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

The nature of the promotional effect of Fe addition to Rh/TiO 2 and Rh/CeO 2 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 TiO 2, the CeO 2-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/CeO 2 are also redshifted relative to Rh/TiO 2, which results from a weaker Rh–CO interaction, likely due to the increased reducibility of the CeO 2 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 confirmingmore » the role of Fe as a disrupter of large Rh o crystallites and regulator of CO dissociation and CH 4 formation.« less
 [1] ;  [2] ;  [3]
  1. Stony Brook Univ., Stony Brook, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Stony Brook Univ., Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
Journal ID: ISSN 1011-372X; R&D Project: CO007; KC0301050
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Catalysis Letters
Additional Journal Information:
Journal Volume: 146; Journal Issue: 9; Journal ID: ISSN 1011-372X
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; heterogeneous catalysis; infrared spectroscopy; CO hydrogenation; FeRh alloy; ethanol
OSTI Identifier: