Studies on sampling methods for PCDDs and PCDFs in stack emission

Polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) in stack emission exist both as vapor and sorbed onto the surface of particles. The partition between the two phases is of a dynamic nature and changes rapidly with temperature. When monitoring stack emissions, a sampling method must be used that efficiently collects both phases as well as any condensation aerosol formed in the sampling train. In this study, the two sampling methods used in Sweden, the cooled probe polyurethane foam plug (PUFP) sampling train and the sampling train recommended by the Swedish Environmental Protection Board has been tested for particle collection ability. The results show that an aerosol filter has to be introduced after the condensor in order to collect particle bound PCDDs and PCDFs efficiently.     

大气微生物粒子与飘尘粒子的关系

用ＡＮＤＥＲＳＥＮ生物粒子采样器和光散射气溶胶粒子计数器，在北京西单对大气细菌、真菌和飘尘粒子的浓度、粒度分布及它们之间的关系进行了观测和研究。结果表明，大气细菌的粒度是负偏态分布，大气真菌是对数正态分布，飘尘是正偏态分布。大气细菌浓度与飘尘浓度的比值冬季大，为１１９５３８；夏季小，为２４２１７；年平均比值为６７５１７，＞２．０μｍ的菌尘比值为１５２５３８７，２．０μｍ～８．２μｍ的菌尘比值为３３１８，＞８．２μｍ的菌尘比值为３９４。大气真菌浓度与飘尘浓度的比值冬季大，为２１２７７０；夏季小，为６５５８５；年平均比值为１３５３４４，＜２．０μｍ的菌尘比值为９５２６９８，２．０μｍ～８．２μｍ的菌尘比值为５３４３，＞８．２μｍ的菌尘比值为２６３２。     

Monitoring the transport of biomass burning emissions in South America

The atmospheric transport of biomass burning emissions in the South American and African continents is being monitored annually using a numerical simulation of air mass motions; we use a tracer transport capability developed within RAMS (Regional Atmospheric Modeling System) coupled to an emission model. Mass conservation equations are solved for carbon monoxide (CO) and particulate material (PM2.5). Source emissions of trace gases and particles associated with biomass burning activities in tropical forest, savanna and pasture have been parameterized and introduced into the model. The sources are distributed spatially and temporally and assimilated daily using the biomass burning locations detected by remote sensing. Advection effects (at grid scale) and turbulent transport (at sub-grid scale) are provided by the RAMS parameterizations. A sub-grid transport parameterization associated with moist deep and shallow convection, not explicitly resolved by the model due to its low spatial resolution, has also been introduced. Sinks associated with the process of wet and dry removal of aerosol particles and chemical transformation of gases are parameterized and introduced in the mass conservation equation. An operational system has been implemented which produces daily 48-h numerical simulations (including 24-h forecasts) of CO and PM2.5, in addition to traditional meteorological fields. The good prediction skills of the model are demonstrated by comparisons with time series of PM2.5 measured at the surface.     

Chromatographic measurement of molecular markers of sources of atmospheric aerosol particles

Various organic compounds in aerosol particles in ambient air near a coniferous forest fire in Boulder, Colorado were identified as molecular markers of wood burning and forest fires. Particle samples were collected by filtering small volumes of air. The samples were analysed using thermal desorption followed by gas chromatographic separation and detection, a highly sensitive analytical method. Several compounds unique to softwood combustion were identified in the samples. Additionally, a predominance of odd-carbon-numbered n-alkanes over the corresponding even-carbon-numbered n-alkanes was observed. This predominance is a well-documented molecular pattern indicative of epicutical waxes in plants.     

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.     

Environmental impact and health risk assessment of volatile organic compound emissions during different seasons in Beijing

Volatile organic compounds (VOCs) are major contributors to air pollution. Based on the emission characteristics of 99 VOCs that daily measured at 10 am in winter from 15 December 2015 to 17 January 2016 and in summer from 21 July to 25 August 2016 in Beijing, the environmental impact and health risk of VOC were assessed. In the winter polluted days, the secondary organic aerosol formation potential (SOAP) of VOC (199.70 ± 15.05 μg/m³) was significantly higher than that on other days. And aromatics were the primary contributor (98.03%) to the SOAP during the observation period. Additionally, the result of the ozone formation potential (OFP) showed that ethylene contributed the most to OFP in winter (26.00% and 27.64% on the normal and polluted days). In summer, however, acetaldehyde was the primary contributor to OFP (22.00% and 21.61% on the normal and polluted days). Simultaneously, study showed that hazard ratios and lifetime cancer risk values of acrolein, chloroform, benzene, 1,2-dichloroethane, acetaldehyde and 1,3-butadiene exceeded the thresholds established by USEPA, thereby presenting a health risk to the residents. Besides, the ratio of toluene-to-benzene indicated that vehicle exhausts were the main source of VOC pollution in Beijing. The ratio of m-/p-xylene-to-ethylbenzene demonstrated that there were more prominent atmospheric photochemical reactions in summer than that in winter. Finally, according to the potential source contribution function (PSCF) results, compared with local pollution sources, the spread of pollution from long-distance VOCs had a greater impact on Beijing.     

