Abstract
The global consumption and production of pharmaceuticals is increasing concomitantly with concern regarding their environmental fate and effects. Active pharmaceutical ingredients are mainly released into the aquatic environment through wastewater effluent discharge. Once in the environment, pharmaceuticals can undergo processes of natural attenuation, i.e. dilution, sorption, transformation, depending on physico-chemical properties of the compound, such as water solubility, lipophilicity, vapour pressure, and environmental conditions, such as pH, temperature and ionic strength. A major natural attenuation process is the sorption on dissolved organic matter, colloids, suspended solids and sediments, which in turn control pharmaceuticals distribution, residence time and persistence in aquatic systems. Here we review studies of sorption capacity of natural sorbents to pharmaceuticals. These report on the importance of several environmental and sorbent-specific properties, such as the composition, quality, and amount of the sorbent, and the environmental pH, which determines the speciation of both the sorbent and compound. The importance of accounting for distribution processes on freshwater sorbents for any determination of environmental concentrations of pharmaceuticals is apparent, while the reliability of surrogate standards for measuring dissolved organic matter (DOM) distribution is evaluated in the context of the need for robust environmental risk assessment protocols.
Similar content being viewed by others
References
Ågerstrand M, Berg C, Björlenius B et al (2015) Improving environmental risk assessment of human pharmaceuticals. Environ Sci Technol 49:5336–5345. https://doi.org/10.1021/acs.est.5b00302
Agunbiade FO, Moodley B (2015) Occurrence and distribution pattern of acidic pharmaceuticals in surface water, wastewater and sediment of the Msunduzi River, Kwazulu-Natal, South Africa. Environ Toxicol Chem. https://doi.org/10.1002/etc.3144
Al-Khazrajy OSA, Boxall ABA (2016) Impacts of compound properties and sediment characteristics on the sorption behaviour of pharmaceuticals in aquatic systems. J Hazard Mater. https://doi.org/10.1016/j.jhazmat.2016.05.065
Arnold KE, Brown AR, Ankley GT et al (2014) Medicating the environment: assessing risks of pharmaceuticals to wildlife and ecosystems. Philos Trans R Soc B 369:20130569. https://doi.org/10.1098/rstb.2013.0569
Bai Y, Wu F, Liu C et al (2008) Interaction between carbamazepine and humic substances: a fluorescence spectroscopy study. Environ Toxicol Chem 27:95–102. https://doi.org/10.1897/07-013.1
Benotti MJ, Trenholm RA, Vanderford BJ et al (2009) Pharmaceuticals and endocrine disrupting compounds in U.S. drinking water. Environ Sci Technol 43:597–603. https://doi.org/10.1021/es801845a
Boxall AB, Rudd MA, Brooks BW et al (2012) Pharmaceuticals and personal care products in the environment: what are the big questions? Environ Health Perspect 120:1221–1229
Brausch JM, Connors KA, Brooks BW, Rand GM (2012) Human pharmaceuticals in the aquatic environment: a review of recent toxicological studies and considerations for toxicity testing. Rev Environ Contam Toxicol 218:1–99
Bu Q, Wang B, Huang J et al (2013) Pharmaceuticals and personal care products in the aquatic environment in China: a review. J Hazard Mater 262:189–211. https://doi.org/10.1016/j.jhazmat.2013.08.040
Cardoso O, Porcher J-M, Sanchez W (2014) Factory-discharged pharmaceuticals could be a relevant source of aquatic environment contamination: review of evidence and need for knowledge. Chemosphere 115:20–30. https://doi.org/10.1016/j.chemosphere.2014.02.004
