| 1. |
- Lundstedt-Enkel, Katrin, et al.
(författare)
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A Statistical Resampling Method To Calculate Biomagnification Factors Exemplified with Organochlorine Data from Herring (Clupea harengus) Muscle and Guillemot (Uria aalge) Egg from the Baltic Sea
- 2005
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Ingår i: ENVIRONMENTAL SCIENCE & TECHNOLOGY. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 39:21, s. 8395-8402
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Tidskriftsartikel (refereegranskat)abstract
- A novel method for calculating biomagnification factors is presented and demonstrated using contaminant concentration data from the Swedish national monitoring program regarding organochlorine contaminants (OCs) in herring (Clupea harengus) muscle and guillemot (Uria aalge) egg, sampled from 1996 to 1999 from the Baltic Sea. With this randomly sampled ratios (RSR) method, biomagnification factors (BMFRSR) were generated and denoted with standard deviation (0) as a measure of the variation. The BMFRSR were calculated by randomly selecting one guillemot egg out of a total of 29 and one herring out of a total of 74, and the ratio was determined between the concentration of a given OC in that egg and the concentration of the same OC in that herring. With the resampling technique, this was performed 50 000 times for any given OC, and from this new distribution of ratios, BMFRSR for each OC were calculated and given as geometric mean (GM) with GM standard deviation (GMSD) range, arithmetic mean (AM) with AMSD range, and minimum (BMFMIN) as well as maximum (BMFMAX) biomagnification factors. The 14 analyzed OCs were p,p'DDT and its metabolites p,p'DDE and p,p'DDD, polychlorinated biphenyls (PCB congeners: CB28, CB52, CB101, CB118, CB138, CB153, and CB180), hexachlorocyclohexane isomers (alpha-, beta-, and gamma HCH), and hexachlorobenzene (HCB). Multivariate data analysis (MVDA) methods, including principal components analysis (PCA), partial least squares regression (PLS), and PLS discriminant analyses (PLS-DA), were first used to extract information from the complex biological and chemical data generated from each individual animal. MVDA were used to model similarities/dissimilarities regarding species (PCA, PLS-DA), sample years (PLS), and sample location (PLS-DA) to give a deeper understanding of the data that the BMF modeling was based upon. Contaminants that biomagnify, that had BMFRSR significantly higher than one, were p,p'DDE, CB118, HCB, CB138, CB180, CB153, beta HCH, and CB28. The contaminants that did not biomagnify were p,p'DDT, p,p'DDD, alpha HCH, CB101, and CB52. Eventual biomagnification for gamma HCH could not be determined. The BMFRSR for OCs present in herring muscle and guillemot egg showed a broad span with large variations for each contaminant. To be able to make reliable calculations of BMFs for different contaminants, we emphasize the importance of using data based upon large numbers of, as well as well-defined, individuals.
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| 2. |
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| 3. |
- Bidleman, Terry F., et al.
(författare)
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Bromoanisoles and Methoxylated Bromodiphenyl Ethers in Macroalgae from Nordic Coastal Regions
- 2019
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Ingår i: Environmental Science. - London : Royal Society of Chemistry. - 2050-7887 .- 2050-7895. ; , s. 881-892
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Tidskriftsartikel (refereegranskat)abstract
- Marine macroalgae are used worldwide for human consumption, animal feed, cosmetics and agriculture. In addition to beneficial nutrients, macroalgae contain halogenated natural products (HNPs), some of which have toxic properties similar to those of well-known anthropogenic contaminants. Sixteen species of red, green and brown macroalgae were collected in 2017–2018 from coastal waters of the northern Baltic Sea, Sweden Atlantic and Norway Atlantic, and analyzed for bromoanisoles (BAs) and methoxylated bromodiphenyl ethers (MeO-BDEs). Target compounds were quantified by gas chromatography-low resolution mass spectrometry (GC-LRMS), with qualitative confirmation in selected species by GC-high resolution mass spectrometry (GC-HRMS). Quantified compounds were 2,4-diBA, 2,4,6-triBA, 2′-MeO-BDE68, 6-MeO-BDE47, and two tribromo-MeO-BDEs and one tetrabromo-MeO-BDE with unknown bromine substituent positions. Semiquantitative results for pentabromo-MeO-BDEs were also obtained for a few species by GC-HRMS. Three extraction methods were compared; soaking in methanol, soaking in methanol–dichloromethane, and blending with mixed solvents. Extraction yields of BAs did not differ significantly (p > 0.05) with the three methods and the two soaking methods gave equivalent yields of MeO-BDEs. Extraction efficiencies of MeO-BDEs were significantly lower using the blend method (p < 0.05). For reasons of simplicity and efficiency, the soaking methods are preferred. Concentrations varied by orders of magnitude among species: ∑2BAs 57 to 57 700 and ∑5MeO-BDEs < 10 to 476 pg g−1 wet weight (ww). Macroalgae standing out with ∑2BAs >1000 pg g−1 ww were Ascophyllum nodosum, Ceramium tenuicorne, Ceramium virgatum, Fucus radicans, Fucus serratus, Fucus vesiculosus, Saccharina latissima, Laminaria digitata, and Acrosiphonia/Spongomorpha sp. Species A. nodosum, C. tenuicorne, Chara virgata, F. radicans and F. vesiculosus (Sweden Atlantic only) had ∑5MeO-BDEs >100 pg g−1ww. Profiles of individual compounds showed distinct differences among species and locations.
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| 4. |
- Lundstedt-Enkel, Katrin, et al.
(författare)
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Multivariate Data Analyses of Chlorinated and Brominated Contaminants and Biological Characteristics in Adult Guillemot (Uria aalge) from the Baltic Sea
- 2005
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Ingår i: ENVIRONMENTAL SCIENCE & TECHNOLOGY. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 39:22, s. 8630-7
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Tidskriftsartikel (refereegranskat)abstract
- Adult guillemot (Uria aalge) birds, 10 females and 10 males, drowned in trawl nets near Stora Karlso in the Baltic Sea, were collected in 2000. Several of the animals' biological characteristics were recorded. The birds' pectoral muscles were individually analyzed for their concentrations of organochlorines (M) and brominated flame retardants (BFRs), dichlorodiphenyltrichloroethanes (DDTs), polychlorinated biphenyls (PCBs), hexachlorocyclohexanes, trans-nonachlor, hexachlorobenzene, hexabromocyclododecane (HBCD), and polybrominated diphenyl ethers (PBDEs). The dominating contaminant was p,p'-dichlorodiphenyldichloroethylene (p,p'-DDE) with a geometric mean concentration of 12 900 ng/g lipid weight (Iw). The concentration of Sigma PBDE (80 ng/g Iw) was similar to that of HBCD (65 ng/g Iw). The total concentration of all OCs was approximately 150 times higher than that of all BFRs. For the statistical evaluation of the data, we used multivariate analysis techniques such as principal components analysis, partial least-squares (PLS) regression, and PLS discriminant analyses. No differences between the two sexes were found, either in contaminant concentrations or in biological characteristics. We found that some biological characteristics covaried with the concentrations of several Us and BFRs, e.g., a negative correlation between liver weight and concentration of contaminants. The concentrations of most Us but not of BFRs showed a decrease with increasing lipid content. Further, a PLS model with M as X and BFRs as Y showed that the contaminants formed two groups, each with distinctive correlation patterns. The PLS model could be used to predict with varying accuracy the concentration of BFRs in the individual muscles from their concentration of OCs.
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| 5. |
- Lundstedt-Enkel, Katrin, et al.
(författare)
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Multivariate data analysis of organochlorines and brominated flame retardants in Baltic Sea guillemot (Uria aalge) egg and muscle.
- 2006
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Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 65, s. 1591-1599
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Tidskriftsartikel (refereegranskat)abstract
- Concentrations of organochlorines (OCs) and brominated flame-retardants (BFRs) were determined in guillemot (Uria aalge) eggs from the island of Stora Karlso in the Baltic Sea where 10 eggs/year were collected in the years 2000, 2001 and 2002. The dominating contaminant in egg was p,p'-dichlorodiphenyldichloroethylene (p,p'-DDE) with a geometric mean (GM) concentration of 18200 ng/g lipid weight (lw). The GM concentration in egg of hexabromocyclododecane (HBCD) of 140 ng/glw, was significantly higher than that of polybrominated diphenyl ether (summation operatorPBDE) of 77 ng/glw. For the evaluation of the data multivariate data analysis techniques namely principal components analysis (PCA), partial least squares regression (PLS), soft independent modelling of class analogy (SIMCA classification), and PLS discriminant analysis (PLS-DA), were used. We investigated whether the eggs' biological characteristics co-varied with egg concentrations of OCs and BFRs, and found e.g., significant negative correlations between egg weight and concentrations of HCB and p,p'-DDE. A PLS model with analyzed BFRs as the Y matrix and OCs as the X matrix could, with varying accuracy, calculate the concentrations of BFRs in the individual egg from their concentrations of OCs (e.g., R(2)Y of 0.89 for BDE47, and of 0.50 for HBCD). Lastly, we compared the contaminant concentrations in the eggs to those in previously analyzed pectoral muscles from adult guillemots from Stora Karlso, from the year 2000. A PLS-DA model, showed that some of the contaminants (e.g., HBCD and CB28) had significantly higher concentrations in egg than in muscle, although 7 of the 14 contaminants showed no difference in concentrations between the two matrices.
