Disinfection is an essential process in the treatment of municipal wastewater before the treated wastewater can be discharged to the environment. Hillsborough County's Northwest Regional Water Reclamation Facility (NWRWRF) in Tampa, Florida, currently uses ultraviolet (UV) light for disinfection. However, this method has proven expensive to implement and maintain, and may not be effective if the light transmission is poor. For these reasons, Hillsborough County is considering switching from UV light to sodium hypochlorite for disinfection. However, hypochlorite (chlorine) disinfection has disadvantages as well, such as the production of disinfection by-products (DBPs) such as trihalomethanes (THM) and haloacetic acids (HAAs), which may have adverse impacts on the quality of surface waters that receive the treated wastewater. Therefore, the objectives of this research are (1) to compare NWRWRF typical operating conditions and water quality to those of two nearby facilities (River Oaks and Dale Mabry Advanced Wastewater Treatment Plants) that currently employ chlorine disinfection, (2) to determine the chlorine demand of treated effluent from NWRWRF, (3) to quantify the DBP formation potential of treated effluent from NWRWRF, and (4) to determine the effects of temperature, reaction time, and chlorine dose on chlorine demand and THM formation. To inform laboratory experiments, the quality of final effluent was monitored at NWRWRF and at two nearby wastewater treatment plants that currently use hypochlorite for disinfection. At these two facilities, pH of 7.0-8.0, chemical oxygen demand (COD) of 12-26 mg/L, alkalinity of 200-250 mg/L as CaCO3, chlorine residual of 1.5-6.0 mg/L, and total trihalomethanes of 100-190 ix μg/L (mostly chloroform) were observed. Conditions at NWRWRF were similar to those at Dale Mabry and River Oaks AWWTP, suggesting that chlorine demand and THM formation at NWRWRF would be similar to those at the two AWWTP, if chlorination is to be used. THM experimental results agreed with this suggestion. Chlorine dose and temperature effects on the free chlorine residual and THMs production in NWRWRF filtered wastewater effluent were determined. Filtered effluent was collected and transported to USF laboratory where it was tested for 3 different chlorine doses (6 mg/L, 9 mg/L and 12 mg/L as Cl2) and 3 different temperatures (16°C, 23°C, and 30°C) at 7 different contact times (15, 30, 45, 60, 75, 90, and 120 min) in duplicate. The total number of batches prepared was: 3 different chlorine doses × 3 different temperatures × 7 different reaction times = 126 reactors. According to Florida Administrative code 62-600.440, total chlorine residual should be at least 1 mg/L after a contact time of at least 15 min at peak hourly flow. Also, according to Florida Administrative code 62-600.440, if effluent wastewater has a concentration of fecal coliforms greater than 10,000 per 100 mL before disinfection, FDEP requires that the product of the chlorine concentration C (in mg/L as Cl2) and the contact time t (in minutes) be at least 120. Results showed that free chlorine residual was always above 1 mg/L in 15 min contact time for all chlorine doses and temperatures tested in this thesis. However, to be conservative, thesis conclusions and recommendations were based on the more stringent regulation: C*t ≥ 120 mg.min/L, assuming that the number of fecal coliform in NWRWRF wastewater effluent exceeds 10,000 per 100 mL prior to disinfection. The analysis showed that free chlorine residual for 6 mg/L was below the FDEP standard at all temperatures. At 16 °C and 23 °C, chlorine doses of 9 and 12 mg/L resulted in an appropriate free chlorine residual above the FDEP standard. However, a chlorine dose of 12 mg/L was resulting in high residual, which means high THM would be expected. Therefore, at 16 x and 23°C, 9 mg/L would be preferable. At 30 °C, only the chlorine dose of 12 mg/L met the standard at all contact times. As expected, free chlorine residual decreased with an increase in temperature from 23°C to 30°C. Surprisingly, the residual at 16°C was lower than residual at 23°C. The production of THMs increased with higher contact time in all the experiments completed. Chlorine dose didn't have an effect on THM formation at 23°C, but it did at 30°C and 16°C, where THM concentrations were generally higher with the increase of chlorine dose. Temperature effect was noticed in most of the experiments, where THM production was usually higher at higher temperatures, except some cases where formation was similar for different temperatures. Chloroform, dichlorobromomethane, dibromochloromethane production ranges were respectively: 20-127 μg/L, 18-59 μg/L, and 3-7 μg/L. Bromoform concentrations were not observed in this experiment at any temperature or chlorine dose. According to Florida