Occurrence, distribution and risk assessment of antibiotics at various aquaculture stages in typical aquaculture areas surrounding the Yellow Sea

The pollution of antibiotics commonly existed throughout the entire aquaculture process,but the residues of antibiotics at different aquaculture stages have rarely been studied. This study investigated the occurrence, distribution and risk assessment of antibiotics at different aquaculture stages (the non-aquaculture stage, the early aquaculture stage, the middle aquaculture stage, and the late aquaculture stage) in two typical marine aquaculture areas (Mahegang River and Dingzi Bay) surrounding the YellowSea. Fluoroquinolones and tetracyclineswere commonly used antibiotics in the aquaculture of these areaswith high detection frequencies (17% to 83%). Compared among four aquaculture stages, the highest concentration of antibiotics (9032.08 ng/L) in aquaculture ponds was detected at the late aquaculture stage. And the antibiotic pollution level of natural water was directly related to the aquaculture stages. Similarly, at the aquaculture stages, the detection frequency of antibiotics in sediments was higher than that at the non-aquaculture stage. Based on the correlation analysis, the concentration of main antibiotics in water showed a positive correlation with total nitrogen (p<0.05) and chlorophyll a (p<0.01), while it showed a negative correlation with salinity (p<0.01) in coastal water of the Dingzi Bay. According to the risk assessment,with the development of aquaculture stages, the selection pressure of fluoroquinolones and tetracyclines on resistant bacteria had increased. And the ecological risks caused by sulfonamides and tetracyclines to aquatic organisms had also increased markedly. Overall, this study may provide a reference for formulating regulatory policies regarding antibiotic use at different aquaculture stages.     

Sorption of tylosin and sulfamethazine on solid humic acid

Tylosin(TYL) and sulfamethazine(SMT) are ionizable and polar antimicrobial compounds,which have seeped into the environment in substantial amounts via fertilizing land with manure or sewage. Sorption of TYL and SMT onto humic acid(HA) may affect their environmental fate. In this study, the sorption of TYL and SMT on HA at different conditions(pH, ionic strength) was investigated. All sorption isotherms fitted well to the Henry and Freundlich models and they were highly nonlinear with values of n between 0.5 and 0.8, which suggested that the HA had high heterogeneity. The sorption of TYL and SMT on HA decreased with increasing p H(2.0–7.5), implying that the primary sorption mechanism could be due to cation exchange interactions between TYL~+/SMT~+ species and the functional groups of HA.Increasing ionic strength resulted in a considerable reduction in the K_d values of TYL and SMT,hinting that interactions between H bonds and π–π EDA might be an important factor in the sorption of TYL and SMT on HA. Results of Fourier transform infrared(FT-IR) and ~13C-nuclear magnetic resonance(NMR) analysis further demonstrated that carboxyl groups and O-alkyl structures in the HA could interact with TYL and SMT via ionic interactions and H bonds,respectively. Overall, this work gives new insights into the mechanisms of sorption of TYL and SMT on HA and hence aids us in assessing the environmental risk of TYL and SMT under diverse conditions.     

施用粪肥蔬菜基地抗生素残留的研究进展

从施用粪肥的土壤及蔬菜中抗生素的含量与分布特征、抗生素残留对土壤微生物数量、酶活性及对蔬菜产量、品质的影响方面进行了综述,为进一步对施用粪肥蔬菜基地抗生素残留的研究提供参考。结果表明:规模养殖场产生的畜禽粪便作为有机肥料施入蔬菜基地,可造成土壤抗生素残留污染,并可通过干扰土壤微生物的群落结构与功能及土壤酶活性而影响土壤肥力,甚至可被作物吸收累积从而危及农产品质量安全。     

Removal of tetracycline from aqueous solution by a Fe3O4 incorporated PAN electrospun nanofiber mat

Pollution of antibiotics, a type of emerging contaminant, has become an issue of concern, due to their overuse in human and veterinary application, persistence in environment and great potential risk to human and animal health even at trace level. In this work, a novel adsorbent, Fe₃O₄ incorporated polyacrylonitrile nanofiber mat (Fe-NFM), was successfully fabricated via electrospinning and solvothermal method, targeting to remove tetracycline (TC), a typical class of antibiotics, from aqueous solution. Field emission scanning electron microscopy and X-ray diffraction spectroscopy were used to characterize the surface morphology and crystal structure of the Fe-NFM, and demonstrated that Fe-NFM was composed of continuous, randomly distributed uniform nanofibers with surface coating of Fe₃O₄ nanoparticles. A series of adsorption experiments were carried out to evaluate the removal efficiency of TC by the Fe-NFM. The pseudo-second-order kinetics model fitted better with the experimental data. The highest adsorption capacity was observed at initial solution pH 4 while relative high adsorption performance was obtained from initial solution pH 4 to 10. The adsorption of TC on Fe-NFM was a combination effect of both electrostatic interaction and complexation between TC and Fe-NFM. Freundlich isotherm model could better describe the adsorption isotherm. The maximum adsorption capacity calculated from Langmuir isotherm model was 315.31 mg/g. Compared to conventional nanoparticle adsorbents which have difficulties in downstream separation, the novel nanofiber mat can be simply installed as a modular compartment and easily separated from the aqueous medium, promising its huge potential in drinking and wastewater treatment for micro-pollutant removal.     

