Does micropollutant removal by solar photo‐Fenton reduce ecotoxicity in municipal wastewater? A comprehensive study at pilot scale open reactors

Ibáñez, G. Rivas; Bittner, Michal; Toušová, Zuzana; Campos-Mañas, Marina Celia; Agüera, Ana; López, J.L. Casas; Pérez, J.A. Sánchez; Hilscherová, Klára

doi:10.1002/jctb.5212

Cited by 25 publications

(4 citation statements)

References 39 publications

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“…Additionally, these results confirmed the feasibility of using LED photo-Fenton for the elimination of EDs and indicated that lower wavelengths showed higher effectiveness, yet lower energy uptake (de la Obra et al 2017). Besides, a recent study confirmed the removal of estrogenic activity (< 0.007 ng L −1 of equivalents of estradiol represented as EQ-E2) from wastewater after treatment by modified photo-Fenton at near neutral pH (Rivas Ibáñez et al 2017). Although some studies have already assessed the performance of LED as a radiation source in photo-Fenton aiming at the removal of CECs (Carra et al 2015;de la Obra et al 2017;Davididou et al 2017;Chávez et al 2019), most of these studies are conducted either in synthetic matrixes or in wastewater samples spiked with target contaminants and none of them have yet investigated the impact of LED irradiated photo-Fenton upon estrogenic activity of real municipal wastewater.…”

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confidence: 76%

LED irradiated photo-Fenton for the removal of estrogenic activity and endocrine disruptors from wastewater treatment plant effluent

Silva

Costa

Starling

et al. 2021

Environ Sci Pollut Res

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The goal of this work was to evaluate the performance of the LED irradiated photo-Fenton process on the removal of (i) estrogenic activity and (ii) seven endocrine disruptors (EDs) (4-octylphenol, 4-nonylphenol, bisphenol A, estrone, 17β-estradiol, 17α-ethinylestradiol, and estriol) from real wastewater treatment plant effluent (WWTPE). EDs are a group of contaminants of emerging concern present in WWTPE and which may be recognized by hormone receptors, thus harming animal and human health. The yeast estrogenic screen test (YES) was used to quantify estrogenic activity promoted by EDs in WWTPE samples before and after photo-Fenton treatment. Tests were performed following a factorial design with different iron (20, 40, and 60 mg L −1) and hydrogen peroxide (100, 200, and 300 mg L −1) concentrations in a laboratory scale LED photoreactor (λ = 455 nm, 1.5 L, 1.6 × 10 −6 Einstein s −1). EDs were analyzed by gas chromatography coupled to a mass spectrometer. Control experiments consisted of Fenton process, iron only, LED irradiation only, and H 2 O 2 only. Optimum experimental conditions for LED photo-Fenton resulted in 62% removal of estrogenic activity and 59% mineralization. In addition, treated WWTPE was not toxic to Aliivibrio fischeri and more than 80% of EDs were removed during LED irradiated photo-Fenton. Although Fenton process showed similar efficiency to that obtained by LED photo-Fenton, a higher volume of sludge was generated in the dark. Finally, results obtained in this study confirm the applicability of LED irradiated photo-Fenton process for improving the quality of WWTPE as an alternative to solar photo-Fenton in case solar radiation is not available, thus reducing hazards associated to WWTPE reuse or discharge.

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mentioning

confidence: 76%

LED irradiated photo-Fenton for the removal of estrogenic activity and endocrine disruptors from wastewater treatment plant effluent

Silva

Costa

Starling

et al. 2021

Environ Sci Pollut Res

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“…This work screened 74 OMCs (mainly pharmaceuticals and some of their transformation products (TPs)) due to their frequent identification in UWW effluents. , The analysis was performed with a 1200 LC system (Agilent Technologies, Foster City, CA) with a XDB C18 50 × 4.6 mm and 1.8 μm particle size analytical column (Agilent Technologies, Santa Clara, CA), coupled to a hybrid quadrupole-linear ion trap-mass spectrometer (QqLIT) 5500 QTRAP from Sciex Instruments (Foster City, CA) equipped with a TurboIon Spray source featuring electrospray ionization (ESI), operating in positive (ESI+) and negative (ESI−) modes. The source settings were ionspray voltage, 4500 V; curtain gas, 25 (arbitrary units); GS1, 50 psi; GS2, 40 psi; and temperature, 550 °C.…”

Section: Methodsmentioning

confidence: 99%

“…74 OMCs (pharmaceuticals and some of their transformation products (TPs)) were screened in this work due to their frequent identification in UWW effluents [20][21] aluminium (MiroSun, Alanod, Germany), with a concentration factor of 1, 4.5 m of total irradiated surface, and illuminated water volume is 45L over a total volume of 60L. The flow rate used was 30 L/min.…”

Section: Organic Microcontaminantsmentioning

confidence: 99%

Reclamation of Real Urban Wastewater Using Solar Advanced Oxidation Processes: An Assessment of Microbial Pathogens and 74 Organic Microcontaminants Uptake in Lettuce and Radish

Aguas

Hincapié

Martínez-Piernas

et al. 2019

Environ. Sci. Technol.

