Supporting Information Biological responses to activated carbon ...
Supporting Information
Biological responses to activated carbon amendments in sediment remediation ELISABETH M.-L. JANSSEN, †* BARBARA A. BECKINGHAM, ‡ †
Institute of Biogeochemistry and Pollutant Dynamics, Swiss Federal Institute of Technology (ETH), Universitätsstrasse 16, 8092 Zürich, Switzerland ‡
Center for Applied Geoscience, University Tübingen, Hölderlinstrasse 12, 72074 Tübingen, Germany
Number of Figures: 1 Number of Tables: 5 Number of pages: 12
S1
Biodynamic Modeling The simplified differential equation and its solution in closed form of the biodynamic model are described by dCorg dt
= k s ⋅ Cs + k w ⋅ Cw − ke ⋅ Corg (t )
(Eq. 1)
(k s ⋅ Cs + k w ⋅ Cw ) ⋅ (1 − e − ke ⋅t ) ke
(Eq. 2)
Corg (t ) =
The change of chemical tissue concentration in the organism is described by the sum of uptake from solids and water minus elimination processes. Contaminant uptake from water is described by an aqueous uptake rate constant, kw (L g-1 d-1), and the water contaminant concentration, Cw (μg/L). For filter feeders, Cw refers to the surficial water concentration and kw is further defined as the product of filtration rate (FR, L g-1 d-1), and aqueous assimilation efficiency (AEaq). The assimilation efficiency describes the fraction of contaminant that is assimilated into the organism (e.g., through the skin or gut wall) relative to the contaminant concentration to which the organism was exposed. For deposit feeders that do not filter water, the aqueous uptake rate, kw, describes the passive assimilation of contaminants through the water by dermal exposure and Cw can either be the surficial water, the pore water or a combination (e.g. when worms pump water through subsurface borrows for oxygenation). The contaminant uptake from sediment, ks, is described by the product of the organism’s ingestion rate or particle uptake rate (IR, g g-1 d-1), the contaminant sediment concentration Cs (μg g-1 dw), and the organism’s contaminant assimilation efficiency from ingested solids (AEs). The assimilation efficiency can vary greatly among organisms because it is dependent upon the digestive chemistry in the gut (e.g. (Ahrens, Hertz et al. 2001; Arnot and Gobas 2004) and references herein). Assimilation of pollutants through the aqueous phase is often dominated by the uptake of particulates with the water (Burton and Johnston 2010). Activated carbon amendments reduce (a) the aqueous concentration (Cw), and (b) reduce the assimilation efficiency from the solids (AEs) because the availability is much lower from AC than from native sediment. The value of AEs has to be modified for amended sediment accordingly:
S2
AEs
amended
= Fsed ⋅ AEssed + (1 − Fsed ) ⋅ AEsAC
(Eq. 3)
with AEsamended being the assimilation efficiency from the AC amended sediment, Fsed being the fraction of chemicals that remains on the sediment, AEssed being the assimilation efficiency from untreated sediment and AEsAC being the assimilation efficiency from AC. The value for Fsed can be estimated from the ratio of water concentration from well mixed slurries at quasi steady state with and without AC present. Fsed
CwAC = noAC Cw
(Eq. 4)
with CwAC and CwnoAC being the water concentrations before and after AC addition, assuming linear partitioning at low aqueous concentrations. Pathways that account for loss of contaminants from the organism’s tissue have to be subtracted from those uptake terms (Eq. 1 and 2). Loss can occur by elimination, described by the exponential rate constant ke (g g-1 d-1), when pollutants un-assimilated in the gut or gills are excreted. Exponential growth rates can be added to the loss term accounting for growth dilution (pseudo elimination). Similarly, other loss mechanisms can be included, e.g., biotransformation, however, in the case of polychlorinated biphenyls and the species employed for the modeling below, transformation can be neglected.
S3
Table S1. Values of physiological and model parameters for the benthic invertebrates used to model polychlorinated biphenyl concentrations in their tissue after 28 days. Sediment and aqueous concentrations were used as reported in the respective studies, range reported when multiple sediments were used for exposure.
