本實驗用鈉鋁矽酸玻璃（NaAlSi2O6）碎塊，在氫氧化鈉溶液中合成方沸石，以便研究玻璃溶解與沸石晶核生成之關係。實驗的條件為：玻璃碎塊大小分9∼14目和5∼8目，0.75M、0.5M和0.25M氫氧化鈉溶液，1/60與1/80之固/液比，150℃、180℃與210℃，飽和蒸汽壓。
實驗結果顯示，玻璃的溶解速率隨溫度與氫氧化鈉溶液濃度的增加而增加；溫度與濃度不變時，玻璃溶解速率隨固／液比減少而增加；也隨玻璃粒徑之減少而增加。方沸石晶核的生成量隨時間約成常態分布曲線的關係。玻璃成分在溶液中的濃度隨時間的增加而增加，當溶液濃度最高時，方沸石晶核生成量最大。溶解較快之反應系統，當玻璃接近完全溶解時，溶液濃度達最高，當溶液濃度下降到穩定狀態時（即方沸石的飽和濃度），晶核生成才停止。溶解較慢之反應系統，當玻璃完全溶解前溶液濃度達最高，當玻璃完全溶解時，溶液濃度已下降到穩定狀態，此時晶核生成已停止。

Synthetic glass (Na2O  Al2O3  4SiO2) was used as the starting material to synthesize analcime in NaOH solutions in order to investigate the relationship between the glass dissolution and the nucleation of analcime. The experiments have been carried out under the conditions of 150℃, 180℃, and 210℃; 0.75M, 0.5M and 0.25M NaOH solutions; solid/liquid ratios of 1/60 and 1/80; and vapor pressure.
Experimental results show that the dissolution rate of the glass increases with increasing temperature and concentration of NaOH solution, and also increases with decreasing solid/liquid ratio and grain size of the glass. The amount of nuclei versus time plots displays a normal distribution curve. The concentration of dissolved glass in solution increases with time until it attains the maximum where the amount of analcime nuclei reaches its maximum as well. If the glass dissolution rate is high, the solution concentration attains its maximum near the complete dissolution.

摘要 I
第一章 緒論
第一節 前言 1
第二節 前人研究 1
第三節 研究目的 3
第二章 研究方法
第一節 實驗材料 4
第二節 實驗儀器 5
第三節 實驗步驟 6
第三章 實驗結果
第一節 生成物之鑑定 10
第二節 玻璃的溶解與方沸石的生成 10
第三節 粒徑分布 35
第四節 方沸石晶體生長曲線 35
第五節 晶核形成曲線 54
第六節 方沸石含水量之計算 54
第七節 玻璃溶解過程中溶液濃度的變化 55
第四章 討論
（一）方沸石晶體生長速率與玻璃溶解速率 86
（二）方沸石之粒徑 91
（三）玻璃溶解與晶核形成關係 93
第五章 結論 108
致謝 109
參考文獻 110
附錄 113

