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Methodologies to assess the fate of polar organic compounds in aquatic environments
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM). (ITMo)
2010 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Polar organic compounds (POCs) are chemicals with polar functional groups in their structure. The functional groups make the compounds hydrophilic and less prone to partition with biota. However, the knowledge of their fate is limited due to difficulties associated with their measurements. Although, the persistence of POCs in the environment is generally low, they are considered to be semi-persistent compounds due to their continuous introduction to the environment via wastewater. Studies have shown that complex mixtures of POCs of different classes may have synergistic toxic effects on biota at environmental concentration levels. Therefore, it is important to develop analytical methods in order to establish the occurrence and fate of POCs in aquatic environments.

In Study I, a positive correlation between the sorption of a novel poly(ethylene-co-vinyl acetate-co-carbon monoxide) (PEVAC) material and the theoretical logarithmic dissociation partition coefficient (Log D) for seven POCs was observed. The PEVAC material showed an enhanced sorption of the POCs compared to the silicone material. Study II, demonstrated that the PEVAC sampler assess the freely dissolved concentration of POCs in aquatic environments. The results showed that the PEVAC polymer is an attractive alternative to silicone for mimicing the biological uptake of POCs in aquatic environments. Additionally, Study II showed that total extraction is appropriate for determination of the freely dissolved concentration of uncharged POCs with Log KOW < 2.67 in natural water.

In study III, a novel bag-solid phase extraction (bag-SPE) technique was compared to a conventional SPE-technique. Despite that the extraction efficiencies for POCs in wastewater were lower using the bag-SPE method, the two methods showed similar detection limits due to the lower ion-suppression experienced with the bag-SPE.

In study IV the bag-SPE method was further developed with the aim of lowering the detection limits for POCs. Detection limits (LOD) below 13 ng/L showed that the bag-SPE method was suitable for determination of POCs in surface sea water.

 

Place, publisher, year, edition, pages
Stockholm: Department of Applied Environmental Science (ITM), Stockholm University , 2010. , 25 p.
Keyword [en]
Passive equilibrium sampler, Absorbent, Polar organic compounds, Liquid chromatography-mass spectrometry, Partitioning coefficient, Fulvic acid, Sediment, PEVAC, Bag-SPE, Solid phase extraction, Pharmaceuticals, Wastewater, Sea water, UPLC-QToF
National Category
Environmental Sciences Analytical Chemistry
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-35552ISBN: 978-91-7447-003-1 (print)OAI: oai:DiVA.org:su-35552DiVA: diva2:287487
Public defence
2010-02-12, Nordenskiöldsalen, Geovetenskapens hus, Svante Arrhenius väg 12, Stockholm, 10:00 (Swedish)
Opponent
Supervisors
Projects
This research was financially supported by European Union (European Commission, FP6 Contract No. 003956) “Novel Methods for Integrated Risk Assessment of Cumulative Stressors in the Environment” (NoMiracle) and by the Swedish research council Formas.
Available from: 2010-01-21 Created: 2010-01-18 Last updated: 2010-01-18Bibliographically approved
List of papers
1. Evaluation of poly(ethylene-co-vinyl acetate-co-carbon monoxide) and polydimethylsiloxane for equilibrium sampling of polar organic contaminants in water.
Open this publication in new window or tab >>Evaluation of poly(ethylene-co-vinyl acetate-co-carbon monoxide) and polydimethylsiloxane for equilibrium sampling of polar organic contaminants in water.
2009 (English)In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 28, no 9, 1874-80 p.Article in journal (Refereed) Published
Abstract [en]