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In this study, disinfection of urban wastewater (UWW) with two solar processes (H2O2-20 mg/L, and photo-Fenton 10 mg/L-Fe 2+ /20 mg/L-H2O2 at natural water pH) at pilot scale using a 60L-Compound Parabolic Collector reactor for irrigation of raw-eaten vegetables (lettuce and radish) has been investigated. Several microbial targets (total coliforms, Escherichia coli, Salmonella spp, and Enterococcus spp) naturally occurring in UWW and 74 organic microcontaminants (OMCs) were monitored. Disinfection results showed no significant differences between both processes, showing the following inactivation resistance order: Salmonella spp. < E. coli < total coliforms < Enterococcus spp. Reductions of target microorganisms to concentrations below the limit of detection (LOD) was achieved in all cases with cumulative solar UV (QUV) ranged from 12 to 40 kJ/L (90 min to 5 hours). Solar photo-Fenton showed a reduction of 66% of OMCs and solar/H2O2 of 56% in 4 hours treatment. Irrigation of radish and lettuce with solar treated effluents, secondary effluents and mineral water was performed for 6 and 16 weeks, respectively. The presence of bacteria was monitored in surfaces and uptake of leaves, fruit and also in soil. The bacterial concentrations detected were below the LOD in the 81.2% (lettuce) and the 87.5% (radish) of the total number of samples evaluated. Moreover, uptake of OMCs was reduced above 70% in crops irrigated with solar treated effluents in comparison with secondary effluents of UWW.

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“…The strategy was carried out with an initial dose of 30 mg L -1 H2O2 and fed four iron additions every 5 min to municipal wastewater. Fe-EDDS was used to conquer the problem of iron solubility and achieved similar effects in endocrine removal, as well as phytotoxicity and cytotoxicity (Rivas Ibáñez et al, 2017).…”

Section: Fenton Reagentsmentioning

confidence: 99%

Optimization strategies for efficient dosage of H2O2 in Fenton and photo-Fenton processes

