Nitrogen Fixation in a Plasma/Liquid Interfacial Reaction and Its Switching between Reduction and Oxidation,The Journal of Physical Chemistry C

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Nitrogen Fixation in a Plasma/Liquid Interfacial Reaction and Its Switching between Reduction and Oxidation
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-04-14 , DOI: 10.1021/acs.jpcc.0c02392
Tatsuya Sakakura ₁ , Naoya Murakami ₂ , Yoshiyuki Takatsuji ₁ , Tetsuya Haruyama ₁

Affiliation

There are multiple active species at the interface between the discharged gas phase and the water phase. Activated nitrogen species are generated in the nitrogen plasma gas by dielectric barrier discharge (DBD). The reaction at the interface between the gas phase containing the activated nitrogen species and water phase (P/L reaction) can produce nitrogen-derived compounds (N-compounds) in water. We have already clarified the mechanism of the P/L reaction focusing on highly active atomic nitrogen in a previous study. In this study, we report the mechanism of the P/L reaction by excited but metastable nitrogen molecules. Involving excited nitrogen molecules [N₂(A³Σ_u⁺)] with a long lifetime, the reaction selectivity of N-compounds was clarified by quantitative analysis. Moreover, the active species in the water phase (H·, HO·, H₂O₂) of the P/L reaction were measured, and the involvement of the reaction in the generation of N-compounds was confirmed. The findings clarify that each activated nitrogen species reacts differently with H₂O. These results suggest that the occurrence of either an oxidation reaction or a reduction reaction can be regulated by controlling the activated nitrogen species.

中文翻译：

等离子体/液体界面反应中的固氮及其在还原和氧化之间的转换

在排出的气相和水相之间的界面处有多种活性物质。通过介电势垒放电（DBD）在氮等离子体气体中生成活化的氮物质。在包含活化氮物质的气相和水相之间的界面处的反应（P / L反应）可在水中产生源自氮的化合物（N化合物）。在先前的研究中，我们已经阐明了针对高活性原子氮的P / L反应机理。在这项研究中，我们报告了受激发但亚稳态氮分子发生的P / L反应机理。涉及激发氮分子[N ₂（A ³ Σ _ù⁺）]寿命长，通过定量分析可以明确N化合物的反应选择性。另外，测定了P / L反应的水相（H·，HO·，H ₂ O ₂）中的活性种，确认了反应参与了N化合物的生成。这些发现表明每种活化的氮物质与H ₂ O反应不同。这些结果表明，可以通过控制活化的氮物质来调节氧化反应或还原反应的发生。

更新日期：2020-04-24

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