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Bioavailability of organic contaminants in a changing climate
Umeå University, Faculty of Science and Technology, Department of Chemistry.
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The effects of predicted future climate change was investigated with special emphasis on the association of organic contaminants with dissolved organic carbon (DOC) in the Baltic Sea.

An automated method was developed for the measurements of DOC - water distribution constants at realistic DOC concentrations in brackish water. The method proved to be valid for 30 organic contaminants with different structural elements in the 5 – 100 mg car bon/L DOC concentration range. There were limitations of this method. Firstly, its applicability is limited towards contaminants with lower affinity to DOC. Secondly, at higher (>100 mg carbon/L) DOC concentrations the sorption of contaminants was underest imated.

Afterwards, water samples were collected from 15 points within the Baltic Sea in a north - south gradient t o examine the spatial differences in DOC characteristics and sorption properties . The DOC samples were analyzed using proton nuclear magnetic resonance and ultraviolet spectroscopy. Results from both techniques indicated that the aromatic nature of the DOC pool increased towards the northern Baltic Sea. This was expected as the freshwater inflow has high significance in controlling the hydrograp hic conditions in the Bothnian Bay. Sorption of organic contaminants was subsequently measured in the same samples. The results showed decreased sorption from north to south for hydrophobic contaminants such as chlorinated benzenes but for contaminants lik e tributyl - phosphate no spatial tendencies were observed. The data generated was used to determine molecular descriptors of DOC using linear free energy relationships. The results indicated a higher significance of hy drogen bond donor/acceptor functional g roups of the DOC in the south.

Changes in contaminant distribution were simulated in model pelagic ecosystems at possible endpoints predicted by future climate change scenarios. Separate and combined effects of temperature a nd DOC were studied in mesocosms. The results indicated interesting tendencies. Increased temperature resulted in increased losses in the amounts of organic contaminants. Increased DOC levels promoted sedimentation and sorption of contaminants to particulate matter and biota. Hi gher amounts of contaminants were retained. The combined effects of the two factors led to and overall decrease in dissolved amounts. Higher losses or increased sedimentation and sorption to particles were also observed depending on contaminant properties.

Place, publisher, year, edition, pages
Umeå: Umeå University , 2015. , 82 p.
Keyword [en]
climate change, organic contaminants, sorption, dissolved organic carbon, bioavailability
National Category
Analytical Chemistry Environmental Sciences
Identifiers
URN: urn:nbn:se:umu:diva-98828ISBN: 978-91-7601-220-8 (print)OAI: oai:DiVA.org:umu-98828DiVA: diva2:783854
Public defence
2015-02-20, Södra Hörsalen, KBC Huset, Umeå, 10:00 (English)
Opponent
Supervisors
Projects
EcoChange
Available from: 2015-01-30 Created: 2015-01-27 Last updated: 2015-02-02Bibliographically approved
List of papers
1. Elimination of interferences caused by simultaneous use of deuterated and carbon-13 standards in GC-MS analysis of polycyclic aromatic hydrocarbons (PAHs) in extracts from passive sampling devices
Open this publication in new window or tab >>Elimination of interferences caused by simultaneous use of deuterated and carbon-13 standards in GC-MS analysis of polycyclic aromatic hydrocarbons (PAHs) in extracts from passive sampling devices
2013 (English)In: Analytical Methods, ISSN 1759-9660, E-ISSN 1759-9679, Vol. 5, no 12, 2925-2928 p.Article in journal (Refereed) Published
Abstract [en]

Two types of isotope-labelled reference compounds are typically used for the passive sampling of polycyclic aromatic hydrocarbons. One type is added before the exposure of the sampler and is called a performance reference compound (PRC). The other is the laboratory internal standard, which is spiked into the sample after extraction (dialysis) from the membrane and is used for quantification. Generally, PRCs are deuterium-labelled while internal standards are C-13-labelled. Interference originating from the internal standards occurs when the molecular ions of the PRCs gradually lose deuterium in the ion source to generate fragments that overlap with the molecular ions of the C-13-labelled internal standards. This can cause significant systematic errors in quantification. Gas chromatography-high resolution time-of-flight mass spectrometry (GC-HRTOF-MS) was used to investigate the degree of interference at varying virtual resolutions of the MS instrument, and it was shown that many of the spectral interferences can be avoided by using high MS resolutions (35 000 or better).

National Category
Analytical Chemistry
Identifiers
urn:nbn:se:umu:diva-76820 (URN)10.1039/c3ay40419f (DOI)000319819000003 ()
Available from: 2013-07-15 Created: 2013-07-15 Last updated: 2017-08-31Bibliographically approved
2. Automated method for determination of dissolved organic carbon–water distribution constants of structurally diverse pollutants using pre-equilibrium solid-phase microextraction
Open this publication in new window or tab >>Automated method for determination of dissolved organic carbon–water distribution constants of structurally diverse pollutants using pre-equilibrium solid-phase microextraction
2015 (English)In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 34, no 2, 266-274 p.Article in journal (Refereed) Published
Abstract [en]

