Science of the Total Environment 668 (2019) 1064–1076

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Science of the Total Environment

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Metal solubility and transport at a contaminated landfill site – From the

source zone into the groundwater
Uddh Söderberg T. a,⁎, Berggren Kleja D. b,c, Åström M. a, Jarsjö J. d, Fröberg M. b, Svensson A. a, Augustsson A. a
a
Department of Biology and Environmental Science, Linnaeus University, Kalmar, Sweden
b
Swedish Geotechnical Institute, Olaus Magnus väg 35, Linköping, Sweden
c
Department of Soil and Environment, Swedish University of Agricultural Sciences, Box 7014, Uppsala, Sweden
d
Department of Physical Geography, Stockholm University, Stockholm, Sweden

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Metal solubility and transport from a

contaminated landfill site were investi-
gated.
• Numerous methods were adopted in
this high-resolution field- and labora-
tory study.
• Efficient cation retention, likely due to
high pH. As and Sb showed higher mo-
bility.
• Waste zone Kd values were highly vari-
able but not correlated to basic geo-
chemistry.
• Soil metal concentrations decreased
abruptly below the landfill.

a r t i c l e i n f o a b s t r a c t

Article history: Risks associated with metal contaminated sites are tightly linked to material leachability and contaminant mobil-
Received 20 December 2018 ity. In this study, metal solubility and transport were characterized within a glass waste landfill through
Received in revised form 25 February 2019 i) lysimeter-collection of pore water and standardized batch leaching tests, ii) soil profiles extending from the
Accepted 1 March 2019
landfill surface, through unsaturated soil underneath, and into the groundwater zone, and iii) groundwater sam-
Available online 3 March 2019
ples upstream, at, and downstream of the landfill. The soil analyzes targeted both pseudo-total and geochemi-
Editor: Jay Gan cally active concentrations of contaminant metals (As, Cd, Pb, Sb) and basic soil geochemistry (pH, org. C, Fe,
Mn). Water samples were analyzed for dissolved, colloid-bound and particulate metals, and speciation modelling
Keywords: of the aqueous phase was conducted. The results revealed a highly contaminated system, with mean metal con-
Soil and groundwater metal pollution centrations in the waste zone between 90 and 250 times the regional background levels. Despite severe contam-
Glass waste ination of the waste zone and high geochemically active fractions (80–100%) of all contaminant metals as well as
Soil:Solution partitioning (Kd) elevated concentrations in landfill pore water, the concentrations of Cd and Pb decrease abruptly at the transition
Leachability between landfill and underlying natural soil and no indication of groundwater contamination was found. The ef-
Mobility
ficient cation retention is likely due to the high pH. However, the sorption of As and Sb is weaker at such high pH,
Colloids
which explains their higher mobility from the pore water zone into groundwater. The field soil:solution

⁎ Corresponding author.
E-mail address: terese.uddh-soderberg@lnu.se (T. Uddh Söderberg).

https://doi.org/10.1016/j.scitotenv.2019.03.013
0048-9697/© 2019 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076
partitioning (Kd) displayed a high spatial variability within the waste zone (the highest Kd variability was seen
for Pb, ranging from 140 to 2,900,000 l kg−1), despite little variability in basic geochemical variables, which we
suggest is due to waste material heterogeneity.
© 2019 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
1. Introduction
According to the European Environment Agency, there are about
2.5 million potentially contaminated sites within the EU member states,
and the contamination has in the majority of cases arisen from waste
disposal (Van Liedekerke et al., 2014). A key factor for the risks posed
by metal pollutants at such settings is the potential for leaching, mobili-
zation and subsequent spreading from the primary source areas. The
characterization of contaminant spreading thus plays a central role in
the risk assessment frameworks adopted by many national environ-
mental agencies. The generic approaches are, however, both simplified
and uncertain, where a lack of holistic studies with field measurements
of metal release from contaminated soil/waste horizons and subsequent
migration into hydrological systems (Pandey et al., 2014; Sungur et al.,
2015) leaves us with critical knowledge gaps regarding field-scale
metal mobility and transport, and net effects in downstream recipients.
In this context, the present paper addresses, firstly, waste zone metal
release. In internationally well-accepted and spread risk assessment
models, such as those from the US EPA and Dutch RIVM, soil:solution
partitioning (defined by the Kd value; l kg−1) are used to approximate
the contaminant mobilization in the source zone (Brand et al., 2007;
Swedish, 2009; U.S. EPA., 1991). The Kd value is expressed as a constant
based on the metal concentration associated with the solid soil phase
(mg/kg) and that of the soil solution (mg/l) (Allison and Allison, 2005;
U.S. EPA., 1999). Site specific Kd values may be determined from labora-
tory leaching tests; either in batch or column set-ups or according to ex-
traction protocols (TS 14405, ISO/TS 21268-2, TS 14429, TS 149977, SS-
EN 12457-2), or sometimes from field sampling of soil and pore water.
Few have, however, compared the laboratory and field approaches
(Sauvé et al., 2000). Anyway, we know that soil:solution partitioning
differs greatly between sites, and in general it is well linked to differ-
ences in basic soil or pore water geochemistry (Carlon et al., 2004;
Degryse et al., 2009; Janssen et al., 1997; Sauvé et al., 2000). Considering
this naturally high variability in soil:solution partitioning, it may not
come as a surprise that soil contamination is sometimes followed by
groundwater contamination as well (Khalil, 2012; Kumari et al., 2014;
Zheng et al., 2013), and sometimes not (Ahmed and Sulaiman, 2001;
Clausen et al., 2011; Jensen et al., 2000). However, while several studies
have characterized metal solubility or Kd values for different media and
their connection to soil properties, a review of 245 scientific papers and
reports by Allison and Allison (2005) concluded that none of the inves-
tigated papers addressed waste systems (waste piles, landfills etc.). Al-
most 15 years later that conclusion still seems to hold. The studies
which have addressed Kd variability have dealt mainly with natural
soil, and exclusively characterized differences between sites (de Souza
Braz et al., 2013; Fanger et al., 2006; Janssen et al., 1997), thus leaving
intra-site variability poorly investigated. From a risk assessment per-
spective, this means uncertainties regarding the representativeness
when applying single Kds.
Laboratory experiments have contributed to a relatively detailed un-
derstanding of processes involved in metal(loid) leaching from contam-
inated soil and waste matrices under different conditions, e.g. according
to de Matos et al. (2001), but an outlook beyond these small lab scales
and well-defined conditions reveals unanswered questions regarding
the whole process chain from waste material leaching and metal release
to pore water, transport in the unsaturated zone, and finally migration
into groundwater. Consequently, it is not surprising that available
models that aim to simulate metal transport often fail to adequately
1065
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assess contaminant travel times and/or total transport in pore water
and groundwater systems (Jarsjö et al., 2017; Malmstrom et al., 2008;
Persson et al., 2011).
To contribute to filling the knowledge gaps regarding metal solubil-
ity, partitioning and transport at sites with waste material contamina-
tion, the first aim of this paper is to present how metals are released
to pore water in the waste zone (landfill) of an industrial site affected
by N100 years of glass production, and the subsequent metal migration
through the natural soil under the landfill and finally to groundwater.
Additional aims are to define within-site variability in soil:solution
partitioning (Kd values) and to investigate how well standardized
batch-leaching tests reflect metal solubility in the waste zone.
2. Method
2.1. Study site
The study was conducted at Pukeberg glassworks site (Fig. 1), where
coloured and crystal glass have been manufactured since 1871. This site
is one of the most extensively investigated glassworks settings in Kal-
mar and Kronoberg counties in south-eastern Sweden. The major raw
materials used by the glassworks were sand of quartz and feldspar,
soda (NaCO3), potash (K2CO3), calcite (CaCO3), dolomite (MgCO3
·CaCO3), witherite (BaCO3) and oxides of different metals, for example
As, Cd, Co, Cr, Cu, Ni, Pb, Sb and Zn (Hermelin and Welander, 1986;
Magnusson, 1971). While the majority of modern glass waste (bottles/
jars and industrial glass waste) does not contain toxic metals in signifi-
cant quantities, and thus does not release such elements through
leaching (Disfani et al., 2012; Imteaz et al., 2012), coloured artistic
glass and crystal glass of the kind produced in the study region often
contain high amounts of a range of metals (Hermelin and Welander,
1986; Magnusson, 1971). Most of the waste generated (crushed glass,
discarded raw material batches, grinding and acid sludges, old oven
and demolition debris etc.) has been deposited on the factory's landfill,
which covers an area of approximately 15,000 m2 and has an average
depth of 1.6 m. The waste is currently mixed with natural soil, partly
due to various forms of excavation work at the property, but also as a re-
sult of the establishment of vegetation and soil at the surface of the
landfill since it was taken out of use in the 1970s.
The site is located in the northern part of the Nybro esker, in an area
mainly containing sandy glacifluvial materials (SGU, 2017b). The pri-
mary rock is granite (SGU, 2017b), with a 4–9 m thick overlying layer
of Quaternary deposits (SGU, 2017b). The area around the landfill gently
slopes from southwest to northeast, which also is the general ground-
water flow direction (Fig. 1). The hydraulic gradient is about 2% and
the hydraulic conductivity on average 3.5 × 10−6 m/s. These parameters
were calculated from water level measurements in groundwater sam-
pling wells at the site and the Bouwer and Rice Slug-test (Bouwer,
1989). The local catchment area is approximately 0.30 km2, estimated
from topographical maps (Dingham, 2002; Stone et al., 2015). The land-
fill is located at the northeast end of this catchment (Fig. 1), where dis-
charge into the St Sigfrid stream occurs. The theoretical dilution (under
full mixing) of pore water that penetrates from the landfill into the
groundwater beneath is thus about 20, calculated as the ratio between
the catchment area upstream of the landfill (0.30 km2) and the area of
the landfill (0.015 km2). The water infiltration of the region is estimated
to about 0.18 m/year (Törnqvist, 2015), which gives an annual water
1066 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076

