Tesi: "Advanced Oxydation Processes (AOP)"

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Abouzlam, Manhal. "Optimisation d'un procédé de traitement des eaux par ozonation catalytique". Thesis, Poitiers, 2014. http://www.theses.fr/2014POIT2251/document.

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Le principal objectif de la thèse est l'optimisation d'un procédé d'oxydation avancée par la mise en œuvre des outils de l'automatique moderne.Le procédé considéré concerne l'ozonation catalytique utilisé pour traiter les eaux résiduaires industrielles. L'optimisation de ce procédé consiste à contrôler l'abattement des polluants tout en minimisant le coût de fonctionnement du procédé. La mesure en ligne de la concentration en polluant est fournie par l'absorbance, grandeur corrélée à la DCO. Le procédé est alors considéré comme un système à une entrée, la puissance du générateur d'ozone, et deux sorties, l'ozone dans les évents et l'absorbance.L'identification du procédé a mené à l'estimation d'un modèle linéaire pour construire les lois de commande et d'un modèle non-linéaire, de type modèle de Wiener, pour tester les correcteurs en simulation avant les essais expérimentaux.Les trois commandes testées, la commande par modèle interne, la commande optimale et la commande H∞, permettent de rejeter des perturbations sur la concentration en polluant dans les effluents à traiter. Des analyses de stabilité du système bouclé, vis-à-vis de retards sur la commande, ont été menées.Les résultats expérimentaux obtenus ont permis de conclure sur les gains significatifs apportés par ces développements.La méthodologie développée pour cette application peut être étendue à d'autres procédés afin de faciliter le développement industriel des procédés d'oxydation avancée
The main goal of the PhD thesis focuses on the optimization of an advanced oxidation process by implementing the modern control tools.The considered process is a lab-scale pilot of industrial wastewater treatment by catalytic ozonation. The optimization of this process is achieved by controlling the pollutant abatement while minimizing the high operating costs. The online measurement of the pollutant concentration is provided by the absorbance which is correlated with COD. Therefore, the process is considered as a system with one input, the ozone generator power, and two outputs, the ozone gas concentration at the top of the reactor and the absorbance.A linear model of the process was identified. It allowed calculating the control laws. And a nonlinear model, with a so-called Wiener model structure, was also identified to test the controllers in simulation before the experiments.The three control methods applied, the internal model control, the optimal control and the H∞ control, allow rejecting disturbance on the pollutant concentration of the effluent to be treated.The stability of closed-loop system with delayed control input was analyzed.The experimental results show the significant benefits provided by this closed-loop system.The methodology developed for this application can be extended to other processes to facilitate the industrial development of advanced oxidation processes

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Stříteský, Luboš. "Využití oxidačních procesů (AOP) pro odstraňování mikropolutantů". Master's thesis, Vysoké učení technické v Brně. Fakulta stavební, 2013. http://www.nusl.cz/ntk/nusl-226161.

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This thesis deals with advanced oxidation processes (AOPs) and it’s use for removal of micropollutants from wastewater. The first chapter explains the need AOPs, water quality, pollution and substances that are present in the water. Further, the first chapter outlines approach of the current legislation to micropollutants. The second chapter explains the theory and principle of operation of AOPs. This chapter is divided into two sections. The first section describes AOPs, which were tested at selected WWTP. In the second section, there are described some other AOPs. The third chapter is a literature retrieval of AOPs dealing with the removal of micropollutants. This chapter is focused on the removal of hormones by AOPs using ozone-based AOPs. The fourth chapter describes the actual testing of selected AOPs. The chapter describes selected WWTP, pilot-scale AOP unit and test results. In the last chapter there is designed and described full-scale AOP tertiary unit for removing of micropollutants. The last chapter also contains economic analysis of the proposed tertiary unit.

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RAMAKRISHNAN, BALAJI. "TREATMENT OF MTBE CONTAMINATED WATERS USING AIR STRIPPING AND ADVANCED OXIDATION PROCESSES". University of Cincinnati / OhioLINK, 2005. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1131024170.

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Korichi, Noussaiba. "Epuration d'effluents pharmaceutiques par plasmas non thermiques couplés à des procédés catalytiques". Electronic Thesis or Diss., Orléans, 2023. http://www.theses.fr/2023ORLE1057.

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Le travail de cette thèse vise à étudier un procédé hybride pour le traitement de molécules organiques dans l’eau. Il s’agit du procédé Plasma Non Thermique (NTP) couplé à la catalyse hétérogène de type (Fenton-like). Le paracétamol est utilisé comme la molécule modèle pour cette étude. Deux configurations différentes de réacteur plasma de type Décharge à Barrière Diélectrique (DBD) ont été utilisées : (i) un réacteur multipointes-plan en mode statique ; (ii) un réacteur coaxial tubulaire avec écoulement de la solution à traiter. Afin d’évaluer la synergie entre les deux procédés (plasma et catalyse), les traitements ont été appliqués séparément puis couplés. Les effets synergiques du procédé couplé plasma-catalyse ont été démontré en termes de taux de dégradation, de rendement énergétique et également en termes de la minéralisation de polluant, correspondant à une diminution de la charge organique de la solution avec la conversion du carbone organique en carbone inorganique. La première partie du travail réalisée avec le réacteur multipointes-plan a permis d’établir le rôle efficace du couplage plasma-catalyse en comparaison avec le procédé de plasma seul. En effet, en couplage, une minéralisation de 54 % a été atteinte après traitement de 60 minutes et que le rendement énergétique est augmenté d’un facteur de deux, réduisant ainsi le coût du traitement. Les travaux réalisés sur le réacteur coaxial ont permis d’étudier l’effet de nombreux paramètres sur le couplage plasma-catalyse comme la composition du gaz injecté, du débit de gaz et de liquide, la position du catalyseur par rapport à la décharge plasma, etc. Nous avons ainsi pu montrer l’intérêt de travailler dans un gaz riche en oxygène sur les cinétiques de dégradation et de minéralisation ainsi que le rôle de la puissance électrique appliquée sur les mécanismes d’oxydation. Par exemple, il a été possible d’obtenir une minéralisation de 70 % après 90 min de traitement sous air alors que sous O₂/N₂ (80/20 sccm), la minéralisation atteignait 95 %. La stabilité du catalyseur a également été étudiée en termes de minéralisation après plusieurs réutilisations du catalyseur. Nous avons également démontré le rôle du radical hydroxyle (·OH) sur le traitement avec l’utilisation de piégeurs de radicaux. Effectivement, en présence du méthanol, consommateur des radicaux hydroxyles, une diminution de la dégradation de près de de 50 % a été obtenue et aucune minéralisation n’a été observée
The work of this PhD thesis aims at studying a hybrid process for the treatment of organic molecules in water. It consists of the Non Thermal Plasma (NTP) process coupled with heterogeneous catalysis (Fenton-like type). Paracetamol is used as the target molecule for this study. Two different configurations of Dielectric Barrier Discharge (DBD) plasma reactor were used: (i) a multi-needles-to-plane reactor in static mode; (ii) a coaxial tubular reactor with flow of the solution to be treated. In order to evaluate the synergy between the two processes (plasma and catalysis), the treatments were applied separately and then coupled. The synergistic effects of the coupled plasma-catalysis process were demonstrated in terms of degradation rate, energy yield, and also in terms of pollutant mineralization, corresponding to a decrease of the organic molecules load in the solution with the conversion of organic carbon into inorganic carbon. The first part of the work carried out with the multi-needles-to-plane reactor allowed to establish the effective role of the plasma-catalysis coupling in comparison with the plasma process alone. Indeed, in coupling, a mineralization of 54% was reached after the 60 minutes of treatment and the energy yield was increased by a factor of two, thus reducing the cost of treatment. The work carried out on the coaxial reactor allowed us to study the effect of many parameters on plasma-catalysis coupling efficiency such as the composition of the injected gas, the gas and liquid flow rate, the position of the catalyst in relation to the plasma discharge, etc. We were thus able to show the interest of working in an oxygen-rich gas on kinetics of degradation and mineralization as well as the role of applied electrical power on the oxidation mechanisms. As an example, it was possible to obtain a mineralization of 70 % after 90 minutes under air, whereas under O₂/N₂ (80/20 sccm), the mineralization reached 95 %. The stability of the catalyst was also studied in terms of mineralization after several reuses of the catalyst. We also demonstrated the role of the hydroxyl radical (·OH) on the treatment with the use of radical scavengers. Indeed, the presence of methanol, known as a scavenger of hydroxyl radicals, a decrease of the degradation of nearly 50% was obtained and no mineralization was observed

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CIOTTI, CESARE. "Advanced oxidation processes (AOPs) as innovative technology for the remediation of contaminated sites". Doctoral thesis, Università degli Studi di Roma "Tor Vergata", 2008. http://hdl.handle.net/2108/626.

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Il problema della contaminazione dei terreni e delle acque di falda da composti organici biorecalcitranti sta diventando sempre più preoccupante agli occhi della comunità scientifica e dell’opinione pubblica. L’aumento del numero di siti contaminati da tali sostanze sta spingendo alla graduale sostituzione delle tradizionali operazioni di smaltimento in discarica con tecnologie che consentano la bonifica attraverso la riduzione del carico inquinante fino al raggiungimento di concentrazioni residue non pericolose per la salute umana. Tra i possibili processi alternativi, i processi avanzati di ossidazione chimica (AOP) possono costituire una potenziale soluzione a molti casi di contaminazione da composti organici. Se opportunamente progettati, tali sistemi possono condurre alla completa mineralizzazione degli inquinanti o, eventualmente, alla loro trasformazione in molecole più facilmente biodegradabili. Il loro principio operativo è basato sull’ idea di generare un pool di specie ossidanti altamente reattive. I diversi AOP si differenziano solo nel modo in cui tale pool di sostanze viene generato. Una volta prodotte, tali specie sono in grado di reagire efficacemente con i principali inquinanti di interesse ambientale. Inoltre, alcuni AOP sono in grado di trattare efficacemente anche composti adsorbiti sulla superficie del suolo, in quanto le specie radicaliche ne favoriscono il desorbimento rendendole disponibili all’ossidazione in fase acquosa. Le caratteristiche degli AOP li rendono perfettamente idonei come tecnologia di bonifica in-situ. In questa configurazione, si prevede l’iniezione nel sottosuolo della soluzione ossidante senza la necessità di rimuovere il terreno e di estrarre le acque di falda. Il presente studio è stato sviluppato con l’intento di perseguire un duplice obiettivo: da un lato approfondire le conoscenze di base sui meccanismi di azione degli AOP, al fine di sviluppare criteri di progettazione innovativi; dall’altro valutare l’applicabilità di diversi processi AOP a situazioni rappresentative dei siti contaminati tipicamente riscontrati in Italia. Il primo obiettivo è stato perseguito mediante uno studio di base finalizzato ad identificare la relazione tra condizioni operative del processo e formazione di specie radicaliche e non, nei sistemi di ossidazione basati sul reattivo di Fenton, sul processo a persolfato attivato e sul processo di ossidazione basato sugli acidi perossi-organici (perossiacidi). Il secondo obiettivo è stato invece perseguito sviluppando un approccio progettuale incentrato sulla redazione di studi di fattibilità. Tale approccio ha consentito di arrivare, nel caso del processo Fenton, fino alla realizzazione di un intervento di ossidazione chimica in-situ (ISCO) in scala pilota per la bonifica di un sito contaminato da MtBE, mentre nel caso del sistema a persolfato attivato e dei perossiacidi si è limitato alla fase di studio di fattibilità in scala di laboratorio. La progettazione delle diverse fasi sperimentali é stata, ove possibile, effettuata utilizzando il metodo Rotatable Central Composite (RCC), mentre i risultati ottenuti sono stati interpolati mediante opportuni strumenti statistici, come il Metodo delle Superfici di Risposta (RSM) al fine di individuare le relazioni quantitative tra le prestazioni dei processi investigati e le condizioni operative impiegate. La presente tesi è stata scritta dedicando ad ogni tecnologia presa in esame una prima parte bibliografica, nella quale la tecnologia viene introdotta e ne vengono messe in evidenza le caratteristiche, seguita da una seconda parte in Appendice, dove i risultati sperimentali ottenuti vengono mostrati e discussi attraverso una selezione delle pubblicazioni prodotte durante il triennio di svolgimento del dottorato di ricerca, compreso tra il 2004 ed il 2007, e sottomesse a riviste specializzate del settore o presentate nell’ambito di convegni internazionali.
The contamination of soil and groundwater by means of bio-recalcitrant organic compounds, is becoming a matter of concern for scientific community and public opinion. The increase of the number of contaminated sites, is forcing to gradually switch from traditional dump disposal, towards innovative technologies which are capable of reaching the remediation goals, thus reducing the pollutant load to concentrations which are considered harmless for human health. Among the innovative ones, Advanced Oxidation Processes (AOPs) could represent a potential solution to be applied for remediating contamination by bio-recalcitrant organic compounds. Their operative principle is based upon the idea of generating a pool of highly-oxidative species. The AOPs differ only by the way in which this pool is generated. Once formed, these species are capable to effectively react with most of common pollutants such as hydrocarbons, chlorinated solvents, polycyclic aromatic hydrocarbons and polychlorobiphenyls until their complete oxidation to carbon dioxide and water, or at worst their transformation to more bio-degradable products. Moreover, some AOPs are able to effectively tackle sorbed compounds, since oxidative radicals can desorb these compounds from the soil surface, thus allowing their oxidation in aqueous phase. Besides, it is worth pointing out that the AOPs characteristics make them suitable to be applied as in-situ remediation technologies. In this configuration, the oxidant is injected directly into the subsurface without the need of soil excavation or groundwater extraction. The present study has been developed with the intention of achieving a two-fold objective: on the one hand, to better understand the fundamental mechanisms of AOPs, in order to develop innovative criteria for their design; on the other hand, to assess the feasibility of different AOPs to those situations which are somehow representative of the Italian contaminated sites. The first objective was pursued by developing a fundamental study aimed to identify the relationship between the process operating conditions and the formation of radical and non-radical species for Fenton’s process, activated persulfate and peroxy-acid oxidation processes. The second objective was instead pursued by developing, based on the experimental results of the fundamental study, a design approach based on the execution of feasibility studies. In case of Fenton’s process, a pilot-scale In-Situ Chemical Oxidation (ISCO) treatment for the remediation of an MtBE-contaminated site was developed, whereas in the case of activated persulfate and peroxy-acid oxidation technologies a lab-scale feasibility test was carried out. The design of the different experimental phases was performed, as much as possible, by applying the Rotatable Central Composite method (RCC), whereas the relationships between process performance and applied operating conditions was found by handling and interpolating the experimental results by proper statistical tools based on the Response Surface Method (RSM). In this Ph.D. thesis, each tested AOP is first discussed in a bibliographic part, where the process is introduced and its main features are explained, based on the available and updated literature. The main findings obtained in this part and the innovation introduced with respect to the state of the art is also described in this section of the Ph.D. thesis. The details of these results are shown in the second section of the thesis, which consists of four Appendices, where a selection of papers submitted either to international conferences and peer-reviewed journals during my Ph.D. research are included.