Parameter, unit Filtration rate (FR), L water/ g dry wt / d Aqueous assimilation efficiency (AEaq), % Aqueous uptake rate constant (kw) = FR x AEaq L water / g dry wt / d Ingestion rate (IR), g / g dry wt / d Sediment assimilation efficiency from sediment (AEs), % Sediment assimilation efficiency from amended sediment (AEsamended), % Elimination rate constant (ke), 1/d
Neanthes arenaceodentata4
Macoma balthica5 2
Corbicula fluminea5 45
50
20
0.5
Lumbriculus variegatus6
17.8
3.5
0.25
0.03
10.7
7
20
20
20
0.36
1.4
1.4
1.0
0.04
0.04
0.04
0.51
Sediment PCB concentration (Cs) µg/g
1.2
3.0-7.0
6.5
6.8-87.4
Aqueous concentration (CwnoAC) after amendment (CwAC) µg/L
0.02
0.04-0.05
0.2
0.8-2.5
0.004
0.01-0.03
0.0001-0.0006 0.04-0.063
S4
Figure S1. Measured tissue concentrations of polychlorinated biphenyls against predicted values employing the biodynamic model for Macoma balthica (blue)(McLeod, Van den Heuvel-Greve et al. 2007), Neanthes arenaceodentata (green)(Janssen, Croteau et al. 2010), Corbicula fluminea (red)(McLeod, Van den Heuvel-Greve et al. 2007) , Lumbriculus variegatus (orange)(Sun, Werner et al. 2009) exposed to untreated (open symbols) and activated carbon amended sediments (closed symbols). Error bar represent one standard deviation of the measured concentrations. Solid line represents the linear fit of all data (N = 148), dashed lines represent the 1:1, 2:1 and 1:2 relationships.
S5
Table S2. Survival: Effects of activated carbon amendment on benthic invertebrates relative to exposure to untreated sediment. #
Species
1
Abra nitida
2
Americamysis bahia
3
Ampelisca abdita
4
Amphiura spp.
5
Asellus aquaticus
6
Asellus aquaticus
7
Asellus aquaticus
8
Corbicula fluminea
9
Corbicula fluminea
10
Corbicula fluminea
11
Corophium volutator
12
Gammarus pulex
13
Gammarus pulex
14
Hinia reticulata
15
Leptocheirus plumulosus
16
Limnodrilus sp.
17
Lumbriculus variegatus
18
Lumbriculus variegatus
19
Lumbriculus variegatus
20
Lumbriculus variegatus
21
Lumbriculus variegatus
22
Lumbriculus variegatus
23
Macoma balthica
24
Macoma nasuta
25
Mytilus edulis
26
Nassanus nitidus (H. reticulata)
Effect on survival no
yes (positive)
yes (positive) no no
yes (positive) yes (positive) yes (positive)
yes (negative) no no
yes (positive)
yes (negative) no no
Notes Thin layer cap (0.5, 3 cm AC) to dioxin/furan polluted sediment Improved survival in contaminated sediment
(Josefsson, Schaaning et al. 2012)
Amendment to uncontaminated sediment
(Kupryianchyk, Reichman et al. 2011)
Improved survival in contaminated sediment
See #[1] above
Amendment to contaminated sediment
Amendment to contaminated sediment
Survival 12% higher as for untreaded sediment (85%), 0.7% AC resulted in 95% survival Survival 12% lower as for untreaded sediment (85%), 2.5% AC resulted in 75% survival 1.3% AC same survival as untreated sediment Amendment of 25% AC
Survival is 30% in 3-30% AC and only 0-5% survival in untreated, polluted sediment Survival in untreated sediment 80-85%; with 3, 6, 15, 30% AC: survival: 40, 5, 0, 0; LC50 = 3.1%
(Josefsson, Schaaning et al. 2012)
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Noori et al. 2013) (McLeod, Luoma et al. 2008) (McLeod, Luoma et al. 2008) (McLeod, Luoma et al. 2008)
(Jonker, Suijkerbuijk et al. 2009)
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Cornelissen, Breedveld et al. 2006) (Millward, Bridges et al. 2005) (Sun and Ghosh 2007)
no
(Beckingham and Ghosh 2011)
no
(Beckingham and Ghosh 2011)
no
(Nybom, Werner et al. 2012)
no
(Kupryianchyk, Noori et al. 2013)
no yes (positive)
(Ho and Burgess 2004)
(Jonker, Suijkerbuijk et al. 2009)
no
no
(Ho and Burgess 2004)
(Koelmans and Jonker 2011)
no
no
Reference
(McLeod, Van den Heuvel-Greve et al. 2007)
Survival increased by 83%, (only 17% survival in untreated, polluted sediment)
(Cho, Smithenry et al. 2007)
(Tomaszewski and Luthy 2008)
(Josefsson, Schaaning et al. 2012)
S6
27
Neanthes arenaceodentata
28
Neanthes arenaceodentata
29
Neanthes arenaceodentata
30
Neanthes arenaceodentata
31
Nereis diversicolor
32
Nereis spp.
