Hydrothermal Synthesis and Characterization of Niobium-containing Silicalite-1 Molecular Sieves with MFI Structure

Yong Sig Ko; HyunTae Jang; Inha University

Journal of Industrial and Engineering Chemistry, Vol.13, No.5, 764-771, September, 2007

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Hydrothermal Synthesis and Characterization of Niobium-containing Silicalite-1 Molecular Sieves with MFI Structure

Yong Sig Ko^†, HyunTae Jang¹, and Inha University²

Department of Advanced Material Chemistry, Shinsung College, Dangjin-gun 343-860, Korea
¹Department of Chemical Engineering, Hanseo University, Seosan 356-706, Korea
²Department of Chemical Engineering, College of Engineering, Inha University, Inchon 402-751, Korea

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Abstract:Niobium silicalite-1 (NbS-1) molecular sieves with MFI structure were prepared using the hydrothermal synthesis method. X-ray diffraction, scanning and transmission electron microscopies, Fourier transform infrared spectroscopy, ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy, 29 Si magic-angle spinning nuclear magnetic resonance spectroscopy, ammonia temperature-programmed desorption (NH3-TPD), physical adsorption of nitrogen and elemental analysis were then performed to evaluate their physico-chemical properties and to provide evidences for the incorporation of Nb5+ into the zeolite framework. The unit cell volume of niobium silicalite-1 increased linearly with increasing niobium content, suggesting isomorphous substitution of Si4+ by Nb5+ in the lattice framework. The framework infrared spectrum showed a characteristic absorption band at 963 cm-1, probably due to Si-O-Nb linkages. In the UV-vis spectrum, the absorption assigned to the presence of Nb5+ in the zeolite framework was observed at around 200 nm. In addition, NH3-TPD studies revealed weak acidity in niobium silicalite-1 due possibly to [Nb...(OH)-Si] sites in the framework.

Keywords:niobium;niobium silicalite-1;hydrothermal synthesis;NH3-TPD;isomorphous substitution;characterization;FT-IR;UV-vis DRS

[References]

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Jo HJ, Ahn BJ, Gang MS, Ko SB, Chang W, J. Ind. Eng. Chem., 12(5), 689 (2006)
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[1] U.S. Patent 4, 410, 501 (1983)

[2] Dongare MK, Singh P, Moghe PP, Ratnasamy P, Zeolites, 11, 690 (1991)

[3] Fricke R, Kosslick H, Tuan VA, Grohmann I, Pilz W, Storek W, Walther G, Zeolites and Microporous Crystals, Studies in Surface Science and Catalysis, T. Hattori and T. Yashima Eds., 83, p. 57, Elsevier, Amsterdam (1993)

[4] Wang GR, Wang XQ, Wang XS, Yu SX, Zeolites and Microporous Crystals, Studies in Surface Science and Catalysis, T. Hattori and T. Yashima Eds., 83, p. 67, Elsevier, Amsterdam (1993)

[5] Prasad Rao PRH, Belhekar AA, Hegde SG, Ramaswamy AV, Ratnasamy P, J. Catal., 141, 595 (1993)

[6] Tuel A, Ben Taarit Y, Zeolites, 14, 18 (1994)

[7] Sen T, Chatterjee M, Sivasanker S, J. Chem. Soc., Commun., 207 (1995)

[8] Jo HJ, Ahn BJ, Gang MS, Ko SB, Chang W, J. Ind. Eng. Chem., 12(5), 689 (2006)

[9] Heon UM, Kang M, J. Ind. Eng. Chem., 11(4), 540 (2005)

[10] Reddy KR, Ramaswamy AV, Ratnasamy P, J. Catal., 143, 275 (1993)

[11] Yoshida S, Tanaka T, Okada M, Funabiki T, J. Chem. Soc.-Faraday Trans., 80, 119 (1984)

