DESARROLLO DE NUEVAS ESTRATEGIAS BASADAS EN LA INTEGRACIÓN DE PROCESOS FOTOQUÍMICOS SOLARES CON OTRAS TÉCNICAS AVANZADAS PARA EL TRATAMIENTO DE AGUAS RESIDUALES COMPLEJAS

En la presente Tesis Doctoral se estudió la degradación de una mezcla de ocho compuestos fenólicos mediante diferentes procesos de oxidación avanzada. Se trataron mediante proceso foto-Fenton solar donde aplicando un diseño experimental tipo Doehlert se determinó que el proceso se puede extender hasta valores por encima de pH 2.8, probablemente debido a la formación de complejos del hierro con los compuestos fenólicos. En el tratamiento mediante ozono y la combinación de ozono con luz se estudió el efecto que la concentración de contaminante, el pH y la dosis de ozono tienen sobre el proceso. En general, la combinación del ozono con la luz resultó más eficaz en los casos más desfavorables, es decir, aquellos en los que la dosis de ozono era baja y/o el pH más ácido. La mineralización resultó ser superior en la combinación de ozono con luz y se alcanzó la detoxificación de las muestras en ambos ensayos. Se analizó la toxicidad mediante diferentes bioensayos, resultando el compuesto 2,4-dinitrofenol ser el más toxico para todos los ensayos. Para la monitorización de los contaminantes en los tratamientos, se midieron matrices de Excitación/Emisión (EMM) de fluorescencia. En el caso del proceso foto-Fenton, a los 12 minutos, todos los cromóforos habían desaparecido. En el tratamiento con ozono, se observa la aparición de nuevos cromóforos cuya intensidad va disminuyendo con el tiempo de tratamiento sin llegar a desaparecer por completo. Se han realizado matrices de Excitación/Emisión (EEMs) para estudiar la posible formación de complejos entre sustancias tipo húmicas (STH) y el hierro, así como los posibles cambios experimentados a lo largo del proceso foto-Fenton. Mediante análisis de factores paralelos (PARAFAC) se identificaron tres componentes. Se determinó la constante de estabilidad de los componentes con el Fe(III) a diferentes valores de pH, obteniéndose el máximo para pH 5. Los experimentos fotoquímicos empleando STH y Fe(III), en presencia y ausencia de H2O2, mostraron la dependencia del pH de los componentes modelados. En vista de la capacidad de las STH aisladas a partir de residuos urbanos de actuar como complejantes del Fe, se consideró la posibilidad de emplear otro tipo de residuos como material de partida; en concreto se empleó alperujo para la extracción de STH. Se probaron diferentes condiciones de extracción, obteniéndose los mejores resultados para valores de pH elevados y tiempos de digestión largos. Se comprobó la capacidad fotocatalíca de la STH extraídas y se profundizó en el estudio de la generación de especies radicales. Demostrada la utilidad de las EEMs y PARAFAC para profundizar en el conocimiento de mezclas complejas y teniendo en cuenta la dificultad que supone la aplicación del análisis matemático, se decidió colaborar en el desarrollo de una interfaz gráfica de usuario que facilitara dicho análisis. La aplicación EEMlab facilita la carga, pretratamiento y análisis mediante PARAFAC de sets de datos muy numerosos. Se creó un ejemplo con muestras que contenían mezclas de compuestos conocidos en diferentes proporciones y se empleó EEMlab para la corrección, preprocesamiento y análisis de los datos, validando la utilidad de la aplicación.In this Doctoral Thesis, the degradation of a mixture of eight phenolic compounds by means of different advanced oxidation processes has been studied. An experimental methodology, based in Doehlert matrixes, was employed to analyze the effect of operational parameters on photo-Fenton process, and the results show that pH range can be extended clearly above 2.8, probably due to complexation of iron with the phenolic substances. In ozonation and ozone-UVA-Vis combination, the effect of pH, ozone dose and pollutants concentration were studied. Generally, O3/UVA-Vis was more efficient only in the experiments with worst operational conditions (low ozone dose and acid pH values). However, mineralization was better for the ozone UVA-vis combination. The toxicity was monitored along the degradation processes by means of different biotoxicity assays and in all cases a good detoxification was reached, being 2,4-dinitrophenol the most toxic pollutant. In order to monitor the pollutants along the treatment, excitation emission fluorescence matrixes (EEM) were recorded. In photo-Fenton process, chromophores were destroyed at 12 min of treatment. In ozonation, new chromophores appeared and partially disappeared at the end of the treatment. To gain further insight into the complexation of humic like substances (HLS) and Fe(III) and into the possible changes of the complex along the photo-Fenton process, EEMs were recorded and analyzed by PARAFAC (PARallel Analysis FACtor). Three