Catalytic Reduction of NO2 with Hydrogen on Pt Field Emitter Tips: Kinetic Instabilities on the Nanoscale

JS McEwen, P Gaspard, Y De Decker, C Barroo… - Langmuir, 2010 - ACS Publications
Langmuir, 2010ACS Publications
The catalytic reduction of NO2 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 H2/P NO2 …
The catalytic reduction of NO2 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 PH2/PNO2 pressure ratios is analyzed. Similar patterns are reported under FIM conditions. Corresponding density functional theory (DFT) calculations for the adsorption of NO2 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.
ACS Publications
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