Administrative code 62-302.530, Criteria for Surface Water Quality Classifications, the Florida Department for Environmental Protection (FDEP) set the following limits for THM concentrations in wastewater effluent to be as the following; 470 μg/L for chloroform, 22 μg/L for dichlorobromomethane, 34 μg/L for dibromochloromethane, and 360 μg/L for bromoform. Experimental results on NWRWRF filtered effluent showed that only dichlorobromomethane exceeded the limits set by FDEP at about 30 min contact time for all temperatures and chlorine doses tested. However, according to Florida Administrative code 62- 302-400, proposed changes to the code have set higher DCBM limit of 57 μg/L. Chlorination would be recommended at NWRWRF if the DCBM regulated limit increases to 57 μg/L. The recommended chlorine dose would be 9 mg/L for water temperatures around 16-23 °C and 12 mg/L for water temperatures around 30 °C

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O objetivo deste trabalho foi avaliar o desempenho da combinação dos processos de interozonização e sistemas pós-filtros adsorvedores na remoção de compostos orgânicos precursores e na formação de subprodutos da desinfecção, em particular os trialometanos (THM). Os ensaios foram desenvolvidos com a água filtrada proveniente da estação de tratamento de água do Alto da Boa Vista, localizada no município de São Paulo, tipo convencional, com água bruta oriunda de reservatório com elevado estado de eutrofização. O aparato experimental é constituído de um sistema de ozonização com quatro colunas em série e tempo de detenção hidráulica total de 16 minutos; e, por um sistema de quatro pós-filtros adsorvedores com diferentes tipos de carvão ativado granular, filtros F1 e F3 dotados de carvão mineral (CAG1, betuminoso) e filtros F2 e F4 compostos por carvão vegetal (CAG2, casca de coco) sendo todos operados em paralelo com valores de Tempo de Contato de Leito Vazio (TCLV) entre 15 e 20 minutos. Duas colunas receberam como afluente água filtrada pré-ozonizada (F1 e F2) e as demais colunas apenas água filtrada (F3 e F4). Os resultados indicaram que a ozonização não alterou de forma significativa os parâmetros utilizados para avaliação dos precursores, COT e UV-254 nm, e nem o THM. Inicialmente, os resultados de remoção de COT permaneceram elevados, próximos de 80% caracterizando a saturação dos leitos em torno de 240 dias para os filtros F1 e F3 (CAG1) e apenas 30 dias, com eficiências baixas para os filtros F2 e F4 (CAG2). Para THM a saturação foi próxima de 65 dias para ambos os carvões e as eficiências iniciais foram de 90% e 75%, para os filtros com CAG1 e CAG2, respectivamente. Com todos os leitos saturados, os resultados ainda indicaram boa remoção de compostos causadores de gosto e odor. Neste trabalho, os sistemas de pós-filtros adsorvedores de CAG foram efetivos para o controle das substâncias precursoras e a redução da formação de THMs, com melhores resultados para o carvão mineral CAG1 (betuminoso) independentemente do sistema de interozonização. / The main purpose of this work was to evaluate the performance of a combination of processes - inter-ozonization and post-filter GAC adsorbers systems, on the control of organic precursors and disinfection byproducts, especially trihalomethanes (THM). The experience was conducted with filtered water produced at Alto da Boa Vista conventional WTP, located at São Paulo city, where raw water comes from a high eutrofic lake. The experimental setup consists of an ozonation system with four column shaped contactors arranged in series with 16 minutes total hydraulic detention time; and, a system of four pilot scale adsorbers with different types of granular activated carbon (GAC) media, F1 and F3 filters with mineral GAC media (GAC1, bituminous) and F2 and F4 filters with vegetal GAC media (GAC2, coconut shell), all operated in parallel with empty bed contact time (EBCT) between 15 and 20 minutes. Two columns were fed with filtered and pre-ozonated water (F1 and F2) and the other two were fed with filtered water only (F3 and F4). It was observed that ozonation did not affect significantly results of precursors parameters, TOC and UV-254, and neither THM. Initially, TOC removal remained high, near 80% delineating the bed saturation around 240 days to F1 and F3 filters (GAC1) and only 30 days with low efficiency for filters F2 and F4 (GAC2). The THM bed saturation time was nearly 65 days for both media and initial efficiencies were 90% and 75% to GAC1 and GAC2, respectively. With all beds saturated, still there was a good taste and odor producing substances removal. In this work, the systems of GAC adsorbents post-filters were effective for the control of precursors and to reduce the formation of THM\'s, with better results for the CAG1 (bituminous) regardless of the use of inter-ozonization.

