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This article was downloaded by: [Mrs Mary Ann Muller]On: 19 June 2015, At: 11:15Publisher: Taylor & FrancisInforma Ltd Registered in England and Wales Registered Number: 1072954 Registered office: Mortimer House,37-41 Mortimer Street, London W1T 3JH, UK Ozone: Science & Engineering: The Journal of the
International Ozone Association
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Oxidation of Emerging Contaminants during Pilot-Scale
Ozonation of Secondary Treated Municipal Effluent
Saileshkumar Singha, Rajesh Setha, Shahram Tabeab & Paul Yangb
a Civil and Environmental Engineering Department, University of Windsor, Windsor, Ontario
N9B 3P4, Canada
b Ontario Ministry of the Environment, Ontario M7A 1N3, Canada
Accepted author version posted online: 02 Feb 2015.Published online: 02 Feb 2015.
To cite this article: Saileshkumar Singh, Rajesh Seth, Shahram Tabe & Paul Yang (2015): Oxidation of Emerging Contaminants
during Pilot-Scale Ozonation of Secondary Treated Municipal Effluent, Ozone: Science & Engineering: The Journal of the
International Ozone Association, DOI:
To link to this article:
PLEASE SCROLL DOWN FOR ARTICLE Taylor & Francis makes every effort to ensure the accuracy of all the information (the "Content") containedin the publications on our platform. However, Taylor & Francis, our agents, and our licensors make norepresentations or warranties whatsoever as to the accuracy, completeness, or suitability for any purpose of theContent. Any opinions and views expressed in this publication are the opinions and views of the authors, andare not the views of or endorsed by Taylor & Francis. The accuracy of the Content should not be relied upon andshould be independently verified with primary sources of information. Taylor and Francis shall not be liable forany losses, actions, claims, proceedings, demands, costs, expenses, damages, and other liabilities whatsoeveror howsoever caused arising directly or indirectly in connection with, in relation to or arising out of the use ofthe Content.
This article may be used for research, teaching, and private study purposes. Any substantial or systematicreproduction, redistribution, reselling, loan, sub-licensing, systematic supply, or distribution in anyform to anyone is expressly forbidden. T Ozone: Science & Engineering, 37: 1–7Copyright 2015 International Ozone AssociationISSN: 0191-9512 print / 1547-6545 onlineDOI: 10.1080/01919512.2014.998755 Oxidation of Emerging Contaminants during Pilot-Scale
Ozonation of Secondary Treated Municipal Effluent

Saileshkumar Singh,Rajesh Seth,Shahram Tabe,and Paul Yang
1Civil and Environmental Engineering Department, University of Windsor, Windsor, Ontario N9B 3P4, Canada 2Ontario Ministry of the Environment, Ontario M7A 1N3, Canada The transformation of 41 target emerging contaminants in precautionary principle dictates that their discharge to the secondary treated municipal wastewater effluent in Canada environment should be limited to the extent possible.
was examined at pilot-scale, at transferred ozone doses of Studies conducted in various parts of the world have 2.8 mg/L (0.46 O3/mg DOC) and 4.4 mg/L (0.72 mg O3/mgDOC). In general, transformation efficiencies of CECs either detected the presence of several CECs in potable water increased or were retained at the higher ozone dose. The sources (Auriol et al. Benotti et al. Daughton and higher ozone dose of 0.72 mg O3/mg DOC (Zspec = 0.6 mg Ternes Huber et al. Tabe et al. Municipal O3/mg DOC) was sufficient to transform 21 of the 31 detected wastewater treatment plants are an important point source CECs by over 80% as well as achieving the disinfection target for many CECs released to such sources (Daughton and of < 200 MPN E. coli per 100 mL. Ternes Petrovi´c et al. It makes logical sense to treat and remove the CECs from the municipal wastewater Emerging Concern, Municipal Wastewater, Pharma- effluent (MWWE) when their concentration is higher, rather than from a water supply for potable water in which they Secondary Treated Effluent, Wastewater Treatment have been diluted several orders of magnitude (Oneby et al.
Tabe et al. The conventional technologies totreat MWWE are efficient in removing suspended solids, organics, and nutrients. However, they are not effective inremoving many CECs that are present in trace quantities Studies in the 1990s reported trace amounts of contami- (Ternes Hence, new treatment technologies or addi- nants in wastewater treatment plant effluent that could induce tional treatment processes are required to remove these CECs, estrogenic effects and were suspected to be responsible for which are normally low molecular weight compounds in the feminization of male fish in water bodies receiving such the size range of about 150 to 500 Daltons (Snyder et al.
