南京市一次霾污染过程中水溶性离子分布特征
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摘要
使用MARGA离子在线分析仪ADI2080对2017年12月27日～2018年1月5日南京市PM_(2.5)化学组分进行连续采样分析,结合气象要素和大气环境监测数据,探讨了霾污染过程中水溶性离子的时间分布特征及其来源特征.结果表明:霾日中南京水溶性离子浓度为121.41μg/m~3,是洁净日的3.2倍.霾污染过程中水溶性离子平均浓度大小顺序为NO_3~-> SO_4~(2-)> NH_4~+> Cl~-> K~+> Ca~(2+)> Mg~(2+),SNA离子占总水溶性离子浓度的91.97%.霾日中水溶性离子日变化均为三峰型,洁净日中Cl~-、SO_4~(2-)和NH_4~+的日变化为单峰型,Ca~(2+)为双峰型,K~+、Mg~(2+)为三峰型.随着空气污染状况的加重,总水溶性离子在PM_(2.5)中的占比不断减少,空气质量为优时占比95.93%,严重污染时为63.25%.霾日中随着污染加重,NH_4~+占总离子的比例稳定在23%左右,SO_4~(2-)占比缓慢减小,NO_3~-占比不断增大.NOR、SOR的日变化在霾日呈双峰型分布,洁净日则较为平稳.观测期间的水溶性离子主要来源有二次转化、煤烟尘、扬尘以及生物质燃烧.
The composition of PM_(2.5) was monitored online continuously by using MARGA 1 S Analyzer ADI 2080 in Nanjing from December 27, 2017 to January 5, 2018. Combined with meteorological elements and atmospheric environmental monitoring data, the time distribution and source characteristics of water-soluble ions in haze pollution process was investigated. The mass concentration of water-soluble ions in Nanjing during the haze pollution was 121.41μg/m~3, 3.2 times of the level in clean days. The order of the average mass concentration of water-soluble ions in the haze pollution process was NO_3~-> SO_4~(2-)> NH_4~+ > Cl~-> K~+ > Ca~(2+) > Mg~(2+).SO_4~(2-), NO_3~- and NH_4~+ accounted for 91.97% of the total water-soluble ions concentration. The diurnal variations of water-soluble ions in haze days were all trimodal, while in clean days, Cl~-, SO_4~(2-)and NH_4~- were unimodal, Ca~(2+) was bimodal, K~+ and Mg~(2+) were trimodal. With the aggravation of the air pollution, the proportion of total water-soluble ions in PM_(2.5) was decreasing. When the air quality was excellent, the proportion was 95.93%, while it was 63.25% when serious pollution occurred. With the increase of pollution in haze days, the proportion of NH_4~+ to total water-soluble ions was stable at around 23%, the proportion of SO_4~(2-)decreased slowly, and the proportion of NO_3~-increased continuously. The diurnal variations of NOR and SOR were bimodal in haze days, while in clear days, they were relatively stable. During the observation period, water-soluble ions were derived mainly from secondary conversion, coal ash, dust, and biomass combustion.
The composition of PM_(2.5) was monitored online continuously by using MARGA 1 S Analyzer ADI 2080 in Nanjing from December 27, 2017 to January 5, 2018. Combined with meteorological elements and atmospheric environmental monitoring data, the time distribution and source characteristics of water-soluble ions in haze pollution process was investigated. The mass concentration of water-soluble ions in Nanjing during the haze pollution was 121.41μg/m~3, 3.2 times of the level in clean days. The order of the average mass concentration of water-soluble ions in the haze pollution process was NO_3~-> SO_4~(2-)> NH_4~+ > Cl~-> K~+ > Ca~(2+) > Mg~(2+).SO_4~(2-), NO_3~- and NH_4~+ accounted for 91.97% of the total water-soluble ions concentration. The diurnal variations of water-soluble ions in haze days were all trimodal, while in clean days, Cl~-, SO_4~(2-)and NH_4~- were unimodal, Ca~(2+) was bimodal, K~+ and Mg~(2+) were trimodal. With the aggravation of the air pollution, the proportion of total water-soluble ions in PM_(2.5) was decreasing. When the air quality was excellent, the proportion was 95.93%, while it was 63.25% when serious pollution occurred. With the increase of pollution in haze days, the proportion of NH_4~+ to total water-soluble ions was stable at around 23%, the proportion of SO_4~(2-)decreased slowly, and the proportion of NO_3~-increased continuously. The diurnal variations of NOR and SOR were bimodal in haze days, while in clear days, they were relatively stable. During the observation period, water-soluble ions were derived mainly from secondary conversion, coal ash, dust, and biomass combustion.
