成都市PM_(10)中碳质气溶胶长期来源特点
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摘要
大气颗粒物中包含多种组分的气溶胶,其中碳质气溶胶由于对人体健康、能见度有较大影响,已受到越来越多的关注.为研究碳质气溶胶的长期变化规律,采集了成都市2009—2013年的PM_(10)样品,对其中所含的无机元素、水溶性离子及碳组分分别进行测定,并使用"PMF(正定矩阵因子分解法)-比值"模型分别对PM_(10)和所含的碳质气溶胶的来源进行分析.结果表明,1月、2月、5月和12月的碳质气溶胶浓度较高,其中1月、2月和12月的OC/EC(有机碳与元素碳质量浓度之比)较高,并且PMF-比值模型计算结果也显示冬季SOC增多,表明冬季可能有更多的二次有机碳(SOC)生成;5月的char-EC/soot-EC(二者质量浓度之比,其中char-EC=EC1-OP,soot-EC=EC2+EC3,它们可更好地区分源类)较高,K含量也较高,表明可能有更多的生物质燃烧排放.PM_(10)解析共发现6类源,依次为地壳扬尘(26.5%)、二次硫酸盐(25.1%)、燃煤&生物质燃烧混合源(17.3%)、二次硝酸盐&二次有机碳混合源(12.3%)、机动车源(11.8%)和水泥尘源(7.0%);碳质气溶胶解析发现,OC主要来源依次为机动车源(38.2%)、燃煤&生物质燃烧混合源(33.1%)和二次有机碳(25.3%),char-EC的主要来源是燃煤&生物质燃烧混合源和机动车源,分别占50.5%和45.4%,soot-EC则主要受机动车影响(达73.2%).研究显示,成都市PM_(10)主要来自于地壳扬尘、二次生成和燃煤&生物质燃烧,而碳质气溶胶主要来自于机动车、燃煤&生物质燃烧.
Atmospheric particulate matter is comprised of a variety of components. Due to the large proportion and the influence on human health and visibility,the carbonaceous aerosol has attracted much attention. For the research on the long-term variation of carbonaceous aerosol,PM_(10) samples were collected during 2009-2013 in Chengdu City. The inorganic elements,water-soluble ions and carbon composition were determined. Moreover,PMF-ratio model is applied to quantify the sources of PM_(10) and carbonaceous aerosol. Results present that concentration of carbonaceous fractions shows it highest value in winter and May. OC/EC ratio is higher in winter and the modeled results show that SOC increased in winter,which might indicate more secondary carbon( SOC) in winter. Furthermore,char-EC/soot-EC and K concentration is higher in May,which may illustrate more biomass combustion in May. Six source categories are identified,including crust dust( 26. 5%),the secondary sulfate( 25. 1%),coal combustion & straw burning( 17. 3%),secondary nitrate & the secondary organic carbon( 12. 3%),vehicle exhaust( 11. 8%),cement dust( 7. 0%). Major contributors to OC in PM_(10) are vehicular exhaust( 38. 2%),coal combustion & straw burning( 33. 1%) and SOC( 25. 3%). The coal combustion & biomass combustion and vehicle exhaustcontributed 50. 5% and 45. 4% of char-EC. Vehicle exhaust dominates soot-EC( 73. 2%) in PM_(10). PM_(10) mainly comes from the crust dust,secondary sulfate,coal combustion & straw burning. The carbonaceous aerosol mainly comes from the vehicle exhaust and coal combustion & straw burning.
