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

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

Research output: Chapter in Book/Report/Conference proceedingConference contributionAcademic

1 Citation (Scopus)
34 Downloads (Pure)

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
Original languageEnglish
Title of host publicationHeterogeneous hydrocarbon oxidation
Place of PublicationWashington, D.C.
PublisherAmerican Chemical Society
Pages319-329
ISBN (Print)0-8412-3422-1
Publication statusPublished - 1996

Publication series

NameACS Symposium Series
Volume638
ISSN (Print)0097-6156

Fingerprint

Molybdenum
Oxygen
Catalysts
Ethane
Ammonia
ethylene
acetonitrile
Hydrogen
Catalyst activity
Experiments

Cite this

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.
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. pp. 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., pp. 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. p. 319-329 (ACS Symposium Series; Vol. 638).

Research output: Chapter in Book/Report/Conference proceedingConference contributionAcademic

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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

SN - 0-8412-3422-1

T3 - ACS Symposium Series

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EP - 329

BT - Heterogeneous hydrocarbon oxidation

PB - American Chemical Society

CY - Washington, D.C.

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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. p. 319-329. (ACS Symposium Series).