Plasma-assisted ammonia synthesis in a packed-bed dielectric barrier discharge reactor: roles of dielectric constant and thermal conductivity of packing materials

Abstract

Abstract In this article, plasma-assisted NH3 synthesis directly from N2 and H2 over packing materials with different dielectric constants (BaTiO3, TiO2 and SiO2) and thermal conductivities (BeO, AlN and Al2O3) at room temperature and atmospheric pressure is reported. The higher dielectric constant and thermal conductivity of packing material are found to be the key parameters in enhancing the NH3 synthesis performance. The NH3 concentration of 1344 ppm is achieved in the presence of BaTiO3, which is 106% higher than that of SiO2, at the specific input energy (SIE) of 5.4 kJ·l−1. The presence of materials with higher dielectric constant, i.e. BaTiO3 and TiO2 in this work, would contribute to the increase of electron energy and energy injected to plasma, which is conductive to the generation of chemically active species by electron-impact reactions. Therefore, the employment of packing materials with higher dielectric constant has proved to be beneficial for NH3 synthesis. Compared to that of Al2O3, the presence of BeO and AlN yields 31.0% and 16.9% improvement in NH3 concentration, respectively, at the SIE of 5.4 kJ·l−1. The results of IR imaging show that the addition of BeO decreases the surface temperature of the packed region by 20.5% to 70.3°C and results in an extension of entropy increment compared to that of Al2O3, at the SIE of 5.4 kJ·l−1. The results indicate that the presence of materials with higher thermal conductivity is beneficial for NH3 synthesis, which has been confirmed by the lower surface temperature and higher entropy increment of the packed region. In addition, when SIE is higher than the optimal value, further increasing SIE would lead to the decrease of energy efficiency, which would be related to the exacerbation in reverse reaction of NH3 formation reactions.