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Environmental Distribution Characteristics and Source Analysis of Antibiotics in Zhejiang Area

Yuyang Lei , Fangfang Li , Jie Ouyang , Minjie Li , Lianghong Guo

Progress in Chemistry ›› 2021, Vol. 33 ›› Issue (8) : 1414 -1425.

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Progress in Chemistry ›› 2021, Vol. 33 ›› Issue (8) : 1414-1425 DOI: 10.7536/PC200766
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Environmental Distribution Characteristics and Source Analysis of Antibiotics in Zhejiang Area
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Abstract

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

Graphical abstract

Keywords

antibiotics / environmental contamination / regional distribution / Zhejiang area

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Yuyang Lei, Fangfang Li, Jie Ouyang, Minjie Li, Lianghong Guo. Environmental Distribution Characteristics and Source Analysis of Antibiotics in Zhejiang Area. Progress in Chemistry, 2021, 33(8): 1414-1425 DOI:10.7536/PC200766

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1 Introduction

At present, antibiotics have been widely used in medical treatment, aquatic products and animal husbandry, and the main veterinary antibiotics are shown in Table 1 and Figure 1. When antibiotics enter organisms, 30% to 90% of them can not be metabolized, so they are discharged into the environment in the form of pathogens through feces and urine[1]. In addition, hospitals and pharmaceutical factories are also important sources of antibiotic emissions[2]. Antibiotics are widely distributed in the environment, and most of them exist in surface water, groundwater and wastewater. Quinolones (QNs) and tetracyclines (TCs) have large adsorption coefficients, and the larger the Kd(>1000 L·kg-1),Kd is, the easier the antibiotics are adsorbed by sediment or soil[3]. Antibiotics have become an environmental problem in many countries. For example, sulfonamides (SAs), fluoroquinolones (FQs), TCs, macrolides and trimethoprim have been detected in the aquatic environment of Vietnam, with concentrations in the 0~6.06 mg·L-1[4]. Antibiotics have been detected in sewage treatment plants and waters in agricultural areas in Germany, mainly from human use[5]. A total of 17 antibiotics, including FQs, SAs, nitroimidazoles and diaminopyrimidines, were detected in the Seine River in France[6]. Antibiotics in the environment have certain physiological effects on organisms. Studies have shown that exposure of nematodes to 1 mg·L-1 sulfamethoxazole (SMZ) can change the histone H3K4me3 site in their bodies, thus causing obesity[7]. The numbers of red blood cells and white blood cells in anchovy exposed to sulfamethazine (SM) were changed[8]. FQs can cause developmental malformations and cardiotoxicity in avian embryos[9]. Exposure of zebrafish to tetracycline (TC), a 20μg·L-1, can promote apoptosis of embryonic cells and cause developmental retardation[10]. Exposure of peripheral blood mononuclear cells to 2 mg·L-1 oxytetracycline (OTC) was associated with DNA damage[11].

2 Environmental Distribution of Antibiotic Residues in Zhejiang

Due to the characteristics of regional economic development in Zhejiang Province, the use of antibiotics is large and widely distributed, and a variety of antibiotic residues are detected in aquaculture wastewater, surface water, groundwater, soil, livestock and poultry manure and other environmental media in Zhejiang Province. The distribution of sampling points in Zhejiang Province for the antibiotic residue study from 2011 to 2019 is shown in Figure 2. The aquaculture industry in Zhejiang is developed, and the sampling points cover the whole area of Zhejiang, the number of which is much higher than that of pharmaceutical enterprises. Hangzhou and Jiaxing are large-scale breeding areas, and the concentration of antibiotics in livestock and poultry manure in Hangzhou is the highest in Zhejiang, reaching the 66.62 mg·kg-1, followed by Ningbo and Jinhua. The detected concentration of antibiotics in livestock and poultry wastewater in Jiaxing is the highest in Zhejiang Province, reaching the 994 000 ng·L-1, and the antibiotics used in livestock and poultry breeding are the main source of antibiotics in Zhejiang environment. In surface water, the two areas with the highest concentrations of antibiotics were Hangzhou and Ningbo, which reached 508.7 ng·L-1 and 328 ng·L-1 respectively, both of which were caused by residents'medication. Antibiotics were not detected in Kaihua section of the upper Qiantang River and Qiandao Lake, and the concentration of antibiotics in Hangzhou Bay, the estuary of the Qiantang River, was 39.62 ng·L-1, but exceeded the 500 ng·L-1 near the hospital in Hangzhou section of the Qiantangjiang River in the middle of the two areas, indicating that the Qiantangjiang River had a buffer effect on the increase of antibiotic concentration. Three important drinking water sources (Hangzhou Qiandao Lake, Lishui Shitang Reservoir and Quzhou Jiangshan Wanyao Reservoir) are far away from livestock and poultry breeding areas, which may be the reason why antibiotics were not detected in the three places. The highest concentrations of antibiotics in soil were detected in Ningbo (324.725μg·kg-1) and Hangzhou (260.14μg·kg-1). Generally speaking, the antibiotic pollution in northern Zhejiang is higher than that in southern Zhejiang, and Hangzhou is the most serious area of antibiotic pollution in northern Zhejiang, followed by Jiaxing and Ningbo.

