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.      

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%.     

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.     

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.      

Oxidative capacities of size-segregated haze particles in a residential area of Beijing

The frequent haze days around the Chinese capital of Beijing in recent years have aroused great attention owing to the detrimental efects on visibility and public health. To discover the potential health efects of the haze, oxidative capacities of airborne particles collected in Beijing during haze and clear days were comparably assessed by a plasmid scission assay. Eleven water-soluble trace elements(As, Cd, Cr, Cu, Mn, Ni, Pb, V, Se, Tl, and Zn) in the size-segregated airborne particles were quantitatively analyzed by inductively coupled plasma mass spectrometry, and most of the watersoluble trace elements were found to mainly concentrate in the fine particle size of 0.56–1.0 μm. In comparison with clear days, the mass concentrations of 11 analyzed water-soluble trace elements remarkably increased during haze days, and the oxidative capacities determined by the plasmid scission assay were markedly elevated accordingly during the haze days under the same dosage of particles as for those during clear days. Water-soluble trace elements in airborne particles, such as Cu, V, and particularly Zn, were found to have significantly positive correlations with the plasmid DNA damage rates. Because Cu, V, and Zn have been considered as bioavailable elements, the evident increase of these elements during haze days may be greatly harmful to human health.     

Size distribution of chemical elements and their source apportionment in ambient coarse, fine, and ultrafine particles in Shanghai urban summer atmosphere

Ambient coarse particles (diameter 1.8-10 μm), fine particles (diameter 0.1-1.8 μm), and ultrafine particles (diameter < 0.1 μm) in the atmosphere of the city of Shanghai were sampled during the summer of 2008 (from Aug 27 to Sep 08). Microscopic characterization of the particles was investigated by scanning electron microscopy coupled with energy dispersive X-ray spectroscopy (SEM/EDX). Mass concentrations of Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Se, Br, Rb, Sr, and Pb in the size-resolved particles were quantified by using synchrotron radiation X-ray fluorescence (SRXRF). Source apportionment of the chemical elements was analyzed by means of an enrichment factor method. Our results showed that the average mass concentrations of coarse particles, fine particles and ultrafine particles in the summer air were 9.38 ± 2.18, 8.82 ± 3.52, and 2.02 ± 0.41 μg/m³, respectively. The mass percentage of the fine particles accounted for 51.47% in the total mass of PM10, indicating that fine particles are the major component in the Shanghai ambient particles. SEM/EDX results showed that the coarse particles were dominated by minerals, fine particles by soot aggregates and fly ashes, and ultrafine particles by soot particles and unidentified particles. SRXRF results demonstrated that crustal elements were mainly distributed in the coarse particles, while heavy metals were in higher proportions in the fine particles. Source apportionment revealed that Si, K, Ca, Fe, Mn, Rb, and Sr were from crustal sources, and S, Cl, Cu, Zn, As, Se, Br, and Pb from anthropogenic sources. Levels of P, V, Cr, and Ni in particles might be contributed from multi-sources, and need further investigation.     

上海城区和临安本底站PM_(2.5)的物化特征及来源解析

2008年4月在上海城区(徐家汇)和浙江临安大气污染本底站2个地区同步采集PM2.5样品,利用场发射扫描电镜(FESEM/EDS)和同步辐射相关技术对两地PM2.5的微观形貌、化学元素组成及来源,以及重金属元素Zn的价态进行了分析.结果表明,徐家汇、临安的PM2.5平均质量浓度分别为(131.6±65.2),(83.5±22.9)μg/m3.徐家汇地区PM2.5主要由烟尘、飞灰、矿物质等组成;临安地区PM2.5中主要为不规则形貌颗粒物.上海城区PM2.5中重金属元素的浓度明显高于临安地区样品.同步辐射X射线吸收近边结构谱的结果显示,两地PM2.5中的Zn元素都以ZnSO4为主要存在形式.富集因子法分析19种元素中,除K、Ca外,其他元素在PM2.5中富集程度上海均高于临安地区.     

