西安市PM_(2.5)中碳质气溶胶污染特征
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摘要
利用热光分析法探究了西安市2017年353个PM_(2.5)样品中的元素碳(EC)、有机碳(OC)、甲醇可萃取有机碳(MSOC)以及热-光分析法得到的7个碳组分(OC1～4、EC1～3)的质量浓度、季节变化趋势以及来源.结果表明,西安市2017年OC、EC以及MSOC的平均质量浓度分别为(17. 56±11. 83)、(4. 08±2. 95)和(11. 10±6. 77)μg·m~(-3). OC质量浓度的季节性趋势为冬季>春季>夏季>秋季; EC为冬季>春季≈秋季>夏季. MSOC/OC比值年平均值为0. 64±0. 20,冬季最高,夏季最低.春季OC和EC相关性较好(r~2=0. 76),而在冬季的相关性较差(r~2=0. 43),说明碳气溶胶的来源不同.采用EC示踪法对二次气溶胶的含量进行估算,SOC的平均含量分别占到了春、夏、秋、冬四季OC质量浓度的51. 9%、38. 4%、37. 3%、44. 0%.采用主成分分析法得出西安市的碳质气溶胶主要来源于燃煤和机动车排放.
Mass concentration,seasonal variation and sources of organic carbon( OC),element carbon( EC),methanol-soluble organic carbon( MSOC),and seven carbon components( OC1-4,EC1-3) were detected by thermal-optical analysis of 353 PM_(2.5) samples in Xi'an in 2017. The results show that the average mass concentrations of OC,EC,and MSOC were( 17. 56 ± 11. 83),( 4. 08 ± 2. 95) and( 11. 10 ± 6. 77) μg·m~(-3),respectively. The seasonal trend of the OC concentration follows the order winter >spring > summer > autumn. The seasonal trend in EC concentration follows the order winter > spring≈autumn > summer. The average MSOC/OC value is 0. 64 ± 0. 20. The highest value is observed in winter and the lowest in summer. The correlation between OC and EC is good in spring( r~2= 0. 76),but the correlation is poor in winter( r~2= 0. 43). These results indicate that the source of the carbon aerosols was different. The content of secondary organic aerosols was estimated by the EC tracing method. The average mass concentration of SOC accounted for 51. 9%,38. 4%,37. 3% and 44. 0% of OC in spring, summer, autumn, and winter,respectively. The main sources of carbonaceous aerosols were analyzed by principal component analysis. The results show that carbonaceous aerosols originate mainly from coal and vehicle emissions in Xi'an.
Mass concentration,seasonal variation and sources of organic carbon( OC),element carbon( EC),methanol-soluble organic carbon( MSOC),and seven carbon components( OC1-4,EC1-3) were detected by thermal-optical analysis of 353 PM_(2.5) samples in Xi'an in 2017. The results show that the average mass concentrations of OC,EC,and MSOC were( 17. 56 ± 11. 83),( 4. 08 ± 2. 95) and( 11. 10 ± 6. 77) μg·m~(-3),respectively. The seasonal trend of the OC concentration follows the order winter >spring > summer > autumn. The seasonal trend in EC concentration follows the order winter > spring≈autumn > summer. The average MSOC/OC value is 0. 64 ± 0. 20. The highest value is observed in winter and the lowest in summer. The correlation between OC and EC is good in spring( r~2= 0. 76),but the correlation is poor in winter( r~2= 0. 43). These results indicate that the source of the carbon aerosols was different. The content of secondary organic aerosols was estimated by the EC tracing method. The average mass concentration of SOC accounted for 51. 9%,38. 4%,37. 3% and 44. 0% of OC in spring, summer, autumn, and winter,respectively. The main sources of carbonaceous aerosols were analyzed by principal component analysis. The results show that carbonaceous aerosols originate mainly from coal and vehicle emissions in Xi'an.
引文
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[2] Nizkorodov S A,Laskin J,Laskin A. Molecular chemistry of organic aerosols through the application of high resolution mass spectrometry[J]. Physical Chemistry Chemical Physics,2011,13(9):3612-3629.
[3] Cao J J,Lee S,Ho K,et al. Spatial and seasonal distributions of atmospheric carbonaceous aerosols in pearl river delta region,China[J]. China Particuology,2003,1(1):33-37.
