Analysis of Antibiotics in Groundwater: A Review
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摘要: 抗生素是一类环境中新型有机污染物，其在地下水系统中的污染状况和环境行为备受关注。本文从污染来源、危害、污染现状、检测技术和迁移转化等方面综述了近年来地下水中抗生素的研究现状。抗生素主要来源于抗生素生产工业、医疗卫生业、畜牧养殖业、水产养殖业等，进入地下水中的微量抗生素不但诱导抗药性细菌的产生，更对原位微生物及人体产生危害。检测技术的进步是抗生素污染研究的重要支撑，目前已有多种抗生素污染的检测技术，其中酶联免疫技术主要用于抗生素污染初步筛查；气相色谱-质谱技术由于需要衍生化等处理过程而较少使用；毛细管电泳技术具有消耗样品量少、分析成本低等优点，但重现性差使其应用受到限制；液相色谱技术是在抗生素检测中应用较普遍的技术，特别是液相色谱-串联质谱技术具有灵敏度高、检出限低、可检测多组分污染物等优点，应用最为广泛。近年来依托于各种检测技术在国内外均有地下水中抗生素检出的报道，其检出浓度范围1~104 ng/L不等，检出种类有磺胺类、喹诺酮类、四环素类及大环内酯类抗生素。抗生素在地下水系统中的迁移转化行为包括吸附、水解、光解、生物降解等过程,其基质复杂、含量低和产物难以定性等问题给检测提出了新的挑战。优化检测方法、开发新的预处理技术、开展全面的地下水污染调查、进行代谢产物定性分析、探索抗生素治理技术等，将是今后地下水中抗生素污染研究的主要方向。
Abstract: Antibiotics as emerging organic pollutants, which do harm to humans and the environment, have aroused widespread attention. The pollution status of antibiotics in groundwater has become a research hotspot. Antibiotics in groundwater mainly derive from the antibiotic production industry, medical and health departments, animal husbandry and aquaculture. The trace-level antibiotics in groundwater increase bacterial resistance, damage human health by reducing immunity, causing abnormal or allergic reaction, carcinogenesis, teratogenesis and mutagenesis. There are various detection techniques for antibiotics in groundwater. For example, enzyme linked immunosorbent assay is usually applied to screen antibiotic contamination. However, Gas Chromatography-Mass Spectrometry is rarely used, due to complicated processes. Capillary Chromatography detection technology has the advantages of low sample consumption and low analysis cost, but the poor reproducibility is its weakness. Liquid Chromatography has been widely used, among which Liquid Chromatography-Tandem Mass Spectrometry is the most commonly used detection technique with high sensitivity, low detection limit and high efficiency. Many studies have reported occurrences of antibiotics in groundwater in many countries. The detected concentrations range from 1 to 104 ng/L, and the detected types are mainly sulfonamides, tetracyclines, quinolones and macrolides antibiotics. Antibiotics in groundwater systems undergo a series of migration and transformation behaviours, such as adsorption, hydrolysis, photolysis and biodegradation. The main research direction for the future, including establishment of perfect detection methods and pretreatment technologies, comprehensive groundwater pollution investigation, analysis of antibiotics metabolites and its toxicity, treatment of antibiotics contamination are also discussed in this paper.-