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

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Status of air pollution in Beijing

A study has been made on elements organic constituents, TSP, SO2,NO2 of atmospheric pollutants in Beijing. 17 elements, and some PAHs, e. g. B(a)P, B(b, j, k)P, and B(g, h, i)P, in airborne particles by X-ray fluorescence spectroscopy and HPLC, GC/MS, have been determined respectively. It has been shown that the elements Pb, Zn, S and Cu were more enriched in fine particles and different valence states of sulfur at various sites. It was found that the concentrations of S6+ and S2-were more than 85% and less than 15% of the total sulfur respectively. Concentrations of major PAHs and sulfur-containing compounds increased in winter and in urban area. High values for Pb and Zn in city, Fe and Mn at industrial area and Cu, Al rural sites were obtained respectively. This implies the functions of different elemental sources of various sites. Thus, elements can be from distingushed anthropogenic and natural sources.The main contribution of SO2 was found of to have same seasonal variation as the anthropogenic el     

Sources and characteristics of the atmospheric aerosol near Damascus,Syria

Coarse (>2 μm) and fine (<2 μm) atmospheric particulate material was collected in the Zabadani Valley, near Damascus, in August 1985, and analyzed for sulfate, nitrate, and about 40 elements. Individual particles were analyzed for chemical and morphological parameters. Particle number concentrations and size distributions were also measured. The physical aerosol characteristics, and particularly the chemical composition indicate that the airborne particles in this arid region are predominantly due to desert soil dispersion, but that there is also some contribution from anthropogenic sources. The crustal elements exhibit atmospheric concentrations which are comparable to those in urban and industrial areas. The anthropogenic elements, on the other hand, are clearly less abundant in the Zabadani Valley than in industrialized regions. The individual particle analysis indicated that there are two major soil dust components with respectively a shale-like and a limestone composition. The data set with the bulk atmospheric concentrations (sum of coarse and fine) was subjected to chemical mass balance receptor modeling in order to assess the impact of the various plausible aerosol sources. It was found that desert soil dispersion is responsible for at least 90% of the total suspended particulate mass concentration, and that the shale and limestone components contribute in about equal proportions.     

Atmospheric concentrations and size distributions of aircraft-sampled Cd,Cu, Pb and Zn over the southern bight of the North Sea

In an effort to assess the atmospheric input of heavy metals to the Southern Bight of the North Sea, aircraft-based aerosol samplings in the lower troposphere were performed between September 1988 and October 1989. Total atmospheric particulate and size-differentiated concentrations of Cd, Cu, Pb and Zn were determined as a function of altitude, wind direction, air-mass history and season. The obtained data are compared with results of ship-based measurements carried out previously and with literature values of Cu, Pb and Zn, for the marine troposphere of the southern North Sea. The results point out the high variability of the concentrations with the meterological conditions, as well as with time and location. The experimentally found particle size distribution are bimodal with a significant difference in fractions of small and large particles. These large aerosol particles have a direct and essential impact on the air-to-sea transfer of anthropogenic trace metals, in spite of their low numerical abundance and relatively low heavy metal content.     

哈尔滨市空气中PM_(10)的元素组成特征分析

2005年8月、10月、12月和2006年4月,在哈尔滨市7个常规空气质量监测点进行了PM10的采样。样品用ICP-AES进行分析,得到了代表春夏秋冬四季空气中PM10的无机化学元素的浓度含量。研究结果表明,PM10中元素质量主要是由Al、Ca、Fe、K、Mg、S、Si7种元素贡献的;各元素由于气象条件和人为因素的影响而存在不同季节差异,地壳元素Al、Si等在春季含量较高,污染元素S、Ti在冬季含量较高;一些人为低浓度污染元素As、Cr、Ni、Pb、Zn、Cu等随着空气污染的加重明显增加;元素的富集状况分析表明,As、Cu、Ni、Pb、S、Zn富集程度较高,污染较严重,受人为污染源影响较大。     

浙江金华秋季干气溶胶中主要化学组分的消光贡献解析

造成雾霾事件的主要原因是高浓度的大气细颗粒物污染.为了深入研究大气细颗粒物的消光来源,本研究采用高时间分辨率气溶胶观测仪器获得了浙江金华秋季PM1主要化学组分浓度及干气溶胶吸收系数和散射系数演变情况.结合有机气溶胶正矩阵因子解析模型(PMF)和多元线性回归方法,建立了拟合优度很高(R2=0.977)的细颗粒物中主要化学组分与干气溶胶消光系数间的定量关系模型.结果表明,观测期间消光贡献最大的是硫酸铵,贡献率为35.1%;其次是硝酸铵,贡献率为26.7%;二次有机气溶胶(SOA)、生物质燃烧有机气溶胶(BBOA)、黑碳(BC)及氯化铵的消光贡献率分别为14.3%、11.2%、8.7%、4.0%.在一些特定污染时段,BBOA具有最大的消光贡献,是导致此时大气能见度大幅度衰减的首要因子.     

