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Determination of cardiovascular drugs in sewage sludge by matrix solid-phase dispersion and ultra-performance liquid chromatography tandem mass spectrometry

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Abstract

The current study presents a single step sample preparation procedure for the simultaneous determination of five antihypertensive (propranolol, losartan, irbesartan, telmisartan, and valsartan), three antiarrhythmic drugs (flecainide, dronedarone, and amiodarone), and one of their metabolites (N-desethylamiodarone) in sludge from municipal sewage treatment plants (STPs). Matrix solid-phase dispersion (MSPD) and ultra-performance liquid chromatography (UPLC) with tandem mass spectrometry (MS/MS) detection were selected as sample preparation and determination techniques, respectively. Under optimal conditions, MSPD extractions were carried out with freeze-dried samples (0.5 g) dispersed on 2 g of C18. Exhaustive extraction of target compounds was achieved with 10 mL of a methanol/acetonitrile/formic acid (30:69:1) solution. The obtained extract was ready for UPLC-MS/MS analysis without any further treatment, except filtration. The overall recoveries of the method (calculated against solvent-based standards) varied from 82 to 124%, with standard deviations in the range from 2 to 16%. Thus, the method was free of matrix effects during electrospray ionization. The achieved limits of quantification stayed between 2 and 10 ng g−1, and the linear response range extended to 5000 ng g−1. The occurrence of target compounds was investigated in sludge from 14 different STPs. High detection frequencies were observed for all compounds, with average concentrations above 100 ng g−1 for six cardiovascular drugs.

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References

  1. Montero Corominas D, García del Pozo J, De Abajo Iglesias FJ. Utilización de antihipertensivos en España (1992-2006). 2009. https://www.aemps.gob.es/medicamentosUsoHumano/observatorio/docs/antihipertensivos.pdf. Accessed 2 May 2018.

  2. Ortiz de García S, Pinto Pinto G, García Encina P, Irusta Mata R. Consumption and occurrence of pharmaceutical and personal care products in the aquatic environment in Spain. Sci Total Environ. 2013;444:451–65.

    Article  CAS  PubMed  Google Scholar 

  3. Stankiewicz A, Giebułtowicz J, Stankiewicz U, Wroczyński P, Nałecz-Jawecki G. Determination of selected cardiovascular active compounds in environmental aquatic samples—methods and results, a review of global publications from the last 10 years. Chemosphere. 2015;138:642–56.

    Article  CAS  PubMed  Google Scholar 

  4. Bueno MJM, Gomez MJ, Herrera S, Hernando MD, Agüera A, Fernández-Alba AR. Occurrence and persistence of organic emerging contaminants and priority pollutants in five sewage treatment plants of Spain: two years pilot survey monitoring. Environ Pollut. 2012;164:267–73.

    Article  CAS  PubMed  Google Scholar 

  5. Giebułtowicz J, Nałecz-Jawecki G. Occurrence of cardiovascular drugs in the sewage-impacted Vistula River and in tap water in the Warsaw region (Poland). Environ Sci Pollut Res. 2016;23:24337–49.

    Article  CAS  Google Scholar 

  6. Bayer A, Asner R, Schüssle W, Kopf W, Weiß K, Seng M, et al. Behavior of sartans (antihypertensive drugs) in wastewater treatment plants, their occurrence and risk for the aquatic environment. Environ Sci Pollut Res. 2014;21:10830–9.

    Article  CAS  Google Scholar 

  7. Gurke R, Robler M, Marx C, Diamond S, Schubert S, Oertel R, et al. Occurrence and removal of frequently prescribed pharmaceuticals and corresponding metabolites in wastewater of a sewage treatment plant. Sci Total Environ. 2015;532:762–70.

    Article  CAS  PubMed  Google Scholar 

  8. Huerta-Fontela M, Galcerán MT, Ventura F. Occurrence and removal of pharmaceuticals and hormones through drinking water treatment. Water Res. 2010;45:1432–42.

    Article  CAS  PubMed  Google Scholar 

  9. Godoy AA, Kummrow F, Pamplin PAZ. Occurrence, ecotoxicological effects and risk assessment of antihypertensive pharmaceutical residues in the aquatic environment-a review. Chemosphere. 2015;138:281–91.

    Article  CAS  PubMed  Google Scholar 

  10. Grabic R, Fick J, Lindberg RH, Fedorova G, Tysklind M. Multi-residue method for trace level determination of pharmaceuticals in environmental samples using liquid chromatography coupled to triple quadrupole mass spectrometry. Talanta. 2012;100:183–95.

    Article  CAS  PubMed  Google Scholar 

  11. Hörsing M, Ledin A, Grabic R, Fick J, Tysklind M, Jansen JC, et al. Determination of sorption of seventy-five pharmaceuticals in sewage sludge. Water Res. 2011;45:4470–82.

