Chemosphere 63 (2006) 365–377

www.elsevier.com/locate/chemosphere
Review

Black carbon: The reverse of its dark side

Albert A. Koelmans a,*, Michiel T.O. Jonker b, Gerard Cornelissen c,1,
Thomas D. Bucheli d, Paul C.M. Van Noort e, Örjan Gustafsson c
a
Department of Environmental Sciences, Aquatic Ecology and Water Quality Management Group (AEW),
Wageningen University, P.O. Box 8080, Ritsemabosweg 32a, 6700 DD Wageningen, The Netherlands
b
Institute for Risk Assessment Sciences (IRAS), Utrecht University, P.O. Box 80176, 3508 TD Utrecht, The Netherlands
c
Department of Applied Environmental Science (ITM), Stockholm University, 10691 Stockholm, Sweden
d
Agroscope FAL Reckenholz, Swiss Federal Research Station for Agroecology and Agriculture (FAL),
Reckenholzstrasse 191, CH-8046 Zürich, Switzerland
e
Institute for Inland Water Management and Wastewater Treatment (RIZA), P.O. Box 17,
8200 AA Lelystad, The Netherlands

Received 3 April 2005; received in revised form 10 August 2005; accepted 16 August 2005
Available online 13 October 2005

Abstract

The emission of black carbon is known to cause major environmental problems. Black carbon particles contribute to
global warming, carry carcinogenic compounds and cause serious health risks. Here, we show another side of the coin.
We review evidence that black carbon may strongly reduce the risk posed by organic contaminants in sediments and
soils. Extremely efficient sorption to black carbon pulls highly toxic polycyclic aromatic hydrocarbons, polychlorinated
biphenyls, dioxins, polybrominated diphenylethers and pesticides into sediments and soils. This increased sorption is
general, but strongest for planar (most toxic) compounds at environmentally relevant, low aqueous concentrations.
Black carbon generally comprises about 9% of total organic carbon in aquatic sediments (median value of 300 sedi-
ments), and then may reduce uptake in organisms by up to two orders of magnitude. This implies that current environ-
mental risk assessment systems for these contaminants may be unnecessarily safe.
Ó 2005 Elsevier Ltd. All rights reserved.

Keywords: Sorption; Bioavailability; Soot; Ecological risk

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 366
2. Strong sorption to pure BC materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 367
3. Predictive models for sorption to BC. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 369

*
Corresponding author. Tel.: +31 317 483201; fax: +31 317 484411.
E-mail address: bart.koelmans@wur.nl (A.A. Koelmans).
1
Present address: Norwegian Geotechnical Institute, P.O. Box 3930, Ullevaal Stadium, N-0806 Oslo, Norway. Tel.: +47 22023082;
fax: +47 22230448.

0045-6535/$ - see front matter Ó 2005 Elsevier Ltd. All rights reserved.
doi:10.1016/j.chemosphere.2005.08.034
366 A.A. Koelmans et al. / Chemosphere 63 (2006) 365–377

4. Sorption to BC in aquatic sediments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 369

5. BC reduces accumulation in aquatic organisms. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 371
6. Implications for management . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 372
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 373
References. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 373

