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Title: Steady-state and isotopic transient kinetics of benzene hydrogenation on nickel catalysts

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

By combining steady-state and isotopic transient experiments which provide both apparent and true kinetic parameters, the authors propose a modeling of the benzene hydrogenation reaction over nickel catalysts at low temperature (below 400 K). The metal surface is shown to be covered mainly with adsorbed hydrogen; only a very small fraction of the surface (about 1%) is covered with reacting intermediates. From the physically significant parameters thus determined, the authors arrive at the rate equation r = k/sub 0/e/sup -E/sub 0//RT/(1 - theta/sub H/)/sup x/P/sub H/P/sub B//sup epsilon/, where E/sub 0/ = 33 +/- 4 kJ/mol, theta/sub H/-the surface coverage with hydrogen, X = 4 +/- 1, and P/sub H/ and P/sub B/-partial pressures of hydrogen and benzene, respectively. The rate-limiting step can be described as a two-body process between (i) the active site, an ensemble of about four adjacent nickel atoms occupied by a chemisorbed benzene molecule, and (ii) a molecular hydrogen species. The concentration of the active ensembles is monitored by the hydrogen coverage, the latter being influenced little by the reservoir of loosely adsorbed benzene which coats and feeds the catalytic surface.

Research Organization:
l'Universite Claude Bernard Lyon I, France
OSTI ID:
5394000
Journal Information:
J. Catal.; (United States), Vol. 105:2
Country of Publication:
United States
Language:
English