Keywords:
- groundwaters /
- antibiotics /
- detection technology /
- migration and transformation
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表 1 抗生素分类
Table 1 Type of antibiotics
抗生素种类 代表性的抗生素 结构特点 抗菌机理 青霉素类
(Penicillins)青霉素G、氨苄青霉素、羟氨苄青霉素(阿莫西林、阿莫仙)、苯唑青霉素等 天然青霉素是从青霉菌培养液中提取获得,半合成青霉素是在中间体6-氨基青霉烷酸(6-APA)侧链上加入不同基团 最早用于临床的抗生素，疗效高，毒性低。主要作用是使易感细菌的细胞壁发育失常，致其死亡 头孢菌素类
(Cephalosporins)头孢氨苄(先锋霉素Ⅳ)、头孢唑啉(先锋霉素Ⅴ)、头孢拉定(先锋霉素Ⅵ)、头孢呋辛(西力欣)、头孢曲松(罗氏芬)、头孢噻肟(凯福隆)、头孢哌酮(先锋必)等 含有头孢烯的半合成抗生素，7-氨基头孢烷酸(7-ACA)的衍生物 该类抗生素可破坏细菌的细胞壁，并在繁殖期杀菌 氨基糖苷类
(Aminoglycosides)链霉素、庆大霉素、霉卡那素、丁胺卡那霉素等 氨基糖与氨基环醇通过氧桥连接而成的苷类抗生素 在有氧情况下，对敏感细菌起杀灭作用，其治疗指数(治疗剂量/中毒剂量)较其他抗生素为低 大环内酯类
(Macrolides)红霉素,阿奇霉素(泰力特、希舒美),克拉霉素，罗它霉素，麦迪霉素，螺旋霉素，交沙霉素等 本类抗生素均含有一个12～16碳的大内酯环，为抑菌剂，仅适用于轻中度感染，但是为目前最安全的抗生素之一 为抑菌剂，仅适用于轻中度感染，但是为目前最安全的抗生素之一 四环素类
(Tetracyclines)四环素、土霉素、金霉素、强力霉素等 其结构均含并四苯基本骨架 广泛用于多种细菌及立克次氏体、衣原体、支原体等所致之感染 氯霉素类
(Chloramphenicols)氯霉素、琥珀氯霉素等 含有对硝基苯基、丙二醇与二氯乙酰胺三个部分 该类抗生素脂溶性高，易进入脑脊液和脑组织，并对很多病原体有效，但可诱发再生障碍性贫血，其应用受到一定限制 林可酰胺类
(Lincosamides)林可霉素、克林霉素等 含有氨基酸和糖苷部分，并通过肽键相连 易与核糖体上的50S核糖体结合，阻碍原核翻译的进行，从而使细菌死亡 磺胺类
(Sulfonamides)磺胺噻唑、磺胺甲基嘧啶、磺胺甲氧哒嗪、磺胺氯哒嗪等 临床常用的磺胺类药物都是以对位氨基苯磺酰胺为基本结构的衍生物，磺酰胺基上的氢可被不同杂环取代，形成不同种类的磺胺药 该类抗生素通过竞争性抑制叶酸代谢循环中的对氨基苯甲酸而抑制细菌性增殖 喹诺酮类
(Quinolones)萘啶酸、环丙沙星、司帕沙星、西他沙星等 目前已有四代喹诺酮类抗生素，结构中均含有羧酸基团，第三代药物分子中均有氟原子，第四代药物在第三代基础上引入8-甲氧基 该类抗生素以细菌的脱氧核糖核酸(DNA)为靶，抑制DNA回旋酶，进一步造成细菌DNA的不可逆损害，达到抗菌效果 
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表 2 不同国家地下水中检出的抗生素种类及其浓度
Table 2 Occurrence of antibiotics and their concentration in groundwater of different countries
国家 检出成分 类别 检测的最高浓度
ρ/(ng·L-1)采样地 参考
文献美
国磺胺甲基异恶唑 磺胺类 1110 美国大范围 [36] 甲氧苄氨嘧啶 磺胺增效剂 18 加利福尼亚州
饮用水水源地下水[37] 磺胺甲基嘧啶 磺胺类 54 畜牧养殖场
附近地下水[38] 磺胺二甲基嘧啶 磺胺类 616 磺胺二甲恶唑 磺胺类 40 磺胺噻唑 磺胺类 305 红霉素 大环内酯类 2380 林可霉素 大环内酯类 416 莫能菌素 大环内酯类 350 泰妙菌素 大环内酯类 29 中
国四环素 四环素类 5.2 天津市蔬菜种植地
地下水[39] 磺胺甲基异恶唑 磺胺类 9.5 磺胺邻二甲氧嘧啶 磺胺类 78.3 氯霉素 酰胺醇类 28.1 环丙沙星 喹诺酮类 42.5 林可霉素 大环内酯类 8.3 磺胺间二甲氧嘧啶 磺胺类 128 广西省养猪场
地下水[40] 磺胺嘧啶 磺胺类 1.47 磺胺间甲氧嘧啶 磺胺类 19 甲氧苄氨嘧啶 磺胺增效剂 1.16 瑞
典环丙沙星 喹诺酮类 14000 制药厂附件村庄井
地下水[15] 依诺沙星 喹诺酮类 1900 恩诺沙星 喹诺酮类 67 洛美沙星 喹诺酮类 35 诺氟沙星 喹诺酮类 31 氧氟沙星 喹诺酮类 160 甲氧苄氨嘧啶 磺胺增效剂 55 德
国脱水红霉素 大环内酯类 49 巴符洲
地下水[26] 磺胺甲恶唑 磺胺类 410 法
国磺胺甲恶唑 磺胺类 3.0 罗纳-阿尔卑斯
区域地下水[41] 甲氧苄氨嘧啶 磺胺增效剂 1.4 罗红霉素 大环内酯类 1.3 西
班
牙四环素 四环素类 141 西班牙东北部
巴塞罗那[42] 土霉素 四环素类 41.0 多西霉素 四环素类 188 金霉素 四环素类 34.2 脱水红霉素 大环内酯类 1.68 阿奇霉素 大环内酯类 1620 罗红霉素 大环内酯类 3.23 克拉霉素 大环内酯类 5.11 交沙霉素 大环内酯类 3.8 螺旋霉素 大环内酯类 2980 替米考星 大环内酯类 820 磺胺甲恶唑 磺胺类 16.6 磺胺嘧啶 磺胺类 37.1 磺胺二甲基嘧啶 磺胺类 29.1 氧氟沙星 喹诺酮类 367 环丙沙星 喹诺酮类 443 诺氟沙星 喹诺酮类 462 单诺沙星 喹诺酮类 543 依诺沙星 喹诺酮类 323 恩诺沙星 喹诺酮类 264 氟甲喹 喹诺酮类 4.3 甲氧苄氨嘧啶 磺胺增效剂 9.4
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