2.1 Pollution of Antibiotics in Water

The breeding industry in Zhejiang Province is particularly developed, with livestock and poultry breeding accounting for 25% of the total agricultural output value of the province, especially pig farming and aquaculture[12]. Hangzhou, the capital of Zhejiang Province, has an aquaculture area of 1.233×105m2, with a total of more than 50 species. The total amount of aquaculture wastewater discharged is as high as 8623 m3 every year, and most of the aquaculture wastewater is mainly discharged into the main basins of Qiantang River, Fuchun River and Lanjiang River[13]. Because there is no complete antibiotic discharge standard in China, the sewage containing a large amount of antibiotics discharged from farms will flow into lakes and rivers. In Zhejiang, the vast majority of drinking water sources come from natural river basins such as Qiantang River, Dongtiaoxi River and Xin'an River, as well as artificial reservoirs such as Qiandao Lake and Wanyao Reservoir[14]. Antibiotic residues in various environmental media may enter the human body through a variety of ways, which has potential health risks.

2.1.1 Antibiotic contamination in wastewater

Wastewater includes farm wastewater, domestic sewage and wastewater from pharmaceutical enterprises and hospitals. It can be seen from Table 2 that the concentration of antibiotics in pharmaceutical wastewater is the highest in Zhejiang wastewater, reaching the 5 718 000 ng·L-1, and the concentration of antibiotics at the outlet of wastewater is similar to that of hospitals in Hangzhou[15][16]. Although the elimination rate of pharmaceutical wastewater treatment plants has reached > 99%, the effluent concentration of FQs antibiotics can still reach the 88 000 ng·L-1. The removal of most antibiotics in the environment mainly depends on microbial degradation, so the detected concentration of antibiotics in the effluent of pharmaceutical wastewater treatment plants and hospitals is still very high, which will increase the risk of bacterial resistance.
The aquaculture industry in Zhejiang Province is not only developed, but also widely distributed, with the focus on the northwest of Zhejiang Province. Jiaxing is an important base of pig breeding and production in Zhejiang Province, and the discharge of pig breeding wastewater exceeds the 4×106t every year. Wei Dan et al. Detected 10 kinds of antibiotics such as TCs, SAs and FQs in the biogas slurry of ten large-scale pig farms, the total concentration was as high as 1 090 000 ng·L-1, of which the concentration of TCs (39 800~1 060 000 ng·L-1) was the highest and the detection rate was as high as 91%, and the detection rate of OTC was the highest among TCs[17]. SAs(0~59 700 ng·L-1) and FQs(750~12 900 ng·L-1) are much lower than TCs. Song Xiaoyan et al. also tested antibiotics in Jiaxing pig-raising wastewater, and the results showed that the types and doses of antibiotics used in different farms in Jiaxing were quite different (as shown in Table 2)[18]. Wang et al. Detected the concentration of antibiotics at the outlets of livestock and poultry farms and the upstream sections of discharge rivers in Jiaxing, Shaoxing, Hangzhou, Huzhou, Ningbo and Jinhua. The results showed that the highest total concentration of antibiotics was detected in Jinhua (30 999 ng·L-1)[19]. Among the detected antibiotics, the concentration of HMMNI was the highest. Although the detection concentration of FF is not high, its detection rate is the highest. The utilization rate of HMMNI in Jiaxing and Ningbo is much higher than that in other areas, and these two areas are also large-scale breeding bases in Zhejiang, but the pollution level is lower than that in Jinhua, which may be due to the high total concentration of antibiotics caused by frequent mixed use of drugs in Jinhua. Wu Liqin et al. Detected antibiotics in wastewater from livestock and poultry farms in Zhejiang Province, and the results showed that the concentration of antibiotics in pig wastewater was higher than that in duck wastewater, and the detection rate of FF in the farm was more than 70%[20]. From the above results, it can be seen that the main types of antibiotics in livestock and poultry wastewater in Zhejiang are SAs (SMT and SMM), TCs (DC, CTC, OTC and TC) and FF, and the detection range is 0~994μg·L-1, but the detected concentration varies greatly between regions, and some antibiotics have a hundred-fold difference.
The two sewage treatment plants mainly receive domestic sewage from local residents, but also include pharmaceutical wastewater and livestock wastewater. The effluent concentration of the two sewage treatment plants is below the 500 ng·L-1, indicating that the contribution of domestic sewage to antibiotics in the environment in Zhejiang is less than that of pharmaceutical and livestock wastewater[21,22]. It is worth noting that the concentration of antibiotics in wastewater is related to the season, and the removal rate of antibiotics in sewage treatment plants varies significantly in different seasons, especially between summer and winter, and the removal rate in summer is lower than that in winter, which may be due to the higher activity of bacteria in activated sludge[22]. The concentration of antibiotics detected in Jiaxing pig farms in spring was 3.7 and 2 times higher than that in autumn and winter, respectively, because the amount of antibiotics used in spring would increase, resulting in high residual concentration.In summer, the water requirement of pigs increased significantly and the activity of bacteria degrading antibiotics also increased, so the detection concentration of antibiotic residues in pig farms in summer was lower[17].

