武汉市大气PM_(2.5)中水溶性离子污染特征及来源
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摘要
于2016年8月—2017年4月采集了武汉市PM2.5样品,使用离子色谱法分析了PM2.5中的水溶性离子(F-、Cl-、SO2-4、NO-3、Na+、NH+4、K+、Mg2+、Ca2+),并研究其污染特征及来源.结果表明,武汉市PM2.5质量浓度变化范围为24.8～215.7μg·m-3,均值为(81.3±38.1)μg·m-3.9种水溶性离子的年均质量浓度占PM2.5质量浓度的29.3%,其中,SO2-4、NO-3、NH+4(三者合称SNA)为主要的水溶性离子,SNA占PM2.5质量浓度的23.3%～32.0%.硫氧化率(SOR)和氮氧化率(NOR)年均值分别为0.4、0.1,说明武汉市大气存在较强的SO2向SO2-4、NO2向NO-3转化的二次过程.观测期间,武汉市的细颗粒物整体呈弱碱性.Ca2+与Mg2+,以及NH+4与NO-3、SO2-4等均有显著相关性,NH+4、NO-3、SO2-4主要以(NH4)2SO4和NH4NO3的形式存在.武汉市全年NO-3/SO2-4比值为0.9,表明固定源贡献相对较大.主成分分析结果表明,武汉市大气PM2.5中水溶性离子主要来自于燃煤及机动车排放、工业生产、扬尘等.
Daily samples of atmospheric PM2.5 were collected from August 2016 to April 2017 in Wuhan,China. The characteristics and sources of the main water-soluble ions( F-,Cl-,SO2-4,NO-3,Na+,NH+4,K+,Mg2+,and Ca2+) in PM2.5 were analyzed by using ion chromatography. The results showed that the mass concentration of PM2.5 ranged from 24.8 to 215.7 μg·m-3 with mean value of( 81.3±38.1) μg·m-3. On average,the total ions accounted for 29.3% of PM2.5 mass. SO2-4、NO-3、NH+4( SNA) was the dominant components of the water-soluble ions in PM2.5,SNA accounted for 23.3% ～32.0% of PM2.5 mass. The mean values of SOR and NOR were 0.4 and 0.1,respectively,indicating that there was a strong secondary process of SO2 to SO2-4 and NO2 to NO-3. PM2.5 samples were alkaline in Wuhan City. The correlation between Ca2+and Mg2+,NH+4 and SO2-4,NH+4 and NO-3 were significant. NH+4,SO2-4 and NO-3 were probably existed in the form of( NH4)2 SO4 and NH4 NO3. In addition,the average ratio of NO-3/SO2-4 is 0.9 in PM2.5,indicating that the stationary source were relatively important as compared to mobile sources. The result of PCA indicated that coal combustion,vehicle emission,industrial production and dust were major contributors to the water-soluble ions of PM2.5 in Wuhan.
Daily samples of atmospheric PM2.5 were collected from August 2016 to April 2017 in Wuhan,China. The characteristics and sources of the main water-soluble ions( F-,Cl-,SO2-4,NO-3,Na+,NH+4,K+,Mg2+,and Ca2+) in PM2.5 were analyzed by using ion chromatography. The results showed that the mass concentration of PM2.5 ranged from 24.8 to 215.7 μg·m-3 with mean value of( 81.3±38.1) μg·m-3. On average,the total ions accounted for 29.3% of PM2.5 mass. SO2-4、NO-3、NH+4( SNA) was the dominant components of the water-soluble ions in PM2.5,SNA accounted for 23.3% ～32.0% of PM2.5 mass. The mean values of SOR and NOR were 0.4 and 0.1,respectively,indicating that there was a strong secondary process of SO2 to SO2-4 and NO2 to NO-3. PM2.5 samples were alkaline in Wuhan City. The correlation between Ca2+and Mg2+,NH+4 and SO2-4,NH+4 and NO-3 were significant. NH+4,SO2-4 and NO-3 were probably existed in the form of( NH4)2 SO4 and NH4 NO3. In addition,the average ratio of NO-3/SO2-4 is 0.9 in PM2.5,indicating that the stationary source were relatively important as compared to mobile sources. The result of PCA indicated that coal combustion,vehicle emission,industrial production and dust were major contributors to the water-soluble ions of PM2.5 in Wuhan.
