Pharmaceutical compounds in aquatic environment in China: locally screening and environmental risk assessment

Abstract

An environmental risk assessment was performed for pharmaceutical compounds present in the aquatic environment of China. Predicted environmental concentration (PEC) of the compounds were calculated according to European Medicines Evaluation Agency (EMEA) guidelines. Available ecotoxicological data compromised by applying a very conservative assessment factor (AF) were employed to calculate the predicted no-effect concentration (PNEC). The screening principle and the risk assessment were based on risk quotient (RQ), which derived from the PEC and related PNEC values. PEC results indicated that all the compounds except sulfadimethoxine and levocarnitine, should carry out phase II risk assessment in EMEA guideline. RQ values suggested that more than 36 pharmaceuticals may be imposed health threats to the aquatic environment; especially the antibiotic therapeutic class including amoxicillin, sulfasalazine, trimethoprim, oxytetracycline and erythromycin showed high RQ values. These substances with high RQ value (RQ≥1) were regarded as top-priority pharmaceuticals for control in the aquatic environment of China. However, the antibiotic substances which had low risk quotient (RQ <1), should be reassessed by its potentially induced resistance under low concentration in future.

Graphical abstract

Keywords

pharmaceuticals / aquatic environment / risk assessment / aquatic toxicity / risk quotient

References

[1] Carlsson C, Johansson A K, Alvan G, Bergman K, Kühler T. Are pharmaceuticals potent environmental pollutants? Part I: environmental risk assessments of selected active pharmaceutical ingredients. The Science of the Total Environment, 2006, 364(1–3): 67–87

[2] Santos L H, Araújo A N, Fachini A, Pena A, Delerue-Matos C, Montenegro M C. Ecotoxicological aspects related to the presence of pharmaceuticals in the aquatic environment. Journal of Hazardous Materials, 2010, 175(1–3): 45–95

[3] Kümmerer K. Antibiotics in the aquatic environment—a review—part I. Chemosphere, 2009, 75(4): 417–434

[4] Ellis J B. Pharmaceutical and personal care products (PPCPs) in urban receiving waters. Environmental pollution, 2006, 144(1): 184–189

[5] Kolpin D W, Furlong E T, Meyer M T, Thurman E M, Zaugg S D, Barber L B, Buxton H T. Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999–2000: a national reconnaissance. Environmental Science and Technology, 2002, 36(6): 1202–1211

[6] Calamari D, Zuccato E, Castiglioni S, Bagnati R, Fanelli R. Strategic survey of therapeutic drugs in the Rivers Po and Lambro in Northern Italy. Environmental Science and Technology, 2003, 37(7): 1241–1248

[7] Managaki S, Murata A, Takada H, Tuyen B C, Chiem N H. Distribution of macrolides, sulfonamides, and trimethoprim in tropical waters: ubiquitous occurrence of veterinary antibiotics in the Mekong Delta. Environmental Science and Technology, 2007, 41(23): 8004–8010

[8] Yu C P, Chu K H. Occurrence of pharmaceuticals and personal care products along the West Prong Little Pigeon River in east Tennessee, USA. Chemosphere, 2009, 75(10): 1281–1286

[9] Yoon Y, Ryu J, Oh J, Choi B G, Snyder S A. Occurrence of endocrine disrupting compounds, pharmaceuticals, and personal care products in the Han River (Seoul, Korea). The Science of the Total Environment, 2010, 408(3): 636–643

[10] Calderón-Preciado D, Jiménez-Cartagena C, Matamoros V, Bayona J M. Screening of 47 organic microcontaminants in agricultural irrigation waters and their soil loading. Water Research, 2011, 45(1): 221–231

[11] Pruden A, Pei R, Storteboom H, Carlson K H. Antibiotic resistance genes as emerging contaminants: studies in northern Colorado. Environmental Science and Technology, 2006, 40(23): 7445–7450

[12] Baquero F, Martínez J L, Cantón R. Antibiotics and antibiotic resistance in water environments. Current Opinion in Biotechnology, 2008, 19(3): 260–265

[13] EMEA. Discussion paper on environmental risk assessment of non-genetically modified organism (non-GMO) containing medicinal products for human use. CPMP/SWP/4447/00 draft corr. The European Agency for the Evaluation of Medicinal Products, 2001

[14] EMEA. Guideline on the environmental risk assessment of medicinal products for human use. CHMP/SWP/4470/00 draft. The European Agency for Evaluation of Medidicinal Products- Pre-Authorisation Evaluation of Medicines for Human Use (Committee for medicinal Products for Human Use), 2005

[15] Grung M, Källqvist T, Sakshaug S, Skurtveit S, Thomas K V. Environmental assessment of Norwegian priority pharmaceuticals based on the EMEA guideline. Ecotoxicology and Environmental Safety, 2008, 71(2): 328–340

