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Enzymes : the new water/wastewater treatment chemicalGarcia, Hector A. 15 June 2011 (has links)
Pharmaceuticals and personal care products (PPCPs) are detected routinely in raw and treated municipal wastewater. Conventional wastewater treatment processes are not effective in removing PPCP; therefore, treated wastewater discharges are one of the main entry points for PPCPs into the aquatic environment, and eventually into drinking water supplies. The use of laccase-catalyzed oxidation for removing low concentrations of PPCPs from municipal wastewater after primary treatment is investigated. Oxybenzone was selected as a representative PPCP. Like many other PPCPs, oxybenzone is not recognized directly by the laccase enzyme. Therefore, mediators were used to expand the oxidative range of laccase, and the efficacy of this laccase-mediator system in primary effluent was evaluated. Eight potential mediators were investigated. The greatest oxybenzone removal efficiencies were observed when 2,2’-azino-bis(3-ethylbenzthiazoline-6sulphonic acid) (ABTS), a synthetic mediator, and acetosyringone (ACE), a natural mediator, were present. An environmentally relevant concentration of oxybenzone (10 µg/L) in primary effluent was removed below the detection limit after two hours of treatment with ABTS, and 95% was removed after two hours of treatment with ACE. Several mediator/oxybenzone molar ratios were evaluated at two different initial oxybenzone concentrations. Higher mediator/oxybenzone molar ratios were required at the lower (environmentally relevant) oxybenzone concentrations, and ACE required higher molar ratios than ABTS to achieve comparable oxybenzone removal. The oxidation mechanisms and kinetics of the ACE mediator was evaluated. A better understanding of the mediator oxidation process would lead to a better design of the laccase-mediator system. An alternative laccase-mediator treatment configuration, which allows the enzyme and mediator to react prior to coming in contact with the target PPCP, was investigated. This treatment configuration shows promise for further development since it might reduce laccase and mediator requirements. Oxidation byproducts generated by the laccase-mediator system were characterized and compared to those generated during ozonation. Enzymatic treatment generated byproducts with higher mass to charge (m/z) ratios, likely due to oxidative coupling reactions. The results of this study suggest that, with further development, a laccase-mediator system has the potential to extend the treatment range of laccase to PPCPs not directly recognized by the enzyme, even in a primary effluent matrix. / text
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Removal mechanisms of pharmaceuticals and personal care products during soil aquifer treatment / 土壌浸透処理における医薬品類の除去機構He, Kai 23 September 2016 (has links)
京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第19987号 / 工博第4231号 / 新制||工||1654(附属図書館) / 33083 / 京都大学大学院工学研究科都市環境工学専攻 / (主査)教授 伊藤 禎彦, 教授 田中 宏明, 准教授 西村 文武 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM
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Interactive effects of wastewater effluent and hypoxia on the metabolic physiology and health of mummichog killifish (Fundulus heteroclitus)Lau, Samantha Chi-Lok January 2020 (has links)
This thesis is organized in “sandwich” format, as recommended by my supervisory committee. It consists of three main chapters. Chapter one is a general introduction and outlines the background information leading to the objectives and hypotheses of my thesis research. Chapter two is a manuscript prepared for submission to a peer-reviewed scientific journal. Chapter three is an overview of the major findings of this thesis, their implications in fish physiology and ecotoxicology, including suggestions of future directions of research. Appendix A contains data from an additional series of experiments that were conducted during my thesis but are not included as a full data chapter. It will be prepared for publication after my defence. / Hypoxia often occurs in aquatic ecosystems that receive effluent from municipal wastewater treatment plants (WWTP). WWTP effluent contains contaminants that could disrupt the complex physiological pathways fish use to cope with hypoxia (e.g., pharmaceuticals, polychlorinated biphenyls, and polycyclic aromatic hydrocarbons), but the effects of WWTP effluent on the physiological responses of fish to chronic hypoxia is poorly understood. We exposed mummichog killifish (Fundulus heteroclitus) to hypoxia (5 and 2 kPa O2) and/or WWTP effluent for 21 days in a full factorial design. We then measured hypoxia tolerance, whole-animal metabolism, gill morphology, haematology, and tissue metabolites. In clean water, killifish responded to chronic hypoxia with improvements