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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

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2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2022, Vol. 16 Issue (11) : 148    https://doi.org/10.1007/s11783-022-1583-y
RESEARCH ARTICLE
Effectiveness of tertiary treatment processes in removing different classes of emerging contaminants from domestic wastewater
Olga S. Arvaniti1,2,3, Marilena E. Dasenaki4, Alexandros G. Asimakopoulos5, Niki C. Maragou3, Vasilios G. Samaras1,6, Korina Antoniou7, Georgia Gatidou1, Daniel Mamais7, Constantinos Noutsopoulos7, Zacharias Frontistis8, Nikolaos S. Thomaidis4, Athanasios S. Stasinakis1()
1. Department of Environment, University of the Aegean, Mytilene 81100, Greece
2. Department of Chemical Engineering, University of Patras, Patras 26504, Greece
3. Department of Agricultural Development, Agrofood and Management of Natural Resources, National and Kapodistrian University of Athens, Psachna 34400, Greece
4. Department of Chemistry, National and Kapodistrian University of Athens, Athens 15771, Greece
5. Department of Chemistry, Norwegian University of Science and Technology, Trondheim NO-7491, Norway
6. Core Labs, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia
7. Sanitary Engineering Laboratory, Department of Water Resources and Environmental Engineering, School of Civil Engineering, National Technical University of Athens, Athens 15780, Greece
8. Department of Chemical Engineering, University of Western Macedonia, Kozani 50132, Greece
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Abstract

● 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.

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.

