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Trends and exposure of naturally produced brominated substances in Baltic biota - with focus on OH-PBDEs, MeO-PBDEs and PBDDs
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The semi-enclosed and brackish Baltic Sea has become heavily polluted by nutrients, anthropogenic organic and inorganic chemicals via human activities. Persistent organic pollutants (POPs) have been thoroughly investigated due to their linkage to toxic effects observed in Baltic biota. There has been far less focus on semi-persistent pollutants e.g. naturally produced oraganohalogen compounds (NOCs) and their disturbances in the environment. This thesis is aimed on assessment of levels and trends of naturally produced brominated compounds in Baltic biota; more specifically on hydroxylated polybrominated diphenyl ethers (OH-PBDEs), methoxylated PBDEs (MeO-PBDEs) and polybrominated dibenzo-p-dioxins (PBDDs). These, NOCs, may originate from production in algae and cyanobacteria. OH-PBDEs and MeO-PBDEs may also be formed as metabolites of polybrominated diphenyl ethers (PBDEs), i.e. well-known commercial flame retardants.

High levels of OH-PBDEs, MeO-PBDEs and PBDDs are shown within Baltic biota (cyanobacteria, algae, mussels, fish), often in much higher concentrations than PBDEs which are possible anthropogenic precursors of OH- and MeO-PBDEs. The levels of OH-PBDEs, MeO-PBDEs and PBDDs are higher in the Baltic Sea than on the west coast of Sweden. Temporal and seasonal variations show fluctuations in concentrations of OH-PBDEs, MeO-PBDEs and PBDDs, possibly related with macroalgal life-cycles. OH-PBDEs, MeO-PBDEs and PBDDs are present in several filamentous macroalgae species, but considering the levels quantified, the time of peak exposure and the species life-cycle the macroalgae, Pilayella, Ceramium and Cladophora are suggested as major natural producers of OH-PBDEs and PBDDs.

The high levels of OH-PBDEs, MeO-PBDEs and PBDDs in the Baltic Sea may affect numerous organisms in the ecosystem. The toxic effects of OH-PBDEs and PBDDs are of particular concern. This thesis stress the importance of assessing and monitoring these substances, since the exposure to OH-PBDEs and PBDDs, during summer, may cause acute effects in Baltic fish and wildlife.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry (MMK), Stockholm University , 2011. , 70 p.
Keyword [en]
Batlic Sea, Natural production, OH-PBDE, MeO-PBDE, PBDD
National Category
Environmental Sciences
Research subject
Environmental Chemistry
Identifiers
URN: urn:nbn:se:su:diva-54421ISBN: 978-91-7447-266-4 OAI: oai:DiVA.org:su-54421DiVA: diva2:393974
Public defence
2011-03-04, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 10:00 (English)
Opponent
Supervisors
Note
At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: In press. Paper 4: Manuscript.Available from: 2011-02-10 Created: 2011-02-01 Last updated: 2011-02-03Bibliographically approved
List of papers
1. Brominated phenols, anisoles, and dioxins present in blue mussels from the Swedish coastline
Open this publication in new window or tab >>Brominated phenols, anisoles, and dioxins present in blue mussels from the Swedish coastline
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2010 (English)In: Environmental science and pollution research international, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 17, no 8, 1460-1468 p.Article in journal (Refereed) Published
Abstract [en]

Introduction  

Naturally occurring hydroxylated polybrominated diphenyl ethers (OH-PBDEs), their methoxylated counterparts (MeO-PBDEs), and polybrominated dibenzo-p-dioxins (PBDDs), together with their potential precursors polybrominated phenols (PBPs) and polybrominated anisoles (PBAs), were analyzed in blue mussels (Mytilus edulis) gathered along the east coast (bordering the Baltic Sea) and west coast of Sweden (bordering the North Sea). Brown algae (Dictyosiphon foenicolaceus) and cyanobacteria (Nodularia spumigena) from the Baltic Sea, considered to be among the primary producers of these compounds, were also analyzed for comparison.

Materials and methods  

The samples were liquid–liquid extracted, separated into a phenolic and a neutral fraction, and subsequently analyzed by gas chromatography–mass spectrometry (GS-MS).

Results and discussion  

The levels of OH-PBDEs, MeO-PBDEs and PBDDs were significantly higher in Baltic Sea mussels than in those from the west coast, whereas the levels of PBPs and PBAs displayed the opposite pattern. The blue mussels from the Baltic Sea contained high levels of all analyzed substances, much higher than the levels of, e.g., polybrominated diphenyl ethers. In addition, the GC-MS chromatogram of the phenolic fraction of the west coast samples was dominated by four unknown peak clusters, three of which were tentatively identified as dihydroxy-PBDEs and the other as a hydroxylated-methyl-tetraBDE.

Conclusions  

Clearly, all of the compounds analyzed are natural products, both in the Baltic and the North Sea. However, the geographical differences in composition may indicate different origin, e.g., due to differences in the occurrence and/or abundance of various algae species along these two coasts or possibly a more extensive dilution on the west coast.

