杭州市大气颗粒物浓度及组分的粒径分布

分别于2008年11月及2009年4~5月及10月采集了杭州大气颗粒物样本,测定了杭州市大气颗粒物及其化学组分[元素碳(EC)/有机碳(OC)、11种水溶性离子、20种元素]的浓度,并研究了其粒径分布特征.结果表明,杭州市大气颗粒物质量浓度、EC和OC的质量浓度、9种离子(SO42-、NO3-、K+、Na+、Cl-、Ca2+、Mg2+、NO2-、F-)浓度的粒径分布均显双峰结构,峰值分别出现在<0.49μm的细粒径段与3.00~7.20 μm的粗粒径段; OC、EC、SO42-、NO3-、NH4+以及主要来自人为源的元素(Cu、Zn、As、Se、Sb、Cd)主要集中在<3.0μm的细颗粒物中;杭州市大气细颗粒物中二次污染严重,细颗粒物主要受工业、交通等人为源影响.     

Characteristics of air particulate matter and their sources inurban and rural area of Beijing, China

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上海大气颗粒物中糖类的组成、粒径分布及来源

为更好地理解大气颗粒物中糖类的来源及其环境影响,利用微孔撞击式采样器(MOUDI)采集了上海市宝山区2012年11月—2013年8月四季节代表性时段18 μm以下11个不同粒径段的大气颗粒物样品,利用硅烷化衍生和GC-MS对10种脱水糖、单糖和糖醇类化合物进行了分析. 结果表明:上海大气颗粒物中所检测的10种糖类化合物的质量浓度之和在春、夏、秋、冬四季采样期的平均值分别为120.3、104.0、292.9和206.0 ng/m3,脱水糖在秋、冬季占主导地位,单糖和糖醇的质量浓度在冬季最低. 绝大部分脱水糖存在于粒径≤1.8 μm的颗粒中,冬、夏季质量浓度最高的粒径段(峰值粒径)为>0.32~0.56 μm,而春、秋季峰值粒径为>0.56~1.0 μm. 单糖和糖醇类化合物在春、夏季时主要存在于粒径>1.8 μm的颗粒中,而秋、冬季时在粒径≤1.8 μm的颗粒中质量浓度较高. 应用PMF(正定矩阵因子分析法)解析出了大气颗粒物中糖类的3个来源——生物质燃烧、植物源土壤有机质和微生物源土壤有机质. 脱水糖全部来源于生物质燃烧,单糖主要来源于植物源土壤有机质,而糖醇主要来源于微生物源土壤有机质;秋、冬季时生物质燃烧对山梨糖醇之外的单糖和糖醇有较大贡献.      

Characteristics of airborne particles inside southern California museums

The concentrations and chemical composition of suspended particulate matter were measured in both the fine and total size modes inside and outside five southern California museums over summer and winter periods. The seasonally averaged indoor/outdoor ratios for particulate matter mass concentrations ranged from 0.16 to 0.96 for fine particles and from 0.06 to 0.53 for coarse particles, with the lower values observed for buildings with sophisticated ventilation systems which include filters for particulate matter removal. Museums with deliberate particle filtration systems showed indoor fine particle concentrations generally averaging less than 10 μg m⁻³. One museum with no environmental control system showed indoor fine particle concentrations averaging nearly 60 μg m⁻³ in winter and coarse particle concentrations in the 30–40 μg m⁻³ range. Analyses of indoor vs outdoor concentrations of major chemical species indicated that indoor sources of organic matter may exist at all sites, but that none of the other measured species appear to have major indoor sources at the museums studied. Significant fractions of the dark-colored fine elemental (black) carbon and soil dust particles present in outdoor air are able to penetrate to the indoor atmosphere of the museums studied, and may constitute a soiling hazard to works of art displayed in museums.     

