Abstract
The biodegradation of fluoxetine, mefenamic acid, and metoprolol using ammonium-nitrite-oxidizing consortium, nitrite-oxidizing consortium, and heterotrophic biomass was evaluated in batch tests applying different retention times. The ammonium-nitrite-oxidizing consortium presented the highest biodegradation percentages for mefenamic acid and metoprolol, of 85 and 64% respectively. This consortium was also capable to biodegrade 79% of fluoxetine. The heterotrophic consortium showed the highest ability to biodegrade fluoxetine reaching 85%, and it also had a high potential for biodegrading mefenamic acid and metoprolol, of 66 and 58% respectively. The nitrite-oxidizing consortium presented the lowest biodegradation of the three pharmaceuticals, of less than 48%. The determination of the selected pharmaceuticals in the dissolved phase and in the biomass indicated that biodegradation was the major removal mechanism of the three compounds. Based on the obtained results, the biodegradation kinetics was adjusted to pseudo-first-order for the three pharmaceuticals. The values of k biol for fluoxetine, mefenamic acid, and metoprolol determined with the three consortiums indicated that ammonium-nitrite-oxidizing and heterotrophic biomass allow a partial biodegradation of the compounds, while no substantial biodegradation can be expected using nitrite-oxidizing consortium. Metoprolol was the less biodegradable compound. The sorption of fluoxetine and mefenamic acid onto biomass had a significant contribution for their removal (6–14%). The lowest sorption coefficients were obtained for metoprolol indicating that the sorption onto biomass is poor (3–4%), and the contribution of this process to the global removal can be neglected.
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References
APHA (2012) Standard methods for the examination of water and wastewater. 22nd ed. American Public Health Association (APHA-AWWA-WEF), Washington, DC
Birkholz DA, Stilson SM, Elliot HS (2014) Analysis of emerging contaminants in drinking water—a review. Comprehensive Water Quality and Purification 2:212–229
Chen F, Ying G, Kong L, Wang L, Zhao J, Zhou L, Zhang L (2011) Distribution and accumulation of endocrine-disrupting chemicals and pharmaceuticals in wastewater irrigated soils in Hebei, China. Environ Pollut 159:1490–1498
Clara M, Kreuzinger N, Strenn B, Gans O, Kroiss H (2005) The solids retention time—a suitable design parameter to evaluate the capacity of wastewater treatment plants to remove micropollutants. Water Res 39:97–106
Daughton CG, Ternes TA (1999) Pharmaceutical and personal care products in the environment: agents of subtle change? Environ Health Perspect 107(Supplement 6):907–938
Dawas A, Gur-Reznik S, Lerman S, Sabbah I, Desoretz C (2014) Co-metabolic oxidation of pharmaceutical compounds by a nitrifying bacterial enrichment. Bioresour Technol 167:336–342
Deblonde T, Cossu-Leguille C, Hartemann P (2011) Emerging pollutants in wastewater: a review of the literature. International Journal of Hygiene and Environmental Healt 214:442–448
EPA (2002) Nitrification. Office of Water (4601 M), Washington DC
Escher BI, Baumgartner R, Koller M, Treyer K, Lienert J, McArdell CS (2011) Environmental toxicology and risk assessment of pharmaceuticals from hospital wastewater. Water Res 45:75–92
Falås P, Baillon-Dhumez A, Andersen HR, Ledin A, la Cour JJ (2012) Suspended biofilm carrier and activated sludge removal of acidic pharmaceuticals. Water Res 46:1167–1175
Falås P, Longrée P, Cour Jansen J, Siegrist H, Hollender J (2013) Micropollutant removal by attached and suspended growth in a hybrid biofilm-activated sludge process. Water Res 47:4498–4506
Fernandez-Fontaina E, Omil F, Lema JM, Carballa M (2012) Influence of nitrifying conditions on the biodegradation and sorption of emerging micropollutants. Water Res 46:5434–5444
