Abstract
Background and purpose
Estrogenic compounds and antibiotic residues in environment are receiving significant attention because of their potential adverse effects on ecosystems and human health. The objectives of this study were to determine the occurrence and seasonal variability of eight kinds of estrogenic compounds and 14 antibiotics. The study developed an occurrence database of the estrogenic compounds and antibiotics in spatial and temporal scale in Jiulongjiang River, South China, to provide useful information for environmental management of this region.
Methods
Eight estrogenic compounds and 14 antibiotic compounds were detected in Jiulongjiang River from 19 sampling sites during high-flow and low-flow season in surface water. The samples were preconcentrated by solid-phase extraction for analysis. Eight estrogenic compounds were analyzed by gas chromatography mass spectrometry (Agilent 7890A-5975C), and antibiotics were determined by liquid chromatography-tandem mass spectrometry (LC–MS/MS) system (ABI 3200 Q TRAP).
Results
All target compounds could be detected, except 17α-ethynylestradiol, sulfamerazine, and ofloxacin. The median concentrations for seven estrogenic compounds ranged from 6.00 to 610.72 ng/L, with the detection frequency range of 16.00–100%. However, the detection frequencies of 13 antibiotics detected varied from 50% to 100%, with the median concentrations ranged from 0.89 to 117.97 ng/L. Seasonal variations were obvious for most estrogenic compounds in Jiulongjiang River, except for octylphenol and estriol. There were significant (P < 0.001) differences for three tetracyclines, sulfadiazine, and sulfamethoxazole between in low-flow season and in high-flow season. Besides, spatially considerable variations in the concentrations were observed for antibiotics, nonylphenol, octylphenol, and bisphenol A.
Conclusion
The Jiulongjiang River water was more seriously contaminated by diethylstilbestrol, estrone, sulfamethazine, and tetracyclines. Higher overall concentration levels of estrogenic compounds and antibiotics were detected in low-flow water than those in high-flow water. The pollution of estrogenic compounds and antibiotics in Jiulongjiang River mainly came from municipal sewage and livestock breeding activities.
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References
Arikan OA, Rice C, Codling E (2008) Occurrence of antibiotics and hormones in a major agricultural watershed. Desalination 226:121–133
Ballesteros-Gomez A, Ruiz FJ, Rubio S, Perez-Bendito D (2007) Determination of bisphenols A and F and their diglycidyl ethers in wastewater and river water by coacervative extraction and liquid chromatography-fluorimetry. Anal Chim Acta 603:51–59
Batt AL, Snow DD, Aga DS (2006) Occurrence of sulfonamide antimicrobials in private water wells in Washington County, Idaho, USA. Chemosphere 64:1963–1971
Benotti MJ, Trenholm RA, Vanderford BJ, Standford BD, Snyder SA (2009) Pharmaceuticals and endocrine disrupting compounds in U.S. drinking water. Environ Sci Technol 43:597–603
Bortone SA, Davis WP, Bundrick CM (1989) Morphological and behavior characters as potential bioindication of exposure to kraft mill effluent. Bull Environ Contam Toxicol 43:370–377
Cargouet M, Perdiz D, Mouatassim-Souali A, Tamisier-Karolak S, Levi Y (2004) Assessment of river contamination by estrogenic compounds in Paris area (France). Sci Total Environ 324:55–66
Chang H, Hu J, Asami M, Kunikane S (2008) Simultaneous analysis of 16 sulfonamide and trimethoprim antibiotics in environmental waters by liquid chromatography-electrospray tandem mass spectrometry. J Chromatogr A 1190:390–393
