Pharmaceutical Chemicals and Endocrine Disrupters in Municipal Wastewater in Tokyo and Their Removal During Activated Sludge Treatment

Laboratory of Organic Geochemistry (LOG), Institute of Symbiotic Science and Technology, Tokyo University of Agriculture and Technology, Fuchu, Tokyo 183-8509, Japan.
Water Research (Impact Factor: 5.53). 11/2006; 40(17):3297-303. DOI: 10.1016/j.watres.2006.06.039
Source: PubMed


We measured six acidic analgesics or anti-inflammatories (aspirin, ibuprofen, naproxen, ketoprofen, fenoprofen, mefenamic acid), two phenolic antiseptics (thymol, triclosan), four amide pharmaceuticals (propyphenazone, crotamiton, carbamazepine, diethyltoluamide), three phenolic endocrine disrupting chemicals (nonylphenol, octylphenol, bisphenol A), and three natural estrogens (17beta-estradiol, estrone, estriol) in 24-h composite samples of influents and secondary effluents collected seasonally from five municipal sewage treatment plants in Tokyo. Aspirin was most abundant in the influent, with an average concentration of 7300 ng/L (n = 16), followed by crotamiton (921 ng/L), ibuprofen (669 ng/L), triclosan (511 ng/L), and diethyltoluamide (503 ng/L). These concentrations were 1 order of magnitude lower than those reported in the USA and Europe. This can be ascribed to lower consumption of the pharmaceuticals in Japan. Aspirin, ibuprofen, and thymol were removed efficiently during primary + secondary treatment (> 90% efficiency). On the other hand, amide-type pharmaceuticals, ketoprofen, and naproxen showed poor removal (< 50% efficiency), which is probably due to their lower hydrophobicity (logKow < 3). Because of the persistence of crotamiton during secondary treatment, crotamiton was most abundant among the target pharmaceuticals in the effluent. This is the first paper to report ubiquitous occurrence of crotamiton, a scabicide, in sewage. Because crotamiton is used worldwide and it is persistent during secondary treatment, it is a promising molecular marker of sewage and secondary effluent.

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    • "Pharmaceutical discharges into the aquatic ecosystem are of environmental concern (Brain et al., 2004; Daughton and Ternes, 1999; Halling-Sørensen et al., 1998; Nakada et al., 2006). On one hand, the continuous input of pharmaceutical active compounds into the water matrix from municipal effluents (ME) and waste water treatment plants (WWTP) gives them a state of pseudopersistence (Hernando et al., 2006), and on the other hand, aquatic biota might be unceasingly exposed to these active ingredients. "
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    ABSTRACT: A battery of biomarkers was evaluated on Ruditapes philippinarum exposed during 14 days to caffeine, ibuprofen, carbamazepine and novobiocin (0.1, 1, 5, 10, 15, and 50µgL(-1)). The battery included general stress (lysosomal membrane stability - LMS) analysed in the hemolymph, and biochemical biomarkers analysed in digestive gland tissues including: biomarkers of phase I (etoxyresorufin O-deethylase - EROD, dibenzylfluorescein dealkylase - DBF), phase II (gluthathione-S-transferase - GST), oxidative stress (gluthathione reductase - GR, gluthathione peroxidase - GPX, lipid peroxidation - LPO), neurotoxicity (acetylcholinesterase activity - AChE), and genotoxicity (DNA damage). Pharmaceuticals tested induced the sublethal responses (even at the environmental range 0.1µgL(-1)). At this low concentration; caffeine, ibuprofen and carbamazepine decreased the LMS significantly compared with controls (p<0.05). The four compounds induced significantly the detoxification metabolism and oxidative stress (p<0.05). Neurotoxicity was noticed in clams exposed to caffeine and carbamazepine (p<0.05). Ibuprofen, carbamazepine and novobiocin produced genotoxic effects (p<0.05). Results from this research validate the use of biomarkers when assessing the effects of pharmaceuticals within a marine environmental risk assessment framework, using as a laboratory bioassay model the species R. philippinarum.
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    • "This drug may be secreted as an unchanged molecule or as an unchanged molecule in conjugation with glucuronide (product of the second phase of detoxication that may be hydrolyzed in the environment) or as a few metabolites: hydroxyibuprofen (two isomers), carboxyibuprofen, and carboxyhydratropic acid (Halling-Sorensen et al. 1998; Buser et al. 1999; Zwiener et al. 2002). Nonetheless, little is still known about the environmental metabolism of ibuprofen, whose concentration in the environment ranges from nanograms per liter to micrograms per liter (Calamari et al. 2003; Bendz et al. 2005; Tauxe-Wuersch et al. 2005; Nakada et al. 2006; Roberts and Thomas 2006; Gómez et al. 2007; Lin et al. 2009; Pailler et al. 2009). Many reports describe only the initial steps of ibuprofen transformation. "
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    ABSTRACT: Recently, the increased use of monocyclic non-steroidal anti-inflammatory drugs has resulted in their presence in the environment. This may have potential negative effects on living organisms. The biotransformation mechanisms of monocyclic non-steroidal anti-inflammatory drugs in the human body and in other mammals occur by hydroxylation and conjugation with glycine or glucuronic acid. Biotransformation/biodegradation of monocyclic non-steroidal anti-inflammatory drugs in the environment may be caused by fungal or bacterial microorganisms. Salicylic acid derivatives are degraded by catechol or gentisate as intermediates which are cleaved by dioxygenases. The key intermediate of the paracetamol degradation pathways is hydroquinone. Sometimes, after hydrolysis of this drug, 4-aminophenol is formed, which is a dead-end metabolite. Ibuprofen is metabolized by hydroxylation or activation with CoA, resulting in the formation of isobutylocatechol. The aim of this work is to attempt to summarize the knowledge about environmental risk connected with the presence of over-the-counter anti-inflammatory drugs, their sources and the biotransformation and/or biodegradation pathways of these drugs.
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    • "A commonly prescribed medication, carbamazepine, CBZ, which is an anti-epileptic and anti-depressant was also studied in another work [18]. This compound was analyzed in influents and secondary effluents collected seasonally from five municipal sewage treatment plants in Tokyo [19], with variable concentration between 10 and 300 ng/L; with a removal efficiency of 0–80%. Average removal efficiency of the amide-type pharmaceuticals, including carbamazepine, was estimated lower than 45% by these authors. "
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    ABSTRACT: Endocrine disrupting compounds, EDCs, are somewhat recently recognized pollutants which are often classed within ‘emerging micropollutants’ in the environment jargon. These compounds are known to interfere with the delicate balance of the endocrine system of animals and man, causing variety of undesirable outcomes. Their sources in natural waters are the domestic and industrial effluents. The main cause of concern with EDCs is their tendency to accumulate in fish causing gender shifts and reduced fecundity. Moreover, their possible interference with the water cycle and concurrent effects on the human endocrine system has been implicated. Increased usage of medication and surfactants in the household; pesticides in agriculture have all add up to the inventory of EDCs in the aqueous systems.
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