Chen Xiaoyang, Liu Yiming, Lai Anqi, Han Shuangshuang, Fan Qi, Wang Xuemei, Ling Zhenhao, Huang Fuxiang, Fan Shaojia
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.
Environ Pollut. 2018 Jan;232:55-64. doi: 10.1016/j.envpol.2017.09.017. Epub 2017 Sep 25.
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.
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。