in hypoxia tolerance – increases in time to loss of equilibrium at 0.5 kPa (tLOE) and decreases in critical O2 tension (Pcrit) – in association with increased gill surface area as a result of regression of the interlamellar cell mass (ILCM). Concurrent exposure to wastewater attenuated the increases in tLOE and gill remodeling in chronic hypoxia, and nearly depleted brain glycogen stores. Therefore, exposure to WWTP effluent can disrupt the physiological mechanisms fish use to cope with chronic hypoxia and impair hypoxia tolerance. My research suggests that the combination of stressors near WWTPs can have interactive effects on the physiology and health of fish. / Thesis / Master of Science (MSc) / Low oxygen conditions, known as ‘hypoxia’, frequently occur in aquatic ecosystems that receive municipal wastewater treatment plant (WWTP) effluent. WWTP effluent is a continuous and complex source of pollution, including contaminants that can disrupt fish physiology, affecting their ability to cope with stressors, like hypoxia. The effects of WWTP effluent on the responses of fish to chronic hypoxia are poorly understood. To address this research gap, I examined the effects of hypoxia and WWTP effluent on chronically exposed mummichog killifish. I provide evidence that combined exposure to hypoxia and wastewater affected hypoxia tolerance, gill structure, and depleted energy stores in the brain. My thesis demonstrates that WWTP effluent can disrupt mechanisms that fish use to cope with chronic hypoxia and impair hypoxia tolerance. These findings contribute to the existing body of work that documents the interactive effects of combined stressors in effluent-dominated ecosystems on the physiology and health of fish.
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The Mechanisms, Products, and Kinetics of Triclosan-Free Chlorine ReactionsRule, Krista Lynn 18 June 2004 (has links)
The kinetics, products, and reaction pathways of triclosan/free chlorine reactions were investigated for the pH range 3.5-11. Although pH dependent speciation occurs in both triclosan and free chlorine, only the reaction between HOCl and the phenolate-triclosan was found to play a significant role in the kinetics. The second order rate constant for the reaction between phenolate-triclosan and HOCl was found to be 5.40 (±1.82) Ã 103 M⁻¹s⁻¹. Three chlorinated triclosan intermediates were tentatively identified based on mass spectral analysis. Additionally, 2,4-dichlorophenol, 2,4,6-trichlorophenol, and chloroform formed under excess free chlorine conditions. The majority of the chloroform formed during the reactions does not form via 2,4-dichlorophenol and 2,4,6-trichlorophenol oxidation. Therefore, the majority of chloroform is likely formed via the oxidation of triclosan's phenolic ring. Based on the identified products, a reaction pathway was proposed for the oxidation of triclosan in the presence of free chlorine. / Master of Science
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Sustainability assessment of wastewater and sludge treatment techniques for removal of compounds from Pharmaceuticals and Personal Care Products (PPCPs)Tarpani, Raphael January 2017 (has links)
Environmental releases of chemical compounds from Pharmaceuticals and Personal Care Products (PPCPs) are receiving growing attention in the scientific community. Most research suggests that the main pathway for these substances to reach the environment is via Wastewater Treatment Plants (WWTPs) due to the effluents from households, industry and hospitals, which can contain substantial amounts of these compounds. Many of these contaminants are poorly treated in conventional WWTPs and are often discharged into the environment with the effluent and sludge, posing ecotoxicological risks to the wildlife and humans. Therefore, it is necessary to limit their release into the environment by controlling their discharge from WWTPs. This can be achieved by adopting advanced wastewater treatment techniques, currently not used as there are no legislative limits on PPCP compounds. However, as the scientific evidence is growing on their adverse impacts, it is only a matter of time before their advanced treatment becomes compulsory. To help guide future developments and inform policy in this area, this work considered a range of advanced treatment techniques with the aim of identifying the most sustainable options. Adopting a life cycle approach and considering all three dimensions of sustainability (economic, environmental and social), nine technologies were assessed on sustainability: four for WWTP effluent and five for sludge treatment. The advanced wastewater treatment methods considered are: (i) granular activated carbon, (ii) nanofiltration, (iii) solar photo-Fenton, and (iv) ozonation. The sludge treatment techniques comprise: (i) anaerobic digestion of sludge