常州春季PM_(2.5)中WSOC和WSON的污染特征与来源解析
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摘要
为了解常州春季大气气溶胶中水溶性有机碳(WSOC)和有机氮(WSON)的特点和来源,在常州市城郊于2017年春季的3月1日~5月30日采集了84个细颗粒物(PM_(2.5))样品.分析了其中的水溶性组分包括水溶性有机碳、水溶性总氮(WSTN)、水溶性离子以及碳质组分(有机碳/元素碳,OC/EC)的浓度,探讨了WSOC和WSON的浓度水平及其来源.结果表明,采样期间,PM_(2.5)、WSOC和WSON日平均浓度分别为101.97、7.63和1.50μg·m~(-3).其中,WSON占WSTN的12.9%,水溶性无机氮主要以NH+4、NO-3两种形式存在,两者占WSTN的86.15%.WSOC与WSON弱相关(r=0.58),说明WSOC和WSON来源并不完全一致.WSOC与SOC、K+、二次离子(SO2-4、NH+4和NO-3)相关,说明WSOC主要来自生物质燃烧和二次转化;WSON与二次离子相关性强,说明主要来自二次转化.风速是影响WSOC和WSON浓度水平的主要因素,WSON与大气压正相关且与温度负相关.主成分分析结果表明,PM_(2.5)主要来自二次形成、扬尘和燃煤、生物质燃烧、海洋等4个来源.后向轨迹分析表明,长距离传输方向气团中PM_(2.5)和WSOC、WSON总浓度高于短距离传输,但不同传输路径中WSON/WSTN占比无明显差异.
To understand the characteristics and sources of water-soluble organic carbon(WSOC) and organic nitrogen(WSON) in atmospheric aerosols during spring in Changzhou,84 fine particle(PM_(2.5)) samples were collected from March 1 to May 30,2017,in Changzhou.The water-soluble components,including water-soluble organic carbon,water-soluble total nitrogen(WSTN),watersoluble ions,and carbonaceous components(OC and EC),were analyzed.The levels of WSOC and WSON and their source characteristics were discussed.The results show that the average concentrations of PM_(2.5),WSOC,and WSON are 101.97,7.63,and1.50 μg·m~(-3),respectively,during the sampling period.The WSON accounts for 12.9% of the WSTN and the water-soluble inorganic nitrogen mainly exists in two forms,that is,NH+4 and NO-3,accounting for 86.15% of the WSTN.The WSOC is weakly correlated with WSON(r=0.58),indicating that WSOC and WSON do not have the same sources.The WSOC is related to SOC,K+,and secondary ions(SO2-4,NH+4,and NO-3),indicating that it is mainly derived from biomass burning and secondary conversion;WSON is strongly correlated to secondary ions,indicating that it is mainly derived from secondary conversion.The wind speed is the main factor affecting the WSOC and WSON concentration levels.Furthermore,the WSON is positively correlated with the air pressure and negatively correlated with the temperature.The results of the principal component analysis show that PM_(2.5) mainly originates from four sources:secondary formation,dust,coal combustion,biomass burning,and the ocean.The backward trajectory analysis indicates that the total concentrations of PM_(2.5),WSOC,and WSON in air masses from long-distance transformation are higher than that from shortdistance transmission,whereas there is no significant difference in the WSON/WSTN ratio from different transmission paths.
To understand the characteristics and sources of water-soluble organic carbon(WSOC) and organic nitrogen(WSON) in atmospheric aerosols during spring in Changzhou,84 fine particle(PM_(2.5)) samples were collected from March 1 to May 30,2017,in Changzhou.The water-soluble components,including water-soluble organic carbon,water-soluble total nitrogen(WSTN),watersoluble ions,and carbonaceous components(OC and EC),were analyzed.The levels of WSOC and WSON and their source characteristics were discussed.The results show that the average concentrations of PM_(2.5),WSOC,and WSON are 101.97,7.63,and1.50 μg·m~(-3),respectively,during the sampling period.The WSON accounts for 12.9% of the WSTN and the water-soluble inorganic nitrogen mainly exists in two forms,that is,NH+4 and NO-3,accounting for 86.15% of the WSTN.The WSOC is weakly correlated with WSON(r=0.58),indicating that WSOC and WSON do not have the same sources.The WSOC is related to SOC,K+,and secondary ions(SO2-4,NH+4,and NO-3),indicating that it is mainly derived from biomass burning and secondary conversion;WSON is strongly correlated to secondary ions,indicating that it is mainly derived from secondary conversion.The wind speed is the main factor affecting the WSOC and WSON concentration levels.Furthermore,the WSON is positively correlated with the air pressure and negatively correlated with the temperature.The results of the principal component analysis show that PM_(2.5) mainly originates from four sources:secondary formation,dust,coal combustion,biomass burning,and the ocean.The backward trajectory analysis indicates that the total concentrations of PM_(2.5),WSOC,and WSON in air masses from long-distance transformation are higher than that from shortdistance transmission,whereas there is no significant difference in the WSON/WSTN ratio from different transmission paths.
