Environmental Pollution 156 (2008) 809–817

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Environmental Pollution
journal homepage: www.elsevier.com/locate/envpol

Relationships between organic matter, black carbon and persistent organic

pollutants in European background soils: Implications for sources and
environmental fate
Jae Jak Nam a, b, Orjan Gustafsson c, Perihan Kurt-Karakus a, Knut Breivik d, e,
Eiliv Steinnes f, Kevin C. Jones a, *
a
Centre for Chemicals Management and Environmental Science Department, Lancaster Environment Centre, Lancaster University, Lancaster LA1 4YQ, United Kingdom
b
National Institute of Agricultural Science and Technology, RDA, 249 Sedun, Suwon 702-701, Republic of Korea
c
Department of Applied Environmental Science (ITM), Stockholm University, 10691 Stockholm, Sweden
d
Norwegian Institute for Air Research, P.O. Box 100, NO-2027 Kjeller, Norway
e
University of Oslo, Department of Chemistry, P.O. Box 1033, NO-0315 Oslo, Norway
f
Department of Chemistry, Norwegian University of Science and Technology, NO-7491 Trondheim, Norway

Total organic carbon and black carbon fractions can play an important role in the storage and cycling of persistent organic pollutants in
background soils.

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

Article history: Black carbon (BC) and total organic carbon (TOC) contents of UK and Norwegian background soils were
Received 20 November 2007 determined and their relationships with persistent organic pollutants (HCB, PAHs, PCBs, co-planar PCBs,
Received in revised form 29 May 2008 PBDEs and PCDD/Fs) investigated by correlation and regression analyses, to assess their roles in influ-
Accepted 30 May 2008
encing compound partitioning/retention in soils. The 52 soils used were high in TOC (range 54–460 mg/g
(mean 256)), while BC only constituted 0.24–1.8% (0.88%) of the TOC. TOC was strongly correlated
Keywords: (p < 0.001) with HCB, PCBs, co-PCBs and PBDEs, but less so with PCDD/Fs (p < 0.05) and PAHs. TOC
Persistent organic pollutants
explained variability in soil content, as follows: HCB, 80%; PCBs, 44%; co-PCBs, 40%; PBDEs, 27%. BC also
Soil organic matter
Black carbon
gave statistically significant correlations with PBDEs (p < 0.001), co-PCBs (p < 0.01) and PCBs, HCB, PCDD/
Environmental fate F (p < 0.05); TOC and BC were correlated with each other (p < 0.01). Inferences are made about possible
combustion-derived sources, atmospheric transport and air–surface exchange processes for these
compounds.
Ó 2008 Elsevier Ltd. All rights reserved.

1. Introduction
Organic matter (OM) plays an important role in the partitioning
of persistent organic pollutants (POPs). Batjes (1996) estimated that
there are w220  1011 tonnes of soil C, 70% of which is organic
carbon (OC), with carbonates comprising the remainder. The soil C
pool is triple that present in the atmosphere (76  1011 t) and about
two or three times larger than in the living matter of all terrestrial
ecosystems (Post et al., 1990; Prentice et al., 1998). OM has been
accepted as the principal factor in controlling sorption of organic
chemicals in soils and sediments (Lambert, 1968; Burgess and
Lohmann, 2004; Cornelissen et al., 2005; Sweetman et al., 2005).
Soil organic matter (SOM) is composed of amorphous organic
matter (AOM) and carbonaceous materials such as black carbon
* Corresponding author.
E-mail address: k.c.jones@lancaster.ac.uk (K.C. Jones).
(BC), coal and kerogen. The OM content of soils varies widely, being
particularly abundant in temperate forests, grasslands and peat.
The median contribution of BC as a fraction of total organic carbon
(TOC) is reportedly w4% for soils and w9% for sediments (e.g.
Gustafsson and Gschwend, 1998; Middelburg et al., 1999; Guo et al.,
2004; Cornelissen et al., 2005). BC and other carbonaceous material
has attracted considerable interest from environmental chemists,
because its sorption capacity for some hydrophobic organic com-
pounds (HOCs) may be at least 10–100 times higher than that of
AOM; it is considered a ‘super-sorbent’, and believed to be re-
sponsible for a large part of the sorption/partitioning of some HOCs
in soils and sediments (Gustafsson et al., 1997; Bucheli and
Gustafsson, 2000; Accardi-Dey and Gschwend, 2002; Cornelissen
and Gustafsson, 2005; Cornelissen et al., 2005; Lohmann et al.,
2005). Recent studies have focussed on the contribution of BC and
SOM to the partitioning of POPs in soils, sediments, and atmo-
spherically transported particles, and their environmental longev-
ity (e.g. Gustafsson and Gschwend, 1997; Beyer et al., 2000; Persson

