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  • 1.
    Lam, Monika M.
    Örebro University, School of Science and Technology.
    Characterization of PAC-contaminated soil with the focus on availability, leachability and biological activities2018Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Current risk assessments of polycyclic aromatic compounds (PACs)-contaminated soil are often based on the 16 priority PAHs and do not consider availability of PACs in soil sufficiently. This may lead to uncertainties of the assessment, since important contaminants can be overlooked and only a small fraction of contaminants is available for the uptake for organisms. The overall aim of this thesis was to develop a refined and enhanced analytical approach based on both chemical and bioassay analysis coupled to passive sampling with polyoxymethylene (POM) and leaching tests that can provide a more comprehensive picture of chemical pollution at PAC-contaminated sites. To achieve this, bioassay-specific relative potency factors (REPs) of PACs were determined for the H4IIE-luc bioassay, detecting AhR-mediated activity, and for the VM7luc4E2 transactivation assay, detecting ER-mediated activity for the use in potency-balance analysis. Results of uptake-experiments of PACs in earthworms and POM suggested that POM is a suitable tool to study availability of AhR and ER agonists in soil. Availability and mobility of PACs in soil were investigated by the use of POM and leaching tests. The results of potency-balance analysis showed that in soil samples, in POM-fractions or in leachates, a large fraction of AhR- or ER-agonists remained unexplained, despite the use of a large number of REPs. In addition, coupling of chemical and biological analysis to passive sampling or leaching tests revealed that only a small fraction of the total mass of PACs in the soil is available or leachable in soil. The results suggests that the use of only the total concentration in soil while ignoring unknown toxicants will lead to great uncertainties in the risk assessment. Therefore, effect-based screening using bioassays, taking availability and mobility of compounds into account, as well as a widened chemical analysis should be included in modern hazard- and risk assessment of PAH contaminated soils.

    List of papers
    1. Methylated PACs are more potent than their parent compounds: a study on AhR-mediated activity, degradability and mixture interactions in the H4IIE-luc assay
    Open this publication in new window or tab >>Methylated PACs are more potent than their parent compounds: a study on AhR-mediated activity, degradability and mixture interactions in the H4IIE-luc assay
    Show others...
    (English)Manuscript (preprint) (Other academic)
    National Category
    Other Biological Topics
    Identifiers
    urn:nbn:se:oru:diva-64293 (URN)
    Available from: 2018-01-16 Created: 2018-01-16 Last updated: 2018-01-16Bibliographically approved
    2. Methylated polycyclic aromatic hydrocarbons and/or their metabolites are important contributors to the overall estrogenic activity of polycyclic aromatic hydrocarbon-contaminated soils
    Open this publication in new window or tab >>Methylated polycyclic aromatic hydrocarbons and/or their metabolites are important contributors to the overall estrogenic activity of polycyclic aromatic hydrocarbon-contaminated soils
    2018 (English)In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 37, no 2, p. 385-397Article in journal (Refereed) Published
    Abstract [en]

    In the present study 42 polycyclic aromatic compounds (PACs) were investigated for their estrogenic potential using the VM7Luc4E2 transactivation assay. Relative potencies were determined for mass-balance analysis. In addition, compounds were tested in combination with the estrogen receptor (ER) antagonist vertical bar C vertical bar 182,780 (vertical bar C vertical bar) and the aryl hydrocarbon receptor antagonist/CYP1A1 inhibitor a-naphthoflavone. Luciferase induction and CYP1A1-dependent ethoxyresorufin-O-deethylase (EROD) activity were measured to assess whether the estrogenic activity was elicited by the compound itself and/or by its metabolites. Relative potencies ranged between 10(-7) and 10(-4). The ability of ICI to decrease luciferase activity stimulated by all compounds indicated that the induction responses were ER-dependent. The aryl hydrocarbon receptor antagonist/CYP1A1 inhibitor a-naphthoflavone decreased luciferase induction and EROD activity by several compounds, including the methylated chrysenes, suggesting that metabolites of these chemicals contributed to ER activation. Several PACs, such as acridine and its derivatives, appear to directly activate the ER. Furthermore, extracts of soils from industrial areas were examined using this bioassay, and estrogenic activity was detected in all soil samples. Mass-balance analysis using a combination of relative potencies and chemical analysis of the samples suggested that polycyclic aromatic hydrocarbons (PAHs) and alkylated PAHs, such as 1-and 3-methylchrysene, are important contributors to the overall estrogenic activity. However, these results revealed that a considerable proportion of the estrogenic activity in the soil remained unexplained, indicating the presence of other significant estrogenic compounds.

