MFI형 구조를 갖는 티타늄 및 지르코늄 실리케이트의 선택적 촉매기능

김건중; 김광호; 고완석; 조동수; 김종호

Journal of the Korean Industrial and Engineering Chemistry, Vol.5, No.4, 714-721, August, 1994

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MFI형 구조를 갖는 티타늄 및 지르코늄 실리케이트의 선택적 촉매기능

Selective Catalytic Properties of MFI type Titanium and Zirconium Silicate

김건중, 김광호, 고완석, 조동수, 김종호

초록

수열법으로 티타늄과 지르코늄이 함유된 MFI형 제올라이트를 조제하고, X선 회절법, FT-IR 및 ²⁹Si MAS NMR 분석을 수행하여 티타늄 및 지르코늄의 제올라이트 격자구조 내로의 도입을 검토하였다. 또한 벤젠 수산화반응과 n-hexane 산화반응을 촉매의 특성 검토를 위한 시험반응으로 이용하였다. 순수한 티타니아와 지르코니아 분말은 이들 반응에 대하여 전혀 활성을 나타내지 못하였으나, 티타늄 및 지르코늄 함유 제올라이트 촉매는 두 반응에 대하여 공히 높은 활성을 보였다. 이들 촉매의 활성은 사용한 용매의 종류에 의해 크게 영향을 받았으며, 전환율은 제올라이트 중의 티타늄과 지르코늄 함량의 증가와 더불어 증가하였다.

Titanium and zirconium-containing MFI type zeolites have been prepared hydrothermally. Incorporation of titanium or zirconium into the framework of zeolite has been demonstrated by XRD, FT-IR, ²⁹Si MAS NMR analysis, and the catalytic benzene hydroxylation or n-hexane oxidation was used for checking the properties of catalysts. Pure titania and zirconia powder showed no catalytic activity at all for these reactions but Ti and Zr modified zeolite had the high activities in both reactions. The catalytic activity strongly depended on the kind of solvents, and the conversion of benzene or n-hexane increased with the increasing content of Ti and Zr in zeolites.

[References]

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[1] Groves JT, Nemo TE, J. Am. Chem. Soc., 105, 6243 (1985)

[2] Cook BR, Reinert TJ, Suslick KS, J. Am. Chem. Soc., 108, 7281 (1986)

[3] Herron N, Tolman CA, J. Am. Chem. Soc., 109, 2837 (1987)

[4] Taramasso M, Notari B, U.S. Patent, 4,410,501 (1983)

[5] Neri C, Anfossi B, Esposito A, Buonomo F, Eur. Patent, 0100119 (1984)

[6] Thangaraj A, Kumar R, Ratnasamy P, Appl. Catal., 57, L1 (1990)

[7] Kraushaar B, VanHooff JHC, Catal. Lett., 2, 43 (1989)

[8] Clerici M, Appl. Catal., 68, 249 (1991)

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

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

[11] Kim GJ, Kwon LM, HWAHAK KONGHAK, 26(3), 261 (1988)

[12] Kraushaar B, VanHooff JHC, Catal. Lett., 1, 81 (1988)

[13] Perego G, Bellussi G, Corus C, Taramasso M, Buonomo F, Esposito A, "New Developments in Zeolite Science and Technology," Kodansha and Elsevier, Tokyo, p. 129 (1986)

[14] Thangaraj A, Kumar R, Sivasanker S, Zeolites, 12, 135 (1992)

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

[16] Kim JH, Namba S, Yashima T, "Zeolites as Catalysts, Sorbents and Detergent Builders," Elsevier, Amsterdam, Vol. 46, 71 (1989)

[17] Kim JH, Namba S, Yashima T, Bull. Chem. Soc. Jpn., 61, 1051 (1988)