for agricultural application; (ii) sludge composting, also for agricultural application; (iii) incineration; (iv) pyrolysis; and (v) wet air oxidation. They were assessed on sustainability using over 28 indicators, some of which were also used to evaluate the implication of different treatment techniques for the energy-water-food (EWF) nexus. Multi-Criteria Decision Analysis (MCDA) was applied to aggregate the sustainability indicators into an overall sustainability index for each alternative and identify the most sustainable option(s). The results suggest that, among the four techniques considered for advanced effluent treatment, nanofiltration and granular activated carbon have the lowest life cycle environmental impacts. Although not preferable at all operating ranges, they have the lowest burdens and are, overall, most sustainable. The latter also has the lowest impact on the EWF nexus at mean operating parameter, and is the preferred option as the treated effluent can be used for potable water due lower concerns over the presence of PPCPs. However, the results also suggest that, from the ecotoxicological point of view, there is little benefit in using any of the advanced wastewater treatment techniques assessed. This is due to the life cycle ecotoxicological impacts from the treatment itself being similar or even higher than for the effluent released into the environment untreated. For sludge treatments, anaerobic digestion and pyrolysis are environmentally and economically preferable techniques. The former is the best with respect to the EWF nexus due to the recovery of energy and agricultural fertilizers. In relation to social aspects, wet air oxidation is amongst the most desirable for high resource recovery, together with the two former techniques. The heavy metals content in the sludge applied on agricultural soils is a major concern for freshwater ecotoxicity potential, posing risks orders of magnitude higher than PPCP compounds.
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The Fate of Pharmaceuticals and Personal Care Products in Conventional and Engineered On-Site Wastewater Drain FieldsBeardall, James 01 May 2015 (has links)
Utah State University Division of Environmental Engineering student, under the direction of Ms. Judith L. Sims, has investigated the fate of six pharmaceuticals and personal care products (PPCPs) in conventional and engineered on-site wastewater drain fields. The presence of PPCPs in the environment, especially in aquatic environments, has raised awareness to the effects of PPCPs on aquatic life and the fate of these PPCPs, and has caused regulators to become more involved in setting requirements for the removal of PPCPs from wastewater.
This research investigated the fate of caffeine, acetaminophen, carbamazepine, sulfamethoxazole, progesterone, and fluoxetine in laboratory scaled columns that simulate conventional pipe and gravel on-site wastewater drain fields as well as engineered columns similar to the pipe and gravel simulated columns, but with the addition of media below the gravel layer to enhance PPCP removal via sorption and biodegradation. Results from the month long experiment showed that sulfamethoxazole removal in the columns representing conventional systems peaked at 74%. The other PPCPs were non-detectable. Sulfamethoxazole removal increased to 81% in columns engineered with a layer of sphagnum peat moss beneath the gravel layer and below the method detection limit (5.5 ng/mL) in columns engineered with a layer of charred straw beneath the gravel layer. No other PPCPs analyzed from the engineered columns were detected. Batch experiments indicated that sorption is the main mechanism for PPCP removal with the exception of progesterone, where biodegradation is a major mechanism.
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A Bench-scale Evaluation of the Removal of Selected Pharmaceuticals and Personal Care Products by UV and UV/H₂O₂ in Drinking Water TreatmentCrosina, Quinn Kathleen 12 1900 (has links)
A bench-scale study of the degradation of four selected pharmaceuticals and personal care products (PPCPs) was carried out using UV and UV/H₂O₂ treatment employing low pressure (LP) and medium pressure (MP) lamps. The target substances included the pharmaceutical compounds ibuprofen, naproxen, and gemfibrozil, along with the bactericide triclosan. There were four main objectives of the study, as follows: to evaluate the removal of the target compounds using UV irradiation alone and UV/H₂O₂, to determine the reaction kinetics for direct and indirect photolysis of each selected compound, to determine the influence of major water quality parameters on the efficacy of treatment, and to compare the applied UV and UV/H₂O₂ doses to those that have been found to be effective for disinfection and removal of taste and odour compounds, respectively.