Keywords Micropollutants      Wastewater      PAC      Membranes      UV      Tertiary treatment     
Corresponding Author(s): Athanasios S. Stasinakis   
Issue Date: 06 June 2022
 Cite this article:   
Olga S. Arvaniti,Marilena E. Dasenaki,Alexandros G. Asimakopoulos, et al. Effectiveness of tertiary treatment processes in removing different classes of emerging contaminants from domestic wastewater[J]. Front. Environ. Sci. Eng., 2022, 16(11): 148.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-022-1583-y
https://academic.hep.com.cn/fese/EN/Y2022/V16/I11/148
Class Compound Molecular Formula Μ.W. LogKow* pKa*
PhCs Atenolol (ATEN) C14H22N2O3 266.3 0.16 9.6
Atorvastatin (ATV) C33H35FN2O5 558.3 ? 4.5
Carbamazepin (CBZ) C15H12N2O 236.3 2.45 13.4
Caffeine (CAF) C8H10N4O2 194.2 ?0.07 0.13 / 0.22
Cimetidine (CIM) C10H16N6S 252.3 0.57 6.8
Danofloxacin (DANO) C19H20FN3O3 357.4 0.44 6.04
Diclofenac (DFC) C14H10Cl2NO2Na 318.1 4.60 4.20
Difloxacin (DIF) C21H19F2N3O3 399.4 1.28 4.33 / 9.05
Doxycycline (DC) C22H24N2O8 444.2 ?0.02 4.6
Flumequine (FLU) C14H12FNO3 261.3 2.6 5.4
Lincomycin (LINC) C18H34N2O6S 461.0 0.56 7.6
Methylopredisolone (MEP) C22H30O5 374.5 1.82 13.86
Metronidazol (MTZ) C6H9N3O3 171.2 ?0.02 2.62
Metroprolol (METO) C15H25NO3 267.4 1.88 9.5
Omeprazole (OMP) C17H19N3O3S 345.4 2.23 3.97 / 8.3
Oxolinic acid (OXO) C13H11NO5 261.2 0.94 6.9
Oxytetracycline (OTC) C22H24N2O9 460.4 ?0.90 3.27
Penicilline G (PEN G) C16H18N2O4S 334.4 1.85 2.74 / 12.12
Propanolol (PPL) C16H21NO2 259.3 3.48 9.45
Ranitidine (RAN) C13H22N4O3S 314.4 0.27 2.7 / 8.2
Ronidazole (RZ) C6H8N4O4 200.2 ?0.38 1.2
Tetracycline (TC) C22H24N2O8 444.4 ?1.30 3.3
Tramadol (TRA) C16H25NO2 263.4 2.51 ?
Trimethroprim (TRI) C14H18N4O3 290.3 0.91 7.3
Valsatran (VAL) C24H29N5O3 435.5 3.65 8.15
EDCs Nonylphenol (NP) C15H24O 220.4 4.48 10.28
Triclosan (TCS) C12H7Cl3O2 289.5 4.80 7.9
PFCs Perfluorohexanoic acid (PFHxA) C6HF11O2 314.1 4.37 ?
Perfluoroheptanoic acid (PFHpA) C7HF13O2 364.1 2.80 ?
Perfluorooctanoic acid (PFOA) C8HF15O2 414.1 3.60 2.5
Perfluorononanoic acid (PFNA) C9HF17O2 464.1 4.50 ?
Perfluorooctanesulfonate (PFOS) C8HF17O3S 522.1 4.30 ?3.27
BTRs 1Η-benzotriazole (BTR) C6H5N3 119.1 1.23 8.37
5,6-dimethyl-1H-benzotriazole or xylytriazole (5,6 DMTR or XTR) C8H9N3 147.2 2.06 9.28
1-hydroxybenzotriazole (OHBTR) C6H5N3O 135.1 0.69 7.39
Tolyltriazole (TTR) C7H7N3 133.2 1.89 8.5
BTHs 2-aminobenzothiazole (ABTH) C7H5N2S 150.2 1.89 3.94
Benzothiazole (BTH) C7H5NS 135.2 2.01 1.2
Tab.1  Characteristics of the emerging contaminants (ECs) that were studied in the present research
Class Compound Microfiltration (%) Ultrafiltration (%) Nanofiltration (%) UV (%) PAC (%)
PhCs Atenolol (ATEN) ΝR ΝR ΝR ΝR 55 (15)
Atorvastatin (ATV) 60 (1) 69 (7) 93 (2) 74 (7) 85 (7)
Carbamazepin (CBZ) 17 (16) 23 (9) 15 (13) 11 (18) 55 (11)
Caffeine (CAF) ΝR 2 (12) ΝR ΝR 8 (25)
Cimetidine (CIM) ΝR ΝR 14 (23) 35 (18) 79 (7)
Danofloxacin (DANO) ΝR 8 (20) ΝR ΝR 64 (23)
Diclofenac (DFC) 5 (23) 26 (6) 31 (7) 6 (24) 33 (18)
Difloxacin (DIF) 13 (20) 42 (4) 38 (4) ΝR 75 (9)
Doxycycline (DC) 7 (14) 1 (15) 39 (19) 5 (13) 43 (17)
Flumequine (FLU) 3 (10) 29 (12) 5 (7) 6 (10) 51 (10)
Lincomycin (LINC) 1 (9) 2 (15) 4 (16) 4 (22) 39 (11)
Methylopredisolone (MEP) ΝR 10 (4) ΝR 43 (13) 29 (3)
Metronidazol (MTZ) 8 (9) 10 (9) ΝR ΝR 33 (12)
Metroprolol (METO) ΝR ΝR ΝR ΝR 71 (12)
Omeprazole (OMP) 14 (29) 24 (26) 18 (34) 21 (33) 84 (10)
Oxolinic acid (OXO) ΝR 11 (18) ΝR ΝR 45 (15)
Oxytetracycline (OTC) 10 (16) 40 (27) 63 (16) 12 (15) 62 (11)
Penicilline G (PEN G) 8 (3) 11 (5) ΝR ΝR 17 (11)
Propanolol (PPL) 1 (4) ΝR 30 (27) 9 (31) 94 (2)
Ranitidine (RAN) ΝR ΝR ΝR 6 (26) 74 (11)
Ronidazole (RZ) 10 (8) 13 (7) 11 (7) 7 (9) 48 (9)
Tetracycline (TC) ΝR 10 (12) 25 (13) 28 (15) 36 (15)
Tramadol (TRA) ΝR 5 (9) 4 (11) 3 (15) 35 (11)
Trimethroprim (TRI) ΝR ΝR ΝR ΝR 54 (8)
Valsatran (VAL) 16 (15) 41 (12) 38 (14) 39 (15) 33 (23)
EDCs Nonylphenol (NP) 17 (6) 20 (3) 14 (14) 15 (3) 39 (7)
Triclosan (TCS) ΝR 27 (9) 31 (8) ΝR 44 (20)
PFCs Perfluorohexanoic acid (PFHxA) ΝR ΝR ΝR 13 (0) 17 (5)
Perfluoroheptanoic acid (PFHpA) ΝR ΝR 5 (4) 12 (2) 20 (6)
Perfluorooctanoic acid (PFOA) 5 (4) 9 (1) 15 (4) 15 (6) 18 (4)
Perfluorononanoic acid (PFNA) 15 (7) 27 (4) 34 (4) 14 (7) 13 (7)
Perfluorooctanesulfonate (PFOS) 12 (10) 24 (5) 31 (4) 23 (7) 30 (6)
BTRs 1Η-benzotriazole (BTR) 8 (12) ΝR ΝR 21 (17) 46 (18)
5,6-dimethyl-1H-benzotriazole (5,6 DMTR or XTR) ΝR ΝR 10 (9) ΝR 75 (15)
1-hydroxybenzotriazole (OHBTR) ΝR ΝR ΝR ΝR ΝR
Tolyltriazole (TTR) ΝR ΝR ΝR ΝR 63 (16)
BTHs 2-aminobenzothiazole (ABTH) ΝR ΝR 4 (12) 4 (4) 73 (14)
Benzothiazole (BTH) ΝR ΝR ΝR ΝR 54 (22)
Tab.2  Mean removal (%) of target emerging contaminants during different wastewater tertiary treatment processes
Fig.1  Removal of emerging contaminants with (a) MF followed by UF and (b) MF followed by NF.
Fig.2  Removal of emerging contaminants with MF followed by UV radiation.
Fig.3  Removal of emerging contaminants with MF followed by PAC addition.
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