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  • 1.
    Bergknut, Magnus
    Umeå University, Faculty of Science and Technology, Chemistry.
    Characterization of PAH-contaminated soils focusing on availability, chemical composition and biological effects2006Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The risks associated with a soil contaminated by polycyclic aromatic hydrocarbons (PAHs) are generally assessed by measuring individual PAHs in the soil and correlating the obtained amounts to known adverse biological effects of the PAHs. The validity of such a risk estimation is dependent on the presence of additional compounds, the availability of the compounds (including the PAHs), and the methods used to correlate the measured chemical data and biological effects. In the work underlying this thesis the availability, chemical composition and biological effects of PAHs in samples of soils from PAH-contaminated environments were examined. It can be concluded from the results presented in the included papers that the PAHs in the studied soils from industrial sites were not generally physically trapped in soil material, indicating that the availability of the PAHs was not restricted in this sense. However, the bioavailable fraction of the PAHs, as assessed by bioassays with the earthworm Eisenia Fetida, could not be assessed by a number of abiotic techniques (including: solid phase micro extraction, SPME; use of semi-permeable membrane devices, SPMDs; leaching with various solvent mixtures, leaching using additives, and sequential leaching) and it seems to be difficult to find a chemical method that can accurately assess the bioavailability of PAHs. Furthermore, it was shown that PAH-polluted samples may be extensively chemically characterized by GC-TOFMS using peak deconvolution, and over 900 components can be resolved in a single run. The chemical characterization also revealed that samples that appeared to be similar in terms of their PAH composition were heterogeneous in terms of their overall composition. Finally, single compounds from this large set of compounds, which correlated with different biological effects, could be identified using the multivariate technique partial least squares projections to latent structures (PLS). This indicates that PLS may provide a valid alternative to Effect Directed Analysis (EDA), an established method for finding single compounds that correlate to the toxicity of environmental samples. Thus, the instrumentation and data evaluation tools used in this thesis are clearly capable of providing a broad chemical characterization as well as linking the obtained chemical data to results from bioassays. However, the link between the chemical analyses and the biological tests could be improved as as an organic solvent that solubilised virtually all of the contaminants was used during the chemical analysis while the biological tests were performed in an aqueous solution with limited solubility for a number of compounds. Consequently the compounds probably have a different impact in the biological tests than their relative abundance in profiles obtained by standard chemical analyses suggests. The availability and bioavailability of contaminants in soil also has to be studied further, and such future studies should focus on the molecular interactions between the contaminants and different compartments of the soil. By doing so, detailed knowledge could be obtained which could be applied to a number of different contaminants and soil types. Such studies would generate the data needed for molecular-based modelling of availability and bioavailability, which would be a big step forward compared to current risk assessment practices.

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  • 2.
    Bergknut, Magnus
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Laudon, Hjalmar
    Jansson, Stina
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Larsson, Anna
    Gocht, Tilman
    Wiberg, Karin
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Atmospheric deposition, retention, and stream export of dioxins and PCBs in a pristine boreal catchment2011In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 159, no 6, p. 1592-1598Article in journal (Refereed)
    Abstract [en]

    The mass-balance between diffuse atmospheric deposition of organic pollutants, amount of pollutants retained by the terrestrial environment, and levels of pollutants released to surface stream waters was studied in a pristine northern boreal catchment. This was done by comparing the input of atmospheric deposition of polychlorinated dibenzo-p-dioxins and furans (PCDD/Fs) and PCBs with the amounts exported to surface waters. Two types of deposition samplers were used, equipped with a glass fibre thimble and an Amberlite sampler respectively. The measured fluxes showed clear seasonality, with most of the input and export occurring during winter and spring flood, respectively. The mass balance calculations indicates that the boreal landscape is an effective sink for PCDD/Fs and PCBs, as 96.0-99.9 % of received bulk deposition was retained, suggesting that organic pollutants will continue to impact stream water in the region for an extended period of time.

  • 3.
    Bergknut, Magnus
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Laudon, Hjalmar
    Wiberg, Karin
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Dioxins, PCBs, and HCB in soil and peat profiles from a pristine boreal catchment2010In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 158, no 7, p. 2518-2525Article in journal (Refereed)
    Abstract [en]

    The aim of this study was to explore how atmospherically derived soil pollution is affected by environmental processes at two typical boreal catchment landscape type settings: wetlands and forested areas. Measurements of hydrophobic organic compounds (HOCs) in forest soil and peat from an oligotrophic mire at various depths were performed at a remote boreal catchment in northern Sweden. HOCs in peat were evenly distributed throughout the body of the mire while levels of HOCs in the forest soil increased with increased amount of organic matter. Evaluation of HOC composition by principal component analysis (PCA) showed distinct differences between surface soils and deeper soil and peat samples. This was attributed to vertical transport, degradation and/or shifting sources over time. The calculated net vertical transport differed between surface layers (0.3%) and deeper soils (8.0%), suggesting that vertical transport conditions and processes differ in the deeper layers compared to the surface layers.