Chemical characteristics and sources of water-soluble organic aerosol in southwest suburb of Beijing

PM_2.5 filter sampling and components measurement were conducted in autumn and winter from 2014 to 2015 at a suburban site (referred herein as “LLH site”) located in the southwest of Beijing. The offline aerosol mass spectrometry (offline-AMS) analysis and positive matrix factorization (PMF) were applied for measurement and source apportionment of water-soluble organic aerosol (WSOA). Organic aerosol (OA) always dominated PM_2.5 during the sampling period, especially in winter. WSOA pollution was serious during the polluted period both in autumn (31.1 µg/m³) and winter (31.9 µg/m³), while WSOA accounted for 54.4% of OA during the polluted period in autumn, much more than that (21.3%) in winter. The oxidation degree of WSOA at LLH site was at a high level (oxygen-to-carbon ratio, O/C=0.91) and secondary organic aerosol (SOA) contributed more mass ratio of WSOA than primary organic aerosol (POA) during the whole observation period. In winter, coal combustion OA (CCOA) was a stable source of OA and on average accounted for 25.1% of WSOA. In autumn, biomass burning OA (BBOA) from household combustion contributed 38.3% of WSOA during polluted period. In addition to oxygenated OA (OOA), aqueous-oxygenated OA (aq-OOA) was identified as an important factor of SOA. During heavy pollution period, the mass proportion of aq-OOA to WSOA increased significantly, implying the significant SOA formation through aqueous-phase process. The result of this study highlights the concentration on controlling the residential coal and biomass burning, as well as the research needs on aqueous chemistry in OA formation.     

Characteristics of atmospheric volatile organic compounds in urban area of Beijing: Variations, photochemical reactivity and source apportionment

Atmospheric volatile organic compounds (VOCs) were observed by an on-line gas chromatography-flame ionization detector monitoring system from November 2016 to August 2017 in Beijing. The average concentrations were winter (40.27 ± 25.25 μg/m³) > autumn (34.25 ± 19.90 µg/m³) > summer (32.53 ± 17.39 µg/m³) > spring (24.72 ± 17.22 µg/m³). Although benzene (15.70%), propane (11.02%), ethane (9.32%) and n-butane (6.77%) were the most abundant species, ethylene (14.07%) and propene (11.20%) were the key reactive species to ozone formation potential (OFP), and benzene, toluene, ethylbenzene, m-xylene + p-xylene and o-xylene (54.13%) were the most reactive species to secondary organic aerosol formation potential (SOAFP). The diurnal and seasonal variations indicated that diesel vehicle emission during early morning, gasoline vehicle emission at the traffic rush hours and coal burning during the heating period might be important sources. Five major sources were further identified by positive matrix factorization (PMF). The vehicle exhaust (gasoline exhaust and diesel exhaust) was found to be contributed most to atmospheric VOCs, with 43.59%, 41.91%, 50.45% and 43.91%, respectively in spring, summer, autumn and winter; while solvent usage contributed least, with 11.10%, 7.13%, 14.00% and 19.87%, respectively. Biogenic emission sources (13.11%) were only identified in summer. However, both vehicle exhaust and solvent usage were identified to be the key sources considering contributions to the OFP and SOAFP. Besides, the contributions of combustion during heating period and gasoline evaporation source during warm seasons to OFP and SOAFP should not be overlooked.     

西南涡对气溶胶光学厚度变化特征的影响研究

为研究西南涡对气溶胶光学厚度(AOD)的影响,本研究利用2008—2010年的西南涡个例数据与对应时间段的中分辨率成像光谱仪(MODIS)卫星遥感观测AOD数据,并结合降水量、风速、相对湿度、温度等气象资料进行了分析研究.结果发现,2008—2010年产生干涡31个,强降水涡29个,弱降水涡26个.总体而言,干涡过境后使AOD增加而降水涡过境后使AOD减少,且弱降水涡比强降水涡削减作用强.春季产生的西南涡对AOD的影响最大,夏季产生的干涡过境后会使AOD减少,夏季的弱降水涡过境后会使AOD增加.不同季节产生的不同类型西南涡过境后致使AOD变化的主导气象因子不同.总体而言,较大的风速对AOD具有显著的削减作用;干涡中较小的风速、温度和相对湿度是使AOD增加的主要因素;弱降水涡中较大的风速和产生的降水是使AOD减少的主要因素,但夏季产生的弱降水涡中影响AOD的主要因素是风速、温度和湿度;强降水涡中无明显的主导因素.     

晋城市冬季环境空气中挥发性有机物的污染特征及来源解析

采集晋城市冬季环境空气样品,利用色谱-质谱仪分析了其挥发性有机物(VOCs)的组份特征,运用PMF、特征比值、后向轨迹模型对其来源进行了研究,并计算了臭氧和二次有机气溶胶的生成潜势,探讨了其环境影响.结果表明,观测期间,晋城市VOCs平均浓度为93.35μg·m~(-3),其中烷烃类化合物浓度为52.91μg·m~(-3),在VOCs中占比较高为56.68%;PMF分析VOCs排放源有工业排放源、燃烧源、机动车源、溶剂使用源和植物源,贡献率分别为33.71%、30.27%、26.28%、9.00%和0.74%;特征比值法分析中,苯/甲苯和异戊烷/正戊烷比值分别为1.58±0.68和2.07±0.43,介于道路来源与燃煤源之间,为两者混合来源.后向轨迹聚类3个代表性气团均来自西北方向,分别占比50%、25%和25%,西北方向的工业污染可能会对晋城市VOCs造成影响;观测期间,晋城市空气质量指数、总VOCs浓度和机动车源贡献率在风速较小时(3 m·s-1)分别为143、162.48μg·m~(-3)和46.16%,各数值均高于风速较大(3~6.9 m·s-1)时(60、35.72μg·m~(-3)和16.15%);芳香烃类化合物的臭氧和二次有机气溶胶生成潜势分别为98.89μg·m~(-3)和1.21μg·m~(-3),占总生成潜势的37.28%和97.01%,是两种生成潜势最高的VOCs化合物种类.因此,控制工业、机动车和燃烧排放是控制晋城市环境空气中VOCs污染的主要途径.