Atmospheric particulate matter is comprised of a variety of components. Due to the large proportion and the influence on human health and visibility,the carbonaceous aerosol has attracted much attention. For the research on the long-term variation of carbonaceous aerosol,PM_(10) samples were collected during 2009-2013 in Chengdu City. The inorganic elements,water-soluble ions and carbon composition were determined. Moreover,PMF-ratio model is applied to quantify the sources of PM_(10) and carbonaceous aerosol. Results present that concentration of carbonaceous fractions shows it highest value in winter and May. OC/EC ratio is higher in winter and the modeled results show that SOC increased in winter,which might indicate more secondary carbon( SOC) in winter. Furthermore,char-EC/soot-EC and K concentration is higher in May,which may illustrate more biomass combustion in May. Six source categories are identified,including crust dust( 26. 5%),the secondary sulfate( 25. 1%),coal combustion & straw burning( 17. 3%),secondary nitrate & the secondary organic carbon( 12. 3%),vehicle exhaust( 11. 8%),cement dust( 7. 0%). Major contributors to OC in PM_(10) are vehicular exhaust( 38. 2%),coal combustion & straw burning( 33. 1%) and SOC( 25. 3%). The coal combustion & biomass combustion and vehicle exhaustcontributed 50. 5% and 45. 4% of char-EC. Vehicle exhaust dominates soot-EC( 73. 2%) in PM_(10). PM_(10) mainly comes from the crust dust,secondary sulfate,coal combustion & straw burning. The carbonaceous aerosol mainly comes from the vehicle exhaust and coal combustion & straw burning.
引文
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[27]刘贵荣.基于比值法的源解析技术研究[D].天津:南开大学,2015.
[28]YANG Fumo,TAN Jihua,ZHAO Qingquan,et al.Characteristics of PM2.5speciation in representative megacities and across China[J].Atmospheric Chemistry and Physics,2011,11:5207-5219.
[29]TIAN Yingze,SHI Guoliang,Huangfu Yanqi,et al.Seasonal and regional variations of source contributions for PM10and PM2.5in urban environment[J].Science of the Total Environment,2016,557:697-704.
[30]LIM H J,TURPIN B J.Origins of primary and secondary organic aerosol in Atlanta:results of time-resolved measurements during the Atlanta supersite experiment[J].Environmental Science&Technology,2002,36(21):4489-4496.
[31]CHEN Yuan,XIE Shaodong,LUO Bin.Characteristics and origins of carbonaceous aerosol in the Sichuan Basin China[J].Atmospheric Environment,2014,94:215-223.
[32]HAN Yongming,CAO Junji,CHOW J C,et al.Evaluation of the thermal/optical reflectance method for discrimination between soot and char EC[J].Chemosphere,2007,69:569-574.
[33]CAO Junji,ZHU Chongshu,TIE Xuexi,et al.Characteristics and sources of carbonaceous aerosols from Shanghai China[J].Atmospheric Chemistry and Physics,2013,13(2):803-817.
[34]PAATERO P.User's guide for positive matrix factorization programs PMF2 and PMF3,Part 1-2:Tutorial[M].Helsinki,Finland:Univerisity of Helsinki,2007.
[35]YE Zhaolian,LIU Jiashu,GU Aijun et al.Chemical characterization of fine particulate matter in Changzhou,China,and source apportionment with offline aerosol mass spectrometry[J].Atmospheric Chemistry and Physics,2017,4(17):2573-2592.
[36]KOCAK M,MIHALOPOULOS N,TUTSAK E,et al.PM10and PM2.5composition over the Central Black Sea:origin and seasonal variability[J].Environmental Science and Pollution Research,2015,22(22):18076-18092.
[37]CHAN Y C,SIMPSON R W,MCTAINSH G H.Source apportionment of PM2.5and PM10aerosols in Brisbane(Australia)by receptor modelling[J].Atmospheric Environment,1999,33(19):3251-3268.
[38]MAGIERA T,JABLONSKA M,STRZYSZCZ Z.Morphological and mineralogical forms of technogenic magnetic particles in industrial dusts[J].Atmospheric Environment,2011,45(25):4281-4290.
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[41]PANT P,HARRISON R M.Critical review of receptor modelling for particulate matter:a case study of India[J].Atmospheric Chemistry and Physics,2012,49:1-12.