[12] Tanaka T, Ooe M, Funabiki T, Yoshida S, J. Chem. Soc.-Faraday Trans., 82, 35 (1986)

[13] Tanabe T, Nishimura Y, Kawasaki S, Funabiki T, Yoshida S, J. Chem. Soc. Chem. Commun., 506 (1987)

[14] Tanabe K, CHEMTECH, October, 628 (1991)

[15] Brandao P, Philippou A, Rocha J, Anderson MW, Catal. Lett., 80, 99 (2002)

[16] Nishimura M, Asakura K, Iwasawa Y, J. Chem. Soc. Chem. Commun., 1660 (1986)

[17] Shirai M, Ichikumi N, Asakura K, Wasawa JI, Catal. Today, 8, 57 (1990)

[18] Desponds O, Keiski RL, Somorjai GA, Catal. Lett., 19, 17 (1993)

[19] Okazaki S, Wada N, Catal. Today, 16, 349 (1993)

[20] Ziolek M, Sobczak I, Nowak I, Decyk P, Lewandowska A, Kujawa J, Microporous Mesoporous Mater., 35, 195 (2000)

[21] Morikawa A, Togashi A, Catal. Today, 16, 333 (1993)

[22] Philippou A, Brandao P, Ghanbari-Siahkali A, Dwyer J, Rocha J, Anderson MW, Appl. Catal. A: Gen., 207(1-2), 229 (2001)

[23] Jehng JM, Wachs IE, Catal. Today, 16, 417 (1993)

[24] Kushimoto T, Ozawa Y, Baba A, Matsuda H, Catal. Today, 16, 571 (1993)

[25] Rocha J, Brandao P, Pedrosa de Jesus JD, Philippou A, Anderson MW, Chem. Commun., 471 (1999)

[26] Prakash AM, Kevan L, J. Am. Chem. Soc., 120(50), 13148 (1998)

[27] Ziolek M, Nowak I, Zeolites, 18, 356 (1997)

[28] Sobczak I, Decyk P, Ziolek M, Daturi M, Lavalley JC, Kevan L, Prakash AM, J. Catal., 207, 101 (2002)

[29] Hari Prasad Rao PR, Ramaswamy AV, Ratnasamy P, J. Catal., 137, 225 (1992)

[30] Reddy KR, Ramaswamy AV, Ratnasamy P, J. Chem. Soc. Chem. Commun., 1613 (1992)

[31] Ko YS, Ahn WS, Korean J. Chem. Eng., 15(4), 423 (1998)

[32] Shibata M, Gabelica Z, Zeolites, 19, 246 (1997)

[33] Mal NK, Ramaswamy V, Rajamohanan PR, Ramaswamy AV, Microporous Mater., 12, 331 (1997)

[34] Boccuti MR, Rao KM, Zecchina A, Leofanti G, Petrini G, Structure and Reactivity of Surfaces, Studies in Surface Science and Catalysis, C. Morterra, A. Zecchina and G. Costa Eds., 48, p. 133, Elsevier, Amsterdam (1989)

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

[36] Breck DW, Zeolite Molecular Sieves: Structure, Chemistry and Use, p. 415, Wiley, New York (1974)

[37] Reddy JS, Kumar R, Ratnasamy P, Appl. Catal., 57, L1 (1990)

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

[39] van der Pol AJHP, Verduyn AJ, Hooff JHC, Appl. Catal. A: Gen., 92, 113 (1992)

[40] Rakshe B, Ramaswamy V, Hegde SG, Vetrivel R, Ramaswamy AV, Catal. Lett., 45, 41 (1997)

[41] Ben Taarit Y, Tuel A, Velmasco N, Naccache C, Fr. Patent 9 203 364 (1992)

[42] Tuel A, Ben Taarit Y, J. Chem. Soc., Chem. Commun., 1578 (1992)

[43] Axon SA, Klinowski, Appl. Catal. A: Gen., 81, 27 (1992)