The residual antibiotics in the environment have lately caused widespread concerns. However, little information is available on the antibiotic bioaccumulation and its health risk in drinking water resources of South China. Therefore, the occurrence, distribution, and health risk of four quinolone antibiotics including ofloxacin (OFX), norfloxacin (NOR), ciprofloxacin (CIP), and enrofloxacin (ENR) in the Qingshitan reservoir using high-performance liquid chromatography were investigated. Results revealed that the concentrations in water, sediment, and edible fish ranged from 3.49-660.13 ng/L, 1.03-722.18 μg/kg, and 6.73-968.66 μg/kg, respectively. The ecological risk assessment via the risk quotient (RQ) method showed that the values in sediment were all greater than 1, posing a high risk to the environment. The health risk index of water samples was at the maximum acceptable level, with OFX at the top while the rest were at the medium risk level. The main edible fish kinds of the reservoir had high dietary safety and the highest contaminations were found in carnivorous feeding habits and demersal habitat fishes with OFX as the highest magnitude. Source identification and correlation analysis using SPSS showed significant relationships between NOR with pH and turbidity (in water), as well as total phosphor (TP) and total organic carbon (TOC) in sediment. NOR was the highest in sediment which mostly sourced from livestock wastewater, croplands irrigation drain water, and stormwater. Correlations between CIP and ENR with TP were significant, while OFX was positively associated with total nitrogen (TN) which mainly originated from urban sewage as well as directly dosed drugs in fish farms. In conclusion, our results are of great significance for ensuring the safety of drinking water and aquatic products in this region.

College of Environmental Science and Engineering Guilin University of Technology Guilin 541004 China

Coordinated Innovation Center of Water Pollution Control and Water Security in Karst Area Guilin University of Technology Guilin 541004 China

Department of Applied Ecology Faculty of Environmental Sciences Czech University of Life Sciences Prague Kamýcká 129 16500 Prague Czech Republic

Fisheries College Ocean University of China Qingdao 266003 China

Guangxi Key Laboratory of Environmental Pollution Control and Technology Guilin University of Technology Guilin 541004 China

School of Environment and Energy South China University of Technology Guangzhou 510641 China

Sub Campus Depalor Okara University of Agriculture Faisalabad Okara 56130 Pakistan

Zobrazit více v PubMed

Yu ZY. Analysis of current situation of antibiotic abuse and countermeasures. Econ. Res. Guide. 2011;145(35):314–315.

Adachi F, Yamamoto A, Takakura KI, et al. Occurrence of fluoroquinolones and fluoroquinolone-resistance genes in the aquatic environment. Sci. Total Environ. 2013;444(444C):508–514. doi: 10.1016/j.scitotenv.2012.11.077. PubMed DOI

Wu TT, Zhang RJ, Wang YH, et al. Investigation of the typical antibiotics in the sediments of the Yongjiang River, Nanning City, South China. China Environ. Sci. 2013;33(2):336–344.

Ruan YF, Chen JM, Guo CS, et al. Distribution characteristics of typical antibiotics in surface water and sediments from freshwater aquaculture water in Tianjin suburban areas, China. J. Agro-Environ. Sci. 2011;30(12):2586–2593.

Liang X, Chen B, Nie X, et al. The distribution and partitioning of common antibiotics in water and sediment of the Pearl River Estuary, South China. Chemosphere. 2013;92(11):1410–1416. doi: 10.1016/j.chemosphere.2013.03.044. PubMed DOI

Shi H. The Analysis Method of Twenty Antibiotics in the Sediment and its Application. Shanghai: East China Normal University; 2014.

Zhang WR. The Distribution of Typical Antibiotics Strains in the Sediment Environments of Dalian. Dalian: Dalian University; 2014.

Xu C. Contamination of Antibiotics and antibiotics resistance genes in water, soil and sediment of the Three Gorges Reservoir. 2017. Wuhan: the Wuhan Botanical Garden of the Chinese Academy of Sciences (in Chinese).

Yang YT, He XT, Nie XP, et al. Preliminary investigation of three quinolones in the muscle tissues of four fishes collected from the markets in Guangzhou City. J. Environ. Health. 2009;26(2):109–111.