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| 6. |
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| 7. |
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| 8. |
- Aeppli, Christoph, et al.
(författare)
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Use of Cl and C Isotopic Fractionation to Identify Degradation and Sources of Polychlorinated Phenols : Mechanistic Study and Field Application
- 2013
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:2, s. 790-797
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Tidskriftsartikel (refereegranskat)abstract
- The widespread use of chlorinated phenols (CPs) as a wood preservative has led to numerous contaminated sawmill sites. However, it remains challenging to assess the extent of in situ degradation of CPs. We evaluated the use of compound-specific chlorine and carbon isotope analysis (Cl- and C-CSLA) to assess CP biotransformation. In a laboratory system, we measured isotopic fractionation during oxidative 2,4,6-trichlorophenol dechlorination by representative soil enzymes (C. fumago chloroperoxidase, horseradish peroxidase, and laccase from T. versicolor). Using a mathematical model, the validity of the Rayleigh approach to evaluate apparent kinetic isotope effects (AKIE) was confirmed. A small but significant Cl-AKIE of 1.0022 +/- 0.0006 was observed for all three enzymes, consistent with a reaction pathway via a cationic radical species. For carbon, a slight inverse isotope effect was observed (C-AKIE = 0.9945 +/- 0.0019). This fractionation behavior is clearly distinguishable from reported reductive dechlorination mechanisms. Based on these results we then assessed degradation and apportioned different types of technical CP mixtures used at two former sawmill sites. To our knowledge, this is the first study that makes use of two-element CSIA to study sources and transformation of CPs in the environment.
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| 9. |
- Andersson, Agneta, et al.
(författare)
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Microbial food web changes induced by terrestrial organic matter and elevated temperature in the coastal northern Baltic Sea
- 2023
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Ingår i: Frontiers in Marine Science. - : Frontiers Media S.A.. - 2296-7745. ; 10
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Tidskriftsartikel (refereegranskat)abstract
- Climate change has been projected to cause increased temperature and amplified inflows of terrestrial organic matter to coastal areas in northern Europe. Consequently, changes at the base of the food web favoring heterotrophic bacteria over phytoplankton are expected, affecting the food web structure. We tested this hypothesis using an outdoor shallow mesocosm system in the northern Baltic Sea in early summer, where the effects of increased temperature (+ 3°C) and terrestrial matter inputs were studied following the system dynamics and conducting grazing experiments. Juvenile perch constituted the highest trophic level in the system, which exerted strong predation on the zooplankton community. Perch subsequently released the microbial food web from heavy grazing by mesozooplankton. Addition of terrestrial matter had a stronger effect on the microbial food web than the temperature increase, because terrestrial organic matter and accompanying nutrients promoted both heterotrophic bacterial production and phytoplankton primary production. Moreover, due to the shallow water column in the experiment, terrestrial matter addition did not reduce the light below the photosynthesis saturation level, and in these conditions, the net-autotrophy was strengthened by terrestrial matter enrichment. In combination with elevated temperature, the terrestrial matter addition effects were intensified, further shifting the size distribution of the microbial food web base from picoplankton to microphytoplankton. These changes up the food web led to increase in the biomass and proportion of large-sized ciliates (>60 µm) and rotifers. Despite the shifts in the microbial food web size structure, grazing experiments suggested that the pathway from picoplankton to nano- and microzooplankton constituted the major energy flow in all treatments. The study implies that the microbial food web compartments in shallow coastal waters will adjust to climate induced increased inputs of terrestrial matter and elevated temperature, and that the major energy path will flow from picoplankton to large-sized ciliates during the summer period.
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| 10. |
- Andersson, Agneta, et al.
(författare)
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Projected future climate change and Baltic Sea ecosystem management
- 2015
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Ingår i: Ambio. - : Springer. - 0044-7447 .- 1654-7209. ; 44:Supplement 3, s. S345-S356
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Tidskriftsartikel (refereegranskat)abstract
- Climate change is likely to have large effects on the Baltic Sea ecosystem. Simulations indicate 2-4 degrees C warming and 50-80 % decrease in ice cover by 2100. Precipitation may increase similar to 30 % in the north, causing increased land runoff of allochthonous organic matter (AOM) and organic pollutants and decreased salinity. Coupled physical-biogeochemical models indicate that, in the south, bottom-water anoxia may spread, reducing cod recruitment and increasing sediment phosphorus release, thus promoting cyanobacterial blooms. In the north, heterotrophic bacteria will be favored by AOM, while phytoplankton production may be reduced. Extra trophic levels in the food web may increase energy losses and consequently reduce fish production. Future management of the Baltic Sea must consider the effects of climate change on the ecosystem dynamics and functions, as well as the effects of anthropogenic nutrient and pollutant load. Monitoring should have a holistic approach, encompassing both autotrophic (phytoplankton) and heterotrophic (e.g., bacterial) processes.
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| 11. |
- Andersson, Patrik, et al.
(författare)
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An introduction to QSARs
- 2006
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Ingår i: Using chemistry in environmental and health risk assessment. - : US-AB Universitetsservice, Stockholm. - 9171784144 ; , s. 51-74
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Bokkapitel (refereegranskat)
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| 12. |
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| 13. |
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| 14. |
- Andersson, Patrik, et al.
(författare)
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Multivariate modeling of polychlorinated biphenyl-induced CYP1A activity in hepatocytes from three different species : ranking scales and species differences
- 2000
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Ingår i: Environmental Toxicology and Chemistry. - : Wiley. - 0730-7268 .- 1552-8618. ; 19:5, s. 1454-1463
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Tidskriftsartikel (refereegranskat)abstract
- Cytochrome P4501A–induced activity of 20 selected polychlorinated biphenyls (PCBs) was evaluated by measuring ethoxyresorufin-O-deethylase and methoxyresorufin-O-demethylase activities induced in the hepatocytes of cynomolgus monkeys, male castrated pigs, and chicken embryos. Quantitative structure-activity relationships have been established, including 52 physi-cochemical parameters and different measures of the dose-response curves. Relative effect potencies are predicted for the 154 tetra-to hepta-PCBs and reported for the most potent congeners according to both EC50 and maximal response values. Important physicochemical parameters of the PCBs as related to the modeled activity are parts of their ultraviolet absorption spectra, the Henry's law constant, the ionization potential, and the octanol-water partition coefficient. Interspecies differences were found in terms of varied sensitivity to different structural subgroups of the compounds. The chicken hepatocyte assay showed the most specific structure-activity relationship, with high activity for the non-ortho PCBs, whereas the pig hepatocytes responded even for some di- to tetra-ortho PCBs. An interspecies response, the principal induction potency, is presented for the 41 most potent PCBs. These responses showed strong correlation with the toxic equivalency factors and are likely to be useful in risk assessment of the compounds.
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| 15. |
- Andersson, Patrik, et al.
(författare)
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The internal barriers of rotation for the 209 polychlorinated biphenyls
- 1997
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Ingår i: Environmental Science and Pollution Research. - 0944-1344 .- 1614-7499. ; 4:2, s. 75-81
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Tidskriftsartikel (refereegranskat)abstract
- The internal barrier of rotation (Erot) was calculated for all 209 polychlorinated biphenyls (PCBs) by using a semi-empirical method, viz. the Austin Model 1 (AM1) Hamiltonian. The difference in total energy between a forced planar state and an optimised twisted structure was defined as Erot. The Erot values were in the range of 8.33 to 483 kJ/mol, and were significantly influenced by the number of chlorine atoms in ortho position. An additional structural characteristic of the PCBs influencing Erot of ortho substituted congeners was substitution by chlorine atoms in vicinal meta positions, which is assumed to prevent outward bending of ortho substituents. This so-called buttressing effect contributed with 4 to 31 kJ/mol per added chlorine atom. In conclusion, the internal barrier of rotation, calculated for all 209 PCBs, provides an important structure dependent physico-chemical parameter for multivariate modelling of future quantitative structure-activity and structure-property relationships (QSARs/QSPRs).
