Skip to main content
SpringerLink
Log in

Occurrence, removal, and risk assessment of antibiotics in 12 wastewater treatment plants from Dalian, China

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

In this study, the occurrence and removal efficiencies of 31 antibiotics, including 11 sulfonamides (SAs), five fluoroquinolones (FQs), four macrolides (MLs), four tetracyclines (TCs), three chloramphenicols (CAPs), and four other antibiotics (Others), were investigated in 12 municipal wastewater treatment plants (WWTPs) in Dalian, China. A total of 29 antibiotics were detected in wastewater samples with the concentration ranging from 63.6 to 5404.6 ng/L. FQs and SAs were the most abundant antibiotic classes in most wastewater samples, accounting for 42.2 and 23.9% of total antibiotic concentrations, respectively, followed by TCs (16.0%) and MLs (14.8%). Sulfamethoxazole, erythromycin, clarithromycin, azithromycin, ofloxacin, and norfloxacin were the most frequently detected antibiotics; of these, the concentration of ofloxacin was the highest in most of influent (average concentration = 609.8 ng/L) and effluent (average concentration = 253.4 ng/L) samples. The removal efficiencies varied among WWTPs in the range of −189.9% (clarithromycin) to 100% (enoxacin, doxycycline, etc), and more than 50% of antibiotics could not be efficiently removed with the removal efficiency less than 65%. An environmental risk assessment was also performed in the WWTP effluents by calculating the risk quotient (RQ), and high RQ values (>1) indicated erythromycin and clarithromycin might cause the ecological risk on organisms in surrounding water near discharge point of WWTPs in this area, which warrants further attention.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3

Similar content being viewed by others

References

  • Alcock RE, Sweetman A, Jones KC (1999) Assessment of organic contaminant fate in waste water treatment plants I: selected compounds and physicochemical properties. Chemosphere 38:2247–2262

    Article  CAS  Google Scholar 

  • Andreozzi R, Marotta R, Paxeus N (2003) Pharmaceuticals in STP effluents and their solar photodegradation in aquatic environment. Chemosphere 50:1319–1330

    Article  CAS  Google Scholar 

  • Batt AL, Bruce IB, Aga DS (2006) Evaluating the vulnerability of surface waters to antibiotic contamination from varying wastewater treatment plant discharges. Environ Pollut 142:295–302

    Article  CAS  Google Scholar 

  • Blackwell PA, Kay P, Ashauer R, Boxall ABA (2009) Effects of agricultural conditions on the leaching behaviour of veterinary antibiotics in soils. Chemosphere 75:13–19

    Article  CAS  Google Scholar 

  • Castiglioni S, Bagnati R, Fanelli R, Pomati F, Calamari D, Zuccato E (2006) Removal of pharmaceuticals in sewage treatment plants in Italy. Environ Sci Technol 40:357–363

    Article  CAS  Google Scholar 

  • Clara M, Kreuzinger N, Strenn B, Gans O, Kroiss H (2005a) The solids retention time—a suitable design parameter to evaluate the capacity of wastewater treatment plants to remove micropollutants. Water Res 39:97–106

    Article  CAS  Google Scholar 

  • Clara M, Strenn B, Gans O, Martinez E, Kreuzinger N, Kroiss H (2005b) Removal of selected pharmaceuticals, fragrances and endocrine disrupting compounds in a membrane bioreactor and conventional wastewater treatment plants. Water Res 39:4797–4807

    Article  CAS  Google Scholar 

  • Du J, Zhao HX, Chen JW (2015) Simultaneous determination of 23 antibiotics in mariculture water using solid-phase extraction and high performance liquid chromatography-tandem mass spectrometry. Chinese J Chromatogr 33:348–353 (in Chinese)

    Article  CAS  Google Scholar 

  • Gao L, Shi Y, Li W, Niu H, Liu J, Cai Y (2012) Occurrence of antibiotics in eight sewage treatment plants in Beijing, China. Chemosphere 86:665–671

