同位素结合PMF模型解析珠三角PM_(2.5)来源研究  

Source of PM_(2.5) in the Pearl River Delta by isotope combined with PMF model

作　　者：苏涛[1,2] 李婷婷 陈多宏 田崇国 宗政[4] 张干[1] 李军[1] SU Tao;LI Tingting;CHEN Duohong;TIAN Chongguo;ZONG Zheng;ZHANG Gan;LI Jun(State Key Laboratory of Organic Geochemistry,Guangdong Key Laboratory of Environmental Protection and Resources Utilization,Guangzhou Institute of Geochemistry,Chinese Academy of Sciences,Guangzhou 510640,Guangdong,China;University of Chinese Academy of Sciences,Beijing 100049,China;Guangdong Ecological and Environmental Monitoring Center,Guangzhou 510308,Guangdong,China;Key Laboratory of Coastal Environmental Processes and Ecological Remediation,Yantai Institute of Coastal Zone Research,Chinese Academy of Sciences,Yantai 264003,Shandong,China)

机构地区：[1]中国科学院广州地球化学研究所,有机地球化学国家重点实验室广东省环境资源利用与保护重点实验室,广东广州510640 [2]中国科学院大学,北京100049 [3]广东省生态环境监测中心,广东广州510308 [4]中国科学院烟台海岸带研究所海岸环境过程与生态修复重点实验室,山东烟台264003

出　　处：《地球化学》2024年第3期320-329,共10页Geochimica

基　　金：广东省自然科学基金面上项目(2019A1515011175);广东省省级科技计划项目(2020B1212060053)联合资助。

摘　　要：二次气溶胶是大气细颗粒物(PM_(2.5))中最多的组分,客观识别其来源是PM_(2.5)源解析的难点,也是精确控制PM_(2.5)污染来源的关键。本研究在广东省鹤山超级大气监测站采集了76个PM_(2.5)样品,分析了其碳质组分(元素碳和有机碳)、水溶性离子(SO_(4)^(2-)、NH4^(+)、K^(+)、Ca^(2+)、Cl^(-)、Na^(+)、Mg^(2+)、NO_(2)^(-)和NO_(3)^(-))和金属元素(Fe、Cr、Cu、Mn、Ni、Pb、V、Zn、Cd、As)共20种化学组分,测定了7个PM_(2.5)代表样品的总碳(TC)放射性碳(^(14)C)。基于PM_(2.5)化学组分的PMF模型结果显示,生物质燃烧、海盐、土壤扬尘、轮船排放、工业过程、燃煤源和二次气溶胶分别贡献PM_(2.5)的18.98%、4.32%、13.85%、7.61%、14.08%、12.72%和30.03%。基于已发表的δ^(15)N(NO_(3)^(-))、δ^(18)O(NO_(3)^(-))结果,利用贝叶斯模型定量解析了NO_(3)^(-)的来源,并应用线型回归将PMF模型解析的二次气溶胶源再分配给一次颗粒源,结果显示,燃煤源(36.50%)、生物燃料源(29.35%)、土壤扬尘+海盐源(21.00%)和移动源(13.15%)是珠三角PM_(2.5)的主要来源。二次分配后PMF模型结果中TC的非化石源贡献与基于^(14)C结果的相对误差小于9%,说明PMF模型能很好地捕获PM_(2.5)主要贡献源,并且较准确地源解析珠三角的PM_(2.5),研究结果可为区域污染防治政策措施的制定提供科学依据。Secondary aerosols are the most abundant components of atmospheric fine particulate matter(PM_(2.5)),and objectively identifying their sources is a difficult task in the analysis of PM_(2.5) sources,and it is the key to accurately controlling the pollution of PM_(2.5).In this study,76 PM_(2.5) samples were collected at the Heshan Super Atmospheric Monitoring Station in Guangdong province.A total of 20 chemical components including organic carbon,elemental carbon,water-soluble ions(SO_(4)^(2-),NH4^(+),K^(+),Ca^(2+),Cl^(-),Na^(+),Mg^(2+),NO_(2)^(-),and NO_(3)^(-)),and metal elements(Fe,Cr,Cu,Mn,Ni,Pb,V,Zn,Cd,and As)were analyzed.Seven representative PM_(2.5) samples were analyzed for the radiocarbon(^(14)C)of total carbon(TC).The source apportion of PM_(2.5) by the PMF model showed that biomass combustion,sea salt,soil dust,ship emissions,industrial processes,coal burning,and secondary aerosols account for 18.98%,4.32%,13.85%,7.61%,14.08%,12.72%,and 30.03%of PM_(2.5),respectively.Based on the published and measured stable isotopes of oxygen and nitrogen(δ^(15)N-NO_(3)^(-)andδ^(18)O-NO_(3)^(-)),the Bayesian mixing model was used to apportion the source of-NO3 to coal combustion,traffic emission,and biogenic sources.The secondary aerosol source was then subdivided into three sources according to the discrepancy in the source apportion of-NO3 between PMF and Bayesian mixing model results.The results show that coal-related sources(36.50%),biofuel sources(29.35%),soil dust^(+)sea salt(21.00%),and mobile sources(13.15%)are the main sources of PM_(2.5) in the Pearl River Delta.The model performance was also estimated by ^(14)C-TC of seven samples.After secondary redistribution,the relative error between the modern carbon proportion of TC in the PMF model results and the modern carbon proportion of TC based on ^(14)C results was less than 9%,indicating the good performance of the developed method.The results of this study can provide a scientific basis for the formulation of regional pollution prevention and control poli

关 键 词：珠三角 大气细颗粒物 PMF模型 ^(15)N ^(14)C 

分 类 号：P402[天文地球—大气物理学与大气环境]