Spatial and temporal variability of contaminants of emerging concern in a drinking water source.

The spatial-temporal behaviour of contaminants of emerging concern (CECs) are not well-documented in drinking water sources, including in Quebec, Canada. In this study, a set of seven contaminants, which are more frequently reported in water sources, were monitored from May 2016 to August 2017 at ten locations within an urbanized watershed (lakes and rivers) in Quebec, Canada. Samples were collected between a wastewater plant discharge (upstream) and the intake of a drinking water plant (downstream). The results showed that three (acetaminophen, salicylic acid, caffeine) out of seven CECs were consistently detected at a range of up to a few hundred ng L-1 at all sampling stations throughout the sampling period with a detection frequency between 51% and 94%. Upstream of two wastewater plant discharge locations, six CECs were measured above the detection limit compared to other locations where only three CECs (acetaminophen, salicylic acid, caffeine) were detected. Most of the CEC concentrations were higher (a few ng L-1) during late winter in comparison with the summer, in both years 2016 and 2017. The results highlight that the wastewater effluents and septic system effluents are significant sources of CECs that are released into the surface water. Moreover, the results help to identify the spatio-temporal patterns, which is a crucial element to understand the fate of CECs in water sources submitted to extreme weather conditions during the year. This research also provides baseline data for CEC occurrence at different points across lakes, rivers, and tributaries which will be useful for future ecotoxicological studies.

Tracking domestic wastewater and road de-icing salt in a municipal drinking water reservoir: Acesulfame and chloride as co-tracers.

Developing strategies to identify the origins of contaminants in watersheds is crucial for source water protection. The use of multiple tracers improves the ability to identify contamination events originating from various land use activities. The objective of this study was to evaluate the use of acesulfame and chloride as co-tracers to represent the impact of pollution originating from wastewater and road de-icing on water quality in a municipal drinking water source. The study included a two-year sampling and water quality analysis program in numerous locations within a drinking water reservoir comprising a lake (upstream) and a river (downstream) which supply raw water to a municipal water treatment plant. Results showed that the spatial variability of acesulfame and chloride within the watershed of the lake-river systems depends on the location of contaminant sources, mainly municipal wastewater and septic tank discharges (for acesulfame) and the presence of small tributaries of the lake and river (for chloride). Temporal variability of the tracers under study differed according to the sampling location and was mainly affected by seasonal conditions. Correlation analyses between the two tracers in lake and river waters (in terms of concentrations and loads) made it possible to pinpoint the probable origins of contamination. The assessment of the spatio-temporal variability of these co-tracers within the lake-river watersheds allowed for the delineation of priority intervention zones as a decision-making tool for municipal authorities in improving drinking water source protection.

Occurrence and seasonality of raw and drinking water contaminants of emerging interest in five water facilities.

The goal of this work was to investigate the occurrence of contaminants of emerging interest (CEI) in source surface water (SW; river water) and drinking water (DW; tap water) from five drinking water treatment plants (DWTPs) in the Province of Québec, Canada. A total of 28 sampling campaigns were conducted to collect SW and DW samples from each DWTP from June 2016 to July 2017. The seven targeted CEI, including acetaminophen, salicylic acid, caffeine, carbamazepine, ibuprofen, sulfamethoxazole and drospirenone, were analyzed using solid-phase extraction-ultra pressure liquid chromatography-mass spectrometry (SPE-UPLC-MS/MS) for all collected water samples. The selected CEI were detected in all SW and DW samples, with the exception of drospirenone, which occurred in amounts that were below the limit of detection in one DWTP in June and July 2016. In all the SW samples, caffeine was detected and had the highest median concentration range (12.3-91.0 ng/L), followed by acetaminophen (7.9-85.0 ng/L) and salicylic acid (21.6-39.0 ng/L). In the DW samples, salicylic acid was detected and had the highest median concentration range (20.5-50 ng/L), followed by caffeine (5.2-21.8 ng/L), and acetaminophen (5.0-7.7 ng/L). Carbamazepine, ibuprofen, and sulfamethoxazole primarily occurred in amounts between the limit of detection and limit of quantification in SW and occurred below the limit of detection in DW. All the DWTPs exhibited a similar trend in the removal of CEI, which include acetaminophen (≤97.6%), followed by caffeine (71.0-86.5%) and salicylic acid (<50.0%). Varying levels of efficiencies were observed among the removal strategies for CEI under study, which were mainly associated with the contaminant concentration in SW in the case of acetaminophen, and with the treatment processes in the case of caffeine and salicylic acid.