Chee-Sanford JC, Aminov RI, Krapac IJ, Garrigues-Jeanjean N, Mackie RI (2001) Occurrence and diversity of tetracycline resistance genes in lagoons and groundwater underlying two swine production facilities. Appl Environ Microbiol 67:1494–1502
Chen CY, Wen TY, Wang GS (2007) Determining estrogenic steroids in Taipei waters and removal in drinking water treatment using high-flow solid-phase extraction and liquid chromatography/tandem mass spectrometry. Sci Total Environ 378:352–365
Choi K, Kim Y, Park J, Park CK, Kim MY, Kim HS, Kim P (2008) Seasonal variations of several pharmaceutical residues in surface water and sewage treatment plants of Han River, Korea. Sci Total Environ 405:120–128
Colborn T, vom Saal FS, Soto AM (1993) Developmental effects of endocrine disrupting compounds in wildlife and humans. Environ Health Perspect 101:378–384
Damstra T, Barlow S, Bergman A, Kavlock R, Van Der Kraak G (2002) Global assessment of the state-of-the-science of endocrine disruptors. Available at: International Programme on Chemical Safety, World Health Organisation. http://www.who.int/ipcs/publications/endocrine_disruptors/en/
Daughton CG, Ternes TA (1999) Pharmaceuticals and personal care products in the environment: agents of subtle change? Environ Health Perspect 107(Suppl 6):907–938
Fatima T, Mercier F, Le Bot B, Eurin J, Tuc Dinh Q, Clement M, Chevreuil M (2008) Occurrence and fate of antibiotics in the Seine River in various hydrological conditions. Sci Total Environ 393:84–95
Fromme H, Kuchler T, Otto T, Pilz K, Muller J, Wenzel A (2002) Occurrence of phthalates and bisphenol A and F in the environment. Water Res 36:1429–1438
Gong J, Ran Y, Yang Y (2008) Contamination of estrogenic compounds in the surface water of Guangzhou reach of the Pearl River. Environ Chem (in Chinese) 27(2):242–244
Hanselman TA, Graetz DA, Wilkie AC (2003) Manure-borne estrogens as potential environmental contaminants: a review. Environ Sci Technol 37:5471–5478
Heberer T (2002) Occurrence, fate, and removal of pharmaceutical residues in theaquatic environment: a review of recent research data. Toxicol Lett 131:5–17
Heemken OP, Reincke H, Stachel B (2001) The occurrence of xenoestrogens in the Elbe river and the North Sea. Chemosphere 45:245–259
Hintemann T, Schneider C, Scholer HF (2006) Field study using two immunoassays for the determination of estradiol and ethinylestradiol in the aquatic environment. Water Res 40:2287–2294
Huang YW, Twidwell DK, Elrod JC (2003) Occurrence and effects of endocrine disrupting chemicals in the environment. Pract Periodical Haz Toxic Radioactive Waste Mgmt 7:241–252
Jesus GM, Ma V, Silvia Diaz-Cruz M (2010) LC-QqLIT MS analysis of nine sulfonamides and one of their acetylated metabolites in the Llobregat River basin. Quantitative determination and qualitative evaluation by IDA experiments. Anal Bioanal Chem 397:1325–1334
Jiang L, Chen SY, Yang R, Ren ZY, Yin DQ (2008) Occurrence of antibiotics in the aquatic environment of the Changjiang Delta, China. Environ Chem 27:371–374 (in Chinese)
Jiang L, Hu X, Yin D, Zhang H, Yu Z (2011) Occurrence, distribution and seasonal variation of antibiotics in the Huangpu River, Shanghai, China. Chemosphere 82:822–828
Jobling S, Sumpter JP (1993) Detergent components in sewage effluent are weakly oestrogenic to fish: an in vitro study using rainbow trout (Oncorhynchus mykiss) hepatocytes. Aquat Toxicol 27:361–372
Jobling S, Casey D, Gray TR, Oehlmann J, Oehlmann US, Pawlowski S, Baunbeck T, Turner AP, Tyler CR (2004) Comparative responses of mollusks and fish to environmental estrogens and an estrogenic effluent. Aquat Toxicol 66:207–222
