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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 Envir Sci Eng    2014, Vol. 8 Issue (1) : 62-68    https://doi.org/10.1007/s11783-013-0518-z
RESEARCH ARTICLE
Removal of pharmaceutical and personal care products by sequential ultraviolet and ozonation process in a full-scale wastewater treatment plant
Qian SUI1,2,4, Jun HUANG2, Shuguang LU1, Shubo DENG2, Bin WANG2, Wentao ZHAO3,4, Zhaofu QIU1, Gang YU2()
1. State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai 200237, China; 2. School of Environment, THU – VEOLIA Joint Research Center for Advanced Environmental Technology, Tsinghua University, Beijing 100084, China; 3. State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092, China; 4. State Environmental Protection Key Laboratory of Microorganism Application and Risk Control (MARC), Tsinghua University, Beijing 10084, China
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Abstract

The application of appropriate advanced treatment process in the municipal wastewater treatment plants (WWTPs) has become an important issue considering the elimination of emerging contaminants, such as pharmaceutical and personal care products (PPCPs). In the present study, the removal of 13 PPCPs belonging to different therapeutic classes by the sequential ultraviolet (UV) and ozonation process in a full-scale WWTP in Beijing was investigated over the course of ten months. Most of the target PPCPs were effectively removed, and the median removal efficiencies of individual PPCPs, ranging from -13% to 89%, were dependent on their reaction rate constants with molecular ozone. Noticeable fluctuation in the removal efficiencies of the same PPCPs was observed in different sampling campaigns. Nevertheless, the sequential UV and ozonation process still made a significant contribution to the total elimination of most PPCPs in the full-scale WWTP, by compensating for the poor or fluctuant removal performance of PPCPs by biologic treatment process.

Keywords PPCPs      advanced treatment      ozone      fluctuation      removal contribution     
Corresponding Author(s): YU Gang,Email:yg-den@tsinghua.edu.cn   
Issue Date: 01 February 2014
 Cite this article:   
Qian SUI,Gang YU,Jun HUANG, et al. Removal of pharmaceutical and personal care products by sequential ultraviolet and ozonation process in a full-scale wastewater treatment plant[J]. Front Envir Sci Eng, 2014, 8(1): 62-68.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-013-0518-z
https://academic.hep.com.cn/fese/EN/Y2014/V8/I1/62
Fig.1  Schematic diagram of the treatment process and the sampling sites ( = 58 in total) in the full-scale WWTP
Fig.2  Comparison of PPCP concentrations in grab and 2-h composite samples: (a) MBR effluent; (b) ozonation effluent. Only the PPCPs with concentrations exceeding limit of quantification (LOQ) in at least one sample were shown. RSDs were listed above the column of each PPCP. *** denoted one of the duplicate was below LOQ while the other was above
Fig.3  Removal efficiencies of PPCPs by sequential UV and ozonation process ( = 8) in the full-scale WWTP (as in some sampling campaigns, the concentrations of several PPCPs in the MBR effluents were below LOQ, their removal efficiencies could not be calculated or shown in the Figure)
Fig.4  Median removal efficiencies of target PPCPs plotted against their rate constants for the reaction with molecular ozone [,,-]
Fig.5  Concentration of target PPCPs in the effluent of MBR, UV unit and ozone chamber
Fig.6  Contribution of the sequential UV and ozonation process ( = 8) to the total elimination of PPCPs in the full-scale WWTP
