Occurrence and fate of typical antibiotics in wastewater treatment plants in Harbin, North-east China

Highlights

• The concentration distributions and removals of 12 antibiotics were investigated.

• Macrolides and fluoroquinolones presented relatively higher concentrations.

• The removal of antibiotics did not differ among the different treatment processes.

Abstract

As a new pollutant, antibiotics in the environment and their removal in wastewater treatment plants (WWTPs) have gained considerable attention. However, few studies investigated antibiotics in the north-eastern areas of China. By employing high-performance liquid chromatography-tandem mass spectrometry, the concentration distribution and removal of 12 antibiotics belonging to four types (cephalosporins, sulfonamides, fluoroquinolones, and macrolides) were investigated in influents and effluents as well as the removal efficiencies of four typical treatment processes in 18 wastewater treatment plants of Harbin City, north-eastern China. Macrolides and fluoroquinolones presented relatively higher detection concentrations and rates both in the water and in the sludge phases. Sulfonamides and cephalosporins displayed higher detection concentrations in the water phase. The representative antibiotics in influents and effluents included ROX, NOR, OFL, SMX, AZI, and CLA, with detection rates above 95%. The detection rates of the other six antibiotics exceeded 30%. In the sludge, the other five antibiotics, except SMX, presented relatively higher detection concentrations and rates, with detection rates greater than 95%. For cephalosporin, the detection rates of CTX and CFM in the sludge were 0. The removal efficiencies for the 12 antibiotics differed greatly, with average values ranging from 30% to 80% and the highest values for cephalosporin. The removal of antibiotics did not differ significantly among the four different treatment processes.

Graphical abstract

Keywords

Antibiotics / WWTPs / Occurrence / Removal efficiency

References

[1] Arimori K, Miyamoto S, Fukuda K, Nakamura C, Nakano M (1998). Characteristic difference in gastrointestinal excretion of clarithromycin and roxithromycin. Biopharmaceutics & Drug Disposition, 19(7): 433–438

[2] Ashfaq M, Li Y, Wang Y W, Chen W J, Wang H, Chen X Q, Wu W, Huang Z Y, Yu C P, Sun Q (2017). Occurrence, fate, and mass balance of different classes of pharmaceuticals and personal care products in an anaerobic-anoxic-oxic wastewater treatment plant in Xiamen, China. Water Research, 123: 655–667

[3] Bing L, Tong Z (2010). Biodegradation and adsorption of antibiotics in the activated sludge process. Environmental Science & Technology, 44: 3468–3473

[4] Blair B, Nikolaus A, Hedman C, Klaper R, Grundl T (2015). Evaluating the degradation, sorption, and negative mass balances of pharmaceuticals and personal care products during wastewater treatment. Chemosphere, 134: 395–401

[5] Cha J M, Yang S, Carlson K H (2006). Trace determination of beta-lactam antibiotics in surface water and urban wastewater using liquid chromatography combined with electrospray tandem mass spectrometry. Journal of Chromatography. A, 1115(1–2): 46–57

[6] Clara M, Strenn B, Gans O, Martinez E, Kreuzinger N, Kroiss H (2005). Removal of selected pharmaceuticals, fragrances and endocrine disrupting compounds in a membrane bioreactor and conventional wastewater treatment plants. Water Research, 39(19): 4797–4807

[7] Du J, Fan Y, Qian X (2015). Occurrence and behavior of pharmaceuticals in sewage treatment plants in eastern China. Frontiers of Environmental Science & Engineering, 9(4): 725–730

[8] Feitosa-Felizzola J, Temime B, Chiron S (2007). Evaluating on-line solid-phase extraction coupled to liquid chromatography–ion trap mass spectrometry for reliable quantification and confirmation of several classes of antibiotics in urban wastewaters. Journal of Chromatography. A, 1164(1–2): 95–104

[9] Franklin A M, Williams C F, Andrews D M, Woodward E E, Watson J E (2016). Uptake of three antibiotics and an antiepileptic drug by wheat crops spray irrigated with wastewater treatment plant effluent. Journal of Environmental Quality, 45(2): 546–554

