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Fenton and UV-Vis Based Advanced Oxidation Processes in Wastewater Treatment

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Fenton and UV-Vis Based Advanced Oxidation Processes in Wastewater Treatment UNIVERSITAT DE BARCELONA FACULTAT DE QUÍMICA DEPARTAMENT D’ENGINYERIA QUÍMICA I METAL·LÚRGIA Fenton and UV-vis based advanced oxidation processes in wastewater treatment: Degradation, mineralization and biodegradability enhancement. Miguel Rodríguez Barcelona, April, 2003 Programa de Doctorado de Ingeniería Química Ambiental Biennio 1998-2000 Memoria presentada por Miguel Rodríguez, Ingeniero Químico, para optar al grado de Doctor en Ingeniería Química Miguel Rodríguez La presente Tesis ha sido realizada en el Departamento de Ingeniería Química y Metalurgia de la Universidad de Barcelona, bajo la dirección del Dr. Santiago Esplugas Vidal, quien autoriza su presentación: Dr. Santiago Esplugas Vidal Barcelona, Abril de 2002 Al Prof. Sergio Miranda, pilar fundamental en mi transitar por la vida universitaria. Por fortuna la vida está llena de momentos como estos. Por ello, nunca abandones, siempre será mejor perseverar y ver como al final todo llega, así como llega el sol cada mañana. Miguel En honor a la verdad, el espacio para los agradecimientos podría ocupar un capítulo de esta tesis, y más que una exageración es una manera de expresar el haber tenido la fortuna de trabajar y compartir con tanta gente y de quienes siempre recibí ayuda, aprecio, amistad y solidaridad razones por las cuales estoy muy agradecido. Trataré sin embargo, en un buen ejercicio de síntesis. resumir sin dejar a nadie en el olvido. En primer lugar quiero agradecer al convenio ULA-CONICIT por el otorgamiento de la beca para la realización de este doctorado al igual que al DR. Santiago Esplugas, quien aceptó ser mi tutor y de quien he recibido amistad, confianza , conocimientos y toda su ayuda para llevar a feliz término esta tesis doctoral. Gracias por todo Santi. Toda ésta invalorable experiencia ha sido posible por el compartir diario con mucha gente de gran calidad humana. No puedo olvidar mis primeros días de trabajo con Andreas. Los dias interminables y continuos de trabajo con Vitaliy y ya cerca del final con Florian. To Dr. Gurol and her research’s group in San Diego State University, especially to Melissa, who always gave me her help to make easier the difficulty of having to speak in another language. Thanks a lot for every thing. En otras de mis andanzas en la búsqueda del conocimiento y de la experiencia requerida para asumir en el futuro con buena base la responsabilidad de seguir en el mundo de la investigación, tuve la oportunidad de compartir con el grupo del Dr. César Pulgarin, de la Escuela Politecnica Federal de Lausane, Suiza. De ellos solo puedo decir que se me metieron en el alma. Gracias Sandra, Víctor, Giovanna, Ricardo, Isabel, y por supuesto César, por toda la ayuda y la amistad que recibí de ustedes. Antes de finalizar todo este periplo, también tuve la oportunidad de compartir y aprender de los amigos de la Plataforma Solar de Almería. A Sixto, Julián, Julia, Wolfgang, Agustín, Sonia y Antonio, para todos mi agradecimiento. Ya habia advertido que seria largo, pero ya casi termino, solo que ahora viene un agradecimiento muy especial. Todo este andar de trabajo por estos centros de investigación, siempre tuvo como centro principal, la Universidad de Barcelona, y de ella, el Departamento de Ingeniería Química y Metalúrgica, donde por supuesto pasé la mayoria de estos 4 largos años. A todos sus profesores, gracias, y muy especialmente, Jaime Giménez, Carmen Sans, Carmen González, Esther Chamarro y David Curcó. También para el personal de este departamento de quien siempre he recibido el mejor de los tratos y debo resaltar de ellos al Sr. Antonio y al Sr. Somoza (quien ya lamentablemente no está entre nosotros) personas que al inicio fueron de mucha ayuda y luego pasaron a ser mis amigos. Mi agradecimiento también a el resto de amigos que han estado todos estos años, y de alguna manera han contribuido para que los mismos sean mas llevaderos, me refiero a Marta, Esther, Alicia, Neus, Cristina, Nadia, Eva y Fares. En medio de tantos nombres y momentos especiales, hay alguien para quien cualquier cosa que diga podría resultar poco. Alguno de ustedes pueden imaginarse a quien me refiero, y no puede ser otra que a mi amiga del alma, a la que por espacio de todos estos años siempre ha estado y de la que nunca podré olvidarme. Han sido tantos momentos compartidos, tanto trabajo juntos, tantas conversaciones y también de alguna discusión, como es lógico, pero ella siempre estuvo allí. No puede ser otra que mi amiga Sandra. Para tí, lo mejor de mis sentimientos para agradadecer todo lo que has hecho por mí. Finalmente, hay gente que no ha estado en los laboratorios, pero si que han estado en mis dias, mis recuerdos y en mi vida