长春秋季细颗粒物中有机气溶胶组成特征及来源
详细信息    查看全文 | 推荐本文 |
  • 英文篇名:Molecular Composition and Source Apportionment of Fine Organic Aerosols in Autumn in Changchun
  • 作者:吴瑕 ; 曹芳 ; 翟晓瑶 ; 范美益 ; 张世春 ; 章炎麟
  • 英文作者:WU Xia;CAO Fang;ZHAI Xiao-yao;FAN Mei-yi;ZHANG Shi-chun;ZHANG Yan-lin;Yale-NUIST Center on Atmospheric Environment,International Joint Laboratory on Climate and Environment Change (ILCEC) ,School of Applied Meteorology,Nanjing University of Information Science & Technology;Key Laboratory of Meteorological Disaster,Ministry of Education (KLME) ,Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters (CIC-FEMD) ,Nanjing University of Information Science & Technology;Northeast Institute of Geography and Agroecology,Chinese Academy of Sciences;
  • 关键词:PM_(2.5) ; 有机碳(OC) ; 元素碳(EC) ; 非极性有机化合物 ; 主成分分析-多元线性回归(PCA-MLR)模型 ; 来源解析
  • 英文关键词:PM_(2.5);;organic carbon (OC);;elemental carbon (EC);;non-polar organic compounds;;PCA-MLR model;;source apportionment
  • 中文刊名:HJKZ
  • 英文刊名:Environmental Science
  • 机构:南京信息工程大学应用气象学院气候与环境变化国际合作联合实验室大气环境中心;南京信息工程大学气象灾害预报预警与评估协同创新中心气象灾害教育部重点实验室;中国科学院东北地理与农业生态研究所;
  • 出版日期:2019-03-26 15:25
  • 出版单位:环境科学
  • 年:2019
  • 期:v.40
  • 基金:国家重点研发计划项目(2017YFC0212302);; 国家自然科学基金项目(91644103,41603104);; 江苏省自然科学杰出青年基金项目(BK20180040)
  • 语种:中文;
  • 页:HJKZ201908006
  • 页数:9
  • CN:08
  • ISSN:11-1895/X
  • 分类号:44-52
摘要
利用大流量采样器采集了长春城郊2016年10月至2016年11月大气细颗粒物(PM_(2.5))样品共40套,分析了颗粒物中的有机碳(OC)、元素碳(EC)以及非极性有机化合物(主要包括正构烷烃、多环芳烃以及藿烷类化合物)和生物质燃烧标志物左旋葡聚糖的质量浓度,并用分子标记物、特征比值及主成分分析-多元线性回归(PCA-MLR)模型等方法探讨了有机气溶胶的主要来源.结果表明,观测期间PM_(2.5)的平均质量浓度为(79. 0±55. 7)μg·m~(-3),OC和EC的平均质量浓度分别为(20. 7±15. 6)μg·m~(-3)和(2. 2±1. 1)μg·m~(-3),分别占PM_(2.5)的26. 2%和2. 8%.所测非极性有机化合物的总平均浓度为(186. 3±104. 5) ng·m~(-3),浓度高低顺序为正构烷烃[(101. 3±67. 0) ng·m~(-3)]>多环芳烃[(81. 4±46. 0) ng·m~(-3)]>藿烷类化合物[(3. 8±1. 9) ng·m~(-3),其主要来源包括煤燃烧源、生物质燃烧源以及交通源.主成分分析-多元线性回归模型得出该地区有机气溶胶主要排放源的相对贡献依次是煤燃烧源(47. 0%)、生物质燃烧源(42. 6%)和交通源(10. 4%).本研究结果可为我国东北地区有机气溶胶污染防控提供科学依据.