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| 16. |
- Andersson, Patrik, et al.
(författare)
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Ultraviolet absorption characteristics and calculated semi-empirical parameters as chemical descriptors in multivariate modelling of polychlorinated biphenyls
- 1996
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Ingår i: Journal of Chemometrics. - 0886-9383 .- 1099-128X. ; 10:2, s. 171-185
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Tidskriftsartikel (refereegranskat)abstract
- The structural variation within the polychlorinated biphenyls (PCBs) was characterized by using principal component analysis (PCA). A multivariate model was evolved from 52 physicochemical descriptors including measured ultraviolet (UV) absorption spectra, calculated semiempirical parameters (AM1) and properties captured from the literature. Parameters calculated by using the AM1-Hamiltonian were e.g. heat of formation, dipole moments, ionization potential and the barrier of internal rotation. The UV spectra were measured and digitized in the range 200-300 nm. The multivariate model revealed that most of the information within the set of physicochemical parameters was related to molecular size. Descriptors depending on size were e.g. GC retention times, partition coefficients and a subset of semiempirically derived energy terms. Important also were parameters reflecting differences in substitution patterns and related to electronic and steric properties, such as UV absorption in the wavelength region 245-300 nm, the barrier of internal rotation and the ionization potential. The developed model describes the large variation in physicochemical characteristics within the PCBs. The importance of a broad chemical characterization is illustrated by a quantitative structure-activity relationship (QSAR) for the potency of inhibition of intercellular communication for 27 structurally diverse tetra- to heptachlorinated PCBs.
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| 17. |
- Andersson, Patrik, et al.
(författare)
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Ultraviolet absorption spectra of all 209 polychlorinated biphenyls evaluated by principal component analysis
- 1997
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Ingår i: Fresenius' Journal of Analytical Chemistry. - : Springer Science and Business Media LLC. - 0937-0633 .- 1432-1130. ; 357:8, s. 1088-1092
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Tidskriftsartikel (refereegranskat)abstract
- The ultraviolet absorption spectra of all 209 polychlorinated biphenyls (PCBs) were recorded in the range 200-300 nm and displayed two important absorption maxima, viz., the main-band, lambda(max) 200-225 nm, and the kappa-band, lambda(max) 245-265 nm. By utilising principal component analysis, substitution related spectral characteristics of the PCBs, underlying the main patterns of the spectra, were examined. Captured in the multivariate evaluation were e.g., the importance of chlorine atoms in ortho positions, determining the intensity and existence of the kappa-band, chlorine substitution in para-para position, and the total number of chlorine atoms. The measured UV-spectra of all 209 polychlorinated biphenyls provide important physico-chemical descriptors for use in future quantitative structure-activity and structure-property relationship (QSAR/QSPR) studies.
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| 18. |
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| 19. |
- Antoniou, Maria G., et al.
(författare)
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Required ozone doses for removing pharmaceuticals from wastewater effluents
- 2013
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Ingår i: Science of the Total Environment. - Amsterdam : Elsevier BV. - 1879-1026 .- 0048-9697. ; 456, s. 42-49
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Tidskriftsartikel (refereegranskat)abstract
- The aim of the this study was to investigate the ozone dosage required to remove active pharmaceutical ingredients (APIs) from biologically treated wastewater of varying quality, originated from different raw wastewater and wastewater treatment processes. Secondary effluents from six Swedish wastewater treatment plants (WWTP) were spiked with 42 APIs (nominal concentration 1 mu g/L) and treated with different O-3 doses (0.5-12.0 mg/L ozone) in bench-scale experiments. In order to compare the sensitivity of APIs in each matrix, the specific dose of ozone required to achieve reduction by one decade of each investigated API (DDO3) was determined for each effluent by fitting a first order equation to the remaining concentration of API at each applied ozone dose. Ozone dose requirements were found to vary significantly between effluents depending on their matrix characteristics. The specific ozone dose was then normalized to the dissolved organic carbon (DOC) of each effluent. The DDO3/DOC ratios were comparable for each API between the effluents. 15 of the 42 investigated APIs could be classified as easily degradable (DDO3/DOC <= 0.7), while 19 were moderately degradable (0.7 < DDO3/DOC <= 1.4), and 8 were recalcitrant towards O-3-treatment (DDO3/DOC > 1.4). Furthermore, we predict that a reasonable estimate of the ozone dose required to remove any of the investigated APIs may be attained by multiplying the experimental average DDO3/DOC obtained with the actual DOC of any effluent. (C) 2013 Elsevier B.V. All rights reserved.
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| 20. |
- Antoniou, Maria G., et al.
(författare)
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Variability in required ozone doses for removing pharmaceuticals from wastewater effluents
- 2013
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Ingår i: Proceedings of the 13th International Conference on Environmental Science and Technology. - : Global Nest, Secretariat. - 9789607475510
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Konferensbidrag (refereegranskat)abstract
- Aim of study. The aim of the present study was to investigate the ozone dosage required to remove active pharmaceutical ingredients (APIs) from biologically treated wastewater of varying quality originating from different wastewater treatment processes. Methods. Secondary effluents from six Swedish wastewater treatment plants (VWVTP) were spiked with 42 APIs (nominal concentration 1pg/L) and treated with different 03 doses (0.5-12.0 mg/L ozone) in bench-scale experiments (Antoniou et al, 2012). Concentrations of APIs were measured by SPE extraction using OASIS HLB cartridges followed by quantification using LC-MS-MS (Grabic et al, 2012).. Results. For each wastewater effluent a profile of sensitivity of each API to a range of ozone doses were generated as shown in Figure 1.
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| 21. |
- Assefa, Anteneh, et al.
(författare)
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Airborne dioxins and other POPs in the Baltic Sea environment: the potential of using metals as source markers
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Atmospheric sources are major contributors of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the Baltic Sea environment. In this study, we investigated the potential of using trace metals along with PCDD/F levels and seasonal trends as markers of important source types for PCDD/Fs in air. Levels of PCDD/F congeners (n=17) and metals (n=16) were measured in summer and winter air using high volume sampling at a rural field station (Aspvreten, Sweden). During winter, levels were on average 20 times higher than in summer (5.1 ± 5.8 fg TEQ m-3 and 0.26 ± 0.18 fg TEQ m-3, respec- tively) mostly due to a higher fraction of PCDFs. The increased levels were pronounced in air masses from southern (S) and eastern (E) compass sectors. Most of the detected metals (n=12) were positively and significantly correlated with the PCDF congeners for all compass sectors (Cd, Co, Cu, Fe, K, Mn, Pb, Sb, and Zn) during winter season. The average correlation coefficient (r) value for the correlation between PCDF congeners and these metals was 0.85 and p values generally below <0.05. In contrast, polychlorinated biphenyls (PCBs) and hexachlorobenzene (HCB) showed no significant correlations with detected metals except for HCB and Cr (r=0.60 and p<0.01). The wide range of candidate metals as source markers for PCDD/F emissions, and the lack of an up-to-date extensive compilation of source characteristics for metal emission from various sources, limited the use of the metals as source markers in the current study. Although, the study was not able to pin-point primary PCDD/F sources for Baltic air, we demonstrated a promising approach for source tracing of PCDD/F in air.
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| 22. |
- Assefa, Anteneh, et al.
(författare)
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Source-apportionment shows why dioxin levels have not declined in Baltic fish
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Levels of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs, “dioxins”) in fatty fish of the Baltic Sea have remained high despite declines in environmental levels since the 1980s. This has raised human health concerns and restricted marketing of Baltic herring and salmon within the European Union. Thus, there is an urgent need to identify and control current PCDD/F emission sources. Analysis presented here explains why PCDD/Fs levels in fish have stopped declining or even increased in recent decades. We show that contributions of “thermal” sources (e.g., waste incineration) of PCDD/Fs to Baltic fish have declined since the 1990s, but not contributions of sources associated with the manufacture and use of chlorophenols (particularly tetrachlorophenol and pentachlorophenol, TCP and PCP, respectively). Moreover, the discrepancy between declines in levels of dioxins in abiotic compartments (e.g. sediments and air), and stable or increasing levels in biota can be explained by the persistently high bioavailability of PCDD/Fs associated with TCP and PCP type sources.
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| 23. |
- Assefa, Anteneh, et al.
