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.    2018, Vol. 12 Issue (6) : 7    https://doi.org/10.1007/s11783-018-1053-8
RESEARCH ARTICLE
Occurrence, removal, and environmental risks of pharmaceuticals in wastewater treatment plants in south China
Huang Huang1,2, Jie Wu1,2, Jian Ye1,2, Tingjin Ye3, Jia Deng1,2, Yongmei Liang1,2(), Wei Liu1,2()
1. School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou 510006, China
2. Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Guangzhou 510006, China
3. Foshan Water Group Co., Ltd., Foshan 528000, China
 Download: PDF(473 KB)   HTML
 Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
Abstract

Five pharmaceuticals were detected in wastewater treatment plants in southern China.

Biological treatment was the most effective process for PhACs removal.

Metoprolol showed negative removal during secondary treatment process.

The pharmaceuticals studied posed a low environmental risk to aquatic ecosystems.

Pharmaceutically active compounds in wastewater released from human consumption have received considerable attention because of their possible risks for aquatic environments. In this study, the occurrence and removal of 10 pharmaceuticals in three municipal wastewater treatment plants in southern China were investigated and the environmental risks they posed were assessed. Nifedipine, atenolol, metoprolol, valsartan and pravastatin were detected in the influent wastewater. The highest average concentration in the influents was observed for metoprolol (164.6 ng/L), followed by valsartan (120.3 ng/L) in August, while median concentrations were higher in November than in August. The total average daily mass loadings of the pharmaceuticals in the three plants were 289.52 mg/d/person, 430.46 mg/d/person and 368.67 mg/d/person, respectively. Elimination in the treatment plants studied was incomplete, with metoprolol levels increasing during biological treatment. Biological treatment was the most effective step for PhACs removal in all of the plants studied. Moreover, the removal of PhACs was observed with higher efficiencies in August than in November. The WWTP equipped with an Unitank process exhibited similar removals of most PhACs as other WWTPs equipped with an anoxic/oxic (A/O) process or various anaerobic-anoxic-oxic (A2/O) process. The environmental risk assessment concluded that all of the single PhAC in the effluents displayed a low risk (RQ<0.1) to the aquatic environments.

