Investigating the Impacts of Nonacyl Peroxy Nitrates on the Global Composition of the Troposphere Using a 3-D Chemical Transport Model, STOCHEM-CRI
Investigating the Impacts of Nonacyl Peroxy Nitrates on the Global Composition of the Troposphere Using a 3-D Chemical Transport Model, STOCHEM-CRI
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使用 3-D 化学输运模型 STOCHEM-CRI 研究九酰基过氧硝酸盐对对流层整体组成的影响
DOI：
10.1021/acsearthspacechem.0c00133
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发表时间：
2020
影响因子：
3.4
通讯作者：
Khan M
中科院分区：
文献类型：
--
作者：
Khan M
在对流层上层，非酰基过氧硝酸盐(RO2NO2)是氮氧化物的储存物。这些化合物的低热稳定性意味着它们只在对流层上层观察到的低温下才会成为NOxat的重要汇。与过氧硝酸甲酯(CH3O2NO2)和另外的44RO2NO2的形成和降解有关的化学过程已被纳入全球三维化学传输模型STOCHEM-CRI。研究了添加RO2NO2化学物质对NOx收支的影响，进而影响臭氧、羟基自由基(OH)和硝酸根(NO3)的形成。研究发现，CH3O2NO2的加入增加了对流层NOx(+3.0%)、臭氧(+2.0%)、OH(+4.0%)和NO3(+8.8%)的负荷。然而，其余44个RO2NO2显著增加了对流层的NOx(+4.4%)、臭氧(+3.4%)、OH(+5.5%)和NO3(+11.1%)的全球负荷，其中NOx的最大混合率高达25%，臭氧的混合率高达14%，OH的混合率高达20%，NO3的混合率高达50%。由于另外44种RO2NO2的加入，全球氧化性物种(如OH)的负担增加，导致甲烷等温室气体的寿命显著缩短(∼为6%)。模拟的CH3O2NO2混合比与测量结果合理一致，这是唯一可用的广泛数据集。
Nonacyl peroxy nitrates, RO2NO2, act as a reservoir species for NOxin the upper troposphere. The low thermal stability of these compounds means that they only become a significant sink of NOxat 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 RO2NO2have been incorporated into the global three-dimensional chemical transport model, STOCHEM-CRI. The study investigates the effect of the addition of RO2NO2chemistry 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 CH3O2NO2led 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 RO2NO2contribute 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 NOxof up to 25%, ozone up to 14%, OH up to 20%, and NO3up to 50%. The increase in the global burden of oxidizing species such as OH due to the addition of 44 other RO2NO2led to a significant decrease in the lifetimes of greenhouse gases such as methane (∼6%). The modeled mixing ratios of CH3O2NO2were in reasonable agreement with measurements, the only extensive data set available.
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