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  • 1.
    Assefa, Anteneh
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Dept. of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU), Uppsala, Sweden .
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Klanova, Jana
    Wiberg, Karin
    Tracing the sources of PCDD/Fs in Baltic Sea air by using metals as source markers2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 3, p. 544-552Article in journal (Refereed)
    Abstract [en]

    The atmosphere is the major contributor of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the Baltic Sea environment. In this study, we investigated the potential of using metals along with PCDD/Fs as markers of important emission sources of PCDD/Fs in air. The air concentrations of PCDD/F congeners (n = 17), other persistent organic pollutants (n = 8) and metals (n = 16) were determined in summer and winter air using high volume samplers at a rural field station (Aspvreten, Sweden) located close to the Baltic Sea coast. During winter, PCDD/F levels were on average 20 times higher than in summer (5.1 +/- 5.8 fg toxicity equivalents (TEQ) m-3 and 0.26 +/- 0.18 fg TEQ m-3, respectively) mostly due to a higher fraction of PCDFs. The increased levels of PCDD/Fs were pronounced mainly in air masses that had travelled from southern (S) and eastern (E) compass sectors. A principal component analysis (PCA) of metal levels in Scots pine (Pinus sylvestris) needles sampled to reflect various air emission source types helped to identify potential marker metals for selected known atmospheric emission sources of PCDD/Fs and to rank among the candidate source types. Brown coal burning, domestic burning and heavy oil burning appeared to be the source types that contribute most of the PCDD/Fs in Baltic Sea air. The current study demonstrates a successful approach for source tracing of PCDD/Fs in air, where integrated indices from seasonal and spatial patterns of PCDD/Fs as well as metal source markers were used to trace and rank sources.

  • 2.
    Balk, Fabian G. P.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Swiss Federal Institute of Aquatic Science and Technology, Switzerland.
    Winkens Pütz, Kerstin
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Swedish Museum of Natural History, Sweden.
    Ribbenstedt, Anton
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Gomis, Melissa I.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Université Paris-Saclay, France.
    Filipovic, Marko
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. NIRAS Sweden AB, Sweden.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Children's exposure to perfluoroalkyl acids - a modelling approach2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 11, p. 1875-1886Article in journal (Refereed)
    Abstract [en]

    Adults are mainly exposed to per- and polyfluoroalkyl substances (PFASs) via ingestion of food, inhalation of air and ingestion of dust, whereas for children the exposure to PFASs is largely unknown. This study aimed to reconstruct the serum concentrations of perfluorooctanoic acid (PFOA), perfluorooctane sulfonic acid (PFOS) and perfluorohexane sulfonic acid (PFHxS) in children after infancy up to 10.5 years of age and to test if dietary intake is the major exposure pathway for children to PFOA, PFOS and PFHxS after infancy. For this work, a dataset from a Finnish child cohort study was available, which comprised serum concentrations of the studied perfluoroalkyl acids (PFAAs) and PFAS concentration measurements in dust and air samples from the children's bedrooms. The calculated PFAA intakes were used in a pharmacokinetic model to reconstruct the PFAA serum concentrations from 1 to 10.5 years of age. The calculated PFOA and PFOS intakes were close to current regulatory intake thresholds and diet was the major exposure medium for the 10.5 year-olds. The one-compartment PK model reconstructed median PFOA and PFOS serum concentrations well compared to corresponding measured median serum concentrations, while the modelled PFHxS serum concentrations showed a constant underestimation. The results imply that children's exposure to PFOA and PFOS after breastfeeding and with increasing age resembles the exposure of adults. Further, the children in the Finnish cohort experienced a rather constant exposure to PFOA and PFOS between 1 and 10.5 years of age. The PFHxS exposure sources and respective pharmacokinetic parameter estimations need further investigation.

  • 3.
    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.

  • 4.
    Binnington, Matthew J
    et al.
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada.
    Lei, Ying D
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada.
    Pokiak, Lucky
    Tuktoyaktuk Hunters and Trappers Committee, Tuktoyaktuk, Canada.
    Pokiak, James
    Tuktoyaktuk Hunters and Trappers Committee, Tuktoyaktuk, Canada.
    Ostertag, Sonja K
    Freshwater Institute, Fisheries and Oceans Canada, Winnipeg, Canada.
    Loseto, Lisa L
    Freshwater Institute, Fisheries and Oceans Canada, Winnipeg, Canada.
    Chan, Hing M
    Department of Biology, University of Ottawa, Ottawa, Canada .
    Yeung, Leo W. Y.
    Department of Chemistry, University of Toronto, Toronto, Canada .
    Huang, Haiyong
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada .
    Wania, Frank
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada .
    Effects of preparation on nutrient and environmental contaminant levels in Arctic beluga whale (Delphinapterus leucas) traditional foods2017In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 19, no 8, p. 1000-1015Article in journal (Refereed)
    Abstract [en]

    For Canadian Arctic indigenous populations, marine mammal (MM) traditional foods (TFs) represent sources of both important nutrients and hazardous environmental contaminants. Food preparation is known to impact the nutrient and environmental contaminant content of processed items, yet the impacts of preparation on indigenous Arctic MM TFs remain poorly characterized. In order to determine how the various processes involved in preparing beluga blubber TFs affect their levels of nutrients and environmental contaminants, we collected blubber samples from 2 male beluga whales, aged 24 and 37 years, captured during the 2014 summer hunting season in Tuktoyaktuk, Northwest Territories, and processed them according to local TF preparation methods. We measured the levels of select nutrients [selenium (Se), polyunsaturated fatty acids (PUFAs)] and contaminants [organochlorine pesticides, perfluoroalkyl and polyfluoroalkyl substances (PFASs), polybrominated diphenyl ethers, polychlorinated biphenyls, polycyclic aromatic hydrocarbons (PAHs), mercury (Hg)] in raw and prepared (boiled, roasted, aged) beluga blubber TFs. The impacts of beluga blubber TF preparation methods on nutrient and environmental contaminant levels were inconsistent, as the majority of processes either did not appear to influence concentrations or affected the two belugas differently. However, roasting and ageing beluga blubber consistently impacted certain compounds: roasting blubber increased concentrations of hydrophilic substances (Se and certain PFASs) through solvent depletion and deposited PAHs from cookfire smoke. The solid-liquid phase separation involved in ageing blubber depleted hydrophilic elements (Se, Hg) and some ionogenic PFASs from the lipid-rich liquid oil phase, while PUFA levels appeared to increase, and hydrophobic persistent organic pollutants were retained. Ageing blubber adjacent to in-use smokehouses also resulted in considerable PAH deposition to processed samples. Our findings demonstrated that contaminant concentration differences were greater between the two sets of whale samples, based on age differences, than they were within each set of whale samples, due to variable preparation methods. When considering means to minimize human contaminant exposure while maximizing nutrient intake, consumption of aged liquid from younger male whales would be preferred, based on possible PUFA enhancement and selective depletion of hydrophilic environmental contaminants in this food item.

  • 5.
    Bohlin, P.
    et al.
    Resarch Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Audy, O.
    Resarch Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Skrdliková, L.
    Resarch Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Kukucka, Petr
    Resarch Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Pribylová, P.
    Resarch Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Prokes, R.
    Resarch Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Vojta, S.
    Resarch Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Klánová, J.
    Resarch Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Outdoor passive air monitoring of semi volatile organic compounds (SVOCs): a critical evaluation of performance and limitations of polyurethane foam (PUF) disks2014In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 16, no 3, p. 433-444Article in journal (Refereed)
    Abstract [en]

    The most commonly used passive air sampler (PAS) (i.e. polyurethane foam (PUF) disk) is cheap, versatile, and capable of accumulating compounds present both in gas and particle phases. Its performance for particle associated compounds is however disputable. In this study, twelve sets of triplicate PUF-PAS were deployed outdoors for exposure periods of 1-12 weeks together with continuously operated active samplers, to characterize sampling efficiency and derive sampling rates (R-S) for compounds belonging to 7 SVOC classes (including particle associated compounds). PUF-PAS efficiently and consistently sampled polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs), polycyclic aromatic hydrocarbons (PAHs), and eight novel brominated flame retardant (nBFR) compounds. Low accuracy and lack of sensitivity was observed for most polychlorinated dibenzo-p-dioxins/furans PCDD/Fs and polybrominated diphenyl ethers (PBDEs) (under the conditions of this study), with the exception of some congeners which may be used as qualitative markers for their respective classes. Application of compound specific R-S was found crucial for all compounds except PCBs. Sampling efficiency of the particle associated compounds was often low.

  • 6.
    Bohlin, Pernilla
    et al.
    Research Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Audy, Ondrej
    Research Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Skrdliková, Lenka
    Research Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Kukucka, Petr
    Research Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Vojta, Simon
    Research Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Pribylová, Petra
    Research Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Prokes, Roman
    Research Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Cupr, Pavel
    Research Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Klánová, Jana
    Research Centre for Toxic Compounds in the Environment (RECETOX), Faculty of Science, Masaryk University, Brno, Czech Republic .
    Evaluation and guidelines for using polyurethane foam (PUF) passive air samplers in double-dome chambers to assess semi-volatile organic compounds (SVOCs) in non-industrial indoor environments2014In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 16, no 11, p. 2617-2626Article in journal (Refereed)
    Abstract [en]

    Indoor air pollution has been recognized as an important risk factor for human health, especially in areas where people tend to spend most of their time indoors. Many semi-volatile organic compounds (SVOCs) have primarily indoor sources and are present in orders of magnitude higher concentrations indoors than outdoors. Despite this, awareness of SVOCs in indoor air and assessment of the link between indoor concentrations and human health have tagged behind those of outdoor air. This is partially related to challenges associated with indoor sampling of SVOCs. Passive air samplers (PASs), which are widely accepted in established outdoor air monitoring networks, have been used to fill the knowledge gaps on indoor SVOCs distribution. However, their applicability for indoor environments and the assessment of human health risks lack sufficient experimental data. To address this issue, we performed an indoor calibration study of polyurethane foam (PUF) PAS deployed in a double-dome chamber, covering both legacy and new SVOC classes. PUF-PAS and a continuous low-volume active air sampler (AAS) were co-deployed for a calibration period of twelve weeks. Based on the results from this evaluation, PUF-PAS in a double-bowl chamber is recommended for indoor sampling and health risk assessment of gas phase SVOCs, including novel brominated flame retardants (nBFR) providing sufficient exposure time is applied. Data for particle associated SVOCs suffered from significant uncertainties caused by low level of detection and low precision in this study. A more open chamber design for indoor studies may allow for higher sampling rates (R-s) and better performance for the particle associated SVOCs.