fluorescent components were identified in all cases. The interaction of HLS with Fe(III) was characterized by determining the stability constants of the components with Fe (III) at different pH values, which reached their highest value at pH = 5. Photochemical experiments, with and without H2O2, showed pH-dependent trends for the modeled components. Taking into account the ability of humic substances to act as iron complexing agents, the possibility of employing olive mill wastes as a source of HLS was considered. Different extractions conditions were tested and best results were obtained for high pH values and long digestion times. Photocatalytic activity of the obtained substances was proved and the generation of reactive species was further studied. EEMs and PARAFAC seems to be a useful tool to gain further insight into complex mixtures, but the mathematical analysis in not easy. Taking this into account, we decided to collaborate in the development of a graphical user interface. The EEMlab application facilitates the load, preprocess and PARAFAC analysis of big data sets. An example dataset with already know mixtures of compounds at different concentrations was created. EEMlab was used to correct, preprocess and analyze the data set in order to probe the EEMlab utility.En la present Tesi Doctoral es va estudiar la degradació d'una mescla de huit compostos fenòlics per mitja de diversos processos d'oxidació avançada. Es van tractar pel procés foto-Fenton solar, on aplicant un disseny experimental del tipus Doehlert es va determinar que el procés es pot estendre fins un valor per damunt de pH 2.8, probablement a causa de la formació de complexes del ferro amb els compostos fenòlics. En el tractament per ozó i la combinació ozó amb llum, es va estudiar l'efecte que la concentració del contaminant, el pH i la dosi d'ozó tenen en el procés. En general, la combinació d'ozó amb llum va resultar més eficaç en els casos més desfavorables, es a dir, aquells en els quals la dosi d'ozó era baixa i/o el pH més àcid. La mineralització va resultar ser superior en la combinació d'ozó amb llum i es va aconseguir la detoxificació de les mostres en ambdós assajos. Es va analitzar la toxicitat mitjançant diferent bioassajos, resultant el compost 2,4-dinitrofenol ser el més tòxic per a tot els assajos. Per a la monitorització dels contaminants en els tractaments, es mesuraren matrius de Excitació/Emissió (EEMs) de fluorescència. En el cas del procés foto-Fenton, als 12 minuts, tots els cromòfors havien desaparegut. En el tractament amb ozó, va observar-se l'aparició de nous cromòfors, la intensitat dels quals va disminuint amb el temps de tractament, sense arribar a desaparèixer completament. Es van realizar matrius de Excitació/Emissió (EMMs) per estudiar la possible formació de complexes entre les substàncies tipus húmiques (STH) i el ferro, així com els possibles canvis experimentats al llarg del procés foto-Fenton. Mitjançant l'anàlisi de factors paral·lels (PARAFAC) s'identificaren tres components. Es va determinar la constant de estabilitat dels components amb el Fe(III) a diferents valors de pH, obtenint-se'n el màxim per a un pH de 5. Els experiments fotoquímics empleant STH i Fe(III), en presència i absència de H2O2, mostraren la dependència amb el pH dels components modelats. En vista de la capacitat de les STH aïllades de residus orgànics urbans d'actuar com complexants del ferro, es va considerar la possibilitat d'utilitzar un altre tipus de residu com material de partida; concretament s'empleà el residu sòlid generat en l'obtenció de l'oli d'oliva en un procés en dos fases (pinyolada) per a l'extracció de STH. Es van provar diferents condicions d'extracció, obtenint-se'n els millors resultats per a valors de pH elevats i temps de digestió llargs. Es va comprovar la capacitat fotocatalítica de les STH extretes i es va profundizar en l'estudi de la generació d'espècies radicalàries. Demostrada la utilitat de les EMMs i PARAFAC per a aprofundir en el coneixement de mescles complexes i comptant amb la dificultat que suposa l'aplicació de l'anàlisi matemàtic, es va decidir colaborar en el desenvolupament d'una interfície gràfica d'usuari que facilitarà l'anàlisi. L'aplicació EMMlab facilita la càrrega, pretractament i anàlisi mitjançant PARAFAC de sets de dades molt nombrosos. Es va crear un exemple amb mostres que contenien mescles de compostos coneguts en diferents proporcions i es va emprar EEMlab per a la correcció, preprocessament i anàlisi de les dades, validant la utilitat de l'aplicacióGarcía Ballesteros, S. (2017). DESARROLLO DE NUEVAS ESTRATEGIAS BASADAS EN LA INTEGRACIÓN DE PROCESOS FOTOQUÍMICOS SOLARES CON OTRAS TÉCNICAS AVANZADAS PARA EL TRATAMIENTO DE AGUAS RESIDUALES COMPLEJAS [Tesis doctoral no publicada]. Universitat Politècnica de València. https://doi.org/10.4995/Thesis/10251/95602TESI

