Contaminant Exposure and Transport from Three Potential Reuse Waters within a Single Watershed.

Global demand for safe and sustainable water supplies necessitates a better understanding of contaminant exposures in potential reuse waters. In this study, we compared exposures and load contributions to surface water from the discharge of three reuse waters (wastewater effluent, urban stormwater, and agricultural runoff). Results document substantial and varying organic-chemical contribution to surface water from effluent discharges (e.g., disinfection byproducts [DBP], prescription pharmaceuticals, industrial/household chemicals), urban stormwater (e.g., polycyclic aromatic hydrocarbons, pesticides, nonprescription pharmaceuticals), and agricultural runoff (e.g., pesticides). Excluding DBPs, episodic storm-event organic concentrations and loads from urban stormwater were comparable to and often exceeded those of daily wastewater-effluent discharges. We also assessed if wastewater-effluent irrigation to corn resulted in measurable effects on organic-chemical concentrations in rain-induced agricultural runoff and harvested feedstock. Overall, the target-organic load of 491 g from wastewater-effluent irrigation to the study corn field during the 2019 growing season did not produce substantial dissolved organic-contaminant contributions in subsequent rain-induced runoff events. Out of the 140 detected organics in source wastewater-effluent irrigation, only imidacloprid and estrone had concentrations that resulted in observable differences between rain-induced agricultural runoff from the effluent-irrigated and nonirrigated corn fields. Analyses of pharmaceuticals and per-/polyfluoroalkyl substances in at-harvest corn-plant samples detected two prescription antibiotics, norfloxacin and ciprofloxacin, at concentrations of 36 and 70 ng/g, respectively, in effluent-irrigated corn-plant samples; no contaminants were detected in noneffluent irrigated corn-plant samples.

Food, Beverage, and Feedstock Processing Facility Wastewater: a Unique and Underappreciated Source of Contaminants to U.S. Streams.

Process wastewaters from food, beverage, and feedstock facilities, although regulated, are an under-investigated environmental contaminant source. Food process wastewaters (FPWWs) from 23 facilities in 17 U.S. states were sampled and documented for a plethora of chemical and microbial contaminants. Of the 576 analyzed organics, 184 (32%) were detected at least once, with concentrations as large as 143 µg L-1 (6:2 fluorotelomer sulfonic acid), and as many as 47 were detected in a single FPWW sample. Cumulative per/polyfluoroalkyl substance concentrations up to 185 µg L-1 and large pesticide transformation product concentrations (e.g., methomyl oxime, 40 µg L-1; clothianidin TMG, 2.02 µg L-1) were observed. Despite 48% of FPWW undergoing disinfection treatment prior to discharge, bacteria resistant to third-generation antibiotics were found in each facility type, and multiple bacterial groups were detected in all samples, including total coliforms. The exposure-activity ratios and toxicity quotients exceeded 1.0 in 13 and 22% of samples, respectively, indicating potential biological effects and toxicity to vertebrates and invertebrates associated with the discharge of FPWW. Organic contaminant profiles of FPWW differed from previously reported contaminant profiles of municipal effluents and urban storm water, indicating that FPWW is another important source of chemical and microbial contaminant mixtures discharged into receiving surface waters.

Urban Stormwater: An Overlooked Pathway of Extensive Mixed Contaminants to Surface and Groundwaters in the United States.

Increasing global reliance on stormwater control measures to reduce discharge to surface water, increase groundwater recharge, and minimize contaminant delivery to receiving waterbodies necessitates improved understanding of stormwater-contaminant profiles. A multiagency study of organic and inorganic chemicals in urban stormwater from 50 runoff events at 21 sites across the United States demonstrated that stormwater transports substantial mixtures of polycyclic aromatic hydrocarbons, bioactive contaminants (pesticides and pharmaceuticals), and other organic chemicals known or suspected to pose environmental health concern. Numerous organic-chemical detections per site (median number of chemicals detected = 73), individual concentrations exceeding 10 000 ng/L, and cumulative concentrations up to 263 000 ng/L suggested concern for potential environmental effects during runoff events. Organic concentrations, loads, and yields were positively correlated with impervious surfaces and highly developed urban catchments. Episodic storm-event organic concentrations and loads were comparable to and often exceeded those of daily wastewater plant discharges. Inorganic chemical concentrations were generally dilute in concentration and did not exceed chronic aquatic life criteria. Methylmercury was measured in 90% of samples with concentrations that ranged from 0.05 to 1.0 ng/L.

Reconnaissance of Mixed Organic and Inorganic Chemicals in Private and Public Supply Tapwaters at Selected Residential and Workplace Sites in the United States.