[4] Turpin B J,Huntzicker J J. Secondary formation of organic aerosol in the Los Angeles basin:A descriptive analysis of organic and elemental carbon concentrations[J]. Atmospheric Environment. Part A. General Topics,1991,25(2):207-215.
[5]关攀博,师华定,高庆先,等.中国地区黑碳气溶胶的气候效应模拟[J].环境工程技术学报,2017,7(4):418-423.Guan P B,Shi H D,Gao Q X,et al. Study on black carbon aerosol simulation of climate effect in China[J]. Journal of Environmental Engineering Technology,2017,7(4):418-423.
[6] Forster P, Ramaswamy V, Artaxo P, et al. Changes in atmospheric constituents and in radiative forcing[A]. In:Solomon S,Qin D,Manning M,et al(Eds.). Climate Change2007:The physical science basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change[M]. Cambridge:Cambridge University Press,2007. 129-234.
[7]张华,马井会,郑有飞.黑碳气溶胶辐射强迫全球分布的模拟研究[J].大气科学,2008,32(5):1147-1158.Zhang H,Ma J H,Zheng Y F. The study of global radiative forcing due to black carbon aerosol[J]. Chinese Journal of Atmospheric Sciences,2008,32(5):1147-1158.
[8] Rogge W F, Mazurek M A, Hildemann L M, et al.Quantification of urban organic aerosols at a molecular level:Identification, abundance and seasonal variation[J].Atmospheric Environment. Part A. General topics,1993,27(8):1309-1330.
[9] Chen Q C,Ikemori F,Higo H,et al. Chemical structural characteristics of HULIS and other fractionated organic matter in urban aerosols:Results from mass spectral and FT-IR analysis[J]. Environmental Science&Technology,2016,50(4):1721-1730.
[10]田鹏山,曹军骥,韩永明,等.关中地区冬季PM2. 5中碳气溶胶的污染特征及来源解析[J].环境科学,2016,37(2):427-433.Tian P S,Cao J J,Han Y M,et al. Pollution characteristics and sources of carbonaceous aerosol in PM2. 5during winter in Guanzhong area[J]. Environmental Science,2016,37(2):427-433.
[11] Baumgartner J, Zhang Y X, Schauer J J,et al. Highway proximity and black carbon from cookstoves as a risk factor for higher blood pressure in rural China[J]. Proceedings of the National Academy of Sciences of the United States of America,2014,111(36):13229-13234.
[12] Offenberg J H,Baker J E. Aerosol size distributions of elemental and organic carbon in urban and over-water atmospheres[J].Atmospheric Environment,2000,34(10):1509-1517.
[13] Heal M R,Kumar P,Harrison R M. Particles,air quality,policy and health[J]. Chemical Society Reviews,2012,41(19):6606-6630.
[14] Jimenez J L,Canagaratna M R,Donahue N M,et al. Evolution of organic aerosols in the atmosphere[J]. Science,2009,326(5959):1525-1529.
[15] Kanakidou M,Seinfeld J H,Pandis S N,et al. Organic aerosol and global climate modelling:A review[J]. Atmospheric Chemistry and Physics,2005,5(4):1053-1123.
[16] Decesari S,Mircea M,Cavalli F,et al. Source attribution of water-soluble organic aerosol by nuclear magnetic resonance spectroscopy[J]. Environmental Science&Technology,2007,41(7):2479-2484.
[17] 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.
[18] Willoughby A S,Wozniak A S,Hatcher P G. A molecular-level approach for characterizing water-insoluble components of ambient organic aerosol particulates using ultrahigh-resolution mass spectrometry[J]. Atmospheric Chemistry and Physics,2014,14(18):10299-10314.
[19] Chen Q C, Ikemori F, Mochida M. Light Absorption and excitation-emission fluorescence of urban organic aerosol components and their relationship to chemical structure[J].Environmental Science&Technology,2016,50(20):10859-10868.
[20] Sciare J, D'Argouges O, Sarda-Estève R, et al. Large contribution of water-insoluble secondary organic aerosols in the region of Paris(France)during wintertime[J]. Journal of Geophysical Research:Atmospheres, 2014, 116(D22):D22203.
[21] 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.