    Article  CAS  Google Scholar 

  • Garcia-Galan M J, Gonzalez Blanco S, Lopez Roldan R, Diaz-Cruz S, Barcelo D (2012) Ecotoxicity evaluation and removal of sulfonamides and their acetylated metabolites during conventional wastewater treatment. Sci Total Environ 437:403–412

  • Göbel A, Thomsen A, McArdell CS, Joss A, Giger W (2005) Occurrence and sorption behavior of sulfonamides, macrolides, and trimethoprim in activated sludge treatment. Environ Sci Technol 39(11):3981–3989

    Article  Google Scholar 

  • Göbel A, McArdell CS, Joss A, Siegrist H, Giger W (2007) Fate of sulfonamides, macrolides, and trimethoprim in different wastewater treatment technologies. Sci Total Environ 372:361–371

    Article  Google Scholar 

  • Golet EM, Alder AC, Giger W (2002) Environmental exposure and risk assessment of fluoroquinolone antibacterial agents in wastewater and river water of the Glatt Valley Watershed, Switzerland. Environ Sci Technol 36:3645–3651

    Article  CAS  Google Scholar 

  • Golet EM, Xifra I, Siegrist H, Alder AC, Giger W (2003) Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil. Environ Sci Technol 37(15):3243–3249

    Article  CAS  Google Scholar 

  • Gulkowska A, Leung HW, So MK, Taniyasu S, Yamashita N, Yeunq LWY, Richardson BJ, Lei AP, Giesy JP, Lam PKS (2008) Removal of antibiotics from wastewater by sewage treatment facilities in Hong Kong and Shenzhen, China. Water Res 42:395–403

    Article  CAS  Google Scholar 

  • Gust M, Fortier M, Garric J, Fournier M, Gagné F (2013) Effects of short-term exposure to environmentally relevant concentrations of different pharmaceutical mixtures on the immune response of the pond snail Lymnaea stagnalis. Sci Total Environ 445-446:210–218

    Article  CAS  Google Scholar 

  • Halling-Sorensen B, Lutzhoft H, Andersen HR, Ingerslev F (2000) Environmental risk assessment of antibiotics: comparison of mecillinam, trimethoprim and ciprofloxacin. J Antimicrob Chemoth 461:53–58

    Article  Google Scholar 

  • He X, Deng M, Wang Q, Yang Y, Yang Y, Nie X (2016) Residues and health risk assessment of quinolones and sulfonamides in cultured fish from Pearl River Delta, China. Aquaculture 458:38–46

    Article  CAS  Google Scholar 

  • Huerta C, Rodriguez L (2002) Risk of clinical blood dyscrasia in a cohort of antibiotic users. Pharmacotherapy 22:630–636

    Article  Google Scholar 

  • Iatrou EI, Stasinakis AS, Thomaidis NS (2014) Consumption-based approach for predicting environmental risk in Greece due to the presence of antimicrobials in domestic wastewater. Environ Sci Pollut R 21:12941–12950

    Article  CAS  Google Scholar 

  • Isidori M, Lavorgna M, Nardelli A, Pascarella L, Parrella A (2005) Toxic and genotoxic evaluation of six antibiotics on non-target organisms. Sci Total Environ 346:87–98

    Article  CAS  Google Scholar 

  • Johnson AC, Keller V, Dumont E, Sumpter JP (2015) Assessing the concentrations and risks of toxicity from the antibiotics ciprofloxacin, sulfamethoxazole, trimethoprim and erythromycin in European rivers. Sci Total Environ 511:747–755

    Article  CAS  Google Scholar 

  • Karthikeyan KG, Meyer MT (2006) Occurrence of antibiotics in wastewater treatment facilities in Wisconsin, USA. Sci Total Environ 361:196–207

    Article  CAS  Google Scholar 

  • Kasprzyk-Hordern B, Dinsdale RM, Guwy AJ (2009) The removal of pharmaceuticals, personal care products, endocrine disruptors and illicit drugs during wastewater treatment and its impact on the quality of receiving waters. Water Res 43:363–380

