北京城区大气金属元素干湿沉降特征
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摘要
为研究北京市大气中金属元素的干湿沉降特征,评估不同观测方法的差异性,于2014年5月至2015年4月在北京城区同步采集了混合沉降和湿沉降样品.利用电感耦合等离子体质谱仪(ICP-MS)测定了样品中19种金属(Na、Mg、Al、K、Ca、V、Cr、Mn、Fe、Cu、Zn、As、Se、Mo、Cd、Sb、Tl、Th和U)的浓度.结果表明,混合沉降样品中各金属浓度[7 160.68μg·L~(-1)(Ca)～0.02μg·L~(-1)(Th)]普遍高于湿沉降样品[4 237.74μg·L~(-1)(Ca)～0.01μg·L~(-1)(Th)].两种样品中相同金属的富集因子差异较小,其中Cu、As、Tl、Zn、Cd、Se和Sb的富集因子均大于100,表明这些重金属主要来自人为污染源.气团轨迹分析表明,北京城区降水过程主要受偏南气团的影响,其中来自西南气团的降水样品中Ca、Mg、Fe、Al、Cu、Mo、U和Th等金属浓度较高,而来自南部的气团K、Zn、Mn、Sb、Cd和Tl等金属浓度较高.观测期间大气中金属元素的混合沉降通量变化于3 591.35 mg·(m~2·a)~(-1)(Ca)～0.01 mg·(m~2·a)~(-1)(Th),湿沉降通量变化于1 847.78 mg·(m~2·a)~(-1)(Ca)～0.01mg·(m~2·a)~(-1)(Th).混合沉降与湿沉降差减得到19种金属的干沉降通量变化于1 743.57 mg·(m~2·a)~(-1)(Ca)～0.01mg·(m~2·a)~(-1)(Th).大气颗粒物的粒径大小对金属的干湿沉降过程具有重要影响.
To characterize the dry and wet deposition of atmospheric trace elements in urban Beijing,both active and passive samplers were used to collect bulk and wet sedimentation samples between May 2014 and April 2015.The concentrations of 19 trace elements(Na,Mg,Al,K,Ca,V,Cr,Mn,Fe,Cu,Zn,As,Se,Mo,Cd,Sb,Tl,Th,and U) in the samples were analyzed by inductively coupled plasma mass spectrometry(ICP-MS).The results show that the concentrations of metals in bulk deposition samples[7 160.68μg·L~(-1)(Ca)-0.02μg·L~(-1)(Th)] were generally higher than those in wet deposition samples[4 237.74μg·L~(-1)(Ca)-0.01μg·L~(-1)(Th)],but the enrichment factors of each metal in the two kinds of samples were less different.Of note,the enrichment factors of Cu,As,Tl,Zn,Cd,Se,and Sb were all larger than 100,thus indicating that these heavy metals were mainly from anthropogenic sources.The statistical analysis of the air mass trajectory shows that the precipitation chemistry in urban Beijing is mainly affected by southward air flows.The air mass originating from the southwest region always had higher concentrations of Ca,Mg,Fe,Al,Cu,Mo,U,and Th,whereas the air mass from the south had higher concentrations of K,Zn,Mn,Sb,Cd,and Tl.During the observation period,the bulk deposition fluxes of metals varied from 3 591.35 mg·(m~2·a)~(-1)(Ca)-0.01 mg·(m~2·a)~(-1)(Th),and wet deposition fluxes varied from 1 847.78 mg·(m~2·a)~(-1)(Ca)-0.01 mg·(m~2·a)~(-1)(Th).The dry deposition fluxes of the 19 metals varied from 1 743.57 mg·(m~2·a)~(-1)(Ca)-0.01 mg·(m~2·a)~(-1)(Th).The particle size has important implications in the evaluation of the relative importance of dry deposition versus wet deposition during the scavenging of trace elements in air.
