This study investigated the biodegradation potential of five pharmaceutical micropollutants, acetaminophen, ibuprofen, carbamazepine, sulfamethoxazole and erythromycin, under aerobic conditions. First, theoretical aerobic biodegradation potential of these pharmaceuticals was investigated using the BIOWIN models of the Estimation Programs Interface Suite. The results were then compared with data from activated sludge experiments. The main novelty of this work was that it showed why deviations occurred between theoretical and experimental results. For example, erythromycin was found as the least biodegradable compound in BIOWIN models. On the other hand, carbamazepine proved to be the least biodegradable under experimental conditions. To explain such deviations, biodegradation mechanisms, biodegradation rates and biosorption of pharmaceuticals were taken into consideration. One reason for deviation is that the predictive BIOWIN models consider the single pharmaceutical and relate biodegradability to molecular structure alone. These two points often lead to underestimation of biodegradation. On the other hand, the present study revealed that biodegradation of pharmaceuticals can be enhanced under the microbial and operating conditions of an activated sludge system. Pharmaceuticals can be used as secondary substrates if biodegradable substances are present in an activated sludge. More importantly, they can often be used as cometabolites in the presence of nitrifiers. Also, compared to predicted results, a poorer sorption is observed in activated sludge, indicating that these pharmaceuticals would degrade in liquid phase. Databases/predictive tools are very helpful to have an initial idea about biodegradability. But, in estimation of real biodegradability, there is a need to consider the factors highlighted in this work.
This is a preview of subscription content, access via your institution.
Buy single article
Instant access to the full article PDF.
Tax calculation will be finalised during checkout.
Subscribe to journal
Immediate online access to all issues from 2019. Subscription will auto renew annually.
Tax calculation will be finalised during checkout.
Abegglen C, Joss A, McArdell CS, Fink G, Schlüsener MP, Ternes TA, Siegrist H (2009) The fate of selected micropollutants in a single-house MBR. Water Res 43:2036–2046. https://doi.org/10.1016/j.watres.2009.02.005
Aissaoui S, Ouled-Haddar H, Sifour M, Beggah C, Benhamada F (2017) Biological removal of the mixed pharmaceuticals: diclofenac, ibuprofen, and sulfamethoxazole using a bacterial consortium. Iran J Biotechnol 15:135
Alexy R, Kümpel T, Kümmerer K (2004) Assessment of degradation of 18 antibiotics in the closed bottle test. Chemosphere 57:505–512. https://doi.org/10.1016/j.chemosphere.2004.06.024
Almeida B, Kjeldal H, Lolas I, Knudsen AD, Carvalho G, Nielsen KL, Barreto Crespo MT, Stensballe A, Nielsen JL (2013) Quantitative proteomic analysis of ibuprofen-degrading Patulibacter sp. strain I11. Biodegradation 24:615–630. https://doi.org/10.1007/s10532-012-9610-5
Alvarino T, Suarez S, Lema JM, Omil F (2014) Understanding the removal mechanisms of PPCPs and the influence of main technological parameters in anaerobic UASB and aerobic CAS reactors. J Hazard Mater 278:506–513. https://doi.org/10.1016/j.jhazmat.2014.06.031
Alvarino T, Nastold P, Suarez S, Omil F, Corvini PFX, Bouju H (2016) Role of biotransformation, sorption and mineralization of 14C-labelled sulfamethoxazole under different redox conditions. Sci Tot Environ 542:706–715. https://doi.org/10.1016/j.scitotenv.2015.10.140
Beelen ESE (2007) Municipal Waste Water Treatment Plant (WWTP) effluents: a concise overview of the occurrence of organic substances. Association of River Waterworks-RIWA