Kang J, Kondo F (2002) Effects of bacterial counts and temperature on the biodegradation of bisphenol A in river water. Chemosphere 49:493–498
Karthikeyan KG, Meyer MT (2006) Occurrence of antibiotics in wastewater treatment facilities in Wisconsin, USA. Sci Total Environ 361:196–207
Kathryn DB, Jerzy K, Bruce T, Timothy HC, Douglas BM (2006) Occurrence of antibiotics in hospital, residential, and dairy, effluent, municipal wastewater, and the Rio Grande in New Mexico. Sci Total Environ 366:772–783
Kay P, Blackwell PA, Boxall ABA (2005) Transport of veterinary antibiotics in overland flow following the application of slurry to arable land. Chemosphere 59:951–959
Kim SD, Cho J, Kim IS, Vanderford BJ, Snyder SA (2007) Temporal and spatial trends in the occurrence of human and veterinary antibiotics in aqueous and river sediment matrices. Environ Sci Technol 41:50–57
Kolodziej EP, Harter T, Sedlak DL (2004) Dairy wastewater, aquaculture and spawning fish as sources of steroid hormones in the aquatic environment. Environ Sci Technol 38:6377–6384
Kolpin DW, Furlong ET, Meyer MT, Thurman EM, Zaugg SD, Barber LB, Buxton HT (2002) Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999–2000: a national reconnaissance. Environ Sci Technol 36:1202–1211
Kümmerer K (2009) Antibiotics in the aquatic environment—a review—part I. Chemosphere 75:417–434
Labadie P, Budzinski H (2005) Determination of steroidal hormone profiles along the Jalle d’Eysines River (near Bordeaux, France). Environ Sci Technol 39:5113–5120
Lei B, Huang S, Zhou Y, Wang D, Wang Z (2009) Levels of six estrogens in water and sediment from three rivers in Tianjin area, China. Chemosphere 76:36–42
Lin XH, Li YY, He JY (2009) Analysis of estrogens and antibiotics residues in raw meat in Guangzhong. South China J Prev Med 35:71–73
Lissemore L, Hao CY, Yang P, Sibley PK, Mabury S, Solomon KR (2006) An exposure assessment for selected pharmaceuticals within a watershed in Southern Ontario. Chemosphere 54:661–668
Lopez-Roldan R, De Alda ML, Gros M (2010) Advanced monitoring of pharmaceuticals and estrogens in the Llobregat River basin (Spain) by liquid chromatography-triple quadrupole-tandem mass spectrometry in combination with ultra performance liquid chromatography-time of flight-mass spectrometry. Chemosphere 80:1337–1344
Luo Y, Xu L, Rysz M, Wang Y, Zhang H, Alvarez PJ (2011) Occurrence and transport of tetracycline, sulfonamide, quinolone, and macrolide antibiotics in the Haihe River Basin, China. Environ Sci Technol 45:1827–1833
Noppe H, Verslycke T, De Wulf E (2007) Occurrence of estrogens in the Scheldt estuary: a 2-year survey. Ecotox Environ Safe 66:1–8
Pruden A, Pei RT, Storteboom H, Carlson KH (2006) Antibiotic resistance genes as emerging contaminants: studies in Northern Colorado. Environ Sci Technol 40:7445–7450
Roepke TA, Snyder MJ, Cherr GN (2005) Estradiol and endocrine disrupting compounds adversely affect development of sea urchin embryos at environmentally relevant concentrations. Aquat Toxicol 71:155–173
Rysz M, Alvarez PJJ (2004) Amplification and attenuation of tetracycline resistance in soil bacteria: aquifer column experiments. Water Res 38:3705–3712
Schwab RW, Hayes EP, Fiori JM, Mastrocco FJ, Roden NM, Cragin D (2005) Human pharmaceuticals in US surface waters: a human health risk assessment. Regul Toxicol Pharmacol 42:296–312
Silva E, Rajapakse N, Kortenkamp A (2002) Something from “nothing” eight weak estrogenic chemicals combined at concentrations below NOECs produce significant mixture effects. Environ Sci Technol 36:1751–1756