        Organic aerosols have attracted increasing attention recently due to their significant contribution to fine particles (PM_(2.5))and their complex components and sources. In this study,a total of 40 PM_(2.5) samples were collected simultaneously with high-volume samplers in Changchun from 16~(th) Oct to 29~(th) Nov 2016. Organic carbon( OC),elemental carbon( EC),non-polar organic compounds including n-alkanes,polycyclic aromatic hydrocarbons (PAHs),and hopanes,and levoglucosan in atmospheric fine particles were analyzed. The main sources of organic aerosols were identified by molecular markers,diagnostic ratios,and a principal component analysis-multiple liner regression( PCA-MLR) model. The results showed that the average mass concentration of PM_(2.5) was( 79. 0 ±55. 7) μg·m~(-3),and the averaged OC and EC mass concentrations were( 20. 7 ± 15. 6) μg·m~(-3) and( 2. 2 ± 1. 1) μg·m~(-3),which accounted for 26. 2% and 2. 8% of PM_(2.5),respectively. The total average concentration of the tested non-polar organic compounds was( 186. 3 ± 104. 5) ng·m~(-3) and,in descending order,this was composed of n-alkane( 101. 3 ± 67. 0) ng·m~(-3),polycyclic aromatic hydrocarbons( 81. 4 ± 46. 0) ng·m~(-3),hopanes( 3. 8 ± 1. 9) ng·m~(-3). The PCA-MLR model results showed that the relative contributions of the main sources of organic aerosols were coal combustion( 47. 0%),biomass burning( 42. 6%),and traffic emission( 10. 4%).
引文
[1]郭新彪,魏红英.大气PM2.5对健康影响的研究进展[J].科学通报,2013,58(13):1171-1177.Guo X B,Wei H Y.Progress on the health effects of ambient PM2.5pollution[J].Chinese Science Bulletin,2013,58(13):1171-1177.
    [2]Matsumoto H,Inoue K.Mutagenicity of a polar portion in the neutral fraction separated from organic extracts of airborne particulates[J].Archives of Environmental Contamination and Toxicology,1987,16(4):409-416.
    [3]Kleefeld S,Hoffer A,Krivácsy Z,et al.Importance of organic and black carbon in atmospheric aerosols at Mace Head,on the west coast of Ireland(53°19'N,9°54'W)[J].Atmospheric Environment,2002,36(28):4479-4490.
    [4]Ji Y M,Zhao J,Terazono H,et al.Reassessing the atmospheric oxidation mechanism of toluene[J].Proceedings of the National Academy of Sciences of the United States of America,2017,114(31):8169-8174.
    [5]Ng N L,Kroll J H,Chan A W H,et al.Secondary organic aerosol formation from m-xylene,toluene,and benzene[J].Atmospheric Chemistry and Physics,2007,7(14):3909-3922.
    [6]Turpin B J,Saxena P,Andrews E.Measuring and simulating particulate organics in the atmosphere:problems and prospects[J].Atmospheric Environment,2000,34(18):2983-3013.
    [7]PopeⅢC A,Burnett R T,Thun M J,et al.Lung cancer,cardiopulmonary mortality,and long-term exposure to fine particulate air pollution[J].The Journal of the American Medical Association,2002,287(9):1132-1141.
    [8]Yu J Z,Huang X H H,Ho S S H,et al.Nonpolar organic compounds in fine particles:quantification by thermal desorptionGC/MS and evidence for their significant oxidation in ambient aerosols in Hong Kong[J].Analytical and Bioanalytical Chemistry,2011,401(10):3125-3139.
    [9]Schnelle-Kreis J,Orasche J,Abbaszade G,et al.Application of direct thermal desorption gas chromatography time-of-flight mass spectrometry for determination of nonpolar organics in low-volume samples from ambient particulate matter and personal samplers[J].Analytical and Bioanalytical Chemistry,2011,401(10):3083-3094.
    [10]Simoneit B R T,Kobayashi M,Mochida M,et al.Composition and major sources of organic compounds of aerosol particulate matter sampled during the ACE-Asia campaign[J].Journal of Geophysical Research:Atmospheres,2004,109(D19):D19S10.
    [11]del Rosario Sienra M,Rosazza N G,Préndez M.Polycyclic aromatic hydrocarbons and their molecular diagnostic ratios in urban atmospheric respirable particulate matter[J].Atmospheric Research,2005,75(4):267-281.
