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Occurrence and fate of emerging and legacy flame retardants: from indoor environments to remote areas
Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. (MIX)
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Persistent organic pollutants (POPs) are toxic chemicals that can be found in various matrices in all corners of the planet, including remote areas such as the Arctic.  Several POPs are known and monitored but given the abundance of new chemicals in commerce about which little is known, chemicals that may be new POPs are constantly being screened for. The use of flame retardants, particularly brominated flame retardants (BFRs), has been increasing for decades. PBDEs and HBCDDs are two types of BFRs that have historically been used in large volumes but recently faced legislative restrictions. However, in order to meet fire safety standards, these BFRs have been replaced by a variety of emerging flame retardants (EFRs) about which little is known especially concerning their toxicity, production volumes, and environmental behavior. The main purpose of this thesis was to investigate the occurrence and fate in indoor and outdoor environments of several EFRs and compare them with PBDEs, HBCDDs, and legacy POPs.

Several indoor environments in the city of Stockholm, Sweden were sampled for dust, indoor air, and ventilation system air (Paper II).  Results from these samples revealed a number of EFRs that humans are exposed to and that are emitted from buildings through ventilation systems. These included DDC-CO, DBE-DBCH, PBT, HBB, EHTBB, and BEH-TEBP. PBDE levels seem to be declining compared to previous studies in Stockholm.  Outdoor air and soil were sampled across transects of Stockholm (Paper II) and Birmingham, United Kingdom (Paper III).  Results from these samples showed the presence of many of the same EFRs in the outdoor environment that were found in indoor environments.  Urban pulses in air were discovered for PBDEs in both cities and for some EFRs in Stockholm, indicating that the cities are sources of EFRs to the outdoor environment.  Atmospheric deposition samples were taken at two sites in northern Sweden (Paper I).  Three EFRs (DDC-CO, DBE-DBCH, and BTBPE) and two current-use pesticides (trifluralin and chlorothalonil) were identified, indicating these compounds’ potential for long range transport and global contamination.  Other legacy POPs such as HCH, PCBs, and PBDEs were measured in the deposition samples as well.  The bulk of deposition was comprised of HCH and PCBs with only minor contributions from PBDEs, chlordanes, and emerging compounds.  Finally, passive and active air sampling methods were compared for BFRs in offices in Beijing, China.  Some EFRs were identified in indoor air from China; however, BDE-209 was the most predominant compound found (Paper IV).  Air samples collected with passive samplers generally had measured FR concentrations within a factor of 2-3 of those collected with active samplers. The use of a GFF in the passive samplers resulted in concentrations of particle-bound contaminants such as BDE-209 that were more comparable to those in active samples. The positioning of the PUF in the passive samplers affected the sampling rates for gaseous compounds and particle retention on PUFs was shown to be a large source of uncertainty in passive sampling.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science and Analytical Chemistry, Stockholm University , 2015. , 34 p.
Keyword [en]
Flame retardant, emerging, legacy, polybrominated diphenyl ethers, PBDE, HBCDD, long range transport, dust, air, soil, atmospheric deposition
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-116443ISBN: 978-91-7649-132-4 (print)OAI: oai:DiVA.org:su-116443DiVA: diva2:806433
Public defence
2015-05-29, William-Olssonsalen, Geovetenskapens hus, Svante Arrhenius Väg 14, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
EU, FP7, Seventh Framework Programme, 264600
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: Manuscript. Paper 4: Manuscript.

 

Available from: 2015-05-06 Created: 2015-04-20 Last updated: 2015-06-24Bibliographically approved
List of papers
1. Atmospheric deposition of persistent organic pollutants and chemicals of emerging concern at two sites in northern Sweden
Open this publication in new window or tab >>Atmospheric deposition of persistent organic pollutants and chemicals of emerging concern at two sites in northern Sweden
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2014 (English)In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 16, no 2, 298-305 p.Article in journal (Refereed) Published
Abstract [en]

Bimonthly bulk atmospheric deposition samples (precipitation + dry particle) were taken for one year at an arctic (Abisko, 68°20’ N, 19°03’ E) and a sub-arctic (Krycklan 64°14’N, 19°46’E ) location in northern Sweden using Amberlite IRA- 743 as an absorbent for hydrophobic pollutants. The samples were analyzed by gas chromatography – high resolution mass spectrometry (GC-HRMS) for polychlorinated biphenyls (PCBs), legacy organochlorine pesticides (OCPs = hexachlorocyclohexanes and chlordane-related compounds), polybrominated diphenyl ethers (PBDEs) and emerging chemicals.  Higher deposition rates of most compounds were observed at the more northern site despite its receiving less precipitation and being more remote.  HCHs and PCBs made up the bulk of the total deposition at both sites.  Five emerging chemicals were detected: the current-use pesticides trifluralin and chlorothalonil; and non-BDE flame retardants 1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane (TBECH), 1,2-bis (2,4,6-tribromophenoxy) ethane (BTBPE), and Dechlorane Plus (DP).  A decrease in the fraction of the anti isomer of DP was observed at the arctic site, indicating isomer-selective degradation or isomerization during long range transport.  Air parcel back trajectories revealed a greater influence from air originating over the ocean at the more northern site. The differences in these air sources were reflected in higher ΣHCH to ΣPCB ratios compared to the more southern site, as HCHs are related to volatilization from the ocean and Abisko is located <100 km from the Norwegian coast, while PCBs are emitted from continental sources.

