Abstract
In this work, 38 different organic emerging contaminants (ECs), belonging to various chemical classes such as pharmaceuticals (PhCs), endocrine-disrupting chemicals (EDCs), benzotriazoles (BTRs), benzothiazoles (BTHs), and perfluorinated compounds (PFCs), were initially identified and quantified in the biologically treated wastewater collected from Athens’ (Greece) Sewage Treatment Plant (STP). Processes already used in existing STPs such as microfiltration (MF), nanofiltration (NF), ultrafiltration (UF), UV radiation, and powdered activated carbon (PAC) were assessed for ECs’ removal, under the conditions that represent their actual application for disinfection or advanced wastewater treatment. The results indicated that MF removed only one out of the 38 ECs and hence it was selected as pretreatment step for the other processes. UV radiation in the studied conditions showed low to moderate removal for 5 out of the 38 ECs. NF showed better results than UF due to the smaller pore sizes of the filtration system. However, this enhancement was observed mainly for 8 compounds originating from the classes of PhCs and PFCs, while the removal of EDCs was not statistically significant. Among the various studied technologies, PAC stands out due to its capability to sufficiently remove most ECs. In particular, removal rates higher than 70% were observed for 9 compounds, 22 were partially removed, while 7 demonstrated low removal rates. Based on our screening experiments, future research should focus on scaling-up PAC in actual conditions, combining PAC with other processes, and conduct a complete economic and environmental assessment of the treatment.
Similar content being viewed by others
References
Ababneh A N, Abu-Dalo M A, Horn C, Hernandez M T (2019). Polarographic determination of benzotriazoles and their sorption behavior on granular activated carbon. International Journal of Environmental Science and Technology, 16(2): 833–842
Acero J L, Benitez F J, Real F J, Teva F (2017). Removal of emerging contaminants from secondary effluents by micellar-enhanced ultrafiltration. Separation and Purification Technology, 181: 123–131
Akhoundi A, Nazif S (2020). Life-cycle assessment of tertiary treatment technologies to treat secondary municipal wastewater for reuse in agricultural irrigation, artificial recharge of groundwater, and industrial usages. Journal of Environmental Engineering, 146(6): 04020031
Arvaniti O S, Asimakopoulos A G, Dasenaki M E, Ventouri E I, Stasinakis A S, Thomaidis N S (2014). Simultaneous determination of eighteen perfluorinated compounds in dissolved and particulate phases of wastewater, and in sewage sludge by liquid chromatography-tandem mass spectrometry. Analytical Methods, 6(5): 1341–1349
Arvaniti O S, Stasinakis A S (2015). Review on the occurrence, fate and removal of perfluorinated compounds during wastewater treatment. Science of the Total Environment, 524–525: 81–92
Arvaniti O S, Ventouri E I, Stasinakis A S, Thomaidis N S (2012). Occurrence of different classes of perfluorinated compounds in Greek wastewater treatment plants and determination of their solid-water distribution coefficients. Journal of Hazardous Materials, 239–240: 24–31
Asimakopoulos A G, Ajibola A, Kannan K, Thomaidis N S (2013). Occurrence and removal efficiencies of benzotriazoles and benzothiazoles in a wastewater treatment plant in Greece. Science of the Total Environment, 452–453: 163–171
Bahnmüller S, Loi C H, Linge K L, Gunten U, Canonica S (2015). Degradation rates of benzotriazoles and benzothiazoles under UV-C irradiation and the advanced oxidation process UV/H2O2. Water Research, 74: 143–154
Bellona C, Drewes J E, Xu P, Amy G (2004). Factors affecting the rejection of organic solutes during NF/RO treatment-a literature review. Water Research, 38(12): 2795–2809