引文
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Zhang R,Tao J,Hsu S C,et al.2013.Chemical characterization and source apportionment of PM2.5 in Beijing: seasonal perspective [J].Atmospheric Chemistry & Physics,13(14):7053-7074
Zhao P S,Dong F,He D,et al.2013.Characteristics of concentrations and chemical compositions for PM2.5 in the region of Beijing,Tianjin and Hebei,China[J].Atmospheric Chemistry and Physics,13(9):4631-4644
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张帆,成海容,王祖武,等.2012.武汉大气PM2.5中微量元素的污染特征和来源分析[J].武汉大学学报(工学版),45(6):757-761
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Contini D,Genga A,Cesari D,et al.2010.Characterization and source apportionment of PM10 in an urban background site in Lecce[J].Atmospheric Research,95:40-54
曹军骥.2014.PM2.5与环境[M].北京:科学出版社.67-154
成海容,王祖武,冯家良,等.2012.武汉市城区大气PM2.5的碳组分与源解析[J].生态环境学报,21(9):1574-1579
戴永立,陶俊,林泽健,等.2013.2006—2009 年我国超大城市霾天气特征及影响因子分析[J].环境科学,34(8):2925-2932
Dai Q L,Bi X H,Liu B S,et al.2018.Chemical nature of PM2.5 and PM10 in Xi′an,China: Insights into primary emissions and secondary particle formation[J].Environmental Pollution,240:155
Fang Y,Naik V,Horowitz L W,et al.2013.Air pollution and associated human mortality: the role of air pollutant emissions,climate change and methane concentration increases from the preindustrial period to present[J].Atmospheric Chemistry and Physics,13(3):1377-1394
Hassanvand M S,Naddafi K,Faridi S,et al.2014.Indoor/outdoor relationships of PM10,PM2.5,and PM1 mass concentrations and their water-soluble ions in a retirement home and a school dormitory [J].Atmospheric Environment,82(1):375-382
Heo J B,Hopke P,Yi S M.2009.Source apportionment of PM2.5 in seoul,Korea[J].Atmospheric Chemistry Physics,9: 4957-4971
Ho K F,Lee S C,Chak K C,et al.2003.Characterization of chemical species in PM2.5 and PM10 aerosols in Hong Kong[J].Atmospheric Environment,37(1): 31-39
Hu M,Wu Z J,Slanina J,et al.2008.Acidic gases,ammonia and water-soluble ions in PM2.5 at a coastal site in the Pearl River Delta,China[J].Atmospheric Environment,42(25):6310-6320
Huang D S,Xu J H,Zhang S Q.2012.Valuing the health risks of particulate air pollution in the Pearl River Delta,China[J].Environmental Science & Policy,15(1): 38-47
Iii C A P,Burnett R T,Thun M J,et al.2002.Lung cancer,cardiopulmonary mortality,and long-term exposure to fine particulate air pollution[J].Journal of the American Medical Association,287(9):1132-1141
Tao J,Shen Z X,Zhu C S,et al.2012.Seasonal variations and chemical characteristics of sub-micrometer particles (PM1) in Guangzhou,China[J].Atmospheric Research,118(3):222-231
Kaneyasu N,Yoshikado H,Mizuno T,et al.1999.Chemical forms and sources of extremely high nitrate and chloride in winter aerosol pollution in the Kanto Plain of Japan[J].Atmospheric Environment,33(11):1745-1756
Kang C,Lee H S,Kang B,et al.2004.Chemical characteristics of acidic gas pollutants and PM2.5 species during hazy episodes in Seoul,South Korea[J].Atmospheric Environment,38(28):4749-4760
Kerminen V,Hillamo R,Teinil K,et al.2001.Ion balances of size-resolved tropospheric aerosol samples: implications for the acidity and atmospheric processing of aerosols[J].Atmospheric Environment,35(31): 5255-5265
Larsen R K Ⅲ,Baker J E.2003.Source apportionment of polycyclic aromatic hydrocarbons in the urban atmosphere: a comparison of three methods[J].Envirnment Science & Technology,37(9):1873-1881
李莉,安静宇,严茹莎.2015.基于细颗粒物来源追踪技术的2013年12月上海市严重污染过程的PM2.5的源贡献分析[J].环境科学,36(10): 3543-3553
林瑜,叶芝祥,杨怀金,等.2017.成都市中心城区大气PM1的污染特征及来源解析[J].中国环境科学,37(9):3220-3226
Liu B S,Wu J H,Zhang J Y,et al.2017.Characterization and source apportionment of PM2.5,based on error estimation from EPA PMF 5.0 model at a medium city in China[J].Environmental Pollution,222:10-22