no
(Millward, Bridges et al. 2005)
no
(Janssen, Choi et al. 2012)
(Janssen, Croteau et al. 2010)
no
(Janssen, Oen et al. 2011)
no no no
Survival similar between uncapped and AC-cap, but lower for AC compared to non-active cap
(Cornelissen, Breedveld et al. 2006)
(Josefsson, Schaaning et al. 2012)
S7
Table S3. Growth: Effects of activated carbon amendment on benthic invertebrates relative to exposure to untreated sediment. #
Species
1
Asellus aquaticus
2
Asellus aquaticus
3
Corbicula fluminea
4
Corbicula fluminea
5
Gammarus pulex
6
Gammarus pulex
7
Leptocheirus plumulosus
8
Lumbriculus variegatus
9
Macoma balthica
10
Mytilus edulis
11
Neanthes arenaceodentata
12
Neanthes arenaceodentata
13
Neanthes arenaceodentata
14
Neanthes arenaceodentata
15
Nassanus nitidus (H. reticulata)
16
Abra nitida
17
Amphiura spp.
Effect on growth yes (negative) No
yes (negative) no no no no
yes (negative) no no
yes (negative) yes (negative) no no no no no
Notes EC50 = 5.3%, amendment to polluted sediment amendment to unpolluted sediment
Reduced growth at 1.3% and 25% AC, but large deviation among replicates 0.7% AC (reduced growth only at higher dose) Amendment to unpolluted sediment
Amendment to contaminated sediment
sediment specific, AC size and dose effect
50% less growth in AC amended sediment Reduced growth for 2 out of 5 sediments 3 out of 5 sediments show no effect
Thin layer cap (0.5, 3 cm AC) to dioxin/furan polluted sediment See # [14] above See # [14] above
Reference (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (McLeod, Luoma et al. 2008) (McLeod, Luoma et al. 2008)
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Millward, Bridges et al. 2005) (Nybom, Werner et al. 2012)
(McLeod, Van den Heuvel-Greve et al. 2007) (Tomaszewski and Luthy 2008) (Millward, Bridges et al. 2005) (Janssen, Choi et al. 2012) (Janssen, Oen et al. 2011)
(Janssen, Choi et al. 2012)
(Josefsson, Schaaning et al. 2012) (Josefsson, Schaaning et al. 2012) (Josefsson, Schaaning et al. 2012)
S8
Table S4. Lipid content: Effects of activated carbon amendment on benthic invertebrates relative to exposure to untreated sediment. #
Species
1
Hinia reticulata
2
Leptocheirus plumulosus
3
Lumbriculus variegatus
4
Lumbriculus variegatus
5
Lumbriculus variegatus
6
Lumbriculus variegatus
7
Macoma nasuta
8
Neanthes arenaceodentata
9
Neanthes arenaceodentata
10
Neanthes arenaceodentata
11
Neanthes arenaceodentata
12
Neanthes arenaceodentata
13
Neanthes arenaceodentata
14
Nereis diversicolor
15
Nereis (spp.)
16
Nassanus nitidus (H. reticulata)
Effect on lipid content no no
yes (negative) no no
yes (negative) no
yes (negative) yes (positive)
yes (negative) no no no no no no
Notes
Reference (Cornelissen, Breedveld et al. 2006)
5-15% lower lipid content, in sediment without AC: lipid increases over time Ex situ, with field-amended sediments
dose effect, but high variability especially when organisms were loosing weight 66% lower lipid content in AC amendment
Ex situ, lipid content increased by 50% from average of 0.4% to 0.6% Slightly reduced lipid content for amendment to 1 out of 5 sediments In situ
4 out of 5 sediments show no effect
Thin layer cap (0.5, 3 cm AC) to dioxin/furan polluted sediment See # [14] above
(Millward, Bridges et al. 2005)
(Jonker, Suijkerbuijk et al. 2009) (Sun and Ghosh 2007)
(Beckingham and Ghosh In prep) (Nybom, Werner et al. 2012) (Cho, Smithenry et al. 2007)
(Janssen, Croteau et al. 2010) (Janssen, Oen et al. 2011)
(Janssen, Choi et al. 2012)
(Millward, Bridges et al. 2005) (Janssen, Oen et al. 2011)
(Janssen, Choi et al. 2012)
(Cornelissen, Breedveld et al. 2006) (Josefsson, Schaaning et al. 2012) (Josefsson, Schaaning et al. 2012)
S9
Table S5. Behavior: Effects of activated carbon amendment on benthic invertebrates relative to exposure to untreated sediment. #
Species
1
Asellus aquaticus
2
Asellus aquaticus
3
Asellus aquaticus
4
Asellus aquaticus
5
Asellus aquaticus
6
Asellus aquaticus
7
Corophium volutator
8
Gammarus pulex
9
Gammarus pulex
10
Gammarus pulex
11
Gammarus pulex
12
Gammarus pulex
13
Gammarus pulex
14
Lumbriculus variegatus
15
Lumbriculus variegatus
16
Lumbriculus variegatus
17
Lumbriculus variegatus
Effect on behavior no no no no no no
yes (negative)
Notes avoidance, amendment to polluted sediment
(Kupryianchyk, Reichman et al. 2011)
locomotion, amendment to unpolluted sediment
(Kupryianchyk, Reichman et al. 2011)
avoidance, amendment to unpolluted sediment locomotion, amendment to polluted sediment ventilation, amendment to polluted sediment