1. Introduction nized to catalyze various chemical reactions in the atmo-

Black carbon (BC) is a product of weathering of gra-
phitic carbon in rocks (Dickens et al., 2004) and of
incomplete combustion of fossil fuels and vegetation
(Seiler and Crutzen, 1980; Goldberg, 1985; Carcaillet
et al., 2002; Cochrane, 2003). Incomplete combustion
of fossil fuels leads to re-condensation reactions in the
gas phase that produce highly aromatic globular struc-
tures in grape-like aggregates (soot) (Goldberg, 1985).
Besides soot, incomplete combustion of biomass also
yields less structured, carbonized residues from parental
materials (chars). The characteristics of BC (reviewed
elsewhere: Goldberg, 1985; Middelburg et al., 1999;
Schmidt and Noack, 2000; Allen-King et al., 2002; Mor-
awska and Zhang, 2002; Schmidt et al., 2002; Song
et al., 2002; Huang et al., 2003) vary widely, but gener-
ally, BC particles have a three-dimensional structure
composed of stacked aromatic sheets, particle sizes in
the nm–lm range, high but variable specific surface
areas (SSA) ranging from 2 to 776 m2/g (Bucheli and
Gustafsson, 2000; Karapanagioti et al., 2000; Jonker
and Koelmans, 2002a; Rockne et al., 2002; Braida
et al., 2003; Sander and Pignatello, 2005) and a nanop-
orosity in the <10 Å width range (Rockne et al., 2002;
Fernandes et al., 2003; Cornelissen et al., 2004a).
During the past century, increased biomass burning
and fossil fuel consumption have drastically increased
the input of BC to the environment (Griffin and Gold-
berg, 1983). Due to atmospheric circulation and surface
run-off, BC is dispersed hemisphere-wide and can be
found in the atmosphere (Novakov et al., 1974; Am-
mann et al., 1998; Buseck and Pósfai, 1999; Cochrane,
2003), soils (Glaser et al., 2000; Schmidt and Noack,
2000; Schmidt et al., 2002; Song et al., 2002; Bucheli
et al., 2004; Van den Heuvel et al., 2005), ice (Chylek
et al., 1992; Lavanchy et al., 1999; Hansen and Naza-
renko, 2004), in fresh water sediments (Gustafsson
et al., 1997; Gustafsson and Gschwend, 1997, 1998; Jon-
ker and Smedes, 2000; Schmidt and Noack, 2000; Mitra
et al., 2002; Song et al., 2002; Van den Heuvel et al.,
2005) and marine sediments (Smith et al., 1973; Masiello
and Druffel, 1998; Middelburg et al., 1999; Dickens
et al., 2004). Rivers may discharge considerable fractions
of the BC buried annually to the oceans (Mitra et al.,
2002; Mannino and Harvey, 2004). During the past dec-
ades, many negative effects of BC in the environment
have been reported. For example, BC has been recog-
sphere (Ammann et al., 1998; Buseck and Pósfai, 1999;
Cochrane, 2003) such as formation of nitrous acid,
which contributes to photochemical ozone and smog
formation. Furthermore, BC is an important constituent
of aerosols, highly capable of absorbing solar radiation,
thereby negatively influencing our climate (Charlock
and Sellers, 1980; Jacobson, 2001; Ramanathan et al.,
2001). Recently, it has been shown that precipitation
of black soot on snow may be responsible for 25% of
the observed global warming over the past century,
due to a reduced reflectance of sunlight on arctic ice
(Hansen and Nazarenko, 2004). Finally, BC has been re-
ported to cause several respiratory and cardiovascular
diseases in humans (Mumford et al., 1987; Ward,
1999; Morawska and Zhang, 2002; Avakian et al.,
2002; Armstrong et al., 2004). Particulate air pollution
contains ultra-fine soot globules that migrate deep into
the lungs and carry very toxic, often carcinogenic com-
pounds such as polycyclic aromatic hydrocarbons
(PAH) (Avakian et al., 2002; Morawska and Zhang,
2002; Armstrong et al., 2004). Many have lost their lives
due to air pollution related illnesses; especially asphalt-,
coke plant-, and gas-workers, chimney sweeps, carbon
electrode manufacturers, or victims of smoke related
accidents (Pott, 1775; Boglioli and Taff, 1995; Ward,
1999; Armstrong et al., 2004).
In contrast to these harmful effects, it was recently
discovered that BC also has an advantageous role in
the environment. Soots, chars, and soot-like materials
such as coal probably offer the most important binding
phases for PAHs in the environment (Gustafsson and
Gschwend, 1997; Dachs and Eisenreich, 2000; Jonker
and Smedes, 2000; Jonker and Koelmans, 2001; Jonker
and Koelmans, 2002a; Cornelissen et al., 2004a,b; Loh-
mann and Lammel, 2004; Lohmann et al., 2005). Like-
wise, they appear to act as ÔsupersorbentÕ for other,
man-made chemicals, such as polychlorinated biphenyls
(PCBs) (Jonker and Smedes, 2000; Jonker and Koel-
mans, 2002a; Bucheli and Gustafsson, 2003; Cornelissen
et al., 2004a), polychlorinated dibenzo-p-dioxins and
furans (Bärring et al., 2002; Persson et al., 2002), and
polybrominated diphenylethers (Bärring et al., 2002),
thereby connecting the global cycle of persistent organic
pollutants (POPs) to that of BC. Sorption of POPs to
BC is hypothesized to affect a large number of impor-
tant environmental processes, including global POP
transport, uptake and biomagnification of POPs in
 A.A. Koelmans et al. / Chemosphere 63 (2006) 365–377
organisms, and deposition of allochtonous POPs at con-
tinental margins. Hence, understanding the binding
mechanisms of POPs to BC is crucial for the under-
standing of human and ecological risks as well as the
global cycling of these chemicals.
In the late 1970s–early 1980s, the scientific commu-
nity reached consensus that the organic matter content
