(145e) Models and Observations of Plasma-Catalytic Nitrogen Oxidation

Coupled plasma and catalyst enables reaction yields that exceed the contributions of the individual components. Reliable kinetic models are essential to rationalize observations and to guide the identification of appropriate plasma-catalyst combinations. Kinetic models of plasma- and of heterogeneous-catalytic-chemistries are individually well developed. Models to couple the two are still primitive. Here, we demonstrate DFT-parametrized microkinetic models to couple plasma and surface reactions. The models are applied to N₂ oxidation, an alternative nitrogen fixation process, enabled only with coupled non-thermal plasma and catalysts. We compare the intrinsic activity of Pt and Au under plasma conditions. We build integral reactor models coupling simplified plasma reaction and surface reaction networks to predict product yield. We first show plasma excited species can enhance turnover frequencies of both Pt and Au. The enhancing potential of catalysts to chemical yield from plasma, however, are condition- and material- dependent. Plasma/Pt generates more or comparable nitric oxide than plasma/Au under most thermal and plasma parametric conditions. Plasma/Au outperforms plasma/Pt under low thermal but high plasma excitations. Results are compared against experimental observations, highlighting that material selection must consider plasma properties, thermal conditions and reactor configurations.