The reaction of ethylene with ammonia, without gaseous oxygen, to acetonitrile over gamma-Al2O3 supported molybdenum catalysts was studied. The effects of molybdenum loading and pretreatment on the catalytic activity were investigated. Experiments showed that the activity at the semi-steady-state is highly structure sensitive. Pretreated in oxygen, the catalyst is highly selective towards CH3CN, with COx formed as side product. Pretreated in hydrogen, the catalyst is more active but less selective, with ethane formed as side product. Two mechanisms were deduced: 1) ammoxidation mechanism with consumption of lattice oxygen. 2) oxidative ammonolysis with coproduction of ethane, without lattice oxygen consumption. The steady-state activity was independent of pretreatment and no oxygen containing products were observed, indicating that mechanism 1) can gradually change into 2) when removable lattice oxygen becomes depleted. The product distribution indicated that the mechanisms can be active simultaneously and separately. Mechanism 2 appeared to be operational on a MoO2-like structure
|Title of host publication||Heterogeneous hydrocarbon oxidation|
|Place of Publication||Washington, D.C.|
|Publisher||American Chemical Society|
|Publication status||Published - 1996|
|Name||ACS Symposium Series|
Peeters, I., Grondelle, van, J., & Santen, van, R. A. (1996). The oxidative ammonolysis of ethylene to acetonitrile over gamma-Al2O3 supported molybdenum catalysts. In Heterogeneous hydrocarbon oxidation (pp. 319-329). (ACS Symposium Series; Vol. 638). Washington, D.C.: American Chemical Society.