January 2014 Slow Sand Filtration (Biofilm reactors): a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas, Kai Bester Department of Environmental Science, Aarhus University, Roskilde, Denmark 1 moes@dmu.dk kb@dmu.dk Disposition › Background › Objectives › The Set-up and Results › Discussion and Conclusion Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Background: The Problem XENOBIOTICS CONVENTIONAL WATER TREATMENT MICROPOLLUTANTS Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Background: Possible Solutions › Activated carbon and Reverse Osmosis TRAB act. carbon › Advanced Oxidation Processes Bouillides WTP › Biological Processes Rielli.com Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Background: Biofilm Reactors › Biofilm Reactors = porous media + biofilm (Biofilters) (Sand) › Affordable, robust and suitable for small WWTP’s › Constructed soil biofilters eliminate micro-pollutants from wastewater effluents. › Effectiveness: hydraulic residence-time, compounds residence time and biological activity. › Mechanisms and most efficient biofilm reactor configuration? Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Disposition › Background › Objectives › The Set-up and Results › Conclusion Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Objective: Efficiency XENOBIOTICS CONVENTIONAL WATER TREATMENT MICROPOLLUTANTS BIOFILM REACTOR (Filter media and biofilms) SORPTION + DEGRADATION Sorption or degradation? Transport? Aerobic or anaerobic? %? Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Aim: Understanding mechanisms What is happening in the reactor? › Adsorption or degradation? › Observed removal in soil = adsorption + degradation › Observed removal in sand ≈ degradation › Transport? › Observed transport in soil = adsorption + porosity › Observed transport in sand ≈ porosity › Sand particles known size and even distribution Quartz-sand biofilm reactor › Aerobic or anaerobic? › Aerobic degradation >> Anaerobic degradation › Sand-based biofilm reactor operated aerobically Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Disposition › Background › Objectives › The Set-up and Results › Conclusion Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 The Set Up: Which compounds? Pharmaceuticals Diclofenac and propranolol Detected in WWTP’s effluents (ng L-1 ) Diclofenac Fungicides Propiconazole and tebuconazole. Detected in WWTP’s effluents (ng L-1 ) Tebuconazole X-ray contrast media Iopromid, iohexol and iomeprol Detected in WWTP’s effluents (µg L-1 ) Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas Iohexol January 2014 The Set-up: Biofilm reactor TRANSPORT Ø = 5 cm2 On-Line measurements 29 cm REMOVAL Tank ”WWTP” Effluent Tank ”clean” + Oxygen consumption + TOC Off-line measurements Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Transport: Results Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 The Set Up: Biofilm reactor TRANSPORT Ø = 5 cm2 Off-line measurements 29 cm REMOVAL Tank ”WWTP” Effluent Tank ”clean” + Oxygen consumption + TOC Off-line measurements Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Removal: Oxygen and TOC Oxygen (mg / L) 10 9 8 7 6 5 4 3 2 1 0 TOC (mg C / L) 12 27% 10 8 6 60% 0% 27% 4 2 0 25 µl/min 200 µl/min Inlet Outlet 25 µl/min 200 µl/min Inlet Outlet Oxygen consumption and TOC removal for min. and max. flows Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Removal: Method Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 15 Removal: kinetics (k’s) Agrees with O2 and TOC… -5 -5 Diclofenac y = -0.0401x R² = 0.93 -3 -3 -1 y = -0.1431x R² = 0.37 -1 0 -5 10 20 30 40 0 50 -5 Iopromid y = -0.0462x R² = 0.81 -3 10 Iohexol -3 20 30 40 50 -5 Iomeprol y = -0.1012x R² = 0.83 -3 0 10 20 30 40 0 50 -2 -2 -1 0 0 0 10 20 30 40 50 10 20 30 40 50 30 40 50 0 10 20 30 40 50 Propiconazole Tebuconazole -1 y = -0.0899x R² = 0.68 -1 -1 -1 ln(Coutlet/Cinlet) Propranolol 0 10 20 Hydraulic Residence Time (h) Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Disposition › Background › Objectives › The Set-up and Results › Discussion and Conclusion Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Similar studies Parameter Present study Reungoat et al. (2011) Scheytt et al. (2006) Matamoros (2007) Water type Real wastewater effluent Real wastewater effluent Syntetic wastewater Raw wastewater Hydraulic loading rate [m3 m-2 h-1] 0.01176 6 0.00917 0.0029 Filter (particle size [mm]) Quartz sand (0.21-0.29) Sand (2.25) Sandy sediment (0.063-0.630) (foc=0.13%) Coarse gravel (8-16) Gravel(0-4) Initial TOC/DOC [mg C L-1] 4.86 and 7.58 11.2 ± 0.4 (DOC) Not tested Not tested HRT [h] 9.01 2 0.108 (unsaturated) 342 Diclofenac Removal (%) 41.7 ± 2 20 ± 10 (graph) 35 39 ± 22 Diclofenac Degr. Rate [h-1] 0.040 (kA=0.0041 m/h*) Not tested 0.37 kA=0.004 