Seasonal variation of polychlorinated biphenyl congeners in surficial sediment, trapped settling material, and suspended particulate material in Lake Michigan, USA.

A unique time series of surface sediment, trapped settling material, and suspended particulate material polychlorinated biphenyl (PCB) samples were collected at a 45-m deep site off Grand Haven (MI, USA) over a 14-month period. Both concentrations and congener distributions remained constant for the sediments, although there were seasonal and interannual variability in the other matrices. Trapped settling material and suspended particulate material PCB concentrations were substantially lower (~50%) in 1997 than in the samples from December 1997 through July 1998. The cause could not be determined from the data collected, but there were some very large storms during the winter-spring period of 1998, resulting in major sediment resuspension throughout the southern basin. Observed seasonal variation in PCB concentration and congener distribution on particles likely was due to the changes in particle composition. These include particle size and the source of particles (such as the amount of resuspended sediment in trapped settling material), and the role of diagenesis of the organic matter on particles.

Predicting bioavailability of sediment-associated organic contaminants for Diporeia spp. and oligochaetes.

Biota-sediment accumulation factors (BSAF) were calculated for Diporeia spp. and oligochaete worms exposed to polychlorinated biphenyls (PCBs) and polycyclic aromatic hydrocarbons (PAHs) from field-collected sediment. These data were compared to the contaminant fraction extracted from sediment with Tenax resin using a 24 h extraction. A previous laboratory study suggested a linear relationship between log BSAF and the contaminant fraction rapidly desorbed from sediment. However, the BSAF data in our study did not fit this relationship. Better predictive regressions for both PCBs and PAHs were found when the log of the lipid-normalized organism contaminant concentrations were plotted against the log of the Tenax-extracted organic carbon-normalized sediment contaminant concentration. Regression lines for the two species had the same slope, but the Diporeia intercept was 2.3 times larger. When adjusted for a 6 h Tenax extraction, based on a regression between 6 and 24 h Tenax extractions, data from this study and two other studies that included multiple oligochaete species fit a single predictive regression. The exception included some PAHs that fell below the regression line. Thus, a single relationship generally predicted bioaccumulation across sediments, compound classes, oligochaete species, and among laboratories.

Time-dependent toxicity of dichlorodiphenyldichloroethylene to Hyalella azteca.

Temporal effects on body residues of dichlorodiphenyldichloroethylene (DDE) associated with mortality in the freshwater amphipod Hyalella azteca were evaluated. Toxicokinetics and body residues were determined from water-only exposures that varied from 4 to 28 d, and DDE concentrations ranging from 0.0013 to 0.045 micromol L(-1). Uptake and elimination parameters were not affected significantly by the various temporal and concentration treatments. Uptake rate coefficients ranged from 134.3 to 586.7 ml g(-1) h(-1), and elimination rate coefficients ranged from 0.0011 to 0.0249 h(-1). Toxicity metric values included body residue for 50% mortality at a fixed sample time (LR50) and mean lethal residue to produce 50% mortality from individual exposure concentrations (MLR50) for live organisms and dead organisms. A twofold increase occurred in the MLR50 values calculated using live organisms compared to MLR50 values using dead organisms. Toxicity and kinetic data were fit to a damage assessment model that allows for the time course for toxicokinetics and damage repair, demonstrating the time-dependence of body residues to toxicity. The DDE appeared to act through a nonpolar narcosis mode of action for both acute and chronic mortality in H. azteca. Furthermore, the temporal trend in the toxic response using body residue as the dose metric is steep and found to be similar to another chlorinated hydrocarbon, pentachlorobenzene, but was more potent than that found for polycyclic aromatic hydrocarbons (PAHs).

Effect of 3,4,3',4'-tetrachlorobiphenyl on the reworking behavior of Lumbriculus variegatus exposed to contaminated sediment.

