东北亚冬季PM_(2.5)水溶性离子空间分布特征及来源
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摘要
为探讨东北亚冬季PM_(2.5)水溶性离子空间分布特征及来源,测定了2017～2018年沈阳冬季PM_(2.5)水溶性离子浓度.结果显示:沈阳冬季PM_(2.5)水溶性离子平均质量浓度为28.5±11.9μg/m~3,二次离子(SO_4~(2-)、NO_3~-和NH_4~+)的浓度最高,分别占总水溶性离子质量浓度的31.0%、22.4%和19.2%.运用离子化学计量学关系、相关性和主成分分析,探讨了沈阳冬季PM_(2.5)水溶性离子的可能来源.并整合了东北亚冬季(中国东北、韩国、日本)近20a来PM_(2.5)水溶性离子数据,发现沿着东亚冬季风,东北亚冬季PM_(2.5)水溶性离子浓度从中国东北,经韩国海岸、韩国和济州岛,日本海岸至日本整体呈下降趋势,在韩国和日本出现局部上升,且在不同区域,不同水溶性离子占比明显不同.其中,韩国冬季PM_(2.5)中SO_4~(2-)、Ca~(2+)和K~+受外来源影响显著,NO_3~-和NH_4~+主要来自本地源,Cl~-、Na~+和Mg~(2+)主要来自本地源或海源;日本中部冬季PM_(2.5)中SO_4~(2-)、NO_3~-、NH_4~+和K~+主要来自本地源,Cl~-、Ca~(2+)、Na~+和Mg~(2+)主要来自本地源或海源.
To explore the spatial distribution and sources of water-soluble ions in winter PM_(2.5) of Northeast Asia,we determined the concentrations of PM_(2.5) water-soluble ions in Shenyang during winter of 2017～2018.The concentrations of the total water-soluble ions in winter PM_(2.5) of Shenyang was(28.5±11.9)μg/m~3,and the concentrations of secondary ions(SO_4~(2-)、NO_3~-、NH_4~+)were the highest,accounting for 31.0%,22.4%and 19.2%of total water-soluble ions in mass fraction.We investigated the sources of winter PM_(2.5) water-soluble ions in Shenyang by the ion stoichiometry,correlation analysis of water-soluble ions and primary component analysis.By combining our results with previously reported data in Northeast Asia region(northeast China,South Korea and Japan)in recent 20years,we found a downwind decreasing pattern in concentrations of winter PM_(2.5) water-soluble ions from the northeast China,through the South Korea,coastal South Korea and Jeju Island,and the coast of Japan to Japan except some peaks at stations near densely populated areas(e.g.,South Korea and Japan).Water-soluble ions showed significant regional differences in percentage of mass fraction in the total water-soluble ions in PM_(2.5).In the winter PM_(2.5) of South Korea,SO_4~(2-),Ca~(2+)and K~+were significantly affected by external sources.NO_3~-and NH_4~+were mainly from local sources,while Cl~-,Na~+and Mg~(2+)were dominantly sourced from local sources or sea salt.In Central Japan,SO_4~(2-),NO_3~-,NH_4~+,Ca~(2+)and K~+were originated from local sources,while Cl~-,Na~+and Mg~(2+)were dominantly sourced from local sources or sea salt.