0269-7491/$ – see front matter Ó 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.envpol.2008.05.027
810 J.J. Nam et al. / Environmental Pollution 156 (2008) 809–817
et al., 2002; Meijer et al., 2003; Bucheli et al., 2004; Burgess and
Lohmann, 2004; Cornelissen and Gustafsson, 2004, 2005; Lohmann
et al., 2005).
POP is a generic term, encompassing several families of com-
pounds. They have certain features in common; they are persistent
in the environment, have low aqueous solubilities and high affini-
ties for lipids and organic matter. Indeed, their partitioning to OM
strongly contributes to their environmental persistence. Many POPs
are also ‘semi-volatile’ under ambient temperatures and may exist
in the vapour phase in the atmosphere. They may be subject to
long-range atmospheric transport (LRAT) and undergo repeated
air–surface exchange (‘hopping’), so that they may reach remote
environmental compartments/sinks over time (Wania and Mackay,
1993, 1996; Beyer et al., 2000; Klecka et al., 2000; Meijer et al.,
2003; Sweetman et al., 2005). For example, POPs includes the
polychlorinated dibenzo-p-dioxins and -furans (PCDD/Fs), poly-
chlorinated biphenyls (PCBs) and some organochlorine (OC) pes-
ticides. Related chemical classes include the polybrominated
diphenyl ethers (PBDEs) and the polycyclic aromatic hydrocarbons
(PAHs). Different POPs have different sources into the environment.
Some have been intentionally produced (e.g. the PCBs and PBDEs),
others have been deliberately released into the environment (OC
pesticides). Others are formed and released accidentally during
incomplete combustion, such as the PCDD/Fs and PAHs. Some may
be either accidentally formed or incidentally released from various
combustion processes (co-PCBs, PCBs and PBDEs). Some POPs may
therefore enter the environment as an atmospheric emission as-
sociated with BC, from a range of incomplete combustion processes.
Examples include: natural (e.g. forest) fires, domestic burning of
coal or wood, accidental fires, ‘trash’ or ‘backyard burning’ and
vehicle exhausts. Several of these have been implicated as sources
for PCDD/Fs (Sakai et al., 1993; Yasuhara et al., 2003).
There is also evidence that BC can be an important component
of the atmospheric aerosol, capable of influencing POPs partition-
ing and transport (Ribes et al., 2003; Bucheli et al., 2004; Lohmann
and Lammel, 2004; Cornelissen et al., 2005). BC is typically a few
percent of the atmospheric aerosol burden; it constitutes several
Fig. 1. Possible scenarios for the relationship between POPs and SOM (with a focus on BC) and the inferences which can be made about their sources, fate, and transport.
hundred ng/m3 in air in rural locations and several thousand ng/m3
in urban centres (Lohmann and Lammel, 2004). POPs sources may
be numerous, diverse and with uncertainties over their relative
contribution. For example, hexachlorobenzene (HCB) is a pesticide,
an industrial chemical and intermediate, and a combustion by-
product, as well as being re-volatilised from environmental sur-
faces, but it is rather unclear which source dominates (Barber et al.,
2005). There are also uncertainties over whether the environ-
mental occurrence of co-PCBs are primarily caused by accidental
formation during combustion (Sakai et al., 1993; Yasuhara et al.,
2003), volatilization from technical PCB mixtures containing traces
of co-PCBs (Breivik et al., 2002b; Takasuga et al., 2006) or incidental
combustion of such mixtures (Breivik et al., 2002a,b). International
regulations are restricting production and emissions of POPs
(UNECE, 1979; UNEP, 2001).
Soils are important to the global cycle of POPs; they receive POPs
via atmospheric deposition or direct applications and have sub-
stantial storage capacity for POPs, which is a function of their OM
content/type. A series of articles draws attention to the role of
background soils (i.e. those in rural/remote areas and receiving only
atmospheric deposition) in global POPs budgets and air–surface
exchange and the influence of SOM on these processes (Meijer
et al., 2002, 2003; Hassanin et al., 2004, 2005; Nam et al., 2008).
This article extends the studies on POPs in background soils, by
examining their relationship with different fractions of SOM. Spe-
cifically, BC and TOC are quantified in a set of well characterized
background surface soils from western Europe, chosen because
they reflect regional trends in atmospheric deposition/exchange of
POPs (see Meijer et al., 2002), which have been analyzed previously
for HCB, PAHs, PCBs, PBDEs, co-PCBs and PCDD/Fs. Correlation and
regression analysis are used to make inferences about the likely
sources, atmospheric transport, re-cycling and SOM interactions of
these POPs. Fig. 1 presents a conceptual approach which is used to
discuss the data. It shows different scenarios for how a relationship
between POPs and BC, TOC/SOM may develop in the environment,
and how the analysis of background soils can help to shed light on
their relative importance. Associations can develop between a POP
 J.J. Nam et al. / Environmental Pollution 156 (2008) 809–817 811

and BC during emission, transport/deposition, or in the soil itself.

(142–3140)

(21–4440)
(21–4440)
(69–3140)
PCDD/Fs (pg/g)

(69–792)
Alternatively, a POP may not form an association with BC, because
they did not ‘meet’ on their journey from source to soil. Presumably
there will be differences between chemicals and locations/envi-

726

718
1090
279

706
ronments in the likelihood of these associations developing – de-
pendent on the contribution in time and space of the different
sources of POP and BC. The purpose here was to use the data set to

Co-PCBs (pg/g)

(6.0–483)
(6.0–251)
(9.2–251)

(12–483)
(6.0–60)
explore these issues.

