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自20世纪青霉素问世以来,各类抗生素不仅作为主要的抗感染药物广泛用于人和动物的疾病防治,还作为重要的生长促进剂应用于畜禽及水产养殖业[2]。进入人和动物体内的抗生素不能被完全吸收和代谢,大部分以原形或活性代谢产物的形式通过粪便和尿液直接排入环境或进入污水处理厂,而目前污水处理工艺并不能将抗生素完全去除,造成了抗生素在环境中的不断累积[3-4]。我国是世界上最大的抗生素生产国和消费国[5]。据估算,2013年我国抗生素总使用量约为16.2万吨,人均使用量大约是英美等发达国家的6倍,因此,抗生素带来的环境污染可能更为严重[6]。
作为抗生素最重要的归宿地之一,自然水体中的抗生素污染问题已引起人们广泛关注。研究指出,河流和湖泊面临的抗生素污染风险比海洋和地下水更大[7]。但是,目前对于我国主要河流和湖泊中抗生素的污染现状还缺乏详细的梳理。水体中的抗生素不仅会对水生生物产生直接毒害作用,还会改变微生物群落的结构和功能,并促进抗生素抗性基因(antibiotic resistance genes, ARGs)的产生和传播,从而对人类健康与生态系统的稳定性产生巨大威胁[8-9]。抗生素对水体中微生物群落结构和功能的影响,还会干扰微生物驱动的氮循环过程,已经成为水体富营养化和温室气体排放的重要影响因素[10-11]。
本文在梳理我国河流和湖泊中抗生素污染现状的基础上,进一步总结了抗生素对水生生态系统造成的生态风险,综述了抗生素对水体微生物群落以及氮转化过程的影响,最后提出了抗生素污染对水生生态系统影响的研究展望,以期加强人们对水体中抗生素污染的认识。
水体中抗生素污染现状及其对氮转化过程的影响研究进展
Progress in current pollution status of antibiotics and their influences on the nitrogen transformation in water
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摘要: 近年来,抗生素引起的环境污染和生态风险备受关注。作为抗生素最重要的归宿地之一,自然水体中的抗生素污染日益加剧。逐渐累积的抗生素给水生生态系统带来风险,并会改变微生物群落的结构和功能,已成为水体中物质循环过程的重要影响因子。该文总结了我国河流和湖泊中抗生素的污染现状及其对水生生态系统产生的风险,综述了抗生素对水体中微生物群落以及硝化、反硝化和厌氧氨氧化等氮转化过程的影响。我国主要河流和湖泊中均有抗生素检出,类型包括磺胺类、四环素类、喹诺酮类和大环内酯类等,不同水体中抗生素的污染类型及浓度差异显著。目前,有关抗生素给水生生态系统造成的生态风险和对微生物群落的影响研究较多,而抗生素抗性基因在水环境中的传播扩散机制还需要更全面和深入的探索。抗生素可以通过改变氮循环功能微生物、酶活性和功能基因等影响水体中氮转化过程。对反硝化过程主要表现为抑制作用,对硝化过程的影响与其浓度和类型有关,而对厌氧氨氧化和硝酸盐异化还原为铵过程的影响研究相对匮乏。后续研究中还应探索水动力,盐度,水深和氧化还原梯度等典型水环境条件下,氮转化过程对抗生素的响应,为全面揭示抗生素对水体氮转化过程的影响提供依据。Abstract: In recent years, the environmental contamination and ecological risk caused by antibiotics have attracted much attention. As one of the main sinks of antibiotics, the pollution of antibiotics in natural waters has been aggravating. The accumulation of antibiotics brings high risk to the aquatic ecosystem, affecting the structure and function of the microbial community, and it has become an important influencing factor for nutrient cycle in aquatic ecosystem. This paper reviewed the current pollution status of antibiotics in rivers and lakes in China and their risks to aquatic ecosystem. The effects of antibiotics on microbial community, nitrification, denitrification and anaerobic ammonium oxidation (Anammox) in waters were further systematically summarized. Antibiotics were detected in almost all major rivers and lakes in China. The main types of antibiotics include sulfonamides, tetracyclines, quinolones and macrolides. The differences in pollution type and concentration of antibiotics among rivers and lakes were significant. Previous researches mainly focused on the ecological risks of antibiotics to aquatic ecosystems and their effects on microbial communities, while the dissemination mechanism of antibiotic resistance genes in aquatic environment needs more comprehensive and in-depth exploration. Generally, antibiotics could affect the nitrogen transformation in water by changing functional microorganisms, enzyme activity and functional genes related to nitrogen cycle. According to existing researches, antibiotics mainly inhibit the denitrification process, but their effects on nitrification were related to concentration and type. However, the effects of antibiotics on Anammox and dissimilatory nitrate reduction to ammonium (DNRA) have been rarely reported. Furthermore, the responses of nitrogen transformation to antibiotics under typical water environment conditions such as hydrodynamic force, salinity, water depth and redox gradient, should be explored to comprehensively reveal the effects of antibiotics on nitrogen transformation in waters.
