Structure sensitivity of the methanation reaction : H2-induced CO dissociation on nickel surfaces

The dissociation of CO serves both as a model test reaction on single crystals and as a relevant reaction step for industrial methanation. We combined extensive density functional theory calculations, ultra-high vacuum experiments on well-defined single crystals, and catalytic activity measurements...

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Veröffentlicht in:Journal of catalysis 2008-04, Vol.255 (1), p.6-19
Hauptverfasser: ANDERSSON, M. P, ABILD-PEDERSEN, F, ROSTRUP-NIELSEN, J. R, NØRSKOV, J. K, CHORKENDORFF, I, REMEDIAKIS, I. N, BLIGAARD, T, JONES, G, ENGBAEK, J, LYTKEN, O, HORCH, S, NIELSEN, J. H, SEHESTED, J
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Sprache:eng
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Zusammenfassung:The dissociation of CO serves both as a model test reaction on single crystals and as a relevant reaction step for industrial methanation. We combined extensive density functional theory calculations, ultra-high vacuum experiments on well-defined single crystals, and catalytic activity measurements on supported catalysts in a study of the dissociation mechanism of CO on Ni surfaces. We found that this process is highly structure-sensitive and also is sensitive to the presence of hydrogen: Under ultra-high vacuum, with no hydrogen present, the dissociation proceeds through a direct route in which only undercoordinated sites (e.g., steps) are active. Under methanation conditions, the dissociation also proceeds most favorably over undercoordinated sites, but through a COH species. [PUBLICATION ABSTRACT]
ISSN:0021-9517
1090-2694
DOI:10.1016/j.jcat.2007.12.016