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.     

北京市大气颗粒物及其铅的来源识别和解析

2005年9月—2006年9月,在北京的北郊(昌平区)、城区和南郊(房山区)3个采样点位共采集总悬浮颗粒物(TSP)样品166个. 用ICP-AES和ICP-MS方法测量Pb等29个无机元素. 应用正矩阵因子分析方法识别的TSP的3组主要来源为土壤扬尘源、建筑源和燃煤源;2组次要来源为有色冶金源和燃油源. 北京市大气颗粒物中Pb的2个主要来源为燃煤源和有色冶金源,分别占总量的19%～39%和49%～62%;次要来源有土壤扬尘源和建筑源,分别占总量的2%～4%和7%～8%. 北京市北郊、城区和南郊的ρ(Pb)年均值分别为102,142和179 ng/m3. 燃煤源排放的铅分布比较均衡,在3个采样点位ρ(Pb)大体持平;而有色冶金源排放的铅有明显的采样点位差异,具有南高北低的趋势,这提示有色冶金源的主要方位是在北京的南边. 北京市大气ρ(Pb)有可观的下降空间. 铅排放削减和有关环境管理措施的主要对象应为涉铅的有色冶金行业. 对原料煤中铅含量的监测、控制和管理也应予以重视.      

北京大气气溶胶小颗粒的测量与解析

本项研究是对空气动力学直径小于2．5μm的气溶胶粒子进行测量分析。为此在北京设立2个采样点,分别从1989年4月30日到1989年5月16日和从1989年5月20日到1990年5月14日进行采样。样品用热光碳分析仪分析其中的有机碳(OC)和元素碳(EC),用X射线荧光光谱仪分析其中的28种元素,用离子色谱分析其中的,表征了北京大气中小颗粒气溶胶的化学特征。对所得的数据用化学质量平衡模式(CMB)法进行处理,得出了各种污染源对气溶胶小颗粒的贡献率。      

Chemical characteristics of cloudwater over Maoer Mountain district

Samples of cloudwater, rainwater and ambient aerosol were collected over Maoer Mountain in the northeast of Guangxi Province in March 1988. The pH value of cloudwater ranged from 3.37 to 6.20 with a mean value of 4.34. SO42- , NO3- , NH4+, Ca2+ and H+ were the principal ionic species of cloudwater. The advance of cold fronts into Maoer Mountain appeared to lead to higher major ionic concentration and acidity than that of warm fronts. The relative acidity and concentration of NO3- of cloudwater were much greater than that of aerosol samples. With the exception of. NO3- and H+, most of the concentration of SO42- and NH4+ in cloudwater came from the nucleation scavenging of aerosol. Gaseous nitric acid and organic acid from local may be one of the important source of cloudwater acidity. Compared with other sites, Maoer Mountain can be as a clean contrast station for studying acidic precipitation in Guangdong and Guangxi provinces.     

北京地面扬尘的理化特性及其对大气颗粒物污染的影响

通过采集北京有代表性的53个采样点的地面扬尘样品和典型区（交通区、工业区以及居民住宅区）3个采样点的气溶胶样品,分析研究了地面扬尘中主要元素和离子的浓度、空间分布、来源及其对大气颗粒物污染的贡献.结果表明,Ca、S、Cu、Zn、Ni、Pb和Cd是地面扬尘中的主要污染元素,Ca²⁺、SO^2-₄、Cl^-、K⁺、Na⁺和NO^-₃ 是地面扬尘中的主要离子.Al、Ti、Sc、Co和Mg主要来源于地壳源,Cu、Zn、Ni和Pb 主要来源于交通排放和煤燃烧,Fe、Mn和Cd主要来源于工业排放、煤燃烧和油燃烧.Ca²⁺和SO^2-₄主要来源于建筑活动、建筑材料和二次气粒转化,Cl^-和Na⁺主要来源于工业废水处理和化学工业排放,NO^-₃和K⁺主要来源于机动车排放、NO_x的光化学反应和生物质燃烧.北京地区矿物气溶胶的本地源,即地面扬尘,在不同季节的贡献量分别为2002年春季约30%, 2002年夏季约70%, 2003年秋季约80%, 2002年冬季约20%.地面扬尘中一些主要元素Ca、S、Cu、Zn、Ni、Pb、Fe、Mn和Cd 的污染水平分别为76%、 87%、 75%、 80%、 82%、 90%、 45%、 51%和94%,它们对PM₁₀中相应元素的贡献率分别为20%～45%、 5%～18%、 4%～50%、 2%～46%、 4%～52%、 5%～20%、 30%～60%、 20%～40%和2%～25%.来自交通活动和建筑活动的地面扬尘是北京大气颗粒物污染的重要来源之一.     

