CHARACTERIZATION AND CATALYTIC PROPERTIES OF TITANIUM SILICALITE-1 CATALYST

Ko YS; Ahn WS

Korean Journal of Chemical Engineering, Vol.15, No.2, 182-191, March, 1998

Titanium silicalite 1 (TS-1) catalyst was prepared by three different hydrothermal synthesis methods. XRD, elemental analysis, SEM, IR, ²⁹Si MAS NMR, UV-vis DRS, physical adsorption of nitrogen, and EXAFS analysis were then performed to evaluate its physical properties. For a test of catalytic activity, liquid phase 2-butanol oxidation and 1-hexene epoxidation using hydrogen peroxide as an oxidant were conducted. The crystal size of the TS-1 catalyst was shown to have a considerable effect on the 1-hexene epoxidation, and smaller crystals resulted in higher activity.

Keywords:TS-1;Characterization;Morphology;Oxidation;Epoxidation

[References]

Babonneau F, Daeuff S, Leaustic A, Sanchez C, Cartier C, Verdaguer M, Inorg. Chem., 27, 3166 (1988)
Behrens P, Felsche J, Vetter S, Schults-Ekloff G, Jaeger NI, Nieman WJ, J. Chem. Soc.-Chem. Commun., 678 (1991)
Blasco T, Camblor MA, Corma A, Perez-Pariente J, J. Am. Chem. Soc., 115, 11806 (1993)
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Bordiga S, Boscherini F, Coluccia S, Genoni F, Lamberti C, Leofanti G, Marchese L, Petrini G, Vlaic G, Zecchina A, Catal. Lett., 26(1-2), 195 (1994)
Clark RJH, "Chemistry of Titanium and Vanadium," El-sevier, Amsterdam, 272 (1968)
Clerici MG, Ingallina P, J. Catal., 140, 71 (1993)
Esposito A, Neri C, Buonomo F, "Process for Oxidizing Alcohols to Aldehydes and/or Ketones," U.S. Patent, 4,480,135 (1984)
Frenkel AI, Stern EA, Voronel A, Qian M, Newville M, Phys. Rev., B, Condens. Matter, 48, 12449 (1993)
Greegor R, Lytle FW, Sandstrom DR, Wong J, Schultz P, J. Non-Cryst. Solids, 55, 27 (1983)
Huybrechts DRC, Buskens PL, Jacobs PA, J. Mol. Catal., 71, 129 (1992)
Huybrechts DRC, De Bruycker L, Jacobs PA, Nature, 345, 240 (1990)
Huybrechts DRC, Vaesen I, Li HX, Jacobs PA, Catal. Lett., 8, 237 (1991)
Kim GJ, Cho BR, HWAHAK KONGHAK, 31(6), 658 (1993)
Kim JK, Ko YS, Kim TJ, Ahn WS, HWAHAK KONGHAK, 33(4), 511 (1995)
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Kraushaar B, van Hooff JHC, Catal. Lett., 2, 43 (1989)
Lee JH, Jung KT, Shul YG, HWAHAK KONGHAK, 34(6), 765 (1996)
Notari B, Catal. Today, 18, 163 (1993)
Padovan M, Genoni F, Leofanti G, Petrini G, Trezza G, Zecchina A, "Study on Titanium Silicate Synthesis," Stud. Surf. Sci. Catal., 63, Poncelet, G., Jacobs, P.A., Grange, P. and Delmon, B., Eds., Elsevier, Amsterdam, 431 (1991)
Reddy JS, Kumar R, Ratnasamy P, Appl. Catal., 58, L1 (1990)
Reddy KM, Kaliaguine S, Sayari A, Ramaswamy AV, Reddy VS, Bonneviot L, Catal. Lett., 23(1-2), 175 (1994)
Schultz E, Ferrini C, Prins R, Catal. Lett., 14, 221 (1992)
Tangaraj A, Kumar R, Mirajkar SP, Ratnasamy P, J. Catal., 130, 1 (1991)
Taramasso M, Perego G, Notari B, "Preparation of Porous Crystalline Synthetic Materials Comprised of Silicon and Titanium Oxides," U.S. Patent, 4,410,501 (1983)
Tatsumi T, Nakamura M, Negishi S, Tominaga H, J. Chem. Soc.-Chem. Commun., 476 (1990)
Trong OD, Bonneviot L, Bittar A, Sayari A, Kaliaguine S, J. Mol. Catal., 74, 233 (1992)
Tuel A, Diab J, Gelin P, Dufaux M, Dutel JF, Taarit YB, J. Mol. Catal., 63, 95 (1990)
vander Pol AJHP, Verduyn AJ, Van Hooff JHC, Appl. Catal., 92, 113 (1992)
vander Pol AJHP, van Hooff JHC, Appl. Catal. A: Gen., 106, 97 (1993)
Yarker CA, Johnson PAV, Wright AC, Wong J, Greegor RB, Lytle FW, Sinclair RN, J. Non-Cryst. Solids, 79, 117 (1986)
Zecchina A, Spoto G, Bordiga S, Ferrero A, Petrini G, Leofanti G, Padovan M, "Framework and Extraframework Ti in Titanium-Silicalite: Investigation by Means of Physical Methods," Zeolite Chemistry and Catalysis, Jacobs, P.A., Jaeger, N.I., Kubelkova, L. and Wichterlova, B., eds., Elsevier, Amsterdam, 251 (1991)