Wang H, Ren L, Yu X, et al. Antibiotic residues in meat, milk and aquatic products in Shanghai and human exposure assessment. Food Control. 2017;80:217–225. doi: 10.1016/j.foodcont.2017.04.034. DOI

Naik OA, Shashidhar R, Rath D, et al. Characterization of multiple antibiotic resistance of culturable microorganisms and metagenomic analysis of total microbial diversity of marine fish sold in retail shops in Mumbai, India. Environ. Sci. Pollut. Res. Int. 2017;25(7):6228–6239. doi: 10.1007/s11356-017-0945-7. PubMed DOI

Uchida K, Konishi Y, Harada K, et al. Monitoring of antibiotic residues in aquatic products in urban and rural areas of Vietnam. J. Agric. Food Chem. 2016;64(31):6133–6138. doi: 10.1021/acs.jafc.6b00091. PubMed DOI

Bakeraustin C, Mcarthur JV, Tuckfield RC, et al. Antibiotic resistance in the shellfish pathogen Vibrio parahaemolyticus isolated from the coastal water and sediment of Georgia and South Carolina, USA. J. Food Prot. 2008;71(12):2552–2558. doi: 10.4315/0362-028X-71.12.2552. PubMed DOI

Richardson BJ, Lam PKS, Martin M. Emerging chemicals of concern: Pharmaceuticals and personal care products (PPCPs) in Asia, with particular reference to Southern China. Mar. Pollut. Bull. 2005;50(9):913–920. doi: 10.1016/j.marpolbul.2005.06.034. PubMed DOI

Liu X. Pollution Level, Source and Ecological Risk of Typical Antibiotics in the Dongting Lake, China. Jinan: Shandong Normal University; 2017.

Turiel E, Bordin G, Rodríguez AR. Trace enrichment of (fluoro)quinolone antibiotics in surface waters by solid-phase extraction and their determination by liquid chromatography-ultraviolet detection. J. Chromatogr. A. 2003;1008(2):145–155. doi: 10.1016/S0021-9673(03)00975-0. PubMed DOI

Ying G G. Antibiotic use and pollution in the river basins of China. The 30th Academic Annual Meeting of China Chemical Society. 2016 (in Chinese).

Sun K. Contamination Characteristics and Ecological Risk Assessment of Typical Antibiotics in the Water of the Hongze Lake. Nanjing: Nanjing Agricultural University; 2015.

Wang J W. Distribution characteristics and ecological risk assessment of antibiotics in surface water of Xi’an section of Weihe river. 2018. Xi’an: Xi’an University of Technology (in Chinese).

Chen L, Qian JP, Zhang L, et al. Investigation and evaluation of water quality of Qingshtan reservoir in Guilin city. Guangdong Agric. Sci. 2013;40(5):160–164.

Zheng YL, Han PL, Dai JF, et al. Change of Inflow Runoff into the Qingshitan Reservoir in Guilin City. Water Conserv. Sci. Technol. Econ. 2012;18(8):46–48.

Liang Y, Chen G, Zeng H, et al. Characteristics and risk assessment of organochlorine pesticide residues in surface sediments collected at the Qingshitan Reservoir. Toxicol. Environ. Chem. Rev. 2016;98(5–6):658–668. doi: 10.1080/02772248.2015.1133384. DOI

Cheng YP, Kang P, et al. Pollution characteristics and potential ecological risk assessment of heavy metals in sediments of Qingshitan reservoir. Yangtze River. 2017;48(10):24–29.

Kall J. Limnology: Inland Water Ecosystem. Beijing: Higher Education Press; 2011.

Miu ZL, Zong FS, Jiang YP. Study on Hydrographic Karst and Tourism Resources in Guilin. Wuhan: China University of Geosciences Press; 2004.

Qi SS, Yang X. Study on ecological restoration mode of reservoir eutrophication by fish cage culture. Environ. Sci. Manag. 2012;37(11):151–154.

