Comparing Polychaete and
Polyethylene Uptake to Assess
Sediment Resuspension Effects on
C A R E Y L . F R I E D M A N , *, ‡
R O B E R T M . B U R G E S S ,†
M O N I Q U E M . P E R R O N ,†
M A R K G . C A N T W E L L ,†K A Y T . H O ,†A N D
R A I N E R L O H M A N N‡
U.S. Environmental Protection Agency, ORD/NHEERL, Atlantic
Ecology Division, Narragansett, Rhode Island, 02882,
Graduate School of Oceanography, University of Rhode Island,
Narragansett, RI, 02882, and Harvard School of Public
Health, Department of Environmental Health,
Boston, MA, 02115
Received December 29, 2008. Revised manuscript received
February 17, 2009. Accepted February 20, 2009.
Polyethylene sampler uptake was compared to polychaete
uptake to assess bioavailability of polychlorinated biphenyls
U.S.) sediment, contaminated with PCBs, was resuspended
under four different water column oxidation conditions:
under helium, and no resuspension (control). Residuals were
Nereis virens and to polyethylene (PE) passive samplers.
Few significant differences between the four resuspension
treatments were observed: under aeration, three of 23 PCBs
analyzed showed significant increases in polychaete
accumulation, while resuspension alone showed increased
concentrations in PE samplers for nine of 23 PCBs. Otherwise,
no differences were observed and overall we concluded
that resuspension had no effect on residual PCB availability.
The relationship between disequilibrium-corrected PE and lipid-
normalized polychaete PCB concentrations was nearly 1:1
are taken up similarly into PE and lipid. On average, PE
samplers suggested dissolved PCB concentrations 3.6 times
on a congener-specific basis this was only observed for
partitioning suggested lower dissolved concentrations than
those based on lipid. Organic carbon (OC)-water and OC and
average dissolved concentrations 29 and 10 times greater,
respectively, than those estimated with lipid-water partitioning.
can provide a more reliable estimate of bioavailability than
Sediments are capable of strongly sorbing hydrophobic
organic contaminants (HOCs) in the marine environment
(1). Over time, contaminated sediments can be a source of
HOCs and a significant health risk to aquatic food webs.
Many HOCs bioaccumulate in the benthos and biomagnify
HOCs is traditionally assessed by measuring HOC uptake
estimate bioavailability (6-10). In this study, we compared
and to polyethylene (PE) passive samplers in a standard
bioaccumulation test for different sediment treatments.
To mitigate risk to aquatic ecosystems, contaminated
sediments are commonly removed by dredging. However,
the effectiveness of dredging at reducing risk has been
questioned (11). In particular, it is not known whether
resuspension or disruption of natural sediment redox condi-
tions during dredging alters the bioavailability of particle-
associated HOCs. Several studies have shown that aeration
of sediment porewater and/or solids increases HOC parti-
and POM) to the aqueous phase (12, 13). Since dissolved
concentrations correlate to bioavailability (7, 9, 14, 15),
While some studies have investigated HOC desorption and
changes in bioavailability during sediment resuspensions
(PCBs) from field sediments. Bioavailability was assessed by
as well as in PE passive samplers.
Use of PE and other passive samplers to estimate
bioavailability is based on equilibrium partitioning theory
(EqP). EqP proposes HOCs reach a predictable equilibrium
distribution between sediment organic carbon (OC), pore-
water, and biota lipid (17). Since freely dissolved HOCs (i.e.,
HOCs available for partitioning and not associated with
DOM/POM) have historically been difficult to measure,
bioavailability is often estimated from OC-normalized sedi-
distribution of OC and does not account for sequestration
in desorption rates (1, 18, 19). Nonpolar passive samplers
circumvent these issues by absorbing porewater HOCs via
partitioning of freely dissolved HOCs only. Conducting
bioaccumulation tests with passive samplers would reduce
the amount of space, time, and expense involved with using
While other passive samplers such as polydimethylsiloxane
(SPMDs) have shown success as biomimetic tools (6-10),
are lower than analytical detection limits, and SPMDs are
difficult to work with because they contain triolein, a lipid-
aromatic hydrocarbon (PAH) uptake in PE and bioaccumu-
lation in marine polychaetes has already been shown with
PE uptake capable of explaining2/3of polychaete uptake
* Corresponding author phone: (401) 874-6268; fax: (401) 874-
6811; e-mail: firstname.lastname@example.org.
