Sorption of p-aminobenzoic acid (pABA) and five sulfonamide antibiotics to loess Chernozem topsoil amended with varied additions of pig slurry was investigated in batch trials. In unfertilized soil, partition coefficients (Kd) of sulfonamides ranged from 0.3 to 2.0. Strong sorption nonlinearity (1/n = 0.5 to 0.8) was best fitted by the Freundlich isotherm (R2 = 0.7 to 1.0) and was indicative for specific sorption mechanisms. Adsorption to pig slurry was much stronger, and nondesorbable portions were increased compared with soil. However, in a mixture of soil and slurry (50:1 w/w), sorption of the antibiotics was significantly decreased at a lower concentration range of pABA and the sulfonamides. This was attributed to competitive adsorption of dissolved organic matter (DOM) constituents from manure. An increase in pig slurry amendment resulted in increased total organic matter, DOM concentration, and ionic strength, but pH decreased. As a result, the nonadsorbed portions of pABA, sulfanilamide, and sulfadiazine (logD(ow)< -0.4) ranged from 47% to 82% of the applied concentration in the differently manured substrates. Dissolved fractions of the antibiotics reached a maximum at a soil-slurry ratio of 9:1 and decreased with further addition of manure. This decrease was related to the formation of less-effective DOM associates in solution. The adsorbed and desorbed portions of the less-polar substances--sulfadimidine, sulfadimethoxine, and sulfapyridine (logD(ow) > 0.1)--remained nearly constant in the presence of increased manure input. The pH changes caused by manure amendment strongly affected ionisation status of the latter compounds, thus resulting in increased adsorption, which compensated the mobilizing effect of DOM. It is suggested that the effect of manure be considered in test methods to determine the soil retention of pharmaceutical substances.
Sulfonamide antibiotics can enter agricultural soils by fertilisation with contaminated manure. While only rough estimations on the extent of such applications exist, this pathway results in trace level contamination of groundwater. Therefore, we studied the transport of three sulfonamides in leachates from field lysimeters after application of a sulfonamide-contaminated liquid manure. In a 3-year period, the sulfonamides were determined in 64% to 70% of all leachate samples at concentrations between 0.08 to 56.7 µg L −1 . Furthermore, sulfonamides were determined in leachates up to 23 months after application, which indicated a mediumto long-term leaching risk. Extreme dry weather conditions resulted in highest dislocated amounts of sulfonamides in two of the three treatments. Furthermore, soil management such as tillage and cropping affected the time between application and breakthrough of sulfonamides and the intra-annual distribution of sulfonamide loads in leachates. Although the total sulfonamide leaching loads were low, the concentrations exceeded the limit value of the European Commission of 0.1 µg biocide L −1 in drinking water in more than 50% of all samples. Furthermore, the medium-term mean concentration of the sulfonamides ranged from 0.08 and 4.00 µg L −1 , which was above the limit value of the European Commission in 91 out of 158 samples. Therefore, sulfonamides applied to soils in liquid manure under common agricultural practice may cause environmental and health risks which call for a setting up of more long-term studies on the fate of antibiotics.
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