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Rani, Rupam. "REMOVAL OF EMERGING CONTAMINANTS FROM AQUEOUS SOLUTION BY OZONE -BASED PROCESSES". Master's thesis, Temple University Libraries, 2013. http://cdm16002.contentdm.oclc.org/cdm/ref/collection/p245801coll10/id/214782.

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Civil Engineering
M.S.Env.E.
The presence of emerging contaminants (ECs) in water and wastewater systems has become a subject of significant concern worldwide. These emerging contaminants are complex organic molecules which potentially affect human health and environment. Conventional wastewater treatment plants are unable to completely remove these contaminants from water and therefore can discharge them into environment. The need to develop effective methods for ECs removal is essential. This study assess the potential of ozone based advanced oxidation processes (AOP) to oxidize number of emerging contaminants. Different combinations of ozone with hydrogen peroxide and sodium persulfate were tested. For this study 1-4, dioxane, perfluorinated compounds (PFCs), N,N-Diethyl-metatoluamide, and three pharmaceuticals sulfamethoxazole, trimethoprim and carbamazepine have been selected. The effect of different process parameters such as chemical dosages, ozone weight percent, ozone flow rates, etc. on destruction of ECs were examined. It was observed that 1, 4-dioxane were persistent to direct ozone reaction, however were easily oxidized by hydroxyl radical. However, ozonation was solely very effective (> 99 %) in removing pharmaceuticals such as sulfamethoxaole, trimethoprim and carbamazepine. It was not very efficient for the removal of perfluorinated compound and N,N-Diethylmeta-toluamide. The operational conditions were optimized for maximum removal of every compound and their influence on the degradation process is discussed.
Temple University--Theses

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Brienza, Monica. "Solar Advanced Oxidation Processes for removing emerging contaminants in wasterwater". Thesis, Perpignan, 2015. http://www.theses.fr/2015PERP0001.

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Les usines de traitement des eaux usées ne sont pas prévues pour traiter les polluants émergeants, substances organiques, tels des résidus de médicament, des produits phytosanitaires ou des hormones. Par conséquent, elles sont la source principale d’émission de micropolluants récalcitrants dans l’environnement. La Directive DCE 2000/60/CE demande un "bon statu chimique et biologique” de tous les plans d'eau d'ici 2015. L’objectif principal de cette thèse de doctorat a été d’adopter une méthode respectueuse de l’environnement pour traiter ces polluants. La méthode choisie est basée sur le processus d’oxydation avancée (POA). Elle se base sur la génération par voie solaire, et in situ, d’espèces radicalisées hautement réactives (HO● et/ou SO4-), en se focalisant sur la photocatalyse hétérogène et homogène. Les performances de l'POA ont été évaluées en comparant les taux de dégradation et/ou reminéralisassions des micropolluants. Ce critère a été complété par l'identification des sous-produits, de ses transformations associés et de mesures de toxicité. A cet effet, des tests standards d'écotoxicité ainsi que d'activité oestrogénique ont été réalisés, par la méthode toxicologique ISO ou par le test spécifique inhérent au contrôle de l’activité oestrogénique des eaux usées. Les technologies basées sur les processus d’oxydation avancée par voie solaire peuvent être des méthodes prometteuses de traitement des eaux usées. Toutes les molécules testées sont systématiquement dégradées, même celles présentes à de basses concentrations. La compatibilité environnementale a systématiquement été améliorée. L’irrigation des cultures en réutilisant des eaux usées devient possible
Wastewater effluents are the major source of micropollutants in the environment. These recalcitrant compounds that can be escape from wastewater treatment plant (WWTP) are called emerging contaminants. It is necessary to improve the efficiency of wastewater treatment plants. In fact, Water Framework Directive required a “good chemical and biological status” of all water bodies until 2015. The major aim of the dissertation was to contribute to improve the evaluation of solar advanced oxidation processes, and more specifically heterogeneous and homogeneous photocatalysis, for removing emerging contaminants from wastewater effluents. In this objective, the efficiency of AOPS was not only evaluated with the degradation and/or mineralization rates of the micropollutants. This necessary criterion was completed with the identification of the by-products and the associated transformation pathways, but also with toxicity measurements. This last point was explored with standard ecotoxicity tests and also estrogenic activity that represent a specific test relevant to characterize an identified risk associated to the discharge of effluents into the environment.All the experimental results obtained during this dissertation tends to demonstrate that solar advanced oxidation processes has the potential to open new feasible remediation strategies for WWTPs effluent tertiary treatment before wastewater reuse in irrigation for instance. All the tested molecules have systematically been degraded, high number of micro-organic pollutants initially presented in a mixture were removed even at very low concentration, environmental compatibility is systematically improved

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Feng, Ling. "Advanced oxidation processes for the removal of residual non-steroidal anti-inflammatory pharmaceuticals from aqueous systems". Thesis, Paris Est, 2013. http://www.theses.fr/2013PEST1109/document.

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La thèse a porté principalement sur la mise en œuvre de procédés d'oxydation avancée permettant l'élimination de trois anti-inflammatoires non stéroïdiens, le kétoprofène, le naproxène et le piroxicam dans l'eau. Ces trois composés sont parmi les médicaments les plus utilisés, dont la présence dans les eaux naturelles présente potentiellement un risque toxicologique. En raison de la faible efficacité d'élimination des produits pharmaceutiques par les stations traditionnels de traitement des eaux usées, les scientifiques se sont mis à la recherche de technologies de traitements efficaces et respectueuses de l'environnement. Les procédés d'oxydation avancée, comme l'ozonation-biofiltration, l'électro-Fenton et l'oxydation anodique peuvent permettre d'atteindre la destruction presque complète des polluants étudiés et de ce fait ils ont suscité un intérêt grandissant au cours des deux dernières décennies. Tout d'abord, ce travail s'intéresse à l'élimination de certains produits pharmaceutiques dans des solutions synthétiques préparées dans l'eau de robinet à l'aide des procédés électro-Fenton et oxydation anodique dans une cellule électrochimique équipée d'une anode de platine ou de diamant dopé au bore et d'une cathode de feutre de carbone. Cette étude a été menée à l'échelle du laboratoire. Les vitesses d'élimination des molécules pharmaceutiques ainsi que le degré de minéralisation des solutions étudiées ont été déterminées sous différentes conditions opératoires. Pendant ce temps, les sous-produits de l'oxidation générés au cours de la minéralisation ont également été identifiés, ce qui nous a permis de proposer les voies d'oxydation possible pour chaque composé pharmaceutique en présence du radical hydroxyl •OH. Enfin, l'évolution de la toxicité au cours des traitements a été suivie en utilisant la méthode Microtox, basée sur l'inhibition de la fluorescence des bactéries Vibrio fischeri. Dans la deuxième partie de ce travail de thèse, les trois anti-inflammatoires non stéroïdiens ont été ajoutés dans une eau déminéralisée ou dans une eau de surface. Ces eaux ont été traitées à l'aide de différentes doses d'ozone; puis le traitement à l'ozone à été combiné à un traitement biologique par biofiltration. Un biofilm biologique déposé à la surface d'un filtre de charbon actif a été utilisé pour déterminer la biodégradabilité des sous-produits d'oxydation formés dans les eaux de surface ozonée. L'identification des intermédiaires formés lors des processus de traitement et des contrôles de toxicité bactérienne ont été menées pour évaluer la voie de dégradation des produits pharmaceutiques et des effets biologiques potentiels, respectivement
The thesis mainly focused on the implementation of advanced oxidation processes for the elimination of three non-steroidal anti-inflammatory drugs-ketoprofen, naproxen and piroxicam in waters. The three compounds are among the most used medicines, whose presence in waters poses a potential ecotoxicological risk. Due to the low pharmaceuticals removal efficiency of traditional wastwater treatement plants, worldwide concerns and calls are raised for efficient and eco-friendly technologies. Advanced oxidation processes, such as ozonation-biofiltration, electro-Fenton and anodic oxidation processes, which attracted a growing interest over the last two decades, could achieve almost complete destruction of the pollutants studied. Firstly, removal of selected pharmaceuticals from tap water was investigated by electrochemical advanced oxidation processes “electro-Fenton” and “anodic oxidation” with Pt or boron-doped diamond anode and carbon felt cathode at lab-scale. Removal rates and minieralization current efficencies under different operatioanl conditions were analysed. Meanwhile, intermediates produced during the mineralization were also identified, which helps to propose plausible oxidation pathway of each compound in presence of •OH. Finally, the evolution of the global toxicity of treated solutions was monitored using Microtox method, based on the fluorescence inhibition of Vibrio fischeri bacteria. In the second part, the three nonsteroidal anti-inflammatory molecules added in organics-free or surface water were treated under varying ozone treatment regimes with the quite well established technology ozone/biofiltration. A bench-scale biological film was employed to determine the biodegradability of chemical intermediates formed in ozonized surface water. Identification of intermediates formed during the processes and bacterial toxicity monitoring were conducted to assess the pharmaceuticals degradation pathway and potential biological effects, respectively

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Hou, Liwei. "Metal oxide synthesis and its application in the heterogeneous catalytic oxidation processes, using H2O2 or peroxydisulfate as oxidant". Thesis, Poitiers, 2013. http://www.theses.fr/2013POIT2271/document.

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Parmi les procédés avancés d'oxydation (AOPs), les procédés de type Fenton (réactif de Fenton: Fe2+/H2O2) et les procédés d'oxydation par le persulfate, sont décrits comme des procédés très performants. Le procédé Fenton est une voie prometteuse et attractive pour le traitement d'une large variété de composés organiques polluants, difficiles à traiter par les voies classiques de dépollution. Au cours du procédé Fenton, des radicaux hydroxyles, molécules à fort pouvoir oxydant capable de réagir avec pratiquement tous types de composés organiques et inorganiques, sont générés. De même, du fait de la structure similaire entre H2O2 et les ions peroxydisulfate, ces derniers peuvent se décomposer en radicaux sulfates (SO4-•), un autre type d'oxydant hautement réactif pouvant réagir avec les composés organiques. Cependant, les procédés Fenton et d'activation du peroxydisulfate classiques présentent plusieurs inconvénients. En effet, la solution doit être acidifiée avant la réaction, et des procédés complexes de purification / séparation sont nécessaires après réaction. Afin de contourner ces inconvénients, le développement de procédés de traitement hétérogènes est proposé pour le traitement de l'eau. Dans cette optique de développement de procédés économes, les oxydes de fer comme la magnétite sont proposés comme remplaçants des sels solubles de fer. Une utilisation de tels matériaux, à l'état solide, présente des avantages indéniables, dont la séparation aisée de l'espèce active après réaction par sédimentation ou filtration. Dans le cadre de ce travail de doctorat, différents types d'oxydes de fer, hématite ou magnétite, ont été synthétisés en milieu liquide ionique. La morphologie, les propriétés structurales, les rapports de surface FeII/FeIII, les surfaces spécifiques, les tailles de domaine cristallin, etc. ont été évaluées. Deux molécules différentes, la tétracycline (TC) et le phenol, couramment utilisées dans l'industrie chimique, ont été sélectionnées comme polluants modèles afin d'évaluer les performances des matériaux préparés pour leur élimination. Une partie importante du travail de doctorat a donc été l'étude des propriétés des matériaux pour l'élimination de polluants organiques par le procédé Fenton hétérogène. Les résultats montrent clairement que les principaux facteurs affectant les performances du procédé sont reliés aux propriétés de la phase active, du fait du caractère surfacique des réactions. La stabilité des systèmes catalytiques préparés est néanmoins une propriété cruciale également étudiée. Le manuscrit de doctorat met donc l'accent sur la conception de matériaux originaux destinés à une utilisation dans les procédés avancés d'oxydation dans l'eau
Fenton reaction (Fenton reagent: (Fe2+/H2O2)) and persulfate oxidation process, as advanced oxidation processes, are powerful oxidations used world around. Fenton reaction has been evidenced to be a promising and attractive treatment method for the degradation of a wide variety of hazardous organic pollutants, which are difficult to be treated using traditional soft treatment technologies. During Fenton process, free hydroxyl radicals (HO•), strong oxidant molecules capable of reacting with practically all types of organic and inorganic compounds, are generated. In the meanwhile, due to the similar structure between H2O2 and peroxydisulfate ions, peroxydisulfate ions can be decomposed to sulfate radicals (SO4-•), another kind of highly active oxidant that can react with organic compounds. However, the classical Fenton or peroxydisulfate activation processes present some disadvantages. Indeed, the solution needed acidification before carrying out the reaction and complex separation processes have to be applied after reaction. To overcome these drawbacks, heterogeneous catalytic oxidation processes were introduced for wastewater treatment. In this line, magnetite was evidenced as potential substituent to soluble iron ions, and it offers significant advantages such as an easy separation after reaction since the active material can be easily recovered by sedimentation or filtration for further used. In this PhD work, iron oxides, hematite and magnetite, were synthesized using an ionic liquid mediated process. The morphology, structural properties, FeII/FeIII surface ratios, specific surface areas (SSA), mean particle diameters, site densities, etc. were evaluated. Two different model pollutants (tetracycline (TC) and phenol), which are widely used chemicals all over the world, were selected to evaluate the performance of the prepared active materials. A significant part of the PhD study was then on the study of heterogeneous Fenton-like reaction for phenol and TC degradation. Experiments showed that the main factors affecting the heterogeneous Fenton-like system are related to the heterogeneous active phase properties, due to the surface reaction nature occurring over iron oxide surface. However, stability of this active phase, with progressive dissolution under reaction, is also a real challenge. This PhD manuscript, focusing on the design of highly active materials for advanced oxidation processes (AOPs), is constituted of five experiment result parts

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Domergue, Lionel. "Étude de la régénération d’adsorbants par oxydation indirecte". Thesis, Rennes 1, 2019. http://www.theses.fr/2019REN1S028.