O objetivo deste trabalho foi avaliar o desempenho da combinação dos processos de interozonização e sistemas pós-filtros adsorvedores na remoção de compostos orgânicos precursores e na formação de subprodutos da desinfecção, em particular os trialometanos (THM). Os ensaios foram desenvolvidos com a água filtrada proveniente da estação de tratamento de água do Alto da Boa Vista, localizada no município de São Paulo, tipo convencional, com água bruta oriunda de reservatório com elevado estado de eutrofização. O aparato experimental é constituído de um sistema de ozonização com quatro colunas em série e tempo de detenção hidráulica total de 16 minutos; e, por um sistema de quatro pós-filtros adsorvedores com diferentes tipos de carvão ativado granular, filtros F1 e F3 dotados de carvão mineral (CAG1, betuminoso) e filtros F2 e F4 compostos por carvão vegetal (CAG2, casca de coco) sendo todos operados em paralelo com valores de Tempo de Contato de Leito Vazio (TCLV) entre 15 e 20 minutos. Duas colunas receberam como afluente água filtrada pré-ozonizada (F1 e F2) e as demais colunas apenas água filtrada (F3 e F4). Os resultados indicaram que a ozonização não alterou de forma significativa os parâmetros utilizados para avaliação dos precursores, COT e UV-254 nm, e nem o THM. Inicialmente, os resultados de remoção de COT permaneceram elevados, próximos de 80% caracterizando a saturação dos leitos em torno de 240 dias para os filtros F1 e F3 (CAG1) e apenas 30 dias, com eficiências baixas para os filtros F2 e F4 (CAG2). Para THM a saturação foi próxima de 65 dias para ambos os carvões e as eficiências iniciais foram de 90% e 75%, para os filtros com CAG1 e CAG2, respectivamente. Com todos os leitos saturados, os resultados ainda indicaram boa remoção de compostos causadores de gosto e odor. Neste trabalho, os sistemas de pós-filtros adsorvedores de CAG foram efetivos para o controle das substâncias precursoras e a redução da formação de THMs, com melhores resultados para o carvão mineral CAG1 (betuminoso) independentemente do sistema de interozonização. / The main purpose of this work was to evaluate the performance of a combination of processes - inter-ozonization and post-filter GAC adsorbers systems, on the control of organic precursors and disinfection byproducts, especially trihalomethanes (THM). The experience was conducted with filtered water produced at Alto da Boa Vista conventional WTP, located at São Paulo city, where raw water comes from a high eutrofic lake. The experimental setup consists of an ozonation system with four column shaped contactors arranged in series with 16 minutes total hydraulic detention time; and, a system of four pilot scale adsorbers with different types of granular activated carbon (GAC) media, F1 and F3 filters with mineral GAC media (GAC1, bituminous) and F2 and F4 filters with vegetal GAC media (GAC2, coconut shell), all operated in parallel with empty bed contact time (EBCT) between 15 and 20 minutes. Two columns were fed with filtered and pre-ozonated water (F1 and F2) and the other two were fed with filtered water only (F3 and F4). It was observed that ozonation did not affect significantly results of precursors parameters, TOC and UV-254, and neither THM. Initially, TOC removal remained high, near 80% delineating the bed saturation around 240 days to F1 and F3 filters (GAC1) and only 30 days with low efficiency for filters F2 and F4 (GAC2). The THM bed saturation time was nearly 65 days for both media and initial efficiencies were 90% and 75% to GAC1 and GAC2, respectively. With all beds saturated, still there was a good taste and odor producing substances removal. In this work, the systems of GAC adsorbents post-filters were effective for the control of precursors and to reduce the formation of THM\'s, with better results for the CAG1 (bituminous) regardless of the use of inter-ozonization.

