厦门市冬季PM2.5污染情境识别及其与气象条件的关系

为研究厦门市冬季不同PM_2.5污染情境与气象条件和气团轨迹路径特征的关系,结合PM_2.5观测数据,使用AGAGE（Advanced Global Atmospheric Gases Experiment）统计方法识别2014—2018年冬季厦门市PM_2.5观测值、基线值和污染值情境,通过气象数据统计和气团后向轨迹聚类对不同PM_2.5污染情境下气象条件和气团轨迹路径特征进行探究.结果表明:①厦门市冬季不同PM_2.5污染情境下,ρ（PM_2.5）及PM_2.5污染值情境时长占比均呈波动中下降的趋势,具体表现为冬季PM_2.5观测值、污染值和基线值情境下,ρ（PM_2.5）平均值分别从2014年的42.2、90.7、16.4 μg/m3降至2018年的26.3、56.9、8.8 μg/m3,冬季PM_2.5污染值情境时长占比从2014年的10.2%降至2018年的3.0%.②冬季PM_2.5污染值情境下气象要素呈低风速、低气压、高温度、高相对湿度的特征.③冬季到达厦门市的气团轨迹路径中,局地路径由于大气条件稳定易累积形成PM_2.5污染;偏北路径和西北路径易从临近省份携带污染物输入导致PM_2.5污染,属于重要的外源污染输入路径;沿海路径和偏西路径均属于清洁路径,但沿海路径易在福建省北部与偏北路径重合形成污染输入,加强了偏北路径的污染物输送能力.研究显示,近年来厦门市冬季PM_2.5污染有明显减弱趋势,但不利的气象条件和外来污染输入仍会造成PM_2.5污染的发生.      

唐山工业新区冬季采暖期大气污染变化特征研究

为研究唐山工业新区采暖期大气污染变化状况,2009～2010年冬季唐山工业新区的唐山市、迁安市和曹妃甸3个地区观测研究表明,唐山工业新区冬季采暖期间大气污染严重,NO、NO2、SO2、CO、PM2.5和PM10区域平均日均值分别达到（26±28）、（52±27）、（72±53）、（3 500±3 600）、（82±65...     

2017年春夏期间南京地区臭氧污染输送影响及潜在源区

基于南京市空气质量数据与NCEP全球再分析资料,利用后向轨迹模式计算了2017年春夏（4~10月）到达南京城区逐时的24 h近地面气团后向轨迹,并将后向轨迹数据与臭氧质量浓度数据结合,进行轨迹聚类与潜在源区分析.结果表明,2017年南京市臭氧日最大8 h滑动平均浓度在12~261 μg·m^-3,超标共58 d,主要集中在春夏季.臭氧月变化呈现单峰状,其中6月臭氧浓度与超标天数最高,臭氧日变化总体呈单峰状,峰值浓度出现在14：00左右;模拟获得5136条轨迹,其中超标轨迹约占10%,超标轨迹月度分布差异较为明显,5、6两月合计占比约60%,经聚类分析得到气团输送路径共有6条,分别来自东北偏北、西北、西南、东南偏南、东南及东北方向,其中东南与东南偏南方向两类气团出现频率最高,分别为23.33%和20.76%,且对应的臭氧浓度较高,对南京臭氧污染贡献较大;潜在源区分析WPSCF与WCWT的高值区一致性较好,均揭示臭氧污染潜在源区主要分布在常州、无锡、苏州与湖州等环太湖城市,同时周边城市泰州、马鞍山、芜湖、滁州、南通与连云港等地是次要的潜在源区.臭氧污染区域输送贡献明显,需要强化长三角区域联防联控.     

西沙永兴岛大气降水化学特征及来源分析

于2013年对南海西沙永兴岛雨水进行采集,分析了其主要阴阳离子,利用PMF模型对不同离子组成的来源进行解析并运用TrajStat软件模拟后向气团轨迹污染物来源区域的分析.结果表明,永兴岛降水离子浓度顺序为：Cl^-、SO₄^2-、NO₃^-和Na⁺、Ca²⁺、Mg²⁺、NH₄⁺、K⁺.Na⁺和Cl^-是降水中主要的阴阳离子,表现出海洋性降水的特征.SO₄^2-、Mg²⁺、K⁺主要来源于海水,但SO₄^2-也受化石燃料燃烧等影响,而K⁺可能受生物质燃烧的影响.Ca²⁺主要来源于土壤,少数来源于其他影响.NO₃^-主要来源于化石燃料燃烧释放,而NH₄⁺有多种来源,包括内陆人为活动的排放和海洋本身有机物降解过程释放的影响.根据Redfield比,可以初步计算出降水中NO₃^-和NH₄⁺对南海新生产力的贡献约为4.8%~13.5%.后向气团轨迹表明,永兴岛降水的离子来源区域相对复杂,包括我国东北地区、南方区域,以及马来西亚等国家、地区的影响,或者来源于南海局地的影响.     

