聊城市冬季PM_(2.5)中正构烷烃和糖类的污染特征及来源解析
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摘要
为研究聊城市冬季大气PM_(2.5)中正构烷烃和糖类化合物的分子组成、浓度水平及来源,于2017年1～2月在聊城大学进行PM_(2.5)样品采集,对19种(C18～C36)正构烷烃和10种糖类化合物进行分析,并采用主成分分析法(PCA)解析其来源.结果表明,聊城市冬季PM_(2.5)中总正构烷烃的质量浓度为(456. 9±252. 5) ng·m~(-3),其中,灰霾期的质量浓度最高,约为清洁天的2倍,烟火Ⅰ期与Ⅱ期分别为清洁天的0. 9倍和1. 2倍.采样期间碳优势指数(CPI)值为1. 2±0. 1,植物蜡排放的正构烷烃对总正构烷烃的贡献率(%Wax Cn)为3. 1%～36. 0%,表明化石燃料燃烧是聊城市大气中正构烷烃的主要来源.聊城市冬季PM_(2.5)中糖类化合物的总质量浓度为(415. 5±213. 8) ng·m~(-3),其中左旋葡聚糖的浓度最高,其次是半乳聚糖和甘露聚糖,三者共占总糖的91. 6%,表明生物质燃烧源对聊城市大气气溶胶具有重要贡献.主成分分析(PCA)结果表明,聊城市冬季大气气溶胶中正构烷烃和糖类化合物主要来自化石燃料的燃烧和生物质燃烧.
To investigate molecular composition,mass concentrations,and sources of n-alkanes and sugars which are adsorbed in ambient particulate matters in Liaocheng City during winter,PM_(2.5) samples were collected from January 17 to February 15,2017 at Liaocheng University. 19 kinds( C18-C36) of n-alkanes and 10 kinds of sugars were determined using GC-MS. The identification of nalkane and sugar sources were investigated using principal component analysis( PCA). The results showed that the mass concentrations of total n-alkanes in PM_(2.5) during the winter were( 456. 9 ± 252. 5) ng·m~(-3). During the haze period,the concentrations of n-alkanes were two times higher than those on clear days. Additionally,the concentrations of n-alkanes during fireworks event I and fireworks event II were 0. 9 times and 1. 2 times higher than those on clear days. During the sampling period,the Carbon preference index( CPI)was 1. 2 ± 0. 1,and the contribution from plant wax concentrations for n-alkanes( % Wax Cn) was between 3. 1% ～ 36. 0%,indicating that fossil fuels were the major source of n-alkanes in Liaocheng City during the winter. The mass concentrations of saccharides in PM_(2.5) during the winter were( 415. 5 ± 213. 8) ng·m~(-3). Levoglucosan was the most abundant species,followed by galactosan and mannosan,which accounted for more than 91. 6% of total saccharides,indicating that biomass burning was much more significant in Liaocheng City. PCA further suggested that n-alkane and saccharide compounds in atmospheric aerosol during the winter in Liaocheng City were primarily derived from fossil fuel and biomass burning.
To investigate molecular composition,mass concentrations,and sources of n-alkanes and sugars which are adsorbed in ambient particulate matters in Liaocheng City during winter,PM_(2.5) samples were collected from January 17 to February 15,2017 at Liaocheng University. 19 kinds( C18-C36) of n-alkanes and 10 kinds of sugars were determined using GC-MS. The identification of nalkane and sugar sources were investigated using principal component analysis( PCA). The results showed that the mass concentrations of total n-alkanes in PM_(2.5) during the winter were( 456. 9 ± 252. 5) ng·m~(-3). During the haze period,the concentrations of n-alkanes were two times higher than those on clear days. Additionally,the concentrations of n-alkanes during fireworks event I and fireworks event II were 0. 9 times and 1. 2 times higher than those on clear days. During the sampling period,the Carbon preference index( CPI)was 1. 2 ± 0. 1,and the contribution from plant wax concentrations for n-alkanes( % Wax Cn) was between 3. 1% ～ 36. 0%,indicating that fossil fuels were the major source of n-alkanes in Liaocheng City during the winter. The mass concentrations of saccharides in PM_(2.5) during the winter were( 415. 5 ± 213. 8) ng·m~(-3). Levoglucosan was the most abundant species,followed by galactosan and mannosan,which accounted for more than 91. 6% of total saccharides,indicating that biomass burning was much more significant in Liaocheng City. PCA further suggested that n-alkane and saccharide compounds in atmospheric aerosol during the winter in Liaocheng City were primarily derived from fossil fuel and biomass burning.
