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Sources of dioxins and other POPs to the marine environment: Identification and apportionment using pattern analysis and receptor modeling
Umeå University, Faculty of Science and Technology, Chemistry.
2009 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

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.

 

Place, publisher, year, edition, pages
Umeå: Umeå University , 2009. , 69 p.
Keyword [en]
air-water gas exchange, chiral, congener pattern, enantiomer, enantiomeric fraction, fugacity, HCH, hexachlorocyclohexane, homologue profile, indicator congener, isomer pattern, pattern analysis, PCA, PCB, PCDD/F, PMF, polychlorinated dibenzofuran, polychlorinated dibenzo-p-dioxin, polychlorinated biphenyl, positive matrix factorization, principal component analysis, receptor modeling, source apportioning, source, source tracing
National Category
Environmental Sciences Environmental Sciences
Identifiers
URN: urn:nbn:se:umu:diva-22266ISBN: 978-91-7264-792-3 (print)OAI: oai:DiVA.org:umu-22266DiVA: diva2:214190
Public defence
2009-05-29, KB3B1, KBC-huset, Umeå Universitet, Umeå, 13:00 (English)
Opponent
Supervisors
Available from: 2009-05-08 Created: 2009-05-04 Last updated: 2009-05-08Bibliographically approved
List of papers
1. Air–sea gas exchange of HCHs and PCBs and enantiomers of α-HCH in the Kattegat Sea region
Open this publication in new window or tab >>Air–sea gas exchange of HCHs and PCBs and enantiomers of α-HCH in the Kattegat Sea region
2004 (English)In: Environmental Pollution: Volume 128, Issues 1-2, March 2004, Pages 73-83, ISSN 0269-7491, Vol. 128, no 1-2, 73-83 p.Article in journal (Refereed) Published
Abstract [en]

Concentrations and air–water gas exchange of polychlorinated biphenyls (PCBs) and hexachlorocyclohexanes (HCHs) were determined in nine paired air and water samples. The samples were collected monthly in the Kattegat Sea between December 1998 and November 1999. Average fugacity and flux values indicated that PCBs were oversaturated in the water, while HCHs were net deposited. Variations were large over the year, especially during spring and summer. Air parcel back trajectories suggested that air concentrations over the Kattegat Sea are largely dependent of air mass origin. Seasonal trends were detected for airborne HCHs and for PCBs in water. The air and water enantiomeric compositions of α-HCH indicated that a larger portion of α-HCH in air originated from the underlying water during summer than during winter.

Air–water exchange of PCBs and HCHs is studied in the Kattegat Sea and shows to vary seasonally.

Keyword
HCHs, PCBs, Gas exchange, Kattegat Sea, Enantiomer fraction
Identifiers
urn:nbn:se:umu:diva-14198 (URN)doi:10.1016/j.envpol.2003.08.022 (DOI)
Available from: 2007-05-24 Created: 2007-05-24 Last updated: 2011-01-12Bibliographically approved
2. Levels and homologue profiles of PCDD/Fs in sediments along the Swedish coast of the Baltic Sea
Open this publication in new window or tab >>Levels and homologue profiles of PCDD/Fs in sediments along the Swedish coast of the Baltic Sea
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2009 (English)In: Environmental science and pollution research international, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 16, no 4, 396-409 p.Article in journal (Refereed) Published
Abstract [en]

