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Experimentally determined activation energies of propane dehydrogenation catalyzed by ZSM-5 zeolites have been used to test the SET theory. The basis of this theory is that the catalyst system transfers vibrational energy via a resonance process to a specific vibration mode of the reacting molecule. Being excited up to a certain number of vibrational quanta the molecule is brought to reaction. By analyzing the above-mentioned activation energies we found the wave number of this "specific mode" to be 1065 cm-1. This is very close to the rocking vibration of propane (1053 cm-1). We suggest that the propane molecule reacts when excited so that the CH3 group has been forced towards a flat structure with a carbon atom hybridization that is more sp2 than sp3. Consequently there is no way for three H-atoms to bind to the carbon and one of them must leave. This is the starting point of the reaction. The isokinetic temperature of the system was found as Tiso = 727 ± 4 K. From the SET formula for Tiso when both energy-donating (ω) and energy-accepting (ν) vibrations have the same frequency, viz., Tiso = Nhcν/2R, we obtain ν = ω = 1011 ± 6 cm-1. This agrees rather well with the CH3 rocking mode (1053 cm-1) and also with asymmetric "TO4" stretching vibrations of the zeolite structure (ω).

Propane Dehydrogenation Catalyzed by ZSM-5 Zeolites. A Mechanistic Study Based on the Selective Energy Transfer (SET) Theory