2. Materials and methods

101

63.6
128
17.6

89.7
2.1. Soil samples and POP analysis

(135–3010)
The soils for this study were originally sampled from remote/rural woodland

(65–6080)
(80–6080)

(65–6080)
(65–2350)
(WL) (coniferous and deciduous) and grassland (GL) locations, on a latitudinal

PBDEs (pg/g)
transect through the UK and Norway in 1998 (see Meijer et al., 2002 for details).
Surface (0–5 cm) samples were collected after removal of the litter layer with
a stainless steel core sampler. Details of the method, sample information, and

2570

1780
1270
1570
812
properties of the soils have been published previously (Meijer et al., 2002, 2003;
Hassanin et al., 2004, 2005; Nam et al., 2008). The surface 5 cm contains higher SOM
than the sub-surface samples, typically representing decades/centuries of accu-

(1240–12 940)

(1010–22 490)
mulated SOM.

(303–22 490)
(303–12 940)
(303–3110)
2.2. TOC, BC and OM analysis

PCBs (pg/g)
TOC and BC were determined at Stockholm University on 10–100 mg samples.

3810
6410
5940
1230

4680
The soil was first finely ground for 20 min in an automatic ball grinder. TOC analysis
used an elemental analyzer (Carlo Erba, Italy) after samples were treated with HCl in
order to eliminate possible carbonate residues. Full details are given in Gustafsson
et al. (1997). The detection limit of the analyzer was 4.9 mg for C, measured from the

(8.6–11180)
(42–11180)
(56–11180)

(8.6–1055)
(42–4855)
long-term running average (n ¼ 41) of the blank, plus three times the standard

PAHs (ng/g)
deviation of the blank. The BC content was determined with the chemothermal
oxidation method (Gustafsson et al., 1997, 2001; Elmquist et al., 2006). Then,

Geometric means are used and the number of samples used are 27 (woodland, 15; grassland, 12) for UK and 26 for Norway.
amorphous non-pyrogenic organic carbon (OC) was subsequently removed in

641
580

154
318
704
a thermal oxidation procedure at 375  C in a tube furnace continuously supplied
with an atmosphere of air. Thereafter, inorganic carbon (IC) was removed by a mild
acidification in situ in Ag capsules. Total SOM content had also been measured
previously by loss-on-ignition at 450  C at Lancaster University (Meijer et al., 2002,

(159–4110)

(3.9–5210)
(22–5210)
(22–4110)
(22–681)
2003). HCBc (pg/g)

2.3. Statistical methods

880
190
569
1760
1050
Statistical analysis was performed using the programme S-Plus 6 (Insightful
Corp., WA, USA). The correlation between variables was estimated by the standard
Pearson sample correlation coefficient (r). A simple least-square regression model
(15–97)
(11–60)
(17–97)

(11–97)

(11–97)

was applied between variables, and a slope, regression coefficient (R2), and p-value
were derived. The POP, TOC, and BC data were log-normally distributed. They were
OM (%)

therefore logarithmically transformed for statistical analysis. Any sample with data
56

42.1
25.1

77.3
56.3

below the detection limit was eliminated from statistical analysis. A total of 53
samples were used for statistical analysis.
The numbers in parentheses are the number of samples used for statistics.
TOC (mg/g dw)
(79–454)

(54–454)
(86–460)
(55–268)

(54–460)

3. Results and discussion

3.1. General comments on POP concentrations

The numbers in parentheses represent the ranges of the data.
189
365
256
249
104

Table 1 presents mean and range concentrations for HCB, PAHs,

PCBs, PBDEs, co-PCBs and PCDD/Fs for the UK and Norwegian soils.
(0.55–1.64)

(0.45–3.13)
(0.49–2.0)b

(0.45–3.13)
(0.49–2.0)
BC (mg/g dw)

Differences of up to 3–4 orders of magnitude in a given compound/

class were observed in the sample set. The UK is much more heavily
industrialized and with a much higher population and population
1.22
1.36
1.35
1.07

1.27

density than Norway (ca. 60 and <5 million people nationwide, and
243 and 15 people/km2, respectively), leading to the assumption
that UK background soils would generally contain higher POP
Woodland (17)a
Grassland (14)

concentrations. However, HCB, PAHs, PCB, and co-PCB concentra-

tions were, on average, two to four times higher in the Norwegian
All (31)

soils than the UK soils on a dry weight basis; PCDD/F concentrations

were similar in the two countries and PBDEs were slightly higher in
Summary of the data

the UK soils. Differences with land usage were also noted. Wood-
land soils had up to five times higher concentrations than in
Sampling sites

