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Frontiers of Environmental Science & Engineering

Front. Environ. Sci. Eng.    2019, Vol. 13 Issue (3) : 34     https://doi.org/10.1007/s11783-019-1118-3
RESEARCH ARTICLE
Occurrence and fate of typical antibiotics in wastewater treatment plants in Harbin, North-east China
Weihua Wang1, Wanfeng Zhang1, Hong Liang2(), Dawen Gao2()
1. Harbin Environmental Monitoring Center, Harbin 150076, China
2. State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology (HIT), Harbin 150090, China
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Abstract

• 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.

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.

Keywords Antibiotics      WWTPs      Occurrence      Removal efficiency     
This article is part of themed collection: Environmental Antibiotics and Antibiotic Resistance (Xin Yu, Hui Li & Virender K. Sharma)
Corresponding Authors: Hong Liang,Dawen Gao   
Just Accepted Date: 10 April 2019   Issue Date: 13 May 2019
 Cite this article:   
Weihua Wang,Wanfeng Zhang,Hong Liang, et al. Occurrence and fate of typical antibiotics in wastewater treatment plants in Harbin, North-east China[J]. Front. Environ. Sci. Eng., 2019, 13(3): 34.
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http://journal.hep.com.cn/fese/EN/10.1007/s11783-019-1118-3
http://journal.hep.com.cn/fese/EN/Y2019/V13/I3/34
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Weihua Wang
Wanfeng Zhang
Hong Liang
Dawen Gao
Fig.1  Location map of 18 wastewater treatment plants in Harbin, north-eastern China
Fig.2  Schematic diagrams of the four WWTPs with different treatment processes.
CTX CFM CFA SMPD SD SMX AZI CLA ROX NOR OFL FLU
Influent Maxa) 234 175 432 182 1692 809 110 321 2986 2168 2787 45.8
Minb) n.de) n.de) n.de) n.de) n.de) 2.1 n.de) n.de) 14.2 1.5 1.5 n.de)
Averc) 35.1 16.1 80.2 89 191 135 28.0 35.8 500 220 289 7.5
Fred) 78 34 84 89 78 100 95 95 100 100 100 78
Effluent Maxa) 45.5 61.2 99.3 127 708 506 61.2 164 1419 1018 1481 30.4
Minb) n.de) n.de) n.de) n.de) n.de) n.de n.de) n.de) 6 0.8 1.1 n.de
Averc) 6.1 4.8 16 13.6 90.6 87.1 14.1 20.5 332 100 135 3.9
Fred) 67 34 73 84 62 95 95 95 100 100 100 78
Sludge Maxa) n.de) n.de) 15.3 9.2 160 32.6 75.3 82.9 198 526 487 7.5
Minb) n.de) n.de) n.de) n.de) n.de) n.de) n.de) n.de) 3.4 1.1 1.5 n.de)
Averc) n.de) n.de0 0.85 0.51 32.9 3.9 11.6 11.5 66.5 70.9 61.9 2.1
Fred) 0 0 6 6 34 34 95 95 100 100 100 50
Tab.1  Concentrations of target antibiotics in influent (ng/L), effluent (ng/L), and sludge (µg/kg, dw) samples from 18 WWTPs in Harbin, north-eastern China.
Fig.3  Distribution of target antibiotics in 18 WWTPs in Harbin, China.
Fig.4  Removal efficiencies for target antibiotics in different WWTPs.
Fig.5  Concentrations of antibiotics in effluents from different treatment units in the WWTPs.
WWTP Treatment
process
HRTa)
(h)
Sludge retention time (d) Dehydrated sludge per day (t/d) Conventional parameters (mg/L)
CODb) BODc) T-Nd) T-Pe)
I E I E I E I E
W6 AO 16 20 460 619 50 332 11.8 41.2 18.3 7.37 0.70
W15 A2O 6 15?30 20 121 25 63.7 5.8 16.3 10.9 1.9 0.18
W9 CAST 6 15 45 429 30 224 6.6 35.8 11.7 10.1 0.43
W4 CASS 6 18 70 230 20 83.9 6.3 17.5 10.7 5.6 0.25
Tab.2  Process parameters and processing capacities of different WWTPs
1 KArimori, S Miyamoto, KFukuda, CNakamura, MNakano (1998). Characteristic difference in gastrointestinal excretion of clarithromycin and roxithromycin. Biopharmaceutics & Drug Disposition, 19(7): 433–438
2 MAshfaq, Y Li, Y WWang, W JChen, HWang, X Q Chen, W Wu, Z YHuang, C PYu, QSun (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 LBing, Z Tong (2010). Biodegradation and adsorption of antibiotics in the activated sludge process. Environmental Science & Technology, 44: 3468–3473
4 BBlair, A Nikolaus, CHedman, RKlaper, TGrundl (2015). Evaluating the degradation, sorption, and negative mass balances of pharmaceuticals and personal care products during wastewater treatment. Chemosphere, 134: 395–401
5 J MCha, S Yang, K HCarlson (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 MClara, B Strenn, OGans, EMartinez, NKreuzinger, HKroiss (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 JDu, Y Fan, XQian (2015). Occurrence and behavior of pharmaceuticals in sewage treatment plants in eastern China. Frontiers of Environmental Science & Engineering, 9(4): 725–730
8 JFeitosa-Felizzola, BTemime, SChiron (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 A MFranklin, C F Williams, D M Andrews, E E Woodward, J E Watson (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 L HGao, Y L Shi, W H Li, H Y Niu, J M Liu, Y Q Cai (2012). Occurrence of antibiotics in eight sewage treatment plants in Beijing, China. Chemosphere, 86(6): 665–671