To explore the spatial distribution and sources of water-soluble ions in winter PM_(2.5) of Northeast Asia,we determined the concentrations of PM_(2.5) water-soluble ions in Shenyang during winter of 2017～2018.The concentrations of the total water-soluble ions in winter PM_(2.5) of Shenyang was(28.5±11.9)μg/m~3,and the concentrations of secondary ions(SO_4~(2-)、NO_3~-、NH_4~+)were the highest,accounting for 31.0%,22.4%and 19.2%of total water-soluble ions in mass fraction.We investigated the sources of winter PM_(2.5) water-soluble ions in Shenyang by the ion stoichiometry,correlation analysis of water-soluble ions and primary component analysis.By combining our results with previously reported data in Northeast Asia region(northeast China,South Korea and Japan)in recent 20years,we found a downwind decreasing pattern in concentrations of winter PM_(2.5) water-soluble ions from the northeast China,through the South Korea,coastal South Korea and Jeju Island,and the coast of Japan to Japan except some peaks at stations near densely populated areas(e.g.,South Korea and Japan).Water-soluble ions showed significant regional differences in percentage of mass fraction in the total water-soluble ions in PM_(2.5).In the winter PM_(2.5) of South Korea,SO_4~(2-),Ca~(2+)and K~+were significantly affected by external sources.NO_3~-and NH_4~+were mainly from local sources,while Cl~-,Na~+and Mg~(2+)were dominantly sourced from local sources or sea salt.In Central Japan,SO_4~(2-),NO_3~-,NH_4~+,Ca~(2+)and K~+were originated from local sources,while Cl~-,Na~+and Mg~(2+)were dominantly sourced from local sources or sea salt.
引文
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[35]周胜杰,张洪海,杨桂朋.东海PM2.5和PM10中水溶性离子的组成与化学特性[J].中国环境科学,2018,38(3):900-909.Zhou S J,Zhang H M,Yang G P,et al.Distributions and chemical characteristics of water soluble ions in PM2.5 and PM10 over the East China Sea[J].China Environmental Science,2018,38(3):900-909.
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[38]Ryu S Y,Kwon B G,Kim Y J,et al.Characteristics of biomass burning aerosol and its impact on regional air quality in the summer of 2003 at Gwangju,Korea[J].Atmospheric Research,2007,84(4):362-373.
[39]罗笠,高树基,肖化云,等.台湾彭佳屿岛春季TSP中水溶性离子源解析[J].中国环境科学,2017,37(12):4452-4459.Luo L,Gao S J,Xiao H Y,et al.Source apportionment of water-soluble ions in spring TSP of Pengjia Islet,Taiwan[J].China Environmental Science,2017,37(12):4452-4459.
[40]Kang G U,Kim N S,Shin E S.Seasonal Characteristics of Atmospheric PM10 and PM2.5 in Iksan,Korea[J].Korean Journal of Environmental Health,2011,37(1):29-43.
[2]Liu J,Han Y,Tang X,et al.Estimating adult mortality attributable to PM2.5 exposure in China with assimilated PM2.5 concentrations based on a ground monitoring network[J].Science of the Total Environment,2016,568(5):1253-1262.
[3]Hong X U,Chen J Q,Dou-Tai H E,et al.Climatic characteristics of haze weather during heating periods from 1980 to 2015 at Shenyang region[J].Journal of Meteorology&Environment,2017,33(2):87-94.
[4]Hong Y,Li C,Li X,et al.Analysis of Compositional Variation and Source Characteristics of Water-Soluble Ions in PM2.5 during Several Winter-Haze Pollution Episodes in Shenyang,China[J].Atmosphere,2018,9(7):280.
[5]张云海,王扬锋,洪也,等.冬季典型灰霾天气过程的特征分析[J].安徽农业科学,2010,38(15):8016-8017.Zhang Y H,Wang Y F,Hong Y,et al.Analysis on the characteristics of a typical haze weather process in winter[J].Journal of Anhui Agricultural Sciences,2010,38(15):8016-8017.
[6]Calvo A I,Alves C,Castro A,et al.Research on aerosol sources and chemical composition:Past,current and emerging issues[J].Atmospheric Research,2013,120-121(5):1-28.
[7]Lee J H,Yong P K,Moon K C,et al.Fine particle measurements at two background sites in Korea between 1996 and 1997[J].Atmospheric Environment,2001,35(4):635-643.
[8]Cao J J,Shen Z X,Chow J C,et al.Winter and summer PM2.5chemical compositions in fourteen Chinese cities[J].Journal of the Air&Waste Management Association,2012,62(10):1214-1226.
