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Methods to measure mass transfer kinetics, partition ratios and atmospheric fluxes of organic chemicals in forest systems
Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
2016 (English)Doctoral 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.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science and Analytical Chemistry, Stockholm University , 2016. , p. 36
Keywords [en]
Hydrophobic organic chemicals, vegetation, modified Bowen ratio, surface-atmosphere fluxes
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-136008ISBN: 978-91-7649-593-3 (print)ISBN: 978-91-7649-594-0 (print)OAI: oai:DiVA.org:su-136008DiVA, id: diva2:1050334
Public defence
2017-01-20, Nordenskiöldsalen, Geovetenskapens hus, Svante Arrhenius väg 12, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
Swedish Research Council, 2011-3890
Note

At the time of the doctoral defense, the following paper was unpublished and had a status as follows: Paper 3: Manuscript.

Available from: 2016-12-28 Created: 2016-11-28 Last updated: 2016-12-16Bibliographically approved
List of papers
1. Mass transfer of hydrophobic organic chemicals between siliconesheets and through plant leaves and low-density polyethylene
Open this publication in new window or tab >>Mass transfer of hydrophobic organic chemicals between siliconesheets and through plant leaves and low-density polyethylene
2016 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 164, p. 683-690Article in journal (Refereed) Published
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.

Keywords
Passive dosing, PDMS, Mass transfer coefficients, Leaves, LDPE
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-136027 (URN)10.1016/j.chemosphere.2016.08.082 (DOI)000385318200080 ()
Funder
Swedish Research Council, 2011-3890
Available from: 2016-11-29 Created: 2016-11-29 Last updated: 2017-11-29Bibliographically approved
2. A passive dosing method to determine fugacitycapacities and partitioning properties of leaves
Open this publication in new window or tab >>A passive dosing method to determine fugacitycapacities and partitioning properties of leaves
Show others...
2016 (English)In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 18, p. 1325-1332Article in journal (Refereed) Published
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.

Keywords
Hydrophobic organic chemicals, leaves, passive dosing
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-136032 (URN)10.1039/c6em00423g (DOI)000386230300008 ()
Funder
Swedish Research Council, 2011-3890
Available from: 2016-11-29 Created: 2016-11-29 Last updated: 2017-11-29Bibliographically approved
3. Sorptive capacities of leaf lipids for hydrophobic organic chemicals: Lipid characterization and passive dosing experiments
Open this publication in new window or tab >>Sorptive capacities of leaf lipids for hydrophobic organic chemicals: Lipid characterization and passive dosing experiments
Show others...
(English)Manuscript (preprint) (Other academic)
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-136116 (URN)
Funder
Swedish Research Council, 2011-3890
Available from: 2016-11-29 Created: 2016-11-29 Last updated: 2016-11-29Bibliographically approved
4. Comparison of eddy covariance and modified Bowen ratio methods for measuring gas fluxes and implications for measuring fluxes of persistent organic pollutants
Open this publication in new window or tab >>Comparison of eddy covariance and modified Bowen ratio methods for measuring gas fluxes and implications for measuring fluxes of persistent organic pollutants
2016 (English)In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 16, no 8, p. 5315-5322Article in journal (Refereed) Published
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.

National Category
Earth and Related Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-132020 (URN)10.5194/acp-16-5315-2016 (DOI)000376937000033 ()
Available from: 2016-07-05 Created: 2016-07-05 Last updated: 2017-11-28Bibliographically approved

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