| 1. |
- Josefsson, Sarah, 1976-, et al.
(författare)
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Capping efficiency of various carbonaceous and mineral materials for in situ remediation of marine sediments contaminated with PCDD/Fs, OCS and HCB
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- The efficiency of various thin-layer capping materials in reducing the sediment-to-water flux and benthic organism bioaccumulation of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), hexachlorobenzene (HCB) and octachlorostyrene (OCS) was investigated in a boxcosm experiment. The influence of cap layer thickness (0.5-5 cm) and different cap materials were tested using a three-factor experimental design. The capping materials consisted of a passive carrier (coarse or fine limestone material, or a marine clay sediment), and an active material (activated carbon (AC) or kraft lignin) to sequester the contaminants and decrease their bioavailability. Macrofauna was added to the boxes to get a semi-natural bioturbation. The sediment-to-water flux was measured using passive (SPMD) samplers, and the bioaccumulation by the surface-dwelling gastropod Hinia reticulata and the deep-burrowing polychaetes Nereis spp. was determined. Results showed substantial decreases in both flux and bioaccumulation as a result of thin-layer capping. The thickness of the capping layer and the choice of active material were important factors, while the use of different types of passive materials was not statistically significant for any of the observed endpoints. Flux and bioaccumulation decreased with increased cap thickness, and could be further decreased with addition of active material. Activated carbon was more efficient than lignin, and a ~90% reduction of the flux and bioaccumulation, compared to uncapped control sediment, could be achieved with 3 cm caps with 3.3% AC (g C/g ww clay). The reduction was generally larger in the surface-dwelling H. reticulata than in Nereis spp., and the magnitude of the reduction was frequently similar between Nereis spp. and sediment-to-water fluxes. The latter was interpreted to indicate a link between Nereis spp. bioirrigation and sediment-to-water fluxes. Furthermore, the reduction in sediment-to-water flux was dependent on the hydrophobicity of the congeners, with less hydrophobic congeners achieving a larger reduction than more hydrophobic congeners.
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| 2. |
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| 3. |
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| 4. |
- Josefsson, Sarah, 1976-
(författare)
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Fate and transport of POPs in the aquatic environment : with focus on contaminated sediments
- 2011
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Persistent organic pollutants (POPs) are hydrophobic substances that readily sorb to organic matter in particles and colloids instead of being freely dissolved in the water phase. This sorption affects the bioavailability and environmental transport of the POPs. The major part of this thesis concerns the role of sediments as secondary sources of POPs. As the primary emissions decrease, contaminated sediments where POPs have accumulated can become the main source of contamination. If the contaminated sediment by time becomes covered with cleaner layers, the POPs are buried and no longer in contact with the aquatic environment. Experiments in this thesis showed, however, that new invading species can alter the sediment-water dynamics as a result of their bioturbation, i.e. mixing of sediment particles and pore-water. Marenzelleria spp., invading species in the Baltic Sea that burrow deeper than native species, were found to increase the remobilization of buried contaminants. The sediment-to-water flux was inversely related to the burial depth (2-10 cm) of the POP congeners (polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers) and also inversely related to the hydrophobicity of the congener. The flux was therefore most pronounced for less hydrophobic contaminants, which was linked to the bioirrigating behaviour of these species. Marenzelleria spp. also accumulated the buried POPs and increased concentrations in surface sediment. Contaminants previously considered buried at a ’safe’ depth can thus be remobilized as a result of the invasion of Marenzelleria spp. in the Baltic Sea.One method to decrease the remobilization of contaminants from sediments is ’capping’, i.e. a layer of clean material is placed as a cap on the sediment. By amending the cap with active materials, which sequester the POPs and decrease their availability, thinner layers can be used (’active capping’ or ’thin-layer capping’). Results from an experiment with thin-layer capping using different active materials (activated carbon (AC) and kraft lignin) showed that both the sediment-to-water flux and the bioaccumulation by benthic species of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), hexachlorobenzene (HCB) and octachlorostyrene (OCS) decreased with increased thickness of the cap layer (0.5-5 cm). Amendments with active materials further increased the cap efficiency. AC was more efficient than kraft lignin, and a 3 cm cap with 3.3% AC reduced the flux and bioaccumulation with ~90%. The reduction of the sediment-to-water flux was inversely related to the hydrophobicity of the POP, and reductions in the flux had similar magnitudes as reductions in the concentration in deep-burrowing polychaetes, demonstrating the importance of bioturbation for sediment-to-water transport.In a one-year study on the levels of PCDD/Fs, PCBs, and HCB in a coastal area of the Baltic Sea, the correlations between the POP levels and the levels of particles and organic carbon in the water were found to differ for POPs of different structure and hydrophobicity. The levels of PCDD/Fs decreased to one third in May, which could be related to the increased sedimentation, i.e. water-to-sediment transport, during spring bloom.
