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Structure-function relationship during CO2 methanation over Rh/Al2O3 and Rh/SiO2 catalysts under atmospheric pressure conditions

Martin, Natalia M. LU ; Hemmingsson, Felix ; Wang, Xueting ; Merte, Lindsay R. LU ; Hejral, Uta LU ; Gustafson, Johan LU ; Skoglundh, Magnus ; Meira, Debora Motta ; Dippel, Ann Christin and Gutowski, Olof , et al. (2018) In Catalysis Science and Technology 8(10). p.2686-2696
Abstract

The effect of the support material and chemical state of Rh in Rh/A2O3 and Rh/SiO2 model catalysts during CO2 hydrogenation were studied by a combined array of in situ characterisation techniques including diffuse reflectance infrared Fourier transform spectroscopy, energy-dispersive X-ray absorption spectroscopy and high-energy X-ray diffraction at 250-350 °C and atmospheric pressure. CO2 methanation proceeds via intermediate formation of adsorbed CO species on metallic Rh, likely followed by their hydrogenation to methane. The linearly-bonded CO species is suggested to be a more active precursor in the hydrogenation compared to the bridge-bonded species, which seems to be related... (More)

The effect of the support material and chemical state of Rh in Rh/A2O3 and Rh/SiO2 model catalysts during CO2 hydrogenation were studied by a combined array of in situ characterisation techniques including diffuse reflectance infrared Fourier transform spectroscopy, energy-dispersive X-ray absorption spectroscopy and high-energy X-ray diffraction at 250-350 °C and atmospheric pressure. CO2 methanation proceeds via intermediate formation of adsorbed CO species on metallic Rh, likely followed by their hydrogenation to methane. The linearly-bonded CO species is suggested to be a more active precursor in the hydrogenation compared to the bridge-bonded species, which seems to be related to particle size effects: for larger particles mainly the formation of inactive bridge-bonded CO species takes place. Further, analysis of the chemical state of Rh under the reaction conditions reveal a minor formation of RhOx from dissociation of CO2, which is a consequence of the increased activity observed over the Rh/Al2O3 catalyst.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Catalysis Science and Technology
volume
8
issue
10
pages
11 pages
publisher
Royal Society of Chemistry
external identifiers
  • scopus:85047647969
ISSN
2044-4753
DOI
10.1039/c8cy00516h
language
English
LU publication?
yes
id
c6c41b68-de2f-42e3-8809-42c29cb39fba
date added to LUP
2018-06-15 14:56:36
date last changed
2023-11-17 20:21:59
@article{c6c41b68-de2f-42e3-8809-42c29cb39fba,
  abstract     = {{<p>The effect of the support material and chemical state of Rh in Rh/A<sub>2</sub>O<sub>3</sub> and Rh/SiO<sub>2</sub> model catalysts during CO<sub>2</sub> hydrogenation were studied by a combined array of in situ characterisation techniques including diffuse reflectance infrared Fourier transform spectroscopy, energy-dispersive X-ray absorption spectroscopy and high-energy X-ray diffraction at 250-350 °C and atmospheric pressure. CO<sub>2</sub> methanation proceeds via intermediate formation of adsorbed CO species on metallic Rh, likely followed by their hydrogenation to methane. The linearly-bonded CO species is suggested to be a more active precursor in the hydrogenation compared to the bridge-bonded species, which seems to be related to particle size effects: for larger particles mainly the formation of inactive bridge-bonded CO species takes place. Further, analysis of the chemical state of Rh under the reaction conditions reveal a minor formation of RhO<sub>x</sub> from dissociation of CO<sub>2</sub>, which is a consequence of the increased activity observed over the Rh/Al<sub>2</sub>O<sub>3</sub> catalyst.</p>}},
  author       = {{Martin, Natalia M. and Hemmingsson, Felix and Wang, Xueting and Merte, Lindsay R. and Hejral, Uta and Gustafson, Johan and Skoglundh, Magnus and Meira, Debora Motta and Dippel, Ann Christin and Gutowski, Olof and Bauer, Matthias and Carlsson, Per Anders}},
  issn         = {{2044-4753}},
  language     = {{eng}},
  month        = {{01}},
  number       = {{10}},
  pages        = {{2686--2696}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Catalysis Science and Technology}},
  title        = {{Structure-function relationship during CO<sub>2</sub> methanation over Rh/Al<sub>2</sub>O<sub>3</sub> and Rh/SiO<sub>2</sub> catalysts under atmospheric pressure conditions}},
  url          = {{http://dx.doi.org/10.1039/c8cy00516h}},
  doi          = {{10.1039/c8cy00516h}},
  volume       = {{8}},
  year         = {{2018}},
}