Plasma catalysis for ammonia synthesis technology exhibits significant development potential, and improving the synergistic interaction between plasma and catalyst is a challenging research focus. However, current research focuses on efficient catalyst formulation design, but studies on catalyst support material screening and reactor performance optimization are lacking. Therefore, this study first enhanced the ammonia synthesis capability of the reactor and found that the 5 cm ground electrode and center plasma catalysis (CPC) coupling were the optimal system configurations. Support screening tests showed that higher dielectric properties and highly ordered interconnecting pores are crucial to achieving high ammonia concentration production. The SBA-15 (best material) filled system showed the highest reduced electric field (122.97 Td), with a more significant number of high-energy electrons and an average electron energy of up to 3.93 eV. Possible enhanced mechanisms for ammonia synthesis on SBA-15 include: (1) promoting the excitation dissociation process of feed gas in the gas phase and the activation process on the material surface and (2) using ordered tubular channels to suppress the occurrence of plasma-induced reverse reactions. By adjusting the flow rate, ammonia concentration as high as 11737 ppm was achieved, 4.58 times higher than the empty tube. The highest achieved synthesis rate was 5337 μmol/g_cat/h, and the energy yield was 1.04 g_NH3/kWh. Additionally, the study indicated that a nitrogen-rich environment is more beneficial for the progression of the reaction, with the optimal N₂:H₂ molar ratio being 2:1. This work highlights the necessity and significance of optimizing the reaction system, including (1) system configuration, (2) catalyst support material, and (3) operating parameter. Especially, it provides new insights into the design of catalysts in a plasma environment.

中文翻译：

---

解锁高效协同等离子体催化剂氨合成：系统优化和催化剂支持筛选


等离子体催化氨合成技术展现出巨大的发展潜力，提高等离子体与催化剂之间的协同作用是一个具有挑战性的研究热点。然而，目前的研究主要集中在高效的催化剂配方设计，而缺乏催化剂载体材料筛选和反应器性能优化的研究。因此，本研究首先增强了反应器的氨合成能力，发现5 cm接地电极和中心等离子体催化（CPC）耦合是最佳的系统配置。支持筛选测试表明，较高的介电性能和高度有序的互连孔对于实现高氨浓度生产至关重要。 SBA-15（最佳材料）填充系统表现出最高的降低电场（122.97 Td），具有更多数量的高能电子，平均电子能量高达 3.93 eV。 SBA-15上氨合成的可能增强机制包括：（1）促进气相中原料气的激发解离过程和材料表面的活化过程；（2）使用有序管状通道来抑制等离子体的发生。诱发逆反应。通过调节流量，氨浓度高达11737 ppm，是空管的4.58倍。最高合成速率为5337 μmol/g _cat /h，能量产量为1.04 g _NH3 /kWh。此外，研究表明富氮环境更有利于反应的进行，最佳的N ₂ :H ₂ 摩尔比为2:1。 这项工作凸显了优化反应系统的必要性和意义，包括（1）系统配置、（2）催化剂载体材料和（3）操作参数。特别是，它为等离子体环境中的催化剂设计提供了新的见解。