Fernandez-Fontaina E, Carballa M, Omil F, Lema JM (2014) Modelling cometabolic biotransformation of organic micropollutants in nitrifying reactors. Water Res 65:371–383
Fernandez-Fontaina E, Gomes IB, Aga DS, Omil F, Lema JM, Carballa M (2016) Biotransformation of pharmaceuticals under nitrification, nitratation and heterotrophic conditions. Sci Total Environ 541:1439–1447
Ferrando-Climent L, Collado N, Buttiglieri G, Gros M, Rodriguez-Roda I, Rodriguez-Mozaz S, Barceló D (2012) Comprehensive study of ibuprofen and its metabolites in activated sludge batch experiments and aquatic environment. Sci Total Environ 438:404–413
Forrez I, Boon N, Verstraete W, Carballa M (2011) Biodegradation of micropollutants and prospects for water and wastewater biotreatment. Comprehensive Biotechnology 6:485–494
Gerardi MH (2002) Nitrification and denitrification in the activated sludge process. Environmental Protection. Willey Interscience, Nueva York
Grossberger A, Hadar Y, Borch T, Chefetz B (2014) Biodegradability of pharmaceutical compounds in agricultural soils irrigated with treated wastewater. Environ Pollut 185:168–177
Gulde R, Meier U, Schymanski EL, Kohler HE, Helbling DE, Derrer S, Rentsch D, Fenner K (2016) Systematic exploration of biotransformation reactions of amine containing micropollutants in activated sludge. Environ Sci Technol 50:2908–2920
Hata T, Kawai S, Okamura H, Nishida T (2010) Removal of diclofenac and mefenamic acid by the white rot fungus Phanerochaete sordida YK-624 and identification of their metabolites after fungal transformation. Biodegradation 21:681–689
Helbling DE, Johnson DR, Honti M, Fenner K (2012) Micropollutant biotransformation kinetics associate with WWTP process parameters and microbial community characteristics. Environ Sci Technol 46:10579–10588
Henze M, Harremoës P, Arvin E, Jansen J (2002) Wastewater treatment: biological and chemical processes, Third edn. Springer, Heidelberg
Hörsing M, Ledin A, Grabic R, Fick J, Tysklind M, Jansen J, Andersen HR (2011) Determination of sorption of seventy-five pharmaceuticals in sewage sludge. Water Res 45:4470–4482
Jones OAH, Voulvoulis N, Lester JN (2002) Aquatic environmental assessment of the top 25 English prescription pharmaceuticals. Water Res 36:5013–5022
Joss A, Keller E, Alder AC, Göbel A, McArdell CS, Ternes T, Siegrist H (2005) Removal of pharmaceuticals and fragrances in biological wastewater treatment. Water Res 39:3139–3152
Joss A, Zabczynski S, Göbel A, Hoffmann B, Löffer D, McArdell CS, Ternes TA, Thomsen A, Siegrist H (2006) Biological degradation of pharmaceuticals in municipal wastewater treatment: proposing a classification scheme. Water Res 40:1686–1696
Khunjar WO, Mackintosh SA, Skotnicka-Pitak J, Baik S, Aga DS, Love NG (2011) Elucidating the relative roles of ammonia oxidizing and heterotrophic bacteria during the biotransformation of 17α-ethinylestradiol and trimethoprim. Environ Sci Technol 45:3605–3612
Kibbey TCG, Paruchuri R, Sabatini DA, Chen L (2007) Adsorption of beta blockers to environmental surfaces. Environ Sci Technol 41:5349–5356
Kovalova L, Siegrist H, Singer H, Wittmer A, McArdell CS (2012) Hospital wastewater treatment by membrane bioreactor: performance and efficiency for organic micropollutant elimination. Environmental Science & Technology 46:1536–1545
Li J, Bishop PL (2004) Time course observations of nitrifying biofilm development using microelectrodes. J Environ Eng Sci 2:523–528
Luo Y, Guo W, Hao H, Duc Nghiem L, Ibney F, Zhang J, Liang S, Wang X (2014) A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment. Sci Total Environ 473-474:619–641
Maeng SK, Choi BB, Lee KT, Song KG (2013) Influences of solid retention time, nitrification and microbial activity on the attenuation of pharmaceuticals and estrogens in membrane bioreactors. Water Res 47:3151–3162