引文
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[3]Duarte R M B O,Freire S M S C,Duarte A C.Investigating the water-soluble organic functionality of urban aerosols using twodimensional correlation of solid-state13C NMR and FTIR spectral data[J].Atmospheric Environment,2015,116:245-252.
[4]Saxena P,Hildemann L M,Mcmurry P H,et al.Organics alter hygroscopic behavior of atmospheric particles[J].Journal of Geophysical Research:Atmospheres,1995,100(D9):18755-18770.
[5]PadróL T,Tkacik D,Lathem T,et al.Investigation of cloud condensation nuclei properties and droplet growth kinetics of the water-soluble aerosol fraction in Mexico City[J].Journal of Geophysical Research:Atmospheres,2010,115(D9):D09204.
[6]霍宗权,沈振兴,田晶,等.西安市大气PM10中水溶性有机碳的季节变化及来源分析[J].西安交通大学学报,2010,44(9):128-132.Huo Z Q,Shen Z X,Tian J,et al.Seasonal variation and source identification of water-soluble organic carbon in PM10over Xi'an,China[J].Journal of Xi'an Jiaotong University,2010,44(9):128-132.
[7]胡淑圆,谢鸣捷,王格慧,等.宝鸡市大气PM10中水溶性物质的组成及特征研究[J].环境污染与防治,2010,32(3):34-38.Hu S Y,Xie M J,Wang G H,et al.Component and characteristics of water-soluble species in PM10aerosol of Baoji[J].Environmental Pollution and Control,2010,32(3):34-38.
[8]黄众思,修光利,蔡婧,等.大气PM2.5中水溶性有机碳和类腐殖质碳的季节变化特征[J].环境科学学报,2013,33(10):2664-2670.Huang Z S,Xiu G L,Cai J,et al.Seasonal characterization of water-soluble organic carbon and humic-like substance carbon in atmospheric PM2.5[J].Acta Scientiae Circumstantiae,2013,33(10):2664-2670.
[9]Montero-Martínez G,Rinaldi M,Gilardoni S,et al.On the water-soluble organic nitrogen concentration and mass size distribution during the fog season in the Po Valley,Italy[J].Science of the Total Environment,2014,485-486:103-109.
[10]Chen H Y,Chen L D,Chiang Z Y,et al.Size fractionation and molecular composition of water-soluble inorganic and organic nitrogen in aerosols of a coastal environment[J].Journal of Geophysical Research:Atmospheres,2010,115(D22):D22307.
[11]Lin M,Walker J,Geron C,et al.Organic nitrogen in PM2.5aerosol at a forest site in the Southeast US[J].Atmospheric Chemistry and Physics,2010,10(5):2145-2157.
[12]Shi JH,Gao H W,Qi J H,et al.Sources,compositions,and distributions of water-soluble organic nitrogen in aerosols over the China Sea[J].Journal of Geophysical Research:Atmospheres,2010,115(D17):D17303.
[13]Cape J N,Cornell S E,Jickells T D,et al.Organic nitrogen in the atmosphere-Where does it come from?A review of sources and methods[J].Atmospheric Research,2011,102(1-2):30-48.
[14]Reyes-Rodríguez G J,Gioda A,Mayol-Bracero O L,et al.Organic carbon,total nitrogen,and water-soluble ions in clouds from a tropical montane cloud forest in Puerto Rico[J].Atmospheric Environment,2009,43(27):4171-4177.
[15]Hu D W,Li C L,Chen H,et al.Hygroscopicity and optical properties of alkylaminium sulfates[J].Journal of Environmental Sciences,2014,26(1):37-43.
[16]Ansari A S,Pandis S N.Water absorption by secondary organic aerosol and its effect on inorganic aerosol behavior[J].Environmental Science&Technology,2000,34(1):71-77.
[17]González Benítez J M,Cape J N,Heal M R.Gaseous and particulate water-soluble organic and inorganic nitrogen in rural air in southern Scotland[J].Atmospheric Environment,2010,44(12):1506-1514.
[18]Violaki K,Mihalopoulos N.Water-soluble organic nitrogen(WSON)in size-segregated atmospheric particles over the Eastern Mediterranean[J].Atmospheric Environment,2010,44(35):4339-4345.