    Article  CAS  Google Scholar 

  • Kim S, Eichhorn P, Jensen JN, Weber AS, Aga DS (2005) Removal of antibiotics in wastewater: effect of hydraulic and solid retention times on the fate of tetracycline in the activated sludge process. Environ Sci Technol 39:5816–5823

    Article  CAS  Google Scholar 

  • Kimosop SJ, Getenga ZM, Orata F, Okello VA, Cheruiyot JK (2016) Residue levels and discharge loads of antibiotics in wastewater treatment plants (WWTPs), hospital lagoons, and rivers within Lake Victoria Basin, Kenya. Environ Monit Assess 188(9):532. doi:10.1007/s10661-016-5534-6

    Article  Google Scholar 

  • Lane SE, Watts RA, Scott D (2005) European Medicines Agency (EMEA) consensus on the classification of the primary systemic vasculitides (PSV) for epidemiological studies. Rheumatology 441:I22–I22

    Google Scholar 

  • Leung HW, Jin L, Wei S, Tsui MMP, Zhou B, Jiao L, Cheung PC, Chun YK, Murphy MB, Lam PKS (2013) Pharmaceuticals in tap water: human health risk assessment and proposed monitoring framework in China. Environ Health Persp 121:839–846

    Article  Google Scholar 

  • Li W, Shi Y, Gao L, Liu J, Cai Y (2012) Occurrence of antibiotics in water, sediments, aquatic plants, and animals from Baiyangdian Lake in North China. Chemosphere 89:1307–1315

    Article  CAS  Google Scholar 

  • Li W, Shi Y, Gao L, Liu J, Cai Y (2013) Occurrence and removal of antibiotics in a municipal wastewater reclamation plant in Beijing, China. Chemosphere 92:435–444

    Article  CAS  Google Scholar 

  • Li W, Gao L, Shi Y, Liu J, Cai Y (2015a) Occurrence, distribution and risks of antibiotics in urban surface water in Beijing, China. Environ Sci Process Impacts 17(9):1611–1619

  • Li H, Lu X, Li C, Chen J (2015b) Molecular characterization of the liver-expressed antimicrobial peptide 2 (LEAP-2) in a teleost fish, Plecoglossus altivelis: antimicrobial activity and molecular mechanism. Mol Immunol 65:406–415

    Article  CAS  Google Scholar 

  • Lin AY, Yu T, Lin C (2008) Pharmaceutical contamination in residential, industrial, and agricultural waste streams: risk to aqueous environments in Taiwan. Chemosphere 74:131–141

    Article  CAS  Google Scholar 

  • Lin AY, Yu T, Lateef SK (2009) Removal of pharmaceuticals in secondary wastewater treatment processes in Taiwan. J Hazard Mater 167:1163–1169

    Article  CAS  Google Scholar 

  • Lindberg RH, Olofsson U, Rendahl P, Johansson MI, Tysklind M, Andersson B (2006) Behavior of fluoroquinolones and trimethoprim during mechanical, chemical, and active sludge treatment of sewage water and digestion of sludge. Environ Sci Technol 40:1042–1048

    Article  CAS  Google Scholar 

  • Liu JL, Wong MH (2013) Pharmaceuticals and personal care products (PPCPs): a review on environmental contamination in China. Environ Int 59:208–224

    Article  CAS  Google Scholar 

  • Lopez-Serna R, Jurado A, Vazquez-Sune E, Carrera J, Petrovic M, Barcelo D (2013) Occurrence of 95 pharmaceuticals and transformation products in urban groundwaters underlying the metropolis of Barcelona, Spain. Environ Pollut 174:305–315

    Article  CAS  Google Scholar 

  • Miao XS, Bishay F, Chen M, Metcalfe CD (2004) Occurrence of antimicrobials in the final effluents of wastewater treatment plants in Canada. Environ Sci Technol 38:3533–3541

