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  • 1.
    Bidleman, Terry
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Agosta, Kathleen
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Andersson, Agneta
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Brorström-Lundén, Eva
    Haglund, Peter
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Hansson, Katarina
    Laudon, Hjalmar
    Newton, Seth
    Nygren, Olle
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Ripszam, Matyas
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Wiberg, Karin
    Atmospheric pathways of chlorinated pesticides and natural bromoanisoles in the northern Baltic Sea and its catchment2015In: Ambio, ISSN 0044-7447, E-ISSN 1654-7209, Vol. Suppl 3, no 44, p. 472-483Article in journal (Refereed)
    Abstract [en]

    Long-range atmospheric transport is a major pathway for delivering persistent organic pollutants to the oceans. Atmospheric deposition and volatilization of chlorinated pesticides and algae-produced bromoanisoles (BAs) were estimated for Bothnian Bay, northern Baltic Sea, based on air and water concentrations measured in 2011-2012. Pesticide fluxes were estimated using monthly air and water temperatures and assuming 4 months ice cover when no exchange occurs. Fluxes were predicted to increase by about 50 % under a 2069-2099 prediction scenario of higher temperatures and no ice. Total atmospheric loadings to Bothnian Bay and its catchment were derived from air-sea gas exchange and "bulk'' (precipitation ? dry particle) deposition, resulting in net gains of 53 and 46 kg year(-1) for endosulfans and hexachlorocyclohexanes, respectively, and net loss of 10 kg year(-1) for chlordanes. Volatilization of BAs releases bromine to the atmosphere and may limit their residence time in Bothnian Bay. This initial study provides baseline information for future investigations of climate change on biogeochemical cycles in the northern Baltic Sea and its catchment.

  • 2.
    Bidleman, Terry F.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Letter to the Editor regarding 'Celebrating Bidleman's 1988 "Atmospheric Processes"2015In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 5, p. 2586-2586Article in journal (Refereed)
  • 3.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Agosta, Kathleen
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Andersson, Agneta
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Haglund, Peter
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Liljelind, Per
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Hegmans, Alyse
    Jantunen, Liisa M.
    Nygren, Olle
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Poole, Justen
    Ripszam, Matyas
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Sea-air exchange of bromoanisoles and methoxylated bromodiphenylethers in the Northern Baltic2016In: Marine Pollution Bulletin, ISSN 0025-326X, E-ISSN 1879-3363, Vol. 112, no 1-2, p. 58-64Article in journal (Refereed)
    Abstract [en]

    Halogenated natural products in biota of the Baltic Sea include bromoanisoles (BAs) and methoxylated bromodiphenyl ethers (MeO-BDEs). We identified biogenic 6-MeO-BDE47 and 2'-MeO-BDE68 in Baltic water and air for the first time using gas chromatography - high resolution mass spectrometry. Partial pressures in air were related to temperature by: log p/Pa=m/T(K)+b. We determined Henry's law constants (HLCs) of 2,4-dibromoanisole (2,4-DiBA) and 2,4,6-tribromoanisole (2,4,6-TriBA) from 5 to 30°C and revised our assessment of gas exchange in the northern Baltic. The new water/air fugacity ratios (FRs) were lower, but still indicated net volatilization in May-June for 2,4-DiBA and May - September for 2,4,6-TriBA. The net flux (negative) of BAs from Bothnian Bay (38,000km2) between May - September was revised from -1319 to -532kg. FRs of MeO-BDEs were >1, suggesting volatilization, although this is tentative due to uncertainties in their HLCs and binding to dissolved organic carbon.

  • 4.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Agosta, Kathleen
    Andersson, Agneta
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Haglund, Peter
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Nygren, Olle
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Ripszam, Matyas
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Air-water exchange of brominated anisoles in the northern baltic sea2014In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 48, no 11, p. 6124-6132Article in journal (Refereed)
    Abstract [en]

    Bromophenols produced by marine algae undergo O-methylation to form bromoanisoles (BAs), which are exchanged between water and air. BAs were determined in surface water of the northern Baltic Sea (Gulf of Bothnia, consisting of Bothnian Bay and Bothnian Sea) during 2011-2013 and on a transect of the entire Baltic in September 2013. The abundance decreased in the following order: 2,4,6-tribromoanisole (2,4,6-TBA) > 2,4-dibromoanisole (2,4-DBA) ≫ 2,6-dibromoanisole (2,6-DBA). Concentrations of 2,4-DBA and 2,4,6-TBA in September were higher in the southern than in the northern Baltic and correlated well with the higher salinity in the south. This suggests south-to-north advection and dilution with fresh riverine water enroute, and/or lower production in the north. The abundance in air over the northern Baltic also decreased in the following order: 2,4,6-TBA > 2,4-DBA. However, 2,6-DBA was estimated as a lower limit due to breakthrough from polyurethane foam traps used for sampling. Water/air fugacity ratios ranged from 3.4 to 7.6 for 2,4-DBA and from 18 to 94 for 2,4,6-TBA, indicating net volatilization. Flux estimates using the two-film model suggested that volatilization removes 980-1360 kg of total BAs from Bothnian Bay (38000 km(2)) between May and September. The release of bromine from outgassing of BAs could be up to 4-6% of bromine fluxes from previously reported volatilization of bromomethanes and bromochloromethanes.

  • 5.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Andersson, Agneta
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences. Umeå University, Faculty of Science and Technology, Umeå Marine Sciences Centre (UMF).
    Brugel, Sonia
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences. Umeå University, Faculty of Science and Technology, Umeå Marine Sciences Centre (UMF).
    Ericson, Lars
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Haglund, Peter
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Kupryianchyk, Darya
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Lau, Danny C. P.
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Liljelind, Per
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Lundin, Lisa
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Tysklind, Anders
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Bromoanisoles and Methoxylated Bromodiphenyl Ethers in Macroalgae from Nordic Coastal Regions2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, p. 881-892Article in journal (Refereed)
    Abstract [en]

