Please wait a minute...
Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2014, Vol. 8 Issue (6) : 888-894    https://doi.org/10.1007/s11783-014-0735-0
RESEARCH ARTICLE
Occurrence and fate of antibiotics in advanced wastewater treatment facilities and receiving rivers in Beijing, China
Xinwei LI1,2,Hanchang SHI1,*(),Kuixiao LI2,Liang ZHANG2,Yiping GAN2
1. School of Environment, Tsinghua University, Beijing 100084, China
2. Beijing Drainage Group Co. Ltd., Beijing 100044, China
 Download: PDF(311 KB)   HTML
 Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
Abstract

The occurrence and removal of 13 antibiotics were investigated in five wastewater treatment plants (WWTPs) with advanced wastewater treatment processes in Beijing, China. Most of the target antibiotics were detected in the secondary and tertiary effluents, with the concentrations of 4.8–1106.0 and 0.3–505.0 ng·L-1. Fluoroquinolone antibiotics showed relatively high concentrations in all samples (782–1814 ng·L-1). Different tertiary treatment processes showed discrepant antibiotics removal performances. Ozonation process was found more effective in removing target antibiotics compared to the coagulation-flocculation-sedimentation process and sand filtration process. Investigation of the target antibiotics in three typical urban rivers in Beijing was carried out to understand antibiotics occurrence in surface water environment. Eight antibiotics were detected in the studied rivers, with highest concentration of antibiotics in the river which was mainly replenished by reclaimed water. This study showed the necessity of employing more effective advanced treatment facilities to further reduce the discharge amount of antibiotics.

Keywords antibiotics      advanced treatment      urban river      reclaimed water     
Corresponding Author(s): Hanchang SHI   
Online First Date: 12 June 2014    Issue Date: 17 November 2014
 Cite this article:   
Xinwei LI,Hanchang SHI,Kuixiao LI, et al. Occurrence and fate of antibiotics in advanced wastewater treatment facilities and receiving rivers in Beijing, China[J]. Front. Environ. Sci. Eng., 2014, 8(6): 888-894.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-014-0735-0
https://academic.hep.com.cn/fese/EN/Y2014/V8/I6/888
class target antibiotics acronym MW CAS number molecular formula
Fluoroquinolones (QNs) Ofloxacin OFL 361 82419-36-1 C18H20FN3O4
Norfloxacin NOR 319 70458-96-7 C16H18FN3O3
Sulfonamides (SAs) Sulfapyridine SPD 249 144-83-2 C11H11N3O2S
Sulfadiazine SDZ 250 68-35-9 C10H10N4O2S
Sulfamethoxazole SMX 253 723-46-6 C10H11N3O3S
Sulfadimidine SDMD 278 57-68-1 C12H14N4O2S
Trimethoprime (TMP) Trimethoprime TMPs 290 738-70-5 C14H18N4O3
Macrolides (MLs) Roxithromycin ROX 837 80214-83-1 C41H76N2O15
Acetyl Spiramycin ASPM 885 C45H76N2O15
Tetracyclines (TCs) Tetracycline TC 444 60-54-8 C22H24N2O8
Oxytetracycline OTC 460 79-57-2 C22H24N2O9
Chlortetracycline CTC 479 57-62-5 C22H23ClN2O8
Doxycycline DXC 444 564-25-0 C22H24N2O8
Tab.1  Characteristics of selected target antibiotics
WWTP treatment process capacity/(t·d-1) operational dosage
A Inf (*)-UF-O3 -NaClO- Eff (*) 80000 O3: 3.5 mg·L-1NaClO: 5–8 mg·L-1
B Inf (*) -O3 -NaClO-CFS- SF- UV- Eff (*) 60000 O3: 3.5 mg·L-1NaClO: 5–8 mg·L-1UV: 800 J·m-2
C Inf (*) -NaClO-CFS- SF- UV- O3- Eff (*) 40000 O3: 2 mg·L-1NaClO: 5–8 mg·L-11UV: 800 J·m-2
D Inf (*)- CFS- SF- ClO2 - Eff (*) 3000 ClO2: 5.6 mg·L-1
E Inf (*)- CFS- SF- Eff (*) 10000
Tab.2  Information of the investigated advanced treatment processes of WWTPs
