Occurrence and distribution pattern of acidic pharmaceuticals in surface water, wastewater, and sediment of the Msunduzi River, Kwazulu-Natal, South Africa
Tóm tắt
The paucity of information on the occurrence of pharmaceuticals in the environment in African countries led the authors to investigate 8 acidic pharmaceuticals (4 antipyretics, 3 antibiotics, and 1 lipid regulator) in wastewater, surface water, and sediments from the Msunduzi River in the province of KwaZulu-Natal, South Africa, using solid-phase extraction (SPE) and liquid chromatography–mass spectrometry (LC/MS). The method recoveries, limits of detection (LOD), and limits of quantification were determined. The method recoveries were 58.4% to 103%, and the LODs ranged between 1.16 ng/L and 29.1 ng/L for water and between 0.58 ng/g and 14.5 ng/g for sediment. The drugs were all present in wastewater and in most of the surface water and sediment samples. Aspirin was the most abundant pharmaceutical observed, 118 ± 0.82 μg/L in wastewater influent, and the most observed antibiotic was nalidixic acid (25.2–29.9 μg/L in wastewater); bezafibrate was the least observed. The distribution pattern of the antipyretic in water indicates more impact in suburban sites. The solid–liquid partitioning of the pharmaceuticals between sediment and water, measured as the distribution coefficient (log KD) gave an average accumulation magnitude of 10× to 32× in sediments than in water. The downstream distribution patterns for both water and sediment indicate discharge contributions from wastewater, agricultural activities, domestic waste disposal, and possible sewer system leakages. Although concentrations of the pharmaceuticals were comparable with those obtained from some other countries, the contamination of the present study site with pharmaceuticals has been over time and continues at present, making effective management and control necessary. Environ Toxicol Chem 2016;35:36–46. © 2015 SETAC
Từ khóa
Tài liệu tham khảo
Halling-Sorensen, 2002, Toxicity of tetracyclines and tetracycline degradation products to environmentally relevant bacteria, including selected tetracycline-resistant bacteria, Arch Environ Contam Toxicol, 42, 263, 10.1007/s00244-001-0017-2
Brun, 2006, Pharmaceutically active compounds in Atlantic Canadian sewage treatment plant effluents and receiving waters, and potential for environmental effects as measured by acute and chronic aquatic toxicity, Environ Toxicol Chem, 25, 2163, 10.1897/05-426R.1
Carucci, 2006, Biodegradability and toxicity of pharmaceuticals in biological wastewater treatment plants, J Environ Sci Heal A, 41, 1831, 10.1080/10934520600779000
Schwab, 2005, Human pharmaceuticals in US surface waters: A human health risk assessment, Regul Toxicol Pharmacol, 42, 296, 10.1016/j.yrtph.2005.05.005
Benotti, 2009, Microbial degradation of pharmaceuticals in estuarine and coastal seawater, Environ Pollut, 157, 994, 10.1016/j.envpol.2008.10.009
Jones, 2001, Human pharmaceuticals in the aquatic environment: A review, Environ Technol, 22, 1383, 10.1080/09593330.2001.11090873
Lear, 2002, Chloroxylenol- and triclosan-tolerant bacteria from industrial sources, J Indust Microbiol Biot, 29, 238, 10.1038/sj.jim.7000320
Jones, 2003, Potential impact of pharmaceuticals on environmental health, Bull World Health Organ, 81, 768
Snyder, 2005, Pharmaceuticals and EDCs in the US water industry—An update, J Am Water Works Assoc, 97, 32, 10.1002/j.1551-8833.2005.tb07506.x