Safe drinking water at the point-of-use (tapwater, TW) is a United States public health priority. Multiple lines of evidence were used to evaluate potential human health concerns of 482 organics and 19 inorganics in TW from 13 (7 public supply, 6 private well self-supply) home and 12 (public supply) workplace locations in 11 states. Only uranium (61.9 µg L-1, private well) exceeded a National Primary Drinking Water Regulation maximum contaminant level (MCL: 30 µg L-1). Lead was detected in 23 samples (MCL goal: zero). Seventy-five organics were detected at least once, with median detections of 5 and 17 compounds in self-supply and public supply samples, respectively (corresponding maxima: 12 and 29). Disinfection byproducts predominated in public supply samples, comprising 21% of all detected and 6 of the 10 most frequently detected. Chemicals designed to be bioactive (26 pesticides, 10 pharmaceuticals) comprised 48% of detected organics. Site-specific cumulative exposure-activity ratios (∑EAR) were calculated for the 36 detected organics with ToxCast data. Because these detections are fractional indicators of a largely uncharacterized contaminant space, ∑EAR in excess of 0.001 and 0.01 in 74 and 26% of public supply samples, respectively, provide an argument for prioritized assessment of cumulative effects to vulnerable populations from trace-level TW exposures.

Municipal Solid Waste Landfills Harbor Distinct Microbiomes.

Landfills are the final repository for most of the discarded material from human society and its "built environments." Microorganisms subsequently degrade this discarded material in the landfill, releasing gases (largely CH4 and CO2) and a complex mixture of soluble chemical compounds in leachate. Characterization of "landfill microbiomes" and their comparison across several landfills should allow the identification of environmental or operational properties that influence the composition of these microbiomes and potentially their biodegradation capabilities. To this end, the composition of landfill microbiomes was characterized as part of an ongoing USGS national survey studying the chemical composition of leachates from 19 non-hazardous landfills across 16 states in the continental U.S. The landfills varied in parameters such as size, waste composition, management strategy, geography, and climate zone. The diversity and composition of bacterial and archaeal populations in leachate samples were characterized by 16S rRNA gene sequence analysis, and compared against a variety of physical and chemical parameters in an attempt to identify their impact on selection. Members of the Epsilonproteobacteria, Gammaproteobacteria, Clostridia, and candidate division OP3 were the most abundant. The distribution of the observed phylogenetic diversity could best be explained by a combination of variables and was correlated most strongly with the concentrations of chloride and barium, rate of evapotranspiration, age of waste, and the number of detected household chemicals. This study illustrates how leachate microbiomes are distinct from those of other natural or built environments, and sheds light on the major selective forces responsible for this microbial diversity.

Landfill leachate as a mirror of today's disposable society: Pharmaceuticals and other contaminants of emerging concern in final leachate from landfills in the conterminous United States.

Final leachates (leachate after storage or treatment processes) from 22 landfills in 12 states were analyzed for 190 pharmaceuticals and other contaminants of emerging concern (CECs), which were detected in every sample, with the number of CECs ranging from 1 to 58 (median = 22). In total, 101 different CECs were detected in leachate samples, including 43 prescription pharmaceuticals, 22 industrial chemicals, 15 household chemicals, 12 nonprescription pharmaceuticals, 5 steroid hormones, and 4 animal/plant sterols. The most frequently detected CECs were lidocaine (91%, local anesthetic), cotinine (86%, nicotine degradate), carisoprodol (82%, muscle relaxant), bisphenol A (77%, component of plastics and thermal paper), carbamazepine (77%, anticonvulsant), and N,N-diethyltoluamide (68%, insect repellent). Concentrations of CECs spanned 7 orders of magnitude, ranging from 2.0 ng/L (estrone) to 17,200,000 ng/L (bisphenol A). Concentrations of household and industrial chemicals were the greatest (∼1000-1,000,000 ng/L), followed by plant/animal sterols (∼1000-100,000 ng/L), nonprescription pharmaceuticals (∼100-10,000 ng/L), prescription pharmaceuticals (∼10-10,000 ng/L), and steroid hormones (∼10-100 ng/L). The CEC concentrations in leachate from active landfills were significantly greater than those in leachate from closed, unlined landfills (p = 0.05). The CEC concentrations were significantly greater (p < 0.01) in untreated leachate compared with treated leachate. The CEC concentrations were significantly greater in leachate disposed to wastewater treatment plants from modern lined landfills than in leachate released to groundwater from closed, unlined landfills (p = 0.04). The CEC concentrations were significantly greater (p = 0.06) in the fresh leachate (leachate before storage or treatment) reported in a previous study compared with the final leachate sampled for the present study.

Contaminants of emerging concern in fresh leachate from landfills in the conterminous United States.