    Marine macroalgae are used worldwide for human consumption, animal feed, cosmetics and agriculture. In addition to beneficial nutrients, macroalgae contain halogenated natural products (HNPs), some of which have toxic properties similar to those of well-known anthropogenic contaminants. Sixteen species of red, green and brown macroalgae were collected in 2017–2018 from coastal waters of the northern Baltic Sea, Sweden Atlantic and Norway Atlantic, and analyzed for bromoanisoles (BAs) and methoxylated bromodiphenyl ethers (MeO-BDEs). Target compounds were quantified by gas chromatography-low resolution mass spectrometry (GC-LRMS), with qualitative confirmation in selected species by GC-high resolution mass spectrometry (GC-HRMS). Quantified compounds were 2,4-diBA, 2,4,6-triBA, 2′-MeO-BDE68, 6-MeO-BDE47, and two tribromo-MeO-BDEs and one tetrabromo-MeO-BDE with unknown bromine substituent positions. Semiquantitative results for pentabromo-MeO-BDEs were also obtained for a few species by GC-HRMS. Three extraction methods were compared; soaking in methanol, soaking in methanol–dichloromethane, and blending with mixed solvents. Extraction yields of BAs did not differ significantly (p > 0.05) with the three methods and the two soaking methods gave equivalent yields of MeO-BDEs. Extraction efficiencies of MeO-BDEs were significantly lower using the blend method (p < 0.05). For reasons of simplicity and efficiency, the soaking methods are preferred. Concentrations varied by orders of magnitude among species: ∑2BAs 57 to 57 700 and ∑5MeO-BDEs < 10 to 476 pg g−1 wet weight (ww). Macroalgae standing out with ∑2BAs >1000 pg g−1 ww were Ascophyllum nodosumCeramium tenuicorneCeramium virgatumFucus radicansFucus serratusFucus vesiculosusSaccharina latissimaLaminaria digitata, and Acrosiphonia/Spongomorpha sp. Species A. nodosumC. tenuicorneChara virgataF. radicans and F. vesiculosus (Sweden Atlantic only) had ∑5MeO-BDEs >100 pg g−1ww. Profiles of individual compounds showed distinct differences among species and locations.

  • 6.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Brorström-Lundén, Eva
    Hansson, Katarina
    Laudon, Hjalmar
    Nygren, Olle
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Atmospheric transport and deposition of bromoanisoles along a temperate to arctic gradient2017In: Environmental Science and Technology, ISSN 1086-931X, E-ISSN 1520-6912, Vol. 51, no 19, p. 10974-10982Article in journal (Refereed)
    Abstract [en]

    Bromoanisoles (BAs) arise from O-methylation of bromophenols, produced by marine algae and invertebrates. BAs undergo sea-air exchange and are transported over the oceans. Here we report 2,4-DiBA and 2,4,6-TriBA in air and deposition on the Swedish west coast (Råö) and the interior of arctic Finland (Pallas). Results are discussed in perspective with previous measurements in the northern Baltic region in 2011−2013. BAs in air decreased from south to north in the order Råö > northern Baltic > Pallas. Geometric mean concentrations at Pallas increased significantly (p < 0.05) between 2002 and 2015 for 2,4-DiBA but not for 2,4,6-TriBA. The logarithm of BA partial pressures correlated significantly to reciprocal air temperature at the coastal station Råö and over the Baltic, but only weakly (2,4-DiBA) or not significantly (2,4,6-TriBA) at inland Pallas. Deposition fluxes of BAs were similar at both sites despite lower air concentrations at Pallas, due to greater precipitation scavenging at lower temperatures. Proportions of the two BAs in air and deposition were related to Henry’s law partitioning and source regions. Precipitation concentrations were 10−40% of those in surface water of Bothnian Bay, northern Baltic Sea. BAs deposited in the bay catchment likely enter rivers and provide an unexpected source to northern estuaries. BAs may be precursors to higher molecular weight compounds identified by others in Swedish inland lakes.

  • 7.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Jantunen, L. M
    Hung, H
    Ma, J
    Stern, G. A.
    Rosenberg, B
    Racine, J
    Biannual cycles of organochlorine pesticide enantiomers in arctic air suggest changing sources and pathways2014In: Atmospheric Chemistry and Physics Discussions, ISSN 1680-7367, E-ISSN 1680-7375, Vol. 14, no 17, p. 25027-25050Article in journal (Refereed)
    Abstract [en]

    Air samples collected during 1994–2000 at the Canadian arctic air monitoring stationAlert (82300 N, 62200 W) were analyzed by enantiospecific gas chromatography –mass spectrometry for -hexachlorocyclohexane (-HCH), trans-chlordane (TC) and5 cis-chlordane (CC). Results were expressed as enantiomer fractions (EF = quantitiesof (+)/[(+)+(−)] enantiomers), where EFs=0.5, < 0.5 and > 0.5 indicate racemic composition,and preferential depletion of (+) and (−) enantiomers, respectively. Long-termaverage EFs were close to racemic values for -HCH (0.504±0.004, n =197) andCC (0.505±0.004, n =162), and deviated farther from racemic for TC (0.470±0.013,10 n =165). Digital filtration analysis revealed biannual cycles of lower -HCH EFs insummer-fall and higher EFs in winter-spring. These cycles suggest volatilization ofpartially degraded -HCH with EF < 0.5 from open water and advection to Alert duringthe warm season, and background transport of -HCH with EF> 0.5 during the coldseason. The contribution of sea-volatilized -HCH was only 11% at Alert, vs. 32%15 at Resolute Bay (74.68 N, 94.90W) in 1999. EFs of TC also followed biannual cyclesof lower and higher values in the warm and cold seasons. These were in phasewith low and high cycles of the TC/CC ratio (expressed as FTC =TC/(TC+CC)), whichsuggests greater contribution of microbially “weathered” TC in summer-fall vs. winterspring.CC was closer to racemic than TC and displayed seasonal cycles only in 1997–20 1998. EF profiles are likely to change with rising contribution of secondary emissionsources, weathering of residues in the environment, and loss of ice cover in the Arctic.Enantiomer-specific analysis could provide added forensic capability to air monitoringprograms.

  • 8.
    Bidleman, Terry F
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Jantunen, Liisa M
    Kurt‐Karakus, Perihan Binnur
    Wong, Fiona
    Chiral persistent organic pollutants as tracers of atmospheric sources and fate: review and prospects for investigating climate change influences2012In: Atmospheric Pollution Research, ISSN 1309-1042, Vol. 3, no 4, p. 371-382Article in journal (Refereed)
    Abstract [en]

    Elimination of persistent organic pollutants (POPs) under national and international controls reduces “primary” emissions, but “secondary” emissions continue from residues deposited in soil, water, ice and vegetation during former years of high usage. Secondary sources are expected to dominate in the future, when POPs transport and accumulation will be controlled by air–surface exchange and the biogeochemical cycle of organic carbon. Climate change is likely to affect mobilization of POPs through, e.g., increased temperature, loss of ice cover in polar regions, melting glaciers and changes in soil and water microbiology which affect degradation and transformation. Chiral compounds offer advantages for following transport and fate pathways because of their ability to distinguish racemic (newly released or protected from microbial attack) and nonracemic (microbially altered) sources. Here we explain the rationale for this approach and suggest applications where chiral POPs could aid investigation of climate–mediated exchange and degradation processes. Examples include distinguishing agricultural vs. non–agricultural and recently used vs. residual pesticides, degradation and sequestration processes in soil, historical vs. recent atmospheric deposition, sources in arctic air and influence of ice cover on volatilization.