Downloaded by [Mrs Mary Ann Muller] at 11:15 19 June 2015 effluent discharges (Folmar et al. Harries et al. Since then, several other trace contaminants of human and The scientific community has been aware of the disinfec- ecological health concern have been detected in waters and tion property of ozone since the start of the 20th century.
wastewaters (Shon et al. Snyder et al. Ternes Recent studies that demonstrated the potential of ozone to et al. These contaminants are grouped commonly oxidize and transform many CECs have renewed interest in as contaminants of emerging concern (CECs), and include the technology for wastewater treatment and reuse applica- pharmaceutically active compounds (PhACs), personal care tions (Bahr et al. Hansen et al. Snyder et al. products (PCPs), fire retardants, and nanomaterials. Although Ternes et al. Further benefits of ozonation of MWWE evidence of actual observed environmental effects from expo- include an increase in its dissolved oxygen levels, decreases sure to CECs is limited (Bloetscher and Plummer in its chemical oxygen demand, and improvement in aes-thetic characteristics due to reduction in turbidity and color.
Received 2/11/2014; Accepted 11/27/2014 In addition, due to the significant advances in the ozone man- Address correspondence to Dr. Rajesh Seth, Civil and ufacturing technology in the last couple of decades and the Environmental Engineering Department, University of Windsor, experience gained from studies on ozone treatment of water 401 Sunset Avenue, Windsor, Ontario, N9B 3P4, Canada. E-mail: and wastewater, costs for ozone treatment have declined to Ozonation of Secondary Treated Municipal Effluent July–August 2015


become competitive with UV for disinfection (Drury et al.
biological treatment (activated sludge process). The plant Oneby et al. and ozonation is now a matured adds alum after grit removal to enhance coagulation and technology for such applications (Leong et al. phosphorus removal. It discharges the effluent with or with- Although studies have demonstrated the potential for out disinfection to Little River, which leads into the Detroit ozonation to transform effectively many CECs present in River. The plant meets the specified disinfection requirement MWWE, such studies are still limited both in number and of < 200 MPN E. coli/100 mL during the months of April– list of CECs examined. Studies have further shown that the October with UV disinfection. In this study, the municipal effectiveness of such transformations by ozone is strongly wastewater effluent (MWWE) before disinfection was the dependent on the properties of CEC and the matrix, par- feed water (influent) to the pilot unit.
ticularly the nature and concentration of dissolved organic shows the schematics of the pilot unit. It includes carbon (Huber et al. Uslu et al. In addition, an ozone contactor, ozone generator (Lab2B, Triogen, the list of CECs in the water environment continues to grow.
Glasgow, UK), and ozone monitor (Model 454, Teledyne, Hence, there is a continued need to study the ozone and San Diego, USA). A combination of dry air and pure oxy- ozone-based advanced oxidation processes (AOPs) for dif- gen (Praxair Canada) at a rate of 4 L/min was the feed ferent wastewater matrices to better understand and apply gas to generate ozone. The ozone contactor was comprised them for wastewater treatment. The objective of this study of a dissolution chamber (DC) and four reaction chambers was to examine the effect of ozonation of secondary-treated (RC#1 to RC#4). The material of contactor columns was clear MWWE in Ontario, Canada on transformation of selected PVC. The fittings were either ozone-resistant stainless steel CECs as well as disinfection. The 41 selected CECs include or Teflon. MWWE was collected in a 300-L feed tank from antiphlogistics, antibiotics, lipid regulators, estrogen replace- where it was transferred to the top of the DC by a peri- ment agents, and reproductive hormones. The disinfection staltic pump. A coarse bubble glass diffuser dispersed the air target for MWWE in Ontario is < 200 MPN E. coli per enriched with ozone at the bottom of the dissolution cham- 100 mL (Ontario MOE To the best knowledge of ber. The water flowed countercurrent to the rising gas bubbles.