Majewsky M, Gallé T, Yargeau V, Fischer K (2011) Active heterotrophic biomass and sludge retention time (SRT) as determining factors for biodegradation kinetics of pharmaceuticals in activated sludge. Bioresour Technol 102:7415–7421
Mansour F, Al-Hindi M, Saad W, Salam D (2016) Environmental risk analysis and prioritization of pharmaceuticals in a developing world context. Sci Total Environ 557-558:31–43
Martínez MJ, Gomez MJ, Herrera S, Hernando MD, Agüera A, Fernández AR (2012) Occurrence and persistence of organic emerging contaminants and priority pollutants in five sewage treatment plants of Spain: two years pilot survey monitoring. Environ Pollut 164:267–273
Miège C, Choubert JM, Ribeiro L, Eusèbe M, Coquery M (2009) Fate of pharmaceuticals and personal care products in wastewater treatment plants—conception of a database and first results. Environ Pollut 157:1721–1726
Monteiro SC, Boxall ABA (2010) Occurrence and fate of human pharmaceuticals in the environment. Rev Environ Contam Toxicol 202:53–154
Nogueira R, Melo LF (2006) Competition between Nitrospira spp. and Nitrobacter spp. in nitrite-oxidizing bioreactors. Biotechnol Bioeng 95:169–175
Poseidon, detailed report related to the overall duration (2004) Assessment of technologies for the removal of pharmaceuticals and personal care products in sewage, and drinking water facilities to improve the indirect potable water reuse
Quintana JB, Weiss S, Reemtsna T (2005) Pathways and metabolites of microbial degradation of selected acidic pharmaceutical and their occurrence in municipal wastewater treated by a membrane bioreactor. Water Res 39:2654–2664
Radjenovic J, Petrovic M, Barcelo D (2009) Fate and distribution of pharmaceuticals in wastewater and sewage sludge of the conventional activated sludge (CAS) and advanced membrane bioreactor (MBR) treatment. Water Res 43:831–841
Ramil M, El Aref T, Kink G, Scheurer M, Ternes TA (2010) Fate of beta blockers in aquatic-sediment systems: sorption and biotransformation. Environmental Science & Technology 44:962–970
Rattier M, Reungoat J, Keller J, Gernjak W (2014) Removal of micropollutants during tertiary wastewater treatment by biofiltration: role of nitrifiers and removal mechanisms. Water Res 54:89–99
Rieger PG, Meier HM, Gerle M, Vogt U, Groth T, Knackmuss HJ (2002) Xenobiotics in the environment: present and future strategies to obviate the problem of biological persistence. J Biotechnol 94(1):101–123
Rogers HR (1996) Sources, behaviour and fate of organic contaminants during sewage treatment and in sewage sludges. Sci Total Environ 185:3–26
Roos V, Gunnarsson L, Fick J, Larsson DGJ, Rudén C (2012) Prioritising pharmaceuticals for environmental risk assessment: towards adequate and feasible first-tier selection. Sci Total Environ 421-422:102–110
Rosal R, Rodríguez A, Perdigón-Melón JA, Petre A, García-Calvo E, Gómez J, Agüera A, Fernández-Alba AR (2010) Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation. Water Res 44:578–588
Rubirola A, Llorca M, Rodriguez-Mozaz S, Casas N, Rodriguez-Roda I, Barceló D, Buttiglieri G (2014) Characterization of metoprolol biodegradation and its transformation products generated in activated sludge batch experiments and in full scale WWTPs. Water Res 63:21–32
Sathyamoorthy S, Ramsburg CA (2013) Assessment of quantitative structural property relationships for prediction of pharmaceutical sorption during biological wastewater treatment. Chemosphere 92:639–646
Scheurer M, Ramil M, Metcalfe CD, Groh S, Ternes TA (2010) The challenge of analyzing beta-blocker drugs in sludge and wastewater. Anal Bioanal Chem 396:845–856
Spieck E, Bock E (2005) The lithoautotrophic nitrite-oxidizing bacteria. Bergey’s Manual® of Systematic Bacteriology 2:149–153