  • 9.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Centre for Atmospheric Research Experiments, Environment Canada, Ontario, Canada.
    Kurt-Karakus, Perihan B.
    Department of Environmental Engineering, Faculty of Natural Sciences, Architecture and Engineering, Bursa Technical University, Turkey.
    Wong, Fiona
    Department of Applied Environmental Science (ITM), Stockholm University.
    Alegria, Henry A.
    Department of Environmental Science, Policy and Geography, University of South Florida St. Petersburg, U.S.A..
    Jantunen, Liisa M.
    Centre for Atmospheric Research Experiments, Environment Canada, Ontario, Canada.
    Hung, Hayley
    Environment Canada, Ontario, Canada.
    Is there still “new” DDT in North America?: an investigation using proportions of DDT compounds2013In: Occurrence, fate and impact of atmospheric pollutants on environmental and human health / [ed] Laura L. McConnell, Jordi Dachs, Cathleen J. Hapeman, American Chemical Society (ACS), 2013, p. 153-181Chapter in book (Refereed)
    Abstract [en]

    Usage of DDT ceased over four decades ago in Canada and the United States, and since 2000 in Mexico. Potential sources in the North American atmosphere today include emissions of legacy residues from soils and long-range transport from other countries where DDT is still used or recently banned. Distinction of source types is investigated here using proportions of p,p′-DDT, o,p′-DDT, p,p′-DDE and p,p′-DDD. The relative volatilization of DDT compounds can be accurately described by their subcooled liquid vapor pressures (PL); e.g., (p,p′-DDT/p,p′-DDE)AIR = (p,p′-DDT/p,p′-DDE)SOIL x PL, DDT/PL,DDE. Using this model, the expected proportions in air due to volatilization from technical DDT and from soils in Canada, the U.S.A. and Mexico were estimated and expressed as the fractions FDDTE = p,p′-DDT/(p,p′-DDT + p,p′-DDE), FDDTO = p,p′-DDT/(p,p′-DDT + o,p′-DDT), and FDDTD = p,p′-DDT/(p,p′-DDT + p,p′-DDD). FDDTE, FDDTO and FDDTD predicted from soil emissions were compared to compound fractions in ambient air sampled at the Integrated Atmospheric Deposition Network (IADN) of stations on the Great Lakes between Canada and the U.S.A., and at arctic monitoring stations. FDDTE in air at IADN stations on lakes Erie, Ontario, Michigan and Huron were lower than in technical DDT vapor. This is consistent with emissions of aged residues from agricultural land and urban centers near these lakes. By comparison, FDDTE values were higher at stations on Lake Superior where atmospheric DDT is likely due to long-range transport rather than regional soil emissions. FDDTE increased from the early 1990s to 2005 at the Lake Superior stations and at the Canadian arctic station Alert between 2002-2005, whereas a significant decline in FDDTE was observed at the Norwegian arctic station Zeppelin Mountain. The mean FDDTO in air at IADN stations were consistent with either soil emissions or technical DDT composition, but annual values showed significant downward trends at two Canadian stations, and also decreased with time at Zeppelin Mountain (but not at Alert). These trends might signify contribution from “dicofol-type” DDT sources, which have a lower FDDTO than technical DDT or soil emissions, or preferential degradation of p,p′-DDT vs. o,p′-DDT over time. FDDTD in air at IADN stations were lower than in technical DDT vapor, showing the influence of soil sources. The enantiomer proportions of the chiral compounds o,p′-DDT and o,p′-DDD were nonracemic in some soils and ambient air, but enantiospecific analysis has not been done for IADN air samples. It is suggested that isomer, parent/metabolite and enantiomer composition information be incorporated into air monitoring programs to help identify sources.

  • 10.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Laudon, Hjalmar
    Nygren, Olle
    Lokalförsörjningsenheten, Umeå universitet.
    Svanberg, Staffan
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Chlorinated pesticides and natural brominated anisoles in air at three northern Baltic stations2017In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 225, p. 381-389Article in journal (Refereed)
    Abstract [en]

    Abstract Polyurethane foam (PUF) disk passive samplers were deployed at one inland and two island locations in the Bothnian Bay region of the northern Baltic Sea. Uptake was linear over 81–147 d and a temperature range of −2.6 to 14.2 °C for organochlorine pesticides (OCPs) and current-use pesticides (CUPs) having log KOA ≥9 at ambient temperatures. Partial saturation of the PUF disks occurred for the more volatile OCPs hexachlorocyclohexanes (HCHs) and hexachlorobenzene (HCB), and for bromoanisoles (BAs), which are products of bromophenols released by natural and anthropogenic sources. Correction for nonlinear uptake of these was made using experimentally measured PUF-air partition coefficients. Passive-derived air concentrations of pesticides were uniform over the bay and agreed within a factor of 2 or better with levels determined by active (pumped) sampling at one of the island stations. Levels of OCPs were similar to those reported at background sites in the European and Canadian Arctic and at monitoring stations in the central Baltic and southern Scandinavia, indicating long-range transport. The insecticide chlorpyrifos was 10 times lower at bay stations than in the Canadian Arctic. Insight to sources and processes was gained by examining compound profiles. Fractions Falpha = α-HCH/(α-HCH + γ-HCH) and FTC = trans-chlordane/(trans-chlordane + cis-chlordane) at bay stations were higher than in the Norwegian and Finnish Arctic and similar to those at the southern monitoring stations. Volatilization of chlordanes from Baltic seawater may also modify FTC. Higher FTriBA = 2,4,6-TriBA/(2,4,6-TriBA + 2,4-DiBA) distinguished local volatilization from the Baltic Sea versus lower FTriBA found at the inland site and reported in air on the Norwegian coast, suggesting westerly transport from the Atlantic across Norway and Sweden.

