Abstract
Zirconium silicalite-1 (ZS-1) catalysts with MFI structure were prepared using a hydrothermal synthesis method. XRD, SEM, IR,29Si MAS NMR, UV-VIS DRS, physical adsorption of nitrogen, and elemental analysis were then performed to evaluate its physico-chemical properties, and evidences of Zr4+ incorporation into the zeolite framework were provided : The unit cell volume of zirconium silicalite-1 increased linearly with increases in zirconium content, and the characteristic framework i.r. spectra shifted to lower frequencies as Zr4+ was incorporated into the silicalite-1 lattice. For its catalytic reaction test, liquid phase 2-butanol oxidation using hydrogen peroxide as an oxidant was carried out. All of the zirconium silicalite-1 samples synthesized were active for the 2-butanol oxidation, but activities obtained using ZS-1 catalysts were lower than TS-1 catalyst. Zirconium in the zeolite frameworkwas found to be the active site for the 2-butanol oxidation.
Article PDF
Similar content being viewed by others
Avoid common mistakes on your manuscript.
References
Blasco, T., Camblor, M. A., Corma, A. and Perez-Pariente, J., “The State of Ti in Titanoaluminosilicates Isomorphous with Zeolite Β”,J. Am. Chem. Soc.,115, 11806 (1993).
Boccuti, M.R., Rao, K.M., Zecchina, A., Leofanti, G. and Petrini, G., “Spectroscopic Characterization of Silicalite and Titanium Silicalite”, Stud. Surf. Sci. Catal.,48, Morterra, C. et al., eds., Elsevier, Amsterdam, 133 (1989).
Breck, D.W., “Structure of Zeolites by Infrared Spectroscopy”, Zeolite Molecular Sieves, Wiley, New York, 415 (1974).
Clerici, M. G. and Ingallina, P., “Epoxidation of Lower Olefins with Hydrogen Peroxide and Titanium Silicalite”,J. Catal.,140, 71 (1993).
Corma, A., Navarro, M. T. and Perez-Pariente, J., “Synthesis of an Ultralarge Pore Titanium Silicate Isomorphous to MCM-41 and Its Application as a Catalysts for Selective Oxidation of Hydrocarbons”,J. Chem. Soc., Chem. Commun.,147 (1994).
Dongare, M. K., Singh, P., Moghe, P. P. and Ratnasamy, P., “Synthesis and Characterization, and Catalytic Properties of [Zr]-ZSM-5”,Zeolites,11, 690 (1991).
Engelhardt, G. and Michel, D., “High-Resolution Solid-State NMR of Silicates and Zeolites”, John Wiley & Sons, New York, 1987.
Esposito, A., Neri, C. and Buonomo, F., “Process for Oxidizing Alcohols to Aldehydes and/or Ketones”, US patent, 4, 480135, 1984.
Fricke, R., Kosslick, H., Tuan, V. A., Grohmann, I., Pilz, W., Storek, W. and Walther, G., “Study on the Isomorphous Substitution of Silicon by Tetravalent Elements (Zr, Ge, Ti) in the Framework of MFI Type Zeolites”, Stud. Surf. Sci. Catal., 83, Hattori, T. and Yashima, T., eds., Elsevier, Amsterdam, 57 (1993).
Huybrechts, D.R.C., De Bruycker,L. and Jacobs, P.A., “Oxyfunctionalization of Alkanes with Hydrogen Peroxide on Titanium Silicalite”,Nature,345, 240 (1990).
Ko, Y. S. and Ahn, W. S., “Characterization and Catalytic Properties of Titanium Silicalite-1 Catalyst”,Korean J. Chem. Eng.,15(2), 182 (1997a).
Ko, Y. S. and Ahn, W. S., “Isomorphous Substitution of Fe3+ in Zeolite LTL”,Microporous Materials,9, 131 (1997b).
Kraushaar, B. and van Hooff, J.H. C., “A New Method for the Preparation of Titanium-Silicalite (TS-1)”,Catal. Lett.,1, 81 (1988).
Kraushaar, B. and van HooffJ.H. C., “A Test Reaction for Titanium Silicalite Catalysts”,Catal. Lett.,2, 43 (1989).
Perego, G., Bellussi, G., Corno, C., Taramasso, M., Buonomo, F. and Esposito, A., “Titanium Silicalite: A Novel Derivative in the Pentasil Family”, Stud. Surf. Sci. Catal., 28, Murakami, Y., eds., Elsevier, Amsterdam, 129 (1986).
Reddy, J. S., Kumar, R. and Ratnasamy, P., “Titanium Silicalite-2: Synthesis, Characterization and Catalytic Properties”,Appl. Catal.,58, L1 (1990).
Serrano, D. P., Li, H. X. and Davis, M. E., “Synthesis of Titanium-containing ZSM-48”,J. Chem. Soc., Chem. Commun., 745 (1992).
Tangaraj, A., Kumar, R., Mirajkar, S. P. and Ratnasamy, P., “Catalytic Properties of Crystalline Titanium Silicalites”,J. Catal.,130, 1 (1991).
Taramasso, M., Perego, G. and Notari, B., “Preparation of Porous Crystalline Synthetic Material Comprised of Silicon and Titanium Oxides”, US patent, 4, 410501, 1983.
Tatsumi, T., Nakamura, M., Negishi, S. and Tominaga, H., “Shape Selective Oxidation of Alkanes with H2O2 Catalysed by Titanosilicate”,J. Chem. Soc., Chem. Commun., 476 (1990).
van der Pol,A.J.H.P. and van Hooff, J.H.C., “Oxidation of Linear Alcohols with Hydrogen Peroxide over Titanium Silicalite 1”,Appl Catal A:General,106, 97 (1993).
Wang, G.-R., Wang, X.-Q, Wang, X.-S. and Yu, S.-X., “Synthesis and Catalytic Reaction of [Zr] ZSM-5”, Stud. Surf. Sci. Catal., 83, Hattori, T. and Yashima, T., eds., Elsevier, Amsterdam, 67 (1993).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Ko, Y.S., Ahn, W.S. Synthesis and characterization of zirconium silicalite-1. Korean J. Chem. Eng. 15, 423–428 (1998). https://doi.org/10.1007/BF02697133
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1007/BF02697133