 ; or lime
exchangeable soil fractions) (90–98%)a
Fine-grained soil from Cd (34) Column/pile HCl + CaCl2 Column tests: three successive steps with Chloride solution with CaCl2 + HCl was Regeneration of Cl− [61]
Montevecchio, Italy Zn (3600) HCl (0.2 M) + CaCl2 (1.9 M) at pH < 0.5 effective in metal removing from soil (poor and metal
Pb (16,000) followed by seven successive steps with in calcite). The treated soil matrix was precipitation with
CaCl2 (2 M) at pH 6.5. Study of Mn, Fe, Al, sensibly unaffected (total weight CaCl2 at pH 9–12
Mg removal; particle size distribution vs. loss = 3.5%; initial pH 5.6; final pH 5.15) (70–94%)b
metal concentration before and after
treatment

EDTA: ethylenediaminetetraacetatic acid; ADA: N-2acetamidoiminodiacetatic acid; PDA: pyridine-2,6-dicarboxylic acid; NTA: nitrilotriacetatic acid; DTPA: diethylenetriaminepentaacetic acid; M: mol/L; RE:
removal efficiency; L/S: liquid/solid; MF: metal fractionation; Surfact.: surfactants; Red.: reducing agent; Me: molar sum of metals; OM: organic matter; CEC: cation exchange capacity.
a Removal efficiency of the dissolved metals from the leaching solution (varies according to the metal types or the processing conditions).
b Removal efficiency for the whole process (leaching + precipitation).
Table 5
Examples of experimental results in metal removal efficiency according to the leaching method and the soil characteristics
Leaching method Reagents (mol/L) Soil description Soil pH CECa (cmol/kg) Textureb OMc (%) Ca (%) Metal Conc. (␮g/g) REd (%) Ref.
S/S/C (%)
Batch 1 h, 3 steps, pH 4.5 (chelation) EDTA (0.0225) Soil contaminated by 7.4 14.3 68/17/15 8.2 – Pb 65,200 56 [55]
smelting and battery Cd 52 37
recycling operations
Batch 24 h, 12 steps, pH 7–8 (chelation) EDTA (0.00275) Urban soil contaminated by 8.03 12.8 69/24/7 2.8e 18 Cd 6.3 53 [60]
industrial activity Cu 700 49
Pb 800 76