[16] Jones O A H, Voulvoulis N, Lester J N. Aquatic environmental assessment of the top 25 English prescription pharmaceuticals. Water Research, 2002, 36(20): 5013–5022

[17] Stuer-Lauridsen F, Birkved M, Hansen L P, Holten Lützhøft H C, Halling-Sørensen B. Environmental risk assessment of human pharmaceuticals in Denmark after normal therapeutic use. Chemosphere, 2000, 40(7): 783–793

[18] Park S, Choi K. Hazard assessment of commonly used agricultural antibiotics on aquatic ecosystems. Ecotoxicology (London, England), 2008, 17(6): 526–538

[19] Xu W H, Zhang G, Zou S C, Li X D, Liu Y C. Determination of selected antibiotics in the Victoria Harbour and the Pearl River, South China using high-performance liquid chromatography-electrospray ionization tandem mass spectrometry. Environmental Pollution, 2007, 145(3): 672–679

[20] Peng X, Zhang K, Tang C, Huang Q, Yu Y, Cui J. Distribution pattern, behavior, and fate of antibacterials in urban aquatic environments in South China. Journal of Environmental Monitoring, 2011, 13(2): 446–454

[21] Zhao J L, Ying G G, Wang L, Yang J F, Yang X B, Yang L H, Li X. Determination of phenolic endocrine disrupting chemicals and acidic pharmaceuticals in surface water of the Pearl Rivers in South China by gas chromatography-negative chemical ionization-mass spectrometry. The Science of the Total Environment, 2009, 407(2): 962–974

[22] Cao J L, Shi J H, Han R, Li Y, Yang Z F. Seasonal variations in the occurrence and distribution of estrogens and pharmaceuticals in the Zhangweinanyun River System. Chinese Science Bulletin, 2010, 55(27–28): 3138–3144

[23] Huang Q, Yu Y, Tang C, Zhang K, Cui J, Peng X. Occurrence and behavior of non-steroidal anti-inflammatory drugs and lipid regulators in wastewater and urban river water of the Pearl River Delta, South China. Journal of Environmental Monitoring, 2011, 13(4): 855–863

[24] Yang J F, Ying G G, Zhao J L, Tao R, Su H C, Liu Y S. Spatial and seasonal distribution of selected antibiotics in surface waters of the Pearl Rivers, China. Journal of Environmental Science and Health. Part. B, Pesticides, Food Contaminants, and Agricultural Wastes, 2011, 46(3): 272–280

[25] Luo Y, Xu L, Rysz M, Wang Y, Zhang H, Alvarez P J. Occurrence and transport of tetracycline, sulfonamide, quinolone, and macrolide antibiotics in the Haihe River Basin, China. Environmental Science and Technology, 2011, 45(5): 1827–1833

[26] Wei R, Ge F, Huang S, Chen M, Wang R. Occurrence of veterinary antibiotics in animal wastewater and surface water around farms in Jiangsu Province, China. Chemosphere, 2011, 82(10): 1408–1414

[27] Halling-Sørensen B. Algal toxicity of antibacterial agents used in intensive farming. Chemosphere, 2000, 40(7): 731–739

[28] Brain R A, Johnson D J, Richards S M, Sanderson H, Sibley P K, Solomon K R. Effects of 25 pharmaceutical compounds to Lemna gibba using a seven-day static-renewal test. Environmental Toxicology and Chemistry, 2004, 23(2): 371–382

[29] Eguchi K, Nagase H, Ozawa M, Endoh Y S, Goto K, Hirata K, Miyamoto K, Yoshimura H. Evaluation of antimicrobial agents for veterinary use in the ecotoxicity test using microalgae. Chemosphere, 2004, 57(11): 1733–1738

[30] Isidori M, Lavorgna M, Nardelli A, Pascarella L, Parrella A. Toxic and genotoxic evaluation of six antibiotics on non-target organisms. The Science of the Total Environment, 2005, 346(1-3): 87–98

[31] Kim Y, Choi K, Jung J, Park S, Kim P G, Park J. Aquatic toxicity of acetaminophen, carbamazepine, cimetidine, diltiazem and six major sulfonamides, and their potential ecological risks in Korea. Environment International, 2007, 33(3): 370–375

[32] WHO Collaborating Centre, WHO Collaborating Centre for Drug Statistics Methodology, Oslo.

[33] China Medicine Economic Information Net (CMEIN). Chinese Medical Statistical Yearbook (2006–2007). Beijing: China Medicine Economic Information Net, 2007

[34] MistraPharma Wiki Database

[35] Veterinary Substances DataBase (VSDB)

[36] Database E C O T O X.

