Ammonia Decomposition By Microwave Plasma Discharges
Authors: Awaji Majed , Pentecoste Lucile , Gries Thomas , Noël Cédric , Belmahi Mohammed , Belmonte Thierry 
Published: August 2024

The global discourse focuses on future energy vectors, with hydrogen emerging as a robust candidate owing to its established industrial applications. However, a current challenge lies in storing and transporting hydrogen-based fuels. This research focuses on advancing efficient and environmentally friendly techniques for large-scale hydrogen production, leveraging its widespread industrial presence. Ammonia, identified as a promising energy vector, offers advantages in storage and transport over hydrogen. It capitalizes on existing global infrastructures, with approximately 20 million metric tons traded annually, contributing to a total production of 150 million tons annually. If many works focus on producing ammonia by electrical discharges [1], only a few are devoted to ammonia cracking and generally concentrate on catalysis [2].
In this study, we propose an investigation into the decomposition of ammonia by applying microwave (MW) plasma. Utilizing a MW cavity that confines an electromagnetic field excited at 2.45 GHz, we induce electrodeless plasma within a fused silica tube where pure ammonia (NH3) gas flow. At first, the plasma discharge was characterized with Fourier Transform Infrared Spectroscopy (FTIR). This preliminary part of the study exhibited that, for fixed input power (300 W) and fixed working pressure (100 mbar), NH3 decomposition decreased with a flow rate ranging from 0.4 to 2.4 SLM. It also showed that for fixed input power (300 W) and fixed flow rate (2.4 SLM), the NH3 dissociation increased with pressure ranging from 40 to 140 mbar. These experiments exhibited the predominant role of the residence time of ammonia but also reactive species in plasma.
To further understand the NH3 cracking mechanisms, we performed optical emission spectroscopy (OES). This technique allowed us to determine the various light-emitting species produced during NH3 dissociation in the discharge and their physical parameters, such as temperatures and relative densities, as a function of different experimental parameters. We study the influence of gas flow rate ranging from 1 to 15 SLM, input power and near-atmospheric pressure on NH3 cracking and hydrogen (H2) recombination mechanisms. Gas chromatography (GC) was employed to measure the dissociation yield of NH3 and assess the efficiency of the H2 production process.
In parallel, we synthesize iron (Fe) and nickel (Ni) nanoparticles through a plasma solution process. Both metals are abundant and inexpensive; hence, they are good candidates as catalysts for potential industrial applications. In the experimental setup, a pair of tungsten electrodes, connected by a high-voltage cathode, was submerged in an aqueous solution containing Fe and Ni chlorides. One electrode was the high-voltage cathode, while the other was the grounded anode. Pulsed discharges were generated to produce Fe and Ni compounds. The resulting Fe-Ni nanoparticles (NPs) were characterized by transmission electron microscopy (TEM) to determine their shape, size and composition, which depends on the concentrations of the metal chlorides in the electrolyte solution. Those NPs were then coated on silica tubes inserted in the MW reactor at various positions to establish their influence on the NH3 decomposition and H2 recombination processes. The primary goal of this study is to compare the dissociation of NH3 with and without catalysts, aiming to achieve optimal results for H2 production.
This study investigates the impact of experimental parameters on ammonia cracking efficiency within a microwave plasma combined with catalysis. We compare these factors with ruthenium-catalyzed and non-catalyzed thermal processes, recognized as leading methods for ammonia cracking. The goal is to gain insights into the mechanisms of ammonia decomposition in microwave plasmas and evaluate the efficiency of our proposed methodology relative to established thermal processes, contributing to the advancement of sustainable and optimized ammonia cracking practices and decarbonated hydrogen production.

Acknowledgements

The authors would like to thank the Department of Physics, College of Science, Jazan University, Jazan 45142, Saudi Arabia, for the financial support to M. Awaji and SAKOWIN for the financial support to L. Pentecoste.

References

[1] D. Zhou, R. Zhou, R. Zhou, et al., Chem. Eng. J., 421 (2021)
[2] I. Lucentini, X. Garcia, X. Vendrell, J. Llorca, Ind. Eng. Chem. Res., 60 (2021)