    [12]Rogge W F,Hildemann L M,Mazurek M A,et al.Sources of fine organic aerosol.2.Noncatalyst and catalyst-equipped automobiles and heavy-duty diesel trucks[J].Environmental Science&Technology,1993,27(4):636-651.
    [13]Fraser M P,Lakshmanan K.Using levoglucosan as a molecular marker for the long-range transport of biomass combustion aerosols[J].Environmental Science&Technology,2000,34(21):4560-4564.
    [14]Schauer J J,Kleeman M J,Cass G R,et al.Measurement of emissions from air pollution sources.3.C1-C29organic compounds from fireplace combustion of wood[J].Environmental Science&Technology,2001,35(9):1716-1728.
    [15]刁格乐,鲍秋阳,马玉芹.东北地区吉林市大气PM2.5中有机物及重金属的污染特征研究[J].东北师大学报(自然科学版),2018,50(3):147-156.Diao G L,Bao Q Y,Ma Y Q.Research on the PM2.5characteristics of organic matters and heavy metals pollution in Jilin,the Northeast of China[J].Journal of Northeast Normal University(Natural Science Edition),2018,50(3):147-156.
    [16]陆建衡,黄艺,王春宇,等.吉林永安煤矿区土壤及近地表大气尘重金属污染评价[J].工业安全与环保,2018,44(6):5-9,21.Lu J H,Huang Y,Wang C Y,et al.Evaluation of heavy metals pollution to soil and air dust near ground of Yong'an coal mining area in Jilin[J].Industrial Safety and Environmental Protection,2018,44(6):5-9,21.
    [17]鲍秋阳,王毅勇,张学磊,等.吉林市大气PM2.5污染特征及来源分析[J].环境保护科学,2018,44(3):74-79.Bao Q Y,Wang L Y,Zhang X L,et al.Analysis of the characteristics and sources of atmospheric PM2.5pollution in Jilin City[J].Environmental Protection Science,2018,44(3):74-79.
    [18]施云芬,刘月华,李英赞.吉林市大气污染物浓度分布规律[J].环境与健康杂志,2008,25(4):334-336.Shi Y F,Liu Y H,Li Y Z.Distribution regularity of air pollutant concentration in Jilin City[J].Journal of Environment and Health,2008,25(4):334-336.
    [19]崔俊峰,李英华,景丽洁,等.吉林市大气气溶胶中部分有机污染物的分析[J].化工科技,2008,16(1):41-43.Cui J F,Li Y H,Jing L J,et al.Analysis of organic pollutants of atmospheric aerosols in Jilin City[J].Science&Technology in Chemical Industry,2008,16(1):41-43.
    [20]李英华,景丽洁,崔俊峰,等.吉林市大气中PM10和PAHs污染特征[J].辽宁城乡环境科技,2007,27(1):43-44,52.Li Y H,Jing L J,Cui J F,et al.Pollution specialities of PM10and PAHs in atmospheric environment in Jilin[J].Liaoning Urban and Rural Environmental Science&Technology,2007,27(1):43-44,52.
    [21]李成日,崔俊峰,李英华,等.吉林市工业区大气可吸入颗粒物中多环芳烃的分布特征研究[J].吉林化工学院学报,2005,22(4):16-18.Li C R,Cui J F,Li Y H,et al.Study on distribution characteristics of PAHs in inhalable particles in industry area in Jilin City[J].Journal of Jilin Institute of Chemical Technology,2005,22(4):16-18.
    [22]张振斌.长春市某城区气溶胶浓度特征及重金属化学形态分布研究[D].长春:吉林大学,2013.Zhang Z B.Study on the characteristics of concentration and distribution of heavy metals chemical speciation of aerosol in a district of Changchun[D].Changchun:Jilin University,2013.
    [23]Birch M E,Cary R A.Elemental carbon-based method for monitoring occupational exposures to particulate diesel exhaust[J].Aerosol Science and Technology,1996,25(3):221-241.