Carmosini N, Lee LS (2009) Ciprofloxacin sorption by dissolved organic carbon from reference and bio-waste materials. Chemosphere 77:813–820. https://doi.org/10.1016/j.chemosphere.2009.08.003
Daughton C, Ternes T (1999) Special report: pharmaceuticals and personal care products in the environment: agents of subtle change? Environ Health Perspect. https://doi.org/10.1289/ehp.99107s6907
Delle Site A (2001) Factors affecting sorption of organic compounds in natural sorbent/water systems and sorption coefficients for selected pollutants. A review. J Phys Chem Ref Data 30:187–439. https://doi.org/10.1063/1.1347984
Ding Y, Teppen BJ, Boyd SA, Li H (2013) Measurement of associations of pharmaceuticals with dissolved humic substances using solid phase extraction. Chemosphere 91:314–319. https://doi.org/10.1016/j.chemosphere.2012.11.039
EMA (2006) Guideline on the environmental risk assessment of medicinal, pp 1–12
European Comission Joint Research Centre (2003) Technical guidance document on risk assessment in support of Commission Directive 93/67/EEC on risk assessment for new notified substances and Commission Regulation (EC) No. 1488/94 on risk assessment for existing substances. Part II. EUR 20418 EN/2. Eur Chem Bur Part II, pp 7–179
Ferreira Da Silva B, Jelic A, López-Serna R et al (2011) Occurrence and distribution of pharmaceuticals in surface water, suspended solids and sediments of the Ebro river basin, Spain. Chemosphere 85:1331–1339. https://doi.org/10.1016/j.chemosphere.2011.07.051
Filella M (2009) Freshwaters: which NOM matters? Environ Chem Lett 7:21–35. https://doi.org/10.1007/s10311-008-0158-x
Gardner M, Comber S, Scrimshaw MD et al (2012) The significance of hazardous chemicals in wastewater treatment works effluents. Sci Total Environ 437:363–372. https://doi.org/10.1016/j.scitotenv.2012.07.086
Gardner M, Jones V, Comber S et al (2013) Performance of UK wastewater treatment works with respect to trace contaminants. Sci Total Environ 456–457:359–369. https://doi.org/10.1016/j.scitotenv.2013.03.088
Githinji LJM, Musey MK, Ankumah RO (2011) Evaluation of the fate of ciprofloxacin and amoxicillin in domestic wastewater. Water Air Soil Pollut 219:191–201. https://doi.org/10.1007/s11270-010-0697-1
Grenni P, Patrolecco L, Ademollo N et al (2013) Degradation of gemfibrozil and naproxen in a river water ecosystem. Microchem J 107:158–164. https://doi.org/10.1016/j.microc.2012.06.008
Gurr CJ, Reinhard M (2006) Harnessing natural attenuation of pharmaceuticals and hormones in rivers. Environ Sci Technol 40:2872–2876. https://doi.org/10.1021/es062677d
Heberer T (2002) Tracking persistent pharmaceutical residues from municipal sewage to drinking water. J Hydrol 266:175–189. https://doi.org/10.1016/S0022-1694(02)00165-8
Hernandez-Ruiz S, Abrell L, Wickramasekara S et al (2012) Quantifying PPCP interaction with dissolved organic matter in aqueous solution: combined use of fluorescence quenching and tandem mass spectrometry. Water Res 46:943–954. https://doi.org/10.1016/j.watres.2011.11.061
Hernandez-Ruiz S, Wickramasekara S, Abrell L et al (2013) Complexation of trace organic contaminants with fractionated dissolved organic matter: implications for mass spectrometric quantification. Chemosphere 91:344–350. https://doi.org/10.1016/j.chemosphere.2012.11.059
Holbrook RD, Love NG, Novak JT (2004) Sorption of 17-beta-estradiol and 17 alpha-ethinylestradiol by colloidal organic carbon derived from biological wastewater treatment systems. Environ Sci Technol 38:3322–3329