[9]张蕾,姬亚芹,王士宝,等.盘锦市冬季PM2.5水溶性离子特征及来源分析[J].环境科学,2018,39(6):2527-2527.Zhang L,Ji Y Q,Wang S B,et al.Characteristics and source apportionment of water-soluble ions in PM2.5 during winter in Panjin[J].Environmental Science,2018,39(6):2527-2527.
[10]Sekine Y,Takahashi N,Ohkoshi Y,et al.Measurement of PM2.5 and Water-Soluble Ions at Central Tokyo,Japan and Source Apportionment[J].The Global Environmental Engineers,2015,2(2):71-78.
[11]Khan M F,Shirasuna Y,Hirano K,et al.Characterization of PM in ambient air,Yokohama,Japan[J].Atmospheric Research,2010,96(1):159-172.
[12]赵亚南,王跃思,温天雪,等.长白山PM2.5中水溶性离子季节变化特征研究[J].环境科学,2014,35(1):9-14.Zhao Y N,Wang Y S,Wen T X,et al.Seasonal variation of water-soluble ions in PM2.5 at Changbai Mountain[J].Environmental Science,2014,35(1):9-14.
[13]唐孝炎,张远航,邵敏.大气环境化学[M].北京:高等教育出版社,2006:164-169.Tang X Y,Zhang Y H,Shao M.Atmospheric environmental chemistry[M].Beijing:Higher Education Press,2006:164-169.
[14]Gao X,Yang L,Cheng S,et al.Semi-continuous measurement of water-soluble ions in PM2.5 in Jinan,China:Temporal variations and source apportionments[J].Atmospheric Environment,2011,45(33):6048-6056.
[15]苗红妍,温天雪,王璐,等.沈阳大气气溶胶中水溶性无机离子的观测研究[J].环境科学,2016,37(6):2017-2024.Miao H Y,Wen T X,Wang L,et al.Characteristics of water-soluble inorganic ions in atmospheric aerosols in Shenyang[J].Environmental Science,2016,37(6):2017-2024.
[16]Shon Z H,Kim K H,Song S K,et al.Relationship between watersoluble ions in PM2.5 and their precursor gases in Seoul megacity[J].Atmospheric Environment,2012,59(7):540-550.
[17]曲健,李晶,张晶,等.沈阳城区采暖期PM2.5中水溶性离子的化学特征[J].中国环境监测,2015,31(5):57-60.Qu J,Li J,Zhang J,et al.chemica Character of water-soluble ions in PM2.5 in Shenyang City during heating season[J].Environmental Monitoring in China,2015,31(5):57-60.
[18]田景芝,吕健,郑永杰,等.齐齐哈尔市PM2.5中水溶性离子的测定及来源分析[J].科技通报,2016,32(8):221-226.Tian J Z,Lv J,Zheng Y J,et al.Determination and sources analysis of water-soluble ions in atmosphere environment PM2.5 of Qiqihar City[J].Bulletin of Science and Technology,2016,32(8):221-226.
[19]Kim W H,Hwang E Y,Ko H J,et al.Seasonal Composition Characteristics of TSP and PM2.5 Aerosols at Gosan Site of Jeju Island,Korea during 2008~2011[J].Asian Journal of Atmospheric Environment,2013,7(4):217-226.
[20]Choi J K,Heo J B,Ban S J,et al.Chemical characteristics of PM2.5aerosol in Incheon,Korea[J].Atmospheric Environment,2012,60(6):583-592.
[21]Li P,Sato K,Hasegawa H,et al.Chemical characteristics and source apportionment of PM2.5 and long-range transport from Northeast Asia continent to Niigata in Eastern Japan[J].Aerosol&Air Quality Research,2018,18(4):938-956.
[22]Murano K,Mukai H,Hatakeyama S,et al.Trans-boundary air pollution over remote islands in Japan:observed data and estimates from a numerical model[J].Atmospheric Environment,2000,34(29/30):5139-5149.
