Model catalytic studies of liquid organic hydrogen carriers: Dehydrogenation and decomposition mechanisms of dodecahydro-n-ethylcarbazole on pt(111)

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Details zur Publikation

Autor(en): Amende M, Gleichweit C, Werner K, Schernich S, Zhao W, Lorenz MPA, Höfert O, Papp C, Koch M, Wasserscheid P, Laurin M, Steinrück HP, Libuda J
Zeitschrift: ACS Catalysis
Verlag: American Chemical Society
Jahr der Veröffentlichung: 2014
Band: 4
Heftnummer: 2
Seitenbereich: 657-665
ISSN: 2155-5435


Abstract


Liquid organic hydrogen carriers (LOHC) are compounds that enable chemical energy storage through reversible hydrogenation. They are considered a promising technology to decouple energy production and consumption by combining high-energy densities with easy handling. A prominent LOHC is N-ethylcarbazole (NEC), which is reversibly hydrogenated to dodecahydro-N-ethylcarbazole (H -NEC). We studied the reaction of H-NEC on Pt(111) under ultrahigh vacuum (UHV) conditions by applying infrared reflection-absorption spectroscopy, synchrotron radiation-based high resolution X-ray photoelectron spectroscopy, and temperature-programmed molecular beam methods. We show that molecular adsorption of H-NEC on Pt(111) occurs at temperatures between 173 and 223 K, followed by initial C-H bond activation in direct proximity to the N atom. As the first stable dehydrogenation product, we identify octahydro-N-ethylcarbazole (H -NEC). Dehydrogenation to H-NEC occurs slowly between 223 and 273 K and much faster above 273 K. Stepwise dehydrogenation to NEC proceeds while heating to 380 K. An undesired side reaction, C-N bond scission, was observed above 390 K. H-NEC and H-carbazole are the dominant products desorbing from the surface. Desorption occurs at higher temperatures than H-NEC formation. We show that desorption and dehydrogenation activity are directly linked to the number of adsorption sites being blocked by reaction intermediates. © 2014 American Chemical Society.



FAU-Autoren / FAU-Herausgeber

Amende, Maximilian
Lehrstuhl für Physikalische Chemie II
Gleichweit, Christoph
Lehrstuhl für Physikalische Chemie II
Höfert, Oliver
Lehrstuhl für Physikalische Chemie II
Koch, Marcus
Lehrstuhl für Chemische Reaktionstechnik
Laurin, Mathias Dr.
Lehrstuhl für Physikalische Chemie II
Libuda, Jörg Prof. Dr.
Professur für Physikalische Chemie
Papp, Christian PD Dr.
Lehrstuhl für Physikalische Chemie II
Schernich, Stefan
Professur für Physikalische Chemie
Steinrück, Hans-Peter Prof. Dr.
Lehrstuhl für Physikalische Chemie II
Wasserscheid, Peter Prof. Dr.
Lehrstuhl für Chemische Reaktionstechnik
Werner, Kristin
Lehrstuhl für Physikalische Chemie II
Zhao, Wei
Lehrstuhl für Physikalische Chemie II


Zitierweisen

APA:
Amende, M., Gleichweit, C., Werner, K., Schernich, S., Zhao, W., Lorenz, M.P.A.,... Libuda, J. (2014). Model catalytic studies of liquid organic hydrogen carriers: Dehydrogenation and decomposition mechanisms of dodecahydro-n-ethylcarbazole on pt(111). ACS Catalysis, 4(2), 657-665. https://dx.doi.org/10.1021/cs400946x

MLA:
Amende, Maximilian, et al. "Model catalytic studies of liquid organic hydrogen carriers: Dehydrogenation and decomposition mechanisms of dodecahydro-n-ethylcarbazole on pt(111)." ACS Catalysis 4.2 (2014): 657-665.

BibTeX: 

Zuletzt aktualisiert 2018-09-08 um 01:56