Zn 2,650 84
Batch 1 h, 1 step, pH 6 (chelation) EDTA (0.1) Soil contaminated with slags 7.0 – – – 6.2 As 7,540 13 [67]
and metallurgical wastes Cu 4,100 41
Pb 64,195 44
Zn 55,900 38
Batch 22 h, 2 steps (chelation) EDTA (0.25) Calcareous soil (S1) 8.3 – 42% <63 ␮m – 11.6 As 1,200 8 [65]
contaminated by mining and Cd 100 37
smelting activities Pb 32,000 71
Zn 15,000 49
Batch 1 h, 2 steps, pH 4 (acid leaching + Cl− HCl + NaCl (4.3) Soil from battery recycling 7.0 9.5 51/36/13 3e 30 Pb 67,400 >97 [69]
complexation) site
Batch 1 h, 1 step, pH 4 (acid leaching + Cl− HCl + NaCl (5.5) Fine-grained fraction of – – 100% <20 ␮m – 5.7 Pb 2,730 65 [123]
complexation) industrial soil
Column: three steps with HCl HCL + CaCl2 Fine-grained soil 5.6 – 43/29/28f – 0.7 Cd 34 75–80 [61]
(0.2 M) + CaCl2 (1.9 M) at pH < 1 contaminated by mining Zn 3,600 75–80
followed by 7 steps with CaCl2 (2 M) at activities Pb 16,000 90–95
pH 6.5 (acid leaching + Cl−
complexation + ion exchange with Ca2+ )
Batch 1 h, three steps, pH 4.5 (acid leaching) HCL (1) Soil contaminated by 7.4 14.3 68/17/15 8.2 – Pb 65,200 35 [55]
smelting and battery Cd 52 56
recycling operations
Batch 1 h, one step, pH 4 (acid leaching) HCl (2) Soil contaminated with slags 7.0 – – – 6.2 As 7,540 92 [67]
and metallurgical wastes Cu 4,100 42
Pb 64,195 57
Zn 55,900 67
a Cation exchange capacity.
b Sand/silt/clay.
c Organic matter content.
d Removal efficiency.
e Organic carbon content (%).
f The soil was agglomerated before the soil leaching treatment.
21
fractionation data does not always clearly explain metal removal (H+ ) added can react with soil surface sites (layer silicate min-
efficiency because removal efficiency also depends on other erals and/or surface functional groups including, e.g., Al-OH,
factors such as metal concentration and soil geochemistry [56]. Fe-OH, and COOH groups) and enhance desorption of metal
In addition, removal efficiency depends on the metal type cations, which are transferred into the washing fluid [62]. Kuo
to be extracted and the valence of the element. Generally, the et al. [66] showed that acid leaching with 0.1 M HCl contributes
extractability of most cationic heavy metals (e.g., Cd, Cu, Pb, to a significant dissolution of Fe and Al oxide surfaces, and
and Zn) increases when the solution pH decreases. Indeed, at low phyllosilicates. At pH < 2, this dissolution process replaces ion
pH, adsorption onto soil of the cationic heavy metals decreases exchange in metal extraction [66].
and the dissolution of metal compounds increases. On the other Acid leaching may involve strong mineral acid such as
hand, the solubility of oxyanions of the metalloid As increases hydrochloric (HCl), sulfuric (H2 SO4 ), nitric (HNO3 ), phos-
when the solution pH increases [57]. In addition, the adsorp- phoric (H3 PO4 ) or weak organic acid such as acetic acid.
tion of chromium Cr(VI) anionic species is enhanced at low While, acetic acid has been used in field demonstrations at Fort
pH [58]. Hence, the simultaneous treatment of both anionic and Polk in Leesville, LO (Table 1, project #23), the nuisance of
cationic metal species that have dissimilar chemical behavior in odors and its relative low strength limits its efficiency [21].
aqueous solution, can be ineffective. Furthermore, Isoyama and The removal efficiency of different mineral acid types strongly
Wada [58] reported that HCl leaching was relatively efficient depends on the metal type, the soil geochemistry, and the
for chromate (CrO4 2− ) removal from non-allophanic soils but it reagent concentrations (Table 4). Moutsatsou et al. [67] showed
was inefficient for removal of trivalent chromium Cr3+ , particu- that the extraction of metals (As, Cu, Pb, and Zn) from soils,
larly from soils having high cation exchange capacity (CEC) and highly contaminated by metallurgical materials, was more
organic matter content (due to complexation by humic substance effective with HCl compared to H2 SO4 and HNO3 . On the
and adsorption via cation exchange reactions). other hand, Ko et al. [45] showed that: (1) the extraction of Zn
If metal is not under an adsorbed form, the removal efficiency and Ni (cationic) was similar in the use of HCl, H2 SO4 and
depends on solubility of metal compounds in the washing fluid, H3 PO4 ; (2) the extraction rate of As (anionic) was higher for
which are governed by the solubility product (Ks.p.) values. the use of H2 SO4 and H3 PO4 compared to HCl. Unlike HCl,
The treatment of particulate forms of metals is more difficult to the use of H2 SO4 or H3 PO4 acids, which involve competitive
achieve compared to the adsorbed ionic forms [59]. oxyanions (PO4 3− or SO4 2− ), may decrease the re-adsorption
Factors that may limit the applicability and effectiveness of of As anionic species on reactive surfaces of soil [57].
the chemical process include: (1) high clay/silt content; (2) Many experimental and field test results have shown the effi-
high humic content; (3) high content of Fe and Ca element; ciency of the HCl leaching process for extracting heavy metals
(4) high calcite content or high buffering capacity; (5) simulta- from non-calcareous soils. HCl is often used for chemical leach-
neous contamination of both cationic or anionic heavy metals; ing at full-scale (Table 1). The co-dissolution of soil components
(6) high heterogeneity of soil; and (7) metals associated with by acid leaching is a critical parameter from an environmental
residual soil fraction, imbedded in the mineral lattices, or dis- and an economic point of view. Acid leaching strongly affects
crete particle forms. The fine-grained soils may require longer soil structure and causes important losses (up to 50%) of the soil
contact times and may reduce chemical extraction efficiency mineral substances [61] and organic matter [57]. Co-dissolution
[60,61]. Nevertheless, Table 5 reports several leaching processes of the soil matrix increases the consumption of acid reagent and
that have treated soils having a high clay/silt content (>50%). the complexity of the wastewater treatment [61]. Furthermore,
High humic content can inhibit metal extraction because COOH acid leaching causes a high increase in acidity of the treated soil
groups (adsorption sites) on humic substances have high affinity [57]. Acid leaching may be ineffective for soils that have a high
for heavy metals [62]. The corresponding cations of major ele- buffering capacity such as calcareous soils [60]. Although acid
ment Fe and Ca may interfere with chelating process [63–65]. leaching is efficient in extracting metals from the soils, its large-
High calcite content or high buffering capacity may decrease the scale application has numerous disadvantages: (1) strong acids
acid leaching efficiency [60]. High heterogeneity of soils can may destroy the basic nature and the soil structure, thus affect-
affect formulations of extracting fluid and may require multiple ing soil microbiology and fertility; (2) wastewater and processed
process steps. soils need to be neutralized; (3) neutralization of wastewater
creates enormous amount of new toxic residues; (4) disposal of
4.2. Acid extraction solid/liquid residues and processed soil may be problematic; and
(5) cost markedly increases with wastewater processing and soil
Acid extraction is a proven technology to treat soils, neutralization.
sediments, and sludges contaminated by metals and commercial-
scale units are in operation [4]. The pH of the washing fluid plays 4.3. Salt solutions and high-concentration chloride
a significant role in the extractability of heavy metals from soils. solutions
