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THE SELECTIVITY CHANGES IN 1-HEXENE ISOMERIZATION AND ITS RELATION TO ACID PROPERTIES OF Pd/SAPO-11, SAPO-11, AZSM-5, AND H-MORDENITE CATALYSTS
Korean Journal of Chemical Engineering, July 1990, 7(3), 175-181(7), 10.1007/BF02697349
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Abstract
The activity and selectivity patterns for 1-hexene isomerization have been compared in the temperature range of 150-450 ℃ for four different kinds of acidic zeolites(H-mordenite, HZSM-5, SAPO-11 and Pd/SAPO-11) differing both in acid properties and geometric structure. At lower reaction temperatures (150-175℃) the predominant reaction pathway was double bond shift(DBS) and was not influenced by the type of catalyst. At higher temperatures significant shifts in selectivity were observed from DBS to cracking (c) or skeletal rearrangement(SR) depending on the type of catalyst. Temperature programmed desorption(TPD) patterns of chemisorbed NH3 were also determined. Three different peaks were found for the most TPD patterns. The first peak might be associated with Lewis acid-site, and the other two peaks at higher temperatures might be associated with Brnsted acid-sites. It was found that significant loss of strong Brnsted acidity upon Pd loading on SAPO-11. A selectivity correlation at 350℃ showed strong dependence of DBS and cracking on total acidity. The reaction seems well suited for investigation of the interrelation between pore structure and surface acidity in terms of these selectivity factors.
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Thompson R, Wolf EE, Private Communication (1989)
Flanigen EH, Patton RL, Wilson ST, Stud. Surf. Sci. Catal., 37, 13 (1988)
Hasha D, Saldarriga L, Hathaway PE, Cox DF, Davis ME, J. Am. Chem. Soc., 110, 2127 (1988)
Kaiser SW, U.S. Patent, 4,499,327 (1985)
Butler SA, Kaeding WW, U.S. Patent, 3,972,832 (1976)
Miller J, U.S. Patent, 4,689,138 (1987)
Young LB, Butler SA, Kaeding W, J. Catal., 76, 418 (1982)
Vedrine JC, Aroux A, Dejaifve P, Ducerne V, Hoser H, Zhou S, J. Catal., 73, 147 (1982)
Numan J, Cronin J, Cunningham J, J. Catal., 87, 77 (1984)
We are indebred to Dr. J.A. Rabo of Union Carbide Corporation for Providing SAPO-11 and to Dr. R.J. Gormley of the Pittsburgh Energy Technology Center for Providing HZSM-5
Balkrishnan BS, Rao SG, Hedge SG, Kotasthane AN, Kulkarni SB, Ratnaswamy P, J. Catal., 17, 261 (1982)
Halik C, Lercher JA, J. Chem. Soc.-Faraday Trans., 84, 4457 (1988)
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Bond GC, "Catalysis by Metals," p. 256, Academic Press, New York (1962)
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Pines H, "The Chemistry of Catalytic Hydrocarbon Conversions," Academic Press, New York (1981)
Satterfield CN, "Heterogeneous Catalysis in Practice," Ch. 7, McGraw-Hill, New York (1984)