(författare)
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Sources of dioxins in Baltic Sea herring: A modelling study for identification of dioxin sources and quantification of their temporal and spatial impacts
- 2018
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Rapport (övrigt vetenskapligt/konstnärligt)abstract
- This study presents a step-by-step statistical analysis for tracing dioxins sources that have contributed to levels in Baltic herring during the last decades. The study is based on the concentrations of the 17 toxic (2,3,7,8-substituted) dioxin congeners in herring and sediment from the Baltic Sea, and it evaluates how the impacts of the sources may have changed during the studied periods, i.e. 1990–2009 in the Bothnian Bay, 1979–2009 in the Bothnian Sea and 1988–2009 in the Baltic Proper. The modelling technique used (PMF) extracted three dioxin patterns in herring that could be used to obtain source patterns after applying transformation factors. The transformed patterns were compared to real dioxin source patterns available through previous measurement and modelling studies. The identified sources included tetrachlorophenol (TCP), pentachlorophenol/atmospheric background (PCP/AB) and emissions from thermal activities.The results indicate that the thermal source type has been the major contributor of dioxins to Baltic herring during the pre-and post-2000 periods (72% and 59%, respectively). Its impact appears, however, to have declined by 19% in the Bothnian Bay, by 67% in the Bothnian Sea, and by 48% in the Baltic Proper (TEQ-basis). On the other hand, the relative importance of TCP and PCP/AB appear to have increased over time, from 1.4% and 1.5% to 19% and 6.6% in the Bothnian Bay, from 3.3% and 7.2% to 12% and 10% in the Bothnian Sea, and from 8.9% and <1% to 33% and 13% in the Baltic Proper. Comparisons using absolute values (pg TEQ g-1 lipid weight) indicate an increase of the TCP source by five times in the Bothnian Bay from the pre-2000 to the post-2000 period, a slight increase in the Bothnian Sea, and more than a doubling of the levels in the Baltic Proper. The agreement between the trends in the three sub-basins is a good indication for an increased impact of the TCP source during recent years (post-2000). Corresponding analysis for the PCP/AB source type, indicate slightly decreased TEQ levels from the PCP/AB source type in the Bothnian Sea (by ~50%), more than twice as high in the Bothnian Bay, and more than triplicated in the Baltic Proper. While the declining trends of the thermal source type encourages continuing management efforts for air emissions, the apparent increase of TCP and PCP/AB call for more attention to such sources in the Baltic Sea. As the use of technical products containing TCP and PCP have been banned/restricted since the 1970s and 1980s, more focus on contaminated sites may be required in the mitigation actions of such sources.
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| 24. |
- Assefa, Anteneh, et al.
(författare)
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Sources of polychlorinated dibenzo-p-dioxins and dibenzofurans to Baltic Sea herring
- 2019
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Ingår i: Chemosphere. - : Elsevier. - 0045-6535 .- 1879-1298. ; 218, s. 493-500
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Tidskriftsartikel (refereegranskat)abstract
- Levels of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in herring (Clupea harengus) remain high in several parts of the Baltic Sea, despite declines in PCDD/F emissions since the 1980s. The reasons behind this are not well understood. This study applied a statistical modeling approach where sources of PCDD/Fs that contaminate Baltic biota were quantitatively assessed by analyzing existing datasets. PCDD/F patterns were extracted from a herring dataset using positive matrix factorization (PMF). The extracted biota patterns were transformed into sediment patterns using fish-to-sediment transformation factors, and the resulting patterns were compared with known source PCDD/F patterns. The model distinguished three model patterns, which explained 85% of the data. These patterns were matched to tetra-chlorophenol (TCP), penta-chlorophenol/atmospheric background (PCP/AB), and thermal source patterns, respectively. The thermal source was the largest contributor to toxic equivalents (TEQ) in herring, but the level decreased from 42 ± 9.0 pg TEQ g−1 lipid weight (lw) before year 2000 (pre-2000) to 15 ± 2.4 pg TEQ g−1 lw post-2000, i.e., a decline of around one-third in the original TEQ concentration. The contribution of TCP more than doubled, from 2.1 ± 0.62 pg TEQ g−1 lw to 5.6 ± 1.1 pg TEQ g−1 lw, and the relative contribution of PCP/AB also increased. These increasing trends suggest that, as primary air emissions of PCDD/Fs are managed and levels decline, the impact of TCP and PCP/AB sources on Baltic Sea biota will become more important over time and that PCDD/F-contaminated sites in coastal areas and marine environments require more attention.
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| 25. |
- Assefa, Anteneh Taye, et al.
(författare)
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Assessment of PCDD/F Source Contributions in Baltic Sea Sediment Core Records
- 2014
-
Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851 .- 1086-931X .- 1520-6912. ; 48:16, s. 9531-9539
-
Tidskriftsartikel (refereegranskat)abstract
- Spatial and temporal trends of sources of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the Baltic Sea were evaluated by positive matrix factorization (PMF) and principal component analysis (PCA). Sediment cores were sampled at eight coastal, one coastal reference, and six offshore sites covering the northern to the southern Baltic Sea. The cores, which covered the period 1919-2010, were sliced into 2-3 cm disks among which 8-11 disks per core (in total 141 disks) were analyzed for all tetra- through octa-CDD/Fs. Identification and apportionment of PCDD/F sources was carried out using PMF. Five stable model PCDD/F congener patterns were identified, which could be associated with six historically important source types: (i) atmospheric background deposition (ABD), (ii) use and production of pentachlorophenol (PCP), (iii) use and production of tetra-chlorophenol (TeCP), (iv) high temperature processes (Thermal), (v) hexa-CDD-related sources (HxCDD), and (vi) chlorine-related sources (Chi), all of which were still represented in the surface layers. Overall, the last four decades of the period 1920-2010 have had a substantial influence on the Baltic Sea PCDD/F pollution, with 88 +/- 7% of the total amount accumulated during this time. The 1990s was the peak decade for all source types except TeCP, which peaked in the 1980s in the northern Baltic Sea and has still not peaked in the southern part. The combined impact of atmospheric-related emissions (ABD and Thermal) was dominant in the open sea system throughout the study period (1919-2010) and showed a decreasing south to north trend (always >80% in the south and >50% in the north). Accordingly, to further reduce levels of PCDD/Fs in the open Baltic Sea ecosystem, future actions should focus on reducing atmospheric emissions.
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| 26. |
- Assefa, Anteneh Taye, et al.
(författare)
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Temporal Trends of PCDD/Fs in Baltic Sea Sediment Cores Covering the 20th Century
- 2014
-
Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 48:2, s. 947-953
-
Tidskriftsartikel (refereegranskat)abstract
- The pollution trend of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the Baltic Sea region was studied based on depth profiles of PCDD/Fs in sediment cores collected from six-offshore areas, eight coastal sites impacted by industrial/urban emissions, and one coastal reference site. A general trend was observed for the offshore and coastal reference sites with substantial increase in PCDD/F concentrations in the mid-late 1970s and peak levels during 1985-2002. The overall peak year for PCDD/Fs in Baltic Sea offshore areas was estimated (using spline-fit modeling) to 1994 +/- 5 years, and a half-life in sediments was estimated at 29 +/- 11 years. For the industrial/urban impacted coastal sites, the temporal trend was more variable with peak years occurring 1-2 decades earlier compared to offshore areas. The substantial reductions from peak levels (38 +/- 11% and 81 +/- 12% in offshore and coastal areas, respectively) reflect domestic and international actions taken for reduction of the release of PCDD/Fs to the environment. The modeled overall half-life and reductions of PCDD/Fs in offshore Baltic Sea sediment correspond well to both PCDD/F trends in European lakes without any known direct. PCDD/F sources (half-lives 30 and 32 years), and previously modeled reduction in atmospheric deposition of,PCDD/Fs to the Baltic Sea since 1990. These observations support previous findings of a common diffuse source, such as long-range air transport of atmospheric emissions, as the prime source of PCDD/Fs to the Baltic Sea region. The half-life of PCDD/Fs in Baltic Sea offshore sediments was estimated to be approximately 2 and 4-6 times longer than in semirural and urban European air, respectively. This study highlights the need for further international actions to reduce the levels of PCDD/Fs in Baltic Sea air specifically and in European air in general.