Fig. 1. The location of Pukeberg glassworks site in Nybro municipality, southeastern Sweden. The dashed line marks the local catchment area and the dotted line marks the approximate
landfill borders. Sampling site U1 is thus located upstream. Sampling sites L1 to L5 are located at the landfill, and D1 to D4 are located downstream.

flow of ca 2700 m3 through the contaminated wastes (0.18 m/year
×15,000 m2).
2.2. Soil sampling and analyzes
In June 2015, a combination of Sonic drilling and DTH (down the
hole) drilling was used to retrieve intact soil cores. These were collected
at five locations at the landfill (Fig. 1), and consisted of material from
i) the unsaturated waste zone, where glass waste is mixed with natural
soil, ii) the unsaturated natural soil zone, underneath the waste zone
and iii) the saturated zone, i.e. the groundwater zone. Three cores
downstream of the landfill were also retrieved, collected ca 4 m from
the landfill slope, and subsampled every 0.5 m. All in all, 48 soil samples
from the 8 cores were obtained. After the pore water sampling was
completed, soil samples were also collected within a 10 cm radius of
the five lysimeters that were installed for collection of pore water
from the waste zone (see below).
All soil samples were sieved to 2.0 mm (ISO 11464:2006) and mea-
sured for pH and dry weight (ISO 10390:2005 and SS-ISO 11465). A por-
tion of 8.0 g was milled with a centrifugal ball mill before determination
of organic C (org.C) and metal concentrations. Organic C was deter-
mined using a Carlo Erba CN analyzer (Flash1112 series) according to
ISO 10694 and 13878. Pseudo-total metal concentrations were deter-
mined with a Perkin Elmer Sciex ELAN 9000 ICP/MS after digesting
1.0 g of the milled material with Aqua Regia (1HNO3:3HCl) at 90 °C in
a microprocessor controlled digestion block for 2 h.
Geochemically active concentrations of metal cations (Cd, Pb) were
determined after 16 h extraction of 1.0 g sieved soil with 30 ml 0.1 M
HNO3 (Gustafsson and Berggren Kleja, 2005). The corresponding frac-
tion of As, Sb (which form anions), and of Al, Fe and Mn, were deter-
mined after extraction of 1.0 g with 100 ml 0.2 M oxalate/oxalic acid
buffer at pH 3.0, shaken for 4 h in darkness (van Reeuwijk, 2002). The
extracts were analyzed with ICP-SFMS according to SS EN ISO 17294-
1, 17294-2 and EPA-method 200.8.
Finally, batch leaching tests were performed on all soil samples col-
lected around the lysimeters and in soil profiles reaching below the
groundwater table. The aim was to obtain data on waste zone material
leachability according to standard lab protocols, for comparison with
the leachability observed in the field and the leachability along the soil
profile. These batch leaching tests were conducted according to SS-EN
12457-2 and 21268-2, where 22.5 g of field-moist soil was shaken
with 225 ml Milli-Q water alternative 1 mM CaCl2-solution (hence a L/
S ratio of 10) for 24 h. All batch leaching test were run on duplicate sam-
ples. The collected eluates were analyzed for metal concentrations after
both membrane filtering (b0.45 μm) and ultra-filtration (b10 kDalton)
with ICP-SFMS according to SS EN ISO 17294-1, 17294-2 and EPA-
method 200.8, i.e. according to the same protocols as for the pore
water and groundwater samples (see below). The eluates were also an-
alyzed for dissolved organic carbon (DOC) and pH, again according to
 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076
the same methodologies as for pore water and groundwater samples
(see below).
2.3. Quality control and representativeness of sampled soil material
To assess the homogeneity of the sieved soil samples from the waste
zone, eight samples were prepared as triplicates before analyzes of
pseudo-total and geochemically active metal concentrations were con-
ducted (i.e. three different sub-portions of the material were digested/
extracted and analyzed separately). All relative standard deviations
(RSD) were between 4 and 10%, implying stable metal concentrations
in individual sieved subsamples. This further indicates that differences
in metal concentrations between locations (subsamples from different
cores and different depths) reflect true material heterogeneity. The sta-
bility and precision of the sample digestion procedure and of the instru-
ment (method repeatability) was evaluated by analyzing duplicates of
14 milled samples. Again, RSDs were below 10%. Recovery rates of the
analyzed reference materials were between 83 and 112% (QC; USGS
Geochemical Exploration Reference Materials GXR-1, GXR-4, GXR-6,
SdAR-M2), indicating a satisfactory precision in methodology.
2.4. Water sampling and analyzes
Pore water from the waste zone was collected with tension lysime-
ters (Prenart Super Quartz, 2 μm pore size), installed at three locations
at the landfill (Fig. 1) at two depths (30 and 60 cm). Sampling was con-
ducted on seven occasions, in July, August, September, and November
(twice) 2015, and in February and May 2016. A total of 31 pore water
samples were collected.
Six groundwater sampling tubes (30 mm PEH tubes) located up-
stream of, directly at, and downstream of the landfill were installed
(Fig. 1). The three tubes at the landfill (L2, L4 and L5) and one of the
tubes downstream (D3) were installed in the sonic drilling holes
where soil cores were also retrieved. Tube filters were placed to extend
from approximately one meter above to one meter below the ground-
water table. Sampling was conducted according to U.S. Geological Sur-
vey Techniques of Water-Resources Investigations (USGS, 2006), using