For initial ultra-pure water experiments the target compounds were spiked at concentrations of approximately 250 µg/L (~1 µM). In latter ultra-pure water experiments and in the partially-treated water experiments, the selected PPCPs were spiked at a lower range (c~500-1000 ng/L), which is more representative of reported environmental concentrations. In an ultra-pure water matrix, a high LP fluence of 1000 mJ/cm² caused only triclosan to substantially degrade. Furthermore, with LP-UV/H₂O₂ only triclosan and naproxen had average percent removals above 60% at a typical disinfection fluence of 40 mJ/cm² with 100 mg/L H₂O₂. Complete degradation of all four compounds in ultra-pure water was achieved with very high fluences (compared to those used for UV disinfection) with MP-UV alone (at or above 1000 mJ/cm²) or with relatively high fluences for MP-UV/H₂O₂ (200-300 mJ/cm²) with 10 mg/L H₂O₂. Overall, when compared at similar applied fluences, the MP lamp was much more effective than the LP lamp. Furthermore, the addition of H₂O₂ typically increased removal rates, in some cases substantially, through formation and subsequent reaction of the PPCP with the •OH radical.
When target substances were treated all together in an ultra-pure water solution, removals were lower than when they were treated independently at the same individual concentrations (~250 µg/L) this may simply have been the result of a higher total contaminant concentration in solution, which lessened the availability of the •OH radical and incident UV irradiation for degradation of all compounds. On the other hand, removals were improved when the combined target compounds were present at a lower individual concentration range (~750 ng/L), which suggests that removals may be concentration driven, with reduced matrix effects seen at lower overall contaminant concentrations. Furthermore, during the partially-treated water experiments, variability in treatment performance was observed with differing water quality; however, it was not evident which specific quality parameters influenced treatment effectiveness. On the other hand, substantial and sometimes complete, degradation of the target compounds was still seen in the partially-treated water with high MP-UV/H₂O₂ doses (e.g. 300 mJ/cm² + 10 mg/L H₂O₂ and 500 + 10 mg/L H₂O₂).
For the kinetic experiments, compounds were spiked individually in ultra-pure water (c~250 µg/L = ~1µM). The photolysis of the target compounds during treatment was assumed to be a pseudo-first-order reaction. Kinetic parameters were determined for both direct and indirect photolysis for both lamps. The calculated rate constants confirmed the importance of •OH radicals for degradation of these compounds, especially for ibuprofen and gemfibrozil. For ibuprofen and gemfibrozil, direct photolysis rate constants could not be determined for LP-UV because very little degradation was seen at the fluences tested. LP-UV direct phototlysis rate constants for naproxen and triclosan were 0.0002 and 0.0033 cm²/mJ, respectively. Overall rate constants describing degradation of the four compounds due to LP-UV/H₂O₂ ranged from 0.0049 to 0.0124 cm²/mJ. All four compounds had fluence-based reaction rate constants for MP-UV indirect photolysis of approximately 0.01 cm²/mJ, while MP-UV direct photolysis rate constants ranged between 0.0007-0.007 cm²/mJ, with ibuprofen having the lowest and triclosan the highest.
The overall trends were similar to those seen by other researchers for the removal of taste and odour compounds. For example, fluences required for substantial removal were much higher than typical disinfection doses, the MP lamp was more effective than the LP lamp (when compared solely on a fluence-basis), and the addition of H₂O₂ improved removals.
On the whole, UV/H₂O₂ appears to be a very promising technology for the removal of these selected PPCPs during drinking water treatment, and is likely to be equally effective for other, similar contaminants.
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A Bench-scale Evaluation of the Removal of Selected Pharmaceuticals and Personal Care Products by UV and UV/H₂O₂ in Drinking Water TreatmentCrosina, Quinn Kathleen 12 1900 (has links)
A bench-scale study of the degradation of four selected pharmaceuticals and personal care products (PPCPs) was carried out using UV and UV/H₂O₂ treatment employing low pressure (LP) and medium pressure (MP) lamps. The target substances included the pharmaceutical compounds ibuprofen, naproxen, and gemfibrozil, along with the bactericide triclosan. There were four main objectives of the study, as follows: to evaluate the removal of the target compounds using UV irradiation alone and UV/H₂O₂, to determine the reaction kinetics for direct and indirect photolysis of each selected compound, to determine the influence of major water quality parameters on the efficacy of treatment, and to compare the applied UV and UV/H₂O₂ doses to those that have been found to be effective for disinfection and removal of taste and odour compounds, respectively.
