Transport of veterinary medicines from soils to groundwater
Final Report Abstract
One objective was to study the sorption and desorption behavior of sulfadiazine. Short-and long term sorption experiments were performed with the antibiotic sulfadiazine (SDZ) in the plough layer and the subsoil of a loamy sand (Kaldenkirchen, KAL) and a silty loam (Merzenhausen, MRZ). The parameterization of a two-stage, one-rate sorption model combined with a first-order transformation model showed that sorption of SDZ was nonlinear, time-dependent, and affected by pH, with a higher sorption capacity for the loamy sand. Another objective was to study the transport of veterinary medicines using soil columns with special emphasis on preferential flow, the behavior of 4-hydroxy-sulfadiazine (4-OH-SDZ) and the effect of repeated manuring with sulfadiazine containing piggery waste. No preferential transport or colloid-facilitated transport was observed in any of the column transport studies. An additional (irreversible) sorption site was needed in the model description. Besides chemical interactions, the transport of SDZ was affected by the soils hydraulic behavior, with less leaching for lower infiltration rates. The sorption and kinetic parameters of 4-OH-SDZ were similar to those of SDZ. Repeated application of manure from pigs medicated with 14C-labeled SDZ on soil columns with did not show an influence on the shape of the break through curves and on the formation of transformation products. For yet unknown reasons, the transformation product 4-(2-iminopyrimidin-1(2H)-yl) aniline was only formed in considerable amounts in the absence of manure. By upgrading the two-stage one-rate model of Wehrhan (2010), we were able to describe instantaneous sequestration of sulfadiazine in the residual fraction (RES) obtained by harsh extraction of soil and the non-extractable fraction (NER). One objective was to provide experimental evidence on the occurrence or non-occurrence of antibiotics in the deep leachate of soils using lysimeters under natural weather conditions and to obtain complete balances on the fate of the veterinary medicine sulfadiazine. In the KAL lysimeter leachate we measured on one occasion 7.6 ng/L sulfadiazine together with the breakthrough of the tracer bromide and on 4 occasion’s 2-amino-pyrimidin up to 36 ng/L. The distribution of radioactivity in the upper 30 cm soil profile of the lysimeter showed a further dislocation in deeper soil layers of the 0.5 m2 lysimeter, which was especially the case in the loamy sand soil (KAL). In the silty loam soil (MRZ) we measured a 30 to 40% loss of radioactivity in three years and most of the leftover radioactivity was found in the first 10 cm. Extraction of the soil samples showed a noticeable difference between the KAL and MRZ soil. At day 218, ~50% of the applied radioactivity was found in the NER-fractions for both soils (a value comparable with the results of Forster et al 2009). At day 1022, we still found all applied radioactivity back in the KAL soil, with an increase in the NER fraction. For MRZ, we measured a strong decrease in the RES-fraction, indicating that SDZ and metabolites were possibly mineralized, but also the NER fraction became smaller, indicating that SDZ and metabolites could have become bioavailable from the NER fraction. A batch experiment with 14C-SDZ added to soil from the MRZ lysimeter confirmed that a mineralization of up to 10% of the added SDZ after three months is possible, when incubated at 45% of the max. water holding capacity and up to 50-60%, when incubated as slurry. We could isolate and identify a bacterium capable of partly mineralize sulfadiazine and producing the transformation product 2-amino-pyrimidin. Thus, in contrast to previous results, we have strong evidence that mineralization of SDZ could have been the reason for the loss of radioactivity in the lysimeter experiment and a possible mechanism for a degradation pathway of sulfadiazine in soil.
Publications
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2007. Verlagerung des Veterinärantibiotikums Sulfadiazine in Lysimetern. Lysimeters in the Scope of National and International Regulations, 12. Gumpensteiner Lysimetertagung, 17. und 18. April 2007, Gumpenstein, Österreich. S. 81 – 84
Groeneweg, J., Rützel, H., Pütz, T., Vereecken, H.
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2008. Analysis of aged sulfadiazine residues in soils using microwave extraction and liquid chromatagraphy tandem mass spectrometry. Analytical and Bioanalytical Chemistry, Vol. 391. 2008, Issue 3, pp 1029-1038.
Förster, M., Laabs, V., Lamshöft, M., Pütz, T., Amelung, W.
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2008. Der Transport des Antibiotikums Sulfadiazin in Böden: Welchen Effekt hat die Gülle? Mitteilungen der Fachgruppe Umweltchemie und Ökotoxikologie, 14.2008, S. 98 - 101.
Unold, M., Kasteel, R., Groeneweg, J., Vereecken, H.
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2008. Growth-inhibitory effects of sulfonamides at different pH: Dissimilar susceptibility patterns of a soil bacterium and a test bacterium used for antibiotic assays. Chemosphere, Vol. 72. 2008, Issue 5, pp. 836–843.
Tappe, W., Zarfl, C., Kummer, S., Burauel, P., Vereecken, H., Groeneweg, J.
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2008. Re-evaluation of the conformational structure of sulfadiazine species using NMR and ab initio DFT studies and its implication on sorption and degradation. Chemosphere, Vol. 72. 2008, Issue 10, pp. 1448–1454.
Huschek, G., Hollmann, D., Kurowski, N., Kaupenjohann, M., Vereecken, H.
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2009. Sequestration of manure-applied sulfadiazine in soils. Environmental Science & Technology, Vol. 43.2009, Issue 6, pp. 1824–1830.
