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This study investigates the oxidation of selected endocrine disrupting compounds (estrone, 17β-estradiol, estriol and 17α-ethinylestradiol) during ozonation and advanced oxidation of biologically treated municipal wastewater effluents in a pilot scale. Selected estrogenic substances were spiked in the treated wastewater at levels ranging from 1.65...
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... Estrogenic activity was removed completely in Ph for ozonation and O 3 /H 2 O 2 (Guedes Maniero, Maia Bila, & Dezotti, 2008). According to a report, various estrogens (E1, E2, E3 and EE2) were degraded in different oxidation processes as (Pešoutová, Stříteský, & Hlavínek, 2014). The clay was used as a catalyst in the ozonation process to degrade EE2 in an aqueous solution. ...
The widespread occurrence and ubiquitous distribution of estrogens, i.e., estrone (E1), estradiol (E2), and estriol (E3) in our water matrices, is an issue of global concern. Public and regulatory authorities are concerned and placing joint efforts to eliminate estrogens and related environmentally hazardous compounds, due to their toxic influences on the environmental matrices, ecology, and human health, even at low concentrations. However, most of the available literature is focused on the occurrence of estrogens in different water environments with limited treatment options. Thus, a detailed review to fully cover the several treatment processes is needed. This review comprehensively and comparatively discusses many physical, chemical, and biological-based treatments to eliminate natural estrogens, i.e., estrone (E1), estradiol (E2), and estriol (E3) and related synthetic estrogens, e.g., 17α-ethinylestradiol (EE2) and other related hazardous compounds. The covered techniques include adsorption, nanofiltration, ultrafiltration, ultrasonication, photocatalysis of estrogenic compounds, Fenton, Fenton-like and photo-Fenton degradation of estrogenic compounds, electro-Fenton degradation of estrogenic compounds, ozonation, and biological methods for the removal of estrogenic compounds are thoroughly discussed with suitable examples. The studies revealed that treatment plants based on chemical and biological approaches are cost-friendly for removing estrogenic pollutants. Further, there is a need to properly monitor and disposal of the usage of estrogenic drugs in humans and animals. Additional studies are required to explore a robust and more advanced oxidation treatment strategy that can contribute effectively to industrial-scale applications. This review may assist future investigations, monitoring, and removing estrogenic compounds from various environmental matrices. In concluding remarks, a way forward and future perspectives focusing on bridging knowledge gaps in estrogenic compounds removal are also proposed.
... Sarkar et al. (2014) andPešoutová et al. (2014) demonstrated that with the use of peroxone (O3 + H2O2), an estrogen removals 293 greater than 98% were achieved, where the elimination rate of estrogens increased to more than 99% when the H2O2 294 concentration in the solution was increased from 20 to 60 mg L -1 . H2O2 is commonly used as a catalyst in ozone catalytic and295 ozone-photocatalytic treatments, but although estrogen removal is comparable to other combinations of AOPs involving O3 296 (greater than 99%), H2O2 in excess can act as an inhibitor of the process (Pešoutová et al. 2014). ...
The presence of estrogens such as estrone (E1), 17β-estradiol (E2), estriol (E3) and 17α-ethinylestradiol (EE2) in the aquatic environments, even in low concentrations, is an ambient concern that needs an appropriate degradation process in wastewater treatment plants. In this study, a systematic review was carried out to identify the most suitable advanced oxidation processes to remove E1, E2, E3 and EE2 from aqueous effluents. A performance parameter (γ) relating electrical consumption, treated volume and, both initial and final estrogen concentrations was proposed. The initial concentration of estrogen, the kind of water (residual or synthetic) and the pH of the system were the more relevant variables to remove those estrogens. Ozonation was the best treatment for estrogen removal due to the lower γ values as 2.95 10 ² , 6.91 10 ³ and 2.38 10 ³ kWh g ⁻¹ for E1, E2 and EE2, respectively in wastewater and 9.40 10 ⁻² kWh g ⁻¹ (E1) and 8.50 10 ⁻² kWh g ⁻¹ (EE2) in synthetic water, all of them with removal higher than 99%. The operational cost estimated of ozonation was USD$ 23.1/1000 m ³ for E1 and E2 treatment in wastewater.
... Furthermore, COD is a parameter typically used in wastewater treatment for process design and evaluation as well as for regulation. The fact that COD is reduced while DOC only changes slightly during ozonation indicates that ozone treatment transforms the structure of organic matter and mainly forms transformation products via direct oxidation (Ekblad et al., 2019;Liu et al., 2015;Pešoutová et al., 2014). For this reason, dose-dependent elimination can be expected after ozonation, as summarized in Fig. 7. Exposure to biological processes simulated by BOD measurement only indicated a slightly greater dose-dependent removal. ...
