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抗生素是由微生物(包括细菌、真菌、放线菌属)或高等动植物产生的具有抗病原体,能干扰其他细胞发育功能的化学物质,或具有其它活性的一类次级代谢产物[1]. 自1928年青霉素被发现以来,抗生素的发展史已有将近一百年,其为人类的健康及生活做出了不可磨灭的贡献. 目前抗生素类药物大致可以分为七类:β-内酰胺类、磺胺类、喹诺酮类、氯霉素类、四环素类、氨基糖苷类及大环内酯类. β-内酰胺类主要有青霉素类(青霉素、阿莫西林等)和头孢菌素类(头孢氨苄、头孢唑啉等),是临床上最常用和品种最多的抗菌药物[2];磺胺类(磺胺嘧啶、磺胺甲基嘧啶等)可用于治疗链球菌、沙门氏菌、大肠杆菌、葡萄球菌、巴氏杆菌等细菌感染疾病[3],是类广谱抗生素;喹诺酮类(恩诺沙星、氧氟沙星等)与氯霉素类(氟苯尼考、甲砜霉素等)在水产养殖行业被广泛应用[4-5],如诺氟沙星用于治疗美洲鳗鲡气单胞菌属等引起的细菌性疾病[6];四环素类(四环素、土霉素等)不仅广泛应用于细菌感染,还作为生长促进剂投喂给动物;氨基糖苷类(链霉素、卡那霉素)与β-内酰胺等抗生素具有协同作用[7];大环内酯类(阿奇霉素、罗红霉素等)对抑制革兰氏阳性菌及支原体有较高活性[8-9].
据文献报道,在2000年至2015年间,全球抗生素消费量就已经增加了65%,预测2030年全球抗生素消费量比2015年高出200%[10]. 由于畜牧业近年向规模化、集约化快速发展,使其成为抗生素消耗量较大行业,2010年抗生素在畜牧业使用量占全球抗生素年产的2/3,保守估计为6.32万t,到2030年消耗量预计增加到10.56万t[11]. 大量抗生素的使用加之抗生素不能被生物体完全吸收,导致环境及农产品中抗生素相继被检出. 为遏制抗生素污染局势的继续发展,2022年我国新出台了《新污染物治理行动方案》,将抗生素列入重点环保管控对象之一,加强临床抗菌药物及兽用抗菌药监督管理. 并力求到2025年完成一批新污染物环境风险评估[12].
抗生素通过制药企业的工业废水、畜牧及水产养殖废水、医疗及城市污水等途径排放到环境中,经河流或城市内河道进行远距离迁移,最终汇聚于海洋,对生态环境及人类生活造成影响. 抗生素一方面可以抑制环境微生物的生长,甚至杀死微生物,改变环境微生物群落结构,破坏微生态平衡,影响海洋环境中碳、氮、硫等生源要素的地球化学循环;另一方面,海洋环境中持续存在的抗生素还可以诱导耐药菌群或抗生素抗性基因(antibiotic resistant genes,ARGs)产生,ARGs在海洋环境中的持久性残留,在菌群间的迁移、传播和扩增,对生态环境和人体健康都造成巨大威胁. 因此,本文对海洋环境中抗生素和ARGs的来源、赋存、迁移转化和生态风险进行全面综述,并对其发展趋势进行展望,以期为海洋环境中抗生素和ARGs的研究提供参考.
海洋环境中抗生素存在与环境行为研究进展
Advances in research on the presence and environmental behavior of antibiotics in the marine environment
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摘要: 由于抗生素的频繁使用和排放,抗生素不断排放进入水环境,表现为“持续存在”的状态,对生态环境系统造成长期、持续的环境风险,由此导致的环境污染和细菌耐药性是我国及全球都亟待解决的重大环境问题. 抗生素持久性的选择压力会产生抗生素抗性基因(antibiotic resistant genes,ARGs),其在环境中的持久性残留,在菌群间的迁移、传播和扩增,比抗生素残留本身对生态环境的危害更大. 随着海洋资源与环境的持续开发与利用,海洋正逐步成为抗生素和ARGs的重要储存库,海洋环境中的抗生素和ARGs对海洋生态环境和公众健康的威胁同样不容忽视. 本文对海洋环境中抗生素的来源、赋存、迁移转化和生态风险等研究进行分析梳理,对海洋环境中ARGs的环境行为进行综述,以期为海洋环境中抗生素和ARGs环境行为和风险评估研究提供参考,最后对相关研究的发展趋势进行了展望.Abstract: Frequent use and continued discharge of antibiotics lead to their persistence in aquatic environments and cause ecological risk More importantly, the selective stress from antibiotics may contribute to the development of antibiotic resistance. The potential ecological risks of widespread dissemination of antibiotic resistance genes (ARGs) are greater than the antibiotics themselves. With the continuous exploitation and utilization of marine resources, the marine environment is gradually becoming an important reservoir of antibiotics and ARGs. However, the threat of antibiotics and ARGs in the marine environment to the marine ecosystem and public health have not been clarified. The objectives of this paper are to analyze the sources, occurrence, transformation and ecological risks of antibiotics in the marine environment, and assess the environmental behavior of ARGs in marine environments. In addition, we provide an outlook for future studies.