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

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A preliminary analysis of the surface chemistry of atmospheric aerosol particles in a typical urban area of Beijing

Atmospheric aerosol particle samples were collected using an Ambient Eight Stage(Non-Viable) Cascade Impactor Sampler in a typical urban area of Beijing from 27 th Sep.to 5th Oct.,2009.The surface chemistry of these aerosol particles was analyzed using Static Time of Flight-Secondary Ion Mass Spectrometry(Static TOF-SIMS).The factors influencing surface compositions were evaluated in conjunction with the air pollution levels,meteorological factors,and air mass transport for the sampling period.The results show that a variety of organic ion groups and inorganic ions/ion groups were accumulated on the surfaces of aerosol particles in urban areas of Beijing;and hydrophobic organic compounds with short-or middle-chain alkyl as well as hydrophilic secondary inorganic compounds were observed.All these compounds have the potential to affect the atmospheric behavior of urban aerosol particles.PM1.1–2.1and PM3.3–4.7had similar elements on their surfaces,but some molecules and ionic groups demonstrated differences in Time of Flight-Secondary Ion Mass Spectrometry spectra.This suggests that the quantities of elements varied between PM1.1–2.1and PM3.3–4.7.In particular,more intense research efforts into fluoride pollution are required,because the fluorides on aerosol surfaces have the potential to harm human health.The levels of air pollution had the most significant influence on the surface compositions of aerosol particles in our study.Hence,heavier air pollution was associated with more complex surface compositions on aerosol particles.In addition,wind,rainfall,and air masses from the south also greatly influenced the surface compositions of these urban aerosol particles.     

北京郊区农田夏季大气颗粒物质量和离子成分谱分布特征

农业活动是大气颗粒物的重要来源之一.为了研究北京郊区农田大气颗粒物质量和离子成分的分布,探讨其来源,本研究使用8级串联撞击式采样器MOUDI采集了2004年夏季北京远郊菜地的大气颗粒物样品,测量了0.18～18μm粒径段颗粒物质量和水溶性无机离子的粒径分布.细粒子的主要离子成分是SO₄^2-、NO₃^-和NH₄⁺,与温度、湿度和光照等条件相关,推测主要来自农田释放的NH₃与光化学生成的酸性物种的反应.细粒子中的K⁺可能来自植物的排放和生物质的燃烧.粗粒子中Ca²⁺、Mg²⁺、NO₃^-和SO₄^2-可能主要来自土壤颗粒物通过机械过程进入大气,以及其后酸性物种和土壤颗粒物表面的化学反应.研究结果表明,施用的化肥和土壤可能是决定农田大气中颗粒物的重要因素,北京远郊菜地对大气颗粒物可能有着重要的贡献.     