diaria. Me refiero a mi familia, mi mamá, hermanas, sobrinos, quienes seguro habrian querido contribuir mas. Hay siempre sin embargo, alguién que se destaca, que da ese extra, que se entrega mas, y en este caso ha sido mi hermana Nina, a quien le agradezco infinitamente su amor, su compañía, su amistad y su solidaridad. Gracias por ser como eres. No puedo dejar de agradecer a dos amigos que fueron fundamentales para mi estancia en esta hermosa ciudad, ellos son Victor y Ana, para ustedes también mi agradecimiento. Quiero además agradecer a todos esos amigos que a pesar de la distancia, siempre han estado conmigo. A Miguel, Carmen, Luz, Carlos, J. Carlos, la flaca, Domingo, Cerrada, la familia Miranda y tantos otros, que no tendria espacio para nombralos. Finalmente, mi más sentido agradecimiento al país que me vio nacer y de él, a ese pequeño pueblo, El Tocuyo, donde crecieron mis sueños, hoy, uno de ellos se hace realidad. A todos, mil gracias. Índex Index 1.Introduction 1.1. The problematic of water contamination ...................................................... 3 1.2. Studied aqueous solutions............................................................................... 8 1.2.1. Environmental problems caused by phenolic compounds.............................. 9 1.2.2. Environmental problems caused by nitro aromatic compounds ................. 11 1.2.3. Environmental problems caused by DCDE...................................................... 15 1.2.4. Environmental problems caused by textile wastewater .............................. 16 1.3. Methods for the removal of organic compounds in wastewater.................. 18 1.3.1. Incineration ......................................................................................................... 19 1.3.2. Air stripping…. ................................................................................................... 19 1.3.3. Adsorption of organic compound onto activated carbon................................ 20 1.3.4. Wet oxidation ...................................................................................................... 20 1.3.5. Electrochemical oxidation.................................................................................. 21 1.3.6. Photochemical processes .................................................................................... 22 1.3.7. Biological oxidation............................................................................................. 24 1.3.8. Chemical oxidation ............................................................................................. 24 1.3.8.1. UV-based processes................................................................................ 32 1.3.8.1.1. UV/O3 processes....................................................................... 32 1.3.8.1.2. UV/O3/H2O2 process................................................................. 33 1.3.8.1.3. Fe3+/UV-vis process ................................................................. 34 1.3.8.1.4. UV/TiO2 (Heterogeneous photocatalysis) ............................ 34 1.3.8.2. H2O2 –based processes ............................................................................ 35 1.3.8.2.1. H2O2/UV process ............................................................... 35 1.3.8.2.2. H2O2/O3 process ....................................................................... 36 1.3.8.2.3. Fenton and photo-Fenton reaction........................................... 36 1.3.9. AOPs combined with biological treatment ................................................ 38 i Índex 2. Objectives......................................................................................................... 43 3. Removal of nitrobenzene and phenol by Fenton process. Kinetic model 3.1. Introduction ................................................................................................................. 49 3.2. Experimental ...................................................................................................... 53 3.2.1. Reagents ............................................................................................................... 53 3.2.2. Experimental device and procedure (reactor A)........................................ 53 3.2.3. Analytical determinations ........................................................................ 55 3.2.3.1. HPLC...................................................................................................... 55 3.2.3.2. pH ........................................................................................................... 56 3.2.4. Range of experimental variables for NB and phenol degradation.............. 56 3.3. Results and discussion for NB degradation 3.3.1. Intermediates in the degradation of NB............................................................ 59 3.3.2. Estimation
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