†U.S. Environmental Protection Agency.
‡University of Rhode Island.
†Harvard School of Public Health.
Environ. Sci. Technol. 2009, 43, 2865–2870
10.1021/es803695n CCC: $40.75
Published on Web 03/18/2009
2009 American Chemical SocietyVOL. 43, NO. 8, 2009 / ENVIRONMENTAL SCIENCE & TECHNOLOGY92865
Many sediment-dwelling organisms actively ingest sedi-
ment (21, 22), allowing organisms to equilibrate faster than
during an exposure is to add performance reference com-
pounds (PRCs), nonenvironmental HOCs with properties
PRCs allow an estimation of analytes’ absorption rates,
assuming similar loss and uptake kinetics. We investigated
an alternative method of assessing equilibrium status: a
the same PCBs measured in our bioaccumulation test and
method we were able to calculate PCB exchange rate
coefficients to correct for disequilibrium without extrapolat-
ing from similar compounds.
Collectively, the main objectives of this study were to (1)
determine whether sediment resuspension under various
redox conditions causes differences in PCB availability as
measured by marine polychaete and PE sampler uptake; (2)
compare polychaete and PE uptake of PCBs to determine if
porewater PCB concentrations calculated from biota, PE
sampler, and sediment concentrations to assess whether PE
samplers or sediment geochemistry provide more accurate
estimates of exposure.
Materials and Methods
Resuspension. Sediment from the New Bedford Harbor
(NBH) U.S. EPA Superfund site (MA) was collected in
at 4 °C until use. Four treatments were evaluated: “Resus-
pension”, “Resuspension with Air”, “Resuspension with
Helium”, and “No Resuspension”. Each began with the
addition of 3 L aliquots of homogenized NBH sediment to
lids. Fifty-three L of Narragansett Bay, RI (NB) seawater (20
°C, 30 ‰) was added to each drum and lids were fastened.
For each drum, a stainless steel drive shaft and impeller
connected to a heavy duty mixing motor were inserted into
the drum through a hole in the lid (see Supporting Informa-
tion (SI) for more details).
For two of the four drums, air and helium (respectively)
to gas cylinders. Flow rates were 600-3600 mL/min for air
and 300-3000 mL/min for helium, depending on dissolved
oxygen (DO) measurements. Sediments were resuspended
of each day and at one hour intervals, measurements of
overlying water temperature, air temperature, salinity, pH,
seawater were removed from each drum and replaced with
16 L of fresh NB seawater to simulate daily tidal exchanges
in the upper portion of New Bedford Harbor (27). On the
for four days before overlying water was removed. Gas flow
into the air and helium treatments was continued for 18 h
after mixing was concluded. Sediments were transferred to
holding chambers and kept at 4 °C in the dark for three days
until the start of the bioaccumulation study.
Bioaccumulation Exposure System. Twenty-eight day
exposures were performed based on guidance by U.S. EPA
× 12 cm) with a cylindrical coil of 3.0 mm plastic mesh
received 200 mL of sediment from the resuspension treat-
ments. Overlying flow-through seawater (NB, 30‰) was
distributed to each chamber via a siphoning gravity dilutor
at a mean flow rate of 5.8 ((1.9) mL/min for ∼10 volumetric
turnovers per day. Exposures were kept at 20 °C with
continuous aeration under a 12 h light/12 h dark cycle.