A long-term (1975–1988) study of atmospheric SO42−: Regional contributions and concentration trends

A long-term study of aerosol SO₄²⁻ concentrations ([SO₄²⁻]) has been conducted at Mayville in the western and Whiteface Mountain in the northeastern New York State. From 1975 to 1988, 2382 daily aerosol samples were collected at Whiteface Mountain using high-volume samplers. Similarly, 1863 samples were collected at Mayville for the 1981–1988 period. Both sites are downwind of large SO₂ sources in the Midwest. Whiteface Mountain is located approximately 600 km to the northeast of Mayville. The [SO₄²⁻] at Mayville were approximately twice that of Whiteface Mountain. The highest concentrations at both locations were observed in summer and the lowest during winter. Photochemical reactions appear to be the primary reason for this behavior. Air trajectories (Hefter model) were used to relate the observed [SO₄²⁻] with the upwind SO₂ source regions. In addition, a method based on V/Se ratios was used to resolve SO₄²⁻ contributions between Midwestern sources and those in the East Coast. Approximately, two-thirds or more of the total SO₄²⁻ at the two sites was derived from the Midwestern emissions. At Whiteface Mountain the [SO₄²⁻] for summer months from 1975 to 1988 suggest a decrease of approximately 3% per year between 1978 and 1988. A similar decrease was also observed in SO₂ emissions.     

珠三角典型地区大气细颗粒物中有机物质的化学组成研究

本文主要利用热解-气相色谱质谱联用技术(Py-GC/MS)对珠三角典型区域的大气颗粒物的化学特征进行研究,讨论了不同地区样品的化学和来源组成。结果显示,不同样品热解产物的组成具有一定的类似性。这些化合物均以脂肪烃(24. 6%～52. 2%)、脂肪酸(5. 0%～43. 6%)、芳香化合物(14. 7%～36. 3%)为主,另外还包括苯酚类化合物(0. 68%～11. 5%)、呋喃类化合物(0. 26%～5. 86%)、含N化合物(4. 80%～10. 2%)和含S化合物(NA～0. 67%)等,表明这些样品主要由芳香碳和脂肪链结构组成,连接有含氧、氮等杂原子基团。同时不同地区的气溶胶样品的热解产物也具有一定的差异性,反映了气溶胶中有机质的组成、来源是有差异的,如从化样品中植物来源贡献是最多的,其次是珠海,广州最少。另外不同季节采集的气溶胶样品的热解产物也表现出一定的差异性,一般情况下夏季样品中生物质来源贡献更多,而冬季样品中则是老化的气溶胶更多。     

城区大气颗粒物中有机氯农药的含量与分布

采用FA-3型气溶胶粒度分布采样器采样,对北京和天津2个样点夏季大气中不同粒径颗粒物上有机氯农药残留量进行分析.在所有分级样品中均检测出δ-HCH,p,p'-DDD和p,p'-DDT,其他有机氯农药只在部分样品中被检出.北京样中HCHs(α-HCH+β-HCH+γ-HCH+δ-HCH)含量为0.240ng/m3,DDTs(p,p'-DDT+p,p'-DDD+p,p'-DDE)含量为0.962ng/m3,天津样品中HCHs含量为0.581 ng/m3,DDTs含量为1.874ng/m3.天津样中有机氯农药残留明显高于北京样.大气颗粒物上的有机氯农药粒径分布特征为:北京样中HCHs和DDTs含量随粒径均呈单峰分布,而天津样中HCHs呈三峰态分布,DDTs呈较弱的单峰态分布.HCHs和DDTs两类化合物的质量中值直径和分散度分别在2.1～2.5μm和3.1～3.7μm范围内.      

Chemical composition of aerosols in winter/spring in Beijing

In 1999 aerosol samples were collected by cascade at Meteorological Tower in Beijing.The 12 group aerosol samples obtained were analyzed using PIXE method,which resulted in 20 elemental concentrations and size distribution of elemental concentrations.From the observation,the elemental concentrations,size distribution of elemental concentrations and their variations are analyzed.It shows that concentrations of most elements in aerosols increase greatly compared with those in the past except that the concentrations of V,K,Sr,and the source of aerosols has changed greatly in the past decade.Fine mode aerosols increase more rapidly in the past decade,which may be due to the contribution of coal combustion and automobile exhaust.Pb contait in aerosol is much higher than that at the beginning of 1980s,and has a decreasing trend in recent years because of using non-leaded gasoling.     

