POTENTIAL AND LIMITATIONS OF (ADVANCED) OXIDATION PROCESSES IN WATER AND WASTEWATER TREATMENT
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1 Titelmasterformat durch Klicken bearbeiten POTENTIAL AND LIMITATIONS OF (ADVANCED) OXIDATION PROCESSES IN WATER AND WASTEWATER TREATMENT Torsten C. Schmidt, Holger Lutze Cairo, February 19, 2013
2 Outline Introduction/Overview of Oxidative Processes Examples of our Recent Work: Lab Scale: Mechanistic Investigations with Probe Compounds: Degradation of Micropollutants Pilot Scale: Implementation of Ozonation in Drinking Water Treatment (Full Scale: Advanced Treatment of Wastewater Effluents) Conclusions and Outlook
3 Use of Oxidation Processes in Water Treatment Advantages: Constant process performance No disposal of concentrates or solids (compared with AC sorption or membrane filtration) Areas of Use: Drinking water Disinfection, Decolorization, Fe(II) and Mn(II) Removal, Micropollutant Elimination Municipal wastewater Disinfection, Further elimination of micropollutants Industrial wastewater High purity industrial process waters
4 Modified after U. von Gunten, eawag Important Considerations in Oxidative Treatment Processes Oxidation Lifetime Pollutants Oxidation Mechanisms CO 2, H 2 O Kinetics Prediction of elimination based on properties possible? Scavenging by matrix components Possible loss of efficiency, Oxidation byproducts Transformation products Biodegradability D Toxicological effects Energy Demand/Carbon Footprint?
5 Effect of Oxidative Transformation: Reduction of Estrogenicity Estrogenically active compound Transformation product Oxidation 17b-Estradiole (E2) binds binds? Effect Effect? Estrogen Receptor Modified after U. von Gunten, eawag
6 Reduction of Estrogenic Effects (EEEQ) of 17a- Ethinylestradiole by Oxidative Processes Relative EE2 or EEEQ EE2 EEEQ Relative EEEQ Relative EE dose, M Chlorine r 2 = r 2 = Relative EEEQ dose, M Bromine Relative EE2 Relative EEEQ dose, M Ozone r 2 = Relative EE2 Relative EE2 or EEEQ Relative EEEQ OH radical r 2 = Relative EE2 Relative EEEQ Chlorine dioxide r 2 = Relative EE2 Relative EEEQ Ferrate r 2 = Relative EE UV fluence, mj/cm dose, M dose, M Lee et al a-Ethinylestradiole (EE2) Reduction of estrogenicity is proportional to concentration decline of EE2 Modified after U. von Gunten, eawag
7 Oxidation + Biological Filtration: Reduction of Toxic Effects in Whole Effluents Adapted from S. Zimmermann, EPFL Data from WWTP Regensdorf, CH: Bioluminescence suppression Algae test (photosynthesis) Algae test (growth) YES Assay Acetylcholinesterase suppression Elimination by ozonation and slow sand filtration in %
8 Overview Advanced Oxidation Processes UV based Ozone based H 2 O 2 based No Chemicals UV/TiO 2 UV/H 2 O 2 UV/O 3 O3/H2O2 Vacuum UV (VUV) Fenton Ultrasound O 3 /AC Ozonation H 2 O+Ultrasound OH +H H 2 O + VUV( nm) OH +H TiO 2 + hn h + + e - OH + O 2 - H 2 O 2 + UVC 2 OH (F = 1) Also direct photolysis H 2 O 2 OH O 3 +UVC H 2 O 2 OH+O 2 OH- yield: 50% [Jarocki et al., in prep.] 2O 3 + HO OH +3O 2 O 3 + AC OH + O 2 O 3 + (OH -, NOM) OH Fe(II) Fe(III) [Fe(III)HO 2 ] 2+ HO 2 H 2 O 2 ph < 4
