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.    2016, Vol. 10 Issue (3) : 491-501    https://doi.org/10.1007/s11783-016-0837-y
RESEARCH ARTICLE
Fate and removal of typical pharmaceutical and personal care products in a wastewater treatment plant from Beijing: a mass balance study
Jie GAO1,2, Jun HUANG1(), Weiwei CHEN1,3, Bin WANG1, Yujue WANG1, Shubo DENG1, Gang YU1
1. State Key Joint Laboratory of Environment Simulation and Pollution Control (SKJLESPC), Beijing Key Laboratory of Emerging Organic Contaminants Control (BKLEOCC), School of Environment, Tsinghua University, Beijing 100084, China
2. Beijing Municipal Solid Waste and Chemical Management Center, Beijing 100084, China
3. Xiamen Urban Planning and Design Institute, Xiamen 361012, China
 Download: PDF(646 KB)   HTML
 Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
Abstract

The fate and removal of pharmaceuticals and personal care products (PPCPs) in wastewater treatment plants (WWTPs) has received great attention during the last decade. Numerous data concerning concentrations in the water phase can be found in the literature, however corresponding data from sludge as well as associated mass balance calculations are very limited. In the present study, the adsorbed and dissolved concentrations of 9 PPCPs were investigated in each unit of a WWTP in Beijing, China. Based on the calculation of mass balance, the relative mass distribution and removal efficiency of each target compound was obtained at each process. The amount of PPCPs entering into the WWTP ranged from 12 g·d1 to 3848 g·d1. Five target compounds (caffeine, chloramphenicol, bezafibrate, clofibric acid, and N,N-diethyl-meta-toluamide) were effectively removed, with rates of 57%–100%. Negative removal efficiencies were obtained for sulpiride, metoprolol, nalidixic acid, and carbamazepine, ranging from -19% to -79%. PPCPs mainly existed in dissolved form (≥92%) in both the raw influent and the final effluent. The sludge cake carried a much lower amount of PPCPs (17 g·d1) compared with the discharged effluent (402 g·d1). In A2/O treatment tanks, the anaerobic and anoxic tanks showed good performance for PPCPs removal, and the amount of adsorbed PPCPs was increased. The results reveal that both the dissolved and the adsorbed phases should be considered when assessing the removal capacity of each A2/O tank.

Keywords PPCPs      A2/O      mass balance      removal efficiency      sludge     
Corresponding Author(s): Jun HUANG   
Online First Date: 16 March 2016    Issue Date: 05 April 2016
 Cite this article:   
Jie GAO,Jun HUANG,Weiwei CHEN, et al. Fate and removal of typical pharmaceutical and personal care products in a wastewater treatment plant from Beijing: a mass balance study[J]. Front. Environ. Sci. Eng., 2016, 10(3): 491-501.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-016-0837-y
https://academic.hep.com.cn/fese/EN/Y2016/V10/I3/491
Fig.1  Schematic diagram of the treatment process and sampling sites
Fig.2  Concentrations (a) and composition profiles (b) of target PPCPs in water samples dissolved phase
