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Characterization of PAH-contaminated soils focusing on availability, chemical composition and biological effects
Umeå University, Faculty of Science and Technology, Chemistry.
2006 (English)Doctoral 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.

Place, publisher, year, edition, pages
Umeå: Kemi , 2006. , 58 p.
Keyword [en]
polycyclic aromatic hydrocarbons, PAHs, availability, bioavailability, chemical analysis, characterization, GC-TOFMS, bioassay, toxicity, biological testing, multivariate methods, PCA, PLS
National Category
Environmental Sciences
Identifiers
URN: urn:nbn:se:umu:diva-789ISBN: 91-7264-095-2 (print)OAI: oai:DiVA.org:umu-789DiVA: diva2:144540
Public defence
2006-06-01, KB3B1, KBC, Umeå Universitet, Umeå, 13:00 (English)
Opponent
Supervisors
Available from: 2006-05-09 Created: 2006-05-09 Last updated: 2010-02-01Bibliographically approved
List of papers
1. Assessment of the availability of polycyclic aromatic hydrocarbons from gasworks soil using different extraction solvents and techniques
Open this publication in new window or tab >>Assessment of the availability of polycyclic aromatic hydrocarbons from gasworks soil using different extraction solvents and techniques
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2004 (English)In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 23, no 8, 1861-1866 p.Article in journal (Refereed) Published
Abstract [en]

This study was designed to assess the availability of polycyclic aromatic hydrocarbons (PAHs) present at a gasworks site to different soil remediation techniques. The study examined the effect on PAH availability of using different organic solvents, the degree of pretreatment, and the extraction time. In total, 25 PAHs (with two to six fused rings) and five carbonyl derivatives were measured. The results indicated that the PAHs and their derivatives were bound loosely to the surface of the studied soil and that there were no significant kinetic boundaries associated with the extraction of the PAHs. Furthermore, it was concluded that the studied soil was not suitable for bioremediation, as the concentration of PAHs with low molecular weight were limited. However, pressurized liquid extraction (PLE) with methanol as the solvent extracted 97% of all PAHs and PAH-derivatives, indicating that extraction may be effective as part of a soil remediation technique for old gasworks soils.

Keyword
hydrocarbons, extraction, soil, availability, gasworks
Identifiers
urn:nbn:se:umu:diva-14289 (URN)doi:10.1897/03-201 (DOI)15352473 (PubMedID)
Available from: 2007-08-17 Created: 2007-08-17 Last updated: 2017-12-14Bibliographically approved
2. Comparison of techniques for estimating PAH bioavailability: uptake in Eisenia fetida, passive samplers and leaching using various solvents and additives.
Open this publication in new window or tab >>Comparison of techniques for estimating PAH bioavailability: uptake in Eisenia fetida, passive samplers and leaching using various solvents and additives.
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2007 (English)In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 145, no 1, 154-60 p.Article in journal (Refereed) Published
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

Keyword
1-Butanol/chemistry, Animals, Biological Availability, Chemistry; Physical, Excipients/chemistry, Membranes, Methanol/chemistry, Oligochaeta/*metabolism, Permeability, Polycyclic Hydrocarbons; Aromatic/analysis/*pharmacokinetics, Polysorbates/chemistry, Principal Component Analysis/methods, Soil Pollutants/analysis/*pharmacokinetics, Solid Phase Microextraction/methods, Solvents/chemistry, beta-Cyclodextrins/chemistry
Identifiers
urn:nbn:se:umu:diva-12588 (URN)doi:10.1016/j.envpol.2006.03.052 (DOI)16713049 (PubMedID)
Available from: 2007-04-12 Created: 2007-04-12 Last updated: 2017-12-14Bibliographically approved
3. Characterization and classification of complex PAH samples using GC-qMS and GC-TOFMS
Open this publication in new window or tab >>Characterization and classification of complex PAH samples using GC-qMS and GC-TOFMS
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2006 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 65, no 11, 2208-2215 p.Article in journal (Refereed) Published
Abstract [en]

The aim of this study was to compare the polycyclic aromatic hydrocarbon (PAH) contents in a number of complex samples, including soil samples from industrial sites, anti-skid sand, urban dust and ash samples from municipal solid waste incinerators. The samples were characterized by routine analysis of PAHs (gas chromatography–quadrupole mass spectrometry) and gas chromatography–time of flight mass spectrometry (GC–TOFMS). Classification of the samples by principal component analysis (PCA) according to their composition of PAHs revealed that samples associated with traffic and the municipal incinerator formed homogeneous clusters, while the PAH-contaminated soils clustered in separate groups. Using spectral data to resolve co-eluting chromatographic peaks, 962 peaks could be identified in the GC–TOFMS analysis of a pooled sample and 123–527 peaks in the individual samples. Many of the studied extracts included a unique set of chemicals, indicating that they had a much more diverse contamination profile than their PAH contents suggested. Compared to routine analysis, GC–TOFMS provided more detailed information about each sample and in this study a large number of alkylated PAHs were found to be associated with the corresponding unsubstituted PAHs. The possibility to filter peaks according to different criteria (e.g. to include only peaks that were detected in the analysis of another sample) was explored and used to identify unique as well as common compounds within samples. This procedure could prove to be valuable for obtaining relevant chemical data for use in conjunction with results from various biological test systems.

Keyword
Anti-skid sand, Urban dust; Traffic, Creosote, Peak deconvolution, PCA
Identifiers
urn:nbn:se:umu:diva-10919 (URN)doi:10.1016/j.chemosphere.2006.05.050 (DOI)16839586 (PubMedID)
Available from: 2007-04-11 Created: 2007-04-11 Last updated: 2017-12-14Bibliographically approved
4. Identification of potentially toxic compounds in complex extracts of environmental samples using GC-MS and multivariate data analysis
Open this publication in new window or tab >>Identification of potentially toxic compounds in complex extracts of environmental samples using GC-MS and multivariate data analysis
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2007 (English)In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 26, no 2, 208-17 p.Article in journal (Refereed) Published
Abstract [en]

In this study, we examined 31 samples of varying chemical composition, including samples of soils from gasworks, coke production sites, and sites where wood preservatives were heavily used; ash and soot from municipal solid waste incinerators; antiskid sand; and dust from areas with heavy road traffic. The samples were comprehensively chemically characterized, especially their polycyclic aromatic compound contents, using gas chromatography–time-of-flight mass spectrometry, whereas their biological effects were assessed using dehydrogenase activity, root growth (Hordeum vulgare), reproduction of springtails (Folsomia candida), algal growth (Desmodesmus subspicatus), germinability (Sinapis alba), Vibrio fischeri, DR-CALUX, and Ames Salmonella assays. The number of compounds detected in the samples ranged from 123 to 527. Using the multivariate regression technique of partial-least-squares projections to latent structures, it was possible to find individual compounds that exhibited strong correlations with the different biological responses. Some of the results, however, indicate that a broader chemical characterization may be needed to identify all the compounds that may cause the measured biological responses.

Keyword
Soil, Polycyclic aromatic compounds, Bioassay, Multivariate techniques
Identifiers
urn:nbn:se:umu:diva-12347 (URN)doi:10.1897/06-204R.1 (DOI)
Available from: 2007-06-12 Created: 2007-06-12 Last updated: 2017-12-14Bibliographically approved

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