Issue 47, 2010
From the journal:

Physical Chemistry Chemical Physics

Dynamic response of chlorine atoms on a RuO2(110) model catalyst surface

Jan Philipp Hofmann,a   Stefan Zweidinger,a   Ari Paavo Seitsonen,bc   Attila Farkas,a   Marcus Knapp,a   Olivier Balmes,d   Edvin Lundgren,e   Jesper N. Andersene  and  Herbert Over*a  

* Corresponding authors

a Physikalisch-Chemisches Institut, Justus-Liebig-Universität Giessen, Heinrich-Buff-Ring 58, D-35392 Giessen, Germany
E-mail: Herbert.Over@phys.chemie.uni-giessen.de
Web: http://www.uni-giessen.de/cms/physchem/over
Fax: ++49-641-9934559

b IMPMC, CNRS & Université Pierre et Marie Curie, 4 place Jussieu, case 115, F-75252 Paris, France

c Physikalisch-Chemisches Institut der Universität Zürich, Winterthurerstrasse 190, CH-8057 Zürich, Switzerland

d Beamline ID03, European Synchrotron Radiation Facility (ESRF), BP 220, F-38043 Grenoble Cedex 9, France

e Department of Synchrotron Radiation Research, Lund University, Sölvegatan 14, S-22362 Lund, Sweden

Abstract

The dynamic behavior of surface accommodated chlorine atoms on RuO2(110) was studied by a variety of experimental methods including high resolution core level shift, thermal desorption-, and in situ infrared spectroscopy as well as in situ surface X-ray diffraction in combination with state-of-the-art density functional theory calculations. On the chlorinated RuO2(110) surface the undercoordinated oxygen atoms have been selectively replaced by chlorine. These strongly bound surface chlorine atoms shift from bridging to on-top sites when the sample is annealed in oxygen, while the reverse shift of Cl from on-top into bridge positions is observed during CO exposure; the vacant bridge position is then occupied by either chlorine or CO. For the CO oxidation reaction over chlorinated RuO2(110), the reactant induced site switching of chlorine causes a site-blocking of the catalytically active one-fold coordinatively unsaturated (1f-cus) Ru sites. This site blocking reduces the number of active sites and, even more important, on-top Cl blocks the free migration of the adsorbed reactants along the one-dimensional 1f-cus Ru rows, thus leading to a loss of catalytic activity.

Graphical abstract: Dynamic response of chlorine atoms on a RuO2(110) model catalyst surface

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Article information

DOI
https://doi.org/10.1039/C0CP01126F
Article type
Paper
Submitted
08 Jul 2010
Accepted
30 Sep 2010
First published
22 Oct 2010

Phys. Chem. Chem. Phys., 2010,12, 15358-15366

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Dynamic response of chlorine atoms on a RuO2(110) model catalyst surface

J. P. Hofmann, S. Zweidinger, A. P. Seitsonen, A. Farkas, M. Knapp, O. Balmes, E. Lundgren, J. N. Andersen and H. Over, Phys. Chem. Chem. Phys., 2010, 12, 15358 DOI: 10.1039/C0CP01126F

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