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Physicochemical Controls on Transport of
Veterinary Pharmaceuticals and Hormones
to Surface Waters
Cheng-Hua Liu, Ya-Hui C...
 U.S.: about 14,600
tons of antibiotics in
livestock production
 China: about 84,240
tons of antibiotics in
livestock pr...
Antibiotics in ecosystems exert
selection pressure on bacteria
for antibiotic resistance.
Futures Magazine,
AgBioResearch, MSU
Spring/Summer, 2015
Black carbon (BC) up to 45%
of SOC
Czimczik & Masiello, 2007
BC o...
Biochar soil amendment to
reduce the transport &
bioavailability of antibiotics
Biochar amended Soil
leaching selective
pr...
Sequestration of lincomycin
 Lincomycin, one of lincosamides, is persistent and
frequently detected in the environment.
...
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0 100 200 300 400 500 600 700 800
0
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BM600 pH = 6.0
BM600 pH = 9.8
Langmuir
qt
(g/g)
Ct
(g/L)...
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BM600 pH = 6.0
BM600 pH = 9.8
Amountlincomycinsorbed(g/g)
NaCl Concentration (M)
pH a...
antibiotics
OC release
Extractable OC
released from bull
manure biochar
(produced by 300oC)
in DI water
Dissolved BC = 11%...
Facilitated antibiotics transport by fine
biochar particles
inlet
outlet
A
B
A: Background Solution
B: Antibiotics/BC Susp...
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Completed and ongoing work
 Sorption screening test of 35 biochar samples under pH 6
and pH 9 for 2 and 30 days, respecti...
Peer-Reviewed Journal Publications
Liu, C.-H., Y.-H. Chuang, H. Li, B.J. Teppen, S.A. Boyd, J.M. Gonzalez, C.T. Johnston, ...
Acknowledgment
• Collaborators: Drs. Yingjie Zhang
(MSU), Bin Gao (UF), Johannes
Lehmann (Cornell), Jingdong Mao
(Old Domi...
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Physicochemical Controls On Transport of Veterinary Pharmaceuticals And Hormones To Surface Waters

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Physicochemical Controls On Transport of Veterinary Pharmaceuticals And Hormones To Surface Waters