2.1.2 Antibiotic contamination in surface water

Wastewater and sewage will be treated by treatment plants or directly discharged into surface water in Zhejiang without treatment, and aquaculture is widely distributed in Zhejiang. Wastewater containing antibiotics and antibiotics used in aquaculture will remain in natural watersheds or artificial reservoirs, resulting in antibiotic pollution of surface water.
The Qiantang River is an important river basin in Zhejiang Province. Zhang et al reported the first distribution map of antibiotic pollution in China. The antibiotic discharge density of the Qiantang River is in a high density area[23]. Tong et al. And Wang et al. Have detected antibiotics in Hangzhou section of Qiantang River. The detected types and concentrations of antibiotics are quite different. The reason is that the sampling point of the latter is near the hospital, so the concentration of antibiotics is high, but much lower than that of hospital wastewater (1998.8 ng·L-1). The reason may be that the large runoff of Qiantang River plays a dilution role[22][19][16]. Antibiotics were not detected in Kaihua section of the upper reaches of Qiantang River, but FQs and TCs were detected in Hangzhou Bay, the estuary of Qiantang River, and the concentrations were similar to Tong's results, ranging from 10~50 ng·L-1[24][25][22]. Li Peipei et al. Detected the residues of FQs in Zhoushan and Wenzhou mariculture farms respectively. CIP in FQs was detected in Zhoushan mariculture farm, but no FQs was detected in Wenzhou mariculture farm[24]. He Xin et al. Used HPLC-Q-TOF-MS technology to determine 42 antibiotics in Zhejiang freshwater aquaculture basin, and no antibiotics were detected in Kaihua section of Qiantang River.However, SAs were detected in the confluence of Fenshui River and Fuchun River in Tonglu, Fen Lake in Jiaxing, Yang Lake in Shaoxing, Jindong Reservoir (Shantang) in Jinhua and Qiankouyang in Linghu Lake in Huzhou, but the types of residual antibiotics were different in different waters[26]. ENR was also detected in Qiankouyang, Linghu, Huzhou, which is one of the three famous freshwater fish bases in China, so the concentration of antibiotics is higher than that in other areas, and there are more kinds of antibiotics. Zong Yanan et al. And Wang Ruijie et al. Detected the presence of TCs and β-lactam antibiotics in Lujiang River and Yuehu Lake in Ningbo respectively, and the highest concentration was generally in the 100~328 ng·L-1, which was higher than the detected concentration of antibiotics in other river basins in Zhejiang[27][28]. The high concentration of antibiotics in Yuehu Lake may be due to the relatively dense population in Ningbo, and the use of antibiotics by residents has become the main source of antibiotics. The use of antibiotics in industrial and agricultural areas may be the main source of antibiotics in Lujiang. There were many kinds of antibiotics (SAs, FQs, TCs, β-lactams, macrolides and furazolidones) in surface water in Zhejiang Province, and the concentration range was 0~508.7 ng·L-1. Except near Qiantang River Hospital, the concentration of antibiotics in most natural watersheds is low, which is much lower than that in wastewater. The antibiotic concentrations in surface water are detailed in Table 3.