Förster, M., Laabs, V., Lamshöft, M., Groeneweg, J., Zühlke, S., Spiteller, M., Krauss, M., Kaupenjohann, M., Amelung, W.
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2009. Transport and transformation of sulfadiazine in soil columns packed with a silty loam and a loamy sand. Journal of Contaminant Hydrology, Vol. 103. 2009, Issues 1–2, pp. 38–47.
Unold, M., Kasteel, R., Groeneweg, J., Vereecken, H.
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2009. Transport of Manure-Based Applied Sulfadiazine and Its Main Transformation Products in Soil Columns. Vadose Zone Journal, Vol. 8. 2009, No. 3, p. 677-689.
Unold, M., Simunek, J., Kasteel, R., Groeneweg, J., Vereecken, H.
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2010. Long-term sorption and desorption of sulfadiazine in soil: Experiments and modeling. Journal of Environmental Quality, Vol. 39. 2010, No. 2, pp. 654-666.
Wehrhan, A., Streck, T., Groeneweg, J., Vereecken, H., Kasteel, R.
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2010. Transformation and sorption of the veterinary antibiotic sulfadiazine in two soils: a short-term batch study. Environmental Science and Technology, Vol. 44. 2010, Issue 12, pp. 4651–4657.
Kasteel, R., Mbo, C.M., Unold, M., Groeneweg, J., Vanderborght, J., Vereecken, H.
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2010. Transport of sulfadiazine in undisturbed soil columns: the effect of flow rate and applied mass. Journal of Environmental Quality, Vol. 39. 2010, Issue 6, pp. 2147-2159.
Unold, M., Kasteel, R., Groeneweg, J., Vereecken H.
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2011. Dissipation and sequestration of the veterinary antibiotic sulfadiazine and its metabolites under field conditions. Environmental Science and Technology, Vol. 45. 2011, Issue 12, pp. 5216–5222.
Rosendahl, I., Siemens, J., Groeneweg, J., Linzbach, E., Laabs, V., Herrmann, C., Vereecken, H., Amelung, W.
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2012. Long-term sorption and sequestration dynamics of the antibiotic sulfadiazine- a batch study. Journal of Environmental Quality, Vol. 41. 2012, No. 5, pp. 1497-1506.
Sittig, S., Kasteel, R., Groeneweg, J., Vereecken, H.
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2012. Persistence of the fluoroquinolone antibiotic Difloxacin in soil and lacking effects on N-turnover. Journal of Environmental Quality, Vol. 412012, No. 4, pp. 1275-1283.
Rosendahl, I., Siemens, J., Kindler, R., Groeneweg, J., Zimmermann, J., Czerwinsky, S., Lamshöft, M., Laabs, V., Wilke, B.M., Vereecken, H., Amelung, W.
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2013. Abundance and transferability of antibiotic resistance as related to the fate of sulfadiazine in maize rhizosphere and bulk soil. FEMS Microbiology Ecology, Vol. 83.2013, Issue 1, pp. 125 - 134.
Jechalke, S., Kopmann, C., Rosendahl, I., Groeneweg, J., Krögerrecklenfort, E., Zimmerling, U., Weichelt, V., Siemens, J., Amelung, W., Heuer, H., Smalla, K.
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2013. Degradation of sulfadiazine by Microbacterium lacus strain SDZm4 isolated from lysimeters three years after manuring with slurry from pigs medicated with 14C-labelled sulfadiazine. Applied and Environmental Microbiology, vol. 79. 2013, no. 8, pp. 2572-2577.
Tappe, W., Herbst, M., Hofmann, D., Koeppchen, S., Kummer, S., Thiele, B., Groeneweg, J.
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2013. Effect of repeated application of sulfadiazine-contamined pig manure on the abundance and diversity of ammonia- and nitrite oxidizers in the root-rhizosphere complex of pasture plants under field conditions. Frontiers in Microbiology, Vol. 4.2013, Article 22.
Ollivier, J., Schacht, D., Groeneweg, J., Engel, M., Wilke, B.M., Kleineidam, K., Schloter, M.
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2013. Effects of slurry from sulfadiazine (SDZ) and Difloxacin (DIF) medicated pigs on the structural diversity of microorganisms in bulk and rhizosphere soil. Soil Biology and Biochemistry,
Vol. 62. 2013, pp. 82–91.
Reichel, R., Rosendahl, I., Peeters, E.T.H.M., Focks, A., Groeneweg, J., Bierl, R., Schlichting, A., Amelung, W., Thiele-Bruhn, S.
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2013. Increased Abundance and Transferability of Resistance Genes after Field Application of Manure from Sulfadiazine-Treated Pigs. Applied and Environmental Microbiology, vol. 79. 2013, no. 5, pp. 1704-1711.
Jechalke, S., Kopmann, C., Rosendahl, I., Groeneweg, J., Weichelt, V., Krögerrecklenfort, E., Brandes, N., Nordwig, M., Ding, G.C., Siemens, S., Heuer, H., Smalla, K.
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2014. Dynamics of transformation of the veterinary antibiotic sulfadiazine in two soils. Chemosphere, Vol. 95. 2014, pp. 470–477.
Sittig, S., Kasteel, R., Groeneweg, J., Hofmann, D., Thiele, B., Köppchen, S., Vereecken, H.