Dissolved organic carbon (DOC) plays a key role in determining the environmental fate of semivolatile organic environmental contaminants. The goal of the present study was to develop a method using commercially available hardware to rapidly characterize the sorption properties of DOC in water samples. The resulting method uses negligible-depletion direct immersion solid-phase microextraction (SPME) and gas chromatography–mass spectrometry. Its performance was evaluated using Nordic reference fulvic acid and 40 priority environmental contaminants that cover a wide range of physicochemical properties. Two SPME fibers had to be used to cope with the span of properties, 1 coated with polydimethylsiloxane and 1 coated with polystyrene divinylbenzene polydimethylsiloxane, for nonpolar and semipolar contaminants, respectively. The measured DOC–water distribution constants showed reasonably good reproducibility (standard deviation ≤ 0.32) and good correlation (R2 = 0.80) with log octanol–water partition coefficients for nonpolar persistent organic pollutants. The sample pretreatment is limited to filtration, and the method is easy to adjust to different DOC concentrations. These experiments also utilized the latest SPME automation that largely decreases total cycle time (to 20 min or shorter) and increases sample throughput, which is advantageous in cases when many samples of DOC must be characterized or when the determinations must be performed quickly, for example, to avoid precipitation, aggregation, and other changes of DOC structure and properties. The data generated by this method are valuable as a basis for transport and fate modeling studies.

Keyword
pre-equilibrium solid-phase microextraction, dissolved organic carbon–water distribution constant, organic contaminant
National Category
Organic Chemistry
Identifiers
urn:nbn:se:umu:diva-98927 (URN)10.1002/etc.2805 (DOI)000348994200007 ()25393710 (PubMedID)
Available from: 2015-01-28 Created: 2015-01-28 Last updated: 2017-08-31Bibliographically approved
3. Dissolved organic carbon quality and sorption of organic pollutants in the Baltic Sea in light of future climate change
Open this publication in new window or tab >>Dissolved organic carbon quality and sorption of organic pollutants in the Baltic Sea in light of future climate change
Show others...
2015 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 3, 1445-1452 p.Article in journal (Refereed) Published
Abstract [en]

Regional climate change scenarios predict increased temperature and precipitation in the northern Baltic Sea, leading to a greater runoff of fresh water and terrestrial dissolved organic carbon (DOC) within the second part of the 21st century. As a result, the current north to south gradient in temperature and salinity is likely to be shifted further toward the south. To examine if such climate change effects would cause alterations in the environmental fate of organic pollutants, spatial variations of DOC quality and sorption behavior toward organic contaminants were examined using multiple analytical methods. The results showed declining contents of aromatic functional groups in DOC along a north to south gradient. Similarly, the sorption of a diverse set of organic contaminants to DOC also showed spatial differences. The sorption behavior of these contaminants was modeled using poly parameter linear energy relationships. The resulting molecular descriptors indicated clear differences in the sorption properties of DOC sampled in northern and southern parts of the Baltic Sea, which imply that more organic contaminants are sorbed to DOC in the northern part. The extent of this sorption process determines whether individual contaminants will partition to biota via direct uptake or through sorption to DOC, which serves as food source for bacteria-based food-webs.

National Category
Chemical Sciences Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-98929 (URN)10.1021/es504437s (DOI)000349060300026 ()
Available from: 2015-01-28 Created: 2015-01-28 Last updated: 2017-08-31Bibliographically approved
4. Effects of predicted climatic changes on fates of organic contaminants in brackish water mesocosms
Open this publication in new window or tab >>Effects of predicted climatic changes on fates of organic contaminants in brackish water mesocosms
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(English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026Article in journal (Refereed) Accepted
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-98931 (URN)
Available from: 2015-01-28 Created: 2015-01-28 Last updated: 2017-08-31
5. Projected future climate change and Baltic Sea ecosystem management
Open this publication in new window or tab >>Projected future climate change and Baltic Sea ecosystem management
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2015 (English)In: Ambio, ISSN 0044-7447, E-ISSN 1654-7209, Vol. 44, no Suppl 3, S345-S356 p.Article in journal (Refereed) Published
Abstract [en]

Climate change is likely to have large effectson the Baltic Sea ecosystem. Simulations indicate 2–4 Cwarming and 50–80 % decrease in ice cover by 2100.Precipitation may increase *30 % in the north, causingincreased land runoff of allochthonous organic matter(AOM) and organic pollutants and decreased salinity.Coupled physical–biogeochemical models indicate that, inthe south, bottom-water anoxia may spread, reducing codrecruitment and increasing sediment phosphorus release,thus promoting cyanobacterial blooms. In the north,heterotrophic bacteria will be favored by AOM, whilephytoplankton production may be reduced. Extra trophiclevels in the food web may increase energy losses andconsequently reduce fish production. Future managementof the Baltic Sea must consider the effects of climatechange on the ecosystem dynamics and functions, as wellas the effects of anthropogenic nutrient and pollutant load.Monitoring should have a holistic approach, encompassingboth autotrophic (phytoplankton) and heterotrophic (e.g.,bacterial) processes.

Place, publisher, year, edition, pages
Springer, 2015
Keyword
Climate change, Allochthonous organic matter, Primary production, Bacterial production, Food web, Monitoring
National Category
Chemical Sciences Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-98932 (URN)10.1007/s13280-015-0654-8 (DOI)000362290800003 ()26022318 (PubMedID)
Note

Supplement: 3 Special Issue: SI

Available from: 2015-01-28 Created: 2015-01-28 Last updated: 2017-10-24Bibliographically approved

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