Benítez F J, Real F J, Acero J L, Casas F (2017). Use of ultrafiltration and nanofiltration processes for the elimination of three selected emerging contaminants: Amitriptyline hydrochloride, methyl salicylate and 2-phenoxyethanol. Environment Protection Engineering, 43(3): 125–141
Berg P, Hagmeyer G, Gimbel R (1997). Removal of pesticides and other micropollutants by nanofiltration. Desalination, 113(2–3): 205–208
Bo L, Gao N, Liu J, Gao B (2015). The competitive adsorption of pharmaceuticals on granular activated carbon in secondary effluent. Desalination and Water Treatment, 57(36): 17023–17029
Bolong N, Ismail A F, Salim M R, Matsuura T (2009). A review of the effects of emerging contaminants in wastewater and options for their removal. Desalination, 239(1–3): 229–246
Bourgin M, Beck B, Boehler M, Borowska E, Fleiner J, Salhi E, Teichler R, von Gunten U, Siegrist H, McArdell C S (2018). Evaluation of a full-scale wastewater treatment plant upgraded with ozonation and biological post-treatments: Abatement of micropollutants, formation of transformation products and oxidation by-products. Water Research, 129: 486–498
Buth J M, Ross M R, McNeill K, Arnold W A (2011). Removal and formation of chlorinated triclosan derivatives in wastewater treatment plants using chlorine and UV disinfection. Chemosphere, 84(9): 1238–1243
Carlson J C, Stefan M I, Parnis J M, Metcalfe C D (2015). Direct UV photolysis of selected pharmaceuticals, personal care products and endocrine disruptors in aqueous solution. Water Research, 84: 350–361
Chen J, Zhang P (2006). Photodegradation of perfluorooctanoic acid in water under irradiation of 254 nm and 185 nm light by use of persulfate. Water Science and Technology, 54(11–12): 317–325
Collivignarelli M C, Abbà A, Miino M C, Caccamo F M, Torretta V, Rada E C, Sorlini S (2021). Disinfection of wastewater by uv-based treatment for reuse in a circular economy perspective. Where are we at? International Journal of Environmental Research and Public Health, 18(1): 1–24
Dasenaki M E, Thomaidis N S (2015). Multianalyte method for the determination of pharmaceuticals in wastewater samples using solid-phase extraction and liquid chromatography-tandem mass spectrometry. Analytical and Bioanalytical Chemistry, 407(15): 4229–4245
Deegan A M, Shaik B, Nolan K, Urell K, Oelgemöller M, Tobin J, Morrissey A (2011). Treatment options for wastewater effluents from pharmaceutical companies. International Journal of Environmental Science & Technology, 8(3): 649–666
Deng H (2020). A review on the application of ozonation to NF/RO concentrate for municipal wastewater reclamation. Journal of Hazardous Materials, 391: 122071
Dhangar K, Kumar M (2020). Tricks and tracks in removal of emerging contaminants from the wastewater through hybrid treatment systems: A review. Science of the Total Environment, 738: 140320
Dubey M, Rajpal A, Vellanki B P, Kazmi A A (2022). Occurrence, removal, and mass balance of contaminants of emerging concern in biological nutrient removal-based sewage treatment plants: Role of redox conditions in biotransformation and sorption. Science of the Total Environment, 808: 152131
Dulov A, Dulova N, Trapido M (2013). Photochemical degradation of nonylphenol in aqueous solution: the impact of pH and hydroxyl radical promoters. Journal of Environmental Sciences-China, 25(7): 1326–1330
Eggen R I, Hollender J, Joss A, Schärer M, Stamm C (2014). Reducing the discharge of micropollutants in the aquatic environment: the benefits of upgrading wastewater treatment plants. Environmental Science & Technology, 48(14): 7683–7689
Fatta-Kassinos D, Meric S, Nikolaou A (2011). Pharmaceutical residues in environmental waters and wastewater: current state of knowledge and future research. Analytical and Bioanalytical Chemistry, 399(1): 251–275