Several mechanisms contribute to the extraction of metals from
soil using an acid solution: (1) desorption of metal cations via The use of diluted acid solutions containing chloride salts
ion exchange; (2) dissolution of metal compounds; and (3) dis- (such as CaCl2 ) may be an effective alternative to the acid
solution of soil mineral components (e.g., Fe–Mn oxides) which leaching at high concentrations. The processed soil is practically
may contain metal contaminants [61,66]. At low pH, the protons unaffected by the saline leaching with diluted acid. Indeed, the
co-dissolution of the soil matrix is less significant and the pH reagents used should be cost effective; (5) metal recovery should
of the final soil is not significantly lower compared to initial be cost effective [11,52,56,63]. The main advantage of the use
soil [61]. Kuo et al. [66] reported that the removal efficiency of chelating agent (such as EDTA) compared to strong acids
of Cd from rice soils with a 0.001 M HCl and 0.1 M NaCl2 (such as HCl) is that chelating agents cause less destruction of
solution was similar to the removal efficiency obtained with the soil structure. However, EDTA presents two main disad-
the acid leaching using a 0.01 M HCl solution. The increase vantages compared to HCl: (1) the chemical products are more
in the removal of cationic metals (such as Pb2+ and Cd2+ ) expensive; (2) EDTA may pose a serious ecological threat if it is
with CaCl2 addition in the acid leaching results from two not recycled or destroyed in the washing process because EDTA
processes: (1) ion exchange of Ca2+ with Pb2+ /Cd2+ on the has a low biodegradability degree (resistant to chemical and bio-
reactive surface sites of soil matrix; (2) formation of stable and logical degradation) and has the potential for remobilizing heavy
soluble metal chloro-complexes with chloride ions Cl− (e.g., metals in the environment [73,74].
Cd2+ + yCl− ⇔ CdCly 2−y ) [61,66]. Isoyama and Wada [62] Many chelating agents have been tested and compared
reported that a second washing step with 0.1 M CaCl2 (after (Table 4). Peters [52] showed that EDTA, nitrilotriacetic acid
a 1 M HCl leaching step) was used to prevent a re-adsorption (NTA) and acid citric were effective, while other chelating agents
of the extracted Pb on cation exchange sites of silicate layer such as gluconate, oxalate, Citranox, and ammonium acetate
minerals having a permanent negative charge. The destruction were ineffective in removing Cu, Pb, and Zn from Aberdeen
of a soil’s physico-chemistry and microbiology is minimized Proving Ground soils. Carboxilic acids such as EDTA and NTA
by using successive leaching steps with a solution of CaCl2 at are chelating agents hydrolytically stable at high temperature
low concentrations (0.1 M) and slightly acidified [66,68]. and pH levels [75]. However, NTA is not recommended for use
Several researchers investigated the use of chloride salt in soil remediation because it is hazardous for human health
solutions at high concentrations (>1 M) and acidic conditions [74]. Moreover, EDTA forms more stable complexes with most
for removing high Pb concentrations from soils (Table 4). of the heavy metals when compared to NTA [75].
The chloride ions Cl− at high concentrations form soluble EDTA is recognized as the most effective synthetic chelating
chloro-complexes with Pb2+ such as PbCl3− and PbCl4 2− [69]. agent to remove heavy metal (especially Pb, Cd, Cu, and Zn)
However, Eh and pH parameters must be monitored for obtain- from soils because of: (1) EDTA has a strong chelating abil-
ing the optimum thermodynamic conditions and preventing the ity for cationic heavy metals; (2) EDTA leaching process can
formation of an insoluble compound PbCl2 [70]. In high ionic treat a broad range of soil types; and (3) EDTA is recoverable
strength solutions, the sodium cation Na+ (of the concentrated and reusable (low biodegradability degree) [56,64,73,76]. The
NaCl solutions) may play a significant role in Pb extraction via EDTA leaching process has been well demonstrated through
ion exchange [69]. The acidified NaCl solutions were more effi- many laboratory studies to extract metal cations bound on soil
cient (or comparable) than conventional extractants (EDTA and particles (Table 4). On the other hand, EDTA appears ineffective
HCl) for removing Pb from clayey or fine-grained soils (Table 5). for extracting anionic metal As (Table 5).
Unlike the leaching with concentrated HCl, the concentrated Metal removal efficiency with EDTA highly depends on
NaCl solution is effective in removing Pb from calcareous soils soil characteristics and metal fractionation (Table 6). In gen-
without a high Ca extraction [71]. The leaching with an acidi- eral, EDTA is effective in removing metal cations bound to
fied 2 M NaCl solution (enhanced with an oxidant agent) has exchangeable, carbonate and organic fraction, while EDTA is
been tested at pilot-scale for the remediation of highly Pb- less efficient in extracting metals bounds to reducible/Fe–Mn
contaminated soils (Table 1, projects #29 and 30). The free oxide fraction [11,54,65]. Elliott and Shastri [53] have demon-
chloride ions are often recycled and the extracted metals are strated that oxalate was more effective than EDTA to remove the
recovered by: (1) chemical precipitation with addition of sul- metals associated with Fe–Mn oxides of soil (attacks the hydrous
fide, hydroxide, carbonate compounds or (2) electrochemical oxides). The metals bound to residual fraction are not extracted
coagulation/reduction (Table 4). Meunier et al. [72] showed that by EDTA (Table 6). Unlike acid leaching (low concentration),
the electrochemical coagulation treatment was more effective the EDTA complexing process may be efficient in treating cal-
than chemical precipitation for removing the dissolved metals careous soils [54,60]. However, EDTA may contribute to the
from acidic and saline leachate; however its cost is higher. co-dissolution of calcite, thus reducing removal efficiency of
metals [65].
4.4. Chelant extraction The low selectivity of EDTA causes high consumption of the
reagent due to the potential chelation with other cations, such
Since chelating agents have the ability to form stable metal as Ca2+ and Fe3+ , dissolved in the washing solution [64]. Com-
complexes, their use offers a promising approach for the extrac- petition in the metal–EDTA system is controlled by dissolved
tion of metals from contaminated soils. There are five major metal concentrations, reaction kinetics and certain soil parame-
factors in the selection of chelating agents for metal extraction ters. Factors affecting the stability of metal chelate include: (1)
from soils: (1) chelating agents should be able to form highly the size and number of rings; (2) ligand substituents on the rings;
stable complexes over a wide pH range; (2) the metal com- (3) the nature of the metal; (4) pH of the washing solution; and
plexes that are formed should be nonadsorbable on soil surfaces; (5) high content of calcite (CaCO3 ) in the soil [75]. The con-
(3) the chelating agents should have a low biodegradability if centration of Fe3+ in the washing solution is a crucial parameter
the reagents is to be recycled for reuse in the process; (4) the for the stability of metal–EDTA complexes because Fe3+ may
24
Table 6
Examples of metal removal efficiency with EDTA according to the soil characteristics and metal fractionation
Leaching method (EDTA Soil description Soil characterization Metal Conc. (␮g/g) Metal fractionationa (%) REb (%) Ref.
dosage)