引文
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[19]商嵩,范美益,曹芳,等.基于高分辨率在线气溶胶监测仪数据分析南京北郊冬季PM2.5中水溶性离子污染特性[J].科学技术与工程,2018,18(11):337-342.Gao S, Fan M Y, Cao F, et al. Characteristics and source of water soluble inorganic ions in PM2.5 based on high resolution MARGA data in Nanjing[J]. Science Technology and Engineering, 2018,18(11):337-342.
[20] HJ 663-2013环境空气质量评价技术规范(试行)[S].HJ 663-2013 Technical regulation for ambient air quality assessment(on trial)[S].
[21] Park S S, Ondov J M, Harrison D, et al. Seasonal and shorter-term variations in particulate atmospheric nitrate in Baltimore[J].Atmospheric Environment, 2005,39(11):2011-2020.
[22]周瑶瑶,马嫣,郑军,等.南京北郊冬季霾天PM2.5水溶性离子的污染特征与消光作用研究[J].环境科学,2015,36(6):1926-1934.Zhou Y Y, Ma Y, Zheng J, et al. Pollution characteristics and light extinction effects of water-soluble ions in PM2.5 during winter hazy days at north suburban Nanjing[J]. Environmental Science, 2015,36(6):1926-1934.
[23] Fan S J, Fan Q, Yu W, et al. Atmospheric boundary layer characteristics over the Pearl River Delta, China, during the summer of2006:measurement and model results[J]. Atmospheric Chemistry&Physics, 2011,11(11):6297-6310.
[24] HJ 633-2012环境空气质量指数(AQI)技术规定(试行)[S].HJ 633-2012 Technical regulation on ambient air quality index(on trial)[S].
[25] GB 3095-2012环境空气质量标准[S].GB 3095-2012 Ambient air quality standards[S].
[26]秦阳,朱彬,邹嘉南,等.南京夏秋季节大气干沉降水溶性离子特征及来源分析[J].环境科学,2016,37(6):2025-2033.Qin Y, Zhu B, Zhou J N, et al. Characteristics and source apportionment of water-soluble ions in dry deposition in the summer and autumn of Nanjing[J]. Environmental Science, 2016,37(6):2025-2033.
[27] Matsumoto, K, and Tanaka, H. Formation and dissociation of atmospheric particulate nitrate and chloride:an approach based on phase equilibrium[J]. Atmospheric Environment, 1996,30(4):639-648.
[28]银燕,童尧青,魏玉香,等.南京市大气细颗粒物化学成分分析[J].大气科学学报,2009,32(6):723-733.Yin Y,Dong Y Q,Wei Y X,et al. The analysis of chemistry composition of fine mode particles in Nanjing[J]. Transactions of Atmospheric Sciences, 2009,32(6):723-733.
[29] Kerminen V M, Hillamo R, Teinila K, et al. Ion balances of size-resolved tropospheric aerosol samples:implications for the acidity and atmospheric processing of aerosols[J]. Atmospheric Environment, 2001,35(31):5255-5265.
[30] Gao Y,Arimoto R,Duce R A, et al. Atmospheric non-sea-salt sulfate, nitrate and methanesulfonate over the China Sea[J]. Journal of Geophysical Research Atmospheres,1996,101(D7):12601-12611.
[31]李友平,周洪,张智胜,等.成都市城区PM2.5中二次水溶性无机离子污染特征[J].环境科学,2014,35(12):4439-4445.Li Y R,Zhou H, Zhang Z S, et al. Pollution characteristics of secondary water-soluble inorganic ions of PM2.5 in urban Chengdu,China[J]. Environmental Science,2014,35(12):4439-4445.
[32]段卿.南京北郊大气气溶胶化学组分特征分析[D].南京:南京信息工程大学,2015.Duan Q. The Analysis of aerosol chemical composition characteristics in nanjing northern suburb[D]. Nanjing:Nanjing University of Information Science&Technology, 2015.
[33] 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.
