The oxidative ammonolysis of ethylene to acetonitrile over gamma-Al2O3 supported molybdenum catalysts

I. Peeters, J. Grondelle, van, R.A. Santen, van

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Uittreksel

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
Originele taal-2Engels
TitelHeterogeneous hydrocarbon oxidation
Plaats van productieWashington, D.C.
UitgeverijAmerican Chemical Society
Pagina's319-329
ISBN van geprinte versie0-8412-3422-1
StatusGepubliceerd - 1996

Publicatie series

NaamACS Symposium Series
Volume638
ISSN van geprinte versie0097-6156

Vingerafdruk

Molybdenum
Oxygen
Catalysts
Ethane
Ammonia
ethylene
acetonitrile
Hydrogen
Catalyst activity
Experiments

Citeer dit

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 (blz. 319-329). (ACS Symposium Series; Vol. 638). Washington, D.C.: American Chemical Society.
Peeters, I. ; Grondelle, van, J. ; Santen, van, R.A. / The oxidative ammonolysis of ethylene to acetonitrile over gamma-Al2O3 supported molybdenum catalysts. Heterogeneous hydrocarbon oxidation. Washington, D.C. : American Chemical Society, 1996. blz. 319-329 (ACS Symposium Series).
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abstract = "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",
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Peeters, I, Grondelle, van, J & Santen, van, RA 1996, The oxidative ammonolysis of ethylene to acetonitrile over gamma-Al2O3 supported molybdenum catalysts. in Heterogeneous hydrocarbon oxidation. ACS Symposium Series, vol. 638, American Chemical Society, Washington, D.C., blz. 319-329.

The oxidative ammonolysis of ethylene to acetonitrile over gamma-Al2O3 supported molybdenum catalysts. / Peeters, I.; Grondelle, van, J.; Santen, van, R.A.

Heterogeneous hydrocarbon oxidation. Washington, D.C. : American Chemical Society, 1996. blz. 319-329 (ACS Symposium Series; Vol. 638).

Onderzoeksoutput: Hoofdstuk in Boek/Rapport/CongresprocedureConferentiebijdrageAcademic

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T1 - The oxidative ammonolysis of ethylene to acetonitrile over gamma-Al2O3 supported molybdenum catalysts

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N2 - 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

AB - 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

M3 - Conference contribution

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T3 - ACS Symposium Series

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BT - Heterogeneous hydrocarbon oxidation

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Peeters I, Grondelle, van J, Santen, van RA. The oxidative ammonolysis of ethylene to acetonitrile over gamma-Al2O3 supported molybdenum catalysts. In Heterogeneous hydrocarbon oxidation. Washington, D.C.: American Chemical Society. 1996. blz. 319-329. (ACS Symposium Series).