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Behavior of fluoroquinolones and trimethoprim during mechanical, chemical, and active sludge treatment of sewage water and digestion of sludge
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.
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2006 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 40, no 3, 1042-1048 p.Article in journal (Refereed) Published
Abstract [en]

The behavior and fate of three fluoroquinolones (norfloxacin, ofloxacin, and ciprofloxacin), one sulfonamide (sulfamethoxazole), and trimethoprim were investigated at a sewage treatment plant in Umeå, Sweden, in 2004. This plant uses conventional mechanical, chemical, and activated sludge methods to treat the sewage water and digest the sludge; the dewatered digested sludge is pelleted (dry weight > 90% of total weight). Raw sewage water and particles as well as effluents and sludge from specific treatment areas within the plant were sampled. In addition to quantifying the antibiotics within the plant, we characterized the sample matrixes to facilitate evaluation of the results. Of the five substances examined, only norfloxacin, ciprofloxacin, and trimethoprim were present in concentrations higher than their limits of quantification. Norfloxacin and ciprofloxacin sorbed to sludge in a manner that was independent of changes in pH during sewage treatment, and more than 70% of the total amount of these compounds passing through the plant was ultimately found in the digested sludge. The results suggest that fluoroquinolones undergo thermal degradation during pelleting, but more studies are needed to confirm this. Trimethoprim was found in the final effluent at approximately the same concentration and mass flow as in the raw sewage, and could not be quantified in any solid sample. Predicted environmental concentrations, based on consumption data for Umeå municipality, correlated well with the results obtained, especially when the predicted concentrations were corrected to account for the amount of each active substance excreted in urine. The results obtained were compared to those of previous studies of these three substances' behavior and fate and were found to be similar, although some of the other plants studied employed the various treatment steps in different orders.

Place, publisher, year, edition, pages
Washington: American Chemical Society , 2006. Vol. 40, no 3, 1042-1048 p.
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:umu:diva-5050DOI: 10.1021/es0516211OAI: oai:DiVA.org:umu-5050DiVA: diva2:144403
Available from: 2006-04-07 Created: 2006-04-07 Last updated: 2017-12-14Bibliographically approved
In thesis
1. Determination of Antibiotics in the Swedish Environment with Emphasis on Sewage Treatment Plants
Open this publication in new window or tab >>Determination of Antibiotics in the Swedish Environment with Emphasis on Sewage Treatment Plants
2006 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [sv]

Metoder har utvecklats för att kunna bestämma tolv antibiotikasubstanser, vanliga inom human medicin, i miljöprover. Fokus lades på trimetoprim samt substanser från följande grupper: fluorokinoloner, sulfonamider, penicilliner, cefalosporiner, nitroimidazoler, tetracykliner samt makrolider. Vid extraktion användes fast-fas extraktion för vattenprover och ultraljuds-assisterad fast-fas/vätske extraktion för fasta prover. För separering och bestämning användes vätskekromatografi tandemmasspektrometri. Interna standarder nyttjades för att öka noggrannhet och precision. Extraktionsutbyte låg mellan 50% och 100% för vattenfaser och 14% och 100% för fasta faser. Koncentrationer och massflöden bestämdes för antibiotikasubstanser i inkommande och utgående vatten och slam, från fem avloppreningsverk i Sverige, samt i avloppsvatten från ett sjukhus. I sjukhusavloppsvattnet så påträffades ciprofloxacin (en fluorokinolon) och metronidazol (en nitroimidazol) i höga halter (µg/L nivå). Screening-studien vid de fem avloppsreningsverken visade att norfloxacin, ofloxacin, ciprofloxacin och doxycyklin ofta förekom i inkommande och utgående vatten och slam. Trimetoprim och sulfametoxazol påvisades inte i slam men förekom i snarlika koncentrationer i det utgående vattnet relativt det inkommande. I vattenfasen så förekom de sex antibiotikasubstanserna i ng/L nivån och i slam förekom norfloxacin, ofloxacin, ciprofloxacin, och doxycyklin i låga mg/kg nivån. En studie genomfördes där beteendet hos antibiotikasubstanser under avloppsrening studerades. De två fluorokinolonerna, norfloxacin och ciprofloxacin, adsorberade till slam och mindre än 5% av den totala mängd som kommer till avloppsreningsverket påvisades i det utgående vattnet. I slam var motsvarande andel 70%. Resultat från en process som värmebehandlar rötat avvattnat slam antyder att cirka 50% av de två fluorokinolonerna bryts ner. Trimetoprim adsorberade inte till slam och 100% av total mängd återfanns i det utgående vattnet. Teoretiska beräkningar av koncentrationer och massflöden visade god korrelation till kvantitativa resultat. Ökad noggrannhet i beräkningarna fås genom att beakta stabilitet och fasfördelning. Effekten av antibiotikasubstanser i miljön är idag okänd. Resultat från testprotokoll där deras toxicitet bedöms är i många fall irrelevanta. Tester där organismer är kroniskt exponerade av biologiskt aktiva substanser vid låga koncentrationer är få. Dessutom så fokuserar de ej på de stora potentiella effekterna såsom utveckling eller bevaring av resistenta stammar av bakterier i miljön. Ytterligare studier av förekomst, öde och effekt av antibiotikasubstanser i miljön är nödvändiga.