To better understand the composition of contaminants of emerging concern (CECs) in landfill leachate, fresh leachate from 19 landfills was sampled across the United States during 2011. The sampled network included 12 municipal and 7 private landfills with varying landfill waste compositions, geographic and climatic settings, ages of waste, waste loads, and leachate production. A total of 129 out of 202 CECs were detected during this study, including 62 prescription pharmaceuticals, 23 industrial chemicals, 18 nonprescription pharmaceuticals, 16 household chemicals, 6 steroid hormones, and 4 plant/animal sterols. CECs were detected in every leachate sample, with the total number of detected CECs in samples ranging from 6 to 82 (median = 31). Bisphenol A (BPA), cotinine, and N,N-diethyltoluamide (DEET) were the most frequently detected CECs, being found in 95% of the leachate samples, followed by lidocaine (89%) and camphor (84%). Other frequently detected CECs included benzophenone, naphthalene, and amphetamine, each detected in 79% of the leachate samples. CEC concentrations spanned six orders of magnitude, ranging from ng L(-1) to mg L(-1). Industrial and household chemicals were measured in the greatest concentrations, composing more than 82% of the total measured CEC concentrations. Maximum concentrations for three household and industrial chemicals, para-cresol (7 020 000 ng L(-1)), BPA (6 380 000 ng L(-1)), and phenol (1 550 000 ng L(-1)), were the largest measured, with these CECs composing 70% of the total measured CEC concentrations. Nonprescription pharmaceuticals represented 12%, plant/animal sterols 4%, prescription pharmaceuticals 1%, and steroid hormones <1% of the total measured CEC concentrations. Leachate from landfills in areas receiving greater amounts of precipitation had greater frequencies of CEC detections and concentrations in leachate than landfills receiving less precipitation.

GeoChip-based analysis of microbial functional gene diversity in a landfill leachate-contaminated aquifer.

The functional gene diversity and structure of microbial communities in a shallow landfill leachate-contaminated aquifer were assessed using a comprehensive functional gene array (GeoChip 3.0). Water samples were obtained from eight wells at the same aquifer depth immediately below a municipal landfill or along the predominant downgradient groundwater flowpath. Functional gene richness and diversity immediately below the landfill and the closest well were considerably lower than those in downgradient wells. Mantel tests and canonical correspondence analysis (CCA) suggested that various geochemical parameters had a significant impact on the subsurface microbial community structure. That is, leachate from the unlined landfill impacted the diversity, composition, structure, and functional potential of groundwater microbial communities as a function of groundwater pH, and concentrations of sulfate, ammonia, and dissolved organic carbon (DOC). Historical geochemical records indicate that all sampled wells chronically received leachate, and the increase in microbial diversity as a function of distance from the landfill is consistent with mitigation of the impact of leachate on the groundwater system by natural attenuation mechanisms.

Impact of geochemical stressors on shallow groundwater quality.

Groundwater monitoring wells (about 70 wells) were extensively installed in 28 sites surrounding Lake Texoma, located on the border of Oklahoma and Texas, to assess the impact of geochemical stressors to shallow groundwater quality. The monitoring wells were classified into three groups (residential area, agricultural area, and oil field area) depending on their land uses. During a 2-year period from 1999 to 2001 the monitoring wells were sampled every 3 months on a seasonal basis. Water quality assay consisted of 25 parameters including field parameters, nutrients, major ions, and trace elements. Occurrence and level of inorganics in groundwater samples were related to the land use and temporal change. Groundwater of the agricultural area showed lower levels of ferrous iron and nitrate than the residential area. The summer season data revealed more distinct differences in inorganic profiles of the two land use groundwater samples. There is a possible trend that nitrate concentrations in groundwater increased as the proportions of cultivated area increased. Water-soluble ferrous iron occurred primarily in water samples with a low dissolved oxygen concentration and/or a negative redox potential. The presence of brine waste in shallow groundwater was detected by chloride and conductivity in oil field area. Dissolved trace metals and volatile organic carbons were not in a form of concentration to be stressors. This study showed that the quality of shallow ground water could be related to regional geochemical stressors surrounding the lake.

Groundwater quality surrounding Lake Texoma during short-term drought conditions.

Water quality data from 55 monitoring wells during drought conditions surrounding Lake Texoma, located on the border of Oklahoma and Texas, was compared to assess the influence of drought on groundwater quality. During the drought month of October, water table levels were three feet (0.9 m) lower compared with several months earlier under predrought climate conditions. Detection frequencies of nitrate (> 0.1 mg/l), orthophosphates (> 0.1 mg/l), chlorides (> MCL), and sulfates (> MCL) all increased during drought. Orthophosphate level was higher during drought. Largest increases in concentration were nitrate under both agriculture lands and in septic tank areas. An increase in ammonium-nitrogen was only detected in the septic tank area. The study showed that stressors such as nitrate and total salts could potentially become a health or environmental problem during drought.