Size and structure effects controlling the stability of the liquid organic hydrogen carrier dodecahydro- N -ethylcarbazole during dehydrogenation over pt model catalysts

Amende M, Gleichweit C, Schernich S, Höfert O, Lorenz MPA, Zhao W, Koch M, Obesser K, Papp C, Wasserscheid P, Steinrück HP, Libuda J (2014)


Publication Type: Journal article, Original article

Publication year: 2014

Journal

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

Publisher: American Chemical Society

Book Volume: 5

Pages Range: 1498-1504

Journal Issue: 8

DOI: 10.1021/jz500157r

Abstract

Hydrogen can be stored conveniently using so-called liquid organic hydrogen carriers (LOHCs), for example, N-ethylcarbazole (NEC), which can be reversibly hydrogenated to dodecahydro-N-ethylcarbazole (H-NEC). In this study, we focus on the dealkylation of H-NEC, an undesired side reaction, which competes with dehydrogenation. The structural sensivity of dealkylation was studied by high-resolution X-ray photoelectron spectroscopy (HR-XPS) on AlO-supported Pt model catalysts and Pt(111) single crystals. We show that the morphology of the Pt deposit strongly influences LOHC degradation via C-N bond breakage. On smaller, defect-rich Pt particles, the onset of dealkylation is shifted by 90 K to lower temperatures as compared to large, well-shaped particles and well-ordered Pt(111). We attribute these effects to a reduced activation barrier for C-N bond breakage at low-coordinated Pt sites, which are abundant on small Pt aggregates but are rare on large particles and single crystal surfaces. © 2014 American Chemical Society.

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APA:

Amende, M., Gleichweit, C., Schernich, S., Höfert, O., Lorenz, M.P.A., Zhao, W.,... Libuda, J. (2014). Size and structure effects controlling the stability of the liquid organic hydrogen carrier dodecahydro- N -ethylcarbazole during dehydrogenation over pt model catalysts. Journal of Physical Chemistry Letters, 5(8), 1498-1504. https://dx.doi.org/10.1021/jz500157r

MLA:

Amende, Maximilian, et al. "Size and structure effects controlling the stability of the liquid organic hydrogen carrier dodecahydro- N -ethylcarbazole during dehydrogenation over pt model catalysts." Journal of Physical Chemistry Letters 5.8 (2014): 1498-1504.

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