The role of Ir in ternary Rh-based catalysts for syngas conversion to C 2 + oxygenates

Vassiliki Alexandra Glezakou; John E. Jaffe; Roger Rousseau; Donghai Mei; Shawn M. Kathmann; Karl O. Albrecht; Michel J. Gray; Mark A. Gerber

doi:10.1007/s11244-012-9836-9

The role of Ir in ternary Rh-based catalysts for syngas conversion to C ₂ ⁺ oxygenates

Vassiliki Alexandra Glezakou, John E. Jaffe, Roger Rousseau, Donghai Mei, Shawn M. Kathmann, Karl O. Albrecht, Michel J. Gray, Mark A. Gerber

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

12 Scopus citations

Abstract

Transition metal modified Rh-catalysts can be used for converting syngas (CO + H ₂) into C ₂ ⁺ oxygenates. It has been found that Mn has a favorable effect in the selectivity towards oxygenates, while addition of Ir to the binary Rh-Mn catalysts significantly increases the space-time-yield (STY) of C ₂ ⁺ oxygenates, mainly by formyl formation at the early stages of conversion. Quantum mechanical calculations used to investigate the distribution of promoter sites in Rh-rich nanoparticles show that moderately high Mn/Ir ratios result in particles with all 3 metals on the surface, and that Ir atoms act as co-adsorption sinks of CO and H leading to HCO in the initial stages.

Original language	English
Pages (from-to)	595-600
Number of pages	6
Journal	Topics in Catalysis
Volume	55
Issue number	7-10
DOIs	https://doi.org/10.1007/s11244-012-9836-9
State	Published - Jul 2012
Externally published	Yes

Funding

Acknowledgments This work was supported by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy Biomass Program. The Pacific Northwest National Laboratory (PNNL) is operated by Battelle for the DOE under Contract DE-AC05-76RL01830. A portion of the research was performed using EMSL, a national science user facility sponsored by the Department of Energy’s Office of Biological and Environmental Research located at PNNL.

Funders	Funder number
Department of Energy
Office of Energy Efficiency and Renewable Energy Biomass Program
PNNL
U.S. Department of Energy
Biological and Environmental Research

Keywords

DFT models
Ir-Mn-Rh nanoparticle
Syngas conversion

Access to Document

10.1007/s11244-012-9836-9

Cite this

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abstract = "Transition metal modified Rh-catalysts can be used for converting syngas (CO + H 2) into C 2 + oxygenates. It has been found that Mn has a favorable effect in the selectivity towards oxygenates, while addition of Ir to the binary Rh-Mn catalysts significantly increases the space-time-yield (STY) of C 2 + oxygenates, mainly by formyl formation at the early stages of conversion. Quantum mechanical calculations used to investigate the distribution of promoter sites in Rh-rich nanoparticles show that moderately high Mn/Ir ratios result in particles with all 3 metals on the surface, and that Ir atoms act as co-adsorption sinks of CO and H leading to HCO in the initial stages.",

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AU - Glezakou, Vassiliki Alexandra

AU - Jaffe, John E.

AU - Rousseau, Roger

AU - Mei, Donghai

AU - Kathmann, Shawn M.

AU - Albrecht, Karl O.

AU - Gray, Michel J.

AU - Gerber, Mark A.

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AB - Transition metal modified Rh-catalysts can be used for converting syngas (CO + H 2) into C 2 + oxygenates. It has been found that Mn has a favorable effect in the selectivity towards oxygenates, while addition of Ir to the binary Rh-Mn catalysts significantly increases the space-time-yield (STY) of C 2 + oxygenates, mainly by formyl formation at the early stages of conversion. Quantum mechanical calculations used to investigate the distribution of promoter sites in Rh-rich nanoparticles show that moderately high Mn/Ir ratios result in particles with all 3 metals on the surface, and that Ir atoms act as co-adsorption sinks of CO and H leading to HCO in the initial stages.

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