Kinetics of the water-gas shift reaction over Rh/Al2O 3 catalysts

Canan Karakaya; Robin Otterstätter; Lubow Maier; Olaf Deutschmann

doi:10.1016/j.apcata.2013.10.030

Kinetics of the water-gas shift reaction over Rh/Al₂O ₃ catalysts

Canan Karakaya, Robin Otterstätter, Lubow Maier, Olaf Deutschmann

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

46 Scopus citations

Abstract

The kinetics of the water-gas shift (WGS) reaction over Rh/Al ₂O₃ catalyst is studied experimentally and numerically. Using the experimentally determined conversion in WGS, reverse WGS, and preferential oxidation of CO over a catalytically coated disk and over a honeycomb monolith, a thermodynamically consistent multi-step reaction mechanism with the associated rate expressions was developed. Both the experimental configurations were numerically simulated coupling models for the flow field with this heterogeneous reaction mechanism. The main reaction path for CO ₂ formation on this catalyst is concluded to be the direct oxidation of CO with O species at high temperatures, whereas the formation of the carboxyl (COOH) group is significant at temperature below 600 C. The reaction kinetics reproduced the experimental observations, also for the subsystems of hydrogen and CO oxidation.

Original language	English
Pages (from-to)	31-44
Number of pages	14
Journal	Applied Catalysis A: General
Volume	470
DOIs	https://doi.org/10.1016/j.apcata.2013.10.030
State	Published - 2014
Externally published	Yes

Funding

This work was supported by Deutsche Forschungsgemeinschaft (DFG) . We thank S. Tischer and H. Karadeniz (KIT) for their supports in using DETCHEM™ and R.J. Kee (Colorado School of Mines) for collaboration during the development of the stagnation flow reactor and many fruitful discussions.

Funders	Funder number
Deutsche Forschungsgemeinschaft

Keywords

Carboxyl
Kinetics
Modeling
Rhodium
Stagnation-flow reactor
Water-gas shift

Access to Document

10.1016/j.apcata.2013.10.030

Cite this

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title = "Kinetics of the water-gas shift reaction over Rh/Al2O 3 catalysts",

abstract = "The kinetics of the water-gas shift (WGS) reaction over Rh/Al 2O3 catalyst is studied experimentally and numerically. Using the experimentally determined conversion in WGS, reverse WGS, and preferential oxidation of CO over a catalytically coated disk and over a honeycomb monolith, a thermodynamically consistent multi-step reaction mechanism with the associated rate expressions was developed. Both the experimental configurations were numerically simulated coupling models for the flow field with this heterogeneous reaction mechanism. The main reaction path for CO 2 formation on this catalyst is concluded to be the direct oxidation of CO with O species at high temperatures, whereas the formation of the carboxyl (COOH) group is significant at temperature below 600 C. The reaction kinetics reproduced the experimental observations, also for the subsystems of hydrogen and CO oxidation.",

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AU - Karakaya, Canan

AU - Otterstätter, Robin

AU - Maier, Lubow

AU - Deutschmann, Olaf

PY - 2014

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AB - The kinetics of the water-gas shift (WGS) reaction over Rh/Al 2O3 catalyst is studied experimentally and numerically. Using the experimentally determined conversion in WGS, reverse WGS, and preferential oxidation of CO over a catalytically coated disk and over a honeycomb monolith, a thermodynamically consistent multi-step reaction mechanism with the associated rate expressions was developed. Both the experimental configurations were numerically simulated coupling models for the flow field with this heterogeneous reaction mechanism. The main reaction path for CO 2 formation on this catalyst is concluded to be the direct oxidation of CO with O species at high temperatures, whereas the formation of the carboxyl (COOH) group is significant at temperature below 600 C. The reaction kinetics reproduced the experimental observations, also for the subsystems of hydrogen and CO oxidation.

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