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Antibiotics in Our Streams How Much is There and Where Are They Coming From?

Antibiotics in Our Streams How Much is There and Where Are They Coming From?. Colorado State University Kenneth Carlson (kcarlson@engr.colostate.edu) Sung-Chul Kim Shinwoo Yang October, 2005. Annual Antimicrobials Usage. 2002 Animal Health Industry Sales. Human Used Pharmaceuticals:

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Antibiotics in Our Streams How Much is There and Where Are They Coming From?

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  1. Antibiotics in Our StreamsHow Much is There and Where Are They Coming From? Colorado State University Kenneth Carlson (kcarlson@engr.colostate.edu) Sung-Chul Kim Shinwoo Yang October, 2005

  2. Annual Antimicrobials Usage 2002 Animal Health Industry Sales

  3. Human Used Pharmaceuticals: STP as point source Veterinary Pharmaceuticals: Manure as fertilizer  Soil  Surface Runoff or Leaching through sub-surface Risk to Drinking Water and Watershed Ecology Sources, Distribution and Sinks of Pharmaceuticals in the Environment Sources from: K Kummerer, Pharmaceuticals in the Environment, Springer

  4. Main Objectives • Monitoring Occurrence of Human and Animal Antibiotics in Water and Sediment • Monitoring Occurrence in Animal Waste Lagoons and Manure • Evaluating Transport Pathways and Mechanisms • Evaluating Fate of Antibiotics and Waste Management Practice (BMPs)

  5. Tetracyclines a pKa Compounds R R R R 1 2 3 4 pK pK pK 1 2 3 Oxytetracycline(OTC) O H OH C H H 3.3 7.3 9.1 3 3.3 7.4 Chlortetracycline(CTC) H OH Cl 9.3 Minocycline(MNC) H H H 2.8 5.0 7.8 Demeclocycline(DMC) H OH H Cl Melocycline(MCC) OH CH - Cl 2 Tetracycline(TC) H OH CH H 3.3 7.7 9.7 3 3.5 7.7 Doxycycline(DXC) O H H CH H 9.5 3

  6. N O S C H 3 N Cl N N N C H N 3 C H 3 C H O 3 N N C H O N C H N 3 3 Sulfonamides R Name R pKa Name Sulfametho - Sulfathiazole xazole (STZ) (SMX) Sulfachloro - Sulfamerazine pyridazine (SMR) (SCP) Sulfadimeth - Sulfamethazine oxine (SMT) (SDM)

  7. Macrolides Tylosin Erythromycin Roxithromycin

  8. Ionophores Monensin Naracin Salinomycin

  9. Main Objectives • Monitoring Occurrence of Human and Animal Antibiotics in Water and Sediment • Monitoring Occurrence in Animal Waste Lagoons and Manure • Evaluating Transport Pathways and Mechanisms • Evaluating Fate of Antibiotics and Waste Management Practice

  10. Solid Phase Extraction (SPE) Procedure 3mL MeOH 3mL HCL(5%,v/v) 3mL DI Flow Rate 2mL/min 33mL DI Water 22.5mL MeOH HLB

  11. Schematic Diagram of the Sediment Sample Preparation Sample (Air dried) TCs and SAs: Mcllvaine Buffer Solution (pH 4.0) MLs and IPs: Ammonium Hydroxide Buffer (pH 10.0) Pre-Extraction Clean-up (SPE) Evaporation and Reconstitution Nitrogen Gas Water Bath (50C) 50l Sample + 70l mobile phase A HPLC/MS/MS Analysis

  12. High Performance Liquid Chromatography Tandem Mass Spectrometry (HPLC/MS/MS)

  13. Quality Assurance: Recovery,Limit of Quantification (LOQ)

  14. Sampling Sites Description Sampling Site 1: Pristine watershed Sampling Site 2: Rural landscape Sampling Site 3: Urban influenced Wastewater Reclamation Facility Sampling Site 4: Heavily agricultural influenced area Sampling Site 5: Both urban and agricultural influenced area  Sampling Sites  Dairy ■ Feedlots ▲ Ranches ★USGS Gages