a peristaltic pump connected to a flow cell (YSI 659 MDS), on the
same occasions as the sampling of the tension lysimeters. A total of 34
groundwater samples were collected.
Field measurements of pH, conductivity (cond.), dissolved oxygen
(dis. oxygen), ORP (Oxidation-Reduction Potential) and temperature
were conducted on groundwater samples. pH and conductivity on pore
water samples from the lysimeters were measured using a Hanna pH-
meter 8519 N and Jenwey 4510 Conductivity meter (methods SS-EN
ISO 10523:2012 and SS-EN 27888). Alkalinity (alk.), orto-phosphate
(PO4) and UV-absorbance (254 nm) were measured on all water samples
according to SS 028139, SS-EN ISO 6878:2005 and US EPA Method 415.3
(Perkin Elmer UV/VIS spectrometer Lambda XLS+). Dissolved organic
carbon was measured with IR detection (SS-EN 1484) and macro anions,
fluoride (F), chloride (Cl) and sulphate (SO4), were determined with ion
chromatography (SS-EN ISO 10304-1). The specific UV-absorbance
(SUVA) was then determined as the UV-absorbance divided by DOC.
Metal concentrations in both pore water and groundwater were de-
termined with ICP-SFMS according to SS EN ISO 17294-1, 17294-2 and
EPA-method 200.8. The distribution of the metals and metalloids in dis-
solved, particulate or colloid bound forms, were investigated by analyz-
ing digested, membrane filtered (0.45 μm) and ultra-filtered (b10 kD)
samples, respectively.
2.5. Modelling of metal speciation in water with Visual MINTEQ
Visual MINTEQ (Gustafsson, 2016) was used to calculate the free ion
activity, saturation indices for minerals and percentage distribution of
dissolved species in all water samples (membrane filtered and ultra-
filtered samples) and eluates from batch leaching tests (ultra-filtered
1067
samples). Solution speciation was estimated using the thermodynamic
data of the Visual database, which mostly relies on the NIST Critical Sta-
bility constants database (Smith et al., 2003). The site-specific data used
in the model were pH, alkalinity, DOC, and concentrations of F, Cl, SO4,
PO4, Ca, Mg, Na, K, Fe, Mn, Al, Si, As, Ba, Cd, Co, Cu, Pb, Sb and Zn. To de-
scribe the binding of metals to DOC, the Stockholm Humic Model (SHM)
was used (Gustafsson, 2001; Gustafsson et al., 2003) and the Davies
equation was used for activity correction. Saturation indices were
assessed for all As, Cd, Pb and Sb mineral phases included in the
Visual MINTEQ database, and also for duftite (PbCuAsO 4(OH)),
hydroxymimetite (Pb5(AsO4)3OH), mimetite (Pb5(AsO4)3 Cl), lead
silicate (PbSiO3) and shultenite (PbHAsO4). The latter four minerals
were added as previous investigations have pointed to their poten-
tial for affecting Pb and As solubility (Bajda, 2010; Inegbenebor
et al., 1989; Lee and Nriagu, 2007; Lindsay, 1979; Magalhaes and
Dejesus, 1988; Sjöstedt et al., 2018).
2.6. Statistical analyzes
Soil:solution metal partitioning coefficients (Kd values) were ana-
lyzed with linear regression models using the program R 3.0.2 (R Core
Team, 2017). For each metal, a model with four predictor variables
was fitted, namely: soil pH, soil organic C, soil Fe content, and soil con-
centration of the metal in question. Kd and pH values were repeatedly
sub-sampled at each station. Therefore, the data was analyzed as linear
mixed effects models with the sampling station included as a random
factor. Predictors and responses were log transformed when necessary
to obtain homoscedastic model residuals. Models were fitted with re-
stricted maximum likelihoods (REML), using the function lme in the R
package nlme (Pinheiro et al., 2017). We used model simplification by
stepwise elimination of non-significant predictors (criterion for dele-
tion p N 0.05; (Crawley, 2007), so that final models only contained sig-
nificant predictors (if any). The coefficients of significant predictors
and the model intercepts were used to build predictive model equa-
tions. Marginal R-squared values of the final models were calculated
using the function r.squaredGLMM in R package MuMIn (Barton, 2013).
2.7. Regional background concentrations
Regional background concentrations in soil and groundwater
(delimited to a 45 km radius around Pukeberg) were retrieved from
the Geological Survey of Sweden (SGU, 2017a). The soil background
data refer to the fine fraction of natural (C horizon) till soil. Data on Sb
in groundwater in the region were not available at SGU. Hence addi-
tional groundwater data were collected from the Swedish Nuclear
Fuel and Waste Management C. (SKB) Site Characterization database
(SICADA) for Simpevarp (SKB, 2016). Simpevarp has the same primary
bedrock as Pukeberg and may give representative regional background
values for Sb.
3. Results and discussion
3.1. Solid phase characterization
In accordance with consultant investigations conducted between
year 2002 and 2012 (Elert and Höglund, 2012; Fanger et al., 2003), the
metals As, Cd, Pb and Sb were clearly elevated in the landfill waste
zone, with mean pseudo-total metal concentrations exceeding the
background levels of regional till soil by factors of about 120, 160, 90
and 250, respectively (Table 1). The fraction of geochemically active
forms ranged from 80% (As) to 100% (Cd) (Fig. 2a), while concentrations
after batch leaching with CaCl2 were below 1.5%.
The highest metal concentrations of the waste zone were found to-
wards the bottom of the landfill, but they decreased abruptly in the un-
derlying unsaturated natural soil zone (Fig. 2a); reaching background
concentrations already within the upper 20 cm for Cd and Pb and
1068 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076

