Synthesis and Characteristics of ZSM-5 Zeolite Prepared from Water Glass

Hoon-Hee Woo; Ji-Sook Hong; Jeong-Kwon Suh; Kwan-Young Lee; Jung-Min Lee

Journal of Industrial and Engineering Chemistry, Vol.10, No.4, 645-652, July, 2004

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Synthesis and Characteristics of ZSM-5 Zeolite Prepared from Water Glass

Hoon-Hee Woo, Ji-Sook Hong, Jeong-Kwon Suh , Kwan-Young Lee^{1, †}, and Jung-Min Lee

Applied Chemistry & Engineering Division, Korea Research Institute of Chemical Technology, Daejeon 305-600, Korea
¹Department of Chemical Engineering, Korea University, Seoul 136-701, Korea

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ZSM-5 was synthesized from water glass as the silica source and Al(OH)₃ as Al source. Water glass is an inexpensive silica source, but controlling the reactant composition was difficult because of the high alkali content in water glass. Considering environmental and economic concerns, we propose a new alkali extraction method using methanol to remove the alkali ingredients from water glass. When the MeOH/SiO₂ molar ratio was 3, the maximum extraction of alkali components occurred. After extracting with MeOH, the filtrates were analyzed by UV spectroscopy and titration methods, and we determined the Al₂O₃:SiO₂:Na₂O: H₂O molar ratio to be 1:58:7.55:1510. Crystallization by hydrothermal synthesis was performed at various reaction temperatures and times. Characterizations were carried out by means of XRD and SEM. ZSM-5 display a characteristic MFI peak in its XRD pattern and its crystals have planar shapes and 1 ~ 2 μm particle sizes. Alkali extraction using methanol in a template-free system is a better method for controling the level of Na₂O in water glass used for ZSM-5 synthesis.

Keywords:ZSM-5;water glass;extraction;hydrothermal synthesis;template-free

[References]

Barrer RM, J. Chem. Soc., 127, 2158 (1948)
Broussard L, Shoemaker DP, J. Am. Chem. Soc., 82, 1041 (1960)
Kostinko JA, ACS Symp. Ser. 218, G.D. Stucky and F.G. Dwyer, Eds., p. 3, ACS, Washington, D.C. (1983)
Lee KH, Shin DH, J. Ind. Eng. Chem., 9(5), 584 (2003)
Barrer RM, Zeolites, 1, 130 (1981)
Ryu JC, Ryu TG, Yoo SJ, Hwang JY, Kim YH, Yang HS, J. Ind. Eng. Chem., 9(6), 735 (2003)
Breck DW, Zeolites Molecular Sieves, 10th Ed., p. 771, Wiley, New York (1974)
U.S. Patent, 3,702,886 (1972)
Schwieger W, Berk KH, Freude D, Hunger M, Pfeifer H, ACS Symp. Ser. 398, M.L. Occelli and H.E. Robson, Eds., p. 274, ACS, Los Angeles (1989)
Nastro A, Aiello R, Successful Design Catal., 44, 227 (1988)
Narita E, Sato K, Yatabe N, Okabe T, Ind. Eng. Chem. Prod. Res. Dev., 24, 507 (1985)
Berak JM, Mostowcz R, Stud. Surf. Sci. Catal., 28, 47 (1985)
Shiralkar VP, Clearfield A, Zeolites, 9, 363 (1989)
Dai FY, Suzuki M, Takahashi H, Saito T, Am. Chem. Soc., 18, 244 (1989)
Schwieger W, Berk KH, Freude D, Hunger M, Pfeifer H, Zeolite Synthesis, ACS Symp. Ser. 398, M.L. Occelli and H.E. Robson, Eds., p. 244, ACS, Los Angeles (1989)
Beagley B, Dwyer J, Fitch FR, Mann R, Walter J, J. Phys. Chem., 88, 1744 (1984)
Kulkarni SB, Shiralkar VP, Kotasthane AN, Borade RB, Ratnasamy P, Zeolites, 2, 313 (1982)
Zhdanove SR, Adv. Chem. Ser. 101, E.M. Flanigen and R.W. Grose, Eds., p. 20, ACS, Washington, D.C. (1971)
Pingovschi E, Merches M, Kim CS, Rev. Roum. Chim., 34, 1055 (1989)
Ciric J, J. Colloid Interface Sci., 28, 315 (1968)
Shiralkar VP, Joshi PN, Eapen MJ, Rao BS, Zeolites, 11, 511 (1991)
Xu WY, Li JQ, Li WY, Zhang HM, Liang BC, Zeolites, 9, 468 (1989)
Nastro A, Ciambelli P, Crea F, Aiello R, J. Therm. Anal., 33, 941 (1988)
Jansen JC, Engelen CWR, van Bekkum H, ACS Symp. Ser. 398, M.L. Occelli and H.E. Robson, Eds., p. 257, ACS, Los Angeles (1989)
Coudurier G, Naccache C, Verkine JC, J. Chem. Soc.-Chem. Commun., 24, 1414 (1982)
Triantafillidis CS, Vlessidis AG, Evmiridis NP, Microporous Mesoporous Mater., 47, 369 (2001)
Huang CL, Yu WC, Lee TY, Chem. Eng. Sci., 41, 625 (1986)
Das J, Bhattacharya A, Mitra S, Kumar SR, J. Ind. Chem. Soc., 69, 167 (1991)
Shiralkar VP, Clearfield A, Zeolites, 9, 363 (1989)
Kim SS, Jainisha S, Thomas J, Chem. Mater., 15, 1664 (2003)
Gregg SJ, Adsorption, Surface Area and Porosity, 2nd Ed., p. 195, Academic Press, London (1982)