Keywords Pharmaceuticals      Wastewater treatment      Pearl River Delta      Occurrence      Removal      Risk assessment     
Corresponding Author(s): Yongmei Liang,Wei Liu   
Issue Date: 19 August 2018
 Cite this article:   
Huang Huang,Jie Wu,Jian Ye, et al. Occurrence, removal, and environmental risks of pharmaceuticals in wastewater treatment plants in south China[J]. Front. Environ. Sci. Eng., 2018, 12(6): 7.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-018-1053-8
https://academic.hep.com.cn/fese/EN/Y2018/V12/I6/7
Fig.1  Schematic diagrams of the WWTPs studied
Fig.2  Concentration ranges of PhACs in the influents of three WWTPs in the PRD area
Fig.3  Average daily mass loadings of target PhACs in three WWTPs
PhAC August
WWTPA WWTPB-1 WWTPB-2 WWTPB-3 WWTPC
Influent Primary effluent Secondary effluent Final effluent Influent Primary
effluent
Secondary
effluent
Final effluent Influent Primary
effluent
Secondary
effluent
Final effluent Influent Primary
effluent
Secondary
effluent
Final effluent Influent Primary
effluent
Secondary
effluent
Final effluent
NIP 23.0 19.0 9.0 6.0 29.8 25.6 18.7 3.2 -- -- -- -- 11.4 9.0 4.8 2.7 6.8 6.0 5.4 0
ATE 10.0 8.0 4.9 0 -- -- -- -- -- -- -- -- -- -- -- -- -- -- -- --
MET 386.8 300.0 415.9 405 96.6 80.7 97.6 97.6 221.5 198.9 252.4 252.2 169.7 150.5 198.5 198.3 78 74.2 141.6 119.6
VAL 211.0 198.0 98.0 72.0 87.4 73.0 12.2 8.4 96.4 93.1 46.8 41.0 96.5 80.3 13.4 10.5 200.9 192.2 101.6 90.1
PRA 112.0 108.0 64.0 53.0 67.9 61.9 47.5 47.1 123.9 122.8 85.8 68.8 54.6 54.1 32.6 28.9 98.3 94.6 62.3 52.9
Tab.1  Average PhACs concentrations (ng/L) in the effluents from various treatment units of three WWTPs
PhAC November
WWTPA WWTPB-1 WWTPB-2 WWTPB-3 WWTPC
Influent Primary
effluent
Secondary
effluent
Final effluent Influent Primary
effluent
Secondary
effluent
Final effluent Influent Primary
effluent
Secondary
effluent
Final effluent Influent Primary
effluent
Secondary
effluent
Final effluent Influent Primary
effluent
Secondary
effluent
Final effluent
NIP 34.3 31.1 21.3 19.8 32.0 28.8 25.3 20.5 -- -- -- -- 18.1 16.1 8.8 7.2 48.6 43.3 19.4 17.5
ATE 12.3 10.6 7.7 6.73 -- -- -- -- -- -- -- -- -- -- -- -- -- -- -- --
MET 116.8 116.5 171.7 197.1 382.6 376.5 615.3 613.2 206.0 208.8 330.4 329.3 119.7 115.2 126.1 121.0 49.5 43.4 145.7 138.1
VAL 278.2 253.2 180.5 153.9 587.2 500.9 253.7 171.3 132.7 113.5 86.1 75.2 280.5 267.9 31.3 25.1 146.5 113.5 51.7 46.3
PRA 180.5 165.3 96.9 72.9 131.9 97.6 94.6 74.2 594.1 316.8 77.8 45.8 158.3 117.9 75.5 66.3 144.3 113.8 65.6 58.4
Tab.2  
Fig.4  Overall PhACs removal efficiencies of various treatment processes in three WWTPs (Missing values were undetectable in the influent or effluent samples)
NIP ATE MET VAL PRA
August WWTPA Primary 17.4 20.0 22.4 6.2 3.6
Secondary 43.5 31.0 -30.0 47.4 39.3
Disinfection 13.0 49.0 2.8 12.3 9.8
Total 73.9 100.0 -4.7 65.9 52.7
WWTPB-1 Primary 14.1 -- 16.4 16.4 8.9
Secondary 23.3 -- -17.5 69.6 21.1
Disinfection 51.9 -- 0 4.4 0.6
Total 89.3 -- -1.1 90.4 30.6
WWTPB-2 Primary -- -- 10.2 3.4 0.9
Secondary -- -- -24.2 48.1 29.8
Disinfection -- -- 0.1 6.0 13.7
Total -- -- -13.8 57.5 44.4
WWTPB-3 Primary 20.9 -- 11.3 8.5 16.8
Secondary 37.3 -- -28.3 69.3 39.5
Disinfection 17.9 -- 0.1 3.0 6.7
Total 76.1 -- -16.9 89.1 46.9
WWTPC Primary 12.0 -- 4.8 4.3 3.7
Secondary 8.5 -- -86.3 45.1 32.8
Disinfection 79.5 -- 28.2 5.7 9.6
Total 100.0 -- -53.3 55.1 46.2
November WWTPA Primary 9.3 13.9 0.3 8.9 8.4
Secondary 28.6 23.4 -47.3 26.1 37.9
Disinfection 4.4 7.8 -21.8 9.6 13.3
Total 42.2 45.3 -68.8 44.7 59.6
WWTPB-1 Primary 10.2 -- 1.6 14.7 26.0
Secondary 10.7 -- -62.4 42.1 2.3
Disinfection 15.1 -- 0.5 14.0 15.5
Total 36.0 -- -60.3 70.8 43.8
WWTPB-2 Primary -- -- -1.3 14.5 46.7
Secondary -- -- -59.0 20.6 40.2
Disinfection -- -- 0.6 8.2 5.4
Total -- -- -59.8 43.3 92.3
WWTPB-3 Primary 11.0 -- 3.6 4.5 25.5
Secondary 40.6 -- -9.1 84.3 26.8
Disinfection 8.4 -- 4.3 2.2 5.8
Total 60.1 -- -1.1 91.1 58.1
WWTPC Primary 10.9 -- 12.3 22.6 21.1