Soil pH CECc (cmol/kg) Sand/Silt/Clay OMd (%) Ca (%) F1 F2 F3 F4 F5
(%)
Batch leaching 24 h 1 Soil from battery site, 7.6 – – 0.7 6 Cd 27 10e 26 23 22 20 <10 [54]
step, pH 4 (0.2 mol/L) St-Jean-sur-Richelieu, Pb 24,600 2e 47 43 5 2 98
Canada Zn 241 2e 12 48 21 17 58
Batch leaching 30 min, 1 Soil from storage facility, 7.5 9 52/33/16 12.5 – Cd 56 <1 36 9 7 48 35 [76]
step (0.02 mol/L) Montreal, Canada .5 Pb 17,944 <1 60 19 2 18 66
Zn 8940 <1 40 50 <1 9 42
Ni 364 4 8 21 8 59 15
Heap leaching, 24 h, 4 Soil from mining site, 7.1 23 56/32/11 9.3 – Pb 1243 <1e 24 <1 56 8 80 [78]
steps (0.04 mol/kg) Mezica Valley, Slovenia .3 Zn 1190 <1e 8 2 15 61 19
Batch leaching, 30 min, 1 Artificially contaminated 4.7 52 42/33f 2.4 0.1 Cd 269 80 7 11 2 0 >95 [73]
step, pH 7 soil Pb 2510 39 38 19 4 0 >95
(0.002 mol/L) Ni 605 23 7 4 61 4 40
Batch leaching, 24 h, 1 Soil from smelter site, – – – – – Cd 280 26 12 22 38 2 53 [53]
step, pH 6 (1 mol/L) Palmerton, PA Pb 812 17 7 44 26 6 <10
Zn 2700 20 8 38 6 28 28
a F1 = exchangeable, F2 = acid soluble/carbonate bound, F3 = reducible/Fe–Mn oxides bound, F4 = oxidizable/organic matter bound, F5 = residual.
b Removal efficiency.
c Cation exchange capacity.
d Organic matter content.
e Water soluble + exchangeable fractions.
f Sand/silt + clay.
form more stable complexes with EDTA (log K = 26.5 at 25 ◦ C metals while acidic surfactant could be employed for extracting
and ionic strength = 0.01) compared to the most heavy metals the metals bound to carbonate and oxide. Several laboratory
such as Cu (log K = 19.7), Pb (19), Zn (17.5), Cd (17.4) [56,63]. studies showed that cationic forms of metals can be extracted
The complexation interference of Ca2+ appears less problematic from contaminated soils and sediments by anionic biosurfactant
(thermodynamically) because Ca2+ forms much less stable com- solutions [80–83]. However, the metal extraction by biosurfac-
plexes with EDTA (log K = 10.65) than Cd, Cu, Pb, and Zn [63]. tants has not yet been performed for large-scale remediation
On the other hand, a recent study [64] showed that Ca2+ is the projects [84].
main competitive cation because CaCO3 is strongly dissolved
in the EDTA leaching solution at pH 4–5, thus concentrations of 4.6. Reducing and oxidizing agents
Ca2+ in the leaching solution is very high compared to the tar-
geted heavy metal for the chelation with EDTA. Furthermore, Reducing and oxidizing agents provide yet another option
complexation competition between heavy metals (such as Zn vs. to enhance solubilization of metals since chemical oxida-
Pb) may occur in leaching process [77]. tion/reduction can convert metals to more soluble forms.
Metal extraction also depends on the combination of many USBOM and USEPA have conducted laboratory research on Pb
parameters such as EDTA/metal molar ratio, leaching method extraction involving redox manipulations and valence changes
(batch vs. column/pile leaching), mode of reagent addition (sin- to promote solubilization and recovery of various Pb compounds
gle step vs. successive extraction steps with low reagent dosage), from synthetic contaminated soils [75]. Some laboratory studies
solution pH, liquid/solid ratio, and extraction time (Table 4). showed that the addition of reducing agents can enhance metal
Multiple-step procedures with a low EDTA dosage gave best mobilization by EDTA [11,51,52]. The use of reducing agents
results compared to the single-step mode with a high dosage contributes to the dissolution of Fe–Mn oxides, thus enhancing
[78]. Leaching with EDTA is usually performed at pH 4–8 metal removal bound to Fe–Mn fraction in the EDTA leaching
(Tables 4 and 6). At low pH values, the EDTA–metal complexes process [51].
can be re-adsorbed on soil surface sites [74]. Several oxidant agents are also used to enhance the removal
EDTA regeneration is a crucial parameter to the leaching pro- of metals. Lahoda and Grant [85] proposed the use of an oxi-
cess in order to avoid the release of EDTA into the environment. dizing agent to enhance the solubilization of metals from fine
EDTA must be recycled in order to keep treatment costs at a rea- particles into a soil washing process comprising particle sepa-
sonable level [76]. Several procedures have been proposed for ration, metal solubilization, and metal precipitation. Lin et al.
EDTA regeneration (or degradation) and the removal of the met- [70] used sodium hypochlorite (NaClO) as an oxidizer agent
als from the leaching solution: (1) metal precipitation and EDTA in the chloride-based leaching process (2 M NaCl at pH 2) to
regeneration via addition of the chemical agents; (2) electro- extract metallic Pb-particles (smaller than 0.15 mm) and other
chemical procedures; (3) ion exchange resin; (4) nano-filtration; Pb-species from highly contaminated soils (washing results are
(5) degradation of EDTA by oxidation and metal recovery by reported in Table 1, projects #29 and 30). Reddy and Chintham-
absorption (Table 4). For instance, Lim et al. [73] have proposed reddy [86] reported that complete removal of Cr from clayey
a protocol of regeneration and metal-precipitation using three soils (artificially contaminated) was achieved with the leach-
steps: (1) metal substitution with Fe3+ to form Fe-EDTA + Me2+ ; ing process using a 0.1 M potassium permanganate (KMnO4 )
(2) metal precipitation with Na2 HPO4 to form metal phosphate; solution.
and (3) Fe precipitation and EDTA regeneration with NaOH
addition to form Na2 -EDTA + Fe(OH)3 . With this process, the 4.7. Integrated process train of chemical extraction
metal recovery was 85%, 89%, and 90% of the extracted Pb, Cd,
and Ni, respectively. Reused EDTA was slightly less efficient On large-scale operations, leaching methods are classified
compared to fresh EDTA in metal removal [73]. into two main classes: (1) percolation leaching such as heap/pile
leaching or vat leaching; (2) agitated leaching based on batch
4.5. Surfactant-enhanced solubilization step or continuous procedure [49]. In the heap leaching process,
soil is piled in a heap and the leach solution is sprayed over the
Although the use of surfactants is more suitable for the treat- top of the heap, and allowed to percolate downward through the
ment of organic contaminants, the removal of metals from soil heap [49]. The agitated leaching method is performed under
by surfactants is also an interesting chemical procedure to be turbulent flow conditions. For soil treatment at commercial-
investigated. Recently, the use of surfactants has been studied scale, heap/pile leaching appears more cost effective [61,63,78];
to enhance the EDTA leaching process for metals mobiliza- however the extraction processes can be slow and metal con-
tion from soils [76]. The surfactant addition in washing solution centrations must be relatively high. Agitation leaching is an