Snyder SA, Trenholm RA, Snyder EM, Burce GM, Pleus RC, Hemming JDC (2008) Toxicological relevance of EDCs and pharmaceuticals in drinking water. American Water Works Association Research Foundation Report pp322
Staples CA, William JB, Blessing RL, Varineau PT (1999) Measuring the biodegradability of nonylphenol ether caroxylates, octylphenol ether carboxylates, and nonylphenol. Chemosphere 38:3925–3931
Stasinakis SA, Gatidou G, Mamais D, Thomaidis SN, Lekkas DT (2008) Occurrence and fate of endocrine disrupters in Greek sewage treatment plants. Water Res 42:1796–1804
Tamtam F, Mercier F, Le Bot B, Eurin J, Tuc Dinh Q, Clement M (2008) Occurrence and fate of antibiotics in the Seine River in various hydrological conditions. Sci Total Environ 393:84–95
Ternes TA (1998) Occurrence of drugs in German sewage treatment plants and rivers. Water Res 32:3245–3260
Ternes TA, Kreckel P, Mueller J (1999) Behaviour and occurrence of estrogens in municipal sewage treatment plants-II. Aerobic batch experiments with activated sludge. Sci Total Environ 225:91–99
Vethaak AD, Lahr J, Schrap SM (2005) An integrated assessment of estrogenic contamination and biological effects in the aquatic environment of The Netherlands. Chemosphere 59:511–524
Watkinson AJ, Murby EJ, Kolpin DW (2009) The occurrence of antibiotics in an urban watershed: from wastewater to drinking water. Sci Total Environ 407:2711–2723
Xiao YH (2009) Available from http://news.qq.com
Xie JJ (2009) Available from http://e.cdqss.com/html/2009-09/16/content_77457.htm
Xu WH, Zhang G, Zou SC, Li XD, Liu YC (2007) Determination of selected antibiotics in the Victoria Harbour and the Pearl River, South China using high performance liquid chromatography-electrospray ionization tandem mass spectrometry. Environ Pollut 145:672–679
Xu WH, Zhang G, Zou SC, Ling ZH, Wang GL, Ya W (2009) A preliminary investigation on the occurrence and distribution of antibiotics in the Yellow River and its tributaries, China. Water Environ Res 81:248–254
Ying GG, Kookana RS, Ru YJ (2002) Occurrence and fate of hormone steroids in the environment. Environ Int 28:545–551
Yoon Y, Ryu J, Oh J (2010) Occurrence of endocrine disrupting compounds, pharmaceuticals, and personal care products in the Han River (Seoul, South Korea). Sci Total Environ 408:636–643
Yuan C, Li J, Geng W (2009) Investigation of veterinary drug residues in raw meat in Harbin. Chin J Public Health 25:747–748
Zhang X, Li QZ, Li GX, Yan CZ (2009) Levels of estrogenic compounds in Xiamen Bay Sediment, China. Mar Pollut Bull 58:1210–1216
Zhang DD, Lin L, Luo Z, Yan C, Zhang X (2011) Occurrence of selected antibiotics in Jiulongjiang River in various seasons, South China. J Environ Monit 13:1593–1601
Zou S, Xu W, Zhang R, Tang J, Chen Y, Zhang G (2011) Occurrence and distribution of antibiotics in coastal water of the Bohai Bay, China: impacts of river discharge and aquaculture activities. Environ Pollut. doi:10.1016/j.envpol.2011.04.037
Zuccato E, Castiglioni S, Bagnati R, Fanelli R (2010) Source, occurrence and fate of antibiotics in the Italian aquatic environment. J Hazard Mater 179:1042–1048
Acknowledgments
This work is financially supported by International Cooperation of Ministry Science and Technology of China (No. 2009DFB90120).
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Zhang, X., Zhang, D., Zhang, H. et al. Occurrence, distribution, and seasonal variation of estrogenic compounds and antibiotic residues in Jiulongjiang River, South China. Environ Sci Pollut Res 19, 1392–1404 (2012). https://doi.org/10.1007/s11356-012-0818-z
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DOI: https://doi.org/10.1007/s11356-012-0818-z