Secondary 49.0 -- -206.8 42.1 33.4
Disinfection 4.0 -- 15.4 3.7 5.0
Total 64.0 -- -179.1 68.4 59.5
Tab.3  Removal efficiencies (%) of PhACs detected in various treatment unit of three WWTPs
Fig.5  Estimated RQs of the PhACs in effluents of WWTPs for acute toxicity of daphnia, fish, and algae
1 Backhaus T, Scholze M, Grimme L H (2000). The single substance and mixture toxicity of quinolones to the bioluminescent bacterium Vibrio fischeri. Aquatic Toxicology (Amsterdam, Netherlands), 49(1-2): 49–61
https://doi.org/10.1016/S0166-445X(99)00069-7 pmid: 10814806
2 Behera S K, Kim H W, Oh J E, Park H S (2011). 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, 409(20): 4351–4360
https://doi.org/10.1016/j.scitotenv.2011.07.015 pmid: 21807398
3 Brennan P J, Greenberg G, Miall W E, Thompson S G (1982). Seasonal variation in arterial blood pressure. British Medical Journal (Clinical Research Ed.), 285(6346): 919–923
https://doi.org/10.1136/bmj.285.6346.919 pmid: 6811068
4 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
https://doi.org/10.1021/es048550a pmid: 15984773
5 Hernando M D, Mezcua M, Fernández-Alba A R, Barceló D (2006). Environmental risk assessment of pharmaceutical residues in wastewater effluents, surface waters and sediments. Talanta, 69(2): 334–342
https://doi.org/10.1016/j.talanta.2005.09.037 pmid: 18970571
6 Huang Q, Yu Y, Tang C, Zhang K, Cui J, Peng X (2011). Occurrence and behavior of non-steroidal anti-inflammatory drugs and lipid regulators in wastewater and urban river water of the Pearl River Delta, South China. Journal of Environmental Monitoring, 13(4): 855– 863
https://doi.org/10.1039/c1em10015g pmid: 21412553
7 Huerta-Fontela M, Galceran M T, Ventura F (2011). Occurrence and removal of pharmaceuticals and hormones through drinking water treatment. Water Research, 45(3): 1432–1442
https://doi.org/10.1016/j.watres.2010.10.036 pmid: 21122885
8 Kasprzyk-Hordern B, Dinsdale R M, Guwy A J (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 Research, 43(2): 363–380
https://doi.org/10.1016/j.watres.2008.10.047 pmid: 19022470
9 Khan S J, Ongerth J E (2002). Estimation of pharmaceutical residues in primary and secondary sewage sludge based on quantities of use and fugacity modelling. Water Science and Technology, 46(3): 105–113
pmid: 12227595
10 Kosma C I, Lambropoulou D A, Albanis T A (2014). Investigation of PPCPs in wastewater treatment plants in Greece: occurrence, removal and environmental risk assessment. Science of the Total Environment, 466-467(1): 421–438
https://doi.org/10.1016/j.scitotenv.2013.07.044 pmid: 23933429
11 Lolić A, Paíga P, Santos L H M L, Ramos S, Correia M, Delerue-Matos C (2015). Assessment of non-steroidal anti-inflammatory and analgesic pharmaceuticals in seawaters of North of Portugal: Occurrence and environmental risk. Science of the Total Environment, 508(3): 240–250
https://doi.org/10.1016/j.scitotenv.2014.11.097 pmid: 25481252
12 Lv M, Sun Q, Hu A, Hou L, Li J, Cai X, Yu C P (2014). Pharmaceuticals and personal care products in a mesoscale subtropical watershed and their application as sewage markers. Journal of Hazardous Materials, 280: 696–705
https://doi.org/10.1016/j.jhazmat.2014.08.054 pmid: 25232652
13 Papageorgiou M, Kosma C, Lambropoulou D (2016). Seasonal occurrence, removal, mass loading and environmental risk assessment of 55 pharmaceuticals and personal care products in a municipal wastewater treatment plant in Central Greece. Science of the Total Environment, 543(A): 547–569
14 Peng X, Ou W, Wang C, Wang Z, Huang Q, Jin J, Tan J (2014). Occurrence and ecological potential of pharmaceuticals and personal care products in groundwater and reservoirs in the vicinity of municipal landfills in China. Science of the Total Environment, 490(8): 889–898
https://doi.org/10.1016/j.scitotenv.2014.05.068 pmid: 24908648
15 Quinn B, Gagné F, Blaise C (2009). Evaluation of the acute, chronic and teratogenic effects of a mixture of eleven pharmaceuticals on the cnidarian, Hydra attenuata. Science of the Total Environment, 407(3): 1072–1079