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Key words:
- antibiotics /
- water /
- ecological risk /
- microbial community /
- nitrogen transformation
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表 1 中国主要流域上覆水中抗生素的浓度(ng·L−1)
Table 1. The concentrations of antibiotics in the overlying water of major river basins in China(ng·L−1)
抗生素
Antibiotics松花江
Songhua RiverM辽河
MLiaohe RiverM海河
MHaihe River黄河
Yellow River淮河
Huaihe River长江
Yangtze RiverM珠江
MPearl River磺胺类 磺胺甲恶唑 2.1—73.1 670.3 64.1 ND—56.0 2.6—11.0 0.43—37.6 138.0 磺胺嘧啶 ND—13.9 — 184.0 — 0.002—0.66 ND—18.0 18.7 磺胺二甲嘧啶 — 15.9 — — ND—1.7 0.24—218.0 — 四环素类 四环素 — 39.0 16.1 3.7—64.9 ND—1.7 ND—13.1 349.7 土霉素 — 188.5 ND 4.6—83.5 ND—3.9 ND—0.97 359.4 金霉素 — 25.1 21.9 — — ND—0.95 33.0 喹诺酮类 诺氟沙星 ND—2.4 256.0 188.0 17.1—79.0 — ND—136.0 54.2 氧氟沙星 0.01—1.8 632.5 374.0 1.5—23.4 — ND—15.8 703.4 恩诺沙星 ND—1.1 70.4 184.0 2.7—20.9 — ND—0.89 ND 大环内酯类 红霉素 ND—7.3 — 4.6 4.5—23.3 — ND—7.3 70.2 脱水红霉素 — 2834.4 — ND—102.0 — ND—121.0 301.0 罗红霉素 — 741.0 235.0 0.2—14.1 — ND—1.8 366.0 参考文献 [12-13] [14-15] [16-17] [18-19] [20] [21-22] [23-24] 注:“M”表示水体中抗生素浓度的最大值;“ND”表示未检出或低于检测限;“—”表示无数据(下同)。
Note: "M" means maximum concentration of antibiotics in water; "ND" means not detected or below the detection limit; "—" means no data (the same below).表 2 中国主要流域沉积物中抗生素的浓度(ng·g−1)
Table 2. The concentrations of antibiotics in sediment of major river basins in China(ng·g−1)
抗生素
AntibioticsM松花江
MSonghua River辽河
Liaohe RiverM海河
MHaihe River黄河
Yellow River淮河
Huaihe River长江
Yangtze RiverM珠江
MPearl River磺胺类 磺胺甲恶唑 ND ND—2.6 — — ND—0.12 0.14—2.0 ND 磺胺嘧啶 — — 1.2 — ND—0.055 ND—0.57 ND 磺胺二甲嘧啶 — ND—1.0 5.7 — 0.057—0.22 ND—3.2 3.2 四环素类 四环素 — ND—8.0 135.0 3.2—26.8 0.012—1.8 ND—7.1 206.0 土霉素 — ND—384.6 422.0 1.2—11.5 ND 0.16—0.93 99.0 金霉素 — ND—12.3 10.9 — — ND—0.95 23.2 喹诺酮类 诺氟沙星 10.4 ND—52.5 5770.0 