9 Comparison of Advanced Oxidative Processes No Chemicals Ultrasound Vacuum UV UV based Ozone based H 2 O 2 based UV/H 2 O 2 (TiO 2 ) Fenton UV/O 3 O 3 /H 2 O 2 Energy demand O 3 /AC Ozonation O 3 Br - HOBr/OBr - H 2 O 2 Br - Negative Effects - BrO 3-3 NDMA O 3 / OH Loss of oxidation efficiency via matrix scavenging, assimilable organic carbon formation, unknown transformation products
10 Modified after U. von Gunten, eawag Describing Pollutant Removal Typical second order kinetic constants for a pollutant P: dp = dt 0 k ox P ) ) ln P k ox t P = Oxidant Ozone ~ 500 OH Radicals ~ 2000 Chlorine ~ 300 Chlorodioxide ~ 100 Ferrate(VI) ~ 50 No. of publ. kinetic const. k (ca. 2008) ph, T! Determination kinetic constants: Direct measurements Indirect measurements (Competition kinetics) Quantitative structure activity relationships (QSARs) Estimation from similar oxidants Quantification oxidant exposure: Matrix dependent Dosage dependent Consideration of secondary oxidants
11 Mechanistic Investigations
12 Degradation of Micropollutants: Example Diclofenac HOOC H N O 3 Diclofenac (Non-Steroidal Anti- Inflammatory Drug) HOOC O 3 H N Possible sites of ozone attack Ref.: Sein et al. (2008), Environ. Sci. Technol. 42, 6656
13 Degradation of Micropollutants: Example Diclofenac O C CH 2 OH H N O 3 O O C OH O CH 2 O N H O C OH CH 2 - O 3. N - H + O 3 + H 2 O OH + O 2 + OH Ref.: Sein et al. (2008), Environ. Sci. Technol. 42, 6656
14 [Diclofenac] and [Products] / µm Diclofenac Degradation in Presence of t-buoh COOH CH 2 N O [Ozone] / µm ([Diclofenac] 0 = 50 µm) Diclofenac Iminoquinone (major intermediate) 2,6-Dichloroaniline Ref.: Sein et al. (2008), Environ. Sci. Technol. 42, 6656
15 Suggested Reaction Mechanism for the Formation of the Iminoquinone Intermediate CO 2 H CH 2. N CO 2 H CH 2 O 3 / - O N 2. O H 1,2 H-shift HO. CO 2 H CH 2 N O 2 Iminoquinone O CO 2 H CH 2 N - HO 2. HO O O CO 2 H CH 2 N Ref.: Sein et al. (2008), Environ. Sci. Technol. 42, 6656
16 Pilot-Scale Study
17 SEBES Syndicat des Eaux du Barrage d'esch-sur-sûre Provides drinking water for ca. 80% of the population of Luxemburg The drinking water treatment plant was build up in 1969 SEBES Modernization of treatment and increase of water production to m 3 /d planned Surface area: 3,8 km 2 Capacity: 60 Mill. m 3
18 Simplified Scheme of the Pilot Plant Raw Water Preozonation ph Adjustment/Flocculation Membrane Filtration ph Adjustment/Flocculation Membrane Filtration Postozonation Biological Filtration
19 Pilot Study SEBES
20 t[s] Accompanying Lab Studies: Ozone Scavenging RW O3 UF O3 UF AOP c(o3) [mg/l] Ozone half life time vs. ozone dose preozonation (RW O 3 ), postozonation (UF O 3 ) and AOP O 3 /H 2 O 2 (UF AOP)
21 Ozone exposure [M s] Accompanying Lab Studies: Disinfection Efficiency 0,03 0,025 0,02 0,015 0,01 99% inactivation B. subtilis spores RW O3 UF O3 UF AOP 0, c(o 3 ) [mg/l] Ozone exposure vs. ozone dose; preozonation (RW O 3 ), postozonation (UF O 3 ) and AOP O 3 /H 2 O 2 (UF AOP); reaction time 500 s, DOC: raw water 2 mg/l, UF filtrate 1 mg/l, alkalinity: 0.4 mm, ph: 7
