Gs. Nivarthy et al., THE INFLUENCE OF ACIDITY ON ZEOLITE H-BEA CATALYZED ISOBUTANE N-BUTENE ALKYLATION/, MICROPOROUS AND MESOPOROUS MATERIALS, 22(1-3), 1998, pp. 379-388
The influence of the concentration of acid sites for isobutane/n-buten
e alkylation on zeolite BEA with varying degrees of Na+ ion exchange i
s reported. All catalysts studied showed complete n-butene conversion
over a significant time-on-stream. Isooctanes were the dominating prod
ucts over H-BEA, while the importance of di- and multiple alkylation i
ncreased with increasing Na+ concentration in the zeolite. In parallel
, the integral number of turnovers per catalytic site markedly decreas
ed. The acid site deactivation is affiliated with blocking by hexadeca
ne species. The higher rate of catalyst deactivation with increasing d
egree of Na+ exchange is thus attributed to the increase in the probab
ility of having a further butene molecule added to a C-8 alkoxy group
in place of undergoing hydride transfer from isobutane to desorb as is
ooctane. This is a direct result of the decreasing concentration of al
koxy groups that can react with n-butene while maintaining the same ra
te of olefin transport through the pores. Addition of a strong hydride
donor/acceptor molecule (adamantane) indicates that the product compo
sition of the isooctane isomers is determined by their lifetime as alk
oxy groups. The longer the lifetime before experiencing hydride transf
er, the closer the product composition approaches the chemical equilib
rium. (C) 1998 Elsevier Science B.V. All rights reserved.