期刊
JOURNAL OF PHYSICS D-APPLIED PHYSICS
卷 50, 期 15, 页码 -出版社
IOP PUBLISHING LTD
DOI: 10.1088/1361-6463/aa6229
关键词
kinetic modelling; ammonia production; nitrogen-hydrogen discharge; surface reaction; non-equilibrium atmospheric-pressure plasma; plasma catalysis
Detailed plasma kinetics modelling is presented of a low electron energy N-2-H-2 atmospheric-pressure discharge for ammonia synthesis. The model considers both electron and vibrational kinetics, including excited N-2(X,V) and H-2( X,V) species, and surface reactions such as those occurring by the Eley-Rideal and Langmuir-Hinshelwood mechanisms and dissociative adsorption of molecules. The predictions of the model are compared to the measured NH3 concentration produced in a packed-bed dielectric barrier discharge reactor as a function of process parameters such as input gas composition and applied voltage. Unlike typical low-pressure plasma processes, under the plasma conditions considered here (reduced electric field E/N in the range 30-50 Td, electron density of the order 10(8) cm(-3)), the influence of ions is not significant. Instead, the reactions between radicals and vibrationally-excited molecules are more important. The active species in surface reactions, such as surface-adsorbed atomic nitrogen N(s) or hydrogen H(s), are found to be predominantly generated through the dissociative adsorption of molecules, in contrast to previously proposed mechanisms for plasma catalysis under low-pressure, high-E/N conditions. It is found that NH radicals play an important role at the early stages of the NH3-generation process, NH in turn is produced from N and H-2(V). Electron kinetics is shown to play a critical role in the molecular dissociation and vibrational excitation reactions that produce these precursors. It is further found that surface-adsorbed atomic hydrogen H(s) takes a leading role in the formation of NH3, which is another significant difference from the mechanisms in conventional thermo-chemical processes and low-pressure plasmas. The applied voltage, the gas temperature, the N-2: H-2 ratio in the input gas mixture and the reactivity of the surface material are all found to influence the ammonia production. The calculated results reproduce the observed trends in the dependence of NH3 production on the N-2/H-2 ratio in the input gas mixture and the applied voltage.
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