Hudson N, Baker A, Reynolds D (2007) Fluorescence analysis of dissolved organic matter in natural, waste, and polluted waters-a review. River Res Appl 23:631–649. https://doi.org/10.1002/rra.1005FLUORESCENCE
Kim HJ, Lee DS, Kwon JH (2010) Sorption of benzimidazole anthelmintics to dissolved organic matter surrogates and sewage sludge. Chemosphere 80:256–262. https://doi.org/10.1016/j.chemosphere.2010.04.029
Kinch MS, Haynesworth A, Kinch SL, Hoyer D (2014) An overview of FDA-approved new molecular entities: 1827–2013. Drug Discov Today 19:1033–1039. https://doi.org/10.1016/j.drudis.2014.03.018
Kookana RS, Williams M, Boxall ABA et al (2014) Potential ecological footprints of active pharmaceutical ingredients: an examination of risk factors in low-, middle-and high-income countries. Philos Trans R Soc B 369:20130586
Koumaki E, Mamais D, Noutsopoulos C (2016) Environmental fate of non-steroidal anti-inflammatory drugs in river water/sediment systems. J Hazard Mater. https://doi.org/10.1016/j.msec.2004.08.001
Lahti M, Oikari A (2011) Pharmaceuticals in settleable particulate material in urban and non-urban waters. Chemosphere 85:826–831. https://doi.org/10.1016/j.chemosphere.2011.06.084
Larsson DGJ (2014) Pollution from drug manufacturing: review and perspectives. Philos Trans R Soc Lond B Biol Sci 369:20130571. https://doi.org/10.1098/rstb.2013.0571
Le Guet T, Hsini I, Labanowski J, Mondamert L (2018) Sorption of selected pharmaceuticals by a river sediment: role and mechanisms of sediment or Aldrich humic substances. Environ Sci Pollut Res. https://doi.org/10.1007/s11356-018-1684-0
Leenheer JA, Croué JP (2003) Peer reviewed: characterizing aquatic dissolved organic matter. Environ Sci Technol 37:18A–26A. https://doi.org/10.1021/es032333c
Li Z, Sobek A, Radke M (2015) Flume experiments to investigate the environmental fate of pharmaceuticals and their transformation products in streams. Environ Sci Technol 49:6009–6017. https://doi.org/10.1021/acs.est.5b00273
Lin AYC, Lin CA, Tung HH, Chary NS (2010) Potential for biodegradation and sorption of acetaminophen, caffeine, propranolol and acebutolol in lab-scale aqueous environments. J Hazard Mater 183:242–250. https://doi.org/10.1016/j.jhazmat.2010.07.017
Liu R, Wilding A, Hibberd A, Zhou JL (2005) Partition of endocrine-disrupting chemicals between colloids and dissolved phase as determined by cross-flow ultrafiltration. Environ Sci Technol 39:2753–2761. https://doi.org/10.1021/es0484404
Löffler D, Römbke J, Meller M, Ternes TA (2005) Environmental fate of pharmaceuticals in water/sediment systems. Environ Sci Technol 39:5209–5218. https://doi.org/10.1021/es0484146
Lützhøft HCH, Vaes WHJ, Freidig AP et al (2000) Influence of pH and other modifying factors on the distribution behavior of 4-quinolones to solid phases and humic acids studied by “negligible-depletion” SPME-HPLC. Environ Sci Technol 34:4989–4994. https://doi.org/10.1021/es000917y
Malik OA, Hsu A, Johnson LA, de Sherbinin A (2015) A global indicator of wastewater treatment to inform the sustainable development goals (SDGs). Environ Sci Policy 48:172–185. https://doi.org/10.1016/j.envsci.2015.01.005
Maoz A, Chefetz B (2010) Sorption of the pharmaceuticals carbamazepine and naproxen to dissolved organic matter: role of structural fractions. Water Res 44:981–989. https://doi.org/10.1016/j.watres.2009.10.019
Martínez-Hernández V, Meffe R, Herrera S et al (2014) Sorption/desorption of non-hydrophobic and ionisable pharmaceutical and personal care products from reclaimed water onto/from a natural sediment. Sci Total Environ 472:273–281. https://doi.org/10.1016/j.scitotenv.2013.11.036