Table 1
Soil pseudo-total metal concentrations in the three analyzed zones at the landfill and the unsaturated natural soil zone downstream the landfill, together with basic physicochemical pa-
rameters. Metal concentrations in mg/kg dry weight. Data from each individual soil core is provided in the Supplementary information (Table S-1).

Contaminant metals

As Cd Pb Sb Fe Al Mn pH (H2O) Org. C (%)

Regional background (45 km radius around Pukeberg), N = 34. Depth: approximately 0.6–1.0 m
Min-Max 0.57–2.6 0.031–0.18 6.2–59 0.057–0.32 6300–32,500 4900–22,500 92–450 4.3–5.6
Mean ± SE 1.2 ± 0.091 0.078 ± 0.006 18 ± 2.3 0.15 ± 0.0091 16,400 ± 770 10,800 ± 920 230 ± 14 5 ± 0.056

Unsaturated glass waste zone, N = 13. Depth: approximately 0–1.5 m

Min-Max 35–390 3.0–22 560–4300 9.9–78 10,300–25,000 3000–12,000 190–1900 6.8–7.6 1.2–7.8
Mean ± SE 140 ± 30 13 ± 1.8 1700 ± 270 38 ± 5.1 16,000 ± 1100 9100 ± 710 510 ± 120 7.2 ± 0.1 3.0 ± 0.5

Unsaturated natural soil zone under the landfill, N = 20. Depth: approximately 1.5–4.0 m
Min-Max 0.8–36 0.005–0.3 11–41 0.40–9.8 11,500–18,000 6500–15,000 170–320 6.8–8.3 0.006–0.42
Mean ± SE 5.2 ± 1.8 0.087 ± 0.021 19 ± 1.8 2.2 ± 0.49 14,000 ± 410 10,000 ± 510 240 ± 8.0 7.6 ± 0.090 0.089 ± 0.024

Saturated natural soil zone under the landfill, N = 4. Depth: approximately 4.0–5.5 m
Min-Max 2.8–3.9 0.053–0.10 6.4–20 0.38–0.75 15,500–22,000 11,300–18,000 280–490 8.0–8.3 0.006–0.027
Mean ± SE 3.3 ± 0.23 0.088 ± 0.012 16 ± 3.1 0.48 ± 0.090 18,000 ± 1600 14,000 ± 1500 370 ± 45 8.1 ± 0.058 0.014 ± 0.006

Unsaturated natural soil zone downstream the landfill, N = 11. Depth: approximately 0–2.0 m
Min-Max 0.8–2.5 0.005–0.10 12–28 0.10–0.40 12,000–19,000 8000–13,000 200–530 5.2–7.3 0.012–3.3
Mean ± SE 1.6 ± 0.18 0.055 ± 0.015 17 ± 1.4 0.21 ± 0.028 14,000 ± 620 9600 ± 470 260 ± 29 6.0 ± 0.21 0.68 ± 0.30

70 cm for As and Sb. All contaminant metal concentrations in all soil
samples downstream of the landfill slope, about 4 m away, were also
comparable or close to regional background levels (Table 1).
Concentrations of Fe and Al represented levels that are normal for
the natural till soil of the region and Mn was slightly elevated
(Table 1). The variable which stands out as non-representative is the
pH value, which was clearly elevated in both the waste zone and
below (Table 1).
3.2. In situ aqueous phase characterization
Within the waste zone, elevated metal concentrations were also
found in the lysimeter pore waters, where the concentrations of all
metals were significantly higher than in both local and regional ground-
water (Table 2). The difference between pore water and landfill ground-
water concentrations were on average 200 and 910 times for Cd and Pb,
respectively (Fig. 2b); thus, much larger than one would expect from di-
lution (applying the theoretical dilution factor of 20 presented in the
site description (Section 2.1)). The concentrations of Cd and Pb in
groundwater wells at the landfill were comparable to regional back-
ground levels, and also not elevated when compared to the sampling
well upstream (Table 2). They also complied to the drinking water stan-
dards of the World Health Organization (WHO, 2011). Groundwater As
and Sb were, however, elevated compared to both regional background
levels and drinking water criteria in several sampling tubes at and
downstream of the landfill (Table 2). Thus, these elements were less
strongly retained than the cationic metals.
The most distinct features of the basic water chemistry, summarized
in Table 3, were the high alkalinity – matching the high pH values of the
system - and the high fluoride concentrations. The remaining variables
were within normal ranges for till soils of the region (SGU, 2016; SKB,
2016), and all groundwater samples were oxic (Eh N290 mV). The
high metal concentrations in the waste zone pore water were mainly
(N67%) associated with dissolved forms, even though colloids were sig-
nificant carriers for Pb (24% of the total content) and Sb (15%) (Fig. 3a).
Association with colloids was, however, non-existent for all metals in
the groundwater (Fig. 3a).
From the Visual MINTEQ modelling we see that the soluble As and
Sb, in both pore water and groundwater, occurred entirely as free, reac-
tive ions (HAsO42−, H2AsO4−, Sb(OH)6−) in the soluble (b10 kD) fraction.
In contrast, the two cations showed some degree of complex formation
(Fig. 3b). In pore water, the organic complexes dominated for Pb (86% of
the total dissolved Pb). The second most important Pb complexing li-
gand was carbonate, accounting for 12% of the total Pb speciation in
solution. This makes Pb the element with by far the lowest fraction as
free ions. The complexation with Cd was also mainly with DOC (27%)
and carbonates (9.4%). Minor complexation (b1%) was simulated with
hydroxides, sulphates, phosphates, chlorides and fluorides. In general,
the distribution between free dissolved ions, dissolved inorganic ions
and organic complexes was similar in the waste zone pore water sam-
ples and in groundwater (Fig. 3b), even though the surrounding solid
phase material differ significantly in composition.
Despite the relatively high contaminant metal concentrations in
pore water of the waste zone, none of the mineral phases plausible for
the four metals according to the Visual MINTEQ database were assessed
to reach supersaturation. All groundwaters were undersaturated with
respect to the mineral phases investigated. Saturations indices for min-
erals, simulated in Visual MINTEQ, are presented in the Supplementary
information (Table S-4).
3.3. Leaching of metals from glass waste material and subsequent migration
to groundwater
The observed high fraction of geochemically active metal forms
(Fig. 2a) in association with elevated metal concentrations in pore wa-
ters of the waste zone (Table 2; Fig. 3) imply that a significant part of
the waste zone material is susceptible to leaching. That metal concen-
trations clearly increase towards the bottom of the landfill (Fig. 2a) is,
however, more likely due to older and younger wastes differing in com-
position than to the migration of contaminants from upper landfill hori-
zons. This, we argue, is because of the sharp disappearance of metal
contaminants in the unsaturated soil underneath the landfill (Fig. 2a).
Before 1969, for example, the glass raw material was prepared in the
glass works factory. It involved mixing of a variety of powdered metal
oxides, and discarded batch mixtures were thrown at the landfill, prob-
ably leading to both higher total metal concentrations than in younger
waste materials and a higher leachability of the material.
Although leachable in the waste zone, the sharp decrease in concen-
trations of cation-forming metals (Pb and Cd) immediately under the
landfill (Fig. 2a) implies that these metals are efficiently trapped over
very short distances (decimeters) as the metal-rich pore water perco-
lates into the natural soil. It has previously been shown that little or
no impact from metal leaching may be detected in groundwater down-
stream sites with landfilled mixed municipal waste (Christensen et al.,
2001; Kjeldsen et al., 2002; Mor et al., 2006), although examples to
the contrary also exist (Kiddee et al., 2014). Our results demonstrate
how efficient, and over how short distances, the immobilization of
aqueous species may be under favorable conditions, at least for cations.
 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076 1069

