污水中抗生素生化去除研究进展

综述了活性污泥法、膜生物反应器、人工湿地等国内外常见抗生素生化去除方法的优缺点与适用范围,通过工艺对比发现,膜生物反应器和人工湿地能有效去除污水中的抗生素,活性污泥法对抗生素的去除率不高,且选择性较强;污泥龄和水力停留时间对抗生素的去除率有着显著影响,多数情况下反应器的运行改进也能提高抗生素的去除效果。针对抗生素污染问题,提出了采取加强型的复合式处理工艺、开展分区研究、出台相关管理政策等建议。     

Determination and health risk assessment of enrofloxacin,flumequine and sulfamethoxazole in imported Pangasius catfish products in Thailand

The goals of this study were to determine the levels of three antibiotics – enrofloxacin, flumequine and sulfamethoxazole – in Pangasius catfish products imported into Thailand and to assess the health risks from consumption. To extract these antibiotic residues, acetonitrile, methanol and a small amount of formic acid were used as solvents. Determination of the antibiotics after extraction steps was carried out by liquid chromatography coupled with tandem mass spectrometry (LC-MS/MS) technique. The results showed that 14 and 3 samples of Pangasius catfish products were contaminated with enrofloxacin and sulfamethoxazole, respectively. No flumequine residue was found. While the concentration levels of these antibiotics in most contaminated samples were lower than the European Union (EU) standard, one sample was found to contain sulfamethoxazole at 245.91 µg kg^?1, which was higher than the EU standard (100 µg kg^?1), indicating the likelihood that some contaminated freshwater fish products are widely distributed in Thai markets. Notably, the concentration levels of enrofloxacin in samples of Pangasius catfish with skin were higher than in non-skin products, suggesting that products with skin might retain more antibiotic residues than non-skin products. Although the hazard quotient showed that consuming imported Pangasius catfish products, based on the current consumption rate, will not adversely affect consumer health, antibiotic residues in Pangasius catfish products imported into Thailand should be continually monitored.     

中国北方地区水体中四环素族抗生素残留现状分析

为了更好了解北方市政污水等水体中四环素族抗生素残留现状,采用固相萃取方法对中国北方地区市政污水样品进行富集和净化,以高效液相色谱-串联质谱法分析样品中四环素族抗生素残留量。在调查的13个污水样品中四环素族抗生素普遍检出,且浓度分别达到四环素1114.27ng/L、土霉素2175.65ng/L、金霉素149.09ng/L和强力霉素187.45ng/L。结果表明,在我国近岸污水排放中依然有大量四环素类抗生素存在,应加强对近岸海洋环境中抗生素残留的监测与管理。     

水环境中抗生素的来源分布及对健康的影响

综述了水环境中抗生素污染的主要类型、来源及对生态和健康的影响,指出医用抗生素、农林牧渔用抗生素和企业废水中的抗生素是其主要污染来源.水环境中的抗生素污染改变了水生微生物菌群,导致耐药菌株的产生,在农副产品中残留,造成严重的过敏反应和毒副作用,并增加了患者的经济负担.提出了职能部门加强管理,提高医药工作人员的业务水平,选择最佳治疗方案,加强健康教育,合理使用农林牧渔业的抗生素等预防管理措施.     

Mass flows and removal of antibiotics in two municipal wastewater treatment plants

The mass flows and removal of 20 antibiotics of seven classes in two wastewater treatment plants (WWTPs) of Hong Kong were investigated in different seasons of a whole year, using bihourly 24 h flow proportional composite samples. Antibiotics were detected at concentrations of 3.2-1718, 1.3-1176 and 1.1-233 ng L⁻¹ in influents, secondary and disinfection effluents. Total daily discharges of all the detected antibiotics from effluents of Shatin and Stanley WWTPs were 470-710 and 3.0-5.2 g d⁻¹, respectively. Ampicillin, cefalexin, sulfamethoxazole, sulfadiazine, sulfamethazine, chlortetracycline and vancomycin were effectively (52-100%) eliminated by activated sludge process while ampicillin and cefalexin were effectively (91-99%) eliminated by disinfection. Bihourly variation analysis showed that concentrations of the major antibiotics in influents varied more significantly in Stanley WWTP which served small communities.     

Trends in the occurrence of human and veterinary antibiotics in the sediments of the Yellow River, Hai River and Liao River in northern China

The occurrence of four classes of 17 commonly used antibiotics (including fluoroquinolones, tetracycline, sulfonamides, and macrolides) was investigated in the sediments of the Yellow River, Hai River and Liao River in northern China by using rapid resolution liquid chromatography-tandem mass spectrometry. Higher concentrations were detected for most antibiotics in the sediments of the Hai River than in the sediments of the other rivers. Norfloxacin, ofloxacin, ciprofloxacin and oxytetracycline in the three rivers were most frequently detected with concentrations up to 5770, 1290, 653 and 652 ng/g, respectively. High frequencies and concentrations of the detected antibiotics were often found in the downstream of large cities and areas influenced by feedlot and fish ponds. Good fitted linear regression equations between antibiotic concentration and sediment physicochemical properties (TOC, texture and pH) were also found, indicating that sediment properties are important factors influencing the distribution of antibiotics in the sediment of rivers.     