兰州西固地区气溶胶污染源的鉴别

本实验测定了兰州西固地区气溶胶中13种元素含量。用主因子分析(PFA)和目标转移因子分析(TTFA)法对数据进行处理,分辨出细粒子六个源和粗粒子四个源,并计算出各源对总悬浮颗粒物(TSP)的贡献,发现煤飞灰是当地的一个主要污染源。     

Effects of Asian dust events on atmospheric bacterial communities at different distances downwind of the source region

Aeolian dust particles arising from arid and semiarid zones are known to carry microbes by air currents. The effect of wind-borne bacteria on atmospheric bacterial population at various downwind distances from the dust source regions must be clarified, but has not yet been reported. This study monitored the bacterial abundance and community composition in outdoor aerosol samples in Beijing, China, which is close to the Asian dust source regions, and compared them with the results obtained in a distant region(Osaka, Japan).The Asian dust collected in Beijing contained(4 ± 3) × 10~4 bacterial cells/m~3, approximately~4 times higher than in Osaka. On 15 April 2015, Beijing experienced severe Asian dust events with a 1000-fold increase in bacterial abundance, relative to non-Asian dust days. Dominant bacterial phyla and classes in Asian dust collected in Beijing were Actinobacteria, Bacilli and Acidobacteria, and the bacterial community composition varied more widely than in Osaka.The bacterial community compositions differed between the Beijing and Osaka dusts, even for the same Asian dust events. These results indicated that aerosol bacterial communities nearer the dust source are more affected by eolian dust than their distant counterparts.     

城市雾天单个矿物颗粒物理和化学特征

应用场发射扫描电镜(FESEM)和带能谱的扫描电镜(SEM-EDX)对北京冬季雾天和正常天气下收集的4个样品进行研究.雾天中矿物颗粒的数量-粒度分布的峰值出现在0.1～0.3 μm和1～2.5 μm之间,并且发现雾天出现的二次矿物颗粒的数量百分含量(4.67%)高于正常天气条件(0.12%).单个矿物颗粒的EDX能谱显示,雾天和正常天气中单个矿物颗粒的主要化学成分有一定的差别,尤其是S元素.矿物颗粒分为9种不同类型:"富Si"、"富Ca"、"富S"、"富Fe""富Mg"、"富Al"、"富Ti"、"富K"和"富Cl",其中雾天"富Ca"中55%的颗粒含有Ca(50%±1.2%)和S(37%±1.6%),"富S"中72%的颗粒含有S(44%±1.5%)和Ca(33%±2%),说明了雾天中绝大部富集S的颗粒物中同时富集Ca,这在一定程度上说明了北京市大气中这些含Ca的碱性矿物对雾水酸性有一定的缓冲作用.雾天样品中S/Ca的平均比值为6.11,如果以冬季正常天气条件下S/Ca的均值0.73为背景值,雾天中S/Ca的比值是冬季正常天气的8倍,可见雾天中颗粒物表面的硫化现象相当严重,同时也显示出雾天SO2向硫酸盐的转化率比较高.     

北京及周边地区夏季大气颗粒物区域污染特征

本地排放和区域传输共同影响着北京及周边地区的空气质量.2007年8月在北京清华大学、密云水库、河北任丘和内蒙古商都采集颗粒物样品并获得了PM_2.5质量浓度和TSP中22种无机元素的时空分布特征. 4个观测点PM_2.5质量浓度高低顺序为任丘>清华>密云>商都.二次污染元素S和一次污染元素Zn、Pb、Cu、As、Sb、Ni、Cd、In、Se在任丘的PM中含量最高,表明该观测点受人为源影响最为显著,其较弱的日变化幅度表明高浓度PM主要由本地源贡献;商都地区污染元素浓度随时间变化波动最为剧烈,受气象条件导致的传输影响较大;清华和密云的S、Pb、Cd、In、As、Zn的相关系数均大于0.70,其来源具有一定相似性;在锯齿型污染过程的开始和结束,密云各元素浓度值达到和区域背景点商都观测期间最低值相近的水平,表明密云可以表征西北洁净空气的区域特征; PM峰值阶段,整个地区高浓度硫酸盐的均匀分布（约10 μg/m³）证实了锯齿型区域污染的二次性本质.结合元素富集因子的不同分布特征讨论了各地区PM的可能来源及相互影响     