Fig.3  Dissolved (a) and adsorbed (b) concentrations of target PPCPs in different types of sludge
PPCPsraw influentprimary effluentanaerobicanoxicoxicsecondary effluentprimary sludgereturn sludgeexcess sludgedigested sludge (in)digested sludge (out)thickened sludgesludge cake
SP9080190396445104412720013
CF38483684316206652173112004
MTP70611362802968316810001
CP552242510200000
NA1214315737210900000
CBZ64671332853579218810000
DEET1040989644129174176723341139
CA31212967591301100000
BZ2635418437110900000
Tab.1  Total mass of PPCPs in each process unit (g·d-1)
Fig.4  Variation of PPCPs dissolved mass in the receiving river with distance from the discharge point
Fig.5  Relative mass distribution of caffeine (a) and DEET (b) in each process unit
PPCPsprimary treatmentsecondary treatmentWWTP b)
anaerobicanoxicoxictotal a)
SP8838-125-33-19
CF5915520100100
MTP11535-112-37-19
CP598475-3509899
NA-26-3616-30-44-79
CBZ-61442-151-39-46
DEET5477-159392
CA33823-743657
BZ-387-8116958
Tab.2  Removal efficiencies of PPCPs in each unit (%)
1 W C Li. Occurrence, sources, and fate of pharmaceuticals in aquatic environment and soil. Environmental Pollution, 2014, 187: 193–201
https://doi.org/10.1016/j.envpol.2014.01.015
2 S Kaplan. Review: pharmacological pollution in water. Critical Reviews in Environmental Science and Technology, 2013, 43(10): 1074–1116
https://doi.org/10.1080/10934529.2011.627036
3 D Wang, Q Sui, S G Lu, W T Zhao, Z F Qiu, Z W Miao, G Yu. Occurrence and removal of six pharmaceuticals and personal care products in a wastewater treatment plant employing anaerobic/anoxic/aerobic and UV processes in Shanghai, China. Environmental Science and Pollution Research International, 2014, 21(6): 4276–4285
https://doi.org/10.1007/s11356-013-2363-9
4 X Chang, M T Meyer, X Liu, Q Zhao, H Chen, J A Chen, Z Qiu, L Yang, J Cao, W Shu. Determination of antibiotics in sewage from hospitals, nursery and slaughter house, wastewater treatment plant and source water in Chongqing region of Three Gorge Reservoir in China. Environmental Pollution, 2010, 158(5): 1444–1450
https://doi.org/10.1016/j.envpol.2009.12.034
5 R Loos, R Carvalho, D C António, S Comero, G Locoro, S Tavazzi, B Paracchini, M Ghiani, T Lettieri, L Blaha, B Jarosova, S Voorspoels, K Servaes, P Haglund, J Fick, R H Lindberg, D Schwesig, B M Gawlik. EU-wide monitoring survey on emerging polar organic contaminants in wastewater treatment plant effluents. Water Research, 2013, 47(17): 6475–6487
https://doi.org/10.1016/j.watres.2013.08.024
6 Q Sui, J Huang, S Deng, G Yu, Q Fan. 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
7 R Loos, G Locoro, S Contini. Occurrence of polar organic contaminants in the dissolved water phase of the Danube River and its major tributaries using SPE-LC-MS2 analysis. Water Research, 2010, 44(7): 2325–2335
https://doi.org/10.1016/j.watres.2009.12.035
8 United States Environmental Protection Agency. Method 1694: Pharmaceuticals and Personal Care Products in Water, So il, Sediment, and Biosolids by HPLC/MS/MS. Washington, 2007.