Atmospheric trace elements over source regions for Chinese dust: concentrations,sources and atmospheric deposition on the Loess plateau

The mass-particle size distributions of up to 17 trace elements in aerosol particle samples from dust storm and non-dust storm periods were determined for three sites in or near the source regions of Chinese dust. The mass of particulate material in the atmosphere at the sites is dominated by mineral aerosol particles. An absolute principal component analysis of the non-dust storm elemental data for the loess region allows the estimation of the mass contributions from two coarse-particle classes (soil dust and dust associated with pollutants), and two fine-particle classes (soil dust and anomalously enriched). For most elements (Al, Si, Ca, Fe, Ti, K, S and As), the mass-particle size distributions (MSDs) were approximately log-normal. The mass-median diameters (MMDs) of the soil-derived elements tended to decrease with distance from the desert region and when the dust storms subsided. Total dry deposition velocities were calculated by fitting a log-normal distribution to the aerosol data and calculating deposition rates for 100 particle-size intervals using a two-layer deposition model. The mean dry-deposition rates and fluxes were highest during dust storms over desert regions. In thloess region, the calculated dry deposition velocities of soil derived elements (Al, Si, Ca, Fe and Ti) during non-dust storm periods were from 3.1 to 3.7 cm s⁻¹. From the estimated mass-particles size distributions, the coarser and finer mineral particles were found to benriched with Ca, Fe, Ti and K relative to Al or Si. On a yearly basis, the dry atmospheric input to the Loess Plateau was mainly attributable to normal transport processes, i.e. non-dust storm conditions. Wet deposition fluxes estimated from scavenging ratios indicate that dry deposition dominated the total atmospheric deposition of mineral aerosol. The deposition of aerosol particles associated with coal burning or other anthropogenic sources also was considerable on the Loess Plateau.     

隧道大气细颗粒物及其元素的粒径分布特征

对比研究了隧道和大气环境中不同粒径细颗粒物 (切割粒径分别为0.03,0.06,0.108,0.17,0.26,0.40,0.65,1.0,1.6和2.5 μm) 中S,K,Ca,Ti,Mn,Fe,Zn,Pb,Al,Si,Cu和V等12种痕量元素的浓度. 结果表明:隧道中不同粒径细颗粒物的数浓度和质量浓度在上下班高峰时段出现明显峰值,且隧道细颗粒物在0.108 μm粒径处的数浓度和在2.5 μm粒径处的质量浓度分别是大气环境对照值的15.2和40.0倍;在隧道传输过程中质量浓度增加的痕量元素有 Si,Ca,Fe,Al,Ti,Zn,Mn,Cu和V,减小的有S,Pb,Zn和K;地壳元素(Si,Ca,Fe,Al和Ti)的质量浓度总和占隧道细颗粒物中痕量元素质量浓度总和的87%,表明土壤扬尘仍是隧道大气细颗粒物的主要来源.      

Sources and composition of aerosol from Khartoum,Sudan

Aerosol sampling was carried out during December 1989 in Khartoum, Sudan, using Nuclepore membrane filters. Twenty-four aerosol samples were collected and analysed by X-ray fluorescence (XRF) spectrometry and particle-induced X-ray emission (PIXE). In addition, individual particle analysis was also performed on 19 samples using electron probe X-ray microanalysis (EPXMA). Good agreement between XRF and PIXE results was obtained for most of the elements. Enrichment factor calculations indicated that soil dispersion is the dominant source for most elements in the aerosol. However, certain elements showed high enrichment factors indicating the presence of anthropogenic sources. From a comparison with available literature data it appeared that the enrichment factors for the enriched elements in the Khartoum aerosol are among the lowest recorded values for urban aerosol. Absolute principal components analysis (APCA) was performed on the data and confirmed the findings from the enrichment factor calculations, i.e. a dominant soil dispersion source and an anthropogenic source for some of the elements. Because of the very limited number of impotant aerosol sources, the data set was reporduced by the APCA model with a reasonable degree of success. Single particle analysis also showed that most of the particles were soil dust. These particles could further be differentiated into alumino-silicates, quartz and CaCO₃ particles. Some of the particles were found to originate from combustion sources. EPXMA gave clues to the process of formation for some of the particles from combustion sources.     