of soils and sediments was the main binding phase for
POPs (Chiou et al., 1979; Karickhoff et al., 1979). A sin-
gle partition coefficient for organic matter appeared to
suffice to quantify the equilibrium distribution of indi-
vidual POPs between water and sediments or soils. This
is the essence of the equilibrium partition theory (EPT)
(Chiou et al., 1979; Karickhoff et al., 1979), widely used
for POP risk assessment procedures in many Western
countries. During the past two decades, EPT persisted,
although a growing body of evidence showed that the
theory was too simple. Observations conflicting with
the one domain sorption model (as reviewed by Pigna-
tello and Xing, 1996; Luthy et al., 1997; Allen-King
et al., 2002; Huang et al., 2003) included (a) too high
in situ sediment–water partition coefficients (McGroddy
and Farrington, 1995; Pignatello and Xing, 1996; Ten
Hulscher et al., 1997; Jonker and Smedes, 2000), (b)
sorption competition among chemicals and non-linear
sorption isotherms (Pignatello and Xing, 1996; Huang
et al., 1997; Cornelissen et al., 2000), and (c) the occur-
rence of multiple desorption rates rather than a single
rate (Karickhoff and Morris, 1985; Brusseau et al.,
1991; Pignatello and Xing, 1996; Cornelissen et al.,
1997; Cornelissen et al., 2000). Even recent polyparame-
ter linear free energy relationships for natural organic
matter (Goss and Schwarzenbach, 2001; Nguyen et al.,
2005) cannot explain the elevated sorption observations
in the field. Consequently, explanations for these obser-
vations were sought in differences between in essence
two types of organic matter (Luthy et al., 1997). The
condensed (Weber et al., 1992, 1999), ÔglassyÕ (Xing
et al., 1996; Xing and Pignatello, 1997), or Ôhigh-sur-
face-area carbonaceousÕ (Chiou and Kile, 1998; Chiou
et al., 2000) structures of organic matter were held
responsible for the high in situ sorption strengths, the
very low desorption rates, and the non-linear and com-
petitive adsorption. Only the so-called ÔsoftÕ, Ôamor-
phousÕ (Weber et al., 1992, 1999), or ÔrubberyÕ (Xing
et al., 1996; Xing and Pignatello, 1997) domains of or-
ganic matter should allow fast, linear and non-competi-
tive partitioning as predicted by EPT. Consequently,
overall sorption behaviour has been described as Ôdual
mode sorptionÕ.
In summary, empirical data have convincingly re-
futed EPT and have shown that a refined, at least
dual-mode sorption model is needed. However, the nat-
ure of the condensed carbon phase and the modes of
sorption to this phase remained rather speculative until
the late 1990s. Only during the past few years, the pres-
367
ence of black carbon in sediments has convincingly been
linked to the aforementioned, deviant sorption observa-
tions and was proposed as their main explanation
(McGroddy and Farrington, 1995; Maruya et al.,
1996; Gustafsson and Gschwend, 1997; Gustafsson
et al., 1997; Chiou and Kile, 1998; Naes et al., 1998;
Kleineidam et al., 1999; Chiou et al., 2000; Jonker and
Smedes, 2000; Karapanagioti et al., 2000; Lohmann,
2003). Early observations that prompted the attention
to BC were high in situ sediment–water distribution
coefficients for pyrogenic PAHs (McGroddy and Far-
rington, 1995), significant regressions between sediment
soot content and distribution coefficients for PAHs
(Gustafsson and Gschwend, 1997; Gustafsson et al.,
1997), and higher distribution coefficients for PAHs
and PCBs with a planar molecular structure, as opposed
to non-planar PCBs, in BC containing sediment layers
(Jonker and Smedes, 2000). Recent investigations have
now proven that BC is capable of extremely efficiently
sorbing particular toxic chemicals. From an environ-
mental health perspective, the most important question
of course is, whether this binding is strong enough
to render these chemicals much less harmful than
anticipated.
In this paper, we (a) explain the strong sorption to
BC from recent mechanistic insights, (b) summarize
models for sorption to BC, (c) quantitatively elucidate
the role of BC in sorption to aquatic sediments, (d) high-
light the beneficial effects of BC in sediment for bioaccu-
mulation of POPs, and (e) deduce consequences for risk
assessment and decision makers.
2. Strong sorption to pure BC materials
The cause of the deviations from EPT lies in the high
affinity and non-linear sorption of POPs to free, high-en-
ergy sites on the BC surface. The availability of free sites
will be high in situations where BC particles and colloids
are freely dispersed in water, like in the marine or fresh
water column or in groundwater. Marine dissolved or-
ganic matter (DOM) was indeed hypothesized to con-
tain 4–22% of BC (Masiello and Druffel, 1998). Recent
studies provide direct evidence for the presence of BC
in estuarine (Mannino and Harvey, 2004) or riverine
(Kim et al., 2004) DOM. The detection of rock-weath-
ered petrogenic BC in pre-industrial marine sediments
also implies that riverine presence and transport of BC
is substantial (Mitra et al., 2002; Dickens et al., 2004).
In these aqueous environments, BC is expected to have
the highest accessibility for dissolved molecules, an ex-
cess of available surface compared to concentrations of
potentially competing co-adsorbates, and the lowest po-
tential blocking of sorption sites by other materials, e.g.,
humic substances. The affinity of POPs for ÔpureÕ BC in-
deed is extremely high (Fig. 1). It surpasses the affinity