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This Thesis work addresses the challenge of designing hydrogen peroxide (H2O2) dosage Strategies for improving Fenton and photo-Fenton applications. The determination of the H2O2 dosage scheme that minimizes hydrogen peroxide consumption while meeting the specified treatment outcome is crucial for the practicality of Fenton and photo-Fenton processes, as well as for further understanding the effect of the dosage. A first part of the research addresses this challenge by providing a problem formulation, identifying and discussing objectives and constraints, and the nature of the optimal solution. From this point, the Thesis presents a novel dosage model and a consequent methodology aimed at experimentally optimizing the dosage profile along a discretized time horizon following recipe optimization concepts. The approach is parallel to the numerical solution of the model-based optimization problem posed by H2O2. The methodology is validated in the remediation of a Paracetamol (PCT) solution, and the obtained results are assessed and discussed in regard of the evolution of the concentration of hydrogen peroxide, the contaminant (PCT), and Total Organic Carbon (TOC). The concentration of dissolved oxygen (DO), which is also monitored, allows providing a more comprehensive explanation of the nature of the process. A second part focuses on the practical limitations of this scheme by adopting a hybrid methodology between open and closed loop approaches and it is based on three different stages: (i) one-shot initial H2O2 addition (ii) continuous H2O2 dosage until reaching a specific dissolved oxygen (DO) level and (iii) on-off control of H2O2 dosage using DO slope as control variable. The proposed strategy is validated in the remediation of a Paracetamol solution (100 mg L-1) and the results are assessed using H2O2 consumption and mineralization rate and level as performance criteria. The final tuning of the proposed strategy consists of: (i) only 40% of the stoichiometric H2O2 concentration, (ii) continuous feeding of H2O2 until a 4 mg L-1 DO concentration is attained, and (iii) on-off control dosage selecting DO slope set-points in 0.1 and 0.2 mg L-1 1 min-1. The dosage scheme and settings developed in this second part show an improvement of the process performance by ~ 15% with respect to the same H2O2 amount in a single-addition. Finally, the third part generalizes this strategy by expanding its application and exploring and assessing its performance on different water matrix (natural water and distilled water), different contaminant concentrations, and different contaminants (paracetamol and sulfamethazine) and mixtures. Towards this end, a set of assays were planned and executed involving Paracetamol and Sulfamethazine. In particular, assays performed on sulfamethazine presented higher efficiency (mg of TOC removed per mg of H2O2 consumed), which increased 25-35% with respect to the results obtained with only one-shot initial addition. Furthermore, a deeper analysis of the results allowed detecting and assessing the option of a redesign of the dosage scheme by removing the idea of a specific DO set point and directly addressing the control of the DO slope. Hence, this thesis also opens new research lines in regard to increasing the simplicity and robustness of this efficient control strategy of the photo-Fenton process. Aquest treball de tesi aborda el repte de dissenyar estratègies de dosificació de peròxid d'hidrogen (H2O2) per millorar les aplicacions dels processos Fenton i foto-Fenton. La determinació d'una estratègia de dosificació d'H2O2 que en minimitzi el consum mentre s'assoleixen els objectius del tractament especificat és crucial per a l'aplicació pràctica dels processos de Fenton i foto-Fenton, així com per a la millor comprensió de l'efecte de la dosificació. Una primera part de la investigació aborda aquest repte proporcionant una formulació del problema, identificant i discutint objectius i restriccions, i la naturalesa de la solució òptima. A partir d'aquest punt, la tesi presenta un nou model de dosificació i una metodologia derivada que pretén optimitzar experimentalment el perfil de dosificació al llarg d'un horitzó temporal convenientment discretitzat seguint conceptes d'optimització de receptes. L'enfocament és paral·lel a la solució numèrica del problema d'optimització basat en models i la metodologia que se'n deriva es valida en el tractament d'una solució de paracetamol (PCT). Els resultats obtinguts s'avaluen i es discuteixen en relació amb l'evolució de la concentració de peròxid d'hidrogen, el contaminant (PCT) i el carboni orgànic total (TOC). La concentració d'oxigen dissolt (DO), que també es controla, permet donar una explicació més completa de la naturalesa del procés . Una segona part se centra en les limitacions pràctiques d'aquest esquema mitjançant l'adopció d'una metodologia híbrida entre el control en llaç obert i el control en llaç tancat. La metodologia es basa en tres etapes diferents: (i) addició inicial H2O2 inicial (ii) dosificació contínua d'H2O2 fins a arribar a un determinat nivell d'oxigen dissolt (DO) i (iii) control on-off de la dosi d'H2O2 utilitzant el pendent de DO com a variable de control. L'estratègia proposada es valida en el tractament d'una solució de paracetamol (100 mg L-1) i els resultats s'avaluen utilitzant el consum de H2O2 i la taxa i el nivell de mineralització com a criteris de rendiment. L'ajust final de l'estratègia proposada es concreta de la següent manera: (i) només el 40% de la concentració estequiomètrica de H2O2, (ii) alimentació contínua de H2O2 fins a l'assoliment d'una concentració de 4 mg de L-1 DO i (iii) dosificació sota un control on-off seleccionant els valors de pendent de DO entre 0,1 i 0,2 mg L-1 1 min-1. L'esquema de dosificació i la configuració desenvolupats en aquesta segona part mostren una millora del rendiment del procés d'un 15% respecte al que s'obté amb mateixa quantitat de H2O2 en una única addició. Finalment, la tercera part generalitza aquesta estratègia ampliant la seva aplicació, explorant i avaluant el seu rendiment en diferents matrius d'aigua (aigua natural i aigua destil·lada), diferents concentracions de contaminants, diferents contaminants (paracetamol i sulfametazina) i mescles. Amb aquesta finalitat, es van planificar i executar un conjunt d'assajos que van incloure paracetamol i sulfametazina. En particular, els assajos realitzats amb sulfametazina van presentar una eficiència més elevada (mg de TOC eliminats per mg d'H2O2 consumit), que va augmentar entre un 25 i un 35% respecte als resultats obtinguts amb només una única incorporació inicial. A més, una anàlisi més profunda dels resultats va permetre detectar i avaluar l'opció d'un redisseny de l'esquema de dosificació eliminant la idea d'un punt de referència específic de DO i abordant directament el control del pendent de DO. Per tant, aquesta tesi també obre noves línies de recerca per augmentar la simplicitat i robustesa d'aquesta estratègia de control eficient del procés de foto-Fenton.

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Does micropollutant removal by solar photo‐Fenton reduce ecotoxicity in municipal wastewater? A comprehensive study at pilot scale open reactors

Cited by 25 publications

References 39 publications

LED irradiated photo-Fenton for the removal of estrogenic activity and endocrine disruptors from wastewater treatment plant effluent

LED irradiated photo-Fenton for the removal of estrogenic activity and endocrine disruptors from wastewater treatment plant effluent

Reclamation of Real Urban Wastewater Using Solar Advanced Oxidation Processes: An Assessment of Microbial Pathogens and 74 Organic Microcontaminants Uptake in Lettuce and Radish

Optimization strategies for efficient dosage of H2O2 in Fenton and photo-Fenton processes

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