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Use of non-targeted environmetrics and comprehensive two-dimensional gas chromatography to assess sewage treatment plant removal efficiencies of structurally diverse organic contaminants
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.
(English)Manuscript (preprint) (Other academic)
Abstract [en]

This study provides a new tool for the systematic and comprehensive screening of chemicals present in sewage and simultaneous assessment of sewage treatment plant (STP) removal efficiencies. Flow proportional samples were collected from a Swedish municipal STP, subjected to non-discriminating extraction and clean-up, and analyzed by comprehensive two-dimensional gas chromatography mass spectrometry (GCxGC-MS). Comparative environmetrics were used for outlier screening and removal efficiency assessment. The overall removal efficiency was good, but about 200 compounds were poorly extracted (<65%), of which 68 were tentatively identified based on their mass spectra and GC retention behavior. Most of the poorly extracted compounds were found in the aqueous phase of the effluent, with concentrations ranging from 0.2 to 12 000 ng L-1. Two amides (carbamazepine and diethyltoluamide (DEET)) were completely dissolved and not removed at all during treatment. Most of the compounds were aromatic (68%) or S,N,O-heterocyclic (31%) and chemically rather stable. All the compounds contained polar functional groups or moieties, which increase their water solubility and make them more prone to pass the STP unaffected. The new approach was used to identify new and emerging compounds, and generate information that could be used to improve current or design new STP treatment technologies.

National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:umu:diva-51311OAI: oai:DiVA.org:umu-51311DiVA: diva2:478977
Available from: 2012-01-17 Created: 2012-01-17 Last updated: 2012-01-18Bibliographically approved
In thesis
1. Removal processes in sewage treatment plants: Sludge quality and treatment efficiency of structurally diverse organic compounds
Open this publication in new window or tab >>Removal processes in sewage treatment plants: Sludge quality and treatment efficiency of structurally diverse organic compounds
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Large and ever-increasing numbers of chemicals, including large quantities of a broad spectrum of organic compounds are used in modern society. More than 30 000 of the more than 100 000 chemical substances registered in the EU are estimated to be daily used, of which many will be discharged into the waste-streams handled by municipal sewage treatment plants (STPs). The main objective of the work underlying this thesis was to improve understanding of the relationships between the characteristics of sewage contaminants and their sewage treatment efficiency. Further objectives were to examine the relationships between socio-economic uses of chemicals and sludge quality, and the effects of regulatory actions on sludge quality.

The quality of the sewage sludge and the levels and distribution patterns of the sludge contaminants, both within and between the STPs, seem to remain quite constant over time. The overall findings indicate that the levels of contaminants in sewage sludge seem to be largely independent of the location, size and treatment techniques applied at the STPs, and generally, of the types of human activity connected to them. The total and relative concentrations of the sludge contaminants were found to be fairly constant on a dry weight basis, with some exceptions, indicating that the pollutants originate from broad usage and diffuse dispersion rather than (industrial) point sources. The proportion of cyclic methylsiloxanes recovered in sludge seems to strongly depend on their vapour pressure, which decreases with the number of siloxane units. The higher water solubility and biodegradability of organophosphorus flame retardants and plasticizers than polybrominated diphenyl ethers (PBDEs) were also reflected in lower percentages (relative to their national use) found in sludge.

Significant time-trends in levels of a-third of the sludge contaminants included in the annual national measurement program were detected over a period of seven years. The levels of compounds displaying significant time-trends generally decreased following declines in the quantities used nationally. However, a quarter of these compounds showed increasing trends, of which the linear methylsiloxanes followed the same trend as used quantities. The decaBDE was also found to be increasing in sludge, probably as a result of the phase-out of pentaBDE and octaBDE.

The results indicate that the STP removal efficiency of anthropogenic substances, in Sweden, is generally good and that STPs, at least those in cold climates, do not efficiently remove certain polar contaminants. A non-targeted screening (by use of environmetrics and GCxGC-TOFMS) was performed and found to fulfil the objective to assess the STP removal efficiency, with emphasis to systematically analyse which compound classes that are not efficiently removed using the current STP technology. Many polar aromatic compounds were identified to be poorly removed.

The acquired data on levels, profiles and variations in sludge contaminants (sludge quality) extend both the available information and understanding of the degree and nature of sludge contamination, which should help attempts to track changes in its contaminants and revisions, if necessary, of guideline values. This thesis also contributes to improve the knowledge base for the development of future STP technologies, and that archived sewage sludge can be used in retrospective analysis of new and emerging pollutants.

Place, publisher, year, edition, pages
Umeå: Umeå universitet, 2012. 90 p.
Keyword
Environmetrics, flame retardants, GCxGC, non-targeted screening, mass flow, metals, plasticizers, poorly removed contaminants, POP, PPCP, prediction, Principal Component Analysis, removal efficiency, sewage, sewage treatment plants, sludge, sludge adsorption, sources, time-trend analysis
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-51315 (URN)978-91-7459-356-3 (ISBN)
Public defence
2012-02-10, Naturvetarhuset, Hörsal N320, Umeå universitet, Umeå, 10:00 (English)
Opponent
Supervisors
Available from: 2012-01-20 Created: 2012-01-17 Last updated: 2012-01-18Bibliographically approved

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Olofsson, UlrikaHaglund, Peter

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