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Title: Kinetic and mechanistic study of cyclohexene disproportionation: example of irreversible hydrogen transfer

Journal Article · · J. Catal.; (United States)

The kinetics and mechanism of cyclohexane disproportionation, as well as its structure sensitivity, have been studied over a variety of Group VIII metal catalysts (i.e., Pt, Pd, and Ni). The goal of this work was to better understand how hydrogen transfer occurs in heterogeneous catalysis. Three reactions were studied: cyclohexene disproportionation, cyclohexene hydrogenation, and benzene hydrogenation. A gas-phase, microcatalytic reactor was used to obtain the data. The results were analyzed in terms of their activities, apparent activation energies, and selectivities. It was found that all the catalysts (except 0.001% Pt/Al/sub 2/O/sub 3/) were active catalysts for benzene hydrogenation. The apparent E/sub a/'s were between 42 and 50 kJ/mole. The activities decreased in the following manner, Pt > Ni > Pd. In contrast, during cyclohexene disproportionation, the apparent E/sub a/'s varied among catalysts (Pt approx. = 84, Pd approx. = 50, and Ni approx. = 25 kJ/mole), but their activities at 100/sup 0/C were similar (except 0.01 and 0.001% Pt/Al/sub 2/O/sub 3/). There existed a transition temperature below which the correct stoichiometry for cyclohexene disproportionation was observed, and above which the selectivity (measured as moles cyclohexane produced/moles benzene produced) decreased with temperature. This transition temperature varied with type of metal (T was 60/sup 0/C for Ni, 90/sup 0/C for Pd, and 110/sup 0/C for Pt).

Research Organization:
Univ. of Massachusetts, Amherst (USA)
OSTI ID:
7052918
Journal Information:
J. Catal.; (United States), Vol. 111:2
Country of Publication:
United States
Language:
English