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

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 (2014)


Publication Type: Journal article, Original article

Publication year: 2014

Journal

Original Authors: Amende M., Gleichweit C., Werner K., Schernich S., Zhao W., Lorenz M.P.A., Höfert O., Papp C., Koch M., Wasserscheid P., Laurin M., Steinrück H.-P., Libuda J.

Publisher: American Chemical Society

Book Volume: 4

Pages Range: 657-665

Journal Issue: 2

DOI: 10.1021/cs400946x

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.

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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.

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