Spieck E, Lipski A (2011) Cultivation, growth physiology, and chemotaxonomy of nitrite-oxidizing bacteria. Methods Enzymol 486:109–130
Stuart M, Lapworth D, Crene E, Hart A (2012) Review of risk from potential emerging contaminants in UK groundwater. Sci Total Environ 416:1–21
Suarez S, Lema JM, Omil F (2010) Removal of pharmaceutical and personal care products (PPCPs) under nitrifying and denitrifying conditions. Water Res 44:3214–3224
Sui Q, Huang J, Deng S, Yu G, Fan Q (2010) Occurrence and removal of pharmaceuticals, caffeine and DEET in wastewater treatment plants of Beijing, China. Water Res 44:417–426
Tadkaew N, Hai FI, McDonakd JA, Khan SJ, Nghiem LD (2011) Removal of trace organics by MBR treatment: the role of molecular properties. Water Res 45:2439–2451
Tauxe-Wuersch A, De Alencastro LF, Grandjean D, Tarradellas J (2005) Occurrence of several acidic drugs in sewage treatment plants in Switzerland and risk assessment. Water Res 39:1761–1772
Ternes T (1998) Occurrence of drugs in German sewage treatment plants and rivers. Water Res 32:3245–3260
Ternes T, Joss A (2006) Human pharmaceuticals, hormones and fragrances: the challenge of micropollutants in urban water management. IWA Publishing. UK
Ternes TA, Janex-Habibi MJ, Knacker T, Kreuzinger N, Siegrist H (2004) Assessment of technologies for the removal of pharmaceuticals and personal care products in sewage and drinking water facilities to improve the indirect potable water reuse. Project acronym. POSEIDON. Contract No. EVKI-CT-2000-00047
Torres AX, Buitrón G (2012) Biodegradation of nonylphenols using nitrifying sludge, 4-chlorophenol-adapted consortia and activated sludge in liquid and solid phases. Environ Technol 33:1727–1737
Tran NH, Urase T, Kusakabe O (2009) The characteristics of enriched nitrifier culture in the degradation of selected pharmaceutically active compounds. J Hazard Mater 171:1051–1057
Tran NH, Urase T, Ngo HH, Hu J, Ong SL (2013) Insight into metabolic and cometabolic activities of autotrophic and heterotrophic microorganisms in the biodegradation of emerging trace organic contaminants. Bioresour Technol 146:721–731
Trenholm RA, Vanderford BJ, Holady JC, Rexing DJ, Snyder SA (2006) Broad range analysis of endocrine disruptors and pharmaceuticals using gas chromatography and liquid chromatography tandem mass spectrometry. Chemosphere 65:1990–1998
Urase T, Kikuta T (2005) Separate estimation of adsorption and degradation of pharmaceutical substances and estrogens in the activated sludge process. Water Res 39:1289–1300
Verlicchi P, Aukidy MA, Zambello E (2012) Occurrence of pharmaceutical compounds in urban wastewater: removal, mass load and environmental risk after a secondary treatment—a review. Sci Total Environ 429:123–155
Vieno N, Tuhkanen T, Kronberg L (2007) Elimination of pharmaceuticals in sewage treatment plants in Finland. Water Res 41:1001–1012
Vulliet E, Cren-Olivé C (2011) Screening of pharmaceuticals and hormones at the regional scale, in surface and groundwaters intended to human consumption. Environ Pollut 159:2929–2934
Wick A, Fink G, Joss A, Siegrist H, Ternes TA (2009) Fate of beta blockers and psycho-active drugs in conventional wastewater treatment. Water Res 43:1060–1074
Yi T, Harper WF (2007) The link between nitrification and biotransformation of 17α-ethinylestradiol. Environ Sci Technol 41:4311–4316
Zhao J, Li Y, Zhang C, Zeng Q, Zhou Q (2008) Sorption and degradation of bisfenol A by aerobic activated sludge. J Hazard Mater 155:305–311
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Velázquez, Y.F., Nacheva, P.M. Biodegradability of fluoxetine, mefenamic acid, and metoprolol using different microbial consortiums. Environ Sci Pollut Res 24, 6779–6793 (2017). https://doi.org/10.1007/s11356-017-8413-y
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DOI: https://doi.org/10.1007/s11356-017-8413-y