    Place, publisher, year, edition, pages
    John Wiley & Sons, 2018
    Keywords
    Estrogen receptor–mediated activity; Relative potency; Metabolite; VM7Luc4E2 transactivation assay; Mass-balance analysis
    National Category
    Environmental Sciences Earth and Related Environmental Sciences
    Identifiers
    urn:nbn:se:oru:diva-61710 (URN)10.1002/etc.3958 (DOI)000423425700009 ()28834568 (PubMedID)2-s2.0-85041099349 (Scopus ID)
    Funder
    Knowledge Foundation, 2013/0157
    Available from: 2017-11-13 Created: 2017-11-13 Last updated: 2018-02-12Bibliographically approved
    3. Polyoxymethylene (POM) is a suitable tool for effect-based hazard assessment of PAC-contaminated soil
    Open this publication in new window or tab >>Polyoxymethylene (POM) is a suitable tool for effect-based hazard assessment of PAC-contaminated soil
    Show others...
    (English)Manuscript (preprint) (Other academic)
    National Category
    Other Biological Topics
    Identifiers
    urn:nbn:se:oru:diva-64300 (URN)
    Available from: 2018-01-16 Created: 2018-01-16 Last updated: 2018-01-26Bibliographically approved
    4. Occurrence and leachability of polycyclic aromatic compounds in contaminated soils: Chemical and bioanalytical characterization
    Open this publication in new window or tab >>Occurrence and leachability of polycyclic aromatic compounds in contaminated soils: Chemical and bioanalytical characterization
    Show others...
    2018 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 622-623, p. 1476-1484Article in journal (Refereed) Published
    Abstract [en]

    An important concern regarding sites contaminated with polycyclic aromatic compounds (PACs) is the risk of groundwater contamination by release of the compounds from soils. The goal of this study was to investigate the occurrence and leachability of 77 PACs including polycyclic aromatic hydrocarbons (PAHs) and heterocyclic aromatic compounds (NSO-PACs) among total aryl hydrocarbon receptor (AhR) agonists in soils from historical contaminated sites. A novel approach combining chemical and bioanalytical methods in combination with characterization of leachability by use of a column leaching test was used. Similar profiles of relative concentrations of PACs were observed in all soils, with parent PAHs accounting for 71 to 90% of total concentrations in soils. Contribution of oxy-PAHs, alkyl-PAHs and N-PACs ranged from 2 to 9%, 3 to 9% and 1 to 14%, respectively. Although the contributions of groups of PACs were small, some compounds were found in similar or greater concentrations than parent PAHs. Leachable fractions of 77 PACs from soils were small and ranged from 0.002 to 0.54%. Polar PACs were shown to be more leachable than parent PAHs. The contribution of analyzed PACS to overall AhR-mediated activities in soils and leachates suggests presence of other AhR agonists in soils, and a potential risk. Only a small fraction of AhR agonists was available in soils, indicating an overestimation of the risk if only total initial concentrations in soils would be considered in risk assessment. The results of the study strongly support that focus on 16US EPA PAHs may result in inadequate assessment of risk and hazard of PACs in complex environmental samples.

