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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 |
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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·d−1 to 3848 g·d−1. 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·d−1) compared with the discharged effluent (402 g·d−1). 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.
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Keywords
PPCPs
A2/O
mass balance
removal efficiency
sludge
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Corresponding Author(s):
Jun HUANG
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Online First Date: 16 March 2016
Issue Date: 05 April 2016
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|
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
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