Nationwide reconnaissance of contaminants of emerging concern in source and treated drinking waters of the United States: Pharmaceuticals.
ABSTRACT: Mobile and persistent chemicals that are present in urban wastewater, such as pharmaceuticals, may survive on-site or municipal wastewater treatment and post-discharge environmental processes. These pharmaceuticals have the potential to reach surface and groundwaters, essential drinking-water sources. A joint, two-phase U.S. Geological Survey-U.S. Environmental Protection Agency study examined source and treated waters from 25 drinking-water treatment plants from across the United States. Treatment plants that had probable wastewater inputs to their source waters were selected to assess the prevalence of pharmaceuticals in such source waters, and to identify which pharmaceuticals persist through drinking-water treatment. All samples were analyzed for 24 pharmaceuticals in Phase I and for 118 in Phase II. In Phase I, 11 pharmaceuticals were detected in all source-water samples, with a maximum of nine pharmaceuticals detected in any one sample. The median number of pharmaceuticals for all 25 samples was five. Quantifiable pharmaceutical detections were fewer, with a maximum of five pharmaceuticals in any one sample and a median for all samples of two. In Phase II, 47 different pharmaceuticals were detected in all source-water samples, with a maximum of 41 pharmaceuticals detected in any one sample. The median number of pharmaceuticals for all 25 samples was eight. For 37 quantifiable pharmaceuticals in Phase II, median concentrations in source water were below 113ng/L. For both Phase I and Phase II campaigns, substantially fewer pharmaceuticals were detected in treated water samples than in corresponding source-water samples. Seven different pharmaceuticals were detected in all Phase I treated water samples, with a maximum of four detections in any one sample and a median of two pharmaceuticals for all samples. In Phase II a total of 26 different pharmaceuticals were detected in all treated water samples, with a maximum of 20 pharmaceuticals detected in any one sample and a median of 2 pharmaceuticals detected for all 25 samples. Source-water type influences the presence of pharmaceuticals in source and treated water. Treatment processes appear effective in reducing concentrations of most pharmaceuticals. Pharmaceuticals more consistently persisting through treatment include carbamazepine, bupropion, cotinine, metoprolol, and lithium. Pharmaceutical concentrations and compositions from this study provide an important base data set for further sublethal, long-term exposure assessments, and for understanding potential effects of these and other contaminants of emerging concern upon human and ecosystem health.
Project description:The widespread utilization of organic compounds in modern society and their dispersion through wastewater have resulted in extensive contamination of source and drinking waters. The vast majority of these compounds are not regulated in wastewater outfalls or in drinking water while trace amounts of certain compounds can impact aquatic wildlife. Hence it is prudent to monitor these contaminants in water sources until sufficient toxicological data relevant to humans becomes available. A method was developed for the analysis of 36 trace organic contaminants (TOrCs) including pharmaceuticals, pesticides, steroid hormones (androgens, progestins, and glucocorticoids), personal care products and polyfluorinated compounds (PFCs) using a single solid phase extraction (SPE) technique with ultra-high performance liquid chromatography coupled to tandem mass spectrometry (UHPLC-MS/MS). The method was applied to a variety of water matrices to demonstrate method performance and reliability.UHPLC-MS/MS in both positive and negative electrospray ionization (ESI) modes was employed to achieve optimum sensitivity while reducing sample analysis time (<20 min) compared with previously published methods. The detection limits for most compounds was lower than 1.0 picogram on the column while reporting limits in water ranged from 0.1 to 15 ng/L based on the extraction of a 1 L sample and concentration to 1 mL. Recoveries in ultrapure water for most compounds were between 90-110%, while recoveries in surface water and wastewater were in the range of 39-121% and 38-141% respectively. The analytical method was successfully applied to analyze samples across several different water matrices including wastewater, groundwater, surface water and drinking water at different stages of the treatment. Among several compounds detected in wastewater, sucralose and TCPP showed the highest concentrations.The proposed method is sensitive, rapid and robust; hence it can be used to analyze a large variety of trace organic compounds in different water matrixes.