Norway (21)

matched grassland soils. This may be explained by differences in

scavenging/deposition mechanisms between woodland and grass-
All (52)
Table 1

land soils (Meijer et al., 2002), and/or the turnover/mixing pro-

UK

b
c
a

cesses and degradation rates operating in different soil systems

812 J.J. Nam et al. / Environmental Pollution 156 (2008) 809–817

(Hassanin et al., 2004). The paradigm about these background soils
primarily simply reflecting proximity to sources therefore appears
to be incorrect. Rather, the soils appear to be more reflective of ‘sink
conditions’ – their tendency to receive (i.e. to scavenge gaseous and
particulate POPs via the canopy, or to receive high loadings of wet
deposition due to location), and retain those inputs (e.g. in higher
OM content soils of colder environments).
3.2. Comments on the methodology to determine BC
BC comes in different forms (e.g. charred, soot, graphite), as
discussed by Elmquist et al. (2006). This is one of the several rea-
sons why the determination of BC in environmental samples is
challenging (Hammes et al., 2007); no one method is optimal for all
BC forms. OC-rich matrices such as peat are particularly challenging
(e.g. Gustafsson et al., 2001). The CTO-375 method employed here
is the most widely used and has been the most thoroughly evalu-
ated in inter-laboratory comparisons and in applications to differ-
ent BC standard materials. Indeed, it appears to provide favorable
results in inter-comparisons (e.g. Middelburg et al., 1999; Elmquist
et al., 2004; Hammes et al., 2007). It is good for measuring soot-BC
but is not able to measure all char-BC (Elmquist et al., 2006;
Hammes et al., 2007).
One concern with samples of high TOC is that charring can occur
during the BC determination, thus producing artifacts. This was
a question that arose in the study, because several of these surface
soil samples had very high TOC contents. However, there are good
reasons to believe that the BC determinations reflect the field sit-
uation, rather than analytical artifacts. These are:
a. laboratory tests of potential charring suggest little influence
from most OM matrices, but with the greatest effects when
analyzing plankton and N-rich macromolecules, rather than
soils (e.g. Gustafsson et al., 1997, 2001; Hammes et al., 2007);
b. the CTO-375 method reports lower BC than other methods,
indicating that there will be less risk of inadvertent inclusion of
non-BC OM (e.g. Currie et al., 2002; Hammes et al., 2007);
c. CTO-375-based BC measurements are better able to explain the
environmental distribution of PAHs and PCDD/Fs in field
samples than TOC (e.g. Gustafsson and Gschwend, 1997; Pers-
son et al., 2002; Cornelissen et al., 2006). This would not be the
case if BC were an artifact of charred OC production; and
d. the relations between soil PAHs and TOC and BC have been
examined in detail elsewhere (Nam et al., 2008) and will not be
discussed in great detail here. Note, however, that this study
showed that a range of PAH compounds correlate with BC in
the UK woodland samples, while they do not correlate with
TOC. Such results would simply not be possible if the BC
measurements were faulty or an artifact of TOC charring during
the CTO-375 procedure. For these reasons, we have confidence
in discussing the relationships between soil BC and HCB, PCBs,
PBDEs and PCDD/Fs here.
content of the Norwegian soils (86–460, mean of 365 mg/g dw) was
about two times that of the UK samples (54–454, mean of 189 mg/
g dw). Similar BC contents have been reported for surface soils from
Switzerland (mean of 1.9 mg/g), but TOC contents measured here
were about four times higher than those in the Swiss samples
(mean of 65 mg/g) (Bucheli et al., 2004). BC was therefore a small
proportion of the TOC in all the samples – between 0.24 and 1.81%
(mean 0.88%) in the UK soils and between 0.14 and 1.52% (mean
0.42%) in the Norwegian ones.
Some differences were observed between the UK grassland and
forest soils (see Table 1). As expected, the grassland had lower TOC
contents (range of 55–268 mg/g (104), compared to 79–454 mg/g
(249)), but also a narrower range and average BC composition
(range of 0.55–1.64 mg/g (1.07), compared to 0.49–2.0 mg/g (1.35)).
The narrow range in soil BC values reflects the ‘background’ nature
of these soils, since large BC particulates settle out close to source
(e.g. tens micro meter from local fires and fossil fuel burning), and
the background environment receives a fairly uniform deposition
of the finer aerosols (e.g. a micro meter or so, from wood burning,
etc.) which undergo LRAT. It therefore might be presumed that the
low ratio (<1%) of BC to TOC would cause POP partitioning to SOM
to be dominated by TOC rather than BC in these soils. Soil BC
loadings represent cumulative inputs, over many centuries pre-
dominantly via combustion. Much of this historically derived ma-
terial is via natural (biomass) burning (Druffel, 2004; Preston and
Schmidt, 2006), and – because of the stability of soil BC – will pre-
date the inputs of several compound classes. In more recent times it
will include inputs from fossil fuel burning.
3.4. Correlation analyses with the whole data set
Correlation coefficients derived for the whole sample data set
are presented in Table 2. The same exercise was also performed on
subsets of the soils, namely the UK soils only (‘UK all’), the UK
woodland soils (‘UK wood’), the UK grassland soils (‘UK grassland’),
and the Norwegian soils (‘Norway only’) (see SI Tables 1–4).
3.4.1. Correlations between C parameters
When the set of soils was taken as a whole, BC and TOC were
statistically correlated at the p < 0.01 level. They were also corre-
lated in the subset of UK soils (at the p < 0.001 level).
3.4.2. Correlations between TOC/BC and POPs
There were highly significant (p < 0.001) correlations with TOC
for HCB, PCBs, co-PCBs, PBDEs (and p < 0.05 for the PCDD/Fs) across
the whole set of soils (Table 2). Although total PAHs did not cor-
relate with TOC across all the soils, selected individual compounds
did (Nam et al., 2008). These correlations provide clear evidence of
the role of AOM in retention of POPs in soils.
Table 2 also presents the correlation coefficient data between
POPs and soil BC content. For each compound/class, there was also
a statistically significant correlation with BC, although it was lower