Antibiotic contamination also exists in surface water of other provinces in China. The highest concentration of SAs antibiotics was detected in Baiyangdian Lake of Hebei Province, including SMZ(0~940 ng·L-1), SD(0.86~505 ng·L-1), NOR(0~156 ng·L-1), and other antibiotics were lower than 100 ng·L-1. TCs and SAs were the main antibiotics, followed by SD(0~56.2 ng·L-1), OTC(0~48.7 ng·L-1) and DC(0~39.7 ng·L-1), and other antibiotics were lower than 30 ng·L-1. SAs and FQs were the main pollution antibiotics in Dongting Lake, followed by SD(0~61.28 ng·L-1), SMZ(0~47.41 ng·L-1) and CIP(0~36.17 ng·L-1), and other antibiotics were lower than 30 ng·L-1[29]. In Taihu Lake of Jiangsu Province, TCs and SAs were the main antibiotics, followed by SMT(0~654 ng·L-1), TC(0~125 ng·L-1) and SMZ(7.6~91 ng·L-1), and other antibiotics were lower than 50 ng·L-1[30,31]. In the Huangpu River of Shanghai, TCs dominated in June, TC(15.07~113.89 ng·L-1), OTC(12.99~84.54 ng·L-1), other antibiotics were lower than 30 ng·L-1, SAs dominated in December, SMZ(14.85~623.27 ng·L-1), the highest concentrations of other antibiotics were generally in the range of 40~60 ng·L-1[32]. The concentration of antibiotics detected in freshwater lakes and reservoirs in Zhejiang is lower than that in Baiyangdian, which may be due to the fact that the sampling point of Baiyangdian is close to the sewage outlet[33]. In Zhejiang, except for the sampling points near Yuehu Lake and Qiantang River Hospital in Ningbo, the concentrations in other basins were similar to those in Poyang Lake and Dongting Lake. Although Poyang Lake and Dongting Lake also receive aquaculture wastewater, as the two largest freshwater lakes in China, they may have a strong buffer capacity for the increase of antibiotics or the sampling point is far away from the wastewater discharge outlet[34,35]. In Jiangsu, Zhejiang and Shanghai, the highest concentrations of antibiotics in Qiantang River and lakes in Zhejiang were lower than those in Taihu Lake in Jiangsu and Huangpu River in Shanghai, and the concentrations of antibiotics in the northern part of Taihu Lake were higher, where there were many farms.The reason why the concentration of antibiotics in Huangpu River is higher than that in Zhejiang lakes may be that the sampling point is near the farm, and the highest concentration of antibiotics in Zhejiang surface water is near the hospital[31].
Compared with developed countries, the concentration of SMX in Lake Mead, the largest reservoir in the United States, is 0.28~1200 ng·L-1[36]. Clarithromycin (CLA) was dominant in the Tama River, Japan, with the highest concentration reaching the 233 ng·L-1, and SMX was dominant in the river near Mount Akagi, exceeding the 70 ng·L-1[37]. Concentrations of SAs and FQs in European rivers are generally lower than in 100 ng·L-1,TCs and lower than in 10 ng·L-1[38], and SAs have not been detected in Spanish, Italian, French, or British rivers. The concentration of antibiotics in Zhejiang natural watershed is lower than that in the United States, higher than that in Europe, and similar to that in Japan. Because Lake Mead mainly receives wastewater from the city of Las Vegas, where tourism and vacation industries are developed, Lake Mead is a vulnerable water body, so the concentration is high[36]. However, the difference is that the detection of antibiotics in rivers in Japan provides the main contribution to the use of drugs by residents, while in Zhejiang, the use of drugs by aquaculture is the main factor.