Unveiling the Dependence between Hydroxyl Radical Generation and Performance of Fenton Systems with Complexed Iron

[EN] Humiclike substances (HLS) have been demonstrated to be useful auxiliaries to drive the (photo)-Fenton process at mild pH, by avoiding iron inactivation via formation of active complexes. However, the actual performance of the process is affected by a manifold of opposite processes. In this work, the generation of hydroxyl radical-like reactive species in the Fentonlike process has been investigated using electron paramagnetic resonance, employing 5,5-dimethyl-1-pyrroline-N-oxide as a probe molecule. The signal obtained with the Fe(II)-HLS-H2O2 system at pH = was very intense but decreased with time, in line with the difficult reduction of the formed Fe(III) to Fe(II). On the contrary, the signal of the Fe(III)-HLS-H2O2 system was weak but stable. The most intense signal was observed at HLS concentration of ca. 30 mg/L. Interestingly, the performance of the Fenton system at pH = 5 to degrade caffeine followed the same trends, although caffeine removal was very low after 1 h of irradiation. The results were more evident in a solar simulated photo-Fenton process, where an increase in the abatement of caffeine was observed until an HLS concentration of 30 mg/L, where 98% removal was reached after 1 h.The authors want to acknowledge the financial support from Ministerio de Ciencia, Innovacion y Universidades (RTI2018-097997-B-C31) and European Union (645551-RISE-2014, MAT4TREAT). P.G.-N. would like to thank Spanish Ministerio de Economia y Competitividad for her fellowship (BES-2016-077962).García-Negueroles, P.; García-Ballesteros, S.; Amat Payá, AM.; Laurenti, E.; Arqués Sanz, A.; Santos-Juanes Jordá, L. (2019). Unveiling the Dependence between Hydroxyl Radical Generation and Performance of Fenton Systems with Complexed Iron. ACS Omega. 4(26):21698-21703. https://doi.org/10.1021/acsomega.9b02241S216982170342

Sustainable Magnetic Materials (from Chitosan and Municipal Biowaste) for the Removal of Diclofenac from Water