    Article  CAS  Google Scholar 

  • Minh TB, Leung HW, Loi IH, Chan WH, So MK, Mao JQ, Choi D, Lam JCW, Zheng G, Martin M, Lee JHW, Lam PKS, Richardson BJ (2009) Antibiotics in the Hong Kong metropolitan area: ubiquitous distribution and fate in Victoria Harbour. Mar Pollut Bull 58:1052–1062

    Article  CAS  Google Scholar 

  • Michael I, Rizzo L, McArdell CS, Manaia CM, Merlin C, Schwartz T, Dagot C, Fatta-Kassinos D (2013) Urban wastewater treatment plants as hotspots for the release of antibiotics in the environment: a review. Water Res 47(3):957–995

    Article  CAS  Google Scholar 

  • Mohapatra S, Huang C, Mukherji S, Padhye LP (2016) Occurrence and fate of pharmaceuticals in WWTPs in India and comparison with a similar study in the United States. Chemosphere 159:526–535

    Article  CAS  Google Scholar 

  • Pei R, Kim S, Carlson KH, Pruden A (2006) Effect of river landscape on the sediment concentrations of antibiotics and corresponding antibiotic resistance genes (ARG). Water Res 40:2427–2435

    Article  CAS  Google Scholar 

  • Roberts PH, Thomas KV (2006) The occurrence of selected pharmaceuticals in wastewater effluent and surface waters of the lower Tyne catchment. Sci Total Environ 356:143–153

    Article  CAS  Google Scholar 

  • Santos JL, Aparicio I, Alonso E (2007) Occurrence and risk assessment of pharmaceutically active compounds in wastewater treatment plants. A case study: Seville city (Spain). Environ Int 33:596–601

    Article  CAS  Google Scholar 

  • Sarmah AK, Meyer MT, Boxall ABA (2006) A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics (VAs) in the environment. Chemosphere 65:725–759

    Article  CAS  Google Scholar 

  • Senta I, Terzic S, Ahel M (2008) Simultaneous determination of sulfonamides, fluoroquinolones, macrolides and trimethoprim in wastewater and river water by LC-tandem-MS. Chromatographia 68:747–758

    Article  CAS  Google Scholar 

  • Stolze Y, Eikmeyer F, Wibberg D, Brandis G, Karsten C, Krahn I, Schneiker-Bekel S, Viehoever P, Barsch A, Keck M, Top EM, Niehaus K, Schlueter A (2012) IncP-1 beta plasmids of Comamonas sp and Delftia sp strains isolated from a wastewater treatment plant mediate resistance to and decolorization of the triphenylmethane dye crystal violet. Microbiol-Sgm 158:2060–2072

    Article  CAS  Google Scholar 

  • Topp E, Renaud J, Sumarah M, Sabourin L (2016) Reduced persistence of the macrolide antibiotics erythromycin, clarithromycin and azithromycin in agricultural soil following several years of exposure in the field. Sci Total Environ 562:136–144

    Article  CAS  Google Scholar 

  • Van Doorslaer X, Dewulf J, Van Langenhove H, Demeestere K (2014) Fluoroquinolone antibiotics: an emerging class of environmental micropollutants. Sci Total Environ 500:250–269

    Article  Google Scholar 

  • Verlicchi P, Al Aukidy M, Galletti A, Petrovic M, Barcelo D (2012) Hospital effluent: investigation of the concentrations and distribution of pharmaceuticals and environmental risk assessment. Sci Total Environ 430:109–118

    Article  CAS  Google Scholar 

  • Vieno N, Tuhkanen T, Kronberg L (2007) Elimination of pharmaceuticals in sewage treatment plants in Finland. Water Res 41:1001–1012

    Article  CAS  Google Scholar 

  • Watkinson AJ, Murby EJ, Costanzo SD (2007) Removal of antibiotics in conventional and advanced wastewater treatment: implications for environmental discharge and wastewater recycling. Water Res 41:4164–4176

    Article  CAS  Google Scholar 

  • Watkinson AJ, Murby EJ, Kolpin DW, Costanzo SD (2009) The occurrence of antibiotics in an urban watershed: from wastewater to drinking water. Sci Total Environ 407:2711–2723

