Nitrogen Fixation by Benzene into Pyridine and Aniline in Water/Nitrogen Plasma,Journal of the American Society for Mass Spectrometry

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Nitrogen Fixation by Benzene into Pyridine and Aniline in Water/Nitrogen Plasma
Journal of the American Society for Mass Spectrometry ( IF 3.1 ) Pub Date : 2023-08-25 , DOI: 10.1021/jasms.3c00236
Dongbo Mi ₁ , Yunpeng Zhang ₁ , Yongpeng Yu ₁ , Pengkun Qi ₁ , Xiaofeng Dong ₁ , Yan-Chun Li ₂

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We demonstrated direct conversion of benzene into pyridine and aniline, assisted through exact mass measurements (m/z 80.0494, 93.0574, and 94.0651, respectively), through the interaction of benzene with water/nitrogen vapor plasma produced by corona discharge. Systematic analysis using a series of isotopic standards indicated that formation of pyridine and aniline occurred through the reaction between neutral benzene and reactive N⁺(OH₂)₂ in water/nitrogen plasma; exact mass measurements of products and intermediates supported this hypothesis. As the proportion of water vapor in plasma increased over time, the reaction proceeded from exclusive formation of protonated pyridine to formation of protonated aniline as the main product; theoretical simulations indicated that the presence of water vapor promoted proton migration to elicit formation of protonated aniline. The reactions we discovered suggest a new mechanism for direct nitrogen fixation.

中文翻译：

苯在水/氮等离子体中固氮成吡啶和苯胺

我们通过苯与电晕放电产生的水/氮蒸气等离子体的相互作用，通过精确的质量测量（m / z分别为 80.0494、93.0574 和 94.0651），演示了苯直接转化为吡啶和苯胺。使用一系列同位素标准品进行系统分析表明，中性苯与水/氮等离子体中的反应性N ⁺ (OH ₂ ) ₂反应生成吡啶和苯胺。产品和中间体的精确质量测量支持了这一假设。随着等离子体中水蒸气的比例随着时间的推移而增加，反应从仅形成质子化吡啶发展到形成质子化苯胺作为主要产物；理论模拟表明，水蒸气的存在促进了质子迁移，从而引发质子化苯胺的形成。我们发现的反应提出了一种直接固氮的新机制。

更新日期：2023-08-25

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