    [24]周敏,陈长虹,王红丽,等.上海秋季典型大气高污染过程中有机碳和元素碳的变化特征[J].环境科学学报,2013,33(1):181-188.Zhou M,Chen C H,Wang H L,et al.The variation characteristics of organic and element carbon during air pollution episodes in autumn in Shanghai,China[J].Acta Scientiae Circumstantiae,2013,33(1):181-188.
    [25]魏巧珍,王宇红,李盛,等.基于PCA-MLR模型的兰州市大气PM2.5污染来源解析[J].环境卫生学杂志,2017,7(4):267-273.Wei Q Z,Wang Y H,Li S,et al.The source apportionment of PM2.5based on PCA-MLR model in Lanzhou City[J].Journal of Environmental Hygiene,2017,7(4):267-273.
    [26]边璐,李田,侯娟.PMF和PCA/MLR法解析上海市高架道路地表径流中多环芳烃的来源[J].环境科学,2013,34(10):3840-3846.Bian L,Li T,Hou J.Source apportionment of polycyclic aromatic hydrocarbons using two mathematical models for runoff of the Shanghai elevated inner highway,China[J].Environmental Science,2013,34(10):3840-3846.
    [27]Duan J C,Tan J H,Wang S L,et al.Roadside,urban,and rural comparison of size distribution characteristics of PAHs and carbonaceous components of Beijing,China[J].Journal of Atmospheric Chemistry,2012,69(4):337-349.
    [28]He L Y,Hu M,Huang X F,et al.Measurement of emissions of fine particulate organic matter from Chinese cooking[J].Atmospheric Environment,2004,38(38):6557-6564.
    [29]Schauer J J,Kleeman M J,Cass G R,et al.Measurement of emissions from air pollution sources.5.C1-C32organic compounds from gasoline-powered motor vehicle[J].Environment Science&Technology,2002,36(6):1169-1180.
    [30]Chen Y J,Zhi G R,Feng Y L,et al.Measurements of emission factors for primary carbonaceous particles from residential rawcoal combustion in China[J].Geophysical Research Letters,2006,33(20):L20815.
    [31]Turpin B J,Cary R A,Huntzicker J J.An in situ,time-resolved analyzer for aerosol organic and elemental carbon[J].Aerosol Science and Technology,1990,12(1):161-171.
    [32]李杏茹,白羽,陈曦,等.北京冬季重污染过程大气细颗粒物化学组成特征及来源分析[J].环境化学,2018,37(11):2397-2409.Li X R,Bai Y,Chen X,et al.Chemical composition and source apportionment of PM2.5during winter in Beijing[J].Environmental Chemistry,2018,37(11):2397-2409.
    [33]徐足飞,曹芳,高嵩,等.南京北郊秋季PM2.5碳质组分污染特征及来源分析[J].环境科学,2018,39(7):3033-3041.Xu Z F,Cao F,Gao S,et al.Characteristics and source analysis of carbonaceous components of PM2.5during autumn in the northern suburb of Nanjing[J].Environmental Science,2018,39(7):3033-3041.
    [34]鞠法帅,王鑫彤,韩德文,等.金华地区PM2.5中的极性有机示踪物[J].环境科学学报,2017,37(8):3054-3064.Ju F S,Wang X T,Han D W,et al.Polar organic tracers in PM2.5in Jinhua[J].Acta Scientiae Circumstantiae,2017,37(8):3054-3064.
    [35]Feng J L,Hu M,Chan C K,et al.A comparative study of the organic matter in PM2.5from three Chinese megacities in three different climatic zones[J].Atmospheric Environment,2006,40(21):3983-3994.
    [36]Simoneit B R T.Organic matter of the troposphere-III:characterization and sources of petroleum and pyrogenic residues in aerosols over the western United States[J].Atmospheric Environment,1984,18(1):51-67.
    [37]袁杨森,刘大锰,车瑞俊,等.北京夏季大气颗粒物中有机污染源的生物标志物示踪[J].中国科学院研究生院学报,2007,24(5):601-611.Yuan Y S,Liu D M,Che R J,et al.Source tracing of biomarkers in the organic pollutants from atmospheric particulates in Beijing city during summer[J].Journal of the Graduate School of the Chinese Academy of Sciences,2007,24(5):601-611.