Sediments were added to exposure chambers and the
seawater system started three days prior to the addition of
polychaetes. One polychaete (Nereis virens; 3-5 g wet) was
added to each chamber, with five replicate chambers for
replicates was prepared using 200 mL of noncontaminated
Long Island Sound (LIS) sediment per chamber, collected
April 26, 2005 (40°07.95′, 72°52.70′) and sieved through 2
mm, as a control (30). Two pieces of ∼1 cm2precleaned
(extracted 24 h twice with dichloromethane) low density PE
(51 µm thickness; Carlisle Plastics, Inc., Minneapolis, MN)
were added to each chamber. One piece was buried ∼1 cm
pierced with a plastic cable tie and woven onto the mesh
added to the chambers (n ) 5, day -3) and on the last day
of the test (n ) 5, day 28). Tissue samples were collected on
day 0 as blanks (n ) 5) and on day 28. PE samplers were
collected on day 0 as blanks (n ) 5) and on day 28. On day
28, polychaetes and PE were removed from sediments by
sieving through a 1 mm stainless steel sieve and rinsed with
20 °C seawater. Sediments and PE were stored at -4 °C until
analysis. Polychaetes were directly placed in 400 mL static
depuration chambers containing 100 g of LIS sediment and
250 mL seawater. Each chamber contained one polychaete
and was continuously aerated. After 24 h, polychaetes were
sieved from depuration sediments, rinsed with seawater,
weighed, and frozen at -4 °C in the dark until analysis.
PE Equilibration Exposure System. PE samplers were
equilibrated for 72 h with a 21.2 µg PCB/L 80:20 v:v
methanol-water mixture following the methods of Booij et
al. (23). PCB congeners in the spiking solution included CBs
126, 128, 138, 153, 156, 157, 167, 169, 170, 180, 189, and 206
(Ultra Scientific, North Kingstown, RI). After equilibration,
initial PCB concentrations, while the remainder were stored
at 4 °C in the dark until use. Sediments with varying levels
of OC were prepared by mixing sand (Narragansett Beach,
RI; rinsed with deionized water and muffled at 400 °C), LIS
sediments, and 2 mm sieved peat moss (Type BP-C, Berger
were prepared with the following nominal OC contents: 0,
1, 2, 5, 7.5, and 10%. For the 0% OC sediment, only sand was
OC) were mixed 50:50 with sand. The 2% OC sediment was
LIS alone. The 5, 7.5, and 10% OC sediments were prepared
by mixing LIS sediment with peat moss in ratios of ∼13:1,
7:1, and 4:1, respectively. A subsample of each treatment
buried approximately 1 cm into the sediment. NB seawater
(30‰) was distributed to each chamber at a mean flow rate
of 6.0 ((1.6) mL/min. Exposures were kept at 20 °C with
continuous aeration under a 12 h light/12 h dark cycle, as
for 28 days, at which time samplers were removed from the
chambers, rinsed with seawater, and stored at 4 °C in the
dark until analysis.
Tissue, Sediment, and PE Extraction. Internal standard
(CB198) was added to all tissue, sediment, and PE before
extraction. Sediment and tissue were extracted three times
PE were extracted twice with dichloromethane. See SI for
details. All samples were stored at 4 °C in the dark until
2866 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 43, NO. 8, 2009
Analytical Chemistry. PCB concentrations were deter-
mined with a 5890 series II gas chromatograph equipped
with a 7673A autosampler and electron capture detector
in Lohmann et al. (31). Twenty three PCB congeners were
quantified, including CBs 8,18, 28, 44, 52, 66, 99, 101, 105,
110, 118, 128, 138, 151, 153, 170, 180, 183, 187, 194, 195, 206,
and 209. Tissue and PE PCB concentrations were blank-
corrected. National Institute of Standards and Technology
89 ( 16% and 77 ( 20% from tissues and sediments,
respectively. Analytical blanks and IS-spiked blanks were
added to each analysis as quality assurance measures.
Total Organic Carbon, Black Carbon, and Grain Size
Analyses. For total organic carbon (TOC) and BC analyses,
sediments were dried and large shell material removed.