ventilation, amendment to unpolluted sediment
no
inconsistent, avoidance for 4,7,15%AC amendments but not for 25% amentdment avoidance, amendment to polluted sediment
no
locomotion, amendment to unpolluted sediment
no no no no
yes (negative) yes (negative) yes (negative) no
Reference
avoidance, amendment to unpolluted sediment locomotion, amendment to polluted sediment ventilation, amendment to polluted sediment
ventilation, amendment to unpolluted sediment egestion, 92% reduction in 1 to 25% AC
egestion, dose and particle size dependend reproduction, sediment specific, study not designed to measure reproduction avoidance
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Jonker, Suijkerbuijk et al. 2009)
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Jonker, Suijkerbuijk et al. 2009) (Nybom, Werner et al. 2012)
(Nybom, Werner et al. 2012) (Nybom, Werner et al. 2012)
S10
References Ahrens, M. J., J. Hertz, et al. (2001). "The effect of body size on digestive chemistry and absorption efficiencies of food and sediment-bound organic contaminants in Nereis succinea (Polychaeta)." Journal of Experimental Marine Biology and Ecology 263: 185-209. Arnot, J. A. and F. A. Gobas (2004). "A food web bioaccumulation model for organic chemicals in aquatic ecosystems." Environ Toxicol Chem 23(10): 2343-2355. Beckingham, B. and U. Ghosh (2011). "Field scale reduction of PCB bioavailability with activated carbon amendment to river sediments." Environmental Science and Technology 45: 1056710574. Beckingham, B. and U. Ghosh (In prep). "Observations of limited secondary effects with activated carbon amendment to Grasse River, NY USA." Burton, A. G. and E. L. Johnston (2010). "Assessing contaminated sediments in the context of multiple stressors." Environmental Toxicology and Chemistry 29(12): 2625-2643. Cho, Y. M., D. W. Smithenry, et al. (2007). "Field methods for amending marine sediment with activated carbon and assessing treatment effectiveness." Marine Environmental Research 64(5): 541-555. Cornelissen, G., G. D. Breedveld, et al. (2006). "Bioaccumulation of native polycyclic aromatic hydrocarbons from sediment by a polychaete and a gastropod: freely dissolved concentrations and activated carbon amendment." Environ Toxicol Chem 25(9): 2349-2355. Ho, K. T. and R. M. Burgess (2004). "Use of powdered coconut charcoal as a toxicity identification and evaluation manipulation for organic toxicants in marine sediments." Environmental Toxicology and Chemistry 23(9): 2124-2131. Janssen, E. M., Y. Choi, et al. (2012). "Assessment of nontoxic, secondary effects of sorbent amendment to sediments on the deposit-feeding organism Neanthes arenaceodentata." Environmental Science and Technology 46(7): 4134-4141. Janssen, E. M. L., M. N. Croteau, et al. (2010). "Measurement and modeling of polychlorinated biphenyl bioaccumulation from sediment for the marine polychaete Neanthes arenaceodentata and response to sorbent amendment " Environmental Science & Technology 44: 2857-2863. Janssen, E. M. L., A. M. P. Oen, et al. (2011). "Assessment of field-related influences on polychlorinated biphenyl exposures and sorbent amendment using polychaete bioassays and passive sampler measurements." Environmental Toxicology and Chemistry 30(1): 173-180. Jonker, M. T., M. P. Suijkerbuijk, et al. (2009). "Ecotoxicological effects of activated carbon addition to sediments." Environmental Science & Technology 43(15): 5959-5966. Josefsson, S., M. Schaaning, et al. (2012). "Capping efficiency of various carbonaceous and mineral materials for in situ remediation of polychlorinated dibenzo-p-dioxin and dibenzofuran contaminated marine sediments: Sediment-to-water fluxes and bioaccumulation in boxcosm tests." Environmental Science and Technology 46: 3343-3351. Koelmans, A. and M. Jonker (2011). "Effects of black carbon on bioturbation-induced benthic fluxes of polychlorinated biphenyls." Chemosphere 84: 1150-1157. Kupryianchyk, D., A. Noori, et al. (2013). "Bioturbation and Dissolved Organic Matter Enhance Contaminant Fluxes from Sediment Treated with Powdered and Granular Activated Carbon." Environmental Science and Technology doi: 10.1021/es3040297. Kupryianchyk, D., E. P. Reichman, et al. (2011). "Ecotoxicological effects of activated carbon amendments on macroinvertebrates in non-polluted and polluted sediments " Environmental Science and Technology 45(19): 8567-8574.