  • 7.
    Bolinius, Dämien J.
    et al.
    Stockholm University, Faculty of Science, Stockholm University Baltic Sea Centre.
    Sobek, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Löf, Marie F.
    Stockholm University, Faculty of Science, Stockholm University Baltic Sea Centre.
    Undeman, Emma
    Stockholm University, Faculty of Science, Stockholm University Baltic Sea Centre.
    Evaluating the consumption of chemical products and articles as proxies for diffuse emissions to the environment2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 10, p. 1427-1440Article in journal (Refereed)
    Abstract [en]

    In this study we have evaluated the use of consumption of manufactured products (chemical products and articles) in the EU as proxies for diffuse emissions of chemicals to the environment. The content of chemical products is relatively well known. However, the content of articles (products defined by their shape rather than their composition) is less known and currently has to be estimated from chemicals that are known to occur in a small set of materials, such as plastics, that are part of the articles. Using trade and production data from Eurostat in combination with product composition data from a database on chemical content in materials (the Commodity Guide), we were able to calculate trends in the apparent consumption and in-use stocks for 768 chemicals in the EU for the period 2003-2016. The results showed that changes in the apparent consumption of these chemicals over time are smaller than in the consumption of corresponding products in which the chemicals are present. In general, our results suggest that little change in chemical consumption has occurred over the timespan studied, partly due to the financial crisis in 2008 which led to a sudden drop in the consumption, and partly due to the fact that each of the chemicals studied is present in a wide variety of products. Estimated in-use stocks of chemicals show an increasing trend over time, indicating that the mass of chemicals in articles in the EU, that could potentially be released to the environment, is increasing. The quantitative results from this study are associated with large uncertainties due to limitations of the available data. These limitations are highlighted in this study and further underline the current lack of transparency on chemicals in articles. Recommendations on how to address these limitations are also discussed.

  • 8.
    Bolinius, Dämien Johann
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Mayer, Philipp
    Jahnke, Annika
    A passive dosing method to determine fugacitycapacities and partitioning properties of leaves2016In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 18, p. 1325-1332Article in journal (Refereed)
    Abstract [en]

    The capacity of leaves to take up chemicals from the atmosphere and water in fl uences how contaminantsare transferred into food webs and soil. We provide a proof of concept of a passive dosing method tomeasure leaf/polydimethylsiloxane partition ratios ( K leaf/PDMS ) for intact leaves, using polychlorinatedbiphenyls (PCBs) as model chemicals. Rhododendron leaves held in contact with PCB-loaded PDMSreached between 76 and 99% of equilibrium within 4 days for PCBs 3, 4, 28, 52, 101, 118, 138 and 180.Equilibrium K leaf/PDMS extrapolated from the uptake kinetics measured over 4 days ranged from 0.075(PCB 180) to 0.371 (PCB 3). The K leaf/PDMS data can readily be converted to fugacity capacities of leaves( Z leaf ) and subsequently leaf/water or leaf/air partition ratios ( K leaf/water and K leaf/air ) using partitioning datafrom the literature. Results of our measurements are within the variability observed for plant/air partitionratios ( K plant/air ) found in the literature. Log K leaf/air from this study ranged from 5.00 (PCB 3) to 8.30(PCB 180) compared to log K plant/air of 3.31 (PCB 3) to 8.88 (PCB 180) found in the literature. The methodwe describe could provide data to characterize the variability in sorptive capacities of leaves that wouldimprove descriptions of uptake of chemicals by leaves in multimedia fate models.

  • 9.
    Brännvall, Evelina
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Kumpiene, Jurate
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Fly ash in landfill top covers: a review2016In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 18, no 1, p. 11-21Article in journal (Refereed)
    Abstract [en]

    Increase of energy recovery from municipal solid waste by incineration results in the increased amounts of incineration residues, such as fly ash, that have to be taken care of. Material properties should define whether fly ash is a waste or a viable resource to be used for various applications. Here, two areas of potential fly ash application are reviewed: the use of fly ash in a landfill top cover either as a liner material or as a soil amendment in vegetation layer. Fly ashes from incineration of three types of fuel are considered: refuse derived fuel (RDF), municipal solid waste incineration (MSWI) and biofuel. Based on the observations, RDF and MSWI fly ash is considered as suitable materials to be used in a landfill top cover liner. Whereas MSWI and biofuel fly ashes based on element availability for plant studies, could be considered suitable for the vegetation layer of the top cover. Responsible application of MSWI ashes is, however, warranted in order to avoid element accumulation in soil and elevation of background values over time.

  • 10. Chilkoor, Govinda
    et al.
    Upadhyayula, Venkata Krishna Kumar
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Gadhamshetty, Venkataramana
    Koratkar, Nikhil
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Sustainability of renewable fuel infrastructure: a screening LCA case study of anticorrosive graphene oxide epoxy liners in steel tanks for the storage of biodiesel and its blends2017In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 19, no 2, p. 141-153Article in journal (Refereed)
    Abstract [en]

    Biodiesel is a widely used fuel that meets the renewable fuel standards developed under Energy Policy Act of 2005. However, biodiesel is known to pose a series of abiotic and biotic corrosion risks to storage tanks. A typical practice (incumbent system) used to protect the tanks from the risks include: (i) coat the interior surface of the tank with solvent free epoxy (SFE) liner, and (ii) add a biocide in the tank. We present a screening-level, life cycle assessment study to evaluate and compare the environmental performance of graphene-oxide (GO)-epoxy (GOE) liner with the incumbent system. TRACI is used as an impact assessment tool to model midpoint environmental impacts for the ten categories: global warming potential (GWP, kg CO2 eq.); acidification potential (AP, kg SO2 eq.); potential human health damage impacts due to carcinogens (HH-CP, CTUh) and non-carcinogens (HH-NCP, CTUh); potential respiratory effects (REP, kg PM2.5 eq); eutrophication potential (EP, kg N eq); ozone depletion potential (ODP kg CFC-11 eq); ecotoxicity potential (ETXP, CTUe); smog formation potential (SFP kg O3 eq); and fossil fuel depletion potential (FFDP MJ surplus). The equivalent functional unit of the LCA study is designed to protect the 30 m2 of the interior surface (unalloyed steel sheet) of a 10,000 liters biodiesel tank against abiotic and biotic corrosion during its service life of 20 years. Overall, this LCA study highlights an improved environmental performance for the GOE liner compared to the incumbent system; GOE-liner system showed: 91% lower ODP impacts; 59% smaller for REP; 62% smaller for AP; 67-69% smaller for GWP and HH-CP; 72-76% smaller for EP, SFP, and FFDP; and 81-83% smaller for ETXP and HH-NCP categories. The scenario analysis study reveals that these potential impacts change by less than 15% when the GOE liners are functionalized with silanized-GO nanosheets or GO-reinforced, polyvinyl carbazole to improve the antimicrobial properties. The results from uncertainty analysis indicate that the impacts for the incumbent system are more sensitive to changes in key modeling parameters compared to that for GOE liner system.

  • 11.
    Coll, Claudia
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Lindim, Claudia
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Sobek, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Sohn, Michael D.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Prospects for finding Junge variability-lifetime relationships for micropollutants in the Danube river2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 9, p. 1489-1497Article in journal (Refereed)
    Abstract [en]

    Persistence of chemical pollutants is difficult to measure in the field. Junge variability-lifetime relationships, correlating the relative standard deviation of measured concentrations with residence time, have been used to estimate persistence of air pollutants. Junge relationships for micropollutants in rivers could provide evidence that half-lives of compounds estimated from laboratory and field data are representative of half-lives in a specific system, location and time. Here, we explore the hypothesis that Junge relationships could exist for micropollutants in the Danube river using: (1) concentrations of six hypothetical chemicals modeled using the STREAM-EU fate and transport model, and (2) concentrations of nine micropollutants measured in the third Joint Danube Survey (JDS3) combined with biodegradation half-lives reported in the literature. Using STREAM-EU, we found that spatial and temporal variability in modeled concentrations was inversely correlated with half-life for the four micropollutants with half-lives <= 90 days. For these four modeled micropollutants, we found Junge relationships with slopes significantly different from zero in the temporal variability of concentrations at 88% of the 67 JDS3 measurement sites, and in the spatial variability of concentrations on 36% out of 365 modeled days. A Junge relationship significant at the 95% confidence level was not found in the spatial variability of nine micropollutants measured in the JDS3, nor in STREAM-EU-modeled concentrations extracted for the dates and locations of the JDS3. Nevertheless, our model scenarios suggest that Junge relationships might be found in future measurements of spatial and temporal variability of micropollutants, especially in temporal variability of pollutants measured downstream in the Danube river.

  • 12.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Goldenman, Gretta
    Herzke, Dorte
    Lohmann, Rainer
    Miller, Mark
    Ng, Carla A.
    Patton, Sharyle
    Scheringer, Martin
    Trier, Xenia
    Vierke, Lena
    Wang, Zhanyun
    DeWitt, Jamie C.
    The concept of essential use for determining when uses of PFASs can be phased out2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 11, p. 1803-1815Article, review/survey (Refereed)
    Abstract [en]

    Because of the extreme persistence of per- and polyfluoroalkyl substances (PFASs) and their associated risks, the Madrid Statement argues for stopping their use where they are deemed not essential or when safer alternatives exist. To determine when uses of PFASs have an essential function in modern society, and when they do not, is not an easy task. Here, we: (1) develop the concept of essential use based on an existing approach described in the Montreal Protocol, (2) apply the concept to various uses of PFASs to determine the feasibility of elimination or substitution of PFASs in each use category, and (3) outline the challenges for phasing out uses of PFASs in society. In brief, we developed three distinct categories to describe the different levels of essentiality of individual uses. A phase-out of many uses of PFASs can be implemented because they are not necessary for the betterment of society in terms of health and safety, or because functional alternatives are currently available that can be substituted into these products or applications. Some specific uses of PFASs would be considered essential because they provide for vital functions and are currently without established alternatives. However, this essentiality should not be considered as permanent; rather, constant efforts are needed to search for alternatives. We provide a description of several ongoing uses of PFASs and discuss whether these uses are essential or non-essential according to the three essentiality categories. It is not possible to describe each use case of PFASs in detail in this single article. For follow-up work, we suggest further refining the assessment of the use cases of PFASs covered here, where necessary, and expanding the application of this concept to all other uses of PFASs. The concept of essential use can also be applied in the management of other chemicals, or groups of chemicals, of concern.