Fernandes M J, Paíga P, Silva A, Llaguno C P, Carvalho M, Vázquez F M, Delerue-Matos C (2020). Antibiotics and antidepressants occurrence in surface waters and sediments collected in the north of Portugal. Chemosphere, 239: 124729
Frontistis Z (2019). Degradation of the nonsteroidal anti-inflammatory drug piroxicam from environmental matrices with UV-activated persulfate. Journal of Photochemistry and Photobiology A Chemistry, 378: 17–23
Gago-Ferrero P, Bletsou A A, Damalas D E, Aalizadeh R, Alygizakis N A, Singer H P, Hollender J, Thomaidis N S (2020). Wide-scope target screening of > 2000 emerging contaminants in wastewater samples with UPLC-Q-ToF-HRMS/MS and smart evaluation of its performance through the validation of 195 selected representative analytes. Journal of Hazardous Materials, 387: 121712
García L, Leyva-Díaz J C, Díaz E, Ordóñez S (2021). A review of the adsorption-biological hybrid processes for the abatement of emerging pollutants: Removal efficiencies, physicochemical analysis, and economic evaluation. Science of the Total Environment, 780: 146554
Gil A, Taoufik N, García A M, Korili S A (2018). Comparative removal of emerging contaminants from aqueous solution by adsorption on an activated carbon. Environmental Technology, 40(23): 3017–3030
Hansen M C, Børresen M H, Schlabach M, Cornelissen G (2010). Sorption of perfluorinated compounds from contaminated water to activated carbon. Journal of Soils and Sediments, 10(2): 179–185
Hori H, Hayakawa E, Einaga H, Kutsuna S, Koike K, Ibusuki T, Kiatagawa H, Arakawa R (2004). Decomposition of environmentally persistent perfluorooctanoic acid in water by photochemical approaches. Environmental Science & Technology, 38(22): 6118–6124
Ioannidi A, Frontistis Z, Mantzavinos D (2018). Destruction of propyl paraben by persulfate activated with UV-A light emitting diodes. Journal of Environmental Chemical Engineering, 6(2): 2992–2997
Karpińska J, Kotowska U (2021). New aspects of occurrence and removal of emerging pollutants. Water (Basel), 13(17): 2418
Karthikraj R, Kannan K (2017). Mass loading and removal of benzotriazoles, benzothiazoles, benzophenones, and bisphenols in Indian sewage treatment plants. Chemosphere, 181: 216–223
Kazner C, Lehnberg K, Kovalova L, Wintgens T, Melin T, Hollender J, Dott W (2008). Removal of endocrine disruptors and cytostatics from effluent by nanofiltration in combination with adsorption on powdered activated carbon. Water Science and Technology, 58(8): 1699–1706
Khanzada N K, Farid M U, Kharraz J A, Choi J, Tang C Y, Nghiem L D, Jang A, An A K (2020). Removal of organic micropollutants using advanced membrane-based water and wastewater treatment: A review. Journal of Membrane Science, 598: 117672
Kim I, Yamashita N, Tanaka H (2009). Performance of UV and UV/H2O2 processes for the removal of pharmaceuticals detected in secondary effluent of a sewage treatment plant in Japan. Journal of Hazardous Materials, 166(2–3): 1134–1140
Kovalova L, Knappe D R, Lehnberg K, Kazner C, Hollender J (2013). Removal of highly polar micropollutants from wastewater by powdered activated carbon. Environmental Science and Pollution Research International, 20(6): 3607–3615
Lange C, Kuch B, Metzger J W (2014). Determination of the occurrence and elimination of endocrine disrupting compounds (EDCs) in municipal wastewater treatment plants (WWTP). Computational Water, Energy, and Environmental Engineering, 3(1): 1–7
Lee S H, Cho Y J, Lee M, Lee B D (2019). Detection and treatment methods for perfluorinated compounds in Wastewater Treatment Plants. Applied Sciences (Basel, Switzerland), 9(12): 2500
Lehnberg K, Kovalova L, Kazner C Wintgens T, Schettgen T, Melin T, Hollender J, Dott W (2009). Removal of selected organic micropollutants from WWTP effluent with powdered activated carbon and retention by nanofiltration. In: Kim Y J, ed. Atmospheric and Biological Environmental Monitoring. Dordrecht: Springer, 161–178