[EN] The photodegradation of an aqueous solution of diclofenac (DCF) has been attempted in the presence of hydrogen peroxide and organic/inorganic hybrid magnetic materials under simulated and real solar light. The hybrid magnetic materials have been prepared via coprecipitation synthesis starting from iron(II) and iron(III) inorganic salts in the presence of bioderived organic products (i.e., chitosan or bio-based substances isolated from commercially available composted urban biowastes) acting as stabilizers of the iron-containing phase. In addition to the as prepared hybrid materials, the corresponding materials obtained after a pyrolytic step at low temperature (550 degrees C) have been tested. The obtained results evidenced the capability of the materials to activate hydrogen peroxide at mild pH promoting DCF (photo) degradation. All the materials feature also as adsorbents since a decrease of DCF is observed also when working in the dark and in the absence of hydrogen peroxide.This work was realized with financial support for academic interchange from the Marie Sklodowska-Curie Research and Innovation Staff Exchange project, funded by the European Commission H2020-MSCA-RISE-2014 within the framework of the research project Mat4treaT (Project number: 645,551). Politecnico di Torino is gratefully acknowledged for funding project Starting Grant RTD (project number: 54_RSG17NIR01).Nisticò, R.; Bianco Prevot, A.; Magnacca, G.; Canone, L.; García-Ballesteros, S.; Arqués Sanz, A. (2019). Sustainable Magnetic Materials (from Chitosan and Municipal Biowaste) for the Removal of Diclofenac from Water. Nanomaterials. 9(8):1-14. https://doi.org/10.3390/nano908109111498Applying the Circular Economy Lens to Waterhttp://circulatenews.org/2017/01/applying-the-circular-economy-lens-to-water/Petrie, B., Barden, R., & Kasprzyk-Hordern, B. (2015). A review on emerging contaminants in wastewaters and the environment: Current knowledge, understudied areas and recommendations for future monitoring. Water Research, 72, 3-27. doi:10.1016/j.watres.2014.08.053Bethi, B., Sonawane, S. H., Bhanvase, B. A., & Gumfekar, S. P. (2016). Nanomaterials-based advanced oxidation processes for wastewater treatment: A review. Chemical Engineering and Processing - Process Intensification, 109, 178-189. doi:10.1016/j.cep.2016.08.016Andreozzi, R. (1999). Advanced oxidation processes (AOP) for water purification and recovery. Catalysis Today, 53(1), 51-59. doi:10.1016/s0920-5861(99)00102-9Oturan, M. A., & Aaron, J.-J. (2014). Advanced Oxidation Processes in Water/Wastewater Treatment: Principles and Applications. A Review. Critical Reviews in Environmental Science and Technology, 44(23), 2577-2641. doi:10.1080/10643389.2013.829765Ghatak, H. R. (2014). Advanced Oxidation Processes for the Treatment of Biorecalcitrant Organics in Wastewater. Critical Reviews in Environmental Science and Technology, 44(11), 1167-1219. doi:10.1080/10643389.2013.763581Richardson, S. D., & Ternes, T. A. (2017). Water Analysis: Emerging Contaminants and Current Issues. Analytical Chemistry, 90(1), 398-428. doi:10.1021/acs.analchem.7b04577Minella, M., Marchetti, G., De Laurentiis, E., Malandrino, M., Maurino, V., Minero, C., … Hanna, K. (2014). Photo-Fenton oxidation of phenol with magnetite as iron source. Applied Catalysis B: Environmental, 154-155, 102-109. doi:10.1016/j.apcatb.2014.02.006Nadejde, C., Neamtu, M., Hodoroaba, V.-D., Schneider, R. J., Paul, A., Ababei, G., & Panne, U. (2015). Tannic acid- and natural organic matter-coated magnetite as green Fenton-like catalysts for the removal of water pollutants. Journal of Nanoparticle Research, 17(12). doi:10.1007/s11051-015-3290-0Nadejde, C., Neamtu, M., Hodoroaba, V.-D., Schneider, R. J., Paul, A., Ababei, G., & Panne, U. (2015). Green Fenton-like magnetic nanocatalysts: Synthesis, characterization and catalytic application. Applied Catalysis B: Environmental, 176-177, 667-677. doi:10.1016/j.apcatb.2015.04.050Munoz, M., de Pedro, Z. M., Casas, J. A., & Rodriguez, J. J. (2015). Preparation of magnetite-based catalysts and their application in heterogeneous Fenton oxidation – A review. Applied Catalysis B: Environmental, 176-177, 249-265. doi:10.1016/j.apcatb.2015.04.003Palma, D., Bianco Prevot, A., Celi, L., Martin, M., Fabbri, D., Magnacca, G., … Nisticò, R. (2018). Isolation, Characterization, and Environmental Application of Bio-Based Materials as Auxiliaries in Photocatalytic Processes. Catalysts, 8(5), 197. doi:10.3390/catal8050197Franzoso, F., Nisticò, R., Cesano, F., Corazzari, I., Turci, F., Scarano, D., … Mártire, D. O. (2017). Biowaste-derived substances as a tool for obtaining magnet-sensitive materials for environmental applications in wastewater treatments. Chemical Engineering Journal, 310, 307-316. doi:10.1016/j.cej.2016.10.120Nisticò, R., Cesano, F., Franzoso, F., Magnacca, G., Scarano, D., Funes, I. G., … Parolo, M. E. (2018). From biowaste to magnet-responsive materials for water remediation from polycyclic aromatic hydrocarbons. Chemosphere, 202, 686-693. doi:10.1016/j.chemosphere.2018.03.153Nisticò, R., Franzoso, F., Cesano, F., Scarano, D., Magnacca, G., Parolo, M. E., & Carlos, L. (2016). Chitosan-Derived Iron Oxide Systems for Magnetically Guided and Efficient Water Purification Processes from Polycyclic Aromatic Hydrocarbons. ACS Sustainable Chemistry & Engineering, 5(1), 793-801. doi:10.1021/acssuschemeng.6b02126Nisticò, R., Celi, L. R., Bianco Prevot, A., Carlos, L., Magnacca, G., Zanzo, E., & Martin, M. (2018). Sustainable magnet-responsive nanomaterials for the removal of arsenic from contaminated water. Journal of Hazardous Materials, 342, 260-269. doi:10.1016/j.jhazmat.2017.08.034Standard Methods Online Standard Methods for the Examination of Water and Wastewaterhttp://standardmethods.org/Amat, A. ., Arques, A., Beneyto, H., Garcı́a, A., Miranda, M. A., & Seguı́, S. (2003). Ozonisation coupled with biological degradation for treatment of phenolic pollutants: a mechanistically based study. Chemosphere, 53(1), 79-86. doi:10.1016/s0045-6535(03)00450-8Pérez-Estrada, L. A., Malato, S., Gernjak, W., Agüera, A., Thurman, E. M., Ferrer, I., & Fernández-Alba, A. R. (2005). Photo-Fenton Degradation of Diclofenac:  Identification of Main Intermediates and Degradation Pathway. Environmental Science & Technology, 39(21), 8300-8306. doi:10.1021/es050794