[19]徐玢花.上海PM2.5中水溶性有机氮的浓度特征和来源解析[D].上海:上海大学,2015.Xu B H.Characteristics and sources of water-soluble organic nitrogen in PM2.5in Shanghai,China[D].Shanghai:Shanghai University,2015.
[20]Ambonguilat S,Gallard H,Garron A,et al.Evaluation of the catalytic reduction of nitrate for the determination of dissolved organic nitrogen in natural waters[J].Water Research,2006,40(4):675-682.
[21]Andreae M O,Gelencsér A.Black carbon or brown carbon?The nature of light-absorbing carbonaceous aerosols[J].Atmospheric Chemistry and Physics,2006,6(10):3131-3148.
[22]Laskin A,Smith J S,Laskin J.Molecular characterization of nitrogen-containing organic compounds in biomass burning aerosols using high-resolution mass spectrometry[J].Environmental Science&Technology,2009,43(10):3764-3771.
[23]Samy S,Robinson J,Rumsey I C,et al.Speciation and trends of organic nitrogen in southeastern U.S.?ne particulate matter(PM2.5)[J].Journal of Geophysical Research:Atmospheres,2013,118(4):1996-2006.
[24]Rastogi N,Zhang X L,Edgerton E S,et al.Filterable watersoluble organic nitrogen in fine particles over the southeastern USA during summer[J].Atmospheric Environment,2011,45(33):6040-6047.
[25]zel M Z,Ward M W,Hamilton J F,et al.Analysis of organic nitrogen compounds in urban aerosol samples using GCxGC-TOF/MS[J].Aerosol Science and Technology,2010,44(2):109-116.
[26]Matsumoto K,Yamamoto Y,Kobayashi H,et al.Water-soluble organic nitrogen in the ambient aerosols and its contribution to the dry deposition of fixed nitrogen species in Japan[J].Atmospheric Environment,2014,95:334-343.
[27]Matsumoto K,Yamato K.Uncertainties in the measurements of water-soluble organic nitrogen in the aerosol[J].Atmospheric Environment,2016,144:220-225.
[28]Duan F K,Liu X D,He K B,et al.Measurements and characteristics of nitrogen-containing compounds in atmospheric particulate matter in Beijing,China[J].Bulletin of Environmental Contamination and Toxicology,2009,82(3):332-337.
[29]徐玢花,杜艳,胡俊超,等.上海PM2.5中水溶性有机氮的污染特征[J].地球化学,2016,45(2):190-198.Xu B H,Du Y,Hu J C,et al.Characteristics of water-soluble organic nitrogen in PM2.5in Shanghai[J].Geochimica,2016,45(2):190-198.
[30]Ho K F,Ho S S H,Huang R J,et al.Characteristics of watersoluble organic nitrogen in fine particulate matter in the continental area of China[J].Atmospheric Environment,2015,106:252-261.
[31]石金辉,韩静,范得国,等.青岛大气气溶胶中水溶性有机氮对总氮的贡献[J].环境科学,2011,32(1):1-8.Shi J H,Han J,Fan D G,et al.Contribution of water soluble organic nitrogen to total nitrogen in atmospheric aerosols in Qingdao[J].Environmental Science,2011,32(1):1-8.
[32]Nakamura T,Ogawa H,Maripi D K,et al.Contribution of water soluble organic nitrogen to total nitrogen in marine aerosols over the East China Sea and western North Pacific[J].Atmospheric Environment,2006,40(37):7259-7264.
[33]Ye Z L,Liu J S,Gu A J,et al.Chemical characterization of fine particulate matter in Changzhou,China,and source apportionment with offline aerosol mass spectrometry[J].Atmospheric Chemistry and Physics,17(4):2573-2592.
[34]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.
[35]刘佳澍,顾远,马帅帅,等.常州夏冬季PM2.5中无机组分昼夜变化特征与来源解析[J].环境科学,2018,39(3):980-989.Liu J S,Gu Y,Ma S S,et al.Day-night differences and source apportionment of inorganic components of PM2.5during summerwinter in Changzhou city[J].Environmental Science,2018,39(3):980-989.
[36]张桂香,闫雨龙,郭利利,等.太原市大气PM2.5中碳质组成及变化特征[J].环境科学,2015,36(3):780-786.Zhang G X,Yan Y L,Guo L L,et al.Composition and variation characteristics of atmospheric Carbonaceous species in PM2.5in Taiyuan,China[J].Environmental Science,2015,36(3):780-786.
[37]杜祯宇.北京市水溶性有机碳来源与光吸收特征研究[D].北京:清华大学,2014.Du Z Y.Research on the sources and optical properties of watersoluble organic carbon in Beijing[D].Beijing:Tsinghua University,2014.
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