    Article  CAS  Google Scholar 

  • Wang HL, Che BG, Duan AL, Mao JW, Dahlgren RA, Zhang MH, Zhang HQ, Zeng AB, Wang XD (2014) Toxicity evaluation of β-diketone antibiotics on the development of embryo-larval zebrafish (Danio rerio). Environ Toxicol 29(10):1134–1146

    Article  CAS  Google Scholar 

  • Wang H, Wang B, Zhao Q, Zhao Y, Fu C, Feng X, Wang N, Su M, Tang C, Jiang F, Zhou Y, Chen Y, Jiang Q (2015) Antibiotic body burden of Chinese school children: a multisite biomonitoring-based study. Environ Sci Technol 49(8):5070–5079

    Article  CAS  Google Scholar 

  • Xiao Y, Chang H, Jia A, Hu J (2008) Trace analysis of quinolone and fluoroquinolone antibiotics from wastewaters by liquid chromatography-electrospray tandem mass spectrometry. J Chromatogr A 1214:100–108

    Article  CAS  Google Scholar 

  • Xu W, Zhang G, Li X, Zou S, Li P, Hu Z, Li J (2007) Occurrence and elimination of antibiotics at four sewage treatment plants in the Pearl River Delta (PRD), South China. Water Res 41:4526–4534

    Article  CAS  Google Scholar 

  • Xue B, Zhang R, Wang Y, Liu X, Li J, Zhang G (2013) Antibiotic contamination in a typical developing city in south China: occurrence and ecological risks in the Yongjiang River impacted by tributary discharge and anthropogenic activities. Ecotox Environ Safe 92:229–236

    Article  CAS  Google Scholar 

  • Yuan X, Qiang Z, Ben W, Zhu B, Qu J (2015) Distribution, mass load and environmental impact of multiple-class pharmaceuticals in conventional and upgraded municipal wastewater treatment plants in East China. Environmental Science-Processes & Impacts 17(3):596–605

    Article  Google Scholar 

  • Zhang Q, Ying G, Pan C, Liu Y, Zhao J (2015) Comprehensive evaluation of antibiotics emission and fate in the river basins of China: source analysis, multimedia modeling, and linkage to bacterial resistance. Environ Sci Technol 49:6772–6782

    Article  CAS  Google Scholar 

  • Zhou L, Ying G, Liu S, Zhao J, Yang B, Chen Z, Lai H (2013) Occurrence and fate of eleven classes of antibiotics in two typical wastewater treatment plants in South China. Sci Total Environ 452:365–376

    Article  Google Scholar 

  • Zorita S, Martensson L, Mathiasson L (2009) Occurrence and removal of pharmaceuticals in a municipal sewage treatment system in the south of Sweden. Sci Total Environ 407:2760–2770

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This research was financially supported by the National Natural Science Foundation (21277017, 21677023) and the Fundamental Research Funds for the Central Universities (DUT15LK40). And we also gratefully acknowledge the support from the Open Project of State Key Laboratory of Urban Water Resource and Environment (Harbin Institute of Technology, QAK 201606).

Author information

Authors and Affiliations

  1. Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Linggong Road 2, Dalian, 116024, China

    Xin Zhang, Hongxia Zhao, Juan Du, Chen Shen, Feng Tan, Jingwen Chen & Xie Quan

  2. Dalian Haixin Detection Technology Co., Ltd, Dalian, 116020, China

    Yixuan Qu

Authors
  1. Xin Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Hongxia Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Juan Du
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Yixuan Qu
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Chen Shen
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Feng Tan
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Jingwen Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Xie Quan
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Hongxia Zhao.

Additional information

Responsible editor: Roland Kallenborn

Electronic supplementary material

ESM 1

(DOCX 141 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, X., Zhao, H., Du, J. et al. Occurrence, removal, and risk assessment of antibiotics in 12 wastewater treatment plants from Dalian, China. Environ Sci Pollut Res 24, 16478–16487 (2017). https://doi.org/10.1007/s11356-017-9296-7

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-017-9296-7

Keywords

Search

Navigation