ChemRxiv
These are preliminary reports that have not been peer-reviewed. They should not be regarded as conclusive, guide clinical practice/health-related behavior, or be reported in news media as established information. For more information, please see our FAQs.
1/1
2 files
0/0

Plasma-Catalytic Ammonia Synthesis Beyond the Equilibrium Limit

preprint
submitted on 30.01.2020 and posted on 31.01.2020 by Prateek Mehta, Patrick M. Barboun, Yannick Engelmann, David B. Go, Annemie Bogaerts, William F. Schneider, Jason C. Hicks
We explore the consequences of non-thermal 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 N2 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 N2 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 non-thermal plasmas and catalysts to affect transformations at conditions inaccessible through thermal routes.

Funding

FA9550-18-1-0157

DE-SC-0016543

History

Email Address of Submitting Author

pmehta1@alumni.nd.edu

Institution

University of Notre Dame

Country

USA

ORCID For Submitting Author

0000-0001-6233-8072

Declaration of Conflict of Interest

No conflict of interest

Exports

Logo branding

Exports