S11
McLeod, P. B., S. N. Luoma, et al. (2008). "Biodynamic modeling of PCB uptake by Macoma balthica and Corbicula fluminea from sediment amended with activated carbon." Environmental Science and Technology 42(2): 484-490. McLeod, P. B., M. J. Van den Heuvel-Greve, et al. (2007). "Biological uptake of polychlorinated biphenyls by Macoma balthica from sediment amended with activated carbon." Environmental Toxicology and Chemistry 26(5): 980-987. Millward, R. N., T. S. Bridges, et al. (2005). "Addition of activated carbon to sediments to reduce PCB bioaccumulation by a polychaete (Neanthes arenaceodentata) and an amphipod (Leptocheirus plumulosus)." Environmental Science & Technology 39(8): 2880-2887. Nybom, I., D. Werner, et al. (2012). "Responses of Lumbriculus variegatus to activated carbon amendments in uncontaminated sediments." Environmental Science and Technology 46(23): 12895–12903. Sun, X., D. Werner, et al. (2009). "Modeling PCB mass transfer and bioaccumulation in a freshwater oligochaete before and after amendment of sediment with activated carbon." Environmental Science & Technology 43(4): 1115-1121. Sun, X. L. and U. Ghosh (2007). "PCB bioavailability control in Lumbriculus variegatus through different modes of activated carbon addition to sediments." Environmental Science & Technology 41(13): 4774-4780. Tomaszewski, J. E. and R. G. Luthy (2008). "Field deployment of polyethylene devices to measure PCB concentrations in pore water of contaminated sediment." Environmental Science & Technology 42(16): 6086-6091.
S12
Biological responses to activated carbon amendments in sediment remediation ELISABETH M.-L. JANSSEN, †* BARBARA A. BECKINGHAM, ‡ †
Institute of Biogeochemistry and Pollutant Dynamics, Swiss Federal Institute of Technology (ETH), Universitätsstrasse 16, 8092 Zürich, Switzerland ‡
Center for Applied Geoscience, University Tübingen, Hölderlinstrasse 12, 72074 Tübingen, Germany
Number of Figures: 1 Number of Tables: 5 Number of pages: 12
S1
Biodynamic Modeling The simplified differential equation and its solution in closed form of the biodynamic model are described by dCorg dt
= k s ⋅ Cs + k w ⋅ Cw − ke ⋅ Corg (t )
(Eq. 1)
(k s ⋅ Cs + k w ⋅ Cw ) ⋅ (1 − e − ke ⋅t ) ke
(Eq. 2)
Corg (t ) =
The change of chemical tissue concentration in the organism is described by the sum of uptake from solids and water minus elimination processes. Contaminant uptake from water is described by an aqueous uptake rate constant, kw (L g-1 d-1), and the water contaminant concentration, Cw (μg/L). For filter feeders, Cw refers to the surficial water concentration and kw is further defined as the product of filtration rate (FR, L g-1 d-1), and aqueous assimilation efficiency (AEaq). The assimilation efficiency describes the fraction of contaminant that is assimilated into the organism (e.g., through the skin or gut wall) relative to the contaminant concentration to which the organism was exposed. For deposit feeders that do not filter water, the aqueous uptake rate, kw, describes the passive assimilation of contaminants through the water by dermal exposure and Cw can either be the surficial water, the pore water or a combination (e.g. when worms pump water through subsurface borrows for oxygenation). The contaminant uptake from sediment, ks, is described by the product of the organism’s ingestion rate or particle uptake rate (IR, g g-1 d-1), the contaminant sediment concentration Cs (μg g-1 dw), and the organism’s contaminant assimilation efficiency from ingested solids (AEs). The assimilation efficiency can vary greatly among organisms because it is dependent upon the digestive chemistry in the gut (e.g. (Ahrens, Hertz et al. 2001; Arnot and Gobas 2004) and references herein). Assimilation of pollutants through the aqueous phase is often dominated by the uptake of particulates with the water (Burton and Johnston 2010). Activated carbon amendments reduce (a) the aqueous concentration (Cw), and (b) reduce the assimilation efficiency from the solids (AEs) because the availability is much lower from AC than from native sediment. The value of AEs has to be modified for amended sediment accordingly:
S2
AEs
amended
= Fsed ⋅ AEssed + (1 − Fsed ) ⋅ AEsAC
(Eq. 3)
with AEsamended being the assimilation efficiency from the AC amended sediment, Fsed being the fraction of chemicals that remains on the sediment, AEssed being the assimilation efficiency from untreated sediment and AEsAC being the assimilation efficiency from AC. The value for Fsed can be estimated from the ratio of water concentration from well mixed slurries at quasi steady state with and without AC present. Fsed
CwAC = noAC Cw
(Eq. 4)
with CwAC and CwnoAC being the water concentrations before and after AC addition, assuming linear partitioning at low aqueous concentrations. Pathways that account for loss of contaminants from the organism’s tissue have to be subtracted from those uptake terms (Eq. 1 and 2). Loss can occur by elimination, described by the exponential rate constant ke (g g-1 d-1), when pollutants un-assimilated in the gut or gills are excreted. Exponential growth rates can be added to the loss term accounting for growth dilution (pseudo elimination). Similarly, other loss mechanisms can be included, e.g., biotransformation, however, in the case of polychlorinated biphenyls and the species employed for the modeling below, transformation can be neglected.