  • 13.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Ng, Carla A.
    Wang, Zhanyun
    Scheringer, Martin
    Why is high persistence alone a major cause of concern?2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 5, p. 781-792Article, review/survey (Refereed)
    Abstract [en]

    Persistence is a hazard criterion for chemicals enshrined in chemical regulation worldwide. In this paper, we argue that the higher the persistence of a chemical, the greater the emphasis that it should be given in chemicals assessment and decision making. We provide case studies for three classes of highly persistent chemicals (chlorofluorocarbons, polychlorinated biphenyls, and per-and polyfluoroalkyl substances) to exemplify problems unique to highly persistent chemicals, despite their otherwise diverse properties. Many well-known historical chemical pollution problems were the result of the release of highly persistent chemicals. Using evaluative modeling calculations, we demonstrate that if a chemical is highly persistent, its continuous release will lead to continuously increasing contamination irrespective of the chemical's physical-chemical properties. We argue that these increasing concentrations will result in increasing probabilities of the occurrence of known and unknown effects and that, once adverse effects are identified, it will take decades, centuries or even longer to reverse contamination and therefore effects. Based on our findings we propose that high persistence alone should be established as a sufficient basis for regulation of a chemical, which we term the P-sufficient approach. We argue that regulation on high persistence alone is not over-precautionary given the historical and ongoing problems that persistent chemicals have caused. Regulation of highly persistent chemicals, for example by restriction of emissions, would not only be precautionary, but would serve to prevent poorly reversible future impacts.

  • 14.
    de Wit, Cynthia A.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Johansson, Anna-Karin
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Sellström, Ulla
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Lindberg, Peter
    Mass balance study of brominated flame retardants in female captive peregrine falcons2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 7, p. 1115-1131Article in journal (Refereed)
    Abstract [en]

    Little is known about brominated flame retardant (BFR) dynamics in birds, especially large molecules such as decabromodiphenyl ether (BDE-209). In particular, bioaccumulation from food and transfer dynamics to eggs are poorly understood. Therefore, an input-output mass balance study of tri-decaBDEs, DBDPE and HBCDD was performed in three female peregrine falcons from a captive breeding program by analyzing their naturally contaminated food (quail, chicken (cockerels)), plasma, feces and eggs. Predominant BFRs in cockerels and quail were BDE-209 and DBDPE, as well as HBCDD in quail. The predominant BFRs found in falcon plasma were BDE-209, -153 and -183, in eggs, HBCDD, BDE-209 and -153 and in feces, BDE-209. Mean absorption efficiencies (AE) for the tetra-octabrominated BDEs ranged from 84-100% and 70% for HBCDD. The AEs for BDE-206, -207, -208 and -209 varied due to the large variability seen for feces fluxes. All egg/plasma ratios for BDEs were similar and greater than one (range 1.1-2.7), including for BDE-209, indicating efficient transfer from females to the eggs. Excretion via egg-laying was approximately 6.0-29% of the initial, pre-breeding body burden of individual penta-decaBDE congeners, (15-45% for BDE-206). HBCDD was not detected in plasma but was found in eggs, also indicating efficient transfer and excretion via eggs. Input fluxes from food exceeded the output fluxes (feces, eggs) indicating considerable metabolism for tetra-octaBDEs, possibly also for the nona-decaBDEs and HBCDD. Bioaccumulation factors calculated from lipid weight concentrations in plasma and food (BAF(p)) were highest for BDE-208 (31), -153 (23), -209 (19) and -207 (16) and from eggs and food (BAF(e)), were highest for HBCDD (140), BDE-153 (41), -208 (42), BDE-207 (24) and BDE-209 (21). BAF(e) and BAF(p) values were below 10 for BDE-47, -99 and -100. For one falcon, egg results were available from three different years and estimated half-lives were 65 d (BDE-99), 624 d (BDE-153), 31 d (BDE-154), 349 d (BDE-183), 77 d (BDE-196) and 89 d (BDE-197).

  • 15. Di Guardo, Antonio
    et al.
    Gouin, Todd
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Scheringer, Martin
    Environmental fate and exposure models: advances and challenges in 21st century chemical risk assessment2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 1, p. 58-71Article, review/survey (Refereed)
    Abstract [en]

    Environmental fate and exposure models are a powerful means to integrate information on chemicals, their partitioning and degradation behaviour, the environmental scenario and the emissions in order to compile a picture of chemical distribution and fluxes in the multimedia environment. A 1995 pioneering book, resulting from a series of workshops among model developers and users, reported the main advantages and identified needs for research in the field of multimedia fate models. Considerable efforts were devoted to their improvement in the past 25 years and many aspects were refined; notably the inclusion of nanomaterials among the modelled substances, the development of models at different spatial and temporal scales, the estimation of chemical properties and emission data, the incorporation of additional environmental media and processes, the integration of sensitivity and uncertainty analysis in the simulations. However, some challenging issues remain and require research efforts and attention: the need of methods to estimate partition coefficients for polar and ionizable chemical in the environment, a better description of bioavailability in different environments as well as the requirement of injecting more ecological realism in exposure predictions to account for the diversity of ecosystem structures and functions in risk assessment. Finally, to transfer new scientific developments into the realm of regulatory risk assessment, we propose the formation of expert groups that compare, discuss and recommend model modifications and updates and help develop practical tools for risk assessment. Environmental significance Multimedia environmental fate models are regularly employed in the risk assessment of chemicals. They historically evolved from simple approaches to more refined and integrated modeling tools, often provided as part of a tiered strategy. Much work has been devoted to improving various aspects at the process and environmental description levels, but some issues need further research and model development, such as the capability to properly simulate the behaviour of polar and ionizable chemicals in the environment, the biovailability of chemicals in aquatic and terrestrial environments, and variability in time and space to account for more ecological relevance. At the same time, it is important to avoid paralysis by analysis and develop practical tools for regulatory risk assessment that are fit for purpose. We propose the formation of expert groups to address this task.

  • 16.
    Gewert, Berit
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Plassmann, Merle M.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Pathways for degradation of plastic polymers floating in the marine environment2015In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 17, no 9, p. 1513-1521Article, review/survey (Refereed)
    Abstract [en]

    Each year vast amounts of plastic are produced worldwide. When released to the environment, plastics accumulate, and plastic debris in the world's oceans is of particular environmental concern. More than 60% of all floating debris in the oceans is plastic and amounts are increasing each year. Plastic polymers in the marine environment are exposed to sunlight, oxidants and physical stress, and over time they weather and degrade. The degradation processes and products must be understood to detect and evaluate potential environmental hazards. Some attention has been drawn to additives and persistent organic pollutants that sorb to the plastic surface, but so far the chemicals generated by degradation of the plastic polymers themselves have not been well studied from an environmental perspective. In this paper we review available information about the degradation pathways and chemicals that are formed by degradation of the six plastic types that are most widely used in Europe. We extrapolate that information to likely pathways and possible degradation products under environmental conditions found on the oceans' surface. The potential degradation pathways and products depend on the polymer type. UV-radiation and oxygen are the most important factors that initiate degradation of polymers with a carbon-carbon backbone, leading to chain scission. Smaller polymer fragments formed by chain scission are more susceptible to biodegradation and therefore abiotic degradation is expected to precede biodegradation. When heteroatoms are present in the main chain of a polymer, degradation proceeds by photo-oxidation, hydrolysis, and biodegradation. Degradation of plastic polymers can lead to low molecular weight polymer fragments, like monomers and oligomers, and formation of new end groups, especially carboxylic acids.

  • 17. Jaeger, Anna
    et al.
    Coll, Claudia
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Posselt, Malte
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Mechelke, Jonas
    Rutere, Cyrus
    Betterle, Andrea
    Raza, Muhammad
    Mehrtens, Anne
    Meinikmann, Karin
    Portmann, Andrea
    Singh, Tanu
    Blaen, Phillip J.
    Krause, Stefan
    Horn, Marcus A.
    Hollender, Juliane
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Sobek, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Lewandowski, Joerg
    Using recirculating flumes and a response surface model to investigate the role of hyporheic exchange and bacterial diversity on micropollutant half-lives2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 12, p. 2093-2108Article in journal (Refereed)
    Abstract [en]

    Enhancing the understanding of the fate of wastewater-derived organic micropollutants in rivers is crucial to improve risk assessment, regulatory decision making and river management. Hyporheic exchange and sediment bacterial diversity are two factors gaining increasing importance as drivers for micropollutant degradation, but are complex to study in field experiments and usually ignored in laboratory tests aimed to estimate environmental half-lives. Flume mesocosms are useful to investigate micropollutant degradation processes, bridging the gap between the field and batch experiments. However, few studies have used flumes in this context. We present a novel experimental setup using 20 recirculating flumes and a response surface model to study the influence of hyporheic exchange and sediment bacterial diversity on half-lives of the anti-epileptic drug carbamazepine (CBZ) and the artificial sweetener acesulfame (ACS). The effect of bedform-induced hyporheic exchange was tested by three treatment levels differing in number of bedforms (0, 3 and 6). Three levels of sediment bacterial diversity were obtained by diluting sediment from the River Erpe in Berlin, Germany, with sand (1 : 10, 1 : 1000 and 1 : 100 000). Our results show that ACS half-lives were significantly influenced by sediment dilution and number of bedforms. Half-lives of CBZ were higher than ACS, and were significantly affected only by the sediment dilution variable, and thus by bacterial diversity. Our results show that (1) the flume-setup is a useful tool to study the fate of micropollutants in rivers, and that (2) higher hyporheic exchange and bacterial diversity in the sediment can increase the degradation of micropollutants in rivers.

