Anthelmintics, drugs against parasitic worms, are frequently used in livestock and might act as danger environmental microcontaminants. The present study was designed to monitor the possible circulation of common anthelmintic drug albendazole (ABZ) and its metabolites in the real agriculture conditions. The sheep were treated with the recommended dose of ABZ. Collected faeces were used for the fertilization of a field with fodder plants (alfalfa and clover) which served as feed for sheep from a different farm. The selective ultrasensitive mass spectrometry revealed surprisingly high concentrations of active ABZ metabolite (ABZ-sulphoxide) in all samples (dung, plants, ovine plasma, rumen content and faeces). Our results prove for the first time an undesirable permeation of ABZ metabolites from sheep excrement into plants (used as fodder) and subsequently to other sheep in real agricultural conditions. This circulation causes the permanent exposition of the ecosystems and food-chain to the drug and can promote the development of drug resistance in helminths.

Recently, the widespread use of antibiotic has raised concerns about the potential health risks associated with their microbiological effect. In the present study, we investigated 990 elderly individuals (age ≥ 60 years) from the Cohort of Elderly Health and Environment Controllable Factors in West Anhui, China. A total of 45 representative antibiotics and two antibiotic metabolites were monitored in urine samples through liquid chromatography electrospray tandem mass spectrometry. The results revealed that 34 antibiotics were detected in 93.0% of all urine samples and the detection frequencies of each antibiotic varied between 0.2% and 35.5%. The overall detection frequencies of seven human antibiotics (HAs), 10 veterinary antibiotics (VAs), three antibiotics preferred as HAs (PHAs), and 14 preferred as VAs (PVAs) in urines were 27.4%, 62.9%, 30.9% and 72.7%, respectively. Notably, the samples with concentrations of six PVAs (sulfamethoxazole, trimethoprim, oxytetracycline, danofloxacin, norfloxacin and lincomycin) above 5000 ng/mL accounted for 1.7% of all urine samples. Additionally, in 62.7% of urine samples, the total antibiotic concentration was in the range of the limits of detection to 20.0 ng/mL. Furthermore, the elderly individuals with the sum of estimated daily intakes of VAs and PVAs more than 1 μg/kg/day accounted for 15.2% of all participants, and a health risk related to change in gut microbiota under antibiotic stimulation was expected in 6.7% of the elderly individuals. Especially, ciprofloxacin was the foremost contributor to the health risk, and its hazard quotient value was more than one in 3.5% of all subjects. Taken together, the elderly Chinese people were extensively exposed to VAs, and some elderly individuals may have a health risk associated with dysbiosis of the gut microbiota.

Frequently detected residuals of antibiotics in crops has drawn increasing attention from research community and the general public. This study was conducted under the controlled environmental conditions to investigate the uptake, translocation and distribution of three different veterinary antibiotics (VAs) in plants of Zea mays L. (maize, the third largest crop in the world, especially in China) and the associated mechanisms. The distribution color-maps of mixed-VAs showed that the highest RCF (root concentration factors) values of chlortetracycline (CTC) and sulfamethoxazole (SMZ) were found in the 0.5–2.0 mm zone (cell division zone), while the highest RCF value of sulfathiazole (ST) was in the 6.0–8.0 mm zone (elongation zone) of root tips (0.5–10.0 mm) after 120 h of exposure to VAs. The translocation factor (TF) of CTC was greater than 1.0, but the TFs of SMZ and ST were less than 1.0 under addition of single antibiotic. However, the TFs of three VAs were all greater than 1.0 at the end of exposure under addition of mixed-VAs. The dissipation of antibiotics by maize was also demonstrated by harvesting all plant parts in an enclosed system. The possible mechanisms for uptake and translocation of VAs in maize were investigated by adding multiple respiration inhibitors into the culture solution. The RCFs of VAs were suppressed heavily by salicylhydroxamic acid (SHAM) and sodium azide (NaN3), which indicates that the uptake of VAs was an active process. The results of TFs and stem concentration factors (SCFs) of CTC and SMZ in HgCl2 treatments revealed that the translocation of VAs was associated with the aquaporin activity in maize. The findings from this study will have significant implications for the management of crop food contamination by VAs and for the development of phytoremediation technology for antibiotics in the environment.