2.1.3 Antibiotic contamination in drinking water sources

Antibiotics in drinking water sources can come from surface water, aquaculture, or soil contamination. According to the Zhejiang Regulation on the Protection of Drinking Water Sources, the Zhejiang Provincial Department of Water Resources and the Zhejiang Provincial Department of Ecology and Environment published the list of drinking water sources above the county level on June 19, 2020 (cited). Among the 94 water sources, there are 20 natural river basin water sources and 74 reservoirs. He Xin et al and Zheng Chongying et al did not detect the presence of antibiotics in the three water sources of Qiandao Lake in Hangzhou, Shitang Reservoir in Lishui and Wanyao Reservoir in Jiangshan, Quzhou, and He Xin et al did not detect the presence of antibiotics in the East and West Tiaoxi River, a river-type water source[26][39][26]. However, Li Yong and others detected antibiotics in Hongqiao and Cengang reservoirs in Zhoushan, mainly furazolidone, with concentrations of about 20 ng·L-1 and 55 ng·L-1, respectively[40]. Zhoushan is the area with the highest production of aquatic products in Zhejiang (1.67×109kg·Year-1), and its use of antibiotics is also higher than other areas, which may be the reason for the detection of antibiotics in Zhoushan Reservoir. Although the Zhejiang government attaches great importance to the protection of water sources and strictly manages the drinking water environment, it is worth noting that the concentration of antibiotics in Zhoushan Reservoir has reached the level of surface water.

2.2 Distribution of Antibiotics in the Manure of Livestock and Poultry

In addition to being discharged into the environment in the form of wastewater, the residual antibiotics in animals in farms are also discharged into the environment in the form of feces. Pig farming plays an important role in livestock and poultry farming in Zhejiang, accounting for 69.9% of livestock and poultry farming[12]. The data of Wang Li et al and Wang et al show that Hangzhou is the most serious area of antibiotic residues in pig manure, exceeding 60 mg·kg-1, Ningbo and Jinhua also exceed 50 mg·kg-1, other areas are in 20 mg·kg-1, Hangzhou, Jinhua and Ningbo use more TCs, Jinhua uses more SAs than other areas[41][42]; The concentrations of three kinds of TCs in pig manure collected by Shen et al in ten areas of Zhejiang Province were not very different, and the highest was CTC, but the feeding amount of CTC was 2 to 4 times that of OTC and TC, which indicated that the metabolic degree of different antibiotics in animals was also different, so the amount of antibiotics used in aquaculture and medicine could only determine the residual amount of antibiotics in the environment to a certain extent[43]. The concentration of antibiotics in chicken manure and cattle manure was lower than that in pig manure, and SAs and TCs were mainly used in pigs and poultry, while SAs was not detected in cattle manure[44]. The concentration of antibiotics in feces was higher in Hangzhou, Ningbo and Jinhua, where the livestock and poultry breeding industry was more developed. The main antibiotics detected were SAs, TCs and FQs, among which the detected concentration of TCs was the highest, the main types were similar to those of livestock and poultry wastewater, and the detected concentration range was 0~66.62 mg·kg-1. The values of antibiotic concentrations in feces are shown in Table 4.

