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对流层高层臭氧浓度较高时期主导三维臭氧分布的因素

Factors dominating 3-dimensional ozone distribution during high tropospheric ozone period.

作者信息

Chen Xiaoyang, Liu Yiming, Lai Anqi, Han Shuangshuang, Fan Qi, Wang Xuemei, Ling Zhenhao, Huang Fuxiang, Fan Shaojia

机构信息

School of Atmospheric Sciences/Guangdong Province Key Laboratory for Climate Change and Natural Disaster Studies, Sun Yat-sen University, Guangzhou 510275, China.

National Satellite Meteorological Center, Beijing 100081, China; School of Earth Sciences and Resources, China University of Geosciences, Beijing 100083, China.

出版信息

Environ Pollut. 2018 Jan;232:55-64. doi: 10.1016/j.envpol.2017.09.017. Epub 2017 Sep 25.

Abstract

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 O-precursor sensitivity along the vertical O profiles was investigated. Two sensitive scenarios, which had cut 30% anthropogenic NO or VOC emissions, showed that O-precursor indicators, specifically the ratios of O/NOy, HO/HNO or HO/NO, could partly distinguish the O-precursor sensitivity between VOCs-sensitive and NOx-sensitive along the vertical profiles. In urban area, the O-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 O peaks at the near-ground layer and 2 km above ground height, respectively.

摘要

对2012年8月一个原位监测网络和5个臭氧探空仪的数据进行了分析,在8月8日前后观测到了一次对流层高层臭氧事件。利用社区多尺度空气质量(CMAQ)模型及其过程分析工具,研究了臭氧垂直剖面不同高度处臭氧混合比高值的影响因素和机制。应用了一个没有来自MOZART4-GEOS5的化学初始和边界条件(ICBCs)的敏感情景,来研究平流层-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高臭氧峰值主要由STE主导。过程分析结果表明:在市区,地面高度约2公里处的第二个峰值主要由当地光化学产生引起。第三个峰值(近地面)主要由来自郊区/农村地区的上风输送引起;在郊区/农村地区,臭氧的当地光化学产生主导了从地面到约3公里高度的高臭氧混合比。此外,还研究了指标沿垂直臭氧剖面区分臭氧前体敏感性的能力。两个削减了30%人为NO或VOC排放的敏感情景表明,臭氧前体指标,特别是O/NOy、HO/HNO或HO/NO的比值,能够沿垂直剖面部分区分VOCs敏感和NOx敏感之间的臭氧前体敏感性。在市区,臭氧前体关系从边界层内的VOCs敏感转变为地面高度约1-3公里处的NOx敏感,进一步证实了输送和光化学产生分别在近地面层和地面高度2公里处的高臭氧峰值中的主导作用。

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