Journal of Molecular Catalysis A-Chemical, Vol.201, No.1-2, 283-288, 2003
Kinetics of the catalytic coupling reaction of carbon monoxide to diethyl oxalate over Pd-Fe/alpha-Al2O3 catalyst
The reaction kinetics of the catalytic coupling reaction of carbon monoxide to diethyl oxalate was studied in the presence of ethyl nitrite over supported palladium catalyst in gaseous phase at atmospheric pressure. The experiments were performed in a continuous flow fixed-bed differential type reactor. It was discovered that the rate-determining step is the surface reaction between adsorbed species and that ethyl nitrite dissociates into ethoxy radical (EtO-) and NO species and are adsorbed on two active sites. The kinetic model was proposed, with which some observations concerning with the reaction behaviors of the system can be readily accounted for. In the presence of hydrogen, the kinetics of the reaction system was also investigated. It was revealed that hydrogen, with adsorption and dissociation, reacts with adsorbed ethoxy radical to ethanol. (C) 2003 Elsevier Science B.V. All rights reserved.