长江三角洲霾天气PM_(2.5)中水溶性离子特征及来源解析
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摘要
于2016年12月13日～2017年1月5日采集了徐州、东山、南京、寿县4个站点的PM_(2.5)样品,分析了水溶性离子的组成及其来源,并结合天气形势分析了长江三角洲地区大范围霾天气的形成消散及水溶性离子的时间变化特征.结果表明:观测期间徐州站PM_(2.5)平均质量浓度171.5μg/m~3,远高于其他3个站点,4个站点最主要的离子成分均为NO_3~-,SO_4~(2–),NH_4~+,Cl~-和Ca~(2+).在同一天气系统影响下,长江三角洲大范围区域污染物浓度变化基本一致,在没有大的区域输送的静稳天气下,各站点离子浓度容易受局地源影响,徐州站受燃煤影响,南京站受化学工业源影响为主,2个站点以SO_4~(2–)为主,东山站三面环湖,Cl~-在静稳天气有大幅上升,达到了6.12μg/m~3,寿县站受当地农业活动氨排放影响,NH_4~+有大幅上升,达到了25.09μg/m~3.4个站点PM_(2.5)和水溶性离子质量浓度随时间的变化趋势一致.弱高压的均压场形势下,并伴随有逆温层出现时有利于污染物的累积.主成分分析发现4个站点二次转化对PM_(2.5)有着最大的贡献率,4个站点贡献率分别为39.83%、42.27%、50.56%和38.40%.
PM_(2.5) samples were collected at four cities(Xuzhou,Dongshan,Nanjing and Shouxian)from December 13~(th) 2016 to January 5~(th) 2017 to investigate the composition and source of water-soluble ions in this study.Moreover,the time variation of these ionic species coupled with the local meteorological conditions was analysed to shed light on the haze formation and dissipation mechanism in the Yangtze River Delta Region(YRD).The results revealed that:during the observation period,the average mass concentration of PM_(2.5) in Xuzhou was 171.5μg/m~3,which was much greater than the average mass concentration in the other three sites.The most important ionic components were NO_3~-,SO_4~(2–),NH_4~+,Cl~-and Ca~(2+).The variations of ionic components were due to the combined effects of emissions and weather systems.Under the influence of the same weather system,the pollutant concentration varied consistently in different areas of YRD.Under the static weather condition without obvious regional transport,the ion concentrations were mainly affected by the local sources.Xuzhou was mainly affected by the coal.Nanjing was mainly affected by the chemical industrial source.The major component in both Xuzhou and Nanjing was SO_4~(2–).Dongshan is surrounded by the lake on three sides,and Cl~-increased significantly to 6.12μg/m~3 under the static weather condition.Shouxian was mainly affected by the ammonia emissions of local agricultural activities,and NH_4~+increased significantly to 25.09μg/m~3.The concentration of PM_(2.5) and water-soluble ions of four sites varied with time consistently.When YRD was controlled by the weak high pressure accompanied with the uniform pressure field,this weather pattern was favorable for pollutant accumulation.The principal component analysis indicated that secondary formation had the largest contribution to PM_(2.5) concentration,with the contribution rates of 39.83%,42.27%,50.56% and 38.40% at Xuzhou,Nanjing,Dongshan,Shouxian,respectively.
PM_(2.5) samples were collected at four cities(Xuzhou,Dongshan,Nanjing and Shouxian)from December 13~(th) 2016 to January 5~(th) 2017 to investigate the composition and source of water-soluble ions in this study.Moreover,the time variation of these ionic species coupled with the local meteorological conditions was analysed to shed light on the haze formation and dissipation mechanism in the Yangtze River Delta Region(YRD).The results revealed that:during the observation period,the average mass concentration of PM_(2.5) in Xuzhou was 171.5μg/m~3,which was much greater than the average mass concentration in the other three sites.The most important ionic components were NO_3~-,SO_4~(2–),NH_4~+,Cl~-and Ca~(2+).The variations of ionic components were due to the combined effects of emissions and weather systems.Under the influence of the same weather system,the pollutant concentration varied consistently in different areas of YRD.Under the static weather condition without obvious regional transport,the ion concentrations were mainly affected by the local sources.Xuzhou was mainly affected by the coal.Nanjing was mainly affected by the chemical industrial source.The major component in both Xuzhou and Nanjing was SO_4~(2–).Dongshan is surrounded by the lake on three sides,and Cl~-increased significantly to 6.12μg/m~3 under the static weather condition.Shouxian was mainly affected by the ammonia emissions of local agricultural activities,and NH_4~+increased significantly to 25.09μg/m~3.The concentration of PM_(2.5) and water-soluble ions of four sites varied with time consistently.When YRD was controlled by the weak high pressure accompanied with the uniform pressure field,this weather pattern was favorable for pollutant accumulation.The principal component analysis indicated that secondary formation had the largest contribution to PM_(2.5) concentration,with the contribution rates of 39.83%,42.27%,50.56% and 38.40% at Xuzhou,Nanjing,Dongshan,Shouxian,respectively.