368 A.A. Koelmans et al. / Chemosphere 63 (2006) 365–377
9 was unavailable for partitioning to water (Jonker and
8 for this fraction range from decades to millennia (Jonker
Log K (l/kg)
7 PAHs from BC is most effective with organic solvents
Native PAHs
PCDFs
6 added P AHs
PAHs
PBDEs
PCDDs
5 non ortho PCBs
ortho PCBs
EPT prediction
4
3 4 5 6 7 8
log Kow
Fig. 1. Selected (lab-derived) KBC values (added PAH/PCB,
native PAH; PCDFs, PCDDs, PBDEs; PAHs; ortho, non-ortho
PCB), measured with the polyoxymethylene solid phase extrac-
tion method (Jonker and Koelmans, 2001; Jonker and Koel-
mans, 2002a), or the soot cosolvency-column method (Bucheli
and Gustafsson, 2000, 2003; Bärring et al., 2002), as a function
of organic pollutant hydrophobicity (expressed as octanol–
water partition coefficient, Kow), and compared to EPT-
predicted sorption, according to log KOC = 0.97 log Kow  0.12
(Xia, 1998; Lohmann et al., 2005). All KBC values are on a mass
basis. Carbon mass-based KOC values are converted to organic
matter mass based KOM values using an approximate factor of 2
(KOC  2KOM). Kow values are from Hawker and Connell
(1988) (PCBs), Booij et al. (1998) (PAHs), Govers and Krop
(1998) (PCDD/Fs), and WHO/IPCS (1994) (PBDEs).
for ÔnormalÕ sediment or soil organic matter with up to
three orders of magnitude and the absolute height of
BC-water distribution coefficients (KBC) ranges up to
109 l/kg for native PAHs (Jonker and Koelmans,
2002a). In other words, for these chemicals EPT may
underestimate sorption to BC a thousand times. Yet,
the variation in reported values among chemicals and
types of ÔpureÕ BC is very large (Fig. 1). Apart from dif-
ferences in measuring methods employed, this variation
originates from four reasons: Differences in the mode of
POP fixation to BC, differences in POP loading, differ-
ences in type of BC, and differences in type of POP.
Below, we will briefly discuss these four factors.
First, in the literature, two modes of POP fixation are
proposed for BC particles: (a) physical occlusion inside
restricted pores or between aromatic macrostructures
during BC formation, and (b) reversible adsorption on
exterior and pore surfaces after BC formation. The
occlusion hypothesis partly stems from the observation
that native, BC-associated PAHs have much higher
KBC values than added PAHs (Jonker and Koelmans,
2001, 2002a). From the differences it was estimated that
within two months, still 50–95% of the native PAHs
Koelmans, 2002a). Supercritical fluid extraction of the
same native PAHs showed that typical removal times
et al., 2005). The occlusion hypothesis is further sup-
ported by the observation that solvent extraction of
that are capable of swelling the soot matrix (Jonker
and Koelmans, 2002b), thereby exposing any occluded
molecules (Jonker and Koelmans, 2002b; Braida et al.,
2003). Conversely, other observations point to a limited
importance of occlusion. Basically, combustion science
would predict PAHs to reside largely at the exterior of
soot particles (Siegmann et al., 2002), as was indeed
observed by electron microscopy for PAHs sorbed to
coal and charcoal (Ghosh et al., 2000). Furthermore,
for several BC samples (Niessner and Wilbring, 1989;
Panne et al., 2000) and samples containing BC (Water-
man et al., 2000), thermal desorption of PAHs appeared
to be complete within a few hours. The remaining frac-
tion of native PAHs is not internally occluded, but re-
sides on accessible (external) surfaces. There, they are
involved in Langmuir or Freundlich-type sorption equi-
libria (see below), based on Van der Waals interactions
(Toth, 2002; Schwarzenbach et al., 2003), and compete
with POPs from external sources (ÔaddedÕ or Ôallochton-
ousÕ chemicals) for the available surfaces. From these
two complementary fixation mechanisms (occlusion vs.
adsorption) we can explain the remaining three factors
that cause variation in KBC values.
Second, high POP loadings lead to lower KBC values
at the higher end of non-linear isotherms. This particular
non-linearity can be explained from variable site geome-
tries and energies, as well as from saturation of surface
adsorption sites. Nonlinear sorption for added chemicals
to pure BC, expressed through reported Freundlich coef-
ficients ÔnF,BCÕ in the Freundlich equation q ¼ K F;BC C nF;BC
(where q and C are the sorbed and dissolved concentra-
tions at equilibrium, and KF,BC is the Freundlich coeffi-
cient for sorption to BC) ranges from 0.24 to 1.0
(individual measurement average 0.62 ± 0.22, n = 12;
Bucheli and Gustafsson, 2000; Kleineidam et al., 2002;
Cornelissen and Gustafsson, 2004; Yang et al., 2004).
A few reports show statistically preferable (compared
to Freundlich) fits of sorption data to two-site Langmuir
models (Al-Bahrani and Martin, 1976; Sander and Pig-
natello, 2005), suggesting two distinct types of sites on
BC, but information on this is scant. Nevertheless, at
very low concentrations, monolayer adsorption by a
mechanistically singular process can be expected (Van
Noort et al., 2004). This monolayer adsorption can be
described with a Langmuir isotherm:
q ¼ bCQ=ð1 þ bCÞ ð1Þ
where Q is the maximum sorption capacity, and b is
the sorption affinity. Eq. (1) implies that KBC values
 A.A. Koelmans et al. / Chemosphere 63 (2006) 365–377
approach bQ at C < 1/b. At concentrations below
<100 ng/l, isotherm non-linearity was found to be not
significant (Accardi-Dey and Gschwend, 2002; Cornelis-