Project description:When chemical or microbial contaminants are assessed for potential effect or possible regulation in ambient and drinking waters, a critical first step is determining if the contaminants occur and if they are at concentrations that may cause human or ecological health concerns. To this end, source and treated drinking water samples from 29 drinking water treatment plants (DWTPs) were analyzed as part of a two-phase study to determine whether chemical and microbial constituents, many of which are considered contaminants of emerging concern, were detectable in the waters. Of the 84 chemicals monitored in the 9 Phase I DWTPs, 27 were detected at least once in the source water, and 21 were detected at least once in treated drinking water. In Phase II, which was a broader and more comprehensive assessment, 247 chemical and microbial analytes were measured in 25 DWTPs, with 148 detected at least once in the source water, and 121 detected at least once in the treated drinking water. The frequency of detection was often related to the analyte's contaminant class, as pharmaceuticals and anthropogenic waste indicators tended to be infrequently detected and more easily removed during treatment, while per and polyfluoroalkyl substances and inorganic constituents were both more frequently detected and, overall, more resistant to treatment. The data collected as part of this project will be used to help inform evaluation of unregulated contaminants in surface water, groundwater, and drinking water.
Project description:Despite the fact that there are tens of thousands of thermal baths in existence, knowledge about the occurrence of pharmaceutically active compounds (PhACs) in untreated thermal wastewater is very limited. Because used thermal water is typically legally discharged into surface waters without any treatment, the effluent poses environmental risks for the receiving water bodies. The aim of this study was to show the occurrence patterns and spatiotemporal characteristics of 111 PhACs in thermal wastewater. Six thermal water outflows of different thermal baths were tested in different seasons in the Budapest metropolitan region (Hungary), and diurnal analysis was performed. After solid-phase extraction, the samples were analysed and quantified by coupling supercritical fluid chromatography and mass spectrometry to perform simultaneous multi-residue drug analysis. The results confirm that water discharge pipes directly transport pharmaceuticals into surface water bodies; 34 PhACs were measured to be over the limit of quantification at least once, and 21 of them were found in more than one water sample. The local anaesthetic drug lidocaine, antiepileptic carbamazepine, analgesic derivative tramadol and illicit drug cocaine were detected in more than half of the samples. Caffeine, metoprolol and bisoprolol (cardiovascular drugs), benzoylecgonine (cocaine metabolite), diclofenac (NSAID), citalopram (antidepressant) and certain types of hormones also have a significant frequency of 30-50%. However, the occurrence and concentrations of PhACs vary according to the season and number/types of visitors. As demonstrated by the diurnal fluctuation, drug contamination of thermal waters can significantly vary, even for similar types of baths; furthermore, the quantity and types of some pollutants rapidly change in the discharged thermal wastewater.
Project description:The occurrence and fate of pharmaceutical and personal care products in the environment are of increasing public importance because of their ubiquitous nature and documented effects on wildlife, ecosystems, and potentially humans. One potential, yet undefined, source of entry of pharmaceuticals into the environment is via the land application of municipal wastewater onto permitted lands. The objective of the present study is to determine the extent to which pharmaceuticals are mitigated by or exported from managed tree plantations irrigated with municipal wastewater. A specific focus of the present study is the presence of pharmaceutical compounds in groundwater and surface water discharge. The study site is a municipality that land-applies secondary treated wastewater onto 930 hectares of a 2000-hectare managed hardwood and pine plantation. A suite of 33 pharmaceuticals and steroid hormones was targeted in the analysis, which consisted of monthly grab sampling of groundwater, surface water, and wastewater, followed by concentration and cleanup via solid phase extraction and separation, detection, and quantification via liquid chromatography coupled with tandem mass spectrometry. More than one-half of all compounds detected in irrigated wastewater were not present in groundwater and subsequent surface water. However, antibiotics, nonsteroidal anti-inflammatory drugs, caffeine, and other prescription and over-the-counter drugs remained in groundwater and were transported into surface water at concentrations up to 10 ng/L. These results provide important documentation for pharmaceutical fate and transport in forest systems irrigated with municipal wastewater, a previously undocumented source of environmental entry.