引文
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[28]耿彦红,刘卫,单健,等.上海市大气颗粒物中水溶性离子的粒径分布特征[J].中国环境科学,2010,30(12):1585-1589.Geng Y H,Liu W,Shan J,et al.Characterization of major watersoluble ions in size-fractionated particulate matters in Shanghai[J].China Environmental Science,2010,30(12):1585-1589.
[29]王念飞,陈阳,郝庆菊,等.苏州市PM2.5中水溶性离子的季节变化及来源分析[J].环境科学,2016,37(12):4482-4489.Wang N F,Chen Y,Hao Q J,et al.Seasonal variation and source analysis of the water-soluble inorganic ions in fine particulate matter in Suzhou[J].Environmental Science,2016,37(12):4482-4489.
[30]Aota Y,Kumagai M,Ishikawa K.Over twenty years trend of chloride ion concentration in Lake Biwa[J].Journal of Limnology,2003,62(1s):42-48.
[31]Harrison R M,Msibi M I,Kitto A M N,et al.Atmospheric chemical transformations of nitrogen compounds measured in the northsea experiment,September 1991[J].Atmospheric Environment,1994,28(9):1593-1599.
[2]Calcabrini A,Meschini S,Marra M,et al.Fine environmenta lparticulate engenders alterations in human lung epithelial A549cells[J].Environmental Research,2004,95(1):0-91.
[3]Vedal S.Ambient particles and health:lines that divide[J].Journal of the Air&Waste Management Association,1997,47(5):551-581.
[4]Chow J C,Watson J G,Kuhns H,et al.Source profiles for industrial mobile,and area sources in the big bend regional aerosol visibility and observational study[J].Chemosphere,2004,54(2):0-208.
[5]Monks P S,Granier C,Fuzzi S,et al.Atmosphericcomposition change-global and regional air quality[J].Atmospheric Environment,2009,43(33):5268-5350.
[6]Menon S,Genio A D D,Koch D,et al.GCM simulations of the aerosol indirect effect:Sensitivity to cloud parameterization and aerosol burden[J].Journal of Atmospheric Sciences,2002,59(3):692-713.
[7]Chen R J,Peng R D,Meng X,et al.Seasonal variation in the acute effect of particulate air pollution on mortality in the China Air Pollution and Health Effects Study(CAPES)[J].Science of the Total Environment,2013,450-451(Complete):259-265.
[8]Yao X,Lau A P S,Fang M,et al.Size distributions and formation of ionic species in atmospheric particulate pollutantsin Beijing,China:1-inorganic ions[J].Atmospheric Environment,2003,37(21):2991-3000.
[9]吴烈善,孔德超,孙康,等.香河夏季PM2.5水溶性无机离子组分特征[J].中国环境科学,2015,35(10):2925-2933.Wu L C,Kong D C,Sun K,et al.Characteristics of water-soluble inorganic ions of PM2.5 in summer at Xianghe[J].China Environmental Science,2015,35(10):2925-2933.
[10]蔡阳阳,杨复沫,贺克斌,等.北京城区大气干沉降的水溶性离子特征[J].中国环境科学,2011,31(7):1071-1076.Cai Y Y,Yang F M,He K B,et al.Characteristics of water-soluble ions in dry deposition in urban Beijing[J].China Environmental Science,2011,31(7):1071-1076.
[11]Wang Y,Zhuang G S,Zhang X Y,et al.The ion chemistry,seasonal cycle and sources of PM2.5 and TSP aerosol in Shanghai[J].Atmospheric Environment,2006,40(16):2935-2952.
[12]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.
[13]Tan J H,Duan J C,Chen D H,et al.Chemical characteristics of haze during summer and winter in Guangzhou[J].Atmospheric Research,2009,94(2):0-245.
[14]何俊杰,吴耕晨,张国华,等.广州雾霾期间气溶胶水溶性离子的日变化特征及形成机制[J].中国环境科学,2014,34(5):1107-1112.He J J,Wu K C,Zhang G H,et al.Diurnal variations and formation mechanisms of water-soluble inorganic ions in aerosols during a haze-fog period in Guangzhou[J].China Environmental Science,2014,34(5):1107-1112.
[15]王曼婷,朱彬,王红磊,等.长江三角洲冬季一次霾过程气溶胶及其水溶性离子的区域分布特征[J].环境科学,2015,(7):2337-2345.Wang M T,Zhu B,Wang H L,et al.Composition and regional characteristics of atmosphere aerosol and its water soluble ionsover the Yangtze River Delta Region in a winter haze period[J].Environmental Science,2015,(7):2337-2345.
