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化学进展 2021, Vol. 33 Issue (8): 1414-1425 DOI: 10.7536/PC200766 前一篇   后一篇

• 综述 •

浙江地区抗生素残留的环境分布特征及来源分析

雷雨洋1,2, 李方方2,3, 欧阳洁2,3, 李敏杰3,*(), 郭良宏2,3,*()   

  1. 1 中国计量大学生命科学学院 杭州 310018
    2 中国计量大学环境与健康科学研究院 杭州 310018
    3 中国计量大学质量与安全工程学院 杭州 310018
  • 收稿日期:2020-07-28 修回日期:2020-09-02 出版日期:2021-08-20 发布日期:2020-12-28
  • 通讯作者: 李敏杰, 郭良宏
  • 基金资助:
    国家自然科学基金项目(21878302)
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Environmental Distribution Characteristics and Source Analysis of Antibiotics in Zhejiang Area

Yuyang Lei1,2, Fangfang Li2,3, Jie Ouyang2,3, Minjie Li3(), Lianghong Guo2,3()   

  1. 1 College of Life Sciences, China Jiliang University,Hangzhou 310018, China
    2 Institute of Environmental and Health Science,Hangzhou 310018, China
    3 College of Quality and Safety Engineering, China Jiliang University,Hangzhou 310018, China
  • Received:2020-07-28 Revised:2020-09-02 Online:2021-08-20 Published:2020-12-28
  • Contact: Minjie Li, Lianghong Guo
  • Supported by:
    National Natural Science Foundation of China(21878302)

近年来在天然水体、土壤、动植物及其排泄物中都检测到了抗生素的存在,抗生素在环境中的残留已经引起广泛关注。本文调研和梳理了2011~2019年间针对浙江地区各种环境介质中抗生素残留状况的相关研究工作,对浙江地区废水、地表水、地下水、土壤和养殖畜禽粪便等环境介质中抗生素残留的主要种类、污染水平和分布特征进行了分析总结,并对抗生素残留的可能来源进行了分析。结果显示,浙江地区环境中抗生素残留的主要种类为四环素类、磺胺类、氟喹诺酮和氯霉素类。杭州、金华、嘉兴等地的畜禽养殖废水中检测出较高浓度抗生素,最高至994 μg·L-1;畜禽粪便中达到了66.62 mg·kg-1,为浙江地区环境中抗生素污染的主要来源之一。制药废水中的抗生素浓度更是达到了5.7 mg·L-1,这些废水虽然经过污水处理厂处理,但在部分处理过的废水中仍能检出抗生素,浓度最高达88 μg·L-1,并被直接排入天然水体。水产养殖区域中残留的抗生素也会不经处理直接进入地表水中,导致地表水污染,浙江地表水中抗生素浓度最高为508.7 ng·L-1,但是大部分流域小于100 ng·L-1。迄今为止,尚未在千岛湖、丽水石塘水库、衢州江山碗窑水库和东西苕溪等饮用水水源地中检测到抗生素,但舟山地区饮用水源中抗生素浓度达到了55 ng·L-1。虽然地表水中抗生素残留水平相对较低,由于这些水体用于水产养殖、畜禽饮水及农田灌溉,使得环境中的抗生素流入畜禽及农作物中,最终可能导致食品污染。因此,未来工作中需要对浙江各地区进行抗生素环境残留的全面、持续调查,结合浙江地区地域特征及经济发展特色,加强环境中抗生素迁移转化规律的研究,并及时开展抗生素环境污染对生态系统和人体健康效应的研究。

关键词： 抗生素, 环境污染, 分布特征, 浙江地区

In recent years, antibiotics have been detected in natural water bodies, soil, animals and plants and their excreta and have attracted widespread attention. This review summarizes and analyzes the studies published between 2011 and 2019 on the investigations of antibiotic residues in various environmental media in Zhejiang area. The results show that tetracyclines, sulfonamides, fluoroquinolones and chloramphenicols are the dominant antibiotics in the aquatic environment of Zhejiang. The concentration of antibiotics reaches 994 μg·L-1 in the wastewater of farming livestock and poultry in Hangzhou, Jinhua, and Jiaxing, and it is as high as 66.62 mg·kg-1 in the livestock and poultry manure, suggesting that the livestock and poultry breeding industry is one of the major sources of antibiotic pollution in the environment in Zhejiang. Furthermore, the concentration of antibiotics in the pharmaceutical wastewater reaches 5.7 mg·L-1. It is noted that antibiotics are still detected in the effluents of wastewater treatment plants, and their concentrations could reach 88 μg·L-1. The treated wastewaters are directly discharged into natural water. Residual antibiotics in the aquaculture areas could also enter the surface water directly without treatment. The concentration of antibiotics in the surface water of Zhejiang is 508.7ng·L-1, but for most of the basin, the concentration is less than 100 ng·L-1. Until now no antibiotics have been detected in the drinking water sources in Zhejiang such as Qiandao Lake, Lishui Shitang Reservoir, Quzhou Jiangshan Wanyao Reservoir and Tiaoxi River. However, in Zhoushan, the concentration of antibiotics in drinking water sources has reached 55 ng·L-1. Although the levels of the antibiotic residues in the surface water are relatively low, their impacts should not be underestimated. These water bodies serve as water sources for aquaculture, livestock and poultry, and farmland irrigation, therefore the antibiotics residues could get back into livestock, poultry and crops, and potentially cause food contamination. It is thus recommended that future research could focus on continuous and comprehensive monitoring of antibiotic residues in the environment in Zhejiang, the fate and transformation of antibiotics due to the unique environmental factors and industrial structures of the region, and their potential adverse effect on ecological systems and human health.

