Tropospheric ozone production regions and the intercontinental origins of surface ozone over Europe
Tropospheric ozone production regions and the intercontinental origins of surface ozone over Europe
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DOI：
10.1016/j.atmosenv.2015.04.049
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发表时间：
2015-07-01
影响因子：
5
通讯作者：
Shallcross, Dudley E.
中科院分区：
文献类型：
--
作者：
Derwent, Richard G.;Utembe, Steven R.;Shallcross, Dudley E.
在全球拉格朗日化学迁移模型中实施了臭氧标记标签计划，以确定欧洲地面臭氧的洲际来源。平流层和对流层的交换使整个欧洲产生了3至5 ppb，而中东、亚洲和太平洋区域的中纬度地区则产生了6至8 ppb。北美洲和北大西洋中纬度地区的地面臭氧水平为十亿分之十至十六。可观的洲际臭氧生产发生在大陆区域的顺风和表面层之上。来自热带地区的洲际臭氧形成和传输贡献了约4ppb，与中纬度地区相比效率低得多。有近60种化学过程驱动洲际臭氧的形成，其中HO2 + NO，CH3O2 NO和CH3COO2 + NO反应是最重要的。臭氧的产生似乎是由二次反应产物的OH氧化驱动的，而不是主要排放的VOC的氧化。最大的洲际臭氧贡献量为：从北美到欧洲基准站约为20 ppb，从亚洲到北美基准站约为14 ppb，从亚洲到欧洲基准站约为10 ppb。洲际臭氧生成和迁移的变化可能导致北方半球中纬度基线臭氧监测站的季节性臭氧趋势和季节性周期的变化。(C)2015爱思唯尔有限公司版权所有。
Ozone tagged labelling schemes have been implemented in a global Lagrangian chemistry-transport model to identify the intercontinental origins of surface ozone in Europe. Stratosphere troposphere exchange gave rise to between 3 and 5 ppb across Europe, whereas the mid-latitudes of the Middle East, Asia and the Pacific Ocean region contributed 6-8 ppb. Surface ozone levels of 10-16 ppb were associated with the mid-latitudes of North America and the North Atlantic Ocean regions. Appreciable intercontinental ozone production occurred downwind of continental regions and above the surface layer. Intercontinental ozone formation and transport from tropical regions contributed about 4 ppb and was much less efficient compared with that from mid-latitudes. There were approaching 60 chemical processes driving intercontinental ozone formation, of which the HO2 + NO, CH3O2 NO and CH3COO2 + NO reactions were the most important. Ozone production appeared to be driven by OH oxidation of secondary reaction products rather than the oxidation of primary emitted VOCs. The largest intercontinental ozone contributions amounted to about 20 ppb from North America to European baseline stations, 14 ppb from Asia to North American baseline stations and 10 ppb from Asia to European baseline stations. It is possible that changing intercontinental ozone production and transport could have led to seasonal ozone trends and shifts in seasonal cycles at northern hemisphere mid-latitude baseline ozone monitoring stations. (C) 2015 Elsevier Ltd. All rights reserved.