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Du fait du coût élevé de certains matériaux adsorbants d’intérêt pour le traitement de la micropollution organique, l’étude a porté sur la régénération de matériaux adsorbants de type zéolithes hydrophobes et monolithe de carbone dans le cas de l’adsorption du bisphénol A et du diclofénac comme micropolluants réfractaires. Des procédés d’oxydation avancée impliquant des espèces radicalaires HO• (réaction de Fenton, électro-Fenton) et SO₄• – (activation de persulfate par voie thermique) ont été utilisés pour assurer la régénération des matériaux par désorption et dégradation oxydative des polluants fixés. La production de radicaux HO• au sein de la phase aqueuse circulant au niveau de l’adsorbant n’est pas suffisamment efficace pour sa régénération. Il a donc été envisagé de générer les radicaux au plus près des molécules adsorbées. Au cours de ce travail, une méthode sensible d’analyse par polarographie de H₂O₂ a été développée et validée pour le suivi des expériences avec les procédés mettant en jeu la réaction de Fenton. Pour différentes zéolithes, le catalyseur de la réaction de Fenton à base de fer a été incorporé préalablement dans la zéolithe. Pour le monolithe de carbone, les propriétés de conduction du matériau ont été mises à profit en l’utilisant comme cathode pour l’application du procédé électro-Fenton permettant de produire les radicaux HO• directement au sein du matériau. Cela a conduit à améliorer les performances de la régénération avec toutefois une diminution de son efficacité au cours de cycles successifs adsorption/régénération
The elimination of organic micropollutants often requires the use of adsorption processes among the water treatments. The aim of our study is to regenerate two expensive materials (hydrophobic zeolites and carbon monoliths) to increase their life expectancy and decrease their investing cost. Two organic contaminants were targeted : diclofenac and bisphenol A, which are refractory pollutants. Advanced oxidation processes involve radical species, HO• (Fenton and electro-Fenton reactions) and SO₄• – (thermal activation of persulfate ion). These oxidants were used to decompose the adsorbed pollutants and thus regenerate the adsorbents. The HO• production, within the core of aqueous phase, did not reach satisfactory regeneration, and a loss of adsorption capacity was observed. Furthermore, during this study, a sensitive polarographic analytical method was developed and validated for the quantification of H₂O₂ in the aqueous phase. This method was used to follow in situ the Fenton reaction. The location of the catalyst in a closer vicinity of the adsorbed species was then optimized and the iron catalyst was impregnated in the host, prior to the adsorption, on different types of hydrophobic zeolites. Concerning carbon monolith, the electro-Fenton process was carried out using the material as the cathode thanks to its electrical conductivity. Consequently, HO• are produced in the porosity of monolith. This latter property enhanced the degradation of adsorbed solutes. The overall performances were increased compared to the homogeneous Fenton process. Nonetheless, a decrease of the adsorption capacities with adsorption-regeneration cycles was observed

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Yang, Weilu. "Electrochemical advanced oxidation processes for emerging organic contaminants removal with graphene-based modified carbon felt electrode". Thesis, Paris Est, 2019. http://www.theses.fr/2019PESC2025.

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Grâce au développement continu de technologies d'analyse environnementale, certains produits chimiques, qui sont reconnus être nocif, ont récemment attiré l'attention, puisqu'ils constituent un menace pour l'environnement et la santé publique.Parmi ces polluants émergent, les produits pharmaceutiques et de soins personnels (PPSP)sont devenus le cibles dela recherche internationale. La chine est le plus grand producteur et le marché des médicaments dans le monde. Avec le développement de l'économie sociale et l'amélioration du niveau de vie de la population, de la production et de l'utilisation de divers PPSP présents en chine augmente rapidement. Par comparaison avec les polluants classiques, ces contaminants émergents sont généralement difficiles à analyser en raison de la limitation de technologies analytiques et de sa faible concentration dans les eaux naturelles.Les usines traditionnelles de traitement des eaux usées ne peuvent pas éliminer efficacement ces produits. La recherche sur l'évaluation des risques et le contrôle des nouveaux contaminants émergents, en chine constitue actuellement un grand défi. Il est donc essentiel de renforcer la recherche sur l'évaluation des risques pour l'environnement et les technologies de traitement efficaces pour éliminer ces polluants émergents. Les procédés d'oxydation avancée (POA) constituent une technologie de traitement efficace et ont été largement utilisés dans le traitement des polluants organiques réfractaires tels que les la destruction des contaminants émergents en milieu aqueux à cause de leur forte pouvoir d'oxydation permettant une minéralisation in situ des polluants. Le graphite, comme un nouveau type de matériau carbone adsorbant, est devenue un matériau d'électrode pour le traitement de la pollution due à son excellente conductivité et surface spécifique très élevée. Toutefois, son application dans les AOPs n'a pas été largement étudié et le mécanisme d'oxydation n'a pas été expliquée de manière systématique. Par conséquent, ce travail présent une étude détaillée sur le rôle des électrodes graphite modifiées dans les procédés électrochimiques d'oxydation avancée (PEOA) avec la préparation électrochimique des électrodes modifiées au graphène par exfoliation, et leur application dans le PEOA "électro-Fenton" (EF) pour le traitement des contaminants émergents. Ainsi le cathode en feutre de carbone modifiée au graphène a permis de d'éliminer différents contaminants émergents sans utilisation d'ions ferreux (catalyseur du procédé électro-Fenton) car les radicaux hydroxyles sont générés à travers d'un procédure catalytique grâce à la dopage du graphène à l'azote. Ensuite les cinétiques de dégradation et de minéralisation ainsi que les mécanismes d'oxydation de différents contaminants émergents ont été explorées
In recent years, with the continuous development of environmental analysis technologies, some chemicals, which have long been recognized but recently attracted attention, have been continuously entering the environment and threatening human health and ecological environment. The emergence of these new pollutants have attracted wide attention. Among them, pharmaceuticals and personal care products (PPCPs) have become international research hotspots. China is the largest medicine producer and market in the world. With the development of social economy and the improvement of people's living standards, the production and use of various PPCPs in China are increasing rapidly. Compared with the traditional pollutants, the new emerging contaminants are generally difficult to be analyzed due to the limitation of analytical technologies and its low concentration in water. The traditional sewage treatment plants can not achieve efficient degradation and removal effects. The research on risk assessment and control of new emerging contaminants in China is still a big challenge. It is necessary to strengthen the research on potential environmental risk assessment and efficient treatment technology. Advanced oxidation processes (AOPs), as an efficient pollutant treatment technology, has been widely used in the treatment of refractory organic pollutants such as new emerging contaminants in water because of its strong oxidation ability, which can effectively degrade and mineralize pollutants in water. Graphene, as a new type of carbon material, has become an efficient adsorbent and catalyst for pollution treatment due to its excellent conductivity and high specific surface area. However, its application in AOPs has not been widely reported and its mechanism has not been systematically explained. Based on this, this paper studied the role of graphene modified electrodes in electrochemical advanced oxidation processes (EAOPs) with the preparation of graphene by electrochemical exfoliation, application of graphene modified electrodes to electrochemical Fenton (EF) process for the degradation of new emerging contaminants; the construction of in-situ iron-free EAOPs with cathodes modified with nitrogen-doped graphene for abatement of new emerging contaminants and the mechanism of highly efficient catalysis with nitrogen-doped graphene have been explored

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Cabrera-Codony, Alba. "Siloxane removal in the energy recovery of biogas: sequential adsorption/oxidation processes". Doctoral thesis, Universitat de Girona, 2016. http://hdl.handle.net/10803/399731.

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The thesis deals with removal of organosilicon compounds in the energy recovery of biogas. Alternative adsorbents for the siloxane removal were studied, and the physical and chemical mechanisms involved in the siloxane adsorption were discovered, which improved the yield of the adsorption and regeneration technologies using both activated carbons and zeolites. Moreover, several technologies based on advanced oxidation processes have been applied in order to regenerate and reuse the exhausted adsorbents. The thesis studies the siloxane removal at lab-scale close to real scenario conditions, including the competitive adsorption with compounds usually found in biogas, in the presence of humidity and with the same gas matrix, which allowed to select the most efficient materials for this purpose. Therefore, the knowledge reported in the thesis dissertation is directly transferable to field application to upgrade the siloxane removal system
Aquesta tesi estudia l'eliminació de compostos volàtis de silici (siloxans) per la recuperació energètica del biogàs. Es van estudiar diferents adsorbents per l'adsorció de siloxans, determinants les propietats físico-químiques superficials que en condicionen l'eficiència, permetent millorar el rendiment de l'adsorció i permetent la regeneració en carbons actius i zeolites esgotats. La tesi estudia l'eliminació de siloxans a escala de laboratori en condicions properes a les reals del biogàs, incloent l'adosrció competitiva amb altres compostos orgànics volàtics, en presència d'humitat i amb diferents matrius gasoses, la qual cosa va permetre seleccionar els materials òptims per aquest propòsit.Per tant el coneixement derivat d'aquesta tesi és directament transferible per tal de millorar els sistemes d'eliminació siloxanes

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Andrade, Juliano de Almeida. "Otimização da reação de fenton visando aplicações na remediação in-situ e ex-situ de aguas subterraneas". [s.n.], 2005. http://repositorio.unicamp.br/jspui/handle/REPOSIP/249632.

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Orientador: Wilson de Figueiredo Jardim
Dissertação (mestrado) - Universidade Estadual de Campinas, Instituto de Quimica
Made available in DSpace on 2018-08-05T10:39:52Z (GMT). No. of bitstreams: 1 Andrade_JulianodeAlmeida_M.pdf: 3254677 bytes, checksum: 72d1e108844df115bda11c77f7fd1337 (MD5) Previous issue date: 2005
Mestrado
Quimica Analitica
Mestre em Química

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Liu, Fuzhen. "Remediation of soil contaminated by organic pollutants using Tween 80 and electrochemical advanced oxidation processes". Thesis, Paris Est, 2020. http://www.theses.fr/2020PESC2055.

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Sous la direction du professeur Mehmet Oturan et du professeur Hui Zhang, j’ai fini toutes les parties des thèses. Un article a été publié dans SCI et les autres parties sont prêtes à se soumettre à la revue. Maintenant, je modifie les papiers et les thèses. Les difficultés sont la détection des contaminants parce qu’il a besoin de la machine de fluorescence et de la méthode d’extraction complexe
Soil contaminated by petroleum-hydrocarbons is a serious environmental problem since it is toxic to agriculture and human. And the polycyclic aromatic hydrocarbons (PAHs) in petroleum-hydrocarbons possess carcinogenicity, teratogenicity, mutagenicity, low volatility and poor solubility properties. Moreover, PAHs are persistent in soil and difficult to be degraded. Hence, effective methods are essential to remedy soil contaminated by petroleum-hydrocarbons and particularly the PAHs. Among various remediation methods, soil washing (SW) combined with surfactant is a promising techniques since it is an economical and effective approach. This technology promotes the transformation of contaminants from soil to aqueous solution, which is especially applied for heavily contaminated soil. However, a soil washing solution highly loaded with surfactant and contaminants is produced. Therefore, effective treatment of soil washing solution is a challenge for promoting the application of surfactants and the remediation of contaminated soil. The combination of soil washing process and electrochemical advanced oxidation processes (EAOPs) constitutes an effective technique for the treatment of soil washing solution. In this paper, Tween 80 was applied as surfactant during soil washing process. The lipophilic part of Tween 80 tends to contaminants or soil particles and the hydrophilic part has tendency to the aqueous phase. Thus, Tween 80 promotes the transformation of hydrophobic organic contaminants from soil to aqueous phase. Then the soil washing solution highly loaded with contaminants and surfactant was treated by EAOPs, processes based on the generation of strong oxidant species such as hydroxyl radicals (•OH), sulfate radicals (SO4•−) and active chlorine (•Cl), are one of the most efficient methods for degrading refractory organic pollutants in soil washing solution. The effect of EAOPs including electro-oxidation (EO), electro-Fenton (EF), sulfate radical-based advanced oxidation processes (AOPs) was investigated in the degradation of petroleum-hydrocarbons. Besides, a potential advanced oxidation process including the presence of chlorine s was applied for treating soil washing solution which contains polycyclic aromatic hydrocarbons (PAHs) and Tween 80

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Wu, Yanlin. "Application of Fe(III)-EDDS complex in advanced oxidation processes : 4-ter-butylphenol degradation". Thesis, Clermont-Ferrand 2, 2014. http://www.theses.fr/2014CLF22455/document.

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Dans cette étude, un nouveau complexe de fer est utilisé dans des processus d’oxydation avancée pour la dégradation de polluants organiques présents dans l’eau. Le fer ferrique (Fe(III)) et l’acide éthylène diamine-N,N’-disuccinique (EDDS) forment un complexe Fe(III)-EDDS dont la structure a été mise en évidence durant ce travail. Les propriétés photochimiques du complexe ont ensuite été évaluées en fonction de différents paramètres physico-chimiques dont le pH qui est apparu comme un paramètre clé pour l’efficacité des processus testés. Ensuite nous avons donc travaillé sur l’utilisation de ce complexe dans les processus de Fenton modifié, photo-Fenton et comme activateur des persulfates (S2O82-). Nos expériences ont été réalisées en présence du 4-tert-butylphénol (4-t-BP) qui est connu pour être un perturbateur endocrinien. Nous avons ensuite mis en évidence les conditions optimales du traitement pour la dégradation du 4-t-BP. Il est apparu que le pH joue un rôle très important et qu’en présence de ce complexe de fer, l’efficacité est plus importante pour des pH neutre ou légèrement basique. L’identification des radicaux oxydants responsables de la dégradation du polluant a également été réalisée. Dans ce cadre nous avons montré que le radical sulfate joue un rôle plus important que le radical hydroxyle lors du processus d’activation des persulfates
Advanced Oxidation Processes (AOPs) have been proved to be successfully applied in the treatment of sewage. It can decolorize the wastewater, reduce the toxicity of pollutants, convert the pollutants to be a biodegradable by-product and achieve the completed mineralization of the organic pollutants. The Fenton technologies which are performed by iron-activated hydrogen peroxide (H2O2) to produce hydroxyl radical (HO•) has been widely investigated in the past few decades. Recently, Sulfate radical (SO4•-) which was produced by the activation of persulfate (S2O82-) is applied to the degradation of organic pollutants in water and soil. It is a new technology recently developed. It is also believed to be one of the most promising advanced oxidation technologies.In this study, a new iron complex is introduced to the traditional Fenton reaction. The ferric iron (Fe(III)) and Ethylene diamine-N,N′-disuccinic acid (EDDS) formed the complex named Fe(III)-EDDS. It can overcome the main disadvantage of traditional Fenton technology, which is the fact that traditional Fenton technology can only perform high efficiency in acidic condition. Simultaneously, EDDS is biodegradable and it is one of the best environment-friendly complexing agents. On the other hand, the transition metal is able to activate S2O82- to generate SO4•-. Therefore, Fe(III)-EDDS will also be applied to activate S2O82- in the present study. 4-tert-Butylphenol (4-t-BP) has been chosen as a target pollutant in this study. It is widely used as a chemical raw material and is classified as endocrine disrupting chemicals due to the estrogenic effects. The 4-t-BP degradation rate (R4-t-BP) is used to indicate the efficiency of the advanced oxidation processes which are based on Fe(III)-EDDS utilization. The main contents and conclusions of this research are shown as follows:In the first part, the chemical structure and properties of Fe(III)-EDDS and the 4-t-BP degradation efficiency in UV/Fe(III)-EDDS system were studied. The results showed that Fe(III)-EDDS was a stable complex which was formed by the Fe(III) and EDDS with the molar ratio 1:1. From the photoredox process of Fe(III)-EDDS, the formation of hydroxyl radical was confirmed including that HO• is the main species responsible for the degradation of 4-t-BP in aqueous solution. Ferrous ion (Fe(II)) was also formed during the reaction. With the increasing Fe(III)-EDDS concentration, 4-t-BP degradation rate increased but is inhibited when the Fe(III)-EDDS concentration was too high. Indeed, Fe(III)-EDDS is the scavenger of HO•. pH value had a significant effect on the degradation efficiency of 4-t-BP that was enhanced under neutral or alkaline conditions. On the one hand, Fe(III)-EDDS presented in the FeL-, Fe(OH)L2-, Fe(OH)2L3-, Fe(OH)4- four different forms under different pH conditions and they had different sensitivity to the UV light. On the other hand, pH value affected the cycle between Fe(III) and Fe(II ). The formation of hydroperoxy radicals (HO2•) and superoxide radical anions (O2•-) (pka = 4.88) as a function of pH was also one of the reasons. It was observed that O2 was an important parameter affecting the efficiency of this process. This effect of O2 is mainly due to its important role during the oxidation of the first radical formed on the pollutant. (...)