[2]唐孝炎,张远航,邵敏.大气环境化学[M].北京:高等教育出版社,2006:1-739.Tang X Y,Zhang Y H, Shao M. Atmospheric Environmental Chemistry[M]. Beijing:Higher Education Press, 2006:1-739.
[3] Zhang T, Cao J J, Tie X X, et al. Water-soluble ions in atmospheric aerosols measured in Xi'an, China:Seasonal variations and sources[J].Atmospheric Research, 2011,102(1):11 0-119.
[4]薛国强.南京及周边城市气溶胶质量浓度及其水溶性离子和元素特征分析[D].南京:南京信息工程大学,2014.Xue G Q. Characterization of water soluble ions and elements of aerosol in Nanjing and cities arrounding[D]. Nanjing:Nanjing University of Information Science&Technology, 2014.
[5]张秋晨,朱彬,龚佃利.南京地区大气气溶胶及水溶性无机离子特征分析[J].中国环境科学,2014,34(2):311-316.Zhang Q C, Zhu B, Gong D L. Characterization of water-soluble ion species of aerosol in Nanjing, China[J]. China Environmental Science,2014,34(2):31 1-316.
[6]陈静,杨鹏,韩军彩,等.基于高分辨率MARGA数据分析石家庄PM2.5成分谱特征[J].中国环境科学,2015,35(9):2594-2604.Chen J, Yang P, Han J C, et al. Analysis of PM2.5 spectrum characteristics in Shijiazhuang based on high resolution MARGA data[J]. China Environmental Science, 2015,35(9):2594-2604.
[7] Yao X H, 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):4223-42.
[8]薛国强,朱彬,王红磊.南京市大气颗粒物中水溶性离子的粒径分布和来源解析[J].环境科学,2014,35(5):1633-1643.Xue G Q, Zhu B,Wang H L. Size distribution and source apportionment of soluble ions in aerosol in Nanjing[J]. Environmental Science,2014,35(5):1633-1643.
[9]张蕾,姬亚芹,王士宝,等.盘锦市冬季PM2.5水溶性离子特征及来源分析[J].环境科学,2018,39(6):2521-2527.Zhang L, Ji Y Q, Wang S B, et al. Characteristics and source apportionment of water-soluble ions in PM2.5 during winter in Panjin[J]. Environmental Science, 2018,39(6):2521-2527.
[10]王曼婷,朱彬,王红磊,等.长三角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,2015,36(7):2337-2345.Wang M T, Zhu B, Wang H L,et al. Composition and regional characteristics of atmosphere aerosol and its water soluble ions over the Yangtze River Delta Region in a winter haze period[J].Environmental Science,2015,36(7):2337-2345.
[11]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,2017,37(10):360 1-3610.Jiang L, Zhu B, 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, 2017,37(10):3601-3610.
[12]张程,于兴娜,安俊琳,等.南京北郊不同大气污染程度下气溶胶化学组分特征[J].环境科学,2017,38(12):4932-4942.Zhang C, Yu X N, An J L, et al. Aerosol chemical characteristics for different air pollution levels in north suburban Nanjing[J].Environmental Science, 2017,38(12):4932-4942.
[13] Wang H L, Zhu B, Shen L J, et al. 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, 2015,123:370-379.
[14] Wang H L,An J L,Cheng M T,et al. One year online measurements of water-soluble ions at the industrially polluted town of Nanjing, China:Sources, seasonal and diurnal variations[J]. Chemosphere, 2016,148:526-536.
[15] Liu Z R,Gao W K,Yu Y C,et al. Characteristics of PM2.5 mass concentrations and chemical species in urban and background areas of China:emerging results from the CARE-China network[J].Atmospheric Chemistry&Physics, 2018,18(12):1-34.
[16]王红磊,沈利娟,晶升,等.长三角一次重污染事件中气溶胶粒径谱及水溶性离子分布特征[J].三峡生态环境监测,2018,3(2):34-47.Wang H L, Shen L J, Lv S, et al. Distribution characteristics of aerosol size and water-soluble ions during a heavy pollution event in Yangtze River Delta[J]. Ecology and Environmental Monitoring of Three Gorges, 2018,3(2):34-47.
[17] Makkonen U, Virkkula A, Mantykentta J, et al. Semi-continuous gas and inorganic aerosol measurements at a Finnish urban site:comparisons with filters, nitrogen in aerosol and gas phases, and aerosol acidity[J]. Atmospheric Chemistry and Physics, 2012,12(272).