Boethling RS, Costanza J (2010) Domain of EPI suite biotransformation models. SAR QSAR Environ Res 21:415–443. https://doi.org/10.1080/1062936X.2010.501816
Boethling RS, Sommer E, DiFiore D (2007) Designing small molecules for biodegradability. Chem Rev 107:2207–2227. https://doi.org/10.1021/cr050952t
Çeçen F, Tezel U, Kocamemi BA (2017) Experimental assessment of the inhibitory effect and biodegradation of hazardous pollutants. In: Çeçen F, Tezel U (eds) Hazardous pollutants in biological treatment systems: Fundamentals and a guide to experimental research. IWA Publishing, London, pp 183–237. https://doi.org/10.2166/9781780407715_183
Chen Y, Rosazza JP (1994) Microbial transformation of ibuprofen by a Nocardia species. Appl Environ Microbiol 60:1292–1296
Clara M, Kreuzinger N, Strenn B, Gans O, Kroiss H (2005a) The solids retention time—a suitable design parameter to evaluate the capacity of wastewater treatment plants to remove micropollutants. Water Res 39:97–106. https://doi.org/10.1016/j.watres.2004.08.036
Clara M, Strenn B, Gans O, Martinez E, Kreuzinger N, Kroiss H (2005b) Removal of selected pharmaceuticals, fragrances and endocrine disrupting compounds in a membrane bioreactor and conventional wastewater treatment plants. Water Res 39:4797–4807. https://doi.org/10.1016/j.watres.2005.09.015
Coates A, Hu Y, Bax R, Page C (2002) The future challenges facing the development of new antimicrobial drugs. Nat Rev Drug Discovery 1:895–910
De Gusseme B, Vanhaecke L, Verstraete W, Boon N (2011) Degradation of acetaminophen by Delftia tsuruhatensis and Pseudomonas aeruginosa in a membrane bioreactor. Water Res 45:1829–1837. https://doi.org/10.1016/j.watres.2010.11.040
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. https://doi.org/10.1016/j.watres.2012.07.037
Fernandez-Fontaina E, Pinho I, Carballa M, Omil F, Lema JM (2013) Biodegradation kinetic constants and sorption coefficients of micropollutants in membrane bioreactors. Biodegradation 24:165–177. https://doi.org/10.1007/s10532-012-9568-3
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. https://doi.org/10.1016/j.scitotenv.2015.10.010
Gauthier H, Yargeau V, Cooper DG (2010) Biodegradation of pharmaceuticals by Rhodococcus rhodochrous and Aspergillus niger by co-metabolism. Sci Total Environ 408:1701–1706. https://doi.org/10.1016/j.scitotenv.2009.12.012
Göbel A, Thomsen A, McArdell CS, Joss A, Giger W (2005) Occurrence and sorption behavior of sulfonamides, macrolides, and trimethoprim in activated sludge treatment. Environ Sci Technol 39:3981–3989. https://doi.org/10.1021/es048550a
Göktas RK, MacLeod M (2017) Hazardous pollutants in the water environment. In: Çeçen F, Tezel U (eds) Hazardous pollutants in biological treatment systems: Fundamentals and a guide to experimental research. IWA Publishing, London, pp 17–58. https://doi.org/10.2166/9781780407715_017
Gül G (2016) Antibiotic resistant Pseudomonas sp. BIOMIG1 protects susceptible bacteria from disinfectants. MSc Thesis, Institute of Environmental Sciences, Boğaziçi University, Istanbul, Turkey
Hasan HA, Abdullah SRS, Al-Attabi AWN, Nash DAH, Anuar N, Rahman NA, Titah HS (2016) Removal of ibuprofen, ketoprofen, COD and nitrogen compounds from pharmaceutical wastewater using aerobic suspension-sequencing batch reactor (ASSBR). Sep Purif Technol 157:215–221. https://doi.org/10.1016/j.seppur.2015.11.017
Hörsing M, Ledin A, Grabic R, Fick J, Tysklind M, la Cour Jansen J, Andersen HR (2011) Determination of sorption of seventy-five pharmaceuticals in sewage sludge. Water Res 45:4470–4482. https://doi.org/10.1016/j.watres.2011.05.033
