Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases p. 1359 - 1370 (1981)
Update date:2022-08-12
Topics:
Foerster, Horst
Seelemann, Rudolf
Adsorption and isomerization of n-butenes on A-type zeolites containing zinc, silver and cobalt ions have been studied at room temperature by Fourier transform infrared spectroscopy.In the hydrated samples two kinds of water can be distinguished: unspecifically adsorbed water and water specifically interacting with the cations.After complete dehydration no hydroxyl groups are observed in the spectra.The penetration rate of the n-butenes, which generally follows the sequence trans-but-2-ene > but-1-ene > cis-but-2-ene, is sensitive to the occupation of the S2 sites.Upon adsorption, rotation of the butenes becomes restricted.In addition of the donor bond, there is back-donation from the cations into antibonding ?*-orbitals of the butenes, as evidenced by the unexpectedly high cation-specific red-shift of the C=C stretchnig band.While silver containing A-type zeolites are catalytically inactive due to the small charge: radius ratio of the cations, on zeolites axchanged with zinc ions spontaneous isomerization is observed, which is enhanced on samples containing a non-stoichiometric excess of zinc.Addition of the cocatalyst sulphur dioxide greatly increases the isomerization rate.Also, in the case of ZnA zeolites the reaction is first order in both n-butene and SO2 and is in accord with a concerted reaction mechanism which has been shown to occur on A-type zeolites exchanged with alkali and alkaline earth ions.
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