Simultaneous airborne nitric acid and formic acid measurements using a chemical ionization mass spectrometer around the UK: Analysis of primary and secondary production pathways

Simultaneous airborne nitric acid and formic acid measurements using a chemical ionization mass spectrometer around the UK: Analysis of primary and secondary production pathways
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DOI:
10.1016/j.atmosenv.2013.10.008
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发表时间:
2014-02-01
影响因子:
5
通讯作者:
Percival, Carl J.
Percival, Carl J.
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Le Breton, Michael;Bacak, Asan;Percival, Carl J.

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在FAAM BAE-146研究飞机上,使用I-试剂离子在0.8赫兹处使用化学电离质谱仪测量了英国各地首次同时测量甲酸和硝酸的混合比。对整个数据集的分析表明,甲酸和硝酸呈正相关,其他研究表明(例如Veres等人,2011年)。然而,初步证据表明,甲酸是一个突出的直接来源,当O-3水平较高时,甲酸也是一个重要的来源,这表明1-烯烃的臭氧化反应是重要的。轨迹模型能够通过包括主要载体源和丙烯当量1-烯烃水平的臭氧化反应来再现甲酸浓度。对数据档案的检查表明,这些水平的1-烯烃在上午11点后是可能的,但飞行早期的甲酸和硝酸羽流太高,模型无法复制。这些数据表明,硝酸和甲酸之间的关系不能完全归因于相关的光化学生产。在假定光化学羽流中的甲酸和硝酸之间的关系以及1-烯烃的恒定来源的情况下,实现了HCOOH和HNO3的同时测量,以估计飞行轨迹上的OH水平。(C)2013爱思唯尔有限公司。保留所有权利。
The first simultaneous measurements of formic and nitric acid mixing ratios around the United Kingdom were measured on the FAAM BAe-146 research aircraft with a chemical ionization mass spectrometer using I- reagent ions at 0.8 Hz. Analysis of the whole dataset shows that formic acid and nitric acid are positively correlated as illustrated by other studies (e.g. Veres et al., 2011). However, initial evidence indicates a prominent direct source of formic acid and also a significant source when O-3 levels are high, suggesting the importance of the ozonolysis of 1-alkenes. A trajectory model was able to reproduce the formic acid concentrations by both the inclusion of a primary vehicle source and production via ozonolysis of propene equivalent 1-alkene levels. Inspection of data archives implies these levels of 1-alkene are possible after 11 am, but formic acid and nitric acid plumes early in the flight are too high for the model to replicate. These data show the relationship between nitric acid and formic acid cannot solely be attributed to related photochemical production. The simultaneous measurement of HCOOH and HNO3 has been implemented to estimate OH levels along the flight track assuming a relationship between formic and nitric acid in photochemical plumes and a constant source of 1-alkene. (C) 2013 Elsevier Ltd. All rights reserved.