9 Q Sui, J Huang, S Deng, G Yu. Rapid determination of pharmaceuticals from multiple therapeutic classes in wastewater by solid-phase extraction and ultra-performance liquid chromatography tandem mass spectrometry. Chinese Science Bulletin, 2009, 54(24): 4633–4643
https://doi.org/10.1007/s11434-009-0413-y
10 J Martín, D Camacho-Muñoz, J L Santos, I Aparicio, E Alonso. Simultaneous determination of a selected group of cytostatic drugs in water using high-performance liquid chromatography-triple-quadrupole mass spectrometry. Journal of Separation Science, 2011, 34(22): 3166–3177
https://doi.org/10.1002/jssc.201100461
11 A Y Lin, T H Yu, S K Lateef. Removal of pharmaceuticals in secondary wastewater treatment processes in Taiwan. Journal of Hazardous Materials, 2009, 167(1–3): 1163–1169
https://doi.org/10.1016/j.jhazmat.2009.01.108
12 P Guerra, M Kim, A Shah, M Alaee, S A Smyth. Occurrence and fate of antibiotic, analgesic/anti-inflammatory, and antifungal compounds in five wastewater treatment processes. Science of the Total Environment, 2014, 473–474: 235–243
https://doi.org/10.1016/j.scitotenv.2013.12.008
13 Y Chen, G Yu, Q Cao, H Zhang, Q Lin, Y Hong. Occurrence and environmental implications of pharmaceuticals in Chinese municipal sewage sludge. Chemosphere, 2013, 93(9): 1765–1772
https://doi.org/10.1016/j.chemosphere.2013.06.007
14 M Carballa, F Omil, J M Lema. Calculation methods to perform mass balances of micropollutants in sewage treatment plants. Application to pharmaceutical and personal care products (PPCPs). Environmental Science & Technology, 2007, 41(3): 884–890
https://doi.org/10.1021/es061581g
15 C Miège, J M Choubert, L Ribeiro, M Eusèbe, M Coquery. Fate of pharmaceuticals and personal care products in wastewater treatment plants-conception of a database and first results. Environmental Pollution, 2009, 157(5): 1721–1726
https://doi.org/10.1016/j.envpol.2008.11.045
16 Q Sui, J Huang, S Deng, W Chen, G Yu. Seasonal variation in the occurrence and removal of pharmaceuticals and personal care products in different biological wastewater treatment processes. Environmental Science & Technology, 2011, 45(8): 3341–3348
https://doi.org/10.1021/es200248d
17 J L Conkle, J R White, C D Metcalfe. Reduction of pharmaceutically active compounds by a lagoon wetland wastewater treatment system in Southeast Louisiana. Chemosphere, 2008, 73(11): 1741–1748
https://doi.org/10.1016/j.chemosphere.2008.09.020
18 M J Gómez, M J Martínez Bueno, S Lacorte, A R Fernández-Alba, A Agüera. Pilot survey monitoring pharmaceuticals and related compounds in a sewage treatment plant located on the Mediterranean coast. Chemosphere, 2007, 66(6): 993–1002
https://doi.org/10.1016/j.chemosphere.2006.07.051
19 R A Trenholm, B J Vanderford, J C Holady, D J Rexing, S A Snyder. Broad range analysis of endocrine disruptors and pharmaceuticals using gas chromatography and liquid chromatography tandem mass spectrometry. Chemosphere, 2006, 65(11): 1990–1998
https://doi.org/10.1016/j.chemosphere.2006.07.004
20 N Nakada, T Tanishima, H Shinohara, K Kiri, H Takada. Pharmaceutical chemicals and endocrine disrupters in municipal wastewater in Tokyo and their removal during activated sludge treatment. Water Research, 2006, 40(17): 3297–3303
https://doi.org/10.1016/j.watres.2006.06.039
21 S D Costanzo, A J Watkinson, E J Murby, D W Kolpin, M W Sandstrom. Is there a risk associated with the insect repellent DEET (N,N-diethyl-m-toluamide) commonly found in aquatic environments? Science of the Total Environment, 2007, 384(1–3): 214–220
https://doi.org/10.1016/j.scitotenv.2007.05.036
22 W J Sim, J W Lee, J E Oh. Occurrence and fate of pharmaceuticals in wastewater treatment plants and rivers in Korea. Environmental Pollution, 2010, 158(5): 1938–1947
https://doi.org/10.1016/j.envpol.2009.10.036