[42]JEGUIRIM M,KRAIEM N,LAJILI M,et al.The relationship between mineral contents,particle matter and bottom ash distribution during pellet combustion:molar balance and chemometric analysis[J].Environmental Science and Pollution Research,2017,24(11):9927-9939.
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[44]ZHENG G J,DUAN F K,SU H,et al.Exploring the severe winter haze in Beijing:the impact of synoptic weather regional transport and heterogeneous reactions[J].Atmospheric Chemistry and Physics,2014,14(12):2969-2983.
[45]王占山,李云婷,刘保献,等.北京市PM2.5化学组分特征[J].生态学报,2016,36(8):2382-2392.WANG Zhanshan,LI Yunting,LIU Baoxian,et al.Chemical characteristics of PM2.5in Beijing[J].Acta Ecologica Sinica,2016,36(8):2382-2392.
[2]COOKE W F,LIOUSSE C,CACHIER H,et al.Construction of a 1×1 fossil fuel emission data set for carbonaceous aerosol and implementation and radiative impact in the ECHAM4 model[J].Journal of Geophysical Research Atmospheres,1999,104(D18):22137-22162.
[3]CRILLEY L R,AYOKO G A,MAZAHERI M,et al.Factors influencing the outdoor concentration of carbonaceous aerosols at urban schools in Brisbane Australia:implications for children's exposure[J].Environmental Pollution,2016,208:249-255.
[4]胡珊,张远航,魏永杰.珠江三角洲大气细颗粒物的致癌风险及源解析[J].中国环境科学,2009,29(11):1202-1208.HU Shan,ZHANG Yuanhang,WEI Yongjie.Cancer risk level and source apportionment of ambient fine particulate matter in Pearl River Delta[J].China Environmental Science,2009,29(11):1202-1208.
[5]KAUFMAN Y J,TANRE D,BOUCHER O,et al.A satellite view of aerosols in the climate system[J].Nature,2002,419(6903):215-223.
[6]NIU Zhenchuan,WANG Sen,CHEN Jinsheng,et al.Source contributions to carbonaceous species in PM2.5and their uncertainty analysis at typical urban periurban and background sites in southeast China[J].Environmental Pollution,2013,181:107-114.
[7]ACKERMAN A S,TOON O B,STEVENS D E,et al.Reduction of tropical cloudiness by soot[J].Science,2000,288(5468):1042-1047.
[8]ROSENFELD D.Suppression of rain and snow by urban and industrial air pollution[J].Science,2000,287(5459):1793-1796.
[9]NAKAJIMA T,HIGURASHI A,KAWAMOTO K.A possible correlation between satellite-derived cloud and aerosol microphysical parameters[J].Geophysical Research Letters,2011,28(7):1171-1174.
[10]RAMANATHAN V,CRUTZEN P J,KIEHL J T,et al.Aerosols climate and the hydrological cycle[J].Science,2001,294(5549):2119-2124.
[11]BREON F M,TANRE D,GENEROSO S.Aerosol effect on cloud droplet size monitored from satellite[J].Science,2002,295(5556):834-838.
[12]HAN Yongming,CAO Junji,POSMENTIER E S,et al.The effect of acidification on the determination of elemental carbon char and soot-elemental carbon in soils and sediments[J].Chemosphere,2009,75:92-99.
[13]李立伟,戴启立,毕晓辉,等.杭州市冬季环境空气PM2.5中碳组分污染特征及来源[J].环境科学研究,2017,30(3):340-348.LI Liwei,DAI Qili,BI Xiaohui,et al.Characteristics and sources of carbonaceous species in atmospheric PM2.5during winter in Hangzhou City[J].Research of Environmental Sciences,2017,30(3):340-348.
