Infrared spectroscopy investigation of Fe-promoted Rh catalysts supported on Titania and Ceria for CO hydrogenation

Magee, Joseph W.; Palomino, Robert M.; White, Michael G.

doi:10.1007/s10562-016-1801-y

Infrared spectroscopy investigation of Fe-promoted Rh catalysts supported on Titania and Ceria for CO hydrogenation

Journal Article · Mon Jul 04 00:00:00 EDT 2016 · Catalysis Letters

DOI:https://doi.org/10.1007/s10562-016-1801-y· OSTI ID:1333205

Magee, Joseph W. ^[1]; Palomino, Robert M. ^[2]; White, Michael G. ^[3]

Stony Brook Univ., Stony Brook, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Stony Brook Univ., Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

The nature of the promotional effect of Fe addition to Rh/TiO₂ and Rh/CeO₂ catalysts for CO hydrogenation was investigated using FT-IR spectroscopy in an ultrahigh vacuum compatible transmission IR cell. CO adsorption experiments on Rh and FeRh showed vibrational signatures characteristic of linear and bridge bound CO on Rh0 as well as geminal-dicarbonyl species associated with Rh⁺. Compared to TiO₂, the CeO₂-supported catalysts show increased dispersion, reflected by decreased particle size, and a lower signal for linear versus geminal-dicarbonyl bonded CO. The absorption frequencies for CO on Rh/CeO₂ are also redshifted relative to Rh/TiO₂, which results from a weaker Rh–CO interaction, likely due to the increased reducibility of the CeO₂ support. Upon addition of Fe, a new spectral feature is observed and attributed to CO bound to Rh in close contact with Fe, likely as a surface alloy. CO hydrogenation on (Fe)Rh catalysts on both supports was also studied. Compared to bare Rh, Fe containing catalysts promote formate and methoxy species on the surface at lower temperature (180 °C), which suggests an enhancement in methanol selectivity by Fe addition. Furthermore, at higher temperatures (220 °C), the spectral features appear similar, further confirming the role of Fe as a disrupter of large Rh^o crystallites and regulator of CO dissociation and CH₄ formation.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

OSTI ID:: 1333205

Report Number(s):: BNL--113211-2016-JA; KC0301050

Journal Information:: Catalysis Letters, Journal Name: Catalysis Letters Journal Issue: 9 Vol. 146; ISSN 1011-372X

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO hydrogenation
FeRh alloy
ethanol
heterogeneous catalysis
infrared spectroscopy

Infrared spectroscopy investigation of Fe-promoted Rh catalysts supported on Titania and Ceria for CO hydrogenation

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