S3
Table S1. Values of physiological and model parameters for the benthic invertebrates used to model polychlorinated biphenyl concentrations in their tissue after 28 days. Sediment and aqueous concentrations were used as reported in the respective studies, range reported when multiple sediments were used for exposure.
Parameter, unit Filtration rate (FR), L water/ g dry wt / d Aqueous assimilation efficiency (AEaq), % Aqueous uptake rate constant (kw) = FR x AEaq L water / g dry wt / d Ingestion rate (IR), g / g dry wt / d Sediment assimilation efficiency from sediment (AEs), % Sediment assimilation efficiency from amended sediment (AEsamended), % Elimination rate constant (ke), 1/d
Neanthes arenaceodentata4
Macoma balthica5 2
Corbicula fluminea5 45
50
20
0.5
Lumbriculus variegatus6
17.8
3.5
0.25
0.03
10.7
7
20
20
20
0.36
1.4
1.4
1.0
0.04
0.04
0.04
0.51
Sediment PCB concentration (Cs) µg/g
1.2
3.0-7.0
6.5
6.8-87.4
Aqueous concentration (CwnoAC) after amendment (CwAC) µg/L
0.02
0.04-0.05
0.2
0.8-2.5
0.004
0.01-0.03
0.0001-0.0006 0.04-0.063
S4
Figure S1. Measured tissue concentrations of polychlorinated biphenyls against predicted values employing the biodynamic model for Macoma balthica (blue)(McLeod, Van den Heuvel-Greve et al. 2007), Neanthes arenaceodentata (green)(Janssen, Croteau et al. 2010), Corbicula fluminea (red)(McLeod, Van den Heuvel-Greve et al. 2007) , Lumbriculus variegatus (orange)(Sun, Werner et al. 2009) exposed to untreated (open symbols) and activated carbon amended sediments (closed symbols). Error bar represent one standard deviation of the measured concentrations. Solid line represents the linear fit of all data (N = 148), dashed lines represent the 1:1, 2:1 and 1:2 relationships.
S5
Table S2. Survival: Effects of activated carbon amendment on benthic invertebrates relative to exposure to untreated sediment. #
Species
1
Abra nitida
2
Americamysis bahia
3
Ampelisca abdita
4
Amphiura spp.
5
Asellus aquaticus
6
Asellus aquaticus
7
Asellus aquaticus
8
Corbicula fluminea
9
Corbicula fluminea
10
Corbicula fluminea
11
Corophium volutator
12
Gammarus pulex
13
Gammarus pulex
14
Hinia reticulata
15
Leptocheirus plumulosus
16
Limnodrilus sp.
