Industrial & Engineering Chemistry Research, Vol.39, No.7, 2148-2156, 2000
Ethylene epoxidation on Ag-Cs/alpha-Al2O3 catalyst: Experimental results and strategy for kinetic parameter determination
The kinetics of ethylene epoxidation network were studied experimentally over a cesium-doped silver catalyst supported on alpha-Al2O3 pellets in a differential reactor. A variety of rate functions were considered and among these, expressions based on a dual-site Langmuir-Hinselwood mechanism: r(i) = k(i)P(E)P(O)(ni)/(1 + K-E(i) P-E)(2), fitted the data best with an average error of 13.0 and 10.7% for the epoxidation and the complete combustion reactions, respectively. Under the experimental conditions, both reactants influence both reaction rates; however, product influence is negligible because of their small partial pressures present in the reactor. High oxygen/ethylene ratios and lower temperature favored selectivity to the epoxidation reaction. The kinetic parameters obtained from the differential reactor experiments were refined to match the fixed-bed reactor experiments. With this, the average error in predicting both ethylene conversion and selectivity to ethylene oxide was 4.3%. The apparent activation energies for the epoxidation and combustion reactions were 60.7 and 73.2 kJ/mol, respectively.