Journal of the Chemical Society - Faraday Transactions p. 1429 - 1434 (1996)
Update date:2022-08-17
Topics:
Hartmann, Martin
Kevan, Larry
Dehydrated nickel containing silicoaluminophosphates SAPO-11 and SAPO-5 materials are catalytically active for ethene dimerization. There is a striking difference between the catalytic activity due to nickel(I) species in ion-exchange and in framework positions. Both the ethene dimerization activity and the selectivity for the formation of n-butenes is dependent on the location (ion-exchange vs. framework site) of the nickel(I) species and on the channel size (10-ring vs. 12-ring) of the supporting materials. EPR studies show an isolated nickel(I) species A (g∥ = 2.489 and g⊥ = 2.108) which transfers to species E (g1 = 2.680, g2 = 2.474 and g3 = 1.961) after ethene adsorption. This species has been assigned to an NiI-(C2D4)n complex. Subsequently, after heating to 353 K, species B1 (g1 = 2.720, g2 = 2.259 and g3 = 1.996), B2 (g1 = 2.363, g2 = 2.174 and g3 = 2.067) and B3 (g∥ = 2.052 and g⊥ = 2.007), depending of the type of SAPO material, are observed with simultaneous butene formation, detected by gas chromatography. Electron spin-echo modulation analysis allows the assignment of B1, B2 and B3 to NiI-C4D8 complexes with different geometries.
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