Kinetic study of the ethene oxidation by oxygen in the presence of carbon dioxide and steam over Pt/Rh/CeO2/g-Al2O3

R.H. Nibbelke, R.J.M. Kreijveld, J.H.B.J. Hoebink, G.B.M.M. Marin

Research output: Chapter in Book/Report/Conference proceedingConference contributionAcademicpeer-review

Abstract

The oxidation of ethene by oxygen in the presence of steam and carbon dioxide over a commercially available Pt/Rh/CeO2/¿-Al2O3 three-way automotive catalyst was studied. Experiments were carried out in a fixed-bed micro reactor under intrinsic conditions, i.e. in the absence of external and internal mass and heat transport limitations. A kinetic model based on elementary reaction steps was developed for the following range of experimental conditions: a total pressure of 110 kPa, temperatures between 463 and 483 K, ethene inlet partial pressures between 0.04 and 0.14 kPa, oxygen inlet partial pressures between 0.25 and 1.10 kPa and steam and carbon dioxide inlet partial pressures equal to 10 kPa. For these conditions, only the total oxidation of ethene to carbon dioxide and steam was observed. The reaction rate was found to decrease with increasing ethene partial pressure and decreasing oxygen partial pressure. Both carbon dioxide ans steam were found to inhibit the reaction rate. The activity of CeO2 can be neglected at the investigated conditions. The kinetic model comprises the following elementary steps: irreversible adsorption of oxygen and reversible adsorption of ethene on the noble metal surface, followed by a surface reaction between adsorbed ethene and oxygen. The values of the kinetic parameters, i.e. preexponential factors and activation energies, were estimated by non-linear regression of the ethene conversion and found to be physically meaningful.
Original languageEnglish
Title of host publicationCatalysis and automotive pollution control IV : proceedings of the Fourth International Symposium (CAPoC4), Brussels, Belgium, April 9 - 11, 1997
EditorsN. Kruse
Place of PublicationAmsterdam
PublisherElsevier
Pages389-398
ISBN (Print)0-444-82795-1
DOIs
Publication statusPublished - 1998
Eventconference; International Symposium (CAPOC) ; 4 (Brussels) : 1997.04.09-11 -
Duration: 1 Jan 1998 → …

Publication series

NameStudies in Surface Science and Catalysis
Volume116
ISSN (Print)0167-2991

Conference

Conferenceconference; International Symposium (CAPOC) ; 4 (Brussels) : 1997.04.09-11
Period1/01/98 → …
OtherInternational Symposium (CAPOC) ; 4 (Brussels) : 1997.04.09-11

Fingerprint

Steam
Carbon Dioxide
Oxygen
Partial pressure
Oxidation
Kinetics
Reaction rates
Adsorption
Surface reactions
Precious metals
ethylene
Kinetic parameters
Activation energy
Catalysts

Cite this

Nibbelke, R. H., Kreijveld, R. J. M., Hoebink, J. H. B. J., & Marin, G. B. M. M. (1998). Kinetic study of the ethene oxidation by oxygen in the presence of carbon dioxide and steam over Pt/Rh/CeO2/g-Al2O3. In N. Kruse (Ed.), Catalysis and automotive pollution control IV : proceedings of the Fourth International Symposium (CAPoC4), Brussels, Belgium, April 9 - 11, 1997 (pp. 389-398). (Studies in Surface Science and Catalysis; Vol. 116). Amsterdam: Elsevier. https://doi.org/10.1016/S0167-2991(98)80895-1
Nibbelke, R.H. ; Kreijveld, R.J.M. ; Hoebink, J.H.B.J. ; Marin, G.B.M.M. / Kinetic study of the ethene oxidation by oxygen in the presence of carbon dioxide and steam over Pt/Rh/CeO2/g-Al2O3. Catalysis and automotive pollution control IV : proceedings of the Fourth International Symposium (CAPoC4), Brussels, Belgium, April 9 - 11, 1997. editor / N. Kruse. Amsterdam : Elsevier, 1998. pp. 389-398 (Studies in Surface Science and Catalysis).
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title = "Kinetic study of the ethene oxidation by oxygen in the presence of carbon dioxide and steam over Pt/Rh/CeO2/g-Al2O3",
abstract = "The oxidation of ethene by oxygen in the presence of steam and carbon dioxide over a commercially available Pt/Rh/CeO2/¿-Al2O3 three-way automotive catalyst was studied. Experiments were carried out in a fixed-bed micro reactor under intrinsic conditions, i.e. in the absence of external and internal mass and heat transport limitations. A kinetic model based on elementary reaction steps was developed for the following range of experimental conditions: a total pressure of 110 kPa, temperatures between 463 and 483 K, ethene inlet partial pressures between 0.04 and 0.14 kPa, oxygen inlet partial pressures between 0.25 and 1.10 kPa and steam and carbon dioxide inlet partial pressures equal to 10 kPa. For these conditions, only the total oxidation of ethene to carbon dioxide and steam was observed. The reaction rate was found to decrease with increasing ethene partial pressure and decreasing oxygen partial pressure. Both carbon dioxide ans steam were found to inhibit the reaction rate. The activity of CeO2 can be neglected at the investigated conditions. The kinetic model comprises the following elementary steps: irreversible adsorption of oxygen and reversible adsorption of ethene on the noble metal surface, followed by a surface reaction between adsorbed ethene and oxygen. The values of the kinetic parameters, i.e. preexponential factors and activation energies, were estimated by non-linear regression of the ethene conversion and found to be physically meaningful.",
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Nibbelke, RH, Kreijveld, RJM, Hoebink, JHBJ & Marin, GBMM 1998, Kinetic study of the ethene oxidation by oxygen in the presence of carbon dioxide and steam over Pt/Rh/CeO2/g-Al2O3. in N Kruse (ed.), Catalysis and automotive pollution control IV : proceedings of the Fourth International Symposium (CAPoC4), Brussels, Belgium, April 9 - 11, 1997. Studies in Surface Science and Catalysis, vol. 116, Elsevier, Amsterdam, pp. 389-398, conference; International Symposium (CAPOC) ; 4 (Brussels) : 1997.04.09-11, 1/01/98. https://doi.org/10.1016/S0167-2991(98)80895-1