Maskaoui K, Zhou JL (2010) Colloids as a sink for certain pharmaceuticals in the aquatic environment. Environ Sci Pollut Res 17:898–907. https://doi.org/10.1007/s11356-009-0279-1
Maskaoui K, Hibberd A, Zhou JL (2007) Assessment of the interaction between aquatic colloids and pharmaceuticals facilitated by cross-flow ultrafiltration. Environ Sci Technol 41:8038–8043. https://doi.org/10.1021/es071507d
Miao XS, Yang JJ, Metcalfe CD (2005) Carbamazepine and its metabolites in wastewater and in biosolids in a municipal wastewater treatment plant. Environ Sci Technol 39:7469–7475. https://doi.org/10.1021/es050261e
Michael-Kordatou I, Michael C, Duan X et al (2015) Dissolved effluent organic matter: characteristics and potential implications in wastewater treatment and reuse applications. Water Res 77:213–248. https://doi.org/10.1016/j.watres.2015.03.011
Nikolaou A, Meric S, Fatta D (2007) Occurrence patterns of pharmaceuticals in water and wastewater environments. Anal Bioanal Chem 387:1225–1234. https://doi.org/10.1007/s00216-006-1035-8
OECD (1992) OECD 301—guideline for testing of chemicals, pp 1–13
OECD (2000) OECD 106 adsorption—desorption using a batch equilibrium method. OECD Guidel Test Chem. https://doi.org/10.1787/9789264069602-en
Oh S, Shin WS, Kim HT (2016) Effects of pH, dissolved organic matter, and salinity on ibuprofen sorption on sediment. Environ Sci Pollut Res 23:22882–22889. https://doi.org/10.1007/s11356-016-7503-6
Paul SC, Githinji LJM, Ankumah RO et al (2014) Sorption behavior of ibuprofen and naproxen in simulated domestic wastewater. Water Air Soil Pollut. https://doi.org/10.1007/s11270-013-1821-9
Peng N, Wang K, Liu G et al (2014) Quantifying interactions between propranolol and dissolved organic matter (DOM) from different sources using fluorescence spectroscopy. Environ Sci Pollut Res 21:5217–5226. https://doi.org/10.1007/s11356-013-2436-9
Ra JS, Oh SY, Lee BC, Kim SD (2008) The effect of suspended particles coated by humic acid on the toxicity of pharmaceuticals, estrogens, and phenolic compounds. Environ Int 34:184–192. https://doi.org/10.1016/j.envint.2007.08.001
Rowett CJ, Hutchinson TH, Comber SDW (2016) The impact of natural and anthropogenic dissolved organic carbon (DOC), and pH on the toxicity of triclosan to the crustacean Gammarus pulex (L.). Sci Total Environ 565:222–231
Savci S (2013) A review of occurrence of pharmaceuticals in sediments. Afr J Biotechnol 12:4539–4541. https://doi.org/10.5897/AJB2013.12030
Shimizu A, Takada H, Koike T et al (2013) Ubiquitous occurrence of sulfonamides in tropical Asian waters. Sci Total Environ 452–453:108–115. https://doi.org/10.1016/j.scitotenv.2013.02.027
Song W, Guo M (2014) Applied manure and nutrient chemistry for sustainable agriculture and environment
Stein K, Ramil M, Fink G et al (2008) Analysis and sorption of psychoactive drugs onto sediment. Environ Sci Technol 42:6415–6423. https://doi.org/10.1021/es702959a
Sumpter JP, Jobling S (1995) Vitellogenesis as a biomarker for estrogenic contamination of the aquatic environment. Environ Health Perspect 103(Suppl 7):173–178
Svahn O, Bjorklund E (2015) Describing sorption of pharmaceuticals to lake and river sediments, and sewage sludge from UNESCO Biosphere Reserve Kristianstads Vattenrike by chromatographic asymmetry factors and recovery measurements. J Chromatogr A 1415:73–82. https://doi.org/10.1016/j.chroma.2015.08.061
Swan GE, Cuthbert R, Quevedo M et al (2006) Toxicity of diclofenac to Gyps vultures. Biol Lett 2:279–282. https://doi.org/10.1098/rsbl.2005.0425