引文
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[13] Zhang J M,Yang L X,Chen J M,et al. Influence of fireworks displays on the chemical characteristics of PM2. 5in rural and suburban areas in Central and East China[J]. Science of the Total Environment,2016,578:476-484.
[14]张敬巧,吴亚君,张萌,等.聊城冬季一重污染过程PM2. 5污染特征及成因分析[J].环境科学,2018,39(9):4026-4033.Zhang J Q, Wu Y J, Zhang M, et al. PM2. 5Pollution characterization and cause analysis of a winter heavy pollution event,Liaocheng City[J]. Environmental Science,2018,39(9):4026-4033.
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[19] Wang G H,Kawamura K,Xie M J,et al. Selected water-soluble organic compounds found in size-resolved aerosols collected from urban,mountain and marine atmospheres over East Asia[J].Tellus,2011,63(3):371-381.
[20] Kong S F,Li L,Li X X,et al. The impacts of firework burning at the Chinese Spring Festival on air quality:insights of tracers,source evolution and aging processes[J]. Atmospheric Chemistry and Physics,2015,15(4):2167-2184.
[21] Li Y S,Cao J J,Li J J,et al. Molecular distribution and seasonal variation of hydrocarbons in PM2. 5from Beijing during2006[J]. Particuology,2013,11(1):78-85.
[22] Feng J L,Hu J C,Xu B H,et al. Characteristics and seasonal variation of organic matter in PM2. 5at a regional background site of the Yangtze River Delta region, China[J]. Atmospheric Environment,2015,123:288-297.
[23] Gu Z P,Feng J L,Han W L,et al. Characteristics of organic matter in PM2. 5from an e-waste dismantling area in Taizhou,China[J]. Chemosphere,2010,80(7):800-806.
[24] Li J J,Wang G H,Aggarwal S G,et al. Comparison of abundances,compositions and sources of elements, inorganic ions and organic compounds in atmospheric aerosols from Xi'an and New Delhi,two megacities in China and India[J]. Science of the Total Environment,2014,476-477:485-495.
[25] Simoneit B R T,Cox R E,Standley L J. Organic matter of the troposphere-IV. Lipids in harmattan aerosols of Nigeria[J].Atmospheric Environment(1967),1988,22(5):983-1004.
[26] Simoneit B R T,Sheng G Y,Chen X J,et al. Molecular marker study of extractable organic matter in aerosols from urban areas of China[J]. Atmospheric Environment. Part A. General Topics,1991,25(10):2111-2129.
[27] Simoneit B R T,Kobayashi M,Mochida M,et al. Aerosol particles collected on aircraft flights over the northwestern Pacific region during the ACE-Asia campaign:Composition and major sources of the organic compounds[J]. Journal of Geophysical Research,2004,109(D19):D19S09.
[28] Li X R,Guo X Q,LIU X R,et al. Distribution and sources of solvent extractable organic compounds in PM2. 5during 2007Chinese Spring Festival in Beijing[J]. Journal of Environmental Science,2009,21(2):142-149.
[29]李曼,仲勉,荆亮,等.上海PM2. 5中糖类化合物的组成及来源分析[J].上海大学学报(自然科学版),2013,19(4):387-392.Li M,Zhong M,Jing L,et al. Concentrations and sources of saccharides in PM2. 5in Shanghai[J]. Journal of Shanghai University(Natural Science),2013,19(4):387-392.
[30]黄绪,郭云霞,刘剑斌,等.柳州大气PM2. 5中糖类物质的分布特征与指示意义[J].中国环境科学,2017,37(3):838-843.Huang X, Guo Y X, Liu J B, et al. The distribution characteristics and implications of carbohydrates in the PM2. 5of Liuzhou[J]. China Environmental Science,2017,37(3):838-843.
[31] Simoneit B R T,Elias V O. Organic tracers from biomass burning in atmospheric particulate matter over the ocean[J].Marine Chemistry,2000,69(3-4):301-312.