Contents

1 Introduction

2 Environmental distribution of antibiotic residues in Zhejiang

2.1 Contamination of antibiotics in water

2.2 Distribution of antibiotics in the feces of farmed livestock and poultry

2.3 Distribution of antibiotics in soil and sediment

3 Antibiotic residues in food

4 Conclusion and outlook

Key words: antibiotics, environmental contamination, regional distribution, Zhejiang area
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表1 主要兽用抗生素一览
Table 1 Overview of major veterinary antibiotics
Classification Compounds Abbreviation Molecular mass CAS Use/Features
Tetracyclines
TCs		 Doxycycline DC 444.4 564-25-0 A class of broad-spectrum antibiotics produced by Actinomycetes ; Widely used for infections caused by a variety of bacteria and rickettsia, chlamydia, mycoplasma, etc.;As a growth promoter, used in animal feed
Tetracycline TC 444.4 60-54-8
Chlorotetracycline CTC 478.9 57-62-5
Oxytetracycline OTC 460.4 79-57-2
Sulfonamides
SAs		 Sulfamethoxazole SMZ 253.3 723-46-6 Especially effective against Staphylococcus and Escherichia coli
Sulfamethazine/Sulfadimidine SMT 278.3 57-68-1 Used for coccidiosis of livestock and poultry
Broad-spectrum antibacterial drugs
Sulfamonomethoxine SMM 280.3 1220-83-3
Sulfadiazine SD 250.3 68-35-9
Sulfachloropyridazine SCP 284.7 80-32-0
Fluoroquinolones
FQs		 Ofloxacin OFL 361.4 82419-36-1 Broad-spectrum antibacterial drugs
Ciprofloxacin CIP 331.3 85721-33-1 The third-generation quinolone antibacterial drug with strong antibacterial effect
Enrofloxacin ENR 359.4 93106-60-6 This product is designated as a special animal medicine by the country
Norfloxacin NOR 319.3 70458-96-7 Used for infections caused by sensitive bacteria
Chloramphenicols
CPs		 Florfenicol FF 358.2 73231-34-2 Animal-specific drugs, banned for lactating cattle and sheep and poultry during laying period
图1 主要兽用抗生素结构及辛醇水分配系数
Fig. 1 Structure and octanol-water partition coefficient(Kow) of major veterinary antibiotics
图2 浙江地区2011~2019年间环境中抗生素检测采样点分布图
Fig. 2 Environmental distribution map of antibiotic sampling sites in Zhejiang area between 2011 and 2019
表2 浙江地区废水中抗生素的污染水平
Table 2 The concentration of antibiotics in wastewater in Zhejiang
Sample type Sampling area Major antibiotics Concentration/(ng·L-1) Detection rate/% Year ref
Influent Effluent
Hospital Qiantang River Trimethoprim(TMP) 220.8~744.2 / 2012 16
Erythromycin A(ERY-A) 33~1325.5 /
NOR 763~1155.6 /
OFL 90.6~1998.8 /
PWWTPa Southeastern Zhejiang OFL 1 161 000 88 000 / 2017 15
ENR 5 718 000 42 800 /
CIP 4 346 000 320 /
WWTPb Hangzhou OFL 1409 429 / 2011 22
CIP 268 199 /
NOR 268 96 /
WWTP Zhejiang SMZ 426 70* / 2016 21
FWc(Duck) Zhejiang SMT NDd~150 / 2012 20
FF ND~980 /
FW(Pig) Zhejiang SMT ND~193 500 /
SMM ND~3400 /
FW(Pig) Jiaxing OTC 1600~994 000 / 2014 17
CTC 2950~228 000 /
FW(Pig) Jiaxing DC 8750 1050 / 2017 18
SMT 2870 600 /
TC 1780 200 /
CIP 1540 280 /