  15. Site 2 - Aqueous No observed concentration in May and April except Narasin Local small farm might contribute the detection of Narasin Higher concentration in February with high detect frequency For TCs and SAs

  16. Site 3 - Aqueous Higher concentration of human used antibiotics or antimicrobials High concentration of ETM-H2O in low flow and cold temperature

  17. Site 4 - Aqueous 3 IPs were detected

  18. Site 5 - Aqueous Higher concentration of MNS in May

  19. Site 2 - Sediment No measurement for MLs and IPs in February More frequent detection compared to aqueous

  20. Site 3 - Sediment Higher concentration In February for TCs and SAs No IPs except Narasin

  21. Site 4 - Sediment Higher concentration in August for SMT, ETM-H2O, and IPs High concentration Of CTC, STZ, and TLS

  22. Site 5 - Sediment Combination of human used And veterinary medicines

  23. Summary of Measured Concentration at watershed

  24. Pseudo Partitioning Coefficient • Sources from: J Tolls, Environmental Science and Technology (2001), 35, 3397 - 3406

  25. Animal Waste Operations Operation Lagoon Water Manure Dairy 7 7 B eef 6 5 Hog 10 5 Sheep 2 4 Turkey 0 2

  26. Animal Waste Operations

  27. Animal Waste Operations

  28. Animal Waste Operations

  29. Animal Waste Operations

  30. Animal Waste Operations

  31. Column Leaching Experiments • Purposes • Evaluating potential mobility of antibiotics • Estimating partition coefficient (Kd) • Comparing surface runoff field experiment • Expected Results • Mobility: Sulfonamides > Macrolides > Ionophores > Tetracyclines • Kd values: Tetracyclines > Ionophores > Macrolides > Sulfonamides

  32. ID Site name or description Averaged Mean Stream Flow (cfs) a A Eaton Canal 195 B Local Ditch - C Eaton Canal 195 D Graham Seep Ditch 3 E Greeley #2 Canal 119 F Graham Seep Ditch 3 G Eaton Canal 195 H Greeley #2 Canal 119 I Greeley #2 Canal 119 M Agricultural Area 45 N Urban and agricultural combined area a Averaged mean stream flow of canal or ditch was provided by Cache la Poudre River water commitioner and river mean stream flow was adapted from U.S. Geological Survey (USGS). Unknown data is not shown. Mass Loading From Local Irrigation Ditches to Watershed Inflow MNS: 13.0 SLM: 6.0 NRS: 12.6 Outflow MNS: 0.3 SLM: 0.3 NRS: 0.6 Mass Flux MNS: 1.9 SLM: 5.0 NRS: 4.5 Inflow TC: 153.4 CTC: 266.4 Outflow TC: 2.5 CTC: 2.9 Mass Flux TC: 1.6 CTC: 1.1 Inflow STZ: 6.2 SMT: 151.3 Outflow STZ: 0.3 SMT: 3.0 Mass Flux STZ: 4.6 SMT: 2.0 Inflow ETM-H2O: 48.2 TLS: 118.3 Outflow ETM-H2O: 2.1 TLS: 4.2 Mass Flux ETM-H2O: 4.4 TLS: 3.5 Unit of Inflow and Outflow: ton/yr, Mass Flux: %

  33. Conclusions • Occurrence frequency high in semi-arid watershed • Sediment-partitioned concentrations much higher • With different site characteristics and land use, concentration of human and animal antibiotics varies significantly – BMPs can be developed • Surface runoff may contribute to the release of antibiotics or antimicrobials to the environment • Local irrigation ditches might act as intermediate transport pathways

  34. Acknowledgement Colorado State University Dr Amy Pruden Dr Jessica Davis Kathy Doesken Support: United States Department of Agriculture (USDA) National Integrated Water Quality Program Integrated Research, Education, and Extension Competitive Grants Program

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