基于单颗粒气溶胶质谱技术的典型污染过程研究:以浙江省淳安县为例  

Study on a typical aerosol pollution evolution by single particle mass spectrometry:A case study in Chun’an county,Zhejiang province

作　　者：余传冠 陶士康 楼晟荣 朱书慧 周敏 乔利平 贾世超 方文华 黄成 陈长虹 YU Chuan-guan;TAO Shi-kang;LOU Sheng-rong;ZHU Shu-hui;ZHOU Min;QIAO Li-ping;JIA Shi-chao;FANG Wen-hua;HUANG Cheng;CHEN Chang-hong(Environmental Protection Monitoring Station of Chun’an County,Hangzhou 311700,China;State Environmental Protection Key Laboratory of the Formation and Prevention of Urban Air Pollution Complex,Shanghai Academy of Environmental Sciences,Shanghai 200233,China;Shanghai Polytechnic University,Shanghai 201209,China)

机构地区：[1]淳安县环境保护监测站,浙江杭州311700 [2]国家环境保护城市大气复合污染成因与防治重点实验室上海市环境科学研究院,上海200233 [3]上海第二工业大学,上海201209

出　　处：《地球化学》2020年第3期273-286,共14页Geochimica

基　　金：国家重点基础研究发展计划(2018YFC0213801);国家科技支撑计划(2014BAC22B03);国家自然科学基金(21507088);淳安环保项目(CACGZF[2016]24)。

摘　　要：基于单颗粒气溶胶质谱技术,开展浙江省淳安县冬季典型时段大气颗粒物观测研究。基于人工神经网络算法,将本次采集到的颗粒物组分分为元素碳-有机碳(14.9%)、铵盐(13.7%)、硫酸盐-硝酸盐(13.6%)、地壳元素(13.1%)、老化元素碳(12.3%)、有机碳(11.6%)和元素碳(8.0%)等共计10种类别。观测期间,捕捉到3次典型的污染过程,分别为污染积累-爆发增长阶段(Case 1)和两次轻度污染过程(Case 2、Case 3)。不同污染过程显示出不同组分粒径增长率的差异性,其中小粒径段(小于0.7μm)组分构成差别不大,具有较好的一致性,而大粒径段(大于0.7μm)颗粒物类别构成在不同污染过程中差异较大。长距离输送时颗粒物老化严重,硝酸盐等二次组分增多,局地源排放为主时,一次颗粒物元素碳增加,同时铵盐也有增加。研究表明,不利气象条件及区域性外围传输是导致本次高污染的主要原因。高污染期间,颗粒物主要来自北方和西南方向,各占40.2%,其次为长江三角洲本地源贡献,占19.2%。污染爆发增长阶段(Case 1-2),元素碳、元素碳-有机碳和老化元素碳组分明显增多,分别为污染积累阶段(Case 1-1)的2.4倍、3.2倍和3.2倍,表明移动源排放及其老化的二次产物对淳安地区高浓度细颗粒物具有重要贡献。淳安地区富氨现象明显,与本地排放及区域输送密切相关。A single particle aerosol mass spectrometer was employed in this study to analyze the chemical composition of fine particles in the winter in Chun’an County,Zhejiang Province,and perform regional source apportionment.Twelve clusters of chemical compositions,such as ECOC(elemental carbon and organic carbon,14.9%),NH4-rich(13.7%),SN(sulfate-nitrate,13.6%),dust(13.1%),aged EC(12.3%),OC(organic carbon,11.6%),and EC(8.0%),were classified according to the adaptive resonance theory-based clustering method ART-2a.During this field measurement,three typical pollution cases were observed,namely an accumulationexplosion period(Case 1)and two slightly polluted periods(Case 2 and Case 3).Particles in different pollution periods showed different growth factors.The chemical compositions for all periods were similar for the small size range(<0.7μm),while those for the large size range(>0.7μm),such as nitrate observed in the long-distance transport case and EC or NH4-rich particles found in local emissions cases,were distinctive.These results indicated that the main reason for the accumulation-explosion stage(Case 1)was unfavorable meteorological conditions and regional pollution transport.According to the hybrid single-particle Lagrangian integrated trajectory model result,particles were mainly from northern(40.2%),southwestern(40.2%),and regional sources in the YRD(19.2%).During the explosion stage(Cases 1-2),EC,ECOC,and aged EC components increased significantly by up to 2.4,3.2,and 3.2 times those of the accumulation stage(Case 1-1),respectively,thereby indicating that vehicle emissions and their secondary products made a large contribution to the high mass concentration of fine particles in Chun’an County.The abundance of ammonium particles in Chun’an also indicated that local particle pollution was closely related to local emissions and regional transport.

关 键 词：单颗粒气溶胶质谱 细颗粒物 组分类型 淳安县 

分 类 号：P593[天文地球—地球化学] X831[天文地球—地质学]