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Non-iodo-containing trihalomethanes (TTHM) are frequently detected in chlorinated tap water and currently regulated against their carcinogenic potential. Iodinated THM (ITHM) may also form in disinfected with chlorine waters that are high in iodine content, but little is known about their magnitude and variability within the drinking-water pipe distribution network of urban areas. The main objective of this study was to determine the magnitude and variability of ITHM and TTHM levels and their corresponding daily intake estimates within the drinking water distribution systems of Limassol and Nicosia cities of Cyprus, using tap samples collected from individual households (n=37). In Limassol, mean household tap water ITHM and TTHM levels was 0.58 and 38 μg L(-1), respectively. Dichloroiodomethane (DCIM) was the dominant species of the two measured ITHM compounds accounting for 77% of total ITHM and in the range of 0.032 and 1.65 μg L(-1). The range of DCIM concentrations in Nicosia tap water samples was narrower (0.032 - 0.848 μg L(-1)). Mean total iodine concentration in tap water samples from the seaside city of Limassol was 15 μg L(-1) and approximately twice to those observed in samples from the mainland Nicosia city. However, iodine concentrations did not correlate with the ITHM levels. The calculated chronic daily intake rates of ITHM were low when compared with those of TTHM, but because of their widespread occurrence in tap water and their enhanced mammalian cell toxicity, additional research is warranted to assess the magnitude and variability of human ITHM exposures., (Copyright © 2015 Elsevier B.V. All rights reserved.) more...

Gradually-changing shocks associated with potable water quality deficiencies are anticipated for urban drinking-water distribution systems (UDWDS). The impact of structural UDWDS features such as, the number of pipe leaking incidences on the formation of water trihalomethanes (THM) at the geocoded household level has never been studied before. The objectives were to: (i) characterize the distribution of water THM concentrations in households from two district-metered areas (DMAs) with contrasting UDWDS characteristics sampled in two seasons (summer and winter), and (ii) assess the within- and between-household, spatial variability of water THM accounting for UDWDS characteristics (household distance from chlorination tank and service pipe leaking incidences). A total of 383 tap water samples were collected from 193 households located in two DMAs within the UDWDS of Nicosia city, Cyprus, and analyzed for the four THM species. The higher intraclass correlation coefficient (ICC) values for water tribromomethane (TBM) (0.75) followed by trichloromethane (0.42) suggested that the two DMAs differed with respect to these analytes. On the other hand, the low ICC values for total THM levels between the two DMAs suggested a large variance between households. The effect of households nested under each DMA remained significant (p<0.05) for TBM (not for the rest of the THM species) in the multivariate mixed-effect models, even after inclusion of pipe network characteristics. Our results could find use by water utilities in overcoming techno-economic difficulties associated with the large spatiotemporal variability of THM, while accounting for the influence of UDWDS features at points of water use., (Copyright © 2014 Elsevier B.V. All rights reserved.) more...

Potable water samples (N = 74) from 19 zip code locations in a region of Greece were profiled for 13 trace elements composition using inductively coupled plasma mass spectrometry. The primary objective was to monitor the drinking water quality, while the primary focus was to find novel associations in trace elements occurrence that may further shed light on common links in their occurrence and fate in the pipe scales and corrosion products observed in urban drinking water distribution systems. Except for arsenic at two locations and in six samples, rest of the analyzed elements was below maximum contaminant levels, for which regulatory values are available. Further, we attempted to hierarchically cluster trace elements based on their covariances resulting in two groups; one with arsenic, antimony, zinc, cadmium, and copper and the second with the rest of the elements. The grouping trends were partially explained by elements' similar chemical activities in water, underscoring their potential for co-accumulation and co-mobilization phenomena from pipe scales into finished water. Profiling patterns of trace elements in finished water could be indicative of their load on pipe scales and corrosion products, with a corresponding risk of episodic contaminant release. Speculation was made on the role of disinfectants and disinfection byproducts in mobilizing chemically similar trace elements of human health interest from pipe scales to tap water. It is warranted that further studies may eventually prove useful to water regulators from incorporating the acquired knowledge in the drinking water safety plans. more...

Human biomonitoring studies for water contaminants are often accompanied by surveys relying solely on total drinking water consumption rates, thus, failing to account for specific water sources (bottled and tap water) and use habits, such as water used for preparing cold/hot beverages (coffee, tea, juice, etc.). Despite the extensive use of bisphenol A (BPA) in polycarbonate (PC)-based water contact materials, rarely do BPA biomonitoring studies focus on various PC water uses and sources. Better resolved water consumption rates could reduce the uncertainty associated with surrogate daily BPA intake estimates using fine-tuned surveys. This approach provided a proof of concept on inclusion of water consumption from various sources and uses into estimates of daily intake for water contaminants like BPA found in water-contact materials. The next steps would be in quantifying the extent of improvement in exposure assessment that adds value to refined survey designs. more...