For initial ultra-pure water experiments the target compounds were spiked at concentrations of approximately 250 µg/L (~1 µM). In latter ultra-pure water experiments and in the partially-treated water experiments, the selected PPCPs were spiked at a lower range (c~500-1000 ng/L), which is more representative of reported environmental concentrations. In an ultra-pure water matrix, a high LP fluence of 1000 mJ/cm² caused only triclosan to substantially degrade. Furthermore, with LP-UV/H₂O₂ only triclosan and naproxen had average percent removals above 60% at a typical disinfection fluence of 40 mJ/cm² with 100 mg/L H₂O₂. Complete degradation of all four compounds in ultra-pure water was achieved with very high fluences (compared to those used for UV disinfection) with MP-UV alone (at or above 1000 mJ/cm²) or with relatively high fluences for MP-UV/H₂O₂ (200-300 mJ/cm²) with 10 mg/L H₂O₂. Overall, when compared at similar applied fluences, the MP lamp was much more effective than the LP lamp. Furthermore, the addition of H₂O₂ typically increased removal rates, in some cases substantially, through formation and subsequent reaction of the PPCP with the •OH radical.
When target substances were treated all together in an ultra-pure water solution, removals were lower than when they were treated independently at the same individual concentrations (~250 µg/L) this may simply have been the result of a higher total contaminant concentration in solution, which lessened the availability of the •OH radical and incident UV irradiation for degradation of all compounds. On the other hand, removals were improved when the combined target compounds were present at a lower individual concentration range (~750 ng/L), which suggests that removals may be concentration driven, with reduced matrix effects seen at lower overall contaminant concentrations. Furthermore, during the partially-treated water experiments, variability in treatment performance was observed with differing water quality; however, it was not evident which specific quality parameters influenced treatment effectiveness. On the other hand, substantial and sometimes complete, degradation of the target compounds was still seen in the partially-treated water with high MP-UV/H₂O₂ doses (e.g. 300 mJ/cm² + 10 mg/L H₂O₂ and 500 + 10 mg/L H₂O₂).
For the kinetic experiments, compounds were spiked individually in ultra-pure water (c~250 µg/L = ~1µM). The photolysis of the target compounds during treatment was assumed to be a pseudo-first-order reaction. Kinetic parameters were determined for both direct and indirect photolysis for both lamps. The calculated rate constants confirmed the importance of •OH radicals for degradation of these compounds, especially for ibuprofen and gemfibrozil. For ibuprofen and gemfibrozil, direct photolysis rate constants could not be determined for LP-UV because very little degradation was seen at the fluences tested. LP-UV direct phototlysis rate constants for naproxen and triclosan were 0.0002 and 0.0033 cm²/mJ, respectively. Overall rate constants describing degradation of the four compounds due to LP-UV/H₂O₂ ranged from 0.0049 to 0.0124 cm²/mJ. All four compounds had fluence-based reaction rate constants for MP-UV indirect photolysis of approximately 0.01 cm²/mJ, while MP-UV direct photolysis rate constants ranged between 0.0007-0.007 cm²/mJ, with ibuprofen having the lowest and triclosan the highest.
The overall trends were similar to those seen by other researchers for the removal of taste and odour compounds. For example, fluences required for substantial removal were much higher than typical disinfection doses, the MP lamp was more effective than the LP lamp (when compared solely on a fluence-basis), and the addition of H₂O₂ improved removals.
On the whole, UV/H₂O₂ appears to be a very promising technology for the removal of these selected PPCPs during drinking water treatment, and is likely to be equally effective for other, similar contaminants.
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A Bench-scale Evaluation of the Removal of Selected Pharmaceuticals and Personal Care Products by UV and UV/H₂O₂ in Drinking Water TreatmentCrosina, Quinn Kathleen 12 1900 (has links)
A bench-scale study of the degradation of four selected pharmaceuticals and personal care products (PPCPs) was carried out using UV and UV/H₂O₂ treatment employing low pressure (LP) and medium pressure (MP) lamps. The target substances included the pharmaceutical compounds ibuprofen, naproxen, and gemfibrozil, along with the bactericide triclosan. There were four main objectives of the study, as follows: to evaluate the removal of the target compounds using UV irradiation alone and UV/H₂O₂, to determine the reaction kinetics for direct and indirect photolysis of each selected compound, to determine the influence of major water quality parameters on the efficacy of treatment, and to compare the applied UV and UV/H₂O₂ doses to those that have been found to be effective for disinfection and removal of taste and odour compounds, respectively.