2.3 Distribution of antibiotics in soil and sediment

There are two main sources of antibiotics in the soil, one is the adsorption of antibiotics in the surrounding waters to the soil, and the other is that people use livestock and poultry manure containing antibiotics as fertilizer on the land. However, due to the different Kd values of adsorption coefficients of different antibiotics, the distribution concentrations of TCs and FQs in sediments and soils will be different. TCs and FQs have larger Kd values and are easy to exist in sediments and soils[3]. SAs and CPs are easy to exist in water due to their small Kd. Ni Zhongying et al. Detected a variety of antibiotics in the soil of 27 protected vegetable bases in Hangzhou, among which ENR and OTC were the most detected, and the detection rate and concentration of antibiotic residues in the farmland applied with livestock manure organic fertilizer were higher than those in the farmland applied with ordinary chemical fertilizer[45]. The antibiotic residues detected in farmland, woodland and garden soil in Haishu District of Ningbo were also different, TCs were the main antibiotics in farmland and garden, but FQs were the main antibiotics in woodland, the detected concentrations of most antibiotics were similar, between 0~2μg·kg-1, but the detected concentrations of TCs exceeded the 20μg·kg-1,CTC and even exceeded the 300μg·kg-1, which may be related to the surrounding livestock and poultry farms[46]. Li Yong found that the residue of furazolidone in the soil around three reservoirs in Zhoushan, Zhejiang, was much higher than that of the other four antibiotics, reaching the 87.5μg·kg-1, which was higher than that of the reservoir sediment (20μg·kg-1), indicating that these antibiotics would be adsorbed in the soil, and the adsorption was stronger than that in the water sediment[40]. In the sediments of Hangzhou Bay, TCs and FQs are the main components, and their concentrations are also lower than those of the 20μg·kg-1[25]. From the point of view of antibiotic residues in soil and sediment, the main antibiotics detected in soil and sediment were TCs and FQs, and the residues in Hangzhou and Ningbo were higher than those in other areas, and manure application played a major contribution. From Table 4, it can be seen that Hangzhou and Ningbo have higher residues of antibiotics in feces, which leads to higher concentrations in soil. The detected concentration range of antibiotics in soil and sediment in Zhejiang is 0~324.725μg·kg-1, and the specific detected concentration range of samples is shown in Table 5.

3 Antibiotic residues in food

In order to prevent the occurrence of diseases and promote growth, farmers will use antibiotics on livestock, poultry and aquatic animals. In addition to the antibiotics that can not be metabolized in food animals, antibiotics in the environment will re-enter food animals through the food chain and food web, thus causing antibiotic exposure to the human body. On April 1, 2020, China implemented the National Food Safety Standard Maximum Residue Limits of Veterinary Drugs in Food, which clearly stipulates the maximum residues of veterinary antibiotics in animal tissues. Li Ying et al. Detected the presence of antibiotics in freshwater fish and shrimp in Xiaoshan District of Hangzhou, ENR, CIP and OFL were detected, the highest value of ENR reached 750μg·kg-1, and the detection rate of antibiotics in fish was higher than that in shrimp[47]. Huang Xihui et al. Detected TCs residues in poultry food and shrimp in Hangzhou urban area, and found no TCs in eggs. The detection rate of total antibiotics in chicken (52.94%) was the highest, mainly DC and OTC[48]. Liu Shaoying et al. Detected the residues of FQs in food in Hangzhou, and the results showed that the detection rate of FQs in shrimp was the highest (62.5%), even ranked second in eggs, and the detection rate of ENR was the highest in the total samples[49]. Hua Xiaocheng et al did not detect the presence of SAs and FQs in chicken from Wenzhou market, indicating that the use of antibiotics varies greatly among different food animals[50]. SMZ, SM and sulfaquinoxaline were detected in 5 out of 300 chicken breast samples from Ningbo market[51]. Chloramphenicol (CAP) and TC residues were detected in fresh milk and sterilized milk in a major area of Zhejiang Province, but the detection rates were very low (7. 4%) and (2. 1%), indicating that CAP had been used in dairy cows in Zhejiang Province, but the "Veterinary Drug Management Regulations" implemented in China on December 27, 2019 clearly stipulated that CAP was prohibited from being used in food animals[52]. A variety of antibiotic residues were detected in honey from Zhejiang honey production base, and the detection rate of CIP was almost ten times higher than that of other antibiotics[53].
Comparing the test results in Table 6 with the latest food safety standard, it is found that only the ENR in the fish in Xiaoshan District of Hangzhou exceeds the standard, which is much higher than the 100μg·kg-1 in the food standard, and the detection rate (33.3%) is also the highest, indicating that there is a possibility of excessive use of ENR in this batch of fish farms. Other monitoring data were up to the standard and did not exceed the national food standards, indicating that the government in Zhejiang has paid enough attention to the management of antibiotic residues in food.
Although the use of antibiotics has significantly reduced the morbidity and mortality of infectious diseases, with the increase of their use, the adverse effects of antibiotics on human body have gradually emerged. The most common allergic reaction is caused by antibiotics as haptens[54]. Under the condition of normal clinical dosage, many antibiotics (FQs, SAs, TCs and β-lactams) can cause drug-induced liver injury in special population (liver dysfunction), resulting in hepatitis, cholestasis, jaundice and ascites (liver injury)[55]. The use of antibiotics in pregnant and lactating women may have potential teratogenic effects on the fetus[56]. TCs were discovered in the 1960s to cause tooth pigmentation in children[57]. Beta-lactam antibiotics may also cause kidney damage, neutropenia, nerve damage and mitochondrial damage, leading to muscle spasms and seizures in special populations (patients with renal insufficiency/encephalopathy)[54]. FQs can block voltage-gated potassium channels in cardiomyocytes, causing cardiovascular disease, neurotoxicity, and increased risk of tendon rupture[54]. Most of the above adverse reactions are related to the dose of antibiotics, and the residual antibiotics in drinking water and food invisibly increase the intake dose of human body, thus increasing the risk of these adverse reactions in human body (especially in special groups).

