Catalysis by supported clusters: Chemisorption, decomposition and catalytic properties in fischer-tropsch synthesis of Fe3(CO)12, [H Fe3(CO)11]- (and Fe(CO)5) supported on highly divided oxides

F. Hugues; P. Bussiere; Jean-Marie Maurice Basset; D. Commereuc; Y. Chauvin; L. Bonneviot; D. Olivier

doi:10.1016/S0167-2991(09)60288-3

Catalysis by supported clusters: Chemisorption, decomposition and catalytic properties in fischer-tropsch synthesis of Fe₃(CO)₁₂, [H Fe₃(CO)₁₁]- (and Fe(CO)₅) supported on highly divided oxides

F. Hugues, P. Bussiere, Jean-Marie Maurice Basset, D. Commereuc, Y. Chauvin, L. Bonneviot, D. Olivier

Physical Science and Engineering

Research output: Contribution to journal › Article › peer-review

19 Scopus citations

Abstract

Fe(CO)₅, Fe₃(CO)₁₂ and [H Fe₃(CO)₁₁]⁻ supported on Al₂O₃ or MgO exhibit after decomposition under CO + H₂ a very high selectivity for low molecular weight olefins. Characterisation of the supported complexes before and after decomposition has been carried out using Ferromagnetic Resonance, Mössbauer Spectroscopy, Electron Microscopy and analysis of the gas phase. The behaviour of the precursor carbonyl depends on the water content of the support before impregnation: with dehydroxylated alumina and magnesia, thermal decomposition (T < 200°C) into superparamagnetic very small metal particles (q < 15 Å) occurs. Above 200°C, sintering to particles of higher sizes occurs to a certain extent. With hydroxylated alumina and magnesia, thermal decomposition leads to a mixture of superparamagnetic metallic particles and iron oxides. The oxidation of zerovalent icon is due to surface protons with evolution of hydrogen. The resulting high selectivities for low molecular weight olefins (ethylene, propylene) would result from the low particle sizes of metallic iron generated from zerovalent cluster carbonyls.

Original language	English (US)
Pages (from-to)	418-431
Number of pages	14
Journal	Studies in Surface Science and Catalysis
Volume	7
DOIs	https://doi.org/10.1016/S0167-2991(09)60288-3
State	Published - Jan 1 1981

ASJC Scopus subject areas

Catalysis
Condensed Matter Physics
Physical and Theoretical Chemistry
Surfaces, Coatings and Films
Materials Chemistry

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Hugues, F., Bussiere, P., Basset, J-M. M., Commereuc, D., Chauvin, Y., Bonneviot, L., & Olivier, D. (1981). Catalysis by supported clusters: Chemisorption, decomposition and catalytic properties in fischer-tropsch synthesis of Fe₃(CO)₁₂, [H Fe₃(CO)₁₁]- (and Fe(CO)₅) supported on highly divided oxides. Studies in Surface Science and Catalysis, 7, 418-431. https://doi.org/10.1016/S0167-2991(09)60288-3

Hugues, F. ; Bussiere, P. ; Basset, Jean-Marie Maurice ; Commereuc, D. ; Chauvin, Y. ; Bonneviot, L. ; Olivier, D. / Catalysis by supported clusters : Chemisorption, decomposition and catalytic properties in fischer-tropsch synthesis of Fe₃(CO)₁₂, [H Fe₃(CO)₁₁]- (and Fe(CO)₅) supported on highly divided oxides. In: Studies in Surface Science and Catalysis. 1981 ; Vol. 7. pp. 418-431.

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title = "Catalysis by supported clusters: Chemisorption, decomposition and catalytic properties in fischer-tropsch synthesis of Fe3(CO)12, [H Fe3(CO)11]- (and Fe(CO)5) supported on highly divided oxides",

abstract = "Fe(CO)5, Fe3(CO)12 and [H Fe3(CO)11]− supported on Al2O3 or MgO exhibit after decomposition under CO + H2 a very high selectivity for low molecular weight olefins. Characterisation of the supported complexes before and after decomposition has been carried out using Ferromagnetic Resonance, M{\"o}ssbauer Spectroscopy, Electron Microscopy and analysis of the gas phase. The behaviour of the precursor carbonyl depends on the water content of the support before impregnation: with dehydroxylated alumina and magnesia, thermal decomposition (T < 200°C) into superparamagnetic very small metal particles (q < 15 {\AA}) occurs. Above 200°C, sintering to particles of higher sizes occurs to a certain extent. With hydroxylated alumina and magnesia, thermal decomposition leads to a mixture of superparamagnetic metallic particles and iron oxides. The oxidation of zerovalent icon is due to surface protons with evolution of hydrogen. The resulting high selectivities for low molecular weight olefins (ethylene, propylene) would result from the low particle sizes of metallic iron generated from zerovalent cluster carbonyls.",