Liu X G,Sun K,Qu Y,et al.2015.Secondary formation of sulfate andnitrate during a haze episode in megacity Beijing,China[J].Aerosol and Air Quality Research,15(6S):2246-2257
孟琛琛,王丽涛,张芬芬,等.2015.邯郸市 PM2.5中水溶性无机离子污染特征及来源解析[J].环境科学学报,35(11):3443-3451
Mukerjee S,Shadwickb D S,Smith L A,et al.2001.Techniques to assess cross-border air pollution and application to a US-Mexico border region[J].Science of the Total Environment,276(1/3):205-224
Pernigotti D,Belis C A,Spanò L.2016.SPECIEUROPE: The European data base for PM source profiles[J].Atmospheric Pollution Research,7(2):307-314
邱婷,周家斌,肖经汗,等.2015.武汉市秋冬季大气PM2.5中水溶性离子污染特征及来源分析[J].环境污染与防治,37(4):17-20
Russell A G,Mcrae G J,Cass G R.1983.Mathematical modeling of the formation and transport of ammonium nitrate aerosol[J].Atmospheric Environment,17(5):949-964
Shen Z X,Cao J J,Arimoto,R,et al.2009.Ionic composition of TSP and PM2.5 during dust storms and air pollution episodes at Xi′an,China[J].Atmospheric Environment,43(18):2911-2918
Song C,He J,Wu L,et al.2017.Health burden attributable to ambient PM2.5 in China[J].Environmental Pollution,223:575-586
Sun Y L,Wang Z F,Fu P Q,et al.2013.The impact of relativehumidity on aerosol composition and evolution processes during wintertime in Beijing,China[J].Atmospheric Environment,77:927-934
孙韧,张文具,董海燕,等.2014.天津市PM10和PM2.5中水溶性离子化学特征及来源分析[J].中国环境监测,30(2):145-150
滕加泉,程钟,梁丹妮,等.2016.常州市大气PM2.5中水溶性离子组成及来源[J].长江流域资源与环境,25(9):1368-1374
Tau S N,Tarulescu S,Idomir M,et al.2008.Respiratory exposure to air pollutants[J].Journal of Environmental Protection & Ecology,9(1):15-25
Tian M,Wang H B,Chen Y,et al.2016.Characteristics of aerosol pollution during heavy haze events in Suzhou,China [J].Atmospheric Chemistry and Physics,16(11):7357-7371
Voutsa D,Samara C,Manoli E,et al.2014.Ionic composition of PM2.5 at urban sites of northern Greece:secondary inorganic aerosol formation[J].Environmental Science & Pollution Research,21(7):4995
Wang G H,Wang H,Yu Y J,et al.2003.Chemical characterization of water-soluble components of PM10 and PM2.5 atmospheric aerosols in five locations of Nanjing,China[J].Atmospheric Environment,37:2893-2902
Wang H L,Zhu B,Shen L J,et al.2015.Water-soluble ions in atmospheric aerosols measured in five sites in the Yangtze River Delta,China: size-fractionated,seasonal variations and sources[J].Atmospheric Environment,123:370-379
Wang Y,Zhuang G S,Zhang X Y,et al.2006.The ion chemistry,seasonal cycle,and sources of PM2.5 and TSP aerosol in Shanghai[J].Atmospheric Environment,40(16):2935-2952
王明毅,吴洪波.2016.武汉城区春节PM2.5中水溶性无机离子污染特征[J].环境科学与技术,39(6):80-85
王念飞,陈阳,郝庆菊,等.2016.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,37(12):4482-4489
吴丹,蔺少龙,杨焕强,等.2017.杭州市PM2.5中水溶性离子的污染特征及其消光贡献[J].环境科学,38(7):2656-2666
Xu L L,Chen X Q,Chen J S,et al.2012.Seasonal variations and chemical compositions of PM2.5 aerosol in the urban area of Fuzhou,China[J].Atmospheric Research,104-105:264-272
杨懂艳,刘保献,张大伟,等.2015.2012—2013 年间北京市PM2.5中水溶性离子时空分布规律及相关性分析[J].环境科学,36(3):768-773
杨起超,曾立民,唐静玥,等.2014.无锡冬季和春季大气中细粒子化学组分及其特性分析[J].环境化学,33(9):1501-1513
Yao X H,Fang M,Chan C K.2003.The size dependence of chloride depletion in fine and coarse sea-salt particles[J].Atmospheric Environment,37(6):743-751
Zhang L,Vet R,Wiebe A,et al.2008.Characterization of the size-segregated water-soluble inorganic ions at eight Canadian rural sites[J].Atmospheric Chemistry& Physics,8(23):7133-7151
Zhang R,Tao J,Hsu S C,et al.2013.Chemical characterization and source apportionment of PM2.5 in Beijing: seasonal perspective [J].Atmospheric Chemistry & Physics,13(14):7053-7074
Zhao P S,Dong F,He D,et al.2013.Characteristics of concentrations and chemical compositions for PM2.5 in the region of Beijing,Tianjin and Hebei,China[J].Atmospheric Chemistry and Physics,13(9):4631-4644
张丹,翟崇治,周志恩,等.2012.重庆市主城区不同粒径颗粒物水溶性无机组分特征[J].环境科学研究,25(10):1099-1106
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