Aerosol-soil fractionation for Namib Desert samples

Four soil samples, collected in the central Namib Desert, were fractionated by dry sieving and aerosol generation into 16 size fractions in the range 0.15–300 μm diameter. The mass-size function of each soil and the dust (mineral aerosol) generated from the soil were studied. Due to the preferential lifting of smaller soil particles by the air stream, the soil underwent strong physical fractionation resulting in the bulk of the dust being found in the range of 1.3–10.3 μm, whereas the bulk of the soil was found in the range 63–300 μm. The concentrations of 11 elements in eight soil size fractions (from <45 to >300 μm) obtained by dry sieving were measured by X-ray fluorescence analysis while the concentration for these elements in eight size ranges (from <0.15 to >10.3 μm) obtained by aerosol generation were determined by particle-induced X-ray emission. The concentrations of the elements Al, Si, K, Rb and Sr were found to vary by less than a factor of two throughout the particle size range studied. However, the concentration of the elements Ca, Ti, Mn, Fe, Y and Zr increased when the particle size decreased below 150 μm to reach a maximum around 63-45 μm and then to decrease. The concentrations of the elements in the generated aerosol particles were found to be more similar to those in the bulk soil than any particular size fraction. For the aerosol size fraction, elemental enrichment factors were calculated with respect to the composition of average crustal rock, average soil, the bulk Namib soil and the small size fraction of the Namib soil. For several elements, the enrichment factors varied quite significantly, depending on the choice of the reference material. The elemental ratios in the mineral aerosol were also compared to those in the atmospheric aerosol from the Namib Desert. It was confirmed that there is a marine contribution for S, Cl and Sr in the Namib natural aerosol. The composition of the mineral aerosol generated in this study should be useful in source apportionment studies for the Namib Desert and sorrounding regions.     

太原市冬季大气气溶胶的源识别

用可对气溶胶粒径切割的采样器采集了太原市中心1985年冬季的大气气溶胶样品。以X射线荧光法分析出的化学元素作为变量,对数据作了因子分析、标示元素多元回归处理。结果指出,粒径小于2.5μm的细粒子中约有76.5％来自燃煤排放出的SO2转化成硫酸盐,约13.5％来自建筑石料高温烧结;2.5—15μm之间的粗粒子中约有82.8％来自燃煤排放出的煤飞灰;在TSP范围内,混合尘与燃煤两类源的贡献率分别是41.6％和45.2％。源识别结果表明太原市冬季气溶胶主要来自煤炭燃烧,而石油化工、金属冶炼及汽车尾气等源的贡献很小。工业粉尘、基建扬尘、路面及自然风沙等类型的源,主要在大粒径范围内（TSP）才有贡献。 就燃煤源而论,工业用煤对气溶胶（飘尘部分）污染的贡献约是居民用煤的11.8倍,因此,研究解决工业燃煤造成的大气污染是一个主要问题。"      

沈阳冬季灰霾日大气颗粒物元素粒径分布特征

为分析沈阳市冬季灰霾日大气颗粒物元素粒径分布特征,2009年1月14日─2月2日,用安德森分级撞击式采样器进行大气颗粒物分级采样,并用电感耦合等离子体质谱仪(ICP-MS)对各级样品中Na和K等30余种元素进行分析,讨论了灰霾日、非霾日及除夕日大气颗粒物元素质量浓度和富集因子的粒径分布特征及来源. 结果表明:灰霾日大气颗粒物及其元素的质量浓度均高于非霾日,粒径越细,质量浓度越高,越容易富集污染元素.Fe类元素以地壳元素为主,其质量浓度的粒径分布在非霾日呈双峰型,最高峰值出现在9.0～10 μm粗粒径段;该类元素的粒径分布在灰霾日和除夕日呈三峰型,质量浓度的最高峰值也在9.0～10 μm粗粒径段. Mn类元素在非霾日的质量浓度分布与Fe类元素相似,也呈双峰型,最高峰值出现在9.0～10 μm粗粒径段;但其在灰霾日和除夕日呈双峰型,最高峰值却出现在粒径<1.1 μm的细粒径段. K类和Zn类元素的质量浓度和富集因子的粒径分布均呈单峰型,峰值出现在粒径<1.1 μm的细粒径段. K类元素主要来源于烟花爆竹释放;Zn类元素主要源于人为污染,Pb和As等污染元素因其来源不同,在灰霾日和非霾日的表现也不相同.      

