四川盆地城市群臭氧污染时空精细演变特征的观测与模拟

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摘要基于四川盆地污染物浓度和气象数据，结合ERA5再分析资料研究了2019年8月22~28日臭氧（O₃）污染过程的演变及高低空大气环流特征，并利用高分辨率中尺度天气预报模式WRF和多尺度空气质量模型CMAQ探究了O₃形成与传输过程.结果表明：①O₃浓度的分布特征与风向、温度的分布密切相关， O₃高值区主要位于高温和主导风向的下风向区域.污染过程中南亚高压和西太平洋副热带高压稳定地控制整个四川盆地，700和850hPa均受高压控制，盛行下沉气流，地面升温，促进O₃的迅速生成，同时抑制了地面O₃向高空的稀释扩散.②夜间1000m高度上O₃浓度水平和空间分布特征受白天地面O₃_8h浓度分布以及风场传输作用的影响较大.夜间O₃低值主要在盆地底部地区，成都及重庆市区受NO滴定作用影响，为两大低值中心，O₃高值中心受山脉阻挡作用，呈带状堆积在盆地边缘地区.③利用WRF-CMAQ模型中的过程分析量化不同物理化学过程对O₃浓度的相对贡献，垂直传输过程和气相化学是白天O₃的主要来源，干沉降和水平平流为地面O₃的主要汇.④利用ISAM综合源解析方法估算城市间输送对O₃浓度的相对贡献.受东北风输送的影响，模式边界对川东北城市群贡献为58.86%~79.23%；东南风使重庆O₃浓度受边界的影响较大，贡献约为72.50%.NO₂贡献的来源主要为城市自身及周边城市的传输.川东北城市群的NO_x排放较低，来自模式边界以及重庆地区的输入对川东北城市群有较大的贡献.⑤生物源、工业源和交通源对四川盆地O₃浓度的贡献显著，而居民源和电厂的贡献较低.成都、德阳、重庆、眉山、内江、宜宾等城市工业源的贡献率较高.

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关键词 ：臭氧污染, 传输过程, 化学生成, 来源贡献, 数值模拟

Abstract：Based on air pollutants observation and meteorological data in the Sichuan Basin in August 2019, combined with the ERA5 reanalysis data, the changes of upper and lower level weather situation and ozone (O₃) pollution during the episode were examined. In addition, the high-resolution mesoscale weather forecast model WRF and multi-scale air quality model CMAQ were used to explore the formation and transport of O₃. The results showed that:①The distribution characteristics of ozone concentration were closely related to the distribution of wind direction and temperature, and the area of high O₃ value mainly located in the high temperature area and the downwind of dominant wind direction. In the process of pollution, the South Asia High and the West Pacific Subtropical High steadily controlled the entire Sichuan Basin, where 700hPa and 850hPa were controlled by the high pressure, leading to prevailing downdraft, increase of surface temperature, promotion of the rapid O₃ generation, and inhibition of the dilution and diffusion of surface O₃ to the upper air. ②The concentration and spatial distribution of O₃ at 1000m height at night were greatly affected by the distribution of O₃_8h at ground level and the transmission of wind field during the day. The low O₃ values at night were mainly located at the bottom of the basin. Chengdu and Chongqing urban areas were affected by NO titration and were the two remarkable low-value centers in the night. The high-value O₃ centers were blocked by mountains and accumulated in a zonal pattern at the edge of the basin. ③The relative contributions of different physical and chemical processes to O₃ concentration were quantified by process analysis in WRF-CMAQ model. Vertical transport processes and gas phase chemistry were the main sources of daytime O₃, dry sedimentation and horizontal advection were the main sinks of surface O₃. ④The relative contribution of city-to-city transport to O₃ concentration was estimated by ISAM comprehensive source analysis method. Under the influence of northeast wind transport, the contribution of model boundary to northeast Sichuan urban agglomeration was about 58.86%~79.23%. The southeast wind greatly affected the O₃ concentration in Chongqing, contributing about 72.50% from model boundary. The main sources of NO₂ contribution came from city itself and the surrounding regional transmission. The NO_x emission in the northeast Sichuan urban agglomeration was lower than that in other regions of the Sichuan Basin, so the NO₂ concentration imported from the model boundary and Chongqing had a greater contribution to the northeast Sichuan. ⑤Biological sources, industrial sources and transportation sources contributed significantly to O₃ concentration in the Sichuan Basin, while residential energy sources and power plants contributed less. The contribution rate of industrial sector in Chengdu, Deyang, Chongqing, Meishan, Neijiang and Yibin was relatively high.

Key words： ozone pollution transport process chemical process source contribution numerical simulation

收稿日期: 2023-05-31

PACS:

X51

基金资助:国家自然科学基金资助项目（42175174；42105167）；国家重点研发计划（2018YFC0214002）；成都信息工程大学引进人才科研启动项目（KYTZ202127）

通讯作者: 张小玲,教授,xlzhang@ium.cn E-mail: xlzhang@ium.cn

作者简介: 张小玲(1972-),女,甘肃西和人,教授,博士,主要从事大气污染与天气气候、城市气象与环境、环境气象与健康研究.发表论文150余篇.xlzhang@ium.cn.

引用本文:

张小玲, 雷雨, 王聪聪, 吴锴, 杨显玉, 谭钦文, 陆成伟. 四川盆地城市群臭氧污染时空精细演变特征的观测与模拟[J]. 中国环境科学, 2024, 44(1): 1-14. ZHANG Xiao-ling, LEI Yu, WANG Cong-cong, WU Kai, YANG Xian-yu, TAN Qin-wen, LU Cheng-wei. Fine-scale evolution pattern of ozone pollution in the city cluster of Sichuan Basin from observation and modeling perspectives. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(1): 1-14.

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