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Sources, emissions, and occurrence of chlorinated paraffins in Stockholm, Sweden
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
2010 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Chlorinated paraffins (CPs) are ubiquitous environmental contaminants. They fulfill all of the criteria (persistent, toxic, and subject to long-range transport) for persistent organic pollutants (POPs) according to the United Nations Economic Commission for Europe (UNECE). CPs are also under consideration for inclusion in the Stockholm Convention on POPs. Their presence has been shown in various environmental matrices in the industrialized parts of the world, as well as in remote regions such as the Arctic.

The aim of this thesis was to increase the limited knowledge of the presence of CPs in the environment, their sources to the environment, and the resulting human exposure. An analytical procedure for the determination of CPs in environmental samples based on gas chromatography coupled to electron capture detection (GC-ECD) has been developed. GC-ECD is a relatively inexpensive instrument that is fast and easy to operate. These advantages open up the possibility for a comprehensive screening of the occurrence of CPs in the environment, including developing countries.

Furthermore, the occurrence of CPs in ambient air and in indoor air and dust was studied. Elevated CP concentrations in indoor air (<5-210 ng/m3) were observed compared to ambient air (0.7-33 ng/m3), which is indicative of the presence of indoor emission sources. Indoor air and dust concentrations were used to estimate the human exposure to CPs via the indoor environment. Comparison of the estimates to available dietary intake estimates indicated that the indoor exposure pathways are not negligible.

CP concentrations in ambient air from urban Stockholm were higher than in rural Aspvreten, Sweden. This indicates the presence of additional (emission) sources in urban areas compared to rural sites. Additionally, a seasonal variation of air concentrations was observed at both locations, suggesting temperature dependent emission sources for CPs. These observations were supported by a substance flow analysis of CPs performed for Stockholm. This study estimated the major emission sources of CPs to the Stockholm environment to be emissions from painted surfaces and in-place sealants.

Place, publisher, year, edition, pages
Stockholm: Department of Applied Environmental Science, Stockholm University , 2010. , 53 p.
Keyword [en]
Chlorinated paraffins, CPs, polychlorinated n-alkanes, PCAs, Air, Dust, Analysis, Exposure, Emissions
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-43559ISBN: 978-91-7447-162-5 (print)OAI: oai:DiVA.org:su-43559DiVA: diva2:357952
Public defence
2010-11-26, De Geersalen, Geovetenskapens hus, Svante Arrhenius väg 14, 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 2: Manuscript. Paper 3: Manuscript. Paper 4: Manuscript.Available from: 2010-11-03 Created: 2010-10-20 Last updated: 2011-12-27Bibliographically approved
List of papers
1. Photolytic clean-up of biological samples for gas chromatographic analysis of chlorinated paraffins
Open this publication in new window or tab >>Photolytic clean-up of biological samples for gas chromatographic analysis of chlorinated paraffins
2004 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 54, no 8, 1079-1083 p.Article in journal (Refereed) Published
Abstract [en]

A method based on gas chromatography electron capture detection (GC-ECD) for the analysis of chlorinatedparaffins (CPs) in biological samples has been investigated. The method includes photolytic destruction of halogenatedaromatic compounds, such as PCBs, to eliminate some of the interferences in the analysis of CPs in environmental samples. Gel permeation chromatography was used to isolate CPs from the interfering components of Toxaphene andchlordane after the photolysis. GC-ECD gave a detection limit of 20 ng CPs/g fresh muscle tissue. The recovery of CPsfrom a spiked moose liver sample was estimated to 94%.

Keyword
Chlorinated paraffins, CPs, Analysis, Photolysis
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-43397 (URN)10.1016/j.chemosphere.2003.10.030 (DOI)
Available from: 2010-10-11 Created: 2010-10-11 Last updated: 2017-12-12Bibliographically approved
2. Emissions of chlorinated paraffins in Stockholm: A substance flow analysis study
Open this publication in new window or tab >>Emissions of chlorinated paraffins in Stockholm: A substance flow analysis study
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Chlorinated paraffins (CPs) are currently under consideration for classi-fication as persistent organic pollutants. They have been extensively used for many decades in a wide range of applications, particularly in industrial lubricants and building materials. However, very little is known about their levels in the technosphere or about the origins and quantities of their emission into the environment. In this study, sub-stance flow analysis was used to estimate CP emissions from the city of Stockholm, Sweden to different environmental media. The results indi-cate that 16 tonnes of CPs are added to the technosphere in Stockholm annually, and that approximately 0.5 tonnes are emitted to air and wa-ter annually. The estimated emissions to air and water were in reasona-ble agreement with independent emission estimates derived from envi-ronmental monitoring data. The emissions are not directly linked to the annual inflow; instead, they largely originate from the large quantity of CPs that have accumulated in the technosphere over many years. The main sources of the emissions are in-place paints and sealants. The vast majority of the CPs are expected to leave the technosphere as solid waste, but there are uncertainties regarding subsequent CP emissions from solid waste into the environment.