Metals in airborne particulate matter in rural Switzerland

Weekly samples of aerosol in nine size fractions were taken in the period October 1985 to September 1986, and were analyzed for Na, V, Mn, Cu, Zn, As, Cd and Pb.Sampling locations were south of Berne, Switzerland, at elevations of 515, 750, 940 and 1550 m above sea level.The results indicate that the particulate matter concentration decreases with increasing elevation, but the extent of this decrease depends on atmospheric conditions, and is more pronounced during fall and winter when frequent inversion situations occur.During a few weeks in February 1986 unusually high aerosol concentrations were observed with atypical As to Zn ratios. The meteorological situation indicated transport from Eastern Europe.Principal component analysis revealed two to three factors in every size fraction, which were considered to be an ‘anthropogenic’, a ‘soil’ and a ‘large particle’ sodium component.Single particle analysis of one summer and one winter sample (particle size 2–4 μm) provided a variety of particles previously described in the literature as well as nickel and silicon rich particles of unknown origin (summer sample).     

北京夏季典型天气TSP组成和来源对比

于2005年7月选择分别受北方冷空气、海上高压和地方性山谷风影响的3个天气过程条件下,在北京市区和郊区采集了23个大气总悬浮颗粒物(TSP)样品,并采用扫描电镜-X射线能谱技术,根据单颗粒尺度、形貌、特征化学组成解析出各类源对颗粒数浓度的贡献.结果发现:有机/碳质颗粒(占总颗粒数的31.3%,下同)和矿物颗粒(占29.5%)为优势种类,二次源颗粒占10.6%,燃煤飞灰占7.2%,燃煤、机动车排放和建筑施工产生的3类颗粒占4.1%～6.5%.3种天气下颗粒组成特征鲜明,来源差别明显:①冷空气影响下空气质量最好,TSP样品中粒径小于1.0 μm和大于5.0 μm颗粒较多,一次源处于绝对主导地位(占90%);②海上高压控制天气下,粒径为1.0～2.5 μm的颗粒大幅度增加,有大量的次生粒子生成(占10%～20%);③地方性天气中颗粒质量浓度偏高,粒径小于1.0 μm和1.0～2.5 μm颗粒所占比例均较高,但有机/碳质颗粒比例减少, 其他次要种类颗粒增多.市区人为源颗粒的种类最多,对郊区影响明显.      

利用SPAMS研究南宁市四季细颗粒物的化学成分及污染来源

为研究南宁市四季大气颗粒物的化学成分及污染来源,利用单颗粒气溶胶质谱仪(single particle aerosol mass spectrometer,SPAMS)对南宁市2015年四季大气细颗粒物进行观测.SPAMS所测得4个观测阶段大气细颗粒物数浓度与细颗粒物质量浓度线性相关系数均在0.75以上,在一定程度上颗粒物数浓度可反映大气污染状况.南宁市四季大气细颗粒物平均质谱图体现出冬、春两季二次反应生成的污染物质较多.利用自适应共振神经网络分类方法对细颗粒物化学成分进行分类,南宁市细颗粒物各化学成分数浓度占比和污染来源在四季均有差异,且化学成分能体现污染来源.冬季元素碳最高,对应较高的燃煤源;秋季有机碳最高,对应较高的机动车尾气源;夏季富钾颗粒、左旋葡聚糖和矿物质较高,对应较高的生物质燃烧源和扬尘源;春季富钠颗粒和重金属略高.在污染升高过程,生物质燃烧源和燃煤源等贡献较大.     

Microanalysis of the aerosol collected over south-central New Mexico during the alive field experiment,May–December 1989

Thirty-eight size-segregated aerosol samples were collected in the lower troposphere over the high desert of south-central New Mexico, using cascade impactors mounted onboard two research aircraft. Four of these samples were collected in early May, sixteen in mid-July, and the remaining ones in December 1989, during three segments of the ALIVE field initiative. Analytical electron microscope analyses of aerosol deposits and individual particles from these samples were performed to physically and chemically characterize the major particulate species present in the aerosol.Air-mass trajectories arriving at the sampling area in the May program were quite different from those calculated for the July period. In general, the May trajectories showed strong westerly winds, while the July winds were weaker and southerly, consistently passing over or very near the border cities of El Paso, Texas, and Ciudad Juarez, Mexico. Aerosol samples collected during the May period were predominantly fine (0.1–0.5 μm dia.), liquid H₂SO₄ droplets. Samples from the July experiment were comprised mostly of fine, solid (NH₄)₂SO₄ or mostly neutralized sulfate particles. In both sampling periods, numerous other particle classes were observed, including many types with probable terrestrial or anthropogenic sources. The numbers of these particles, however, were small when compared with the sulfates. Composite particle types, including sulfate/crustal and sulfate/carbonaceous, were also found to be present. The major differences in aerosol composition between the May and July samples (i.e. the extensive neutralization of sulfates in the July samples) can be explained by considering the different aerosol transport pathways and the proximity of the July aerosol to the El Paso/Juarez urban plume.Winds during the December experiment were quite variable, and may have contributed to the widely varying aerosol compositions observed in these samples. When the aircraft sampled the El Paso/Juarez urban plume, high concentrations of carbonaceous particles were collected. These C-rich particles were of three distinct types, two of which showed combustion morphologies and the third an irregular morphology. Concurrent aethalometer measurements of aerosol black carbon concentration were well correlated (r = 0.83) with the total carbonaceous particle fraction in the aerosol samples. Carbonaceous particles were not observed in abundance in any of the May or July samples (even when the winds passed over El Paso), and we attribute the high concentrations in December to increased wintertime burning of wood, fossil fuels and other combustibles in the urban area.     

