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Evidence for the Formation of Imidazole from Carbonyls and Reduced Nitrogen Species at the Individual Particle Level in the Ambient Atmosphere
Environmental Science & Technology Letters ( IF 10.9 ) Pub Date : 2020-10-27 , DOI: 10.1021/acs.estlett.0c00722
Xiufeng Lian 1, 2 , Guohua Zhang 1, 3 , Yuxiang Yang 1, 2 , Qinhao Lin 1 , Yuzhen Fu 1, 2 , Feng Jiang 1, 2 , Long Peng 1, 2 , Xiaodong Hu 1, 2 , Duohong Chen 4 , Xinming Wang 1, 3 , Ping’an Peng 1, 3 , Guoying Sheng 1 , Xinhui Bi 1, 3
Affiliation  

While laboratory studies have demonstrated that aqueous reactions between carbonyls and reduced nitrogen species may contribute to the production of N-heterocycle brown carbon (BrC) such as imidazole, there is currently a lack of evidence for this in the atmosphere. We investigated the mixing state of carbonyls, ammonium, amines, and imidazole (as a surrogate of BrC) in cloud residual, interstitial, and cloud-free particles by single-particle mass spectrometry. The results provide the first ambient evidence of the formation of imidazole through reactions between carbonyls and ammonium/amines at the individual particle level. The key evidence for this is that 60% of the imidazole particles are internally mixed with carbonyls and ammonium/amines. The number fraction of imidazole is significantly enhanced in particles with internally mixed carbonyls and ammonium (7.8%)/amines (26.7%), compared with that (1.4%) in all of the cloud-free particles. Furthermore, a higher number fraction of imidazole is observed in all cloud residual and interstitial particles (2.9%) than in the cloud-free particles (1.4%). This is due to the enhancement of amines and/or the synergistic effect of ammonium and amines in the formation of imidazole in cloud residual and interstitial particles. These findings extend the current understanding of the formation and evolution of imidazole-based BrC.

中文翻译:

在大气中单个粒子水平上由羰基和还原氮物种形成咪唑的证据

尽管实验室研究表明,羰基化合物和还原的氮物种之间的水反应可能有助于生成N-杂环棕碳(BrC),例如咪唑,但目前在大气中尚无证据。我们通过单颗粒质谱法研究了羰基,铵,胺和咪唑(作为BrC的替代物)在云残留,填隙性和无云颗粒中的混合状态。该结果提供了第一个环境证据,表明在单个颗粒水平上羰基与铵/胺之间的反应形成了咪唑。关键证据是60%的咪唑颗粒在内部与羰基化合物和铵/胺混合。与所有无云颗粒中的咪唑(1.4%)相比,内部混合有羰基和铵(7.8%)/胺(26.7%)的颗粒中咪唑的数量分数显着提高。此外,在所有云残留和间隙颗粒(2.9%)中观察到的咪唑分数要高于无云颗粒(1.4%)。这是由于胺的增强和/或铵和胺在云残留颗粒和间隙颗粒中形成咪唑时的协同作用所致。这些发现扩展了目前对基于咪唑的BrC的形成和演化的认识。9%)比无云颗粒(1.4%)高。这是由于胺的增强和/或铵和胺在云残留颗粒和间隙颗粒中形成咪唑时的协同作用所致。这些发现扩展了目前对基于咪唑的BrC的形成和演化的认识。9%)比无云颗粒(1.4%)高。这是由于胺的增强和/或铵和胺在云残留颗粒和间隙颗粒中形成咪唑时的协同作用所致。这些发现扩展了目前对基于咪唑的BrC的形成和演化的理解。
更新日期:2020-10-28
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