The aim of the present study was to develop a passive absorptive equilibrium sampler that would enable the determination of the concentrations of polar organic compound (POC) in water more efficiently than existing techniques. To this end, a novel plastic material, poly(ethylene-co-vinyl acetate-co-carbon monoxide) (PEVAC), was evaluated and the results were compared with an existing silicone-based passive absorptive equilibrium device. Seven compounds (imidacloprid, carbendazim, metoprolol, atrazin, carbamazepine, diazinon, and chlorpyrifos), a mixture of pharmaceuticals, and pesticides with a logarithmic octanol-water partition coefficient ranging from 0.2 to 4.77 were selected as model substances for the experiments. The results showed that six of the seven selected POCs reached distribution equilibrium within 4 d in the two materials tested. A linear relation with a regression coefficient of more than 0.8906 between the established logarithmic absorbent-water partition coefficient and the calculated logarithmic dissociation partition coefficient of the selected compounds in the two polymers was observed. The correlation between these two coefficients was within one order of magnitude for the compounds that reached equilibrium in the two polymers, which demonstrates that both materials are suitable for mimicking biological uptake of POCs. The PEVAC material showed an enhanced sorption for all selected compounds compared to the silicone material and up to five times higher enrichment for the most polar compound. Fluorescence analysis of the sampler cross-section, following the uptake of fluoranthene, and proof that the sorption was independent of surface area variations demonstrated that the PEVAC polymer possessed absorptive rather than adsorptive enrichment of organic compounds.

Keyword
Passive equilibrium sampler, Absorbent, Polar organic compounds, Liquid chromatography-mass spectrometry
National Category
Earth and Related Environmental Sciences Natural Sciences
Identifiers
urn:nbn:se:su:diva-34623 (URN)10.1897/09-036.1 (DOI)000268876200011 ()19938334 (PubMedID)
Available from: 2010-01-11 Created: 2010-01-11 Last updated: 2017-12-12Bibliographically approved
2. The Ability of a Novel Sorptive Polymer to Determine the Freely Dissolved Fraction of Polar Organic Compounds in the Presence of Fulvic Acid or Sediment
Open this publication in new window or tab >>The Ability of a Novel Sorptive Polymer to Determine the Freely Dissolved Fraction of Polar Organic Compounds in the Presence of Fulvic Acid or Sediment
2009 (English)In: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650, Vol. 395, no 5, 1525-1532 p.Article in journal (Refereed) Published
Abstract [en]

In the present study, a novel plastic material, poly(ethylene-co-vinyl acetate-co-carbon monoxide) (PEVAC), was evaluated as an absorptive passive equilibrium sampler for determination of the freely dissolved fraction of seven polar organic contaminants (POCs) in the presence of fulvic acid (FA) and sediment. The seven compounds selected were imidacloprid, carbendazim, metoprolol, atrazin, carbamazepine, diazinon and chlorpyrifos, i.e. a mixture of pharmaceuticals and pesticides having logarithmic octanol/water partitioning coefficient (Log KOW) ranging from 0.2 to 4.77.

The experiments demonstrated that the PEVAC sampler is well suited for determination of the freely dissolved fraction of chemicals in aquatic environments. Generally, the freely dissolved fraction of the POCs decreased with increasing hydrophobicity. However, strong interactions with functional groups of the organic matter seemed to dominate the partitioning for imidacloprid and carbendazim, having logarithmic dissociation partition coefficient (Log D) < 1.47, and for metoprolol which is positively charged at neutral pH.

Place, publisher, year, edition, pages
Springer, 2009
Keyword
Partitioning coefficient, Polar organic compounds, Fulvic acid, Sediment, PEVAC, LC-MS
National Category
Analytical Chemistry
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-35503 (URN)10.1007/s00216-009-3100-6 (DOI)000270897000034 ()
Projects
This research was financially supported by European Union (European Commission, FP6 Contract No. 003956) “Novel Methods for Integrated Risk Assessment of Cumulative Stressors in the Environment” (NoMiracle).
Available from: 2010-01-18 Created: 2010-01-18 Last updated: 2017-12-12Bibliographically approved
3. Bag-SPE – A convenient extraction method for screening of pharmaceutical-residues in influent and effluent water from sewage treatment plants
Open this publication in new window or tab >>Bag-SPE – A convenient extraction method for screening of pharmaceutical-residues in influent and effluent water from sewage treatment plants
2009 (English)In: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650, Vol. 395, no 5, 1481-1489 p.Article in journal (Refereed) Published
Abstract [en]