Fig.7  Concentration of DF (a), MA (b) and TP (c) in the MBR effluent, ozone chamber effluent and the corresponding removal contribution of the sequential UV and ozonation process in each month
influent of WWTP a)effluent of A2/O-MBR process
COD b)/(mg·L-1)382-701 (497)12.4-33.6 (16.2)
BOD5c)/(mg·L-1)159-320 (251)<2.0-3.0 (<2.0)
TN d)/(mg·L-1)53.7-73.5 (60.9)7.9-21.5 (12.9)
TP e)/(mg·L-1)6.34-10.30 (7.62)0.04-1.52 (0.13)
NH3-N f)/(mg·L-1)g)0.11-3.45 (0.25)
  Characterization of the influent of the WWTP and effluent of A/O-MBR process
1 Nassef M, Matsumoto S, Seki M, Khalil F, Kang I J, Shimasaki Y, Oshima Y, Honjo T. Acute effects of triclosan, diclofenac and carbamazepine on feeding performance of Japanese medaka fish (Oryzias latipes). Chemosphere , 2010, 80(9): 1095–1100
doi: 10.1016/j.chemosphere.2010.04.073 pmid:20537681
2 Saravanan M, Karthika S, Malarvizhi A, Ramesh M. Ecotoxicological impacts of clofibric acid and diclofenac in common carp (Cyprinus carpio) fingerlings: Hematological, biochemical, ionoregulatory and enzymological responses. Journal of Hazardous Materials , 2011, 195: 188–194
doi: 10.1016/j.jhazmat.2011.08.029 pmid:21885190
3 Luo Y, Xu L, Rysz M, Wang Y, Zhang H, Alvarez P J J. Occurrence and transport of tetracycline, sulfonamide, quinolone, and macrolide antibiotics in the Haihe River Basin, China. Environmental Science & Technology , 2011, 45(5): 1827–1833
doi: 10.1021/es104009s pmid:21309601
4 Yoon Y, Ryu J, Oh J, Choi B G, Snyder S A. Occurrence of endocrine disrupting compounds, pharmaceuticals, and personal care products in the Han River (Seoul, South Korea). Science of the Total Environment , 2010, 408(3): 636–643
doi: 10.1016/j.scitotenv.2009.10.049 pmid:19900699
5 Yang Y, Fu J, Peng H, Hou L, Liu M, Zhou J L. Occurrence and phase distribution of selected pharmaceuticals in the Yangtze Estuary and its coastal zone. Journal of Hazardous Materials , 2011, 190(1-3): 588–596
doi: 10.1016/j.jhazmat.2011.03.092 pmid:21497014
6 Zhou J L, Zhang Z L, Banks E, Grover D, Jiang J Q. Pharmaceutical residues in wastewater treatment works effluents and their impact on receiving river water. Journal of Hazardous Materials , 2009, 166(2-3): 655–661
doi: 10.1016/j.jhazmat.2008.11.070 pmid:19121894
7 Dickenson E R V, Snyder S A, Sedlak D L, Drewes J E. Indicator compounds for assessment of wastewater effluent contributions to flow and water quality. Water Research , 2011, 45(3): 1199–1212
doi: 10.1016/j.watres.2010.11.012 pmid:21144546
8 Huang Q, Yu Y, Tang C, Zhang K, Cui J, Peng X. 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 , 2011, 13(4): 855–863
doi: 10.1039/c1em10015g pmid:21412553
9 Huber M M, Canonica S, Park G Y, von Gunten U. Oxidation of pharmaceuticals during ozonation and advanced oxidation processes. Environmental Science & Technology , 2003, 37(5): 1016–1024
doi: 10.1021/es025896h pmid:12666935
10 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
doi: 10.1016/S0043-1354(02)00570-5 pmid:12697241
11 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 & Technology , 2005, 39(11): 4290–4299
doi: 10.1021/es048396s pmid:15984812
12 Snyder S A, Wert E C, Rexing D J, Zegers R, Drury D D. Ozone oxidation of endocrine disruptors and pharmaceuticals in surface water and wastewater. Ozone Science and Engineering , 2006, 28(6): 445–460
doi: 10.1080/01919510601039726
13 Esplugas S, Bila D M, Krause L G T, Dezotti M. Ozonation and advanced oxidation technologies to remove endocrine disrupting chemicals (EDCs) and pharmaceuticals and personal care products (PPCPs) in water effluents. Journal of Hazardous Materials , 2007, 149(3): 631–642
doi: 10.1016/j.jhazmat.2007.07.073 pmid:17826898
