Catalytic reduction of NO2 with hydrogen on Pt field emitter tips: kinetic instabilities on the nanoscale.
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.
McEwen
J-S
JS
Centre for Nonlinear Phenomena and Complex Systems, Campus Plaine-CP 231, Université Libre de Bruxelles, B-1050 Brussels, Belgium.
Gaspard
P
P
De Decker
Y
Y
Barroo
C
C
Visart de Bocarmé
T
T
Kruse
N
N
D000327:Adsorption; D002384:Catalysis; D006859:Hydrogen / Q000737:chemistry*; D007700:Kinetics; D053768:Metal Nanoparticles / Q000737:chemistry*; D008854:Microscopy, Electron; D009585:Nitrogen Dioxide / Q000737:chemistry*; D010084:Oxidation-Reduction; D010316:Particle Size; D010984:Platinum / Q000737:chemistry*; D013499:Surface Properties
D010984:Platinum; D006859:Hydrogen; D009585:Nitrogen Dioxide