Xu WH, Zhang G, Zou SC, et al. Determination of selected antibiotics in the Victoria Harbour and the Pearl River, South China using highperformance liquid chromatography-electrospray ionization tandem mass spectrometry. Environ. Pollut. 2007;145:672–679. doi: 10.1016/j.envpol.2006.05.038. PubMed DOI

Liang XM, Shi Z, Huang XP, et al. Occurrence of antibiotics in typical aquaculture of the Pearl River Estuary. Ecol. Environ. Sci. 2013;22(2):304–310.

Zhou LJ, Ying GG, Zhao JL, et al. Trends in the occurrence of human and veterinary antibiotics in the sediments of the Yellow River, Hai River and Liao River in northern China. Environ. Pollut. 2011;159(7):1877–1885. doi: 10.1016/j.envpol.2011.03.034. PubMed DOI

He XT, Wang Q, Nie XP, et al. Residues and health risk assessment of sulfonamides in sediment and fish from typical marine aquaculture regions of Guangdong province, China. Environ. Sci. 2014;35(7):2728–2735. PubMed

Lu RK. Soil Argrochemistry Analysis Protocoes. Beijing: Agriculture Science Press; 1999.

Xu J. Application of High Performance Liquid Chromatography in Analysis of Antibiotics in Seafood. Harbin Institute of Technology: Harbin; 2016.

European Commission. Technical Guidance Document on Risk Assessment in support of Commission Directive 93/67/EEC on risk assessment for new notified substances. 2003.

Vryzas Z, Alexoudis C, Papadopouloumourkidou E, et al. Determination and aquatic risk assessment of pesticide residues in riparian drainage canals in northeastern Greece. Ecotoxicol. Environ. Saf. 2011;74(2):174–181. doi: 10.1016/j.ecoenv.2010.04.011. PubMed DOI

Backhaus T, Scholze M, Grimme LH. The single substance and mixture toxicity of quinolones to the bioluminescent bacterium Vibrio fischeri. Aquat. Toxicol. 2000;49(1):49–61. doi: 10.1016/S0166-445X(99)00069-7. PubMed DOI

Ma Y, Li M, Wu M, et al. Occurrences and regional distributions of 20 antibiotics in water bodies during groundwater recharge. Sci. Total Environ. 2015;518–519:498–506. doi: 10.1016/j.scitotenv.2015.02.100. PubMed DOI

Zhang PW, Zhou HD, Zhao GF, et al. Spatial, temporal distribution characteristics and potential risk of PPCPs in surface sediments from Taihu Lake. Environ. Sci. 2016;37(9):3348–3355. PubMed

Piao HS, Tao S, Hu HY, et al. Estimation of sorption coefficients of organic compounds with KOW. Environ. Sci. Technol. 1999;4:8–13.

Guérit I, Bocquené G, James A, et al. Environmental risk assessment: a critical approach of the European TGD in an insitu application. Ecotoxicol. Environ. Saf. 2008;71(1):291–300. doi: 10.1016/j.ecoenv.2008.01.020. PubMed DOI

Ren KJ, Liu Y, Xu JR, et al. Residues characteristics of fluoroquinolones (FQs) in the river sediments and fish tissues in a drinking water protection area of Guangdong Province. Acta Sci. Circum. 2016;36(3):760–766.

Wang L, Chen Q, Zhang J, et al. Incorporating fish habitat requirements of the complete life cycle into ecological flow regime estimation of rivers. Ecohydrology. 2020;13(4):e2204. doi: 10.1002/eco.2204. DOI

Brown KD, Kulis J, Thomson B, et al. Occurrence of antibiotics in hospital, residential, and dairy effluent, municipal wastewater, and the Rio Grande in New Mexico. Sci. Total Environ. 2006;366(2):772–783. doi: 10.1016/j.scitotenv.2005.10.007. PubMed DOI

Chang X, Meyer MT, Liu X, et al. Determination of antibiotics in sewage from hospitals, nursery and slaughter house, wastewater treatment plant and source water in Chongqing region of Three Gorge Reservoir in China. Environ. Pollut. 2010;158(5):1444–1450. doi: 10.1016/j.envpol.2009.12.034. PubMed DOI

Hirsch R, Ternes T, Haberer K, et al. Occurrence of antibiotics in the aquatic environment. Sci. Total Environ. 1999;225(1/2):109–111. doi: 10.1016/S0048-9697(98)00337-4. PubMed DOI

Guo X, Wang N, Xu J, et al. Research progress on environmental exposure levels and environmental fate of veterinary antibiotics. Environ. Sci. Technol. 2014;37(09):76–86.