Fig. 2. a. Depth profiles of metal concentrations in soil at the landfill area. The concentration given for a certain depth interval represents the average for all sampling sites. The error bars
represent the standard error (SE). Profiles for each soil core are presented in the Supplementary information (Fig. S-1). b. Depth profiles of metal concentrations in aqueous phase at the
landfill area. The concentration given for a certain depth interval represents the average for all sampling sites. The error bars represent the standard error (SE).
1070 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076

Table 2
Metal concentrations in membrane filtered water (b0.45 μm). Data from each individual lysimeter and groundwater monitoring wells is provided in the Supplementary information
(Table S-2).

Contaminant metals

As Cd Pb Sb Ca Mg Na K Fe Al Mn

μg/l μg/l μg/l μg/l mg/l mg/l mg/l mg/l μg/l μg/l μg/l

Pore water collected with lysimeters in the waste zone of the landfill (sample N = 31)
Min-Max 0.77–97 2.1–32 2.1–860 6.6–530 4.3–180 0.81–31 11–330 6.6–83 3.0–620 0.030–7800 0.0045–2800
Mean ± SE 24 ± 4 13 ± 1.7 84 ± 30 190 ± 26 89 ± 7.9 5.9 ± 1.3 62 ± 15 29 ± 4.5 50 ± 22 650 ± 340 270 ± 130

Groundwater from monitoring wells at the landfill (sample N = 21)

Min-Max 0.035–15 0.012–0.28 0.0055–0.87 4.8–28 34–72 7.5–11 18–57 12–17 0.17–11 13–66 0.10–510
Mean ± SE 5.3 ± 1.2 0.065 ± 0.013 0.092 ± 0.042 13 ± 1.6 52 ± 2.2 9.0 ± 0.24 24 ± 2.0 15 ± 0.34 2.2 ± 0.52 37 ± 2.9 12 ± 6.6

Groundwater from monitoring wells downstream the landfill (sample N = 11)

Min-Max 0.19–3.1 0.066–0.23 0.0029–0.17 9.9–47 22–79 5.6–12 14–25 6.6–17 0.10–19 7.4–98 5.3–6.1
Mean ± SE 1.5 ± 0.34 0.15 ± 0.018 0.029 ± 0.016 29 ± 4.7 48 ± 6.6 8.2 ± 0.65 19 ± 1.2 11 ± 1.2 3.4 ± 1.7 45 ± 11 5.9 ± 0.082

Groundwater from monitoring wells upstream the landfill (sample N = 3)

Min-Max 0.74–2.2 0.020–0.042 0.013–0.038 0.33–0.50 12–16 2.8–3.7 7.4–8.8 3.0–3.1 0.91–1.6 29–38 1.1–9.8
Mean 1.5 0.028 0.026 0.41 14 3.2 8.1 3.1 1.2 33 5.5

Regional background concentrations in groundwater

N 114 143 142 291 759 764 738 737 686 436 667
Min-Max 0.010–1.0 0.003–0.31 0.005–4.4 0.012–2.2 0.92–110 0.79–14 3.2–71 0.12–5.7 0.30–9100 1.8–1100 0.10–1600
Mean 0.23 0.038 0.61 0.1 14 2.9 12 1.7 220 99 150

3.4. Retention mechanisms
The waste zone solid material in Pukeberg, as well as the pore water
and groundwater sampled at the landfill area, are clearly affected by the
extensive use of various carbonates in glass production. We have previ-
ously described a system of high pH, alkalinity and conductivity, with
high concentrations of base cations (Table 2), and with carbonates dom-
inating the inorganic complexation in the aqueous phase (Fig. 3b). The
majority of the metal cation retention in the waste zone is therefore
probably due to the high pH. Within the current pH interval (7.2–8.2),
the cation sorption is expected to be highly efficient for Cd and Pb;
nearly 100% has previously been reported (Jalali and Najafi, 2018;
Ndiba and Axe, 2010; Rijkenberg and Depree, 2010; Tahervand and
Jalali, 2016; Yang et al., 2003; Zang et al., 2017). This pH-depending re-
tention is explained mainly by intensified electrostatic adsorption to
negatively charged functional groups and/or co-precipitation with Fe/
Al/Mn oxides (Alloway, 2013; Bolan et al., 2014; Naidu et al., 1997;
Violante et al., 2010). The pre-conditions for this process are good in
Pukeberg, as indicated by relatively high concentrations of Fe, Al and
Mn and fair amounts of organic carbon (Table 1). That As and Sb are
less efficiently retained is probably also largely due to the high pH of
the system, where the decrease in positive charged functional groups
is not beneficial for the immobilization of these anion-forming elements
(Goldberg, 2002; Johnson et al., 2005; Leuz et al., 2006; Wang and
Mulligan, 2006; Violante et al., 2010).
The low contribution of potentially mobile aqueous complexes of Cd
(Fig. 3) also favors immobilization processes. For Pb, complexes with
dissolved organic matter are important in the pore waters of the
waste zone as well as in the groundwater. This organic matter complex-
ation obviously facilitates mobility, as described by e.g. Christensen et al.
(1996), Clausen et al. (2011) and Rijkenberg and Depree (2010). The
overall low Pb mobility, however, points to a strong binding of DOC
complexes to the solid phase. In support of this hypothesis there are
studies which have shown that the release of DOC to pore water may
occur parallel to efficient immobilization processes (Kaiser and
Kalbitz, 2012). The potential of DOC retention in soil systems is also