  • 11.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Melymuk, Lisa
    Forty-five years of foam: a retrospective on air sampling with polyurethane foam2019In: Bulletin of Environmental Contamination and Toxicology, ISSN 0007-4861, E-ISSN 1432-0800, Vol. 102, no 4, p. 447-449Article in journal (Refereed)
  • 12.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Nygren, Olle
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Field estimates of polyurethane foam: air partition coefficients for hexachlorobenzene, alpha-hexachlorocyclohexane and bromoanisoles2016In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 159, p. 126-131Article in journal (Refereed)
    Abstract [en]

    Partition coefficients of gaseous semivolatile organic compounds (SVOCs) between polyurethane foam (PUF) and air (KPA) are needed in the estimation of sampling rates for PUF disk passive air samplers. We determined KPA in field experiments by conducting long-term (24-48 h) air sampling to saturate PUF traps and shorter runs (2-4 h) to measure air concentrations. Sampling events were done at daily mean temperatures ranging from 1.9 to 17.5 °C. Target compounds were hexachlorobenzene (HCB), alpha-hexachlorocyclohexane (α-HCH), 2,4-dibromoanisole (2,4-DiBA) and 2,4,6-tribromoanisole (2,4,6-TriBA). KPA (mL g(-1)) was calculated from quantities on the PUF traps at saturation (ng g(-1)) divided by air concentrations (ng mL(-1)). Enthalpies of PUF-to-air transfer (ΔHPA, kJ mol(-1)) were determined from the slopes of log KPA/mL g(-1) versus 1/T(K) for HCB and the bromoanisoles, KPA of α-HCH was measured only at 14.3 to 17.5 °C and ΔHPA was not determined. Experimental log KPA/mL g(-1) at 15 °C were HCB = 7.37; α-HCH = 8.08; 2,4-DiBA = 7.26 and 2,4,6-TriBA = 7.26. Experimental log KPA/mL g(-1) were compared with predictions based on an octanol-air partition coefficient (log KOA) model (Shoeib and Harner, 2002a) and a polyparameter linear free relationship (pp-LFER) model (Kamprad and Goss, 2007) using different sets of solute parameters. Predicted KP values varied by factors of 3 to over 30, depending on the compound and the model. Such discrepancies provide incentive for experimental measurements of KPA for other SVOCs.

  • 13.
    Bidleman, Terry F.
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Breakthrough during air sampling with polyurethane foam: What do PUF 2/PUF 1 ratios mean?2018In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 192, p. 267-271Article in journal (Refereed)
    Abstract [en]

    Frontal chromatography theory is applied to describe movement of gaseous semivolatile organic compounds (SVOCs) through a column of polyurethane foam (PUF). Collected mass fractions (FC) are predicted for sample volume/breakthrough volume ratios (τ = VS/VB) up to 6.0 and PUF bed theoretical plate numbers (N) from 2 to 16. The predictions assume constant air concentrations and temperatures. Extension of the calculations is done to relate the collection efficiency of a 2-PUF train (FC1+2) to the PUF 2/PUF 1 ratio. FC1+2 exceeds 0.9 for PUF 2/PUF 1 ≤ 0.5 and lengths of PUF commonly used in air samplers. As the PUF 2/PUF 1 ratio approaches unity, confidence in these predictions is limited by the analytical ability to distinguish residues on the two PUFs. Field data should not be arbitrarily discarded because some analytes broke through to the backup PUF trap. The fractional collection efficiencies can be used to estimate air concentrations from quantities retained on the PUF trap when sampling is not quantitative.

  • 14.
    Bidleman, Terry Frank
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Air Quality Processes Research Section, Environment Canada.
    Jantunen, L. M.
    Hung, H.
    Ma, J.
    Stern, G. A.
    Rosenberg, B.
    Racine, J.
    Annual cycles of organochlorine pesticide enantiomers in Arctic air suggest changing sources and pathways2015In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 15, no 3, p. 1411-1420Article in journal (Refereed)
    Abstract [en]

    Air samples collected during 1994-2000 at the Canadian Arctic air monitoring station Alert (82 degrees 30'N, 62 degrees 20'W) were analysed by enantiospecific gas chromatography-mass spectrometry for alpha-hexachlorocyclohexane (alpha-HCH), trans-chlordane (TC) and cis-chlordane (CC). Results were expressed as enantiomer fractions (EF = peak areas of (+)/[(+) + (-)] enantiomers), where EFs = 0.5, <0.5 and >0.5 indicate racemic composition, and preferential depletion of (+) and (-) enantiomers, respectively. Long-term average EFs were close to racemic values for alpha-HCH (0.504 +/- 0.004, n = 197) and CC (0.505 +/- 0.004, n = 162), and deviated farther from racemic for TC (0.470 +/- 0.013, n = 165). Digital filtration analysis revealed annual cycles of lower alpha-HCH EFs in summer-fall and higher EFs in winter-spring. These cycles suggest volatilization of partially degraded alpha-HCH with EF < 0.5 from open water and advection to Alert during the warm season, and background transport of alpha-HCH with EF > 0.5 during the cold season. The contribution of sea-volatilized alpha-HCH was only 11% at Alert, vs. 32% at Resolute Bay (74.68 degrees N, 94.90 degrees W) in 1999. EFs of TC also followed annual cycles of lower and higher values in the warm and cold seasons. These were in phase with low and high cycles of the TC / CC ratio (expressed as F-TC = TC/(TC + CC)), which suggests greater contribution of microbially "weathered" TC in summer-fall versus winter-spring. CC was closer to racemic than TC and displayed seasonal cycles only in 1997-1998. EF profiles are likely to change with rising contribution of secondary emission sources, weathering of residues in the environment, and loss of ice cover in the Arctic. Enantiomer-specific analysis could provide added forensic capability to air monitoring programs.

  • 15.
    Bidleman, Terry Frank
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Centre for Atmospheric Research Experiments, Environment Canada, Canada.
    Jantunen, Liisa M.
    Binnur Kurt-Karakus, Perihan
    Wong, Fiona
    Hung, Hayley
    Ma, Jianmin
    Stern, Gary
    Rosenberg, Bruno
    Chiral Chemicals as Tracers of Atmospheric Sources and Fate Processes in a World of Changing Climate2013In: Mass Spectrometry, ISSN 2186-5116, Vol. 2, no 19, Special Issue: Proceedings of 19th International Mass Spectrometry Conference, p. S0019-Article in journal (Refereed)
    Abstract [en]

    Elimination of persistent organic pollutants (POPs) under national and international regulations reduces “primary” emissions, but “secondary” emissions continue from residues deposited in soil, water, ice and vegetation during former years of usage. In a future, secondary source controlled world, POPs will follow the carbon cycle and biogeochemical processes will determine their transport, accumulation and fate. Climate change is likely to affect mobilisation of POPs through e.g., increased temperature, altered precipitation and wind patterns, flooding, loss of ice cover in polar regions, melting glaciers, and changes in soil and water microbiology which affect degradation and transformation. Chiral compounds offer advantages for following transport and fate pathways because of their ability to distinguish racemic (newly released or protected from microbial attack) and nonracemic (microbially degraded) sources. This paper discusses the rationale for this approach and suggests applications where chiral POPs could aid investigation of climate-mediated exchange and degradation processes. Multiyear measurements of two chiral POPs, trans-chlordane and α-HCH, at a Canadian Arctic air monitoring station show enantiomer compositions which cycle seasonally, suggesting varying source contributions which may be under climatic control. Large-scale shifts in the enantioselective metabolism of chiral POPs in soil and water might influence the enantiomer composition of atmospheric residues, and it would be advantageous to include enantiospecific analysis in POPs monitoring programs.