[22]杜博涵,黄晓锋,何凌燕,等.宁波市PM2. 5中碳组分的时空分布特征和二次有机碳估算[J].环境科学,2015,36(9):3128-3134.Du B H,Huang X F,He L Y,et al. Seasonal and spatial variations of carbon fractions in PM2. 5in Ningbo and the estimation of secondary organic carbon[J]. Environmental Science,2015,36(9):3128-3134.
[23]吕喆,韩力慧,程水源,等.北京城区冬夏季含碳气溶胶浓度特征及区域传输对灰霾形成影响[J].北京工业大学学报,2018,44(3):463-472.LüZ, Han L H, Cheng S Y, et al. Characteristics of carbonaceous aerosols and influence of regional transport on haze formation in winter and summer in urban of Beijing[J]. Journal of Beijing University of Technology,2018,44(3):463-472.
[24]曹军骥,李顺诚,李杨,等. 2003年秋冬季西安大气中有机碳和元素碳的理化特征及其来源解析[J].自然科学进展,2005,15(12):1460-1466.
[25]叶招莲,刘佳澍,李清,等.常州夏秋季PM2. 5中碳质气溶胶特征及来源[J].环境科学,2017,38(11):4469-4477.Ye Z L, Liu J S, Li Q, et al. Characteristics and source identification of carbonaceous aerosols in PM2. 5measurements during summer and fall in Changzhou[J]. Environmental Science,2017,38(11):4469-4477.
[26] Turpin B J,Huntzicker J J. Identification of secondary organic aerosol episodes and quantitation of primary and secondary organic aerosol concentrations during SCAQS[J]. Atmospheric Environment,1995,29(23):3527-3544.
[27]徐宏辉,徐婧莎,何俊,等.杭甬地区大气中含碳气溶胶特征及来源分析[J].环境科学,2018,39(8):3511-3517.Xu H H,Xu J S,He J,et al. Characteristics and source analysis of atmospheric carbonaceous aerosols in the cities of Hangzhou and Ningbo[J]. Environmental Science,2018,39(8):3511-3517.
[28]董娅玮,杜新黎,李扬扬,等.西安市区大气中PM2. 5和PM10质量浓度污染特征[J].中国环境监测,2015,31(5):45-49.Dong Y W,Du X L,Li Y Y,et al. Pollution characteristics of mass concentration of PM2. 5and PM10in Xi'an city[J].Environmental Monitoring in China,2015,31(5):45-49.
[29] Turpin B J,Lim H J. Species contributions to PM2. 5mass concentrations:revisiting common assumptions for estimating organic mass[J]. Aerosol Science and Technology,2001,35(1):602-610.
[30] Mihara T,Mochida M. Characterization of solvent-extractable organics in urban aerosols based on mass spectrum analysis and hygroscopic growth measurement[J]. Environmental Science&Technology,2011,45(21):9168-9174.
[31] Huang H, Ho K F, Lee S C, et al. Characteristics of carbonaceous aerosol in PM2. 5:Pearl Delta River Region,China[J]. Atmospheric Research,2012,104-105:227-236.
[32]李曼.上海市PM2. 5中水溶性有机组分的组成特征、季节变化及来源解析[D].上海:上海大学,2013.Li M. Chemical composition,seasonal variation and sources of water-soluble organic components in PM2. 5in Shanghai[D].Shanghai:Shanghai University,2013.
[33] Du Z Y,He K B,Cheng Y,et al. A yearlong study of watersoluble organic carbon in Beijing II:Light absorption properties[J]. Atmospheric Environment,2014,89:235-241.
[34] Zhao L,Lun X X,Li R N,et al. Deposition of PM2. 5sulfate in the spring on urban forests in Beijing,China[J]. Atmosphere,2017,8(1):3.
[35] Zhang J K,Ji D S,Liu Z R,et al. New characteristics of submicron aerosols and factor analysis of combined organic and inorganic aerosol mass spectra during winter in Beijing[J].Atmospheric Chemistry and Physics Discussions,2015,15(13):18537-18576.
[36] Sun Y L,Du W,Fu P Q,et al. Primary and secondary aerosols in Beijing in winter:sources,variations and processes[J].Atmospheric Chemistry and Physics,2016,16(13):8309-8329.
[37] Na K,Sawant A A,Song C,et al. Primary and secondary carbonaceous species in the atmosphere of Western Riverside County,California[J]. Atmospheric Environment,2004,38(9):1345-1355.
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