武汉市PM_(2.5)中二元羧酸的污染特征及来源解析
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摘要
在武汉市工业区和交通区展开了PM_(2.5)样品采集,研究了PM_(2.5)中二元羧酸的化学组成、污染水平及来源。二元羧酸在工业区为103.1～2 219.2ng/m~3,年平均值为958.4ng/m~3;在交通区为66.9～2 176.8ng/m~3,年平均值为749.7ng/m~3。丙二酸/丁二酸(C_3/C_4,质量比,下同)表明,武汉市二元羧酸主要来自机动车尾气排放;己二酸/壬二酸(C_6/C_9)表明,二元羧酸的人为源贡献大于自然源。正定矩阵因子分解(PMF)模型解析结果显示,工业区中二次源占13.7%,建筑扬尘占23.1%,机动车尾气排放占37.0%,生物质燃烧占26.2%;交通区中二次源占8.9%,建筑扬尘占24.9%,机动车尾气排放占51.8%,生物质燃烧占14.4%。潜在源区贡献因子(PSCF)分析得出,武汉市夏季二元羧酸主要受到南部季风的影响,冬季主要受到西部冷空气的影响。
PM_(2.5) samples were collected in an industrial area and a traffic area to investigate the composition,concentration and source of dicarboxylic acids in PM_(2.5).The mass concentration of dicarboxylic acids in industry area was 103.1-2 219.2 ng/m~3,with the annual average of 958.4 ng/m~3,while the mass concentration in traffic area was 66.9-2 176.8 ng/m~3,with the annual average of 749.7 ng/m~3.Malonate/succinic acid(C_3/C_4,mass ratio,the same below)showed that the dicarboxylic acids in Wuhan were mainly derived from the influence of motor vehicle emissions,and adipic acid/azelaic acid(C_6/C_9)indicated that the anthropogenic contribution of dicarboxylic acids was greater than that of natural source.The results of positive matrix factorization(PMF)model showed that the secondary sources accounted for 13.7%in the industrial area,dust for 23.1%,motor vehicle emissions for 37.0%,and biomass combustion for 26.2%.Secondary sources accounted for 8.9% in the traffic area,dust for 24.9%,motor vehicle emissions for 51.8%,and biomass combustion for 14.4%.The analysis of the potential source contribution function(PSCF)suggested that the dicarboxylic acids in Wuhan were mainly affected by the southern monsoon in summer,and cold air from the west in winter.
PM_(2.5) samples were collected in an industrial area and a traffic area to investigate the composition,concentration and source of dicarboxylic acids in PM_(2.5).The mass concentration of dicarboxylic acids in industry area was 103.1-2 219.2 ng/m~3,with the annual average of 958.4 ng/m~3,while the mass concentration in traffic area was 66.9-2 176.8 ng/m~3,with the annual average of 749.7 ng/m~3.Malonate/succinic acid(C_3/C_4,mass ratio,the same below)showed that the dicarboxylic acids in Wuhan were mainly derived from the influence of motor vehicle emissions,and adipic acid/azelaic acid(C_6/C_9)indicated that the anthropogenic contribution of dicarboxylic acids was greater than that of natural source.The results of positive matrix factorization(PMF)model showed that the secondary sources accounted for 13.7%in the industrial area,dust for 23.1%,motor vehicle emissions for 37.0%,and biomass combustion for 26.2%.Secondary sources accounted for 8.9% in the traffic area,dust for 24.9%,motor vehicle emissions for 51.8%,and biomass combustion for 14.4%.The analysis of the potential source contribution function(PSCF)suggested that the dicarboxylic acids in Wuhan were mainly affected by the southern monsoon in summer,and cold air from the west in winter.
引文
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[2]BHATTU D,TRIPATHI S N.CCN closure study:effects of aerosol chemical composition and mixing state[J].Journal of Geophysical Research:Atmospheres,2015,120(2):766-783.
[3]NARUKAWA M,KAWAMURA K,HATSUSHIKA H,et al.Measurement of halogenated dicarboxylic acids in the arctic aerosols at polar sunrise[J].Journal of Atmospheric Chemistry,2003,44(3).