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).     

上海霾与非霾期间大气颗粒物光学特性垂直分布特征和质量浓度对比研究

采用美国国家航空航天局的云-气溶胶激光雷达红外开拓者卫星搭载的正交极化云-气溶胶激光雷达数据产品,包括消光系数、光学厚度、总后向散射系数、体积退偏比和色比,结合地面监测的颗粒物质量浓度,分析上海大气相对湿度小于80%霾发生期间气溶胶光学属性的垂直分布特征和颗粒物质量浓度变化,并与非霾期间进行比较.结果表明:霾期间532 nm和1064 nm消光系数在垂直高度上(海拔:0~10 km)均大于非霾期间,且大多数霾期间颗粒物在整层大气的光学厚度大于非霾期间.在近地面,霾期间大气颗粒物散射能力大于非霾期间.各垂直高度层,霾与非霾期间小粒径和规则气溶胶占主导地位.霾期间近地面大粒径颗粒物在霾期间所占比例大于非霾期间;2.0~4.0 km高度层,霾和非霾期间细颗粒所占比例接近;4.0~10.0 km高度层,霾期间细颗粒气溶胶所占比例大于非霾期间.PM1、PM2.5和PM10质量浓度在霾期间均大于非霾期间,且霾期间细颗粒物所占比例明显增加.颗粒物质量浓度和比值PM1/PM2.5和PM2.5/PM10分别随霾污染程度的加重而升高.冬季颗粒物质量浓度最高,主要来自细颗粒物的贡献;而春季PM10质量浓度高于其它季节.     

Estimate of municipal refuse incinerator contribution to Philadelphia aerosol using single particle analysis—II. Ambient measurements

In a study to differentiate between municipal refuse incinerator particles and other particles in urban air, samples were collected on Teflon and nuclepore filters in dichotomous samplers and analyzed by scanning electron microscopy (SEM) and energy dispersive X-ray spectrometry. The samples included ambient aerosol from two sites in the Philadelphia area, representing different meteorological conditions. The same samples were previously analyzed by bulk techniques including X-ray fluorescence and instrumental neutron activation analysis.Particles emitted from incinerators rich in Zn, Cl and K were clearly identified in ambient samples, both in the coarse (2.5–10 μm) and fine aerosol fraction (<2.5 μm). The contribution of incinerators emission was from zero up to 10% of the coarse aerosol mass. Similar particles that contained also Zn and Cl were observed, but they did not originate in refuse incineration. Minerals and biologicals were the most dominant components of the coarse aerosol fraction; sulfates dominate the fine fraction. One of the case studies provided evidence for the missing chlorine in the fine fraction. Apparently fine chlorides emitted from incinerators reacted with ambient sulfates to form mixed sulfates of Zn and K. Good agreement was obtained between the measured coarse aerosol mass concentration and the one estimated by electron microscopy.     

青岛大气降水中微量元素的浓度及溶解度

利用2016年6月~2017年5月在青岛采集的35个降水样品,分析其中8种微量元素的总态和溶解态浓度,讨论了大气降水中微量元素的浓度及其溶解度的变化特征,并探讨了影响大气降水中微量元素溶解度的因素.结果表明,青岛降水中微量元素的总态浓度以Al和Fe的最高,其次是Zn、Mn、Ba、Pb、Sr、V的较低;溶解态浓度以Zn的最高,其次是Al、Mn、Fe、Ba、Sr、Pb和V的较低;溶解度以地壳元素Al和Fe的最低,为5%左右,受到人为源影响的元素溶解度相对较高,Pb和Ba的为10%~40%,Mn和Sr的为20%~60%,Zn和V溶解度最高,平均约为55%.季节变化显示不同元素总态和溶解态浓度基本呈现冬、春季明显高于夏、秋季,溶解度基本表现为春季最高.持续降雨的前后期微量元素的总态和溶解态浓度均呈现明显降低,但溶解度的变化趋势在不同降雨过程中不一致,pH变化是控制降水中微量元素溶解度的主要因子.     