[10] Gao L H, Shi Y L, Li W H, Niu H Y, Liu J M, Cai Y Q (2012). Occurrence of antibiotics in eight sewage treatment plants in Beijing, China. Chemosphere, 86(6): 665–671

[11] Göbel A, Thomsen A, Mcardell C S, Joss A, Giger W (2005). Occurrence and sorption behavior of sulfonamides, macrolides, and trimethoprim in activated sludge treatment. Environmental Science & Technology, 39(11): 3981–3989

[12] Goebel A, McArdell C S, Joss A, Siegrist H, Giger W (2007). Fate of sulfonamides, macrolides, and trimethoprim in different wastewater treatment technologies. Science of the Total Environment, 372(2–3): 361–371

[13] Golet E M, Alder A C, Giger W (2002). Environmental exposure and risk assessment of fluoroquinolone antibacterial agents in wastewater and river water of the Glatt Valley Watershed, Switzerland. Environmental Science & Technology, 36(17): 3645–3651

[14] Guo X Y, Wang N, Jing X U, Jiao S J, Wang Z C, Shan Z J, Tang W G (2014). Research progress on environmental exposure levels and environmental fate of veterinary antibiotics. Environmental Science & Technology, 37(9): 76–86

[15] Huang H, Wu J, Ye J, Ye T J, Deng J, Liang Y M, Liu W (2018). Occurrence, removal, and environmental risks of pharmaceuticals in wastewater treatment plants in south China. Frontiers of Environmental Science & Engineering, 12(6): 7

[16] Igbinosa I H, Okoh A I (2012). Antibiotic susceptibility profile of Aeromonas species isolated from wastewater treatment plant. TheScientificWorldJournal, 2012: 1–6

[17] Jiang M, Wang L, Ji R (2010). Biotic and abiotic degradation of four cephalosporin antibiotics in a lake surface water and sediment. Chemosphere, 80(11): 1399–1405

[18] Li B, Zhang T (2011). Mass flows and removal of antibiotics in two municipal wastewater treatment plants. Chemosphere, 83(9): 1284–1289

[19] Li B, Zhang T, Xu Z, Fang H H (2009). Rapid analysis of 21 antibiotics of multiple classes in municipal wastewater using ultra performance liquid chromatography-tandem mass spectrometry. Analytica Chimica Acta, 645(1–2): 64–72

[20] Li X W, Shi H C, Li K X, Zhang L, Gan Y P (2014). Occurrence and fate of antibiotics in advanced wastewater treatment facilities and receiving rivers in Beijing, China. Frontiers of Environmental Science & Engineering, 8(6): 888–894

[21] Lin A Y C, Yu T H, Lateef S K (2009). Removal of pharmaceuticals in secondary wastewater treatment processes in Taiwan. Journal of Hazardous Materials, 167(1–3): 1163–1169

[22] Liu H Q, Lam J C W, Li W W, Yu H Q, Lam P K S (2017a). Spatial distribution and removal performance of pharmaceuticals in municipal wastewater treatment plants in China. Science of the Total Environment, 586: 1162–1169

[23] Liu J, Lu J J, Tong Y B, Li C (2017b). Occurrence and elimination of antibiotics in three sewage treatment plants with different treatment technologies in Urumqi and Shihezi, Xinjiang. Water Science and Technology, 75(6): 1474–1484

[24] Minh T B, Leung H W, Loi I H, Chan W H, So M K, Mao J Q, Choi D, Lam J C, Zheng G, Martin M (2009). Antibiotics in the Hong Kong metropolitan area: Ubiquitous distribution and fate in Victoria Harbour. Marine Pollution Bulletin, 58(7): 1052–1062

[25] Müller E, Schüssler W, Horn H, Lemmer H (2013). Aerobic biodegradation of the sulfonamide antibiotic sulfamethoxazole by activated sludge applied as co-substrate and sole carbon and nitrogen source. Chemosphere, 92(8): 969–978

[26] Piotrowska M, Przygodzinska D, Matyjewicz K, Popowska M (2017). Occurrence and variety of beta-lactamase genes among Aeromonas spp. Isolated from urban wastewater treatment plant. Frontiers in Microbiology, 8: 863–874

[27] Roberts P H, Thomas K V (2006). The occurrence of selected pharmaceuticals in wastewater effluent and surface waters of the lower Tyne catchment. Science of the Total Environment, 356(1): 143–153