  • 18. Jahnke, Annika
    et al.
    Sobek, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Bergmann, Melanie
    Bräunig, Jennifer
    Landmann, Madlen
    Schäfer, Sabine
    Escher, Beate I.
    Emerging investigator series: effect-based characterization of mixtures of environmental pollutants in diverse sediments2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 12, p. 1667-1679Article in journal (Refereed)
    Abstract [en]

    This study investigated whether cell-based bioassays were suitable to characterize profiles of mixture effects of hydrophobic pollutants in multiple sediments covering remote Arctic and tropical sites to highly populated sites in Europe and Australia. The total contamination was determined after total solvent extraction and the bioavailable contamination after silicone-based passive equilibrium sampling. In addition to cytotoxicity, we observed specific responses in cell-based reporter gene bioassays: activation of metabolic enzymes (arylhydrocarbon receptor: AhR, peroxisome proliferator activated receptor gamma: PPAR) and adaptive stress responses (oxidative stress response: AREc32). No mixture effects were found for effects on the estrogen, androgen, progesterone and glucocorticoid receptors, or they were masked by cytotoxicity. The bioanalytical equivalent concentrations (BEQ) spanned several orders of magnitude for each bioassay. The bioavailable BEQs (passive equilibrium sampling) typically were 10-100 times and up to 420 times lower than the total BEQ (solvent extraction) for the AhR and AREc32 assays, indicating that the readily desorbing fraction of the bioactive chemicals was substantially lower than the fraction bound strongly to the sediment sorptive phases. Contrarily, the bioavailable BEQ in the PPAR assay was within a factor of five of the total BEQ. We identified several hotspots of contamination in Europe and established background contamination levels in the Arctic and Australia.

  • 19.
    Johansson, Jana H.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Salter, Matthew E.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Acosta Navarro, Juan Camilo
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Leck, Caroline
    Stockholm University, Faculty of Science, Department of Meteorology .
    Nilsson, E. Douglas
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Global transport of perfluoroalkyl acids via sea spray aerosol2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 4, p. 635-649Article in journal (Refereed)
    Abstract [en]

    Perfluoroalkyl acids (PFAAs) are persistent organic pollutants found throughout the world's oceans. Previous research suggests that long-range atmospheric transport of these substances may be substantial. However, it remains unclear what the main sources of PFAAs to the atmosphere are. We have used a laboratory sea spray chamber to study water-to-air transfer of 11 PFAAs via sea spray aerosol (SSA). We observed significant enrichment of all PFAAs relative to sodium in the SSA generated. The highest enrichment was observed in aerosols with aerodynamic diameter < 1.6 mm, which had aerosol PFAA concentrations up to similar to 62 000 times higher than the PFAA water concentrations in the chamber. In surface microlayer samples collected from the sea spray chamber, the enrichment of the substances investigated was orders of magnitude smaller than the enrichment observed in the aerosols. In experiments with mixtures of structural isomers, a lower contribution of branched PFAA isomers was observed in the surface microlayer compared to the bulk water. However, no clear trend was observed in the comparison of structural isomers in SSA and bulk water. Using the measured enrichment factors of perfluorooctanoic acid and perfluorooctane sulfonic acid versus sodium we have estimated global annual emissions of these substances to the atmosphere via SSA as well as their global annual deposition to land areas. Our experiments suggest that SSA may currently be an important source of these substances to the atmosphere and, over certain areas, to terrestrial environments.

  • 20.
    Johansson, Jana H.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Shi, Yali
    Salter, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Spatial variation in the atmospheric deposition of perfluoroalkyl acids: source elucidation through analysis of isomer patterns2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 7, p. 997-1006Article in journal (Refereed)
    Abstract [en]

    To evaluate the relevance of different proposed sources of perfluoroalkyl acids (PFAAs) to air, their isomer patterns were analyzed in deposition samples collected from five geographical locations: two urban sites in China (>360 km from known operational fluorochemical manufacturing facilities), one remote marine site in the Azores archipelago and two Swedish sites representing urban and background conditions. Despite variable contributions from linear perfluorooctanoic acid (PFOA) in the samples, the pattern of branched PFOA isomers was similar to those of technical standards manufactured using electrochemical fluorination (ECF). This indicates that atmospheric fate processes have little influence on the isomer profiles of PFOA and that the relative contribution of PFOA manufactured using ECF (typically 20-26% branched isomers) and telomerization (typically one single linear isomer) can be determined in atmospheric deposition samples by analyzing the proportions of branched and linear isomers. In Chinese samples, branched isomers contributed 15-25% to the total loading of PFOA, indicating that the samples were dominated by ECF PFOA. Samples in the Azores had 8-10% contribution from branched PFOA isomers, indicating an approximately equal influence of ECF and telomer sources. Only three of the samples collected in Sweden displayed a quantifiable contribution from branched PFOA isomers (8-13% of overall PFOA loading in the samples). One branched PFNA isomer was observed in samples from the marine sites. Direct manufacturing discharges, transport of sea spray aerosols and degradation of precursors are all suggested to be contributing sources, albeit to different extents, to PFAAs in air at the different geographical locations where precipitation was sampled.

  • 21.
    Koch, Alina
    et al.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Jonsson, Micael
    Department of Ecology and Environmental Science, Umeå University, Umeå, Sweden.
    Ahrens, Lutz
    Section for Organic Environmental Chemistry and Ecotoxicology, Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU), Uppsala, Sweden.
    Wang, Thanh
    Örebro University, School of Science and Technology.
    Point source characterization of per- and polyfluoroalkyl substances (PFASs) and extractable organofluorine (EOF) in freshwater and aquatic invertebrates2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 11, p. 1887-1898Article in journal (Refereed)
    Abstract [en]

    Major point sources of per- and polyfluoroalkyl substances (PFASs) cause ubiquitous spread of PFASs in the environment. In this study, surface water and aquatic invertebrates at three Swedish sites impacted by PFAS point sources were characterized, using homologue, isomer and extractable organofluorine (EOF) profiling as well as estimation of bioaccumulation factors (BAFs) and mass discharge. Two sites were impacted by fire training (sites A and R) and the third by industrial runoff (site K). Mean Σ25PFASs concentration in water was 1920 ng L-1 at site R (n = 3), which was more than 20- and 10-fold higher than those from sites A and K, respectively. PFOS was the most predominant PFAS in all waters samples, constituting 29-79% of Σ25PFAS concentrations. Several branched isomers were detected and they substantially contributed to concentrations in surface water (e.g. 49-78% of ΣPFOS) and aquatic invertebrates (e.g. 15-28% of ΣPFOS). BAFs in the aquatic invertebrates indicated higher bioaccumulation for long chain PFASs and lower bioaccumulation for branched PFOS isomers compared to linear PFOS. EOF mass balance showed that Σ25target PFASs in water could explain up to 55% of EOF at site R. However, larger proportions of EOF (>92%) remained unknown in water from sites A and K. Mass discharges were for the first time estimated for EOF and revealed that high amounts of EOF (e.g. 8.2 g F day-1 at site A) could be transported by water to recipient water bodies relative to Σ25PFASs (e.g. 0.15 g day-1 at site A). Overall, we showed that composition profiling, BAFs and EOF mass balance can improve the characterization of PFASs around point sources.

  • 22. Koch, Alina
    et al.
    Kärrman, Anna
    Yeung, Leo W. Y.
    Jonsson, Micael
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Ahrens, Lutz
    Wang, Thanh
    Point source characterization of per- and polyfluoroalkyl substances (PFASs) and extractable organofluorine (EOF) in freshwater and aquatic invertebrates2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 11, p. 1887-1898Article in journal (Refereed)
    Abstract [en]

    Major point sources of per- and polyfluoroalkyl substances (PFASs) cause ubiquitous spread of PFASs in the environment. In this study, surface water and aquatic invertebrates at three Swedish sites impacted by PFAS point sources were characterized, using homologue, isomer and extractable organofluorine (EOF) profiling as well as estimation of bioaccumulation factors (BAFs) and mass discharge. Two sites were impacted by fire training (sites A and R) and the third by industrial runoff (site K). Mean Σ25PFASs concentration in water was 1920 ng L−1 at site R (n = 3), which was more than 20- and 10-fold higher than those from sites A and K, respectively. PFOS was the most predominant PFAS in all waters samples, constituting 29–79% of Σ25PFAS concentrations. Several branched isomers were detected and they substantially contributed to concentrations in surface water (e.g. 49–78% of ΣPFOS) and aquatic invertebrates (e.g. 15–28% of ΣPFOS). BAFs in the aquatic invertebrates indicated higher bioaccumulation for long chain PFASs and lower bioaccumulation for branched PFOS isomers compared to linear PFOS. EOF mass balance showed that Σ25target PFASs in water could explain up to 55% of EOF at site R. However, larger proportions of EOF (>92%) remained unknown in water from sites A and K. Mass discharges were for the first time estimated for EOF and revealed that high amounts of EOF (e.g. 8.2 g F day−1 at site A) could be transported by water to recipient water bodies relative to Σ25PFASs (e.g. 0.15 g day−1 at site A). Overall, we showed that composition profiling, BAFs and EOF mass balance can improve the characterization of PFASs around point sources.

  • 23.
    Li, Zhe
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Kaserzon, Sarit L.
    Plassmann, Merle M.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Sobek, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Gómez Ramos, Maria José
    Radke, Michael
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    A strategic screening approach to identify transformation products of organic micropollutants formed in natural waters2017In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 19, no 4, p. 488-498Article in journal (Refereed)
    Abstract [en]

    Many transformation products (TPs) from organic micropollutants are not included in routine environmental monitoring programs due to limited knowledge of their occurrence and fate. An efficient method to identify and prioritize critical compounds in terms of environmental relevance is needed. In this study, we applied a strategic screening approach based on a case-control concept to identify TPs formed along wastewater-impacted rivers. Time-integrated samples were collected over one week at both ends of a river stretch downstream of a wastewater treatment plant (WWTP) outfall and were analyzed by ultrahigh performance liquid chromatography interfaced with quadrupole time-of-flight mass spectrometry (UHPLC-QToF-MS/MS). The screening procedure of the high-resolution MS (HRMS) datasets consisted of three major steps: (i) screening for parent compounds (PCs) attenuated along the stretch; (ii) prediction of potential TPs from these PCs; and (iii) screening for TPs from this list with an increasing trend along the stretch. In total, 32 PCs decreased along the investigated river stretches. From these PCs, eight TPs had increasing concentrations along the studied stretches and could be tentatively identified. The identification of one TP (benzamide) was confirmed by its corresponding reference standard, while no standards were available for the remaining TPs.