sen and Gustafsson, 2004) and KBC values can be com-
pared directly.
Third, different types of BC have different KBC val-
ues. This variation among different types of BC is clearly
reduced upon normalisation to BC specific surface area
(SSA; which is proportional to Q) (Bucheli and Gustafs-
son, 2000; Van Noort et al., 2004). Statistical analysis of
a consistent (one methodology, only linear portion of
isotherms) dataset (Jonker and Koelmans, 2002a) fur-
ther revealed that KBC for added PCBs and PAHs was
negatively correlated with the sorbentsÕ average pore-
diameter. This points to adsorption sites located in
micropores, which the added POPs may enter depending
on pore- and adsorbate size (Jonker and Koelmans,
2002a; Mastral et al., 2002; Yang et al., 2004). Reported
nanopore dimensions for BC (<4–10 Å, Gustafsson
et al., 2001; Rockne et al., 2002; Cornelissen et al.,
2004a) indeed are of similar magnitude as molecular
thicknesses of many POPs (Van Noort et al., 2003). Still,
different types of BC show considerable variation in SSA
and pore properties.
Fourth, as for adsorbate properties, KBC for native
PAHs was positively correlated to PAH molecular vol-
ume. This is consistent with the occlusion mechanism,
since larger PAHs will face more difficulties in leaving
the solid matrix due to steric hindrance. Nonetheless, this
also agrees to the surface association mechanism, since
larger PAHs also have larger surface for Van der Waals
interaction (Jonker and Koelmans, 2002a; Schwarzen-
bach et al., 2003; Van Noort et al., 2004). For added
PCBs and PAHs, indeed, correlations have been reported
with molecular surface area (Jonker and Koelmans,
2002a; Van Noort et al., 2004), as well as with molecular
planarity (Jonker and Koelmans, 2002a; Cornelissen
et al., 2004a), and hydrophobicity, as parameterized by
the octanol-to-water partition coefficient, Kow (Bärring
et al., 2002; Jonker and Koelmans, 2002a). These corre-
lations can be understood by taking a closer look at pro-
cesses occurring at the molecular level.
3. Predictive models for sorption to BC
Models for sorption of POPs to BC are important,
because we need estimation methods for the thousands
of chemicals that never will be tested in expensive and
laborious experimental studies. To date, two thermo-
dynamic models have been reported (Gustafsson and
Gschwend, 1997; Van Noort, 2003) that estimate the
Langmuir affinity b in Eq. (1). Because BC is composed
of macro-aromatic structures (Goldberg, 1985; Gustafs-
son and Gschwend, 1997; Allen-King et al., 2002), both
models assume that adsorption to BC surfaces is ther-
369
modynamically similar to sorption onto pure PAH crys-
tals. Hence, differences among BC types are supposed to
originate from differences in maximum sorption capaci-
ties (Q in Eq. (1)), not from differences in intrinsic Lang-
muir affinities (b in Eq. (1)). The first published model
(Gustafsson and Gschwend, 1997) uses inputs of the
chemicalÕs subcooled liquid aqueous solubility, melting
point, and melting entropy, as well as an estimate of
the BC SSA, and assumes that PAH sorption can be
considered as a fusion (solid precipitation) onto a planar
BC surface. Upon sorption the molecules loose degrees
of freedom with respect to rotation and translation. This
model provided reasonable estimates of KBC for four
compounds on one type of BC that was obtained by
controlled chemo-thermal oxidation of sediment at
375 °C (Gustafsson and Gschwend, 1997; Cornelissen
et al., 2004a). The second model (Van Noort, 2003) uses
inputs of the chemicalÕs solid solubility and melting en-
tropy, and of BCÕs SSA. This model assumes the sorbed
state to be that of a translationally restricted, two-
dimensional rotationally restricted sorbed (2D-RRS)
gas. Analyses of various datasets with this model (Van
Noort, 2003; Van Noort et al., 2004, 2005) showed that
POP sorption to BC is (a) proportional to SSA, (b)
lower for compounds with a larger adsorbate–sorbent
contact area, (c) lower for non-planar, ÔthickÕ sorbates,
and (d) higher for adsorbents with a higher organic car-
bon fraction (fOC). So, for non-planar, ÔthickÕ sorbates
less surface is available, which points to sorption in
micropores, an observation that fully agrees with the
abovementioned correlation of KBC values with average
pore diameter (Jonker and Koelmans, 2002a).
In summary, recent empirical data and conceptual
models fit into one consistent view that reversible sorp-
tion to ÔpureÕ BC is surface adsorption with a probable
contribution of surfaces in pores. SSA, organic carbon
fraction, contact area, and sorbate ÔthicknessÕ can ex-
plain the major part of the variation in BC-water distri-
bution coefficients at low aqueous concentrations
(Bucheli and Gustafsson, 2000; Jonker and Koelmans,
2002a; Van Noort et al., 2004). The high contact area
between adsorbing chemicals and the planar, PAH-like
BC surfaces, and the high SSA of BC explains the extre-
mely high sorption. An important question, however, is
whether this strong sorption behavior also applies to BC
in sediments.
4. Sorption to BC in aquatic sediments
If both absorption in organic matter and adsorption
to BC contribute significantly to overall sorption of
POPs to sediments, the non-linear Langmuir isotherm
(1) for BC can be extended with a term for linear sorp-
tion to ÔnormalÕ organic matter, to explain experimental
data in the pg/l–lg/l range. In the vast majority of
