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ABSTRACT: Enantiomeric analysis can be used as a complementary tool for source apportionment of chiral compounds, particularly for alpha-HCH. In this study we used archived samples from studies related to the distribution of POPs in air-water and air-soil-grass systems. Such approach is based on the behaviour of chiral compounds released into the atmosphere from a primary source, when they are expected to show racemic or close to racemic composition. Contrarily, when chiral compounds have been reemitted from secondary sources (e.g. water or soil), their enantiomeric signatures are frequently non-racemic and are similar to the signature of the secondary source. To show such evidence, extracts from passive air samples deployed throughout Europe were analyzed for the enantiomers of alpha-HCH. The proximity to a large water body showed a high impact on the enantiomeric signatures: Baltic air had enantiomeric fractions (EFs) <0.500, while Mediterranean air had predominantly EFs >0.500. Similarly, Atlantic air showed a latitude influence: above 50 degrees N most EFs <0.500, whereas at latitudes below 50 degrees N, EFs were >0.500. A similar trend was also observed for EFs of alpha-HCH measured in air samples from a latitudinal transect during an Atlantic cruise. This transect shows that samples from higher latitudes (above 40 degrees N) have EF <0.500, whereas in the more southern samples (African coast and Southern Atlantic), there is no clear trend for EFs. Inland air samples showed a large range in EF values, with racemic signatures for samples with the highest alpha-HCH concentrations and an increasing spread in the EFs for lower alpha-HCH concentrations. As expected, the EF values of alpha-HCH in air, soils and grass were also impacted by latitude. Correlations between EFs and geographic characteristics of the sampling locations, as well as alpha-HCH concentrations, alpha-/gamma-isomer ratios, or temperature suggest that enantioselective analysis can give additional information on the distribution and sources of alpha-HCH in the environment.
Environment international 02/2010; 36(4):316-22. · 4.79 Impact Factor
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ABSTRACT: Surface seawater and boundary layer atmospheric samples were collected on the FS Polarstern during cruise ARKXX in the North Atlantic and Arctic Ocean in 2004. Samples were analyzed for persistent organic pollutants (POPs), with a focus on organochlorine pesticides, including hexachlorocyclohexanes (HCHs), chlordanes, DDTs, hexachlorobenzene (HCB), and polycyclic aromatic hydrocarbons. In addition, the enantiomer fractions (EFs) of pesticides, notably alpha-HCH and cis-chlordane (CC), were determined. Concentrations of dissolved HCB increased from near Europe (approximately 1-2 pg/L) toward the high Arctic (4-10 pg/L). For dissolved HCB, strongest correlations were obtained with the average air or water temperature during sampling, not latitude. In the western Arctic Ocean, surface waters with elevated concentrations of HCB (5-10 pg/ L) were flowing out of the Arctic Ocean as part of the East Greenland current In contrast to dissolved compounds, atmospheric POPs did not display trends with temperature. Air-water exchange gradients suggested net deposition for all compounds, though HCB was closest to air-water equilibrium. EFs for alpha-HCH in seawater ranged from 0.43 to 0.50, except for two samples from 75 degrees N in the East Greenland Sea, with EFs of 0.31 and 0.37. Lowest EF (0.47) for CC were also at 75 degrees N, other samples had EFs from 0.49 to 0.52. It is suggested that samples from around 75 degrees N in the Greenland Gyre represented a combination of surface and older/deeper Arctic water.
Environmental Science and Technology 09/2009; 43(15):5633-9. · 5.23 Impact Factor
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ABSTRACT: Variability in the enantioselective degradation of chiral organochlorine pesticides (alpha-HCH, cis- and trans-chlordane (CC and TC), and o,p'-DDT) in the field and laboratory was investigated. Background soils presumably receive the same EF signature of a compound via atmospheric deposition and then degrade that compound in a way that can vary over small spatial areas. Background soils from woodland and grassland areas were sampled to compare chiral signatures and determine the spatial variability within a few square meters. The enantiomer fractions, EF = areas of the (+)/[(+)+(-)]-enantiomers, showed variability between and within ecosystems. For example, the EF of CC varied between 0.272 -and 0.558 in nine samples taken over a few square meters, and a range of 0.431-0.506 was found within depths of a few centimeters. Woodland and grassland soils were spiked with alpha-HCH, TC, CC, and o,p'-DDT, and one portion was placed in the field to monitor changes in EF under in situ conditions and the other taken to the laboratory. In general, the enantiomer degradation preferences in the laboratory paralleled those in the field, with some differences. Soil organic matter content and pH exerted a minor influence on this variability. The results of this study have implications for the use of chiral compounds to make inferences about air-soil exchange and for the mechanisms of biodegradation/ biotransformation of anthropogenic compounds in soils.
Environmental Science and Technology 08/2007; 41(14):4965-71. · 5.23 Impact Factor
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ABSTRACT: Enantiomeric analysis can be used as a complementary tool for source apportionment of chiral compounds, particularly for α-HCH. In this study we used archived samples from studies related to the distribution of POPs in air–water and air–soil–grass systems. Such approach is based on the behaviour of chiral compounds released into the atmosphere from a primary source, when they are expected to show racemic or close to racemic composition. Contrarily, when chiral compounds have been reemitted from secondary sources (e.g. water or soil), their enantiomeric signatures are frequently non-racemic and are similar to the signature of the secondary source. To show such evidence, extracts from passive air samples deployed throughout Europe were analyzed for the enantiomers of α-HCH. The proximity to a large water body showed a high impact on the enantiomeric signatures: Baltic air had enantiomeric fractions (EFs) < 0.500, while Mediterranean air had predominantly EFs > 0.500. Similarly, Atlantic air showed a latitude influence: above 50°N most EFs < 0.500, whereas at latitudes below 50°N, EFs were > 0.500. A similar trend was also observed for EFs of α-HCH measured in air samples from a latitudinal transect during an Atlantic cruise. This transect shows that samples from higher latitudes (above 40°N) have EF < 0.500, whereas in the more southern samples (African coast and Southern Atlantic), there is no clear trend for EFs. Inland air samples showed a large range in EF values, with racemic signatures for samples with the highest α-HCH concentrations and an increasing spread in the EFs for lower α-HCH concentrations. As expected, the EF values of α-HCH in air, soils and grass were also impacted by latitude. Correlations between EFs and geographic characteristics of the sampling locations, as well as α-HCH concentrations, α-/γ-isomer ratios, or temperature suggest that enantioselective analysis can give additional information on the distribution and sources of α-HCH in the environment.
Environment International.