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| 27. |
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| 28. |
- Assefa, Anteneh, 1983-
(författare)
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Tracing and apportioning sources of dioxins using multivariate pattern recognition techniques
- 2015
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- High levels of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs) in edible fish in the Baltic Sea have raised health concerns in the Baltic region and the rest of Europe. Thus, there are urgent needs to characterize sources in order to formulate effective mitigation strategies. The aim of this thesis is to contribute to a better understanding of past and present sources of PCDD/Fs in the Baltic Sea environment by exploring chemical fingerprints in sediments, air, and biota. The spatial and temporal patterns of PCDD/F distributions in the Baltic Sea during the 20th century were studied in Swedish coastal and offshore sediment cores. The results showed that PCDD/F levels peaked in 1975 (± 7 years) in coastal and 1991 (± 5 years) in offshore areas. The time trends of PCDD/Fs in the sediment cores also showed that environmental half-lives of these pollutants have been shorter in coastal than in offshore areas (15 ± 5 and 29 ± 14 years, respectively). Consequently, there have been remarkable recoveries in coastal areas, but slower recovery in offshore areas with 81 ± 12% and 38 ± 11% reductions from peak levels, respectively.Source-to-receptor multivariate modeling by Positive Matrix Factorization (PMF) showed that six types of PCDD/F sources are and have been important for the Baltic Sea environment: PCDD/Fs related to i) atmospheric background, ii) thermal processes, iii) manufacture and use of tetra-chlorophenol (TCP) and iv) penta-chlorophenol (PCP), v) industrial use of elementary chlo- rine and the chloralkali-process (Chl), and vi) hexa-CDD sources. The results showed that diffuse sources (i and ii) have consistently contributed >80% of the total amounts in the Southern Baltic Sea. In the Northern Baltic Sea, where the biota is most heavily contaminated, impacts of local sources (TCP, PCP and Chl) have been higher, contributing ca. 50% of total amounts. Among the six sources, only Thermal and chlorophenols (ii-iv) have had major impacts on biota. The impact of thermal sources has, however, been declining as shown from source apportioned time-trend data of PCDD/Fs in Baltic herring. In contrast, impacts of chlorophenol-associated sources generally increased, remained at steady-state or slowly decreased during 1990-2010, suggesting that these sources have substantially contributed to the persistently high levels of PCDD/Fs in Baltic biota.Atmospheric sources of PCDD/Fs for the Baltic region (Northern Europe) were also investigated, and specifically whether the inclusion of parallel measurements of metals in the analysis of air would help back-tracking sources. PCDD/Fs and metals in high-volume air samples from a rural field station near the shore of the central Baltic Sea were measured. The study focused on the winter season and air from the S and E sectors, as these samples showed elevated levels of PCDD/Fs, particularly PCDFs. Several metals were found to correlate significantly with the PCDFs. The wide range of candidate metals as source markers for PCDD/F emissions, and the lack of an up-to-date extensive compilation of source characteristics for metal emission from vari- ous sources, limited the use of the metals as source markers. The study was not able to pin-point primary PCDD/F sources for Baltic air, but it demonstrated a new promising approach for source tracing of air emissions. The best leads for back-tracking primary sources of atmospheric PCDD/Fs in Baltic air were seasonal trends and PCDD/F congener patterns, pointing at non-industrial related thermal sources related to heating. The non-localized natures of the sources raise challenges for managing the emissions and thus societal efforts are required to better control atmospheric emissions of PCDD/Fs.
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| 29. |
- Assefa, Anteneh, et al.
(författare)
-
Tracing the sources of PCDD/Fs in Baltic Sea air by using metals as source markers
- 2018
-
Ingår i: Environmental Science. - Cambridge : Royal Society of Chemistry. - 2050-7887 .- 2050-7895. ; 20:3, s. 544-552
-
Tidskriftsartikel (refereegranskat)abstract
- The atmosphere is the major contributor of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the Baltic Sea environment. In this study, we investigated the potential of using metals along with PCDD/Fs as markers of important emission sources of PCDD/Fs in air. The air concentrations of PCDD/F congeners (n = 17), other persistent organic pollutants (n = 8) and metals (n = 16) were determined in summer and winter air using high volume samplers at a rural field station (Aspvreten, Sweden) located close to the Baltic Sea coast. During winter, PCDD/F levels were on average 20 times higher than in summer (5.1 +/- 5.8 fg toxicity equivalents (TEQ) m-3 and 0.26 +/- 0.18 fg TEQ m-3, respectively) mostly due to a higher fraction of PCDFs. The increased levels of PCDD/Fs were pronounced mainly in air masses that had travelled from southern (S) and eastern (E) compass sectors. A principal component analysis (PCA) of metal levels in Scots pine (Pinus sylvestris) needles sampled to reflect various air emission source types helped to identify potential marker metals for selected known atmospheric emission sources of PCDD/Fs and to rank among the candidate source types. Brown coal burning, domestic burning and heavy oil burning appeared to be the source types that contribute most of the PCDD/Fs in Baltic Sea air. The current study demonstrates a successful approach for source tracing of PCDD/Fs in air, where integrated indices from seasonal and spatial patterns of PCDD/Fs as well as metal source markers were used to trace and rank sources.
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| 30. |
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| 31. |
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| 32. |
- Badea, Silviu-Laurentiu, 1980-
(författare)
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Association of hydrophobic organic compounds to organic material in the soil system
- 2013
-
Licentiatavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Contaminated soils and sediments have been identified as significant secondary sources of organic contaminants. Leaching tests may be useful tools to estimate the mobility of contaminants via the water phase and thereby the risk for groundwater and surface water contamination. The influence of soil composition (peat and clay content) on the leachability was investigated in batch leaching experiments for chemically diverse hydrophobic organic compounds (HOCs: PCP, PAHs, HCB, HCHs, PCBs, and TCDD/Fs). The above mentioned compounds were analyzed by both GC-LRMS (gas chromatography coupled with low resolution mass spectrometry (GC-HRMS) and GC-HRMS (gas chromatography coupled with high resolution mass spectrometry). Also the the leachability of eleven selected PCBs from naturally aged soil (Västervik, Sweden) was investigated in relation to the composition and concentration of dissolved organic matter at different pH (2 to 9), using a pH static test with initial acid/base addition. The the composition and of dissolved organic matter (DOM) at different pH values was explored by FTIR spectroscopy. The results were evaluated by orthogonal projections to latent structures (OPLS).Generally, for all model compounds studies, the Kd-values showed a variability of 2-3 orders of magnitude depending on the matrix composition. The Kd-values of moderately hydrophobic compounds, (e.g. HCHs, PCP and Phe), were correlated mainly with the organic matter content of soil. For more hydrophobic compounds (e.g.BaA, HCB and PCB 47), the leachability decreased as the proportions of OM and clay contents increased. The Kd-values of 1,3,6,8-TCDD and 1,3,6,8-TCDF were positively correlated with peat content but negatively correlated with clay content, while for PCB 153 and PCB 155 the correlations were reversed. The log Kd-values of all target PCBs decreased with increased pH values and the log Kd-values were highly correlated with the concentration of total organic carbon (TOC) in the leachates. The FTIR analysis of DOM showed that the least chlorinated and hydrophobic PCB congeners (i.e. PCB 28) might be associated with the hydrophilic fraction (i.e. carboxylic groups) of DOM. Our study demonstrated how complex interaction between the organic matter, clay components, pH and DOC influences the leachability of HOCs in a compound-specific manner.
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| 33. |
- Badea, Silviu-Laurentiu, et al.
(författare)
-
Leachability and desorption of PCBs from soil and their dependency on pH and dissolved organic matter
- 2014
-
Ingår i: Science of the Total Environment. - : Elsevier BV. - 0048-9697 .- 1879-1026. ; 499, s. 220-227
-
Tidskriftsartikel (refereegranskat)abstract
- pH affects both soil–water partitioning coefficient (Kd) of polychlorinated biphenyls (PCBs) and dissolved organic matter (DOM), thereby influencing PCBs' leachability from contaminated soils. To explore these incompletely understood interactions, the leachability of 11 selected PCBs in a naturally aged soil was investigated in pH static leaching tests spanning a wide pH range (2 to 9). The Kd was calculated for each of the PCBs, based on their observed concentrations in the soil and leachates obtained from each test. The concentration and composition of DOM in each leachate were also determined, the latter using FTIR spectroscopy. Correlations between the DOM's FTIR spectra and Kd values were investigated by orthogonal projections to latent structures. The log Kd-values varied among the PCB congeners and were most variable at low pH, but the values for all studied congeners decreased with increasing pH, by up to 3 log units (for PCB 187). In the pH 5–7 interval, an abrupt decrease in log Kd values with increases in pH was observed, although the total organic carbon content remained relatively stable. The FTIR data indicate that fulvic and humic acids in DOM partially deprotonate as the pH rises from 5 to 7.
