MCM-41 분자체의 합성에 초기 pH가 미치는 영향

김화중; 유재철

Journal of the Korean Industrial and Engineering Chemistry, Vol.8, No.3, 463-472, June, 1997

Export Citation

MCM-41 분자체의 합성에 초기 pH가 미치는 영향

The Effect of Initial pH on the Synthesis of Mesoporous Molecular Sieve, MCM-41

김화중, 유재철

초록

Mesoporous 분자체인 MCM-41의 합성시, 수열 반응 전에 실시되는 반응용액의 초기 pH 조절이 MCM-41의 합성 및 특성에 미치는 영향에 관하여 연구하였다. 반응중간에 추가적인 pH의 조절없이, 초기 반응용액에 대한 1회의 pH 조절을 통하여 30Å에서 40Å에 이르는 기공 크기 및 1000㎡/g 이상의 높은 비표면적을 갖는 MCM-41 분자체를 합성할 수 있었다. 그 결과, pH 조절은 실리카원으로 사용되는 polymeric Na⁺-silicate로부터 반응성이 높은 monomeric Na⁺-silicate를 원활하게 공급되도록 하여 우수한 열적 안정성을 나타내며 hexagonal 구조가 발달된 MCM-41의 명성에 큰 영향을 미친다는 것을 확인할 수 있었다

A mesoporous molecular sieve, MCM-41, was synthesized and the effent of various initial pH of reaction mixtures on the synthesis and physical properties of MCM-41 was investigated. Adjustment of initial pH for reaction mixtures was made before starting hydrothermal reaction rather than during the reaction. Highly crystalline MCM-41 which shows pore diameters of 30Å to 40Å and specific surface areas greater than l000㎡/g has been successfully prepared through a single adjustment of initial pH. Results also suggest that the initial pH adjustment has a significant effect on the formation of MCM-41 with a long-range ordered hexagonal array and an excellent thermal stability. Finally, it is speculated that the adjustment of initial pH might accelerate the dissolution of stable polymeric sodium silicate to highly reactive monomeric sodium silicate resulting in well-ordered MCM-41.

[References]

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[1] IUPAC Manual of Symbols and Termunology, Appendix 2, Part 1, Colloid and Surface Chemistry, Pure Appl. Chem., 31, 578 (1972)

[2] Chen NY, Degnan TF, Chem. Eng. Process., 32 (1988)

[3] Weekman VW, Voltz SE, Nace DM, Ind. Eng. Chem. Process Des. Dev., 10, 530 (1971)

[4] Chen NY, Garwood WE, Catal. Rev.-Sci. Eng., 28, 185 (1986)

[5] Dwyer FG, Lewis FJ, Schneider FH, Chem. Eng., 5, 90 (1976)

[6] Dessau RM, Schlenker JL, Higgins JB, Zeolites, 10, 522 (1990)

[7] Bekkum HV, Flanigen EM, Jansen JC, Stud. Surf. Sci. Catal., 58, 137 (1990)

[8] Davis ME, Saldarriage C, Montes C, Garces C, Crowder C, Nature, 331, 698 (1988)

[9] Bekkum HV, Flanigen EM, Jansen JC, Stud. Surf. Sci. Catal., 58, 24 (1990)

[10] Eastermann M, McCuster LB, Baerlocher C, Merrouche A, Kessler H, Nature, 352, 320 (1991)

[11] Szostak R, Molecular Sieves Principles of Synthesis and Identification, Van Nostrand Reinhold, New York, 205 (1989)

[12] Vaughan DEW, Lussier RJ, In Proceeding of the 5th International Conference on Zeolites, L.V.C. Rees, Ed, Hyden. 94 (1980)

[13] Meier WM, In Studies in Surface Science & Catalsis, Y. Murakami, A. Iijima, and J.W. Ward, Eds., Elsevier Science, 28, 13 (1986)

[14] Vaughan DEW, ACS Symp. Ser., 368, 308 (1988)

[15] Landis ME, Aufdembrink BA, Chu P, Johnson ID, Kirker GW, Rubin MK, J. Am. Chem. Soc., 113, 3189 (1991)

[16] Kresge CT, Leonowicz ME, Roth WJ, Vartuli J, Beck JS, Nature, 359, 710 (1992)

[17] Landis ME, J. Am. Chem. Soc., 113, 3189 (1991)

[18] Yanagisawa T, Shimizu T, Kazuyuki K, Kato C, Bull. Chem. Soc. Jpn., 63, 988 (1990)

[19] Kresge CT, Leonowicz ME, Roth WJ, Vartuli JC, U.S. Patent, 5,098,684 (1992)

[20] Kresge CT, Leonowicz ME, Roth WJ, Vartuli JC, U.S. Patent, 5,102,643 (1992)

[21] Hue QS, Margolese DI, Ciesla U, Feng PY, Gier TE, Sieger P, Leon R, Petroff PM, Schuth F, Stucky GD, Nature, 368(6469), 317 (1994)

[22] Huo Q, Margolese DL, Cielsa U, Demuth DG, Feng P, Gier TE, Sieger A, Firouzi BF, Chmelka BF, Schuth F, Stucky GD, Chem. Mater., 6, 1176 (1994)

[23] Chen CY, Li HX, Davis ME, Microporous Mater., 2, 27 (1993)

[24] Steel A, Carr SW, Anderson MW, J. Chem. Soc.-Chem. Commun., 1571 (1994)

[25] Vartuli JC, Schmidt KD, Kresge CT, Roth WJ, Leonowicz M, McCullen SB, Hellring SD, Beck JS, Schlenker JL, Olson DH, Sheppard EW, In Zeolites and Related Microporous Materials, State of the Art 1994, Studies in Surface Science and Catalysis, Weitkamp, J., Karge, H.G, Pfeifer, J. and Holderich, W., Eds., Elsevier Science, 84, 53 (1994)

[26] Monnier A, Schuth F, Huo Q, Kumar D, Margolese D, Maxwell RS, Stucky CD, Krishnamurty M, Petroff PM, Firouzi A, Janicke M, Chmelka BF, Science, 26, 1299 (1993)

[27] Xiu S, Zhao GQ, Millar GJ, Ind. Eng. Chem., 35, 2075 (1996)

[28] Ryoo R, Kim JM, J. Chem. Soc.-Chem. Commun., 711 (1995)

[29] Ryoo R, Kim JM, Shin CH, Lee JY, 11th International Zeolite Conference (IZC), Seoul, Korea (1996)

[30] Schmidt R, Akporiaye D, Stocker M, HanrikEllestad O, In Zeolites and Related Microporous Materials: State of the Art 1994, Studies in Surface Science and Catalysis, J. Weitkamp, H.G. Karge, J. Pfeifer, W. Holderich, Eds., Elsevier Science, 84, 61 (1994)