Hyland KC, Dickenson ER, Drewes JE, Higgins CP (2012) Sorption of ionized and neutral emerging trace organic compounds onto activated sludge from different wastewater treatment configurations. Water Res 46:1958–1968. https://doi.org/10.1016/j.watres.2012.01.012
Jones OAH, Voulvoulis N, Lester JN (2002) Aquatic environmental assessment of the top 25 English prescription pharmaceuticals. Water Res 36:5013–5022. https://doi.org/10.1016/S0043-1354(02)00227-0
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. https://doi.org/10.1016/j.watres.2005.05.031
Joss A, Zabczynski S, Göbel A, Hoffmann B, Löffler 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. https://doi.org/10.1016/j.watres.2006.02.014
Kang AJ, Brown AK, Wong CS, Yuan Q (2018) Removal of antibiotic sulfamethoxazole by anoxic/anaerobic/oxic granular and suspended activated sludge processes. Biores Technol 251:151–157. https://doi.org/10.1016/j.biortech.2017.12.021
Kassotaki E, Buttiglieri G, Ferrando-Climent L, Rodriguez-Roda I, Pijuan M (2016) Enhanced sulfamethoxazole degradation through ammonia oxidizing bacteria co-metabolism and fate of transformation products. Water Res 94:111–119. https://doi.org/10.1016/j.watres.2016.02.022
Khan NA, Khan SU, Ahmed S, Farooqi IH, Yousefi M, Mohammadi AA, Changani F (2019) Recent trends in disposal and treatment technologies of emerging-pollutants-A critical review. TrAC Trends Anal Chem 122:115744. https://doi.org/10.1016/j.trac.2019.115744
Kim S, Chen J, Cheng T, Gindulyte A, He J, He S, Li Q, Shoemaker BA, Thiessen PA, Yu B, Zaslavsky L, Zhang J, Bolton EE (2019) PubChem 2019 update: improved access to chemical data. Nucleic Acids Res 8(47):D1102–1109. https://doi.org/10.1093/nar/gky1033[PubMed PMID: 30371825]
Madikizela LM, Chimuka L (2017) Occurrence of naproxen, ibuprofen, and diclofenac residues in wastewater and river water of KwaZulu-Natal Province in South Africa. Environ Monit Assess 189:348
Marchlewicz A, Guzik U, Wojcieszyńska D (2017) Dynamics of ibuprofen biodegradation by Bacillus sp. B1 (2015b). Archives of Environmental Protection 43:60–64. https://doi.org/10.1515/aep-2017-0020
Marco-Urrea E, Perez-Trujillo M, Vicent T, Caminal G (2009) Ability of white-rot fungi to remove selected pharmaceuticals and identification of degradation products of ibuprofen by Trametes versicolor. Chemosphere 74:765–772. https://doi.org/10.1016/j.chemosphere.2008.10.040
Müller E, Schüssler W, Horn H, Lemmer H (2013) Aerobic biodegradation of the sulfonamide antibiotic sulfamethoxazole by activated sludge applied as co-substrate and sole carbon and nitrogen source. Chemosphere 92:969–978. https://doi.org/10.1016/j.chemosphere.2013.02.070
Naghdi M, Taheran M, Brar SK, Kermanshahi-pour A, Verma M, Surampalli RY (2018) Biotransformation of carbamazepine by laccase-mediator system: kinetics, by-products and toxicity assessment. Process Biochem 67:147–154. https://doi.org/10.1016/j.procbio.2018.02.009
Nendza, M (2014) Environmental quality standard erythromycin, Umweltbundesamt (UBA). https://webetox.uba.de/webETOX/public/basics/literatur/download.do;jsessionid=5ABC79729770788A08390BD09CBB997C?id=33. Accessed 19 January 2020
Pavan M, Worth AP (2008) Review of estimation models for biodegradation. QSAR Comb Sci 27:32–40. https://doi.org/10.1002/qsar.200710117
Peng L, Kassotaki E, Liu Y, Sun J, Dai X, Pijuan M, Rodriguez-Roda I, Buttiglier G, Ni BJ (2017) Modelling cometabolic biotransformation of sulfamethoxazole by an enriched ammonia oxidizing bacteria culture. Chem Eng Sci 173:465–473. https://doi.org/10.1016/j.ces.2017.08.015
Plosz BG, Langford KH, Thomas KV (2012) An activated sludge modeling framework for xenobiotic trace chemicals (ASM-X): assessment of diclofenac and carbamazepine. Biotechnol Bioeng 109:2757–2769. https://doi.org/10.1002/bit.24553