The impact of commonly-used livestock antibiotics on soil nitrogen transformations under varying redox conditions is largely unknown. Soil column incubations were conducted using three livestock antibiotics (monensin, lincomycin and sulfamethazine) to better understand the fate of the antibiotics, their effect on nitrogen transformation, and their impact on soil microbial communities under aerobic, anoxic, and denitrifying conditions. While monensin was not recovered in the effluent, lincomycin and sulfamethazine concentrations decreased slightly during transport through the columns. Sorption, and to a limited extent degradation, are likely to be the primary processes leading to antibiotic attenuation during leaching. Antibiotics also affected microbial respiration and clearly impacted nitrogen transformation. The occurrence of the three antibiotics as a mixture, as well as the occurrence of lincomycin alone affected, by inhibiting any nitrite reduction, the denitrification process. Discontinuing antibiotics additions restored microbial denitrification. Metagenomic analysis indicated that Proteobacteria, Bacteroidetes, Actinobacteria, and Chloroflexi were the predominant phyla observed throughout the study. Results suggested that episodic occurrence of antibiotics led to a temporal change in microbial community composition in the upper portion of the columns while only transient changes occurred in the lower portion. Thus, the occurrence of high concentrations of veterinary antibiotic residues could impact nitrogen cycling in soils receiving wastewater runoff or manure applications with potential longer-term microbial community changes possible at higher antibiotic concentrations.

Florfenicol is one of the most-used antimicrobial agents in global fish farming. Nevertheless, in most countries, its use is not conducted in accordance with good practices. The aim of this work was to evaluate the leaching of florfenicol from coated fish feed into the water. Analytical methods were developed and validated for the quantitation of florfenicol in medicated feed and water by UHPLC-MS/MS. Florfenicol residues in the water were quantified after 5- and 15-min exposures of the medicated feed in the water at 22 and 28 °C and at pH 4.5 and 8.0. The influence of pellet size and three coating agents (vegetable oil, carboxymethylcellulose, and low-methoxylated pectin) on the leaching of the drug was also assessed. Pellet size, coating agent, water temperature, and time of exposure significantly (p < 0.05) affected florfenicol leaching, while water pH did not interfere with the leaching. Coating with vegetable oil was the most efficient method to reduce florfenicol leaching, while coating with carboxymethylcellulose presented the highest leaching (approximately 60% after 15 min at 28 °C). Thus, the coating agent has a significant effect on the florfenicol leaching rate and, consequently, on the necessary dose of the drug to be administered. Moreover, it is worth mentioning that higher florfenicol leaching will pose a greater risk to environmental health, specifically in terms of the development of bacteria resistant to florfenicol. Additional studies are needed with other polymers and veterinary drugs used in medicated feed for fish farming.

The combination of emerging antibiotic resistance and lack of discovery of new antibiotic classes poses a threat to future human welfare. Antibiotics are administered to livestock at a large scale and these may enter the environment by the spreading of manure on agricultural fields. They may leach to groundwater, especially in the Netherlands which has some of the most intensive livestock farming and corresponding excessive manure spreading in the world. This study investigates the presence of antibiotics in groundwater in two regions with the most intensive livestock farming in the Netherlands. If so, the hydrochemical conditions were further elaborated. Ten multi-level wells with in total 46 filters were sampled, focusing on relatively young, previously age-dated groundwater below agricultural fields. Twenty-two antibiotics were analyzed belonging to the following antibiotic groups: tetracyclines, sulfonamides, trimethoprims, β-lactams, macrolides, lincosamides, quinolones, nitrofurans and chloramphenicol. The samples were analyzed for these antibiotics by LC-MS/MS ESI-POS/NEG (MRM) preceded by solid phase extraction which resulted in importantly low detection limits. Six antibiotics were found above detection limits in 31 filters in seven wells: sulfamethazine, sulfamethoxazole, lincomycin, chloramphenicol, ciprofloxacin, and sulfadiazine. The concentrations range from 0.3 to 18 ng L−1. Sulfonamides were detected at all measured depths down to 23 meters below surface level with apparent groundwater ages up to 40 years old. No antibiotics were detected below the nitrate/iron redox cline, which suggests that the antibiotics might undergo degradation or attenuation under nitrate-reducing redox conditions. This study provides proof that antibiotics are present in groundwater below agricultural areas in the Netherlands due to the spreading of animal manure.

We evaluated the occurrence of 12 veterinary antibiotics and a beta agonist over spatial and temporal scales in Shell Creek, an intensively agricultural watershed in Nebraska, using Polar Organic Chemical Integrative Samplers (POCIS). Twelve pharmaceuticals were detected with concentrations ranging from 0.0003 ng/L to 68 ng/L. The antibiotics measured at the highest time-weighted average concentrations were lincomycin (68 ng/L) and monensin (49 ng/L), and both compounds were detected at increased concentrations in summer months. Analysis of variance indicates that mean concentrations of detected pharmaceuticals have no significant (p > 0.01) spatial variation. However, significant temporal differences (p < 0.01) were observed. This study demonstrates the utility of passive samplers such as POCIS for monitoring ambient levels of pharmaceuticals in surface waters.

