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Screening of human antibiotic substances and determination of weekly mass flows in five sewage treatment plants in Sweden
Umeå University, Faculty of Science and Technology, Chemistry.
Umeå University, Faculty of Science and Technology, Chemistry.
Umeå University, Faculty of Science and Technology, Chemistry.
Umeå University, Faculty of Science and Technology, Chemistry.
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2005 (English)In: Environmental Science and Technology, ISSN 0013-936X, 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.

Place, publisher, year, edition, pages
2005. Vol. 39, no 10, 3421-3429 p.
URN: urn:nbn:se:umu:diva-14358DOI: 10.1021/es048143zOAI: diva2:154029
Available from: 2007-08-17 Created: 2007-08-17Bibliographically 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.
antibiotics, environment, sewage treatment plants, antibiotika, miljö, avloppsreningsverk
National Category
Environmental Sciences
urn:nbn:se:umu:diva-745 (URN)91-7264-045-6 (ISBN)
Public defence
2006-04-28, KB3B1, KBC-huset, Umeå, 13:00 (English)
Available from: 2006-04-07 Created: 2006-04-07 Last updated: 2009-06-09Bibliographically approved

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Lindberg, RichardTysklind, MatsAndersson, Barbro
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