Fig.1  Locations and sampling sites of the five WWTPs and three rivers in Beijing. A, B, C, D and E represent the locations of five WWTPs. ? represent the sampling sites in three urban rivers
Fig.2  Concentrations of target antibiotics in the secondary effluents of 5 municipal WWTPs in Beijing
Fig.3  Total concentrations of major antibiotic groups in the reclaimed wastewater (a) and removal efficiencies during advanced treatment (b)
Fig.4  Concentrations of target?antibiotics in three urban rivers
1 Jones O A, Voulvoulis N, Lester J N. The occurrence and removal of selected pharmaceutical compounds in a sewage treatment works utilising activated sludge treatment. Environmental Pollution, 2007, 145(3): 738–744
https://doi.org/10.1016/j.envpol.2005.08.077 pmid: 16891046
2 Rosal R, Rodríguez A, Perdigón-Melón J A, Petre A, Garcóa-Calvo E, Gümez M J, Agüera A, Fernández-Alba A R. Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation. Water Research, 2010, 44(2): 578–588
https://doi.org/10.1016/j.watres.2009.07.004 pmid: 19628245
3 Jelic A, Gros M, Ginebreda A, Cespedes-Sánchez R, Ventura F, Petrovic M, Barcelo D. Occurrence, partition and removal of pharmaceuticals in sewage water and sludge during wastewater treatment. Water Research, 2011, 45(3): 1165–1176
https://doi.org/10.1016/j.watres.2010.11.010 pmid: 21167546
4 Xue B, Zhang R, Wang Y, Liu X, Li J, Zhang G. 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. Ecotoxicology and Environmental Safety, 2013, 92: 229–236
https://doi.org/10.1016/j.ecoenv.2013.02.009 pmid: 23478166
5 Kleywegt S, Pileggi V, Yang P, Hao C, Zhao X, Rocks C, Thach S, Cheung P, Whitehead B. Pharmaceuticals, hormones and bisphenol A in untreated source and finished drinking water in Ontario, Canada—occurrence and treatment efficiency. Science of the Total Environment, 2011, 409(8): 1481–1488
https://doi.org/10.1016/j.scitotenv.2011.01.010 pmid: 21315426
6 Watkinson A J, Murby E J, Costanzo S D. Removal of antibiotics in conventional and advanced wastewater treatment: implications for environmental discharge and wastewater recycling. Water Research, 2007, 41(18): 4164–4176
https://doi.org/10.1016/j.watres.2007.04.005 pmid: 17524445
7 Jia A, Wan Y, Xiao Y, Hu J. Occurrence and fate of quinolone and fluoroquinolone antibiotics in a municipal sewage treatment plant. Water Research, 2012, 46(2): 387–394
https://doi.org/10.1016/j.watres.2011.10.055 pmid: 22118907
8 Zhou L J, Ying G G, Liu S, Zhao J L, Yang B, Chen Z F, Lai H J. Occurrence and fate of eleven classes of antibiotics in two typical wastewater treatment plants in South China. Science of the Total Environment, 2013, 452-453: 365–376
https://doi.org/10.1016/j.scitotenv.2013.03.010 pmid: 23538107
9 Huber M M, G?bel A, Joss A, Hermann N, L?ffler D, McArdell C S, Ried A, Siegrist H, Ternes T A, von Gunten U. Oxidation of pharmaceuticals during ozonation of municipal wastewater effluents: a pilot study. Environmental Science and Technology, 2005, 39(11): 4290–4299
https://doi.org/10.1021/es048396s pmid: 15984812
10 Huber M M, Korhonen S, Ternes T A, von Gunten U. Oxidation of pharmaceuticals during water treatment with chlorine dioxide. Water Research, 2005, 39(15): 3607–3617
https://doi.org/10.1016/j.watres.2005.05.040 pmid: 16061268
11 Lee Y, von Gunten U. Oxidative transformation of micropollutants during municipal wastewater treatment: comparison of kinetic aspects of selective (chlorine, chlorine dioxide, ferrate VI, and ozone) and non-selective oxidants (hydroxyl radical). Water Research, 2010, 44(2): 555–566