The reworking response (bioturbation) of the oligochaete Lumbriculus variegatus was measured by following the burial rate and spread of a 137Cs marker layer translating worm activity into a biological burial rate (Wb) and a biological diffusion rate constant (Db) for surficial sediment mixing. Reworking was measured at 10 and 22 degrees C in two sediments: a reference site sediment dosed with 3,4,3',4'-tetrachlorobiphenyl (TCBP) and a field-collected sediment from a polychlorinated biphenyl (PCB)-contaminated site in Dicks Creek (DCC, Middletown, OH, USA). The body residue associated with response to TCBP also was determined. Reduction in the temperature from 22 to 10 degrees C reduced both Wb and Db by a factor of approximately two. The internal TCBP concentration to reduce the Wb by 50% was 96 nmol/g (95% CI 45-225 nmol/g) and 124 nmol/g (40-547 nmol/g) (28 and 36 microg/g) wet weight at 22 and 10 degrees C, respectively, and was independent of temperature. The Wb for the DCC sediment was lower than observed for the highest TCBP treatment. The internal body residue for total PCB for worms exposed to DCC sediment was 20-fold lower than TCBP in worms exposed to the lowest TCBP treatment on a molar basis. Comparing body residues of total PCB to TCBP assumes that the PCB congeners act additively on a molar basis. The DCC site contained a higher proportion of coarse material and a lower organic carbon concentration. The difference in sediment characteristics was assumed to be responsible for differences in the Wb.

Comparing behavioral and chronic endpoints to evaluate the response of Lumbriculus variegatus to 3,4,3',4'-tetrachlorobiphenyl sediment exposures.

The response of Lumbriculus variegatus to 3,4,3',4'-tetrachlorobiphenyl (TCBP) was examined with feeding behavior and changes in carbon assimilation by using stable carbon isotopes at 22 and 10 degrees C. The classical measure of feeding behavior determined on a subset of sediment for which the biological burial rate was determined in a companion study allowed direct method comparison. This comparison helped address relationships between biological burial rate, feeding rate, and bioaccumulation. The change in stable isotope composition reflects the total metabolic activity by measuring carbon assimilation rate and was compared to feeding rate, biological burial rate (as determined in the companion study), and reproduction. Decreasing the temperature from 22 to 10 degrees C resulted in a twofold reduction in feeding rate and carbon assimilation. The fractional decline in feeding rate relative to the control mimicked the decline in the biological burial rate with increasing TCBP concentration that was found in the companion study. The bioaccumulation factor declined with increasing TCBP sediment concentration, tracking the feeding rate decline. Stable isotope measures showed differences in metabolic rates between the exposure temperatures but did not distinguish a metabolic rate change at 22 degrees C among TCBP treatments. Likewise, reproduction declined from 22 to 10 degrees C, with no reproduction at 10 degrees C. Like the stable isotope measure, no dose response was found among TCBP treatments at 22 degrees C. The reduction in carbon assimilation rate tracked the reduction in reproduction with lower temperature.

Investigating the role of desorption on the bioavailability of sediment-associated 3,4,3',4'-tetrachlorobiphenyl in benthic invertebrates.

Only a fraction of all sediment-associated hydrophobic organic contaminants are bioavailable, and a simple Tenax extraction procedure may estimate this fraction. Bioavailability is assumed to coincide with the rapidly and, possibly, slowly desorbing sediment-associated contaminant. River sediment was spiked with radiolabeled (14C) and nonradiolabeled (12C) 3,4,3',4'-tetrachlorobiphenyl (TCBP), and desorption kinetics using Tenax extraction were obtained at 10 degrees C and 22 degrees C. Bioaccumulation was measured in Lumbriculus variegatus, Chironomus tentans, and Hyalella azteca. Desorption of TCBP was triphasic at 22 degrees C and slowed at 10 degrees C to show only biphasic kinetics. The rapidly desorbing fractions decreased with increasing TCBP sediment concentration. The biota sediment accumulation factors, biota accumulation factors, and sediment clearance coefficients (ks) also decreased with increasing sediment TCBP concentration. The rapidly plus slowly desorbing fractions and the total TCBP desorbed when 99.9% of the rapidly desorbing fraction had desorbed were used to estimate bioavailable TCBP. These Tenax-based fractions did not explain the decreasing bioavailability with increasing TCBP load. Several factors, such as animal behavior and TCBP water solubility limitations, were evaluated to explain the concentration effect, but the most likely cause was severe diffusion limitations in whole sediment that were not predicted by the fully mixed Tenax extraction. Therefore, desorbing fractions determined by Tenax extraction overestimated the bioavailable fractions in sediments.