Direct evidence for the correlation between surface carbon and CO + H2 selectivity on iron and iron-Ruthenium catalysts prepared from metal carbonyl clusters

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Abstract

In situ Mössbauer studies and simultaneous catalytic reactions of CO + H2 mixtures at 1 and 20 bars pressure to form olefins were carried out on Fe and Fe-Ru bimetallic catalysts prepared by impregnation of Cab-O-Sil® with a hexane solution of Fe3(CO)12 and a mixture of Fe3(CO)12 and Ru3(CO)12. Under reaction conditions the main component of the Mössbauer spectra(I.S. = 0.0 mm s-1 and Q.S. = 0.5 mm s-) can be assigned to the reacting species of surface carbon, which can be distinguished from χ-carbide which has also formed during the reaction. In the presence of ruthenium, the spectra are very similar to those measured on iron, but a large χ-carbide signal with hyperfine splitting cannot be detected. From the kinetic and in situ Mössbauer experiments carried out under different conditions, direct evidence was found for the formation of mobile, reactive carbon which participates in the production of olefins and higher hydrocarbons. It can be transformed either into other types of carbon, one of which is responsible for methane formation, or into that species responsible for catalyst deactivation. A possible mechanism is discussed in this paper.

Original languageEnglish
Pages (from-to)205-218
Number of pages14
JournalJournal of Molecular Catalysis
Volume17
Issue number2-3
DOIs
Publication statusPublished - 1982

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Catalyst selectivity
Ruthenium
Iron
Catalysts
Olefins
Carbon
Carbides
Metals
Catalyst deactivation
Hexane
Impregnation
Methane
Hydrocarbons
Kinetics
Experiments

ASJC Scopus subject areas

  • Engineering(all)

Cite this

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title = "Direct evidence for the correlation between surface carbon and CO + H2 selectivity on iron and iron-Ruthenium catalysts prepared from metal carbonyl clusters",
abstract = "In situ M{\"o}ssbauer studies and simultaneous catalytic reactions of CO + H2 mixtures at 1 and 20 bars pressure to form olefins were carried out on Fe and Fe-Ru bimetallic catalysts prepared by impregnation of Cab-O-Sil{\circledR} with a hexane solution of Fe3(CO)12 and a mixture of Fe3(CO)12 and Ru3(CO)12. Under reaction conditions the main component of the M{\"o}ssbauer spectra(I.S. = 0.0 mm s-1 and Q.S. = 0.5 mm s-) can be assigned to the reacting species of surface carbon, which can be distinguished from χ-carbide which has also formed during the reaction. In the presence of ruthenium, the spectra are very similar to those measured on iron, but a large χ-carbide signal with hyperfine splitting cannot be detected. From the kinetic and in situ M{\"o}ssbauer experiments carried out under different conditions, direct evidence was found for the formation of mobile, reactive carbon which participates in the production of olefins and higher hydrocarbons. It can be transformed either into other types of carbon, one of which is responsible for methane formation, or into that species responsible for catalyst deactivation. A possible mechanism is discussed in this paper.",
author = "K. L{\'a}z{\'a}r and Z. Schay and L. Guczi",
year = "1982",
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AU - Lázár, K.

AU - Schay, Z.

AU - Guczi, L.

PY - 1982

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N2 - In situ Mössbauer studies and simultaneous catalytic reactions of CO + H2 mixtures at 1 and 20 bars pressure to form olefins were carried out on Fe and Fe-Ru bimetallic catalysts prepared by impregnation of Cab-O-Sil® with a hexane solution of Fe3(CO)12 and a mixture of Fe3(CO)12 and Ru3(CO)12. Under reaction conditions the main component of the Mössbauer spectra(I.S. = 0.0 mm s-1 and Q.S. = 0.5 mm s-) can be assigned to the reacting species of surface carbon, which can be distinguished from χ-carbide which has also formed during the reaction. In the presence of ruthenium, the spectra are very similar to those measured on iron, but a large χ-carbide signal with hyperfine splitting cannot be detected. From the kinetic and in situ Mössbauer experiments carried out under different conditions, direct evidence was found for the formation of mobile, reactive carbon which participates in the production of olefins and higher hydrocarbons. It can be transformed either into other types of carbon, one of which is responsible for methane formation, or into that species responsible for catalyst deactivation. A possible mechanism is discussed in this paper.

AB - In situ Mössbauer studies and simultaneous catalytic reactions of CO + H2 mixtures at 1 and 20 bars pressure to form olefins were carried out on Fe and Fe-Ru bimetallic catalysts prepared by impregnation of Cab-O-Sil® with a hexane solution of Fe3(CO)12 and a mixture of Fe3(CO)12 and Ru3(CO)12. Under reaction conditions the main component of the Mössbauer spectra(I.S. = 0.0 mm s-1 and Q.S. = 0.5 mm s-) can be assigned to the reacting species of surface carbon, which can be distinguished from χ-carbide which has also formed during the reaction. In the presence of ruthenium, the spectra are very similar to those measured on iron, but a large χ-carbide signal with hyperfine splitting cannot be detected. From the kinetic and in situ Mössbauer experiments carried out under different conditions, direct evidence was found for the formation of mobile, reactive carbon which participates in the production of olefins and higher hydrocarbons. It can be transformed either into other types of carbon, one of which is responsible for methane formation, or into that species responsible for catalyst deactivation. A possible mechanism is discussed in this paper.

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