Changes in disinfectant type could trigger a cascade of reactions releasing pipe-anchored metals/metalloids into finished water. However, the effect of pre-formed disinfection by-products on the release of sorbed contaminants (arsenic-As in particular) from drinking water distribution system pipe scales remains unexplored. A bench-scale study using a factorial experimental design was performed to evaluate the independent and interaction effects of trihalomethanes (TTHM) and haloacetic acids (HAA) on arsenic (As) release from either scales-only or scale-biofilm conglomerates (SBC) both anchored on asbestos/cement pipe coupons. A model biofilm (Pseudomonas aeruginosa) was allowed to grow on select pipe coupons prior experimentation. Either TTHM or HAA individual dosing did not promote As release from either scales only or SBC, detecting <6 μg AsL(-1) in finished water. In the case of scales-only coupons, the combination of the highest spike level of TTHM and HAA significantly (p<0.001) increased dissolved and total As concentrations to levels up to 16 and 95 μg L(-1), respectively. Similar treatments in the presence of biofilm (SBC) resulted in significant (p<0.001) increase in dissolved and total recoverable As up to 20 and 47 μg L(-1), respectively, exceeding the regulatory As limit. Whether or not, our laboratory-based results truly represent mechanisms operating in disinfected finished water in pipe networks remains to be investigated in the field., (Copyright © 2013 Elsevier B.V. All rights reserved.) more...

Water contamination and noise have been consistently the least assessed environmental/lifestyle exposures in pregnancy-birth cohorts (PBC). Water quality surveillance data collected during the past decade within urban drinking-water distribution systems call for re-evaluation of water and health issues in the developed world. The objectives of this scientific commentary were to (i) highlight the extent of appraisal of water contamination in exposure assessment studies of PBC, worldwide, and (ii) propose recommendations to increase awareness of emerging water-related risks through their improved representation into PBC study designs in urban centers. Three scientific literature databases (Scopus, PubMed, and Web of Science) were used for a systematic search on worldwide PBC and their publications that considered water contamination and health outcomes. Publicly-available e-databases (ENRIECO, BIRTHCOHORTS, and CHICOS) were also employed for detailed exploration of existing European Union (EU)-based PBC. Out of the 76 PBC identified in the EU territory, only 12 of them incorporated water contamination into their study designs. Among which only 6 PBC published scientific articles that either included data on water contamination and/or water intake estimates. Trihalomethanes but not other disinfection by-products were mostly studied in the PBC around the globe, while fluoride, atrazine, perfluorinated compounds, tetrachloroethylene, and lead were studied to a lesser extent as water contaminants. It appears that chemical-based water contamination and corresponding human exposures represent a largely underappreciated niche of exposure science pertaining to pregnant mother and children's health in PBC. Future PBC studies should grasp this opportunity to substantially reform elements of water contamination in their exposure assessment protocols and effectively combine them with their epidemiological study designs., (© 2013.) more...

A fast-growing bottled water market is occasionally challenged by reports calling for contaminant leaching from water-contact materials (plastics). Our focus was on leaching of antimony (Sb) and brominated compounds expressed by total soluble bromine (Br) measurements, including those of polybrominated diphenyl ethers (PBDE). Studies are lacking on concomitant leaching of two or more inorganic plastic constituents from the same bottle. A market-representative basket survey of bottled water was initiated in Boston, USA supermarkets. Bottled water classes sampled were: i) non-carbonated (NCR), ii) carbonated (CR), and iii) non-carbonated and enriched (NCRE). Plastic bottle materials sampled were: polyethylene terephthalate (PET), high-density polyethylene (HDPE), polystyrene (PS), and polycarbonate (PC). Storage conditions for the 31 bottled water samples were: 23°C temperature, no-shaking and 12h/12h light/dark for 60days of equilibration. Average Br and Sb concentrations after 60-days of storage followed the order of NCR more...

Microbial-, and chemical-based burden of disease associated with lack of access to safe water continues to primarily impact developing countries. Cost-effective health risk-mitigating measures, such as of solar disinfection applied to microbial-contaminated water stored in plastic bottles have been increasingly tested in developing countries adversely impacted by epidemic water-borne diseases. Public health concerns associated with chemical leaching from water packaging materials led us to investigate the magnitude and variability of antimony (Sb) and bromine (Br) leaching from reused plastic containers (polyethylene terephthalate, PET; and polycarbonate, PC) subject to UV and/or temperature-driven disinfection. The overall objective of this study was to determine the main and interactive effects of temperature, UV exposure duration, and frequency of bottle reuse on the extent of leaching of Sb and Br from plastic bottles into water. Regardless of UV exposure duration, frequency of reuse (up to 27 times) was the major factor that linearly increased Sb leaching from PET bottles at all temperatures tested (13-47 °C). Leached Sb concentrations (∼360 ng L(-1)) from the highly reused (27 times) PET bottles (minimal Sb leaching from PC bottles, <15 ng L(-1)) did not pose a serious risk to human health according to current daily Sb acceptable intake estimates. Leached Br concentrations from both PET and PC containers (up to ∼15 μg L(-1)) did not pose a consumer health risk either, however, no acceptable daily dose estimates exist for oral ingestion of organo-brominated, or other plasticizers/additives compounds if they were to be found in bottled water at much lower concentrations. Additional research on potential leaching of organic chemicals from water packaging materials is deemed necessary under relevant environmental conditions., (Copyright © 2011 Elsevier Ltd. All rights reserved.) more...

