Acidic-Basic Properties of Catalysts for Conversion of Biomass Dusan Stosic
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Acidic-basic properties of catalysts for conversion of biomass Dusan Stosic To cite this version: Dusan Stosic. Acidic-basic properties of catalysts for conversion of biomass. Other. Université Claude Bernard - Lyon I, 2012. English. NNT : 2012LYO10284. tel-00946707 HAL Id: tel-00946707 https://tel.archives-ouvertes.fr/tel-00946707 Submitted on 14 Feb 2014 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. N° d’ordre 284-2012 Année 2012 THESE DE L‘UNIVERSITE DE LYON Délivrée par L’UNIVERSITE CLAUDE BERNARD LYON 1 ECOLE DOCTORALE DE CHIMIE Pour l’obtention du DIPLOME DE DOCTORAT (arrêté du 7 août 2006) Présentée et soutenue publiquement le 18 Décembre 2012 par Dušan STOŠIû TITLE : Acidic-basic properties of catalysts for conversion of biomass TITRE : Propriétés acido-basiques de catalyseurs pour la conversion de la biomasse Directeur de thèse : Mme Aline Auroux JURY Mme. A. AUROUX Directeur de thèse Mme. S. BENNICI Co-encadrant M. F. DUMEIGNIL Rapporteur M. A. TRAVERT Rapporteur M. J.-M. LANCELIN Examinateur M. J.-L. DUBOIS Examinateur Mme. V. RAKIC Examinateur M. J.-L. COUTURIER Membre invité UNIVERSITE CLAUDE BERNARD - LYON 1 Président de l’Université M. François-Noël GILLY Vice-président du Conseil d’Administration M. le Professeur Hamda BEN HADID Vice-président du Conseil des Etudes et de la Vie Universitaire M. le Professeur Philippe LALLE Vice-président du Conseil Scientifique M. le Professeur Germain GILLET Secrétaire Général M. Alain HELLEU COMPOSANTES SANTE Faculté de Médecine Lyon Est – Claude Bernard Directeur : M. le Professeur J. ETIENNE Faculté de Médecine et de Maïeutique Lyon Sud – Charles Administrateur provisoire : M. le Professeur G. Mérieux KIRKORIAN Directeur : M. le Professeur D. BOURGEOIS UFR d’Odontologie Institut des Sciences Pharmaceutiques et Biologiques Directeur : Mme la Professeure C. VINCIGUERRA. Institut des Sciences et Techniques de la Réadaptation Directeur : M. le Professeur Y. MATILLON Département de formation et Centre de Recherche en Biologie Directeur : M. le Professeur P. FARGE Humaine COMPOSANTES ET DEPARTEMENTS DE SCIENCES ET TECHNOLOGIE Faculté des Sciences et Technologies Directeur : M. le Professeur F. De MARCHI Département Biologie Directeur : M. le Professeur F. FLEURY Département Chimie Biochimie Directeur : Mme le Professeur H. PARROT Département GEP Directeur : M. N. SIAUVE Département Informatique Directeur : M. le Professeur S. AKKOUCHE Département Mathématiques Directeur : M. le Professeur A. GOLDMAN Département Mécanique Directeur : M. le Professeur H. BEN HADID Département Physique Directeur : Mme S. FLECK Département Sciences de la Terre Directeur : Mme la Professeure I. DANIEL UFR Sciences et Techniques des Activités Physiques et Sportives Directeur : M. C. COLLIGNON Observatoire de Lyon Directeur : M. B. GUIDERDONI Polytech Lyon Directeur : M. P. FOURNIER Ecole Supérieure de Chimie Physique Electronique Directeur : M. G. PIGNAULT Institut Universitaire de Technologie de Lyon 1 Directeur : M. C. VITON Institut Universitaire de Formation des Maîtres Directeur : M. R. BERNARD Institut de Science Financière et d'Assurances Directeur : Mme la Professeure V. MAUME- DESCHAMPS Acknowledgments This work has been accomplished from November 2009 to December 2012 in the Institut de Recherches sur la Catalyse et l’Environnement de Lyon (IRCELYON). I would like to express my very great appreciation to Madam Aline Auroux for her valuable and constructive suggestions during the planning and development of this research work. Her willingness to give her time so generously has been very much appreciated. This work could not be done without her help. I would like to express my deep gratitude to Madam Simona Bennici for her patient guidance, enthusiastic encouragement and useful critiques of this research work. Her fast reactions to solve the problems substantially speed up my work. Special thanks go to Madam Vesna Rakiü without whom I would not come in to this research institute. From our long conversations about research, but also about music, literature and politics I have learned a lot. I wish to thank Mr. Jean-Luc Dubois, Mr. Jean-Luc Couturier and Mr. Christophe Calais from ARKEMA Company for sharing their knowledge and results. Especially, I am grateful to Mr. Dubois, scientific advisor of Arkema, for his suggestions and corrections in publishing scientific articles. They have been of immense help to me. I wish to thank to Mr. Franck Dumeignil for managing