  • 24.
    Li, Zhe
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Undeman, Emma
    Stockholm University, Faculty of Science, Stockholm University Baltic Sea Centre.
    Papa, Ester
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    High-throughput evaluation of organic contaminant removal efficiency in a wastewater treatment plant using direct injection UHPLC-Orbitrap-MS/MS2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 3, p. 561-571Article in journal (Refereed)
    Abstract [en]

    The removal efficiency (RE) of organic contaminants in wastewater treatment plants (WWTPs) is a major determinant of the environmental impact of these contaminants. However, RE data are available for only a few chemicals due to the time and cost required for conventional target analysis. In the present study, we applied non-target screening analysis to evaluate the RE of polar contaminants, by analyzing influent and effluent samples from a Swedish WWTP with direct injection UHPLC-Orbitrap-MS/MS. Matrix effects were evaluated by spiking the samples with isotope-labeled standards of 40 polar contaminants. For 85% of the compounds, the matrix effects in the influent and effluent were not significantly different. Approximately 10000 compounds were detected in the wastewater, of which 319 were identified by using the online database mzCloud. Level 1 identification confidence was achieved for 31 compounds for which we had reference standards, and level 2 was achieved for the remainder. RE was calculated from the ratio of the peak areas in the influent and the effluent from the non-target analysis. Good agreement was found with RE determined from the target analysis of the target compounds. The method generated reliable estimates of RE for large numbers of contaminants with comparatively low effort and is foreseen to be particularly useful in applications where information on a large number of chemicals is needed.

  • 25.
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Can the Stockholm convention address the spectrum of chemicals currently under regulatory scrutiny? Advocating a more prominent role for modeling in POP screening assessment2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 1, p. 32-37Article in journal (Refereed)
    Abstract [en]

    Frameworks for chemical regulation are based on the science at the time they were written. Today some regulations are being applied to a much broader spectrum of chemicals than we had knowledge of when the regulations were written. This entails a risk that the regulations are being used outside of their chemical application domain. This question is explored using the POP screening assessment in the Stockholm convention, which was developed 20 years ago. Using perfluorinated alkyl acids (PFAAs) as an example, it is shown that the assessment can lead to false negative conclusions. A second case study using octamethylcyclotetrasiloxane (D4) illustrates that there is also a risk of false positives. The risk for false negative classification of PFAAs is due to the inclusion of a screening criterion - bioaccumulation - that is not a requirement for adverse effects of chemicals in remote regions. For D4 the risk of false positive classification stems from the four screening criteria (persistence, bioaccumulation, long-range transport, and adverse effects) applying to different environmental media/compartments. The major lesson is that applying the POP screening procedure to the broad spectrum of chemicals in modern commerce will require that we rely less on the individual screening criteria and more on the comparison of estimated exposure and the thresholds for effects stipulated in Annex D, paragraph 2 of the convention. Models have an important role to play in this context and should become more strongly integrated into the POP screening process. Environmental significance This paper illustrates some limitations of the Stockholm convention, one of the most important tools for regulation of chemicals at the global scale. It shows that the criteria to screen for new POPs can lead to false negative and false positive conclusions when applied to chemicals that lie outside of the chemical domain of the screening procedure. This problem is clearly attributed to breaking down the complex processes of chemical transport, fate and exposure into simple indicators, a strategy which cannot be successful across a wide spectrum of chemicals. Integrated transport, fate and exposure models are advocated as a solution.

  • 26.
    McLachlan, Michael S.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Undeman, Emma
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Stockholm University, Faculty of Science, Stockholm University Baltic Sea Centre.
    Zhao, Fangyuan
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Predicting global scale exposure of humans to PCB 153 from historical emissions2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 5, p. 747-756Article in journal (Refereed)
    Abstract [en]

    Predicting human exposure to an environmental contaminant based on its emissions is one of the great challenges of environmental chemistry. It has been done successfully on a local or regional scale for some persistent organic pollutants. Here we assess whether it can be done at a global scale, using PCB 153 as a test chemical. The global multimedia fate model BETR Global and the human exposure model ACC-HUMAN were employed to predict the concentration of PCB 153 in human milk for 56 countries around the world from a global historical emissions scenario. The modeled concentrations were compared with measurements in pooled human milk samples from the UNEP/WHO Global Monitoring Plan. The modeled and measured concentrations were highly correlated (r = 0.76, p < 0.0001), and the concentrations were predicted within a factor of 4 for 49 of 78 observations. Modeled concentrations of PCB 153 in human milk were higher than measurements for some European countries, which may reflect weaknesses in the assumptions made for food sourcing and an underestimation of the rate of decrease of concentrations in air during the last decades. Conversely, modeled concentrations were lower than measurements in West African countries, and more work is needed to characterize exposure vectors in this region.

  • 27.
    Mustajärvi, Lukas
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Eriksson-Wiklund, Ann-Kristin
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Gorokhova, Elena
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Jahnke, Annika
    Sobek, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Transferring mixtures of chemicals from sediment to a bioassay using silicone-based passive sampling and dosing2017In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 19, no 11, p. 1404-1413Article in journal (Refereed)
    Abstract [en]

    Environmental mixtures of chemicals consist of a countless number of compounds with unknown identity and quantity. Yet, chemical regulation is mainly built around the assessment of single chemicals. Existing frameworks for assessing the toxicity of mixtures require that both the chemical composition and quantity are known. Quantitative analyses of the chemical composition of environmental mixtures are however extremely challenging and resource-demanding. Bioassays may therefore serve as a useful approach for investigating the combined toxicity of environmental mixtures of chemicals in a cost-efficient and holistic manner. In this study, an unknown environmental mixture of bioavailable semi-hydrophobic to hydrophobic chemicals was sampled from a contaminated sediment in a coastal Baltic Sea area using silicone polydimethylsiloxane (PDMS) as an equilibrium passive sampler. The chemical mixture was transferred to a PDMS-based passive dosing system, and its applicability was demonstrated using green algae Tetraselmis suecica in a cell viability assay. The proportion of dead cells increased significantly with increasing exposure level and in a dose–response manner. At an ambient concentration, the proportion of dead cells in the population was nearly doubled compared to the control; however, the difference was non-significant due to high inter-replicate variability and a low number of replicates. The validation of the test system regarding equilibrium sampling, loading efficiency into the passive dosing polymer, stability of the mixture composition, and low algal mortality in control treatments demonstrates that combining equilibrium passive sampling and passive dosing is a promising tool for investigating the toxicity of bioavailable semi-hydrophobic and hydrophobic chemicals in complex environmental mixtures.

  • 28.
    Newton, Seth
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Bidleman, Terry
    Bergknut, Magnus
    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, E-ISSN 2050-7895, 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°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.

  • 29.
    Nordqvist, Kerstin
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Architecture and Water.
    Galfi, Helen
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Architecture and Water.
    Österlund, Helene
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Architecture and Water.
    Marsalek, Jiri
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Architecture and Water.
    Westerlund, Camilla
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Architecture and Water.
    Viklander, Maria
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Architecture and Water.
    Measuring solid concentrations in urban stormwater and snowmelt: a new operational procedure2014In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 16, no 9, p. 2172-2183Article in journal (Refereed)
    Abstract [en]

    A comparative study of five methods measuring suspended sediment or solid concentrations in water–sediment mixtures indicated that, depending on the method used, broadly varying results can be obtained. For water–sediment mixtures containing sand size particles, the standard TSS method produced negatively biased results, accounting for 0 to 90% of the present solids; the negative bias directly depended on the magnitude of the sand fraction in the water–sediment mixture. The main reason for the differences between the TSS and the rest of the methods laid in the handling of samples; in the former methods, whole samples were analysed, whereas the TSS analysis was performed on sub-samples withdrawn from the water sample, the withdrawal process tending to exclude large particles. The methods using whole water–solid samples, rather than aliquots withdrawn from such samples, produced accurate estimates of solid concentrations, with a fairly good precision. Two whole-sample methods were studied in detail, a slightly modified standard SSC-B method and the newly proposed operational procedure referred to as the Multiple Filter Procedure (MFP), using three filters arranged in a series with decreasing pore sizes (25, 1.6 and 0.45 µm). Both methods assessed accurately concentrations of solids in a broad range of concentrations (200–8000 mg L−1) and particle sizes (0.063–4.0 mm). The newly introduced MFP was in good agreement with the SSC procedure, the differences between the two procedures not exceeding the standard bias defined for the SSC-B method. The precision of both SSC and MFP was generally better than ±10%. Consequently, these methods should be used when the total mass of transported solids is of interest.

  • 30. Nyberg, Elisabeth
    et al.
    Awad, Raed
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Bignert, Anders
    Ek, Caroline
    Sallsten, Gerd
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Inter-individual, inter-city, and temporal trends of per- and polyfluoroalkyl substances in human milk from Swedish mothers between 1972 and 20162018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 8Article in journal (Refereed)
    Abstract [en]

    Inter-individual, inter-city, and temporal trends of 19 per- and polyfluoroalkyl substances (PFASs) were investigated in human milk collected in Stockholm (1972-2016) and Gothenburg (2007-2015), Sweden. The concentrations of perfluorohexane sulfonate (PFHxS), perfluorononanoate (PFNA), perfluorodecanoate (PFDA), perfluoroundecanoate (PFUnDA), and perfluorotridecanoate (PFTrDA) in human milk from Stockholm increased significantly over the entire monitoring periods, whereas branched (Br) and linear (L) isomers of perfluorooctane sulfonamide (FOSA) decreased. In human milk from Gothenburg, significant downward trends were detected for perfluorododecanoate (PFDoDA), PFHxS and Br-perfluorooctane sulfonate (Br-PFOS) over the last decade. This declining trend was also observed for perfluorohexanoate (PFHxA), PFHxS, perfluorooctanoate (PFOA) and Br-PFOS in Stockholm over the same time period. No significant differences were observed in concentrations or relative PFAS profiles between Stockholm and Gothenburg. However, a comparison of the PFAS profile in Stockholm milk revealed distinct profiles for the time periods 1972-1996, 2000-2012, and 2013-2016, reflecting a shift in exposure over time. The lower bound estimated daily intake (EDI) for Sigma PFAS concentrations in infants ranged from 7.1-40 ng per kg body weight per day (ng/kg bw/d) in Stockholm and from 5.2-25 ng/kg bw/d in Gothenburg over the studied time period, consistent with other European countries. Overall these data indicate that exposure to some legacy PFASs via breastmilk is declining, presumably as a result of regulation and phase-out initiatives. However, increasing concentrations for other PFASs and a shift in the overall PFAS profile in recent years may pose an ongoing health risk to infants.