Keyword
Persistent organic pollutants, atmospheric deposition, emerging chemicals, flame retardants, pesticides, PCB
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-100210 (URN)10.1039/C3EM00590A (DOI)000331504100014 ()
Note

Funding agencies:

Swedish Research Council Formas, 2007-1454; Foundation in Memory of Oscar and Lili Lamm; European Union, 264600; European Community; International Incoming Fellowships, 252025; ECOCHANGE program of the Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning; Umea University 

Available from: 2014-01-29 Created: 2014-01-29 Last updated: 2017-12-06Bibliographically approved
2. Emerging Flame Retardants, PBDEs, and HBCDDs in Indoor and Outdoor Media in Stockholm, Sweden
Open this publication in new window or tab >>Emerging Flame Retardants, PBDEs, and HBCDDs in Indoor and Outdoor Media in Stockholm, Sweden
2015 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 5, 2912-2920 p.Article in journal (Refereed) Published
Abstract [en]

Dust, indoor air, outgoing air from ventilation systems, outdoor air, and soil were sampled in and around Stockholm, Sweden during the winter and spring 2012. The concentrations of several emerging flame retardants (EFRs), polybrominated diphenyl ethers (PBDEs), and isomers of hexabromocyclododecane (HBCDD) were measured. The most commonly found EFR was 1,2-dibromo-4-(1,2 dibromoethyl)cyclohexane (TBECH or DBE-DBCH), which was found in nearly all indoor, ventilation, and outdoor air samples, most dust samples, but not in soil samples. Other frequently detected EFRs included pentabromotoluene (PBT), hexabromobenzene (HBB), 2,3,4,5-tetrabromo-ethylhexylbenzoate (EHTBB), 2,3,4,5-tetrabromo-bis(2-ethylhexyl) phthalate (BEH-TEBP), and decabromodiphenyl ethane (DBDPE). PBDE concentrations were significantly lower in air and dust samples compared to a previous study in Stockholm. In outdoor air, DBE-DBCH, PBT, EHTBB, DBDPE, and PBDEsshowed an “urban pulse” with concentrations increasing as samples were taken in more urban areas compared to rural areas. These EFRs show similar environmental behavior asPBDEs. Higher brominated BDEs showed this same urban pulse in soil but lower brominated BDEs did not. Air–soil fugacity fractions were calculated, and these indicated that most compounds are undergoing net deposition from atmosphere to soil, with the higher brominated PBDEs furthest from equilibrium.

Keyword
flame retardants, emerging, polybrominated diphenyl ethers, PBDE, HBCD, dust, indoor air, outdoor air, soil, ventilation
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-115805 (URN)10.1021/es505946e (DOI)000350611100043 ()
Funder
EU, FP7, Seventh Framework Programme, 264600
Available from: 2015-04-01 Created: 2015-04-01 Last updated: 2017-12-04Bibliographically approved
3. Concentrations of legacy and emerging flame retardants in air and soil on a rural-urban transect in the UK West Midlands
Open this publication in new window or tab >>Concentrations of legacy and emerging flame retardants in air and soil on a rural-urban transect in the UK West Midlands
2016 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 148, 195-203 p.Article in journal (Refereed) Published
Abstract [en]

Passive air samples were collected monthly for 6 months from 8 sites along a transect of Birmingham, United Kingdom between June 2012 and January 2013. Soil samples were collected once at each site. Average concentrations of BDE-209, ΣPBDEs17:183 and ΣPBDEs in ambient air were 150, 49, and 180 pg m−3, respectively. Atmospheric concentrations of PBDEs were negatively correlated with distance from the city centre, exhibiting an “urban pulse”. The average ΣHBCDD air concentration was 100 pg m−3, however concentrations were not correlated with distance from the city centre. Several emerging flame retardants (EFRs) were identified in air and/or soil samples: 2,3,4,5-tetrabromo-bis(2-ethylhexyl) phthalate (BEH-TEBP), 1,2-dibromo-4-(1,2 dibromoethyl)cyclohexane (TBECH or DBE-DBCH), allyl 2,4,6-tribromophenyl ether (ATE), 2-bromoallyl 2,4,6-tribromophenyl ether (BATE), decabromodiphenyl ethane (DBDPE), and dechlorane plus (DP or DDC-CO). Average concentrations of BDE-209, ΣPBDEs17:183 and ΣPBDEs in soil were 11, 3.6, and 15 ng g−1 soil organic matter. PBDE concentrations in soil were higher at sites closest to the city centre, however correlations with distance from the city centre were not significant. BDEs-47 and -99 contributed more to ΣPBDEs in soil samples than air samples, but in both, the predominant congener was BDE-209. BATE was more abundant in air than soil but ATE was abundant in soil but not air.

Keyword
PBDEs, HBCDD, HBCD, EFRs, Air, Soil
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-116506 (URN)10.1016/j.chemosphere.2016.01.034 (DOI)000371099700023 ()
Funder
EU, FP7, Seventh Framework Programme, 264600NERC - the Natural Environment Research Council, NE/G01146X/1
Available from: 2015-04-21 Created: 2015-04-21 Last updated: 2017-12-04Bibliographically approved
4. Comparisons of indoor active and passive air sampling methods for emerging and legacy halogenated flame retardants in Beijing, China offices
Open this publication in new window or tab >>Comparisons of indoor active and passive air sampling methods for emerging and legacy halogenated flame retardants in Beijing, China offices
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(English)Manuscript (preprint) (Other academic)
Keyword
air sampling, semi-volatile, passive, active, flame retardant, emerging, polybrominated diphenyl ether, BDE-209
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-116507 (URN)
Funder
EU, FP7, Seventh Framework Programme, 264600
Available from: 2015-04-21 Created: 2015-04-21 Last updated: 2016-01-29Bibliographically approved

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