https://doi.org/10.1016/j.watres.2009.11.045 pmid: 20015530
12 Wang P, He Y L, Huang C H. Reactions of tetracycline antibiotics with chlorine dioxide and free chlorine. Water Research, 2011, 45(4): 1838–1846
https://doi.org/10.1016/j.watres.2010.11.039 pmid: 21168893
13 Nakada N, Shinohara H, Murata A, Kiri K, Managaki S, Sato N, Takada H. Removal of selected pharmaceuticals and personal care products (PPCPs) and endocrine-disrupting chemicals (EDCs) during sand filtration and ozonation at a municipal sewage treatment plant. Water Research, 2007, 41(19): 4373–4382
https://doi.org/10.1016/j.watres.2007.06.038 pmid: 17632207
14 Ternes T A, Stüber J, Herrmann N, McDowell D, Ried A, Kampmann M, Teiser B. Ozonation: a tool for removal of pharmaceuticals, contrast media and musk fragrances from wastewater? Water Research, 2003, 37(8): 1976–1982
https://doi.org/10.1016/S0043-1354(02)00570-5 pmid: 12697241
15 Xu W, Zhang G, Li X, Zou S, Li P, Hu Z, Li J. Occurrence and elimination of antibiotics at four sewage treatment plants in the Pearl River Delta (PRD), South China. Water Research, 2007, 41(19): 4526–4534
https://doi.org/10.1016/j.watres.2007.06.023 pmid: 17631935
16 Zhang H, Liu P, Feng Y, Yang F. Fate of antibiotics during wastewater treatment and antibiotic distribution in the effluent-receiving waters of the Yellow Sea, northern China. Marine Pollution Bulletin, 2013, 73(1): 282–290
https://doi.org/10.1016/j.marpolbul.2013.05.007 pmid: 23768979
17 Li W, Shi Y, Gao L, Liu J, Cai Y. Occurrence and removal of antibiotics in a municipal wastewater reclamation plant in Beijing, China. Chemosphere, 2013, 92(4): 435–444
https://doi.org/10.1016/j.chemosphere.2013.01.040 pmid: 23399307
18 Tong C, Zhuo X, Guo Y. Occurrence and risk assessment of four typical fluoroquinolone antibiotics in raw and treated sewage and in receiving waters in Hangzhou, China. Journal of Agricultural and Food Chemistry, 2011, 59(13): 7303–7309
https://doi.org/10.1021/jf2013937 pmid: 21630710
19 Zorita S, M?rtensson L, Mathiasson L. Occurrence and removal of pharmaceuticals in a municipal sewage treatment system in the south of Sweden. Science of the Total Environment, 2009, 407(8): 2760–2770
https://doi.org/10.1016/j.scitotenv.2008.12.030 pmid: 19157523
20 Vieno N M, H?rkki H, Tuhkanen T, Kronberg L. Occurrence of pharmaceuticals in river water and their elimination in a pilot-scale drinking water treatment plant. Environmental Science and Technology, 2007, 41(14): 5077–5084
https://doi.org/10.1021/es062720x pmid: 17711226
21 Gracia-Lor E, Sancho J V, Serrano R, Hernández F. Occurrence and removal of pharmaceuticals in wastewater treatment plants at the Spanish Mediterranean area of Valencia. Chemosphere, 2012, 87(5): 453–462
https://doi.org/10.1016/j.chemosphere.2011.12.025 pmid: 22221664
22 Karthikeyan K G, Meyer M T. Occurrence of antibiotics in wastewater treatment facilities in Wisconsin, USA. Science of the Total Environment, 2006, 361(1–3): 196–207
https://doi.org/10.1016/j.scitotenv.2005.06.030 pmid: 16091289
23 Behera S K, Kim H W, Oh J E, Park H S. Occurrence and removal of antibiotics, hormones and several other pharmaceuticals in wastewater treatment plants of the largest industrial city of Korea. Science of the Total Environment, 2011, 409(20): 4351–4360
https://doi.org/10.1016/j.scitotenv.2011.07.015 pmid: 21807398