Occurrence and fate of ozonation disinfection by-products in two Canadian drinking water systems.

The occurrence and the fate of 18 ozonation by-products (OBPs) (17 different aldehydes and bromate) were studied over one year in two Canadian drinking water systems. This is the first and only study reporting the occurrence of all these non-halogenated aldehydes (NON-HALs) and haloacetaldehydes (HALs) simultaneously, based on the multi-point monitoring of water in full-scale conditions from source to distribution network. In general, the application of both post-ozonation and liquid chlorine contributed to the formation of OBPs (aldehydes and bromate). NON-HALs were present in higher concentrations than HALs. Formaldehyde, acetaldehyde, glyoxal and methylglyoxal were the most common forms of NON-HALs in the two water systems that were studied. Chloral hydrate (CH), the hydrated form of trichloroacetaldehyde, was the most dominant HAL observed. The nature of the organic matter and the water temperature proved to be important parameters for explaining the variability of aldehydes. Summer and autumn (warm seasons) were more favorable for the formation of chloral hydrate and bromate. The highest concentrations of NON-HALs were observed in spring.

Spatio-temporal variability of tastes and odors of drinking water within a distribution system.

The threshold of human perception in the detection of tastes and odors (T&O) relating to compounds in drinking water is variable. For example, chlorine can be detected at the ppm level and geosmin can be perceived at the ppt level. In this paper, sensory tests (using a human panel), physicochemical analyses (total and free residual chlorine, temperature, metals, geosmin, and 2-methylisoborneol (2MIB)) and microbiological analyses (algae, Actinomycetes and heterotrophic plate count) were performed for water samples collected during a seventeen-month period at ten different locations of a municipal distribution network of Quebec City (Canada). The results showed that different flavors(1) assessed by a panel and aggregated into global flavor intensity (GFI) vary considerably spatially and seasonally. Multiple regression analysis showed that the factors best explaining the variability of GFI are (in order) the season, the location, the concentration of total residual chlorine and the presence of cyanobacteria. Results also demonstrate that chlorine has a masking effect on other T&O.

Spatial variations of human health risk associated with exposure to chlorination by-products occurring in drinking water.

During disinfection, chlorine reacts with organic matter present in drinking water and forms various undesirable chlorinated by-products (CBPs). This paper describes a study of the spatial variability of human health risk (i.e., cancer effects) from CBP exposure through drinking water in a specific region. The region under study involves nine drinking water distribution systems divided into several zones based on their characteristics. The spatial distribution of cancer risk (CR) was estimated using two years of data (2006-2008) on various CBP species. In this analysis, trihalomethanes (THMs) and haloacetic acids (HAAs) served as surrogates for CBPs. Three possible routes of exposure (i.e., via ingestion, inhalation and dermal contact) were considered for each selected compound. The cancer risk assessment involved estimating a unit risk (R(T)) in each zone of the selected distribution systems. A probabilistic analysis based on Monte Carlo simulations was employed. Risk assessment results showed that cancer risk varied between systems, but also within individual systems. As a result, the population of the same region was not exposed to the same risk associated with CBPs in drinking water. Unacceptable levels (i.e., R(T) > 10(-4)) for the estimated CR were determined for several zones in the studied region. This study demonstrates that a spatial-based analysis performed to represent the spatial distribution of risk estimates can be helpful in identifying suitable risk management strategies. Suggestions for improving the risk analysis procedure are also presented.

Estimation of chlorination by-products presence in drinking water in epidemiological studies on adverse reproductive outcomes: a review.

Chlorination of drinking water is essential to prevent waterborne disease. However, chlorine reacts with organic matter present in surface waters to form various by-products. In the last decade, several epidemiological studies have been conducted to determine the connection between exposure to these chlorination by-products (CBPs) and human health defects, such as adverse reproductive outcomes. However, the methodology used to assess exposure of pregnant women in these studies had serious limitations, particularly in relation to determining CBP presence in the subject's tap water. The purpose of this paper is to critically review of methods used to evaluate the CBP presence in a subject's tap water for exposure assessment purposes in epidemiological studies focused on adverse reproductive outcomes and CBPs in drinking water. Interest is directed more precisely at space-time features related to CBPs for an optimal estimation of their presence in a subject's tap water.