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.     

北京大气PM2.5中铅的同位素测定和来源研究

用石英滤膜连续采集北京2003-02～2003-03的12个PM_2.5样品,进行无机多元素、OC、EC和铅同位素丰度比的分析测定.对样品进行聚类分析,结合气象信息讨论了分组结果,描述了2003年春北京市的2个大气铅污染过程.2个污染过程均表现出铅含量高,²⁰⁶Pb/²⁰⁷Pb丰度比低的特点.Al、Ca、K等地壳元素的含量与Pb的含量负相关,表明土壤尘对铅的贡献不大.比较Pb、As、Zn、Se和Al、Ca等地壳元素含量的相关性,2个铅污染过程是由有色冶金排放和燃煤排放共同主导的.而02-28～03-02的铅污染过程中,燃煤排放贡献增大,有色冶金排放贡献下降.结果表明,汽油无铅化以后,北京市春季大气颗粒物中的铅主要来源于有色冶金排放与燃煤排放.     

玉龙雪山PM2.5稳定碳同位素特征及来源分析

于2020年4~8月在青藏高原东南部玉龙雪山进行PM_2.5采样,共采集44个样本,测定其水溶性离子成分、水溶性有机碳(WSOC)浓度、总碳(TC)浓度及其稳定碳同位素组成(δ¹³C_TC).结果表明,玉龙雪山春夏季TC浓度分别为(7.1±3.8)μg/m³和(2.9±0.7)μg/m³,WSOC浓度分别为(3.3±2.1)μg/m³和(1.5±0.4)μg/m³,均呈现春高夏低的变化趋势.春夏季δ¹³C_TC值分别为(-24.7±1.0)‰和(-26.0±0.6)‰,春季较夏季偏正,表明可能受到不同来源影响.通过对非海盐钾离子(nss-K⁺)相关性、NASA火点图及后向轨迹分析可知,东南亚地区春季生物质燃烧可能是主导原因.利用贝叶斯模型计算玉龙雪山PM_2.5中TC来源贡献,结果表明春季主要来源于生物质燃烧和煤燃烧,贡献比分别为60.6%和23.5%;夏季主要来源于生物质燃烧、植物蒸发和机动车排放,同时二次有机气溶胶形成对TC的贡献也不可忽视.     

雾过程对北京市大气颗粒物理化特征的影响

为了解北京市雾中发生的气溶胶物理化学过程,分别在雾和非雾期间采集了大气颗粒物样品,并使用扫描电子显微镜和x-射线能谱仪分析了所采集的大气颗粒物的微观形貌、粒度分布和化学组成.晴天低污染期间采集的样品中单个颗粒物主要由一次排放的碳粒聚集体和球形飞灰组成;沙尘期间主要由矿物颗粒和碳粒聚集体组成;而在雾期间则出现了大量的由液相反应生成的长条状Ca-K-S颗粒以及主要由硫酸盐所组成的似圆状颗粒.本研究中,雾期间大气中0.2 μm以上颗粒物的数浓度较晴天低污染期间高5～8倍.此外,非雾期间大气颗粒物数浓度随着粒度的增加而降低,而雾期间则在0.4μm附近出现了新模态.结果表明,雾中活跃的大气非均相反应极大地改变了颗粒物的形貌、化学组成、粒度分布等特性.