Sediments were ground, treated with HCl, and analyzed for
%C on a Carlo Erba NA 1500 elemental analyzer (Fisons
model MJ2K Hydro 2000A and Mastersizer 2000 (Malvern,
Worcestershire, UK). Sediments were characterized as clays
(0-3.9 µm), silts (3.91-62.5 µm), or sands (62.5-2000 µm).
by a protected least significant difference (PLSD) multiple
comparison to identify specific differences between means.
Software used to conduct analyses included Statistica 6.1
Inc., Cary, NC). To determine the minimum number of
replicates needed to detect significant differences between
of 95%, the power equation described by Snedecor and
Cochran (34) was used.
Results and Discussion
Sediment. TOC ranged from 6.71 to 7.15% and BC from 0.67
to 0.81% (Supporting Information Table S1). There were no
treatments. However, resuspension significantly increased
compared to no resuspension. Neither sand nor silt was
significantly different among the three resuspended treat-
ments. Clay content did not change compared to no
PCB concentrations in all postresuspension, prebioac-
treatments for all PCBs measured except CB209, for which
the resuspension with air treatment had greater concentra-
tions than all other treatments (p ) 0.0061; SI Figure S1).
This suggests that resuspension under a wide range of
For all treatments, statistical comparison of PCBs in
postresuspension, prebioaccumulation sediments to PCBs
in sediments collected from bioaccumulation chambers on
day 28 demonstrated that sediment concentrations did not
change during exposures (data not shown).
Polychaetes. Polychaetes in all treatments showed 100%
survival except for the no resuspension treatment (80%).
from all NBH treatments compared to the LIS reference
at the limits of analytical detection; data not shown).
sediment concentrations. For example, concentrations of
CB28 were ∼1.3 × 105µg/kg OC in sediment but ∼8.0 × 104
µg/kg lipid in tissue. In other words, biota-sediment ac-
cumulation factors (BSAFs) were <1 for all PCBs (SI Figure
S3), where BSAFs are defined as
Of the 23 PCBs measured, only CB183 bioaccumulated in
greater concentrations in the air treatment compared to the
209 bioaccumulated in greater concentrations in the air
treatment compared to all other treatments (p < 0.0001 and
p ) 0.0034, respectively). Thus, using a recommended
(28, 29), only three of 23 PCBs showed increases in biota
exposed to the air treatment. Given these findings, we used
lipid concentration variance data to estimate the minimum
number of replicates necessary to detect a significant
means with a power of 0.95 for the more concentrated PCBs
in NBH sediments. Five replicates was enough to detect as
little as a 10% difference for CB28, while for CBs 153, 128,
and 170, even a 25% difference from the no resuspension
S2). Since CB28 was the most concentrated PCB in NBH
sediment, and NBH sediment is highly contaminated, our
results imply that resuspension of sediments under a range
of oxidation conditions does not influence the bioaccumu-
lation of PCBs by benthic polychaetes. The results of the
power test suggest that the number of replicates recom-
mended by testing guidance (used by regulatory agencies)
results emphasize the need for more precise sampling
techniques, which ideally should also reduce the physical
Polyethylene. Only sediment PE concentrations are
discussed here; water column PE samplers were near
detection limits. PCB concentrations in PE were lower than
present at ∼4.0 × 104µg/kg in PE compared to ∼1.3 × 105
µg/kg OC in sediment and ∼8.0 × 104µg/kg lipid in tissue.
For CBs 8, 18, 28, 44, 52, 66, 99, 101, and 110, PE from the
resuspension alone treatment accumulated significantly
greater concentrations than all other treatments, including
the control (p < 0.0001 to 0.0355). It is not clear why PE took
treatment, but not treatments with gas addition. To test
whether gases stripped dissolved PCBs from resuspension
possible due to volatilization using air-water partition
coefficients from Schenker et al. (35). Only ∼20 µg per 3 L
have been lost; this is insignificant relative to the difference
all other treatment PEs.
that, overall, resuspension under extreme conditions does
not change residual availability of PCBs and therefore likely
will not change availability in the field.
