Ammonia decomposition in a dielectric barrier discharge plasma: Insights from experiments and kinetic modeling. (5th May 2023)

• Record Type: Journal Article
• Authors: Andersen, J.A.; van 't Veer, K.; Christensen, J.M.; Østberg, M.; Bogaerts, A.; Jensen, A.D.
• Is Part Of: Chemical engineering science. Volume 271(2023)
• Publication Date: 2023-05-05
• Subjects: Ammonia Decomposition -- DBD Plasma -- Clean Hydrogen -- Chemical Kinetics Model -- Micro-Discharges; Chemical engineering -- Periodicals; Génie chimique -- Périodiques; Chemical engineering; Periodicals; Electronic journals; 660
• DOI: 10.1016/j.ces.2023.118550
• Languages: English
• ISSNs: 0009-2509

Abstract

Highlights: The plasma achieved an NH3 conversion of 82 % at a specific energy input of 18 kJ/Nl. NH3 decomposition was found to be initiated by electron dissociation collisions. Higher energy transfer through micro-discharges promoted the NH3 decomposition. Introduction of packing material resulted in a lower conversion of 37%. Re-formation of NH3 occurred through an Eley-Rideal reaction with NH2 and H(s). Abstract: Utilizing ammonia as a storage medium for hydrogen is currently receiving increased attention. A possible method to retrieve the hydrogen is by plasma-catalytic decomposition. In this work, we combined an experimental study, using a dielectric barrier discharge plasma reactor, with a plasma kinetic model, to get insights into the decomposition mechanism. The experimental results revealed a similar effect on the ammonia conversion when changing the flow rate and power, where increasing the specific energy input (higher power or lower flow rate) gave an increased conversion. A conversion as high as 82 % was achieved at a specific energy input of 18 kJ/Nl. Furthermore, when changing the discharge volume from 31 to 10 cm 3, a change in the plasma distribution factor from 0.2 to 0.1 was needed in the model to best describe the conversions of the experiments. This means that a smaller plasma volume caused a higher transfer of energy through micro-discharges (non-uniform plasma), which was found to promote the decomposition of ammonia. These results indicate that it is the collisions between NH3 and the high-energy electrons that initiate the decomposition. Moreover, the rate of ammonia destruction was found by the model to be in the order of 10 22 molecules/(cm 3 s) during the micro-discharges, which is 5 to 6 orders of magnitude higher than in the afterglows. A considerable re-formation of ammonia was found to take place in the afterglows, limiting the overall conversion. In addition, the model revealed that implementation of packing material in the plasma introduced high concentrations of surface-bound hydrogen atoms, which introduced an additional ammonia re-formation pathway through an Eley-Rideal reaction with gas phase NH2 . Furthermore, a more uniform plasma is predicted in the presence of MgAl2 O4, which leads to a lower average electron energy during micro-discharges and a lower conversion (37 %) at a comparable residence time for the plasma alone (51 %).