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表 1 国内外近海海域水体中抗生素浓度水平(单位:ng·L−1)
Table 1. Levels of antibiotic concentration in domestic and international offshore waters(ng·L−1)
洲
State国家
Country海域
Sea磺胺类
Sulfonamides大环内酯类
Macrolidesβ-内酰胺类
Beta-lactams喹诺酮类
Quinolones四环素类
Tetracyclines其他类
Others参考文献
References亚洲 中国 渤海 磺胺甲恶唑(3—140) 红霉素(4—150) — 氧氟沙星(3—5100)
诺氟沙星(3—6800)— — [26] 北黄海 总磺胺量(nd—584.32 )
磺胺甲恶唑(nd—167.40)— — — — — [27] 黄海南部 磺胺甲恶唑(nd—48) 红霉素(nd—48) — — — 氟苯尼考(nd—42) [28] 黄东海 磺胺甲恶唑(nd—1.363) — — — — 甲氧苄胺嘧啶(0.269—2.88) [29] 东海 总磺胺量2.0—156.5 总大环内酯(2.9—77.0)
克林霉素(1.2—1507.9)— 总喹诺酮量(8.6—185.2) 总四环素量(1.0—6.5) 林可酰胺类总含量(2.5—1688.4),
林可霉素(0.9—180.8)[30] 维多利亚海湾(南海) — 红霉素(4.7—1730)
头孢氨苄(6.1—493)阿莫西林
(0.64—76)氧氟沙星 (8.1—1140) — 甲氧苄啶(2.6—216) [31] 南海 磺胺甲恶唑(nd—0.53) 罗红霉素(0.16–0.18 )克拉霉素(nd—0.04);D3—红霉(0.06—0.10) — — — 氟苯尼考(nd—0.52 ) [32] 韩国 南海 甲氧苄氨嘧啶(nd—5.3) 红霉素 (nd—0.2) — 诺氟沙星(nd—0.5)
氧氟沙星(nd—12.4)— 林可霉素(nd—438) [33] 新加坡 沿海 — — — — — 三氯生(nd—10.5) [34] 伊朗 波斯湾 — 阿奇霉素(0.3—4.8) — 诺氟沙星(19—68) 四环素(4.0—71) — [35] 沙特阿拉伯 红海 磺胺甲恶唑(31.5—62.4 ) — — — — 甲硝唑(51.0—178.6), 甲氧苄啶(nd—45.6) [36] 欧洲 西班牙 加的斯湾 — 阿奇霉素(nd—1.2);红霉素(nd—0.3) — — — 氟甲喹(nd—0.1)
林可霉素(nd—0.4)
奥硝唑(nd—5.1)[37] 地中海海滩 磺胺甲恶唑(9) — — — — 甲氧苄啶(1) [38] 欧洲 比利时 大西洋东部北海海湾 磺胺甲恶唑(13—96) — — — — 甲氧苄啶(13—29) [39] 希腊 东地中海 — 克拉霉素(nd—1.5) 阿莫西林(nd—127.8) — — 甲氧苄啶(nd—3.4)
甲硝唑(nd—8.2)[40] 德国 波罗的海 磺胺甲恶唑(nd—42) 罗红霉素(nd—16)
克拉霉素(nd—14)— — — — [41] 公海 威尼斯沿海 磺胺甲恶唑(nd—7.2) 克拉霉素(nd—8.7) — — — — [41] 亚得里亚海北部 磺胺甲恶唑(nd—4.1) 红霉素 (nd—5.8) — — — — [41] 波罗的海南部 磺胺甲恶唑(nd—311) — — 恩诺沙星(nd—208) — 甲氧苄啶(nd—279) [42] 欧洲和亚洲 希腊和土耳其 爱琴海和达达尼尔海峡 磺胺甲恶唑(nd—11) 克拉霉素(nd—16) — — — — [41] 北美洲 美国 切萨皮克湾 磺胺甲基异恶唑(nd—14.8) 阿奇霉素(nd—2.7);罗红霉素(nd—5.9);克拉霉素(nd—9.7) — 诺氟沙星(nd—94.1)
恩诺沙星(nd—17.8)— — [43] 太平洋 磺胺甲恶唑(nd—6.4) 红霉素 (nd—86);
罗红霉素(nd—141);
克拉霉素(nd—130)— — — — [41] 旧金山湾 磺胺甲恶唑(13—61) 红霉素(nd—217) — — — — [41] 哥斯达黎加 哥斯达黎加沿海海域 — — 苯甲异噁唑青霉素 (70—7571) 诺氟沙星(38—1744) 强力霉素
(74—73722)— [44] 南极洲 南极海水 — 克林霉素(<0.1) — 环丙沙星(4—218) — 甲氧苄啶(<0.1) [45] 备注:“—”为未进行检测;“nd”为未检出 表 2 中国海洋环境中ARGs的分布
Table 2. Distribution of ARGs in coastal marine environment of China
海洋环境
Seas检测出的ARGs
The detected ARGs参考文献
References渤海 sul1、sul2、tetO、tetW、tetB、tetM、tetH、tetX、ermB [63] 黄海 sul1、sul2、tetG、tetX、ermF、ermT、qnrS、qnrA、qnrB [64] 东海 sul1、sul2、tetC、tetW、dfrA13,blaPSE-1 [65] 南海 sul1、sul2、tetG、tetC、cmle1、cmle3、qnrS [66] 海南东寨港 sul1、sul2、dfrA1;tetA、tetC、tetG、tetM;cata1、cata2、cmle1、cmle3;qnrS [67] -
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