Hydrothermal Alumination of Zeolites

作者: Jacek Klinowski

DOI: 10.1016/S0167-2991(08)60514-5

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摘要: Magic-angle-spinning (MAS) NMR, quadrupole nutation infrared spectroscopy and X-ray diffraction measurements all indicate that aluminium atoms eliminated from the framework of zeolite Y by hydrothermal treatment (ultrastabilization) can be subsequently reinserted into with aqueous solutions strong bases (preferably KOH) at elevated temperatures. The extent efficiency reaction depend on temperature, duration especially kind concentration solution. degree crystallinity thermal stability products are primarily controlled composition parent material, while realumination is determined number available tetrahedral Si(0Al) sites. have a very different Si,Al distribution as-prepared same Al content. realumination-dealumination process performed in cyclic fashion yielding wide variety second-generation catalysts. 27 NMR reveals presence four kinds dealuminated Y: (F), non-framework (NFT), distorted (DFT) octahedral (NFO). DFT bonded to hydroxyl groups formed during dealumination. In realuminated samples both NFO NFT intensity signal correspondingly reduced. 1 H MAS confirms has taken place. sample contains twice as many Bronsted acid sites than ultrastable precursor and, an accuracy 20%, zeolite. However, not associated product accessible pyridine sample.

参考文章(45)
Pascal P. Man, Jacek Klinowski, Quadrupole nutation 27Al NMR studies of isomorphous substitution of aluminium in the framework of zeolite Y Chemical Physics Letters. ,vol. 147, pp. 581- 584 ,(1988) , 10.1016/0009-2614(88)80272-0
Clarence D. Chang, Stuart D. Hellring, Joseph N. Miale, Kirk D. Schmitt, P. W. Brigandi, E. L. Wu, Insertion of aluminium into high-silica-content zeolite frameworks. Part 3.—Hydrothermal transfer of aluminium from Al2O3 into [Al]ZSM-5 and [B]ZSM-5 Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases. ,vol. 81, pp. 2215- 2224 ,(1985) , 10.1039/F19858102215
Hermann K. Beyer, Ita M. Belenykaja, Ferenc Hange, Mia Tielen, Piet J. Grobet, Peter A. Jacobs, Preparation of high-silica faujasites by treatment with silicon tetrachloride Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases. ,vol. 81, pp. 2889- 2901 ,(1985) , 10.1039/F19858102889
F.M.M. Geurts, A.P.M. Kentgens, W.S. Veeman, 27Al nutation NMR of zeolites Chemical Physics Letters. ,vol. 120, pp. 206- 210 ,(1985) , 10.1016/0009-2614(85)87041-X
G. Engelhardt, U. Lohse, E. Lippmaa, M. Tarmak, M. M�gi, 29Si‐NMR‐Untersuchungen zur Verteilung der Silicium‐und Aluminiumatome im Alumosilicatgitter von Zeolithen mit Faujasit‐Struktur Zeitschrift für anorganische und allgemeine Chemie. ,vol. 482, pp. 49- 64 ,(1981) , 10.1002/ZAAC.19814821106
E. Lippmaa, M. Maegi, A. Samoson, G. Engelhardt, A. R. Grimmer, Structural studies of silicates by solid-state high-resolution silicon-29 NMR Journal of the American Chemical Society. ,vol. 102, pp. 4889- 4893 ,(1980) , 10.1021/JA00535A008
Michael W. Anderson, Jacek Klinowski, Liu Xinsheng, Alumination of highly siliceous zeolites Journal of The Chemical Society, Chemical Communications. pp. 1596- 1597 ,(1984) , 10.1039/C39840001596
A Corma, C Rodellas, V Fornes, Characterization of acid surfaces by adsorption of 2,6-dimethylpyridine Journal of Catalysis. ,vol. 88, pp. 374- 381 ,(1984) , 10.1016/0021-9517(84)90014-9
Michael W. Anderson, Jacek Klinowski, Zeolites treated with silicon tetrachloride vapour. IV. Acidity Zeolites. ,vol. 6, pp. 455- 466 ,(1986) , 10.1016/0144-2449(86)90030-8
Jacek Klinowski, T. Adrian Carpenter, John M. Thomas, The origin of 29Si spin–lattice relaxation in zeolites: a means of rapid acquisition of n.m.r. spectra and of probing internal sites in microporous catalysts Journal of The Chemical Society, Chemical Communications. pp. 956- 958 ,(1986) , 10.1039/C39860000956