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| 34. |
- Badea, Silviu-Laurentiu, et al.
(författare)
-
Leachability of PCBs in soil and its pH and dissolved organic matter (DOM) dependency
-
Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- The leachability of eleven selected PCBs from naturally aged soil (Västervik, Sweden) was investigated in relation to the composition and concentration of dissolved organic matter at different pH (2 to 9), using a pH static test with initial acid/base addition. The batch leaching tests were performed on 50 g aliquots of a PCBs contaminated soil at a liquid to solid ratio (L/S) of 10 L/Kg. The PCBs were analyzed by gas chromatography coupled with high resolution mass spectrometry (GC-HRMS). The composition and of dissolved organic matter (DOM) at different pH values was explored by FTIR spectroscopy. The correlation between the FTIR data obtained for DOM and the log Kd values of PCBs was explored by orthogonal projections to latent structures (OPLS). The log Kd-values of all target PCBs decreased with increased pH values and the log Kd-values were highly correlated with the concentration of total organic carbon (TOC) in the leachates. For the lower chlorinated congener, PCB 28, this correlation was weaker. The variation of fractions of concentrations of mono-ortho to di-ortho PCBs (PCB 66 to PCB 52 and PCB 105 to PCB 101) indicated an influence of the ortho-chlorine atoms through pH effects on their leachability. The FTIR analysis of DOM showed that the least chlorinated and hydrophobic PCB congeners (i.e. PCB 28) might be associated with the hydrophilic fraction (i.e. carboxylic groups) of the DOM.
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| 35. |
- Badea, Silviu, et al.
(författare)
-
The influence of soil composition on the leachability of selected hydrophobic organic compounds (HOCs) from soils using a batch leaching test
- 2013
-
Ingår i: Journal of Hazardous Materials. - : Elsevier. - 0304-3894 .- 1873-3336. ; 254, s. 26-35
-
Tidskriftsartikel (refereegranskat)abstract
- The influence of soil composition (peat and clay content) on the leachability was investigated in batch leaching experiments for chemically diverse hydrophobic organic compounds (HOCs: PCP, PAHs, HCB, HCHs, PCBs, and TCDD/Fs). An experimental design was applied to generate 8 diverse soil matrices, and the results were evaluated by orthogonal projections to latent structures (OPLS), as well as compound specific response surface models. Overall, the distribution coefficients (log Kd) of model HOCs were in the range of approx. 2.0–5.7. The Kd-values of HCHs, phenanthrene and PCP were positively correlated with the peat content. Kd-values of benzo(a)anthracene, HCB, and PCB 47 were positively correlated with both peat and clay content. The Kd-values of 1,3,6,8-TCDD and 1,3,6,8-TCDF were positively correlated with peat content but negatively correlated with clay content, while for PCB 153 and PCB 155 the correlations were reversed. The correlation between the Kd-values and the compounds’ Kow-values was linearly for compounds with log Kow <6. For HOCs with log Kow > 6, the Kd-values were leveling off, possibly due to small particles in the leachates. Our study demonstrated how complex interaction between both the organic matter and clay components influences the leachability of HOCs in a compound-specific manner.
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| 36. |
- Bengtsson-Palme, Johan, 1985, et al.
(författare)
-
Elucidating selection processes for antibiotic resistance in sewage treatment plants using metagenomics
- 2016
-
Ingår i: Science of the Total Environment. - : Elsevier BV. - 0048-9697 .- 1879-1026. ; 572, s. 697-712
-
Tidskriftsartikel (refereegranskat)abstract
- Sewage treatment plants (STPs) have repeatedly been suggested as “hotspots” for the emergence and dissemination of antibiotic-resistant bacteria. A critical question still unanswered is if selection pressures within STPs, caused by residual antibiotics or other co-selective agents, are sufficient to specifically promote resistance. To address this, we employed shotgun metagenomic sequencing of samples from different steps of the treatment process in three Swedish STPs. In parallel, concentrations of selected antibiotics, biocides and metals were analyzed. We found that concentrations of tetracycline and ciprofloxacin in the influent were above predicted concentrations for resistance selection, however, there was no consistent enrichment of resistance genes to any particular class of antibiotics in the STPs, neither for biocide and metal resistance genes. The most substantial change of the bacterial communities compared to human feces occurred already in the sewage pipes, manifested by a strong shift from obligate to facultative anaerobes. Through the treatment process, resistance genes against antibiotics, biocides and metals were not reduced to the same extent as fecal bacteria. The OXA-48 gene was consistently enriched in surplus and digested sludge. We find this worrying as OXA-48, still rare in Swedish clinical isolates, provides resistance to carbapenems, one of our most critically important classes of antibiotics. Taken together, metagenomics analyses did not provide clear support for specific antibiotic resistance selection. However, stronger selective forces affecting gross taxonomic composition, and with that resistance gene abundances, limit interpretability. Comprehensive analyses of resistant/non-resistant strains within relevant species are therefore warranted.
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| 37. |
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| 38. |
- Bergknut, Magnus, et al.
(författare)
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Assessment of the availability of polycyclic aromatic hydrocarbons from gasworks soil using different extraction solvents and techniques
- 2004
-
Ingår i: Environmental Toxicology and Chemistry. - : Wiley. - 0730-7268 .- 1552-8618. ; 23:8, s. 1861-1866
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Tidskriftsartikel (refereegranskat)abstract
- This study was designed to assess the availability of polycyclic aromatic hydrocarbons (PAHs) present at a gasworks site to different soil remediation techniques. The study examined the effect on PAH availability of using different organic solvents, the degree of pretreatment, and the extraction time. In total, 25 PAHs (with two to six fused rings) and five carbonyl derivatives were measured. The results indicated that the PAHs and their derivatives were bound loosely to the surface of the studied soil and that there were no significant kinetic boundaries associated with the extraction of the PAHs. Furthermore, it was concluded that the studied soil was not suitable for bioremediation, as the concentration of PAHs with low molecular weight were limited. However, pressurized liquid extraction (PLE) with methanol as the solvent extracted 97% of all PAHs and PAH-derivatives, indicating that extraction may be effective as part of a soil remediation technique for old gasworks soils.
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| 39. |
- Bergknut, Magnus, et al.
(författare)
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Characterization and classification of complex PAH samples using GC-qMS and GC-TOFMS
- 2006
-
Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 65:11, s. 2208-2215
-
Tidskriftsartikel (refereegranskat)abstract
- The aim of this study was to compare the polycyclic aromatic hydrocarbon (PAH) contents in a number of complex samples, including soil samples from industrial sites, anti-skid sand, urban dust and ash samples from municipal solid waste incinerators. The samples were characterized by routine analysis of PAHs (gas chromatography–quadrupole mass spectrometry) and gas chromatography–time of flight mass spectrometry (GC–TOFMS). Classification of the samples by principal component analysis (PCA) according to their composition of PAHs revealed that samples associated with traffic and the municipal incinerator formed homogeneous clusters, while the PAH-contaminated soils clustered in separate groups. Using spectral data to resolve co-eluting chromatographic peaks, 962 peaks could be identified in the GC–TOFMS analysis of a pooled sample and 123–527 peaks in the individual samples. Many of the studied extracts included a unique set of chemicals, indicating that they had a much more diverse contamination profile than their PAH contents suggested. Compared to routine analysis, GC–TOFMS provided more detailed information about each sample and in this study a large number of alkylated PAHs were found to be associated with the corresponding unsubstituted PAHs. The possibility to filter peaks according to different criteria (e.g. to include only peaks that were detected in the analysis of another sample) was explored and used to identify unique as well as common compounds within samples. This procedure could prove to be valuable for obtaining relevant chemical data for use in conjunction with results from various biological test systems.