  • 31. Okkenhaug, G
    et al.
    Almas, A R
    Morin, Nicolas
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Norwegian Geotechnical Institute (NGI), Oslo, Norway .
    Hale, S E
    Arp, H P H
    The presence and leachability of antimony in different wastes and waste handling facilities in Norway2015In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 17, no 11, p. 1880-1891Article in journal (Refereed)
    Abstract [en]

    The environmental behaviour of antimony (Sb) is gathering attention due to its increasingly extensive use in various products, particularly in plastics. Because of this it may be expected that plastic waste is an emission source for Sb in the environment. This study presents a comprehensive field investigation of Sb concentrations in diverse types of waste from waste handling facilities in Norway. The wastes included waste electrical and electronic equipment (WEEE), glass, vehicle fluff, combustibles, bottom ash, fly ash and digested sludge. The highest solid Sb concentrations were found in WEEE and vehicle plastic (from 1238 to 1715 mg kg−1) and vehicle fluff (from 34 to 4565 mg kg−1). The type of acid used to digest the diverse solid waste materials was also tested. It was found that HNO3:HCl extraction gave substantially lower, non-quantitative yields compared to HNO3:HF. The highest water-leachable concentration for wastes when mixed with water at a 1:10 ratio were observed for plastic (from 0.6 to 2.0 mg kg−1) and bottom ash (from 0.4 to 0.8 mg kg−1). For all of the considered waste fractions, Sb(V) was the dominant species in the leachates, even though Sb(III) as Sb2O3 is mainly used in plastics and other products, indicating rapid oxidation in water. This study also presents for the first time a comparison of Sb concentrations in leachate at waste handling facilities using both active grab samples and DGT passive samples. Grab samples target the total suspended Sb, whereas DGT targets the sum of free- and other chemically labile species. The grab sample concentrations (from 0.5 to 50 μg L−1) were lower than the predicted no-effect concentration (PNEC) of 113 μg L−1. The DGT concentrations were substantially lower (from 0.05 to 9.93 μg L−1) than the grab samples, indicating much of the Sb is present in a non-available colloidal form. In addition, air samples were taken from the chimney and areas within combustible waste incinerators, as well as from the vent of WEEE sorting facility. The WEEE vent had the highest Sb concentration (from <100 to 2200 ng m−3), which were orders of magnitude higher than the air surrounding the combustible shredder (from 25 to 217 ng m−3), and the incinerator chimney (from <30 to 100 ng m−3). From these results, it seems evident that Sb from waste is not an environmental concern in Norway, and that Sb is mostly readily recovered from plastic and bottom ash.

  • 32. Oltmanns, J.
    et al.
    Licht, O.
    Bitsch, A.
    Bohlen, M. -L.
    Escher, S. E.
    Silano, V.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Serafimova, R.
    Kass, G. E. N.
    Merten, C.
    Development of a novel scoring system for identifying emerging chemical risks in the food chain2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 2, p. 340-353Article in journal (Refereed)
    Abstract [en]

    The European Food Safety Authority (EFSA) is responsible for risk assessment of all aspects of food safety, including the establishment of procedures aimed at the identification of emerging risks to food safety. Here, a scoring system was developed for identifying chemicals registered under the European REACH Regulation that could be of potential concern in the food chain using the following parameters: (i) environmental release based on maximum aggregated tonnages and environmental release categories; (ii) biodegradation in the environment; (iii) bioaccumulation and in vivo and in vitro toxicity. The screening approach was tested on 100 data-rich chemicals registered under the REACH Regulation at aggregated volumes of at least 1000 tonnes per annum. The results show that substance-specific data generated under the REACH Regulation can be used to identify potential emerging risks in the food chain. After application of the screening procedure, priority chemicals can be identified as potentially emerging risk chemicals through the integration of exposure, environmental fate and toxicity. The default approach is to generate a single total score for each substance using a predefined weighting scenario. However, it is also possible to use a pivot table approach to combine the individual scores in different ways that reflect user-defined priorities, which enables a very flexible, iterative definition of screening criteria. Possible applications of the approaches are discussed using illustrative examples. Either approach can then be followed by in-depth evaluation of priority substances to ensure the identification of substances that present a real emerging chemical risk in the food chain.

  • 33.
    Panagopoulos, Dimitri
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Lawrence Berkeley National Laboratory, USA.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    A critical assessment of the environmental fate of linear and cyclic volatile methylsiloxanes using multimedia fugacity models2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 1, p. 183-194Article in journal (Refereed)
    Abstract [en]

    We apply multimedia models to systematically evaluate the fate profile of cyclic volatile methyl siloxanes (VMS) D-4, D-5 and D-6, and the linear VMS L-4 and L-5 using recently reported measurements of their partition ratios between organic carbon and water (K-OC), their salting out constants (K-s), and their enthalpy of sorption to organic carbon (Delta H-OC). Our assessment follows a multi-stage strategy where the environmental fate of the chemicals is explored in generic regional models with increasing fidelity to the real system and in a region-specific model. Modeled emissions of VMS to air remained in air and were degraded or advected out of the system with overall residence times ranging from 2.4 to 2.5 days, while emissions to water resulted in accumulation in sediment and longer residence times ranging from 29.5 to 1120 days. When emitted to water the modeled residence times of VMS in the sediment exceeded the REACH criterion for persistence in freshwater sediments. Reported K-OC measurements for D-5 differ by 1 log unit, which results in a 500-day difference in the overall residence times calculated in the generic regional modeling. In the specific-region modeling assessment for Adventfjorden, Svalbard in Norway, the different K-OC measurements of D5 resulted in a 200-day difference in overall residence times. Model scenarios that examined combinations of previously published Delta H-OC or enthalpy of phase change between octanol and water (Delta H-OW) for D5 in combination with the range of the K-OC measurements resulted in 1100-days difference in overall residence times. Our results demonstrate that residence times of VMS in aquatic systems are highly sensitive to their degree of sorption to organic carbon, and that residence times of VMS likely exceed several persistence criteria and therefore they cannot be considered as non-persistent. Environmental significance Volatile methylsiloxanes (VMS) are a group of organosilicon chemicals that are used in personal care products and in the production of silicone polymers. VMS have been found at considerable levels in the air, in sediments and in aquatic organisms. We examine the fate of VMS using multimedia models in aquatic environments and we study their residence times in generic and specific environmental scenarios. Our calculations suggest that the residence times of VMS exceed several persistence criteria in aquatic environments and therefore they cannot be regarded as non-persistent chemicals.

  • 34. Pankratova, Nadezda
    et al.
    Crespo, Gaston A.
    Afshar, Majid Ghahraman
    Crespi, Miquel Coll
    Jeanneret, Stephane
    Cherubini, Thomas
    Tercier-Waeber, Mary-Lou
    Pomati, Francesco
    Bakker, Eric
    Potentiometric sensing array for monitoring aquatic systems2015In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 17, no 5, p. 906-914Article in journal (Refereed)
    Abstract [en]

    Since aquatic environments are highly heterogeneous and dynamic, there is the need in aquatic ecosystem monitoring to replace traditional approaches based on periodical sampling followed by laboratory analysis with new automated techniques that allow one to obtain monitoring data with high spatial and temporal resolution. We report here on a potentiometric sensing array based on polymeric membrane materials for the continuous monitoring of nutrients and chemical species relevant for the carbon cycle in freshwater ecosystems. The proposed setup operates autonomously, with measurement, calibration, fluidic control and acquisition triggers all integrated into a self-contained instrument. Experimental validation was performed on an automated monitoring platform on lake Greifensee (Switzerland) using potentiometric sensors selective for hydrogen ions, carbonate, calcium, nitrate and ammonium. Results from the field tests were compared with those obtained by traditional laboratory analysis. A linear correlation between calcium and nitrate activities measured with ISEs and relevant concentrations measured in the laboratory was found, with the slopes corresponding to apparent single ion activity coefficients and. Good correlation between pH values measured with ISE and CTD probes (SD = 0.2 pH) suggests adequate reliability of the methodology. 

  • 35.
    Parajulee, Abha
    et al.
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada.
    Lei, Ying Duan
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada.
    Cao, Xiaoshu
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada.
    McLagan, David S.
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology. Department of Chemistry, University of Toronto, Toronto, Canada .
    Mitchell, Carl P. J.
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada.
    Wania, Frank
    Department of Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Canada.
    Comparing winter-time herbicide behavior and exports in urban, rural, and mixed-use watersheds2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 5, p. 767-779Article in journal (Refereed)
    Abstract [en]

    The presence of pesticides in streams in winter, five to six years following bans on their municipal use suggests that complicated transport behaviour, such as subsurface retention and/or accumulation of pesticides and its release during storms, could be important for understanding recovery time frames following bans or legislation that aim to reduce chemical inputs. We investigated late fall and winter dynamics of four herbicides in paired urban and rural watersheds in Toronto, Canada during rainfall and snowmelt. The range of average concentrations and loads of the sum of atrazine, metolachlor, 2,4-D and mecoprop overlapped in the two types of watersheds, with slightly higher average concentrations in the rural watershed. Relatively consistent herbicide concentration-discharge patterns (i. e. dilution) were observed in the urban sub-watersheds during rainfall, while concentration-discharge patterns were much more variable in the rural watershed. This suggests relatively uniform transport pathways across the urban sub-watersheds, compared to the rural watershed. Concentration-discharge patterns of the neutral herbicides atrazine and metolachlor were similar in both watersheds during snowmelt, though varying discharge patterns resulted in divergent timings of peak concentrations. In contrast, the acidic pesticides 2,4-D and mecoprop, which are primarily associated with urban uses, showed much more variable behavior across both watersheds and merit further investigation. Overall, this work highlights the need to consider pesticide dynamics throughout the year in order to more thoroughly assess the longterm efficacy of legislation governing their use.