Determination of 28-Day Equilibrium Status and Es-
timating Bioaccumulation from PE Samplers. Previous
PCBs (e.g., CBs 21, 38, 50, and 61) as PRCs to correct for
disequilibrium is not practical due to their presence in NBH
sediments or coelution with other congeners. To determine
percent equilibration reached, we conducted a desorption
study with PE samplers impregnated with PCBs native to
NBH sediments and clean sediments with varying OC
VOL. 43, NO. 8, 2009 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 2867
content. With this approach, target analytes can be used to
have to be extrapolated from other compounds.
After 28 days of exposure, the fraction desorbed of each
congener was determined:
where CPE,0is the PCB concentration in impregnated PE at
time t of exposure (t ) 28 days; µg/kg PE). Since the OC
content of NBH sediments is ∼7% (SI Table S1), desorption
data from exposures to sediment with an OC content most
closely matching that of NBH sediments (4.6%) was chosen
for calculating exchange rate coefficients. The percent PCB
desorbed from spiked PE decreased with increasing log Kow
is reasonable given that increasing molecular mass corre-
sponds to decreasing diffusivity in water (37). However, the
rate coefficients of lower log KowPCBs are more accurate
than those of higher log Kow. The exchange rate coefficient,
ke(hr-1), for each congener was determined as follows:
Values of kewere in the 0.0003 to 0.001 h-1range (Table
1). These are between the field and laboratory ranges of ke
is reasonable considering that field deployments of PE in
(26) were stagnant (5-15 cm depth) while laboratory
deployments were well-mixed. Our deployment conditions
were between these two extremes.
then calculated (Table 1):
where CPE,t(B)is the concentration in the PE deployed in the
bioaccumulation test after 28 days (i.e., t ) 28). For all
study, the best fit linear relationship between CPE,∞and Clip
and the correlation coefficient (r2) was 0.877 (intercept )
1615). Vinturella et al. (20) showed that uptake of PAHs by
N. virens and PE were linearly correlated (r2) 0.65) with a
slope of 0.67. These relationships allow equilibrium PE
of HOCs from sediments.
on lipid concentrations using lipid-water partition coef-
ficients (Klip--w) obtained from Schwarzenbach et al. (37):
and based on PE concentrations using PE-water partition
coefficients (KPE-w) obtained from Adams et al. (25):
concentrations was determined (Figure 2). The correlation
was still high (r2) 0.865), but the slope was 0.278 (intercept
) 0.014), indicating that PE and polychaete lipid displayed
The deviation in slope from ∼1 is partially due to greater
uptake of higher log KowPCBs (CBs 101-170) in polychaetes
TABLE 1. For PCBs Which Showed Greater Desorption than
15%: log Kow, % Desorption, keCalculated from % Desorption,
CPE,∞Calculated from ke, and Ctissfor Comparison (CPE,∞and
Ctissfrom Resuspension Alone Treatment)
[(1-CPE,28 days/CPE,0)] ×
aHawker and Connell. ref 36.
Fraction desorbed )
1 - e-ket
FIGURE 1. PCB concentrations in Nereis virens on a lipid basis
polyethylene samplers. Linear best fit y ) 0.948 × + 1615, r2)
0.877 (n ) 48).
FIGURE 2. Porewater dissolved PCB concentrations calculated
using lipid-water partitioning versus porewater dissolved PCB
concentrations calculated using PE-water partitioning. Linear
best fit y ) 0.278 × + 0.014, r2) 0.865 (n ) 48).
2868 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 43, NO. 8, 2009
(1.1-4.2 times) and lesser uptake of the lower log KowPCBs
(CBs 18-66) relative to PE samplers (0.05-0.60 times). This
less efficient depuration kinetics for these PCBs (e.g., 25,
Though it is possible that N. virens metabolized some
lower log KowPCBs (38-40), metabolism did not appear to
be a factor as assessed by BSAFs, with the exception of CB8
0.1, but was not found to be an outlier; SI Figure S3).
Therefore, the low slope (0.278) in Figure 2 still indicates
This is likely because polychaetes ventilate overlying oxy-
genated water (∼3 mL/min for N. virens (41)) and were thus
exposed to a combination of contaminated porewater and
clean overlying water, whereas PE were primarily exposed
from both lipid and PE samplers are listed in SI Table S3).