The main theme of this thesis is the usage of the test investigating the formation potential of trihalogenmethanes (THM FP) and its comparison with conventional indicators of water quality (CODMn, A254 and colours). As for the experimental part of the thesis, rating of the effectiveness of selected technological procedures has been applied (e.g.: coagulation, adsorption and ozonation in the act of treatment of artificially prepared water model with a higher content of humic substances in laboratory conditions). Based on the obtained results, it was found that the common indicators of water quality have very similar attributes and also complete each other. On the contrary, those attributes of indicators may not be sufficient in case of the evaluation of water quality with high content of humic substances. The findings made illustrate that the THM FP test enables the accurate evaluation of water quality, especially in connection with the content of an organic material susceptible to chemical changes. THM formation potential has proved its high value and also has confirmed that it can appropriately complete the other standarts that are being used for assessing the quality of treated water up to nowadays.

La désinfection de l’eau de consommation et des piscines induit la formation de sous-produits (SPD) potentiellement nocifs pour la santé, parmi lesquels les trihalométhanes (THM), les acides haloacétiques (HAA) et les chloramines (CAM). La difficulté d’estimer l’exposition humaine à ces SPD empêche de cerner précisément les risques sanitaires possiblement associés (i.e., cancérigènes, reprotoxiques, irritatifs). Nos travaux s’articulent autour d’une méthodologie consistant à intégrer des données d’occurrence environnementales à des modèles toxicocinétiques à base physiologique (TCBP) pour améliorer les mesures de l’exposition aux SPD. Cette approche multidisciplinaire veut prendre en compte de manière aussi appropriée que possible les deux composantes majeures des variations de cette exposition : les variations spatio-temporelles des niveaux de contamination environnementale et l’impact des différences inter- et intra-individuelles sur les niveaux biologiques. Cette thèse, organisée en deux volets qui explorent chacun successivement des aspects environnemental et biologique de la problématique, vise à contribuer au développement de cette stratégie innovante d’estimation de l’exposition et, plus généralement, à des meilleures pratiques en la matière. Le premier volet de la thèse s’intéresse à l’exposition en milieu domestique (i.e., résultant de l’utilisation de l’eau potable au domicile) et est consacré au cas complexe des THM, les plus abondants et volatils des SPD, absorbables par ingestion mais aussi par inhalation et voie percutanée. Les articles I et II, constitutifs de ce volet, documentent spécifiquement la question des variations inter- et intra- journalières de présence des SPD en réseau et de leurs impacts sur les estimateurs de l’exposition biologique. Ils décrivent l’amplitude et la diversité des variations à court terme des niveaux environnementaux, présentent les difficultés à proposer une façon systématique et « épidémiologiquement » pratique de les modéliser et proposent, de manière originale, une évaluation des mésestimations, somme toute modestes, des mesures biologiques de l’exposition résultant de leurs non-prise en compte. Le deuxième volet de la thèse se penche sur l’exposition aux SPD en piscine, d’un intérêt grandissant au niveau international, et se restreint au cas jugé prioritaire des piscines publiques intérieures. Ce volet envisage, pour quantifier l’exposition dans ce contexte particulier, l’extension de l’approche méthodologique préconisée, élaborée originellement pour application dans un contexte domestique : d’abord, à travers une analyse approfondie des variations des niveaux de contamination (eau, air) des SPD en piscine en vue de les modéliser (article III); puis en examinant, dans le cas particulier du chloroforme, le THM le plus abondant, la possibilité d’utiliser la modélisation TCBP pour simuler des expositions en piscine (article IV). Les résultats mettent notamment en évidence la difficulté d’appréhender précisément la contamination environnementale autrement que par un échantillonnage in situ tandis que la modélisation TCBP apparait, sur le plan toxicologique, comme l’outil le plus pertinent à ce jour, notamment au regard des autres approches existantes, mais qu’il convient d’améliorer pour mieux prédire les niveaux d’exposition biologique. Finalement, ces travaux illustrent la pertinence et la nécessité d’une approche multidisciplinaire et intégratrice et suggère, sur cette base, les pistes à explorer en priorité pour mieux évaluer l’exposition aux SPD et, in fine, cerner véritablement les risques sanitaires qui en résultent. / Disinfection of drinking and swimming pool waters disinfection is