Abstract [en]

Methods were developed for determining levels in environmental samples of twelve antibiotics that are commonly used in human medicine: trimethoprim and substances from the following groups: fluoroquinolones, sulfonamides, penicillins, cephalosporines, nitroimidazoles, tetracyclines and macrolides. These substances were extracted from liquid and solid samples by solid phase extraction and ultrasonic-assisted liquid/solid extraction, respectively. Liquid chromatography tandem mass spectrometry was then used to separate and quantify them, and internal standards were added to improve the accuracy and precision of the determinations. Extraction yields from aqueous and solid phases were in the ranges 50 - 100% and 14 - 100%, respectively. Concentrations and mass flows of antibiotic substances were determined in a hospital effluent and in the raw sewage water, final effluent, and sludge from five sewage treatment plants (STPs) scattered across Sweden. High levels (in the µg/L range) of ciprofloxacin (a fluoroquinolone) and metronidazole (a nitroimidazole), were found in the hospital effluent. The screening study of the five sewage treatment plants revealed that norfloxacin, ofloxacin, ciprofloxacin, and doxycycline were frequently present in the raw sewage water, final effluent and sludge. Trimethoprim and sulfamethoxazole were not detected in the sludge, but these substances were present in the final effluents at concentrations close to those of the raw sewage water. In the aqueous phase, these six antibiotics were present in the ng/L range and in the solid phase, norfloxacin, ofloxacin, ciprofloxacin, and doxycycline were present in the low mg/kg range. The behaviour of the antibiotic substances during sewage water treatment was also investigated in one of the STPs. The two fluoroquinolones, norfloxacin and ciprofloxacin, sorbed to sludge, and less than 5% of the total amounts that entered the STP were found in the final effluent. In sludge, the corresponding figure was 70%. Results from a process in which digested dewatered sludge was treated with heat (producing pellets) indicated that approximately 50% of the two fluoroquinolones had been degraded. Trimethoprim did not sorb to sludge and 100% of its total amount was found in the final effluent. Theoretical calculations of concentrations and mass flows correlated well with quantitative results for the antibiotics that were frequently detected, but not for the others. In order to increase the accuracy of the calculations, the stability and phase distribution of the antibiotics should be considered. The effects of antibiotics present in the environment are currently unknown. Results of test protocols to assess their toxicity are often irrelevant, and there have been few tests in which organisms have been chronically exposed to biologically active substances at low concentrations. In addition, these tests have not addressed the immense potential of antibiotics in the environment to induce the development of resistant strains of bacteria and to maintain populations of resistant strains. Further studies of the occurrence, fate, and, effects of antibiotic substances in the environment are required.

Place, publisher, year, edition, pages
Umeå: Kemi, 2006. 31 p.
Keyword
antibiotics, environment, sewage treatment plants, antibiotika, miljö, avloppsreningsverk
National Category
Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-745 (URN)91-7264-045-6 (ISBN)
Public defence
2006-04-28, KB3B1, KBC-huset, Umeå, 13:00 (English)
Opponent
Supervisors
Available from: 2006-04-07 Created: 2006-04-07 Last updated: 2009-06-09Bibliographically approved
2. 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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