Probing the electronic structure of an active catalyst surface under high-pressure reaction conditions: the oxidation of methanol over copper |
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Authors: | A. Knop-Gericke M. Hävecker T. Schedel-Niedrig R. Schlögl |
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Affiliation: | (1) Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Germany |
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Abstract: | The active phase of a bulk metallic copper catalyst is investigated by surface sensitive X-ray absorption spectroscopy at the oxygen K-edge and the Cu L-edges in the total electron yield mode under practical steady state flow-through conditions. The active catalyst surface contains oxygen atoms revealing significant spectral differences compared to those of known copper oxides. The partial oxidation of methanol to formaldehyde is correlated to the abundance of this copper suboxide. These oxygen atoms probe defects of the copper lattice, which represent catalytically active sites. The suboxide is undetectable under UHV conditions. The total oxidation of methanol is catalysed by a conventional copper(I) oxide species and the abundance of carbon dioxide in the gas phase is increasing with decreasing integrated intensity of the oxide species. This revised version was published online in July 2006 with corrections to the Cover Date. |
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Keywords: | catalytical oxidation of methanol over copper partial oxidation copper suboxide copper(I) oxide total oxidation in situ O K-XANES |
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