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In Situ Identification of NNH and N2H2 by Using Molecular-Beam Mass Spectrometry in Plasma-Assisted Catalysis for NH3 Synthesis
ACS Energy Letters ( IF 19.3 ) Pub Date : 2021-11-29 , DOI: 10.1021/acsenergylett.1c02207
Hao Zhao 1, 2 , Guohui Song 2, 3 , Zhe Chen 1 , Xiaofang Yang 1, 4 , Chao Yan 2 , Shota Abe 1 , Yiguang Ju 2 , Sankaran Sundaresan 1 , Bruce E. Koel 1
Affiliation  

Ammonia synthesis at 533 K and atmospheric pressure was investigated in a coaxial dielectric barrier discharge (DBD) plasma reactor without packing and with porous γ-Al2O3, 5 wt % Ru/γ-Al2O3, or 5 wt % Co/γ-Al2O3 catalyst particles. Gas-phase species were monitored in situ using an electron impact molecular-beam mass spectrometer (EI-MBMS). Gas-phase species NNH and N2H2 were first identified under common conditions of plasma-assisted ammonia synthesis and were present at levels comparable to that of NH3 in the plasma discharge. Concentrations of NNH, N2H2, and NH in a reactor packed with γ-Al2O3 or other particles were lower than those observed in an empty reactor, while the concentration of NH3 increased. These observations point to the importance of NNH and N2H2 in plasma-assisted surface reactions in ammonia synthesis. Reaction pathways of direct adsorption of gas-phase NNH and N2H2 on solid surfaces and subsequent reactions were proposed. This study demonstrated that in situ identification of gas-phase species via EI-MBMS provides a powerful approach to study the kinetics of plasma-assisted catalysis.

中文翻译:

在等离子辅助催化合成 NH3 中使用分子束质谱法原位鉴定 NNH 和 N2H2

在无填料和多孔 γ-Al 2 O 3、5 wt% Ru/γ-Al 2 O 3或 5 wt% Co的同轴介质阻挡放电 (DBD) 等离子体反应器中研究了 533 K 和大气压下的氨合成/γ-Al 2 O 3催化剂颗粒。使用电子碰撞分子束质谱仪 (EI-MBMS)原位监测气相物质。气相物质 NNH 和 N 2 H 2首次在等离子体辅助氨合成的常见条件下被发现,并且在等离子体放电中的含量与 NH 3相当。NNH、N 2 H的浓度如图2所示,填充有γ-Al 2 O 3或其他颗粒的反应器中的NH低于在空反应器中观察到的,而NH 3的浓度增加。这些观察表明 NNH 和 N 2 H 2在氨合成中的等离子体辅助表面反应中的重要性。提出了气相NNH和N 2 H 2在固体表面直接吸附的反应途径及后续反应。该研究表明,通过EI-MBMS原位鉴定气相物质为研究等离子体辅助催化的动力学提供了一种强有力的方法。
更新日期:2022-01-14
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