Humic like substances for the treatment of scarcely soluble pollutants by mild photo-Fenton process

[EN] Humic-like substances (HLS) extracted from urban wastes have been tested as auxiliaries for the photo Fenton removal of thiabendazole (TBZ) under simulated sunlight. Experimental design methodology based on Doehlert matrices was employed to check the effects of hydrogen peroxide concentration, HLS amount as well as TBZ loading; this last parameter was studied in the range 25-100 mg/L, to include values below and above the limit of solubility at pH = 5. Very satisfactory results were reached when TBZ was above solubility if HLS and H2O2 amounts were high. This could be attributed to an interaction of HLS-TBZ that enhances the solubility of the pollutant. Additional evidence supporting the latter interaction was obtained by fluorescence measurements (excitation emission matrices) and parallel factor analysis (PARAFAC). (C) 2018 Elsevier Ltd. All rights reserved.Authors want to acknowledge the financial support of Spanish Ministerio de Economia y Competitividad (CTQ2015-69832-C04) and European Union (645551-RISE-2014, MAT4TREAT). The present work was partially supported by UNLP (11/X679), ANPCyT (PICT-2015-0374A) and CONICET (PIP: 12-2013-01-00236CO). B. Caram thank the CONICET for his research graduate grant. F. S. Garcia Einschlag is a research member of CONICET.Caram, B.; García-Ballesteros, S.; Santos-Juanes Jordá, L.; Arqués Sanz, A.; Garcia-Einschlag, FS. (2018). Humic like substances for the treatment of scarcely soluble pollutants by mild photo-Fenton process. Chemosphere. 198:139-146. https://doi.org/10.1016/j.chemosphere.2018.01.074S13914619

Humic-like substances from urban waste as auxiliaries for photo-Fenton treatment: a fluorescence EEM-PARAFAC study