[Referenced By]

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[1] Barrer RM, J. Chem. Soc., 127, 2158 (1948)

[2] Broussard L, Shoemaker DP, J. Am. Chem. Soc., 82, 1041 (1960)

[3] Kostinko JA, ACS Symp. Ser. 218, G.D. Stucky and F.G. Dwyer, Eds., p. 3, ACS, Washington, D.C. (1983)

[4] Lee KH, Shin DH, J. Ind. Eng. Chem., 9(5), 584 (2003)

[5] Barrer RM, Zeolites, 1, 130 (1981)

[6] Ryu JC, Ryu TG, Yoo SJ, Hwang JY, Kim YH, Yang HS, J. Ind. Eng. Chem., 9(6), 735 (2003)

[7] Breck DW, Zeolites Molecular Sieves, 10th Ed., p. 771, Wiley, New York (1974)

[8] U.S. Patent, 3,702,886 (1972)

[9] Schwieger W, Berk KH, Freude D, Hunger M, Pfeifer H, ACS Symp. Ser. 398, M.L. Occelli and H.E. Robson, Eds., p. 274, ACS, Los Angeles (1989)

[10] Nastro A, Aiello R, Successful Design Catal., 44, 227 (1988)

[11] Narita E, Sato K, Yatabe N, Okabe T, Ind. Eng. Chem. Prod. Res. Dev., 24, 507 (1985)

[12] Berak JM, Mostowcz R, Stud. Surf. Sci. Catal., 28, 47 (1985)

[13] Shiralkar VP, Clearfield A, Zeolites, 9, 363 (1989)

[14] Dai FY, Suzuki M, Takahashi H, Saito T, Am. Chem. Soc., 18, 244 (1989)

[15] Schwieger W, Berk KH, Freude D, Hunger M, Pfeifer H, Zeolite Synthesis, ACS Symp. Ser. 398, M.L. Occelli and H.E. Robson, Eds., p. 244, ACS, Los Angeles (1989)

[16] Beagley B, Dwyer J, Fitch FR, Mann R, Walter J, J. Phys. Chem., 88, 1744 (1984)

[17] Kulkarni SB, Shiralkar VP, Kotasthane AN, Borade RB, Ratnasamy P, Zeolites, 2, 313 (1982)

[18] Zhdanove SR, Adv. Chem. Ser. 101, E.M. Flanigen and R.W. Grose, Eds., p. 20, ACS, Washington, D.C. (1971)

[19] Pingovschi E, Merches M, Kim CS, Rev. Roum. Chim., 34, 1055 (1989)

[20] Ciric J, J. Colloid Interface Sci., 28, 315 (1968)

[21] Shiralkar VP, Joshi PN, Eapen MJ, Rao BS, Zeolites, 11, 511 (1991)

[22] Xu WY, Li JQ, Li WY, Zhang HM, Liang BC, Zeolites, 9, 468 (1989)

[23] Nastro A, Ciambelli P, Crea F, Aiello R, J. Therm. Anal., 33, 941 (1988)

[24] Jansen JC, Engelen CWR, van Bekkum H, ACS Symp. Ser. 398, M.L. Occelli and H.E. Robson, Eds., p. 257, ACS, Los Angeles (1989)

[25] Coudurier G, Naccache C, Verkine JC, J. Chem. Soc.-Chem. Commun., 24, 1414 (1982)

[26] Triantafillidis CS, Vlessidis AG, Evmiridis NP, Microporous Mesoporous Mater., 47, 369 (2001)

[27] Huang CL, Yu WC, Lee TY, Chem. Eng. Sci., 41, 625 (1986)

[28] Das J, Bhattacharya A, Mitra S, Kumar SR, J. Ind. Chem. Soc., 69, 167 (1991)

[29] Shiralkar VP, Clearfield A, Zeolites, 9, 363 (1989)

[30] Kim SS, Jainisha S, Thomas J, Chem. Mater., 15, 1664 (2003)

[31] Gregg SJ, Adsorption, Surface Area and Porosity, 2nd Ed., p. 195, Academic Press, London (1982)