4.5—104.8 — 0.15—20.5 444.0 氧氟沙星 10.0 ND—51.4 635.0 5.1—49.7 — 0.29—84.2 157.0 恩诺沙星 15.1 ND—25.7 — 1.4—29.5 — 0.31—1.4 1.4 大环内脂类 红霉素 63.8 ND—175.4 — 0.95—5.4 — — 62.4 脱水红霉素 — — 67.7 — — ND—14.0 97.3 罗红霉素 — ND—229.3 11.7 0.87—3.7 — ND—13.5 141.0 参考文献 [13] [25] [26] [18] [20] [21-22] [23-24] 表 3 中国典型湖泊上覆水中抗生素的浓度(ng·L−1)
Table 3. The concentrations of antibiotics in the overlying water of typical lakes in China(ng·L−1)
抗生素
Antibiotics太湖
Taihu Lake巢湖
Chaohu Lake洞庭湖
Dongting Lake洪湖
Honghu Lake白洋淀
Baiyang Lake南四湖
Nansi Lake淀山湖
Dianshan Lake磺胺类 磺胺甲恶唑 0.06—490.6 ND—171.6 ND—47.4 ND—254.9 0.71—452.0 ND—62.0 0—646.0 磺胺嘧啶 0.07—15.0 ND—54.7 ND—61.3 ND—322.5 ND—642.0 ND—139.0 ND—211.0 磺胺二甲嘧啶 0.02—12.8 ND—214.0 ND—14.9 ND—172.4 0.14—47.7 ND—39.0 ND—408.0 四环素类 四环素 0.13—69.0 ND—17.8 ND—21.5 ND—965.7 ND—27.5 ND—126.0 0.19—11.6 土霉素 0.10—11.7 ND—4.9 ND ND—2199.5 ND—156.0 ND—5.9 0.01—187.2 金霉素 0.13—91.7 ND—4.0 ND—6.5 ND—828.9 ND—25.3 ND—3.2 0.01—58.6 喹诺酮类 诺氟沙星 0.06—31.3 ND—80.6 ND—1.7 — 1.2—123.0 ND—74.8 0.07—229.2 氧氟沙星 0.07—57.8 1.2—182.7 ND—0.53 ND—105.1 0.06—1000.0 ND—50.0 ND—25.0 恩诺沙星 3.3—52.7 ND—82.7 ND—4.6 — ND—182.0 ND—0.94 0.13—22.8 大环内酯类 红霉素 0.07—272.3 ND—136.2 — ND — ND—29.9 ND—564.7 脱水红霉素 — — — — 0.18—273.0 ND—16.0 — 罗红霉素 0.03—60.2 ND — ND 0.14—526.0 ND—89.0 ND—116.0 参考文献 [34-35] [36-38] [39-40] [37,41] [30,42] [43-44] [37,45] 表 4 中国典型湖泊沉积物中抗生素的浓度(ng·g−1)
Table 4. The concentrations of antibiotics in sediment of typical lakes in China(ng·g−1)
抗生素
Antibiotics太湖
Taihu Lake巢湖
Chaohu Lake洞庭湖
Dongting Lake洪湖
Honghu Lake白洋淀
Baiyang Lake南四湖
Nansi Lake淀山湖
