Factors dominating 3-dimensional ozone distribution during high tropospheric ozone period.
Factors dominating 3-dimensional ozone distribution during high tropospheric ozone period.
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DOI：
10.1016/j.envpol.2017.09.017
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发表时间：
2018
影响因子：
8.9
通讯作者：
Xiaoyang Chen;Yiming Liu;Anqi Lai;Shuangshuang Han;Q. Fan;Xuemei Wang;Z. Ling;F. Huang;S. Fan
中科院分区：
文献类型：
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作者：
Xiaoyang Chen;Yiming Liu;Anqi Lai;Shuangshuang Han;Q. Fan;Xuemei Wang;Z. Ling;F. Huang;S. Fan
分析了2012年8月对流层臭氧浓度高的实况监测网和5个臭氧探测仪的观测数据，并利用CMAQ模式及其过程分析工具研究了不同层次臭氧垂直廓线上臭氧混合比高的影响因素和机制。利用MOZART 4-GEOS 5中一个不含化学初始和边界条件的敏感情景，研究了平流层-对流层交换（STE）对垂直臭氧的影响。模拟结果表明，对流层顶附近的第一个臭氧高峰由STE主导。过程分析结果表明：在市区，第二个峰值出现在距地面约2km处，主要是由本地光化学产物引起的。第三个峰值（近地面）主要是由来自郊区/农村地区的逆风输送造成的;在郊区/农村地区，当地的臭氧光化学生产占主导地位的高臭氧混合比从地面到约3公里的高度。此外，指标区分O3-前驱物敏感性沿着垂直O3剖面的能力进行了研究。两种敏感情景（削减30%的人为NOx或VOC排放）表明，O3-前体物指标，特别是O3/NOy、H2 O2/HNO 3或H2 O2/NOZ的比值，可以部分区分O3-前体物对VOCs敏感和NOx敏感的沿着垂直剖面。在城市地区，O3-前体物的关系从边界层内的VOCs敏感转移到NOx敏感的约1-3公里的地面高度，进一步证实了交通和光化学生产的主导作用，在近地面层和2公里的地面高度，分别高O3峰值。
Data from an in situ monitoring network and five ozone sondes are analysed during August of 2012, and a high tropospheric ozone episode is observed around the 8th of AUG. The Community Multi-scale Air Quality (CMAQ) model and its process analysis tool were used to study factors and mechanisms for high ozone mixing ratio at different levels of ozone vertical profiles. A sensitive scenario without chemical initial and boundary conditions (ICBCs) from MOZART4-GEOS5 was applied to study the impact of stratosphere-troposphere exchange (STE) on vertical ozone. The simulation results indicated that the first high ozone peak near the tropopause was dominated by STE. Results from process analysis showed that: in the urban area, the second peak at approximately 2 km above ground height was mainly caused by local photochemical production. The third peak (near surface) was mainly caused by the upwind transportation from the suburban/rural areas; in the suburban/rural areas, local photochemical production of ozone dominated the high ozone mixing ratio from the surface to approximately 3 km height. Furthermore, the capability of indicators to distinguish O3-precursor sensitivity along the vertical O3profiles was investigated. Two sensitive scenarios, which had cut 30% anthropogenic NOXor VOC emissions, showed that O3-precursor indicators, specifically the ratios of O3/NOy, H2O2/HNO3or H2O2/NOZ, could partly distinguish the O3-precursor sensitivity between VOCs-sensitive and NOx-sensitive along the vertical profiles. In urban area, the O3-precursor relationship transferred from VOCs-sensitive within the boundary layer to NOx-sensitive at approximately 1–3 km above ground height, further confirming the dominant roles of transportation and photochemical production in high O3peaks at the near-ground layer and 2 km above ground height, respectively.