天津市城市扬尘及土壤尘单颗粒质谱特征
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摘要
为探究城市扬尘及不同类型的土壤尘单颗粒质谱特征,使用SPAMS(单颗粒气溶胶质谱仪)对天津城市扬尘及不同类型土壤尘(菜地、果园、林地、农田)进行分析.结果表明:天津城市扬尘粒径在0.5~1.0μm之间的占比较高;4种土壤尘在不同粒径段的分布略有差异,整体而言小粒径段(0.2~1.0μm)占比低于大粒径段(1.0~2.0μm),说明土壤尘更易分布在大粒径段.在小粒径段,天津城市扬尘颗粒含有更多的碳组分及硫酸盐,大粒径段含有较多的金属、氯、硝酸盐、磷酸盐及硅酸盐组分.与城市扬尘相比,土壤尘中~(23)Na~+、~(46)NO_2~-峰强显著降低,~(39)K~+、~(35)Cl~-、~(42)CNO~-峰强增高,通过其峰强比值分布可将城市扬尘与土壤尘明显区分.与城市扬尘相比,土壤尘中含碳颗粒显著减少,同时出现钾类颗粒.城市扬尘作为一种混合源,含碳颗粒可能受多种排放源(机动车、燃煤等)影响,而土壤尘中钾类颗粒可能与农作物施肥有关.两种源类含~(27)Al~+、~(26)CN~-、~(35)Cl~-、~(42)CNO~-、~(46)NO_2~-、~(76)Si O_3~-、~(79)PO_3~-的颗粒占比均高于50%,其中~(40)Ca~+、~(46)NO_2~-和~(62)NO_3~-颗粒在天津城市扬尘中占比更高,~(76)Si O_3~-颗粒在土壤尘中占比更高,表明天津城市扬尘中更多的颗粒含有钙和硝酸盐组分,土壤尘中含硅酸盐颗粒较多.与机动车尾气、生物质燃烧等排放的颗粒物相比,天津城市扬尘及土壤尘中含~(97)HSO_4~-颗粒占比较低,表明天津城市扬尘及土壤尘颗粒中含有更少的硫酸盐,可作为将天津城市扬尘、土壤尘与其他源类区分的指标.
In order to investigate the characteristics of single urban raised dust and four types of soil dust( i.e.,vegetable,orchard,wood and cropland soils),single particle aerosol mass spectrometry( SPAMS) was used to analyze the characteristics. Results showed more urban raised dust appeared between 0. 5 and 1. 0 μm. Compared with other sources,the size distribution of four soil dust had slight differences. Generally speaking,the fraction of soil particle in the range of 0. 2-1. 0 μm was lower than 1. 0-2. 0 μm,indicating the soil dust prefer to concentrating in larger size. As for urban raised dust,more carbonaceous species and sulfate appear in smaller particle size,while more metal,chlorine,nitrate,phosphate and silicate in the larger size. Compared with urban raised dust,in soil dust,~(23)Na~+and~(46)NO_2~-intensified significantly,while~(39)K~+,~(35)Cl~-and~(42)CNO~- weakened,the urban raised dust and soil dust can be distinguished based on the distribution of the specific intensity ratios. Moreover,the classification results showed that the carbonaceous particles in soil dust decreased,while the K particles appeared. The urban raised dust was considered as a mixed source. The carbonaceous species particles in urban raised dust may from different sources such as vehicle and coal burning,and more K particles in soil dust may relate to the fertilization. Particles containing~(27)Al~+,~(26)CN~-,~(35)Cl~-,~(42)CNO~-,~(46)NO_2~-,~(76)Si O_3~-and ~(79)PO_3~-dominated( exceeding 50%) in both urban raised and soil dusts,with~(40)Ca~+,~(46)NO_2~-,~(22)NO_3~-obviously in urban raised dust and ~(76)SiO_3~- in soil dust,indicating more calcium andnitrate species in urban raised dust and more silicate in soil dust. Fewer ~(97)HSO_4~- particles showed limited sulfate in urban raised dust and soil dust,which can be the tracer to differentiate from other sources.