  1. 1. Physicochemical Controls on Transport of Veterinary Pharmaceuticals and Hormones to Surface Waters Cheng-Hua Liu, Ya-Hui Chuang, Wei Zhang, Hui Li, Brian J. Teppen, Stephen A. Boyd Department of Plant, Soil and Microbial Sciences, Michigan State University, East Lansing, MI Javier M. Gonzalez, National Soil Erosion Research Lab, USDA-ARS, West Lafayette, IN Cliff T. Johnston, Dept. of Agronomy, Purdue University, West Lafayette, IN Washington, DC, October 12, 2016
  2. 2.  U.S.: about 14,600 tons of antibiotics in livestock production  China: about 84,240 tons of antibiotics in livestock production Antibiotics have been widely detected in soils, sediments, and waters. Why Antibiotics?
  3. 3. Antibiotics in ecosystems exert selection pressure on bacteria for antibiotic resistance.
  4. 4. Futures Magazine, AgBioResearch, MSU Spring/Summer, 2015 Black carbon (BC) up to 45% of SOC Czimczik & Masiello, 2007 BC on average 13.7% of SOC Reisser et al., 2016 DBC about 11% of DOC in surface waters Jaffé et al., 2013 Physicochemical control on fate and transport of antibiotics  Sorption to soil phases  Facilitated transport of antibiotics by fine particles Lehmann, 2007. Nature
  5. 5. Biochar soil amendment to reduce the transport & bioavailability of antibiotics Biochar amended Soil leaching selective pressure Plant uptake Sorption Primary soil geosorbents: amorphous organic matter (AOM), black carbon (BC) & clay (CL)
  6. 6. Sequestration of lincomycin  Lincomycin, one of lincosamides, is persistent and frequently detected in the environment.  MW: 406.54 g/mol  logKow: 0.2  Sw: 927 mg L-1  pKa: 7.6 0 2 4 6 8 10 12 14 0 20 40 60 80 100 Fraction(%) pH pKa = 7.6 LMC+ LMC0 Cheng-Hua Liu Liu, C.-H.; Chuang, Y.-H.; Li, H.; Teppen, B. J.; Boyd, S. A.; Gonzalez, J. M.; Johnston, C. T.; Lehmann, J.; Zhang, W., Sorption of Lincomycin by Manure-Derived Biochars from Water. J. Environ. Qual. 2016, 45, (2), 519-527.
  7. 7. 0 20 40 60 80 100 120 140 160 180 200 0 200 400 600 800 1000 0 20 40 60 80 100 120 140 160 180 200 0 200 400 600 800 1000 0 20 40 60 80 100 120 140 160 180 200 0 200 400 600 800 1000 0 20 40 60 80 100 120 140 160 180 200 0 200 400 600 800 1000 BM300 BM400 BM500 BM600 DM300 DM400 DM600 PS300 PS400 PS500 PS600 qt (g/g) Time (day) RDW500 DDM500 DDM600 CDM500 CDMW500 WW500 𝒒 𝒕 = 𝑲𝒊𝒅 𝒕 𝟏/𝟐 + 𝑪 Long-termsorptionkinetics Intra-particlediffusionmodel Short-term fast surface reaction Long-term slow pore diffusion Biochar had long-term sequestration potential for antibiotics.
  8. 8. 0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 BM600 pH = 6.0 BM600 pH = 9.8 Langmuir qt (g/g) Ct (g/L) LMC LMC LMC Electrostatic interactions LMC Non-electrostatic interactions LMC LMC 0 2 4 6 8 10 12 14 0 20 40 60 80 100 Fraction(%) pH pKa = 7.6 LMC Non-electrostatic interactions 2-day quasi-sorption isotherm Biochar surface pH << pkapH =6 Biochar surface pH >> pkapH =10
  9. 9. 0 0.01 0.05 0.1 200 300 400 500 600 BM600 pH = 6.0 BM600 pH = 9.8 Amountlincomycinsorbed(g/g) NaCl Concentration (M) pH and ionic strength effects LMC LMC 0 2 4 6 8 10 12 14 0 20 40 60 80 100 Fraction(%) pH pKa = 7.6 Na Na Na pH << pKa LMC LMC LMC Biochar surface Na Na Na Na Na LMC Na Na Biochar surface pH >> pKa
  10. 10. antibiotics OC release Extractable OC released from bull manure biochar (produced by 300oC) in DI water Dissolved BC = 11% of DOC in surface water BM300 BM400 BM500 BM600 DM300 DM400 DM600 PS300 PS400 PS500 PS600 CDM500 CDMW500 DDM500 DDM600 FW500 FW600 RDM500 PW500 PW600 WW500 YL500 BS500 TS500 TW500 ARS450 CS300 CS400 CS600 OK300 OK400 OK600 Pi300 Pi400 Pi600 MC600 KW450 DSW_ CB500 BSG500 BP300 BP450 BP600 BG300 BG450 BG600 0 4 8 12 16 20 24 28 Extractableorganiccarbon(%) ADOC WDOC BDOC Base-extractable OC could be up to 24% of total carbon in biochars
  11. 11. Facilitated antibiotics transport by fine biochar particles inlet outlet A B A: Background Solution B: Antibiotics/BC Suspension Peristaltic Pump Fraction Collector Column UV-Vis LC/MSMS Solution pH 7 Lincomycin (LCM) pKa 7.6, 80% cations Oxytetracycline (OTC) pKa 3.2, 7.5, 8.9; 74% zwitterions Sulfamethoxazole (SMX) pKa 1.6, 5.7; 95% anions
  12. 12. 0 1 2 3 4 5 6 7 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 0 1 2 3 4 5 6 7 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 0 1 2 3 4 5 6 7 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 C/C0 LCM only BC/LCM_Free LCM BC/LCM_BC-co-transported LCM Pore volume 0.1 mM 1 mM 10 mM IS(mM) MR(%) Free-LCM BC-sorbed LCM Total LCM 0.1 49.4 - 49.4 1 86.6 - 86.6 10 96.5 - 96.5 LCM-BC 0.1 3.3 75.4 78.7 1 7.6 16.9 24.4 10 15.8 2.0 17.8 Colloid-facilitated transport has higher environmental risk Solute transport has higher environmental risk Desorption from immobile BC should also be concerned
  13. 13. Completed and ongoing work  Sorption screening test of 35 biochar samples under pH 6 and pH 9 for 2 and 30 days, respectively (completed)  180-day sorption kinetics and two-day quasi-equilibrium sorption studies for 4 biochar samples (completed)  360-day long-term sorption kinetics for 17 biochars (completed)  Attenuation effect of sorption by organic acids (completed)  Quantification and characterization of extractable organic carbon from biochar (completed)  Facilitated transport of antibiotics by fine biochar particles: ionic strength (completed), and pH effect (ongoing)  Rainfall simulation study with soil box (ongoing)
  14. 14. Peer-Reviewed Journal Publications Liu, C.-H., Y.-H. Chuang, H. Li, B.J. Teppen, S.A. Boyd, J.M. Gonzalez, C.T. Johnston, J. Lehmann, and W. Zhang. 2016. Sorption of lincomycin by manure-derived biochars from water. Journal of Environmental Quality, 45(2), 519-527. Stoof, C.R., A.I. Gevaert, C. Baver, B. Hassanpour, V.L. Morales, W. Zhang, D. Martin, S.K. Giri, and T.S. Steenhuis. 2016. Can pore-clogging by ash explain post-fire runoff? International Journal of Wildland Fire, 25(3), 294-305. Wang, B., W. Zhang, H. Li, H. Fu, X. Qu, and D. Zhu. 201_. Micropore clogging by dissolved black carbon: A new perspective on sorption irreversibility and kinetics of hydrophobic organic contaminants to black carbon. Environmental Pollution (in revision). Liu, C.-H., Y.-H. Chuang, H. Li, B.J. Teppen, S.A. Boyd, and W. Zhang. 201_. Dependence of lincomycin sorption on biochar physicochemical properties (in preparation). Liu, C.-H., Y.-H. Chuang, H. Li, B.J. Teppen, S.A. Boyd, and W. Zhang. 201_. Long-term sorption kinetics of lincomycin to manure-derived biochars (in preparation). Liu, C.-H., Y.-H. Chuang, H. Li, S.A. Boyd, J. Lehmann, B.J. Teppen, J.D. Mao, and W. Zhang. 201_. Quantification and characteristics of dissolved organic matter released from biochars (in preparation). Liu, C.-H., Y.-H. Chuang, H. Li, J.P. Zarnetske, S.A. Boyd, B.J. Teppen, and W. Zhang. 201_. Black carbon nanoparticles facilitated transport of antibiotics in saturated porous media (in preparation). 12 conference presentations & 16 invited presentations. 3 graduate students, 1 postdoc, 1 visiting student, & 1 high school student.
  15. 15. Acknowledgment • Collaborators: Drs. Yingjie Zhang (MSU), Bin Gao (UF), Johannes Lehmann (Cornell), Jingdong Mao (Old Dominion Univ.), Verónica L. Morales (ETH Zurich), Dongqiang Zhu (Peking University). The research was supported by Agriculture and Food Research Initiative Competitive Grant No. 2013-67019-21377 from the USDA National Institute of Food and Agriculture. Thank you!

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