Kim, 2007, Occurrence and removal of pharmaceuticals and endocrine disruptors in South Korean surface, drinking, and waste waters, Water Res, 41, 1013, 10.1016/j.watres.2006.06.034
López-Roldán, 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, 10.1016/j.chemosphere.2010.06.042
Löffler, 2003, Determination of acidic pharmaceuticals, antibiotics and ivermectin in river sediment using liquid chromatography-tandem mass spectrometry, J Chromatogr A, 1021, 133, 10.1016/j.chroma.2003.08.089
Kim, 2006, Occurrence of ionophore antibiotics in water and sediments of a mixed-landscape watershed, Water Res, 40, 2549, 10.1016/j.watres.2006.04.036
Kinney, 2008, Bioaccumulation of pharmaceuticals and other anthropogenic waste indicators in earthworms from agricultural soil amended with biosolid or swine manure, Environ Sci Technol, 42, 1863, 10.1021/es702304c
Fick, 2009, Contamination of surface, ground, and drinking water from pharmaceutical production, Environ Toxicol Chem, 28, 2522, 10.1897/09-073.1
Dougherty, 2010, Occurrence of herbicides and pharmaceutical and personal care products in surface water and groundwater around Liberty Bay, Puget Sound, Washington, J Environ Qual, 39, 1173, 10.2134/jeq2009.0189
Metcalfe, 2003, Distribution of acidic and neutral drugs in surface waters near sewage treatment plants in the lower Great Lakes, Environ Toxicol Chem, 22, 2881, 10.1897/02-627
Glassmeyer, 2005, Transport of chemical and microbial compounds from known wastewater discharges: Potential for use as indicators of human fecal contamination, Environ Sci Technol, 39, 5157, 10.1021/es048120k
Khetan, 2007, Human pharmaceuticals in the aquatic environment: A challenge to green chemistry, Chem Rev, 107, 2319, 10.1021/cr020441w
Maruya, 2014, 334
Thomas, 2005, Tracking acidic pharmaceuticals, caffeine, and triclosan through the wastewater treatment process, Environ Toxicol Chem, 24, 25, 10.1897/04-144R.1
Conn, 2006, Occurrence and fate of organic contaminants during onsite wastewater treatment, Environ Sci Technol, 40, 7358, 10.1021/es0605117
Godfrey, 2007, Pharmaceuticals in on-site sewage effluent and ground water, western Montana, Ground Water, 45, 263, 10.1111/j.1745-6584.2006.00288.x
Carrara, 2008, Fate of pharmaceutical and trace organic compounds in three septic system plumes, Ontario, Canada, Environ Sci Technol, 42, 2805, 10.1021/es070344q
Swartz, 2006, Steroid estrogens, nonylphenolethoxylate metabolites, and other wastewater contaminants in groundwater affected by a residential septic system on Cape Cod, MA, Environ Sci Technol, 40, 4894, 10.1021/es052595+
Standley, 2008, Wastewater-contaminated groundwater as a source of endogenous hormones and pharmaceuticals to surface water ecosystems, Environ Toxicol Chem, 27, 2457, 10.1897/07-604.1
Agunbiade, 2014, Pharmaceuticals as emerging organic contaminants in Umgeni River water system, KwaZulu-Natal, South Africa, Environ Monit Assess, 186, 7273, 10.1007/s10661-014-3926-z
Manickum, 2014, 584
Statistics South Africa., 2012
Umgeni Water., 2011
American Public Health Association., 2005
Lindqvist, 2005, Occurrence of acidic pharmaceuticals in raw and treated sewages and in receiving waters, Water Res, 39, 2219, 10.1016/j.watres.2005.04.003
Castiglioni, 2005, A multiresidue analytical method using solid-phase extraction and high-pressure liquid chromatography tandem mass spectrometry to measure pharmaceuticals of different therapeutic classes in urban wastewaters, J Chromatogr A, 1092, 206, 10.1016/j.chroma.2005.07.012