The present work aimed to study the effect of ozonation on the organic sum parameters linked to enhanced biodegradability. Laboratory experiments were conducted with the effluent of four Austrian urban wastewater treatment plants with low food to microorganism ratios and different matrix characteristics. Biochemical oxygen demand over 5 days (BOD5) was measured before ozonation and after application of different specific ozone doses (Dspec) (0.4, 0.6 and 0.8 g O3/g DOC). Other investigated organic parameters comprised chemical oxygen demand (COD), dissolved organic carbon (DOC), UV absorption at 254 nm (UV254), which are parameters that are applied in routine wastewater analysis. Carbamazepine and benzotriazole were measured as reference micropollutants. The results showed a dose-dependent increase in biological activity after ozonation; this increase was linked to the enhanced biodegradability of substances that are recalcitrant to biodegradation in conventional activated sludge treatment. The highest relative change was determined for BOD5, which already occurred between 0 and 0.4 g O3/g DOC for all samples. Increasing the Dspec to 0.6 and 0.8 g O3/g DOC resulted in a less pronounced increase. DOC was not substantially decreased after ozonation, which was consistent with a low reported degree of mineralization, while partial oxidation led to a quantifiable decrease in COD (7 to 17%). Delta UV254 and the decline in specific UV absorption after ozonation clearly correlated with Dspec. In contrast, for COD and biodegradable DOC (BDOC), a clear dose-response pattern was identified only after exposure to BOD5 measurement. Indications for improved biodegradability were further supported by the rise in the BOD5/COD ratio. The results indicated that subsequent biological processes have a higher degradation potential after ozonation. The further reduction in biodegradable organic carbon emission by the combination of ozonation and biological post treatment represents another step towards sustainable water resource management in addition to micropollutant abatement.
... Similar removal rates of EDCs with concentrations of the same order of magnitude were also reported with the ozonation process in previous studies (Huber et al., 2005;Zhang et al., 2008). Pešoutová et al. carried out a pilot scale study on removals of EDCs in secondary effluents by ozonation, and excellent removal efficiencies are found for estrone (99.8%) and EE (99.7%) with an ozone dose of 4.4 mg/L (Pesoutova et al., 2014). In the pilot system, O 3 /CMF unit has an excellent performance in removing more than 80% of EDCs. ...
... EE has the highest amount among the 5 EDCs, and 91.3% of EE can be removed in O 3 /CMF unit. The high removal efficiency of EE by the ozonation is also reported by Maniero et al. (2008) and Pesoutova et al. (2014). Zhang et al. studied the degradation of EE in the secondary effluent from WWTP, and showed that the initial ozone and natural organic matter concentrations significantly affected its degradation efficiency. ...
This study aims to address organic micropollutants in secondary effluents from municipal wastewater treatment plants (WWTPs) by first identification of micropollutants in different treatment units, and second by evaluating an advanced treatment process for removals of micropollutants. In secondary effluents, 28 types of pharmaceutical and personal care products (PPCPs), 5 types of endocrine disrupting chemicals (EDCs) and 3 types of odorous compounds are detected with total concentrations of 513±57.8 ng/L, 991±36.5 ng/L, 553±48.3 ng/L, respectively. An integrated process consisting of in-situ ozonation, ceramic membrane filtration (CMF) and biological active carbon (BAC) filtration is investigated in a pilot scale (1000 m³/d) for removal of micropollutants in secondary effluents. The total removal efficiencies of PPCPs, EDCs and odorous compounds are 98.5%, 95.4%, and 91.1%, respectively. Removal mechanisms of emerging organic contaminants (EOCs) and odorous compounds are discussed based on their physicochemical properties. The remarkable removal efficiencies of micropollutants by the pilot system is attributed to synergistic effects of combining ozonation, ceramic membrane filtration and BAC filtration. This study provides a cost-effective and robust technology with the capability of treating secondary effluents for reuse applications.
... UV radiation can also be employed to enhance the ozone decomposition by producing highly reactive HO• radicals. The fact that COD is reduced while DOC only changed slightly during the ozonation process indicated that ozone treatment transformed the structure of organic matter and formed transformation products mainly via direct oxidation (Pešoutová et al., 2014). UV photolysis of O 3 in water yields H 2 O 2 , which in turn reacts with UV radiation or O 3 to form HO•. The degradation of less reactive compounds can be enhanced by HO• radicals. ...