香河夏季PM2.5水溶性无机离子组分特征

2013年6月在中科院香河观测站对大气气溶胶化学组分特征进行研究.对PM2.5和PM10质量浓度进行在线监测,结果表明,观测期间PM2.5和PM10质量浓度均值与方差分别为(151.78±82.48)μg/m3和(250.47±106.99)μg/m3;SNA(SO42-、NO3-、NH4+)占PM2.5质量浓度的44.8%,且大多富集在粒径0.5~2.5μm的细颗粒物中.硫氧化率(SOR)、氮氧化率(NOR)平均值分别为0.35、0.31,SO2主要通过非均相的氧化反应转化为SO42-,NOx主要通过白天光化学反应转化为NO3-;灰霾和轻雾天较高的SOR和NOR表明,灰霾和轻雾天相比于清洁天有较多的SO2、NOx转化为SO42-、NO3-.气流后向轨迹分析表明灰霾和轻雾天空气质量受经过河北、山东及江苏北部气流影响.     

北京地区秋冬季大气污染特征及成因分析

为了研究近两年北京地区PM2. 5污染特征及成因变化,利用常规观测资料和改进的后向轨迹模型(Traj Stat)对2016～2017年秋冬季大气重污染时段的颗粒物浓度、气象要素和气团传输路径进行了综合分析.结果表明,研究期间北京地区共发生13次持续2 d以上的重污染事件,冬季过程约占61. 5%,且污染程度和持续时间均高于秋季.地面受弱气压场控制、高湿度、静小风以及较低的混合层高度,加之北京三面环山的特殊地势是导致秋冬季静稳型污染频发的重要因素,重污染期间PM2. 5/PM10的平均比值高达0. 86.累积阶段气团主要来自于西北、偏西、西南和东南方向,其中西南和东南路径为典型污染传输通道,轨迹频率为21. 6%.此外,采用WRF-CAMx模型定量估算了2016年12月16～22日典型过程中本地和外来污染源对北京PM2. 5的贡献,结果发现不同气团输送条件下,二者的贡献差异较大.当南部气团输入时,本地贡献会显著下降,以外部区域输送为主导;若气流来自西北方向情况则相反.污染过程期间,本地贡献为16. 5%～69. 3%.     

Verification of the geographical origin of modeled air-mass trajectories by means of the isotope composition of rainwater during the SALLJEX experiment

The SALLJEX experiment was held during the summer 2002–2003. It consisted of three-dimensional observation of the atmosphere to study the structure of the low level jet along the eastern slopes of the Andes. Daily precipitation water samples were collected at two stations (Resistencia and Salta) in northern Argentina and isotope content was analyzed. The isotope data were used in conjunction with air parcel trajectories obtained from a 3-D kinematic model (3D-MTC) developed by the University of Sao Paulo, Brazil. Values of deuterium excess were related with air masses of continental origin, whilst low values were associated with air masses with longer oceanic trajectories. Furthermore, although data are scarce, results show that oxygen-18 and deuterium excess in rainwater are related with the occurrence of the low level jet.     

Long-range atmospheric transport of three toxaphene congeners across Europe. Modeling by chained single-box FATEMOD program