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| 5. |
- Danielsson, Conny, 1977-
(författare)
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Trace analysis of dioxins and dioxin-like PCBs using comprehensive two-dimensional gas chromatography with electron capture detection
- 2006
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs), two groups of struc-turally related chlorinated aromatic hydrocarbons, generally referred to as “dioxins” are of great concern due to their extreme toxicity and presence in all compartments of the environment. Since they occur at very low levels, their analysis is complex and challenging, and there is a need for cost-efficient, reliable and rapid analytical alternatives to the expensive methods in-volving use of gas chromatography high-resolution mass spectrometry (GC-HRMS). It is im-portant to routinely monitor food and feed items to detect contaminations at an early stage. For the regulation of dioxins and dioxin-like PCBs in food and feed according to current legis-lation, large numbers of samples have to be analysed. Furthermore, soils at many industrial sites are also contaminated with dioxins and need remediation. In order to optimize the cost-efficiency of reclamation activities it is important to acquire information about the levels and distribution of dioxins in the contaminated areas. The aim of the studies underlying this thesis was to investigate the potential of comprehen-sive two-dimensional gas chromatography with a micro-electron capture detector (GC × GC-µECD) as a cost-effective method for analysing dioxins and dioxin-like PCBs in food, feed, fly ash and contaminated soils. Quantification studies of dioxins and dioxin-like PCBs were con-ducted and results were compared with GC-HRMS reference data. Generally, there was good agreement between both the congener-specific results and data expressed as total toxic equiva-lents (TEQs). The developed GC × GC-µECD method meets the European Community (EC) requirements for screening methods for control of dioxins and dioxin-like PCBs in food and feed. The presented results also indicate that GC × GC-µECD has potential to be used as a routine method for the congener-specific analysis of 2,3,7,8-PCDD/Fs and dioxin-like PCBs in matrices such as food and feed, fly ash and soil. However, to fully exploit the potential of the GC × GC-µECD technique, it should be combined with a fast and cost-efficient sample preparation procedure. Therefore, a number of certified reference materials (CRMs) were extracted using a new shape-selective pressurized liquid extraction technique with integrated carbon fractionation (PLE-C), and the purified extracts were analysed for PCDD/Fs using GC × GC-µECD. The results compared well with the certified values of a fly ash and a sandy soil CRM, but they were much too high for a com-plex clay soil CRM. It was concluded that this combination of techniques was very promising for screening ash and highly permeable soils. Further assessments and method revisions are still required before GC × GC-µECD can be used on a routine basis, and available software packages need to be refined in order to accelerate the data-handling procedures, which currently restrict the sample throughput.
