이온교환된 Faujasite형 제올라이트의 촉매적 안정성에 대한 시차열분석 및 양자화학적 고찰; 1. Ni<sup>2+</sup>-Faujasite계

김명철; 김종택

Journal of the Korean Industrial and Engineering Chemistry, Vol.4, No.1, 75-81, March, 1993

이온교환된 Faujasite형 제올라이트의 촉매적 안정성에 대한 시차열분석 및 양자화학적 고찰; 1. Ni²⁺-Faujasite계

Differential Thermal Analysis and Quantum Chemical Consideration for Cata1ytic Stability of Ion Exchanged Faujasite Type Zeolite 1. Ni²⁺-Faujasite계

김명철, 김종택

초록

Ni²⁺-Faujasite의 열화학적 안정성을 시차열분석(DTA), 열중량분석(TGA), X선 회절분석(XRD) 및 양자화학적 계산을 통해 고찰하였다. Ni²⁺-Faujasite의 탈수현상은 373-773 K의 온로 구간에서 나타났다. 골격내 T자리를 표현하는 분자모델을 설정하여 전체 에너지와 Wiberg 결합차수를 CND0/2 분자궤도법을 통해 계산하였다. 계산된 결과는 제올라이트의 결정성 감소가 골격내 Al-O결합의 약화에 직접적으로 연관되어 있음을 나타내었다.

The thermochemical stability of Ni²⁺-Faujasite was studied by differential thermal analysis(DTA), thermal gravitational analysis(TGA), X-ray diffraction analysis(XRD) and quantum chemical calculations. Dehydration of Ni²⁺-Faujasite was observed at 373-773K. A CNDO/2 calculations have been applied on cluster models for the representative T sites in faujasite to get total energy and wiberg bond orders. It has proved that the decrease of zeolitic crystallinity is directly related to the weakening of Al-O bonds in framework.

[References]

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[1] Rabo JA, "Zeolite Chemistry and Catalysis," ACS Monograph 171, Washington D.C. (1976)

[2] Murakami Y, "New Developments in Zeolite Science and Technology," Kodansa, Tokyo, pp. 725-732 (1986)

[3] Murakami Y, "New Developments in Zeolite Science and Technology," Kodansa, Tokyo, pp. 811-818 (1986)

[4] Arribas J, J. Catal., 104, 135 (1987)

[5] Aparicio LM, J. Catal., 104, 381 (1987)

[6] Chang CD, "Hydrocarbons from Methanol," Marcel Dekker Inc., New York, pp. 4-35 (1983)

[7] Murakami Y, "New Developments in Zeolite Science and Technology," Kodansa, Tolyo, pp. 875-882 (1986)

[8] Garbwski, J. Phys. Chem., 86, 98 (1988)

[9] Thomas J, J. Am. Chem. Soc., 110, 1801 (1988)

[10] Godber J, J. Phys. Chem., 93, 1409 (1989)

[11] Andersson SLT, J. Phys. Chem., 93, 4913 (1989)

[12] Jozef JVD, J. Phys. Chem., 92, 6740 (1988)

[13] Jozef JVD, J. Phys. Chem., 92, 6747 (1988)

[14] Karge HG, J. Phys. Chem., 94, 765 (1990)

[15] Beran S, J. Phys. Chem., 89, 5586 (1985)

[16] Beran S, J. Phys. Chem., 94, 335 (1990)

[17] No KT, Kim JS, Huh YY, Kim WK, Jhon MS, J. Phys. Chem., 91, 740 (1987)

[18] Coughlam B, Keane MA, Zeolites, 11, 12 (1991)

[19] Subhash B, "Zeolite Catalysis Principles and Applications," CRC Press, Boca Raton (1990)

[20] Pople JA, "Approximate Molecular Orbital Theory," McGraw Hill, New York (1970)

[21] Beran S, J. Phys. Chem., 86, 111 (1982)

[22] Padraig JO, Dwyer J, J. Phys. Chem., 92, 3005 (1988)

[23] Olson DH, J. Phys. Chem., 74, 2758 (1970)

[24] Breck DW, "Zeolite Molecular Sieves," John Wiley & Sons, New York, 369 (1974)

[25] Kim JT, Kim MC, Okamoto Y, Imanaka T, J. Catal., 115, 319 (1989)

[26] Heo NH, Patalinghug WC, Seff K, J. Phys. Chem., 90, 3931 (1986)