the authors of this article, this study was first of its kind in Ozonated wastewater from the DC entered the first reaction chamber (RC#1) from bottom and flowed upwards. Similarly,the flow entered the column RC#2 from top and the columnsRC#3 and RC#4 from bottom. The column RC#4 provided MATERIALS AND METHODS
additional contact time to ensure that effluent from the pilot unit did not contain any residual ozone. When operated incontinuous flow mode at a flow rate of 4 L/min, the hydraulic A pilot plant was established at the Little River Pollution retention time (HRT) in each of the DC and RC#1 - 3 was Control Plant (LRPCP), Windsor, Ontario, Canada for ozone 1.7 min, and was 10 min in RC#4.
treatment of secondary-treated MWWE. LRPCP has a treat- Dissolved organic carbon (DOC) and total organic car- ment capacity of 73,000 m3/day. The treatment process bon (TOC) was analyzed as per Standard Method 5310 consists of preliminary and primary treatment, followed by Downloaded by [Mrs Mary Ann Muller] at 11:15 19 June 2015 FIGURE 1.
Schematic of the pilot unit.
S. Singh et al.
July–August 2015 (Clesceri et al. with a Shimadzu TOC-VCSH analyzer, Transformation of CECs at TOD of 4.4 mg/L
Kyoto, Japan. The ozone monitor measured ozone concen- (0.72 mg O3/mg DOC)
trations in the ozone-enriched feed gas and the vent gas.
presents the data related to the concentration of These concentrations were used to calculate transferred ozone the detected CECs, and their transformation on reaction with dose (TOD) and ozone transfer efficiency. The ozone trans- ozone at TOD of 4.4 mg/L (0.72 mg O3/mg DOC).
fer efficiencies were ∼50%. The concentration of residual Significant variation in concentrations of CECs in MWWE ozone in the aqueous phase was measured as per Method was observed during the two experimental runs, which is quite 4500-O3 of Standard Methods (Clesceri et al. The common in literature as well (Tabe et al. Ternes UV254 absorbance was measured with a Varian Cary 50 Scan although the concentration of ibuprofen during one of the spectrophotometer (Palo Alto, CA, USA). The characteristics experimental runs was unusually high which needs to be fur- of MWWE before and after ozonation were determined in ther investigated. The results show that ozonation is effective the Environmental Engineering Laboratories at the University in transforming the majority of the detected CECs.
of Windsor. Samples packed in ice were shipped overnight The transformations of all drugs in the antiphlogistics to Mass Spectroscopy Laboratory of Ontario Ministry of the group were above 90%, except for ketoprofen for which the Environment (Toronto, Canada) for the analyses of the target range was 79–86%. Earlier studies have also reported above CECs using LC/MS-MS.
90% reduction of acetaminophen, diclofenac, indomethacin, The DOC of MWWE was similar during the two exper- and naproxen at ozone doses up to 0.5 mg O3/mg DOC (Bahr imental runs and measured at 6.1 mg/L and accounted for et al. Reungoat et al. Reungoat et al. Rosal greater than 95% of the TOC. MWWE pH was in the range et al. For ibuprofen, studies have reported less than 6.9–7.1, temperature 18–21 ◦C, and alkalinity 95–180 mg/L 50% removal at ozone doses up to 0.5 mg O3/mg DOC and as CaCO3. The ozone dose in the first experimental run was above 90% transformation at an ozone dose of 0.8 mg O3/mg 8.8 mg/L (TOD = 4.4 mg/L or 0.72 mg O3/mg DOC). Ozone DOC or higher (Bahr et al. Snyder et al. Ternes doses in the second experimental run were 8.8 mg/L (TOD = et al. Wert et al. The literature is variable on 4.4 mg/L or 0.72 mg O3/mg DOC) and 5.6 mg/L (TOD = ketoprofen. At TOD/DOC ratio of 0.6–0.8, ketoprofen trans- 2.8 mg/L or 0.46 mg O3/mg DOC). The specific ozone con- formation reported by Bahr et al. is 82%, then by Kim sumption (Zspec), i.e., the ratio of ozone consumption to the and Tanaka it ranges from 31 to 71%.
initial DOC, at TODs of 4.4 and 2.8 mg/L was calculated to In the fluoroquinolones subgroup of antibiotics, transfor- be 0.6 and 0.43 mg O3/mg DOC, respectively.