    Place, publisher, year, edition, pages
    Elsevier, 2018
    Keywords
    Alkyl-PAHs; Oxy-PAHs; NSO-heterocyclic compounds; Ah receptor; H4IIE-luc bioassay; Column leaching test
    National Category
    Environmental Sciences
    Identifiers
    urn:nbn:se:oru:diva-64301 (URN)10.1016/j.scitotenv.2017.12.015 (DOI)000426349000143 ()2-s2.0-85038841340 (Scopus ID)
    Funder
    Knowledge Foundation, 2013/0157
    Note

    Funding Agencies:

    Applicera and Formas  210-2014-87 

    Canada Research Chair program  

    State Administration of Foreign Experts Affairs  GDT20143200016 

    P.R. China  

    Chinese Academy of Sciences  

    Distinguished Visiting Professorship in the School of Biological Sciences of the University of Hong Kong  

    Natural Science and Engineering Research Council of Canada  326415-07 

    Western Economic Diversification Canada  6578  6807  000012711 

    Canada Foundation for Infrastructure  

    Available from: 2018-01-16 Created: 2018-01-16 Last updated: 2018-08-16Bibliographically approved
  • 2.
    Lam, Monika M.
    et al.
    Örebro University, School of Science and Technology.
    Bülow, Rebecca
    Örebro University, School of Science and Technology.
    Engwall, Magnus
    Örebro University, School of Science and Technology.
    Giesy, John P.
    University of Saskatchewan, Saskatoon, Saskatchewan, Canada.
    Larsson, Maria
    Örebro University, School of Science and Technology.
    Methylated PACs are more potent than their parent compounds: a study on AhR-mediated activity, degradability and mixture interactions in the H4IIE-luc assayManuscript (preprint) (Other academic)
  • 3.
    Lam, Monika M.
    et al.
    Örebro University, School of Science and Technology.
    Bülow, Rebecca
    Örebro University, School of Science and Technology.
    Engwall, Magnus
    Örebro University, School of Science and Technology.
    Giesy, John P.
    Department of Veterinary Biomedical Sciences and Toxicology Centre, University of Saskatchewan, Saskatoon, Canada.
    Larsson, Maria
    Örebro University, School of Science and Technology.
    Methylated PACs Are More Potent than Their Parent Compounds: A Study on AhR-mediated Activity, Degradability and Mixture Interactions in the H4IIE-luc Assay2018In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 37, no 5, p. 1409-1419Article in journal (Refereed)
    Abstract [en]

    Twenty-six polycyclic aromatic compounds (PACs; including native polycyclic aromatic hydrocarbons [PAHs], hydroxylated PAHs, alkylated and oxygenated PAHs, and [alkylated] heterocyclic compounds) were investigated for their aryl hydrocarbon receptor (AhR)-mediated potencies in the H4IIE-luc bioassay. Potential degradabilities of PACs were investigated by use of various durations of exposure (24, 48, or 72 h), and various mixtures of PACs including PAHs, alkylated and oxygenated PAHs, and heterocyclic compounds were tested for their joint AhR-mediated potency. Additive behaviors of PACs in mixtures were studied by comparing observed mixture potencies with mixture potencies predicted by use of the concentration addition model. Methylated derivatives were more potent than their parent compounds in the H4IIE-luc assay. A time-dependent decrease in relative potency was observed for all AhR-active compounds, which may be indicative of in vitro biotransformation. Monomethylated compounds seemed to be more rapidly transformed than analogous unsubstituted compounds. In addition, the results showed that the predictive power of the concentration addition model increased with the number of compounds, suggesting additivity in multicomponent mixtures. Due to the greater potency of methylated derivatives and their ubiquitous occurrence, there is a need for further research on the toxicity and mixture behavior of these environmentally and toxicologically relevant compounds.

