Effect of Porous Catalyst Support on Plasma-Assisted Catalysis for Ammonia Synthesis br

We report on the effect of catalyst support particle porosity on the conversion of NH3 synthesis from N2 and H2 in a coaxial dielectric barrier discharge (DBD) plasma reactor. The discharge was created using an AC applied voltage with the reactor at room temperature and near atmospheric pressure (550 Torr). Two different particles of almost equal diameter (similar to 1.5 mm)-porous silica (SiO2) ceramic beads (average pore size: 8 nm) and smooth, nonporous soda lime glass beads-were compared in the DBD reactor. As the pore size in the SiO2 particles was smaller than the Debye length, penetration of the plasma into the pores of the particles was unlikely; however, reactive species generated in the plasma outside the particles could diffuse into the pores. The N2 conversion and energy yield of NH3 increased with applied voltage for both particle types, and these values were consistently higher when using the SiO2 beads. Discharge and plasma properties were estimated from Lissajous plots and using calculations with the BOLSIG+ software. The effect of these two different catalyst supports on the physical properties of the discharge was negligible. High resolution optical emission spectra revealed that the concentrations of N2+, atomic N, and atomic H (H alpha, H beta) in the plasma discharge were lower with the porous SiO2 beads than with the glass beads at every applied voltage tested. This indicates that these active species participate in heterogeneous reactions at support particle surfaces and that the larger surface area presented by the porous particles led to higher rates of depletion of these intermediates and a higher rate of ammonia synthesis.

Automated summary

This study investigates the effect of catalyst support particle porosity on the conversion of NH3 synthesis. The results show that porous silica particles have higher conversion rate and energy yield. High-resolution optical emission spectra indicate that the concentrations of active species in the plasma discharge are lower for the porous material, suggesting their involvement in heterogeneous reactions.