Pomies M, Choubert JM, Wisniewski C, Miège C, Budzinski H, Coquery M (2015) Lab-scale experimental strategy for determining micropollutant partition coefficient and biodegradation constants in activated sludge. Environ Sci Pollut Res 22:4383–4395. https://doi.org/10.1007/s11356-014-3646-5
Quintana JB, Weiss S, Reemtsma 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. https://doi.org/10.1016/j.watres.2005.04.068
Rittmann BE, McCarty PL (2001) Stoichiometry and bacterial energetics. Principles and Applications, Environmental Biotechnology, pp 126–164
Rossmassler K, Kim S, Broeckling CD, Galloway S, Prenni J, Susan K (2019) Impact of primary carbon sources on microbiome shaping and biotransformation of pharmaceuticals and personal care products. Biodegradation 30:127–145. https://doi.org/10.1007/s10532-019-09871-0
Rücker C, Kümmerer K (2012) Modeling and predicting aquatic aerobic biodegradation–a review from a user’s perspective. Green Chem 14:875–887. https://doi.org/10.1039/C2GC16267A
Smook TM, Zho H, Zytner RG (2008) Removal of ibuprofen from wastewater: comparing biodegradation in conventional, membrane bioreactor, and biological nutrient removal treatment systems. Water Sci Technol 57:1–8. https://doi.org/10.2166/wst.2008.658
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. https://doi.org/10.1016/j.watres.2010.02.040
Svahn O, Bjorklund E (2019) Extraction efficiency of a commercial espresso machine compared to a stainless-steel column pressurized hot water extraction (PHWE) system for the determination of 23 pharmaceuticals, antibiotics and hormones in sewage sludge. Appl Sci 9:1509. https://doi.org/10.3390/app9071509
Ternes TA, Herrmann N, Bonerz M, Knacker T, Siegrist H, Joss A (2004a) A rapid method to measure the solid–water distribution coefficient (Kd) for pharmaceuticals and musk fragrances in sewage sludge. Water Res 38:4075–4084. https://doi.org/10.1016/j.watres.2004.07.015
Ternes T, Janex-Habibi ML, Knacker T, Kreuzinger N, Siegrist H (2004b) 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. Contract No. EVK1-CT-2000-00047
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. https://doi.org/10.1016/j.jhazmat.2009.06.114
Tunkel J, Howard PH, Boethling RS, Stiteler W, Loonen H (2000) Predicting ready biodegradability in the Japanese Ministry of International Trade and Industry test. Environ Toxicol Chem 19:2478–2485. https://doi.org/10.1002/etc.5620191013
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. https://doi.org/10.1016/j.watres.2005.01.015
US EPA (2012) Estimation Programs Interface Suite™ for Microsoft® Windows, v 4.11. United States Environmental Protection Agency, Washington, DC, USA
Verlicchi P, Al Aukidy M, Zambello E (2012) Occurrence of pharmaceutical compounds in urban wastewater: removal, mass load and environmental risk after a secondary treatment—a review. Sci Tot Environ 429:123–155. https://doi.org/10.1016/j.scitotenv.2012.04.028
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. https://doi.org/10.1016/j.watres.2008.11.031
Wu S, Zhang L, Chen J (2012) Paracetamol in the environment and its degradation by microorganisms. Appl Microbiol Biotechnol 96:875–884. https://doi.org/10.1007/s00253-012-4414-4
This work was supported by the Bogazici University Research Fund (BAP Grant 13000).
Conflict of interest
No conflicts are present.
Editorial responsibility: Samareh Mirkia.
About this article
Cite this article
Çeçen, F., Gül, G. Biodegradation of five pharmaceuticals: estimation by predictive models and comparison with activated sludge data. Int. J. Environ. Sci. Technol. 18, 327–340 (2021). https://doi.org/10.1007/s13762-020-02820-y
- Activated sludge