Yang, 2005, Simultaneous extraction and analysis of 11 tetracycline and sulfonamide antibiotics in influent and effluent domestic wastewater by solid-phase extraction and liquid chromatography-electrospray ionization tandem mass spectrometry, J Chromatogr A, 1097, 40, 10.1016/j.chroma.2005.08.027
Pedrouzo, 2009, Estrogens and their conjugates: Determination in water samples by solid-phase extraction and liquid chromatography-tandem mass spectrometry, Talanta, 78, 1327, 10.1016/j.talanta.2009.02.005
Salvia, 2012, Development of a multi-residue method using acetonitrile-based extraction followed by liquid chromatography-tandem mass spectrometry for the analysis of steroids and veterinary and human drugs at trace levels in soil, J Chromatogr A, 1245, 122, 10.1016/j.chroma.2012.05.034
Metcalfe, 2003, Occurrence of neutral and acidic drugs in the effluents of Canadian sewage treatment plants, Environ Toxicol Chem, 22, 2872, 10.1897/02-469
Huschek, 2004, Environmental risk assessment of medicinal products for human use according to European Commission recommendations, Environ Toxicol, 19, 226, 10.1002/tox.20015
Ternes, 2004, A rapid method to measure the solid-water distribution coefficient (K-d) for pharmaceuticals and musk fragrances in sewage sludge, Water Res, 3819, 4075, 10.1016/j.watres.2004.07.015
Ferrari, 2003, Ecotoxicological impact of pharmaceuticals found in treated wastewaters: Study of carbamazepine, clofibricacid, and diclofenac, Ecotox Environ Safe, 55, 359, 10.1016/S0147-6513(02)00082-9
Rabiet, 2006, Consequences of treated water recycling as regards pharmaceuticals and drugs in surface and ground waters of a medium-sized Mediterranean Catchment, Environ Sci Technol, 40, 5282, 10.1021/es060528p
Watkinson, 2009, The occurrence of antibiotics in an urban watershed: From wastewater to drinking water, Sci Total Environ, 407, 2711, 10.1016/j.scitotenv.2008.11.059
Hartmann, 1998, Identification of fluoroquinolone antibiotics as the main source of umuC genotoxicity in native hospital wastewater, Environ Toxicol Chem, 17, 377, 10.1897/1551-5028(1998)017<0377:IOFAAT>2.3.CO;2
Department of Health, South Africa., 2003
Mohlala, 2010, Drug prescription habits in public and private health facilities in 2 provinces in South Africa, Eastern Medit Heal J, 16, 324, 10.26719/2010.16.3.324
Rodil, 2009, Multi-residue analytical method for the determination of emerging pollutants in water by solid-phase extraction and liquid chromatography-tandem mass spectrometry, J Chromatogr A, 1216, 2958, 10.1016/j.chroma.2008.09.041
Sringernyuang, 2000
Watanabe, 2010, Use and environmental occurrence of antibiotics in free stall dairy farms with manure forage fields, Environ Sci Technol, 44, 6591, 10.1021/es100834s
Ellis, 2006, Pharmaceutical and personal care products (PPCPs) in urban receiving waters, Environ Pollut, 144, 184, 10.1016/j.envpol.2005.12.018
Loos, 2009, EU-wide survey of polar organic persistent pollutants in European river waters, Environ Pollut, 157, 561, 10.1016/j.envpol.2008.09.020
Kolpin, 2002, Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999-2000: A national reconnaissance, Environ Sci Technol, 36, 1202, 10.1021/es011055j
Batt, 2006, Evaluating the vulnerability of surface waters to antibiotic contamination from varying wastewater treatment plant discharges, Environ Pollut, 142, 295, 10.1016/j.envpol.2005.10.010
Yan, 2013, Antibiotics in the surface water of the Yangtze Estuary: Occurrence, distribution and risk assessment, Environ Pollut, 175, 22, 10.1016/j.envpol.2012.12.008
Gurr, 2006, Harnessing natural attenuation of pharmaceuticals and hormones in rivers, Environ Sci Technol, 40, 2872, 10.1021/es062677d
Glassmeyer, 2008
Boxall, 2008