Synthesis and Characterization of Micro/Mesoporous Molecular
Transcription
Synthesis and Characterization of Micro/Mesoporous Molecular
Advanced Micro- and Mesoporous Materials eds. K. Hadjiivanov, V. Valtchev, S. Mintova, G. Vayssilov Heron Press, Sofia, 2008 Synthesis and Characterization of Micro/Mesoporous Molecular Sieves Prepared from ZSM-5 Zeolite S. Habib1 , J.-D. Comparot2 , F. Launay1 , S. Laforge2 , Y. Millot1 , J.-L. Paillaud3 , C. Faust3 , P. Magnoux2 , A. Gédéon1 1 Laboratoire Systèmes Interfaciaux à l’Echelle Nanométrique, CNRS-UMR 7142, Université Pierre et Marie Curie, case 196, 4, place Jussieu, 75252 Paris cedex 05, France 2 Laboratoire de Catalyse en Chimie Organique, CNRS-UMR 6503, Université de Poitiers, 40, avenue du recteur Pineau, 86022 Poitiers cedex, France 3 Laboratoire de Matériaux à Porosité Contrôlée, CNRS-UMR 7016, Ecole Nationale Supérieure de Chimie de Mulhouse, 3, rue Alfred Werner, 68093 Mulhouse cedex, France Abstract Zeolite/mesoporous molecular sieves of ZSM-5/Al-MCM-41 type have been prepared using the zeolite as silica-alumina source in the presence of cetyltrimethylammonium chloride (CTACl) under hydrothermal conditions. The structure, cristallinity and textural properties of the synthesized samples, as well as of the starting material, were investigated by X-ray diffraction (XRD) and adsorption/desorption of nitrogen. The stability of the ZSM-5/MCM-41 materials was studied through their treatment in boiling water for 5 days. The results indicate that these solids are much hydrothermally stable than the conventional Al-MCM-41 and a mechanical mixture with similar Si/Al ratio. The addition of a silica source affords a better structuration of the mesoporous part of the material in comparison to samples synthesized from the sole zeolite crystals. The activity of the micro/mesoporous samples towards the acid-catalysed transformation of methylcyclohexane is compared to those of ZSM-5, Al-MCM-41 and a mechanical mixture. 1 Introduction Microporous aluminosilicates, with their uniform channel size, unique molecular shape selectivity, as well as strong acidity and good thermal/hydrothermal stability, have been widely used as acid catalysts. However, the slow intracrystalline diffusivity and the small micropore size of zeolites have limited their 186