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我国北方地区对流层中下层臭氧收支
Ozone Budget in the Lower and Middle Troposphere over North China
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摘要: 为了揭示我国北方地区对流层中下层臭氧(O3) 的形成机理以及周边地区的污染输送对我国北方地区对流层中下层O3收支的影响, 在与外场观测数据比较分析的基础上, 利用全球化学输送模式(MOZART-2) 采用收支分析方法定量分析了影响我国北方地区对流层中下层O3的各个物理化学过程。结果表明:我国北方地区对流层下层O3最重要的来源是光化学生成作用, 约占总来源的58.3%(41.5 Tg), 光化学生成反应中HO2对于O3生成的贡献最大; 最大的汇是干沉降过程, 约占总汇的43.2%(26.2Tg); 水平净输送作用对我国北方地区对流层中下层O3收支的影响非常大, 在我国北方地区对流层下层, 41.6%左右的O3来自水平净输送, 随高度增加, 水平输送影响增大, 我国北方地区对流层中层大约81.5%的O3来自水平净输送。Abstract: Photochemical reaction, transportation and deposition are the main processes that effect ozone concentrations in troposphere.Quantitative estimation of troposphere ozone budget and the effect of intercontinental transport are very important in order to reveal ozone formation mechanism and the impacts of transport on troposphere ozone over North China. MOZART-2, a global chemical transport model (model of ozone and related tracers, Version 2) is used to assess physical and chemical processes that influence the budget of lower and middle troposphere ozone in North China.Ozone sonde data obtained by TAPTO (The Transport of Air Pollution and Troposphere Ozone over China) field campaign are compared with model results for reference. The comparison shows that MOZART-2 represents the vertical distributions of ozone in the lower and middle troposphere over North China very well, while for the upper troposphere, ozone concentrations are overestimated by the model. Budget analysis indicates that in the lower troposphere over North China, photochemical production (41.5 Tg) contributes about 58.3 % of the total ozone sources, and oxidation of NO by HO2 is the largest contributor especially. The largest consumption process in lower troposphere is dry deposition, accounting for about 43.2 % of the total ozone sinks. Ozone chemical budget varies with seasons notably. It reaches its maximum in summer due to strong photochemical reactions, while the minimum chemical budget occurs in winter because of low temperature and weak reactions.The chemical production of ozone is more than the chemical loss in the lower troposphere in the whole year. But for middle troposphere, chemical loss exceeds chemical production all year except in summer. In summer, ozone precursors in the boundary layer can be transported to upper level of troposphere due to the active convection, and the photochemical reactions of more ozone precursors lead to more ozone production. Net horizontal transport plays an important role in ozone budget in the low and middle troposphere over North China. About 41.6 % ozone in lower troposphere comes from net horizontal transport. As the height increases, wind speed rises, and the influence of net horizontal transport enhances. Nearly 81.5 % ozone in the middle troposphere comes from net horizontal transport. Constrained by simulating ability for sub-grid processes, the model tends to overestimate ozone concentration in upper troposphere and near the tropopause over middle to high northern latitudes. Modeling for sub-grid processes such as stratosphere-troposphere exchange (STE) should be improved to comprehend mechanism of ozone in the whole troposphere in depth.
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图 1 地面至25km的O3浓度模拟值与观测值比对
Fig. 1 Comparison of simulated O3 with the observed from ground to 25 km
图 2 地面至12km的O3浓度模拟值与观测值比对
Fig. 2 Comparison of simulated O3 with the observed from ground to 12 km
图 3 2004年我国北方地区臭氧光化学收支年变化
(a) 对流层下层, (b) 对流层中层
Fig. 3 Annual circle of O3 photochemical budget in North China of 2004
(a) lower troposphere, (b) middle troposphere
图 4 2004年我国北方地区的O3干沉降年变化
Fig. 4 Annual circle of O3 dry deposition in North China of 2004
图 5 2004年我国北方地区的O3水平输送量年变化
(a) 对流层下层, (b) 对流层中层
Fig. 5 Annual circle of O3 horizontal transport in North China of 2004
(a) lower troposphere, (b) middle troposphere
表 1 2004年我国北方地区对流层中下层O3年收支(单位:Tg)
Table 1 Annual O3 budget in the lower and middle troposphere over North China of 2004 (unit:Tg)
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