Removal of antibiotics from urban wastewater by constructed wetland optimization

Seven mesocosm-scale constructed wetlands (CWs), differing in their design characteristics, were set up in the open air to assess their efficiency to remove antibiotics from urban raw wastewater. A conventional wastewater treatment plant (WWTP) was simultaneously monitored. The experiment took place in autumn. An analytical methodology including HPLC-MS/MS was developed to measure antibiotic concentrations in the soluble water fraction, in the suspended solids fraction and in the WWTP sludge. Considering the soluble water fraction, the only easily eliminated antibiotics in the WWTP were doxycycline (61 ± 38%) and sulfamethoxazole (60 ± 26%). All the studied types of CWs were efficient for the removal of sulfamethoxazole (59 ± 30-87 ± 41%), as found in the WWTP, and, in addition, they removed trimethoprim (65 ± 21-96 ± 29%). The elimination of other antibiotics in CWs was limited by the specific system-configuration: amoxicillin (45 ± 15%) was only eliminated by a free-water (FW) subsurface flow (SSF) CW planted with Typha angustifolia; doxycycline was removed in FW systems planted with T. angustifolia (65 ± 34-75 ± 40%), in a Phragmites australis-floating macrophytes system (62 ± 31%) and in conventional horizontal SSF-systems (71 ± 39%); clarithromycin was partially eliminated by an unplanted FW-SSF system (50 ± 18%); erythromycin could only be removed by a P. australis-horizontal SSF system (64 ± 30%); and ampicillin was eliminated by a T. angustifolia-floating macrophytes system (29 ± 4%). Lincomycin was not removed by any of the systems (WWTP or CWs). The presence or absence of plants, the vegetal species (T. angustifolia or P. australis), the flow type and the CW design characteristics regulated the specific removal mechanisms. Therefore, CWs are not an overall solution to remove antibiotics from urban wastewater during cold seasons. However, more studies are needed to assess their ability in warmer periods and to determine the behaviour of full-scale systems.     

Highly organic natural media as permeable reactive barriers: TCE partitioning and anaerobic degradation profile in eucalyptus mulch and compost

The occurrence, removal efficiency and seasonal variation of 22 antibiotics, including eight fluoroquinolones, nine sulfonamides and five macrolides, were investigated in eight sewage treatment plants (STPs) in Beijing, China. A total of 14 antibiotics were detected in wastewater samples, with the maximum concentration being 3.1 μg L⁻¹ in the influent samples and 1.2 μg L⁻¹ in the effluent samples. The most frequently detected antibiotics were ofloxacin, norfloxacin, sulfadiazine, sulfamethoxazole, erythromycin and roxithromycin; of these, the concentration of ofloxacin was the highest in most of the influent and effluent samples. Eighteen antibiotics were detected in the sludge samples, with concentrations ranging from 1.0 × 10⁻¹ to 2.1 × 10⁴ μg kg⁻¹. The dominant antibiotics found in the sludge samples were the fluoroquinolones, with ofloxacin having the highest concentration in all the sludge samples. The antibiotics could not be removed completely by the STPs, and the mean removal efficiency ranged from −34 to 72%. Of all the antibiotics, the fluoroquinolones were removed comparatively more efficiently, probably due to their adsorption to sludge. Seasonal variation of the antibiotics in the sludge samples was also studied. The concentrations of antibiotics in winter were higher than in spring and autumn. Since the total levels of the fluoroquinolones detected in the influent samples were lower than the predicted no-effect concentration (PNEC) of 8.0 μg L⁻¹, the residues of these antibiotics would be unlikely to have adverse effects on microorganisms involved in sewage treatment processes.     

Potential for natural and enhanced attenuation of sulphanilamide in a contaminated chalk aquifer

Understanding antibiotic biodegradation is important to the appreciation of their fate and removal from the environment. In this research an Isotope Ratio Mass Spectrometry(IRMS)method was developed to evaluate the extent of biodegradation of the antibiotic,sulphanilamide, in contaminated groundwater. Results indicted an enrichment in δ~(13)C of8.44‰ from-26.56(at the contaminant source) to-18.12‰(300 m downfield of the source).These results confirm reductions in sulphanilamide concentrations(from 650 to 10 mg/L)across the contaminant plume to be attributable to biodegradation(56%) vs. other natural attenuation processes, such as dilution or dispersion(42%). To understand the controls on sulphanilamide degradation ex-situ microcosms assessed the influence of sulphanilamide concentration, redox conditions and an alternative carbon source. Results indicated, high levels of anaerobic capacity(~50% mineralisation) to degrade sulphanilamide under high(263 mg/L), moderate(10 mg/L) and low(0.02 mg/L) substrate concentrations. The addition of electron acceptors; nitrate and sulphate, did not significantly enhance the capacity of the groundwater to anaerobically biodegrade sulphanilamide. Interestingly, where alternative carbon sources were present, the addition of nitrate and sulphate inhibited sulphanilamide biodegradation. These results suggest, under in-situ conditions, when a preferential carbon source was available for biodegradation, sulphanilamide could be acting as a nitrogen and/or sulphur source. These findings are important as they highlight sulphanilamide being used as a carbon and a putative nitrogen and sulphur source, under prevailing iron reducing conditions.     

武汉市东湖抗生素污染现状及生态风险评估

对东湖水域内16个点位进行采样,采用超高效液相色谱-三重四极杆质谱联用仪对28种抗生素做了污染现状调查及生态风险评估。研究发现,有20种抗生素在不同点位被检出,检出浓度由高到低为：喹诺酮类、氯霉素类和磺胺类,污染物检出情况总体呈现“南高北低,东高西低”的结果。考虑到东湖南部采样点位周边有多个农业种植、水产养殖和畜禽养殖地及其对东湖的潜在抗生素污染,证实了人类活动与抗生素污染密切相关。对抗生素采用风险商法做生态风险评估,结果表明,东湖南部采样点位的恶喹酸和氟甲喹的生态环境风险处于较低水平,其他抗生素的生态风险可以忽略。