Background, aims, and scope  Since toxaphene (polychlorocamphene, polychloropinene, or strobane) mixtures were applied for massive insecticide use in the 1960s to replace the use of DDT, some of their congeners have been found at high latitudes far away from the usage areas. Especially polychlorinated bornanes have demonstrated dominating congeners transported by air up to the Arctic areas. Environmental fate modeling has been applied to monitor this phenomenon using parallel zones of atmosphere around the globe as interconnected environments. These zones, shown in many meteorological maps, however, may not be the best way to configure atmospheric transport in air trajectories. The latter could also be covered by connecting a chain of simple model boxes. We aim to study this alternative approach by modeling the trajectory chain using catchment boxes of our FATEMOD model. Polychlorobornanes analyzed in biota of the Barents Sea offered one case to study this modeling alternative, while toxaphene has been and partly still is used massively at southern East Europe and around rivers flowing to the Aral Sea. Materials and methods  Pure model substances of three polychlorobornanes (toxaphene congeners P26, P50, and P62) were synthesized, their environmentally important thermal properties measured by differential scanning calorimetry, as evaluated from literature data, and their temperature dependences estimated by the QSPR programs VPLEST, WATSOLU, and TDLKOW. The evaluated property parameters were used to model their atmospheric long-range transport from toxaphene heavy usage areas in Ukraine and Aral/SyrDarja/AmuDarja region areas, through East Europe and Northern Norway (Finnmarken) to the Barents Sea. The time period used for the emission model was June 1997. Usual weather conditions in June were applied in the model, which was constructed by chaining FATEMOD model boxes of the catchment’s areas along assumed maximal air flow trajectories. Analysis of the three chlorobornanes in toxaphene mixtures function as a basis for the estimates of emission levels caused by its usage. High estimate (A) was taken from contents in a Western product chlorocamphene and low estimate (B) from mean contents in Russian polychloroterpene products to achieve modeled water concentrations. Bioaccumulation to analyzed lipid of aquatic biota at the target region was estimated by using statistical calculation for persistent organic pollutants in literature. Results  The results from model runs A and B (high and low emission estimate) for levels in sea biota were compared to analysis results of samples taken in August 1997 at Barents Sea. The model results (ng g⁻¹ lw): 4–95 in lipid of planktovores and 7–150 in lipid of piscivores, were in fair agreement with the analysis results from August 1997: 21–31 in Themisto libellula (chatka), 26–42 in Boreocadus saida (Polar cod), and 5–27 in Gadus morhua (cod) liver. Discussion  The modeling results indicate that the application of chained simple multimedia catchment boxes on predicted trajectory is a useful method for estimation of volatile airborne persistent chemical exposures to biota in remote areas. For hazard assessment of these pollutants, their properties, especially temperature dependences, must be estimated by a reasonable accuracy. That can be achieved by using measurements in laboratory with pure model compounds and estimation of properties by thermodynamic QSPR methods. The property parameters can be validated by comparing their values at an environmental temperature range with measured or QSPR-estimated values derived by independent methods. The chained box method used for long-range air transport modeling can be more suitable than global parallel zones modeling used earlier, provided that the main airflow trajectories and properties of transported pollutants are predictable enough. Conclusions  Long-range air transport modeling of persistent, especially photo-resistant organic compounds using a chain of joint simple boxes of catchment’s environments is a feasible method to predict concentrations of pollutants at the target area. This is justified from model results compared with analytical measurements in Barents Sea biota in August 1997: three of six modeled values were high and the other three low compared to the analysis results. The order of magnitude level was similar in both modeled (planktovore and piscivore) and observed (chatka and polar cod) values of lipid samples. The obtained results were too limited to firm validation but are sufficient to justify feasibility of the method, which prompts one to perform more studies on this modeling system. Recommendations and perspectives  For assessment of the risk of environmental damages, chemical fate determination is an essential tool for chemical control, e.g., for EU following the REACH rules. The present conclusion of applicability of the chained single-box multimedia modeling can be validated by further studies using analyses of emissions and target biota in various other cases. To achieve useful results, fate models built with databases having automatic steps for most calculations and outputs accessible to all chemical control professionals are essential. Our FATEMOD program catchments at environments and compound properties listed in the database represent a feasible tool for local, regional, and, according our present test results, for global exposure predictions. As an extended use of model, emission estimates can be achieved by reversed modeling from analysis results of samples corresponding to the target area. This article is dedicated to the memory of Professor Alexander B Terentiev (who passed away in November 2006), our true friend. With his Institute of Organo-Element Compounds, Russian Academy of Science, Moscow, he was an important main organizer of the six joint Finnish–Russian seminars (every third year since 1989) on the field (‘Chemistry and Ecology of Organo-Element Compounds’). He prompted us especially to search properties and environmental fates for various polyhalogen compounds. We remember him for his friendly character and great sense of humor.     

华东森林及高山背景区域SO2、NOx、CO本底特征

国家大气背景监测福建武夷山站是中国华东区域背景站点之一,可代表华东森林及高山区域背景状况。为了解该区域的大气背景状况,评估区域污染现状以及污染物输送在区域污染中的作用,选取福建武夷山背景站2011年3月至2012年2月主要气体污染物（SO₂、NO_x、CO）为期1年的监测数据,研究各污染物在不同时间尺度的浓度变化特征和相关关系,以及与气象因子的相关关系,并利用后向轨迹模式探讨区域输送对华东森林及高山背景区域各气体污染物质量浓度的影响。结果表明,武夷山背景点监测期间SO₂、NO_x、CO的平均质量浓度分别为3.9、5.1、409.8 μg/m³,且具有明显的季节变化特征,春、冬季明显高于夏、秋季;三者日变化幅度均很小,呈现出单谷型分布型态,说明武夷山背景点受人为活动的影响很小,主要受气象条件影响;相关性分析结果显示,SO₂与NO_x浓度相关性较好,与湿度有较好的负相关,与风速在冬季具有一定的正相关,NO_x与CO浓度在秋季和冬季的相关性较好,且二者与温度的负相关性较好。后向轨迹分析结果表明,SO₂全年最大浓度峰值主要来自北方采暖季燃煤排放的远距离输送影响,NO_x、CO全年最大值则源于生物质燃烧的远距离输送影响。     

Kosetice, Czech Republic--ten years of air pollution monitoring and four years of evaluating the origin of persistent organic pollutants

The regional observatory Kosetice is a central European background station. Unique continuous monitoring from 1988 on is held here. POP (persistent organic pollutant) concentration values of air samples from Kosetice taken between 1996 and 2005 were statistically processed. Values of Czech ambient air quality standards were not exceeded. Concentrations of polycyclic aromatic hydrocarbons reached two maxima, in 1996 and 2001-2002. Polychlorinated biphenyls concentrations reached the highest values in 1997 and 1998 and hexachlorocyclohexanes concentrations in 1998. DDTs, hexachlorobenzene and pentachlorobenzene were analysed as well. Long-range transport of pollutants between 2002 and 2005 was evaluated using the Potential Source Contribution Function hybrid receptor model. Indicated potential source areas of PCBs coincide with many well-known urban and industrialised areas, while the indicated potential source areas of HCHs and DDTs coincide with many agricultural and/or forested regions and the potential source areas of HCB comprise all land use types.