Liao C, Kim U J, Kannan K (2018). A review of environmental occurrence, fate, exposure, and toxicity of benzothiazoles. Environmental Science & Technology, 52(9): 5007–5026
Luo Y, Guo W, Ngo H H, Nghiem L D, Hai F I, Zhang J, Liang S, Wang X C (2014). A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment. Science of the Total Environment, 473–474: 619–641
Michael I, Frontistis Z, Fatta-Kassinos D (2013). Removal of pharmaceuticals from environmentally relevant matrices by advanced oxidation processes (AOPs). Comprehensive Analytical Chemistry, 62: 345–407
Michael-Kordatou I, Iacovou M, Frontistis Z, Hapeshi E, Dionysiou D D, Fatta-Kassinos D (2015). Erythromycin oxidation and ERY-resistant Escherichia coli inactivation in urban wastewater by sulfate radical-based oxidation process under UV-C irradiation. Water Research, 85: 346–358
Mohammad A W, Teow Y H, Ang W L, Chung Y T, Oatley-Radcliffe D L, Hilal N (2015). Nanofiltration membranes review: Recent advances and future prospects. Desalination, 356: 226–254
Molé R A, Good C J, Stebel E K, Higgins J F, Pitell S A, Welch A R, Minarik T A, Schoenfuss H L, Edmiston P L (2019). Correlating effluent concentrations and bench-scale experiments to assess the transformation of endocrine active compounds in wastewater by UV or chlorination disinfection. Chemosphere, 226: 565–575
Noutsopoulos C, Mamais D, Mpouras T, Kokkinidou D, Samaras V, Antoniou K, Gioldasi M (2014). The role of activated carbon and disinfection on the removal of endocrine disrupting chemicals and non-steroidal anti-inflammatory drugs from wastewater. Environmental Technology, 35(6): 698–708
Petala A, Mantzavinos D, Frontistis Z (2021). Impact of water matrix on the photocatalytic removal of pharmaceuticals by visible light active materials. Current Opinion in Green and Sustainable Chemistry, 28: 100445
Rivera-Jaimes J A, Postigo C, Melgoza-Alemán R M, Aceña J, Barceló D, López de Alda M (2018). Study of pharmaceuticals in surface and wastewater from Cuernavaca, Morelos, Mexico: Occurrence and environmental risk assessment. Science of the Total Environment, 613–614: 1263–1274
Rodriguez-Narvaez O M, Peralta-Hernandez J M, Goonetilleke A, Bandala E R (2017). Treatment technologies for emerging contaminants in water: A review. Chemical Engineering Journal, 323: 361–380
Samaras V G, Thomaidis N S, Stasinakis A S, Lekkas T D (2011). An analytical method for the simultaneous trace determination of acidic pharmaceuticals and phenolic endocrine disrupting chemicals in wastewater and sewage sludge by gas chromatography-mass spectrometry. Analytical and Bioanalytical Chemistry, 399(7): 2549–2561
Schröder H F, José H J, Gebhardt W, Moreira R F P M, Pinnekamp J (2010). Biological wastewater treatment followed by physicochemical treatment for the removal of fluorinated surfactants. Water Science and Technology, 61(12): 3208–3215
Shon H K, Phuntsho S, Chaudhary D S, Vigneswaran S, Cho J (2013). Nanofiltration for water and wastewater treatment: A mini review. Drinking Water Engineering and Science, 6(1): 47–53
Sivaranjanee R, Kumar P S (2021). A review on remedial measures for effective separation of emerging contaminants from wastewater. Environmental Technology and Innovation, 23: 101741
Son H S, Choi S B, Zoh K D, Khan E (2007). Effects of ultraviolet intensity and wavelength on the photolysis of triclosan. Water Science and Technology, 55(1–2): 209–216
Stasinakis A S, Thomaidis N S, Arvaniti O S, Asimakopoulos A G, Samaras V G, Ajibola A, Mamais D, Lekkas T D (2013). Contribution of primary and secondary treatment on the removal of benzothiazoles, benzotriazoles, endocrine disruptors, pharmaceuticals and perfluorinated compounds in a sewage treatment plant. Science of the Total Environment, 463–464: 1067–1075
