Little is known about the occurrence and the fate of veterinary drugs in the environment. Therefore, a liquid chromatography/tandem mass spectrometry method was developed and employed to investigate in detail the distribution and persistence of the frequently used tetracyclines and tylosin in a field fertilized with liquid manure on April 2000 and April 2001; soil sampling was performed in May 2000, November 2000, and May 2001. We detected 4.0 mg/kg tetracycline and 0.1 mg/kg chlortetracycline in the liquid manure of April 2000, as well as comparable amounts in the liquid manure of April 2001. In the soil samples of May 2001, the highest average concentrations of 86.2 (0-10 cm), 198.7 (10-20 cm), and 171.7 microg/kg (20-30 cm) tetracycline and 4.6-7.3 micro/kg chlortetracycline (all three sublayers) were found. At soil depths between 30 and 90 cm, as well as in soil or groundwater, tetracyclines could not be detected. In addition, oxytetracycline and tylosin could not be detected in any sample investigated. We conclude that tetracyclines enter the environment in significant concentrations via repeated fertilizations with liquid manure, build up persistent residues, and accumulate in soil. Therefore, tetracyclines may have a potential risk and investigations on the environmental effects of these antibiotics are necessary.
Recently we showed that tetracyclines tend to persist and may accumulate in sandy soils after repeated fertilizations with liquid manure. We continued these field investigations from 2001 to 2003 and observed no further accumulation of tetracyclines in soil, but found that the average tetracycline concentration remained higher than 150 microg/kg soil. From 2000 to 2002, approximately 330 g tetracycline, 7 g chlortetracycline, 28 g sulfamethazine, and 57 g sulfadiazine per hectare were transferred via liquid manure to the topsoil (0-30 cm). Nevertheless, no leaching of tetracyclines into deeper soil segments or groundwater was observed. Furthermore, we developed new analytical methods for the detection of various sulfonamides in liquid manure, soil, and groundwater. Investigation of the same fields used in the tetracycline study showed that sulfamethazine occurred in concentrations approximately two orders of magnitude lower than that of tetracycline in the plow layer. Although there apparently were very low concentrations of sulfamethazine in soil, we detected it in groundwater sampled by suction probes at 1.4 m below soil surface in the spring of 2002. Further investigations confirmed these findings. To our knowledge, this is the first direct evidence of continuous leaching of a veterinary drug from soil into groundwater under field conditions. We conclude that tetracyclines and sulfonamides show distinctly different environmental behaviors. One explanation may be their different sorption coefficients in soil, indicating (in part) their different mobilities in this ecosystem.
Pig-house dust originates from feed, bedding, feces, and the animals themselves. If the animals receive drugs such as antibiotics, residues of these substances may occur in manure, in the air, or on surfaces of the respective animal house. In a retrospective study, we investigated dust samples collected during two decades from the same piggery for the occurrence of various antibiotics. In 90% of these samples, we detected up to five different antibiotics, including tylosin, various tetracyclines, sulfamethazine, and chloramphenicol, in total amounts up to 12.5 mg/kg dust. High dust exposure in animal confinement buildings is believed to be a respiratory health hazard because of the high content of microorganisms, endotoxins, and allergens. Further risks may arise from the inhalation of dust contaminated with a cocktail of antibiotics. Apart from that, our data provide first evidence for a new route of entry for veterinary drugs in the environment.
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