14 Garoma T, Umamaheshwar S K, Mumper A. Removal of sulfadiazine, sulfamethizole, sulfamethoxazole, and sulfathiazole from aqueous solution by ozonation. Chemosphere , 2010, 79(8): 814–820
doi: 10.1016/j.chemosphere.2010.02.060 pmid:20303138
15 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
doi: 10.1016/j.watres.2007.06.038 pmid:17632207
16 Sui Q, Huang J, Deng S B, 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
doi: 10.1016/j.watres.2009.07.010 pmid:19674764
17 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
doi: 10.1016/j.watres.2011.07.026 pmid:21864879
18 Sui Q, Huang J, Deng S B, Chen W W, Yu G. 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
doi: 10.1021/es200248d pmid:21428396
19 Sui Q, Huang J, Deng S B, Yu G. 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
doi: 10.1007/s11434-009-0413-y
20 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
doi: 10.1016/j.watres.2007.04.005 pmid:17524445
21 Schaar H, Clara M, Gans O, Kreuzinger N. Micropollutant removal during biological wastewater treatment and a subsequent ozonation step. Environmental Pollution , 2010, 158(5): 1399–1404
doi: 10.1016/j.envpol.2009.12.038 pmid:20085854
22 Gabet-Giraud V, Miège C, Choubert J M, Ruel S M, Coquery M. Occurrence and removal of estrogens and beta blockers by various processes in wastewater treatment plants. Science of the Total Environment , 2010, 408(19): 4257–4269
doi: 10.1016/j.scitotenv.2010.05.023 pmid:20633734
23 Coelho A D, Sans C, Agüera A, Gómez M J, Esplugas S, Dezotti M. Effects of ozone pre-treatment on diclofenac: intermediates, biodegradability and toxicity assessment. Science of the Total Environment , 2009, 407(11): 3572–3578
doi: 10.1016/j.scitotenv.2009.01.013 pmid:19249077
24 Dodd M C, Buffle M O, Von Gunten U. Oxidation of antibacterial molecules by aqueous ozone: moiety-specific reaction kinetics and application to ozone-based wastewater treatment. Environmental Science & Technology , 2006, 40(6): 1969–1977
doi: 10.1021/es051369x pmid:16570623
25 Javier Benitez F, Acero J L, Real F J, Roldán G. Ozonation of pharmaceutical compounds: rate constants and elimination in various water matrices. Chemosphere , 2009, 77(1): 53–59
doi: 10.1016/j.chemosphere.2009.05.035 pmid:19545885
26 Rosal R, Rodríguez A, Perdigón-Melón J A, Petre A, García-Calvo E, Gómez M J, Agüera A, Fernández-Alba A R. Degradation of caffeine and identification of the transformation products generated by ozonation. Chemosphere , 2009, 74(6): 825–831
doi: 10.1016/j.chemosphere.2008.10.010 pmid:19036403
27 Dantas R F, Sans C, Esplugas S. Ozonation of propranolol: transformation, biodegradability, and toxicity assessment. Journal of Environmental Engineering , 2011, 137(8): 754–759
doi: 10.1061/(ASCE)EE.1943-7870.0000377
28 Yue C, Seth R, Tabe S, Zhao X, Yang P. Systematic investigation of parameters affecting ozonation oxidation of emerging contaminants. Journal-American Water Works Association , 2012, 104(1): 45–46
29 Gagnon C, Lajeunesse A, Cejka P, Gagne F, Hausler R. Degradation of selected acidic and neutral pharmaceutical products in a primary-treated wastewater by disinfection processes. Ozone Science and Engineering , 2008, 30(5): 387–392
doi: 10.1080/01919510802336731
30 Andreozzi R, Raffaele M, Nicklas P. Pharmaceuticals in STP effluents and their solar photodegradation in aquatic environment. Chemosphere , 2003, 50(10): 1319–1330
doi: 10.1016/S0045-6535(02)00769-5 pmid:12586163
31 Eriksson J, Svanfelt J, Kronberg L. A photochemical study of diclofenac and its major transformation products. Photochemistry and Photobiology , 2010, 86(3): 528–532
doi: 10.1111/j.1751-1097.2009.00703.x pmid:20158668
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