[14]杨佳美,戴启立,刘保双,等.关中地区背景点位环境空气PM2.5来源解析与多模型结果对比[J].环境科学研究,2017,30(2):184-192.YANG Jiamei,DAI Qili,LIU Baoshuang,et al.Source apportionment of ambient PM2.5at background sites in Guanzhong area,China:comparison of results obtained by multiple models[J].Research of Environmental Sciences,2017,30(2):184-192.
[15]魏欣,毕晓辉,董海燕,等.天津市夏季灰霾与非灰霾天气下颗粒物污染特征与来源解析[J].环境科学研究,2012,25(11):1193-1200.WEI Xin,BI Xiaohui,DONG Haiyan,et al.Characteristics and sources of particulate matter during hazy and non-hazy episodes in Tianjin City in summer[J].Research of Environmental Sciences,2012,25(11):1193-1200.
[16]吴琳,沈建东,冯银厂,等.杭州市灰霾与非灰霾日不同粒径大气颗粒物来源解析[J].环境科学研究,2014,27(4):373-381.WU Lin,SHEN Jiandong,FENG Yinchang,et al.Comparison of carbon species measurement results in atmospheric particulate matter:elemental analysis and TOR methods[J].Research of Environmental Sciences,2014,27(12):373-381.
[17]KIM K H,SEKIGUCHI K,KUDO S.Characteristics of atmospheric elemental carbon(char and soot)in ultrafine and fine particles in a roadside environment Japan[J].Aerosol and Air Quality Research,2011,11(1):1-12.
[18]CHOW J C,WATSON J G,PRITCHETT L C,et al.The DRI thermal/optical reflectance carbon analysis system:description evaluation and applications in U.S.air quality studies[J].Atmospheric Environment,1993,27:1185-1201.
[19]CAO Junji,LEE Shuncheng,HO Kinfai,et al.Characteristics of carbonaceous aerosol in Pearl River Delta region China during 2001winter period[J].Atmospheric Environment,2003,37(11):1451-1460.
[20]HOPKE P K.Recent developments in receptor modeling[J].Atmospheric Environment,2003,37(11):1451-1460.
[21]PAATERO P,EBERLY S,BROWN S G,et al.Methods for estimating uncertainty in factor analytic solutions[J].Atmospheric Measurement Techniques,2013,6(4):7593-7631.
[22]PAATERO P,TAPPER U.Analysis of different modes of factor analysis as least square fit problems[J].Chemometrics and Intelligent Laboratory Systems,1993,18(2):183-194.
[23]PAATERO P.Least square formulation of robust nonnegative factor analysis[J].Chemometrics and Intelligent Laboratory Systems,1997,37:23-35.
[24]PAATERO P,EBERLY S,BROWN S G,et al.Methods for estimating uncertainty in factor analytic solutions[J].Atmospheric Measurement Techniques,2014,6(4):7593-7631.
[25]王苏蓉,喻义勇,王勤耕,等.基于PMF模式的南京市大气细颗粒物源解析[J].中国环境科学,2015,35(12):3535-3542.WANG Surong,YU Yiyong,WANG Qingeng,et al.Source apportionment of PM2.5in Nanjing by PMF[J].China Environmental Science,2015,35(12):3535-3542.
[26]王琴,张大伟,刘保献,等.基于PMF模型的北京市PM2.5来源的时空分布特征[J].中国环境科学,2015,35(10):2917-2924.WANG Qin,ZHANG Dawei,LIU Baoxian,et al.Spatial and temporal variations of ambient PM2.5source contributions using positive matrix factorization[J].China Environmental Science,2015,35(10):2917-2924.
[27]刘贵荣.基于比值法的源解析技术研究[D].天津:南开大学,2015.
[28]YANG Fumo,TAN Jihua,ZHAO Qingquan,et al.Characteristics of PM2.5speciation in representative megacities and across China[J].Atmospheric Chemistry and Physics,2011,11:5207-5219.