[32] 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.
[33] Simoneit B R T. Biomass burning—a review of organic tracers for smoke from incomplete combustion[J]. Applied Geochemistry,2002,17(3):129-162.
[34] Simoneit B R T. A review of biomarker compounds as source indicators and tracers for air pollution[J]. Environmental Science and Pollution Research,1999,6(3):159-169.
[35] Engling G, Lee J J, Tsai Y W, et al. Size-resolved anhydrosugarcomposition in smoke aerosol from controlled field burning of rice straw[J]. Aerosol Science and Technology,2009,43(7):662-672.
[36] Oros D R,Abas M R B,Omar N Y M J,et al. Identification and emission factors of molecular tracers in organic aerosols from biomass burning:Part 3. Grasses[J]. Applied Geochemistry,2006,21(6):919-940.
[37] JaegerⅢC H,Lindow S E,Miller W,et al. Mapping of sugar and amino acid availability in soil around roots with bacterial sensors of sucrose and tryptophan[J]. Applied and Environmental Microbiology,1999,65(6):2685-2690.
[38] Speranza A,Calzoni G L,Pacini E. Occurrence of mono-or disaccharides and polysaccharide reserves in mature pollen grains[J]. Sexual Plant Reproduction,1997,10(2):110-115.
[39] Wan E C H,Yu J Z. Analysis of sugars and sugar polyols in atmospheric aerosols by chloride attachment in liquid chromatography/negative ion electrospray mass spectrometry[J].Environmental Science&Technology,2007,41(7):2459-2466.
[40] Wang G H,Li J J,Cheng C L,et al. Observation of atmospheric aerosols at Mt. Hua and Mt. Tai in central and east China during spring 2009-part 2:Impact of dust storm on organic aerosol composition and size distribution[J]. Atmospheric Chemistry and Physics 2012,12:4065-4080.
[41] Garg A K,Kim J K,Owens T G,et al. Trehalose accumulation in rice plants confers high tolerance levels to different abiotic stresses[J]. Proceedings of the National Academy of Sciences of the United States of America,2002,99(25):15898-15903.
[42] Bauer H,Claeys M,Vermeylen R,et al. Arabitol and mannitol as tracers for the quantification of airborne fungal spores[J].Atmospheric Environment,2008,42(3):588-593.
[43]梁林林,Engling G,段凤魁,等.北京市大气气溶胶中糖类化合物的组成及来源[J].环境科学,2015,36(11):3935-3942.Liang L L,Engling G,Duan F K,et al. Composition and source apportionments of saccharides in atmospheric particulate matter in Beijing[J]. Environmental Science,2015,36(11):3935-3942.
[44] Pacini E. From anther and pollen ripening to pollen presentation[J]. Plant Systematics and Evolution,2000,222(1-4):19-43.
[2] Huang R J,Zhang Y L,Bozzetti C,et al. High secondary aerosol contribution to particulate pollution during haze events in China[J]. Nature,2014,514(7521):218-222.
[3] Meng J J,Wang G H,Li J J,et al. Seasonal characteristics of oxalic acid and related SOA in the free troposphere of Mt. Hua,central China:implications for sources and formation mechanisms[J]. Science of the Total Environment,2014,493:1088-1097.
[4]李杏茹,杜熙强,王英锋,等.保定市大气气溶胶中正构烷烃的污染水平及来源识别[J].环境科学,2013,34(2):441-447.Li X R,Du X Q,Wang Y F,et al. Pollution characteristics and source identification of atmospheric particulate matters n-alkanes in Baoding city[J]. Environmental Science,2013,34(2):441-447.
[5] Simoneit B R T. The organic chemistry of marine sediments[J].Chemical Oceanography,1978,7:233-311.
[6] 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(1967),1984,18(1):51-67.
[7] Simoneit B R T. Application of molecular marker analysis to reconcile sources of carbonaceous particulates in tropospheric aerosols[J]. Science of the Total Environment,1984,36:61-72.
[8] 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.
[9] Rogge W F,Hildemann L M,Mazurek M A,et al. Sources of fine organic aerosol. 3. Road dust, tire debris, and organometallic brake lining dust:roads as sources and sinks[J].Environmental Science&Technology,1993,27(9):1892-1904.