[EN] In this work, analysis of excitation-emission-matrices (EEM) has been employed to gain further insight into the characterization of humic like substances (HLS) obtained from urban wastes (soluble bio-organic substances, SBOs). In particular, complexation of these substances with iron and changes along a photo-Fenton process have been studied. Recorded EEMs were decomposed by using parallel factor analysis (PARAFAC). Three fluorescent components were identified by PARAFAC modeling of the entire set of SBO solutions studied. The EEM peak locations (lambda(ex)/lambda(em)) of these components were 310-330 nm/400-420 nm (C1), 340-360 nm/450-500 nm (C2), and 285 nm/335-380 nm (C3). Slight variations of the maximum position of each component with the solution pH were observed. The interaction of SBO with Fe(III) was characterized by determining the stability constants of the components with Fe(III) at different pH values, which were in the order of magnitude of the ones reported for humic substances and reached their highest values at pH = 5. Photochemical experiments employing SBO and Fe(III), with and without H2O2, showed pH-dependent trends for the evolution of the modeled components, which exhibited a strong correlation with the efficiency reported for the photo-Fenton processes in the presence of SBO at different pH values.This work was supported by Generalitat Valenciana, Conselleria d'Ecuacio, Cultura i esport, Spain (GV/2015/074), Spanish Ministerio de Economia y Competitividad (CTQ2015-69832-C4-4-R) and by the Marie Sklodowska-Curie Research and Innovation Staff Exchange project funded by the European Commission H2020-MSCA-RISE-2014 (Project number: 645551). F. S. G. E. and L. C. are researchers from CONICET, Argentina.García-Ballesteros, S.; Constante, M.; Vicente Candela, R.; Mora Carbonell, M.; Amat Payá, AM.; Arques Sanz, A.; Carlos, L.... (2017). Humic-like substances from urban waste as auxiliaries for photo-Fenton treatment: a fluorescence EEM-PARAFAC study. Photochemical & Photobiological Sciences. 16:38-45. https://doi.org/10.1039/c6pp00236fS384516Malato, S., Fernández-Ibáñez, P., Maldonado, M. I., Blanco, J., & Gernjak, W. (2009). Decontamination and disinfection of water by solar photocatalysis: Recent overview and trends. Catalysis Today, 147(1), 1-59. doi:10.1016/j.cattod.2009.06.018WANG, J. L., & XU, L. J. (2012). Advanced Oxidation Processes for Wastewater Treatment: Formation of Hydroxyl Radical and Application. Critical Reviews in Environmental Science and Technology, 42(3), 251-325. doi:10.1080/10643389.2010.507698Pignatello, J. J., Oliveros, E., & MacKay, A. (2006). Advanced Oxidation Processes for Organic Contaminant Destruction Based on the Fenton Reaction and Related Chemistry. Critical Reviews in Environmental Science and Technology, 36(1), 1-84. doi:10.1080/10643380500326564Papoutsakis, S., Miralles-Cuevas, S., Oller, I., Garcia Sanchez, J. L., Pulgarin, C., & Malato, S. (2015). Microcontaminant degradation in municipal wastewater treatment plant secondary effluent by EDDS assisted photo-Fenton at near-neutral pH: An experimental design approach. Catalysis Today, 252, 61-69. doi:10.1016/j.cattod.2015.02.005Klamerth, N., Malato, S., Agüera, A., & Fernández-Alba, A. (2013). Photo-Fenton and modified photo-Fenton at neutral pH for the treatment of emerging contaminants in wastewater treatment plant effluents: A comparison. Water Research, 47(2), 833-840. doi:10.1016/j.watres.2012.11.008De Luca, A., Dantas, R. F., & Esplugas, S. (2015). Study of Fe(III)-NTA chelates stability for applicability in photo-Fenton at neutral pH. 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Waste sourced bio-based substances for solar-driven wastewater remediation: Photodegradation of emerging pollutants. Chemical Engineering Journal, 235, 236-243. doi:10.1016/j.cej.2013.09.009Avetta, P., Berto, S., Bianco Prevot, A., Minella, M., Montoneri, E., Persico, D., … Arques, A. (2015). Photoinduced transformation of waste-derived soluble bio-based substances. Chemical Engineering Journal, 274, 247-255. doi:10.1016/j.cej.2015.03.126Gomis, J., Gonçalves, M. G., Vercher, R. F., Sabater, C., Castillo, M.-A., Prevot, A. B., … Arques, A. (2015). Determination of photostability, biocompatibility and efficiency as photo-Fenton auxiliaries of three different types of soluble bio-based substances (SBO). Catalysis Today, 252, 177-183. doi:10.1016/j.cattod.2014.10.015Berkovic, A. M., García Einschlag, F. S., Gonzalez, M. C., Pis Diez, R., & Mártire, D. O. (2013). Evaluation of the Hg2+binding potential of fulvic acids from fluorescence excitation–emission matrices. Photochem. Photobiol. 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Electron Transfer between Iron Minerals and Quinones: Estimating the Reduction Potential of the Fe(II)-Goethite Surface from AQDS Speciation. Environmental Science & Technology, 47(24), 14161-14168. doi:10.1021/es403658gLopes, L., de Laat, J., & Legube, B. (2002). Charge Transfer of Iron(III) Monomeric and Oligomeric Aqua Hydroxo Complexes:  Semiempirical Investigation into Photoactivity. Inorganic Chemistry, 41(9), 2505-2517. doi:10.1021/ic011029

Selective ablation with UV lasers of a-Si:H thin film solar cells in direct scribing configuration

Monolithical series connection of silicon thin-film solar cells modules performed by laser scribing plays a very important role in the entire production of these devices. In the current laser process interconnection the two last steps are developed for a configuration of modules where the glass is essential as transparent substrate. In addition, the change of wavelength in the employed laser sources is sometimes enforced due to the nature of the different materials of the multilayer structure which make up the device. The aim of this work is to characterize the laser patterning involved in the monolithic interconnection process in a different configurations of processing than the usually performed with visible laser sources. To carry out this study, we use nanosecond and picosecond laser sources working at 355nm of wavelength in order to achieve the selective ablation of the material from the film side. To assess this selective removal of material has been used EDX (energy dispersive using X-ray) analysi