Jiang L, Hu XL, Yin DQ, et al. Occurrence, distribution and seasonal variation of antibiotics in the Huangpu River, Shanghai. China. Chemosphere. 2011;82(6):822–828. doi: 10.1016/j.chemosphere.2010.11.028. PubMed DOI

Li J, Zhang R, Wang R, et al. Distribution characteristics and ecological risk assessment of antibiotic pollution in Xiaoqing River watershed. J. Agro-Environ. Sci. 2016;35(7):1384–1391.

Wu X, Zou H, Zhu R, et al. Occurrence, distribution and ecological risk of aantibiotics in surface water of the Gonghu Bay, Taihu Lake. Environ. Sci. 2016;37(12):4596–4604. PubMed

Zhu T, Song Z, Duan B, et al. Research on pollution and health risk by antibiotics in source water of Shiyan Reservoir in Shenzhen. J. Environ. Health. 2013;30(11):1003–1006.

Gao L, Li X, Zhang Y, et al. Research on pollution characteristics of antibiotics in Qinghe River in Beijing. Ecol. Sci. 2014;33(1):83–92.

Nowara A, Burhenne J, Spiteller M. Binding of fluoroquinolone carboxylic acid derivatives to clay minerals. J. Agric. Food Chem. 1997;45(4):1459–1463. doi: 10.1021/jf960215l. DOI

Li BY. Study on Adsorption and Biodegradation of Norfloxacin in Soil. Zhengzhou: Zhengzhou University; 2010.

Liu C, Li Y. Research Progress of Adsorption and Degradation of Ciprofloxacin in Soil. Beijing Agriculture. 2016, (4) (in Chinese).

Wang LP, Zhang MK, Zheng SA. Adsorption–desorption characteristics and biological effects of enrofloxacin in agricultural soils. Chin. J. Soil Sci. 2008;39(2):393–397.

Jing LD, Wang Y, Ma Z, et al. Study on degradation kinetics of Ofloxacin at sediment–water interface. J. Southwest Univ. Nation. (Natural Science Edition). 2016;42(4):409–413.

Dai JF, Yang Y, Fang RJ, et al. Water quality analysis and segmentation of the pollution loads in different spatial scales of the upstream of Lijiang River. China Rural Water Hydropower. 2017;4:67–71.

Huang J, Xue YL, Xu H, et al. Residual levels of fluoroquinolones in freshwater fish from aquatic products markets in Guiyang. J. Environ. Health. 2017;34(2):139–141.

Sun YC. Analysis and Distribution Characteristics of FQs in Environmental Water and Aquatic Product and its Effect on Environmental Stress. Harbin Institute of Technology: Harbin; 2014.

Zhang LY. Optimization of Quinolone Antibiotics Detection Method and in Water Photolysis and Hydrolysis Characteristics Research. Jilin: Jilin Agricultural University; 2016.

Carrasquillo AJ, Bruland GL, Mackay AA, et al. Sorption of ciprofloxacin and oxytetracycline zwitterions to soils and soil minerals: influence of compound structure. Environ. Sci. Technol. 2008;42(20):7634–7642. doi: 10.1021/es801277y. PubMed DOI

Zou S, Xu W, Zhang R, et al. Occurrence and distribution of antibiotics in coastal water of the Bohai Bay, China: impacts of river discharge and aquaculture activities. Environ. Pollut. 2011;159(10):2913–2920. doi: 10.1016/j.envpol.2011.04.037. PubMed DOI

Fu H, Li X, Wang J, et al. Impacts of p H on adsorption of quinolones by PAC. China Water Wastewater. 2017;33(17):64–67.

Huang S, Zang C, Du S, et al. Study on the relationships among pH, dissolved oxygen and chlorophyll a I: aquaculture water. Chin. J. Environ. Eng. 2011;5(6):1201–1208.