author = "F. Hugues and P. Bussiere and Basset, {Jean-Marie Maurice} and D. Commereuc and Y. Chauvin and L. Bonneviot and D. Olivier",

year = "1981",

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doi = "10.1016/S0167-2991(09)60288-3",

language = "English (US)",

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Hugues, F, Bussiere, P, Basset, J-MM, Commereuc, D, Chauvin, Y, Bonneviot, L & Olivier, D 1981, 'Catalysis by supported clusters: Chemisorption, decomposition and catalytic properties in fischer-tropsch synthesis of Fe₃(CO)₁₂, [H Fe₃(CO)₁₁]- (and Fe(CO)₅) supported on highly divided oxides', Studies in Surface Science and Catalysis, vol. 7, pp. 418-431. https://doi.org/10.1016/S0167-2991(09)60288-3

Catalysis by supported clusters : Chemisorption, decomposition and catalytic properties in fischer-tropsch synthesis of Fe₃(CO)₁₂, [H Fe₃(CO)₁₁]- (and Fe(CO)₅) supported on highly divided oxides. / Hugues, F.; Bussiere, P.; Basset, Jean-Marie Maurice; Commereuc, D.; Chauvin, Y.; Bonneviot, L.; Olivier, D.

In: Studies in Surface Science and Catalysis, Vol. 7, 01.01.1981, p. 418-431.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Catalysis by supported clusters

T2 - Chemisorption, decomposition and catalytic properties in fischer-tropsch synthesis of Fe3(CO)12, [H Fe3(CO)11]- (and Fe(CO)5) supported on highly divided oxides

AU - Hugues, F.

AU - Bussiere, P.

AU - Basset, Jean-Marie Maurice

AU - Commereuc, D.

AU - Chauvin, Y.

AU - Bonneviot, L.

AU - Olivier, D.

PY - 1981/1/1

Y1 - 1981/1/1

N2 - Fe(CO)5, Fe3(CO)12 and [H Fe3(CO)11]− supported on Al2O3 or MgO exhibit after decomposition under CO + H2 a very high selectivity for low molecular weight olefins. Characterisation of the supported complexes before and after decomposition has been carried out using Ferromagnetic Resonance, Mössbauer Spectroscopy, Electron Microscopy and analysis of the gas phase. The behaviour of the precursor carbonyl depends on the water content of the support before impregnation: with dehydroxylated alumina and magnesia, thermal decomposition (T < 200°C) into superparamagnetic very small metal particles (q < 15 Å) occurs. Above 200°C, sintering to particles of higher sizes occurs to a certain extent. With hydroxylated alumina and magnesia, thermal decomposition leads to a mixture of superparamagnetic metallic particles and iron oxides. The oxidation of zerovalent icon is due to surface protons with evolution of hydrogen. The resulting high selectivities for low molecular weight olefins (ethylene, propylene) would result from the low particle sizes of metallic iron generated from zerovalent cluster carbonyls.

AB - Fe(CO)5, Fe3(CO)12 and [H Fe3(CO)11]− supported on Al2O3 or MgO exhibit after decomposition under CO + H2 a very high selectivity for low molecular weight olefins. Characterisation of the supported complexes before and after decomposition has been carried out using Ferromagnetic Resonance, Mössbauer Spectroscopy, Electron Microscopy and analysis of the gas phase. The behaviour of the precursor carbonyl depends on the water content of the support before impregnation: with dehydroxylated alumina and magnesia, thermal decomposition (T < 200°C) into superparamagnetic very small metal particles (q < 15 Å) occurs. Above 200°C, sintering to particles of higher sizes occurs to a certain extent. With hydroxylated alumina and magnesia, thermal decomposition leads to a mixture of superparamagnetic metallic particles and iron oxides. The oxidation of zerovalent icon is due to surface protons with evolution of hydrogen. The resulting high selectivities for low molecular weight olefins (ethylene, propylene) would result from the low particle sizes of metallic iron generated from zerovalent cluster carbonyls.

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U2 - 10.1016/S0167-2991(09)60288-3

DO - 10.1016/S0167-2991(09)60288-3

M3 - Article

AN - SCOPUS:20344394327

VL - 7

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EP - 431

JO - Studies in Surface Science and Catalysis

JF - Studies in Surface Science and Catalysis

SN - 0167-2991

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