    Article  CAS  PubMed  Google Scholar 

  12. Berthod L, Whitley DC, Roberts G, Sharpe A, Greenwood R, Mills GA. Quantitative structure-property relationships for predicting sorption of pharmaceuticals to sewage sludge during waste water treatment processes. Sci Total Environ. 2017;579:1512–20.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  13. Lajeunesse A, Smyth SA, Barclay K, Sauvé S, Gagnon C. Distribution of antidepressant residues in wastewater and biosolids following different treatment processes by municipal wastewater treatment plants in Canada. Water Res. 2012;46:5600–12.

    Article  CAS  PubMed  Google Scholar 

  14. González-Mariño I, Rodríguez I, Quintana JB, Cela R. Matrix solid-phase dispersion followed by gas chromatography-mass spectrometry for the determination of triclosan and methyl triclosan in sludge and sediments. Anal Bioanal Chem. 2010;398:2289–97.

    Article  CAS  PubMed  Google Scholar 

  15. Ivanová L, Mackulak T, Grabic R, Golovko O, Koba O, Stanová AV, et al. Pharmaceuticals and illicit drugs—a new threat to the application of sewabe sludge in agriculture. Sci Total Environ. 2018;634:606–15.

    Article  CAS  PubMed  Google Scholar 

  16. Boix C, Ibáñez M, Fabregat-Safont D, Morales E, Pastor L, Sancho JV, et al. Behaviour of emerging contaminants in sewage sludge after anaerobic digestion. Chemosphere. 2016;163:296–304.

    Article  CAS  PubMed  Google Scholar 

  17. Kuhn J, Götting C, Kleesiek K. Simultaneous measurement of amiodarone and desethylamiodarone in human plasma and serum by stable isotope dilution liquid chromatography-tandem mass spectrometry assay. J Pharm Biomed Anal. 2010;51:210–6.

    Article  CAS  PubMed  Google Scholar 

  18. Montes R, Rodríguez I, Casado J, López-Sabater MC, Cela R. Determination of the cardiac drug amiodarone and its N-desethyl metabolite in sludge samples. J Chromatogr A. 2015;1394:62–70.

    Article  CAS  PubMed  Google Scholar 

  19. Celano R, Rodríguez I, Cela R, Rastrelli L, Piccinelli AL. Liquid chromatography quadrupole time-of-flight mass spectrometry quantification and screening of organophosphate compounds in sludge. Talanta. 2014;118:312–20.

    Article  CAS  PubMed  Google Scholar 

  20. Li M, Sun Q, Li Y, Lv M, Lin L, Wu Y, et al. Simultaneous analysis of 45 pharmaceuticals and personal care products in sludge by matrix solid-phase dispersion and liquid chromatography tandem mass spectrometry. Anal Bioanal Chem. 2016;408:4953–64.

    Article  CAS  PubMed  Google Scholar 

  21. Wasik A, Kot-Wasik A, Namiesnik J. New trends in sample preparation techniques for the analysis of the residues of pharmaceuticals in environmental samples. Curr Anal Chem. 2016;12:280–302.

    Article  CAS  Google Scholar 

  22. Baker SA. Matrix solid phase dispersion. J Biochem Biophys Methods. 2007;70:151–62.

    Article  CAS  Google Scholar 

  23. Capriotti AL, Cavaliere C, Foglia P, Samperi R, Stampachiacchiere S, Ventura S, et al. Recent advances and developments in matrix solid-phase dispersion. TrAC Trends Anal Chem. 2015;71:186–93.

    Article  CAS  Google Scholar 

  24. Kasprzyk-Hordern B, Dinsdale RM, Guwy AJ. The effect of signal suppression and mobile phase composition on the simultaneous analysis of multiple classes of acidic/neutral pharmaceuticals and personal care products in surface water by solid-phase extraction and ultra performance liquid chromatography. Talanta. 2008;74:1299–312.

    Article  CAS  PubMed  Google Scholar 

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Acknowledgements

This study has been financially supported by Xunta de Galicia and the Spanish Government (projects GRC-ED431C 2017/36 and CTQ2015-68660-P). I.C. acknowledges a postdoctoral grant to Xunta de Galicia. We also thank Indrops laboratories for providing most of the sludge samples used in this research.

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Authors and Affiliations

  1. Department of Analytical Chemistry, Nutrition and Food Sciences. Institute for Research and Food Analysis (IIAA), Universidade de Santiago de Compostela, 15782, Santiago de Compostela, Spain

    Gabriela Castro, Inmaculada Carpinteiro, Isaac Rodríguez & Rafael Cela

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  1. Gabriela Castro
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  2. Inmaculada Carpinteiro
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  3. Isaac Rodríguez
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  4. Rafael Cela
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Correspondence to Inmaculada Carpinteiro or Isaac Rodríguez.

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Castro, G., Carpinteiro, I., Rodríguez, I. et al. Determination of cardiovascular drugs in sewage sludge by matrix solid-phase dispersion and ultra-performance liquid chromatography tandem mass spectrometry. Anal Bioanal Chem 410, 6807–6817 (2018). https://doi.org/10.1007/s00216-018-1268-3

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  • DOI: https://doi.org/10.1007/s00216-018-1268-3

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