m/h* Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Similar studies Parameter Present study Reungoat et al. (2011) Scheytt et al. (2006) Matamoros (2007) Water type Real wastewater effluent Real wastewater effluent Syntetic wastewater Raw wastewater Hydraulic loading rate [m3 m-2 h-1] 0.01176 6 0.00917 0.0029 Filter (particle size [mm]) Quartz sand (0.21-0.29) Sand (2.25) Sandy sediment (0.063-0.630) (foc=0.13%) Coarse gravel (8-16) Gravel(0-4) Initial TOC/DOC [mg C L-1] 4.86 and 7.58 11.2 ± 0.4 (DOC) Not tested Not tested HRT [h] 9.01 2 0.108 (unsaturated) 342 Diclofenac Removal (%) 41.7 ± 2 20 ± 10 (graph) 35 39 ± 22 Diclofenac Degr. Rate [h-1] 0.040 (kA=0.0041 m/h*) Not tested 0.37 kA=0.004 m/h* Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Similar studies Parameter Present study Reungoat et al. (2011) Scheytt et al. (2006) Matamoros (2007) Water type Real wastewater effluent Real wastewater effluent Syntetic wastewater Raw wastewater Hydraulic loading rate [m3 m-2 h-1] 0.01176 6 0.00917 0.0029 Filter (particle size [mm]) Quartz sand (0.21-0.29) Sand (2.25) Sandy sediment (0.063-0.630) (foc=0.13%) Coarse gravel (8-16) Gravel(0-4) Initial TOC/DOC [mg C L-1] 4.86 and 7.58 11.2 ± 0.4 (DOC) Not tested Not tested HRT [h] 9.01 2 0.108 (unsaturated) 342 Diclofenac Removal (%) 41.7 ± 2 20 ± 10 (graph) 35 39 ± 22 Diclofenac Degr. Rate kA kA=0.0041 m/h Not tested nd kA=0.004 m/h Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Comparing data Target compound Propranolol k [h-1] 0.143 % Removal at 98 µl/min 94±2 Other studies Incubated sludge K: 0.096 h-1-0.113 h-1 (S- and R-enantiomers) Ribeiro et al. 2013 Diclofenac 0.040 41±2 Propiconazole Tebuconazole - 17±3 58±4 Iohexol 0.101 57±3 % Removal sand filters 39-35 (Matamoros et al. 2007 Scheytt et al. 2006) No previous data No previous data % Removal MBBR 79 Sand reactor, getting started (Hapeshi et al.2013) Iomeprol 0.090 85±0.2 Iopromide 0.046 58±0.3 No previous data % Removal sand filter - drinking water 13 (Zearley and Summers 2012) Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Conclusions › Sand biofilm reactors are easy to control due to hydraulics and minimized sorption processes › Micro-pollutants (some considered reclacitrant) can be eliminated by the sand biofilm reactor › Operation over 10 months without signs of clogging › Low flows (1000 m 3 h -1 ) filter-area of 85.000 m2 › Biofilter thickness can be increased (meaning less filterarea) Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Acknowdledgements › AUFF grant: Advanced water purification using bio-inorganic nanocatalysts and soil filters. › The personnel of WWTP Bjergmarken that was always extremely helpful considering provisions of samples and data on their WWTP. › Aasbjørn Haaning Nielsen and Jes Vollertsen of Aalborg University helped with setting up the oxygen sensing. Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 Thanks for your attention LITERATURE › Hapeshi, E., Lambrianides, A., Koutsoftas, P., Kastanos, E., Michael, C. and Fatta-Kassinos, D. (2013) Investigating the fate of iodinated X-ray contrast media iohexol and diatrizoate during microbial degradation in an MBBR system treating urban wastewater. Environ Sci Pollut Res Int. › Kadlec, R.H. and Knight, R.L. (1996) Treatment Wetlands, Lewis Publishers, Boca Raton, New York, London, Tokyo. › Matamoros, V., Arias, C., Brix, H. and Bayona, J.M. (2007) Removal of Pharmaceuticals and Personal Care Products (PPCPs) from Urban Wastewater in a Pilot Vertical Flow Constructed Wetland and a Sand Filter. Environmental Science & Technology 41(23), 8171-8177. › Reungoat, J., Escher, B.I., Macova, M. and Keller, J. (2011) Biofiltration of wastewater treatment plant effluent: Effective removal of pharmaceuticals and personal care products and reduction of toxicity. Water Research 45(9), 2751-2762. › Ribeiro, A.R., Afonso, C.M., Castro, P.M.L. and Tiritan, M.E. (2013) Enantioselective biodegradation of pharmaceuticals, alprenolol and propranolol, by an activated sludge inoculum. Ecotoxicology and Environmental Safety 87(0), 108-114. › Scheytt, T.J., Mersmann, P. and Heberer, T. (2006) Mobility of pharmaceuticals carbamazepine, diclofenac, ibuprofen, and propyphenazone in miscible-displacement experiments. Journal of Contaminant Hydrology 83(1–2), 53-69. › Zearley, T.L. and Summers, R.S. (2012) Removal of Trace Organic Micropollutants by Drinking Water Biological Filters. Environmental Science & Technology 46(17), 9412-9419. Sand Biofilm Reactors: a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas January 2014 January 2014 Slow Sand Filtration (Biofilm reactors): a solution to remove micro-pollutants in small WWTP’s effluents? Mònica Escolà Casas, Kai Bester Department of Environmental Science, Aarhus University, Roskilde, Denmark 25 moes@dmu.dk kb@dmu.dk