3.3. General comments on BC and TOC concentrations Table 2

Correlation coefficients for all soilsa

Data on the soil BC and TOC contents are presented in Table 1. BC TOC HCB PCBs PBDEs Co-PCBs PCDD/Fs PAHs
TOC data – which showed a very strong correlation with SOM BC 1.00
(r ¼ 0.98***; significant at P < 0.001 level) – were used for the sta- TOC 0.41** 1.00
tistical analysis. The range (mean) values for BC, TOC and OM were HCB 0.32* 0.89*** 1.00
PCBs 0.34* 0.72*** 0.78*** 1.00
0.45–3.13 (1.3) mg/g, 54–460 (256) mg/g, and 11–97 (56)%, re-
PBDEs 0.60*** 0.57*** 0.47*** 0.46*** 1.00
spectively. These ranges were less than an order of magnitude for Co-PCBs 0.39** 0.64*** 0.46*** 0.90*** 0.34* 1.00
each C parameter – much less than for the POP concentrations. PCDD/Fs 0.34** 0.31* 0.32* 0.73*** 0.44*** 0.69*** 1.00
There was also very little difference for these three parameters PAHs 0.08 0.18 0.23 0.00 0.07 0.10 0.44** 1.00
between the UK and Norwegian soils. The BC contents were 0.49– *p < 0.05, **p < 0.01, ***p < 0.001; the data were log-transformed before analysis.
a
2.0 (1.22) and 0.45–3.13 (1.36) mg/g dw, respectively, while the TOC N ¼ 53.
 J.J. Nam et al. / Environmental Pollution 156 (2008) 809–817
than for their relationship with TOC. Although HCB, PCBs, and
PCDD/Fs were correlated to BC, the coefficients are quite low. Of all
the compound groups, the correlation with PBDEs was the most
statistically significant (p < 0.001). In terms of the concepts pre-
sented in Fig. 1, these results indicate that POPs reaching these
European background soils may either have been emitted together
with BC (process 1A in Fig. 1), and/or been deposited to soils fol-
lowing atmospheric transport (2B) and/or become associated with
each other in the surface soils (process 4B). However, as just noted,
they have a stronger association with TOC. This may be – at least in
part – because BC constitutes on average <1% of the TOC (Nguyen
et al., 2004), but it may also vary with location. However, it is clear
that AOM plays a more important role in partitioning and retention
of POPs in the soil system than BC.
As just noted, PBDEs have the strongest association with BC. One
explanation may be that emissions from incomplete combustion
represent a more significant source of PBDEs than previously
imagined (e.g. releases during accidental fires) (e.g. Farrar et al.,
2004). PBDEs may be more affected by local pollution sources
rather than LRAT, compared to other POPs. If this is the case, it is
perhaps surprising that the co-PCBs and PCDD/Fs – compound
groups with a clearer source inventory link to incomplete com-
bustion should not show a similar correlation (see below for further
discussion).
3.4.3. Correlations between the compound groups
POP concentrations generally correlate very strongly with each
other in these European background soils (Table 2). HCB, PCBs,
PBDEs, co-PCBs and PCDD/Fs are all highly significantly correlated
with each other (with an exception – see below). This indicates that
these POPs’ families generally share common source areas (e.g.
urban/populated locations) and atmospheric transport/deposition
pathways and/or they are similarly retained by common soil stores
(i.e. high OM soils may retard POP re-emissions and degradation in
general). The exception to the general observation just referred to is
that HCB is only correlated with PCDD/Fs at the p < 0.05 level. This
may be because: combustion sources are not so important for HCB
as other sources (e.g. past agricultural usage) (Meijer et al., 2003;
Barber et al., 2005), while they may be important for PCDD/Fs and
PBDEs (Hassanin et al., 2004) (i.e. PCDD/F and PBDE source areas
are predominantly urban, while HCB may be rural/urban); and/or
HCB is the most likely compound to undergo repeated air–surface
exchange, to find soils high in OM, while PBDEs and PCDD/Fs may
be retained more effectively by soils closer to their source. PCBs
provide an interesting case: co-PCBs are present in technical PCB
formulations (Takasuga et al., 2006) and it is therefore perhaps not
surprising that PCBs and co-PCBs have the highest correlation
coefficients between compounds (Table 2), reflecting common
sources. However, there are also differences between them, with
co-PCBs strongly correlated with BC (see SI Tables). This indicates
that the planar PCB and PCDD/F molecules have a stronger affinity
than the ‘regular’ PCBs for BC, as has been shown in sorption ex-
periments (e.g. Barring et al., 2002; Bucheli et al., 2004). For PCBs, it
appears that both combustion-derived and non-combustion-
derived emissions may be important as sources to the environment
