It is inevitable that carbon nanotubes (CNTs) will be released to and widely dispersed in environmental ecosystems, given their numerous expected applications. Determination of their potential for bioaccumulation by ecological receptors is thus critical. Previous, research involving several different terrestrial and benthic organisms has indicated that CNTs spiked to soils or sediments do not bioaccumulate. Conversely, we report here distinctly different uptake and depuration behaviors for an aquatic organism, Daphnia magna, in a water-only system. After 48 h of exposure of this organism to a 0.4 microg/mL solution of dispersed nanotubes, the CNTs comprised 6.3 +/- 1.5% of the residual organism dry mass. Moreover, these organisms were unable to excrete the nanotubes to either clean artificial freshwater or filtered Lake Kontiolampi water after 24 h depuration periods, even though the lake water had a substantial concentration of natural organic matter. Addition of algae to the water during the depuration period did result however in release of a significant fraction (approximately 50-85%) of the accumulated CNTs within the first few hours, but little thereafter. Light microscopy results suggest that the vast majority of the accumulated CNTs remained in the organisms' guts and were not absorbed into cellular tissues.
A simple method for analyzing masses of water suspended fullerenes (nC60) in Daphnia magna by extracting to toluene and measuring by ultraviolet-vis spectrophotometry was developed. This method was used to assess bioaccumulation and depuration rates by daphnia after nC60 exposure in artificial freshwater. Accumulation was rapid during the first few hours, and based on accumulation modeling, 90% of the steady-state concentration was reached in 21 h. After exposure for 24 h to a 2 mg/L fullerene solution, the daphnia accumulated 4.5+/-0.7 g/kg wet weight, or 0.45% of the organism wet mass. Daphnids exposed to 2 mg/L fullerenes for 24 h eliminated 46 and 74% of the accumulated fullerenes after depuration in clean water for 24 and 48 h, respectively. Transmission electron microscopy revealed that the majority of the fullerenes present in the gut of daphnids were large agglomerates. The significant fullerene uptake and relatively slow depuration suggest that D. magna may play a role as a carrier of fullerene from one trophic level to another. Additionally, D. magna may impact the fate of suspended fullerene particles in aquatic ecosystems by their ability to pack fullerene agglomerates into larger particles than were found in the exposure water, and then excrete agglomerates that are not stable in water, causing them to settle out of solution. This process decreases fullerene exposure to other aquatic organisms in the water column but may increase exposure to benthic organisms in the sediment.
An environmentally realistic method to test fullerene (C(60) ) toxicity to the benthic organism Chironomus riparius was created by allowing suspended fullerenes to settle down, making a layer on top of the sediment. To test the hypothesis that higher food concentrations will reduce toxic responses, two food concentrations were tested (0.5 and 0.8% Urtica sp.) in sediment containing fullerene masses of 0.36 to 0.55 mg/cm(2) using a 10-d chronic test. In the 0.5% food level treatments, there were significant differences in all growth-related endpoints compared with controls. Fewer effects were observed for the higher food treatment. Fullerene agglomerates were observed by electron microscopy in the gut, but no absorption into the gut epithelial cells was detected. In the organisms exposed to fullerenes, microvilli were damaged and were significantly shorter. The potential toxicity of fullerene to C. riparius appears to be caused by morphological changes, inhibiting larval growth.
Activated carbon (AC) amendment is a recently developed sediment remediation method. The strong hydrophobic organic contaminant sorption efficiency of AC has been shown in several studies, but effects on benthic organisms require more investigation. The AC induced effects on egestion rate, growth and reproduction of Lumbriculus variegatus were studied by applying bituminous coal based AC in three different particle size fractions, namely <63 μm (90%, AC(p)), 63-200 μm (AC(m)) and 1000 μm (AC(g)), to natural uncontaminated (HS) and artificial sediment (AS). Egestion rate, growth and reproduction decreased with increasing AC concentration and finer AC particle fractions, effects being stronger on HS than on AS sediment. Lipid content in AS was reduced already at the lowest AC doses applied (AC(p) and AC(m) 0.05%, AC(g) 0.25%). In addition, hormesis-like response was observed in growth (AS) and reproduction (AS, HS) indicating that AC may disturb organisms even at very low doses. Potential ecological effects need to be further evaluated in an amendment- and site-specific manner.