aims at assisting desorption or/and dispersion of contaminants interesting method for soil treatment because it can allow aggres-
from soils. When the metals are closely associated with organic sive and effective extraction of the metal contaminants from soils
contaminants, washing by surfactants can be more effective. [44]. The column washing tests resulted better metal removal
Association between metal and soil substrates, and acidic or efficiency rather than batch tests [11,78]. Abumaizar and Smith
basic conditions are important parameters for soil washing suc- [11] reported that the continuous flow in the column promoted
cess with surfactants. Mulligan et al. [79] indicate that a caustic the flushing of the reaction reagent/metal complex and mini-
surfactant could be used for removing the organically associated mized the re-adsorption of complex on the soil surface.
After dissolution of the metal compounds, it is necessary to cal extraction of this concentrated fraction to dissolve the metals
separate the leaching solution from the residual solid phase of (Table 1, projects #17–27, 29, 30, and 33). For example, a com-
soil. The resulting solution containing metals can be treated by bination of the BESCORP physical separation technology and
various aqueous processes such as precipitation, sedimentation, the COGNIS-Terramet Pb extraction process has been efficient
complexation, electrochemical techniques, liquid ion exchange, at Superfund site in New Brighton, MN (Table 1, project #20).
resin ion exchange, or membrane technologies to recover met- In this case, the sand fraction is treated by density separation
als (Table 4). Solvent extraction techniques make it possible (jig), while fine fractions are treated by chemical leaching. The
to selectively transfer certain ionic metal species present in Pb removal efficiency for the fine fractions ranged from 65% to
an aqueous washing solution to an organic liquid phase if the 77%. Lead concentrates were delivered to a Pb smelting facility.
extracted metal compounds are preferentially soluble in the Many soil washing processes are based on simple particle size
organic phase [49]. The washed soil is usually rinsed with water separation using hydroclassification and attrition scrubbing with
to remove the residual extracting agents from the soil. Depending water-based fluid. Particle size separation is often used before
on the soil characteristics and reagents used, the resulting ‘clean’ chemical extraction, with the assumption that the fines contain
soil fraction can be returned to the site or must be disposed most of the metal contamination. Since metal concentrations are
off-site. usually high in the fine fraction, the practice of direct disposal is
inappropriate. Chemical extraction may be used for the decon-
4.8. Advantages/disadvantages of chemical extraction tamination of the fine fractions and can allow metals recovery
technologies in a saleable form or concentrated form.
Soil washing systems may involve other combination types
The advantages/disadvantages significantly diverge accord- depending on the soil matrix characteristics, metal speciation
ing to the reagents and extraction method used. Specific and type of metal to be treated. The combination of PS/CE can
comments were discussed in the preceding sections. Gener- be reversed (e.g., chemical leaching followed by wet screening)
ally, the principals advantages of chemical procedures compared or may involve a simultaneous process of PS/CE methods. For
to physical separation are: (1) the sorbed metal forms can be instance, certain processes use attrition scrubbing chemically
treated; (2) certain metal compounds can be dissolved; (3) enhanced with acids, surfactants or chelating agents followed by
the fine-grained soils may be treated in certain cases; (4) the a wet screening/hydrocycloning stage to separate the fine parti-
extracted metals may be easily recovered by a wide variety cles/washing solution (containing the pollutants) from the clean
of methods. Chemically enhanced soil washing can become fraction (Table 1, projects #28, 31, and 32). The grinding and
attractive if the chemical reagents are recycled, detoxified or crushing process of soil particles may be a pre-treatment option
not hazardous. for enhancing the efficiency of the chemical extraction treat-
The large-scale application of chemical extraction processes ment. The use of ultrasounds may accelerate the surface cleaning
presents numerous disadvantages: (1) the use of chemical agents of soil particle and improve the leaching of metals [87–89].
significantly increase processing costs; (2) the processed soil The influence of ultrasounds contributes through several mecha-
may be inappropriate for revegetation and on-site disposal nisms (not fully understood) such as the micro-fragmentation of
because the physico-chemical and microbiological properties particles, and disturbance of solid/liquid interface by cavitation
have been affected; (3) the presence of toxic chemical agents [87].
in the final soil or the residual sludge may be problematic for The soil washing treatments aim at completely decontami-
disposal; (4) the presence of certain chemical agents in the wash nating the site by removing metals from the soil matrix. Table 1
fluid can complicate water recycling and treatment, thus increas- reports the treatment efficiency for total metal concentrations.
ing cost of the overall process; and (5) the treatment of sludges However, the aspect of reduction in metal leachability to below
rich in metal can be difficult. The chemical agents involved standard TCLP is also important in the quality results of soil
may cause other environmental problems. For instance, the soil washing. The ideal goal of an extraction strategy is to recover
treated by EDTA leaching may potentially be hazardous to reuse metals for reuse and resale, however, metal recovery is often
if a part of the chelating agent remains in the soil. Wastewaster not practicable for projects that lack economic viability or
treatment may produce large amounts of toxic sludges that must technical feasibility for the extraction and recovery processes.
be carefully managed. The generated toxic sludges (containing metals), which are
recalcitrant to a metal recovery treatment, may require a stabi-
5. Combination of physical separation and chemical lization/solidification process prior to disposal. In many cases,
extraction soil washing is used to reduce the metal concentrations to an
acceptable level or to considerably reduce the volume of con-
Table 1 reports 18 processes combining physical and chemi- taminated soil.
cal procedures. The complementary use of the physical particle
separation and chemical leaching procedures provides a very 6. Status of soil washing technology
useful tool for decontaminating the soils affected with metals.
