Fate of pharmaceuticals (PhCs) in sewage sludge and proposal of indicator substances for monitoring Sabine Konradi, Ines Vogel, Environmental Agency in Dessau, Germany Workshop „Pharmaceuticals in Soil, Sludge and Slurry” 18 th of June 2013, Dessau, Germany
Fate of PhCs in sludge and proposal of indicator substances Overview Aim of the talk 1. Regulation sewage sludge usage in agriculture Provoke Discussion on 2. Fate of PhCs during How to sewage treatment classify and predict 3. Priorization strategy fate and effects of PhCs 4. Fate of PhCs in sludge/soil in sludge and soil 5. Terrestrial Ecotoxicity PhCs based on literature data? 6. List of indicator substances 7. Conclusion and future Research
How are human PhCs distributed in the environment? faeces, urine Disposal sewage sewage into toilett sewage treatment sewage sludge as sewage sludge as plant (STP) fertilizer for agriculture fertilizer for agriculture surface water soil plants groundwater mikro- drinking water organisms insects worms
Why addressing PhCs in sewage sludge? Disposal of 2.100.000 tons Ts/year sewage sludge in Germany Disposal of 2.100.000 tons Ts/year sewage sludge in Germany ~ 1Mio t/a Landscaping of sewage sludge disposed on soil Burning No regulation Agriculture for PhCs (Statist. Bundesamt 2009) adopted from Prof. Ulf Theilen , Kompetenzzentrum ZEuUS, Presentation: Zukunft Klärschlammverwertung und -entsorgung
German sewage sludge usage ordinance Good news: In agriculture is under revision Draft of German “Abfallklärschlamm Verordnung” AbfklärV Regulation on oganic pollutants Category1: Previously Category3: pollutants of concern that regulated pollutants are not regulated Ø Dioxines / Furane Ø Phtalates, Ø Triclosan Ø PCB No threshold values but Monitoring lower threshold values New concept of sewage sludge Category2: Pollutants currently at quality certificates high environ. concentrations Monitoring via certified organisations Ø PAH Polyaromatic Hydrocarbons Ø PFT perfluorated tensides NEW: Hygiene Standards for sewage New legal limit values sludge to kill pathogenes Category4: pollutants that are Bad news: no regulation, readily degradable, monitoring planned for PhCs No limit values, no Monitoring adopted from a Presentation of Prof. Ulf Theilen, Kompetenzzentrum ZEuUS, TH Mittelhessen
HOWEVER: Since Draft is still under debate Overview We aim to provide scientific evidence for PhCs of concern in sludge and soil 1. Regulation sewage sludge to suggest for usage in agriculture regulatory monitoring (category 3) 2. Fate of PhCs during sewage treatment Identify indicator PhCs of high concern 3. Priorization strategy • high occurrence in sludge and soil 4. Fate of PhCs in sludge/soil • high sorption potential • low degradation 5. Terrestrial Ecotoxicity PhCs • toxic to terrestric organisms 6. List of indicator substances 7. Conclusion and future Research
What fate of PhCs in sewage treatment plant STP? Waste water INFLUENT Conventional Monitoring Pharmaceuticals and Metabolites C PhC Only Concentrations: Influent, Effluent Sorption Sorption Too simple view Pharmaceutical (l) Pharmaceutical (s) Conventional clearance Biological Biological S transformation transformation T Minera- Minera- C influent - Ceffluent = lisation lisation P removal from water Transformation phase Product CH4 C02 H2O Sorption to sludge Solid phase Water phase metabolites and NER are not considered SEWAGE SLUDGE EFFLUENT Pharmaceutical (ER) Pharmaceutical (l) Metabolites (s) + NER C PhC Metabolites (l)
Sewage Sludge is a sink for pollutants Waste water INFLUENT Conventional Monitoring Pharmaceuticals and Metabolites C PhC Only Concentrations: Influent, Effluent Sorption Sorption Pharmaceutical (l) Pharmaceutical (s) HOWEVER Accumulation of pollutants High amount of Pollutants can S waste water accumulate in sludge Sludge throughput T because of recycling P sludge recycling long retention time Retention time Retention time 6-12 hours about 10-60 Days Sludge is a sink for Solid phase Water phase pollutants SEWAGE SLUDGE EFFLUENT Pharmaceutical (ER) Pharmaceutical (l) C PhC Metabolites (l)
