Journal
ACS CATALYSIS
Volume 10, Issue 12, Pages 6726-6734Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c00684
Keywords
plasma catalysis; nonthermal plasma; ammonia synthesis; thermodynamic equilibrium; kinetic modeling
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Funding
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Sustainable Ammonia Synthesis Program [DE-SC-0016543]
- U.S. Air Force Office of Scientific Research [FA9550-18-1-0157]
- Eilers Graduate Fellowship for Energy Related Research from the University of Notre Dame
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We explore the consequences of nonthermal plasma-activation on product yields in catalytic ammonia synthesis, a reaction that is equilibrium-limited at elevated temperatures. We employ a minimal microkinetic model that incorporates the influence of plasma-activation on N-2 dissociation rates to predict NH3 yields into and across the equilibrium-limited regime. NH3 yields are predicted to exceed bulk thermodynamic equilibrium limits on materials that are thermal-rate-limited by N-2 dissociation. In all cases, yields revert to bulk equilibrium at temperatures at which thermal reaction rates exceed plasma-activated ones. Beyond-equilibrium NH3 yields are observed in a packed bed dielectric barrier discharge reactor and exhibit sensitivity to catalytic material choice in a way consistent with model predictions. The approach and results highlight the opportunity to exploit synergies between nonthermal plasmas and catalysts to affect transformations at conditions inaccessible through thermal routes.
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