  • 16.
    Bidleman, Terry Frank
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Centre for Atmospheric Research Experiments (CARE), Environment Canada, 6248 Eighth Line, Egbert, ON, L0L 1N0, Canada.
    Stern, Gary A.
    Tomy, Gregg T.
    Hargrave, Barry T.
    Jantunen, Liisa M.
    Macdonald, Robie W.
    Scavenging amphipods: sentinels for penetration of mercury and persistent organic chemicals into food webs of the deep arctic ocean2013In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 47, no 11, p. 5553-5561Article in journal (Refereed)
    Abstract [en]

    Archived specimens of the scavenging amphipod Eurythenes gryllus, collected from 2075 to 4250 m below the surface on five expeditions to the western and central Arctic Ocean between 1983 and 1998, were analyzed for total mercury (∑Hg), methyl mercury (MeHg), polychlorinated biphenyls (PCBs) and other industrial or byproduct organochlorines (chlorobenzenes, pentachloroanisole, octachlorostyrene), organochlorine pesticides (OCPs), and polybrominated diphenyl ethers (PBDEs). Median ∑Hg concentrations ranged from 70 to 366 ng g(-1) wet weight (ww). MeHg concentrations (3.55 to 23.5 ng g(-1) ww) accounted for 1.7 to 20.1% (median 3.7%) of ∑Hg. ∑Hg and MeHg were positively and significantly correlated with ww (∑Hg r(2) = 0.18, p = 0.0004, n = 63; MeHg r(2) = 0.42, p = 0.0004, n = 25), but not significantly with δ(13)C nor δ(15)N. Median concentrations of total persistent organic pollutants (POPs) ranged from 9750 to 156 000 ng g(-1) lipid weight, with order of abundance: ∑TOX (chlorobornanes quantified as technical toxaphene) > ∑PCBs > ∑DDTs > ∑chlordanes > ∑mirex compounds > ∑BDEs ∼ ∑chlorobenzenes ∼ octachlorostyrene > α-hexachlorocyclohexane ∼ hexachlorobenzene ∼ pentachloroanisole. Enantioselective accumulation was found for the chiral OCPs o,p'-DDT, cis- and trans-chlordane, nonachlor MC6 and oxychlordane. Lipid-normalized POPs concentrations were elevated in amphipods with lipid percentages ≤10%, suggesting that utilization of lipids resulted in concentration of POPs in the remaining lipid pool. Multidimensional Scaling (MDS) analysis using log-transformed physiological variables and lipid-normalized organochlorine concentrations distinguished amphipods from the central vs western arctic stations. This distinction was also seen for PCB homologues, whereas profiles of other compound classes were more related to specific stations rather than central-west differences.

  • 17. Brommer, Sandra
    et al.
    Jantunen, Liisa M.
    Bidleman, Terry Frank
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Harrad, Stuart
    Diamond, Miriam L.
    Determination of vapor pressures for organophosphate esters2014In: Journal of Chemical and Engineering Data, ISSN 0021-9568, E-ISSN 1520-5134, Vol. 59, no 5, p. 1441-1447Article in journal (Refereed)
    Abstract [en]

    Organophosphate compounds are ubiquitous in the environment and to better understand and predict their environmental transport and fate, well-defined physical-chemical properties are needed. The subcooled liquid-phase vapor pressures at 298.15 K (p298) were determined for 11 chlorinated and nonchlorinated phosphate flame retardants (PFRs) by the capillary gas chromatography retention time method (GC-RT). Values of log (p298/Pa) ranged from -5.22 to -1.32 and enthalpies of vaporization (δ l gH/kJ·mol-1) ranged from 82.0 to 109. Log (p298/Pa) by GC-RT showed good overall agreement with estimates using the Modified Grain Method (EpiSuite) and with the mean of experimental and in silico literature values, whereas values for the chlorinated PFRs appeared to be overestimated. SPARC modeling seriously underestimated p298, especially for the less volatile compounds. The Junge-Pankow adsorption model at 288.15 K predicted that most of the PFRs would be predominantly in the particulate phase in urban air and distributed between the particulate and gaseous phases in background air.

  • 18. Chartrand, Michelle
    et al.
    Passeport, Elodie
    Rose, Carla
    Lacrampe-Couloume, Georges
    Bidleman, Terry F.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Liisa M. Jantunen, Liisa M.
    Sherwood Lollar, Barbara
    Compound specific isotope analysis of hexachlorocyclohexane isomers: a method for source fingerprinting and field investigation of in situ biodegradation2015In: Rapid Communications in Mass Spectrometry, ISSN 0951-4198, E-ISSN 1097-0231, Vol. 29, no 6, p. 505-514Article in journal (Refereed)
    Abstract [en]

    RATIONALE: The manufacturing and uses of hexachlorocyclohexane (HCH) have resulted in a serious environmentalchallenge and legacy. This study highlights the ability of compound specific isotope analysis (CSIA) to distinguishamong various HCH sources and to support the evaluation of the potential for in situ biodegradation in contaminatedgroundwater.

    METHODS: Tests were conducted to verify the absence of significant isotope fractionation during HCH sample preconcentrationincluding dichloromethane extraction, solvent exchange into iso-octane, and H2SO4 clean-up, and analysisby gas chromatography/combustion-isotope ratio mass spectrometry (GC/C-IRMS). The method was then applied tofour Technical Grade (TG) HCH mixtures procured from different sources and to groundwater samples from acontaminated site.

    RESULTS: The pre-concentration method enabled determination of carbon isotope ratios (δ13C values) of HCH isomerswith no significant isotopic fractionation. The TG-HCH mixtures had significantly different δ13C values. Moreover, forany given TG-HCH, all isomers had δ13C values within 1.1‰ of each other – a distinctly uniform fingerprint. At theHCH-contaminated field site, compared with source wells, downgradient wells showed significant (up to 5.1‰)enrichment in 13C and the δ13C values of the HCH isomers were significantly different from each other.

    CONCLUSIONS: A method was successfully developed for the CSIA of HCH isomers that showed potential for HCHsource differentiation and identification of HCH in situ biodegradation. At the HCH-contaminated site, the observedpreferential isotopic enrichment of certain isomers relative to others for a given source allows differentiation betweenbiodegraded and non-biodegraded HCH.

