在 GEOS-Chem 9-02 版中实施 SAPRC-11 机制的全球对流层芳烃化学效应。

IF 4 3区 地球科学 Q1 GEOSCIENCES, MULTIDISCIPLINARY Geoscientific Model Development Pub Date : 2019-01-01 Epub Date: 2019-01-04 DOI:10.5194/gmd-12-111-2019
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B Millet, William C Porter, Jos Lelieveld
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摘要

利用全州空气污染研究中心第 11 版(SAPRC-11)芳烃化学机制对戈达德地球观测系统化学(GEOS-Chem)模型进行了更新,目的是评估最丰富的芳烃(苯、甲苯、二甲苯)对对流层氧化能力非常重要的化学物种的全球和区域影响。基于地表和飞机观测数据进行的模型评估表明,芳烃和臭氧的影响非常一致。通过对 GEOS-Chem 中的简化芳烃化学方案(如标准设置,相关过氧自由基不形成臭氧,氮氧化物也不循环利用)和 SAPRC-11 方案进行比较,可以发现臭氧、羟基自由基和氮氧化物在全球平均水平上的变化相对较小(1%-4%),但在污染源区域附近存在显著的区域差异(5%-20%)。氮氧化物(NO x)在污染源地区减少,而在对流层偏远地区增加,这主要是由于过氧乙酰硝酸酯(PAN)的传输效率更高,而过氧乙酰硝酸酯随 SAPRC 芳烃化学反应而增加。使用更新的芳香族化学成分的模型臭氧混合比增加了多达 5 ppb(超过 10%),尤其是在工业污染地区。臭氧的变化部分是由于芳烃氧化产物对臭氧生成率的直接影响,部分是由于氮氧化物空间分布的改变提高了对流层臭氧的生成效率。改进芳烃的表示对于模拟对流层氧化非常重要。
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Global tropospheric effects of aromatic chemistry with the SAPRC-11 mechanism implemented in GEOS-Chem version 9-02.

The Goddard Earth Observing System with chemistry (GEOS-Chem) model has been updated with the Statewide Air Pollution Research Center version 11 (SAPRC-11) aromatics chemical mechanism, with the purpose of evaluating global and regional effects of the most abundant aromatics (benzene, toluene, xylenes) on the chemical species important for tropospheric oxidation capacity. The model evaluation based on surface and aircraft observations indicates good agreement for aromatics and ozone. A comparison between scenarios in GEOS-Chem with simplified aromatic chemistry (as in the standard setup, with no ozone formation from related peroxy radicals or recycling of NOx) and with the SAPRC-11 scheme reveals relatively slight changes in ozone, the hydroxyl radical, and nitrogen oxides on a global mean basis (1 %-4 %), although remarkable regional differences (5 %-20 %) exist near the source regions. NO x decreases over the source regions and increases in the remote troposphere, due mainly to more efficient transport of peroxyacetyl nitrate (PAN), which is increased with the SAPRC aromatic chemistry. Model ozone mixing ratios with the updated aromatic chemistry increase by up to 5 ppb (more than 10 %), especially in industrially polluted regions. The ozone change is partly due to the direct influence of aromatic oxidation products on ozone production rates, and in part to the altered spatial distribution of NOx that enhances the tropospheric ozone production efficiency. Improved representation of aromatics is important to simulate the tropospheric oxidation.

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来源期刊
Geoscientific Model Development
Geoscientific Model Development GEOSCIENCES, MULTIDISCIPLINARY-
CiteScore
8.60
自引率
9.80%
发文量
352
审稿时长
6-12 weeks
期刊介绍: Geoscientific Model Development (GMD) is an international scientific journal dedicated to the publication and public discussion of the description, development, and evaluation of numerical models of the Earth system and its components. The following manuscript types can be considered for peer-reviewed publication: * geoscientific model descriptions, from statistical models to box models to GCMs; * development and technical papers, describing developments such as new parameterizations or technical aspects of running models such as the reproducibility of results; * new methods for assessment of models, including work on developing new metrics for assessing model performance and novel ways of comparing model results with observational data; * papers describing new standard experiments for assessing model performance or novel ways of comparing model results with observational data; * model experiment descriptions, including experimental details and project protocols; * full evaluations of previously published models.
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