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Oxidation of Phenol and Cresol by Electrochemical Advanced Oxidation Method in Homogeneous Medium: Application to Treatment of A

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Oxidation of Phenol and Cresol by Electrochemical Advanced Oxidation Method in Homogeneous Medium: Application to Treatment of A Oxidation of phenol and cresol by electrochemical advanced oxidation method in homogeneous medium : application to treatment of a real effluent of aeronautical industry Marcio Pimentel To cite this version: Marcio Pimentel. Oxidation of phenol and cresol by electrochemical advanced oxidation method in homogeneous medium : application to treatment of a real effluent of aeronautical industry. Other. Université Paris-Est, 2008. English. NNT : 2008PEST0271. tel-00742470v2 HAL Id: tel-00742470 https://tel.archives-ouvertes.fr/tel-00742470v2 Submitted on 7 May 2010 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. Université Paris-Est Marne-La-Vallée Institut Francilien des Sciences Appliquées (IFSA) Laboratoire Géomatériaux et Géologie de l'Ingénieur THÈSE pour obtenir le grade de Docteur de l’Université Paris-Est Marne-la-Vallée Spécialité : Sciences et Techniques de l'Environnement présentée et soutenue publiquement par Marcio PIMENTEL le 24 septembre 2008 Etudes de l'oxydation de phénol et crésols par l'oxydation électrochimique avancée en milieu homogène. Application au traitement d'effluent de l'industrie aéronautique Phenol and cresols treatment in aqueous solution by electro-Fenton process: Application to the mineralization of aeronautic wastewater industry. Directeur de thèse : Prof. Mehmet A. OTURAN Jury: Président: Prof. Jean Guillaume EON Université Fédérale de Rio de Janeiro Rapporteurs: Dr. Maurice MÉDEBIELLE Université Lyon 1 Prof. Geraldo Lippel SANT´ANNA JR. Université Fédérale de Rio de Janeiro Examinateurs: Prof. Márcia W. Carvalho DEZOTTI Université Fédérale de Rio de Janeiro Dr. Nihal OTURAN Université Paris-Est Marne-la-Vallée Prof. Tito Livio Moitinho ALVES Université Fédérale de Rio de Janeiro © UMLV ii Remerciements Cette thèse a été réalisée par une co-tutelle entre l’Université Féderal de Rio de Janeiro et l'Université Paris-Est de Marne-La-Vallée au laboratoire des Géomatériaux et Géologie de l'Ingénieur au sein de l’équipe chimie de l'environnement avec le financement de l’Armée de l’Air Brésilienne. Je remercie l’Armée de l’Air Brésilienne par la confiance qui m'a été accordée. Je tiens à dire un grand merci à Mehmet A. Oturan, Professeur à l'université de Marne-la-Vallée, pour les conseils précieux, ses commentaires et tout aide qu'il m'a apporté au cours de ce travail. Je tiens à dire merci aussi à Marcia Dezotti, Professeur à l’Université Fédérale de Rio de Janeiro, pour les conseils et l'aide qu'il m'a apporté au cours de ce travail. Je remercie très chaleureusement Nihal Oturan pour toute l'aide qu'elle m'a apportée pour mes expériences. Un grand merci à mon épouse Marcela pour son amour et patience pendant tout ce temps. Je voudrais également remercier toute l'équipe du laboratoire Géomatériaux, surtout les thésards et stagiaires, pour leur bonne humeur, leurs histoires et, particulierment, les commentaires sur football pendant les pauses. Merci à Beytül, Nacho, Samiha, Mababa, Aida, Mustapha, Minir. Vous étiez là quand j'en avais besoin et même pour les autreschoses. iii Abstract of Thesis presented to COPPE/UFRJ as a partial fulfillment of the requirements for the degree of Doctor of Science (D. Sc.) Phenol and cresols treatment in aqueous solution by “electro-fenton” process: Application to the mineralization of aeronautic wastewater industry. Marcio Antonio da Silva Pimentel September/2008 Advisors: Mehmet A. Oturan Márcia Walquíria de Carvalho Dezotti Department: Chemical Engineering The present work verified the efficiency of electro-Fenton to destroy phenolic compounds present in Stripping Aircraft Wastewater. This research aimed to elucidate the influence of the catalyst nature, its concentration and of electric current density in efficiency of electro-Fenton process using an indivisible cell with a carbon felt cathode and platinum or borod doped diamond anodes. The experiments compared the effect of these variables to destroy phenol, cresols and their intermediates. The compounds and many intermediates formed were identified in High Perfomance Liquid Chromatograph and allowed obtaining apparent and/or absolute constants and simplified degradation mechanisms. In optimum conditions, measures of Total Organic Carbon showed high mineralization rates. At the end, the application of electro-Fenton process to high organics loads of real Stripping Aircraft wastewater allowed obtaining almost complete mineralization replacing Pt anode by Boron Doped Diamond. Key words: degradation, phenol, cresols, electro-Fenton. iv SUMMARY INTRODUCTION............................................................................................................................................................. 11 CHAPTER I: BIBLIOGRAPHICAL REVIEW.................................................................................................................. 14 1.1 AIRCRAFT EFFLUENT CHARACTERIZATION ............................................................................................................. 15 1.2 TREATMENT TECHNIQUES TO REMOVE PHENOL AND CRESOLS ............................................................................... 21 1.2.1 Biological Processes.................................................................................................................................. 21 1.2.2 Conventional Physico-Chemical Processes.............................................................................................. 22 1.2.2.1 Activated Carbon Absorption ..................................................................................................................................... 23 1.2.2.2 Chemical precipitation................................................................................................................................................ 23 1.2.2.3 Conventional chemical oxidation............................................................................................................................ 23 1.2.3 Advanced Oxidative Processes (AOPs).................................................................................................... 24 1.2.3.1 Conventional AOPs.................................................................................................................................................... 24 1.2.3.2 Electrochemical Advanced Oxidation Processes ....................................................................................................... 28 1.3 INFLUENTIAL PARAMETERS IN THE ELECTRO -FENTON PROCESS ............................................................................. 37 1.3.1 Electrode nature ........................................................................................................................................ 37 1.3.2 pH .............................................................................................................................................................. 38 1.3.3 Nature and Catalyst Concentration ........................................................................................................... 39 1.3.4 Effect of the medium.................................................................................................................................. 40 1.3.5 Electrolytes ................................................................................................................................................ 41 1.3.6 Dissolved Oxygen concentration ............................................................................................................... 42 1.3.7 Current Density.......................................................................................................................................... 43 1.3.8 Temperature .............................................................................................................................................. 45 1.3.9 Transport Phenomena............................................................................................................................... 45 CHAPTER II: MATERIALS AND METHODES .............................................................................................................. 48 2.1 CHEMICAL PRODUCTS ......................................................................................................................................... 49 2.2. SOLUTIONS PREPARED ........................................................................................................................................ 49 2.3. ANALYTICAL TECHNIQUES .................................................................................................................................... 50 2.3.1 High performance liquid chromatography (HPLC) .................................................................................... 50 2.3.2 Total Organic Carbon (TOC) ..................................................................................................................... 50 2.4 ELECTROCHEMICAL REACTOR .............................................................................................................................
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