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南京北郊地区昼夜大气PM2.5中硫同位素的组成及来源
引用本文:张海潇,沈潇雨,郭照冰,郭庆军,陈善莉,柏杨,王瑾瑾.南京北郊地区昼夜大气PM2.5中硫同位素的组成及来源[J].环境科学研究,2019,32(3):440-446.
作者姓名:张海潇  沈潇雨  郭照冰  郭庆军  陈善莉  柏杨  王瑾瑾
作者单位:南京信息工程大学环境科学与工程学院,江苏 南京 210044;江苏省大气环境监测与污染控制高技术研究重点实验室,江苏 南京 210044;中国科学院地理科学与资源研究所,北京,100101;南京信息工程大学环境科学与工程学院,江苏 南京 210044;江苏省大气环境监测与污染控制高技术研究重点实验室,江苏 南京 210044;南京信息工程大学大气物理学院,江苏 南京 210044;南京信息工程大学环境科学与工程学院,江苏 南京 210044;江苏省大气环境监测与污染控制高技术研究重点实验室,江苏 南京 210044;中国科学院地理科学与资源研究所,北京 100101
基金项目:国家自然科学基金项目(No.41373023,91544229-02,41625006)
摘    要:为研究南京地区昼夜大气PM2.5中的硫同位素组成情况,采用Delta V Advantage同位素质谱仪技术对2016年3-4月南京北郊地区大气PM2.5中昼夜δ34S(硫同位素值)进行分析,结合大气颗粒物化学组成,追溯昼夜大气PM2.5及SO42-的来源.结果表明:南京北郊地区PM2.5和SO42-的整体变化趋势一致,具有同源性.南京北郊地区白天大气PM2.5的δ34S范围为4.23‰~7.16‰,平均值为5.45‰±0.91‰;晚上δ34S的范围为4.20‰~6.73‰,平均值为5.22‰±0.83‰.相较于晚上,白天δ34S略高主要与NOx对SO2的异相氧化反应和机动车尾气的排放有关.重霾天δ34S范围为4.20‰~7.16‰,平均值为5.39‰±0.87‰;清洁天δ34S范围为3.14‰~5.14‰,平均值为4.03‰±0.57‰.重霾天的硫源与燃煤、机动车尾气排放及NOx对SO2的异相氧化反应有关;而清洁天主要受到机动车尾气排放及SO2与O3均相氧化反应的影响.研究显示,南京北郊地区ρ(PM2.5)昼大于夜,而ρ(SO42-)夜大于昼,重霾天大气PM2.5的δ34S高于清洁天,这主要与NOx、SO2、O3的相互转化有关. 

关 键 词:PM2.5  硫同位素  昼夜  SO42-
收稿时间:2018/3/16 0:00:00
修稿时间:2018/10/30 0:00:00

Investigations on Sulfur Isotopic Compositions of Day and Night in Atmospheric PM2.5 in the Northern Suburb of Nanjing City
ZHANG Haixiao,SHEN Xiaoyu,GUO Zhaobing,GUO Qingjun,CHEN Shanli,BAI Yang and WANG Jinjin.Investigations on Sulfur Isotopic Compositions of Day and Night in Atmospheric PM2.5 in the Northern Suburb of Nanjing City[J].Research of Environmental Sciences,2019,32(3):440-446.
Authors:ZHANG Haixiao  SHEN Xiaoyu  GUO Zhaobing  GUO Qingjun  CHEN Shanli  BAI Yang and WANG Jinjin
Affiliation:1.School of Environmental Science and Engineering, Nanjing University of Information Science & Technology, Nanjing 210044, China2.Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Nanjing 210044, China3.Institule of Geographic Sciences and Natural Resources Research, CAS, Beijing 100101, China4.School of Atmospheric Physics, Nanjing University of Information Science & Technology, Nanjing 210044, China
Abstract:To investigate the origin of PM2.5 and sulfate at a suburban site in the north of Nanjing City, PM2.5 samples were collected from March to April 2016, and the Delta V Advantage isotope ratio mass spectrometry was used to analyze the isotopic composition (δ34S) of sulfur during the day and night time. The PM2.5 concentrations were higher at daytime than at night, while sulfate exhibited higher concentrations at night. In general, PM2.5 and sulfate had consistent temporal variation throughout the sampling period. The δ34S values ranged from 4.23‰ to 7.16‰ with an average of 5.45‰±0.91‰ during the daytime. The average δ34S value at night was 5.22‰±0.83‰, ranging from 4.20‰ to 6.73‰. The δ34S values of day and night changed in a similar trend. The higher δ34S values during the daytime could be ascribed to heterogeneous oxidation of SO2 by NOx and motor vehicle emissions. The δ34S values were 4.20‰-7.16‰ in haze days and 3.14‰-5.14‰ in clean days, with the averages of 5.39‰±0.87‰ and 4.03‰±0.57‰, respectively. We found that the sulfur in PM2.5 during haze days were mainly from coal burning, motor vehicle exhaust and heterogeneous oxidation of SO2 by NOx, while motor vehicle exhaust and homogeneous oxidation of SO2 by O3 were the major sources during clean days. The daytime concentration of PM2.5 in the northern suburbs of Nanjing City was greater than that of night, while the concentration of SO42- was greater at night time. The average δ34S value of ambient PM2.5 was higher during haze days than that during clean days, which was likely related to the different oxidation mechanisms of SO2 during haze and clean days. 
Keywords:PM2  5  sulfur isotope  daytime and nighttime  SO42-
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