Occurrence of PhCs in sewage and sludge Psychiatric Psychiatric Analgesics/ Analgesics/ drugs Lipid regulators Antibiotics Beta blocker Hormones Hormones Anti- inflammatories Anti inflammatories Ciprofloxacin Estradiol Bezafibrate Cabamacepine Dicolofenac Fenofibrate Clarithromycin Gemfibrozil Roxithromycin Bergmann A. Monitoring Data on environment concentration of Pharmaceuticals, UBA-FB 001525 Bergmann A. Monitoring Data on environment concentration of Pharmaceuticals, UBA-FB 001525 Zusammenstellung von Monitoring Daten zu Umweltkonzentrationen von Arzneimitteln
Consumption of human antibiotics ~ 450-600t/year in Germany 2002 2006 2007 2008 2009 substance/year 160 tons active 140 120 100 80 60 40 20 0 2002 2007 2009
Fate of PhCs in sewage treatment plant (STP) Waste water INFLUENT Pharmaceuticals and Metabolites Sorption Sorption Pharmaceutical (l) Pharmaceutical (s) Extractable Non-extractable Biological Biological Residue (ER) Residue (NER) S transformation transformation T Minera- Minera- Biological Biological lisation lisation P transformation transformation Transformation Product Min Min CH4 C02 H2O C02 Transformation +H2O Product Solid phase Water phase SEWAGE SLUDGE EFFLUENT Pharmaceutical (ER) Pharmaceutical (l) Metabolites (s) + NER Metabolites (l)
Fate of PhCs in sewage treatment plant (STP) Waste water INFLUENT Conventional Monitoring Pharmaceuticals and Metabolites C Only Concentrations: Influent, Effluent K D sludge % in sludge Sorption Sorption Pharmaceutical (l) Pharmaceutical (s) Research Experiments Extractable Non-extractable Fate/Dissipation of PhCs Biological Biological Residue (ER) kbiol Residue (NER) S • Sorption K D , % sludge transformation transformation T % Transf. Minera- Minera- • Biolog. Transformation Biological Biological lisation lisation P transformation transformation - Transformation rate kbiol. Transformation - % transformation efficiency Product Min Min CH4 C02 H2O C02 Transformation +H2O Product Solid phase Water phase SEWAGE SLUDGE EFFLUENT C C Pharmaceutical (ER) Pharmaceutical (l) Metabolites (s) + NER Metabolites (l)
Flow chart of classification strategy Bergmann 2011 Monitoring Data on Bergmann 2011 Monitoring Data on Start Start Verlicchi P et al. (2012) Review Verlicchi P et al. (2012) Review environment concentration of environment concentration of Monitoring Data 23PhCs Monitoring Data 23PhCs Fate of Pharmaceuticals Fate of Pharmaceuticals Pharmaceuticals Pharmaceuticals Literature Study Literature Study Occurrence Occurrence FATE in STP FATE in STP Phys-Chem. Phys-Chem. in sludge Sorption, Biological Transformation Sorption, Biological Transformation Properties Properties Classification in 0 - 5 no (0) => high relevance (5) Classification in 0 - 5 no (0) => high relevance (5) Total classification Average for occurrence and fate => Ranking Total classification Average for occurrence and fate => Ranking PhCs high Priority PhCs high Priority PhCs high Priority PhCs high Priority PhCs low Priority PhCs low Priority No Risk No occurrence data No occurrence data + Occurrence data + Occurrence data Fate in sludge excluded 7 PhCs 15 PhCs 8 PhCs Terrestrial Final Candidates Final Candidates FATE in Soil Koc FATE in Soil Koc Eco-toxicity for monitoring Verlicchi P et al. 2012 Occurrence of Pharmaceutical Compounds in Urban Wastewater: Removal, Mass Load and Environmental Risk after a Secondary Treatment - A Review
Classification of Occurrence Data - Classification according to range of monitoring data - Maximum concentration observed in STP in Germany were selected - Concentration in sludge in µg/kg normalized to 100% Total solids - concentration in sludge not directly comparable to influent conc. estimated 10% TS Concentration Concentration Class Concentration sludge 10%TS sludge 100%TS concentration Influent µg/L µg/kg µg/kg Very low 0 < 0.1 < 0.1 < 1 1 0.1 — 1 0.1 — 1 1 — 10 low 2 1 — 5 1 — 5 10 — 50 moderate 3 5 — 10 5 — 10 50 — 100 intermediate high 4 10 — 50 10 — 50 100 — 500 5 >50 >50 >500 very high
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