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

Journal article
(Original article)


Publication Details

Author(s): Vines F, Lykhach Y, Staudt T, Lorenz MPA, Papp C, Steinrück HP, Libuda J, Neyman K, Görling A
Journal: Chemistry - A European Journal
Publisher: Wiley-VCH Verlag
Publication year: 2010
Volume: 16
Journal issue: 22
Pages range: 6530-6539
ISSN: 0947-6539


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.



FAU Authors / FAU Editors

Görling, Andreas Prof. Dr.
Lehrstuhl für Theoretische Chemie
Libuda, Jörg Prof. Dr.
Professur für Physikalische Chemie
Lykhach, Yaroslava
Lehrstuhl für Physikalische Chemie II
Papp, Christian PD Dr.
Lehrstuhl für Physikalische Chemie II
Steinrück, Hans-Peter Prof. Dr.
Lehrstuhl für Physikalische Chemie II


Additional Organisation
Exzellenz-Cluster Engineering of Advanced Materials


External institutions with authors

Institució Catalana de Recerca i Estudis Avançats (ICREA) / Catalan Institution for Research and Advanced Studies


Research Fields

D Catalytic Materials
Exzellenz-Cluster Engineering of Advanced Materials
A3 Multiscale Modeling and Simulation
Exzellenz-Cluster Engineering of Advanced Materials


How to cite

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.

BibTeX: 

Last updated on 2019-21-07 at 08:01