To characterize the dry and wet deposition of atmospheric trace elements in urban Beijing,both active and passive samplers were used to collect bulk and wet sedimentation samples between May 2014 and April 2015.The concentrations of 19 trace elements(Na,Mg,Al,K,Ca,V,Cr,Mn,Fe,Cu,Zn,As,Se,Mo,Cd,Sb,Tl,Th,and U) in the samples were analyzed by inductively coupled plasma mass spectrometry(ICP-MS).The results show that the concentrations of metals in bulk deposition samples[7 160.68μg·L~(-1)(Ca)-0.02μg·L~(-1)(Th)] were generally higher than those in wet deposition samples[4 237.74μg·L~(-1)(Ca)-0.01μg·L~(-1)(Th)],but the enrichment factors of each metal in the two kinds of samples were less different.Of note,the enrichment factors of Cu,As,Tl,Zn,Cd,Se,and Sb were all larger than 100,thus indicating that these heavy metals were mainly from anthropogenic sources.The statistical analysis of the air mass trajectory shows that the precipitation chemistry in urban Beijing is mainly affected by southward air flows.The air mass originating from the southwest region always had higher concentrations of Ca,Mg,Fe,Al,Cu,Mo,U,and Th,whereas the air mass from the south had higher concentrations of K,Zn,Mn,Sb,Cd,and Tl.During the observation period,the bulk deposition fluxes of metals varied from 3 591.35 mg·(m~2·a)~(-1)(Ca)-0.01 mg·(m~2·a)~(-1)(Th),and wet deposition fluxes varied from 1 847.78 mg·(m~2·a)~(-1)(Ca)-0.01 mg·(m~2·a)~(-1)(Th).The dry deposition fluxes of the 19 metals varied from 1 743.57 mg·(m~2·a)~(-1)(Ca)-0.01 mg·(m~2·a)~(-1)(Th).The particle size has important implications in the evaluation of the relative importance of dry deposition versus wet deposition during the scavenging of trace elements in air.
引文
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[27] Staelens J,De Schrijver A,van Avermaet P,et al. A comparison of bulk and wet-only deposition at two adjacent sites in Melle(Belgium)[J]. Atmospheric Environment,2005,39(1):7-15.
[2] Zhu J X,Wang Q F,Yu H L,et al. Heavy metal deposition through rainfall in Chinese natural terrestrial ecosystems:evidences from national-scale network monitoring[J].Chemosphere,2016,164:128-133.
[3] Al-Khashman O A, Jaradat A Q, Salameh E. Five-year monitoring study of chemical characteristics of Wet atmospheric precipitation in the southern region of Jordan[J]. Environmental Monitoring and Assessment,2013,185(7):5715-5727.
[4] Connan O,Maro D,Hébert D,et al. Wet and dry deposition of particles associated metals(Cd,Pb,Zn,Ni,Hg)in a rural wetland site, Marais Vernier, France[J]. Atmospheric Environment,2013,67:394-403.
[5] Muezzinoglu A,Cizmecioglu S C. Deposition of heavy metals in a Mediterranean climate area[J]. Atmospheric Research,2006,81(1):1-16.
[6] Grantz D A,Garner J H B,Johnson D W. Ecological effects of particulate matter[J]. Environment International,2003,29(2-3):213-239.
[7] Breuning-Madsen H,Awadzi T W. Harmattan dust deposition and particle size in Ghana[J]. CATENA,2005,63(1):23-38.
[8] Paode R D, Sofuoglu S C, Sivadechathep J, et al. Dry Deposition fluxes and mass size distributions of Pb,Cu,and Zn measured in Southern Lake michigan during AEOLOS[J].Environmental Science&Technology,1998,32(11):1629-1635.
[9] Sakata M,Marumoto K. Dry deposition fluxes and deposition velocities of trace metals in the Tokyo metropolitan area measured with a water surface sampler[J]. Environmental Science&Technology,2004,38(7):2190-2197.
[10] Omrani M, Ruban V, Ruban G, et al. Assessment of atmospheric trace metal deposition in urban environments using direct and indirect measurement methodology and contributions from wet and dry depositions[J]. Atmospheric Environment,2017,168:101-111.