Table 3
Physicochemical parameters in membrane filtered water (b0.45 μm). Data from each individual lysimeter and groundwater monitoring wells is provided in the Supplementary informa-
tion (Table S-3).

pH Cond. Alk. Dis. oxygen Eh DOC SUVA (254 nm) F Cl SO4 PO4

μS/cm mg HCO3/l DO % mV mg/l l/mg-m mg/l mg/l mg/l μg/l

Pore water collected with lysimeters in the waste zone of the landfill (sample N = 31)
Min-Max 6.1–7.6 110–1900 16–1000 8.7–58 1.4–4.3 0.64–15 0.50–12 2.5–220 7.1–140
Mean ± SE 6.9 ± 0.084 760 ± 86 350 ± 55 16 ± 2.1 2.5 ± 0.13 7.7 ± 0.71 3.2 ± 0.57 19 ± 7.2 50 ± 6.7

Groundwater from monitoring wells at the landfill (sample N = 21)

Min-Max 5.9–6.6 160–570 120–250 40–83 290–510 1.9–5.5 0.48–1.9 1.2–3.6 14–22 21–65 1.0–18
Mean ± SE 6.3 ± 0.042 400 ± 25 180 ± 8.2 63 ± 3.0 430 ± 12 3.6 ± 0.20 1.2 ± 0.10 2.1 ± 0.14 19 ± 0.52 40 ± 2.2 5.9 ± 1.3

Groundwater from monitoring wells downstream the landfill (sample N = 11)

Min-Max 5.3–6.1 170–520 69–240 54–76 400–520 1.9–4.7 0.53–1.7 0.63–5.2 13–29 12–49 1.0–17
Mean ± SE 5.9 ± 0.082 330 ± 31 150 ± 21 66 ± 1.9 520 ± 11 2.8 ± 0.26 1.2 ± 0.13 2.8 ± 0.57 19 ± 1.2 28 ± 3.5 7.6 ± 1.8

Groundwater from monitoring wells upstream the landfill (sample N = 3)

Min-Max 5.8–5.9 79–120 28–22 67–77 440–480 1.9–2.3 0.94–1.5 0.36–0.44 11–14 14–15 23–36
Mean ± SE 5.9 ± 0.045 100 ± 22 31 ± 2.5 72 ± 5.1 460 ± 24 2.1 ± 0.23 1.2 ± 0.30 0.40 ± 0.040 12 ± 1.3 14 ± 0.25 30 ± 6.5

Regional background concentrations in groundwater

N 897 895 688 38 238 674 738 735 545
Min-Max 4.6–8.5 35–622 0.20–300 280–530 0.6–26 0.040–1.8 2.1–135 2.4–88 2.0–110
Mean 6.3 150 34 430 3.2 0.31 19 15 14
 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076 1071

Fig. 3. a): Average metal partitioning in pore water (N = 7) and groundwater samples (N = 8), distributed among dissolved, colloid bound and particulate bound fractions. The
distributions were determined from ultra-filtered (10 kD), membrane filtered (0.45 μm) and digested samples. b): Distribution among free ion, inorganic complexes and DOC
complexes in dissolved (ultra-filtered, 10 kD) water samples. Results from Visual MINTEQ modelling. The As and Sb forms (HAsO24, H2AsO− −
4 , Sb(OH)6 ) are treated as free ions, despite
their association with OH−, since they behave as free (reactive) ions. The inorganic complexes involve carbonates, hydroxides, sulphates, phosphates, chlorides and fluorides.

implied by studies which present how DOC at deeper soil depths origi-
nates mainly from decomposition at these depths and not from DOC
production near the surface (Fröberg et al., 2006).
From the much lower occurrence of colloids in the groundwater
zone compared to that of the waste zone in Pukeberg (Fig. 3a) one
could hypothesize that the decrease in metal concentration could to
some degree be due to colloid retention. While metal transport may
be governed by binding to colloidal particles (Baumann et al., 2006;
Karathanasis, 1999; Shang and Li, 2011), colloid association may also
prevent spreading in cases where these small units are physically
trapped (Baumann et al., 2006; Buffle and Leppard, 1995; Ranville
et al., 1999). However, since the same decrease in metal concentrations
is seen for membrane filtered and ultra-filtered samples in Pukeberg,
colloid filtering is not plausible as a key controlling factor for the ob-
served metal retention in the waste zone.
3.5. Assessing solubility – batch leaching vs field measurements
Comparing metal concentrations in lysimeter-collected pore water
with eluates from laboratory batch leaching of soil samples collected
around the same lysimeters, we see that concentrations are consistently
higher in the lysimeter-collected pore waters for Cd, Pb and Sb (Fig. 2b
+ Fig. 4). This finding implies that the field leachability of metals in the
waste zone is not adequately captured in the evaluated standard
leaching tests, despite the extensive use and high acceptance of these
protocols. This effect appears to be especially prominent at high concen-
trations, where the implications of erroneous interpretations are gener-
ally the highest too. The maximum concentration in pore water
collected in the field was three (Sb), four (Pb) and eight (Cd) times
the maximum concentration after batch leaching. Perfect correlations
between field and lab measurements can obviously not realistically be
expected since samples taken for laboratory testing represent only a
sub-portion of the total soil volume which has been in contact with
the pore water collected in the lysimeters. However, the consistent ap-
pearance below the 1:1 line of Cd, Pb and Sb indicates a systematic un-
derestimation of the material leachability in the leaching tests. The
probability of the observed difference being of a systematic nature is
also strengthened by similar observations found for the groundwater
zone (not displayed in Fig. 4). Concentrations in groundwater samples
from the installed tubes were between two (Pb and Sb) and five (Cd)
1072 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076