23 J Vanderford B , S A Snyder. Analysis of pharmaceuticals in water by isotope dilution liquid chromatography/tandem mass spectrometry. Environmental Science & Technology, 2006, 40(23): 7312–7320
https://doi.org/10.1021/es0613198
24 L Barron, J Tobin, B Paull. Multi-residue determination of pharmaceuticals in sludge and sludge enriched soils using pressurized liquid extraction, solid phase extraction and liquid chromatography with tandem mass spectrometry. Journal of Environmental Monitoring, 2008, 10(3): 353–361
https://doi.org/10.1039/b717453e
25 K McClellan, R U Halden. Pharmaceuticals and personal care products in archived U.S. biosolids from the 2001 EPA National Sewage Sludge Survey. Water Research, 2010, 44(2): 658–668
https://doi.org/10.1016/j.watres.2009.12.032
26 X S Miao, J J Yang, C D Metcalfe. Carbamazepine and its metabolites in wastewater and in biosolids in a municipal wastewater treatment plant. Environmental Science & Technology, 2005, 39(19): 7469–7475
https://doi.org/10.1021/es050261e
27 N Lindqvist, T Tuhkanen, L Kronberg. Occurrence of acidic pharmaceuticals in raw and treated sewages and in receiving waters. Water Research, 2005, 39(11): 2219–2228
https://doi.org/10.1016/j.watres.2005.04.003
28 C Miège, J M Choubert, L Ribeiro, M Eusèbe, M Coquery. Removal efficiency of pharmaceuticals and personal care products with varying wastewater treatment processes and operating conditions-conception of a database and first results. Water Science and Technology, 2008, 57(1): 49–56
https://doi.org/10.2166/wst.2008.823
29 X Zhao, X C Wang, Z L Chen, H Xu, Q F Zhang. Microbial community structure and pharmaceuticals and personal care products removal in a membrane bioreactor seeded with aerobic granular sludge. Applied Microbiology and Biotechnology, 2015, 99(1): 425–433
https://doi.org/10.1007/s00253-014-5984-0
30 J Roberts, A Kumar, J Du, C Hepplewhite, D J Ellis, A G Christy, S G Beavis. 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, 2016, 541: 1625–1637
https://doi.org/10.1016/j.scitotenv.2015.03.145
31 A C Alder, C Schaffner, M Majewsky, J Klasmeier, K Fenner. Fate of b-blocker human pharmaceuticals in surface water: comparison of measured and simulated concentrations in the Glatt Valley Watershed, Switzerland. Water Research, 2010, 44(3): 936–948
https://doi.org/10.1016/j.watres.2009.10.002
32 B D Blair, J P Crago, C J Hedman, R J F Treguer, C Magruder, L S Royer, R D Klaper. Evaluation of a model for the removal of pharmaceuticals, personal care products, and hormones from wastewater. Science of the Total Environment, 2013, 444: 515–521
https://doi.org/10.1016/j.scitotenv.2012.11.103
33 T Alvarino, S Suarez, J M Lema, F Omil. Understanding the removal mechanisms of PPCPs and the influence ofmain technological parameters in anaerobic UASB and aerobic CAS reactors. Journal of Hazardous Materials, 2014, 278: 506–513
https://doi.org/10.1016/j.jhazmat.2014.06.031
[1] FSE-16001-OF-GJ_suppl_1 Download
[1] Hongcan Cui, Ronghua Xu, Zhong Yu, Yuanyuan Yao, Shaoqing Zhang, Fangang Meng. Tank-dependence of the functionality and network differentiation of activated sludge community in a full-scale anaerobic/anoxic/aerobic municipal sewage treatment plant[J]. Front. Environ. Sci. Eng., 2023, 17(3): 36-.
[2] Tingting Zhu, Zhongxian Su, Wenxia Lai, Jiazeng Ding, Yufen Wang, Yingxin Zhao, Yiwen Liu. Evaluating the impact of sulfamethoxazole on hydrogen production during dark anaerobic sludge fermentation[J]. Front. Environ. Sci. Eng., 2023, 17(1): 7-.
[3] Jingyang Luo, Shiyu Fang, Wenxuan Huang, Feng Wang, Le Zhang, Fang Fang, Jiashun Cao, Yang Wu, Dongbo Wang. New insights into different surfactants’ impacts on sludge fermentation: Focusing on the particular metabolic processes and microbial genetic traits[J]. Front. Environ. Sci. Eng., 2022, 16(8): 106-.