Keyword
Chlorinated paraffins, CPs, substance flow analysis, emissions
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-43557 (URN)
Available from: 2010-10-20 Created: 2010-10-20 Last updated: 2010-10-22Bibliographically approved
3. Chlorinated paraffins in indoor air and dust: Concentrations, congener patterns, and human exposure
Open this publication in new window or tab >>Chlorinated paraffins in indoor air and dust: Concentrations, congener patterns, and human exposure
2011 (English)In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 37, no 7, 1169-1174 p.Article in journal (Refereed) Published
Abstract [en]

Chlorinated paraffins (CPs) are large production volume chemicals used in a wide variety of commercial applications. They are ubiquitous in the environment and humans. Human exposure via the indoor environment has, however, been barely investigated. In the present study 44 indoor air and six dust samples from apartments in Stockholm, Sweden, were analyzed for CPs. and indoor air concentrations are reported for the first time. The sumCP concentration (short chain CPs (SCCPs) and medium chain CPs (MCCPs)) in air ranged from <5-210 ng m(-3) as quantified by gas chromatography coupled to electron ionization tandem mass spectrometry (GC/EI-MS/MS). Congener group patterns were studied using GC with electron capture negative ionization MS (GC/ECNI-MS). The air samples were dominated by the more volatile SCCPs compared to MCCPs. SumCPs were quantified by GC/EI-MS/MS in the dust samples at low mu g g(-1) levels, with a chromatographic pattern suggesting the prevalence of longer chain CPs compared to air. The median exposure to sumCPs via the indoor environment was estimated to be similar to 1 mu g day(-1) for both adults and toddlers. Adult exposure was dominated by inhalation, while dust ingestion was suggested to be more important for toddlers. Comparing these results to literature data on dietary intake indicates that human exposure to CPs from the indoor environment is not negligible.

Keyword
Chlorinated paraffins (CPs), Polychlorinated n-alkanes (PCAs), Indoor environment, Air, Dust, Human exposure
National Category
Natural Sciences
Identifiers
urn:nbn:se:su:diva-66519 (URN)10.1016/j.envint.2011.04.002 (DOI)000293727900003 ()
Note
authorCount :3Available from: 2011-12-27 Created: 2011-12-20 Last updated: 2017-12-08Bibliographically approved
4. Chlorinated paraffins in the Swedish atmosphere: spatial and seasonal variability
Open this publication in new window or tab >>Chlorinated paraffins in the Swedish atmosphere: spatial and seasonal variability
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Chlorinated paraffins (CPs) are ubiquitous environmental contaminants of concern, as indicated by the recent addition of the short-chained CPs as a new Persistent Organic Pollutant (POP) in the United Nations Eco-nomic Commission for Europe (UNECE) Convention on Long-Range Transboundary Air Pollution (CLRTAP) (United Nations, 2010). Howev-er, knowledge about the occurrence of CPs in the environment, and in the atmosphere in particular, is limited. To address this, ambient air samples were collected over a 10 month period at an urban site and a rural site in Sweden, and analyzed for the sum of the short-chained, me-dium-chained and long-chained CPs. The CP concentrations ranged from 0.7-33 ng/m3, and they were significantly higher at the urban site. The low volatile CP congeners dominated in the samples, and this domin-ance was more pronounced at the urban site. Particle-bound and ga-seous CPs were determined separately in several samples, and between 50 and 90 % of the CPs were estimated to be in the gas phase. A clear seasonality in the concentrations was observed, with levels in summer that were about 5 times higher than in winter. This indicates that tem-perature dependent emission from urban sources is a major source of the CPs in air. Diffusive emissions from building materials are likely to make a major contribution.

Keyword
Chlorinated paraffins, CPs, polychlorinated n-alkanes, PCAs, air
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-43556 (URN)
Available from: 2010-10-20 Created: 2010-10-20 Last updated: 2010-10-22Bibliographically approved

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