[23]Ichikawa Y,Naito S,Oohashi H,et al.Seasonal Variation of PM2.5Components Observed in an Industrial Area of Chiba Prefecture,Japan[J].Asian Journal of Atmospheric Environment,2015,9(1):66-77.
[24]Kim B G,Park S U.Transport and evolution of a winter-time Yellow sand observed in Korea[J].Atmospheric Environment,2001,35(18):3191-3201.
[25]Saitoh K,Sera K,Shirai T.Characterization of atmospheric aerosol particles in a mountainous region in northern Japan[J].Atmospheric Research,2008,89(4):324-329.
[26]陈敏.化学海洋学[M].北京:海洋出版社,2009:18-19.Cheng M.Chemical oceanography[M].Beijing:China Ocean Press,2009:18-19.
[27]田莎莎,张显,卞思思,等.沈阳市PM2.5污染组分特征及其来源解析[J].中国环境科学,2019,39(2):487-496.Tian S S,Zhang X,Bian S S,et al.Characteristics of PM2.5 pollution components and their sources in Shenyang[J].China Environmental Science,2019,39(2):487-496.
[28]Zhang T,Cao J J,Tie X X,et al.Water-soluble ions in atmospheric aerosols measured in Xi'an,China:Seasonal variations and sources[J].Atmospheric Research,2011,102(1):110-119.
[29]Hsu,Shih-Chieh,Lee C S L,et al.Ammonium deficiency caused by heterogeneous reactions during a super Asian dust episode[J].Journal of Geophysical Research Atmospheres,2014,119(11):6803-6817.
[30]Luo L,Yao X H,Gao H W,et al.Nitrogen speciation in various types of aerosol in spring over the northwestern Pacific Ocean[J].Atmospheric Chemistry&Physics,2016,16(1):325-341.
[31]黄世鸿,李如祥,沈恒华,等.常州市大气气溶胶颗粒来源解析[J].气象科学,1995,15(2):92-100.Huang S H,Li R X,Shen H H,et al.Analysis of atmospheric aerosol particle source in Changzhou[J].Scientia Meteorologica Sinica,1995,15(2):92-100.
[32]黄辉军,刘红年,蒋维楣,等.南京市PM2.5物理化学特性及来源解析[J].气候与环境研究,2006,11(6):713-722.Huang H J,Liu H N,Jiang W M,et al.Physical and chemical characteristics and source apportionment of PM2.5 in Nanjing[J].Climatic and Environmental Research,2006,11(6):713-722.
[33]余南娇,黄渤,李梅,等.大气细颗粒物扬尘源单颗粒质谱特征[J].中国环境科学,2017,37(4):1262-1268.Yu N J,Huang B,Li M,et al.Single particle characteristics of fine particulate matter in dust[J].China Environmental Science,2017,37(4):1262-1268.
[34]Taylor S R,Mclennan S M.The geochemical evolution of the continental crust[J].Reviews of Geophysics,1995,33(2):241-265.
[35]周胜杰,张洪海,杨桂朋.东海PM2.5和PM10中水溶性离子的组成与化学特性[J].中国环境科学,2018,38(3):900-909.Zhou S J,Zhang H M,Yang G P,et al.Distributions and chemical characteristics of water soluble ions in PM2.5 and PM10 over the East China Sea[J].China Environmental Science,2018,38(3):900-909.
[36]Seinfeld J H,Pandis S N,Noone K,et al.Atmospheric chemistry and physics:from air pollution to climate change[J].Environment Science&Policy for Sustainable Development,1998,40(7):26-26.
[37]Hsu S C,Liu S C,Huang Y T,et al.Long-range southeastward transport of Asian biosmoke pollution:Signature detected by aerosol potassium in Northern Taiwan[J].Journal of Geophysical Research Atmospheres,2009,114(D14):1159-1171.
[38]Ryu S Y,Kwon B G,Kim Y J,et al.Characteristics of biomass burning aerosol and its impact on regional air quality in the summer of 2003 at Gwangju,Korea[J].Atmospheric Research,2007,84(4):362-373.
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