  • 19. Jantunen, Liisa M
    et al.
    Wong, Fiona
    Gawor, Anya
    Kylin, Henrik
    Helm, Paul A
    Stern, Gary A
    Strachan, William M J
    Burniston, Deborah A
    Bidleman, Terry F
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Air Quality Processes Research Section, Environment Canada, Egbert Ontario, Canada.
    20 Years of Air-Water Gas Exchange Observations for Pesticides in the Western Arctic Ocean2015In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 23, p. 13844-13852Article in journal (Refereed)
    Abstract [en]

    The Arctic has been contaminated by legacy organochlorine pesticides (OCPs) and currently used pesticides (CUPs) through atmospheric transport and oceanic currents. Here we report the time trends and air–water exchange of OCPs and CUPs from research expeditions conducted between 1993 and 2013. Compounds determined in both air and water were trans- and cis-chlordanes (TC, CC), trans- and cis-nonachlors (TN, CN), heptachlor exo-epoxide (HEPX), dieldrin (DIEL), chlorobornanes (ΣCHBs and toxaphene), dacthal (DAC), endosulfans and metabolite endosulfan sulfate (ENDO-I, ENDO-II, and ENDO SUL), chlorothalonil (CHT), chlorpyrifos (CPF), and trifluralin (TFN). Pentachloronitrobenzene (PCNB and quintozene) and its soil metabolite pentachlorothianisole (PCTA) were also found in air. Concentrations of most OCPs declined in surface water, whereas some CUPs increased (ENDO-I, CHT, and TFN) or showed no significant change (CPF and DAC), and most compounds declined in air. Chlordane compound fractions TC/(TC + CC) and TC/(TC + CC + TN) decreased in water and air, while CC/(TC + CC + TN) increased. TN/(TC + CC + TN) also increased in air and slightly, but not significantly, in water. These changes suggest selective removal of more labile TC and/or a shift in chlordane sources. Water–air fugacity ratios indicated net volatilization (FR > 1.0) or near equilibrium (FR not significantly different from 1.0) for most OCPs but net deposition (FR < 1.0) for ΣCHBs. Net deposition was shown for ENDO-I on all expeditions, while the net exchange direction of other CUPs varied. Understanding the processes and current state of air–surface exchange helps to interpret environmental exposure and evaluate the effectiveness of international protocols and provides insights for the environmental fate of new and emerging chemicals.

  • 20. Klánová, Jana
    et al.
    Diamond, Miriam
    Jones, Kevin
    Lammel, Gerhard
    Lohmann, Rainer
    Pirrone, Nicola
    Scheringer, Martin
    Balducci, Catia
    Bidleman, Terry
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Bláha, Karel
    Bláha, Luděk
    Booij, Kees
    Bouwman, Henk
    Breivik, Knut
    Eckhardt, Sabine
    Fiedler, Heidelore
    Garrigues, Philippe
    Harner, Tom
    Holoubek, Ivan
    Hung, Hayley
    Macleod, Matthew
    Magulova, Katarina
    Mosca, Silvia
    Pistocchi, Alberto
    Simonich, Staci
    Smedes, Foppe
    Stephanou, Euripides
    Sweetman, Andy
    Šebková, Kateřina
    Venier, Marta
    Vighi, Marco
    Vrana, Branislav
    Wania, Frank
    Weber, Roland
    Weiss, Peter
    Identifying the Research and Infrastructure Needs for the Global Assessment of Hazardous Chemicals Ten Years after Establishing the Stockholm Convention2011In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 45, no 18, p. 7617-7619Article in journal (Refereed)
  • 21.
    Kupryianchyk, Darya
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Giesler, Reiner
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Bidleman, Terry F.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Liljelind, Per
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Lau, Danny Chun Pong
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Sponseller, Ryan A.
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Andersson, Patrik L.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Industrial and natural compounds in filter-feeding black fly larvae and water in 3 tundra streams2018In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 37, no 12, p. 3011-3017Article in journal (Refereed)
    Abstract [en]

    We report concentrations of polychlorinated biphenyls, polybrominated diphenyl ethers, novel flame retardants, and naturally occurring bromoanisoles in water and filter-feeding black fly (Simuliidae) larvae in 3 tundra streams in northern Sweden. The results demonstrate that black fly larvae accumulate a wide range of organic contaminants and can be used as bioindicators of water pollution in Arctic streams.

  • 22. Newton, Seth
    et al.
    Bidleman, Terry
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Bergknut, Magnus
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Racine, Jacinthe
    Laudon, Hjalmar
    Giesler, Reiner
    Wiberg, Karin
    Atmospheric deposition of persistent organic pollutants and chemicals of emerging concern at two sites in northern Sweden2014In: Environmental science: processes & impacts, ISSN 2050-7887, Vol. 16, no 2, p. 298-305Article in journal (Refereed)
    Abstract [en]

    Bimonthly bulk atmospheric deposition samples (precipitation + dry particle) were taken for one year at an arctic (Abisko, 68 degrees 20' N, 19 degrees 03' E) and a sub-arctic (Krycklan 64 degrees 14' N, 19 degrees 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 chlorothabnil; 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 Sigma HCH to Sigma PCB 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.

  • 23. Pućko, Monika
    et al.
    Stern, Gary A.
    Burt, Alexis E.
    Jantunen, Liisa M.
    Bidleman, Terry F.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Macdonald, Robie W.
    Barber, David G.
    Geilfus, Nicolas-X.
    Rysgaard, Søren
    Current use pesticide and legacy organochlorine pesticide dynamics at the ocean-sea ice-atmosphere interface in resolute passage, Canadian Arctic, during winter-summer transition2017In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 580, p. 1460-1469Article in journal (Refereed)
    Abstract [en]

    Here, we present the first detailed analysis of processes by which various current use pesticides (CUPs) and legacy organochlorine pesticides (OCPs) are concentrated in melt ponds that form on Arctic sea ice in the summer, when surface snow is melting and ice eventually breaks up. Four current use pesticides (dacthal, chlorpyrifos, trifluralin, and pentachloronitrobenzene) and one legacy organochlorine pesticide (α-hexachlorocyclohexane) were detected in ponds in Resolute Passage, Canadian Arctic, in 2012. Melt-pond concentrations changed over time as a function of gas exchange, precipitation, and dilution with melting sea ice. Observed increases in melt-pond concentrations for all detected pesticides were associated with precipitation events. Dacthal reached the highest concentration of all current use pesticides in ponds (95 ± 71 pg L− 1), a value exceeding measured concentrations in the under-ice (0 m) and 5 m seawater by &gt; 10 and &gt; 16 times, respectively. Drainage of dacthal-enriched pond water to the ocean during ice break-up provides an important ice-mediated annual delivery route, adding ~ 30% of inventory in the summer Mixed Layer (ML; 10 m) in the Resolute Passage, and a concentrating mechanism with potential implications for exposures to organisms such as ice algae, and phytoplankton.