  • 4.
    Bergknut, Magnus
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Meijer, Sandra
    Halsall, Crispin
    Ågren, Anneli
    Laudon, Hjalmar
    Köhler, Stephan
    Jones, Kevin C
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Wiberg, Karin
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Modelling the fate of hydrophobic organic contaminants in a boreal forest catchment: a cross disciplinary approach to assessing diffuse pollution to surface waters2010In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 158, no 9, p. 2964-2969Article in journal (Refereed)
    Abstract [en]

    The fate of hydrophobic organic compounds (HOCs) in soils and waters in a northern boreal catchment was explored through the development of a chemical fate model in a well-characterised catchment system dominated by two land types: forest and mire. Input was based solely on atmospheric deposition, dominated by accumulation in the winter snowpack. Release from soils was governed by the HOC concentration in soil, the soil organic carbon fraction and soil-water DOC content. The modelled export of selected HOCs in surface waters ranged between 11 and 250ng day(-1) during the snow covered period, compared to 200 and 9600ng/d during snow-melt; highlighting the importance of the snow pack as a source of these chemicals. The predicted levels of HOCs in surface water were in reasonable agreement to a limited set of measured values, although the model tended to over predict concentrations of HOCs for the forested sub-catchment, by over an order of magnitude in the case of hexachlorobenzene and PCB 180. This possibly reflects both the heterogeneity of the forest soils and the complicated and changing hydrology experienced between the different seasons.

  • 5. Bergknut, Magnus
    et al.
    Persson, Per
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Skyllberg, Ulf
    Molecular characterization of brominated persistent pollutants using extended X-ray absorption fine structure (EXAFS) spectroscopy2008In: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650, Vol. 390, no 3, p. 921-928Article in journal (Refereed)
    Abstract [en]

    X-ray absorption fine structure (EXAFS) spectroscopy spectra were collected for three brominated persistent pollutants: 6-bromo-2,4,5-trichlorophenol (BrTriClP), pentabromophenol (PentaBrP) and 3,3',5,5'-tetrabromobisphenol A (TBBA). The substances were selected to be symmetrical (BrTriClP and TBBA) or asymmetrical (PentaBrP) with respect to the atomic Br positions and to differ in the number of bromine and other halide atoms, as well as their relative positions. The asymmetrical PentaBrP was modelled with special detail as not all bromine atoms have identical coordination environments. The studied substances displayed unique EXAFS spectra, which could be used to determine the molecular structure in fair detail. We conclude that EXAFS spectroscopy is a suitable technique for molecular characterization of the comparatively complex molecules within the class of compounds of brominated organic persistent pollutants. A detailed understanding of the EXAFS spectra of the pure compounds opens up possibilities to study the interactions with soil and sediment matrices by means of EXAFS spectroscopy. Figure Brominated organic persistent pollutants are characterized by EXAFS spectroscopy.

  • 6.
    Bergknut, Magnus
    et al.
    Umeå University, Faculty of Science and Technology, Chemistry.
    Sehlin, Emma
    Umeå University, Faculty of Science and Technology, Chemistry.
    Lundstedt, Staffan
    Umeå University, Faculty of Science and Technology, Chemistry.
    Andersson, Patrik L
    Umeå University, Faculty of Science and Technology, Chemistry.
    Haglund, Peter
    Umeå University, Faculty of Science and Technology, Chemistry.
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Chemistry.
    Comparison of techniques for estimating PAH bioavailability: uptake in Eisenia fetida, passive samplers and leaching using various solvents and additives.2007In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 145, no 1, p. 154-60Article in journal (Refereed)
    Abstract [en]

    The aim of this study was to evaluate different techniques for assessing the availability of polycyclic aromatic hydrocarbons (PAHs) in soil. This was done by comparing the amounts (total and relative) taken up by the earthworm Eisenia fetida with the amounts extracted by solid-phase microextraction (SPME), semi-permeable membrane devices (SPMDs), leaching with various solvent mixtures, leaching using additives, and sequential leaching. Bioconcentration factors of PAHs in the earthworms based on equilibrium partitioning theory resulted in poor correlations to observed values. This was most notable for PAHs with high concentrations in the studied soil. Evaluation by principal component analysis (PCA) showed distinct differences between the evaluated techniques and, generally, there were larger proportions of carcinogenic PAHs (4–6 fused rings) in the earthworms. These results suggest that it may be difficult to develop a chemical method that is capable of mimicking biological uptake, and thus estimating the bioavailability of PAHs.

    The total and relative amounts of PAHs extracted by abiotic techniques for assessing the bioavailability of PAHs was found to differ from the amounts taken up by Eisenia fetida.