Source apportionment of PAHs and n-alkanes bound to PM1 collected near the Venice highway

n-Alkanes and polycyclic aromatic hydrocarbons (PAHs) bound to atmospheric particulate matter (PM₁) were investigated in a traffic site located in an urban area of Venice Province (Eastern Po Valley, Italy) during the cold season. Considering the critical situation affecting the Veneto Region concerning the atmospheric pollution and the general lack of information on PM₁ composition and emission in this area, this experimental study aims at determining the source profile, their relative contributions and the dispersion of finer particles. Four sources were identified and quantified using the Positive Matrix Factorization receptor model: (1) mixed combustions related to the residential activities, (2) agricultural biomass burning in addition to the resuspension of anthropogenic and natural debris carried by the wind, (3) gasoline and (4) diesel traffic-related combustions. The role of local atmospheric circulation was also investigated to identify the pollutant sources.     

Anthropogenic contributions to the carbonaceous content of aerosols over the Pacific Ocean

During a joint U.S./U.S.S.R. research cruise from 3 May to 27 July 1987 both total and fine (< 2 μm) particulate material was sampled. This cruise started in the Hawaiian Islands and then proceeded to the Kamchatka peninsula, south to Wellington, New Zealand, south of Australia into the Indian Ocean, to Singapore and then returned to the Hawaiian Islands by sailing just north of the Equator. Particulate samples, collected on quartz fiber and Teflon filters, were analysed for organic and elemental carbon by transmission thermo-optical carbon analysis and for trace elements by energy dispersive X-ray fluorescence.In the Northern Hemisphere the total particulate, organic carbon and elemental carbon concentration ranges were, respectively, 10–25, 0.5–2.5 and 0–0.3 μg m⁻³. In the Southern Hemisphere they were, respectively, 5–10, <0.6 and <0.02 μg m⁻³. In the Northern Hemisphere the fine particulate concentration range was 2–15 μg m⁻³ and the fine fraction varied from 20 to 80% of total aerosol loading. In the Southern Hemisphere the fine particulate loading was 1.2–1.7 μg m⁻³ and was usually less than 20% of the total particulate mass.Chemical mass balance (CMB) modeling was used to determine possible anthropogenic particulate contributions to the ocean aerosol. Readily available source profiles were used for CMB modeling. Sea-salt aerosol was represented by either the conventional EPA marine source profile or by the average of ambient ocean aerosols sampled in very clean mid-ocean regions. Usually 60–90% of ambient particulate mass was “explained” by the CMB model. Sources such as soil, catalytic auto emissions and wood-burning emissions were found to be possible contributors to the ocean aerosol, especially in the Northern Hemisphere. Anthropogenic contributions were estimated to contribute from 10 to 30% of oceanic aerosol mass. Emissions from a hugh forest fire that burned in northern China during the spring of 1987 were possibly detected, but the CMB model cannot distinguish this source from emissions from heating and cooking with wood.Since anthropogenic emissions are mainly combustion emissions which usually contain a large carbon component, carbon data is essential to CMB modeling. The relatively good CMB results obtained in this study suggest that it might be useful to develop source profiles for major emission sources in those countries which contribute most directly to oceanic aerosols. Perhaps characteristic national or regional source profiles could be developed.     

