Effects of Supported Catalyst on the Plasma in a Packed-Bed Dielectric Barrier Discharge Reactor for Ammonia Synthesis

Francisco A. Herrera, Patrick M. Barboun, Prateek Mehta, W. Schneider, J. Hicks, D. Go
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Abstract

Ammonia, a precursor for fertilizers, is crucial to feed the world's population but also it has the potential to be used as an alternative fuel or as a chemical store for renewable energy technologies. The most common process of ammonia production is the Haber-Bosh (H-B) process, a well-optimized method that requires high temperature (~ 700 K) and pressure (~ 1 00 atm) to operate under equilibrium conditions (using thermal catalysis). Alternatively, ammonia can be produced less efficiently close to standard conditions by combining non-thermal plasmas and catalysts (plasma catalysis). Unlike thermal catalysis, in plasma catalysis the non-equilibrium state of the plasma $(T_{electrons}\gg T_{ions},T_{neutrals}$ produces reactive species, such as excited species, that may play an important role in the production of ammonia. The interaction between the plasma and the catalyst can be characterized in two categories: the effect of the plasma on catalysis and the effect of the catalyst on the plasma state. This work focuses on the latter. We use a laboratory-scale, packed bed, dielectric barrier discharge (DBD) reactor to investigate the effects of different supported metal catalysts on the plasma. Optical emission spectroscopy (OES) and electrical measurements are used to estimate various system parameters, including rotational and vibrational temperatures and electron densities, for various supported catalyst configurations (e.g., alumina supported nickel). These parameters are correlated with measurements of ammonia synthesis under identical conditions to assess whether there are significant differences in the plasma under conditions where ammonia synthesis is enhanced.
负载型催化剂对填充床介质阻挡放电合成氨反应器中等离子体的影响
氨是化肥的前体,对养活世界人口至关重要,但它也有可能被用作替代燃料或可再生能源技术的化学储存。最常见的氨生产工艺是Haber-Bosh (H-B)工艺,这是一种经过优化的方法,需要高温(~ 700 K)和压力(~ 100 atm)在平衡条件下操作(使用热催化)。另外,通过结合非热等离子体和催化剂(等离子体催化),可以在接近标准条件的情况下产生效率较低的氨。与热催化不同的是,在等离子体催化中,非平衡态的等离子体T_(电子)+ T_(离子)、T_(中性)会产生活性物质,如激发态物质,这些物质可能在氨的生成中起重要作用。等离子体与催化剂之间的相互作用可以分为两类:等离子体对催化的影响和催化剂对等离子体状态的影响。本文的研究重点是后者。利用实验室规模的填充床介质阻挡放电反应器,研究了不同负载金属催化剂对等离子体的影响。光学发射光谱(OES)和电学测量用于估计各种系统参数,包括旋转和振动温度和电子密度,用于各种负载催化剂配置(例如,氧化铝负载镍)。这些参数与相同条件下氨合成的测量结果相关联,以评估在氨合成增强的条件下血浆中是否存在显着差异。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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