For initial ultra-pure water experiments the target compounds were spiked at concentrations of approximately 250 µg/L (~1 µM). In latter ultra-pure water experiments and in the partially-treated water experiments, the selected PPCPs were spiked at a lower range (c~500-1000 ng/L), which is more representative of reported environmental concentrations. In an ultra-pure water matrix, a high LP fluence of 1000 mJ/cm² caused only triclosan to substantially degrade. Furthermore, with LP-UV/H₂O₂ only triclosan and naproxen had average percent removals above 60% at a typical disinfection fluence of 40 mJ/cm² with 100 mg/L H₂O₂. Complete degradation of all four compounds in ultra-pure water was achieved with very high fluences (compared to those used for UV disinfection) with MP-UV alone (at or above 1000 mJ/cm²) or with relatively high fluences for MP-UV/H₂O₂ (200-300 mJ/cm²) with 10 mg/L H₂O₂. Overall, when compared at similar applied fluences, the MP lamp was much more effective than the LP lamp. Furthermore, the addition of H₂O₂ typically increased removal rates, in some cases substantially, through formation and subsequent reaction of the PPCP with the •OH radical.
When target substances were treated all together in an ultra-pure water solution, removals were lower than when they were treated independently at the same individual concentrations (~250 µg/L) this may simply have been the result of a higher total contaminant concentration in solution, which lessened the availability of the •OH radical and incident UV irradiation for degradation of all compounds. On the other hand, removals were improved when the combined target compounds were present at a lower individual concentration range (~750 ng/L), which suggests that removals may be concentration driven, with reduced matrix effects seen at lower overall contaminant concentrations. Furthermore, during the partially-treated water experiments, variability in treatment performance was observed with differing water quality; however, it was not evident which specific quality parameters influenced treatment effectiveness. On the other hand, substantial and sometimes complete, degradation of the target compounds was still seen in the partially-treated water with high MP-UV/H₂O₂ doses (e.g. 300 mJ/cm² + 10 mg/L H₂O₂ and 500 + 10 mg/L H₂O₂).
For the kinetic experiments, compounds were spiked individually in ultra-pure water (c~250 µg/L = ~1µM). The photolysis of the target compounds during treatment was assumed to be a pseudo-first-order reaction. Kinetic parameters were determined for both direct and indirect photolysis for both lamps. The calculated rate constants confirmed the importance of •OH radicals for degradation of these compounds, especially for ibuprofen and gemfibrozil. For ibuprofen and gemfibrozil, direct photolysis rate constants could not be determined for LP-UV because very little degradation was seen at the fluences tested. LP-UV direct phototlysis rate constants for naproxen and triclosan were 0.0002 and 0.0033 cm²/mJ, respectively. Overall rate constants describing degradation of the four compounds due to LP-UV/H₂O₂ ranged from 0.0049 to 0.0124 cm²/mJ. All four compounds had fluence-based reaction rate constants for MP-UV indirect photolysis of approximately 0.01 cm²/mJ, while MP-UV direct photolysis rate constants ranged between 0.0007-0.007 cm²/mJ, with ibuprofen having the lowest and triclosan the highest.
The overall trends were similar to those seen by other researchers for the removal of taste and odour compounds. For example, fluences required for substantial removal were much higher than typical disinfection doses, the MP lamp was more effective than the LP lamp (when compared solely on a fluence-basis), and the addition of H₂O₂ improved removals.
On the whole, UV/H₂O₂ appears to be a very promising technology for the removal of these selected PPCPs during drinking water treatment, and is likely to be equally effective for other, similar contaminants.