17
Lumbriculus variegatus
18
Lumbriculus variegatus
19
Lumbriculus variegatus
20
Lumbriculus variegatus
21
Lumbriculus variegatus
22
Lumbriculus variegatus
23
Macoma balthica
24
Macoma nasuta
25
Mytilus edulis
26
Nassanus nitidus (H. reticulata)
Effect on survival no
yes (positive)
yes (positive) no no
yes (positive) yes (positive) yes (positive)
yes (negative) no no
yes (positive)
yes (negative) no no
Notes Thin layer cap (0.5, 3 cm AC) to dioxin/furan polluted sediment Improved survival in contaminated sediment
(Josefsson, Schaaning et al. 2012)
Amendment to uncontaminated sediment
(Kupryianchyk, Reichman et al. 2011)
Improved survival in contaminated sediment
See #[1] above
Amendment to contaminated sediment
Amendment to contaminated sediment
Survival 12% higher as for untreaded sediment (85%), 0.7% AC resulted in 95% survival Survival 12% lower as for untreaded sediment (85%), 2.5% AC resulted in 75% survival 1.3% AC same survival as untreated sediment Amendment of 25% AC
Survival is 30% in 3-30% AC and only 0-5% survival in untreated, polluted sediment Survival in untreated sediment 80-85%; with 3, 6, 15, 30% AC: survival: 40, 5, 0, 0; LC50 = 3.1%
(Josefsson, Schaaning et al. 2012)
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Noori et al. 2013) (McLeod, Luoma et al. 2008) (McLeod, Luoma et al. 2008) (McLeod, Luoma et al. 2008)
(Jonker, Suijkerbuijk et al. 2009)
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Cornelissen, Breedveld et al. 2006) (Millward, Bridges et al. 2005) (Sun and Ghosh 2007)
no
(Beckingham and Ghosh 2011)
no
(Beckingham and Ghosh 2011)
no
(Nybom, Werner et al. 2012)
no
(Kupryianchyk, Noori et al. 2013)
no yes (positive)
(Ho and Burgess 2004)
(Jonker, Suijkerbuijk et al. 2009)
no
no
(Ho and Burgess 2004)
(Koelmans and Jonker 2011)
no
no
Reference
(McLeod, Van den Heuvel-Greve et al. 2007)
Survival increased by 83%, (only 17% survival in untreated, polluted sediment)
(Cho, Smithenry et al. 2007)
(Tomaszewski and Luthy 2008)
(Josefsson, Schaaning et al. 2012)
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27
Neanthes arenaceodentata
28
Neanthes arenaceodentata
29
Neanthes arenaceodentata
30
Neanthes arenaceodentata
31
Nereis diversicolor
32
Nereis spp.
no
(Millward, Bridges et al. 2005)
no
(Janssen, Choi et al. 2012)
(Janssen, Croteau et al. 2010)
no
(Janssen, Oen et al. 2011)
no no no
Survival similar between uncapped and AC-cap, but lower for AC compared to non-active cap
(Cornelissen, Breedveld et al. 2006)
(Josefsson, Schaaning et al. 2012)
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Table S3. Growth: Effects of activated carbon amendment on benthic invertebrates relative to exposure to untreated sediment. #
Species
1
Asellus aquaticus
2
Asellus aquaticus
3
Corbicula fluminea
4
Corbicula fluminea
5
Gammarus pulex
6
Gammarus pulex
7
Leptocheirus plumulosus
8
Lumbriculus variegatus
9
Macoma balthica
10
Mytilus edulis
11
Neanthes arenaceodentata
12
Neanthes arenaceodentata
13
Neanthes arenaceodentata
14
Neanthes arenaceodentata
15
Nassanus nitidus (H. reticulata)
16
Abra nitida
17
Amphiura spp.
Effect on growth yes (negative) No
yes (negative) no no no no
yes (negative) no no
yes (negative) yes (negative) no no no no no
Notes EC50 = 5.3%, amendment to polluted sediment amendment to unpolluted sediment
Reduced growth at 1.3% and 25% AC, but large deviation among replicates 0.7% AC (reduced growth only at higher dose) Amendment to unpolluted sediment
Amendment to contaminated sediment
sediment specific, AC size and dose effect
50% less growth in AC amended sediment Reduced growth for 2 out of 5 sediments 3 out of 5 sediments show no effect
Thin layer cap (0.5, 3 cm AC) to dioxin/furan polluted sediment See # [14] above See # [14] above
Reference (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (McLeod, Luoma et al. 2008) (McLeod, Luoma et al. 2008)
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Millward, Bridges et al. 2005) (Nybom, Werner et al. 2012)
(McLeod, Van den Heuvel-Greve et al. 2007) (Tomaszewski and Luthy 2008) (Millward, Bridges et al. 2005) (Janssen, Choi et al. 2012) (Janssen, Oen et al. 2011)
(Janssen, Choi et al. 2012)
(Josefsson, Schaaning et al. 2012) (Josefsson, Schaaning et al. 2012) (Josefsson, Schaaning et al. 2012)
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Table S4. Lipid content: Effects of activated carbon amendment on benthic invertebrates relative to exposure to untreated sediment. #
Species
1
Hinia reticulata
2
Leptocheirus plumulosus
3
Lumbriculus variegatus
4
Lumbriculus variegatus
5
Lumbriculus variegatus
6
Lumbriculus variegatus
7
Macoma nasuta
8
Neanthes arenaceodentata
9
Neanthes arenaceodentata
10
Neanthes arenaceodentata
11
Neanthes arenaceodentata
12
Neanthes arenaceodentata
13
Neanthes arenaceodentata
14
Nereis diversicolor
15
Nereis (spp.)