https://doi.org/10.1016/j.scitotenv.2008.10.022 pmid: 19013635
16 Radjenović J, Petrović M, Barceló D (2009). Fate and distribution of pharmaceuticals in wastewater and sewage sludge of the conventional activated sludge (CAS) and advanced membrane bioreactor (MBR) treatment. Water Research, 43(3): 831–841
https://doi.org/10.1016/j.watres.2008.11.043 pmid: 19091371
17 Roberts J, Kumar A, Du J, Hepplewhite C, Ellis D J, Christy A G, Beavis S G (2016). Pharmaceuticals and personal care products (PPCPs) in Australia’s largest inland sewage treatment plant, and its contribution to a major Australian river during high and low flow. Science of the Total Environment, 541(1): 1625–1637
https://doi.org/10.1016/j.scitotenv.2015.03.145 pmid: 26456435
18 Rosal R, Rodríguez A, Perdigón-Melón J A, Petre A, García-Calvo E, Gómez M J, Agüera A, Fernández-Alba A R (2010). Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation. Water Research, 44(2 2SI): 578–588
https://doi.org/10.1016/j.watres.2009.07.004 pmid: 19628245
19 Subedi B, Kannan K (2015). Occurrence and fate of select psychoactive pharmaceuticals and antihypertensives in two wastewater treatment plants in New York State, USA. Science of the Total Environment, 514(5): 273–280
https://doi.org/10.1016/j.scitotenv.2015.01.098 pmid: 25666287
20 Sui Q, Huang J, Deng S, Chen W, Yu G (2011). Seasonal variation in the occurrence and removal of pharmaceuticals and personal care products in different biological wastewater treatment processes. Environmental Science & Technology, 45(8): 3341–3348
https://doi.org/10.1021/es200248d pmid: 21428396
21 Sun Q, Lv M, Hu A (2014). Seasonal variation in the occurrence and removal of pharmaceuticals and personal care products in a wastewater treatment plant in Xiamen, China. Journal of Hazardous Materials, 277(SI): 69–75
22 United State Environmental Protection Agency (USEPA) (2007). EPA Method 1694: Pharmaceuticals and Personal Care Products in Water, Soil, Sediment, and Biosolids by HPLC/MS/MS
23 Verlicchi P, Al Aukidy M, Zambello E (2012). Occurrence of pharmaceutical compounds in urban wastewater: Removal, mass load and environmental risk after a secondary treatment--a review. Science of the Total Environment, 429: 123–155
https://doi.org/10.1016/j.scitotenv.2012.04.028 pmid: 22583809
24 Verlicchi P, Galletti A, Petrovic M, Barceló D (2010). Hospital effluents as a source of emerging pollutants: An overview of micropollutants and sustainable treatment options. Journal of Hydrology (Amsterdam), 389(3–4): 416–428
https://doi.org/10.1016/j.jhydrol.2010.06.005
25 Vieno N, Tuhkanen T, Kronberg L (2007). Elimination of pharmaceuticals in sewage treatment plants in Finland. Water Research, 41(5): 1001–1012
https://doi.org/10.1016/j.watres.2006.12.017 pmid: 17261324
26 Wang J, Zhang L, Wang F, Liu L, Wang H, and the China National Survey of Chronic Kidney Disease Working Group (2014). Prevalence, awareness, treatment, and control of hypertension in China: Results from a national survey. American Journal of Hypertension, 27(11): 1355–1361
https://doi.org/10.1093/ajh/hpu053 pmid: 24698853
27 Yan Q, Gao X, Chen Y P, Peng X Y, Zhang Y X, Gan X M, Zi C F, Guo J S (2014a). Occurrence, fate and ecotoxicological assessment of pharmaceutically active compounds in wastewater and sludge from wastewater treatment plants in Chongqing, the Three Gorges Reservoir Area. Science of the Total Environment, 470-471(2): 618–630
https://doi.org/10.1016/j.scitotenv.2013.09.032 pmid: 24176710
28 Yan Q, Gao X, Huang L, Gan X M, Zhang Y X, Chen Y P, Peng X Y, Guo J S (2014a). Occurrence and fate of pharmaceutically active compounds in the largest municipal wastewater treatment plant in Southwest China: Mass balance analysis and consumption back-calculated model. Chemosphere, 99(3): 160–170
https://doi.org/10.1016/j.chemosphere.2013.10.062 pmid: 24268750
29 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