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A Bench-scale Evaluation of the Removal of Selected Pharmaceuticals and Personal Care Products by UV and UV/H₂O₂ in Drinking Water TreatmentCrosina, Quinn Kathleen 12 1900 (has links)
A bench-scale study of the degradation of four selected pharmaceuticals and personal care products (PPCPs) was carried out using UV and UV/H₂O₂ treatment employing low pressure (LP) and medium pressure (MP) lamps. The target substances included the pharmaceutical compounds ibuprofen, naproxen, and gemfibrozil, along with the bactericide triclosan. There were four main objectives of the study, as follows: to evaluate the removal of the target compounds using UV irradiation alone and UV/H₂O₂, to determine the reaction kinetics for direct and indirect photolysis of each selected compound, to determine the influence of major water quality parameters on the efficacy of treatment, and to compare the applied UV and UV/H₂O₂ doses to those that have been found to be effective for disinfection and removal of taste and odour compounds, respectively.
For initial ultra-pure water experiments the target compounds were spiked at concentrations of approximately 250 µg/L (~1 µM). In latter ultra-pure water experiments and in the partially-treated water experiments, the selected PPCPs were spiked at a lower range (c~500-1000 ng/L), which is more representative of reported environmental concentrations. In an ultra-pure water matrix, a high LP fluence of 1000 mJ/cm² caused only triclosan to substantially degrade. Furthermore, with LP-UV/H₂O₂ only triclosan and naproxen had average percent removals above 60% at a typical disinfection fluence of 40 mJ/cm² with 100 mg/L H₂O₂. Complete degradation of all four compounds in ultra-pure water was achieved with very high fluences (compared to those used for UV disinfection) with MP-UV alone (at or above 1000 mJ/cm²) or with relatively high fluences for MP-UV/H₂O₂ (200-300 mJ/cm²) with 10 mg/L H₂O₂. Overall, when compared at similar applied fluences, the MP lamp was much more effective than the LP lamp. Furthermore, the addition of H₂O₂ typically increased removal rates, in some cases substantially, through formation and subsequent reaction of the PPCP with the •OH radical.
When target substances were treated all together in an ultra-pure water solution, removals were lower than when they were treated independently at the same individual concentrations (~250 µg/L) this may simply have been the result of a higher total contaminant concentration in solution, which lessened the availability of the •OH radical and incident UV irradiation for degradation of all compounds. On the other hand, removals were improved when the combined target compounds were present at a lower individual concentration range (~750 ng/L), which suggests that removals may be concentration driven, with reduced matrix effects seen at lower overall contaminant concentrations. Furthermore, during the partially-treated water experiments, variability in treatment performance was observed with differing water quality; however, it was not evident which specific quality parameters influenced treatment effectiveness. On the other hand, substantial and sometimes complete, degradation of the target compounds was still seen in the partially-treated water with high MP-UV/H₂O₂ doses (e.g. 300 mJ/cm² + 10 mg/L H₂O₂ and 500 + 10 mg/L H₂O₂).
For the kinetic experiments, compounds were spiked individually in ultra-pure water (c~250 µg/L = ~1µM). The photolysis of the target compounds during treatment was assumed to be a pseudo-first-order reaction. Kinetic parameters were determined for both direct and indirect photolysis for both lamps. The calculated rate constants confirmed the importance of •OH radicals for degradation of these compounds, especially for ibuprofen and gemfibrozil. For ibuprofen and gemfibrozil, direct photolysis rate constants could not be determined for LP-UV because very little degradation was seen at the fluences tested. LP-UV direct phototlysis rate constants for naproxen and triclosan were 0.0002 and 0.0033 cm²/mJ, respectively. Overall rate constants describing degradation of the four compounds due to LP-UV/H₂O₂ ranged from 0.0049 to 0.0124 cm²/mJ. All four compounds had fluence-based reaction rate constants for MP-UV indirect photolysis of approximately 0.01 cm²/mJ, while MP-UV direct photolysis rate constants ranged between 0.0007-0.007 cm²/mJ, with ibuprofen having the lowest and triclosan the highest.
The overall trends were similar to those seen by other researchers for the removal of taste and odour compounds. For example, fluences required for substantial removal were much higher than typical disinfection doses, the MP lamp was more effective than the LP lamp (when compared solely on a fluence-basis), and the addition of H₂O₂ improved removals.
On the whole, UV/H₂O₂ appears to be a very promising technology for the removal of these selected PPCPs during drinking water treatment, and is likely to be equally effective for other, similar contaminants.
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