370 A.A. Koelmans et al. / Chemosphere 63 (2006) 365–377
studies, however, to this end a linear sorption term is
combined with a more empirical Freundlich term: The
first and second term in Eq. (2), respectively (Accardi-
Dey and Gschwend, 2002, 2003; Cornelissen and
Gustafsson, 2004; Cornelissen et al., 2004b; Lohmann
et al., 2005):
q ¼ fOC K OC C þ fBC K F;BC C nF;BC ð2Þ
where KOC is the organic carbon normalised partition
coefficient for linear sorption to ÔnormalÕ organic matter,
and fOC and fBC are fractions of (non-BC) organic- and
black carbon, respectively. Eq. (2) accounts for the non-
occluded POP fraction that is available for partitioning.
Besides BC, other condensed sedimentary phases (not
reviewed here) such as kerogens (Grathwohl, 1990;
Yang et al., 2004) unburned coal (Grathwohl, 1990;
Jonker and Koelmans, 2002a; Cornelissen and Gustafs-
son, 2005a) or weathered oil residues (Jonker et al.,
2003) exhibit similarly high affinities and may also be
accommodated by Eq. (2), by adding extra terms (Kara-
panagioti et al., 2000, 2001). Eq. (2) has been used to
match measured overall sorption with KOC and KF,BC
values for separate ÔpureÕ phases, and measured values
for fOC and fBC in sediment (Cornelissen et al.,
2004a,b; Cornelissen and Gustafsson, 2004; Jonker
et al., 2004). A remarkable observation in these studies
was that predictions of overall sorption using sorption
parameters (KOC, KF,BC, nF) for ÔpureÕ phases exceeded
the actual, experimentally measured sorption. Appar-
ently, KF,BC values for ÔpureÕ BC are not necessarily va-
lid under in situ conditions, where BC and other
sediment constituents are intimately mixed (Cornelissen
and Gustafsson, 2004; Jonker et al., 2004). Probably,
this is due to attenuation of POP sorption to BC by
DOM molecules that block the pores (Jonker and Sme-
des, 2000; Cornelissen and Gustafsson, 2004; Jonker
et al., 2004), or due to surface competition effects by
co-adsorbing POP or DOM molecules (Jonker and Sme-
des, 2000; Jonker et al., 2004; Cornelissen and Gustafs-
son, in press). Still, ÔattenuatedÕ, in situ KF,BC or KBC
values remain relatively high as compared to binding
to ÔamorphousÕ, ÔsoftÕ organic matter only (McGroddy
and Farrington, 1995; Jonker and Smedes, 2000).
Fig. 2 presents a summary of in situ KF,BC values from
different studies, against log Kow. The data for PAHs
are higher than for PCBs. For both compound classes,
the in situ KF,BC literature values appear to agree within
one order of magnitude. For phenanthrene (PHE), the
in situ values also agree with laboratory-derived values.
Calculations with Eq. (2) and such actual in situ values
show that the relative importance of sorption to BC is
significant, and may range from 50% to 90% for PCBs
(Lohmann et al., 2005; Moermond et al., 2005) and from
80% to 95% for PAHs (Accardi-Dey and Gschwend,
2002; Cornelissen et al., 2004b; Lohmann et al., 2005;
Moermond et al., 2005). Depending on the percentage
8.5
PAHs:
y = 0.6997x + 2.8219
7.5
2
R = 0.7908
PCBs:
6.5 y = 1.016x + 0.2469
log KF.BC
2
R = 0.8938
5.5
PAH Moermond PAH Accardi
PAH Lohmann PHE lab data
4.5
PCB Moermond PCB L ohmann
Linear (PCBs) Linear (PAHs)
3.5
4.5 5.5 6.5 7.5
log Kow
Fig. 2. Level of consistency of lab- and field-derived (in situ)
parameter values for sorption of PCBs and PAHs to BC, taken
from the literature (Accardi-Dey and Gschwend, 2003; Moer-
mond et al., 2005; Lohmann et al., 2005). Reported Freundlich
log KF,BC (lg/kgCarbon)/(lg/l)0.7 values for PCBs and PAHs are
plotted against log Kow. For phenanthrene (PHE), the median
and range of a compilation of literature KF,BC data for sorption
to pure BC is given (Bucheli and Gustafsson, 2000; Karapa-
nagioti et al., 2000, 2001; Jonker and Koelmans, 2002a;
Kleineidam et al., 2002; Accardi-Dey and Gschwend, 2003;
Cornelissen and Gustafsson, 2004; Cornelissen et al., 2004b;
Yang et al., 2004), which shows a good agreement to the field
data. The field-data regression equation for the PAHs is used to
estimate a log KF,BC value for the ÔmodelÕ PAHs fluoranthene
and pyrene (Kow = 105.2, KF,BC = 106.5) which is used to model
the effect of BC on sorption and bioaccumulation of POPs in
Figs. 3 and 4.
of BC with respect to total organic carbon (TOC) con-
tent in sediment (%BC), the Freundlich isotherm param-
eters, and the aqueous phase concentration, BC may be
the dominant adsorbent for added POPs. In Fig. 3, we
sketch this importance of BC based on the average
parameters compiled from the literature cited in Fig. 2.
These parameters serve to quantitatively illustrate trends
in the adsorption–absorption ratios. Below C = 0.1 lg/l
(Fig. 3), 1% of BC already may lead to 50% of POP
bound to this phase. In contrast, at higher C (still at
1% BC), sorption of POPs to organic matter overwhelms
sorption to BC due to saturation of the BC surface.
However, the medians of reported %BC for soils and
sediments are 3 and 9 respectively (Gustafsson et al.,
1997; Gustafsson and Gschwend, 1998; Masiello and
Druffel, 1998; Middelburg et al., 1999; Glaser et al.,
2000; Mitra et al., 2002; Hawthorne et al., 2002; Song
et al., 2002; Accardi-Dey and Gschwend, 2003; Bucheli
et al., 2004; Buckley et al., 2004; Cornelissen et al.,
2004a,b; Moermond et al., 2005; Van den Heuvel
et al., 2005), with extremes up to 40% or more for par-
ticular sites (Glaser et al., 2000; Hawthorne et al.,
 A.A. Koelmans et al. / Chemosphere 63 (2006) 365–377