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| 6. |
- Sundqvist, Kristina, 1978-
(författare)
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Sources of dioxins and other POPs to the marine environment : Identification and apportionment using pattern analysis and receptor modeling
- 2009
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- In the studies underlying this thesis, various source tracing techniques were applied to environmental samples from the Baltic region. Comprehensive sampling and analysis of polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) in surface sediments in Swedish coastal and offshore areas resulted in a unique data set for this region. Nearly 150 samples of surface sediments were analyzed for all tetra- to octa-chlorinated PCDD/Fs. The levels showed large spatial variability with hotspots in several coastal regions. Neither Sweden nor the EU has introduced guideline values for PCDD/Fs in sediment, but comparisons to available guidelines and quality standards from other countries indicate that large areas of primarily coastal sediments may constitute a risk to marine organisms. Multivariate pattern analysis techniques and receptor models, such as Principal Component Analysis (PCA) and Positive Matrix Factorization (PMF), were used to trace sources. These analyses suggested that three to six source types can explain most of the observed pattern variations found in the sediment samples. Atmospheric deposition was suggested as the most important source to offshore areas, thus confirming earlier estimates. However, spatial differences indicated a larger fraction of local/regional atmospheric sources, characterized by PCDFs, in the south. This was indicated by the identification of several patterns of atmospheric origin. In coastal areas, the influence of direct emission sources was larger, and among these, chlorophenol used for wood preservation and emissions from pulp/paper production and other wood related industry appeared to be most important. The historic emissions connected to processes involving chemical reactions with chlorine (e.g. pulp bleaching) were found to be of less importance except at some coastal sites. The analysis of PCDD/Fs in Baltic herring also revealed spatial variations in the levels and pollution patterns along the coast. The geographical match against areas with elevated sediment levels indicated that transfer from sediments via water to organisms was one possible explanation. Fugacity, a concept used to predict the net transport direction between environmental matrices, was used to explore the gas exchange of hexachlorocyclohexanes (HCHs) and polychlorinated biphenyls (PCBs) between air and water. These estimates suggested that, in the Kattegat Sea, the gaseous exchange of HCHs primarily resulted in net deposition while PCBs were net volatilized under certain environmental conditions. The study also indicated that, while the air concentrations of both PCBs and γ-HCH are mostly dependent upon the origin of the air mass, the fluctuations in α-HCH were primarily influenced by seasonal changes.
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| 7. |
- Åberg, Annika, 1975-
(författare)
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Fate and exposure assessment of PCDD/Fs at contaminated sites
- 2008
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Licentiatavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Polychlorinated dibenzo-p-dioxins (PCDD) and polychlorinated dibenzo-furans (PCDFs) belong to the most toxic compounds known to science and they are defined as Persistent Organic Pollutants (POPs) under the Stock-holm Convention. The general human exposure to PCDD/Fs is primarily through dietary intake. The importance of contaminated sites as secondary PCDD/F sources (i.e. sources that once received its contamination from a primary source) are getting increased attention. To be able to assess the risks for human exposure at PCDD/F contaminated sites, the environmen-tal distribution of PCDD/Fs and the potential mobilization between dif-ferent environmental media (e.g. food chain transfer) must be known. The primary aim of the work presented in this thesis was to investigate human exposure pathways associated with PCDD/F contaminated sites by combining field measurements and modeling. Site specific field measurements were made at a PCDD/F contaminated site in Sweden and multimedia modeling scenarios were evaluated against site specific data and national reference data. The results show that the congener distributions in exposure media affected by contaminated soil may differ significantly from the distribu-tions found in media from reference locations. Higher chlorinated PCDD/Fs may be transferred into food chains where they contribute to a large fraction of the toxic equivalent concentration (TEQ). Ingestion of locally produced animal food may be an important exposure pathway al-ready at low or moderate PCDD/F soil concentrations. However, the con-gener composition of the source is critical for the exposure. The signifi-cance of the individual exposure routes varies depending on e.g. the spatial distribution and magnitude of the soil contamination, the pro-perties of the exposure media and the human behavior. Multimedia mo-deling can be used in risk assessments as long as model algorithms and model parameters are representative for the superhydrophobic properties of PCDD/Fs. However, selection of physical-chemical PCDD/F properties is a challenge due to large variation in reported values. For some proper-ties, data is scattered or completely lacking
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| 8. |
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| 9. |
- Blum, Kristin M., 1989-, et al.