Behavior of trihalomethanes and haloacetic acids in a drinking water distribution system.

This investigation focused on the seasonal variation and spatial fate of chlorination disinfection by-products (CDBPs) in a drinking water distribution system located in a region where very significant seasonal variations in water temperature and surface water quality occur. The analysis of a large number of collected samples showed that the seasonal and geographical variations of both groups of CDBPs under study--trihalomethanes (THMs) and haloacetic acids (HAAs)--were particularly important in this region. THM levels in summer and fall were, on average, about five times higher than in winter, whereas average HAAs in spring were about four times higher than in winter. THMs increased and stabilized in the extremities of the distribution system, whereas HAAs begin to increase, and then decrease (mainly due to a reduction of dichloroacetic acid). This decrease was significantly higher in warm waters than in cold waters, which led to the hypothesis of microbial degradation of HAAs as water approaches the system extremities. In fact, regression models for the occurrence of both CDBPs showed that the residence time of water was one important parameter in explaining the fate of both CDBPs. The spatio-temporal portrait of both groups of CDBPs that was generated demonstrates that, due to their high intra-seasonal changes, the calculation of average annual levels of these substances for compliance with regulations can vary widely. The results used in the portrait of CDBP behavior are also relevant in terms of exposure assessment for future epidemiological studies on human reproductive outcomes in the region.

Trihalomethanes in drinking water of greater Québec region (Canada): occurrence, variations and modelling.

The levels of trihalomethanes (THMs)--the main species of by-product from water chlorination--were monitored in the distribution systems of the five major drinking water utilities of the greater area of Québec City in order to investigate and model their occurrence on a spatial and seasonal basis. Data for THMs and other water quality and operational parameters associated with their formation were generated through a 16 month sampling program involving several sites representing variable water residence times, from the plant to the system extremity. The results demonstrate that the differences in measured THM levels between the five utilities are mainly due to the variable quality of raw waters, the type of water treatment process being used and the type and levels of applied disinfectant. Depending on the utility, average THM levels were from 1.3 to 2.5 times higher in the system extremities than in the water leaving the treatment plant. Also, average levels of THMs measured in summer at the distribution system extremities were, depending on the utility, from 2.5 to 5 times higher than the average levels measured in winter. The seasonal differences were found to be significantly greater than those observed by others in water utilities in the United States and Europe and are explained in large part by the considerable changes, over the year, in the quality and temperature of surface waters in Southern Quebec. For the live utilities under study, multivariate regression models were developed in order to predict spatial and seasonal variations of THMs. Both residual chlorine demand and temperature were found to be better, statistically, as predictors for THM occurrence. The usefulness of the developed models for routine and long term water quality management, as well as for assessment of human exposure to THMs, are also discussed.

Occurrence of THMs and HAAs in experimental chlorinated waters of the Quebec City area (Canada).

Haloacetic acids (HAAs) and trihalomethanes (THMs) were generated in bench-scale chlorination experiments using treated waters (prior to final chlorination) of the three major drinking water utilities of the Quebec City area. The purpose was to investigate the formation and occurrence of these chlorination by-products (CBPs) on a seasonal basis. Data for HAAs, THMs and other physico-chemical parameters were produced through a six-month sampling program with variable conditions of water quality, water temperature, applied chlorine dose and reaction time. In waters from the three utilities, chloroform (THM specie), dichloroacetic and trichloroacetic acid (HAA species) were the most prevalent compounds due to the low concentrations of bromide in the utilities' raw waters. Significant differences in CBP occurrence were noted between the three utilities' chlorinated waters, mainly due to the type of disinfectant applied to raw water. The use of pre-ozonation, as opposed to pre-chlorination (or direct chlorination) in one of the utilities appears to be the major factor contributing to that utility's potential for compliance with current THM and future HAA standards. Seasonal variations in THMs and HAAs were mainly associated with variations in organic precursors and to changes in water temperature (two parameters which vary widely on a seasonal basis in surface waters of southern Quebec), with CBP occurrence at its highest in spring. Statistical correlations between HAAs and THMs were moderate and only temperature appeared to affect the preponderance of one CBP or the other. Finally, a regression analysis was carried out aimed at associating each CBP to water quality and the experimental parameters. Thanks to their predictive ability, multivariate models seem to be the tools with the best potential for decision-making purposes.