太原市采暖季清洁天与灰霾天PM_(2.5)中水溶性无机离子组成及来源分析
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摘要
为探究太原市采暖季PM_(2.5)水溶性无机离子组成及其来源,于2017年11月至2018年3月在太原城区连续采集大气颗粒物PM_(2.5)样品共151个,并于离子色谱仪中分析样品的9种水溶性无机离子(F~-、Cl~-、NO_3~-、SO_4~(2-)、K~+、Na~+、Ca~(2+)、Mg~(2+)、NH_4~+).结果表明,太原市采暖季PM_(2.5)质量浓度的平均值为77.89±47.16μg·m~(-3),总水溶性无机离子质量浓度平均值为53.21±29.76μg·m~(-3),占PM_(2.5)的68.3%±23.3%,其中SO_4~(2-)、NO_3~-和NH_4~+是PM_(2.5)中最主要的离子成分,NH_4~+在PM_(2.5)中主要以NH_4NO_3、(NH_4)_2SO_4与NH_4Cl等形式存在,NH_4~+、NO_3~-、K~+、SO_4~(2-)和Cl~-等5种离子的爆发性增长对灰霾天污染贡献最大.随着气温回升,硫氧化率和氮氧化率均有一定程度的升高,大气中存在明显的气溶胶二次转化过程.主成分分析表明,燃煤源和二次污染源是太原市采暖季灰霾期间的主要污染源,土壤扬尘为清洁天的首要污染源,大气污染以固定污染源为主,移动污染源为辅.后向轨迹模型显示,采暖季期间气团基本上来自本地和西北方向的内陆排放源.
To research the composition and source of water-soluble inorganic ions of PM_(2.5) in the heating season of Taiyuan city, a total of 151 samples of PM_(2.5) were continuously collected from November 2017 to March 2018 in Taiyuan city, and nine water-soluble inorganic species(F~-, Cl~-, NO_3~-, SO_4~(2-), K~+, Na~+, Ca~(2+), Mg~(2+), NH_4~+) in these samples were analyzed by using an ion chromatograph. The results showed that the mass concentrations of PM_(2.5) and of total water-soluble inorganic ions were 77.89±47.16 μg·m~(-3) and 53.21±29.76 μg·m~(-3), respectively, and those ions accounted for 68.3%±23.3% of PM_(2.5), among them, SO_4~(2-), NO_3~- and NH_4~+ were the most important ionic components in PM_(2.5). NH_4~+ exists mainly in the form of NH_4NO_3,(NH_4)_2SO_4 and NH_4Cl in PM_(2.5). The explosive growth of the five ions(i.e., NH_4~+, NO_3~-, K~+, SO_4~(2-) and Cl~-) were main contributors in haze days., As the temperature went up, the sulfur and nitrogen oxidation rate had a certain degree of elevation, demonstrating a significant aerosol secondary conversion processes in the atmosphere. The principal component analysis indicated that the coal source and the secondary pollution source were the main pollution sources in haze days, while the soil dust was the major pollution source in clean days. Air pollution of Taiyuan city were dominated by fixed pollution sources, supplemented by mobile pollution sources. The backward trajectory model showed that during the heating period air mass came mainly from inland emission sources of the local and of northwest directions.
To research the composition and source of water-soluble inorganic ions of PM_(2.5) in the heating season of Taiyuan city, a total of 151 samples of PM_(2.5) were continuously collected from November 2017 to March 2018 in Taiyuan city, and nine water-soluble inorganic species(F~-, Cl~-, NO_3~-, SO_4~(2-), K~+, Na~+, Ca~(2+), Mg~(2+), NH_4~+) in these samples were analyzed by using an ion chromatograph. The results showed that the mass concentrations of PM_(2.5) and of total water-soluble inorganic ions were 77.89±47.16 μg·m~(-3) and 53.21±29.76 μg·m~(-3), respectively, and those ions accounted for 68.3%±23.3% of PM_(2.5), among them, SO_4~(2-), NO_3~- and NH_4~+ were the most important ionic components in PM_(2.5). NH_4~+ exists mainly in the form of NH_4NO_3,(NH_4)_2SO_4 and NH_4Cl in PM_(2.5). The explosive growth of the five ions(i.e., NH_4~+, NO_3~-, K~+, SO_4~(2-) and Cl~-) were main contributors in haze days., As the temperature went up, the sulfur and nitrogen oxidation rate had a certain degree of elevation, demonstrating a significant aerosol secondary conversion processes in the atmosphere. The principal component analysis indicated that the coal source and the secondary pollution source were the main pollution sources in haze days, while the soil dust was the major pollution source in clean days. Air pollution of Taiyuan city were dominated by fixed pollution sources, supplemented by mobile pollution sources. The backward trajectory model showed that during the heating period air mass came mainly from inland emission sources of the local and of northwest directions.