In order to investigate the characteristics of single urban raised dust and four types of soil dust( i.e.,vegetable,orchard,wood and cropland soils),single particle aerosol mass spectrometry( SPAMS) was used to analyze the characteristics. Results showed more urban raised dust appeared between 0. 5 and 1. 0 μm. Compared with other sources,the size distribution of four soil dust had slight differences. Generally speaking,the fraction of soil particle in the range of 0. 2-1. 0 μm was lower than 1. 0-2. 0 μm,indicating the soil dust prefer to concentrating in larger size. As for urban raised dust,more carbonaceous species and sulfate appear in smaller particle size,while more metal,chlorine,nitrate,phosphate and silicate in the larger size. Compared with urban raised dust,in soil dust,~(23)Na~+and~(46)NO_2~-intensified significantly,while~(39)K~+,~(35)Cl~-and~(42)CNO~- weakened,the urban raised dust and soil dust can be distinguished based on the distribution of the specific intensity ratios. Moreover,the classification results showed that the carbonaceous particles in soil dust decreased,while the K particles appeared. The urban raised dust was considered as a mixed source. The carbonaceous species particles in urban raised dust may from different sources such as vehicle and coal burning,and more K particles in soil dust may relate to the fertilization. Particles containing~(27)Al~+,~(26)CN~-,~(35)Cl~-,~(42)CNO~-,~(46)NO_2~-,~(76)Si O_3~-and ~(79)PO_3~-dominated( exceeding 50%) in both urban raised and soil dusts,with~(40)Ca~+,~(46)NO_2~-,~(22)NO_3~-obviously in urban raised dust and ~(76)SiO_3~- in soil dust,indicating more calcium andnitrate species in urban raised dust and more silicate in soil dust. Fewer ~(97)HSO_4~- particles showed limited sulfate in urban raised dust and soil dust,which can be the tracer to differentiate from other sources.
引文
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[29]SANDERS P G,XU Ning,DALKA T M,et al.Airborne brake wear debris:size distributions,composition,and a comparison of dynamometer and vehicle tests[J].Environmental Science and Technology,2003,37:4060-4069.
[2]LI X,MARING H,SAVOIE D,et al.Dominance of mineral dust in aerosol light-scattering in the North Atlantic trade winds[J].Nature,1996,380(6573):416-419.
[3]TEGEN I,LACIS A A,FUNG I.The influence on climate forcing of mineral aerosols from disturbed soils[J].Nature,1996,380:419-422.
[4]黄玉虎,曲松,宋光武,等.扬尘源粒度组成筛分方法比较[J].环境科学研究,2013,26(5):522-526.HUANG Yuhu,QU Song,SONG Guangwu,et al.Comparison of screening methods of size distribution of fugitive dust source[J].Research of Environmental Sciences,2013,26(5):522-526.
[5]CAI Jing,ZHENG Mei,YAN Caiqing,et al.Application and progress of single particle aerosol time-of-flight mass spectrometry in fine particulate matter research[J].Chinese Journal of Analytical Chemistry,2015,43(5):765-774.
[6]WANG Honglei,AN Junlin,SHEN Lijuan,et al.Mechanism for the formation and microphysical characteristics of submicron aerosol during heavy haze pollution episode in the Yangtze River Delta,China[J].Science of the Total Environment,2014,490:501-508.
[7]ZHANG Y M,ZHANG X Y,SUN J Y,et al.Chemical composition and mass size distribution of PM1at an elevated site in central east China[J].Atmospheric Chemistry and Physics,2014,14(22):12237-12249.
[8]陈多宏,何俊杰,张国华,等.不同天气类型广东大气超级站细粒子污染特征初步研究[J].地球化学,2014,43(3):217-223.CHEN Duohong,HE Junjie,ZHANG Guohua,et al.Preliminary study on the characteristics of fine particle pollution characteristicsfor different weather type in the Guangdong atmospheric supersite[J].Geochimica,2014,43(3):217-223.
[9]杜娟,宋韶华,张志朋,等.桂林市细颗粒物典型排放源单颗粒质谱特征研究[J].环境科学学报,2015,35(5):1556-1562.DU Juan,SONG Shaohua,ZHANG Zhipeng,et al.Single particle characteristics of fine particulate matter emitted from typical sources of Guilin[J].Acta Scientiae Circumstantiae,2015,35(5):1556-1562.
[10]李磊,谭国斌,张莉,等.运用单颗粒气溶胶质谱仪分析柴油车排放颗粒物[J].分析化学,2013,41(12):1831-1836.
[11]TONER S M,SODEMAN D A,PRATHER K A.Single particle characterization of ultrafine and accumulation mode particles from heavy duty diesel vehicles using aerosol time-of-flight mass spectrometry[J].Environmental Science&Technology,2006,40(12):3912-3921.
[12]SHIELDS L G,SUESS D T,PRATHER K A.Determination of single particle mass spectral signatures from heavy-duty diesel vehicle emissions for PM2.5source apportionment[J].Atmospheric Environment,2007,41(18):3841-3852.