Raman spectroscopy was used to investigate sorption mechanisms of cephapirin (CHP), a veterinary antibiotic, onto quartz (SiO₂) and feldspar (KAlSi₃O₈) at different pH. Sorption occurs by electrostatic attraction, monodentate and bidentate complexation. The zwitterion (CHP⁰) adsorbs to a quartz(+) surface by electrostatic attraction of the carboxylate anion group (-COO-) at low pH, but adsorbs to a quartz(-) surface through electrostatic attraction of the pyridinium cation, and possibly COO- bridge complexes, at higher pH. CHP- bonds to quartz(-) surfaces by bidentate complexation between one oxygen of -COO- and oxygen from carbonyl of an acetoxymethyl group. On a feldspar(+/-) surface, CHP⁰ forms monodentate complexes between CO, and possible -COO- bridges and/or electrostatic attachments to localized edge (hydr)oxy-Al surfaces. CHP- adsorbs to feldspar(-) through monodentate CO complexation. Similar mechanisms may operate for other cephalosporins. Results demonstrate, for the first time, that Raman techniques can be effective for evaluating sorption mechanisms of antibiotics. Raman spectroscopy indicates that cephapirin, a veterinary antibiotic, sorbs to quartz and feldspar by electrostatic attraction, and monodentate and bidentate complexation.

Veterinary antibiotics have been detected as contaminants of emerging concern in soil environment worldwide. Animal manure is frequently applied to agricultural fields to improve soil fertility, which can result in introducing large amount of antibiotics into soil environment. However, few attempts have been made to identify the spatial and temporal dynamics of veterinary antibiotics in soil at the hillslope scale with different land uses. This study was performed to explore the pattern and variability of veterinary antibiotics in the soil in response to rainfall events. Results showed that higher concentrations of veterinary antibiotics were generally found in cropland (292.6 ± 280.1 ng/g) and orchard (228.1 ± 230.5 ng/g) than in forestland (13.5 ± 9.9 ng/g). After rainfall events, antibiotics accumulated in the soil at the positions where manure was applied, especially under high-intensity rainfall conditions. However, the antibiotic concentration in soil slightly increased from the top to the bottom of hills, thus indicating the restricted contribution of runoff to antibiotic transport, especially under low-intensity rainfall conditions. In addition, most antibiotics were sequestered in the surface soil (0–10 cm), and higher antibiotic concentrations were observed in deep soil (20–40 cm) in cropland than orchard. The soil aggregate, organic matter, and clay content played important roles in antibiotic sequestration along the hillslope subject to low-, medium-, and large-amount rainfall events, respectively. This study identified that land use, rainfall conditions, and soil structures jointly affect the spatial and temporal variability of antibiotics in soils on hillslopes.

Manure treatment technologies are rapidly developing to minimize eutrophication of surrounding environments and potentially decrease the introduction of antibiotics and antibiotic resistant genes (ARGs) into the environment. While laboratory and pilot-scale manure treatment systems boast promising results, antibiotic and ARG removals in full-scale systems receiving continuous manure input have not been evaluated. The effect of treatment on ARGs is similarly lacking. This study examines the occurrence and transformation of sulfonamides, tetracyclines, tetracycline degradation products, and related ARGs throughout a full-scale advanced anaerobic digester (AAD) receiving continuous manure and antibiotic input. Manure samples were collected throughout the AAD system to evaluate baseline antibiotic and ARG input (raw manure), the effect of hygenization (post-pasteurized manure) and anaerobic digestion (post-digestion manure) on antibiotic and ARG levels. Antibiotics were analyzed by liquid chromatography-tandem mass spectrometry (LC-MS/MS), and the ARGs tet(O), tet(W), sul1 and sul2 were analyzed by quantitative polymerase chain reaction (Q-PCR). Significant reductions in the concentrations of chlortetracycline, oxytetracycline, tetracycline and their degradation products were observed in manure liquids following treatment (p < 0.001), concomitant to significant increases in manure solids (p < 0.001). These results suggest sorption is the major removal route for tetracyclines during AAD. Significant decreases in the epimer-to-total residue ratios for chlortetracycline and tetracycline in manure solids further indicate degradation is desorption-limited. Moreover, sul1 and sul2 copies decreased significantly (p < 0.001) following AAD in the absence of sulfonamide antibiotics, while tetracyclines-resistant genes remained unchanged. A cross-sectional study of dairy farms utilizing natural aeration and liquid-solid separation treatments was additionally performed to compare levels of antibiotics and ARGs found in AAD with the levels in common manure management systems. The concentration of antibiotics in raw manure varied greatly between farms while minimal differences in ARGs were observed. However, significant (p < 0.01) differences in the levels of antibiotics and ARGs (except tet(W)) were observed in the effluents from the three different manure management systems.