(Sakai et al., 1993; Breivik et al., 2002a,b; Yasuhara et al., 2003),
because they correlate strongly with known combustion-derived
compounds (co-PCBs and PCDD/Fs), as well as with TOC.
3.5. Comments on country and soil type differences
Further insights into features and differences between the POPs’
families can be obtained by closer scrutiny of the data from the ‘sub-
sets’ of soils. Compound correlations with BC were observed in the
‘UK all’ data set (Fig. 3 and SI Table 1), whereas they did not when
the Norway data set was being considered (Fig. 3 and SI Table 2). All
813
the compound groups except PCDD/Fs (p < 0.05) were correlated
with BC at the p < 0.01 level in the UK soils. This indicates that the
atmospheric deposition of POPs in association with BC may be more
prevalent in the UK than Norway (i.e. process 1A in Fig. 1), and may
be simply explained by more limited LRAT of BC. However, caution is
needed in interpreting the data, because they also correlate strongly
with TOC (p < 0.01 for PCDD/Fs; p < 0.001 for others), and BC and
TOC correlate with each other (p < 0.001). All the compound groups
also strongly correlate with each other (p < 0.01 or stronger) –
except the PBDEs (not significant with co-PCBs, p < 0.05 with PCDD/
Fs and PCBs), reinforcing the observations about likely common
sources/sinks made earlier. This trend is much clearer if the UK
subsets of soils by land usage are considered (SI Tables 3 and 4).
The relationships between BC or TOC and compounds are gen-
erally less marked in the Norwegian soils. However, the correla-
tions between POPs’ classes in the Norwegian samples are almost
equal to or somewhat increased compared to the ones in the UK
soils, particularly for the PBDEs (SI Tables). An interpretation of
these observations is that sources/transport of POPs to the UK soils
involve some affiliation with BC, whilst their delivery to the more
remote locations of Norway involves alternative (‘non-BC-related’)
sources/transport. Another possibility is that there are different
sources of BC into the UK environment/soils than in Norway (e.g. in
the UK, more and varied anthropogenically related combustion
sources while in Norway, more forest/wood burning) (Novakov and
Hansen, 2004). The latter interpretation is particularly plausible
when considering the demographics and use of wood and fossil fuel
consumption in these countries.
3.6. Additional comments on compound differences
Some contrasting behaviour between compounds has been
highlighted by the data analysis:
i. HCB has rather unique behaviour amongst the compounds
studied. Its principle sources are not BC-related (Barber et al.,
2005). It is strongly associated with TOC across the full set of
soils (Table 2; SI Tables). It is known to move through the at-
mosphere predominantly in the vapour phase (Barber et al.,
2005), and to undergo air–surface exchange more readily than
the other classes of POPs being considered here (Meijer et al.,
2003; Barber et al., 2005). This has presumably facilitated the
development of the strong correlations with TOC/AOM
throughout the study soils. With respect to Fig. 1, HCB has
largely followed the pathways 1B, 2C, 3A and 4C displayed in
Fig. 1.
ii. PBDEs give a different picture. They are significantly associated
with BC throughout the data set in these background soils
from the UK – a major producer, user and emitter of these
compounds (as well as in Norway) (Hassanin et al., 2004;
Prevedouros et al., 2004). However, they have also formed
associations with TOC/AOM. There are thought to be several
routes by which PBDEs are emitted to the environment, and it
has generally been assumed that volatilization of vapour phase
compounds from treated products was the principle one
(Prevedouros et al., 2004). Such gas phase PBDEs may move
and be deposited, then become associated with TOC/BC in the
soils. However, some studies have shown elevated levels as-
sociated with diffuse combustion sources (Farrar et al., 2004;
Hassanin et al., 2004), and these may have been responsible
for emissions of PBDEs associated with BC, accounting for their
correlation in the UK soils. The lighter congener BDE-28 was
more correlated with TOC than BC, while the heavier BDE-99
was more correlated with BC (Fig. 4). So, with respect to Fig. 1,
there is evidence that PBDEs may have followed the pathways
1A and 1B, 2A, 2B and 2C, 3A, 4A and 4C.
814 J.J. Nam et al. / Environmental Pollution 156 (2008) 809–817

11
9 HCB PCBs
10
8

7 9

Log PCBs
Log HCB
6
8
5
7
4

3 UK : Y=1.44X+5.57 (r2=0.26**) 6 UK : Y=1.38X+7.64 (r2=0.28**)

NR : Y=0.14X+7.22 (r2=0.009) NR : Y=0.13X+8.38 (r2=006)
2 5
-1.0 -0.5 0.0 0.5 1.0 1.5 -1.0 -0.5 0.0 0.5 1.0 1.5
Log BC Log BC

