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Criegee 中间体与 NO 的反应产物:实验测量和对流层的影响。

Products of Criegee intermediate reactions with NO: experimental measurements and tropospheric implications.

机构信息

Combustion Research Facility, Sandia National Laboratories, Mailstop 9055, Livermore, California, 94551 USA.

出版信息

Faraday Discuss. 2017 Aug 24;200:313-330. doi: 10.1039/c7fd00007c.

Abstract

The reactions of Criegee intermediates with NO have been proposed as a potentially significant source of the important nighttime oxidant NO, particularly in urban environments where concentrations of ozone, alkenes and NO are high. However, previous efforts to characterize the yield of NO from these reactions have been inconclusive, with many studies failing to detect NO. In the present work, the reactions of formaldehyde oxide (CHOO) and acetaldehyde oxide (CHCHOO) with NO are revisited to further explore the product formation over a pressure range of 4-40 Torr. NO is not observed; however, temporally resolved and [NO]-dependent signal is observed at the mass of the Criegee-NO adduct for both formaldehyde- and acetaldehyde-oxide systems, and the structure of this adduct is explored through ab initio calculations. The atmospheric implications of the title reaction are investigated through global modelling.

摘要

Criegee 中间体与 NO 的反应被认为是重要的夜间氧化剂 NO 的一个潜在重要来源,特别是在臭氧、烯烃和 NO 浓度较高的城市环境中。然而,先前表征这些反应生成 NO 的效率的努力尚无定论,许多研究未能检测到 NO。在本工作中,重新研究了甲醛氧化物 (CHOO) 和乙醛氧化物 (CHCHOO) 与 NO 的反应,以在 4-40 Torr 的压力范围内进一步探索产物形成。未观察到 NO;然而,在甲醛和乙醛氧化物体系中,都在 Criegee-NO 加合物的质量处观察到与时间相关且依赖于 [NO] 的信号,并且通过从头计算探索了该加合物的结构。通过全球建模研究了标题反应的大气影响。

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