24 Yang X, Flowers R C, Weinberg H S, Singer P C. Occurrence and removal of pharmaceuticals and personal care products (PPCPs) in an advanced wastewater reclamation plant. Water Research, 2011, 45(16): 5218–5228
https://doi.org/10.1016/j.watres.2011.07.026 pmid: 21864879
25 Wang H. Ozone kinetics of dimethyl sulfide in the presence of water vapor. Frontiers of Environmental Science and Engineering, 2013, 7(6): 833–835
https://doi.org/10.1007/s11783-013-0570-8
26 Nakada N, Kiri K, Shinohara H, Harada A, Kuroda K, Takizawa S, Takada H. Evaluation of pharmaceuticals and personal care products as water-soluble molecular markers of sewage. Environmental Science and Technology, 2008, 42(17): 6347–6353
https://doi.org/10.1021/es7030856 pmid: 18800500
27 Ikehata K, Gamal El-Din M, Snyder S A. Ozonation and advanced oxidation treatment of emerging organic pollutants in water and wastewater. Ozone Science and Engineering, 2008, 30(1): 21–26
https://doi.org/10.1080/01919510701728970
28 Sui Q, Huang J, Deng S, Yu G, Fan Q. Occurrence and removal of pharmaceuticals, caffeine and DEET in wastewater treatment plants of Beijing, China. Water Research, 2010, 44(2): 417–426
https://doi.org/10.1016/j.watres.2009.07.010 pmid: 19674764
29 Hey G, Grabic R, Ledin A, La Cour Jansen J, Andersen H. Oxidation of pharmaceuticals by chlorine dioxide in biologically treated wastewater. Chemical Engineering Journal, 2012, 185: 236–242
https://doi.org/10.1016/j.cej.2012.01.093
30 Batt A L, Kim S, Aga D S. Comparison of the occurrence of antibiotics in four full-scale wastewater treatment plants with varying designs and operations. Chemosphere, 2007, 68(3): 428–435
https://doi.org/10.1016/j.chemosphere.2007.01.008 pmid: 17316751
31 Adams C, Wang Y, Loftin K, Meyer M. Removal of antibiotics from surface and distilled water in conventional water treatment processes. Journal of Environmental Engineering, 2002, 128(3): 253–260
https://doi.org/10.1061/(ASCE)0733-9372(2002)128:3(253)
32 Canonica S, Meunier L, von Gunten U. Phototransformation of selected pharmaceuticals during UV treatment of drinking water. Water Research, 2008, 42(1–2): 121–128
https://doi.org/10.1016/j.watres.2007.07.026 pmid: 17709124
33 Xu W H, Zhang G, Zou S C, Li X D, Liu Y C. Determination of selected antibiotics in the Victoria Harbour and the Pearl River, South China using high-performance liquid chromatography-electrospray ionization tandem mass spectrometry. Environmental Pollution, 2007, 145(3): 672–679
https://doi.org/10.1016/j.envpol.2006.05.038 pmid: 16996177
34 L?ffler D, Ternes T A. Determination of acidic pharmaceuticals, antibiotics and ivermectin in river sediment using liquid chromatography-tandem mass spectrometry. Journal of Chromatography A, 2003, 1021(1–2): 133–144
https://doi.org/10.1016/j.chroma.2003.08.089 pmid: 14735982
35 Beausse J. Selected drugs in solid matrices: a review of environmental determination, occurrence and properties of principal substances. Trends in Analytical Chemistry, 2004, 23(10–11): 753–761
https://doi.org/10.1016/j.trac.2004.08.005
[1] Qinxue Wen, Shuo Yang, Zhiqiang Chen. Mesophilic and thermophilic anaerobic digestion of swine manure with sulfamethoxazole and norfloxacin: Dynamics of microbial communities and evolution of resistance genes[J]. Front. Environ. Sci. Eng., 2021, 15(5): 94-.
[2] Ying Cui, Feng Tan, Yan Wang, Suyu Ren, Jingwen Chen. Diffusive gradients in thin films using molecularly imprinted polymer binding gels for in situ measurements of antibiotics in urban wastewaters[J]. Front. Environ. Sci. Eng., 2020, 14(6): 111-.