  • 36.
    Posselt, Malte
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Jaeger, Anna
    Schaper, Jonas L.
    Radke, Michael
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Determination of polar organic micropollutants in surface and pore water by high-resolution sampling-direct injection-ultra high performance liquid chromatography-tandem mass spectrometry2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 12, p. 1716-1727Article in journal (Refereed)
    Abstract [en]

    Hyporheic zones (HZs) are dynamic and complex transition regions between rivers and aquifers which are thought to play an important role in the attenuation of environmental micropollutants. Non-steady state and small-scale hyporheic processes which affect micropollutants in the HZ are poorly characterized due to limitations in existing analytical methodologies. In this work we developed a method for high spatio-temporal resolution analysis of polar organic micropollutants (POMs) in hyporheic pore- and surface waters by combining (semi-) automatic low volume sampling techniques with direct-injection ultra-high performance liquid chromatography tandem mass spectrometry. The method is capable of quantifying 25 parent compounds and 18 transformation products (TPs) using only 0.4 mL of water and few preparation steps. Application of the method to both surface and pore water revealed significant (i.e. > an order of magnitude) differences in POM concentrations over small time and spatial scales (i.e. < a few hours and tens of cm, respectively). Guanylurea, a TP of the antidiabetic drug metformin was detected at unprecedentedly high concentrations. Collectively, this method is suitable for in situ characterization of POMs at high spatial and temporal resolution and with minimal disturbance of natural flow paths and infiltration of surface water.

  • 37.
    Reppas-Chrysovitsinos, Efstathios
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Sobek, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Screening-level models to estimate partition ratios of organic chemicals between polymeric materials, air and water2016In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 18, no 6, p. 667-676Article in journal (Refereed)
    Abstract [en]

    Polymeric materials flowing through the technosphere are repositories of organic chemicals throughout their life cycle. Equilibrium partition ratios of organic chemicals between these materials and air (KMA) or water (KMW) are required for models of fate and transport, high-throughput exposure assessment and passive sampling. KMA and KMW have been measured for a growing number of chemical/ material combinations, but significant data gaps still exist. We assembled a database of 363 KMA and 910 KMW measurements for 446 individual compounds and nearly 40 individual polymers and biopolymers, collected from 29 studies. We used the EPI Suite and ABSOLV software packages to estimate physicochemical properties of the compounds and we employed an empirical correlation based on Trouton's rule to adjust the measured KMA and KMW values to a standard reference temperature of 298 K. Then, we used a thermodynamic triangle with Henry's law constant to calculate a complete set of 1273 KMA and KMW values. Using simple linear regression, we developed a suite of single parameter linear free energy relationship (spLFER) models to estimate KMA from the EPI Suite-estimated octanol-air partition ratio (KOA) and KMW from the EPI Suite-estimated octanol-water (KOW) partition ratio. Similarly, using multiple linear regression, we developed a set of polyparameter linear free energy relationship (ppLFER) models to estimate KMA and KMW from ABSOLV-estimated Abraham solvation parameters. We explored the two LFER approaches to investigate (1) their performance in estimating partition ratios, and (2) uncertainties associated with treating all different polymers as a single bulk polymeric material compartment. The models we have developed are suitable for screening assessments of the tendency for organic chemicals to be emitted from materials, and for use in multimedia models of the fate of organic chemicals in the indoor environment. In screening applications we recommend that K-MA and K-MW be modeled as 0.06 x K-OA and 0.06 x K-OW respectively, with an uncertainty range of a factor of 15.

  • 38.
    Rummel, Christoph Daniel
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Adolfsson-Erici, Margaretha
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Jahnke, Annika
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    No measurable cleaning of polychlorinated biphenyls from Rainbow Trout in a 9 week depuration study with dietary exposure to 40% polyethylene microspheres2016In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 18, no 7, p. 788-795Article in journal (Refereed)
    Abstract [en]

    Persistent hydrophobic chemicals sorbed to plastic can be transferred to fish and other aquatic organisms upon ingestion. However, ingestion of plastic could also lead to enhanced elimination of these chemicals if the plastic is less contaminated than the fish. Here, we attempted to measure the influence of ingestion of uncontaminated polyethylene microspheres on the depuration rates of polychlorinated biphenyls (PCBs) in an in vivo fish feeding experiment. Rainbow trout were given feed contaminated with PCBs for two consecutive days, then clean feed for three days to allow for egestion of the contaminated food. A control group of fish were then fed ordinary food pellets and a treatment group were fed pellets that additionally contained 40% by weight polyethylene microspheres. Condition factors and growth rates in both groups were similar, indicating no negative effect of the plastic microspheres on the nutritional status of the fish. Fish were sampled after zero, three, six and nine weeks, homogenized, solvent-extracted and analyzed by GC/MS. PCB concentrations declined in both groups at a rate consistent with growth dilution. There was no significant difference in the elimination rate constants between the control and treatment group, indicating that ingestion of uncontaminated plastic did not cause a measurable enhancement of depuration of PCBs by the fish in this study.

  • 39.
    Schultes, Lara
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Vestergren, Robin
    Volkova, Kristina
    Westberg, Emelie
    Jacobson, Therese
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Per- and polyfluoroalkyl substances and fluorine mass balance in cosmetic products from the Swedish market: implications for environmental emissions and human exposure2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 12, p. 1680-1690Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFASs) are a diverse class of >4700 chemicals used in commercial products and industrial processes. Concerns surrounding PFASs are principally due to their widespread occurrence in humans and the environment and links to adverse health effects. One of the lesser known uses for PFASs is in cosmetic products (CPs) which come into contact with the skin (e.g. hair products, powders, sunblocks, etc.). In the present work, thirty-one CPs from five product categories (cream, foundation, pencil, powder and shaving foam) were analyzed for 39 PFASs by liquid chromatography-tandem mass spectrometry, as well as extractable organic fluorine (EOF) and total fluorine (TF) by combustion ion chromatography (CIC). This multi-platform approach enabled determination of the fraction of fluorine accounted for by known PFASs (i.e. fluorine mass balance). Foundations and powders contained 25 different PFASs with the most frequently detected being perfluorinated carboxylic acids (perfluoroheptanoic acid and perfluorohexanoic acid) and polyfluoroalkyl phosphate esters (PAPs). sigma(14)PAP concentrations up to 470 g g(-1) were measured in products listing mixtures of PAPs as an ingredient. For all samples, sigma(39)PFAS concentrations only explained a small fraction of the EOF and TF, pointing to the presence of unknown organic and/or inorganic fluorinated substances, including polymers. While creams, pencil and shaving foams did not contain measurable concentrations of any of the 39 PFASs targeted here, CIC revealed high to moderate TF content. Overall, these data highlight the need for further investigations into the occurrence of PFASs in CPs and their importance with regards to human and environmental exposure.

  • 40.
    Sha, Bo
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Schymanski, Emma L.
    Ruttkies, Christoph
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Wang, Zhanyun
    Exploring open cheminformatics approaches for categorizing per- and polyfluoroalkyl substances (PFASs)2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 11, p. 1835-1851Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFASs) are a large and diverse class of chemicals of great interest due to their wide commercial applicability, as well as increasing public concern regarding their adverse impacts. A common terminology for PFASs was recommended in 2011, including broad categorization and detailed naming for many PFASs with rather simple molecular structures. Recent advancements in chemical analysis have enabled identification of a wide variety of PFASs that are not covered by this common terminology. The resulting inconsistency in categorizing and naming of PFASs is preventing efficient assimilation of reported information. This article explores how a combination of expert knowledge and cheminformatics approaches could help address this challenge in a systematic manner. First, the splitPFAS approach was developed to systematically subdivide PFASs (for eventual categorization) following a CnF2n+1-X-R pattern into their various parts, with a particular focus on 4 PFAS categories where X is CO, SO2, CH2 and CH2CH2. Then, the open, ontology-based ClassyFire approach was tested for potential applicability to categorizing and naming PFASs using five scenarios of original and simplified structures based on the splitPFAS output. This workflow was applied to a set of 770 PFASs from the latest OECD PFAS list. While splitPFAS categorized PFASs as intended, the ClassyFire results were mixed. These results reveal that open cheminformatics approaches have the potential to assist in categorizing PFASs in a consistent manner, while much development is needed for future systematic naming of PFASs. The splitPFAS tool and related code are publicly available, and include options to extend this proof-of-concept to encompass further PFASs in the future.

  • 41.
    Sobek, Anna
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Bejgarn, Sofia
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Rudén, Christina
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Breitholtz, Magnus
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    The dilemma in prioritizing chemicals for environmental analysis: known versus unknown hazards2016In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 18, no 8, p. 1042-1049Article in journal (Refereed)
    Abstract [en]

    A major challenge for society is to manage the risks posed by the many chemicals continuously emitted to the environment. All chemicals in production and use cannot be monitored and science-based strategies for prioritization are essential. In this study we review available data to investigate which substances are included in environmental monitoring programs and published research studies reporting analyses of chemicals in Baltic Sea fish between 2000 and 2012. Our aim is to contribute to the discussion of priority settings in environmental chemical monitoring and research, which is closely linked to chemical management. In total, 105 different substances or substance groups were analyzed in Baltic Sea fish. Polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans (PCDD/Fs) and polychlorinated biphenyls (PCBs) were the most studied substances or substance groups. The majority, 87%, of all analyses comprised 20% of the substances or substance groups, whereas 46 substance groups (44%) were analyzed only once. Almost three quarters of all analyses regarded a POP-substance (persistent organic pollutant). These results demonstrate that the majority of analyses on environmental contaminants in Baltic Sea fish concern a small number of already regulated chemicals. Legacy pollutants such as POPs pose a high risk to the Baltic Sea due to their hazardous properties. Yet, there may be a risk that prioritizations for chemical analyses are biased based on the knowns of the past. Such biases may lead to society failing in identifying risks posed by yet unknown hazardous chemicals. Alternative and complementary ways to identify priority chemicals are needed. More transparent communication between risk assessments performed as part of the risk assessment process within REACH and monitoring programs, and information on chemicals contained in consumer articles, would offer ways to identify chemicals for environmental analysis.