    Keywords: Bioavailability; Polycyclic aromatic hydrocarbons; Earthworms; Leaching; Hydroxypropyl-β-cyclodextrin; Solid-phase microextraction; Semi-permeable membrane device

  • 7.
    Bergknut, Magnus
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Wiberg, Karin
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Klaminder, Jonatan
    Umeå University, Faculty of Science and Technology, Department of Ecology and Environmental Sciences.
    Vertical and lateral redistribution of POPs in soils developed along a hydrological gradient2011In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 45, no 24, p. 10378-10384Article in journal (Refereed)
    Abstract [en]

    Study of the dispersion of persistent organic pollutants (POPs) throughout the environment is necessitated by their toxicological properties and propensity to accumulate in biota. In this study, we use data from the analysis of three (210)Pb dated soil profiles collected along a 30-m hydrological gradient to demonstrate postdepositional mobility of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs) and polychlorinated biphenyls (PCBs). We found that (i) humus originating from litter exposed to surface fallout during the 1960-1970s contains the highest concentrations of PCDD/Fs and PCBs in the O-horizon of the soils; (ii) accumulation rates of PCDD/Fs and PCBs in the O-horizon (similar to 5.0 and similar to 210 mu g m(-2) yr(-1)) constituted only 9.1% and 3.5%, respectively, of the measured annual input, demonstrating that a minor fraction of the deposited material is retained within the O-horizon; (iii) POP inventories in the upper 0.5-0.9 m of the mineral soil constituted a considerable part (40-70%) of the total pool stored in the soil, implying significant vertical translocation of atmospheric derived POPs; and (iv) increasing downslope inventories of POPs suggest a lateral downward transport of POPs from uphill soils. The findings challenge the commonly accepted view that POPs fallout is effectively retained within O-horizons.

  • 8. Josefsson, Sarah
    et al.
    Bergknut, Magnus
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Futter, Martyn N.
    Jansson, Stina
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Laudon, Hjalmar
    Lundin, Lisa
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Wiberg, Karin
    Persistent Organic Pollutants in Streamwater: Influence of Hydrological Conditions and Landscape Type2016In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 50, no 14, p. 7416-7424Article in journal (Refereed)
    Abstract [en]

    Concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs), and hexachlorobenzene (HCB) in streamwater were measured in a remote catchment in northern Sweden and downstream to the Baltic Sea. Sampling took place at seven sites during two years and under different hydrological conditions: during the snow-free, snow-covered, and spring-flood seasons. Concentrations varied substantially between seasons and were up to 20 times higher during the spring flood compared to the preceding snow-covered period. The increase in concentrations with runoff was due to higher levels of particle-associated contaminants, while the dissolved concentrations remained stable. Particulate-contaminant concentrations were positively correlated primarily to suspended particulate matter (SPM) at sites in areas with a high land-cover fraction of sorted sediment. When upstream sampling locations were compared, a mire-dominated stream had higher concentrations and a lower retention of atmospherically deposited contaminants than a forest stream of the same catchment size. Contaminant concentrations (normalized to volume) did not increase consistently downstream despite the presence of several point sources. However, when normalized to the amount of SPM, concentrations were on average >20 times higher at the outlet in the Baltic Sea compared to the outlet from the remote catchment without point sources.

  • 9.
    Niinipuu, Mirva
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Latham, Kenneth G.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Boily, Jean-Francois
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Bergknut, Magnus
    MTC-Miljötekniskt Center AB, Umeå, Sweden.
    Jansson, Stina
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    The impact of hydrothermal carbonization on the surface functionalities of wet waste materials for water treatment applications2020In: Environmental Science and Pollution Research, ISSN 0944-1344, E-ISSN 1614-7499Article in journal (Refereed)
    Abstract [en]

    Hydrothermal carbonization (HTC) is an energy-efficient thermochemical process for converting wet waste products into value added materials for water treatment. Understanding how HTC influences the physicochemical properties of the resultant materials is critical in optimizing the process for water treatment, where surface functionality and surface area play a major role. In this study, we have examined the HTC of four wet waste streams, sewage sludge, biosludge, fiber sludge, and horse manure at three different temperatures (180 degrees C, 220 degrees C, and 260 degrees C). The physicochemical properties of these materials were examined via FTIR, SEM and BET with their adsorption capacity were assessed using methylene blue. The yield of solid material after hydrothermal carbonization (hydrochar) decreased with increasing temperature for all samples, with the largest impact on horse manure and fiber sludge. These materials also lost the highest degree of oxygen, while HTC had minimal impact on biosludge and sewage sludge. The differences here were due to the varying compositions of each waste material, FTIR identified resonances related to cellulose in horse manure and fiber sludge, which were not detected in biosludge and sewage sludge. Adsorption capacities varied between 9.0 and 68 mg g(-1) with biosludge HTC at 220 degrees C adsorbing the highest amount. Adsorption also dropped drastically at the highest temperature (260 degrees C), indicating a correlation between adsorption capacity and HTC conditions. This was attributed to the loss of oxygen functional groups, which can contribute to adsorption. These results suggest that adsorption properties can be tailored both by selection of HTC temperature and feedstock.

