Pharmaceutical residues in the river Rhine - Results of a one-decade monitoring programme

DVGW-Technologiezentrum Wasser, Karlsruher Strasse 84, 76139 Karlsruhe, Germany.
Journal of Environmental Monitoring (Impact Factor: 2.18). 06/2008; 10(5):664-70. DOI: 10.1039/b800701b
Source: PubMed


In this paper, results of an extensive monitoring programme for pharmaceutical residues in the river Rhine are presented. For one decade (1997 until 2006), the occurrence of widely used human pharmaceuticals like analgesics, lipid regulators, antiepileptics and others has been studied at four locations along the river Rhine. The results of more than 500 analyses clearly prove that compounds such as carbamazepine or diclofenac are regularly found in the river Rhine in concentrations up to several hundred ng per litre. Combining concentration levels with data on water flow enables the calculation of transports, which e.g. for carbamazepine or diclofenac were in the range of several tons per year. The evaluation of the long-term monitoring data shows that only a slight decrease in concentration levels as well as in annual transports can be observed and thus the contamination of the river Rhine by pharmaceutical residues during the last decade has to be regarded as almost constant. Seasonal variations can be detected for bezafibrate, diclofenac and ibuprofen, for which the concentrations are much lower in the summer months. A more effective removal during wastewater treatment in the warmer periods of the year seems to be the major reason for those variations. For carbamazepine, no comparable seasonal effect can be found.

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    • "Despite the worldwide release and occurrence of pharmaceutical residues in the aquatic environment, little is still known about the long-term evaluation of concentrations, especially in groundwater . Many studies deal with concentrations in effluents from wastewater treatment plants (WWTP) (Ternes and Hirsch, 2000; Bueno et al., 2012; Loos et al., 2013; Kostich et al., 2014), surface water (Schwab et al., 2005; Sacher et al., 2008; Loos et al., 2009; Vulliet and Cren-Oliv e, 2011), and groundwater (Sacher et al., 2001; Loos et al., 2010; Maeng et al., 2011; L opez-Serna et al., 2013), although most of them address single sampling campaigns. Time series data related to groundwater have been scarcely published (Wolf et al., 2012; Zemann et al., 2014) despite the fact that they can contribute significantly to a better understanding of substance behavior and long-term threads. "
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    ABSTRACT: Sewage input into a karst aquifer via leaking sewers and cesspits was investigated over five years in an urbanized catchment. Of 66 samples, analyzed for 25 pharmaceuticals, 91% indicated detectable concentrations. The former standard iodinated X-ray contrast medium (ICM) diatrizoic acid was detected most frequently. Remarkably, it was found more frequently in groundwater (79%, median: 54 ng/l) than in wastewater (21%, 120 ng/l), which is supposed to be the only source in this area. In contrast, iopamidol, a possible substitute, spread over the aquifer during the investigation period whereas concentrations were two orders of magnitude higher in wastewater than in groundwater. Knowledge about changing application of pharmaceuticals thus is essential to assess urban impacts on aquifers, especially when applying mass balances. Since correlated concentrations provide conclusive evidence that, for this catchment, nitrate in groundwater rather comes from urban than from rural sources, ICM are considered useful tracers.
    Environmental Pollution 03/2015; 198. DOI:10.1016/j.envpol.2014.11.033 · 4.14 Impact Factor
    • "Several studies proved the contamination of the aquatic environment with pharmaceuticals, for example in the rivers Rhine [8] [9] and Elbe [10] in Germany. But there are still great gaps in knowledge about the discharged drugs. "
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    ABSTRACT: Based on regional prescription data several pharmaceuticals with variable amounts of prescription and corresponding metabolites were selected and analyzed in influent and effluent samples of the sewage treatment plant (STP) in Dresden, Germany. Pharmaceuticals of the following most prescribed therapeutic groups were chosen: antibiotics, antifungals, anticonvulsants, antipsychotics, antidepressants, and cardiovascular active compounds like beta blockers and angiotensin-converting enzyme inhibitors. To analyze the selected compounds, a multi-target method was developed and applied to 24-h composite wastewater samples for three single days in May and June 2014. The method was based on a cleanup of a sample with a volume of 1mL using solid phase extraction followed by a high performance liquid chromatography coupled to a tandem mass spectrometer. Analytes were separated in a 15min chromatographic separation and quantified using 23 Internal Standards and a calibration curve in 40-fold diluted blank urine. The limit of quantification varied between 50 and 200ng/L and for all analytes good accuracy and precision as well as linearity for the calibration curve with the correlation coefficient R(2) higher than 0.99 was reached. A total of 41 and 40 of the selected 55 analytes were detected and quantified in the influent and effluent samples of the studied STP, respectively. Valsartan was the compound with the highest maximum concentration in influent (27.1μg/L) and effluent (15.7μg/L). Furthermore, analytes like bezafibrate, candesartan, carbamazepine, gabapentin, metoprolol, levetiracetam, pregabalin and telmisartan as well as the metabolite O-desmethyl venlafaxine were detectable in influent and effluent samples, respectively, with a concentration higher than 1μg/L. Copyright © 2015 Elsevier B.V. All rights reserved.
    Journal of chromatography. B, Analytical technologies in the biomedical and life sciences 03/2015; 990:23-30. DOI:10.1016/j.jchromb.2015.03.008 · 2.73 Impact Factor
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    • "Samples were never filtrated, but suspended particles were decanted before extraction. The analyses were done using an HPLC–ESI-MS–MS, the method is described in Sacher et al. (2008). Analyses were conducted within one week after arrival. "
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    ABSTRACT: The closed basin of the Lower Jordan Valley with the Dead Sea as final sink features high evapotranspiration rates and almost complete reuse of treated wastewater for irrigation farming. This study focuses on the water transfer schemes and the presence, spreading, and potential accumulation of pharmaceutical residues in the local water resources based on findings of a five-year monitoring program. Overall 16 pharmaceuticals and 9 iodinated X-ray contrast media were monitored in groundwater, surface water, and treated wastewater. A total of 95 samples were taken to cover all geographical settings and flow paths from origin (wastewater) to target (groundwater). Nine substances were detected in groundwater, with concentrations ranging between 11 ng/L and 33,000 ng/L. Sometimes, detection rates were higher than in comparable studies: Diatrizoic acid 75%, iopamidol 42%, iopromide 19%, iomeprol 11%, carbamazepine and iohexol 8%, ibuprofen 6%, and fenofibrate and iothalamic acid 3%. Concentrations in groundwater generally increase from north to south depending on the application of treated wastewater for irrigation. Almost all substances occurred most frequently and with highest concentrations in treated wastewater, followed by surface water and groundwater. As exception, diatrizoic acid was found more frequently in groundwater than in treated wastewater, with concentrations being similar. This indicates the persistence of diatrizoic acid with long residence times in local groundwater systems, but may also reflect changing prescription patterns, which would be in accordance with increasing iopamidol findings and surveys at local hospitals. Trend analyses confirm this finding and indicate a high probability of increasing iopamidol concentrations, while other substances did not reveal any trends. However, no proof of evaporative enrichment could be found. The high spatial and temporal variability of the concentrations measured calls for further systematic studies to assess the long-term evolution of organic trace substances in this reuse setting.
    Science of The Total Environment 08/2014; s 488–489:100–114. DOI:10.1016/j.scitotenv2014.04.063 · 4.10 Impact Factor
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