夏季青岛大气粗细粒子中微量元素的浓度、溶解度及干沉降通量

利用2016年6~7月在青岛采集的PM_(2.5)和总悬浮颗粒物(TSP)样品,分析其中12种微量元素总态和溶解态浓度,讨论了微量元素在粗、细粒子中的浓度及溶解度的分布特征,并估算了微量元素的沉降通量.结果表明,青岛气溶胶中地壳元素Al、Fe、Sr、Mn、Ba总态浓度的55%~60%集中在粗粒子中,人为元素Cr、Ni、V、Zn、Pb、As、Cd的65%~85%集中在细粒子中.但无论是地壳元素还是人为元素其溶解态浓度均主要分布在细粒子中,Al、Fe、Mn、Ba在细粒子中的占比为50%~80%,Cr、Ni、V、Zn、Pb、As、Cd的为70%~90%.微量元素溶解度在细粒子中的高于粗粒子中的,细粒子中微量元素的溶解态浓度与酸组分呈显著正相关,溶解度与p H呈显著负相关,表明酸化作用可能是影响细粒子中微量元素溶解度的主控因子.不同微量元素的总沉降通量中溶解态部分的贡献不同,Al和Fe溶解态部分的贡献仅为1%~2%,Sr、Ba、Cr、Pb的约为30%~40%,Mn、Ni、V、Zn、As、Cd的约为50%~60%.大气沉降的溶解态Fe可支持(194±150)mg·(m2·d)-1浮游植物碳的生产,对黄海初级生产力的贡献约为10%.     

Chemical characteristics of aerosol particles (PM2.5) at a site of Horqin Sand-land in northeast China

Introduction Soil dust derived from the w ind erosion process in arid and sem i-arid region is an im portant factor on the clim ate forcing(Tegen etal., 1996; Sokolik and Toon, 1996). D esert regions in East A sia w ere considered as the m ajor sources fo…     

基于SPAMS的兰州市2018年冬季沙尘天气过程细颗粒物污染特征及来源研究

2018年11月22日-12月1日,兰州市经历了一次远距离传输的沙尘天气过程,为了解此次沙尘天气过程时段细颗粒物污染特征及其污染来源变化特征,本研究基于单颗粒气溶胶质谱仪（SPAMS）细颗粒物自动采集数据,并结合常规污染物自动监测数据和气象因子数据对沙尘天气前后及其过境期间细颗粒物化学组分及污染来源变化情况进行了分析,同时利用后向轨迹模型（HYSPLIT）研究了沙尘气溶胶的输送路径.研究结果表明：受沙尘天气过境影响,兰州市PM₁₀浓度大幅升高,PM_2.5/PM₁₀最小值仅为0.13,SO₂、NO₂、CO质量浓度出现明显降低,而O₃质量浓度在沙尘过境时有所升高;细颗粒物质量浓度与MASS数浓度变化趋势基本一致,细颗粒物的变化趋势可一定程度上反映大气细颗粒物的污染状况;利用自适应共振神经网络法分类后经人工合并将所采集到的细颗粒分为9类：OC、EC、HOC、OCEC、MD、HM、K、Na、LEV;所选时间段内SPAMS采集到的OC（24.8%）类颗粒物数量最多,沙尘过境时MD、LEV、Na类颗粒物占比不同程度增大,其余颗粒物占比减小;沙尘过境时扬尘源、生物质燃烧源、工业工艺源、餐饮及其它源贡献率增加,其中扬尘源增幅最大,而其余源贡献占比减小;后向轨迹HYSPLIT模型输送路径结果显示沙尘天气过程的起源地为塔克拉玛干沙漠,传输方向为经新疆的塔里木盆地塔克拉玛干沙漠进入青海中部,最后影响兰州地区.     

邯郸市可吸入颗粒物上多环芳烃来源识别和解析

环境空气中多环芳烃的来源包括自然源和人为源,本文根据化学质量平衡（CMB）受体模型对邯郸市大气颗粒物中多环芳烃进行源解析,测定邯郸市非采暖季和采暖季可吸入颗粒物中多环芳烃的浓度,对其污染水平进行比较分析。根据污染源调查结果,确定市区多环芳烃的主要排放源类,并建立相应的源成分谱。应用化学质量平衡受体模型解析邯郸市可吸入颗粒物上多环芳烃主要来源的分担率,并根据分析结果针对性提出了多环芳烃污染防治对策。