山东临沂大气夏季典型时段臭氧污染特征及其控制因素分析  

Pollution Characteristic and Control Factor Analysis of Atmospheric Ozone During Summer Typical Periods in Linyi, Shandong

作　　者：杨雪 安馨悦 刘玉启 江春美 张鹏程 李灵婕 赵世阳 张书源 YANG Xue;AN Xin-yue;LIU Yu-qi;JIANG Chun-mei;ZHANG Peng-cheng;LI Ling-jie;ZHAO Shi-yang;ZHANG Shu-yuan(School of Municipal and Environmental Engineering,Shandong Jianzhu University,Ji'nan 250101,China;Ji'nan Ecological Environment Monitoring Center of Shandong Province,Ji'nan 250101,China;Hedong Branch of Linyi Ecologyical Environmental Bureau,Linyi 276034,China;School of Environmental and Material Engineering,Yantai University,Yantai 264005,China)

机构地区：[1]山东建筑大学市政与环境工程学院,济南250101 [2]山东省济南市生态环境监测中心,济南250101 [3]临沂市生态环境局河东分局,临沂276034 [4]烟台大学环境与材料工程学院,烟台264005

出　　处：《环境科学》2022年第2期696-706,共11页Environmental Science

基　　金：国家自然科学基金项目(42005092);山东省自然科学基金项目(ZR2020QD058);山东建筑大学博士科研基金项目(XNBS1936);上海市大气颗粒物污染防治重点实验室开放课题项目(FDLAP19006)。

摘　　要：2020年6月,在山东省临沂城区开展臭氧(O_(3))及其前体物观测实验,基于观测数据结合MCM光化学模式模拟,对6月中旬O_(3)污染特例生成机理及控制机制进行了分析.结果发现,尽管观测期间降水较多,一旦天气转晴,O_(3)迅速积累并超标,1-h和8-hφ(O_(3))超标天数分别为10 d(频率32%)和14 d(45%).O_(3)日变化呈单峰模态,峰值出现在午后16:00.MCM模拟结果表明,光化学污染特例日O_(3)日均净生成反应速率为20×10^(-9)h^(-1),HO_(2)·+NO和RO_(2)·(除CH_(3)O_(2)·外)+NO反应分别贡献O_(3)生成的49.0%~51.1%和37.3%~40.2%;·OH+NO_(2)反应对O_(3)总消耗的贡献约为35.1%~57.4%.VOCs反应活性、增量反应活性RIR和基于EKMA曲线方法结果均表明O_(3)的生成对烯烃(主要优势单体为反-2-戊烯和反-2-丁烯),芳香烃(主要优势单体为对/间-二甲苯和甲苯)更为敏感,而对NO_(x)呈负敏感,即降低φ(VOCs)可使φ(O_(3))显著下降,而降低φ(NO_(x))反而会引起φ(O_(3))的上升.PMF源解析结果表明,溶剂使用挥发源和机动车尾气排放源对以上优势单体VOCs贡献显著.考虑机动车尾气排放NO对O_(3)的滴定效应,控制溶剂使用挥发源可以实现O_(3)污染精准有效控制.In June 2020,an observation experiment of O_(3) and its precursors was carried out in Linyi City,Shandong Province.Based on the observation data and MCM photochemical model simulation,the formation mechanism and control mechanism of an ozone pollution case in mid-June were analyzed.The study found that,despite the high precipitation during the observation period,ozone concentrations rapidly accumulated and exceeded the limits once the weather cleared,with the 1-h average and 8-hφ(O_(3))exceeding the national ambient air quality standards on 10 days(32%in frequency)and 14 days(45%),respectively.The diurnal variation in O_(3) concentration was unimodal and accompanied by the afternoon peak at 16:00.MCM simulation results showed that the daily net reaction rate of O_(3) was 20×10^(-9) h^(-1),and HO_(2)·+NO and RO_(2)·(except CH_(3)O_(2)·)+NO contributed 49.0%-51.1%and 37.3%-40.2%of O_(3) generation,respectively.The contribution of the·OH+NO_(2) reaction to the total consumption of O_(3) was 35.1%-57.4%.The results of VOCs reactivity,relative incremental reactivity(RIR),and the EKMA curve method showed that the generation of O_(3) was more sensitive to alkenes(mainly trans-2-pentene and trans-2-butene)and aromatics(mainly m/p-xylene and toluene)but was negatively sensitive to NO_(x).In other words,the reduction in VOCs concentration would lead to the decrease in O_(3) concentration,whereas the reduction in NO_(x) concentration would lead to the increase in O_(3) concentration.PMF source analysis results showed that volatile sources used by solvents and vehicle exhaust emissions contributed significantly to the above key precursor VOC species.Considering the titration effect of NO from vehicle exhaust emissions on ozone,controlling the use of volatile sources of solvents can realize the control of O_(3) pollution accurately and efficiently.

关 键 词：臭氧(O_(3)) 挥发性有机物(VOCs) 生成机制 主要化学机制(MCM) 经典动力学模拟法(EKMA) 

分 类 号：X51[环境科学与工程—环境工程]