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Determination of Antibiotics in the Swedish Environment with Emphasis on Sewage Treatment Plants
Umeå University, Faculty of Science and Technology, Chemistry.
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 [en]
antibiotics, environment, sewage treatment plants
Keyword [sv]
antibiotika, miljö, avloppsreningsverk
National Category
Environmental Sciences
Identifiers
URN: urn:nbn:se:umu:diva-745ISBN: 91-7264-045-6 (print)OAI: oai:DiVA.org:umu-745DiVA: diva2:144405
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
List of papers
1. Determination of antibiotic substances in hospital sewage water using solid phase extraction and liquid chromatography/mass spectrometry and group analogue internal standards
Open this publication in new window or tab >>Determination of antibiotic substances in hospital sewage water using solid phase extraction and liquid chromatography/mass spectrometry and group analogue internal standards
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2004 (English)In: Chemosphere, ISSN 0045-6535, Vol. 57, no 10, 1479-88 p.Article in journal (Refereed) Published
Abstract [en]

A method for determination of antibiotics in hospital sewage water has been developed and validated. Analogue internal standards for fluoroquinolones, sulfonamides, trimethoprim, β-lactams (penicillins and cephalosporines), nitroimidazoles and tetracyclines were successfully used for calibration and shown to generally improve precision compared to external calibration. Matrix components caused ion suppression/enhancement effects during the MS detection for all analytes studied. Two effects were observed: general suppression and short-term variations in the MS response.

In the hospital sewage water large temporal variations in the analyte concentration were observed during the course of the sampling period (seven grab samples in 13 h). Analyte concentrations varied within the following ranges (in μg l−1): ciprofloxacin, 3.6–101.0; metronidazole, 0.1–90.2; sulfamethoxazole, 0.4–12.8; ofloxacin, 0.2–7.6; trimethoprim, 0.6–7.6; and doxycycline, 0.6–6.7.

Keyword
Antibiotics, LC-MS, Internal standard, Matrix effects, Hospital wastewater
Identifiers
urn:nbn:se:umu:diva-14354 (URN)doi:10.1016/j.chemosphere.2004.09.015 (DOI)
Available from: 2008-01-08 Created: 2008-01-08 Last updated: 2011-01-12Bibliographically approved
2. Screening of human antibiotic substances and determination of weekly mass flows in five sewage treatment plants in Sweden
Open this publication in new window or tab >>Screening of human antibiotic substances and determination of weekly mass flows in five sewage treatment plants in Sweden
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2005 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 39, no 10, 3421-3429 p.Article in journal (Refereed) Published
Abstract [en]

Twelve antibiotic substances for human use, including trimethoprim and representatives of the fluoroquinolone (FQ), sulfonamide (SA), penicillin (PE), cephalosporin (CE), nitroimidazole (NI), tetracycline (TC), and macrolide (MA) groups, were subjected to a screening study at five Swedish sewage treatment plants (STPs) during one week in 2002 and one week in 2003. The analytes were extracted from raw sewage water, final effluent, and sludge by solid-phase extraction (SPE) or liquid-solid extraction (as appropriate) and then identified and quantified by liquid chromatography/tandem mass spectrometry. The most frequently detected antibiotics in the matrices considered in this study were norfloxacin, ofloxacin, ciprofloxacin, trimethoprim, sulfamethoxazole, and doxycycline. The other analytes were only detected in a few samples. Analysis of the weekly mass flows through each STP showed that FQs were partly eliminated from the water during sewage water treatment and the highest amounts of these substances were found in sludge. Sulfamethoxazole and trimethoprim were mainly found in raw sewage water and final effluent, but these substances had balancing mass flows, indicating that they too can withstand sewage water treatment. The mass flow patterns for doxycycline were more complex, with high amounts occurring in sludge in some cases, suggesting that the behavior of this analyte may be more strongly influenced by the treatment process and other variables at individual STPs. The environmental load (the sum of the amounts in the final effluent and sludge) normalized to the number of inhabitants in the catchment area of each investigated STP compared with theoretical predictions based on consumption data (in parentheses) showed good correlations: norfloxacin, 0.8 (0.9); ofloxacin, 0.3 (0.2); ciprofloxacin, 1.3 (3.5); sulfamethoxazole, 0.2 (0.4); trimethoprim, 1.1 (1.0); and doxycycline, 0.7 (0.4) mg per person per week. The results show that reasonably accurate predictions of environmental load of these antibiotics can be time-effectively derived from consumption data without additional measurements.

Identifiers
urn:nbn:se:umu:diva-14358 (URN)10.1021/es048143z (DOI)
Available from: 2007-08-17 Created: 2007-08-17 Last updated: 2017-12-14Bibliographically approved
3. Behavior of fluoroquinolones and trimethoprim during mechanical, chemical, and active sludge treatment of sewage water and digestion of sludge
Open this publication in new window or tab >>Behavior of fluoroquinolones and trimethoprim during mechanical, chemical, and active sludge treatment of sewage water and digestion of sludge
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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
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-5050 (URN)10.1021/es0516211 (DOI)
Available from: 2006-04-07 Created: 2006-04-07 Last updated: 2017-12-14Bibliographically approved
4. Environmental risk assessment of antibiotics in the Swedish environment with emphasis on sewage treatment plants.
Open this publication in new window or tab >>Environmental risk assessment of antibiotics in the Swedish environment with emphasis on sewage treatment plants.
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2007 (English)In: Water Research, ISSN 0043-1354, Vol. 41, no 3, 613-9 p.Article in journal (Refereed) Published
Abstract [en]

The potential risks associated with antibiotics present in the Swedish environment were assessed using concentrations found in hospital effluent, and sewage treatment waters and sludge, in combination with data on their environmental effects obtained from the literature. For the aqueous environment, measured environmental concentrations and effect/no observed effect concentration ratios were much lower than one in most cases. The only exceptions, where concentrations of the investigated substances were high enough to pose potential risks, were the concentrations of the two fluoroquinolones, ofloxacin and ciprofloxacin, in the hospital effluent. Treating digested dewatered sludge by heat did not fully eliminate norfloxacin or ciprofloxacin, thus pellets may still contain high amounts of these substances (sub to low mgkg(-1)dw). In leaching tests less than 1% of the amounts of these fluoroquinolones in the sludge or pellets reached the aqueous phase, indicating that their mobility is limited if sludge is used to fertilize soil.

Keyword
Environmental risk assessment, Antibiotics, Sweden, Sewage treatment plants
Identifiers
urn:nbn:se:umu:diva-10134 (URN)doi:10.1016/j.watres.2006.11.014 (DOI)17187841 (PubMedID)
Available from: 2007-04-11 Created: 2007-04-11 Last updated: 2011-01-11Bibliographically approved

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