the Guerbetol project and welcoming me in his laboratory in Lille. I also thank Mr. Mickaël Capron for being a good host during my stay at his laboratory and Lille. I would like to express my gratitude to Mr. Arnaud Travert and Mr. Sergey Sirotin for their contribution to my work. Special thanks are addressed to the technical services of IRCELYON for valuable technical contributions in Raman, XRD, BET, XPS, and chemical analysis. I had a real pleasure of working with my colleagues who were in Energy Group at IRCELYON during this period: Georgeta Postole, Gareth Whiting, Reem Kourieh, Adrien Mekki-Berrada (thanks for all the great music), Hao Yu, Emil Obeid, Otman Otman, Hongying Zhao, Jingxuan Cai, Didier Grondin, Gabrielle Scalabrino, Zouhair Salama, Emeline Potdevin, Philippe Perron, Emeline Lefebvre and Amira Jabbari-Hichri. Thank you for the help and all the fun we had together. French National Research Agency (ANR-09-CP2D-19) is greatly acknowledged for financial support. Finally, I would like to thank my family for their support and understanding during the last three years. I Contents List of Publications 1 List of Communications 2 1. Background and Objectives 3 2. Experimental Description 13 3. List of Catalysts 20 4. References 25 5. Published Results 29 Publication I 31 Publication II 65 Publication III 103 Publication IV 109 Publication V 121 Publication VI 131 Publication VII 159 6. Conclusions 179 Abstract (English, French) 186 II List of Publications The results of this thesis have been published or submitted to publication in several international journals which are listed below: I. Dušan Stošiü and Aline Auroux, Couplings. In: A. Auroux (ed) Calorimetry and Thermal Methods in Catalysis (Springer Series in Materials Science), Springer, Heidelberg, chapter III. II. Dušan Stošiü and Aline Auroux, Characterization of acid-base sites in zeolites. In: A. Auroux (ed) Calorimetry and Thermal Methods in Catalysis (Springer Series in Materials Science), Springer, Heidelberg, chapter IX. III. Dušan Stošiü, Simona Bennici, Jean-Luc Couturier, Jean-Luc Dubois and Aline Auroux, Influence of surface acid-base properties of zirconia and titania based catalysts on the product selectivity in gas phase dehydration of glycerol, Catalysis Communications 17 (2012) 23–28. IV. Dušan Stošiü, Simona Bennici, Sergey Sirotin, Christophe Calais, Jean-Luc Couturier, Jean-Luc Dubois, Arnaud Travert and Aline Auroux, Glycerol dehydration over calcium phosphate catalysts: effect of acidic-basic features on catalytic performance, Applied Catalysis A General 447-448 (2012) 124-134. V. Dušan Stošiü, Simona Bennici, Vesna Rakiü and Aline Auroux, CeO2-Nb2O5 mixed oxide catalysts: preparation, characterization and catalytic activity in fructose dehydration reaction, Catalysis Today 192 (2012) 160– 168. VI. Dušan Stošiü, Simona Bennici, Vladimir Pavloviü, Vesna Rakiü and Aline Auroux, Tuning the acidity of niobia: characterization and catalytic activity of Nb2O5-MeO2 (Me = Ti, Zr, Ce) mesoporous mixed oxides, ChemCatChem, submitted. VII. Vladislav Rac, Vesna Rakiü, Zoran Miladinoviü, Dušan Stošiü and Aline Auroux, Influence of desalinication proces on the acidity of HZSM-5 zeolite, Thermochimica Acta, accepted. 1 List of Communications I. Conference of Yugoslav Materials Science Society (YUCOMAT), 6í10th Sep., 2010: Herceg Novi, Montenegro, Preparation and characterization of CeO2-Nb2O5 mixed- oxide catalysts, Dušan Stošiü, Vesna Rakiü, Simona Bennici and Aline Auroux, Oral presentation. II. VII International Symposium on Group Five Elements, 8-11th May, 2011: Riccione, Italy, CeO2-Nb2O5 mixed-oxide catalysts: preparation, characterization and catalytic activity, Dušan Stošiü, Vesna Rakiü, Simona Bennici and Aline Auroux, Oral presentation. III. EUROPACAT X Congress, 28th Aug. – 2th Sep., 2011: Glasgow, Scotland, Influence of surface acid-base properties on the product selectivity in gas phase oxidation of glycerol, Dušan Stošiü, Simona Bennici, Jean-Luc Couturier, Jean-Luc Dubois and Aline Auroux, Poster. IV. 12th European Meeting on Environmental Chemistry (EMEC 12), 7-10th Dec., 2011: Clermont-Ferrand, France, Influence of the acid-base properties of oxide catalysts in fructose dehydration to 5-HMF, Reem Kourieh, Dušan Stošiü, Vesna Rakiü, Simona Bennici and Aline Auroux, Poster. V. 15th International Congress on Catalysis (ICC 15), 1-6th July, 2012: Munich, Germany, Reactivity of methanol over Nb2O5-CeO2 multifunctional catalysts: Microcalorimetry, FT-IR, TPR and TPD-MS studies, Dušan Stošiü, Simona Bennici, Vesna Rakiü and Aline Auroux, Poster.