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Mousset, Emmanuel. "Integrated processes for removal of persistent organic pollutants : soil washing and electrochemical advanced oxidation processes combined to a possible biological post-treatment". Thesis, Paris Est, 2013. http://www.theses.fr/2013PEST1130/document.

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Les sols contaminés par les polluants organiques hydrophobes tels que les Hydrocarbures Aromatiques Polycycliques (HAPs) constituent un problème majeur puisqu'ils sont difficilement éliminés et leurs impacts toxicologiques restent significatifs. Comme alternative aux procédés thermiques et physiques traditionnels, les procédés de lavages de sol in situ et ex situ apparaissent être une solution envisageable et efficace et particulièrement pour les fortes pollutions. Cependant, le traitement des solutions fortement chargées de lavages de sol est une autre barrière à surmonter. Une nouvelle approche combinée est proposée pour répondre à ce problème: les procédés de lavages de sol in situ/ex situ combinés à un Procédé Electrochimique d'Oxydation Avancée Electrochimique (PEOA) avec possibilité de recirculer l'effluent (pour réutiliser l'agent extractant) et/ou de combiner avec un post-traitement biologique (pour minimiser le coût énergétique).L'efficacité d'extraction de l'agent extractant tel que l'hydroxypropyl-beta-cyclodextrine (HPCD) est comparé au traditionnel tensioactif non-ionique dénommé Tween 80, dans les solutions synthétiques et réelles de lavages de sol. Une nouvelle méthode sensible d'analyse du Tween 80, basée sur la fluorescence, est développée pour suivre l'oxydation du Tween 80. Deux PEOAs sont comparés : l'électro-Fenton (EF) et l'oxydation anodique (OA). Les anodes de platine (Pt) (dans le procédé EF) et de diamant dopés au bore (BDD) (dans les deux procédés) sont respectivement utilisées pour étudier la recirculation des effluents et la possibilité d'une combinaison avec un post-traitement biologique. Concernant la réutilisation des agents extractants, l'évolution de la biodégradabilité des solutions et l'énergie consommée (en kWh (kg COT)-1) pendant les PEAOs testés, l'HPCD est trouvée être plus avantageuse que le Tween 80. En revanche, en terme d'efficacité d'extraction, de coût des agents extractants et d'impact sur la respirométrie du sol, le Tween 80 paraît être plus avantageux. En prenant en compte tous ces avantages et inconvénients, le Tween 80 pourrait être retenu comme la meilleure solution
Soils contaminated by hydrophobic organic pollutants like polycyclic aromatic hydrocarbons (PAHs) are a common concern since they are extremely difficult to remove and their potential toxicological impacts are significant. As an alternative to traditional thermal or physical treatments, soil washing and soil flushing processes appear to be conceivable and efficient approaches, especially for higher level of pollution. However, the treatment of highly loaded soil washing/flushing solutions is another challenge to overcome. In that way, a new integrated approach is suggested: soil washing/flushing processes combined to an electrochemical advanced oxidation process (EAOP) in a combination with a recirculation loop (to save extracting agents) and/or a biological post-treatment step (to minimize energy cost).Extraction efficiency of the extracting agent like hydroxypropyl-beta-cyclodextrin (HPCD) is compared to the traditional non-ionic surfactant Tween 80 in synthetic and real soil washing solutions. A new simple fluorescent sensitive and selective quantification method is developed to monitor Tween 80 oxidation. Two EAOPs were compared: electro-Fenton (EF) and anodic oxidation (AO). Platinum (Pt) (in EF process) and boron doped diamond (BDD) (in both treatment) anodes are the respective electrodes employed to recycle effluents and to consider a biological post-treatment, respectively. Regarding the extracting agent recovery, the biodegradability evolution of effluent and the energy consumption (in kWh (kgTOC)-1) during EAOP, HPCD is more advantageous than Tween 80. However, in terms of extraction efficiency, costs of extracting agents and impact on soil respirometry, Tween 80 is much more efficient. By considering all these advantages and drawbacks, Tween 80 could still appear to be the best option

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Matysíková, Jana. "Znovu-užití vyčištěných odpadních vod v papírenském a textilním průmyslu". Master's thesis, Vysoké učení technické v Brně. Fakulta stavební, 2012. http://www.nusl.cz/ntk/nusl-225374.

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This thesis deals with Advanced oxidation processes (AOP) and its aplication for textile wastewaters treatment and reuse. AOP is a modern technology which currently recieves increased attention due to it´s high efficiency in removing resistant and hardly-degradable pollution. Thesis consists of search and practical part. Search part is created by three chapters. First chapter describe briefly wastewater reuse. The second chapter deals with Advanced oxidation processes. AOP principle, AOP division and descriotion is included with the strong focus on the ozonation technology. The third chapter presents the textile industry and its wastewaters. The practical part of this thesis consists of two chapters. Chapter 5 describes testing of textile wastewaters decoloration by ozonation in the selected textile copany and its results. This results are used in chapter 6. Chapter 6 is the study of textile industry treatment and reuse in the selected textile company. This study contains the design of two options for wastewater treatment and reuse in the textile processes.

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Olvera, Vargas Hugo. "Study on the fate of pharmaceuticals in aqueous media : synthesis, characterization and detection of biotic and abiotic transformation products using electrochemical advanced oxidation processes and bioconversions". Electronic Thesis or Diss., Paris Est, 2014. http://www.theses.fr/2014PEST1179.

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La pollution des eaux superficielles et souterraines par des composés organiques est bien connue comme une préoccupation majeure de l'environnement dans de nombreux pays. Si les polluants prioritaires sont actuellement surveillés par la directive cadre européenne sur l'eau, il est désormais urgent de prendre en considération les nouveaux polluants dérivés de principes actifs des produits pharmaceutiques et d'identifier leurs produits de transformation à risque. Ce travail de thèse propose une étude globale sur l'état et l'avenir des produis pharmaceutiques dans l'environnement, sur l'exemple de deux pharmaceutiques choisis, dans le cadre de cette importante problématique environnementale. Nous avons donc appliqué les procédés électrochimiques d'oxydation avancée, électro-Fenton (EF), oxydation anodique(OA) et photoélectro-Fenton solaire (PEFS), ainsi que le couplage électro-Fenton/traitement biologique pour une élimination effective des polluants médicamenteux furosémide et ranitidine. Les résultats obtenus confirment l'efficacité de ces technologies électrochimiques pour la minéralisation quasi-totale des produits pharmaceutiques étudiés. En outre, l'utilisation du pré-traitement par EF suivi d'un procédé biologique confirme la capacité de l'EF de transformer les polluants organiques en produits biodégradables qui peuvent être consommés par des microorganismes lors d'un traitement biologique, démontrant ainsi l'applicabilité potentiel de cette technique combinée, en termes d'une consommation énergétique réduite. L'identification des produits de transformation (PTs) des pharmaceutiques étudiés par voie électrochimique (électro-oxydation) et biologique (bioconversion) a été effectuée par différentes techniques d'analyse physico-chimiques. La biotransformation du FRSM a conduit à la formation de trois PT principales; saluamide, pyridinium et un dérivé céto-alcool. Les deux premiers ont aussi été détectés lors du traitement électrochimique, ce qui suggère la probabilité de les trouver dans l'environnement comme les produits de transformation les plus plausibles par des différentes conditions de dégradation. Les tests de toxicité basés sur l'inhibition de la bioluminescence des bactéries marines Vibrio fischeri ont montré que certains PT formés lors de traitement électrochimiques sont plus toxique que la molécule mère, car une augmentation de la toxicité globale de la solution a été observée au début des électrolyses. Néanmoins, la toxicité de la solution est complètement éliminée à la fin des traitements électrochimiques, ce qui indique l'efficacité de ces technologies aussi pour la détoxification des solutions des médicaments traités. Par conséquent, cette étude constitue une contribution importante à l'évaluation des risques environnementaux des produits pharmaceutiques
The present project contributes with valuable data for a better fundamental understanding on the fate of pharmaceutical residues in the environment, dealing with the main challenges concerning this increasingly worrying environmental issue. The used Electrochemical Advanced Oxidation Processes (EAOPs), electro-Fenton (EF) and anodic oxidation (AO), showed to be a very efficient alternative for the mineralization of acid solutions of the pharmaceuticals RNTD and FRSM, attaining almost complete mineralization of the drugs after 6h of electrolysis. A comparative study on the mineralization of RNTD solutions by EF and SPEF processes in a 2.5 L capacity pre-pilot flow plant demonstrates the higher oxidation capacity of SPEF, achieving very good mineralization rates, thus evidencing the potentiality of this technology at greater scale for the treatment of wastewaters containing pharmaceutical products. The application of an EF pre-treatment coupled with a biological process for the degradation of both drugs was conducted. EF pre-pretreatment was capable of enhancing the solution biodegradability envisaging a biological treatment, which efficiently removed the short-chain carboxylic acids that had been formerly generated during the pre-applied electrolysis. In this way, the combination of both processes was confirmed as a very promising technology for the treatment of pharmaceuticals-containing wastewater. Several transformation products (TPs) were detected and identified during the electrochemical oxidation of the studied drugs. Toxicity tests based on the bioluminescence of the marine bacteria V. fischeri. evidenced the toxicity some of these oxidation by-products, since the toxicity of the solution increased on the first stages of the electrolysis. However, the abatement of the toxicity in the final stages of the electrochemical treatments, demonstrated the effectiveness of these technologies for both the mineralization and detoxification of the RNTD and FRSM solutions. The use of the fungi Cunninghanella echinulate for the bioconversion of FRSM led to the formation of three main bio-transofrmation products: the previously identified saluamide and pyridinium, and the new detected keto-alcohol derivate. These TPs were generated by both, biological and electrochemical approches, evidencing their high probability to be found in environmental compartments as the most likely TPs of FRSM by different oxidation conditions. This study is thus presented as a very useful alternative for the assessment of the fate of pharmaceutical residues in the environment

19

Oliveira, Clélia Aparecida da Silva 1972. "Tratamento de corante têxtil por eletrólise, fotólise e fotocatálise utilizando LED UV = Treatment of textile dye by electrolytic, photolytic and photocatalytic processes". [s.n.], 2013. http://repositorio.unicamp.br/jspui/handle/REPOSIP/267750.

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Orientador: Peterson Bueno de Moraes
Dissertação (mestrado) - Universidade Estadual de Campinas, Faculdade de Tecnologia
Made available in DSpace on 2018-08-23T06:55:03Z (GMT). No. of bitstreams: 1 Oliveira_CleliaAparecidadaSilva_M.pdf: 1434373 bytes, checksum: 2411a1ce9b13fbe4e8f7d778c6dfd3ea (MD5) Previous issue date: 2013
Resumo: A indústria têxtil gera elevados volumes de efluentes com alta carga orgânica e compostos recalcitrantes, os quais são tratados por sistemas baseados em processos físicos, químicos e biológicos convencionais. Entretanto, o caráter não destrutivo dos tratamentos convencionais representa um sério problema no setor. Nos últimos 20 anos, os Processos Oxidativos Avançados (POA) têm estado em evidência devido à sua capacidade em degradar inúmeros compostos orgânicos contidos em águas e efluentes. Uma grande quantidade de trabalhos utilizando luz UV a partir de lâmpadas de vapor de mercúrio tem resultado em elevada eficiência de degradação de substratos recalcitrantes incluindo efluentes têxteis; entretanto, demandam elevado consumo de energia elétrica, encarecendo o tratamento. Em contrapartida, o surgimento de Diodos Emissores de Luz Ultravioleta (LED UV) abre novas fronteiras de aplicação no campo de tratamento de águas residuárias, quanto a custo, operacionalidade e tamanho dos sistemas. Nesse trabalho estudou-se a degradação de um efluente têxtil simulado contendo o corante Remazol Azul Brilhante (C.I. Reactive Blue 19) através de processos eletroquímicos e fotoeletroquímicos que utilizam LED UV, utilizando-se dois reatores: um operando em batelada contendo o fotocatalisador TiO2 e o outro, em fluxo, contendo um cátodo (tela cilíndrica de aço-inoxidável), um tubo de quartzo contendo os LED UV e o Anodo Dimensionalmente Estável (ADE 70%TiO2/30%RuO2). Os resultados demonstraram que, no reator de bancada, a eficiência de remoção de cor foi de 100% para concentração inicial de 50 mg L-1 do corante, em 24 horas de tratamento. No reator em fluxo, utilizando Na2SO4 como eletrólito, o processo eletrolítico resultou em eficiência de 65%; o fotoeletrocatalítico, em 68%, operando a 750 L h-1 e em 57,3 mA cm-2. Quando foi utilizado o eletrólito NaCl, obteve-se remoção de 100% da cor em 5 minutos de tratamento a 750 L h-1, independente da concentração inicial do corante utilizada (50 mg L-1 ou 100 mg L-1), da concentração do eletrólito (0,05 M ou 0,1 M), da densidade de corrente (14,3 mA cm-2 , 28,7 mA cm-2 ou 57,3 mA cm-2) e do processo utilizado
Abstract: The textile industry generates large amount of wastewater containing significant organic load and recalcitrant compounds, which in most cases are treated by conventional systems involving physical, chemical and biological processes, the latter represented mainly by activated-sludge treatment. However, the non-destructive profile of conventional treatments is a serious problem for textile-based industry. Over the past 20 years, the study of Advanced Oxidation Processes (AOP) has been carried out due to its high capacity degradation of numerous organic pollutants contained in waters and wastewaters. Research using UV light from mercury vapor lamps usually has resulted in high efficiency degradation of recalcitrant substrates including textile effluents but requires high electrical power consumption besides other drawbacks. In contrast, the emergence of Ultraviolet Light Emitting Diodes (UV LED) opens new perspectives for application on wastewater treatment, concerning efficiency, footprint and costs of the systems. In this work we studied the degradation of a simulated wastewater containing a textile dye, Remazol Brilliant Blue (C.I. Reactive Blue 19) through electrochemical and photoelectrochemical processes using UV LED as ultraviolet radiation source. The experimental apparatus consisted of two systems: the first, a bench-scale reactor containing TiO2 photocatalyst (P25 DEGUSSA) in solution, and another pilot-scale system operated in batch recirculation mode composed of an tubular stainless-steel screen cathode, a quartz tube containing the UV LED and a oxide-coated titanium anode (DSA©30%TiO2/70%RuO2). The results showed total decolorization of a solution containing 50 mg L-1 of RB in 24-hour treatment in the bench-scale reactor. Tests on flow reactor using Na2SO4 as supporting electrolyte resulted in 65% of color removal using electrolytic process and 68% for photoelectrocatalytic process operating at 750 L h-1 and 57.3 mA cm-2. In experiments using the electrolyte NaCl it was obtained 100% in the color degradation within 5 minutes of treatment at 750 L h-1, regardless of the: initial concentration of dye used (50 mg L-1; 100 mg L-1), concentration of the electrolyte (0.05 M; 0.1 M) and current density value (14.3; 28.7; 57.3 mA cm-2)
Mestrado
Tecnologia e Inovação
Mestra em Tecnologia