[28] Rodayan A, Majewsky M, Yargeau V (2014). Impact of approach used to determine removal levels of drugs of abuse during wastewater treatment. Science of the Total Environment, 487(1): 731–739

[29] Salgado R, Marques R, Noronha J P, Carvalho G, Oehmen A, Reis M A (2012). Assessing the removal of pharmaceuticals and personal care products in a full-scale activated sludge plant. Environmental Science and Pollution Research International, 19(5): 1818–1827

[30] Sarmah A K, Meyer M T, Boxall A B (2006). A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics (VAs) in the environment. Chemosphere, 65(5): 725–759

[31] Timraz K, Xiong Y, Al Qarni H, Hong P Y (2017). Removal of bacterial cells, antibiotic resistance genes and integrase genes by on-site hospital wastewater treatment plants: Surveillance of treated hospital effluent quality. Environmental Science. Water Research & Technology, 3(2): 293–303

[32] Wang L, Qiang Z M, Li Y G, Ben W W (2017a). An insight into the removal of fluoroquinolones in activated sludge process: Sorption and biodegradation characteristics. Journal of Environmental Sciences (China), 56: 263–271

[33] Wang W H, Wang H, Zhang W F, Liang H, Gao D W (2017b). Occurrence, distribution, and risk assessment of antibiotics in the Songhua River in China. Environmental Science and Pollution Research International, 24(23): 19282–19292

[34] Wang W H, Zhang W F, Liang H, Gao D W (2018). Seasonal distribution characteristics and health risk assessment of typical antibiotics in the Harbin section of the Songhua River basin. Environmental Technology, , doi: 10.1080/09593330.2018.1449902

[35] Watkinson A J, Murby E J, Kolpin D W, Costanzo S D (2009). The occurrence of antibiotics in an urban watershed: From wastewater to drinking water. Science of the Total Environment, 407(8): 2711–2723

[36] Xu R, Yang Z H, Wang Q P, Bai Y, Liu J B, Zheng Y, Zhang Y R, Xiong W P, Ahmad K, Fan C Z (2018). Rapid startup of thermophilic anaerobic digester to remove tetracycline and sulfonamides resistance genes from sewage sludge. Science of the Total Environment, 612: 788–798

[37] Xu W H, Zhang G, Li X D, Zou S C, Li P, Hu Z H, Li J (2007). Occurrence and elimination of antibiotics at four sewage treatment plants in the Pearl River Delta (PRD), South China. Water Research, 41(19): 4526–4534

[38] Yang S F, Lin C F, Wu C J, Ng K K, Lin A Y C, Hong P K A (2012). Fate of sulfonamide antibiotics in contact with activated sludge—Sorption and biodegradation. Water Research, 46(4): 1301–1308

[39] Yu X, Tang X Y, Zuo J E, Zhang M Y, Chen L, Li Z X (2016). Distribution and persistence of cephalosporins in cephalosporin producing wastewater using SPE and UPLC-MS/MS method. Science of the Total Environment, 569: 23–30

[40] Zhang C H, Wang L L, Gao X Y, He X D (2016). Antibiotics in WWTP discharge into the Chaobai River, Beijing. Archives of Environmental Protection, 42(4): 48–57

[41] Zhang X, Zhao H X, Du J, Qu Y X, Shen C, Tan F, Chen J W, Quan X (2017). Occurrence, removal, and risk assessment of antibiotics in 12 wastewater treatment plants from Dalian, China. Environmental Science and Pollution Research International, 24(19): 16478–16487

[42] Zheng J, Su C, Zhou J W, Xu L K, Qian Y Y, Chen H (2017). Effects and mechanisms of ultraviolet, chlorination, and ozone disinfection on antibiotic resistance genes in secondary effluents of municipal wastewater treatment plants. Chemical Engineering Journal, 317: 309–316

[43] Zhong Z X, Xu J, Zhang Y, Guo C S, Zhang W H (2013). Adsorption of sulfonamides on lake sediments. Frontiers of Environmental Science & Engineering, 7(4): 518–525

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 31870471) and Heilongjiang Natural Science Foundation (No. C2017003).

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