22 Accompanying Lab Studies: Bromate Formation Potential c(bro 3 - )[µg/l] 25 UF O Bromate drinking water standard Bromate TLV RW O 3 UF AOP c(o 3 ) [mg/l] Bromate formation vs. ozone dose, c(br - ): 20 µg/l, complete ozone depletion, preozonation (RW O 3 ), postozonation (UF O 3 ) and AOP O 3 /H 2 O 2 (UF AOP), DOC: RW 2 mg/l, UF 1 mg/l, Alkalinity: 0.4 mm, ph: 7
23 Design of Postozonation
24 Design of Postozonation Q = 1 m 3 /h c(o 3 ) = 1, 3, 5 mg/l c(h 2 O 2 ) = ca. c(o 3 ) Reaction time = 10 min PN 2 PN 3 PN 1 H 2 O 2
25 Residual conc. in % Pilot: Micropollutant Elimination Ozon dose UF O 3 1 mg/l O 3, PN 3 MTBE Dichlorobenzamide Bentazone Carbamazepine Diclofenac Sulfadiazine Raw water Flocculation/UF UF O3 AC filter k O3 : < 10, 700, > 10 3 M -1 s -1
26 Concentration [µg/l] Pilot: Micropollutant Elimination 1,2 1 0,8 0,6 0,4 OH 0,2 H 2 N O S O PN1 PN2 PN3 Sampling point Complete ozone consumption O No transformation of Chlorthalonil M12 by O 3 or OH N AOP O 3 /H 2 O 2, O 3 4 mg/l, H 2 O 2 17 mg/l DOC 1 mg/l, Alkalinity: 0.4 mm, ph: 7
27 Summary of Pilot Study Reservoir O 3 (Preozonation) Intermediate disinfection Intermediate oxidation efficiency Flocculation + UF Bromate formation at high ozone doses O 3 (Postozonation) Good disinfection Lowered oxidation efficiency Increased bromate formation Disinfection modus Synergy via switch between two modi O 3 + H 2 O 2 (Post AOP) Poor disinfection High oxidation efficiency Bromate formation can be controlled Oxidation modus
28 Full-Scale Implementation
29 Research projects Reine Ruhr Elimination of pharmaceutical residues in municipal wastewater treatment plants (WWTP: Schwerte, Bad Sassendorf & Duisburg-Vierlinden) Final report: sser.htm Project management: Dr. Thomas Grünebaum (Ruhrverband, Essen) Lehrstuhl für Siedlungswasserwirtschaft und Umwelttechnik Institut für Siedlungswasserwirtschaft und Abfalltechnik Abteilung für Hygiene, Sozial- und Umweltmedizin 45
30 Elimination [%] Elimination of Selected Target Compounds in Large Scale WWTP Elimination [%] Jochen Türk, IUTA mg Ozone/L, z spec = n.d mg Ozone/L, z spec =
31 Take-home Messages Oxidative Processes can be used to meet (additional) goals of water and wastewater treatment Optimized technical use requires a profound understanding of chemistry of oxidant species including formation of oxidation byproducts For micropollutant elimination detailed knowledge of transformation reaction is needed but enormous effort needed Comprehensive economical and effect-orientied evaluations are still largely lacking
32 Acknowledgements Current and Previous Coworkers in Oxidative Processes: Alexandra Jarocki, Alexandra Beermann, Maike Cyris, Agnes Tekle- Rötering, Sebastian Kowal, Alaa Salma, Myint Sein, emens von Sonntag, Jochen Türk, numerous students Collaborators: Urs von Gunten, Georges Kraus, Jean-Paul Lickes, Stefan Panglisch, André Tatzel Funding: Deutsche Forschungsgemeinschaft, BMWi/AiF, BMBF, Deutsche Bundesstiftung Umwelt, Wasserchemische Gesellschaft, EU MC-ITN ATWARM ANAKON 2011, Zürich Wasser 2012, Neu-Ulm
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