20

Pirgalioglu, Saltuk. "Catalytic Ozonation Of Dye Solutions In A Semi-batch Reactor". Master's thesis, METU, 2008. http://etd.lib.metu.edu.tr/upload/3/12610158/index.pdf.

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Treatment of textile wastewaters containing dye materials using the conventional methods based on biological treatment is not possible. In order to overcome this problem, ozonation based on the oxidation of organic pollutants with ozone gas dissolved in aqueous phase have been studied widely. Catalytic ozonation and advanced oxidation processes (AOP) are also used in order to increase the efficiency of sole ozonation In this work, catalytic ozonation processes in the presence of Copper Sulfide (CuS) powder and a synthesized catalyst by the impregnation of iron on alumina (Fe/Al2O3) were studied separately in the treatment of dye solutions, namely Remazol Brilliant Blue-R (RBBR) and Reactive Black-5 (RB-5). Besides catalytic ozonation runs, ozonation parameters and ozonation mechanism were also studied and a model was developed for the semi-batch ozonation. Both catalysts increased the oxidation of side products measured by the decrease in the amount of total organic carbon (TOC) in the treated dye solutions. Dye removal rates were also enhanced in the treatment of RB-5 dye solutions while no significant effect was observed on dye removal rates of RBBR solutions. TOC removals above 90% were observed in the catalytic ozonation using CuS for both of the dye solutions at pH =10 having initial dye concentration of 100 mg/L. The most significant effect of the catalyst addition was observed at pH = 3 where the TOC removals of non-catalytic ozonation were the lowest. CuS addition increased percent TOC removal at the end of the reaction period of 80 min by 123% in the treatment of 100 mg/L RBBR solution, and by 65% in the treatment of 100 mg/L RB-5 solution at pH = 3. On the other hand, addition of Fe/Al2O3 catalyst increased TOC removal of 100 mg/L RB-5 solution by 52 % at pH = 3. In addition, volumetric mass transfer coefficients (kLa) of ozone in the absence and in the presence of a chemical reaction between dye and ozone were estimated from modeling. A correlation for the enhancement factor of ozone absorbed into dye solutions in terms of initial dye concentration was obtained and reported.

21

Olvera, Vargas Hugo. "Study on the fate of pharmaceuticals in aqueous media : synthesis, characterization and detection of biotic and abiotic transformation products using electrochemical advanced oxidation processes and bioconversions". Thesis, Paris Est, 2014. http://www.theses.fr/2014PEST1179/document.

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La pollution des eaux superficielles et souterraines par des composés organiques est bien connue comme une préoccupation majeure de l'environnement dans de nombreux pays. Si les polluants prioritaires sont actuellement surveillés par la directive cadre européenne sur l'eau, il est désormais urgent de prendre en considération les nouveaux polluants dérivés de principes actifs des produits pharmaceutiques et d'identifier leurs produits de transformation à risque. Ce travail de thèse propose une étude globale sur l'état et l'avenir des produis pharmaceutiques dans l'environnement, sur l'exemple de deux pharmaceutiques choisis, dans le cadre de cette importante problématique environnementale. Nous avons donc appliqué les procédés électrochimiques d'oxydation avancée, électro-Fenton (EF), oxydation anodique(OA) et photoélectro-Fenton solaire (PEFS), ainsi que le couplage électro-Fenton/traitement biologique pour une élimination effective des polluants médicamenteux furosémide et ranitidine. Les résultats obtenus confirment l'efficacité de ces technologies électrochimiques pour la minéralisation quasi-totale des produits pharmaceutiques étudiés. En outre, l'utilisation du pré-traitement par EF suivi d'un procédé biologique confirme la capacité de l'EF de transformer les polluants organiques en produits biodégradables qui peuvent être consommés par des microorganismes lors d'un traitement biologique, démontrant ainsi l'applicabilité potentiel de cette technique combinée, en termes d'une consommation énergétique réduite. L'identification des produits de transformation (PTs) des pharmaceutiques étudiés par voie électrochimique (électro-oxydation) et biologique (bioconversion) a été effectuée par différentes techniques d'analyse physico-chimiques. La biotransformation du FRSM a conduit à la formation de trois PT principales; saluamide, pyridinium et un dérivé céto-alcool. Les deux premiers ont aussi été détectés lors du traitement électrochimique, ce qui suggère la probabilité de les trouver dans l'environnement comme les produits de transformation les plus plausibles par des différentes conditions de dégradation. Les tests de toxicité basés sur l'inhibition de la bioluminescence des bactéries marines Vibrio fischeri ont montré que certains PT formés lors de traitement électrochimiques sont plus toxique que la molécule mère, car une augmentation de la toxicité globale de la solution a été observée au début des électrolyses. Néanmoins, la toxicité de la solution est complètement éliminée à la fin des traitements électrochimiques, ce qui indique l'efficacité de ces technologies aussi pour la détoxification des solutions des médicaments traités. Par conséquent, cette étude constitue une contribution importante à l'évaluation des risques environnementaux des produits pharmaceutiques
The present project contributes with valuable data for a better fundamental understanding on the fate of pharmaceutical residues in the environment, dealing with the main challenges concerning this increasingly worrying environmental issue. The used Electrochemical Advanced Oxidation Processes (EAOPs), electro-Fenton (EF) and anodic oxidation (AO), showed to be a very efficient alternative for the mineralization of acid solutions of the pharmaceuticals RNTD and FRSM, attaining almost complete mineralization of the drugs after 6h of electrolysis. A comparative study on the mineralization of RNTD solutions by EF and SPEF processes in a 2.5 L capacity pre-pilot flow plant demonstrates the higher oxidation capacity of SPEF, achieving very good mineralization rates, thus evidencing the potentiality of this technology at greater scale for the treatment of wastewaters containing pharmaceutical products. The application of an EF pre-treatment coupled with a biological process for the degradation of both drugs was conducted. EF pre-pretreatment was capable of enhancing the solution biodegradability envisaging a biological treatment, which efficiently removed the short-chain carboxylic acids that had been formerly generated during the pre-applied electrolysis. In this way, the combination of both processes was confirmed as a very promising technology for the treatment of pharmaceuticals-containing wastewater. Several transformation products (TPs) were detected and identified during the electrochemical oxidation of the studied drugs. Toxicity tests based on the bioluminescence of the marine bacteria V. fischeri. evidenced the toxicity some of these oxidation by-products, since the toxicity of the solution increased on the first stages of the electrolysis. However, the abatement of the toxicity in the final stages of the electrochemical treatments, demonstrated the effectiveness of these technologies for both the mineralization and detoxification of the RNTD and FRSM solutions. The use of the fungi Cunninghanella echinulate for the bioconversion of FRSM led to the formation of three main bio-transofrmation products: the previously identified saluamide and pyridinium, and the new detected keto-alcohol derivate. These TPs were generated by both, biological and electrochemical approches, evidencing their high probability to be found in environmental compartments as the most likely TPs of FRSM by different oxidation conditions. This study is thus presented as a very useful alternative for the assessment of the fate of pharmaceutical residues in the environment

22

Özcan, Ali. "Degradation of hazardous organic compounds by using electro-fenton technology". Phd thesis, Université Paris-Est, 2010. http://tel.archives-ouvertes.fr/tel-00601213.

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In this thesis, a detailed investigation has been carried out on the use of electro-Fenton technique for the oxidation of the some persistent organic pollutants for the sake of water remediation. This technique produces *OH radicals electrocatalytically and uses them to oxidize the organic pollutants. The overall study can be divided into three parts. In the first part, the removal of selected synthetic dyes and pesticides from water was investigated by using carbon felt (CF) cathode. The oxidation kinetics of the synthetic dyes (Acid Orange 7 and Basic Blue 3) and pesticides (picloram, propham, azinphos-methyl and clopyralid) were determined. Mineralization kinetics of the related organic pollutants in aqueous medium was followed by total organic carbon and chemical oxygen demand analysis. The overall mineralization was obtained in all cases. Identification and quantification of the oxidation by-products of the given synthetic dyes and pesticides were performed by high performance liquid chromatography, gas chromatography-mass spectrometry, liquid chromatography-mass spectrometry and ion chromatography. These systematic analysis showed that the initial organic pollutants were converted into three intermediate forms; organic intermediates, short-chain aliphatic carboxylic acids and inorganic ions. Based on the intermediates identified, a plausible mineralization pathway was proposed for each dye and pesticide.In the second part of the study, the H2O2 production ability of carbon sponge (CS) as a novel cathode material for the electro-Fenton technique was investigated for the first time in the literature. The obtained results indicated that CS has a H2O2 production ability three times higher than the classical cathode CF.In the third and last part, the efficiency of boron doped diamond (BDD) as an anode in the electro-Fenton technique was investigated. Firstly, the oxidation and mineralization ability of BDD was tested for herbicide propham in anodic oxidation conditions. Then, the combination of CS and BDD electrode in the electro-Fenton technique was examined. The obtained results indicated that this combination allowed the most efficient results throughout the thesis. Moreover, the use of BDD anode in the electro-Fenton technique had considerable effect on the oxidation and mineralization of organics and especially carboxylic acids such as oxalic and oxamic acids which were highly resistant to mineralization in the case of Pt anode

23

Adityosulindro, Sandyanto. "Activation of homogeneous and heterogeneous Fenton processes by ultrasound and ultraviolet/visible irradiations for the removal of ibuprofen in water". Phd thesis, Toulouse, INPT, 2017. http://oatao.univ-toulouse.fr/17913/7/aditosulindro-sandyanto.pdf.

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Due to booming consumption and only partial removal by conventional water treatment processes, ibuprofen, a non-steroidal anti-inflammatory drug, has been detected in water resources, raising increasing concerns for possible environmental and health impact. On the other hand, advanced oxidation processes (AOPs), among which Fenton reaction, have shown successful results forremoval of various organic compounds. Traditionally based on the use of hydrogen peroxide and ferrous ions in solution, large-scale application of this AOP is still limited by narrow pH window (2 to 4) and uneasy recovery of iron catalyst. This work investigated Fenton-based oxidation of ibuprofen, and reaction activation by ultrasound (US) irradiation and ultraviolet/visible light (UV/Vis) so as to lower the required concentration of dissolved iron catalyst or improve the activity of heterogeneous counterparts. To that purpose, the efficacy of individual homogeneous AOPs (sonolysis, photolysis, ultrasound/H2O2, light/H2O2, Fenton oxidation) was evaluated first, varying operating parameters such as light wavelength and ultrasound frequency. Then, their two-by-two and overall combinations (sonophotolysis, sono-Fenton, photo-Fenton and sono-photo-Fenton oxidation) were examined with emphasis on the identification of synergistic effects. In particular, combined US/Fenton and Vis/Fenton oxidation were found more effective than the sum of individualprocesses due to sono- and photo-regeneration of ferrous ions. These results also served as a reference for the assessment of heterogeneous systems. Among tested solids, iron-containing zeolite (Fe-ZSM5 type) was shown to be a promising catalyst for peroxide oxidation of ibuprofen due to high efficiency at natural pH and low iron leaching. However, in this case, no more than additive effects was observed between ultrasound/light irradiation and heterogeneous Fenton oxidation. Beside pollutant and Total Organic Carbon conversion, main degradation products were monitored for different processes and some plausible degradation pathways were proposed. Water matrix impact was also addressed using wastewater plant effluent, which resulted into hindered performance of all oxidation processes either due to alkaline buffer or light attenuation effect.

24

Sopaj, Flamur. "Study of the influence of electrode material in the application of electrochemical advanced oxidation processes to removal of pharmaceutic pollutants from water". Phd thesis, Université Paris-Est, 2013. http://tel.archives-ouvertes.fr/tel-00985537.

