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Zero-dimensional kinetic modeling of atmospheric pressure Ar-N2-H2 nonthermalplasma was carried out to gain mechanistic insights into ammonia formationduring plasma-assisted catalysis of ammonia synthesis. The kinetic model wasdeveloped for a coaxial dielectric barrier discharge (DBD) quartz wool-packedbed reactor operating at near room temperature using a kHz-frequency plasmasource. With 30% Ar mixed in a 1:1 N2-H2 plasma at 760 Torr, we find that NH3production is dominated by Eley-Rideal (E-R) surface reactions, which heavilyinvolve surface NHx species derived from N and H radicals in the gas phase,while the influence of excited N2 molecules is negligible. This is contrary tothe commonly proposed mechanism that excited N2 molecules created by Penningexcitation of N2 by Ar (4s) and Ar(4p) plays a significant role in assistingNH3 formation. Our model shows that the enhanced NH3 formation upon Ar dilutionis unlikely due to the interactions between Ar and H species, as excited Aratoms have a weak effect on H radical formation through H2 dissociationcompared to electrons. We find that excited Ar atoms contribute to 28% of the Nradical production in the gas phase via N2 dissociation, while the rest isdominated by electron-impact dissociation. Furthermore, Ar species play anegligible role in the product NH3 dissociation. N2 conversion sensitivityanalyses were carried out for electron density (ne) and reduced electric field(E/N), and contributions from Ar to gas-phase N radical production werequantified. The model can provide guidance on potential reasons for observingenhanced NH3 formation upon Ar dilution in N2-H2 plasmas beyond changes to thedischarge characteristics.

Kinetic Modeling Analysis of Ar Addition to Atmospheric Pressure N2-H2 Plasma for Plasma-Assisted Catalytic Synthesis of NH3