화학공학소재연구정보센터
Catalysis Today, Vol.60, No.3-4, 311-317, 2000
Synthesis of cyclohexylcyclohexanone on bifunctional Pd faujasites. Influence of the balance between the acidity and the metallic function
The transformation of cyclohexanone was carried out on a series of bifunctional PdHFAU catalysts with Pd contents between 0.1 and 0.5 wt.% and framework Si/Al ratios equal to 5, 20, 40 and 100, under the following conditions: flow reactor, 473 K, pressures of cyclohexanone and hydrogen equal to 0.17 and 0.83 bar, respectively. With all the catalysts, cyclohexylcyclohexanone, the formation of which requires successive steps of aldolization, dehydration and hydrogenation, is directly formed. The effect of the balance between the hydrogenating and acid functions of the catalysts (taken as the ratio between their activity for toluene hydrogenation and their number of protonic acid sites, A(H)/B) on their activity, stability and selectivity is the one expected from a bifunctional catalytic process. The activity per protonic site first increases with A(H)/B, then remains constant above a certain value of A(H)/B (0.4 h(-1)), the limiting step of cyclohexylcyclohexanone formation being then cyclohexanone aldolization. The selectivity to cyclohexylcyclohexanone as well as the stability increase with A(H)/B remaining constant for A(H)/B>1 h(-1). While a high selectivity to cyclohexylcyclohexanone is obtained, the catalyst stability is relatively poor due to the retention inside the zeolite micropores of polar tricyclic C-18 compounds.