水环境中抗生素的分布、累积及生态毒理效应

抗生素持续大量使用带来的环境污染和潜在的生态风险已经引起广泛关注。总结了国内外相关研究成果,对水环境中抗生素的污染源及残留水平进行了分析,对抗生素在水生生物体内的累积规律给予了评述,同时对抗生素的生态毒理效应进行了探讨。鉴于我国水环境中抗生素的污染现状,建议未来加强环境相关浓度下抗生素在生物体内的分布与转化、食物链迁移与放大,以及多种抗生素联合效应等方面的研究。     

Spectroscopic study of the degradation of antibiotics and the generation of representative EfOM oxidation products in ozonated wastewater

This study examined effects of ozonation on thirteen fluoroquinolone, macrolide and lincosamide antibiotics present in municipal wastewater. Transformations of effluent organic matter (EfOM) caused by ozonation were characterized using absorbance/fluorescence spectroscopy and high performance size exclusion chromatography (HPSEC). Concentrations of aldehydes and carboxylic acids generated via the oxidation of EfOM were also determined. The absorbance and fluorescence of ozonated wastewater decreased with increasing ozone dose or treatment time. HPSEC data showed that these phenomena corresponded to the oxidation of all EfOM fractions, with some preference towards the degradation of the EfOM molecules with high apparent molecular weight. The removal of antibiotics and production of aldehydes and carboxylic acids were strongly correlated with the changes in both EfOM absorbance and fluorescence. Applications of a model describing the concurrent degradation of trace level contaminants and relative changes of EfOM emission allowed achieving a good fitting between the experimental and modeled ΔC/C₀ vs. ΔA/A₀ and ΔC/C₀ vs. ΔF/F₀ data.     

Occurrence of veterinary antibiotics in animal wastewater and surface water around farms in Jiangsu Province, China

The objective of this investigation was to obtain a broad profile of veterinary antibiotics residues in animal wastewater and surface water around large-scale livestock and poultry farms in Jiangsu Province of China. Therefore, 53 samples collected from 27 large-scale animal farms in 11 cities and counties of Jiangsu Province in 2009, were monitored for 10 selected veterinary antibiotics using solid phase extraction and high performance liquid chromatography/electrospray ionization-tandem mass spectrometry (HPLC/ESI-MS/MS) techniques. Ten veterinary antibiotics were found in animal wastewaters, eight antibiotics were detected in pond waters, and animal farm-effluents and river water samples were contaminated by nine antibiotics. The most frequently detected antibiotics were sulfamethazine (75%), oxytetracycline (64%), tetracycline (60%), sulfadiazine (55%) and sulfamethoxazole (51%) which were detected with a maximum concentration of 211, 72.9, 10.3, 17.0 and 63.6 μg L⁻¹, respectively. The maximum concentration of 0.55 μg L⁻¹ for cyromazine, 3.67 μg L⁻¹ for chlortetracycline, 0.63 μg L⁻¹ for sulfadoxine, 39.5 μg L⁻¹ for doxycycline and 0.64 μg L⁻¹ for sulfaquinoxaline were determined in the collected samples. In general, the maximum concentration of the selected veterinary antibiotics was detected in animal wastewaters except for chlortetracycline in animal farm-effluents. In addition, residue levels of selected veterinary antibiotics in animal wastewater and surface water around the farms were related to animal species and have a high spatial variation.     

Decomposition and mineralization of cefaclor by ionizing radiation: kinetics and effects of the radical scavengers

