In situ sediment amendment with sorbents such as activated carbon (AC) can effectively reduce the bioavailability of hydrophobic organic chemicals such as polychlorinated biphenyls (PCBs). However, there is limited experimental or modeling assessment of how bioavailability changes in sediments impact bioaccumulation in fish - the primary risk driver for exposure to humans and top predators in the aquatic ecosystem. In the present study we performed laboratory aquarium experiments and modeling to explore how PCB sorption in sediments impacted exposure pathways and bioaccumulation in fish. Results showed that freely dissolved PCBs in porewater and overlying water measured by passive sampling were reduced by more than 95% upon amendment with 4.5% fine granular AC. The amendment also reduced the PCB uptake in fish by 87% after 90 days of exposure. Measured freely dissolved concentrations were incorporated in equilibrium and kinetic models for predicting uptake by fish. Predicted uptake using the kinetic model was generally within a factor of 2 for total PCBs measured in fish. The kinetic model output was most sensitive to overlying water PCBs, lipid fraction, and dissolved oxygen concentration (regulating gill ventilation). Our results indicate that by incorporating changes in freely dissolved PCB concentrations in bioaccumulation models it is possible to predict effectiveness of sediment remediation in reducing PCB uptake in fish.

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Uptake of polychlorinated biphenyls (PCBs) by fish is controlled by the bioavailability of ingested PCBs in the gut and the freely dissolved concentration in the water moving across the gills. Prediction of bioaccumulation in fish relies on models that account for these exposure routes, however, these models typically do not account for incidental ingestion of sediment by fish, which is not well studied. The literature values for the PCB assimilation efficiency (AE) in the gut have been reported for compounds in food matrices and not associated with sediment particles. It is also unclear how mitigation strategies that alter PCB bioavailability in sediments affect predictions made by the bioaccumulation models when sediment ingestion is involved. To test the bioavailability of PCBs from treated and untreated sediments, dietary AEs were measured for 16 polychlorinated biphenyl (PCB) congeners in mummichogs (Fundulus heteroclitius) that were fed four experimental diets. Diets consisted of PCB-spiked earthworms, spiked untreated sediment mixed with earthworms, spiked activated carbon (AC)-treated sediment mixed with earthworms, and spiked AC mixed with earthworms. AEs were determined by calculating the ratio of PCB mass in the fish tissue to the PCB mass in the food after a pulse feeding experiment. AEs of PCBs associated with earthworm diet were similar to the values reported in the literature. Fish that were fed the PCB-spiked untreated sediment and AC particles exhibited the highest and lowest AEs respectively over a wide KOW range, respectively. AEs of sediment-bound PCBs were significantly reduced (31 to 93% reduction for different congeners) upon amendment with AC. The present study indicates that assimilation of PCBs can be reduced by sorption to black carbon.