[10] Rogge W F,Hildemann L M,Mazurek M A,et al. Sources of fine organic aerosol. 4. Particulate abrasion products from leaf surfaces of urban plants[J]. Environmental Science&Technology,1993,27(13):2700-2711.
[11] Rogge W F,Hildemann L M,Mazurek M A,et al. Sources of fine organic aerosol. 1. Charbroilers and meat cooking operations[J]. Environmental Science&Technology,1991,25(6):1112-1125.
[12] Wang G H,Kawamura K,Lee S,et al. Molecular,seasonal,and spatial distributions of organic aerosols from fourteen Chinese cities[J]. Environmental Science&Technology,2006,40(15):4619-4625.
[13] Zhang J M,Yang L X,Chen J M,et al. Influence of fireworks displays on the chemical characteristics of PM2. 5in rural and suburban areas in Central and East China[J]. Science of the Total Environment,2016,578:476-484.
[14]张敬巧,吴亚君,张萌,等.聊城冬季一重污染过程PM2. 5污染特征及成因分析[J].环境科学,2018,39(9):4026-4033.Zhang J Q, Wu Y J, Zhang M, et al. PM2. 5Pollution characterization and cause analysis of a winter heavy pollution event,Liaocheng City[J]. Environmental Science,2018,39(9):4026-4033.
[15]张敬巧,王淑兰,罗达通,等.聊城市冬季PM2. 5及水溶性离子污染特征及来源分析[J].环境科学研究,2018,doi:10. 13198/j. issn. 1001-6929. 2017. 04. 22.Zhang J Q,Wang S L,Luo D T,et al. Characterization and source analysis of PM2. 5and water-soluble ions during winter in Liaocheng[J]. Research of Environmental Science,2018,doi:10. 13198/j. issn. 1001-6929. 2017. 04. 22.
[16] Yang L X,Gao X M,Wang X F,et al. Impacts of firecracker burning on aerosol chemical characteristics and human health risk levels during the Chinese New Year Celebration in Jinan,China[J]. Science of the Total Environment,2014,476-477:57-64.
[17] Tian Y Z,Wang J,Peng X,et al. Estimation of the direct and indirect impacts of fireworks on the physicochemical characteristics of atmospheric PM10and PM2. 5[J]. Atmospheric Chemistry and Physics,2014,14(18):9469-9479.
[18]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 of2007 in Beijing[J]. Environmental Science,2009,30(2):589-593.
[19] Wang G H,Kawamura K,Xie M J,et al. Selected water-soluble organic compounds found in size-resolved aerosols collected from urban,mountain and marine atmospheres over East Asia[J].Tellus,2011,63(3):371-381.
[20] Kong S F,Li L,Li X X,et al. The impacts of firework burning at the Chinese Spring Festival on air quality:insights of tracers,source evolution and aging processes[J]. Atmospheric Chemistry and Physics,2015,15(4):2167-2184.
[21] Li Y S,Cao J J,Li J J,et al. Molecular distribution and seasonal variation of hydrocarbons in PM2. 5from Beijing during2006[J]. Particuology,2013,11(1):78-85.
[22] Feng J L,Hu J C,Xu B H,et al. Characteristics and seasonal variation of organic matter in PM2. 5at a regional background site of the Yangtze River Delta region, China[J]. Atmospheric Environment,2015,123:288-297.
[23] Gu Z P,Feng J L,Han W L,et al. Characteristics of organic matter in PM2. 5from an e-waste dismantling area in Taizhou,China[J]. Chemosphere,2010,80(7):800-806.
[24] Li J J,Wang G H,Aggarwal S G,et al. Comparison of abundances,compositions and sources of elements, inorganic ions and organic compounds in atmospheric aerosols from Xi'an and New Delhi,two megacities in China and India[J]. Science of the Total Environment,2014,476-477:485-495.
[25] Simoneit B R T,Cox R E,Standley L J. Organic matter of the troposphere-IV. Lipids in harmattan aerosols of Nigeria[J].Atmospheric Environment(1967),1988,22(5):983-1004.
[26] Simoneit B R T,Sheng G Y,Chen X J,et al. Molecular marker study of extractable organic matter in aerosols from urban areas of China[J]. Atmospheric Environment. Part A. General Topics,1991,25(10):2111-2129.
