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Investigating the Impacts of Nonacyl Peroxy Nitrates on the Global Composition of the Troposphere Using a 3-D Chemical Transport Model, STOCHEM-CRI
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-06-16 , DOI: 10.1021/acsearthspacechem.0c00133
M. Anwar H. Khan 1 , Barnaby Miles 1 , Michael E. Jenkin 2 , Richard G. Derwent 3 , Carl J. Percival 4 , Dudley E. Shallcross 1, 5
Affiliation  

Nonacyl peroxy nitrates, RO2NO2, act as a reservoir species for NOx in the upper troposphere. The low thermal stability of these compounds means that they only become a significant sink of NOx at the low temperatures observed in the upper troposphere. The chemical processes involved with the formation and degradation of methyl peroxy nitrate (CH3O2NO2) and an additional 44 RO2NO2 have been incorporated into the global three-dimensional chemical transport model, STOCHEM-CRI. The study investigates the effect of the addition of RO2NO2 chemistry on the budget of NOx, which in turn impacts the ozone, hydroxyl radical (OH), and nitrate radical (NO3) formation. This investigation found that the addition of CH3O2NO2 led to an increase in the tropospheric burdens of NOx (+3.0%), ozone (+2.0%), OH (+4.0%), and NO3 (+8.8%). However, the other 44 RO2NO2 contribute a significant increment of tropospheric global burdens of NOx (+4.4%), ozone (+3.4%), OH (+5.5%), and NO3 (+11.1%) with the largest mixing ratios of NOx of up to 25%, ozone up to 14%, OH up to 20%, and NO3 up to 50%. The increase in the global burden of oxidizing species such as OH due to the addition of 44 other RO2NO2 led to a significant decrease in the lifetimes of greenhouse gases such as methane (∼6%). The modeled mixing ratios of CH3O2NO2 were in reasonable agreement with measurements, the only extensive data set available.

中文翻译:

使用3-D化学迁移模型STOCHEM-CRI调查壬酰基过氧硝酸盐对对流层全球组成的影响

壬酰基过氧硝酸盐RO 2 NO 2充当对流层上部NO x的储集层。的这些化合物手段低的热稳定性使得它们只能成为NO的显著水槽X在上部对流层中观察到的低的温度。与三维过氧硝酸甲酯(CH 3 O 2 NO 2)和另外的44 RO 2 NO 2的形成和降解有关的化学过程已纳入全球三维化学迁移模型STOCHEM-CRI。研究调查了添加RO 2 NO 2的影响对NO的预算化学X,这反过来又影响臭氧,羟基自由基(OH),和硝酸根(NO 3)的形成。此调查发现,加入的CH 3 ö 2 NO 2导致的增加NO的对流层负担X(+ 3.0%),臭氧(+ 2.0%),OH(+ 4.0%),和NO 3(8.8 %)。然而,其他44 RO 2 NO 2有助于NO的对流层全球负担的显著增量X(+ 4.4%),臭氧(+ 3.4%),OH(+ 5.5%),和NO 3(+ 11.1%)与NO的最大混合比X达到的25%,臭氧达14%,OH高达20%,并且NO3高达50%。由于添加了44种其他RO 2 NO 2而增加了诸如OH之类的氧化性物质的全球负担,导致诸如甲烷之类的温室气体的寿命显着降低(约6%)。CH 3 O 2 NO 2的模拟混合比与测量值合理吻合,这是唯一可用的广泛数据集。
更新日期:2020-07-16
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