在大气射频氦等离子体中通过等离子体催化合成氨

S. C. L. Vervloedt, A. von Keudell
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摘要

通过红外吸收光谱、光学发射光谱以及化学动力学建模,研究了等离子体内催化合成氨的过程。喷砂玻璃用作铁、铂和铜催化剂的载体,表面温度最高可达 150 ○C。结果表明,在 N2/(N2+H2)比值很小的情况下,氨的生产达到最佳状态,浓度随等离子体功率的增加而增加。全局动力学模型与 N2+H2 混合量和吸收等离子功率变化时的数据十分吻合。根据与模型的比较,这与催化剂的存在导致电子动力学发生变化有关。据推测,引入催化剂会增加还原电场,因为它降低了二次电子发射系数。因此,N2 的解离受到刺激,从而促进了 NH3 的形成。这些实验表明,在惰性气体稀释的射频等离子体中,催化剂对等离子体性能的影响可能比等离子体对任何催化表面过程的影响更为重要。
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Ammonia synthesis by plasma catalysis in an atmospheric RF helium plasma
The in-plasma-catalytic synthesis of ammonia from nitrogen and hydrogen admixed to a helium RF plasma is studied with infrared absorption spectroscopy, optical emission spectroscopy, and through chemical kinetics modeling. Sandblasted glass is used as support for iron, platinum, and copper catalysts up to a surface temperature of 150 ○C. It is shown that the optimum ammonia production occurs at very small N2/(N2+H2) ratios with an increase of concentration with plasma power. The global kinetic modelling agrees well with the data for a variation of the N2+H2 admixture and the absorbed plasma power. The introduction of the catalyst enhances ammonia production by up to a factor of 2. Based on the comparison with the modelling, this is linked to a change in the electron kinetics due to the presence of the catalyst. It is postulated that introducing the catalyst increases the reduced electric field, because it reduces the secondary electron emission coefficient. As a result, the dissociation of N2 is stimulated, thereby enhancing the NH3 formation. These experiments show that the impact of the catalyst on the plasma performance in noble gas-diluted RF plasmas can be more important than the impact of the plasma on any catalytic surface process.
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