The typical combination uses physical separation (primarily by This section provides a discussion about the use, at large
size, density or floatability properties) to concentrate particulate scale, of soil washing for the remediation of sites polluted by
forms of metals into a small volume of soil, followed by chemi- metals. The discussion focuses on the status of soil washing
systems employed in the US, Europe, and Canada (Table 1). contaminants [8]. For example, the BioTrol Soil Washing Sys-
Soil washing based on physical separation (SW–PS) is more tem has been employed at the MacGillis and Gibbs Company
employed than processes that use chemical extraction (SW–CE). site in New Brighton, MN in 1992 [95]. In the mid 1990s,
Chemical extraction is more expensive ($ 358–1717 m−3 ) com- the US Army Corps of Engineers (USACE) and the USEPA
pared to physical separation ($ 70–187 m−3 ) [4]. reviewed physical separation technologies and concluded that
these techniques, coupled with chemical extraction, offered the
6.1. Soil washing in Europe most promising method for metal remediation in soils [9].
The co-operation with Dutch environmental firms has con-
SW–PS is relatively well established in Northern Europe, tributed to the establishment and the development of soil
primarily in the Netherlands since the mid 1980s [4,90]. washing in the United States [92,96]. In the early 1990s, the firms
The Netherlands are a pioneering country for the imple- Geraghty & Miller Inc., USA and Heidemij Realisatie of The
mentation of the SW–PS technology in a soil remediation Netherlands formed a joint venture (now called ARCADIS) and
context. For instance, Heidemij (now ARCADIS), has used were incorporated as Alternative Remedial Technologies (ART)
a SW–PS technology since 1983 [91]. Soil washing sys- to introduce the Heidemij soil washing system to the US market
tems used in the Netherlands is particularly appropriate to [92]. The first project contracted under this arrangement was the
treat metal contaminants and typically involve attrition scrub- large-scale remediation of the King of Prussia Superfund site,
bing, hydrocyclones, upstream columns, spirals and froth NJ performed in 1993 [6].
flotation cells [90]. A literature review revealed that many The number of soil washing technologies available at
Dutch environmental companies offer soil washing system commercial-scale for the treatment of metals in the US is dif-
such as: ARCADIS (http://www.arcadis-global.com); A&G ficult to estimate. ITRC [20] compiles a list of 16 soil washing
Milieutechniek (http://www.aengbedrijven.nl); Boskalis Dol- technologies available in the US for full-scale applications.
man (http://www.boskalisdolman.nl) [5]. In 2001, 21 stationary The REACH-IT database [97], which compiles 500 remediation
and four mobile soil washing plants were operational; and technologies, reports only seven vendors of soil washing tech-
855 kt/year were treated between 1991 and 2001 [90]. Envi- nology and one vendor of an acid extraction process. On the other
ronmental Dutch firms have introduced and promoted the hand, FTRT [98] compiles 20 vendors of soil washing or acid
development of SW–PS in the United States in the early 1990s extraction technologies. The main US vendors of soil washing
and in Japan in the early 2000s [92,93]. technologies, presented in Table 1 are: BESCORP; ART Engi-
The SW–PS technology is also well established in Ger- neering LLC; Eddy and Metcalf; and Biogenesis. Various soil
many, Sweden, Norway, and Belgium [5,7,19,91] to treat washing systems have been tested to remove metals from soils in
metal-contaminated soils. Ten Swedish companies and three the framework of Superfund Innovative Technology Evaluation
Norwegian companies offer treatment by soil washing appli- (SITE) demonstration program (Table 1).
cable to metal-contaminated soils [5]. Metso, a Swedish based Although the soil washing technology is available at
company, has been a major supplier of physical separation tech- commercial-scale in the US, its use has been limited for
nologies for European soil washing processes since the 1980s remediation of Superfund sites when compared to the conven-
[34]. Metso was the equipments supplier for the first US project tional solidification/stabilization technology. The Annual Status
of soil washing, conducted by ART [34]. Reports (ASR) database [99] indicates that the soil washing
method has been implemented at only two Superfund sites con-
6.2. Soil washing in the USA taminated with metals: at King of Prussia, NJ (completed) and
at Vineland Chemical Co., NJ (in operation) (Table 1). Table 7
Griffiths [7] reported two soil washing systems developed reports several cases of soil washing projects that have failed
by USEPA in the 1980s: the mobile soil washing system in the framework of the Superfund program and give the prin-
(MSWS) based on chemical extraction, and the volume reduc- cipal reasons for soil washing failure in the remediation of
tion unit (VRU) based on size separation. According to USEPA metals.
[8], the significant applications of SW–PS for remediation of
metal-contaminated soils in the United States began in the 6.3. Soil washing in Canada
early 1990s and the first applications were focused on treating
Pb-contaminated soils of abandoned small arms firing ranges Table 1 reports some examples of soil washing systems per-
(SAFR). For instance, in 1991 US Bureau of Mines presented formed at pilot-scale or full-scale in Canada such as: (1) Tallon
a conceptual physical separation process train for the remedia- Metal Technology in Montreal and Toronto; (2) Toronto Har-
tion of SAFR, which included Pb recovery [9,94]. Since the mid bour Commissioner (THC) treatment train in Toronto; (3) pilot
1990s, Brice Environmental Services Corporation (BESCORP) demonstration by Alex-Sol and INRS; and (4) pilot demonstra-
has had extensive experience for SAFR remediation (Pb removal tion by Dragage Verreault and INRS. Holbein [100] reported on
by density separation) and has also applied physical separa- the soil washing process of Tallon Metal Technology (Guelph,
tion for the remediation of a battery-manufacturing site in 1995 Ontario) for mixed contaminants; the soil treatment involved
(Table 1). Soil washing systems have also been used since the physical separation to treat the coarse fraction, and a chemi-
early 1990s for treatment of soils from wood preserving sites cal process to treat the fines. Three large-scale applications of
contaminated by a mixture of metals (Cu, Cr, and As) and organic Tallon’s treatment system have been applied. Researchers from
Table 7
Examples of deselected soil washing projects in Superfund program
Site location and description Media Metals Reasons of soil washing failure Alternative selected
technology
Sacramento Army Depot, oxidation lagoons, Soil Cr, Pb Costs Solidification/stabilization;