There has been recent growing interest in the presence of antibiotics in different environmental sectors. One considerable concern is the potential development of antibiotic-resistant bacteria in the environment, even at low concentrations. Cefaclor, one of the beta-lactam antibiotics, is widely used as an antibiotic. Kinetic studies were conducted to evaluate the decomposition and mineralization of cefaclor using gamma radiation. Cefaclor, 30 mg/l, was completely degraded with 1,000 Gy of gamma radiation. At a concentration of 30 mg/l, the removal efficiency, represented by the G-value, decreased with increasing accumulated radiation dose. Batch kinetic experiments with initial aqueous concentrations of 8.9, 13.3, 20.0 and 30.0mg/l showed the decomposition of cefaclor using gamma radiation followed a pseudo first-order reaction, and the dose constant increased with lower initial concentrations. At a given radiation dose, the G-values increased with higher initial cefaclor concentrations. The experimental results using methanol and thiourea as radical scavengers indicated that ()OH radicals were more closely associated with the radiolytic decomposition of cefaclor than other radicals, such as e(aq)(-) or ()H. The radical scavenger effects were tested under O(2) and N(2)O saturations for the enhancement of the TOC percentage removal efficiencies in the radiolytic decomposition of cefaclor. Under O(2) saturation, 90% TOC removal was observed with 100,000 Gy. Oxygen is well known to play a considerable role in the degradation of organic substances with effective chain reaction pathways. According to the effective radical reactions, the enhanced TOC percentage removal efficiencies might be based on the fast conversion reactions of e(aq)(-) and ()H with O(2) into oxidizing radicals, such as O(2)(-) and HO(2)(), respectively. 100% TOC removal was obtained with N(2)O gas at 20,000 Gy, as reducing radicals, such as e(aq)(-) and ()H, are scavenged by N(2)O and converted into ()OH radicals, which have strong oxidative properties. The results of this study showed that gamma irradiation was very effective for the removal of cefaclor in aqueous solution. The use of O(2) or N(2)O, with radiation, shows promise as effective radical scavengers for enhancing the TOC or COD removal efficiencies in pharmaceutical wastewaters containing antibiotics. However, the biological toxicity and interactions between various chemicals during the radiolytic treatment, as well as treatments under conditions more representative of real wastewater will require further studies.     

Soil contamination with antibiotics in a typical peri-urban area in eastern China: Seasonal variation, risk assessment, and microbial responses

The prevalence and persistence of antibiotics in soils has become an emerging environmental issue and an increasing threat to soil security and global public health. The problem is more severe in areas undergoing rapid urbanization; however, the ecological risks of antibiotics, seasonal variability, and associated soil microbial responses in peri-urban soils have not been well-explored. The seasonal soil sampling campaigns were conducted in a typical peri-urban watershed in eastern China to investigate distribution of antibiotics. The results demonstrated higher mean concentrations of most antibiotic compounds in winter than in summer in peri-urban soils. The seasonal variations of norfloxacin, enrofloxacin, and ciprofloxacin were more significant than those of other antibiotics, due to their higher migration ability and bioavailability. An ecological risk assessment demonstrated that chlortetracycline, ciprofloxacin, doxycycline, and ofloxacin can pose high risks to soil microorganisms. Furthermore, the coexistence of multiple antibiotics obviously poses higher risks than individual compounds. A redundancy analysis demonstrated that tetracyclines mainly showed negative correlations with Firmicutes and Chloroflexi, and quinolones showed obviously negative correlations with Acidobacteria, Gemmatimonadetes, and Nitrospirae, suggesting potential inhibition from antibiotics on biological activities or biodegradation processes. However, the persistence of antibiotics in soil results in a significant decrease in bacterial diversity and a change in dominant species. Our results provide an overview of the seasonal variability of antibiotics and the associated effects on bacterial communities in peri-urban soils. The results can provide scientific guidance on decreasing soil contamination with antibiotics to enhance soil security in similar areas.     

Fate of antibiotics and antibiotic resistance genes in a full-scale restaurant food waste treatment plant: Implications of the roles beyond heavy metals and mobile genetic elements

Is our food safe and free of the crisis of antibiotics and antibiotic resistance(AR)?And will the derived food waste(FW) impose AR risk to the environment after biological treatment? This study used restaurant FW leachates flowing through a 200 tons-waste/day biological treatment plant as a window to investigate the fate of antibiotics and antibiotic-resistance genes(ARGs) during the acceptance and treatment of FW. Sulfonamides(sulfamethazine, sulfamethoxazole) and quinolones(ciprofloxacin, enrofloxacin, ofloxacin) were detected during FW treatment, while tetracyclines, macrolides and chloramphenicols were not observable. ARGs encoding resistance to sulfonamides, tetracyclines and macrolides emerged in FW leachates.Material flow analysis illustrated that the total amount of antibiotics(except sulfamethazine) and ARGs were constant during FW treatment processes. Both the concentration and total amount of most antibiotics and ARGs fluctuated during treatment, physical processes(screening, centrifugation, solid–liquid and oil–water separation) did not decrease antibiotic or ARGs concentrations or total levels permanently; the affiliated wastewater treatment plant appeared to remove sulfonamides and most ARGs concentrations and total amount. Heavy metals Ni,Co and Cu were important for disseminating antibiotics concentrations and MGEs for distributing ARGs concentrations. Humic substances(fulvic acids, hydrophilic fractions), C-associated and N-associated contents were essential for the distribution of the total amounts of antibiotics and ARGs. Overall, this study implied that human food might not be free of antibiotics and ARGs, and FW was an underestimated AR pool with various determinants. Nonetheless, derived hazards of FW could be mitigated through biological treatment with well-planned daily operations.