8
PBDEs CoPCBs

8 6

Log CoPCBs
Log PBDEs

6 4

4 2
UK : Y=1.77X+6.62 (r2=0.29**)
UK : Y=1.74X+3.45 (r2=0.30**)
NR : Y= 0.84X+6.79 (r2=0.35**) NR : Y=0.52X+4.39 (r2=0.08)
2
-1.0 -0.5 0.0 0.5 1.0 1.5 -1.0 -0.5 0.0 0.5 1.0 1.5
Log BC Log BC

9 PCDD/Fs 10 PAHs

8 8
Log PCDD/Fs

7
Log PAHs

6
6

5 4
4
2
3 UK : Y=1.06X+6.00 (r2=0.20**) UK : Y=0.78X+6.40 (r2=0.05)
NR : Y=0.72X+5.75 (r2=0.09) NR : Y=-0.18X+5.17 (r2=0.007)
2 0
-1.0 -0.5 0.0 0.5 1.0 1.5 -1.5 -1.0 -0.5 0.0 0.5 1.0 1.5
Log BC Log BC

Fig. 2. Regression analysis of POPs with soil BC (captions: UK – - and black line; Norway – , and red line).

iii. Source inventories have pointed to the importance of in- with respect to the emissions of lighter congeners and in-
complete combustion processes as major sources of PCDD/Fs cineration/fires for heavier congeners (Breivik et al., 2002a,b).
and co-PCBs. Field measurements in the rural UK and else- As shown in Fig. 2, the distribution of lighter PCBs can be
where have shown elevated ambient levels linked to domestic explained more effectively by TOC than the heavier ones. With
burning of coal and wood, and the association of PCDD/Fs with respect to Fig. 1, PCBs followed the pathways 1A/B, 2A/B/C, 3A/
BC aerosols (Lohmann et al., 2005; Hassanin et al., 2005). In the B and 4A/B/C.
UK data set, they show significant correlations with BC
(p < 0.05). However, the PCDD/Fs have no correlation with BC
in the Norway data set. One explanation is that local com-
bustion sources such as forest fires and wood burning for
space heating play a more important role as a major BC source Table 3
in Norwegian soils. The relatively low ratio of BC/TOC in the UK Regression of TOC and BC against POP concentration for all soilsa
may be another explanation of the lower correlation than with All TOC BC
TOC. Low BC/TOC ratios in soils may result in POPs partitioning 2
Slope R Significance (p) Slope R2 Significance (p)
predominantly to the AOM. With respect to Fig. 1, it appears
HCB 1.55 0.84 <0.001 0.89 0.10 0.020
that PCDD/Fs and co-PCBs have followed the pathways 1A, 2A/
PCBs 1.01 0.52 <0.001 0.80 0.12 0.010
B, 3B and 4B. PBDEs 0.82 0.28 <0.001 1.32 0.27 <0.001
iv. PCBs and co-PCBs, like HCB, correlated very strongly to TOC. Co-PCBs 1.16 0.48 <0.001 1.19 0.19 0.001
However, they are also linked to BC in the UK. This indicates PCDD/Fs 0.53 0.13 0.008 0.88 0.13 0.008
some combustion-related sources. The major sources of PCBs PAHs 0.21 0.01 0.452 0.08 0.00 0.859
a
(and co-PCBs) are believed to be in urban areas – volatilization Y ¼ b þ aX, the data were log-transformed before analysis.
 J.J. Nam et al. / Environmental Pollution 156 (2008) 809–817 815

9 11
HCB PCBs
8 10
7
9

Log PCBs
Log HCB
6
8
5
7
4

3 UK : Y=1.45X-1.53 (r2=0.80***) 6 UK : Y=1.16X+1.98 (r2=0.60***)

NR : Y=1.31X-0.40 (r2=0.64***) NR : Y=0.97X+2.73 (r2=0.25*)
2 5
3.5 4.0 4.5 5.0 5.5 6.0 6.5 3.5 4.0 4.5 5.0 5.5 6.0 6.5
Log TOC Log TOC

8
PBDEs CoPCBs
7
8
6

Log CoPCBs
Log PBDEs

5
6
4

3
4
UK : Y=1.12X+1.25 (r2=0.35***) 2
UK : Y=1.23X-2.52 (r2=0.45***)
2
NR : Y=1.11X+0.48 (r =0.48 ***
) 1 NR : Y=1.14X-2.17 (r2=0.31**)
2
3.5 4.0 4.5 5.0 5.5 6.0 6.5 3.5 4.0 4.5 5.0 5.5 6.0 6.5
Log TOC Log TOC

9
PCDD/Fs 10 PAHs
8
8
7
Log PCDD/Fs

Log PAHs

6 6

5
4
4
2
3 UK : Y=0.81X+2.07 (r2=0.36***) UK : Y=-0.17X+7.32 (r2=0.007)
NR : Y=1.22X11.20 (r2=0.19*) NR : Y=1.15X-1.12 (r2=0.52***)
2 0
3.5 4.0 4.5 5.0 5.5 6.0 6.5 3 4 5 6
Log TOC Log TOC

Fig. 3. Regression analysis of POPs with soil TOC (captions: UK – - and black line; Norway – , and red line).

