NDLI: Dehydrogenation of Dodecahydro-N-ethylcarbazole on $Pd/Al_{2}O_{3}$ Model Catalysts

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Dehydrogenation of Dodecahydro-N-ethylcarbazole on $Pd/Al_{2}O_{3}$ Model Catalysts

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Laurin, Mathias Amende, Max Görling, Andreas Assenbaum, Daniel Sobota, Marek Wasserscheid, Peter Sanmartín Zanón, Beatriz Papp, Christian Nikiforidis, Ioannis Hieringer, Wolfgang Höfert, Oliver Steinrück, Hans-peter Lykhach, Yaroslava Staudt, Thorsten Libuda, Jörg
Description	Author Affiliation: Sobota M ( Physical Chemistry 2, Department of Chemistry and Pharmacy, University Erlangen-Nuremberg, Egerlandstr. 3, 91058 Erlangen, Germany.)
Abstract	To elucidate the dehydrogenation mechanism of dodecahydro-N-ethylcarbazole $(H_{12}-NEC)$ on supported Pd catalysts, we have performed a model study under ultra high vacuum (UHV) conditions. $H_{12}-NEC$ and its final dehydrogenation product, N-ethylcarbazole (NEC), were deposited by physical vapor deposition (PVD) at temperatures between 120 K and 520 K onto a supported model catalyst, which consisted of Pd nanoparticles grown on a well-ordered alumina film on NiAl(110). Adsorption and thermally induced surface reactions were followed by infrared reflection absorption spectroscopy (IRAS) and high-resolution X-ray photoelectron spectroscopy (HR-XPS) in combination with density functional theory (DFT) calculations. It was shown that, at 120 K, $H_{12}-NEC$ adsorbs molecularly both on the $Al_{2}O_{3}/NiAl(110)$ support and on the Pd particles. Initial activation of the molecule occurs through CH bond scission at the 8a- and 9a-positions of the carbazole skeleton at temperatures above 170 K. Dehydrogenation successively proceeds with increasing temperature. Around 350 K, breakage of one CN bond occurs accompanied by further dehydrogenation of the carbon skeleton. The decomposition intermediates reside on the surface up to 500 K. At higher temperatures, further decay to small fragments and atomic species is observed. These species block most of the absorption sites on the Pd particles, but can be oxidatively removed by heating in oxygen at 600 K, fully restoring the original adsorption properties of the model catalyst.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	41
Volume Number	17
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2011-10-04
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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