Styszko K, Proctor K, Castrignanò E, Kasprzyk-Hordern B (2021). Occurrence of pharmaceutical residues, personal care products, lifestyle chemicals, illicit drugs and metabolites in wastewater and receiving surface waters of Krakow agglomeration in South Poland. Science of the Total Environment, 768: 144360
Tang C Y, Fu Q S, Criddle C S, Leckie J O (2007). Effect of flux (transmembrane pressure) and membrane properties on fouling and rejection of reverse osmosis and nanofiltration membranes treating perfluorooctane sulfonate containing wastewater. Environmental Science & Technology, 41(6): 2008–2014
Tchobanoglous G, Burton F L, Stensel D H (2002). Wastewater Engineering: Treatment Disposal Reuse, 4th ed. Boston, USA: Mc Graw Hill
Thomaidi V S, Stasinakis A S, Borova V L, Thomaidis N S (2015). Is there a risk for the aquatic environment due to the existence of emerging organic contaminants in treated domestic wastewater? Greece as a case-study Journal of Hazardous Materials, 283: 740–747
Vergili I (2013). Application of nanofiltration for the removal of carbamazepine, diclofenac and ibuprofen from drinking water sources. Journal of Environmental Management, 127: 177–187
Wang S, Li L, Yu S, Dong B, Gao N, Wang X (2021). A review of advances in EDCs and PhACs removal by nanofiltration: Mechanisms, impact factors and the influence of organic matter. Chemical Engineering Journal, 406: 126722
Weidauer C, Davis C, Raeke J, Seiwert B, Reemtsma T (2016). Sunlight photolysis of benzotriazoles — Identification of transformation products and pathways. Chemosphere, 154: 416–424
Wilkinson J, Hooda P S, Barker J, Barton S, Swinden J (2017). Occurrence, fate and transformation of emerging contaminants in water: An overarching review of the field. Environmental Pollution, 231(Pt 1): 954–970
Wu B (2019). Membrane-based technology in greywater reclamation: A review. Science of the Total Environment, 656: 184–200
Yamamoto T, Noma Y, Sakai S, Shibata Y (2007). Photodegradation of perfluorooctane sulfonate by UV irradiation in water and alkaline 2-propanol. Environmental Science & Technology, 41(16): 5660–5665
Ye J, Zhou P, Chen Y, Ou H, Liu J, Li C, Li Q (2018). Degradation of 1H-benzotriazole using ultraviolet activating persulfate: Mechanisms, products and toxicological analysis. Chemical Engineering Journal, 334: 1493–1501
Ye X, Guo X, Cui X, Zhang X, Zhang H, Wang M K, Qiu L, Chen S (2012). Occurrence and removal of endocrine-disrupting chemicals in wastewater treatment plants in the Three Gorges Reservoir area, Chongqing, China. Journal of Environmental Monitoring, 14(8): 2204–2211
Yu H W, Park M, Wu S, Lopez I J, Ji W, Scheideler J, Snyder S A (2019). Strategies for selecting indicator compounds to assess attenuation of emerging contaminants during UV advanced oxidation processes. Water Research, 166: 115030
Author information
Authors and Affiliations
Corresponding author
Additional information
Highlights
• Different advanced treatment processes were tested for ECs removal from wastewater.
• UV radiation showed low to moderate removal for 5 of the 38 micropollutants.
• Among tested membrane processes, nanofiltration showed the better performance.
• The use of PAC achieved high or partially removal for 31 out of the 38 compounds.
• The environmental and economical evaluation of a pilot-scale PAC unit is suggested.
Electronic supplementary material
Rights and permissions
About this article
Cite this article
Arvaniti, O.S., Dasenaki, M.E., Asimakopoulos, A.G. et al. Effectiveness of tertiary treatment processes in removing different classes of emerging contaminants from domestic wastewater. Front. Environ. Sci. Eng. 16, 148 (2022). https://doi.org/10.1007/s11783-022-1583-y
Received:
Revised:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11783-022-1583-y