3.7. Regression analysis
Regression coefficients (R2) quantify predictive power, i.e. how
much of the variation in a data set can be explained by the model
applied. Regression coefficients were used to assess the roles of TOC
and BC in dictating POP concentrations in the soil. The slope, re-
gression coefficient (R2), and significance (p) of TOC and BC versus
POPs are presented in Table 3.
Overall TOC explained w84% of the concentration variation for
HCB, w52% for PCB and w28% for PBDE, using the simple least-
square regression (LSR) model. TOC was not useful to explain
the PCDD/Fs variation. By contrast, BC explained 27% or less of the
variation of POPs. TOC had a similar power to account for the
variation of POPs in the UK and Norway data sets (Fig. 3), while
the only situation where BC was a useful predictor of POP con-
centrations was to explain 20–30% in the UK subset (Fig. 2).
This may be because of proximity to pollution sources, as dis-
cussed previously. Nonetheless, even when BC is <1% of the TOC, it
can still explain over 20% of the variation in POP concentrations in
the UK soils. This is presumably because carbonaceous geo-
sorbents (CG) including BC exceed the sorptive capabilities of AOM
(Cornelissen et al., 2005).
The regression relationships are generally weaker in Norway,
where the average SOM content of the samples was >70%. This
abundance of SOM means it takes longer for compounds to ap-
proach steady state with the TOC, and make it harder for POPs to
encounter the comparatively small burden of super-sorbing BC in
this matrix. Secondly, POPs that are associated with BC in the at-
mosphere may have limited susceptibility for LRAT. HCB appears to
be approaching steady state with the TOC contents of European
background soils (Meijer et al., 2003; Barber et al., 2005), while the
PCBs and PBDEs are further from that situation.
3.8. A working hypothesis
The influence of BC on POPs behaviour has received a lot of at-
tention in the literature in recent years. Here, we show that in an
important ‘environmental compartment’ – global background soils –
the nature and extent of their interactions are varied and complex.
Our ‘working hypotheses’ following this study are as follows:
1. Most of the BC in soils originates from historical biomass
burning and fossil fuel combustion, which has accumulated over
many centuries. BC varied between a fairly limited range in these
816 J.J. Nam et al. / Environmental Pollution 156 (2008) 809–817

9
BDE 28 Y=1.08X+5.93 (r2=0.23***) BDE 28 Y=0.53X+3.40 (r2=0.16**)
8 BDE 99 BDE 99
8

Log BDE (pg/g soil)

Log BDE (pg/g soil)

7
6 6
5
4 4

3
2
2
Y=0.74X+3.13 (r2=0.17*) Y=0.73X-0.82 (r2=0.31**)
1
-1.0 -0.5 0.0 0.5 1.0 1.5 3.5 4.0 4.5 5.0 5.5 6.0 6.5
Log BC (mg/g soil) Log TOC (mg/g soil)

PCB 28 Y=0.79X+6.16 (r2=0.12*) PCB 28 Y=0.91X+1.43 (r2=0.43***)

PCB 138 8 PCB 138
8
Log PCB (pg/g soil)

Log PCB (pg/g soil)

6 6

4 4

2 2
Y=0.54X+3.71 (r2=0.05) Y=1.13X-2.28 (r2=0.61***)

-1.0 -0.5 0.0 0.5 1.0 1.5 3.5 4.0 4.5 5.0 5.5 6.0 6.5
Log BC (mg/g soil) Log TOC (mg/g soil)

Fig. 4. Regression analysis of PBDEs and PCBs with soil BC and TOC.

soils, in comparison to the POPs. One explanation for the lack
of – or limited – associations between BC and POPs in soils could
therefore simply be that the bulk of the soil BC is mainly con-
trolled by (cumulative) combustion inputs over many centuries.
2. If this is correct, any significant relationships between POPs and
BC emitted jointly from sources will be masked (‘diluted’) by
the stock of BC (especially for those POPs released to the en-
vironment principally in the last few decades).
3. This – in turn – suggests that whenever significant correlations
between non-combustion-derived POPs and BC do occur, this
may be favoured by POPs that are not extensively associated
with BC during emissions and transport, but are capable of: (i)
multi-hopping (semi-volatile and persistent); (ii) meeting BC
after residing some time in the soil (this is a function of the
relative affinities for BC among the POPs (i.e. those that are
planar) and soil turnover.
Further work should compare the findings of this study (biased
towards rural/remote soils high in TOC) with urban soils, and soils
from other climatic zones. It is hypothesized that both situations
may result in a greater prominence of BC in soil-OM associations.
Greater attention should also be given to better assessing the
contributions of the array of BC forms/domains on POP interactions.
Acknowledgements
J.J. Nam acknowledges the Civil Service Commission (Korea) for
financial support to perform research as a visiting scientist in
Lancaster University. The Lancaster group acknowledges the fi-
nancial support of the European Union AQUATERRA project.
Appendix A. Supplementary data
Supplementary data associated with this article can be found, in
the online version, at doi: 10.1016/j.envpol.2008.05.027.
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