Breck, D. W. (1974) Zeolite Molecular Sieves : John Wiley and Sons, Inc., New York, 761pp.
Breck, D. W., (1964) Crystalline Molecilar Sieves. Jour. of Che. Edu., 41, p.678-p.684
Brock, A. A., Link, G. N., Poitras, P. S., and Thompson, R. W.. (1993) Formation of bimodal zeolite crystal population from clear synthesis solution. Jour. Mater. Chem. 3(8), p.907-908.
Chen, W. H., Hu, H. C., and Lee, T. Y. (1993) Transient crystallization and crystal size distribution of zeolite A. Che. Eng. Sci., 48(21), p.3683-3691.
Derouane, E. G., Detremmerie, S., Gabelica, Z. and Blom, N. (1981) Appl. Catal., 101, p.101
Douglas, R. W. and EL-Shamy, T. M. (1967) Reaction of glasses with aqueous solutions. Jour. Amer. Ceram. Soc., 50, p.1-7.
Dyer, A. and Molyneux, A. (1968) The mobility of water in zeolites — I : Self-diffusion of water in analcime. Jour. of Inorg. and Nuclear Che., 30, p.829-837
Dyer, A. and Yusof, A. M. (1987) Diffusion in heteroionic analcimes: Part I. Sodium-potassium-water system. Zeolites, 7, p.191-196
Dyer, A. and Yusof, A. M. (1989) Diffusion in heteroionic analcimes: Part II. Diffusion of water in sodium/thallium, sodium/lithium, and sodium/ammonium analcimes. Zeolites, 9, p.129-135
Engelhardt, G., Fahike, B.,Magi, M. and Lippmaa, E. (1983) Zeolites, 3,p.292
Flanigen, E. M. (1973) Adv. Chem. Ser., 121, p.119
Golemme, G., Nastro, A., Nagy, J. B., Subotic, B., Crea, F., Aiello, R. (1991) Kinetic study on the nucleation of (Na,TPA)-ZSM-5 zeolite. Zeolites, 11, p.776-783
Gottardi, G. and Galli, E. (1985) Natural Zeolites. Springer-Verlag, Berlin Heidelberg.352pp.
Julius, C. (1968) Kinetics of zeolite A crystallization. Jour. of Colloid and Interfce Science, 28(2), p.315
Kerr, G. T. (1966) Chemistry of crystalline aluminosilicates. Jour. Phys. Chem., 70, p.1047
Kanauss, K. G. and Wolery, T. J. (1988) The dissolution kinetics of quartz as a function of pH and time at 70℃. Geochimica et Cosmochimica Acta, 52, p.43-53.
Lechert, H. and Kacirek, H. (1993) The kinetics of nucleation of X zeolites. Zeolite, 13, p.192-200
Lo, H. J., and Song, S. R. (1994) On the nucleation of zeolites. Jour. of the Geological Socity of China, 37(13), p.335-340.
Lo, H. J., Chen, Y. L., and Song, S. R. (1995) The kinetic study of the crystallization of Na-Ca-silicate hydrate under hydrothermal conditions. Jour. of the Geological Socity of China, 38(3), p.255-264.
Lo, H. J., Chen, Y. L., Yang, J. J., and Song, S. R. (1993) Crystallization kinetics of phillipsite synthesized hydrothermally from synthetic aluminosilicate glass. Acta Geol. Taiwanica, 31.
Mazer, J. M. and Walther, J. V. (1994) Dissolution kinetics of silica glass as a function of pH between 40 and 80℃. Jour. Non-Crystalline Solids, 170, p.32-45.
McNicol, B. D., (1973) Proc. of the 3rd Intl. Conf. on Molecular Sieves, p.21
Thompson, R. W. (1996) Molecular Sieve — Science and Technology, ed. Karge, H. and Weitkamp, J. Springer — Verlage, Heidelberg, ch.1, p.23
White, A. F. and Brantley, S. L. (1995) Chemical weathering rates of silicate minerals. Reviews in Mineralogy, 31.583p. Mineralogical Society of America.
Wiersema, G. S., and Thompson, R. W. (1996) Nucleation and crystal growth of analcime from clear aluminosilicate solutions. Jour. Mater. Chem. 6(10), p.1693-1699.
Yoshinobu Y. and Satoru I. (1998) The crystal structure of analcime. Micro. Mesop. Mater., 21, p.365-370
Zhdanov, S. P. (1970) Some problems of zeolite crystallization. 2nd Intl. Conf. Molecular Sieve Zeolites, p.19-40.
Zhdanov, S. P. (1971) Molecular Sieve Zeolites. Advan. Chem. Ser., 101,p.20
Zhdanov, S. P. and Samulevich, N. N. (1980) Nucleation and crystal growth of zeolites in crystallizing aluminosilicate gels. Proc. 5th Intl. Conf. Zeolites. ed. L. V. Rees, p.75-83.