11 AGöbel, A Thomsen, C SMcardell, AJoss, W Giger (2005). Occurrence and sorption behavior of sulfonamides, macrolides, and trimethoprim in activated sludge treatment. Environmental Science & Technology, 39(11): 3981–3989
12 AGoebel, C S McArdell, A Joss, HSiegrist, WGiger (2007). Fate of sulfonamides, macrolides, and trimethoprim in different wastewater treatment technologies. Science of the Total Environment, 372(2–3): 361–371
13 E MGolet, A C Alder, W Giger (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 X YGuo, N Wang, X UJing, S JJiao, Z CWang, Z JShan, W GTang (2014). Research progress on environmental exposure levels and environmental fate of veterinary antibiotics. Environmental Science & Technology, 37(9): 76–86
15 HHuang, J Wu, JYe, T JYe, JDeng, Y M Liang, W Liu (2018). Occurrence, removal, and environmental risks of pharmaceuticals in wastewater treatment plants in south China. Frontiers of Environmental Science & Engineering, 12(6): 7
16 I HIgbinosa, A I Okoh (2012). Antibiotic susceptibility profile of Aeromonas species isolated from wastewater treatment plant. TheScientificWorldJournal, 2012: 1–6
17 MJiang, L Wang, RJi (2010). Biotic and abiotic degradation of four cephalosporin antibiotics in a lake surface water and sediment. Chemosphere, 80(11): 1399–1405
18 BLi, T Zhang (2011). Mass flows and removal of antibiotics in two municipal wastewater treatment plants. Chemosphere, 83(9): 1284–1289
19 BLi, T Zhang, ZXu, H HFang (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 X WLi, H C Shi, K X Li, L Zhang, Y PGan (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 A Y CLin, T HYu, S KLateef (2009). Removal of pharmaceuticals in secondary wastewater treatment processes in Taiwan. Journal of Hazardous Materials, 167(1–3): 1163–1169
22 H QLiu, J C W Lam, W W Li, H Q Yu, P K S Lam (2017a). Spatial distribution and removal performance of pharmaceuticals in municipal wastewater treatment plants in China. Science of the Total Environment, 586: 1162–1169
23 JLiu, J J Lu, Y B Tong, C Li (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 T BMinh, H W Leung, I H Loi, W H Chan, M K So, J Q Mao, D Choi, J CLam, GZheng, MMartin (2009). Antibiotics in the Hong Kong metropolitan area: Ubiquitous distribution and fate in Victoria Harbour. Marine Pollution Bulletin, 58(7): 1052–1062
25 EMüller, W Schüssler, HHorn, HLemmer (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 MPiotrowska, D Przygodzinska, KMatyjewicz, MPopowska (2017). Occurrence and variety of beta-lactamase genes among Aeromonas spp. Isolated from urban wastewater treatment plant. Frontiers in Microbiology, 8: 863–874
27 P HRoberts, K V Thomas (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 ARodayan, M Majewsky, VYargeau (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 RSalgado, R Marques, J PNoronha, GCarvalho, AOehmen, M AReis (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 A KSarmah, M T Meyer, A B Boxall (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 KTimraz, Y Xiong, HAl Qarni, P YHong (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 LWang, Z M Qiang, Y G Li, W W Ben (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 W HWang, H Wang, W FZhang, HLiang, D WGao (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 W HWang, W F Zhang, H Liang, D WGao (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 A JWatkinson, E JMurby, D WKolpin, S DCostanzo (2009). The occurrence of antibiotics in an urban watershed: From wastewater to drinking water. Science of the Total Environment, 407(8): 2711–2723
36 RXu, Z H Yang, Q P Wang, Y Bai, J BLiu, YZheng, Y RZhang, W PXiong, KAhmad, C ZFan (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 W HXu, G Zhang, X DLi, S CZou, PLi, Z H Hu, J Li (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 S FYang, C F Lin, C J Wu, K K Ng, A Y C Lin, P K A Hong (2012). Fate of sulfonamide antibiotics in contact with activated sludge—Sorption and biodegradation. Water Research, 46(4): 1301–1308
39 XYu, X Y Tang, J E Zuo, M Y Zhang, L Chen, Z XLi (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 C HZhang, L L Wang, X Y Gao, X D He (2016). Antibiotics in WWTP discharge into the Chaobai River, Beijing. Archives of Environmental Protection, 42(4): 48–57
41 XZhang, H X Zhao, J Du, Y XQu, CShen, F Tan, J WChen, XQuan (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 JZheng, C Su, J WZhou, L KXu, Y YQian, HChen (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 Z XZhong, J Xu, YZhang, C SGuo, W HZhang (2013). Adsorption of sulfonamides on lake sediments. Frontiers of Environmental Science & Engineering, 7(4): 518–525
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