OU4, CA Off-site disposal
Zanesville Well Field, OH Soil As, Cr, Hg, Pb Soil volume was much smaller that Off-site disposal
originally projected; determined to be
too expensive
Ewan Property, OU 2, NJ (industrial waste Soil Cr, Cu, Pb Soil volume was much smaller that Off-site disposal
dumping) originally projected
Gould Inc., Portland, OR (battery site) Soil Pb Soil washing was shown to be ineffective Capping the landfill
due to varying site conditions
United Scrap Lead/SIA, OH (lead battery Soil/sediments As, Pb Costs Soil disposed off-site if Pb
recycling) levels above 1550 ␮g/g;
containment of soil below
this level
Myers Property, NJ (pesticide Soil/sediments Cu, Cd, Pb, As Soil washing treatment was not Off-site disposal
manufacturing) successful for As during treatability
study
Data extracted from [124,125].
INRS ETE (University of Quebec) have tested several pilot-scale Acknowledgements

soil washing systems for the decontamination of brownfield soils
located in urban environment [22,101,102]. G. Dermont is thankful to the “Institut National de la
Recherche Scientifique Eau Terre et Environnement” (INRS-
ETE) for their financial support. We would also like to thank
7. Conclusions
Angus Calderhead for his useful comments.
Soil washing is a technology particularly relevant for the
remediation of metal-contaminated soils. The majority of References
projects are based on physical separation technologies which
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Soil Washing For Metal Removal: A Review of Physical/chemical Technologies and Field Applications