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  • 10. Nyman, Madeleine
    et al.
    Bergknut, Magnus
    Umeå University, Faculty of Science and Technology, Chemistry.
    Fant, Marie Louise
    Raunio, Hannu
    Jestoi, Marika
    Bengs, Charlotta
    Murk, Albertinka
    Koistinen, Jaana
    Bäckman, Christina
    Pelkonen, Olavi
    Tysklind, Mats
    Umeå University, Faculty of Science and Technology, Chemistry.
    Hirvi, Timo
    Contaminant exposure and effects in Baltic ringed and grey seals as assessed by biomarkers2003In: Marine Environmental Research, Vol. 55, no 1, p. 73-99Article in journal (Refereed)
    Abstract [en]

    The Baltic Sea ecosystem has suffered from a heavy pollutant load for more than three decades. Persistent organic pollutants (POPs) and heavy metals have been of most concern due to their persistence and toxic properties. Ringed seals (Phoca hispida baltica) and grey seals (Halichoerus grypus) living in the Baltic Sea have been suffering from pathological impairments, including reproductive disturbances, which have resulted in a depressed reproductive capacity. We investigated several biochemical parameters as potential biomarkers for exposure to and effects of the contaminant load in the Baltic seals. Seals from less polluted areas were used as reference material in terms of the pollution load. In both Baltic seal populations, the levels of some biochemical parameters diverged from those in the reference seals, and some of these showed a clear correlation with the individual contaminant load. Of the potential bioindicators, we propose cytochrome P4501A activity and vitamin E levels, in blubber or plasma, as exposure biomarkers for polychlorinated biphenyls (PCBs) and dichlorodiphenyltrichloroethane (DDT) in both species. The arylhydrocarbon receptor-mediated chemical-activated luciferase gene expression (CALUX) response reflects the whole PCB and DDT burden in ringed seals. Retinyl palmitate (vitamin A) levels showed a negative correlation with the individual POP load, and is proposed as potential effect biomarkers for the depletion of the vitamin A stores. As the nutritional levels of both vitamin A and E have an impact on the vitamin levels in the seals, more information on the dietary vitamin levels is needed before any conclusions can be drawn. As the relationship between biochemical parameters and contaminants varied between the two species, species-specific characteristics has to be considered when monitoring the health status and possible toxic effects of the contaminant load in ringed and grey seals.

  • 11. Rosen, Lars
    et al.
    Back, Par-Erik
    Soderqvist, Tore
    Norrman, Jenny
    Brinkhoff, Petra
    Norberg, Tommy
    Volchko, Yevheniya
    Norin, Malin
    Bergknut, Magnus
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Doberl, Gernot
    SCORE: A novel multi-criteria decision analysis approach to assessing the sustainability of contaminated land remediation2015In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 511, p. 621-638Article in journal (Refereed)
    Abstract [en]

    The multi-criteria decision analysis (MCDA) method provides for a comprehensive and transparent basis for performing sustainability assessments. Development of a relevant MCDA-method requires consideration of a number of key issues, e.g. (a) definition of assessment boundaries, (b) definition of performance scales, both temporal and spatial, (c) selection of relevant criteria (indicators) that facilitate a comprehensive sustainability assessment while avoiding double-counting of effects, and (d) handling of uncertainties. Adding to the complexity is the typically wide variety of inputs, including quantifications based on existing data, expert judgements, and opinions expressed in interviews. The SCORE (Sustainable Choice Of REmediation) MCDA-method was developed to provide a transparent assessment of the sustainability of possible remediation alternatives for contaminated sites relative to a reference alternative, considering key criteria in the economic, environmental, and social sustainability domains. The criteria were identified based on literature studies, interviews and focus-group meetings. SCORE combines a linear additive model to rank the alternatives with a non-compensatory approach to identify alternatives regarded as non-sustainable. The key strengths of the SCORE method are as follows: a framework that at its core is designed to be flexible and transparent; the possibility to integrate both quantitative and qualitative estimations on criteria; its ability, unlike other sustainability assessment tools used in industry and academia, to allow for the alteration of boundary conditions where necessary; the inclusion of a full uncertainty analysis of the results, using Monte Carlo simulation; and a structure that allows preferences and opinions of involved stakeholders to be openly integrated into the analysis. A major insight from practical application of SCORE is that its most important contribution may be that it initiates a process where criteria otherwise likely ignored are addressed and openly discussed between stakeholders. (C) 2015 Elsevier B.V. All rights reserved.

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