A hydrotalcite-based catalyst system for the single-stage liquid-phase synthesis of MIBK Original Research Article

A comparative study was performed between Pd supported on activated hydrotalcites bi-functional catalysts and physical mixtures of activated hydrotalcites with Pd supported on carbon nanofibers for the single-stage liquid-phase synthesis of methyl isobutyl ketone from acetone and H2. Since it was found earlier that the dehydration reaction of diacetone alcohol over activated hydrotalcites is the rate-determining step in this process, Mg–Al hydrotalcites were investigated in the condensation of acetone to diacetone alcohol and its dehydration to mesityl oxide to enhance the activity. A correlation between the number of active base sites, as determined by volumetric CO2 adsorption measurements at low pressures, and the activity in the dehydration reaction could be derived. A dependency on the Pd-loading (0–1 wt%) of Pd supported on activated hydrotalcites catalysts was found in the single-stage synthesis of methyl isobutyl ketone, whereas no such an effect was found when using physical mixtures of activated hydrotalcites with Pd on carbon nanofibers. Results from TEM, CO2 chemisorption and N2 physisorption as well as catalytic experiments in the hydrogenation of mesityl oxide and of cyclohexene indicate that this dependency is largely accounted for by entrapment of Pd particles in the agglomerates of the irregular stacks of hydrotalcite platelets, making these sites inaccessible for the reactants.