Monitoring photolysis and (solar photo)-Fenton of enrofloxacin by a methodology involving EEM-PARAFAC and bioassays: Role of pH and water matrix

[EN] The degradation of enrofloxacin (ENR) by direct photolysis, Fenton and solar photo-Fenton processes has been studied in different water matrices, such as ultra-pure water (MQ), tap water (TW) and highly saline water (SW). Reactions have been conducted at initial pH 2.8 and 5.0. At pH = 2.8, HPLC analyses showed a fast removal of ENR by (solar photo)-Fenton treatments in all studied water matrices, whereas a 40% removal was observed after 120 min of photolysis. However, TOC measurements showed that only solar photo-Fenton was able to produce significant mineralization (80% after 120 min of treatment); differences between ENR removal and mineralization can be attributed to the release of important amounts of reaction by-products. Excitation-emission matrices (EEMs) combined with parallel factor analysis (PARAFAC) were employed to gain further insight into the nature of these by-products and their time-course profile, obtaining a 5-component model. EEM-PARAFAC results indicated that photolysis is not able to produce important changes in the fluoroquinolone structure, in sharp contrast with (solar photo)-Fenton, where decrease of the components associated with fluoroquinolone core was observed. Agar diffusion tests employing E. toll and S. aureus showed that the antibiotic activity decreased in parallel with the destruction of the fluoroquinolone core.This paper is part of a project that has received funding from the European Union's Horizon 2020 - Research and Innovation Framework Programme under the H2020 Marie Sklodowska-Curie Actions grant agreement No 765860. The paper reflects only the authors' view and the Agency is not responsible for any use that may be made of the information it contains.Sciscenko, I.; García-Ballesteros, S.; Sabater Marco, C.; Castillo López, M.; Escudero-Oñate, C.; Oller, I.; Arqués Sanz, A. (2020). Monitoring photolysis and (solar photo)-Fenton of enrofloxacin by a methodology involving EEM-PARAFAC and bioassays: Role of pH and water matrix. Science of The Total Environment. 719:1-9. https://doi.org/10.1016/j.scitotenv.2020.137331S1971

Micromecanizado Láser de Componentes de Gran calidad de Acabado Superficial

El uso de láseres pulsados con anchos temporales de nanosegundos y longitudes de onda en el rango Ultravioleta, permiten un preciso control del material abferido, convirtiendo dicha técnica en una herramienta fundamental para mecanizados que requieren de una gran calidad y acabado, con relaciones de aspecto muy altas. Este trabajo presenta un análisis paramétrico de la influencia de las distintas variables de proceso para diferentes tipos de materiales (metálicos, dieléctricos, materiales orgánicos, etc) en la calidad y acabado final. The use of nanoseconds U.V. lasers permits a precise control in ablation’s processes. As a result this tool plays a fundamental role in machining where a high quality and good aspect ratios are required. This paper presents a parametric analysis of the influence of some processing parameters for different types of materials

Pentachlorophenol Removal from Water by Soybean Peroxidase and Iron(II) Salts Concerted Action