[13]HUO Juntao,LU Xiaohui,WANG Xinning,et al.Online single particle analysis of chemical composition and mixing state of crop straw burning particles:from laboratory study to field measurement[J].Environmental Engineering Science,2014,10:244-252.
[14]XU Jiao,LI Mei,SHI Guoliang,et al.Mass spectra features of biomass burning boiler and coal burning boiler emitted particles by single particle aerosol mass spectrometer[J].Science of the Total Environment,2017,598:341-352.
[15]LU Senlin,TAN Zhengying,LIU Pinwei,et al.Single particle aerosol mass spectrometry of coal combustion particles associated with high lung cancer rates in Xuanwei and Fuyuan,China[J].Chemosphere,2017,186:278-286.
[16]李梅,李磊,黄正旭,等.运用单颗粒气溶胶质谱技术初步研究广州大气矿尘污染[J].环境科学研究,2011,24(6):632-636.LI Mei,LI Lei,HUANG Zhengxu,et al.Preliminary study of mineral dust particle pollution using a single particle aerosol mass spectrometer(SPAMS)in Guangzhou[J].Research of Environmental Sciences,2011,24(6):632-636.
[17]SILVA P J,CARLIN R A,PRATHER K A.Single particle analysis of suspended soil dust from Southern California[J].Atmospheric Environment,2000,34(11):1811-1820.
[18]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 Nanjiao,HUANG Bo,LI Mei,et al.Single panicle characteristics of fine particulate matter in dust[J].China Environmental Science,2017,37(4):1262-1268.
[19]冯银厂,吴建会,朱坦,等.济南市和石家庄市扬尘的化学组成[J].城市环境与城市生态,2003(S1):60-62.FENG Yinchang,WU Jianhui,ZHU Tan,et al.Urban fugitive dust chemical composition in Jinan and Shijiazhuang[J].Urban Environment&Urban Ecology,2003(S1):60-62.
[20]LI Lei,HUANG Zhengxu,DONG Junguo,et al.Real time bipolar time-of-flight mass spectrometer for analyzing single aerosol particles[J].International Journal of Mass Spectrometry,2011,303(23):118-124.
[21]AND X H S,HOPKE P K,AND D P F,et al.Classification of single particles analyzed by ATOFMS using an artificial neural network,ART-2A[J].Analytical Chemistry,1999,71(4):860-865.
[22]王燕,彭林,李丽娟,等.晋城城市扬尘化学组成特征及来源解析[J].环境科学,2016,37(1):82-87.WANG Yan,PENG Lin,LI Lijuan,et al.Chemical compositions and sources apportionment of re-suspended dust in Jincheng[J].Chinese Journal of Environmental Science,2016,37(1):82-87.
[23]方小珍,孙列,毕晓辉,等.宁波城市扬尘化学组成特征及其来源解析[J].环境污染与防治,2014,36(1):55-59.FANG Xiaozhen,SUN Lie,BI Xiaohui,et al.The chemical compositions and sources apportionment of re-suspended dust in Ningbo[J].Environmental Pollution&Control,2014,36(1):55-59.
[24]ZHANG Qian,SHEN Zhengxing,CAO Junji,et al.Chemical profiles of urban fugitive dust over Xi'an in the south margin of the Loess Plateau,China[J].Atmospheric Pollution Research,2014,5(3):421-430.
[25]姬亚芹,朱坦,白志鹏,等.天津市土壤风沙尘元素的分布特征和来源研究[J].生态环境学报,2005,14(4):518-522.JI Yaqin,ZHU Tan,BAI Zhipeng,et al.Distribution characteristics and sources of the elements in soil dust[J].Ecology and Environmnet,2005,14(4):518-522.
[26]CHEN Pulong,WANG Tijian,DONG Mei,et al.Characterization of major natural and anthropogenic source profiles for size-fractionated PM in Yangtze River Delta[J].Science of the Total Environment,2017,598:135-145.
[27]HEALY R M,HELLEBUST S,KOURTCHEV I,et al.Source apportionment of PM2.5in Cork Harbour,Ireland using a combination of single particle mass spectrometry and quantitative semi-continuous measurements[J].Atmospheric Chemistry and Physics,2010,10(19):9593-9613.
[28]JOHANSSON C,NORMAN M,BURMAN L.Road traffic emission factors for heavy metals[J].Atmospheric Environment,2008,43(31):4681-4688.
[29]SANDERS P G,XU Ning,DALKA T M,et al.Airborne brake wear debris:size distributions,composition,and a comparison of dynamometer and vehicle tests[J].Environmental Science and Technology,2003,37:4060-4069.