  • 42.
    Song, Shanjun
    et al.
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Ruan, Ting
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Wang, Thanh
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Liu, Runzeng
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Jiang, Guibin
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Occurrence and removal of benzotriazole ultraviolet stabilizers in a wastewater treatment plant in China2014In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 16, no 5, p. 1076-1082Article in journal (Refereed)
    Abstract [en]

    Benzotriazole ultraviolet stabilizers (BZT-UVs) have previously been found in sludge from wastewater treatment plants (WWTPs), which might be potential sources of BZT-UVs to the surrounding environment. In this work, the occurrence and fate of seven emerging 2-hydroxyphenyl substituted BZT-UVs were investigated in a Chinese WWTP. This group of hydrophobic BZT-UVs possess log Kow values ranging from 4.31 to 7.67 which could be associated with their fate in WWTPs. Field samples including 24 h flow composites of influent, effluent and grab sludge samples from different treatment processes were collected and analyzed. Concentrations of BZT-UVs dissolved in aqueous-phases were in the range of 4.88±1.35 (UV-234) to 34.5±12.4 ng L-1 (UV-P) in the primary influent, while only UV-P and UV-328 were detected in the final effluent at concentrations of 10.5±6.59 and 2.74±1.73 ng L-1, respectively. Considering the amount of target BZT-UVs adsorbed to total suspended solids (TSS), the daily mass flux in the primary influent of the WWTP ranged from 22.3 g day(-1) (UV-P, 7.99%) to 74.0 g day-1 (UV-234, 26.5%). Total removal efficiency of the integrated treatment process ranged from 89.7% for UV-P to 99.7% for UV-234 suggesting nearly complete removal. Organic solid sedimentation in primary and secondary clarifiers was the dominant elimination route for BZT-UV analogues, which constituted 96.3% of the total removal efficiency. Advanced treatment (using ultraviolet disinfection) in this plant might further contribute to the high removal efficiencies (ranging from 19.6% to 77.3%).

  • 43.
    Wang, Pu
    et al.
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Zhang, Haidong
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Fu, Jianjie
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Li, Yingming
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Wang, Thanh
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Wang, Yawei
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Ren, Daiwei
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Ssebugere, Patrick
    Department of Chemistry, Makerere University, Kampala, Uganda .
    Zhang, Qinghua
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Jiang, Guibin
    State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China .
    Temporal trends of PCBs, PCDD/Fs and PBDEs in soils from an E-waste dismantling area in East China2013In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 15, no 10, p. 1897-1903Article in journal (Refereed)
    Abstract [en]

    The temporal trends of polychlorinated biphenyls (PCBs), polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and polybrominated diphenyl ethers (PBDEs) were investigated in soils from an E-waste dismantling area in East China between 2005 and 2011. Isotope dilution high resolution gas chromatography/high resolution mass spectrometry (HRGC/HRMS) was employed for the sample analysis. PCB levels declined as expected, while PCDD/Fs generally remained at a constant level during the sampling period, and PBDE concentrations tended to be slightly lower after 2007 although the decline was not statistically significant. The congener profiles indicated that lowly-halogenated congeners of these persistent organic pollutants (POPs) accounted for the decreasing levels and relative proportions of the POPs, suggesting that they have been gradually eliminated from the field soil over the years. However, the concentration levels of some heavy congeners (e.g., CB-209, OCDD and OCDF) showed different trends from those of the lighter ones. The general tendencies of the three types of POPs in soils were consistent with those reported in other studies in this area. The results implied that the enhanced regulations and centralized dismantling action introduced in 2005 might exert a limited influence on these three types of POPs in soils during the sampling period.

  • 44.
    Zhou, Shouming
    et al.
    Department of Chemistry, University of Toronto, Toronto, Canada.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology. Department of Chemistry, University of Toronto, Toronto, Canada.
    Forbes, Matthew W
    Department of Chemistry, University of Toronto, Toronto, Canada.
    Mabury, Scott
    Department of Chemistry, University of Toronto, Toronto, Canada.
    Abbatt, Jonathan P D
    Department of Chemistry, University of Toronto, Toronto, Canada.
    Epoxide formation from heterogeneous oxidation of benzo[a]pyrene with gas-phase ozone and indoor air2017In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 19, no 10, p. 1292-1299Article in journal (Refereed)
    Abstract [en]

    The formation of two classes of epoxide products from the heterogeneous reaction of benzo[a]pyrene (BaP) with gas-phase ozone was demonstrated. BaP was coated on a Pyrex glass tube and oxidized with different concentrations of ozone. After oxidation, the epoxide products were derivatized by N-acetylcystein (NAC) and then analyzed by liquid chromatography-tandem mass spectrometry (LC-MS/MS). The results show that in addition to mono-epoxides, diol-epoxides were also formed. BaP exposed to genuine indoor air also produces mono- and diol-epoxides, having similar chromatograms to those produced by oxidation of BaP by low concentrations of ozone. Although it is well recognized that diol-epoxides are formed from BaP oxidation in the human body and that they exhibit carcinogenicity via formation of adducts with DNA, this is the first demonstration that such classes of compounds can be formed by abiotic heterogeneous oxidation.

  • 45.
    Ågerstrand, Marlene
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Arnold, Kathryn
    Balshine, Sigal
    Brodin, Tomas
    Brooks, Bryan W.
    Maack, Gerd
    McCallum, Erin S.
    Pyle, Greg
    Saaristo, Minna
    Ford, Alex T.
    Emerging investigator series: use of behavioural endpoints in the regulation of chemicals2020In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 22, no 1, p. 49-65Article in journal (Refereed)
    Abstract [en]

    Interest in behavioural ecotoxicology is growing, partly due to technological and computational advances in recording behaviours but also because of improvements of detection capacity facilitating reporting effects at environmentally relevant concentrations. The peer-reviewed literature now contains studies investigating the effects of chemicals, including pesticides and pharmaceuticals, on migration, dispersal, aggression, sociability, reproduction, feeding and anti-predator behaviours in vertebrates and invertebrates. To understand how behavioural studies could be used in regulatory decision-making we: (1) assessed the legal obstacles to using behavioural endpoints in EU chemicals regulation; (2) analysed the known cases of use of behavioural endpoints in EU chemicals regulation; and (3) provided examples of behavioural endpoints of relevance for population level effects. We conclude that the only legal obstacle to the use of behavioural endpoints in EU chemicals regulation is whether an endpoint is considered to be relevant at the population level or not. We also conclude that ecotoxicity studies investigating behavioural endpoints are occasionally used in the EU chemicals regulation, and underscore that behavioural endpoints can be relevant at the population level. To improve the current use of behavioural studies in regulatory decision-making contribution from all relevant stakeholders is required. We have the following recommendations: (1) researchers should conduct robust, well-designed and transparent studies that emphasize the relevance of the study for regulation of chemicals; (2) editors and scientific journals should promote detailed, reliable and clearly reported studies; (3) regulatory agencies and the chemical industry need to embrace new behavioural endpoints of relevance at the population level.

  • 46.
    Ågerstrand, Marlene
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Brenig, Mattheus
    Führ, Martin
    Schenten, Julian
    Refining tools to bridge the gap between academia and chemical regulation: perspectives for WikiREACH2017In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 19, no 12, p. 1466-1473Article, review/survey (Refereed)
    Abstract [en]

    Regulatory hazard and risk assessments of chemical substances have to include all reliable and relevant data to be credible and complete. However, screening the literature for appropriate studies and extracting data is burdensome. Therefore, reducing impediments by making data easily and readily accessible to risk assessors could result in more comprehensive hazard and risk assessments. In this paper, we study WikiPharma, a database that aggregates ecotoxicity data for pharmaceuticals, extracted from peerreviewed studies. The use of the WikiPharma database is explored to develop strategies on how similar tools can bridge between science and policy by providing risk assessors with easily accessible summary data. Specifically, adapting the concept of WikiPharma to industrial chemicals regulated under the REACH regulation is discussed. Experiences with WikiPharma show that there is interest in using peerreviewed studies in regulatory decision-making. However, tools like WikiPharma require constant updates. Hence, as for WikiREACH, effective incentives are needed to motivate researchers to feed in relevant data for regulatory assessments. Besides, support by automated processes can aid in the labourintensive activity of gathering data. To ensure that such a tool is continuously maintained and compatible with the regulatory system, and thereby useful for hazard and risk assessments of chemicals, it would benefit from being developed in collaboration with the major stakeholders in the field, i.e. regulatory agencies, academia, industry, scientific journals, and providers of research network platforms.

  • 47.
    Ågerstrand, Marlene
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Sobek, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Lilja, Karl
    Linderoth, Maria
    Wendt-Rasch, Lina
    Wernersson, Ann-Sofie
    Rudén, Christina
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    An academic researcher's guide to increased impact on regulatory assessment of chemicals2017In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 19, no 5, p. 644-655Article in journal (Refereed)
    Abstract [en]

    The interactions between academic research and regulatory assessment of chemicals may in theory seem straightforward: researchers perform studies, and these studies are used by regulators for decision-making. However, in practice the situation is more complex, and many factors decide a research study's regulatory use. According to several EU chemical legislations, all available and relevant studies can be used in hazard and risk assessment of chemicals. However, in practice, standard tests conducted under GLP and sponsored and provided by industry are predominantly used. Peer-reviewed studies from independent sources are often disregarded or disputed since they often do not comply with regulatory data requirements and quality criteria. To help bridge such a gap, the aim of this paper is to give an overview of the general workings of legislation of chemicals and propose a set of actions to increase the usability of research data. In the end, this may increase the use of academic research for decision-making and ultimately result in more science-based policies. From a policy perspective, useful scientific evidence comprises those studies that are sufficiently reliable and relevant. This is not in contradiction to the aims of research and generally accepted scientific standards.

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