[4]NARUKAWA M,KAWAMURA K,TAKEUCHI K,et al.Distribution of dicarboxylic acids and carbon isotopic compositions in aerosols from 1997Indonesian forest fires[J].Geophysical Research Letters,1999,26(20):3101-3104.
[5]FU P Q,KAWAMURA K,CHENG Y F,et al.Aircraft measurements of polar organic tracer compounds in tropospheric particles(PM10)over central China[J].Atmospheric Chemistry and Physics,2014,14(8):4185-4199.
[6]WU S,SCHWAB J,LIU B,et al.Seasonal variations and source identification of selected organic acids associated with PM10in the coastal area of Southeastern China[J].Atmospheric Research,2015,155:37-51.
[7]成春雷,王格慧,李建军.西安市大气中二元羧酸有机气溶胶组成及来源[J].中国环境科学,2012,32(7):1159-1164.
[8]HSIEH L,CHEN C,WAN M,et al.Speciation and temporal characterization of dicarboxylic acids in PM2.5during a PM episode and a period of non-episodic pollution[J].Atmospheric Environment,2008,42(28):6836-6850.
[9]HEGDE P,KAWAMURA K.Seasonal variations of water-soluble organic carbon,dicarboxylic acids,ketocarboxylic acids,andα-dicarbonyls in the central Himalayan aerosols[J].Atmospheric Chemistry and Physics,2012,12(1):935-982.
[10]CARLTON A G,TURPIN B J,ALTIERI K E,et al.Atmospheric oxalic acid and SOA production from glyoxal:results of aqueous photooxidation experiments[J].Atmospheric Environment,2007,41(35):7588-7602.
[11]WANG H,KAWAMURA K.Stable carbon isotopic composition of low molecular weight dicarboxylic acids and ketoacids in remote marine aerosols[J].Journal of Geophysical Research,2006,111(7):2814-2829.
[12]VAN P D,NEUSUB C,HERRMMAN H.On the abundance and source contributions of dicarboxylic acids in size-resolved aerosol particles at continental sites in central Europe[J].Atmospheric Chemistry and Physics,2014,14(8):3913-3928.
[13]郭浩天,周家斌,余文洋,等.武汉市大气PM2.5中有机酸的季节变化及其来源解析[J].环境科学与技术,2014,37(4):90-95.
[14]JIANG Y,HOU X,ZHUANG G,et al.The sources and seasonal variations of organic compounds in PM2.5in Beijing and Shanghai[J].Journal of Atmospheric Chemistry,2009,62(3):175-192.
[15]MIYAZAKI Y,FU P,ONO K,et al.Seasonal cycles of watersoluble organic nitrogen aerosols in a deciduous broad leaf forest in northern Japan[J].Journal of Geophysical Research:Atmospheres,2014,119(3):1440-1454.
[16]孟静静,侯战方,张二勋,等.黄山PM10中二元羧酸类化合物的季节变化特征及其来源[J].环境科学,2017,38(7):2688-2697.
[17]史国良,陈刚,田瑛泽,等.天津大气PM2.5中碳组分特征和来源分析[J].环境污染与防治,2016,38(1):1-7.
[18]HAFNER W D,HITES R A.Potential sources of pesticides,PCBs,and PAHs to the atmosphere of the Great Lakes[J].Environmental Science&Technology,2003,37(17):3764-3773.
[19]YU S,ZHANG Q,YAN R,et al.Origin of air pollution during a weekly heavy haze episode in Hangzhou,China[J].Environmental Chemistry Letters,2014,12(4):543-550.
[20]周家斌,钱佳,祁士华,等.武汉春季大气PM10浓度及有机组成变化特征[J].环境污染与防治,2009,31(10):100-104.
[21]KUO S,TSAI Y I,TSAI C,et al.Carboxylic acids in PM2.5over Pinus morrisonicola forest and related photoreaction mechanisms identified via Raman spectroscopy[J].Atmospheric Environment,2011,45(37):6741-6750.
[22]CAO J J,ZHU C S,TIE X X,et al.Characteristics and sources of carbonaceous aerosols from Shanghai,China[J].Atmospheric Chemistry and Physics,2013,13(2):803-817.
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