Reaction processes on catalytically active surfaces

In this article results of studies are reported in which in-situ infrared-visible sum-frequency generation (IR-VIS SFG) surface vibrational spectroscopy was combined with density functional theory (DFT) ab initio computations to investigate the adsorption of carbon monoxide (CO) on rhodium (Rh) cata...

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Hauptverfasser: Inderwildi, Oliver Richard (VerfasserIn) , Starukhin, Dzmitry (VerfasserIn) , Volpp, Hans-Robert (VerfasserIn) , Lebiedz, Dirk (VerfasserIn) , Warnatz, Jürgen (VerfasserIn)
Dokumenttyp: Kapitel/Artikel
Sprache:Englisch
Veröffentlicht: 2007
In: Reactive flows, diffusion and transport
Year: 2007, Pages: 311-340
DOI:10.1007/978-3-540-28396-6_12
Online-Zugang:Verlag, Volltext: http://dx.doi.org/10.1007/978-3-540-28396-6_12
Verlag, Volltext: https://link.springer.com/chapter/10.1007/978-3-540-28396-6_12
Volltext
Verfasserangaben:O.R. Inderwildi, D. Starukhin, H.-R. Volpp, D. Lebiedz, O. Deutschmann, and J. Warnatz

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520 |a In this article results of studies are reported in which in-situ infrared-visible sum-frequency generation (IR-VIS SFG) surface vibrational spectroscopy was combined with density functional theory (DFT) ab initio computations to investigate the adsorption of carbon monoxide (CO) on rhodium (Rh) catalyst surfaces at elevated substrate temperatures (Ts ≥ 300K) over a wide pressure-range (pco = 10−8−1000 mbar). The experimental studies demonstrated the reversible molecular adsorption of CO up to a pressure of ca. 10 mbar. For higher CO pressures, however, the onset of a new irreversible dissociative CO adsorption pathway could be observed already at a substrate temperature of Ts=300 K. CO dissociation was found to result in the formation of carbon on the surface as the only detectable dissociation product, indicating that CO dissociation occurs via the Boudouard reaction: 2CO → C(ad) + CO2. 
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