mation of ciprofloxacin and norfloxacin was in the range of71 to >99%. Rosal et al. and Kim and Tanaka have reported 67 to >99% transformation of these drugs at ozone doses between 0.6 and 0.9 mg O3/mg C. The trans- If the concentration of a CEC was below its detection limit formation of enrofloxacin as quantified from one of the two (DL) in ozone-treated MWWE, its transformation efficiency experiments was only 23% as compared to >99% transfor- was calculated only if its concentration in MWWE before mation at TOD/ DOC ratio of ∼ 0.6 reported by Dodd et al.
ozone treatment was equal to or greater than five times the DL. In addition, if a CEC had concentration below its DL in In macrolides subgroup, the transformation efficiency of the ozonated effluent, a value equal to half of its DL was used the antibiotic lincomycin was close to 99%. This is consis- to calculate its transformation efficiency.
tent with the finding by Rosal et al. and Kim andTanaka However, the transformation of erythromycinand roxithromycin at 50% and 3.5% was lower as compared Downloaded by [Mrs Mary Ann Muller] at 11:15 19 June 2015 RESULTS AND DISCUSSION
with > 90% transformation previously reported for the twocompounds at similar ozone doses (Reungoat et al. The results from three experiments from two experi- Reungoat et al. Rosal et al. Schaar et al. mental runs are presented. Out of the total 41 CECs ana- The removal of chlortetracycline and oxytetracycline of lyzed, the following eight CECs were not detected in both the tetracyclines group of antibiotics was between 9 and the experiments: carbadox, chloramphenicol, diethylstilbe- 38%. Mean transformation of doxycycline, meclocycline, and strol, lasalocid A, monensin sodium, sulfachloropyridazine, tetracycline was in the range of 75 to 98%. Dodd et al.
sulfadimethoxine, and warfarin. Results from other experi- have reported >99% reduction of tetracycline from ments (not reported) showed that the Ontario Ministry of wastewater at a TOD/TOC ratio of around 0.3. No data were the Environment's disinfection target of < 200 MPN E. found in the literature on transformation of the remaining coli/100 mL for MWWE was consistently met at TOD of compounds in the group on ozonation of MWWE.
4.4 mg/L but not always at TOD of 2.8 mg/L. The MWWE Ozonation reduced the concentration of sulfamethazine E.coli concentrations in these experiments ranged between and sulfamethoxazole drugs of the sulfonamide group of 2,500– 21,500 MPN/100 mL, which were reduced to between antibiotics by over 99% and their concentration decreased 5–11 and 20–463 MPN/100 mL at TODs of ∼ 4.4 mg/L and to below detection limit or close to the detection limit after 2.8 mg/L, respectively.
ozone treatment. These results are consistent with the findings Ozonation of Secondary Treated Municipal Effluent July–August 2015 Transformation of CECs at TOD of 0.72 mg O3/mg DOC Ozonated Effluent Antibiotic – Fluoroquinolones Antibiotic – Macrolides Antibiotic – Tetracyclines Antibiotic – Sulfonamides Antibiotic – Miscellaneous Estrogen replacement agents Downloaded by [Mrs Mary Ann Muller] at 11:15 19 June 2015 Bisphenol-A (BPA) Ovulation Inhibitors Reproductive Hormones 17-β-Estradiol (E2) Legend: DL: Detection Limit Exp; Experiment ND; Not detected.
S. Singh et al.
July–August 2015


of other studies (Hollender et al. Huber et al. Transformation of CECs at TOD of 2.8 mg/L
Reungoat et al. Snyder et al. (0.46 O3/mg DOC) and TOD of 4.4 mg/L (0.72 mg
The transformation of antidepressant and lipid regulator drugs such as carbamazepine, bezafibrate, clofibric acid, and During the second experimental run, the MWWE was gemfibrozil was above 90%. Bahr et al. have reported treated with two different ozone doses. The concentrations 17 to 21% transformation of bezafibrate and clofibric acid at of target CECs in MWWE are presented in (Exp-2).
ozone dose of 0.4 mg O3/mg DOC. They observed 74 to 98% presents summary of the observed transformation reduction at a higher ozone dose of 0.8 mg O3/mg DOC.
efficiencies of the detected CECs at the two ozone doses.