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Permanent production and use of organic chemicals for many purposes has resulted in their introduction and accumulation in the environment. Depending on their physicochemical properties they can be transported by different ways from the source to very remote regions of the planet. Many organic chemicals are used in agriculture as pesticides for cultures protection or nutrient. Residues of these chemicals can always be found in fields, and under the effect of precipitations they leach and pass in streams and rivers. Pharmaceuticals and personal health care products and other house holding chemicals are continuously introduced in the environment through municipal wastewaters. These substances exhibit, in most of the cases, perturbation effects towards the living organisms, moreover the effect of many of them is not known yet. Despite their concentration in water is low, the exposure of organisms for long periods can lead to negative consequences, but these effects cannot be measured instantly. In order to reduce or avoid the pollution of water with chemicals many water treatment methods has been developed like adsorption of pollutants on adsorbents, membrane filtration, microbiological treatment, chemical oxidation with oxidizing agents and advanced oxidation processes. Most of the methods used in waste water treatment plants (WWTP) do not completely destroy the organic contaminants or they only separate the contaminants from water. Then they have to be deposed somewhere else remaining always a potential source of contamination. Advanced oxidation processes and in particular electrochemical advanced oxidation processes are methods developed later and are proven as more effective as they can completely oxidize the organic matter in water. The subject of this thesis is the use of electro-Fenton, an electrochemical advanced oxidation process for efficient destruction of organic pollutants in aqueous medium. In this method, organic pollutants are eliminated by H hydroxyl radicals (high oxidation power species) which are produced in situ through the Fenton's reagent (H2O2 + Fe2+) itself generated in the solution electrochemically and continuously. In this process, the electrode material is of fundamental importance in order to have an efficient process, so we have studied at large extent the influence of both cathode and anode material in this work. Firstly a systematic study on the oxidation capacity of the process of amoxicillin (AMX) as model pollutant with several anodes materials: BDD, Pt, DSA, PbO2 Carbon felt, Graphite and Carbon fibre was realised. In all cases a stainless steel electrode was used as cathode. The degradation of AMX was followed by HPLC analysis whereas the mineralization efficiency ot the process was measured by total organic carbon analyser (TOC). This revealed that BDD was the most efficient anode for AMX oxidation and DSA was the weakest one. Carbon felt showed a characteristic behaviour; it was very efficient on AMX oxidation but it could not transform AMX to CO2 and H2O. Afterwards four anodes were tested for their influence on electro-Fenton process efficiency namely Pt, BDD, DSA and Carbon felt, the cathode was always carbon felt. Sulfamethazine (SMT) was used as model pollutant. Apparent rate constants have given only moderate values of mineralization for currents lower than 100 mA. Here again the BDD anode was distinguished for its excellent mineralization capacity owing to the additional hydroxyl radicals and other oxidizing species introduced in the system. When electro-Fenton applied good degradation and mineralization results were obtained even with the DSA anode (...)

25

Monteil, Hélène. "Development and implementation of the Bio-electro-Fenton process : application to the removal of pharmaceuticals from water A review on efficiency and cost effectiveness of electro- and bio-electro-Fenton processes: application to the treatment of pharmaceutical pollutants in water. Efficient removal of diuretic hydrochlorothiazide from water by electro-Fenton process using BDD anode: a kinetic and degradation pathway study Electro-Fenton treatment of the widely used analgesic tramadol using BDD anode: a kinetic, energetic and degradation pathway study Efficiency of a new pilot scale continuous reactor for wastewater treatment by electrochemical advanced oxidation processes: influence of operating conditions and focus on hydrodynamics Electrochemical advanced oxidation processes combined with a biological treatment for wastewater treatment: a deep understanding on the influence of operating conditions and global efficiency". Thesis, Paris Est, 2019. http://www.theses.fr/2019PESC2045.

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Les procédés électrochimiques d'oxydation avancée constituent une technologie efficace pour traiter les produits pharmaceutiques car ils permettent la formation d'oxydants puissants tels que les radicaux hydroxyles capables d'éliminer presque tout type de contaminants organiques grâce à leur très haut pouvoir oxydant. Parmi eux, l’électro-Fenton et l’oxydation anodique sont des méthodes respectueuses de l'environnement car ils n'utilisent aucun réactif chimique (oxydation anodique) ou uniquement l'oxygène de l'air et des ions fer en tant que catalyseur (électro-Fenton).Dans cette thèse, quatre produits pharmaceutiques appartenant à des familles différentes ont été sélectionnés en fonction de leur toxicité et de leur présence dans les eaux de l'environnement. Leur élimination de l'eau a été effectuée par électro-Fenton. Les objectifs de ce travail étaient de déterminer (i) les meilleures conditions opératoires à l’échelle du laboratoire (courant et concentration du catalyseur), (ii) la cinétique de dégradation et de minéralisation et enfin (iii) de proposer une voie de minéralisation basée sur des intermédiaires aromatiques, des acides carboxyliques et des ions libérés dans la solution.Comme ces traitements ont été appliqués avec succès, un réacteur pilote composé alternativement d'anodes en BDD et de cathodes en feutre de carbone, doté d’un système d'aération et fonctionnant en mode continu a été construit pour évaluer la faisabilité d’un changement d’échelle et se diriger vers une pré-industrialisation du procédé. Différentes configurations d'électrodes ont été testées. Le débit et le courant se sont avérés être plus influents sur le taux de minéralisation et sur la consommation d'énergie, respectivement. Pour mieux comprendre le rôle du débit et des configurations, une étude hydrodynamique a été réalisée. Le modèle hydrodynamique a été associé à un modèle cinétique de minéralisation afin d'obtenir un modèle permettant de prédire le pourcentage de minéralisation à différentes positions à l'intérieur du réacteur en régime permanent. Ainsi, ce modèle peut aider à optimiser les conditions opératoires et à dimensionner les futurs réacteurs en fonction de l’objectif de minéralisation du traitement (taux de minéralisation élevé, traitement combiné, flux élevé,…).Afin de réduire les coûts opératoires, la combinaison d’un procédé électrochimique et d’un traitement biologique a ensuite été étudiée. Afin d’obtenir un traitement combiné efficace, il a été constaté que le traitement électrochimique devait (i) dégrader l'hydrochlorothiazide (ii) réduire de manière significative la concentration de ses intermédiaires aromatiques car ils inhibent de manière significative l'activité bactérienne, (iii) favoriser la formation de molécules biodégradables telles que les acides carboxyliques. La biodégradation de quatre acides carboxyliques formés lors du traitement par électro-Fenton de l'hydrochlorothiazide a également été étudiée. Il a été démontré qu'ils étaient dégradés de manière séquentielle avec différentes phases de latence et cinétiques de dégradation. Ainsi, pour les minéraliser, un réacteur de type «piston» est recommandé. La combinaison de traitement a ensuite été appliquée à un traitement électrochimique effectué à faible courant avec une anode en BDD et une anode en Platine. Un degré de minéralisation de 38 et 50% a été obtenu par le traitement biologique permettant d'atteindre un taux de minéralisation global de 66 et 85% avec les anodes en BDD et Platine respectivement. Ainsi, cette combinaison de traitement a été un succès, un changement d’échelle du procédé peut alors être envisagé
Electrochemical advanced oxidation processes (EAOPs) constitute an efficient technology to treat the pharmaceuticals as they allow the formation of strong oxidants such as hydroxyl radicals able to remove nearly any type of organic contaminants thanks to their very high oxidation power. Among them the electro-Fenton and anodic oxidation processes are environmentally friendly methods as they use no chemical reagent (anodic oxidation) or only oxygen of air and iron ions as a catalyst (electro-Fenton).In this thesis, four pharmaceuticals from different families and structures were selected based on their toxicity and their occurrence in environmental waters and their removal from water was performed by EAOPs. The objectives of this work were to determine the best operating conditions at lab scale (current and catalyst concentration), investigate the kinetic of degradation and mineralization and finally propose a mineralization pathway based on aromatic intermediates, carboxylic acids and ions released to the solution.As these treatments were successfully applied, a lab scale pilot reactor composed alternately of BDD anodes and carbon felt cathodes with a bottom aeration system and working in the continuous mode was built to scale-up these processes in order to pre-industrialize them. Different configurations of electrodes were tested. The flow rate and the current were found to be more influent on the mineralization rate and on the energy consumption, respectively. To deeper understand the role of the flow rate and the configurations a hydrodynamic study was performed. The hydrodynamic results were gathered with a kinetic model for the mineralization to obtain a model predicting the percentage of mineralization at different position inside the reactor during the steady state. Thus, this model can help to optimize the operating conditions and to size future reactors depending on the mineralization objective of the treatment (high mineralization rate, combined treatment, high flow, …).To reduce operating cost, the combination of an electrochemical process and a biological treatment was then investigated. In this frame, it was found that electrochemical treatment can (i) degrade the hydrochlorothiazide (ii) reduce significantly the concentration of its aromatic intermediates as they were shown to significantly inhibit the bacterial activity, (iii) promote the formation of biodegradable molecules such as carboxylic acids. The biodegradation of four carboxylic acids formed during the electro-Fenton treatment of the hydrochlorothiazide at lab scale was also studied. It was demonstrated that they were sequentially degraded with different lag phases and kinetics of degradation. Thus to mineralize them, a “plug flow” type reactor is recommended. The combination of treatment was then applied with an electrochemical treatment performed at low current with a BDD anode and a Platine anode. A mineralization degree of 38% and 50% were obtained by the biological treatment enabling to globally reach a mineralization rate of 66% and 85% with the BDD and the Platine anodes respectively. Thus this combined treatment was successful and open the way for the scale-up of these processes

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Ganiyu, Soliu. "Electrochemical Advanced Oxidation Processes for removal of Pharmaceuticals from water : Performance studies for sub-stoichiometric titanium oxide anode and hierarchical layered double hydroxide modified carbon felt cathode". Thesis, Paris Est, 2016. http://www.theses.fr/2016PESC1116/document.

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AbstractLes polluants émergents que sont les résidus de produits pharmaceutiques sont devenus une problématique majeure de par leur persistance et leur accumulation continue dans les différents compartiments de l’environnement. Leur élimination est un des challenges majeurs de ce siècle. Les procédés électrochimiques d’oxydation avancée (PEOA) tel que l’oxydation anodique (AO) et l’électro-Fenton (EF) ont démontré leur efficacité pour la dégradation et la minéralisation complète de cette classe de polluant. Un oxyde de titane sous-stœchiométrique déposé par plasma sur un alliage de titane a été étudié comme anode alternative peu coûteuse, stable et efficace au cours des procédés d’OA et d’EF pour la dégradation et la minéralisation de deux pharmaceutiques, l’amoxicilline (AMX) et le propanolol (PPN). Une excellente minéralisation de ces deux composés a été atteinte avec l’anode Ti4O7 comparé à l’utilisation d’une anode dimensionnellement stable (ADS) et d’une anode de platine (Pt) avec des conditions expérimentales similaires, mais une plus faible efficacité a été observé par comparaison à une anode de diamant dopé au bore (DDB) au cours du procédé d’OA. Une quasi-total minéralisation (96%) du PPN a été atteinte avec l’anode Ti4O7 au cours du procédé EF après 8 h d’électrolyse à 120 mA. Plusieurs intermédiaires aromatiques, bicycliques et autres ont été identifiés et quantifiés au cours du traitement électrochimique des deux composés pharmaceutiques, ainsi que des acides carboxyliques à chaîne courte et des ions inorganique comme produits finaux de dégradation. Des voies plausibles de dégradation ont été proposées à partir des intermédiaires identifiés, des ions inorganiques libérés ainsi que des données obtenues sur les acides carboxyliques et le COT. La solution initiale d’AMX a mené à une relativement forte inhibition de la bactérie V. fisheri, qui a ensuite augmenté au cours des premiers stades de l’électro-oxydation de par la formation d’intermédiaires cycliques plus toxiques que la molécule mère, avant de diminuer nettement au cours des étapes suivantes de l’électrolyse. Puisque le Ti4O7 est produit principalement à partir du TiO2, un matériau bon marché et abondant, ce matériau d’anode pourrait être une alternative intéressante pour le traitement des eaux usées industrielles par oxydation électrochimique. Par ailleurs, une cathode de feutre de carbone modifiée par des composés hydroxydes à double couche CoFe (CoFe-LDH/CF) et synthétisée par un procédé solvothermique a été étudiée come catalyseur/électrode pour la dégradation du polluant organique Acide Orange II (AO7) par le procédé EF sur une gamme large de pH. Une excellente minéralisation de ce colorant a été atteinte pour des pH allant de 2 à 7.1, avec une élimination du COT largement supérieure à celle atteinte en utilisant le procédé EF avec une cathode de feutre de carbone brut, quel que soit le pH étudié. La cathode préparée a montré une bonne capacité de réutilisation et peut constituer une alternative pour le traitement des eaux usées à des valeurs de pH naturel
Pharmaceuticals residues as emerging pollutants have become a major concern due to their persistence and continuous accumulation in various environmental compartments and their removal is one the major challenges of this century. Electrochemical advanced oxidation processes (EAOPs) such as anodic oxidation (AO) and electro-Fenton (EF) have shown to be efficient techniques for complete degradation and mineralization of this class of pollutants. A substoichiometric titanium oxide (Ti4O7) deposited on titanium alloy by plasma elaboration was investigated as an alternative stable and efficient low cost anode materials for application in AO and EF for degradation of pharmaceuticals amoxicillin (AMX) and propranolol (PPN) and mineralization of their aqueous solutions. Excellent mineralization of both pharmaceuticals was achieved with Ti4O7 anode compared to dimensional stable anode (DSA) and platinum (Pt) anodes at similar experimental conditions, but less efficient when compared with boron doped diamond (BDD) anode during AO treatment. Almost complete mineralization (96%) was attained with Ti4O7 anode in EF degradation of PPN at 120 mA after 8 h of electrolysis. Several aromatic, bicyclic and other intermediate byproducts were identified and quantified during the electrochemical treatment of both pharmaceuticals, with the final end products in the treated solutions being short-chain carboxylic acids and inorganic ions. Plausible mineralization pathways for both pharmaceuticals were proposed based on the identified intermediates, released inorganic ions and carboxylic acids as well as TOC data. Initial AMX solution shows relatively high inhibition to V. fischeri bacteria, which further increased at the early stage of electrooxidation due to formation of cyclic intermediates more toxic than mother molecules but sharply decreased at the later stage of electrolysis. Since the Ti4O7 is produced mainly from TiO2 which is very cheap and highly abundant material, this anode material could be an interesting alternative electrode in industrial wastewater treatment by electrochemical oxidation. On the other hand, CoFe-layer double hydroxide modified carbon-felt (CoFe-LDH/CF) cathode synthesized by solvothermal process was studied as a heterogeneous catalyst/electrode for degradation of organic pollutant Acid Orange II (AO7) over a wide pH range. Excellent mineralization of this azo dye solution was achieved in pH range 2 – 7.1, with TOC removal much higher than corresponding homogeneous EF with raw carbon-felt (CF) at all pH studied. The prepared cathode exhibited good reusability and can constitute an alternative for the treatment wastewater effluents at neutral pH values

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D\'Avila, Alexandre Coelho da Silva. "Degradação do pesticida amicarbazona em meio aquoso pelo processo TiO2/UV irradiado por luz solar". Universidade de São Paulo, 2012. http://www.teses.usp.br/teses/disponiveis/3/3137/tde-03072013-105850/.

