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Langmuir ; 26(21): 16381-91, 2010 Nov 02.
Article in English | MEDLINE | ID: mdl-20690654

ABSTRACT

The catalytic reduction of NO(2) with hydrogen on a Pt field emitter tip is investigated using both field electron microscopy (FEM) and field ion microscopy (FIM). A rich variety of nonlinear behavior and unusually high catalytic activity around the {012} facets are observed. Our FEM investigations reveal that the correlation function exhibits damped oscillations with a decaying envelope, showing that molecular noise will influence the dynamics of the oscillations. The dependence of the oscillatory period on the P(H(2))/P(NO(2)) pressure ratios is analyzed. Similar patterns are reported under FIM conditions. Corresponding density functional theory (DFT) calculations for the adsorption of NO(2) on Pt{012} in the presence of an external electric field are performed in order to gain an atomistic understanding of the underlying nonlinear phenomena.


Subject(s)
Hydrogen/chemistry , Metal Nanoparticles/chemistry , Nitrogen Dioxide/chemistry , Platinum/chemistry , Adsorption , Catalysis , Kinetics , Microscopy, Electron , Oxidation-Reduction , Particle Size , Surface Properties
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