Methane activation by platinum: Critical role of edge and corner sites of metal nanoparticles

Vines F, Lykhach Y, Staudt T, Lorenz MPA, Papp C, Steinrück HP, Libuda J, Neyman K, Görling A (2010)


Publication Type: Journal article, Original article

Publication year: 2010

Journal

Original Authors: Vines F., Lykhach Y., Staudt T., Lorenz M.P.A., Papp C., Steinrück H.-P., Libuda J., Neyman K.M., Görling A.

Publisher: Wiley-VCH Verlag

Book Volume: 16

Pages Range: 6530-6539

Journal Issue: 22

DOI: 10.1002/chem.201000296

Abstract

Complete dehydrogenation of methane is studied on model Pt catalysts by means of state-of-the-art DFT methods and by a combination of supersonic molecular beams with highresolution photoelectron spectroscopy. The DFT results predict that intermediate species like CH and CH are specially stabilized at sites located at particles edges and corners by an amount of 50-80 kJ mol . This stabilization is caused by an enhanced activity of lowcoordinated sites accompanied by their special flexibility to accommodate adsorbates. The kinetics of the complete dehydrogenation of methane is substantially modified according to the reaction energy profiles when switching from Pt(111) extended surfaces to Pt nanoparticles. The CH and CH formation steps are endothermic on Pt(111) but markedly exothermic on Pt . An important decrease of the reaction barriers is observed in the latter case with values of approximately 60 kJmol for first C - H bond scission and 40 kJ mol for methyl decomposition. DFT predictions are experimentally confirmed by methane decomposition on Pt nanoparticles supported on an ordered CeO film on Cu(111). It is shown that CH generated on the Pt nanoparticles undergoes spontaneous dehydrogenation at 100 K. This is in sharp contrast to previous results on Pt single-crystal surfaces in which CH was stable up to much higher temperatures. This result underlines the critical role of particle edge sites in methane activation and dehydrogenation. © 2010 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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APA:

Vines, F., Lykhach, Y., Staudt, T., Lorenz, M.P.A., Papp, C., Steinrück, H.-P.,... Görling, A. (2010). Methane activation by platinum: Critical role of edge and corner sites of metal nanoparticles. Chemistry - A European Journal, 16(22), 6530-6539. https://dx.doi.org/10.1002/chem.201000296

MLA:

Vines, Francesc, et al. "Methane activation by platinum: Critical role of edge and corner sites of metal nanoparticles." Chemistry - A European Journal 16.22 (2010): 6530-6539.

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