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Os processos oxidativos avançados (POAs) têm sido apontados como alternativa eficiente para a degradação de poluentes recalcitrantes. Entre os POAs, a fotocatálise utilizando luz solar vem sendo muito estudada tendo em vista sua aplicação no tratamento de efluentes aquosos contendo pesticidas. No presente trabalho, estudou-se a degradação do herbicida amicarbazona (AMZ) por meio do processo TiO2/UV em um reator com coletores parabólicos compostos irradiados por luz solar. Os experimentos foram realizados segundo uma matriz Doehlert para o estudo da influência da concentração inicial de AMZ (20-100 mg L-1), da concentração de catalisador (0,1-1 g L-1) e do número de tubos expostos à luz solar (1-9). Amostras retiradas ao longo do tempo foram analisadas quanto às concentrações de AMZ e de carbono orgânico total (TOC). As medidas radiométricas realizadas indicaram que a radiação UVB-UVA correspondeu em média a ca. 4% da radiação solar total incidente entre 310-2800 nm; a actinometria de ferrioxalato indicou fluxo fotônico médio de 3,58×10-5 mol fótons m-2 s-1 para dias ensolarados típicos. O processo TiO2/UV mostrou-se eficiente para degradação do pesticida, que foi totalmente removido antes de 45 minutos de tratamento, para as seguintes condições: [AMZ]0=21,3 mg L-1; [TiO2]=0,5 g L-1; e 7 tubos. Contudo, nesse caso houve apenas ca. 24% de mineralização e na grande maioria dos casos os valores de TOC permaneceram praticamente constantes, o que indica a formação de sub-produtos recalcitrantes, cuja toxicidade e biodegradabilidade devem ser caracterizadas. A análise estatística dos resultados confirma os efeitos importantes da concentração inicial do pesticida e do número de tubos expostos (volume irradiado), cujo aumento permite compensar a menor incidência de radiação solar. Em alguns experimentos os resultados sugeriram que a degradação da AMZ foi favorecida pela maior concentração de TiO2. Na grande maioria dos casos os valores de ACM foram inferiores a 50 m2 kg-1, o que torna este parâmetro interessante para aumento de escala de processos fotocatalíticos irradiados por luz solar empregados no tratamento de efluentes aquosos contendo amicarbazona.
Advanced oxidative processes (AOP) have been considered as an efficient alternative for the degradation of recalcitrant pollutants. Photocatalysis using solar radiation has been studied for the treatment of wastewaters containing pesticides. In this work, the degradation of the herbicide amicarbazone (AMZ) by the TiO2/UV process was studied in a reactor equipped with compound parabolic collectors irradiated by solar light. The experiments were carried out according to a Doehlert matrix to study the effects AMZ initial concentration (20-100 mg L-1), catalyst concentration (0.1-1 g L-1), and number of tubes exposed to solar light (1-9). Samples were analyzed for AMZ and total organic carbon (TOC) concentrations. Radiometric measurements indicated that UVB-UVA radiation corresponded in average to about 4% of the solar radiation between 310-2800 nm; ferrioxalate actinometry resulted in an average photonic flux of 3.58×10-5 mol fótons m-2 s-1 for typical sunny days. The TiO2/UV process showed to be efficient for the degradation of the pesticide, which was completely removed before 45 minutes of treatment, for the following conditions: [AMZ]0=21.3 mg L-1; [TiO2]=0.5 g L-1; and 7 tubes. However, in this case only ca. 24% of mineralization was achieved, and in most cases TOC values remained practically constant, indicating the formation of recalcitrant by-products whose toxicity and biodegradility should be characterized. Statistical analysis of the results confirmed important effects of pesticide initial concentration and number of tubes exposed (irradiated volume), whose increase enables to compensate the lower incidence of solar radiation. Some experimental results suggested that AMZ degradation was favored by higher TiO2 concentrations. In most cases the values of ACM were lower than 50 m2 kg-1, in such a way that this parameter is interesting for scale-up of solar irradiated photocalytic processes used in the treatment of amicarbazone-containing wastewaters.

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Acosta, Arlen Mabel Lastre. "Processos de tratamento não convencionais para degradação do antibiótico sulfadiazina em meio aquoso". Universidade de São Paulo, 2016. http://www.teses.usp.br/teses/disponiveis/3/3137/tde-22082016-102752/.

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A presença de antibióticos no meio ambiente aquático tem causado crescente preocupação mundial. Além dos relatos de resistência de bactérias a antibióticos, essa classe de fármacos também pode causar efeitos tóxicos e atuar como perturbadores endócrinos em diversos organismos vivos e, possivelmente, em humanos. Dentre os antibióticos comumente usados destacam-se as sulfonamidas, detectadas em águas subterrâneas e superficiais. Os processos avançados de oxidação (POA) têm sido apontados como tecnologias eficientes para tratamento de poluentes recalcitrantes em diferentes matrizes aquosas. Dentre os POA, o processo foto-Fenton é uma alternativa para a degradação de compostos não biodegradáveis, incluindo fármacos. Uma vez que a principal limitação do processo é o intervalo de pH (2,5- 4,0), a reação pode ser vantajosamente conduzida empregando-se substâncias bio-orgânicas solúveis (BOS) como agentes complexantes de Fe3+ em condições ligeiramente ácidas (pH 5). Por sua vez, o emprego da energia ultrassônica tem sido menos estudado. Nesse contexto, o objetivo deste trabalho é estudar a degradação do antibiótico sulfadiazina (SDZ) por meio do processo foto-Fenton na presença de substâncias bio-orgânicas solúveis (UVvis/ Fe3+/H2O2/BOS) e do processo de cavitação por meio de ultrassom (US). Os resultados obtidos mostram que a sulfadiazina é eficientemente degradada por ultrassom de alta frequência. As maiores porcentagens e taxas de remoção são obtidas usando menor frequência de operação (580 kHz), maior potência dissipada e em pH ligeiramente ácido (melhor condição: pH 5,5). Além disso, a reação de Fenton, combinada com o tratamento US, melhorou notavelmente a degradação da SDZ, particularmente quando quantidades extras de H2O2 foram adicionadas ao sistema. Por sua vez, o uso de BOS como aditivos no processo foto-Fenton apresenta influência marcante na fotodegradação da SDZ em condições ligeiramente ácidas (pH 5). Os BOS podem estabilizar espécies de ferro em solução aquosa em pH próximos ao neutro, o que constitui uma propriedade de grande interesse. Sob as condições estudadas, o BOS CVT230 foi mais eficiente do que FORSUD, provavelmente devido às diferenças nos grupos funcionais presentes na composição destas substâncias. Finalmente, foram calculados os indicadores de consumo de energia elétrica por ordem de grandeza (EEO) para o processo de ultrassom (1572 kW h m-3 ordem-1) e área do coletor por ordem de grandeza (ACO) para o processo foto-Fenton (8,07 m2 m-3 ordem-1).
The potential impacts of antibiotic residues in the environment have become an emerging concern during recent years due to their relation with the development of resistant bacteria, and in some cases to their ability to cause toxic and endocrine disrupting effects in humans and other living organisms. Highlighted among the commonly used antibiotics are the sulfonamides, detected in groundwater and surface water. Advanced oxidation processes (AOP) might constitute an important alternative to deal with pharmaceuticals degradation. Among them, the photo-Fenton process has been widely used. One of its major drawbacks is the highly acidic pH needed (2,5-4,0) to avoid the formation of photochemically inactive iron oxides and hydroxides. The ability of soluble bio-organic substances (SBO) to complex metal cations such as iron is useful for the development of photo-Fenton at mild acidic conditions (pH 5). In turn, the use of ultrasonic energy has been less studied. In this context, the aim of this work is to study the degradation of the antibiotic sulfadiazine (SDZ) by the photo-Fenton process in the presence of soluble bio-organic substances (UV-vis/Fe3+/H2O2/SBO) and by ultrasonic cavitation (US). The results confirm that SDZ is effectively degraded by highfrequency ultrasound. Higher SDZ percent removals and removal rates were observed for the lowest operating frequency (580 kHz), higher dissipated power, and in slightly acidic solution (pH 5.5). On the other hand, SDZ degradation is highly improved in the case of the US/ Fe(II)/H2O2 system. The use of the SBO as Fenton additives in turn has a remarkable influence in SDZ photodegradation at slightly acid conditions (pH 5). This could be ascertained to the complexation of iron by the SBO, hence maintained in the reaction medium as a photoactive species. Under the studied conditions, the BOS CVT230 was more efficient than FORSUD, probably due to differences in the functional groups present in the composition of these substances. Finally, the figures-of merit electrical energy per order (EEO) and collector area per order (ACO) were calculated for the ultrasound (1572 kW h m-3 ordem-1) and photo-Fenton (8,07 m2 m-3 ordem-1) processes respectively.

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Baloul, Yasmine. "Contribution à l’étude du traitement de résidus médicamenteux dans les milieux aqueux par plasmas non thermiques. Application au paracétamol et à l’ésoméprazole". Thesis, Orléans, 2018. http://www.theses.fr/2018ORLE2008/document.

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De nombreuses molécules médicamenteuses ne sont pas traitées efficacement par les techniques classiques utilisées dans les stations d'épuration et s’accumulent dans les milieux naturels. L’objectif de cette thèse a été de développer un procédé d’oxydation avancée utilisant un plasma non thermique généré par décharge électrique pour le traitement de molécules médicamenteuses et d’identifier le schéma de dégradation d’une des molécules d’étude, à savoir le paracétamol. Les traitements ont été réalisés à l’aide de deux réacteurs : un réacteur multi-pointes avec le plasma au contact direct du liquide à traiter et un réacteur fil-cylindre avec le plasma en amont du liquide à traiter. Des taux de conversion supérieurs à 80% ont pu être obtenus avec des rendements énergétiques, qui peuvent atteindre 8g/kWh et 39 g/kWh pour le paracétamol et l’ésoméprazole, respectivement. La décharge électrique créée entre une pointe et le liquide a été caractérisée par la spectroscopie d’émission optique afin d’observer la présence des espèces oxydantes produites par le plasma et d’estimer la température du milieu faiblement ionisé. Les espèces produites dans le liquide lors de la dégradation du paracétamol et de l’ésoméprazole qui ont été identifiées par la technique HRMS, entre autres, sont principalement des acides carboxyliques ainsi que des produits azotés. L’identification des voies de production pour la formation des principaux produits ont été étudiés particulièrement à l’aide de nombreuses méthodes chimiques comme HPLC/MS, MS/MS, et de différents marquages de paracétamol. Il a été prouvé que les principaux acides carboxyliques produits proviennent de la rupture du cycle aromatique. En conclusion, cette étude nous a permis d’obtenir des rendements énergétiques de traitement des deux molécules d’étude comparables à ceux retrouvés en littérature, et surtout d’établir un chemin de dégradation du paracétamol
Many drug molecules are not effectively treated by conventional techniques used in wastewater treatment plants and accumulate in natural environments. The objective of this thesis was to develop an advanced oxidation process using a non-thermal plasma generated by electric discharge for the treatment of drug molecules (paracetamol and esomeprazole). The NTP treatments were carried out using two reactors: a multiple needle-to-plate reactor with the plasma in direct contact with the liquid to be treated and a wire-cylinder reactor with the plasma up stream of the liquid to be treated. Conversion rates higher than 80% have been obtained with energy yields, which can reach 8 g/kWh and 39 g/kWh for paracetamol and esomeprazole, respectively. The electrical discharge created between the need leand the liquid has been characterized by optical emission spectroscopy to observe the presence of the oxidative species produced by the plasma and to estimate the temperature of the ionized medium. The species produced in the liquid during the degradation of paracetamol and esomeprazole have been identified by the HRMS technique. The produced species, are mainly carboxylic acids as well as nitrogen products. The identification of production pathways for the formation of the main products has been studied particularly using numerous chemical methods such as HPLC/MS, MS/MS, and different labelling of paracetamol. It has been proven that the main carboxylic acids produced come from the breaking of the aromatic ring. In conclusion, this study allowed us to obtain energy efficiencies of treatment of the two study molecules comparable to those found in literature, and especially to establish a pathways of degradation of paracetamol

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Metolina, Patrícia. "Degradação do antibiótico bacitracina zíncica em meio aquoso através de processos oxidativos avançados". Universidade de São Paulo, 2018. http://www.teses.usp.br/teses/disponiveis/3/3137/tde-24092018-082606/.