Keyword
OH-PBDE, MeO-PBDE, PBDD, Polybrominated dibenzo-p-dioxins, Natural formation
National Category
Environmental Sciences
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-53032 (URN)10.1007/s11356-010-0331-1 (DOI)
Available from: 2011-01-19 Created: 2011-01-19 Last updated: 2017-12-11Bibliographically approved
2. Temporal Variations of Polybrominated Dibenzo-p-Dioxin and Methoxylated Diphenyl Ether Concentrations in Fish Revealing Large Differences in Exposure and Metabolic Stability
Open this publication in new window or tab >>Temporal Variations of Polybrominated Dibenzo-p-Dioxin and Methoxylated Diphenyl Ether Concentrations in Fish Revealing Large Differences in Exposure and Metabolic Stability
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2010 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 44, no 7, 2466-73 p.Article in journal (Refereed) Published
Abstract [en]

The concentrations of polybrominated dibenzo-p-dioxins (PBDDs) and polybrominated methoxylated diphenyl ethers (MeO-PBDEs) were investigated in perch (Perca fluviatilis) collected from a Baltic Sea background contaminated area between 1990 and 2005. No temporal trend was found, but large variations were observed - up to 5-fold and 160-fold differences in MeO-PBDE and PBDD concentrations, respectively - between consecutive years, suggesting that retention of these compounds, particularly the PBDDs, is limited. Examination of the congener profiles using principal component analysis (PCA) and correlation analysis indicated that MeO-PBDEs without adjacent substituents (6-MeO-BDE47) or with two adjacent substituents (2'-MeO-BDE68 and 6-MeO-BDE90) are retained more than MeO-PBDEs with three adjacent substituents (6-MeO-BDE85 and 6-MeO-BDE99) and that 1,3,6,8-tetraBDD and 1,3,7,9-tetraBDD are retained more than the other PBDDs which have vicinal hydrogen. Debromination could explain the limited retention of 6-MeO-PBDE85 and 6-MeO-BDE99 and the absence of 2-MeO-BDE123 and 6-MeO-BDE137, and cytochrome P-450 mediated oxidation could explain the limited retention of PBDDs containing vicinal hydrogen. The levels of organobromines, especially MeO-PBDEs, were found to covary with water conditions related to primary production, for example temperature, depth visibility, and inorganic nutrient concentrations, which also favor fish productivity. The results suggest natural production of MeO-PBDEs and PBDDs and imply that they fluctuate considerably over time, as do common marine toxins in fish. Thus, assessments of human and environmental risk should consider both the average and peak concentrations of these contaminants in marine biota.

National Category
Environmental Sciences
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-38578 (URN)10.1021/es9038006 (DOI)000275993700039 ()20180550 (PubMedID)
Available from: 2010-04-19 Created: 2010-04-19 Last updated: 2017-12-12Bibliographically approved
3. Seasonal variations of hydroxylated and methoxylated brominated diphenyl ethers in blue mussels from the Baltic Sea
Open this publication in new window or tab >>Seasonal variations of hydroxylated and methoxylated brominated diphenyl ethers in blue mussels from the Baltic Sea
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2011 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 84, no 4, 527-532 p.Article in journal (Refereed) Published
Abstract [en]

Hydroxylated polybrominated diphenyl ethers (OH-PBDEs) and methoxylated polybrominated diphenyl ethers (MeO-PBDEs) found at high levels in the Baltic biota are mainly natural products, but can also be formed through metabolism or abiotic oxidation of polybrominated diphenyl ethers (PBDEs). The formation of OH-PBDEs is of concern since there is growing evidence of phenolic toxicity. This study investigates seasonal variations in levels of OH-PBDEs and MeO-PBDEs, focusing on an exposed species, the blue mussel (Mytilus edulis), sampled in the Baltic Sea in May, June, August and October of 2008. Both the OH-PBDE and MeO-PBDE levels in the mussels showed seasonal variations from May to October, the highest concentration of each congener appearing in June. The seasonal variation was more marked for OH-PBDEs than in MeO-PBDEs, but all congeners showed the same trends, except 6-MeO-BDE47 and 2′-MeO-BDE68, which did not significantly decline in concentrations after June. Biotic or abiotic debromination is suggested as a possible reason for the rapid decrease in methoxylated penta- and hexa-BDE concentrations observed in blue mussels from June to August, while the tetraBDE concentrations were stable. In addition, 1,3,7/1,3,8-tribrominated dibenzo-p-dioxins showed the same seasonal variation. The seasonal variations indicates natural formation and are unlikely to be due to transformation of anthropogenic precursors. The levels of PBDEs were fairly constant over time and considerably lower than those of the OH-PBDEs and MeO-PBDEs. The timing of the peaks in concentrations suggests that filamentous macro-algae may be important sources of these compounds found in the blue mussels from this Baltic Sea location.

Keyword
OH-PBDE, MeO-PBDE, Natural production, Seasonal variations, Debromination
National Category
Earth and Related Environmental Sciences Chemical Sciences
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-53199 (URN)10.1016/j.chemosphere.2011.01.001 (DOI)000292716000024 ()
Available from: 2011-01-20 Created: 2011-01-20 Last updated: 2017-12-11Bibliographically approved
4. Hydroxylated and methoxylated polybrominated diphenyl ethers and polybrominated dibenzo-p-dioxins in algae and blue mussels from the Swedish coast line - patterns and correlations
Open this publication in new window or tab >>Hydroxylated and methoxylated polybrominated diphenyl ethers and polybrominated dibenzo-p-dioxins in algae and blue mussels from the Swedish coast line - patterns and correlations
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(English)Manuscript (preprint) (Other academic)
National Category
Environmental Sciences
Research subject
Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-54407 (URN)
Available from: 2011-02-01 Created: 2011-02-01 Last updated: 2011-02-03Bibliographically approved

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