Chen S, Wu Z, Yu W, et al. Formation, harmfulness, prevention, control and treatment of waters eutrophication. Environ. Sci. Technol. 1999;22(2):11–15.

Pang HL. Studies on the Sorption Behavior of two Fluoroquinolones on Marine Sediments. Qingdao: Ocean University of China; 2012.

Qin Y, Zhang L, Shi Y, et al. Pollution characteristics and ecological risk assessment of typical antibiotics in the surface water of Hunhe River. Res. Environ. Sci. 2015;28(3):361–368.

Syberg K, Jensen TS, Cedergreen N, et al. On the use of mixture toxicity assessment in REACH and the water framework directive: a review. Hum. Ecol. Risk Assess. 2009;15(6):1257–1272. doi: 10.1080/10807030903304922. DOI

Liu K, Zhang DL, Liu N, et al. Investigation on the typical quinolone antibiotics in the surface sediments of Jiaozhou bay China. Mar. Environ. Sci. 2017;36(05):655–661.

Zhang J, Cheng Y, Feng L, et al. Health risk assessment of antibiotics in the centralized drinking water source in the three gorges reservoir area. Environ. Sci. Technol. 2018;41(8):192–198.

No. 235 Announcement of the Ministry of Agriculture Maximum residue limits of veterinary drugs in animal foods. China Swine Industry. 2002;2010(8):10–12.

National Health and Family Planning Commission of PRC Outline of China's food and nutrition development (2014–2020) Chron. Pathematol. J. 2014;36(2):111–113.

Zhang QP, Li J, Wang CM. Residual level and safety assessment of quinolone antibiotics in aquatic products in Suzhou. Chin. J. Health Lab. Technol. 2012;22(10):2417–2418.

Wu XL. Pollution Characteristics and Health Risk of Quinolones in Vegetables in the Pearl River Delta Region. Guangzhou: Jinan University; 2011.

Li, W., Shi, Y., Gao, L., Liu, J. & Cai, Y. Occurrence of antibiotics in water, sediments, aquatic plants, and animals from Baiyangdian Lake in North China. Chemosphere89(11), 1307–1315 (2012). PubMed

Minh TB, Leung HW, Loi IH, et al. Antibiotics in the Hong Kong metropolitan area: Ubiquitous distribution and fate in Victoria Harbour. Mar. Pollut. Bull. 2009;58:1052–1062. doi: 10.1016/j.marpolbul.2009.02.004. PubMed DOI

Riva, F., Zuccato, E., Davoli, E., Fattore, E. & Castiglioni, S. Risk assessment of a mixture of emerging contaminants in surface water in a highly urbanized area in Italy. J. Hazard. Mater.361, 103–110 (2019). PubMed

Watkinson, A. J., Murby, E. J., Kolpin, D. W. & Costanzo, S. D. The occurrence of antibiotics in an urban watershed: From wastewater to drinking water. Sci. Total Environ.407(8), 2711–2723 (2009). PubMed

Batt AL, Bruce IB, Aga DS. Evaluating the vulnerability of surface waters to antibiotic contamination from varying wastewater treatment plant discharges. Environ. Pollut. 2006;142:295–302. doi: 10.1016/j.envpol.2005.10.010. PubMed DOI

Golet, E. M., Strehler, A., Alder, A. C. & Giger, W. Determination of fluoroquinolone antibacterial agents in sewage sludge and sludge-treated soil using accelerated solvent extraction followed by solid-phase extraction. Anal. Chem.74(21), 5455–5462 (2002). PubMed

Gibs J, Heckathorn HA, Meyer MT, et al. Occurrence and partitioning of antibiotic compounds found in the water column and bottom sediments from a stream receiving two wastewater treatment plant effluents in Northern New Jersey, 2008. Sci. Total Environ. 2013;458–460:107–116. doi: 10.1016/j.scitotenv.2013.03.076. PubMed DOI

Wang GQ, Sun T. Antibiotic residues in aquatic products of Hongze lake investigation and research. Guangdong Chem. 2011;38(1):151–153.

Yang YT, Luan LJ. Residues and health risk assessment of Quinolones in fishes from the markets in Jining City. J. Anhui Agric. Sci. 2015;43(26):141–143.