FW Jiaxing,Shaoxing,Hangzhou,Huzhou,Ningbo,Jinhua HMMNI 199.8~25 874.1 13.9 2018 19
SMM 50~19 990 20.8
SCP 2637.4~6093.9 5.6
FF 30~3396.6 31.9
表3 浙江地区地表水中抗生素的污染水平
Table 3 The concentration of antibiotics in surface water in Zhejiang
Sampling area Major antibiotics Concentration/(ng·L-1) Detection rate/% Year ref
Qiantang River OFL 48.7 / 2011 22
ENR 14.6 /
CIP 10.2 /
Qiantang River NOR 508.7 / 2012 19
PEN-V 447 /
Hangzhou Bay NOR 15.05~39.62 100 2019 25
OTC 11.25~30.24 100
TC 11.06~26.28 100
Lujiang River,Ningbo CTC 133 / 2018 27
TC 128 /
Thiamphenicol(TPC) 104.2 /
Yuehu Lake,Ningbo Ampicillin(AMC) NDa~328 / 2018 28
Cefalexin(LEX) ND~283 /
NOR ND~267 /
SMM ND~219 /
Zhoushan CIP 10 / 2015 24
Kaihua,Upper
Qiantang River		 / / / 2016 26
Tonglu "Two Rivers" SMZ 22.5~36.3 /
SMM 32.3~50.1 /
SCP 18.8~30.6 /
Fenhu Lake,Jiaxing SMZ 44.2~53.6 /
Sulfapyridine(SP) 26.3~41.9 /
Yanghu Lake,Shaoxing SMM 60.5~76.3 /
Jindong Reservoir,Jinhua SMZ 20.33~30.9 /
LinghuLake,Huzhou SMZ 26.8~45 /
SP 18.9~34.5 /
ENR 94.2~113.2 /
表4 浙江地区养殖畜禽粪便中抗生素的污染水平
Table 4 The concentration of antibiotics in the livestock and poultry manure in Zhejiang
Sample source Sampling area Major antibiotics Concentration/
(mg·kg-1),DWa		 Year ref
Pig Huzhou,Jiaxing,Shaoxing,
Zhoushan,Ningbo,Jinhua,
Quzhou,Lishui,Wenzhou,Taizhou		 OTC 1.68~10.4 2014 43
TC 1.01~12.11
CTC 1.28~18.25
Pig Hangzhou CTC 0.32~66.62 2014 41
TC 0.40~7.63
Chickens CTC 1.74~3.32
NOR NDb~2.71
Chickens Zhejiang DC 0.424~9.376 2016 44
CTC 0.981~5.628
SMT 0.0707~4.184
Pig OTC 0.524~16.280
CTC 0.34~15.872
DC 0.178~14.641
TC 0.589~4.145
ENR 0.0064~4.091
Cattle TC 1.74
DC 0.115~2.044
OTC 1.12
Pig Huzhou SD 6.21~16.40 2017 42
SM 6.53~13.97
Hangzhou CTC 17.92~57.95
SM 2.58~10.99
Ningbo CTC 5.51~55.12
OTC 1.19~15.68
SM 3.77~16.50
Jinhua SD 7.43~46.37
SMT 17.55~37.32
TC 16.07~40.39
CTC 4.58~54.74
Wenzhou SD 5.26~14.28
Taizhou SM 6.97~11.32
表5 浙江地区土壤和沉积物中抗生素的污染水平
Table 5 The concentration of antibiotics in soil and sediment in Zhejiang
Sample type Sampling area Major antibiotics Concentration/(μg·kg-1),DWa Detection rate/% Year ref
Soil Chengbei,Zhoushan Furazolidone NDb~87.5 / 2014 40
Soil Haishu,Ningbo CTC ND~324.725 / 2017 46
Soil Hangzhou OTC ND~260.14 62.96 2017 45
ENR ND~102.23 48.15
sediment Hangzhou Bay NOR 5.2~13.6 87.5 2019 25
TC 0.84~5.61 75
OTC 0.75~4.36 75
表6 浙江地区动物性食品中抗生素残留状况
Table 6 Antibiotics residues in animal food in Zhejiang
Area Major antibiotics Concentration Sample source Detection rate Standard ESa(Yes/No) Year ref
/μg·kg-1 /% /μg·kg-1
Hangzhou DC 0.87~7.36 Shrimp/Chicken 16.67 100 / 2018 48
OTC 1.99~12.9 Shrimp/ 9.09 200 No
ENR 0.78~68.3 Chicken/Pork 14.8 100 No
CIP 0.69~66.9 Fish/Shrimp 3.4 100 No
NOR 2.7~10.4 2.3 / /
ENR 4.0~750.0 33.3 100 Yes 2018 47
CIP 2.3~65.9 23.1 100 No
OTC 21.6 1.28 200 No
Ningbo SM 0.418~2.28 Chicken / 100 No 2014 51
SMZ 16.4 / 100 No
Sulfaquinoxaline 2.93 / 100 No
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