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Alkylation of Isobutane with 2-Butene over a HFAU Zeolite. Composition of Coke and Deactivating Effect

1999; American Chemical Society; Volume: 38; Issue: 10 Linguagem: Inglês

10.1021/ie9902232

1520-5045

Jérôme P.G. Pater, Frédéric Cardona, Christine Canaff, N.S. Gnep, G. Szabo, M. Guisnet,

Catalytic Processes in Materials Science

The transformation of an isobutane −2-butene mixture with a 40 weight ratio was carried out in liquid phase at 50 °C on an USHY zeolite with a framework Si/Al ratio of 4.5. The reaction products can be classified into seven families: (a) trimethylpentanes resulting from isobutane alkylation with 2-butene or from isobutane self-alkylation, (b) dimethylhexanes, (c) C8 alkenes, (d) heavy products (mainly C9−C12), (e) light products C5−C7 alkanes, (f) n-butane, and (g) nondesorbed products (coke). These latter products, which are responsible for deactivation, were removed from samples coked for different times, after dissolution of the zeolite in a hydrofluoric acid solution, and analyzed by GC, IR, HNMR, MS, and GC/MS coupling. The coke components were identified as alkyl bicyclic olefinic compounds with 12−28 carbon atoms. IR spectroscopy analysis of the coked zeolite samples shows that coke molecules interact with the protonic sites, this interaction being mainly responsible for deactivation. Large differences can be observed in deactivation of the various reaction steps. The steps which are the more demanding in number (e.g., hydride transfer) or in strength (e.g., isomerization) of the acid sites are preferentially deactivated.