[27] Simoneit B R T,Kobayashi M,Mochida M,et al. Aerosol particles collected on aircraft flights over the northwestern Pacific region during the ACE-Asia campaign:Composition and major sources of the organic compounds[J]. Journal of Geophysical Research,2004,109(D19):D19S09.
[28] Li X R,Guo X Q,LIU X R,et al. Distribution and sources of solvent extractable organic compounds in PM2. 5during 2007Chinese Spring Festival in Beijing[J]. Journal of Environmental Science,2009,21(2):142-149.
[29]李曼,仲勉,荆亮,等.上海PM2. 5中糖类化合物的组成及来源分析[J].上海大学学报(自然科学版),2013,19(4):387-392.Li M,Zhong M,Jing L,et al. Concentrations and sources of saccharides in PM2. 5in Shanghai[J]. Journal of Shanghai University(Natural Science),2013,19(4):387-392.
[30]黄绪,郭云霞,刘剑斌,等.柳州大气PM2. 5中糖类物质的分布特征与指示意义[J].中国环境科学,2017,37(3):838-843.Huang X, Guo Y X, Liu J B, et al. The distribution characteristics and implications of carbohydrates in the PM2. 5of Liuzhou[J]. China Environmental Science,2017,37(3):838-843.
[31] Simoneit B R T,Elias V O. Organic tracers from biomass burning in atmospheric particulate matter over the ocean[J].Marine Chemistry,2000,69(3-4):301-312.
[32] 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.
[33] Simoneit B R T. Biomass burning—a review of organic tracers for smoke from incomplete combustion[J]. Applied Geochemistry,2002,17(3):129-162.
[34] Simoneit B R T. A review of biomarker compounds as source indicators and tracers for air pollution[J]. Environmental Science and Pollution Research,1999,6(3):159-169.
[35] Engling G, Lee J J, Tsai Y W, et al. Size-resolved anhydrosugarcomposition in smoke aerosol from controlled field burning of rice straw[J]. Aerosol Science and Technology,2009,43(7):662-672.
[36] Oros D R,Abas M R B,Omar N Y M J,et al. Identification and emission factors of molecular tracers in organic aerosols from biomass burning:Part 3. Grasses[J]. Applied Geochemistry,2006,21(6):919-940.
[37] JaegerⅢC H,Lindow S E,Miller W,et al. Mapping of sugar and amino acid availability in soil around roots with bacterial sensors of sucrose and tryptophan[J]. Applied and Environmental Microbiology,1999,65(6):2685-2690.
[38] Speranza A,Calzoni G L,Pacini E. Occurrence of mono-or disaccharides and polysaccharide reserves in mature pollen grains[J]. Sexual Plant Reproduction,1997,10(2):110-115.
[39] Wan E C H,Yu J Z. Analysis of sugars and sugar polyols in atmospheric aerosols by chloride attachment in liquid chromatography/negative ion electrospray mass spectrometry[J].Environmental Science&Technology,2007,41(7):2459-2466.
[40] Wang G H,Li J J,Cheng C L,et al. Observation of atmospheric aerosols at Mt. Hua and Mt. Tai in central and east China during spring 2009-part 2:Impact of dust storm on organic aerosol composition and size distribution[J]. Atmospheric Chemistry and Physics 2012,12:4065-4080.
[41] Garg A K,Kim J K,Owens T G,et al. Trehalose accumulation in rice plants confers high tolerance levels to different abiotic stresses[J]. Proceedings of the National Academy of Sciences of the United States of America,2002,99(25):15898-15903.
[42] Bauer H,Claeys M,Vermeylen R,et al. Arabitol and mannitol as tracers for the quantification of airborne fungal spores[J].Atmospheric Environment,2008,42(3):588-593.
[43]梁林林,Engling G,段凤魁,等.北京市大气气溶胶中糖类化合物的组成及来源[J].环境科学,2015,36(11):3935-3942.Liang L L,Engling G,Duan F K,et al. Composition and source apportionments of saccharides in atmospheric particulate matter in Beijing[J]. Environmental Science,2015,36(11):3935-3942.
[44] Pacini E. From anther and pollen ripening to pollen presentation[J]. Plant Systematics and Evolution,2000,222(1-4):19-43.