Fig. 4. Relationship between average metal concentration (μg/l) in ultra-filtered (10 kD) lysimeter-collected pore water and in eluates from batch leaching tests (with H2O and CaCl2).
Ultra-filtered samples should provide the most relevant basis for comparison since batch leaching can result in a high release of colloids.

times those received after batch leaching of the soil removed upon the
installation of these tubes.
Since the same difference applied to both ultra-filtered (b10 kD) and
membrane filtered (b0.45 μm) samples, the higher concentration in ly-
simeter pore waters cannot be the effect of a higher occurrence of col-
loid particles in these waters. Moreover, the metal association to
colloids was higher after the batch leaching tests – either due to a
lower average grain size of the sieved material, or more probably due
to the release of fine particles during shaking (Bergendahl, 2005;
Bergendahl and Grasso, 1998). While the colloidal association was vir-
tually non-existent for all metals except Pb and Sb in the pore waters
(Fig. 3a), it still corresponded to 91% (Pb), 55% (Cd), 27% (As) and 11%
(Sb) of the total concentrations in membrane-filtered water after
batch leaching with H2O – supporting the idea of a significant colloidal
release with this method. For the CaCl2 extraction colloidal associa-
tion compared to the total metal concentration were lower (64, 4,
14 and 4%, respectively), probably due to the aggregating and bridg-
ing potential of the Ca2+ ions which can result in the formation of
some particles that are too large to pass through a 0.45 μm filter
(Dahlgren and Marrett, 1991; Grathwohl and Susset, 2009; Klitzke
and Lang, 2009; Kretzschmar and Sticher, 1997). Grathwohl and
Susset (2009) speculated, but without performing any tests to con-
firm their hypothesis, that the mobilization of fine particles during
shaking was likely to result in an overestimation of metal leaching
in batch leaching set-ups. The results from our study, however,
imply the opposite net effect despite a confirmed release of colloids.
While Meers et al. (2007) presented a good correlation between Cd
concentrations in pore water collected with Rhizon soil moisture sam-
plers and in eluates after CaCl2 leaching, underestimated metal concen-
trations upon batch leaching have been presented before. For example,
de Groot et al. (1998) showed that metal concentrations in 0. 01 M CaCl2
extracts at L/S = 10 where consistently lower than in soil pore water,
and most pronouncedly so for metals with a high tendency of organic
complexation – such as Pb and Cu. Since dilution results in lower DOC
concentrations in CaCl2 extracts (Yin et al., 2002), organic complexation
is also reduced. Also Degryse et al. (2009) have suggested that a de-
crease in DOC complexation can result in lower aqueous phase metal
concentrations after batch leaching. In our dataset this mechanism is
supported by a higher average DOC concentration in lysimeter-
collected pore waters (16 mg/l) than in the solutions after CaCl2 and
H2O leaching (1.7 and 2.4 mg/l, respectively). However, if this was the
sole mechanism, one would expect the effect to be clearer for Pb than
for, eg, Sb, which showed no DOC complexation in the system (Fig. 3).
Other pore water characteristics than DOC content that are important
for the solid-liquid partitioning – such as the pH and ionic strength –
can also differ between field and lab conditions and may thus affect
partitioning assessments (Di Bonito et al., 2008; Fest et al., 2008; van
der Sloot et al., 1996), but the difference is marginal in our case,
 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076 1073

where both the natural pore waters and leaching eluates were
circumneutral (pH = 7.1 in the leaching tests and pH = 6.9 in the
field). Besides differences in the aqueous phase chemistry, alternative
explanations for the lower leachability assessed from batch leaching
may be a relatively short contact time or a higher L/S ratio (Di Bonito
et al., 2008; Ndiba and Axe, 2010; Schuwirth and Hofmann, 2005); but
a recent study by Löv et al. (2019) implies that the contact time in stan-
dardized leaching tests with both CaCl2 and H2O, and at different L/S, is
enough for near-equilibrium conditions to arise. Another contributing
factor may be the removal of coarse grain sizes by standard procedure
pre-treatment (sieving) of the laboratory samples. Under true equilib-
rium conditions, the particle size distribution of the solid phase should
be irrelevant, but it can of course be that the different pore systems in
the waste deposit are not in true equilibrium.
3.6. Substantial intra-site variability in soil:solution partitioning – Kd
values
Fig. 5 presents ranges in partitioning coefficients from a selection of
previously published articles and reports, together with Kds from
Pukeberg. According to several of the earlier studies, which have fo-
cused on Kd variability between different sites, Kd values can be fairly
well predicted from soil and/or pore water characteristics that are
well known to influence metal partitioning. pH is typically the strongest