Background, aim, and scope  The primary aim of this study was to explore the variations in PCDD/F levels and homologue profiles of Baltic surface sediments by comprehensively analyzing polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs) in samples from a large number of sites, encompassing not only previously known hotspot areas, but also sites near other potential PCDD/F sources, in pristine reference areas (in which there was no industrial activity) and offshore sites. Materials and methods  Surface sediment samples (146 in total) were collected at various points along the Swedish coast and offshore areas. In addition, bulk deposition was sampled, monthly, at a single site in northern Sweden during 1 year. The concentrations of tetra- through octa-substituted CDD/Fs were determined in both matrices. Results  Highly elevated concentrations of PCDD/Fs were found at many sites in coastal areas and concentrations were also slightly elevated in some offshore areas. Homologue profiles varied substantially amongst samples from coastal sites, while those from offshore and other pristine sediments were relatively similar. The offshore sediments showed different profiles from those observed in the deposition samples. Sediment levels of PCDD/Fs were not generally significantly correlated to organic carbon levels, except in some pristine areas. Comparison of data obtained in this and previous studies suggest that both their levels and profiles are similar today to those observed 20 years ago in coastal and offshore areas. The only detected trend is that their levels appear to have decreased slightly in the offshore area of the Bothnian Sea. Discussion  The localization of hotspot areas along the coast, the lack of consensus between PCDD/F profiles of sediments and general background, and their weak correlations with organic carbon suggest that PCDD/Fs in the study area largely originate from local/regional emissions. However, due to complicating factors such as sediment dynamics and land upheaval, it is not possible to conclude whether these pollutants derive from recent emissions or from a combination of recent emissions and re-distribution of previous inputs. Conclusions  The results show that: elevated levels of PCDD/Fs are present in both coastal and offshore areas of the Baltic Sea, the major hotspots are close to the shore, and there are large variations in profiles, indicating that local emissions are (or have been) the major causes of pollution. Recommendations and perspectives  In order to identify other hotspot areas and trace sources, comprehensive analysis of PCDD/Fs in surface sediments is needed in all areas of the Baltic Sea that have not been previously investigated. The high levels of PCDD/Fs observed in surface sediments also indicate a need to elucidate whether they are due mainly to current emissions or a combination of recent pollution and re-distribution of historically deposited pollutants. To do so, better understanding of sediment dynamics and present-day inputs, such as riverine inputs, industrial effluents, and leakage from contaminated soil is required. There are indications that contaminated sediments have a regional impact on fish contamination levels. However, as yet there is no statistically robust evidence linking contaminated sediments with elevated levels in Baltic biota. It should also be noted that the Baltic Sea is being massively invaded by the deep-burrowing polychaete Marenzielleria ssp., whose presence in sediments has been shown to increase water concentrations of hydrophobic pollutants. In awareness of this, it is clear that high levels in sediments cannot be ignored in risk assessments. In order to investigate the emission trends more thoroughly, analysis of PCDD/Fs in offshore sediment cores throughout the Baltic Sea is also recommended. Electronic supplementary material  The online version of this article (doi:10.1007/s11356-009-0110-z) contains supplementary material, which is available to authorized users.

Place, publisher, year, edition, pages
Springer Science, 2009
Keyword
Baltic sea, Homologue profiles, Patterns, PCDDs, PCDFs, Polychlorinated dibenzofurans, Polychlorinated dibenzo-p-dioxins, Sediment, Sources
National Category
Environmental Sciences Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-22261 (URN)10.1007/s11356-009-0110-z (DOI)
Available from: 2009-05-04 Created: 2009-05-04 Last updated: 2017-12-13
3. Congener fingerprints of tetra- through octa-chlorinated dibenzo-p-dioxins and dibenzofurans in Baltic surface sediments and their relations to potential sources
Open this publication in new window or tab >>Congener fingerprints of tetra- through octa-chlorinated dibenzo-p-dioxins and dibenzofurans in Baltic surface sediments and their relations to potential sources
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2009 (English)In: Chemosphere, Vol. 77, no 5, 612-20 p.Article in journal (Refereed) Published
Abstract [en]

Comprehensive congener fingerprints of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), including non-2,3,7,8-substituted congeners, in 142 surface sediment samples from the Baltic Sea were characterized by Principal Component Analysis (PCA). The pattern analysis revealed source specific indicators of chlorophenol use, high temperature processes, chlorine bleach/chloralkali production and a source signature suggested to originate from pulp/paper or related production. Congener patterns in sediments from offshore and pristine coastal areas showed strong resemblance to patterns of atmospheric deposition and flue gases, indicating that these sources have high impact in areas that are not affected by point sources. Prominent contributors to the patterns of hotspot areas along the Swedish coast included chlorophenol indicators and a source characterized by hexa-CDDs while the contribution of the traditional chlorine bleach pattern was weaker. This study demonstrates the importance of comprehensive PCDD/F congener analysis for identifying links to candidate sources.