[18]廖碧婷,吴兑,常越,等.广州地区SO4-2-、NO3-、NH4+与相关气体污染特征研究[J].环境科学学报,2014,34(6):1551-1559.Liao B T, Wu D, Chang Y, et al. Characteristics of particulate SO42,NO3-, NH4+and related gaseous pollutants in Guangzhou[J]. Acta Scientiae Cireumstantiae,2014,34(6):1551-1559.
[19]商嵩,范美益,曹芳,等.基于高分辨率在线气溶胶监测仪数据分析南京北郊冬季PM2.5中水溶性离子污染特性[J].科学技术与工程,2018,18(11):337-342.Gao S, Fan M Y, Cao F, et al. Characteristics and source of water soluble inorganic ions in PM2.5 based on high resolution MARGA data in Nanjing[J]. Science Technology and Engineering, 2018,18(11):337-342.
[20] HJ 663-2013环境空气质量评价技术规范(试行)[S].HJ 663-2013 Technical regulation for ambient air quality assessment(on trial)[S].
[21] Park S S, Ondov J M, Harrison D, et al. Seasonal and shorter-term variations in particulate atmospheric nitrate in Baltimore[J].Atmospheric Environment, 2005,39(11):2011-2020.
[22]周瑶瑶,马嫣,郑军,等.南京北郊冬季霾天PM2.5水溶性离子的污染特征与消光作用研究[J].环境科学,2015,36(6):1926-1934.Zhou Y Y, Ma Y, Zheng J, et al. Pollution characteristics and light extinction effects of water-soluble ions in PM2.5 during winter hazy days at north suburban Nanjing[J]. Environmental Science, 2015,36(6):1926-1934.
[23] Fan S J, Fan Q, Yu W, et al. Atmospheric boundary layer characteristics over the Pearl River Delta, China, during the summer of2006:measurement and model results[J]. Atmospheric Chemistry&Physics, 2011,11(11):6297-6310.
[24] HJ 633-2012环境空气质量指数(AQI)技术规定(试行)[S].HJ 633-2012 Technical regulation on ambient air quality index(on trial)[S].
[25] GB 3095-2012环境空气质量标准[S].GB 3095-2012 Ambient air quality standards[S].
[26]秦阳,朱彬,邹嘉南,等.南京夏秋季节大气干沉降水溶性离子特征及来源分析[J].环境科学,2016,37(6):2025-2033.Qin Y, Zhu B, Zhou J N, et al. Characteristics and source apportionment of water-soluble ions in dry deposition in the summer and autumn of Nanjing[J]. Environmental Science, 2016,37(6):2025-2033.
[27] Matsumoto, K, and Tanaka, H. Formation and dissociation of atmospheric particulate nitrate and chloride:an approach based on phase equilibrium[J]. Atmospheric Environment, 1996,30(4):639-648.
[28]银燕,童尧青,魏玉香,等.南京市大气细颗粒物化学成分分析[J].大气科学学报,2009,32(6):723-733.Yin Y,Dong Y Q,Wei Y X,et al. The analysis of chemistry composition of fine mode particles in Nanjing[J]. Transactions of Atmospheric Sciences, 2009,32(6):723-733.
[29] Kerminen V M, Hillamo R, Teinila K, et al. Ion balances of size-resolved tropospheric aerosol samples:implications for the acidity and atmospheric processing of aerosols[J]. Atmospheric Environment, 2001,35(31):5255-5265.
[30] Gao Y,Arimoto R,Duce R A, et al. Atmospheric non-sea-salt sulfate, nitrate and methanesulfonate over the China Sea[J]. Journal of Geophysical Research Atmospheres,1996,101(D7):12601-12611.
[31]李友平,周洪,张智胜,等.成都市城区PM2.5中二次水溶性无机离子污染特征[J].环境科学,2014,35(12):4439-4445.Li Y R,Zhou H, Zhang Z S, et al. Pollution characteristics of secondary water-soluble inorganic ions of PM2.5 in urban Chengdu,China[J]. Environmental Science,2014,35(12):4439-4445.
[32]段卿.南京北郊大气气溶胶化学组分特征分析[D].南京:南京信息工程大学,2015.Duan Q. The Analysis of aerosol chemical composition characteristics in nanjing northern suburb[D]. Nanjing:Nanjing University of Information Science&Technology, 2015.
[33] 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.
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