Dianshan Lake磺胺类 磺胺甲恶唑 ND—49.3 ND—0.5 ND—115.4 ND—505.5 ND—7.9 ND—20.6 ND—99.2 磺胺嘧啶 ND—8.6 — ND—38.7 10.7—1553.4 ND—2.1 ND—11.2 ND—2.2 磺胺二甲嘧啶 ND—99.8 — ND—15.4 ND—57.5 ND—6.9 ND—3.4 ND—5.8 四环素类 四环素 ND—112.2 — ND—84.4 604.2—5750.3 4.8—93.4 ND—4.4 ND—0.2 土霉素 ND—196.7 — ND—42.8 11.6—152.6 4.3—35.4 ND—7.9 ND—0.1 金霉素 0.013—4.3 — ND—83.5 113.0—1053.6 — ND—4.3 ND—7.4 喹诺酮类 诺氟沙星 ND—28.4 — ND — 49.4—1140.0 ND—47.1 ND 氧氟沙星 ND—52.8 — ND ND—34.3 ND—362.0 ND—39.4 ND—0.5 恩诺沙星 — — ND—4.3 — ND—13.0 ND—207.2 ND—88.6 大环内脂类 红霉素 ND—5.6 0.1—0.45 — — ND—3.0 — ND 脱水红霉素 ND—120.3 — — — — ND—1.1 — 罗红霉素 ND—45.2 1.8—10.1 — — ND—302.0 ND—5.8 0.10—0.45 参考文献 [34,46-47] [48] [39,49] [49-50] [30,42,51] [43] [45] 可用数据
Available dataAF
Assessment factor至少1种营养水平短期测定L(E)C50 1000 一种水生无脊椎动物或鱼类长期测定NOEC 100 在2个营养水平上进行2次长期测定NOEC 50 在3个营养水平上进行3次长期测定 10 表 6 我国典型区域地表水体中抗生素的风险熵(RQ)
Table 6. Risk quotients (RQ) of antibiotics in surface water in typical regions of China
抗生素
Antibiotics测试物种
Test species海河
Haihe River渭河
Weihe River长江三角洲
Yangtze River Delta汉江平原
Han River plain珠江三角洲
Pearl River Delta黄河三角洲
Yellow River Delta巢湖
Chaohu Lake太湖
Taihu Lake大通湖
Datong LakeS骆马湖
SLuoma LakeS太湖
STaihu LakeS汉江
SHanjiang River磺胺类 磺胺甲恶唑 藻类 — 10.9 7.987 0.197 0.120 — 2.653 0.259 1.89 11800 1.04 — 磺胺甲基嘧啶 藻类 — — 0.109 0.014 0.005 0.003 — — — — — — 四环素类 四环素 藻类 — — 0.009 0.331 0.014 0.116 0.017 0.559 0.0017 — — >0.1 土霉素 藻类 — 0.197 0.461 0.364 — 0.491 — 4.54 0.0035 — — >0.1 喹诺酮类 诺氟沙星 藻类 11.8 — 0.002 0.084 0.076 0.049 — — — — — — 细菌 — 0.526 — — — — — 2.61 — — — — 氧氟沙星 藻类 17.8 7.89 — 0.094 0.007 0.003 0.019 41.9 0 3.52 — >1 环丙沙星 藻类 0.017 3.66 — — — — — 135 1 — — >0.1 恩诺沙星 藻类 3.76 — — — — — — — 0.77 — — 0.01-1 细菌 — — — — — — — 7.95 — — — — 大环内脂类 红霉素 藻类 — — 0.195 19.075 1 1.165 — — — — — — 脱水红霉素 藻类 11.4 — — — — — — — — — — — 克拉霉素 藻类 2.35 — 0.006 0.045 — 0.119 — — — — — — 阿奇霉素 藻类 — — — — — — — — — — 1.32 — β-内酰胺类 阿莫西林 藻类 32.2 — — — — — — — — — — — 参考文献 [16] [55] [56] [56] [56] [56] [56] [57] [58] [59] [60] [61] 注:“S”表示沉积物中抗生素的风险评价。Note: "S" means the risk assessment of antibiotics in sediment. -
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