Place, publisher, year, edition, pages
Elsevier Ltd, 2009
Keyword
Indicator congener, pattern analysis, PCA, PCDD/F, source tracing
National Category
Environmental Sciences Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-22262 (URN)10.1016/j.chemosphere.2009.08.057 (DOI)
Note
Available online 23 September 2009. Available from: 2009-05-04 Created: 2009-05-04 Last updated: 2010-02-22
4. PCDD/F Source Apportionment in the Baltic Sea Using Positive Matrix Factorization
Open this publication in new window or tab >>PCDD/F Source Apportionment in the Baltic Sea Using Positive Matrix Factorization
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2010 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 44, no 5, 1690-7 p.Article in journal (Refereed) Published
Abstract [en]

Positive Matrix Factorization (PMF) was used to identify and apportion candidate sources of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/F) in samples of offshore and coastal surface sediments from the Baltic Sea. Atmospheric deposition was the dominant source in offshore and pristine areas, in agreement with previous studies. Earlier chlorophenol use and a source suggested origins from pulp and paper production and related industries were identified as important coastal sources. A previously presumed major source, chlorine bleaching of pulp, was of only minor importance for modern Baltic surface sediments. The coastal source impacts were mostly local or regional, but pattern variations in offshore samples indicate that coastal sources may have some importance for offshore areas. Differences between sub-basins also indicated that local and regional air emissions from incineration or other high-temperature processes are more important in the southern Baltic Sea compared to those in northerly areas. These regional differences demonstrated the importance of including offshore sediments from the Bothnian Bay, Gulf of Finland, and other areas of the Baltic Sea in future studies to better identify the major PCDD/F sources to the Baltic Sea.

Place, publisher, year, edition, pages
American Chemical Society, 2010
National Category
Environmental Sciences Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-22263 (URN)10.1021/es9030084 (DOI)000274842000029 ()
Available from: 2009-05-04 Created: 2009-05-04 Last updated: 2017-12-13Bibliographically approved
5. Spatial variation in concentrations and patterns of the PCDD/F and dioxin-like-PCB content in herring from the northern Baltic Sea
Open this publication in new window or tab >>Spatial variation in concentrations and patterns of the PCDD/F and dioxin-like-PCB content in herring from the northern Baltic Sea
2007 (English)In: Journal of Environmental Monitoring, ISSN 1464-0325, E-ISSN 1464-0333, Vol. 9, no 6, 550-556 p.Article in journal (Refereed) Published
Abstract [en]

The purpose of the current study was to investigate spatial and seasonal variation of dioxin and dioxin-like PCB (dl-PCB) content in herring sampled along the northern Baltic Sea coast and map out risk zones for dioxins and dl-PCBs. We further aimed to investigate relationships between congener distribution (pattern) and sampling location and season. The results showed that there were distinct geographical differences in concentrations of dioxins, dibenzofurans and dl-PCBs along the Swedish coast, from the Bothnian Bay to north Baltic Proper, with the highest levels detected in the southern Bothnian Sea. The majority of the locations showed concentrations above the prescribed maximum for dioxin residues (4 TEQ pg g–1 wet weight [w.w.]). If all the edible parts of the fish (muscle, subcutaneous fat and skin) are considered, the estimated concentrations exceeded the prescribed maximum level in the whole study area for herring collected during spring–summer. Concentrations in herring caught during spring–summer compared to concentrations in herring sampled in the autumn indicated seasonal variation. The pattern analysis showed a variation in relative congener concentration at the different sampling locations (spring–summer). Pattern differences were also noticed between seasons.

Place, publisher, year, edition, pages
Cambridge: Royal Society of Chemistry, 2007
National Category
Environmental Sciences Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-22264 (URN)10.1039/b700667e (DOI)
Available from: 2009-05-04 Created: 2009-05-04 Last updated: 2017-12-13Bibliographically approved

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