16
Nassanus nitidus (H. reticulata)
Effect on lipid content no no
yes (negative) no no
yes (negative) no
yes (negative) yes (positive)
yes (negative) no no no no no no
Notes
Reference (Cornelissen, Breedveld et al. 2006)
5-15% lower lipid content, in sediment without AC: lipid increases over time Ex situ, with field-amended sediments
dose effect, but high variability especially when organisms were loosing weight 66% lower lipid content in AC amendment
Ex situ, lipid content increased by 50% from average of 0.4% to 0.6% Slightly reduced lipid content for amendment to 1 out of 5 sediments In situ
4 out of 5 sediments show no effect
Thin layer cap (0.5, 3 cm AC) to dioxin/furan polluted sediment See # [14] above
(Millward, Bridges et al. 2005)
(Jonker, Suijkerbuijk et al. 2009) (Sun and Ghosh 2007)
(Beckingham and Ghosh In prep) (Nybom, Werner et al. 2012) (Cho, Smithenry et al. 2007)
(Janssen, Croteau et al. 2010) (Janssen, Oen et al. 2011)
(Janssen, Choi et al. 2012)
(Millward, Bridges et al. 2005) (Janssen, Oen et al. 2011)
(Janssen, Choi et al. 2012)
(Cornelissen, Breedveld et al. 2006) (Josefsson, Schaaning et al. 2012) (Josefsson, Schaaning et al. 2012)
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Table S5. Behavior: Effects of activated carbon amendment on benthic invertebrates relative to exposure to untreated sediment. #
Species
1
Asellus aquaticus
2
Asellus aquaticus
3
Asellus aquaticus
4
Asellus aquaticus
5
Asellus aquaticus
6
Asellus aquaticus
7
Corophium volutator
8
Gammarus pulex
9
Gammarus pulex
10
Gammarus pulex
11
Gammarus pulex
12
Gammarus pulex
13
Gammarus pulex
14
Lumbriculus variegatus
15
Lumbriculus variegatus
16
Lumbriculus variegatus
17
Lumbriculus variegatus
Effect on behavior no no no no no no
yes (negative)
Notes avoidance, amendment to polluted sediment
(Kupryianchyk, Reichman et al. 2011)
locomotion, amendment to unpolluted sediment
(Kupryianchyk, Reichman et al. 2011)
avoidance, amendment to unpolluted sediment locomotion, amendment to polluted sediment ventilation, amendment to polluted sediment
ventilation, amendment to unpolluted sediment
no
inconsistent, avoidance for 4,7,15%AC amendments but not for 25% amentdment avoidance, amendment to polluted sediment
no
locomotion, amendment to unpolluted sediment
no no no no
yes (negative) yes (negative) yes (negative) no
Reference
avoidance, amendment to unpolluted sediment locomotion, amendment to polluted sediment ventilation, amendment to polluted sediment
ventilation, amendment to unpolluted sediment egestion, 92% reduction in 1 to 25% AC
egestion, dose and particle size dependend reproduction, sediment specific, study not designed to measure reproduction avoidance
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Jonker, Suijkerbuijk et al. 2009)
(Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Kupryianchyk, Reichman et al. 2011) (Jonker, Suijkerbuijk et al. 2009) (Nybom, Werner et al. 2012)
(Nybom, Werner et al. 2012) (Nybom, Werner et al. 2012)
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McLeod, P. B., S. N. Luoma, et al. (2008). "Biodynamic modeling of PCB uptake by Macoma balthica and Corbicula fluminea from sediment amended with activated carbon." Environmental Science and Technology 42(2): 484-490. McLeod, P. B., M. J. Van den Heuvel-Greve, et al. (2007). "Biological uptake of polychlorinated biphenyls by Macoma balthica from sediment amended with activated carbon." Environmental Toxicology and Chemistry 26(5): 980-987. Millward, R. N., T. S. Bridges, et al. (2005). "Addition of activated carbon to sediments to reduce PCB bioaccumulation by a polychaete (Neanthes arenaceodentata) and an amphipod (Leptocheirus plumulosus)." Environmental Science & Technology 39(8): 2880-2887. Nybom, I., D. Werner, et al. (2012). "Responses of Lumbriculus variegatus to activated carbon amendments in uncontaminated sediments." Environmental Science and Technology 46(23): 12895–12903. Sun, X., D. Werner, et al. (2009). "Modeling PCB mass transfer and bioaccumulation in a freshwater oligochaete before and after amendment of sediment with activated carbon." Environmental Science & Technology 43(4): 1115-1121. Sun, X. L. and U. Ghosh (2007). "PCB bioavailability control in Lumbriculus variegatus through different modes of activated carbon addition to sediments." Environmental Science & Technology 41(13): 4774-4780. Tomaszewski, J. E. and R. G. Luthy (2008). "Field deployment of polyethylene devices to measure PCB concentrations in pore water of contaminated sediment." Environmental Science & Technology 42(16): 6086-6091.
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