... UV photolysis of O 3 in water yields H 2 O 2 , which in turn reacts with UV radiation or O 3 to form HO•. The degradation of less reactive compounds can be enhanced by HO• radicals. As a consequence, the UV/O 3 treatment achieved a much better DOC reduction (Pešoutová et al., 2014). The role of pH is important when conducting homogeneous AOPs, as different AOPs operate optimally at different pH values. ...
Urban wastewater treatment plants (WWTPs) are among the main anthropogenic sources for the release of contaminants of emerging concern (CECs) into the environment, which can result in toxic and adverse effects on aquatic organisms and consequently on humans. Unfortunately, WWTPs are not designed to remove CECs and secondary (e.g., conventional activated sludge process, CAS) and tertiary (such as filtration and disinfection) treatments are not effective in the removal of most CECs entering WWTP. Accordingly, several advanced treatment methods have been investigated for the removal of CECs from wastewater, including consolidated (namely, activated carbon (AC) adsorption, ozonation and membranes) and new (such as advanced oxidation processes (AOPs)) processes/technologies. This review paper gathers the efforts of a group of international experts, members of the NEREUS COST Action ES1403 who for three years have been constructively discussing the state of the art and the best available technologies for the advanced treatment of urban wastewater. In particular, this work critically reviews the papers available in scientific literature on consolidated (ozonation, AC and membranes) and new advanced treatment methods (mainly AOPs) to analyse: (i) their efficiency in the removal of CECs from wastewater, (ii) advantages and drawbacks, (iii) possible obstacles to the application of AOPs, (iv) technological limitations and mid to long-term perspectives for the application of heterogeneous processes, and (v) a technical and economic comparison among the different processes/technologies.
... In this liquid waste, EE2 can be found at a concentration of 5 mgL -1 (Nasuhoglu et al., 2012). The degradation of this compound has garnered attention, and several studies have utilized adsorption Ma et al. 2016), biological (Larcher et al., 2013;Yi et al., 2011) and advanced oxidation processes for this purpose (Solcova et al., 2016;Pešoutová et al., 2014;Pessoa et al., 2014). Among these processes, advanced heterogeneous oxidation processes have been successfully used to remove water pollutants (Padovan and Azevedo, 2015;Gotostos et al., 2014;Miranda et al., 2013). ...
In this study, the photocatalytic oxidation by UV-activated TiO2 was investigated for the degradation of a 15 mgL-1 solution of 17 α-ethinylestradiol (EE2) in an ultra-pure water matrix. The TiO2 adsorption, solution pH and catalyst TiO2 concentration were evaluated. Operating as a batch reactor, the system showed a 90% removal, with a 40-min retention time, a pH value of 8 a TiO2 concentration of 0.1 gL-1, and a rate constant of 0.13 min-1 for this experiment. The adsorption was negligible in 2 h at pH 7. As a continuous-flow reactor, the operation achieved an 87% removal with a TiO2 concentration of 0.025 gL-1 at pH 7. Ultraviolet-C (UVC) photolysis presented a removal of 40% in 2 h at pH 7 with the system operating in batch mode. Operating as a sequencing batch, the reactor showed remarkable efficiency in the removal of EE2 in a short period.
... Thus, to reduce the concentration of surfactants, pharmaceuticals and their metabolites in waste-water effluents, some researchers have reported advanced oxidation processes (AOPs), especially for the removal of pharmaceutical from waste water. [27][28][29][30][31][32][33][34] However, to date, there are not many reports on the effect of surfactants on the oxidative transformations of pharmaceuticals, except where we have reported the influence of cationic [34] and anionic surfactants [35] on the oxidative transformation of norfloxacin. ...
Pollution of the aquatic environment by drugs results not only during their manufacture, but also from the excretion of drug residues and the discharge of expired drugs by households and hospitals. The transformation of ciprofloxacin, one of the leading antibiotic drugs, in the presence of surfactants has been investigated. The results provide a better understanding of how ciprofloxacin degrades in aquatic environments by considering the effect of omnipresent surfactants. AbstractThe kinetics of the oxidative transformation, i.e. oxidative degradation, of ciprofloxacin (CIP) by chloramine-T (CAT) in cationic and anionic micelle media during the water chlorination process was studied spectrophotometrically at 275nm and 298K. The influence of added salts (1-10×10-4moldm-3) and solvent polarity of the medium on the reaction was studied. The orders with respect to substrate CIP and oxidant CAT were found to be first order in each. The variation of acid concentrations showed opposite effects in cationic and anionic micellar aggregates. Liquid chromatography-electrospray ionisation mass spectrometry was used to identify degradation products of CIP, which confirmed the full dealkylation of the piperazine ring in CIP as the major product. The piperazine moiety of CIP is the principal active site for the CAT during oxidation. Activation parameters for the CIP degradation in cationic and anionic micelles were evaluated by studying the reaction at different temperatures, which lent further support to the proposed degradation mechanism for CIP. The rate constants were evaluated to confirm the micellar effect from incorporating sodium dodecyl sulfate and cetyltrimethylammonium bromide in the reaction mixture and the intrinsic reactivity constants were determined in the aqueous as well as in the micellar pseudo-phases as 4.85 and 0.0083.