  • 24. Pućko, Monika
    et al.
    Stern, Gary A
    Macdonald, Robie W
    Jantunen, Liisa M
    Bidleman, Terry F
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Wong, Fiona
    Barber, David G
    Rysgaard, Søren
    The delivery of organic contaminants to the Arctic food web: why sea ice matters2015In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 506–507, p. 444-452Article in journal (Refereed)
    Abstract [en]

    For decades sea ice has been perceived as a physical barrier for the loading of contaminants to the Arctic Ocean. We show that sea ice, in fact, facilitates the delivery of organic contaminants to the Arctic marine food web through processes that: 1) are independent of contaminant physical–chemical properties (e.g. 2–3-fold increase in exposure to brine-associated biota), and 2) depend on physical–chemical properties and, therefore, differentiate between contaminants (e.g. atmospheric loading of contaminants to melt ponds over the summer, and their subsequent leakage to the ocean). We estimate the concentrations of legacy organochlorine pesticides (OCPs) and current-use pesticides (CUPs) in melt pond water in the Beaufort Sea, Canadian High Arctic, in 2008, at near-gas exchange equilibrium based on Henry's law constants (HLCs), air concentrations and exchange dynamics. CUPs currently present the highest risk of increased exposures through melt pond loading and drainage due to the high ratio of melt pond water to seawater concentration (Melt pond Enrichment Factor, MEF), which ranges from 2 for dacthal to 10 for endosulfan I. Melt pond contaminant enrichment can be perceived as a hypothetical ‘pump’ delivering contaminants from the atmosphere to the ocean under ice-covered conditions, with 2–10% of CUPs annually entering the Beaufort Sea via this input route compared to the standing stock in the Polar Mixed Layer of the ocean. The abovementioned processes are strongly favored in first-year ice compared to multi-year ice and, therefore, the dynamic balance between contaminant inventories and contaminant deposition to the surface ocean is being widely affected by the large-scale icescape transition taking place in the Arctic.

  • 25. Sánchez-Osorio, José Luis
    et al.
    Macías-Zamora, José Vinicio
    Ramírez-Álvarez, Nancy
    Bidleman, Terry F.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Organochlorine pesticides in residential soils and sediments within two main agricultural areas of northwest Mexico: concentrations, enantiomer compositions and potential sources2017In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 173, p. 275-287Article in journal (Refereed)
    Abstract [en]

    The agricultural Mexicali and Yaqui valleys (MV, YV) in northwest Mexico were heavily treated with organochlorine pesticides in the past. Residential soils and agricultural drain sediments were sampled in 2008–2009 and analyzed for DDTs (o,p′- and p,p′- isomers of DDE, DDD and DDT); hexachlorocyclohexanes (α-, β-, γ- and δ-HCH) and chlordanes (trans-chlordane, cis-chlordane, heptachlor and heptachlor exo-epoxide). Geometric means (GMs) (ng g−1 dry weight) were: MV soils (n = 27) ΣDDT 22, ΣHCH 0.80, ΣCHL 0.88; YV soils (n = 25) ΣDDT 5.0, ΣHCH 0.23, ΣCHL 0.67; MV sediments (n = 3) ΣDDT 5.0, ΣHCH 0.23, ΣCHL 0.53; YV sediments (n = 8) ΣDDT 2.6, ΣHCH 0.12, ΣCHL 0.090. GMs were significantly higher (p &lt; 0.05) in MV than YV soils for ΣDDT and ΣHCH, but not for ΣCHL. Comparison to worldwide regulatory guideline values (RGVs) for residential soils showed all compounds below mean or GM RGVs, but above the lowest RGV in some cases. Low p,p′-DDT/(p,p′-DDT + p,p′-DDE) in most soils indicated aged residues. Lack of p,p′-DDT metabolism might account for its dominance in a few soils. HCH isomer profiles suggested aged technical HCH in the YV, and technical HCH + lindane in the MV. Heptachlor dominated the ΣCHL, probably from application of technical heptachlor as well as chlordane. Chiral compounds were nonracemic in soils and sediments and indicated enantioselective microbial degradation of (+)α-HCH, (−)trans-chlordane, (−)cis-chlordane and (+)o,p′-DDT. Depletion of (+)o,p′-DDT in soils may account for similar enantiomer signatures previously reported in air of northwest Mexico.

  • 26.
    Tysklind, Mats
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Andersson, Agneta
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences. Umeå University, Faculty of Science and Technology, Umeå Marine Sciences Centre (UMF).
    Haglund, Peter
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Bidleman, Terry F.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    A Baltic mystery2014Other (Refereed)
    Abstract [en]

    HNPs are produced by macroalgae (seaweeds), phytoplankton, worms, sponges and other marine organisms. HNPs in the Baltic comprise halocarbons, bromophenols and their transformation products, and other compounds with diverse chemical structures. The HNPs derived from bromophenols are widespread in Baltic algae, fi sh and mussels, and include bromoanisoles, hydroxylated and methoxylated bromodiphenyl ethers (OH- and MeO-BDEs) and polybrominated dibenzo-p-dioxins (PBDDs). Some of these also have anthropogenic origins; bromophenols are used as industrial compounds, while MeO-BDEs and OH-BDEs are metabolites and photolysis products of polybrominated diphenyl ether fl ame retardants. Nonetheless, radiocarbon-14 dating has shown that most of the OH-BDEs and MeO-BDEs found in marine mammals and sponges are natural. The bromophenolderived HNPs have toxic properties which add to the ‘soup’ of anthropogenic toxic chemicals present in the Baltic.

  • 27.
    Weidemann, Eva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Andersson, Patrik L.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Bidleman, Terry
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Boman, Christoffer
    Umeå University, Faculty of Science and Technology, Department of Applied Physics and Electronics.
    Carlin, Danielle J.
    Collina, Elena
    Cormier, Stephania A.
    Gouveia-Figueira, Sandra C.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Gullett, Brian K.
    Johansson, Christer
    Lucas, Donald
    Lundin, Lisa
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Lundstedt, Staffan
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Marklund, Stellan
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Nording, Malin L.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Ortuno, Nuria
    Sallam, Asmaa A.
    Schmidt, Florian M.
    Umeå University, Faculty of Science and Technology, Department of Applied Physics and Electronics.
    Jansson, Stina
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    14th congress of combustion by-products and their health effects-origin, fate, and health effects of combustion-related air pollutants in the coming era of bio-based energy sources2016In: Environmental science and pollution research international, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 23, no 8, p. 8141-8159Article in journal (Refereed)
    Abstract [en]

    The 14th International Congress on Combustion By-Products and Their Health Effects was held in UmeAyen, Sweden from June 14th to 17th, 2015. The Congress, mainly sponsored by the National Institute of Environmental Health Sciences Superfund Research Program and the Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning, focused on the "Origin, fate and health effects of combustion-related air pollutants in the coming era of bio-based energy sources". The international delegates included academic and government researchers, engineers, scientists, policymakers and representatives of industrial partners. The Congress provided a unique forum for the discussion of scientific advances in this research area since it addressed in combination the health-related issues and the environmental implications of combustion by-products. The scientific outcomes of the Congress included the consensus opinions that: (a) there is a correlation between human exposure to particulate matter and increased cardiac and respiratory morbidity and mortality; (b) because currently available data does not support the assessment of differences in health outcomes between biomass smoke and other particulates in outdoor air, the potential human health and environmental impacts of emerging air-pollution sources must be addressed. Assessment will require the development of new approaches to characterize combustion emissions through advanced sampling and analytical methods. The Congress also concluded the need for better and more sustainable e-waste management and improved policies, usage and disposal methods for materials containing flame retardants.