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| 40. |
- Bergknut, Magnus, 1973-
(författare)
-
Characterization of PAH-contaminated soils focusing on availability, chemical composition and biological effects
- 2006
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The risks associated with a soil contaminated by polycyclic aromatic hydrocarbons (PAHs) are generally assessed by measuring individual PAHs in the soil and correlating the obtained amounts to known adverse biological effects of the PAHs. The validity of such a risk estimation is dependent on the presence of additional compounds, the availability of the compounds (including the PAHs), and the methods used to correlate the measured chemical data and biological effects. In the work underlying this thesis the availability, chemical composition and biological effects of PAHs in samples of soils from PAH-contaminated environments were examined. It can be concluded from the results presented in the included papers that the PAHs in the studied soils from industrial sites were not generally physically trapped in soil material, indicating that the availability of the PAHs was not restricted in this sense. However, the bioavailable fraction of the PAHs, as assessed by bioassays with the earthworm Eisenia Fetida, could not be assessed by a number of abiotic techniques (including: solid phase micro extraction, SPME; use of semi-permeable membrane devices, SPMDs; leaching with various solvent mixtures, leaching using additives, and sequential leaching) and it seems to be difficult to find a chemical method that can accurately assess the bioavailability of PAHs. Furthermore, it was shown that PAH-polluted samples may be extensively chemically characterized by GC-TOFMS using peak deconvolution, and over 900 components can be resolved in a single run. The chemical characterization also revealed that samples that appeared to be similar in terms of their PAH composition were heterogeneous in terms of their overall composition. Finally, single compounds from this large set of compounds, which correlated with different biological effects, could be identified using the multivariate technique partial least squares projections to latent structures (PLS). This indicates that PLS may provide a valid alternative to Effect Directed Analysis (EDA), an established method for finding single compounds that correlate to the toxicity of environmental samples. Thus, the instrumentation and data evaluation tools used in this thesis are clearly capable of providing a broad chemical characterization as well as linking the obtained chemical data to results from bioassays. However, the link between the chemical analyses and the biological tests could be improved as as an organic solvent that solubilised virtually all of the contaminants was used during the chemical analysis while the biological tests were performed in an aqueous solution with limited solubility for a number of compounds. Consequently the compounds probably have a different impact in the biological tests than their relative abundance in profiles obtained by standard chemical analyses suggests. The availability and bioavailability of contaminants in soil also has to be studied further, and such future studies should focus on the molecular interactions between the contaminants and different compartments of the soil. By doing so, detailed knowledge could be obtained which could be applied to a number of different contaminants and soil types. Such studies would generate the data needed for molecular-based modelling of availability and bioavailability, which would be a big step forward compared to current risk assessment practices.
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| 41. |
- Bergknut, Magnus, et al.
(författare)
-
Comparison of techniques for estimating PAH bioavailability : uptake in Eisenia fetida, passive samplers and leaching using various solvents and additives.
- 2007
-
Ingår i: Environmental Pollution. - : Elsevier BV. - 0269-7491 .- 1873-6424. ; 145:1, s. 154-60
-
Tidskriftsartikel (refereegranskat)abstract
- The aim of this study was to evaluate different techniques for assessing the availability of polycyclic aromatic hydrocarbons (PAHs) in soil. This was done by comparing the amounts (total and relative) taken up by the earthworm Eisenia fetida with the amounts extracted by solid-phase microextraction (SPME), semi-permeable membrane devices (SPMDs), leaching with various solvent mixtures, leaching using additives, and sequential leaching. Bioconcentration factors of PAHs in the earthworms based on equilibrium partitioning theory resulted in poor correlations to observed values. This was most notable for PAHs with high concentrations in the studied soil. Evaluation by principal component analysis (PCA) showed distinct differences between the evaluated techniques and, generally, there were larger proportions of carcinogenic PAHs (4–6 fused rings) in the earthworms. These results suggest that it may be difficult to develop a chemical method that is capable of mimicking biological uptake, and thus estimating the bioavailability of PAHs. The total and relative amounts of PAHs extracted by abiotic techniques for assessing the bioavailability of PAHs was found to differ from the amounts taken up by Eisenia fetida. Keywords: Bioavailability; Polycyclic aromatic hydrocarbons; Earthworms; Leaching; Hydroxypropyl-β-cyclodextrin; Solid-phase microextraction; Semi-permeable membrane device
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| 42. |
- Bergknut, Magnus, et al.
(författare)
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Identification of potentially toxic compounds in complex extracts of environmental samples using gas chromatography-mass spectrometry and multivariate data analysis
- 2007
-
Ingår i: Environmental Toxicology and Chemistry. - New York : Pergamon. - 0730-7268 .- 1552-8618. ; 26:2, s. 208-217
-
Tidskriftsartikel (refereegranskat)abstract
- In this study, we examined 31 samples of varying chemical composition, including samples of soils from gasworks, coke production sites, and sites where wood preservatives were heavily used; ash and soot from municipal solid waste incinerators; antiskid sand; and dust from areas with heavy road traffic. The samples were comprehensively chemically characterized, especially their polycyclic aromatic compound contents, using gas chromatography-time-of-flight mass spectrometry, whereas their biological effects were assessed using dehydrogenase activity, root growth (Hordeum vulgare), reproduction of springtails (Folsomia candida), algal growth (Desmodesmus subspicatus), germinability (Sinapis alba), Vibrio fischeri, DR-CALUX, and Ames Salmonella assays. The number of compounds detected in the samples ranged from 123 to 527. Using the multivariate regression technique of partial-least-squares projections to latent structures, it was possible to find individual compounds that exhibited strong correlations with the different biological responses. Some of the results, however, indicate that a broader chemical characterization may be needed to identify all the compounds that may cause the measured biological responses.
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| 43. |
- Bergknut, Magnus, et al.
(författare)
-
Identification of potentially toxic compounds in complex extracts of environmental samples using GC-MS and multivariate data analysis
- 2007
-
Ingår i: Environmental Toxicology and Chemistry. - 0730-7268 .- 1552-8618. ; 26:2, s. 208-17
-
Tidskriftsartikel (refereegranskat)abstract
- In this study, we examined 31 samples of varying chemical composition, including samples of soils from gasworks, coke production sites, and sites where wood preservatives were heavily used; ash and soot from municipal solid waste incinerators; antiskid sand; and dust from areas with heavy road traffic. The samples were comprehensively chemically characterized, especially their polycyclic aromatic compound contents, using gas chromatography–time-of-flight mass spectrometry, whereas their biological effects were assessed using dehydrogenase activity, root growth (Hordeum vulgare), reproduction of springtails (Folsomia candida), algal growth (Desmodesmus subspicatus), germinability (Sinapis alba), Vibrio fischeri, DR-CALUX, and Ames Salmonella assays. The number of compounds detected in the samples ranged from 123 to 527. Using the multivariate regression technique of partial-least-squares projections to latent structures, it was possible to find individual compounds that exhibited strong correlations with the different biological responses. Some of the results, however, indicate that a broader chemical characterization may be needed to identify all the compounds that may cause the measured biological responses.
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| 44. |
- Bergknut, Magnus, et al.
(författare)
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Modelling the fate of hydrophobic organic contaminants in a boreal forest catchment : a cross disciplinary approach to assessing diffuse pollution to surface waters
- 2010
-
Ingår i: Environmental Pollution. - : Elsevier BV. - 0269-7491 .- 1873-6424. ; 158:9, s. 2964-2969
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Tidskriftsartikel (refereegranskat)abstract
- The fate of hydrophobic organic compounds (HOCs) in soils and waters in a northern boreal catchment was explored through the development of a chemical fate model in a well-characterised catchment system dominated by two land types: forest and mire. Input was based solely on atmospheric deposition, dominated by accumulation in the winter snowpack. Release from soils was governed by the HOC concentration in soil, the soil organic carbon fraction and soil-water DOC content. The modelled export of selected HOCs in surface waters ranged between 11 and 250ng day(-1) during the snow covered period, compared to 200 and 9600ng/d during snow-melt; highlighting the importance of the snow pack as a source of these chemicals. The predicted levels of HOCs in surface water were in reasonable agreement to a limited set of measured values, although the model tended to over predict concentrations of HOCs for the forested sub-catchment, by over an order of magnitude in the case of hexachlorobenzene and PCB 180. This possibly reflects both the heterogeneity of the forest soils and the complicated and changing hydrology experienced between the different seasons.
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| 45. |
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| 46. |
- Berglund, Åsa M. M., 1978-, et al.