Kinetic study of the ethene oxidation by oxygen in the presence of carbon dioxide and steam over Pt/Rh/CeO2/g-Al2O3. / Nibbelke, R.H.; Kreijveld, R.J.M.; Hoebink, J.H.B.J.; Marin, G.B.M.M.

Catalysis and automotive pollution control IV : proceedings of the Fourth International Symposium (CAPoC4), Brussels, Belgium, April 9 - 11, 1997. ed. / N. Kruse. Amsterdam : Elsevier, 1998. p. 389-398 (Studies in Surface Science and Catalysis; Vol. 116).

Research output: Chapter in Book/Report/Conference proceedingConference contributionAcademicpeer-review

TY - GEN

T1 - Kinetic study of the ethene oxidation by oxygen in the presence of carbon dioxide and steam over Pt/Rh/CeO2/g-Al2O3

AU - Nibbelke, R.H.

AU - Kreijveld, R.J.M.

AU - Hoebink, J.H.B.J.

AU - Marin, G.B.M.M.

PY - 1998

Y1 - 1998

N2 - The oxidation of ethene by oxygen in the presence of steam and carbon dioxide over a commercially available Pt/Rh/CeO2/¿-Al2O3 three-way automotive catalyst was studied. Experiments were carried out in a fixed-bed micro reactor under intrinsic conditions, i.e. in the absence of external and internal mass and heat transport limitations. A kinetic model based on elementary reaction steps was developed for the following range of experimental conditions: a total pressure of 110 kPa, temperatures between 463 and 483 K, ethene inlet partial pressures between 0.04 and 0.14 kPa, oxygen inlet partial pressures between 0.25 and 1.10 kPa and steam and carbon dioxide inlet partial pressures equal to 10 kPa. For these conditions, only the total oxidation of ethene to carbon dioxide and steam was observed. The reaction rate was found to decrease with increasing ethene partial pressure and decreasing oxygen partial pressure. Both carbon dioxide ans steam were found to inhibit the reaction rate. The activity of CeO2 can be neglected at the investigated conditions. The kinetic model comprises the following elementary steps: irreversible adsorption of oxygen and reversible adsorption of ethene on the noble metal surface, followed by a surface reaction between adsorbed ethene and oxygen. The values of the kinetic parameters, i.e. preexponential factors and activation energies, were estimated by non-linear regression of the ethene conversion and found to be physically meaningful.

AB - The oxidation of ethene by oxygen in the presence of steam and carbon dioxide over a commercially available Pt/Rh/CeO2/¿-Al2O3 three-way automotive catalyst was studied. Experiments were carried out in a fixed-bed micro reactor under intrinsic conditions, i.e. in the absence of external and internal mass and heat transport limitations. A kinetic model based on elementary reaction steps was developed for the following range of experimental conditions: a total pressure of 110 kPa, temperatures between 463 and 483 K, ethene inlet partial pressures between 0.04 and 0.14 kPa, oxygen inlet partial pressures between 0.25 and 1.10 kPa and steam and carbon dioxide inlet partial pressures equal to 10 kPa. For these conditions, only the total oxidation of ethene to carbon dioxide and steam was observed. The reaction rate was found to decrease with increasing ethene partial pressure and decreasing oxygen partial pressure. Both carbon dioxide ans steam were found to inhibit the reaction rate. The activity of CeO2 can be neglected at the investigated conditions. The kinetic model comprises the following elementary steps: irreversible adsorption of oxygen and reversible adsorption of ethene on the noble metal surface, followed by a surface reaction between adsorbed ethene and oxygen. The values of the kinetic parameters, i.e. preexponential factors and activation energies, were estimated by non-linear regression of the ethene conversion and found to be physically meaningful.

U2 - 10.1016/S0167-2991(98)80895-1

DO - 10.1016/S0167-2991(98)80895-1

M3 - Conference contribution

SN - 0-444-82795-1

T3 - Studies in Surface Science and Catalysis

SP - 389

EP - 398

BT - Catalysis and automotive pollution control IV : proceedings of the Fourth International Symposium (CAPoC4), Brussels, Belgium, April 9 - 11, 1997

A2 - Kruse, N.

PB - Elsevier

CY - Amsterdam

ER -

Nibbelke RH, Kreijveld RJM, Hoebink JHBJ, Marin GBMM. Kinetic study of the ethene oxidation by oxygen in the presence of carbon dioxide and steam over Pt/Rh/CeO2/g-Al2O3. In Kruse N, editor, Catalysis and automotive pollution control IV : proceedings of the Fourth International Symposium (CAPoC4), Brussels, Belgium, April 9 - 11, 1997. Amsterdam: Elsevier. 1998. p. 389-398. (Studies in Surface Science and Catalysis). https://doi.org/10.1016/S0167-2991(98)80895-1