[16]蒋琳,朱彬,王红磊,等.霾与轻雾天气下水溶性离子的组分特征-冬季长江三角洲地区一次污染过程分析[J].中国环境科学,2017(10):3-12.Jiang L,Zhu bin,Wang H L,et al.Characteristics of water-soluble ions in the haze and mist days in winter in Yangtze River Delta[J].China Environmental Science,2017,(10):3-12.
[17]刀谞,张霖琳,等.京津冀冬季与夏季PM2.5/PM10及其水溶性离子组分区域性污染特征分析[J].环境化学,2015,34(1):60-69.Dao X,Zhang L L,et al.Characteristics of mass and ionic compounds of atmospheric particles in winter and summer of Beijing-TianjinHebei area,China[J].Environmental Chemistry,2015,34(1):60-69.
[18]张宁宁,何元庆,等.丽江市冬季大气总悬浮颗粒物(TSP)中水溶性离子化学特征[J].环境科学,2011,32(3):619-625.Zhang N N,He Y Q,et al.Chemical Characteristic of Water-Soluble Ions in Total Suspended Particles(TSP)at Lijiang Winter Time[J].Environmental Science,2011,32(3):619-625.
[19]吴兑,陈位超,常业谛,等.华南地区大气气溶胶质量谱与水溶性成分谱分布的初步研究[J].热带气象学报,1994,(1):85-96.Wu D,Chen W C,Chang Y D,et al.Preliminary study on thedistribution of atmospheric aerosol mass spectra and water-soluble composition spectra in south China[J].Journal of Tropical Meteorology,1994,(1):85-96.
[20]高山红,刘斌,吴炜.http://222.195.136.24/.Gao S H,Liu B,Wu W.http://222.195.136.24/.
[21]Gao J,Wang T,Zhou X H,et al.Measurement of aerosol number size distributions in the Yangtze River delta in China:formation and growth of particles under polluted conditions[J].Atmospheric Environment,2009,43(4):829-836.
[22]张林静,张秀英,江洪,等.沈阳市降水化学成分及来源分析[J].环境科学,2013,34(6):2081-2088.Zhang L J,Zhang X Y,Jiang H,et al.Chemical characteristicsand source assessment of rainwater at Shenyang[J].Environmental Science,2013,34(6):2081-2088.
[23]郝拉娣,于化东.标准差与标准误[J].编辑学报,2005,17(2):116-118.Hao L D,Yu H D.Standard deviation and standard error of arithmetic mean[J].Acta Editologica,2005,17(2):116-118.
[24]Kato N.Analysis of structure of energy consumption and dynamics of emission of atmospheric species related to the globalenvironmental change(SOx,NOx,and CO2)in Asia[J].Atmospheric Environment,1996,30(5):0-785.
[25]Yao X,Chan C K,Fang M,et al.The water-soluble ionic composition of PM2.5 in Shanghai and Beijing,China[J].Atmospheric Environment,2002,36(26):4223-4234.
[26]Arimoto R,Duce R A,Savoie D L,et al.Relationships among aerosol constituents from Asia and the North Pacific during PEM-West A[J].Journal of Geophysical Research Atmospheres,1996,101(D1):2011-2023.
[27]汤莉莉,汤蕾,花艳,等.苏南三市秋冬季PM2.5中水溶性离子和元素特征及源解析[J].大气科学学报,2015,38(5):686-693.Tang L L,Tang L,Hua Y,et al.Characteristics and source apportionment of water-soluble ions and elements in PM2.5 in three cities of South Jiangsu in autumn and winter[J].Transactions of Atmospheric Sciences,2015,38(5):686-693.
[28]耿彦红,刘卫,单健,等.上海市大气颗粒物中水溶性离子的粒径分布特征[J].中国环境科学,2010,30(12):1585-1589.Geng Y H,Liu W,Shan J,et al.Characterization of major watersoluble ions in size-fractionated particulate matters in Shanghai[J].China Environmental Science,2010,30(12):1585-1589.
[29]王念飞,陈阳,郝庆菊,等.苏州市PM2.5中水溶性离子的季节变化及来源分析[J].环境科学,2016,37(12):4482-4489.Wang N F,Chen Y,Hao Q J,et al.Seasonal variation and source analysis of the water-soluble inorganic ions in fine particulate matter in Suzhou[J].Environmental Science,2016,37(12):4482-4489.
[30]Aota Y,Kumagai M,Ishikawa K.Over twenty years trend of chloride ion concentration in Lake Biwa[J].Journal of Limnology,2003,62(1s):42-48.
[31]Harrison R M,Msibi M I,Kitto A M N,et al.Atmospheric chemical transformations of nitrogen compounds measured in the northsea experiment,September 1991[J].Atmospheric Environment,1994,28(9):1593-1599.