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Synthesis of Metal Oxide-Based Catalysts by Microwave-Assisted Solution Combustion Method Kawthar Frikha

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Synthesis of Metal Oxide-Based Catalysts by Microwave-Assisted Solution Combustion Method Kawthar Frikha Synthesis of metal oxide-based catalysts by microwave-assisted solution combustion method Kawthar Frikha To cite this version: Kawthar Frikha. Synthesis of metal oxide-based catalysts by microwave-assisted solution combustion method. Material chemistry. Université de Haute Alsace, 2020. English. tel-03010014 HAL Id: tel-03010014 https://hal.archives-ouvertes.fr/tel-03010014 Submitted on 17 Nov 2020 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. Année 2020 N° d’ordre : (attribué par le SCD) UNIVERSITÉ DE HAUTE-ALSACE−UNIVERSITÉ DE STRASBOURG ÉCOLE NATIONALE D’INGÉNIEURS DE SFAX−UNIVERSITÉ DE SFAX THESE En cotutelle internationale Pour l’obtention du grade de DOCTEUR DE L’UNIVERSITÉ DE HAUTE-ALSACE ECOLE DOCTORALE : Physique et Chimie-Physique (ED 182) Discipline : Chimie-Physique ET DOCTEUR DE L’ÉCOLE NATIONALE D’INGÉNIEURS DE SFAX ECOLE DOCTORALE : Sciences et Technologies Discipline : Matériaux et Environnement Présentée et soutenue publiquement par Kawthar FRIKHA Le 27 Mai 2020 SYNTHÈSE DE CATALYSEURS D’OXYDES MÉTALLIQUES PAR LA MÉTHODE DE COMBUSTION EN SOLUTION ASSISTÉE PAR MICRO- ONDES Jury : M. Patrick FIEVET, Professeur des Universités, UTINAM, France (Président) M. Jean-Luc ROUSSET, Directeur de Recherche, IRCELyon, France (Rapporteur) Mme. Hanene AKROUT, Maître de Conférences HDR, CERTE, Tunisie (Rapporteur) Mme. Simona BENNICI, Chargée de Recherche HDR, IS2M, France (Examinatrice) M. Lionel LIMOUSY, Professeur des Universités, IS2M, France (Co-Directeur de thèse) M. Jamel BOUAZIZ, Professeur des Universités, LAMA, Tunisie (Co-Directeur de thèse) ACKNOWLEDGMENTS Acknowledgments I would like to thank Prof. Vincent ROUCOULES, director of the Institute of Materials Science of Mulhouse (IS2M), and Prof. Jamel BOUAZIZ, director of the Laboratory of Advanced Materials (LAMA) for welcoming me during the last three years of the PhD study. I would like to thank my thesis committee members: Prof. Patrick FIEVET, Dr. Jean-Luc ROUSSET, Dr. Hanene AKROUT, and Dr. Simona BENNICI for their insightful comments and valuable suggestions on this thesis work. I would like to take this opportunity to thank Prof. Dominique ADOLPHE, the head of the doctoral school in exact science at the University of Haute Alsace (UHA), who was able, despite the extraordinary circumstances, to negotiate the best deal for making possible the PhD defense. I would like to express my sincere gratitude to my supervisors Prof. Lionel LIMOUSY and Prof. Jamel BOUAZIZ for giving me the opportunity to work under their guidance. I greatly appreciate the commitment, the continuous support, and the encouragement throughout the years of the PhD study. My sincere gratitude also goes to Dr. Simona BENNICCI, who provided me an opportunity to join her team−Transfers, Reactivity, Materials for Clean Processes (TRM2P)−, and who gave me access to the laboratory and research facilities. I especially want to thank her for her willingness to give her time so generously. Her constructive suggestions, during the planning and development of this research work, have been very much appreciated. I wish to thank many people; Ms. Laure MICHELIN, Ms. Habiba NOUALI, Ms. Samar HAJJAR- GARREAU, Mr. Ludovic JOSIEN, and Mr. Loic VIDAL, staff of theIS2M institute, for their contribution to this project and for allowing me to learn from them as much as I could; Dr. Kamel CHAARI, who was involved in the implementation of this research project. I also wish to thank my fellow doctoral students and my labmates at IS2M for all the fun we have had. It was great sharing laboratory with all of you! A very special gratitude goes to the Tunisian Ministry of Higher Education and Scientific Research (MESRS), as well as, to the French National Centre for Scientific Research (CNRS) organization for providing financial support, during my stay in France. Last, but not the least, I want to say “thank you” to my family: my parents, my brother and my sister for believing in me and supporting me along the way. I place on record, my sense of gratitude to one and all, who directly or indirectly, have contributed to the accomplishment of this thesis work. i TABLE OF CONTENTS Table of Contents Acknowledgments .............................................................................................................. i Table of Contents .............................................................................................................. ii List of Figures ................................................................................................................. vii List of Tables ................................................................................................................... xii List of Abbreviations .......................................................................................................xiv GENERAL INTRODUCTION ............................................................................................1 Résumé en Français de l’introduction générale ...................................................................5 CHAPTER 1. REVIEW OF THE LITERATURE ..........................................................7 Introduction ...................................................................................................................... 10 1.1 The potential of metal oxides for heterogeneous catalysis...................................... 10 1.1.1 Characteristics of Ni, Co and Cu oxide-based catalytic materials ....................... 11 1.1.1.1 Bulk structure ............................................................................................ 12 1.1.1.2 Surface structure ........................................................................................ 13 1.1.2 Multifunctional catalysts containing Ni, Co or Cu ............................................. 14 1.1.2.1 Ni containing catalysts ............................................................................... 14 1.1.2.2 Co containing catalysts .............................................................................. 15 1.1.2.3 Cu containing catalysts .............................................................................. 15 1.1.3 Characteristics of alumina and its application in catalysis .................................. 16 1.1.4 Alumina-Ni/Co/Cu chemical interaction ............................................................ 18 1.1.5 Applications in heterogeneous catalysis: oxidation of carbon monoxide ............ 20 1.1.5.1 Cobalt oxide (CoxOy) ................................................................................. 21 1.1.5.2 Nickel oxide (NixOy) ................................................................................. 24 1.1.5.3 Copper oxide (CuxOy) ................................................................................ 24 1.1.6 Methods for metal oxides catalytic materials elaboration ................................... 27 1.1.6.1 Ceramic method (solid-state reaction) ........................................................ 27 1.1.6.2 Co-precipitation ......................................................................................... 27 1.1.6.3 Sol-gel ....................................................................................................... 28 1.1.6.4 Impregnation ............................................................................................. 28 1.2 Microwave chemistry for metal oxide catalysts synthesis ...................................... 29 1.2.1 Introduction to microwave chemistry ................................................................ 29 1.2.2 Microwave assisted solution combustion synthesis ............................................ 34 ii TABLE OF CONTENTS 1.2.2.1 Theory of combustion reaction .................................................................. 35 1.2.2.2 Solution combustion parameters ................................................................ 36 1.2.2.2.1 Chemical composition of precursors ..................................................... 37 1.2.2.2.2 Stoichiometry of the reactants (RV/OV ratio) ....................................... 39 1.2.2.2.3 Heating method .................................................................................... 39 1.2.2.3 Mechanism of oxide forming ..................................................................... 40 1.2.2.4 Metal oxides prepared by SCS ................................................................... 41 1.2.2.4.1 Al2O3 ................................................................................................... 41 1.2.2.4.2 NiO ...................................................................................................... 41 1.2.2.4.3 Co3O4 ................................................................................................... 42 1.2.2.4.4 CuO ..................................................................................................... 42 1.2.2.4.5 Ni/Al2O3 .............................................................................................. 43 1.2.2.4.6 Co/Al2O3 .............................................................................................
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