This study addresses the question whether hydrophobic organic chemicals exerting no toxicity at their solubility limit (saturation) can form a toxic mixture. Spiking methods generally do not allow testing exactly at saturation without introducing microcrystals. Passive dosing was thus applied to test the acute toxicity of several high melting point PAHs and their mixtures at the respective saturation levels to aquatic and terrestrial invertebrates. With the aquatic Daphnia magna, anthracene, chrysene, and benzo(a)pyrene resulted in no or limited acute toxicity (0-20%), whereas binary and tertiary mixtures of these resulted in significant acute toxicity (70-88%). Toxicity of PAHs and their mixtures could be fitted with one (sum) chemical activity-response curve in accordance with a similar mode of toxic action (i.e., concentration addition). The effective chemical activity (Ea-50) of 0.029 and the effective concentration on a lipid basis (EC(lipid, eq.)-50) of 95.7 mM were well within the range for baseline toxicity. Similar mixtures showed less toxicity to the terrestrial Folsomia candida due to steady-state body-burdens being below equilibrium partitioning levels. The results of the present study raise questions about the focus of risk assessment schemes and toxicity testing guidelines on individual substances, since apparently non-toxic chemicals might become toxic in a mixture.
Abstract-Passive dosing applies a polymer loaded with test compound(s) to establish and maintain constant exposure in laboratory experiments. Passive dosing with the silicone poly(dimethylsiloxane) was used to control exposure of the terrestrial springtail Folsomia candida to six polycyclic aromatic hydrocarbons (PAHs) in bioconcentration and toxicity experiments. Folsomia candida could move freely on the PAH-loaded silicone, resulting in exposure via air and direct contact. The bioconcentration kinetics indicated efficient uptake of naphthalene, anthracene, and pyrene through air and (near) equilibrium partitioning of these PAHs to lipids and possibly the waxy layer of the springtail cuticle. Toxicities of naphthalene, phenanthrene, and pyrene were related to chemical activity, which quantifies the energetic level and drives spontaneous processes including diffusive biouptake. Chemical activity-response relationships yielded effective lethal chemical activities (La50s) well within the expected range for baseline toxicity (0.01-0.1). Effective lethal body burdens for naphthalene and pyrene exceeded the expected range of 2 to 8 mmol kg À1 fresh weight, which again indicated the waxy layer to be a sorbing phase. Finally, chemical activities were converted into equilibrium partitioning concentrations in lipids yielding effective lethal concentrations for naphthalene and phenanthrene in good correspondence with the lethal membrane burden for baseline toxicity (40-160 mmol kg À1 lipid). Passive dosing was a practical approach for tightly controlling PAH exposure, which in turn provided new experimental possibilities and findings. Environ. Toxicol. Chem. 2013;32:361-369. # 2012 SETAC
The Gold Standard for determining freely dissolved concentrations (C) of hydrophobic organic compounds in sediment interstitial water would be in situ deployment combined with equilibrium sampling, which is generally difficult to achieve. In the present study, ex situ equilibrium sampling with multiple thicknesses of silicone and in situ pre-equilibrium sampling with low density polyethylene (LDPE) loaded with performance reference compounds were applied independently to measure polychlorinated biphenyls (PCBs) in mesocosms with (1) New Bedford Harbor sediment (MA, U.S.A.), (2) sediment and biota, and (3) activated carbon amended sediment and biota. The aim was to cross validate the two different sampling approaches. Around 100 PCB congeners were quantified in the two sampling polymers, and the results confirmed the good precision of both methods and were in overall good agreement with recently published LDPE to silicone partition ratios. Further, the methods yielded C in good agreement for all three experiments. The average ratio between C determined by the two methods was factor 1.4 ± 0.3 (range: 0.6-2.0), and the results thus cross-validated the two sampling approaches. For future investigations, specific aims and requirements in terms of application, data treatment, and data quality requirements should dictate the selection of the most appropriate partitioning-based sampling approach.
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