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Journal of Hazardous Materials 152 (2008) 1–31

Soil washing for metal removal: A review of physical/chemical

Keywords: Heavy metals; Soil washing; Physical separation; Chemical extraction

4.8. Advantages/disadvantages of chemical extraction technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26

1. Introduction first purpose of this review is to present a technical description

Fig. 1. Schematic diagram of typical options used in soil washing processes.

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

Three aspects about physical separation for remediation of

levels; metal recovery by

forms of metal contamination and characteristics of soil matrix;

Physical separation techniques are primarily applicable to

particulate forms of metals: discrete particles or metal-bearing

particles. Physical separation is generally not appropriate for

can significantly improve metal desorption in chemical leaching

alogical phase containing heavy metals is significant to predict

metal contaminant particles (shape, morphology, and miner-

alogical association). Liberation degree refers to the release

is present. The term “carrying phase” refers to another min-

eral phase (Fe-oxides, carbonates, silicates, etc.) with which

the “metal phase” can be associated. Fig. 2 summarizes some

ticulate forms): (a) included in the volume, (b) associated, (c)

tion degree and applicability of particle separation, by gravity

concentration and froth flotation, are briefly discussed for each

state of metal phase (Fig. 2). The mineralogical aspects and

i The study distinguishes the performances of the PS and CE processes.

solid phase speciation of metal-bearing particles can be inves-

tigated by microscopy and spectroscopy technologies such as

shape, clay content, moisture content, humic content, hetero-

and metal contaminants, magnetic properties, and hydrophobic

properties of particle surface [8,9]. The treatment is difficult or

content, United Kingdom (1998)

NATO/CCMS Pilot test of the

unfeasible for the following cases: (1) the metal contaminants

are strongly bound on soil particles; (2) the difference in density

parameters that affect applicability of physical separation tech-

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

G. Dermont et al. / Journal of Hazardous Materials 152 (2008) 1–31

Sacramento Army Depot, oxidation lagoons, Soil Cr, Pb Costs Solidification/stabilization;

Data extracted from [124,125].

INRS ETE (University of Quebec) have tested several pilot-scale Acknowledgements

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