[29]TIAN Yingze,SHI Guoliang,Huangfu Yanqi,et al.Seasonal and regional variations of source contributions for PM10and PM2.5in urban environment[J].Science of the Total Environment,2016,557:697-704.
[30]LIM H J,TURPIN B J.Origins of primary and secondary organic aerosol in Atlanta:results of time-resolved measurements during the Atlanta supersite experiment[J].Environmental Science&Technology,2002,36(21):4489-4496.
[31]CHEN Yuan,XIE Shaodong,LUO Bin.Characteristics and origins of carbonaceous aerosol in the Sichuan Basin China[J].Atmospheric Environment,2014,94:215-223.
[32]HAN Yongming,CAO Junji,CHOW J C,et al.Evaluation of the thermal/optical reflectance method for discrimination between soot and char EC[J].Chemosphere,2007,69:569-574.
[33]CAO Junji,ZHU Chongshu,TIE Xuexi,et al.Characteristics and sources of carbonaceous aerosols from Shanghai China[J].Atmospheric Chemistry and Physics,2013,13(2):803-817.
[34]PAATERO P.User's guide for positive matrix factorization programs PMF2 and PMF3,Part 1-2:Tutorial[M].Helsinki,Finland:Univerisity of Helsinki,2007.
[35]YE Zhaolian,LIU Jiashu,GU Aijun et al.Chemical characterization of fine particulate matter in Changzhou,China,and source apportionment with offline aerosol mass spectrometry[J].Atmospheric Chemistry and Physics,2017,4(17):2573-2592.
[36]KOCAK M,MIHALOPOULOS N,TUTSAK E,et al.PM10and PM2.5composition over the Central Black Sea:origin and seasonal variability[J].Environmental Science and Pollution Research,2015,22(22):18076-18092.
[37]CHAN Y C,SIMPSON R W,MCTAINSH G H.Source apportionment of PM2.5and PM10aerosols in Brisbane(Australia)by receptor modelling[J].Atmospheric Environment,1999,33(19):3251-3268.
[38]MAGIERA T,JABLONSKA M,STRZYSZCZ Z.Morphological and mineralogical forms of technogenic magnetic particles in industrial dusts[J].Atmospheric Environment,2011,45(25):4281-4290.
[39]CHOW J C,WATSON J G,CHEN L W,et al.Equivalence of elemental carbon by thermal/optical reflectance and transmittance with different temperature protocols[J].Environmental Science&Technology,2004,38:4414-4422.
[40]ZHANG Yunfen,XU Hong,TIAN Yingze,et al.The study on vertical variability of PM10and the possible sources on a 220 m tower,in Tianjin,China[J].Atmospheric Environment,2011,45:6133-6140.
[41]PANT P,HARRISON R M.Critical review of receptor modelling for particulate matter:a case study of India[J].Atmospheric Chemistry and Physics,2012,49:1-12.
[42]JEGUIRIM M,KRAIEM N,LAJILI M,et al.The relationship between mineral contents,particle matter and bottom ash distribution during pellet combustion:molar balance and chemometric analysis[J].Environmental Science and Pollution Research,2017,24(11):9927-9939.
[43]戴莉,薛永华,冯银厂,等.成都市大气颗粒物来源解析研究[C]//中国环境科学学会.中国环境科学学会学术年会论文集(第二卷).北京:中国环境科学学会,2009:805-811.
[44]ZHENG G J,DUAN F K,SU H,et al.Exploring the severe winter haze in Beijing:the impact of synoptic weather regional transport and heterogeneous reactions[J].Atmospheric Chemistry and Physics,2014,14(12):2969-2983.
[45]王占山,李云婷,刘保献,等.北京市PM2.5化学组分特征[J].生态学报,2016,36(8):2382-2392.WANG Zhanshan,LI Yunting,LIU Baoxian,et al.Chemical characteristics of PM2.5in Beijing[J].Acta Ecologica Sinica,2016,36(8):2382-2392.