(författare)
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Effects on the food-web structure and bioaccumulation patterns of organic contaminants in a climate-altered Bothnian Sea mesocosms
- 2023
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Ingår i: Frontiers in Marine Science. - : Frontiers Media S.A.. - 2296-7745. ; 10
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Tidskriftsartikel (refereegranskat)abstract
- Climate change is expected to alter global temperature and precipitation patterns resulting in complex environmental impacts. The proposed higher precipitation in northern Scandinavia would increase runoff from land, hence increase the inflow of terrestrial dissolved organic matter (tDOM) in coastal regions. This could promote heterotrophic bacterial production and shift the food web structure, by favoring the microbial food web. The altered climate is also expected to affect transport and availability of organic micropollutants (MPs), with downstream effects on exposure and accumulation in biota. This study aimed to assess climate-induced changes in a Bothnian Sea food web structure as well as bioaccumulation patterns of MPs. We performed a mesocosms-study, focusing on aquatic food webs with fish as top predator. Alongside increased temperature, mesocosm treatments included tDOM and MP addition. The tDOM addition affected nutrient availability and boosted both phytoplankton and heterotrophic bacteria in our fairly shallow mesocosms. The increased tDOM further benefitted flagellates, ciliates and mesozooplankton, while the temperature increase and MP addition had minor effect on those organism groups. Temperature, on the other hand, had a negative impact on fish growth and survival, whereas tDOM and MP addition only had minor impact on fish. Moreover, there were indications that bioaccumulation of MPs in fish either increased with tDOM addition or decreased at higher temperatures. If there was an impact on bioaccumulation, moderately lipophilic MPs (log Kow 3.6 - 4.6) were generally affected by tDOM addition and more lipophilic MPs (log Kow 3.8 to 6.4) were generally affected by increased temperature. This study suggest that both increased temperatures and addition of tDOM likely will affect bioaccumulation patterns of MPs in shallow coastal regions, albeit with counteracting effects.
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| 47. |
- Bidleman, Terry, 1942-, et al.
(författare)
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A review of halogenated natural products in Arctic, Subarctic and Nordic ecosystems
- 2019
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Ingår i: Emerging Contaminants. - : Elsevier. - 2405-6650 .- 2405-6642. ; 5, s. 89-115
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Tidskriftsartikel (refereegranskat)abstract
- Halogenated natural products (HNPs) are organic compounds containing bromine, chlorine, iodine, andrarely fluorine. HNPs comprise many classes of compounds, ranging in complexity from halocarbons tohigher molecular weight compounds, which often contain oxygen and/or nitrogen atoms in addition tohalogens. Many HNPs are biosynthesized by marine bacteria, macroalgae, phytoplankton, tunicates,corals, worms, sponges and other invertebrates. This paper reviews HNPs in Arctic, Subarctic and Nordicecosystems and is based on sections of Chapter 2.16 in the Arctic Monitoring and Assessment Program(AMAP) assessment Chemicals of Emerging Arctic Concern (AMAP, 2017) which deal with the highermolecular weight HNPs. Material is updated and expanded to include more Nordic examples. Much ofthe chapter is devoted to “bromophenolic” HNPs, viz bromophenols (BPs) and transformation productsbromoanisoles (BAs), hydroxylated and methoxylated bromodiphenyl ethers (OH-BDEs, MeO-BDEs) andpolybrominated dibenzo-p-dioxins (PBDDs), since these HNPs are most frequently reported. Othersdiscussed are 2,20-dimethoxy-3,30,5,50-tetrabromobiphenyl (2,20-dimethoxy-BB80), polyhalogenated 10-methyl-1,20-bipyrroles (PMBPs), polyhalogenated 1,10-dimethyl-2,20-bipyrroles (PDBPs), polyhalogenatedN-methylpyrroles (PMPs), polyhalogenated N-methylindoles (PMIs), bromoheptyl- and bromooctylpyrroles, (1R,2S,4R,5R,10E)-2-bromo-1-bromomethyl-1,4-dichloro-5-(20-chloroethenyl)-5-methylcyclohexane (mixed halogenated compound MHC-1), polybrominated hexahydroxanthene derivatives(PBHDs) and polyhalogenated carbazoles (PHCs). Aspects of HNPs covered are physicochemicalproperties, sources and production, transformation processes, concentrations and trends in the physicalenvironment and biota (marine and freshwater). Toxic properties of some HNPs and a discussion of howclimate change might affect HNPs production and distribution are also included. The review concludeswith a summary of research needs to better understand the role of HNPs as “chemicals of emergingArctic concern”.
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| 48. |
- Bidleman, Terry, et al.
(författare)
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Atmospheric pathways of chlorinated pesticides and natural bromoanisoles in the northern Baltic Sea and its catchment
- 2015
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Ingår i: Ambio. - : Springer Science and Business Media LLC. - 0044-7447 .- 1654-7209. ; 44, s. 472-483
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Tidskriftsartikel (refereegranskat)abstract
- Long-range atmospheric transport is a major pathway for delivering persistent organic pollutants to the oceans. Atmospheric deposition and volatilization of chlorinated pesticides and algae-produced bromoanisoles (BAs) were estimated for Bothnian Bay, northern Baltic Sea, based on air and water concentrations measured in 2011-2012. Pesticide fluxes were estimated using monthly air and water temperatures and assuming 4 months ice cover when no exchange occurs. Fluxes were predicted to increase by about 50 % under a 2069-2099 prediction scenario of higher temperatures and no ice. Total atmospheric loadings to Bothnian Bay and its catchment were derived from air-sea gas exchange and bulk'' (precipitation ? dry particle) deposition, resulting in net gains of 53 and 46 kg year(-1) for endosulfans and hexachlorocyclohexanes, respectively, and net loss of 10 kg year(-1) for chlordanes. Volatilization of BAs releases bromine to the atmosphere and may limit their residence time in Bothnian Bay. This initial study provides baseline information for future investigations of climate change on biogeochemical cycles in the northern Baltic Sea and its catchment.
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| 49. |
- Bidleman, Terry F., et al.
(författare)
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Air-water exchange of brominated anisoles in the northern baltic sea
- 2014
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 48:11, s. 6124-6132
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Tidskriftsartikel (refereegranskat)abstract
- Bromophenols produced by marine algae undergo O-methylation to form bromoanisoles (BAs), which are exchanged between water and air. BAs were determined in surface water of the northern Baltic Sea (Gulf of Bothnia, consisting of Bothnian Bay and Bothnian Sea) during 2011-2013 and on a transect of the entire Baltic in September 2013. The abundance decreased in the following order: 2,4,6-tribromoanisole (2,4,6-TBA) > 2,4-dibromoanisole (2,4-DBA) ≫ 2,6-dibromoanisole (2,6-DBA). Concentrations of 2,4-DBA and 2,4,6-TBA in September were higher in the southern than in the northern Baltic and correlated well with the higher salinity in the south. This suggests south-to-north advection and dilution with fresh riverine water enroute, and/or lower production in the north. The abundance in air over the northern Baltic also decreased in the following order: 2,4,6-TBA > 2,4-DBA. However, 2,6-DBA was estimated as a lower limit due to breakthrough from polyurethane foam traps used for sampling. Water/air fugacity ratios ranged from 3.4 to 7.6 for 2,4-DBA and from 18 to 94 for 2,4,6-TBA, indicating net volatilization. Flux estimates using the two-film model suggested that volatilization removes 980-1360 kg of total BAs from Bothnian Bay (38000 km(2)) between May and September. The release of bromine from outgassing of BAs could be up to 4-6% of bromine fluxes from previously reported volatilization of bromomethanes and bromochloromethanes.
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| 50. |
- Bidleman, Terry F., et al.
(författare)
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Atmospheric transport and deposition of bromoanisoles along a temperate to arctic gradient
- 2017
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Ingår i: Environmental Science and Technology. - Washington : American Chemical Society (ACS). - 1086-931X .- 1520-6912 .- 0013-936X .- 1520-5851. ; 51:19, s. 10974-10982
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Tidskriftsartikel (refereegranskat)abstract
- Bromoanisoles (BAs) arise from O-methylation of bromophenols, produced by marine algae and invertebrates. BAs undergo sea-air exchange and are transported over the oceans. Here we report 2,4-DiBA and 2,4,6-TriBA in air and deposition on the Swedish west coast (Råö) and the interior of arctic Finland (Pallas). Results are discussed in perspective with previous measurements in the northern Baltic region in 2011−2013. BAs in air decreased from south to north in the order Råö > northern Baltic > Pallas. Geometric mean concentrations at Pallas increased significantly (p < 0.05) between 2002 and 2015 for 2,4-DiBA but not for 2,4,6-TriBA. The logarithm of BA partial pressures correlated significantly to reciprocal air temperature at the coastal station Råö and over the Baltic, but only weakly (2,4-DiBA) or not significantly (2,4,6-TriBA) at inland Pallas. Deposition fluxes of BAs were similar at both sites despite lower air concentrations at Pallas, due to greater precipitation scavenging at lower temperatures. Proportions of the two BAs in air and deposition were related to Henry’s law partitioning and source regions. Precipitation concentrations were 10−40% of those in surface water of Bothnian Bay, northern Baltic Sea. BAs deposited in the bay catchment likely enter rivers and provide an unexpected source to northern estuaries. BAs may be precursors to higher molecular weight compounds identified by others in Swedish inland lakes.
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