[37] Fick J, Lindberg R H, Tysklind M, Larsson D G. Predicted critical environmental concentrations for 500 pharmaceuticals. Regulatory Toxicology and Pharmacology, 2010, 58(3): 516–523

[38] Estimation Programs Interface (EPI) SuiteTM was developed by the US Environmental Protection Agency’s Office of Pollution Prevention

[39] Pomati F, Netting A G, Calamari D, Neilan B A. Effects of erythromycin, tetracycline and ibuprofen on the growth of Synechocystis sp. and Lemna minor. Aquatic Toxicology (Amsterdam, Netherlands), 2004, 67(4): 387–396

[40] De Lange H J, Noordoven W, Murk A J, Lürling M, Peeters E T. Behavioural responses of Gammarus pulex (Crustacea, Amphipoda) to low concentrations of pharmaceuticals. Aquatic Toxicology (Amsterdam, Netherlands), 2006, 78(3): 209–216

[41] Triebskorn R, Casper H, Scheil V, Schwaiger J. Ultrastructural effects of pharmaceuticals (carbamazepine, clofibric acid, metoprolol, diclofenac) in rainbow trout (Oncorhynchus mykiss) and common carp (Cyprinus carpio). Analytical and Bioanalytical Chemistry, 2007, 387(4): 1405–1416

[42] Kümmerer K. The presence of pharmaceuticals in the environment due to human use—present knowledge and future challenges. Journal of Environmental Management, 2009, 90(8): 2354–2366

[43] Zhou H, Wu C, Huang X, Gao M, Wen X, Tsuno H, Tanaka H. Occurrence of selected pharmaceuticals and caffeine in sewage treatment plants and receiving rivers in Beijing, China. Water Environment Research, 2010, 82(11): 2239–2248

[44] Xu W, Zhang G, Zou S, Ling Z, Wang G, Yan W. A preliminary investigation on the occurrence and distribution of antibiotics in the Yellow River and its tributaries, China. Water Environment Research, 2009, 81(3): 248–254

[45] Chang X, Meyer M T, Liu X, Zhao Q, Chen H, Chen J A, Qiu Z, Yang L, Cao J, Shu W. Determination of antibiotics in sewage from hospitals, nursery and slaughter house, wastewater treatment plant and source water in Chongqing region of Three Gorge Reservoir in China. Environmental Pollution, 2010, 158(5): 1444–1450

[46] Wang L, Ying G G, Zhao J L, Yang X B, Chen F, Tao R, Liu S, Zhou L J. Occurrence and risk assessment of acidic pharmaceuticals in the Yellow River, Hai River and Liao River of north China. The Science of the Total Environment, 2010, 408(16): 3139–3147

[47] Zhao J L, Ying G G, Liu Y S, Chen F, Yang J F, Wang L, Yang X B, Stauber J L, Warne M S. Occurrence and a screening-level risk assessment of human pharmaceuticals in the Pearl River system, South China. Environmental Toxicology and Chemistry, 2010, 29(6): 1377–1384

[48] Zhang D, Lin L, Luo Z, Yan C, Zhang X. Occurrence of selected antibiotics in Jiulongjiang River in various seasons, South China. Journal of Environmental Monitoring, 2011, 13(7): 1953–1960

[49] Jiang L, Hu X, Yin D, Zhang H, Yu Z. Occurrence, distribution and seasonal variation of antibiotics in the Huangpu River, Shanghai, China. Chemosphere, 2011, 82(6): 822–828

[50] Yang Y, Fu J, Peng H, Hou L, Liu M, Zhou J L. Occurrence and phase distribution of selected pharmaceuticals in the Yangtze Estuary and its coastal zone. Journal of Hazardous Materials, 2011, 190(1–3): 588–596

[51] Zou S, Xu W, Zhang R, Tang J, Chen Y, Zhang G. Occurrence and distribution of antibiotics in coastal water of the Bohai Bay, China: impacts of river discharge and aquaculture activities. Environmental Pollution, 2011, 159(10): 2913–2920

[52] Peng X, Yu Y, Tang C, Tan J, Huang Q, Wang Z. Occurrence of steroid estrogens, endocrine-disrupting phenols, and acid pharmaceutical residues in urban riverine water of the Pearl River Delta, South China. The Science of the Total Environment, 2008, 397(1-3): 158–166

[53] Sui Q, Huang J, Deng S, Chen W, Yu G. Seasonal variation in the occurrence and removal of pharmaceuticals and personal care products in different biological wastewater treatment processes. Environmental Science and Technology, 2011, 45(8): 3341–3348

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant No. 41301572); Tsinghua University-Veolia Environnment Joint Research Center for Advanced Environmental Technology.

RIGHTS & PERMISSIONS

2014 Higher Education Press and Springer-Verlag Berlin Heidelberg