Kinetic Study for Plasma Assisted Cracking of NH₃: Approaches and Challenges

Abstract

Ammonia is considered as one of the promising hydrogen carriers toward a sustainable world. Plasma assisted decomposition of NH₃ could provide cost- and energy-effective, low-temperature, on-demand (partial) cracking of NH₃ into H₂. Here, we presented a temperature-dependent plasma-chemical kinetic study to investigate the role of both electron-induced reactions and thermally induced reactions on the decomposition of NH₃. We employed a plasma-chemical kinetic model (KAUSTKin), developed a plasma-chemical reaction mechanism for the numerical analysis, and introduced a temperature-controlled dielectric barrier discharge reactor for the experimental investigation using 1 mol % NH₃ diluted in N₂. As a result, we observed the plasma significantly lowered the cracking temperature and found that the plasma-chemical mechanism should be further improved to better predict the experiment. The commonly used rates for the key NH₃ pyrolysis reaction (NH₃ + M ↔ NH₂ + H + M) significantly overpredicted the recombination rate at temperatures below 600 K. Furthermore, the other identified shortcomings in the available data are (i) thermal hydrazine chemistry, (ii) electron-scattering cross-section data of N_<i>x</i>H_<i>y</i>, (iii) electron-impact dissociation of N₂, and (iv) dissociative quenching of excited states of N₂. We believe that the present study will spark fundamental interest to address these shortcomings and contribute to technical advancements in plasma assisted NH₃ cracking technology.