unavoidable but induces the formation of by-products (DBPs), such as trihalomethanes (THMs), haloacetic acids (HAAs) and chloramines (CAMs), that could be harmful to human health. The still challenging DBP exposure assessment prevent their suspected adverse effects (i.e., cancers, adverse pregnancy outcomes, irritations) to be clearly established. A methodology has been conceptualized which consists of integrating environmental occurrence data with physiologically based toxicokinetic (PBTK) modeling to improve DBP exposure assessment. It was designed to allow both spatial and temporal variations of the environmental contamination and the biological impacts of between- and within- individual differences to be accounted for. This thesis comprised of two parts. Each one investigates successively both environmental and biological aspects. The objective is to contribute to the development of an innovative integrated strategy and to the definition of best practices for DBP exposure assessment. The first part of the thesis, comprising papers I and II, focuses on household exposure (i.e., resulting from drinking water use at home) and on THMs, the most abundant and volatile DBPs that can be absorbed not only by ingestion but also by inhalation and dermal absorption. These two papers investigate particularly the short-term (day-to-day and within-day) variations of THM levels in the drinking water and then their impact on the internal exposure indicators. They described the amplitudes and the diversity of the environmental variations, failed to model them in a systematic and practical way for epidemiological purposes but assessed, for the first time, their impacts on the predicted biological levels which appeared quite low. The second part concerns the exposure to DBPs in swimming pool which is of a growing international interest. Only the allegedly worrying case of public indoor swimming pool was regarded. This section focuses on the feasibility of using the previously mentioned approach, which was first designed for dealing with household exposure, for DBP exposure assessment in swimming pools. First, Paper III investigated the occurrence and spatial and temporal variations of DBPs in both water and air of swimming pools to model them. Focusing on chloroform, the most abundant THM, Paper IV examined the ability and reliability of PBTK modeling to simulate various swimming pool exposure events and predict the resulting biological levels in individuals. The results show, among other things, the difficulty of explaining precisely the environmental contamination and point out the necessity to carry out a minimal in situ sampling to monitor the environmental levels of DBPs. Compared to other approaches, PBTK modeling is a powerful but still to be improved tool for predicting swimming pool exposure. Eventually, these works underline the relevance and the necessity of a multidisciplinary and integrating approach for better estimating exposure to DBPs and therefore health risks. Further issues that should be addressed are recommended.

La désinfection de l’eau de consommation et des piscines induit la formation de sous-produits (SPD) potentiellement nocifs pour la santé, parmi lesquels les trihalométhanes (THM), les acides haloacétiques (HAA) et les chloramines (CAM). La difficulté d’estimer l’exposition humaine à ces SPD empêche de cerner précisément les risques sanitaires possiblement associés (i.e., cancérigènes, reprotoxiques, irritatifs). Nos travaux s’articulent autour d’une méthodologie consistant à intégrer des données d’occurrence environnementales à des modèles toxicocinétiques à base physiologique (TCBP) pour améliorer les mesures de l’exposition aux SPD. Cette approche multidisciplinaire veut prendre en compte de manière aussi appropriée que possible les deux composantes majeures des variations de cette exposition : les variations spatio-temporelles des niveaux de contamination environnementale et l’impact des différences inter- et intra-individuelles sur les niveaux biologiques. Cette thèse, organisée en deux volets qui explorent chacun successivement des aspects environnemental et biologique de la problématique, vise à contribuer au développement de cette stratégie innovante d’estimation de l’exposition et, plus généralement, à des meilleures pratiques en la matière. Le premier volet de la thèse s’intéresse à l’exposition en milieu domestique (i.e., résultant de l’utilisation de l’eau potable au domicile) et est consacré au cas complexe des THM, les plus abondants et volatils des SPD, absorbables par ingestion mais aussi par inhalation et voie percutanée. Les articles I et II, constitutifs de ce volet, documentent spécifiquement la question des variations inter- et intra- journalières de présence des SPD en réseau et de leurs impacts sur les estimateurs de l’exposition biologique. Ils décrivent l’amplitude et la diversité des variations