(författare)
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Mass fluxes per capita of organic contaminants from on-site sewage treatment facilities
- 2018
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Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; :201, s. 864-873
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Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
- This study is the first attempt to quantify environmental fluxes per capita of organic contaminants discharged from on-site sewage treatment facilities (OSSFs) in affected recipients. Five sites were monitored around the River Fyris in Sweden: three mainly affected by OSSFs and two mainly affected by municipal sewage treatment plants (STPs). Gas chromatography-mass spectrometry was used to determine environmental concentrations of 30 anthropogenic contaminants, including organophosphorus compounds, rubber and plastic additives, UV stabilizers, fragrances, surfactant ingredients and polycyclic aromatic hydrocarbons. Uni- and multivariate statistical analysis of the most frequently detected contaminants showed that median fluxes per capita of tris(1,3-dichloro-2-propyl) phosphate, tris(1-chloro-2-propyl) phosphate, tris(2-chloroethyl) phosphate, and n-butylbenzene sulfonamide were similar at OSSF and STP sites, but the mass fluxes per capita of tris-(2-butoxyethyl) phosphate, 2-(methylthio)benzothiazole, and galaxolide, were significantly lower (~2 to 3-fold) at OSSF sites than at STP sites (Mann-Whitney, α = 0.05). Differences between these sites were larger in samples collected in summer and autumn than in samples collected in winter. Deviations likely originated from differences in treatment technology and distances between source and sampling sites. Further studies are needed to characterize mass fluxes per capita of contaminants in waters that directly receive discharges from OSSFs.
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| 10. |
- Ahrens, Lutz, et al.
(författare)
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Screening of PFASs in groundwater and surface water
- 2016
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Rapport (övrigt vetenskapligt/konstnärligt)abstract
- Per- and polyfluoroalkyl substances (PFASs) are emerging organic pollutants characterized by their persistency, and bioaccumulation and toxicity potential. In this study, 26 PFASs were screened in 502 water samples originating from Swedish groundwater, surface water, sewage treatment plant (STP) effluents and landfill leachates. The objectives were to establish baseline concentrations of PFASs in the aquatic environment, to screen for potential sources, and to compare PFAS concentrations with guideline values for estimation of potential effects on the ecosystem and human health. In drinking water source areas, the average ∑26PFAS concentration was 8.4 ng L-1 with a median value of 0.6 ng L-1 (n = 172). The drinking water guideline value of 90 ng L-1 for ∑7PFASs (PFPeA, PFHxA, PFHpA, PFOA, PFBS, PFHxS, PFOS) established by the Swedish National Food Agency was exceeded in 4 samples (2% of the total number of samples in this category). In water not used for drinking water, ∑26PFASs concentrations were on average 142 ng L-1 (median 5.4 ng L-1). The high average PFAS concentrations can be explained by the fact that some samples showed extremely high PFAS concentrations with a maximum ∑26PFASs value of 12 900 ng L-1. In surface water, PFOS concentrations exceeded the annual average Environmental Quality Standard (AA-EQS) of the EU Water Framework Directive (WFD) in 42% of the samples. Among the different water categories, the landfill leachates had the highest average concentration of ∑26PFAS with 487 ng L-1 (median 435 ng L-1, n = 10), followed by surface water (average 112 ng L-1, median 4.1 ng L-1, n = 285), groundwater (average 49 ng L-1, median 0.4 ng L-1, n = 164), STP effluents (average 35 ng L-1, median 26 ng L-1; n = 13) and background screening lakes (remote lakes; average 3.4 ng L-1, median 1.4 ng L-1, n = 10). The composition profile of the PFASs differed between the types of waters showing an even distribution of ∑PFCAs, ∑PFSAs and ∑PFAS precursors in groundwater, whereas in all other water categories (surface water, background lakes, STP effluents and landfill leachates), ∑PFCAs were dominant. As FOSA, PFNA, PFDA, and 6:2 FTSA were frequently detected in drinking water source areas (constituted 20%, 7.3%, 5.9%, and 4.4% of the ∑26PFASs, respectively), it is reasonable to consider the inclusion of these in the Swedish drinking water guideline.
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