Project description:Facilities involved in the manufacture of pharmaceutical products are an under-investigated source of pharmaceuticals to the environment. Between 2004 and 2009, 35 to 38 effluent samples were collected from each of three wastewater treatment plants (WWTPs) in New York and analyzed for seven pharmaceuticals including opioids and muscle relaxants. Two WWTPs (NY2 and NY3) receive substantial flows (>20% of plant flow) from pharmaceutical formulation facilities (PFF) and one (NY1) receives no PFF flow. Samples of effluents from 23 WWTPs across the United States were analyzed once for these pharmaceuticals as part of a national survey. Maximum pharmaceutical effluent concentrations for the national survey and NY1 effluent samples were generally <1 microg/L. Four pharmaceuticals (methadone, oxycodone, butalbital, and metaxalone) in samples of NY3 effluent had median concentrations ranging from 3.4 to >400 microg/L. Maximum concentrations of oxycodone (1700 microg/L) and metaxalone (3800 microg/L) in samples from NY3 effluent exceeded 1000 microg/L. Three pharmaceuticals (butalbital, carisoprodol, and oxycodone) in samples of NY2 effluent had median concentrations ranging from 2 to 11 microg/L. These findings suggest that current manufacturing practices at these PFFs can result in pharmaceuticals concentrations from 10 to 1000 times higher than those typically found in WWTP effluents.
Project description:Utility vaults and underground structures house essential telecommunications, gas, and electric al infrastructure (e.g., transformers, copper wiring) that could contaminate water which accumulates in them. Water is removed from utility vaults during routine infrastructure maintenance. That water is typically released to the storm drain system, raising concerns that polluted water could reach receiving waters. However, no one has measured pollutants in utility vault water. The State Water Resources Control Board (SWRCB) has mandated such measurements as a condition of renewing the National Pollutant Discharge Elimination System Utility Vault Permit. We analyzed 126 priority pollutants in 20 utility vault water samples collected throughout California by Pacific Gas and Electric Company (PG&E). We also estimated the volume of utility vault water discharged and calculated loads. Twenty-one priority pollutants were detected. Metals were commonly found. Only copper (Cu) and zinc (Zn) exceeded water quality criteria. Their maximum concentrations were 791 and 386 ?g/L, respectively. Median Cu and Zn concentrations of 9.66 and 81.6 ?g/L were representative of urban stormwater, suggesting runoff is a source of metals in utility vault water. For San Francisco Bay, Cu and Zn loads from PG&E's utility vault water (0.06 and 0.5 kg/year) were inconsequential compared to previously reported total loads (74,000 and 320,000 kg/year) from stormwater, wastewater treatment plants, etc. For California, utility vault water loads were 5 and 40 kg/year of Cu and Zn. We are the first to report pollutant concentrations in utility vault water. Utility vaults are not a major source of pollutants to receiving waters.
Project description:Potential risks associated with releases of human pharmaceuticals into the environment have become an increasingly important issue in environmental health. This concern has been driven by the widespread detection of pharmaceuticals in all aquatic compartments. Therefore, 22 pharmaceuticals, 6 metabolites and transformation products, belonging to 7 therapeutic groups, were selected to perform a systematic review on their source, fate and occurrence in different aquatic compartments, important issues to tackle the Water Framework Directive (WFD). The results obtained evidence that concentrations of pharmaceuticals are present, in decreasing order, in wastewater influents (WWIs), wastewater effluents (WWEs) and surface waters, with values up to 14 mg L<sup>-1</sup> for ibuprofen in WWIs. The therapeutic groups which presented higher detection frequencies and concentrations were anti-inflammatories, antiepileptics, antibiotics and lipid regulators. These results present a broad and specialized background, enabling a complete overview on the occurrence of pharmaceuticals in the aquatic compartments.
