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Oxidation of methanol on Ru catalyst: Effect of the reagents partial pressures on the catalyst oxidation state and selectivity

MPS-Authors
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Blume,  Raoul
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Hävecker,  Michael
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Zafeiratos,  Spiros
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Teschner,  Detre
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Knop-Gericke,  Axel
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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337719.pdf
(Preprint), 544KB

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Citation

Blume, R., Hävecker, M., Zafeiratos, S., Teschner, D., Knop-Gericke, A., Schlögl, R., et al. (2007). Oxidation of methanol on Ru catalyst: Effect of the reagents partial pressures on the catalyst oxidation state and selectivity. Catalysis Today, 124(1-2), 71-79. doi:10.1016/j.cattod.2007.02.030.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0011-008C-F
Abstract
In situ core level photoelectron spectroscopy and mass spectrometry have been utilized to study the methanol oxidation on a model RuO2 catalyst at pressures ranging from 10-6 to 10-1 mbar. The experiments were carried out varying the O2/CH3OH molecular mixing ratio from 0.25 to 3.3 and the reaction temperature from 350 to 720 K. The Ru 3d5/2 and O 1s core level spectra were used to characterise the dynamic changes in the Ru oxidation state by exposing the oxide pre-catalyst to different reagents partial pressures and temperatures. Full oxidation to CO2 + H2O or partial oxidation to CO + H2O + H2 have been observed in the whole pressure range for specific reaction conditions, which preserve the oxide catalyst state or reduce the oxide to metallic Ru. The selective oxidation to formaldehyde is observed only at pressures in the 10-1 mbar range, catalyzed by a RuO_x surface oxide formed by partial reduction of the oxide pre-catalyst.