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A presença de antibióticos no ecossistema representa um sério risco à saúde humana e animal em virtude do desenvolvimento crescente de resistência bacteriana. Uma vez que a maioria dos antibióticos é persistente à degradação biológica, os processos oxidativos avançados são apontados como uma das tecnologias mais efetivas para decompor esses compostos em águas residuárias. A bacitracina zíncica (Bc-Zn) é um potente antibiótico constituído por uma mistura complexa de peptídeos não-biodegradáveis, conjugados ao zinco. Apesar de ser um antibiótico amplamente consumido na medicina humana e animal, é preocupante a escassez de estudos que investigam sua degradação e destino ambiental. O presente trabalho analisou a degradação da Bc-Zn através dos processos de fotólise direta e UV/H2O2 em diferentes condições de radiação UVC e concentração inicial de H2O2. Os parâmetros cinéticos rendimento quântico da fotólise, constantes cinéticas de pseudo-primeira ordem e constante cinéticas de segunda ordem foram satisfatoriamente estimados pela modelagem do sistema fotoquímico experimental. Os resultados revelaram que a fotólise direta permitiu degradar todos os congêneres da mistura de Bc-Zn nas maiores doses de radiação UVC empregadas. No entanto, não houve remoção de TOC após 120 minutos de irradiação. A adição de H2O2 acelerou substancialmente a fotodegradação do antibiótico, apresentando constantes cinéticas de pseudo-primeira ordem uma ordem de grandeza superiores às obtidas por fotólise direta. Além disso, remoção considerável de até 71% do TOC foi alcançada. A análise estatística demonstrou que a radiação UV foi um fator bem mais significativo para a fotodegradação da Bc-Zn em relação à concentração inicial de H2O2, sendo as melhores condições do processo alcançadas para a maior taxa específica de emissão de fótons (1,11×10-5 Einstein L-1 s-1). Ensaios biológicos com soluções tratadas por fotólise direta e UV/H2O2 indicaram remoção completa da atividade antimicrobiana residual, ainda que os produtos da fotodegradação tenham se mostrado não-biodegradáveis. Análises de toxicidade indicaram que o metal zinco presente no antibiótico é responsável pela a toxicidade no micro-organismo-teste Vibrio fischeri. Estudos adicionais devem ser realizados para identificar os sub-produtos formados, bem como para investigar a degradação da Bc-Zn em efluentes industriais reais.
The presence of antibiotics in ecosystems represents a serious risk to human and animal health, caused by the increase in bacterial resistance. Since most antibiotics resist to biological degradation, advanced oxidation processes are pointed out as the most effective technologies for degrading these compounds in wastewater. Zinc bacitracin (Bc-Zn) is a potent antibiotic with a complex mixture of non-biodegradable peptides conjugated to zinc. Despite being a widely used antibiotic in human and animal medicine, the scarcity of studies dealing with its degradation and environmental fate is a matter of concern. In this work, Bc-Zn degradation by direct photolysis and the UV/H2O2 process was investigated for different UVC radiation conditions and initial H2O2 concentrations. Kinetic parameters, namely the photolysis quantum yield, pseudo-first order kinetic constants and second-order kinetic constants, were satisfactorily estimated from experimental data by modeling the photochemical system. The results showed that all the congeners of the Bc-Zn mixture were photolyzed at the highest UVC doses applied, while no TOC removal was observed after 120 minutes of irradiation. The addition of H2O2 substantially accelerated Bc-Zn photodegradation, with pseudo-first order kinetic constants of one order of magnitude higher than those observed under direct photolysis. In addition, a remarkable removal of up to 71% of TOC was achieved. Statistical analyses showed that UV radiation had a much more important effect on Bc-Zn photodegradation in comparison with initial H2O2 concentration, with the best process conditions achieved for the highest specific photon emission rate (1.11×10-5 Einstein L-1 s-1). Biological assays carried out with the solutions treated by direct photolysis and UV/H2O2 revealed no residual antimicrobial activity, though photodegradation products remained non-biodegradable. In addition, toxicity analyses indicated that the zinc metal present in the antibiotic is responsible for the toxic effect on the test microorganism Vibrio fischeri. Finally, further studies should be performed to identify the by-products formed and to investigate Bc-Zn degradation in real industrial wastewater.

31

Mahdi, Ahmed Moussa. "Elimination de substances pharmaceutiques d'effluents urbains par un procédé d'oxydation avancée basé sur le radical sulfate". Electronic Thesis or Diss., Aix-Marseille, 2013. http://www.theses.fr/2013AIXM4746.

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Ce travail est consacré à l’étude d’un procédé d’oxydation avancée (POA) basé sur la génération de radicaux sulfates (SO4•-) pour l’élimination de substances pharmaceutiques dans le cadre du traitement d’effluents urbains. Quatre substances pharmaceutiques azotées (carbamazépine, diclofénac, sulfaméthoxazole et ciprofloxacine) appartenant à des familles thérapeutiques différentes ont été choisies en tant que contaminants modèles. L’évaluation de la performance cinétique des procédés basés sur la génération de HO• (H2O2/Fe(II) et UV-C/H2O2) et de SO4•- (HSO5-/Co2+, UV-C/S2O82- et UV-C/HSO5-) a été conduite dans des effluents de stations d'épuration traités biologiquement. La comparaison des procédés non photochimiques et photochimiques a été conduite dans les mêmes conditions optimales et montre que les procédés générant des SO4•- sont moins inhibés par la matrice environnementale que les procédés produisant HO•. La réaction de transfert électronique est mise en évidence par l’identification de produits de transformation des contaminants d’étude par chromatographie liquide couplée à un spectromètre de masse à haute résolution. Le début d’oxydation démarre par un transfert d’un électron sur les groupements azotés générant ainsi un radical cation qui réagit avec l’eau ou l’O2. La dégradation du sulfaméthoxazole est le cas le plus évident grâce à sa fonction amine primaire (aniline) qui se transforme en fonction nitro. On peut par conséquent envisager des nouvelles stratégies de traitement des eaux usées urbaines par la génération de SO4•-
This work is devoted to the study of an alternative advanced oxidation process (AOP) generating sulfate radical (SO4•-) for the removal of pharmaceuticals in municipal wastewater effluents. Four nitrogen containing pharmaceuticals (carbamazepine, diclofenac, sulfamethoxazole and ciprofloxacin) belonging to different therapeutic classes were chosen as model contaminants. The evaluation of the kinetic performance of processes based on the generation of HO• (H2O2/Fe(II) and UV-C/H2O2 ) and SO4•- (HSO5-/Co2+, UV-C/S2O82- and UV-C/HSO5- ) was conducted in biologically treated effluent. Comparison of photochemical and non- photochemical processes performed under the same optimal conditions showed that the processes generating SO4•- are less inhibited by the environmental matrix than processes producing HO•. This electron transfer reaction is demonstrated by the identification of transformation products using liquid chromatography coupled to high resolution mass spectrometer. Oxidation of parent compounds starts by an electron transfer reaction on the nitrogen groups thereby generating a cation radical which further reacts with water or O2. The sulfamethoxazole degradation pathway gives more insights into this mechanism due to the primary amine moiety (aniline) which is converted into nitro function. This treatment system can be regarded as a new strategy for the treatment of urban wastewater contaminated by pharmaceutical residues through the generation of SO4•-

32

Loaiza, Ambuludi Silvia. "Étude des propriétés physiques et du comportement mécanique des Basaltes : étude cinétique, mécanistique et toxicologique de l'oxydation dégradante de l'Ibuprofène par l'oxydation avancée électrochimique et photochimique". Thesis, Paris Est, 2012. http://www.theses.fr/2012PEST1145/document.

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La première partie de ce travail de thèse s'inscrit dans le cadre de la dépollution des eaux contaminées par les polluants organiques persistants et plus en particulier par les résidus pharmaceutiques. Des techniques alternatives telles que les procédés d'oxydation avancée (POA) qui utilisent comme agent oxydant les radicaux OH, ont été appliquées à la dégradation et/ou à la minéralisation d'un polluant médicamenteux, l'Ibuprofène, en milieu aqueux. Il a été choisi comme molécule modèle en raison de son grand volume de prescription et de sa présence prouvée dans les effluents des stations d'épuration et dans les eaux naturelles. Notre étude a consisté notamment à la recherche d'optimisation des paramètres opératoires tels que la concentration de H2O2 et de Fe2+ ainsi que leur rapport pour générer les radicaux hydroxyles par le procédé photo-Fenton, et la concentration (et nature) de l'électrolyte de support et l'intensité du courant appliqué pour les procédés électrochimiques électro-Fenton et oxydation anodique. En outre, l'évolution de la toxicité de cette molécule a été suivie par la méthode Microtox au cours du traitement par le procédé d'oxydation anodique. La cinétique d'oxydation et de minéralisation de l'ibuprofène a été étudiée. La constante de réaction d'oxydation de l'ibuprofène avec les radicaux hydroxyles a été déterminée par la méthode de cinétique de compétition comme 3,84 109 M-1 s-1. Nos résultats montrent que l'application de ces procédés est efficace pour éliminer ce produit pharmaceutique de l'eau. On atteint la dégradation complète du polluant, et une minéralisation quasi-totale de la matière organique. La deuxième partie englobe une étude expérimentale sur les propriétés physiques (à différentes échelles) et le comportement mécanique des Basaltes. On a étudié le comportement mécanique et les modes de rupture d'un basalte poreux des Açores. Les résultats sont obtenus lors d'essais en contrainte triaxiale, en conditions totalement drainées et à température ambiante. Ce basalte présente deux modes de déformation. À faible pression de confinement, les échantillons présentent un comportement mécanique fragile et une déformation localisée (bande de cisaillement). Pour des pressions de confinement plus élevées, le basalte présente un comportement ductile et des compactions localisées (bandes de compaction). Les données mécaniques ont permis de déterminer l'enveloppe complète du domaine élastique. La quantification des propriétés physiques de deux types de basaltes des Galápagos a été effectuée à pression et température ambiante. Dans le but d'étudier l'effet de la fissuration sur les propriétés physiques, les échantillons on été soumis à des traitements thermiques. Enfin, pour étudier la réponse de la roche aux conditions de pression auxquelles elle est soumise en profondeur, des mesures de vitesses des ondes sous pression ont été acquises. Les résultats obtenus et l'utilisation de modèles théoriques ont permis de quantifier la densité de fissures initiales et de celles induites par les traitements thermiques, ainsi que le facteur de forme de celles-ci. L'ensemble des propriétés physiques ont permis de mieux comprendre le rôle du réseau poreux de la roche sur les propriétés physiques. Cette étude de laboratoire a été nécessaire pour l'interprétation des données recueillies in situ par sismique réfraction
The first part of this thesis is focused on the remediation of waters contaminated with persistent organic pollutants, in particular pharmaceutical products. Alternative technologies such as the advanced oxidation processes (AOPs), which based on the generation of hydroxyl radicals OH, were applied to the degradation and/or mineralization of a pollutant drug, ibuprofen, in aqueous medium. We chose this pollutant as a model molecule to study due to its large volume of prescription and to its proved presence in the effluents of sewage plants and natural waters. The main objective of this work was the optimization of operational parameters of the applied AOPs. The concentration of H2O2 and Fe2+ reagents ratio to generate hydroxyl radicals for photo-Fenton process, and supporting electrolyte concentration (and the nature) and the applied current for both electro-Fenton and anodic oxidation processes. The oxidation and mineralization kinetics of the ibuprofen were studied and the absolute rate constant for the oxidative degradation of ibuprofen was determined by the competition kinetic method, being 3,84 109 M-1s-1. Toxicity tests of the drug solutions during the anodic oxidation process were carried out by the Microtox method. Our results show that these methods are effective for the degradation of this pharmaceutical product from water. Ibuprofen was completely degraded and the organic matter was almost completely mineralized after the application of these processes. The second part of the thesis includes an experimental study of the physical properties (at different scales) and the mechanical behavior of basaltic rocks. We studied the mechanical behavior and the failure modes of a porous basalt from Azores. Results were acquired under triaxial compression experiments on water saturated samples at room temperature. This basalt presented two modes of deformation. At low confining pressure, the samples exhibited a brittle mechanical behavior and a localized deformation (shear band). For higher confining pressure, this basalt showed a ductile behavior and localized compactions (compaction bands). The mechanical data allows us to plot the full yield surface for the porous basalt. The quantification of the physical properties of two types of basalts from the Galapagos was performed at room temperature and pressure. In order to study the effect of cracking on the physical properties of these basalts, samples were subjected to thermal treatments to induce thermal crack damage. Finally for the less porous basalt, measures of wave velocities under the pressure at which it is subjected in depth were acquired. The obtained results and the following application of models with them allow quantifying the density of initial cracks and of those induced by thermal treatments, as well as quantifying the aspect ratio of cracks. The studied physical properties led to better understand the role of the pore network of the rock in these physical properties. This laboratory study was necessary for the interpretation of data collected in situ by seismic refraction method

33

Mahdi, ahmed Moussa. "Elimination de substances pharmaceutiques d'effluents urbains par un procédé d'oxydation avancée basé sur le radical sulfate". Thesis, Aix-Marseille, 2013. http://www.theses.fr/2013AIXM4746.

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Abstract (sommario):

Ce travail est consacré à l’étude d’un procédé d’oxydation avancée (POA) basé sur la génération de radicaux sulfates (SO4•-) pour l’élimination de substances pharmaceutiques dans le cadre du traitement d’effluents urbains. Quatre substances pharmaceutiques azotées (carbamazépine, diclofénac, sulfaméthoxazole et ciprofloxacine) appartenant à des familles thérapeutiques différentes ont été choisies en tant que contaminants modèles. L’évaluation de la performance cinétique des procédés basés sur la génération de HO• (H2O2/Fe(II) et UV-C/H2O2) et de SO4•- (HSO5-/Co2+, UV-C/S2O82- et UV-C/HSO5-) a été conduite dans des effluents de stations d'épuration traités biologiquement. La comparaison des procédés non photochimiques et photochimiques a été conduite dans les mêmes conditions optimales et montre que les procédés générant des SO4•- sont moins inhibés par la matrice environnementale que les procédés produisant HO•. La réaction de transfert électronique est mise en évidence par l’identification de produits de transformation des contaminants d’étude par chromatographie liquide couplée à un spectromètre de masse à haute résolution. Le début d’oxydation démarre par un transfert d’un électron sur les groupements azotés générant ainsi un radical cation qui réagit avec l’eau ou l’O2. La dégradation du sulfaméthoxazole est le cas le plus évident grâce à sa fonction amine primaire (aniline) qui se transforme en fonction nitro. On peut par conséquent envisager des nouvelles stratégies de traitement des eaux usées urbaines par la génération de SO4•-
This work is devoted to the study of an alternative advanced oxidation process (AOP) generating sulfate radical (SO4•-) for the removal of pharmaceuticals in municipal wastewater effluents. Four nitrogen containing pharmaceuticals (carbamazepine, diclofenac, sulfamethoxazole and ciprofloxacin) belonging to different therapeutic classes were chosen as model contaminants. The evaluation of the kinetic performance of processes based on the generation of HO• (H2O2/Fe(II) and UV-C/H2O2 ) and SO4•- (HSO5-/Co2+, UV-C/S2O82- and UV-C/HSO5- ) was conducted in biologically treated effluent. Comparison of photochemical and non- photochemical processes performed under the same optimal conditions showed that the processes generating SO4•- are less inhibited by the environmental matrix than processes producing HO•. This electron transfer reaction is demonstrated by the identification of transformation products using liquid chromatography coupled to high resolution mass spectrometer. Oxidation of parent compounds starts by an electron transfer reaction on the nitrogen groups thereby generating a cation radical which further reacts with water or O2. The sulfamethoxazole degradation pathway gives more insights into this mechanism due to the primary amine moiety (aniline) which is converted into nitro function. This treatment system can be regarded as a new strategy for the treatment of urban wastewater contaminated by pharmaceutical residues through the generation of SO4•-

34

Mroczko, Dominik. "Zwiększenie efektywności technologicznej usuwania wybranych mikrozanieczyszczeń z wody". Rozprawa doktorska, 2021. https://repolis.bg.polsl.pl/dlibra/docmetadata?showContent=true&id=73615.

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35

Mroczko, Dominik. "Zwiększenie efektywności technologicznej usuwania wybranych mikrozanieczyszczeń z wody". Rozprawa doktorska, 2021. https://delibra.bg.polsl.pl/dlibra/docmetadata?showContent=true&id=73615.

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