Adsorption kinetics of O2 in vibrational non–equilibrium on low–indexed Pt surfaces: Insights from reactive molecular dynamics simulations

Non–thermal plasma catalysis provides an exciting addition to classical heterogeneous or homogeneous catalysis as it possesses the potential of breaking scaling relations that often limit reaction processes. However, a preliminary understanding of how a plasma interacts with a catalytic surface and how it is capable to modify its morphology and composition is still lacking! Thus, we have developed an approach to perform reactive molecular dynamics simulations of vibrationally excited plasma species and to describe corresponding plasma– surface interfaces. This approach was used to study the interactions of vibrationally excited O2 molecules with Pt surfaces of different orientations, where subtile differences could be identified. While at lower temperatures O2 adsorbs as molecularly, under the same conditions vibrationally excited O2 prefers dissociative adsorption, where the degree strongly depends on excitation state (or vibrational temperature), the surface orientation as well as the surface temperature. Also, surface reconstruction with respect to monoatomic O adsorption at higher vibrational levels has been espied from the radial distribution function analyses.