1 isms (Weissenfels et al., 1992; Tracey and Hansen, 1996;
0.9
0.8
Fraction in BC
0.7
0.6
0.5 20%
0.4 10%
0.3 5%
0.2 1%
0.1
0 (West et al., 2001; Jonker et al., 2004; Rust et al.,
1E-06 0.00001 0.0001 0.001 0.01 0.1 1 10
Cw (μg/l)
Fig. 3. Fraction of organic pollutant bound to black carbon as
a function of aqueous concentration C, for 1%, 5%, 10% and
20% black carbon (of total organic carbon). The curves are
calculated with Eq. (2), for the ÔmodelÕ PAHs fluoranthene and
pyrene, with Kow = 105.2, and parameters for in situ sorption to
BC: KF,BC = 106.46 and nF,BC = 0.7. KF,BC is calculated from
log KF,BC = 0.7 log Kow + 2.82 (Fig. 2), derived from three
datasets for in situ sorption to BC (Accardi-Dey and Gsch-
wend, 2003; Moermond et al., 2005; Lohmann et al., 2005). At a
very common, low BC content of 1% of total organic carbon,
black carbon dominates sorption already below 0.1 lg/l. At a
BC content of >10%, and below 0.01 lg/l, normal organic
matter does not contribute substantially to overall sorption
anymore. The modeled POP fractions in BC are relatively
insensitive to log Kow of the POP, because KOC as well as KF,BC
increase with Kow with a slope fairly close to unity.
2002; Buckley et al., 2004). For the aqueous concentra-
tion C, pg/l–ng/l is the environmentally relevant range.
Therefore, we conclude that in the majority of cases
BC will dominate sorption, especially at sites of environ-
mental interest, i.e., in polluted, industrialised, or den-
sely populated regions, where BC levels may be higher
than 1% of TOC. The major consequence of strong sorp-
tion of POPs to BC in sediments is that exposure and
thus toxicity to aquatic organisms may significantly be
limited.
5. BC reduces accumulation in aquatic organisms
A simple biota-to-sediment accumulation factor
(BSAF) often quantifies the bioaccumulation of POPs
from sediment into benthic organisms (Thomann
et al., 1992a,b; Thomann and Komlos, 1999). Because
POPs mainly reside in sediment organic matter and
biota lipids, and the extent of partitioning into biota lip-
ids (quantified by Klip) more or less balances the extent
of partitioning into sediment organic matter (quantified
by KOC), the value for BSAF is approximately one.
During the past decade, however, several studies have
reported BSAF values that are much lower than one,
and provided direct or indirect support for the hypothe-
sis that BC reduces POP accumulation in aquatic organ-
371
Naes et al., 1999; Cretney and Yunker, 2000; Pickard
et al., 2001; West et al., 2001; Jonker et al., 2004;
McLeod et al., 2004; Sundelin et al., 2004; Rust et al.,
2004; Thorson et al., 2004; Cornelissen and Gustafsson,
2005b; Kukkonen et al., 2005; Moermond et al., 2005).
The most relevant observations were (a) lower in situ
BSAFs for PAHs than for PCBs of similar hydrophobic-
ity (Sundelin et al., 2004; Moermond et al., 2005), (b)
lower BSAFs for sediments with higher BC contents
100
2004; Sundelin et al., 2004; Thorson et al., 2004), (c)
lower BSAFs for planar compounds than for non-planar
compounds (Jonker et al., 2004; Kukkonen et al., 2005),
and (d) lower BSAFs for POPs with smaller fast desorb-
ing fractions, most probably due to presence of BC
(Kraaij et al., 2001; Moermond et al., 2005). The most
causal evidence, however, stems from replicated experi-
ments in which lower bioaccumulation was observed in
sediments amended with coal and charcoal (Jonker
et al., 2004), or with diesel soot (Rust et al., 2004), urban
dust and oil-fired power plant soot (Thorson et al.,
2004). For reversibly sorbing (not occluded) POPs, the
explanation for the lower BSAFs is straightforward.
BC enforces adsorption to the sediment and at constant
contaminant loadings, stronger sorption will yield lower
aqueous phase concentrations and less exposure to the
organism. For pyrogenic PAHs, BSAFs are factors of
10–100 lower than those for reversibly sorbing petro-
genic PAHs (Moermond et al., 2005) or PCBs (Weissen-
fels et al., 1992; Pickard et al., 2001; Jonker et al., 2004;
Sundelin et al., 2004; Moermond et al., 2005). However,
native pyrogenic PAHs may constitute a special case, be-
cause significant fractions of these PAHs may be oc-
cluded within the soot core. As stated earlier, removal
times for these occluded fractions range from decades
to millennia (Jonker et al., 2005). Such removal times
are relevant on geological time scales and may be com-
pared with removal times for overall BC degradation
(i.e., 10–20 kyr, Middelburg et al., 1999), but are irrele-
vant for the life cycles of benthic organisms. In sum-
mary, major fractions of native PAHs are shielded
from uptake by organisms, while ÔaddedÕ chemicals
(i.e., PCBs, petrogenic PAHs) that participate in parti-
tioning equilibria, have strongly reduced exposure con-
centrations in the pore water. Still, planar POPs pass
the gut membrane more easily than non-planar ones
(Shaw and Connell, 1984; Willman et al., 1999). The
combination of BC-enforced fixation of planar POPs
in the sediment and this increased rate of membrane pas-
sage, and partial uptake in the gut (Ahrens and Hickey,
2003; McLeod et al., 2004; Cornelissen and Gustafsson,
2005b; Moermond et al., 2005), may lead to idiosyn-
cratic accumulation behaviour. For instance, in sedi-
ments without BC, increased PCB planarity usually
results in increased accumulation, whereas the opposite
372 A.A. Koelmans et al. / Chemosphere 63 (2006) 365–377

