Coupled plasma and catalyst enables reaction yields that exceed the individual components. Kinetic models of plasma chemical reactions and of heterogeneous catalytic reactions are individually well developed. Models that couple both plasma and surface reactions, however, are still primitive. Models without careful parametrization of surface reactions are capable of predicting the qualitative enhancing potential of catalysts to plasma reactions, but are not predictive in comparing the performance of different catalysts. Here, we constructed plasma-appropriate microkinetic models for catalytic N<sub>2</sub> oxidation to NO with Pt and Au. We parametrized the model with DFT-computed kinetic constants. We compare the impacts of plasma-generated vibrational excitations and radicals on the activities of the two metals. We built integral reactor models that coupled a simplified plasma reaction network and surface reactions to compare the NO production in both plasma/Pt and plasma/Au systems. NO yields are comparable between Pt and Au with strong plasma excitations. Pt, however, outperforms Au in NO yields at thermal conditions and with weak plasma excitations. Results are compared against experimental observations, highlighting the potential of plasma-stimulated catalysis to drive endothermic reactions.

Models and observations of plasma-catalytic nitrogen oxidation

ACS Spring Meeting 2021

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