引文
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[22] DUAN F K,HE K B,MA Y L,et al.Concentration and chemical characteristics of PM2.5 in Beijing,China:2001–2002[J].Science of the Total Environment,2006,355(1):264-275.
[23] LAI L Y,SEQUEIRA R.Visibility degradation across Hong Kong:its components and their relative contributions[J].Atmospheric Environment,2001,35(34):5861-5872.
[24] 魏玉香,杨卫芬,银燕,等.霾天气南京市大气PM2.5中水溶性离子污染特征[J].环境科学与技术,2009,32(11):66-71.WEI Y X,YANG W F,YIN Y,et al.Pollution characteristics of Nanjing water-soluble ions in air fine particles under haze days[J].Environmental Science & Technology,2009,32(11):66-71(in Chinese).
[25] OHTA S,OKITA T.A chemical characterization of atmospheric aerosol in Sapporo[J].Atmospheric Environment Part A General Topics,1990,24(4):815-822.
[26] 张立盛,石广玉.相对湿度对气溶胶辐射特性和辐射强迫的影响[J].气象学报,2002,60(2):230-337.ZHANG L S,SHI G Y.The impactof relative humidityon the radiative property and radiative forcingof sulfate aerosol[J].Acta Meteorologica Sinica,2002,60(2):230-337(in Chinese).
[27] CAO G L,ZHANG X Y,GONG S L,et al.Emission inventories of primary particles and pollutant gases for China[J].Chinese Science Bulletin,2011,56(8):781-788.
[28] SHEN Z X,CAO J J,ARIMOTO R,et al.Ionic composition of TSP and PM2.5 during dust storms and air pollution episodes at Xi′an,China[J].Atmospheric Environment,2009,43(18):2911-2918.
[2] DZUBAY T G,STEVENS R K,LEWIS C W,et al.Visibility and aerosol composition in Houston,Texas[J].Environ.sci.technol,1982,16(8):514-525.
[3] 张晓雨.中国中东部地区典型城市大气细颗粒物中化学组成特征及来源解析研究[D].南京:南京大学,2017.ZHANG X Y.Study on chemical characteristics and source apportionments of fine particulates in the typical cities over the central and eastern China[D].Nanjing:Nanjing University,2017(in Chinese).
[4] ZHANG R,WANG G,SONG G,et al.Formation of urban fine particulate matter[J].Chemical Reviews,2015,115(10):3803-3855.
[5] YANG D Y,LIU B X,ZHANG D W,et al.Correlation,seasonal and temporal variation of water-soluble ions of PM2.5 in Beijing during 2012-2013[J].Environmental Science,2015,36(3):768-773.
[6] MENG Z,JIANG X,YAN P,et al.Characteristics and sources of PM2.5 and carbonaceous species during winter in Taiyuan,China[J].Atmospheric Environment,2007,41(32):6901-6908.
[7] 贾小花,解静芳,马翔,等.太原市冬季PM2.5水溶性组分污染特征分析[J].中国环境科学,2013,33(4):599-604.JIA X H,XIE J F,MA X,et al.Analysis of water-soluble constituents in winter of PM2.5 in Taiyuan City[J].China Environmental Science,2013,33(4):599-604(in Chinese).
[8] 王思宇.应用PMF和PCA/APCS方法探究长春市大气中PM2.5来源[D].长春:吉林大学,2016.WANG S Y.Source apportionment of PM2.5 in atmosphere in Changchun using PMF and PCA/APCS methods[D].Changchun:Jilin University,2016(in Chinese).
[9] THURSTON G D,SPENGLER J D.A quantitative assessment of source contributions to inhalable particulate matter pollution in metropolitan Boston[J].Atmospheric Environment,1987,19(1):9-25.
[10] 孙启斌,肖红伟,肖化云,等.南昌市大气降水化学特征及来源分析[J].环境科学研究,2017,30(12):1841-1848.SUN Q B,XIAO H W,XIAO H Y,et al.Chemical characteristics and source apportionment of atmospheric precipitation in Nanchang city[J].Research of Environmental Sciences,2017,30(12):1841-1848(in Chinese).
[11] 王晓琦,周颖,程水源,等.典型城市冬季PM2.5水溶性离子污染特征与传输规律研究[J].中国环境科学,2016,36(8):2289-2296.WANG X Q,ZHOU Y,CHENG S Y,et al.Characterization and regional transmission impact of water-soluble ions in PM2.5 during winter in typical cities[J].China Environmental Science,2016,36(8):2289-2296(in Chinese).
[12] CHENG Z,JIANG J,FAJARDO O,et al.Characteristics and health impacts of particulate matter pollution in China (2001–2011)[J].Atmospheric Environment,2013,65(3):186-194.