Tappin AD, Loughnane JP, McCarthy AJ, Fitzsimons MF (2012) Removal of atrazine from river waters by indigenous microorganisms. Environ Chem Lett 10:89–96. https://doi.org/10.1007/s10311-011-0332-4
Tappin AD, Loughnane JP, McCarthy AJ, Fitzsimons MF (2014) Bacterio-plankton transformation of diazepam and 2-amino-5-chlorobenzophenone in river waters. Environ Sci Process Impacts 16:2227–2236. https://doi.org/10.1039/c4em00306c
Tchobanoglous G, Burton F, Stensel HD, Eddy M (2003) Wastewater engineering: treatment and reuse. McGraw-Hill, Boston
Urrestarazu Ramos EU, Meijer SN, Vaes WHJ et al (1998) Using solid-phase microextraction to determine partition coefficients to humic acids and bioavailable concentrations of hydrophobic chemicals. Environ Sci Technol 32:3430–3435. https://doi.org/10.1021/es980274a
Varga M, Dobor J, Helenkár A et al (2010) Investigation of acidic pharmaceuticals in river water and sediment by microwave-assisted extraction and gas chromatography–mass spectrometry. Microchem J 95:353–358. https://doi.org/10.1016/j.microc.2010.02.010
Verbruggen B, Gunnarsson L, Kristiansson E et al (2018) ECOdrug: a database connecting drugs and conservation of their targets across species. Nucleic Acids Res 46:D930–D936. https://doi.org/10.1093/nar/gkx1024
Wang Y, Zhang M, Fu J et al (2016) Insights into the interaction between carbamazepine and natural dissolved organic matter in the Yangtze Estuary using fluorescence excitation–emission matrix spectra coupled with parallel factor analysis. Environ Sci Pollut Res. https://doi.org/10.1007/s11356-016-7203-2
West CE, Rowland SJ (2012) Aqueous phototransformation of diazepam and related human metabolites under simulated sunlight. Environ Sci Technol 46:4749–4756. https://doi.org/10.1021/es203529z
Xing Y, Chen X, Zhuang J, Chen X (2015) What happens when pharmaceuticals meet colloids. Ecotoxicology 24:2100–2114. https://doi.org/10.1007/s10646-015-1557-y
Yamamoto H, Liljestrand HM, Shimizu Y, Morita M (2003) Effects of physical–chemical characteristics on the sorption of selected endocrine disruptors by dissolved organic matter surrogates. Environ Sci Technol 37:2646–2657. https://doi.org/10.1021/es026405w
Yamamoto H, Nakamura Y, Moriguchi S et al (2009) Persistence and partitioning of eight selected pharmaceuticals in the aquatic environment: laboratory photolysis, biodegradation, and sorption experiments. Water Res 43:351–362. https://doi.org/10.1016/j.watres.2008.10.039
Yang S-F, Lin C-F, Yu-Chen LA, Andy Hong P-K (2011) Sorption and biodegradation of sulfonamide antibiotics by activated sludge: Experimental assessment using batch data obtained under aerobic conditions. Water Res 45(11):3389–3397
Zhou J, Broodbank N (2014) Sediment–water interactions of pharmaceutical residues in the river environment. Water Res 48:61–70. https://doi.org/10.1016/j.watres.2013.09.026
Zhou JL, Liu R, Wilding A, Hibberd A (2007) Sorption of selected endocrine disrupting chemicals to different aquatic colloids. Environ Sci Technol 41:206–213. https://doi.org/10.1021/es0619298
Acknowledgements
The support of AstraZeneca through a studentship awarded to SB is gratefully acknowledged.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
There are no conflict of interest regarding the content of this manuscript, authors, or financial relationship.
Rights and permissions
About this article
Cite this article
Bagnis, S., Fitzsimons, M.F., Snape, J. et al. Processes of distribution of pharmaceuticals in surface freshwaters: implications for risk assessment. Environ Chem Lett 16, 1193–1216 (2018). https://doi.org/10.1007/s10311-018-0742-7
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10311-018-0742-7