Project description:To better characterize Cryptosporidium in the Potomac River watershed, a PCR-based genotyping tool was used to analyze 64 base flow and 28 storm flow samples from five sites in the watershed. These sites included two water treatment plant intakes, as well as three upstream sites, each associated with a different type of land use. The uses, including urban wastewater, agricultural (cattle) wastewater, and wildlife, posed different risks in terms of the potential contribution of Cryptosporidium oocysts to the source water. Cryptosporidium was detected in 27 base flow water samples and 23 storm flow water samples. The most frequently detected species was C. andersoni (detected in 41 samples), while 14 other species or genotypes, almost all wildlife associated, were occasionally detected. The two common human-pathogenic species, C. hominis and C. parvum, were not detected. Although C. andersoni was common at all four sites influenced by agriculture, it was largely absent at the urban wastewater site. There were very few positive samples as determined by Environmental Protection Agency method 1623 at any site; only 8 of 90 samples analyzed (9%) were positive for Cryptosporidium as determined by microscopy. The genotyping results suggest that many of the Cryptosporidium oocysts in the water treatment plant source waters were from old calves and adult cattle and might not pose a significant risk to human health.
Project description:<h4>Background</h4>Pharmaceuticals are known to contaminate tap water worldwide, but the relevant human health risks have not been assessed in China.<h4>Objectives</h4>We monitored 32 pharmaceuticals in Chinese tap water and evaluated the life-long human health risks of exposure in order to provide information for future prioritization and risk management.<h4>Methods</h4>We analyzed samples (n = 113) from 13 cities and compared detected concentrations with existing or newly-derived safety levels for assessing risk quotients (RQs) at different life stages, excluding the prenatal stage.<h4>Results</h4>We detected 17 pharmaceuticals in 89% of samples, with most detectable concentrations (92%) at < 50 ng/L. Caffeine (median-maximum, nanograms per liter: 24.4-564), metronidazole (1.8-19.3), salicylic acid (16.6-41.2), clofibric acid (1.2-3.3), carbamazepine (1.3-6.7), and dimetridazole (6.9-14.7) were found in ? 20% of samples. Cities within the Yangtze River region and Guangzhou were regarded as contamination hot spots because of elevated levels and frequent positive detections. Of the 17 pharmaceuticals detected, 13 showed very low risk levels, but 4 (i.e., dimetridazole, thiamphenicol, sulfamethazine, and clarithromycin) were found to have at least one life-stage RQ ? 0.01, especially for the infant and child life stages, and should be considered of high priority for management. We propose an indicator-based monitoring framework for providing information for source identification, water treatment effectiveness, and water safety management in China.<h4>Conclusion</h4>Chinese tap water is an additional route of human exposure to pharmaceuticals, particularly for dimetridazole, although the risk to human health is low based on current toxicity data. Pharmaceutical detection and application of the proposed monitoring framework can be used for water source protection and risk management in China and elsewhere.
Project description:Recreational and potable water supplies polluted with human wastewater can pose a direct health risk to humans. Therefore, sensitive detection of human fecal pollution in environmental waters is very important to water quality authorities around the globe. Microbial source tracking (MST) utilizes human fecal markers (HFMs) to detect human wastewater pollution in environmental waters. The concentrations of these markers in raw wastewater are considered important because it is likely that a marker whose concentration is high in wastewater will be more frequently detected in polluted waters. In this study, quantitative PCR (qPCR) assays were used to determine the concentrations of fecal indicator bacteria (FIB) Escherichia coli and Enterococcus spp., HFMs Bacteroides HF183, human adenoviruses (HAdVs), and polyomaviruses (HPyVs) in raw municipal wastewater influent from various climatic zones in Australia. E. coli mean concentrations in pooled human wastewater data sets (from various climatic zones) were the highest (3.2 × 10(6) gene copies per ml), followed by those of HF183 (8.0 × 10(5) gene copies per ml) and Enterococcus spp. (3.6 × 10(5) gene copies per ml). HAdV and HPyV concentrations were 2 to 3 orders of magnitude lower than those of FIB and HF183. Strong positive and negative correlations were observed between the FIB and HFM concentrations within and across wastewater treatment plants (WWTPs). To identify the most sensitive marker of human fecal pollution, environmental water samples were seeded with raw human wastewater. The results from the seeding experiments indicated that Bacteroides HF183 was more sensitive for detecting human fecal pollution than HAdVs and HPyVs. Since the HF183 marker can occasionally be present in nontarget animal fecal samples, it is recommended that HF183 along with a viral marker (HAdVs or HPyVs) be used for tracking human fecal pollution in Australian environmental waters.