à court terme des niveaux environnementaux, présentent les difficultés à proposer une façon systématique et « épidémiologiquement » pratique de les modéliser et proposent, de manière originale, une évaluation des mésestimations, somme toute modestes, des mesures biologiques de l’exposition résultant de leurs non-prise en compte. Le deuxième volet de la thèse se penche sur l’exposition aux SPD en piscine, d’un intérêt grandissant au niveau international, et se restreint au cas jugé prioritaire des piscines publiques intérieures. Ce volet envisage, pour quantifier l’exposition dans ce contexte particulier, l’extension de l’approche méthodologique préconisée, élaborée originellement pour application dans un contexte domestique : d’abord, à travers une analyse approfondie des variations des niveaux de contamination (eau, air) des SPD en piscine en vue de les modéliser (article III); puis en examinant, dans le cas particulier du chloroforme, le THM le plus abondant, la possibilité d’utiliser la modélisation TCBP pour simuler des expositions en piscine (article IV). Les résultats mettent notamment en évidence la difficulté d’appréhender précisément la contamination environnementale autrement que par un échantillonnage in situ tandis que la modélisation TCBP apparait, sur le plan toxicologique, comme l’outil le plus pertinent à ce jour, notamment au regard des autres approches existantes, mais qu’il convient d’améliorer pour mieux prédire les niveaux d’exposition biologique. Finalement, ces travaux illustrent la pertinence et la nécessité d’une approche multidisciplinaire et intégratrice et suggère, sur cette base, les pistes à explorer en priorité pour mieux évaluer l’exposition aux SPD et, in fine, cerner véritablement les risques sanitaires qui en résultent. / Disinfection of drinking and swimming pool waters disinfection is unavoidable but induces the formation of by-products (DBPs), such as trihalomethanes (THMs), haloacetic acids (HAAs) and chloramines (CAMs), that could be harmful to human health. The still challenging DBP exposure assessment prevent their suspected adverse effects (i.e., cancers, adverse pregnancy outcomes, irritations) to be clearly established. A methodology has been conceptualized which consists of integrating environmental occurrence data with physiologically based toxicokinetic (PBTK) modeling to improve DBP exposure assessment. It was designed to allow both spatial and temporal variations of the environmental contamination and the biological impacts of between- and within- individual differences to be accounted for. This thesis comprised of two parts. Each one investigates successively both environmental and biological aspects. The objective is to contribute to the development of an innovative integrated strategy and to the definition of best practices for DBP exposure assessment. The first part of the thesis, comprising papers I and II, focuses on household exposure (i.e., resulting from drinking water use at home) and on THMs, the most abundant and volatile DBPs that can be absorbed not only by ingestion but also by inhalation and dermal absorption. These two papers investigate particularly the short-term (day-to-day and within-day) variations of THM levels in the drinking water and then their impact on the internal exposure indicators. They described the amplitudes and the diversity of the environmental variations, failed to model them in a systematic and practical way for epidemiological purposes but assessed, for the first time, their impacts on the predicted biological levels which appeared quite low. The second part concerns the exposure to DBPs in swimming pool which is of a growing international interest. Only the allegedly worrying case of public indoor swimming pool was regarded. This section focuses on the feasibility of using the previously mentioned approach, which was first designed for dealing with household exposure, for DBP exposure assessment in swimming pools. First, Paper III investigated the occurrence and spatial and temporal variations of DBPs in both water and air of swimming pools to model them. Focusing on chloroform, the most abundant THM, Paper IV examined the ability and reliability of PBTK modeling to simulate various swimming pool exposure events and predict the resulting biological levels in individuals. The results show, among other things, the difficulty of explaining precisely the environmental contamination and point out the necessity to carry out a minimal in situ sampling to monitor the environmental levels of DBPs. Compared to other approaches, PBTK modeling is a powerful but still to be improved tool for predicting swimming pool exposure. Eventually, these works underline the relevance and the necessity of a multidisciplinary and integrating approach for better estimating exposure to DBPs and therefore health risks. Further issues that should be addressed are recommended.