Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases p. 3103 - 3118 (1984)
Update date:2022-08-17
Topics:
Bond, Geoffrey C.
Yide, Xu
The hydrogenolysis of n-butane has been studied on 1 and 5percent ruthenium/titania catalysts pretreated in hydrogen at various temperatures and in air at 623 K.Increasing the temperature of reduction of impregnated ruthenium trichloride from 623 to 758 K gives an increase in activity attributed to removal of chloride, but the low activities associated with a strong metal-support interaction (SMSI) are not found until a reduction temperature of 893 K is used.Subsequent oxidation followed by low-temperature reduction gives much higher activities: this is ascribed to spreading of ruthenium oxide over the support, reduction of which affords more highly dispersed metal which easily succumbs to SMSI on a further high-temperature reduction.This interpretation receives some support from temperature-programmed-reduction results.Product distributions are interpreted according to the scheme devised by Kempling and Anderson.The oxidation treatment and low-temperature reduction creates a new type of active site which appears to favour terminal bond splitting in adsorbed n-butane and has greater reactivity for bond splitting in adsorbed C2 and C3 species.This analysis also leads to the conclusions that a second reduction at 623 K does not wholly convert the well dispersed metal to the SMSI state and that not quite all of the oxide formed at 623 K spreads over the support.The strange behaviour of this system is contrasted with that of ruthenium and of platinum supported on silica.
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