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Determination of pharmaceuticals in sewage sludge by pressurized liquid extraction (PLE) coupled to liquid chromatography-tandem mass spectrometry (LC-MS/MS)

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Abstract

In this study, we aimed at optimizing a sensitive and reliable method for a simultaneous determination of 31 pharmaceuticals belonging to predominant therapeutic classes identified in different types of sewage sludge proceeding from conventional and advanced wastewater treatment. Freeze-dried sewage sludge was extracted by pressurized liquid extraction technique using accelerated solvent extractor Dionex 300. In order to minimize interferences with matrix components and to preconcentrate target analytes, solid phase extraction was introduced in the method as a clean-up step. The entire method was validated for linearity, precision, accuracy, and method detection limits (MDLs). The method turned out to be specific, sensitive, and reliable for the analysis of sludge of different composition, type, and retention time in the process. The developed sample preparation protocol and previously published method for LC-MS/MS analysis (Gros et al., Talanta 70:678–690, 2006) were successfully applied to monitor the target pharmaceuticals in different types of sewage sludge, i.e., primary sludge, secondary sludge, treated sludge, and sludge proceeding from pilot-scale membrane bioreactors (MBRs) operating in parallel to the conventional activated sludge treatment. Among the investigated pharmaceuticals, 20 were detected in the sludge proceeding from full-scale installations, whereas the MBR sludge concentrations were below MDLs for several compounds. The highest concentrations were recorded for treated and primary sludge. For example, the mean concentration of ibuprofen in the digested sludge was 299.3 ± 70.9 ng g−1 dw, whereas in the primary sludge, it was enriched up to 741.1 ng g−1 dw. Other pharmaceuticals detected at relatively high concentrations were diclofenac, erythromycin, glibenclamide, ketoprofen, ofloxacin, azithromycin (up to 380.7, 164.2, 190.7, 336.3, 454.7, 299.6 ng g−1 dw in the primary sludge, respectively), gemfibrozil, loratidine, and fluoxetine (up to 189.1, 189.7 and 174.1 ng g−1 dw in the treated sludge, respectively).

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Acknowledgments

The study was financially supported by the Spanish Ministerio de Educación y Ciencia, projects CEMAGUA (CGL2007-64551/HID) and CTM2007-30524-E/TECNO, and Spanish Ministerio de Medio Ambiente y Medio Rural y Marino through the project MMAMRM 010/PC08/3-04. J.R. gratefully acknowledges the I3P Program (Itinerario integrado de inserción profesional), co-financed by CSIC (Consejo Superior de Investigaciones Científicas) and European Social Funds, for a predoctoral grant. Waters (Milford, USA) is gratefully acknowledged for providing the SPE cartridges and Merck (Darmstadt, Germany) for providing the HPLC columns. The authors would like to thank to Mrs. Asuncion Navarro from IDAEA and Ms. Cristina Fàbregas Peret from WWTP Terrassa for their help and support.

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Authors and Affiliations

  1. Department of Environmental Chemistry, IDAEA-CSIC, c/Jordi Girona 18-26, 08034, Barcelona, Spain

    J. Radjenović, A. Jelić, M. Petrović & D. Barceló

  2. Institucio Catalana de Reserca i Estudis Avanzats (ICREA), 08010, Barcelona, Spain

    M. Petrović

  3. Institut Català de Recerca de l’Aigua (ICRA), Parc Científic i Tecnológic de la Universitat de Girona, Pic de Peguera, 15, 17003, Girona, Spain

    D. Barceló

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  1. J. Radjenović
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  2. A. Jelić
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  3. M. Petrović
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  4. D. Barceló
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Correspondence to M. Petrović.

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Radjenović, J., Jelić, A., Petrović, M. et al. Determination of pharmaceuticals in sewage sludge by pressurized liquid extraction (PLE) coupled to liquid chromatography-tandem mass spectrometry (LC-MS/MS). Anal Bioanal Chem 393, 1685–1695 (2009). https://doi.org/10.1007/s00216-009-2604-4

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  • DOI: https://doi.org/10.1007/s00216-009-2604-4

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