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  • 1.
    Ahmadi, Hamid
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Bolinius, Dämien Johann
    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.
    Mass transfer of hydrophobic organic chemicals between siliconesheets and through plant leaves and low-density polyethylene2016In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 164, p. 683-690Article in journal (Refereed)
    Abstract [en]

    Plant leaves play an important role in the fate of hydrophobic organic contaminants (HOCs) in theenvironment. Yet much remains unknown about the permeability of leaves by HOCs. In this pilot studywe measured (i) the kinetics of mass transfer of three polycyclic aromatic hydrocarbons (PAHs) and sixpolychlorinated biphenyls between a spiked and an unspiked sheet of polydimethylsiloxane (PDMS) indirect contact with each other for 24 h and (ii) kinetics of mass transfer of two PAHs through leaves andlow-density polyethylene (LDPE) in a passive dosing experiment by inserting these matrices between thetwo sheets of PDMS for 48 h. The kinetics of mass transfer of fluoranthene between PDMS sheets in directcontact were a factor of 12 slower than those reported in the literature. The kinetics of mass transfer offluorene and phenanthrene through leaves were within the range of those previously reported for 2,4-dichlorophenoxyacetic acid through isolated cuticles. Our results provide a proof-of-concept demon-stration that the passive dosing method applied in this study can be used to measure the mass transfercoefficients of organic chemicals through leaves. Key recommendations for future experiments are toload the PDMS at the highest feasible concentrations to avoid working at analyte levels close to the limitof detection, to keep the leaves moist and to minimize potential pathways for contamination of the PDMSsheets by exposure to laboratory air.

  • 2.
    Bolinius, Damien Johann
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Methods to measure mass transfer kinetics, partition ratios and atmospheric fluxes of organic chemicals in forest systems2016Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Vegetation plays an important role in the partitioning, transport and fate of hydrophobic organic contaminants (HOCs) in the environment. This thesis aimed at addressing two key knowledge gaps in our understanding of how plants exchange HOCs with the atmosphere: (1) To improve our understanding of the uptake of HOCs into, and transfer through, leaves of different plant species which can significantly influence the transport and fate of HOCs in the environment; and (2) To evaluate an experimental approach to measure fluxes of HOCs in the field. The methods presented in papers I, II and III contribute to increasing our understanding of the fate and transport of HOCs in leaves by offering straightforward ways of measuring mass transfer coefficients through leaves and partition ratios of HOCs between leaves, leaf lipids and lipid standards and reference materials like water, air and olive oil. The passive dosing study in paper III in particular investigated the role of the composition of the organic matter extracted from leaves in determining the capacity of the leaves to hold chemicals and found no large differences between 7 different plant species, even though literature data on leaf/air partition ratios (Kleaf/air) varies over 1-3 orders of magnitude. In paper IV we demonstrated that the modified Bowen ratio method can be extended to measure fluxes of persistent organic pollutants (POPs) if the fluxes do not change direction over the course of the sampling period and are large enough to be measured. This approach thus makes it possible to measure fluxes of POPs that usually require sampling times of days to weeks to exceed method detection limits. The experimental methods described in this thesis have the potential to support improved parameterization of multimedia models, which can then be evaluated against fluxes measured in the field using the modified Bowen ratio approach.

  • 3.
    Bolinius, Damien Johann
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Jahnke, Annika
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Helmholtz Centre for Environmental Research (UFZ), Germany.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Comparison of eddy covariance and modified Bowen ratio methods for measuring gas fluxes and implications for measuring fluxes of persistent organic pollutants2016In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 16, no 8, p. 5315-5322Article in journal (Refereed)
    Abstract [en]

    Semi-volatile persistent organic pollutants (POPs) cycle between the atmosphere and terrestrial surfaces; however measuring fluxes of POPs between the atmosphere and other media is challenging. Sampling times of hours to days are required to accurately measure trace concentrations of POPs in the atmosphere, which rules out the use of eddy covariance techniques that are used to measure gas fluxes of major air pollutants. An alternative, the modified Bowen ratio (MBR) method, has been used instead. In this study we used data from FLUXNET for CO2 and water vapor (H2O) to compare fluxes measured by eddy covariance to fluxes measured with the MBR method using vertical concentration gradients in air derived from averaged data that simulate the long sampling times typically required to measure POPs. When concentration gradients are strong and fluxes are unidirectional, the MBR method and the eddy covariance method agree within a factor of 3 for CO2, and within a factor of 10 for H2O. To remain within the range of applicability of the MBR method, field studies should be carried out under conditions such that the direction of net flux does not change during the sampling period. If that condition is met, then the performance of the MBR method is neither strongly affected by the length of sample duration nor the use of a fixed value for the transfer coefficient.

  • 4.
    Bolinius, Damien Johann
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Stockholm Univ, Dept Environm Sci & Analyt Chem ACES, Svante Arrhenius Vag 8, SE-11418 Stockholm, Sweden.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Iadaresta, Francesco
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Holmbäck, Jan
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Lipidor AB, Karolinska Institutet Science Park, Sweden.
    Jahnke, Annika
    Sorptive Capacities of Nonpolymeric Plant Lipids for Hydrophobic Chemicals Determined by Passive Dosing2019In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 53, no 3, p. 1278-1286Article in journal (Refereed)
    Abstract [en]

    Vegetation plays an important role in the partitioning, transport, and fate of semivolatile hydrophobic organic chemicals (HOCs) in the environment. Leaf/air partition ratios (K-leaf/air) of HOCs are highly variable for different plant species. The differences cannot be fully explained by the fraction of lipids in the leaves or the thickness of the cuticle. Our goal was to elucidate the importance of non polymeric lipids in determining K-leaf/air To do this, we extracted organic matter from 7 plant species using solvents that do not extract the polymeric lipids cutin and cutan, to yield extractable organic matter (EOM). We used passive dosing to determine the partition ratios of selected HOCs between the EOM of the leaves and our reference lipid, olive oil (K-EOM/olive oil) In addition, we measured analogous partition ratios for three lipid standards. Proton nuclear magnetic resonance (NMR) spectroscopy was used to characterize the composition of lipids. Differences in K-EOM/olive oil of two polychlorinated biphenyls and four chlorinated benzenes were below a factor of 2 in the plant species studied, indicating that the reported differences in K-leaf/air are not caused by differences in the sorptive capacities of nonpolymeric lipids or that our EOM is not representative of all nonpolymeric leaf lipids.

  • 5.
    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.

  • 6.
    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.

  • 7.
    Bolinius, Dämien
    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.
    Iadaresta, Francesco
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Holmbäck, Jan
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Jahnke, Annika
    Sorptive capacities of leaf lipids for hydrophobic organic chemicals: Lipid characterization and passive dosing experimentsManuscript (preprint) (Other academic)
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