    [38]姚利,李杏茹,郭雪清,等.2007年春节期间北京大气细粒子中正构烷烃的污染特征[J].环境科学,2009,30(2):589-593.Yao L,Li X R,Guo X Q,et al.Pollution characteristics of nalkanes in atmospheric fine particles during spring festival of 2007in Beijing[J].Environmental Science,2009,30(2):589-593.
    [39]Alves C,Pio C,Duarte A.Composition of extractable organic matter of air particles from rural and urban Portuguese areas[J].Atmospheric Environment,2001,35(32):5485-5496.
    [40]赵文昌,程金平,谢海赟,等.环境中多环芳烃(PAHs)的来源与监测分析方法[J].环境科学与技术,2006,29(3):105-107.Zhao W C,Chen J P,Xie H Y,et al.PAHs:Sources,pathway and their monitoring and analysis[J].Environmental Science&Technology,2006,29(3):105-107.
    [41]Pistikopoulos P,Wortham H M,Gomes L,et al.Mechanisms of formation of particulate polycyclic aromatic hydrocarbons in relation to the particle size distribution;effects on meso-scale transport[J].Atmospheric Environment.Part A.General Topics,1990,24(10):2573-2584.
    [42]Katsoyiannis A,Sweetman A J,Jones K C.PAH molecular diagnostic ratios applied to atmospheric sources:a critical evaluation using two decades of source inventory and air concentration data from the UK[J].Environmental Science&Technology,2011,45(20):8897-8906.
    [43]Yunker M B,Macdonald R W,Vingarzan R,et al.PAHs in the Fraser River basin:a critical appraisal of PAH ratios as indicators of PAH source and composition[J].Organic Geochemistry,2002,33(4):489-515.
    [44]Akyüz M,abuk H.Gas-particle partitioning and seasonal variation of polycyclic aromatic hydrocarbons in the atmosphere of Zonguldak,Turkey[J].Science of the Total Environment,2010,408(22):5550-5558.
    [45]Ravindra K,Sokhi R,Van Grieken R.Atmospheric polycyclic aromatic hydrocarbons:source attribution,emission factors and regulation[J].Atmospheric Environment,2008,42(13):2895-2921.
    [46]Cass G R.Organic molecular tracers for particulate air pollution sources[J].Tr AC Trends Analytical Chemistry,1998,17(6):356-366.
    [47]Robinson A L,Donahue N M,Rogge W F.Photochemical oxidation and changes in molecular composition of organic aerosol in the regional context[J].Journal of Geophysical Research:Atmospheres,2006,111(D3):D03302.
    [48]Robinson A L,Subramanian R,Donahue N M,et al.Source apportionment of molecular markers and organic aerosol-1.Polycyclic aromatic hydrocarbons and methodology for data visualization[J].Environmental Science&Technology,2006,40(24):7803-7810.
    [49]He L Y,Hu M,Zhang Y H,et al.Fine particle emissions from on-road vehicles in the Zhujiang Tunnel,China[J].Environmental Science&Technology,2008,42(12):4461-4466.
    [50]Zhang Y X,Schauer J J,Zhang Y H,et al.Characteristics of particulate carbon emissions from real-world Chinese coal combustion[J].Environmental Science&Technology,2008,42(14):5068-5073.
    [51]Mastral A M,Callén M,Murillo R.Assessment of PAHemissions as a function of coal combustion variables[J].Fuel,1996,75(13):1533-1536.
    [52]Khalili N R,Scheff P A,Holsen T M.PAH source fingerprints for coke ovens,diesel and,gasoline engines,highway tunnels,and wood combustion emissions[J].Atmospheric Environment,1995,29(4):533-542.

© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号

地址:北京市海淀区学院路29号 邮编:100083

电话:办公室:(+86 10)66554848;文献借阅、咨询服务、科技查新:66554700