[EN] Soybean peroxidase (SBP) has been employed for the treatment of aqueous solutions containing pentachlorophenol (PCP) in the presence of hydrogen peroxide at pH range 5-7. Reaction carried out with 1mg/L of PCP, 4mg/L of H2O2, and 1.3x10(-9)M of SBP showed a fast initial elimination of PCP (ca. 30% in 20min), but the reaction does not go beyond the removal of 50% of the initial concentration of PCP. Modification in SBP and PCP amounts did not change the reaction profile and higher amounts of H2O2 were detrimental for the reaction. Addition of Fe(II) to the system resulted in an acceleration of the process to reach nearly complete PCP removal at pH 5 or 6; this is more probably due to a synergetic effect of the enzymatic process and Fenton reaction. However, experiments developed in tap water resulted in a lower PCP elimination, but this inconvenience can be partly overcome by leaving the tap water overnight in an open vessel before reaction.We want to acknowledge Davide Mainero from Acea Pinerolese for his collaboration in this research. The authors want to thank the financial support of the European Union (PIRSES-GA-2010-269128, EnvironBOS and Marie Sklodowska-Curie Research and Innovation Staff Exchange projectH2020-MSCA-RISE-2014, Mat4treaT-project number: 645551) and Spanish Ministerio de Educacion y Ciencia (CTQ2015-69832-C4-4-R). Sara Garcia-Ballesteros would like to thank the Spanish Ministerio de Economia y Competitividad for her fellowship (BES-2013-066201).Tolardo, V.; García-Ballesteros, S.; Santos-Juanes Jordá, L.; Vercher Pérez, RF.; Amat Payá, AM.; Arqués Sanz, A.; Laurenti, E. (2019). Pentachlorophenol Removal from Water by Soybean Peroxidase and Iron(II) Salts Concerted Action. 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(2011). Combination of advanced oxidation processes and biological treatments for wastewater decontamination—a review. Science of the Total Environment, 409(20), 4141–4166. https://doi.org/10.1016/j.scitotenv.2010.08.061 .Passardi, F., Cosio, C., Penel, C., & Dunand, C. (2005, July 22). Peroxidases have more functions than a Swiss army knife. Plant Cell Reports. Springer-Verlag. https://doi.org/10.1007/s00299-005-0972-6 .Pera-Titus, M., Garcı́a-Molina, V., Baños, M. A., Giménez, J., & Esplugas, S. (2004). Degradation of chlorophenols by means of advanced oxidation processes: a general review. Applied Catalysis B: Environmental, 47(4), 219–256. https://doi.org/10.1016/j.apcatb.2003.09.010 .Qayyum, H., Maroof, H., & Yasha, K. (2009). Remediation and treatment of organopollutants mediated by peroxidases: a review. Critical Reviews in Biotechnology, 29(2), 94–119. https://doi.org/10.1080/07388550802685306 .Samokyszyn, V. M., Freeman, J. P., Rao Maddipati, K., & Lloyd, R. V. (1995). Peroxidase-catalyzed oxidation of pentachlorophenol. Chemical Research in Toxicology, 8, 349–355 http://pubs.acs.org/doi/pdf/10.1021/tx00045a005 . Accessed 23 June 2017Santos-Juanes, L., Amat, A. M., & Arques, A. (2017a). Strategies to drive photo-Fenton process at mild conditions for the removal of xenobiotics from aqueous systems. Current Organic Chemistry, 21(12), 1074–1083. https://doi.org/10.1136/adc.2010.199901 .Santos-Juanes, L., García Einschlag, F. S., Amat, A. M., & Arques, A. (2017b). Combining ZVI reduction with photo-Fenton process for the removal of persistent pollutants. Chemical Engineering Journal, 310, 484–490. https://doi.org/10.1016/j.cej.2016.04.114 .Sarria, V., Parra, S., Adler, N., Péringer, P., Benitez, N., & Pulgarin, C. (2002). Recent developments in the coupling of photoassisted and aerobic biological processes for the treatment of biorecalcitrant compounds. 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Pergamon. https://doi.org/10.1016/j.envint.2011.04.014

Avances en la fabricación de células y módulos fotovoltaicos de silicio en capa fina mediante láser

El láser es un instrumento omnipresente en la fabricación de módulos fotovoltaicos. Los láser estándar para la interconexión monolítica de dispositivos de lámina delgada de a-Si son láser de estado sólido bombeados por diodo (DPSS) emitiendo en longitudes IR (λ=1064 nm) y en VIS (λ=532 nm). En este trabajo mostramos estudios de ablación de algunos materiales fotovoltaicos (óxidos conductores transparentes (OCT) y a-Si) con láser emitiendo en UV en el régimen de nanosegundos (ns). La afección térmica resultante en la ablación es menor, y por tanto se reduciría el riesgo de cortocircuitos en la interconexión monolítica, convirtiendo a las fuentes láser UV como herramientas prometedoras como alternativa a las fuentes estándar. Laser is an essential tool for photovoltaic modules manufacturing. Nowadays DPSS working at IR ( λ=1064 nm) and VIS (λ=532 nm) wavelengths are standard tools for thin film module fabrication. In this work we present ablation studies of some photovoltaic materials (transparent conductive oxides (TCO) and a-Si) using nanoseconds (ns) laser sources emitting in the UV. The thermal affection is minimized, and therefore it would be reduced the short-circuit formation risk in the monolithic interconnection, demonstrating the potential use of ns laser sources emitting in the UV as promising alternative tools to the standard laser sources