  • 28. Wong, Fiona
    et al.
    Jantunen, Liisa M
    Papakyriakou, Tim
    Staebler, Ralf M
    Stern, Gary A
    Bidleman, Terry F
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Comparison of micrometeorological and two-film estimates of air-water gas exchange for alpha-hexachlorocyclohexane in the Canadian archipelago2012In: Environmental science and pollution research international, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 19, no 6, p. 1908-1914Article in journal (Refereed)
    Abstract [en]

    The air-sea gas exchange of alpha-hexachlorocyclohexane (alpha-HCH) in the Canadian Arctic was estimated using a micrometeorological approach and the commonly used Whitman two-film model. Concurrent shipboard measurements of alpha-HCH in air at two heights (1 and 15 m) and in surface seawater were conducted during the Circumpolar Flaw Lead study in 2008. Sampling was carried out during eight events in the early summer time when open water was encountered. The micrometeorological technique employed the vertical gradient in air concentration and the wind speed to estimate the flux; results were corrected for atmospheric stability using the Monin-Obukhov stability parameter. The Whitman two-film model used the concentrations of alpha-HCH in surface seawater, in bulk air at 1 and 15 m above the surface, and the Henry's law constant adjusted for temperature and salinity to derive the flux. Both approaches showed that the overall net flux of alpha-HCH was from water to air. Mean fluxes calculated using the micrometeorological technique ranged from -3.5 to 18 ng m(-2) day(-1) (mean 7.4), compared to 3.5 to 14 ng m(-2) day(-1) (mean 7.5) using the Whitman two-film model. Flux estimates for individual events agreed in direction and within a factor of two in magnitude for six of eight events. For two events, fluxes estimated by micrometeorology were zero or negative, while fluxes estimated with the two-film model were positive, and the reasons for these discrepancies are unclear. Improvements are needed to shorten air sampling times to ensure that stationarity of meteorological conditions is not compromised over the measurement periods. The micrometeorological technique could be particularly useful to estimate fluxes of organic chemicals over water in situations where no water samples are available.

  • 29. Wong, Fiona
    et al.
    Kurt-Karakus, Perihan
    Bidleman, Terry F.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Fate of Brominated Flame Retardants and Organochlorine Pesticides in Urban Soil: Volatility and Degradation2012In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 46, no 5, p. 2668-2674Article in journal (Refereed)
    Abstract [en]

    As the uses of polybrominated diphenyl ethers (BDEs) are being phased out in many countries, soils could become a secondary emission source to the atmosphere. It is also anticipated that the demand for alternative brominated flame retardants (BFRs) will grow, but little is known about their environmental fate in soils. In this study, the volatility degradation of BFRs and organochlorine pesticides (OCPS) in soil was investigated. A low organic carbon (5.6%) urban soil was spiked with a suite of BFRs and OCPs, followed by incubation under laboratory condition for 360 days. These included BDE- 17, -28, -47, -99; alpha- and beta-1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane (TBECH), beta-1,2,5,6-tetrabromocyclooctane (TBCO), and 2,3-dibromopropyl-2,4,6-tribromophenyl ether (DPTE), OCPs: a-hexachlorocyclohexane (alpha-HCH) and C-13(6)-alpha-HCH, trans-chlordane (TC), and C-13(10)-TC. The volatility of spiked chemicals was investigated using a fugacity meter to measure the soil-air partition coefficient (K-SA). K-SA of some spiked BFRs and OCPs increased from Day 10 to 60 or 90 and leveled off afterward. This suggests that the volatility of BFRs and OCPs decreases over time as the chemicals become more strongly bound to the soil. Degradation of alternative BFRs (alpha- and beta-TBECH, beta-TBCO, DPTE), BDE-17, and alpha-HCH (C-13-labeled and nonlabeled) was evident in soils over 360 days, but no degradation was observed for the BDE-28, -47, -99, and TC (C-13-labeled and nonlabeled). A method to separate the enantiomers of alpha-TBECH and beta-TBCO was developed and their degradation, along with alpha-HCH (C-13-labeled and nonlabeled) was enantioselective. This is the first study which reports the enantioselective degradation of chiral BFRs in soils. Discrepancies between the enantiomer fraction (EF) of chemicals extracted from the soil by dichloromethane (DCM) and air were found. It is suggested that DCM removes both the sequestered and loosely bound fractions of chemicals in soil, whereas air accesses only the loosely bound fraction, and these two pools are subject to different degrees of enantioselective degradation. This calls for caution when interpreting EFs obtained from DCM extraction of soil with EFs in ambient air.

  • 30. Zhang, Lin
    et al.
    Bidleman, Terry F
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Perry, Mary Jane
    Lohmann, Rainer
    Fate of chiral and achiral organochlorine pesticides in the North Atlantic Bloom experiment2012In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 46, no 15, p. 8106-8114Article in journal (Refereed)
    Abstract [en]

    Organochlorine pesticides (OCPs) were measured in the surface seawater and lower atmosphere during the North Atlantic Bloom Experiment in the spring 2008 from samples collected on the R/V Knorr. The gaseous concentration profiles resulted from both long-range transport (LRT) from the Arctic by polar easterlies and local biogeochemical processes. Relatively constant alpha/gamma-hexachlorocyclohexane (HCH) ratios and enantiomer fractions of alpha-HCH indicated that a single water mass was sampled throughout the cruise. Changes in dissolved phase concentrations were dominated by bloom processes (air-water exchange, partitioning to organic particles, and subsequent sinking) rather than LRT. alpha-HCH and dissolved phase trans-chlordanes showed depletion of (+) enantiomer, whereas depletion of the (-) enantiomer was observed for heptachlor exoepoxide (HEPX) and cis-chlordanes. Fugacity ratio calculations suggest that hexachlorobenzene (HCB) and gamma-HCH were depositing from air to water whereas heavier OCPs (chlordanes, HEPX) were evaporating. Dissolved phase concentrations did not decrease with time during the three-week bloom period; neither were lipophilic OCPs drawn down from air to water as previous studies hypothesized. Comparison with Arctic measurements suggested that the Arctic returned higher concentrations of alpha-HCH and HCB through both the atmospheric (polar easterlies) as well as oceanic transport (East Greenland Current) to the lower latitudes.

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