Fig. 5. Variability in Log10 Kd values from Pukeberg (ref 1–3), in relation to a selection of other studies which have focused on compiling Kd data from multiple sites (ref 4–8). The figures
show min-max intervals (bars), with the red asterisks indicating the arithmetic mean values. Most Kd values are based on pseudo-total concentrations of both the solid and aqueous phase.
In the ideal case, free-ion concentrations of the pore water and geochemically active concentrations (representing the sorbed pool) of the solid phase are preferred, since these are the ones
participating in the equilibrium reactions relevant for the Kd coefficient. The improvement in prediction when using the latter concentrations instead of total ones is, however, small
(Degryse et al., 2009).
1074 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076
Table 4
Linear mixed-effects models of soil:solution partitioning coefficients (Kd) for As Cd, Pb and Sb as explained by the following predictor variables: soil pseudo-total metal concentration, pH,
organic C and pseudo-total Fe content. P-values for all predictors are presented, as well as parameter estimates from the final models which only contained statistically significant predictor
variables.
Metal Predictor variables
log [Me] pH log org C
As 0.4517 0.0429* 0.8588
Cd 0.0643 0.1428 0.3947
Pb 0.0013** 0.5864 0.5482
Sb 0.2820 0.0076** 0.6833
*, ** represents p b 0.05 and p b 0.01, respectively.
determinant, together with organic matter, Fe, and/or the solid phase
concentration of the metal in question (Carlon et al., 2004; de Vries
et al., 2011; Degryse et al., 2009; Janssen et al., 1997; Sauvé et al.,
2000). Under ideal conditions, the Kd value should be insensitive to
changes in the solid phase metal concentration (since it is equivalent
to the numerator of the Kd expression). In practice, however, metal
sorption is often not linear – and regression model performance may
therefore be improved by including the solid phase metal concentration
(Sauvé et al., 2000).
From Fig. 5 we see that the Kd values calculated for the Pukeberg
waste zone are highly variable, even though they were calculated for a
single site that has received waste materials from only one specific
type of industry, and with little variation across the site in basic geo-
chemical properties. For most metals the variability is comparable to
that found in studies which have included many different sites, with ev-
ident differences in terms of pollution load and general geochemistry.
The highest Kd variability in the Pukeberg waste zone was seen for Pb,
ranging from 140 to 2,900,000 l kg−1 (field Kd; ref. 1 in Fig. 5). The
variability then decreased in the order As N Cd N Sb, with interval ranges
of [450–98,000], [22–4700] and [62–1300], respectively. Our linear
models further imply that traditional soil attributes play a relatively
low role in the soil:solution partitioning in the system (Table 4). Even
though there was a significant relationship between soil pH and the
Kd values of As in Pukeberg, the model R2 values (5–9%) were low com-
pared to previous studies considering data from multiple sites. For ex-
ample, Sauvé et al. (2000) (ref 8 in Fig. 5) found R2 values in the range
of 29–58% when using only pH as the predictor variable. Combining
pH with log SOM and/or log [Me soil], R2 increased to 56–88% (Sauvé
et al., 2000). Similar or even higher R2 values, after considering pH
and log OC, are presented in the review by Degryse et al. (2009), pre-
senting data from multiple studies. Janssen et al. (1997), too, presented
regression models of good prediction ability, with R2 values from 71 to
85% for a range of metals.
The relatively poor correlation between field Kds and traditional
predictor variables (soil pH, org-C and Fe content; Table 4) in Pukeberg
is probably due to the high variability in Kd combined with a relatively
low variability in the predictor variables. Exemplifying this by pH, the
Pukeberg waste zone sample of lowest pH (6.8) had a hydrogen ion ac-
tivity only 6.3 times the sample with the highest pH (7.6). By compari-
son, Janssen et al. (1997) presented a pH range of 3.8–7.9 for the 20
Dutch contaminated soils for which they estimated Kd values, corre-
sponding to a 12,500 times difference in hydrogen ion activity. And in
the study by Groenenberg et al. (2010) there was a 39,800 times differ-
ence in hydrogen ion activity (pH range 3.7–8.3) when comparing 216
different soils, representing both clean and heavily contaminated soils
from the Netherlands and the UK. Therefore, the data at hand for
Pukeberg indicates that the waste material itself has a more prominent
influence on metal partitioning than the basic soil properties generally
attributed to this role.
4. Conclusion
The most important conclusions that can be drawn from this high-
resolution field and laboratory study are that:
Final regression model Final model marginal R2
log Fe
0.2091 logAsKd = 3.7 + 0.68 × pH 7%
0.5312 – –
0.1797 logPbKd = −2.0 + 1.74 × logPbSoil 87%
0.2011 logPbKd = 8.7–0.46 × pH 9%
i) The long lasting (N100 years) deposition of metal-containing
glass waste to the investigated landfill site is not only reflected
by high total concentrations of As, Cd, Pb and Sb, but also by a
high fraction of geochemically active forms and elevated concen-
trations in pore water. However, despite their leachability in the
waste zone, soil metal concentrations decrease abruptly to back-
ground concentrations (within decimeters) as the landfilled ma-
terial transcends into the natural soil underneath. The main
controlling factor is most probably the high pH of the waste ma-
terial, which has the strongest effect on the cationic metals Cd
and Pb.
ii) Field leachability may not be adequately assessed when
translated from standard batch leaching tests. In this study we
found consistently higher concentrations of Cd, Pb and Sb in
lysimeter-collected pore water than in eluates from the evalu-
ated laboratory batch leaching experiments.
iii) The soil:solution partitioning (Kd values) varied by several
orders of magnitude within the landfill waste zone; basically
within the same range as previously reported for different sites,
with marked differences in basic soil geochemistry. In our
study, however, basic soil properties vary little, and our regres-
sion models imply that traditional soil attributes explain little
of the variability observed in soil:solution partitioning. Instead,
we propose that waste material heterogeneity is more important
in this case, where the contaminated waste zone is characterized
by a high fraction of waste (or non-soil material). The generaliz-
ability of a “waste heterogeneity effect” for metal partitioning,
however, needs to be further evaluated.
iv) Since risk assessment protocols and remediation strategies at
contaminated sites focus to a great degree on the conditions for
contaminant spreading, efforts to pinpoint critical flaws or un-
necessarily uncertain assumptions are of high practical rele-
vance. In this context, both the potentially high metal retention
and the intra-site variability in Kd values have direct implica-
tions. For example, the measured concentrations in groundwater
are much lower than one would predict by applying the national
generic risk assessment model (Swedish, 2009). The difference
was most evident for Cd and Pb, where simulated average con-
centrations in groundwater are 3800 and 57,000 times those actu-
ally found in the field - when applying conservative (minimum)
site-specific Kd values. Applying average Kd values in the model
instead, however, the difference was reduced to 54 and 30
times. This shows the significance of choosing a representative es-
timate for soil:solution partitioning, as well as the need to im-
prove our understanding about which factors that control metal
partitioning. In this study, we have touched upon possible reten-
tion mechanisms, but further analyzes are needed.
CRediT authorship contribution statement
Uddh Söderberg: T.Conceptualization, Methodology, Validation, Formal
analysis, Investigation, Writing - original draft, Visualization. Berggren
 T. Uddh Söderberg et al. / Science of the Total Environment 668 (2019) 1064–1076
Kleja: D.Conceptualization, Methodology, Validation, Formal analysis, In-
vestigation, Writing - original draft, Visualization. Åström: M.Conceptu-
alization, Investigation, Writing - review & editing, Funding acquisition.
Jarsjö: J.Conceptualization, Investigation, Writing - review & editing,
Funding acquisition. Fröberg: M.Investigation, Writing - review &
editing, Funding acquisition. Svensson: A.Formal analysis, Writing - re-
view & editing. Augustsson: A.Conceptualization, Methodology, Valida-
tion, Formal analysis, Investigation, Writing - original draft, Supervision,
Project administration, Funding acquisition.
Acknowledgement
Commercial laboratory Actlabs in Canada, Forest Research labora-
tory in England and ALS Scandinavia AB in Sweden are acknowledged
for excellent analyzes on soil and water samples. We thank Magnus
Törnqvist, a former Bachelor student in hydrology at Stockholm Univer-
sity, for assistance in establishing the delineation of the local catchment
area, and Gitte Laallam, a former Master student in hydrology at
Stockholm University, for assisting in the establishment of the hydraulic
conductivity at the landfill, and finally Malin Ekstedt (Environmental
Office in Nybro Municipality) and David Lokranz (the County Adminis-
trative Board) for their engagement in the project.
Funding: Financial support for this study was provided by the Swed-
ish Geological Survey (grant number 36-1778/2014), the Faculty of
Health and Life Sciences at Linnaeus University and the Swedish Geo-
technical Institute.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.scitotenv.2019.03.013.
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