-0.5

-1
1000 ng/l

log BSAF -1.5

100 ng/l

10 ng/l

-2 1 ng/l

0.1 ng/l
-2.5
0.01 ng/l

-3 0.001 ng/l
0 0.1 0.2 0.3 0.4
BC/TOC ratio

Fig. 4. Log BSAF as a function of the fraction of black carbon (of total organic carbon; BC/TOC ratio), for different concentrations of
PAH in water. The curves simulate uptake in benthic invertebrates and are calculated using Eq. (3), for the ÔmodelÕ PAHs fluoranthene
and pyrene, with Kow = 105.2, and parameters for in situ sorption to BC: KF,BC = 106.46 and nF,BC = 0.7. KF,BC is calculated from
log KF,BC = 0.7 log Kow + 2.82 (Fig. 2), derived from three datasets for in situ sorption to BC (Accardi-Dey and Gschwend, 2003;
Moermond et al., 2005; Lohmann et al., 2005). For pyrene and fluoranthene, the value for g is negligible (Thomann et al., 1992a,b;
Thomann and Komlos, 1999). The steep, negative slope at low BC/TOC shows that already a few percent of black carbon drastically
reduce bioaccumulation. In the environmentally relevant pg/l–ng/l range (lower four curves), and at a median BC/TOC ratio of 0.1,
bioaccumulation is reduced by a factor of 30–200. On (rare) sites with high BC/TOC ratios of 0.4, bioaccumulation may be reduced by
three orders of magnitude.

was observed in (the same) sediments enriched with
small amounts of coal and charcoal (Jonker et al.,
2004). Here, the extra sorption to BC apparently out-
competed the easier membrane passage. This is an
important observation, because planar molecules (pla-
nar PCBs, dioxins) belong to the most toxic, man-made
compounds in the environment (Safe, 1994).
The above indicates that bioaccumulation from sedi-
ments with pyrogenic PAHs, and allochtonous PCBs
may be understood from direct uptake into organism
lipids from pore water, complemented by dietary uptake
from ingested sediment particles. Black carbon limits the
availability of POPs via the pore water, as well as the
availability in the intestinal tract of the organisms. An
important question, however, is under which conditions
BC will limit exposure to such an extent that POPs can-
not exert their toxicity. We will evaluate this using the
concept of the BSAF, with its presumed value of around
one. At steady state, accumulation through both routes
can be described by simple BC-inclusive accumulation
models (Cretney and Yunker, 2000; Thorson et al.,
2004; Cornelissen and Gustafsson, 2005b; Moermond
et al., 2005), such as (Moermond et al., 2005):
 
fBC
K lip þ g 1  K OC
fOC
BSAF ¼   ð3Þ
fBC fBC
1 K oc þ K F;BC C nwF;BC 1
fOC fOC
where g is a food chain multiplier (Thomann et al.,
1992a,b; Thomann and Komlos, 1999). Eq. (3) was ap-
plied to a dataset of in situ BSAF values for a range of
POPs, and adequately described the observed BSAFs,
as well as the order of magnitude higher BSAFs for PCBs
than for PAHs (Moermond et al., 2005). Due to the non-
linear character of sorption to BC, the dependence of
BSAF estimated by Eq. (3) on BC content and POP con-
centration is also highly non-linear. In Fig. 4, we sketch
the effect of BC on BSAF for the ÔmodelÕ PAHs fluoranth-
ene or pyrene, again with sorption parameters compiled
from the literature cited in Fig. 2. In case of a pore water
concentration of 1 ng/l, in sediment of which 10% of the
TOC pool is composed of BC, the BSAF is reduced by a
factor of 30 (Fig. 4) as compared to the situation without
BC. In contrast, at 0.01 ng/l, the reduction is a factor of
100. Reductions of up to a factor of 1000 can be attained
in case of lower aqueous concentrations and/or higher
BC levels such as present at highly contaminated sites.
6. Implications for management
This review summarizes a robust body of evidence
for the thesis that bioaccumulation of POPs in sediments
is partly driven by the presence of BC, and that it usually
is much lower than predicted by EPT. The effect is
strongest at sites with relatively high BC levels
(BC/TOC > 0.05–0.1), and for planar POPs in the nano-
and picogram per litre aqueous concentration range. As
these are the environmentally relevant sites and concen-
trations, and planar POPs usually are the most toxic
chemicals, this has important implications for the assess-
ment of ecological risks and remediation strategies for
 A.A. Koelmans et al. / Chemosphere 63 (2006) 365–377
contaminated sediments. First, the presence of BC low-
ers exposure and toxicological risks of POPs. At many
locations all over the world, POP loadings decrease very
slowly. According to classic EPT, the concomitant de-
crease of exposure is proportional. However, we have
shown that exposure decreases more than proportional.
After all, depending on the BC content, a decrease in
POP concentration may lead to a 10- to 100-fold larger
decrease in concentrations in organisms. This means
that ecological target values will be reached much ear-
lier. Second, the presence of BC may have a positive
implication for sediment remediation. Remediation
strategies aim at lowering total sediment concentrations
until the standards, which are set by the authorities, are
reached. BC may lead to stronger fixation to the sedi-
ment, which implies that the current standards probably
are too safe. Hence, standards could be re-evaluated and
may safely be set to site-specific higher POP levels. Alter-
natively, standard systems could be reset to account for
BC sorption, e.g. by basing standards on freely dissolved
aqueous concentrations rather than total concentrations
in the sediment (Escher and Hermens, 2004). We recom-
mend that these perspectives are further explored in
future international research programmes. The most
important rationale is that cost savings may be in reach,
since the need for sediment remediation may be less.
Acknowledgments
Bernadette Ossendorp and Marten Scheffer are grate-
fully acknowledged for their advice on the manuscript.
Two anonymous reviewers are thanked for their con-
structive comments and suggestions.
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