北京降尘重金属污染水平及其空间变异特征

为了研究北京大气降尘中重金属污染水平及其空间变异特征,分别于2013年6—10月(非采暖期)、2013年11月—2014年3月(采暖期)收集了北京大气降尘样品66份,采用Elan DRC Ⅱ型电感耦合等离子体质谱仪(ICP-MS)测试了样品中的37种重金属质量分数.结果表明:非采暖期北京大气降尘中Cd、Zn、Pb 3种重金属污染最严重,三者质量分数分别为5.3、822.0、177.2 mg/kg,分别超出各自北京背景值的1 065.0%、516.2%和403.1%;采暖期北京大气降尘中Mo、Cd、Bi、Zn 4种重金属污染最严重,四者质量分数分别为8.7、2.7、3.0、660.5 mg/kg,分别超出各自北京背景值的656.9%、495.8%、457.5%和395.2%;与非采暖期相比,采暖期大气降尘重金属中除Zn、Pb、Cd质量分数分别降低了19.6%、25.3%和48.9%外,其余元素的质量分数却有不同程度的升高,其中Sr、Ba、Ce、Cu、Cr、W、La、Ni、Mo、Co等10种重金属质量分数升高了53.2%～176.7%.ArcGIS地统计插值研究表明,非采暖期主要重金属(Cr、Cu、Zn、Zr、Ba和Pb)空间分布呈现出较强的变异性;采暖期降尘中主要重金属存在不同程度的空间变异,Ba和Zn的空间变异较强,二者高值区和低值区相互交错分布;Cu和Pb的空间变异相对较弱,二者高值区和低值区分布均呈规律性分布.元素示踪分析表明,无论是采暖期还是非采暖期,北京降尘重金属污染均主要来源于机动车尾气和垃圾焚烧.      

2008年北京采暖开始前后大气颗粒物化学成分及来源研究

为了系统反映北京采暖开始前后大气颗粒物的特征,于2008年10月底到12月初在北京北三环内城区使用分级式撞击采样仪进行了大气颗粒物采样,并用质子激发X射线荧光分析(PIXE)方法对其中16种化学元素浓度进行了分析.结果表明,采暖开始后16种元素总浓度较采暖期前增长3%,As、Cu在采暖期间的浓度增幅在30%以上,采暖开始后细粒子中Pb浓度增长为27%.富集因子分析结果表明,Cu、As、Pb等元素细粒子的富集因子比1999年同期有明显减小,说明北京近年来实行的环保措施较为有效.     

河北省涞水县大气颗粒物单颗粒分析表征及来源识别

为了解河北省涞水县颗粒物污染特征,采用单颗粒分析技术扫描电镜-X射线能谱法和气团后向轨迹分析技术对该县2015年3个典型污染时段〔即正常管控、严格管控（2015年阅兵期间）及发生严重颗粒物染污〕采集的7个大气颗粒物样品进行了分析表征和来源解析.共测量了1 506个粒径≥0.5 μm的单颗粒,其中粒径小于2.5 μm的颗粒占98%以上,测量结果揭示了细颗粒污染特征.结果表明:①碳质颗粒为主要颗粒物种类,其检出数目占比在90%以上.②非供暖期严格管控时段,当地居民日常生活产生的球形碳质颗粒检出数目占比最高.③非供暖期正常管控时段,机动车排放的碳质集合体颗粒检出数目占比最高,交通污染贡献最大.④供暖期球形碳质颗粒检出数目占比最高,含硫颗粒检出数目占比相对增加,燃煤的贡献最大.3个采样时段48 h气团后向轨迹分析结果表明,在空气质量良好、颗粒物污染水平较低的情况下,影响研究区域空气质量的主要是本地源;雾霾天气（处于严重颗粒物污染时段）时,西南方向外来源和本地源共同构成研究区域的颗粒物污染状态.