[11] Lee D S,Longhurst J W S. A comparison between wet and bulk deposition at an urban site in the U. K[J]. Water,Air,and Soil Pollution,1992,64(3-4):635-648.
[12] Tsai Y I,Kuo S C,Young L H,et al. Atmospheric dry plus wet deposition and wet-only deposition of dicarboxylic acids and inorganic compounds in a coastal suburban environment[J].Atmospheric Environment,2014,89:696-706.
[13] Tian S L, Pan Y P, Wang Y S. Size-resolved source apportionment of particulate matter in urban Beijing during haze and non-haze episodes[J]. Atmospheric Chemistry and Physics Discussions,2015,15(6):9405-9443.
[14] Pan Y P,Wang Y S. Atmospheric wet and dry deposition of trace elements at 10 sites in Northern China[J]. Atmospheric Chemistry and Physics,2015,15(2):951-972.
[15]丛源,陈岳龙,杨忠芳,等.北京平原区元素的大气干湿沉降通量[J].地质通报,2008,27(2):257-264.Cong Y,Chen Y L,Yang Z F,et al. Dry and wet atmospheric deposition fluxes of elements in the plain area of Beijing Municipality,China[J]. Geological Bulletin of China,2008,27(2):257-264.
[16] Balestrini R,Arisci S,Brizzio M C,et al. Dry deposition of particles and canopy exchange:comparison of wet,bulk and throughfall deposition at five forest sites in Italy[J]. Atmospheric Environment,2007,41(4):745-756.
[17] Sparks J P,Walker J,Turnipseed A T,et al. Dry nitrogen deposition estimates over a forest experiencing free air CO2enrichment[J]. Global Change Biology,2008,14(4):768-781.
[18] Duce R A,Hoffman G L,Zoller W H. Atmospheric trace metals at remote northern and southern hemisphere sites:pollution or natural?[J]. Science,1975,187(4171):59-61.
[19] Hernandez L, Probst A, Probst J L, et al. Heavy metal distribution in some French forest soils:evidence for atmospheric contamination[J]. Science of the Total Environment,2003,312(1-3):195-219.
[20] Wang Y Q,Zhang X Y,Draxler R R. Traj Stat:GIS-based software that uses various trajectory statistical analysis methods to identify potential sources from long-term air pollution measurement data[J]. Environmental Modelling&Software,2009,24(8):938-939.
[21] Tian H Z,Zhu C Y,Gao J J,et al. Quantitative assessment of atmospheric emissions of toxic heavy metals from anthropogenic sources in China:historical trend, spatial distribution,uncertainties,and control policies[J]. Atmospheric Chemistry and Physics,2015,15(17):10127-10147.
[22] Desboeufs K,Bon Nguyen E,Chevaillier S,et al. Fluxes and sources of nutrient and trace metal atmospheric deposition in the northwestern Mediterranean[J]. Atmospheric Chemistry and Physics,2018,18(19):14477-14492.
[23] Kyll?nen K, Karlsson V, Ruoho-Airola T. Trace element deposition and trends during a ten year period in Finland[J].Science of the Total Environment,2009,407(7):2260-2269.
[24] Theodosi C,Stavrakakis S,Koulaki F,et al. The significance of atmospheric inputs of major and trace metals to the Black Sea[J]. Journal of Marine Systems,2013,109-110:94-102.
[25] Wong C S C,Li X D,Zhang G,et al. Atmospheric deposition of heavy metals in the Pearl River Delta,China[J]. Atmospheric Environment,2003,37(6):767-776.
[26] Wu Y C,Zhang J P,Ni Z X,et al. Atmospheric deposition of trace elements to Daya Bay,South China Sea:fluxes and sources[J]. Marine Pollution Bulletin,2018,127:672-683.
[27] Staelens J,De Schrijver A,van Avermaet P,et al. A comparison of bulk and wet-only deposition at two adjacent sites in Melle(Belgium)[J]. Atmospheric Environment,2005,39(1):7-15.
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