[Referenced By]

[1] Babonneau F, Daeuff S, Leaustic A, Sanchez C, Cartier C, Verdaguer M, Inorg. Chem., 27, 3166 (1988)

[2] Behrens P, Felsche J, Vetter S, Schults-Ekloff G, Jaeger NI, Nieman WJ, J. Chem. Soc.-Chem. Commun., 678 (1991)

[3] Blasco T, Camblor MA, Corma A, Perez-Pariente J, J. Am. Chem. Soc., 115, 11806 (1993)

[4] Boccuti MR, Rao KM, Zecchina A, Leofanti G, Petrini G, "Spectroscopic Characterization of Silicalite and Titanium Silicalite," Stud. Surf. Sci. Catal., 48, Morterra, C. et. al., eds., Elsevier, Amsterdam, 133 (1989)

[5] Bordiga S, Boscherini F, Coluccia S, Genoni F, Lamberti C, Leofanti G, Marchese L, Petrini G, Vlaic G, Zecchina A, Catal. Lett., 26(1-2), 195 (1994)

[6] Clark RJH, "Chemistry of Titanium and Vanadium," El-sevier, Amsterdam, 272 (1968)

[7] Clerici MG, Ingallina P, J. Catal., 140, 71 (1993)

[8] Esposito A, Neri C, Buonomo F, "Process for Oxidizing Alcohols to Aldehydes and/or Ketones," U.S. Patent, 4,480,135 (1984)

[9] Frenkel AI, Stern EA, Voronel A, Qian M, Newville M, Phys. Rev., B, Condens. Matter, 48, 12449 (1993)

[10] Greegor R, Lytle FW, Sandstrom DR, Wong J, Schultz P, J. Non-Cryst. Solids, 55, 27 (1983)

[11] Huybrechts DRC, Buskens PL, Jacobs PA, J. Mol. Catal., 71, 129 (1992)

[12] Huybrechts DRC, De Bruycker L, Jacobs PA, Nature, 345, 240 (1990)

[13] Huybrechts DRC, Vaesen I, Li HX, Jacobs PA, Catal. Lett., 8, 237 (1991)

[14] Kim GJ, Cho BR, HWAHAK KONGHAK, 31(6), 658 (1993)

[15] Kim JK, Ko YS, Kim TJ, Ahn WS, HWAHAK KONGHAK, 33(4), 511 (1995)

[16] Kim JK, Ko YS, Ann WS, J. Korean Ind. Eng. Chem., 6(4), 626 (1995)

[17] Kraushaar B, van Hooff JHC, Catal. Lett., 1, 81 (1988)

[18] Kraushaar B, van Hooff JHC, Catal. Lett., 2, 43 (1989)

[19] Lee JH, Jung KT, Shul YG, HWAHAK KONGHAK, 34(6), 765 (1996)

[20] Notari B, Catal. Today, 18, 163 (1993)

[21] Padovan M, Genoni F, Leofanti G, Petrini G, Trezza G, Zecchina A, "Study on Titanium Silicate Synthesis," Stud. Surf. Sci. Catal., 63, Poncelet, G., Jacobs, P.A., Grange, P. and Delmon, B., Eds., Elsevier, Amsterdam, 431 (1991)

[22] Reddy JS, Kumar R, Ratnasamy P, Appl. Catal., 58, L1 (1990)

[23] Reddy KM, Kaliaguine S, Sayari A, Ramaswamy AV, Reddy VS, Bonneviot L, Catal. Lett., 23(1-2), 175 (1994)

[24] Schultz E, Ferrini C, Prins R, Catal. Lett., 14, 221 (1992)

[25] Tangaraj A, Kumar R, Mirajkar SP, Ratnasamy P, J. Catal., 130, 1 (1991)

[26] Taramasso M, Perego G, Notari B, "Preparation of Porous Crystalline Synthetic Materials Comprised of Silicon and Titanium Oxides," U.S. Patent, 4,410,501 (1983)

[27] Tatsumi T, Nakamura M, Negishi S, Tominaga H, J. Chem. Soc.-Chem. Commun., 476 (1990)

[28] Trong OD, Bonneviot L, Bittar A, Sayari A, Kaliaguine S, J. Mol. Catal., 74, 233 (1992)

[29] Tuel A, Diab J, Gelin P, Dufaux M, Dutel JF, Taarit YB, J. Mol. Catal., 63, 95 (1990)

[30] vander Pol AJHP, Verduyn AJ, Van Hooff JHC, Appl. Catal., 92, 113 (1992)

[31] vander Pol AJHP, van Hooff JHC, Appl. Catal. A: Gen., 106, 97 (1993)

[32] Yarker CA, Johnson PAV, Wright AC, Wong J, Greegor RB, Lytle FW, Sinclair RN, J. Non-Cryst. Solids, 79, 117 (1986)

[33] Zecchina A, Spoto G, Bordiga S, Ferrero A, Petrini G, Leofanti G, Padovan M, "Framework and Extraframework Ti in Titanium-Silicalite: Investigation by Means of Physical Methods," Zeolite Chemistry and Catalysis, Jacobs, P.A., Jaeger, N.I., Kubelkova, L. and Wichterlova, B., eds., Elsevier, Amsterdam, 251 (1991)