Bioavailability of benzo[a]pyrene (BaP) and 3,3',4,4'-tetrachlorobiphenyl (TCB) was studied in natural lake water containing dissolved organic matter (DOM). Lake water was diluted to give a dissolved organic carbon (DOC) range of 1 to 20 mg/L. Partition coefficients for the model compounds were assessed at different DOM concentrations and over time with three different methods, namely equilibrium dialysis and reverse-phase and liquid-liquid extraction. In addition, biological partition coefficients were estimated from the difference in the bioconcentration of the model compounds in Daphnia magna in the presence and absence of DOM. Results showed that bioavailability of the model compounds was reduced by the presence of DOM. The equilibrium dialysis method gave the best estimates for bioavailability of the model compounds when compared with biologically determined values. Both the reverse-phase and the liquid-liquid extraction overestimated the bioavailable fraction. The more pronounced overestimation of bioavailable fraction of TCB suggested that the sorption of TCB was not only lower but the interaction was also weaker than that of BaP. Increasing DOM concentration produced lower partition coefficients and the effect seemed to be more pronounced when measured by the reverse-phase and the extraction methods.
The sorption efficiency and possible secondary effects of activated carbon (AC) (ø 63-200 μm) was studied with Lumbriculus variegatus in three PCB contaminated sediments applying long AC-sediment contact time (3 years). AC amendment efficiently reduced PCB bioavailability as determined with both, L. variegatus bioaccumulation test and passive samplers. However, dose related secondary effects of AC on egestion rate and biomass were observed (applied doses 0.25% and 2.5% sediment dry weight). The sorption capacity and secondary effects remained similar when the experiments were repeated after three years of AC-sediment contact time. Further, transmission electron microscopy (TEM) samples revealed morphological changes in the L. variegatus gut wall microvilli layer. Sediment properties affected both sorption efficiency and secondary effects, but 2.5% AC addition had significant effects regardless of the sediment. In, conclusion, AC is an efficient and stable sorbent to decrease the bioavailability of PCBs. However, sediment dwelling organisms, such as Oligochaete worms in this study, may be sensitive to the carbon amendments. The secondary effects and possible morphological changes in benthic organisms should not be overlooked as in many cases they form the basis of the aquatic food webs.
Association of benzo[a]pyrene (BaP), pyrene, 3,3¢,4,4¢-tetrachlorobiphenyl (TCB) and 2,2¢,4,4¢-tetrabromo diphenyl ether (TBDE) with natural dissolved organic matter (DOM) was studied. The DOM samples were previously collected from natural waters at five Nordic sites during fall 1999 and spring 2000, isolated by the reverse osmosis method, and thoroughly characterized. The purpose was to determine the essential characteristics that predict the sorption capacity of DOM for hydrophobic contaminants. DOM isolates were dissolved in artificial freshwater to give a dissolved organic carbon concentration of 15 mg L -1 . Partition coefficients (K DOC ) of the model compounds between water and DOM were measured by the equilibrium dialysis method. Further, the bioavailability of BaP and pyrene to Daphnia magna Aquatic Sciences was tested in the presence of DOM with various qualities. A strong negative correlation was found for the K DOC values of BaP (R = -0.922) and pyrene (R = -0.929) with spectral absorbency ratio (A 254 /A 400 ), while the correlation (R = -0.760) was weaker for the K DOC values of TCB. The K DOC values for TCB correlated (R = 0.849) strongly with specific visible absorbency (A 600 /TOC), while the K DOC values for TBDE correlated (R = -0.739) with relative fluorescence emission. Generally, bioavailability of BaP and pyrene to D. magna reflected the measured association of the compounds with DOM. The data emphasize the importance of aromaticity of DOM, estimated by simple spectroscopic methods, in predicting sorption capacity for polycyclic aromatic hydrocarbons. The situation with halogenated compounds still remains unclear.
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