[4] Qian Li, Zhaoping Zhong, Haoran Du, Xiang Zheng, Bo Zhang, Baosheng Jin. Co-pyrolysis of sludge and kaolin/zeolite in a rotary kiln: Analysis of stabilizing heavy metals[J]. Front. Environ. Sci. Eng., 2022, 16(7): 85-.
[5] Mengtian Li, Ge Song, Ruiping Liu, Xia Huang, Huijuan Liu. Inactivation and risk control of pathogenic microorganisms in municipal sludge treatment: A review[J]. Front. Environ. Sci. Eng., 2022, 16(6): 70-.
[6] Lihui Gao, Yijun Cao, Lizhang Wang, Shulei Li. A review on sustainable reuse applications of Fenton sludge during wastewater treatment[J]. Front. Environ. Sci. Eng., 2022, 16(6): 77-.
[7] Di Zhang, Rong Hou, Wenbo Wang, He Zhao. Recovery and reuse of floc sludge for high-performance capacitors[J]. Front. Environ. Sci. Eng., 2022, 16(6): 78-.
[8] Zecong Yu, Keke Xiao, Yuwei Zhu, Mei Sun, Sha Liang, Jingping Hu, Huijie Hou, Bingchuan Liu, Jiakuan Yang. Comparison of different valent iron on anaerobic sludge digestion: Focusing on oxidation reduction potential, dissolved organic nitrogen and microbial community[J]. Front. Environ. Sci. Eng., 2022, 16(6): 80-.
[9] Bin Wang, Gang Yu. Emerging contaminant control: From science to action[J]. Front. Environ. Sci. Eng., 2022, 16(6): 81-.
[10] Yun He, Jianyong Liu, Chengyuan Shen, Xuewen Yi, Xiaowei Li, Xin Huang, Kokyo Oh, Guoji Ding. Innovative method of culturing bdelloid rotifers for the application of wastewater biological treatment[J]. Front. Environ. Sci. Eng., 2022, 16(4): 43-.
[11] Tingwei Gao, Kang Xiao, Jiao Zhang, Wenchao Xue, Chunhai Wei, Xiaoping Zhang, Shuai Liang, Xiaomao Wang, Xia Huang. Techno-economic characteristics of wastewater treatment plants retrofitted from the conventional activated sludge process to the membrane bioreactor process[J]. Front. Environ. Sci. Eng., 2022, 16(4): 49-.
[12] Hasti Daraei, Kimia Toolabian, Ian Thompson, Guanglei Qiu. Biotoxicity evaluation of zinc oxide nanoparticles on bacterial performance of activated sludge at COD, nitrogen, and phosphorus reduction[J]. Front. Environ. Sci. Eng., 2022, 16(2): 19-.
[13] Keke Xiao, Zecong Yu, Kangyue Pei, Mei Sun, Yuwei Zhu, Sha Liang, Huijie Hou, Bingchuan Liu, Jingping Hu, Jiakuan Yang. Anaerobic digestion of sludge by different pretreatments: Changes of amino acids and microbial community[J]. Front. Environ. Sci. Eng., 2022, 16(2): 23-.
[14] Lujun Zhao, Jiaming Shao, Li Xiang, Yiping Feng, Zhihua Wang, Fawei Lin. Co-pyrolysis of oil sludge with hydrogen-rich plastics in a vertical stirring reactor: Kinetic analysis, emissions, and products[J]. Front. Environ. Sci. Eng., 2022, 16(10): 135-.
[15] Caihong Huang, Zhurui Tang, Beidou Xi, Wenbing Tan, Wei Guo, Weixia Wu, Caiyun Ma. Environmental effects and risk control of antibiotic resistance genes in the organic solid waste aerobic composting system: A review[J]. Front. Environ. Sci. Eng., 2021, 15(6): 127-.
Viewed
Full text


Abstract

Cited

  Shared   
  Discussed