https://doi.org/10.1039/C4EM00596A pmid: 25614232
[1] FSE-18022-OF-HH_suppl_1 Download
[1] Zongqun Chen, Wei Jin, Hailong Yin, Mengqi Han, Zuxin Xu. Performance evaluation on the pollution control against wet weather overflow based on on-site coagulation/flocculation in terminal drainage pipes[J]. Front. Environ. Sci. Eng., 2021, 15(6): 111-.
[2] Guolong Zeng, Yiyang Liu, Xiaoguo Ma, Yinming Fan. Fabrication of magnetic multi-template molecularly imprinted polymer composite for the selective and efficient removal of tetracyclines from water[J]. Front. Environ. Sci. Eng., 2021, 15(5): 107-.
[3] Yuan Meng, Weiyi Liu, Heidelore Fiedler, Jinlan Zhang, Xinrui Wei, Xiaohui Liu, Meng Peng, Tingting Zhang. Fate and risk assessment of emerging contaminants in reclaimed water production processes[J]. Front. Environ. Sci. Eng., 2021, 15(5): 104-.
[4] Kangying Guo, Baoyu Gao, Jie Wang, Jingwen Pan, Qinyan Yue, Xing Xu. Flocculation behaviors of a novel papermaking sludge-based flocculant in practical printing and dyeing wastewater treatment[J]. Front. Environ. Sci. Eng., 2021, 15(5): 103-.
[5] Mengqing Ge, Tao Lin, Kemei Zhou, Hong Chen, Hang Xu, Hui Tao, Wei Chen. Characteristics and removal mechanism of the precursors of N-chloro-2,2-dichloroacetamide in a drinking water treatment process at Taihu Lake[J]. Front. Environ. Sci. Eng., 2021, 15(5): 93-.
[6] Lina Gan, Kezhi Li, Hejingying Niu, Yue Peng, Jianjun Chen, Yuandong Huang, Junhua Li. Simultaneous removal of NOx and chlorobenzene on V2O5/TiO2 granular catalyst: Kinetic study and performance prediction[J]. Front. Environ. Sci. Eng., 2021, 15(4): 70-.
[7] Sanjena Narayanasamydamodaran, Jian’e Zuo, Haiteng Ren, Nawnit Kumar. Scrap Iron Filings assisted nitrate and phosphate removal in low C/N waters using mixed microbial culture[J]. Front. Environ. Sci. Eng., 2021, 15(4): 66-.
[8] Yuxin Li, Jiayin Ling, Pengcheng Chen, Jinliang Chen, Ruizhi Dai, Jinsong Liao, Jiejing Yu, Yanbin Xu. Pseudomonas mendocina LYX: A novel aerobic bacterium with advantage of removing nitrate high effectively by assimilation and dissimilation simultaneously[J]. Front. Environ. Sci. Eng., 2021, 15(4): 57-.
[9] Yunping Han, Lin Li, Ying Wang, Jiawei Ma, Pengyu Li, Chao Han, Junxin Liu. Composition, dispersion, and health risks of bioaerosols in wastewater treatment plants: A review[J]. Front. Environ. Sci. Eng., 2021, 15(3): 38-.
[10] Shengjie Qiu, Jinjin Liu, Liang Zhang, Qiong Zhang, Yongzhen Peng. Sludge fermentation liquid addition attained advanced nitrogen removal in low C/N ratio municipal wastewater through short-cut nitrification-denitrification and partial anammox[J]. Front. Environ. Sci. Eng., 2021, 15(2): 26-.
[11] Ragini Pirarath, Palani Shivashanmugam, Asad Syed, Abdallah M. Elgorban, Sambandam Anandan, Muthupandian Ashokkumar. Mercury removal from aqueous solution using petal-like MoS2 nanosheets[J]. Front. Environ. Sci. Eng., 2021, 15(1): 15-.
[12] Kuo Fang, Fei Peng, Hui Gong, Huanzhen Zhang, Kaijun Wang. Ammonia removal from low-strength municipal wastewater by powdered resin combined with simultaneous recovery as struvite[J]. Front. Environ. Sci. Eng., 2021, 15(1): 8-.
[13] Wenyue Li, Min Chen, Zhaoxiang Zhong, Ming Zhou, Weihong Xing. Hydroxyl radical intensified Cu2O NPs/H2O2 process in ceramic membrane reactor for degradation on DMAc wastewater from polymeric membrane manufacturer[J]. Front. Environ. Sci. Eng., 2020, 14(6): 102-.
[14] Dawei Yu, Jianxing Wang, Libin Zheng, Qianwen Sui, Hui Zhong, Meixue Cheng, Yuansong Wei. Effects of hydraulic retention time on net present value and performance in a membrane bioreactor treating antibiotic production wastewater[J]. Front. Environ. Sci. Eng., 2020, 14(6): 101-.
[15] Kehui Liu, Xiaolu Liang, Chunming Li, Fangming Yu, Yi Li. Nutrient status and pollution levels in five areas around a manganese mine in southern China[J]. Front. Environ. Sci. Eng., 2020, 14(6): 100-.
Viewed
Full text


Abstract

Cited

  Shared   
  Discussed