[3] Fang Zhang, Hao Zhang, Ying Yuan, Dun Liu, Chenyu Zhu, Di Zheng, Guanghe Li, Yuquan Wei, Dan Sun. Different response of bacterial community to the changes of nutrients and pollutants in sediments from an urban river network[J]. Front. Environ. Sci. Eng., 2020, 14(2): 28-.
[4] Peng Hu, Changsheng Guo, Yan Zhang, Jiapei Lv, Yuan Zhang, Jian Xu. Occurrence, distribution and risk assessment of abused drugs and their metabolites in a typical urban river in north China[J]. Front. Environ. Sci. Eng., 2019, 13(4): 56-.
[5] Weihua Wang, Wanfeng Zhang, Hong Liang, Dawen Gao. Occurrence and fate of typical antibiotics in wastewater treatment plants in Harbin, North-east China[J]. Front. Environ. Sci. Eng., 2019, 13(3): 34-.
[6] Qinqin Liu, Miao Li, Rui Liu, Quan Zhang, Di Wu, Danni Zhu, Xuhui Shen, Chuanping Feng, Fawang Zhang, Xiang Liu. Removal of trimethoprim and sulfamethoxazole in artificial composite soil treatment systems and diversity of microbial communities[J]. Front. Environ. Sci. Eng., 2019, 13(2): 28-.
[7] Ning Zhang, Xiang Liu, Rui Liu, Tao Zhang, Miao Li, Zhuoran Zhang, Zitao Qu, Ziting Yuan, Hechun Yu. Influence of reclaimed water discharge on the dissemination and relationships of sulfonamide, sulfonamide resistance genes along the Chaobai River, Beijing[J]. Front. Environ. Sci. Eng., 2019, 13(1): 8-.
[8] Jiao Zhang, Zhen Wei, Haifeng Jia, Xia Huang. Factors influencing water quality indices in a typical urban river originated with reclaimed water[J]. Front. Environ. Sci. Eng., 2017, 11(4): 8-.
[9] Xiaoyan Song, Rui Liu, Lujun Chen, Tomoki Kawagishi. Comparative experiment on treating digested piggery wastewater with a biofilm MBR and conventional MBR: simultaneous removal of nitrogen and antibiotics[J]. Front. Environ. Sci. Eng., 2017, 11(2): 11-.
[10] Xiuhong Liu, Hongchen Wang, Qing Yang, Jianmin Li, Yuankai Zhang, Yongzhen Peng. Online control of biofilm and reducing carbon dosage in denitrifying biofilter: pilot and full-scale application[J]. Front. Environ. Sci. Eng., 2017, 11(1): 4-.
[11] Wentao Zhao, Ying Guo, Shuguang Lu, Pingping Yan, Qian Sui. Recent advances in pharmaceuticals and personal care products in the surface water and sediments in China[J]. Front. Environ. Sci. Eng., 2016, 10(6): 2-.
[12] Chaojie Jiang, Lifen Liu, John C. Crittenden. An electrochemical process that uses an Fe0/TiO2 cathode to degrade typical dyes and antibiotics and a bio-anode that produces electricity[J]. Front. Environ. Sci. Eng., 2016, 10(4): 15-.
[13] Shiliang WANG,Hui WANG. Adsorption behavior of antibiotic in soil environment: a critical review[J]. Front. Environ. Sci. Eng., 2015, 9(4): 565-574.
[14] Min LIU,Rusong WANG,Jinlou HUANG. Effects of in situ biological treatments on heavy metal release of urban river sediment[J]. Front.Environ.Sci.Eng., 2014, 8(4): 607-615.
[15] WEI Yimei,ZHANG Yuan,XU Jian,GUO Changsheng,LI Lei,FAN Wenhong. Simultaneous quantification of several classes of antibiotics in water, sediments, and fish muscles by liquid chromatography–tandem mass spectrometry[J]. Front.Environ.Sci.Eng., 2014, 8(3): 357-371.
Viewed
Full text


Abstract

Cited

  Shared   
  Discussed