Abstract

Although surface of amorphous silica is widely accepted to be neutral or slightly acidic, siliceous mesoporous materials have been found to act as excellent acid catalysts by us and other groups. On the other hand the increment in propene production is one of the significant objectives to be achieved in the present petroleum chemistry. Especially the one-path conversion of ethene to propene (ETP reaction, 3C2H4 → 2C3H6) is the most desired process. In our efforts, the specific acid catalysis of mesoporous silica was combined with the catalysis of nickel ion, which could turn the new type of ETP reaction into reality. The one-path conversion of ethene was 68% and the propene selectivity was 48% with 43% of butenes in a continuous gas-flow system at 673 K and an atmospheric pressure. The reactivity of lower olefins and the dependences of the ETP reaction on the contact time and the partial pressure of ethene followed the reaction mechanism consisting of dimerization of ethene to 1-butene, isomerization of 1-butene to 2-, and metathesis of 2-butene and ETP. The Ni-loaded mesoporous silica catalysts were characterized mainly by EXAFS and TPR techniques. The local structures of the nickel species active for the ETP reaction were very similar to that of layered nickel silicate, while those on the inert catalysts were the same as that of NiO particles.

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