Bag-SPE is a solid phase extraction (SPE) technique here applied to sample pharmaceutical residues in wastewater. The device consisting of 20 mg polystyrene-divinylbenzene (PS-DVB) enclosed in a woven polyester-fabric was immersed into 20 mL sample. Extraction of the analytes was performed under gentle rotation (25 rpm) until distribution equilibrium was achieved (4 hours). The extraction efficiency for thirteen pharmaceuticals was evaluated for the bag-SPE sampler compared to a conventional SPE cartridge (Oasis HLB). All analyzes were determined on an ultra performance liquid chromatography (UPLC) coupled to a quadrupole time of flight (QToF) mass spectrometer.

The detection limit of the bag-SPE technique for the analytes in wastewater ranged from 15-100 ng/L with recoveries between 20.7-58.2 % and ion-suppressions between 2.2-53.2 %. Although the extraction efficiencies were lower with the bag-SPE sampler compared to the SPE technique, the two methods showed similar detection limits due to the lower ion-suppression experienced with the bag-SPE. The results demonstrate that bag-SPE is an attractive alternative to the more, in terms of manual handling, demanding SPE-technique.

Place, publisher, year, edition, pages
Springer, 2009
Keyword
Bag-SPE, Solid phase extraction, Pharmaceuticals, Wastewater, UPLC-QToF
National Category
Analytical Chemistry
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-35522 (URN)10.1007/s00216-009-3099-8 (DOI)000270897000030 ()
Projects
This research was financially supported by European Union (European Commission, FP6 Contract No. 003956) “Novel Methods for Integrated Risk Assessment of Cumulative Stressors in the Environment” (NoMiracle) and by the Swedish research council Formas.
Available from: 2010-01-18 Created: 2010-01-18 Last updated: 2017-12-12Bibliographically approved
4. Development of a method for determination of pharmaceutical residues in surface sea water using bag-SPE and UPLC-QToF
Open this publication in new window or tab >>Development of a method for determination of pharmaceutical residues in surface sea water using bag-SPE and UPLC-QToF
(English)Manuscript (preprint) (Other academic)
Abstract [en]

In the present study, a multi-residue method based on a bag –solid phase extraction (bag-SPE) technique was applied to determine the occurrence of ten pharmaceuticals in surface water close to the effluent of a sewage treatment plant (STP) and along a coastal gradient from a STP effluent.

The ten compounds selected were caffeine, atenolol, metoprolol, oxazepam, carbamazepine, ketoprofen, naproxen, ibuprofen, diclofenac and gemfibrozil, i.e. a mixture of pharmaceuticals of different therapeutic classes having logarithmic octanol/water partitioning coefficients (Log KOW) ranging from -0.13 to 4.39.

All analyses were performed using ultra performance liquid chromatography (UPLC) combined with quadrupole time-of-flight (QToF) mass spectrometry.

The detection limit (LOD) of the pharmaceuticals in water ranged from 1.0-13 ng/L. The method showed consistent linear concentration ranges from 25-800 ng/L with regression coefficients (R2) better than 0.9801. The recoveries of the selected analytes ranged from 10.6-64.5 % with relative standard deviations (RSD) of < 16.4 % and inter-day variations of less than 17.7 %.

Although the detection limits (LOD) of the analytes were low, only four of the selected ten pharmaceuticals (caffeine, metoprolol, oxazepam and carbamazepine) showed concentrations in surface water higher than the detection levels. The concentrations of the four pharmaceuticals in sea water range from 4-210 ng/L.

Keyword
Bag-SPE, Solid phase extraction, Pharmaceuticals, Sea water, UPLC-QToF
National Category
Analytical Chemistry
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-35549 (URN)
Projects
This research was financially supported by European Union (European Commission, FP6 Contract No. 003956) “Novel Methods for Integrated Risk Assessment of Cumulative Stressors in the Environment” (NoMiracle) and by the Swedish research council Formas.
Available from: 2010-01-18 Created: 2010-01-18 Last updated: 2016-01-29Bibliographically approved

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