4 Conclusions and outlook

The concentration of antibiotics in surface water in Zhejiang is the lowest in Jiangsu, Zhejiang and Shanghai, which may be due to the implementation of the "five-water co-governance" project in Zhejiang in 2013. The detected concentrations of antibiotic residues in Zhejiang waters were in the following order: sewage treatment plants and livestock and poultry wastewater outlets > watersheds near farms and hospitals > aquaculture reservoirs and natural watersheds > drinking water sources such as Qiandao Lake. The concentration of antibiotics in the whole basin of Qiantang River is lower than that in the 500 ng·L-1. Although it will flow through the areas where high concentrations of antibiotics are discharged, such as hospitals and sewage treatment plants, the Qiantang River has a good buffer capacity, which makes the concentration in the estuary lower than that in the 50 ng·L-1. The aquaculture industry contributed the most to the environmental antibiotics in Zhejiang, among which SAs and TCs were the most widely used in livestock and poultry farming, and FQs were the most widely used in aquaculture. In livestock and poultry farming, pigs contributed the most, followed by poultry. Jiaxing, Hangzhou and Quzhou in the northwest of Zhejiang Province have the top three livestock and poultry manure production in the province, and the total livestock and poultry manure production in the three regions accounts for nearly half of the province[12]. The concentrations of antibiotics in livestock and poultry manure and wastewater in Hangzhou and Jiaxing were the highest in the province, but the detection of antibiotics in Quzhou was relatively lacking. Antibiotic pollution in Ningbo should not be ignored. The concentrations of antibiotics in surface water and livestock manure in Ningbo were higher than those in other areas of Zhejiang Province, and the concentrations of antibiotics in soil were the highest in the province. The demand for pig farming in Jinhua is not low, and the concentration of antibiotics in livestock and poultry manure is second only to that in Hangzhou. Generally speaking, the northern part of Zhejiang is a serious area of antibiotic pollution, and Hangzhou is the most serious in the northern part of Zhejiang. Antibiotics in the environment mainly come from livestock and poultry, but they will return to animals through the food chain and food web.Water, soil, food and other ways of exposure to antibiotics increase the risk of human exposure[58,59].
Although the concentration of antibiotics in natural watersheds is much lower than that in experimental animals, they may be enriched in organisms, resulting in increased concentrations in vivo and posing a potential threat. Therefore, according to the situation of antibiotic pollution in Zhejiang Province, combined with the key issues of antibiotic pollution research.We believe that the future antibiotic research in Zhejiang should: (1) Continue to carry out extensive and comprehensive investigation of the environmental content of antibiotic residues in various regions of Zhejiang, and clarify the level and main types of antibiotic pollution in various regions of Zhejiang. There are obvious differences in the types and quantities of antibiotic pollution in different regions of Zhejiang, especially in the soil and water around the farms and pharmaceutical enterprises, where there are many antibiotic residues and high detection quantities. Continuous and extensive tracking of the level and types of antibiotic pollution will help to explore the characteristics of antibiotic pollution in Zhejiang. (2) Combining with the regional characteristics and economic development characteristics of Zhejiang Province, the migration and transformation law of environmental residual antibiotics and their impact on the ecosystem were studied to promote the exploration of ecological and health hazards and mechanisms of antibiotic pollution. Studies have shown that some antibiotics may have toxic effects on organisms, indicating that antibiotic pollution has posed a potential threat to ecosystems and human health, but the drinking water safety standards and ADI of antibiotics have not yet been established, so it is impossible to carry out a reliable human health risk assessment, which needs further study.

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Funding

National Natural Science Foundation of China(21878302)

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