[13] 张园园.南京北郊PM2.5中水溶性离子特征在线监测研究[D].南京:南京信息工程大学,2017.ZHANG Y Y.Characteristic of water-soluble ions in PM2.5 in the northern suburb of Nanjing based on on-line monitoring[D].Nanjing:Nanjing University of Information Science and Technology,2017(in Chinese).
[14] MING L,JIN L,LI J,et al.PM2.5 in the Yangtze River Delta,China:Chemical compositions,seasonal variations,and regional pollution events[J].Environmental Pollution,2017,223:200-212.
[15] 范美益,曹芳,张园园,等.徐州市冬季大气细颗粒物水溶性无机离子污染特征及来源解析[J].环境科学,2017,38(11):4478-4485.FAN M Y,CAO F,ZHANG Y Y,et al.Characteristics and sources of water soluble inorganic ions in fine particulate matter during winter in Xuzhou[J].Environmental Science,2017,38(11):4478-4485(in Chinese).
[16] 刘晓迪,孟静静,侯战方,等.济南市夏、冬季PM2.5中化学组分的季节变化特征及来源解析[J].环境科学,2018,39(09):4014-4025.LIU X D,MENG J J,HOU Z F,et al.Analysis of seasonal variations in chemical characteristics and sources of PM2.5 during summer and winter in Ji′nan city[J].Environmental Science,2018,39(09):4014-4025(in Chinese).
[17] 刘晓慧,朱彬,高晋徽,等.长江三角洲地区霾判别方法的对比分析[J].环境科学,2014,35(9):3239-3246.LIU X H,ZHU B,GAO J H,et al.Comparative analysis methods of haze distinction over Yangtze River delta region[J].Environmental Science,2014,35(9):3239-3246(in Chinese).
[18] 高韩钰,魏静,王跃思.北京南郊区PM2.5中水溶性无机盐季节变化及来源分析[J].环境科学,2018,39(5):1987-1993.GAO H Y,WEI J,WANG Y S,et al.Seasonal variation and source analysis of water-soluble inorganic salts in PM2.5 in the southern suburbs of Beijing[J].Environmental Science,2018,39(5):1987-1993(in Chinese).
[19] 张腾.太原市采暖季大气颗粒物化学组成特征及来源解析和重污染成因分析[D].太原:太原理工大学,2016.ZHANG T.Study on chemical characteristics and source of particulate matter and heavy pollution analysis in heating season,Taiyuan[D].Taiyuan:Taiyuan University of Technology,2016(in Chinese).
[20] 王新,聂燕,陈红,等.兰州城区大气PM2.5污染特征及来源解析[J].环境科学,2016,37(5):1619-1628.WANG X,NIE Y,CHEN H,et al.Pollution characteristics and source apportionment of PM2.5 in Lanzhou city[J].Environmental Science,2016,37(5):1619-1628(in Chinese).
[21] XIAO H Y,LIU C Q.Chemical characteristics of water-soluble components in TSP over Guiyang,SW China,2003[J].Atmospheric Environment,2004,38(37):6297-6306.
[22] DUAN F K,HE K B,MA Y L,et al.Concentration and chemical characteristics of PM2.5 in Beijing,China:2001–2002[J].Science of the Total Environment,2006,355(1):264-275.
[23] LAI L Y,SEQUEIRA R.Visibility degradation across Hong Kong:its components and their relative contributions[J].Atmospheric Environment,2001,35(34):5861-5872.
[24] 魏玉香,杨卫芬,银燕,等.霾天气南京市大气PM2.5中水溶性离子污染特征[J].环境科学与技术,2009,32(11):66-71.WEI Y X,YANG W F,YIN Y,et al.Pollution characteristics of Nanjing water-soluble ions in air fine particles under haze days[J].Environmental Science & Technology,2009,32(11):66-71(in Chinese).
[25] OHTA S,OKITA T.A chemical characterization of atmospheric aerosol in Sapporo[J].Atmospheric Environment Part A General Topics,1990,24(4):815-822.
[26] 张立盛,石广玉.相对湿度对气溶胶辐射特性和辐射强迫的影响[J].气象学报,2002,60(2):230-337.ZHANG L S,SHI G Y.The impactof relative humidityon the radiative property and radiative forcingof sulfate aerosol[J].Acta Meteorologica Sinica,2002,60(2):230-337(in Chinese).
[27] CAO G L,ZHANG X Y,GONG S L,et al.Emission inventories of primary particles and pollutant gases for China[J].Chinese Science Bulletin,2011,56(8):781-788.
[28] SHEN Z X,CAO J J,ARIMOTO R,et al.Ionic composition of TSP and PM2.5 during dust storms and air pollution episodes at Xi′an,China[J].Atmospheric Environment,2009,43(18):2911-2918.
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