Background, Aim, and Scope: Organoarsenical-containing animal feeds that promote growth and resistance to parasites are mostly excreted unchanged, ending up in nearby wastewater storage lagoons. Earlier work documented the partial transformation of organoarsenicals, such as, 3-nitro-4-hydroxyphenylarsonic acid (roxarsone) to the more toxic inorganic arsenate [As(V)] and 3-amino-4-hydroxyphenylarsonic acid (3-AHPAA). Unidentified roxarsone metabolites using liquid chromatography coupled to inductively coupled plasma mass spectrometry (LC/ICP-MS) were also inferred from the corresponding As mass balance. Earlier batch experiments in our laboratory suggested the presence of organometallic (Cu) complexes during relevant roxarsone degradation experiments. We hypothesized that organocopper compounds were complexed to roxarsone, mediating its degradation in field-collected swine wastewater samples from storage lagoons. The objective of this study was to investigate the role of organometallic (Cu) complexes during roxarsone degradation under aerobic conditions in swine wastewater suspensions, using electrospray ionization mass spectrometry (ES-MS)., Materials and Methods: Two swine wastewater samples differing in % solids content and total recoverable Cu concentrations were reacted with 500 ppb of roxarsone under aerobic conditions for 16 days. LC/ICP-MS and ES-MS were used for As speciation analyses, and characterization of metal-organoarsenical complexes in swine wastewater subsamples, respectively., Results and Discussion: An organocopper roxarsone metabolite was found only in the high-Cu wastewater sample, suggesting the role of Cu in roxarsone degradation under aerobic conditions. The organocopper metabolite was not found in the low-Cu wastewater sample, because roxarsone did not undergo degradation under aerobic conditions even after 16 days., Conclusions: Aerobic degradation of organoarsenicals (roxarsone) has not been documented before. Preliminary dataset from this study illustrates the direct and/or indirect association of particulate Cu in catalyzing roxarsone degradation under aerobic conditions in samples with high % solids content., Recommendations and Perspectives: Concerns regarding the degradation of roxarsone in wastewater to the more toxic inorganic As may be partially linked to the presence of particulate Cu. The presence of Cu in wastewater-suspended particle surfaces has never been coupled before to organoarsenicals degradation reactions, thus, further studies are needed to elucidate the related reaction mechanisms and pathways. Water depth-dependent solid particle distribution profiles in wastewater storage lagoons could provide empirical evidence towards the design of effective degradation practices for nitrophenol-containing compounds, such as, organoarsenical-containing antibiotics, or explosive munitions compounds. more...

Concentrated animal feeding operations around the globe generate large amounts of nitrous oxide (N(2)O) in the surrounding atmosphere. Liquid animal waste systems have received little attention with respect to N(2)O emissions. We hypothesized that the solution chemistry of animal waste aqueous suspensions would promote conditions that lead to N(2)O supersaturation at the liquid/air interface. The concentration of dissolved N(2)O in poultry litter (PL) aqueous suspensions at 25 degrees C was 0.36 microg N(2)O mL(-1), at least an order of magnitude greater than that measured in water in equilibrium with ambient air, suggesting N(2)O supersaturation. There was a nonlinear increase in the N(2)O Henry constants of PL from 2810 atm/mole fraction at 35 degrees C to 17 300 atm/mole fraction at 41 degrees C. The extremely high N(2)O Henry constants were partially ascribed to N(2)O complexation with aromatic moieties. Complexed N(2)O structures were unstable at temperatures > 35 degrees C, supplying the headspace with additional free N(2)O concentrations. more...

Animal wastewater lagoons nearby concentrated animal feeding operations (CAFOs) represent the latest tendency in global animal farming, severely impacting the magnitude of greenhouse gas emissions, including nitrous oxide (N(2)O). We hypothesized that lagoon wastewater could be supersaturated with N(2)O as part of incomplete microbial nitrification/denitrification processes, thereby regulating the N(2)O partitioning in the gaseous phase. The objectives of this study were: (i) to investigate the magnitude of dissolved N(2)O concentrations in the lagoon; and (ii) to determine the extent to which supersaturation of N(2)O occurs in wastewater lagoons. Dissolved N(2)O concentrations in the wastewater samples were high, ranging from 0.4 to 40.5 microg N(2)O mL(-1). Calculated dissolved N(2)O concentrations from the experimentally measured partition coefficients were much greater than those typically expected in aquatic systems (< approximately 0.6 microg N(2)O mL(-1)). Knowledge of the factors controlling the magnitude of N(2)O supersaturation could potentially bridge mass balance differences between in situ measurements and global N(2)O models. more...