PE were better indicators of bioavailable concentrations
than sediment OC. Although well correlated (r2) 0.953),
lipid-based dissolved concentrations were, on average, only
OC-normalized partition coefficients (KOC; SI Figure S5):
where Csedis the concentration of PCBs in the sediment and
et al. (37)). To account for sequestration of congeners for
which BC-normalized partition coefficients (KBC) were avail-
able (31, 42), dissolved PCBs based on both BC and OC
(Cdiss,OC+BC) were calculated using the model proposed by
coefficient (n) of 0.7:
where fBCis fraction BC in sediment. Cdiss,OC+BCwas solved
by iteration. On average, lipid-derived dissolved concentra-
tions were 0.10 times those calculated using OC and BC
partitioning (r2) 0.858; SI Figure S5), though depending on
congener, resuspension treatment, and source of KBC,
individual values ranged widely from 0.07 to 9.2. Variation
of n by (0.1 did not substantially change the relationship.
concentrations by, on average, 29 times, while OC and BC
together overestimated bioavailable concentrations by, on
average, 10 times. PE, on average, estimated bioavailable
concentrations 3.6 times higher than what was observed in
polychaetes, but PE-based estimations were higher for low
log Kow PCBs, and lower for higher chlorinated PCBs. In
addition to polychaete ventilation of clean overlying water,
overestimation by PE could also be due to uncertainties
associated with LFERs on which Klip-w, KPE-w, and Kocare
varies between organisms and species (43), we examined
variability associated with Klip-wby substituting bioconcen-
tration factors (BCFs) from Kraaij et al. (9) for Klip-w. This
only changed slopes by ( 0.02. To examine analytical
uncertainty, PE analytical and replicate variation was quan-
tified. Using CB28 as an example, propagation of error,
including variance of keand CPE,28 days(B), resulted in equi-
librium PE concentration error of ∼50% (calculations in SI).
All uncertainty considered, we conclude that bioaccumu-
using PE samplers within a factor of 2-3.
To summarize, resuspension of PCB-contaminated sedi-
ments under a range of oxidation conditions did not change
or to PE samplers. Because resuspensions were designed to
be extreme relative to field conditions, this implies that
dredging of sediment under an aerated water column will
A statistical power test indicated that five organisms per
treatment in our bioaccumulation test, a number within the
to detect differences in bioaccumulation among treatments
for only the most concentrated PCB in sediments. Because
NBH sediment is highly contaminated on an absolute scale,
we note that testing guidance may recommend insufficient
variability, particularly for less contaminated sites. Partition-
ing of PCBs from sediment porewater into PE samplers was
strongly correlated to the lipid uptake of PCBs in N. virens
with nearly a one-to-one relationship. This suggests PE
samplers can be used as accurate N. virens surrogates in
bioaccumulation tests with HOC-contaminated sediments.
Porewater concentrations, however, differed between those
derived from PE and those based on lipid concentrations.
This could be due to polychaete exposure to clean overlying
water via ventilation versus passive PE uptake of PCBs from
porewater. Part of the difference can also be explained by
the propagation of uncertainties in measurements and
physicochemical constants. Nonetheless, PE samplers can
serve dual purposes with respect to bioaccumulation and
be used with the appropriate linear relationships to (1)
equilibrium porewater concentrations, both within a factor
We acknowledge Stephan A. Ryba and Richard A. McKinney
(U.S. EPA) for assistance with this study. This work was
supported in part by a student services contract from the
U.S. EPA (No. EP06D000527).
Supporting Information Available
Additional details relating to the following: experimental
concentrations; BSAF values; statistical determination of
number of organisms needed to detect differences between
control and treatment bioaccumulation; total sediment OC
and BC concentrations; dissolved PCBs calculated using
different sorptive phases; and calculations showing error
involved in determining dissolved concentrations using PE
samplers. This material is available free of charge via the
Internet at http://pubs.acs.org.
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