  • 4.
    Lam, Monika M.
    et al.
    Örebro University, School of Science and Technology.
    Engwall, Magnus
    Örebro University, School of Science and Technology.
    Denison, Michael S
    Department of Environmental Toxicology, University of California, Davis CA, USA.
    Larsson, Maria
    Örebro University, School of Science and Technology.
    Methylated polycyclic aromatic hydrocarbons and/or their metabolites are important contributors to the overall estrogenic activity of polycyclic aromatic hydrocarbon-contaminated soils2018In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 37, no 2, p. 385-397Article in journal (Refereed)
    Abstract [en]

    In the present study 42 polycyclic aromatic compounds (PACs) were investigated for their estrogenic potential using the VM7Luc4E2 transactivation assay. Relative potencies were determined for mass-balance analysis. In addition, compounds were tested in combination with the estrogen receptor (ER) antagonist vertical bar C vertical bar 182,780 (vertical bar C vertical bar) and the aryl hydrocarbon receptor antagonist/CYP1A1 inhibitor a-naphthoflavone. Luciferase induction and CYP1A1-dependent ethoxyresorufin-O-deethylase (EROD) activity were measured to assess whether the estrogenic activity was elicited by the compound itself and/or by its metabolites. Relative potencies ranged between 10(-7) and 10(-4). The ability of ICI to decrease luciferase activity stimulated by all compounds indicated that the induction responses were ER-dependent. The aryl hydrocarbon receptor antagonist/CYP1A1 inhibitor a-naphthoflavone decreased luciferase induction and EROD activity by several compounds, including the methylated chrysenes, suggesting that metabolites of these chemicals contributed to ER activation. Several PACs, such as acridine and its derivatives, appear to directly activate the ER. Furthermore, extracts of soils from industrial areas were examined using this bioassay, and estrogenic activity was detected in all soil samples. Mass-balance analysis using a combination of relative potencies and chemical analysis of the samples suggested that polycyclic aromatic hydrocarbons (PAHs) and alkylated PAHs, such as 1-and 3-methylchrysene, are important contributors to the overall estrogenic activity. However, these results revealed that a considerable proportion of the estrogenic activity in the soil remained unexplained, indicating the presence of other significant estrogenic compounds.

  • 5.
    Larsson, Maria
    et al.
    Örebro University, School of Science and Technology.
    Lam, Monika M.
    Örebro University, School of Science and Technology.
    van Hees, Patrick
    Örebro University, School of Science and Technology. Eurofins Environment Testing Sweden AB, Lidköping, Sweden.
    Giesy, John P.
    University of Saskatchewan, Saskatoon, Canada.
    Engwall, Magnus
    Örebro University, School of Science and Technology.
    Occurrence and leachability of polycyclic aromatic compounds in contaminated soils: Chemical and bioanalytical characterization2018In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 622-623, p. 1476-1484Article in journal (Refereed)
    Abstract [en]

    An important concern regarding sites contaminated with polycyclic aromatic compounds (PACs) is the risk of groundwater contamination by release of the compounds from soils. The goal of this study was to investigate the occurrence and leachability of 77 PACs including polycyclic aromatic hydrocarbons (PAHs) and heterocyclic aromatic compounds (NSO-PACs) among total aryl hydrocarbon receptor (AhR) agonists in soils from historical contaminated sites. A novel approach combining chemical and bioanalytical methods in combination with characterization of leachability by use of a column leaching test was used. Similar profiles of relative concentrations of PACs were observed in all soils, with parent PAHs accounting for 71 to 90% of total concentrations in soils. Contribution of oxy-PAHs, alkyl-PAHs and N-PACs ranged from 2 to 9%, 3 to 9% and 1 to 14%, respectively. Although the contributions of groups of PACs were small, some compounds were found in similar or greater concentrations than parent PAHs. Leachable fractions of 77 PACs from soils were small and ranged from 0.002 to 0.54%. Polar PACs were shown to be more leachable than parent PAHs. The contribution of analyzed PACS to overall AhR-mediated activities in soils and leachates suggests presence of other AhR agonists in soils, and a potential risk. Only a small fraction of AhR agonists was available in soils, indicating an overestimation of the risk if only total initial concentrations in soils would be considered in risk assessment. The results of the study strongly support that focus on 16US EPA PAHs may result in inadequate assessment of risk and hazard of PACs in complex environmental samples.

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