Transient-response study of CO insertion into CHx surface intermediates on a vanadium-promoted rhodium catalyst

T. Koerts; R.A. Santen, van

doi:10.1016/0021-9517%2892%2990205-V

Transient-response study of CO insertion into CHx surface intermediates on a vanadium-promoted rhodium catalyst

T. Koerts, R.A. Santen, van

Inorganic Materials & Catalysis

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

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Abstract

The rate of CO insertion into surface CHx species was investigated on silica-supported rhodium and rhodium-vanadium catalysts. Isotopically labelled 13CO was used in a transient kinetic experiment under steady-state conditions. A main conclusion is that vanadium promotion does not affect the rate of CO insertion. From temperature-programmed surface reaction measurements the surface concentration of CHx species during steady-state reaction was determined. It is increased by vanadium coadsorption. Combining these data with the selectivity and activity in synthesis gas to oxygenate conversion, a model is derived from which reaction rates of elementary steps and surface concentrations are calculated. Ethanal formation appears to occur at two distinguishable sites. Vanadium promotion decreases the desorption rate of ethanal, enhances the hydrogenation rate to ethanol, and increases the surface concentration of oxygenated intermediates.

Original language	English
Pages (from-to)	13-23
Number of pages	11
Journal	Journal of Catalysis
Volume	134
Issue number	1
DOIs	https://doi.org/10.1016/0021-9517%2892%2990205-V https://doi.org/10.1016/0021-9517(92)90205-V
Publication status	Published - 1992

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title = "Transient-response study of CO insertion into CHx surface intermediates on a vanadium-promoted rhodium catalyst",

abstract = "The rate of CO insertion into surface CHx species was investigated on silica-supported rhodium and rhodium-vanadium catalysts. Isotopically labelled 13CO was used in a transient kinetic experiment under steady-state conditions. A main conclusion is that vanadium promotion does not affect the rate of CO insertion. From temperature-programmed surface reaction measurements the surface concentration of CHx species during steady-state reaction was determined. It is increased by vanadium coadsorption. Combining these data with the selectivity and activity in synthesis gas to oxygenate conversion, a model is derived from which reaction rates of elementary steps and surface concentrations are calculated. Ethanal formation appears to occur at two distinguishable sites. Vanadium promotion decreases the desorption rate of ethanal, enhances the hydrogenation rate to ethanol, and increases the surface concentration of oxygenated intermediates.",

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AU - Santen, van, R.A.

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N2 - The rate of CO insertion into surface CHx species was investigated on silica-supported rhodium and rhodium-vanadium catalysts. Isotopically labelled 13CO was used in a transient kinetic experiment under steady-state conditions. A main conclusion is that vanadium promotion does not affect the rate of CO insertion. From temperature-programmed surface reaction measurements the surface concentration of CHx species during steady-state reaction was determined. It is increased by vanadium coadsorption. Combining these data with the selectivity and activity in synthesis gas to oxygenate conversion, a model is derived from which reaction rates of elementary steps and surface concentrations are calculated. Ethanal formation appears to occur at two distinguishable sites. Vanadium promotion decreases the desorption rate of ethanal, enhances the hydrogenation rate to ethanol, and increases the surface concentration of oxygenated intermediates.

AB - The rate of CO insertion into surface CHx species was investigated on silica-supported rhodium and rhodium-vanadium catalysts. Isotopically labelled 13CO was used in a transient kinetic experiment under steady-state conditions. A main conclusion is that vanadium promotion does not affect the rate of CO insertion. From temperature-programmed surface reaction measurements the surface concentration of CHx species during steady-state reaction was determined. It is increased by vanadium coadsorption. Combining these data with the selectivity and activity in synthesis gas to oxygenate conversion, a model is derived from which reaction rates of elementary steps and surface concentrations are calculated. Ethanal formation appears to occur at two distinguishable sites. Vanadium promotion decreases the desorption rate of ethanal, enhances the hydrogenation rate to ethanol, and increases the surface concentration of oxygenated intermediates.

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DO - 10.1016/0021-9517%2892%2990205-V

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JO - Journal of Catalysis

JF - Journal of Catalysis

SN - 0021-9517

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