... Some recent studies are included in Table 6. Though most of the studies showed an enhancement in ozonation in the presence of UV, a recent pilot scale study by Pešoutová et al. (2014) Fig. 2. UV-visible absorbance spectra of E1, E2, E3 and EE2 (left axis) and P25 TiO 2 nanoparticles (right axis), obtained from measurements by the authors. The UV/H 2 O 2 process has proved to be highly effective compared to utilising photolysis or H 2 O 2 alone. ...
... Although the characteristics of the synthetic wastewater prepared tried to be similar to those of real wastewater, there are important variables not accounted with this simplified wastes that can affect the performance of the evaluated technology[16][17][18]. Because of that, there is an increasing number of manuscripts dealing with the evaluation of the treatment of real wastewater spiked with a specific concentration of POP (the pollutant concentration is increased by adding an extra concentration of the compound)[19][20][21][22]. With this background, the aim of this research work is to study the degradation of four pollutants from real wastewater by CDEO (shown inTable 1) paying attention to the nitrogen species formed during the treatment (nitrate, ammonium and chloramines), in order to study the main oxidation mechanisms related to this process and to increase the knowledge about nitrogen speciation during the electrooxidation process. ...
This work describes the oxidation of caffeine, metoprolol, SMX and progesterone in real wastewater in terms of inorganic nitrogen speciation and help clarify the mechanisms that affect inorganic nitrogen species as final products. In synthetic solutions containing ammonium or nitrate ions, it has been confirmed that reduction of nitrates is a very favored process while oxidation of ammonium is negligible. Role of chloride is demonstrated to be important in the formation of chloramines, as well. These results allow the clarification of the production of nitrates as main products of the oxidation of organic chemicals and the occurrence of ammonium and chloramines in the reaction media, as well as the depletion of nitrogen by gaseous nitrogen production. Results are of a great relevance to interpret the mechanisms proposed in the literature for the treatment of organic wastes by conductive diamond electrochemical oxidation.
... ( Pereira et al., 2012 A removal higher than 99.7% was observed for the 3 estrogens. ( Pesoutova et al., 2014 E2, EE2 and E1 were removed respectively by 92%, 95% and 97%, after 2 min. UV/H 2 O 2 was more efficient than UV or H 2 O 2 alone. ...
Although there are no legal discharge limits for micropollutants into the environment, some regulations have been published in the last few years. Recently, a watch list of substances for European Union-wide monitoring was reported in the Decision 2015/495/EU of 20 March 2015. Besides the substances previously recommended to be included by the Directive 39/2013/EU, namely two pharmaceuticals (diclofenac and the synthetic hormone 17-alpha-ethinylestradiol (EE2)) and a natural hormone (17-beta-estradiol (E2)), the first watch list of 10 substances/groups of substances also refers three macrolide antibiotics (azithromycin, clarithromycin and erythromycin), other natural hormone (estrone (E1)), some pesticides (methiocarb, oxadiazon, imidacloprid, thiacloprid, thiamethoxam, clothianidin, acetamiprid and triallate), a UV filter (2-ethylhexyl-4-methoxycinnamate) and an antioxidant (2,6-di-tert-butyl-4-methylphenol) commonly used as food additive. Since little is known about the removal of most of the substances included in the Decision 2015/495/EU, particularly regarding realistic concentrations in aqueous environmental samples, this review aims to: (i) overview the European policy in the water field; (ii) briefly describe the most commonly used conventional and advanced treatment processes to remove micropollutants; (iii) summarize the relevant data published in the last decade, regarding occurrence and removal in aqueous matrices of the 10 substances/groups of substances that were recently included in the first watch list for European Union monitoring (Decision 2015/495/EU); and (iv) highlight the lack of reports concerning some substances of the watch list, the study of un-spiked aquatic matrices and the assessment of transformation by-products.