Hollender et al. have also reported average 88% and The result shows that the number of CECs detected in the 66% removal of bezafibrate and clofibric acid at ozone doses unozonated MWWE and but not in the ozonated MWWE of 0.6 to 0.67 mg O3/mg DOC. Snyder et al. and increased from three at the TOD of 2.8 mg/L to seven at the Dickenson et al. have reported > 93% transformation TOD of 4.4 mg/L. In general, the transformation of CECs of gemfibrozil at an ozone dose of around 0.3 mg O3/mg C.
was higher at the higher ozone dose. The transformation of Concentrations observed of most of the potential EDCs BPA, carbamazepine, diclofenac, indomethacin, lincomycin, (estrogen replacement agents, ovulation inhibitors, repro- sulfamethoxazole, trimethoprim, and was more than 80% at ductive hormones) were low. Transformations of 19- both ozone doses. There was a noticeable increase in the norethisterone, estrone (E1), estriol (E3), and bisphenol-A transformation of naproxen, ciprofloxacin, bezafibrate, and (BPA) were in the range of 93–99%, which is consistent clofibric acid from 27–67% at TOD of 2.8 mg/L (0.46 O3/mg with values reported in literature (Huber et al. Nakada DOC) to 79– >99% at TOD of 4.4 mg/L (0.72 O3/mg et al. Ternes et al. Wert et al. The trans- DOC). Transformations of enrofloxacin, roxithromycin, formation of E2 was in the range of 14 to 63%. Equilin oxytetracycline, and chlortetracycline were below 30% at both and 17-α-estradiol were detected in concentrations less than the ozone dose.
10 ng/L in one sampling event only and their transformationafter ozonation was 44% and 33%.
shows the transformation observed of CECs at TOD of 4.4 mg/L. For 21 of 31 CECs for whichtransformation efficiency could be calculated, average trans- This study reports results from pilot-scale ozone treat- formation efficiency exceeded 80%. The average trans- ment of secondary-treated municipal wastewater effluent in formation of another six CECs including 17-α-estradiol, Canada for 41 target CECs at TODs of 2.8 mg/L (0.46 O 17-β-estradiol, erythromycin, sulfamerazine, doxycycline, DOC) and 4.4 mg/L (0.72 mg O and tetracycline, was between 30–80%. For the remaining 3/mg DOC). In general, the transformation efficiencies (TEs) of CECs either increased or four (roxithromycin, chlortetracycline, enrofloxacin, and maintained at the higher ozone dose. TEs of > 80% were oxytetracycline; all antibiotics), the average transformation observed at both ozone doses for seven CECs (bisphenol was less than 30%.
A, carbamazepine, diclofenac, indomethacin, lincomycin, Downloaded by [Mrs Mary Ann Muller] at 11:15 19 June 2015 FIGURE 2.
Transformation of CECs at TOD of 4.4 mg/L (0.72 mg O3/mg DOC).
Ozonation of Secondary Treated Municipal Effluent July–August 2015


FIGURE 3.
Transformation of CECs at TOD of 2.8 and 4.4 mg/L.
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The Future Mortality of High Mortality Countries: A Model Incorporating Expert Arguments Garbero, A., Pamuk, E., Garenne, M., Masquelier, B. and Pelletier, F. IIASA Interim ReportOctober 2013 Garbero, A., Pamuk, E., Garenne, M., Masquelier, B. and Pelletier, F. (2013) The Future Mortality of High Mortality Countries: A Model Incorporating Expert Arguments. IIASA Interim Report . IIASA, Laxenburg, Austria, IR-13-017

biotechlerncenter.interpharma.ch

Personalisierte Medizin Wie ist es möglich, dass zwei Menschen mit der gleichen Krankheit unterschiedlich auf die Behandlung mit demselben Medikament reagieren? Die Antwort liegt in den Genen. 1. Weniger Nebenwirkungen dank Pharmakogenomik Vergleicht man das Erbgut zweier Menschen, zum Beispiel das Erbgut einer Schülerin und ihres Banknachbarn, so wird man feststellen, dass sich die beiden Genome an etwa 30 bis 60 Millionen Basenpaaren, den «Buchstaben» des Erbguts, unterscheiden (einzige Ausnahme: der Banknachbar ist zugleich der eineiige Zwilling). Das entspricht etwa 1 bis 2 Prozent des gesamten Erbguts. Noch vor fünf Jahren meinten Wissenschafter, dass sich zwei Menschen nur etwa zu 0,1 Prozent genetisch voneinander unterscheiden.