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.     

废铅酸电池回收制取再生铅合金技术的生命周期评价

废铅酸电池的回收利用已成为铅酸电池行业实现健康持续发展的关键一环.本文采用生命周期评价方法,分析了废铅酸电池回收制取铅合金技术及末端污染控制全过程的环境影响,并与废铅酸电池回收制铅锭再制电池材料和利用原生材料生产电池材料的过程进行了对比研究.结论表明废铅酸电池回收直接制取铅合金过程中铅膏熔炼和合金配制环节在各环境影响指标中的贡献较大(其中全球变暖潜值中占60%和33%,酸化潜值中占33%和54%,人体毒性潜值中占28%和57%),主要为辅助材料及能源动力带来的间接影响;利用原生材料生产电池材料过程的环境影响相对另两个过程更大,归一化的环境影响指标结果中人体毒性潜值、富营养化潜值及酸化潜值最大(分别为2.42×10~(-11)、1.26×10~(-11)和1.08×10~(-11)),其中铅原料生产的贡献比例占绝大部分.废电池回收直接制取再生铅合金与废电池回收制铅锭再制电池材料相比,环境影响表现更优,有利于形成电池生产企业的闭环循环过程,值得应用推广.未来应鼓励以废铅酸电池回收代替相应原生材料生产新电池,同时进一步减少回收过程中使用的资源能源环境影响,以带来更大的环境效益.     

深圳市冬季PM2.5中水溶性有机物的来源特征

利用连续液化采样器（PILS）-超声雾化器-气溶胶化学组分检测仪（ACSM）联用系统,对深圳市冬季PM_2.5中水溶性组分进行在线连续观测,获取高时间分辨率的水溶性有机物（WSOM）,SO₄^2-,NO₃^-,NH₄⁺和Cl^-浓度信息以及WSOM的质谱结构信息.分析结果表明：PM_2.5中水溶性组分的总质量浓度变化范围为4.0~117μg/m³,平均浓度为20.1μg/m³,其中WSOM（25.2%）和SO₄^2-（22.4%）是最主要的贡献组分.ACSM质谱显示WSOM具有氧化态有机气溶胶（OOA）的质谱特征,其氧碳比（O/C）的平均值达到（0.60±0.09）,且WSOM与二次无机离子（SO₄^2-+NO₃^-）和钾（K）有强相关性,与黑碳（BC）的相关性较弱,表明了观测期间WSOM主要来源于二次反应产生的二次有机气溶胶（SOA）和生物质燃烧,与机动车等一次排放没有明显关系.     

南京北郊早春霾污染过程及硫酸盐形成研究

对2016年3月南京北郊PM_2.5进行采样分析,通过样品中的水溶性离子（Na⁺、NH₄⁺、K⁺、Ca²⁺、Mg²⁺、Cl^-、NO₃^-、SO₄^2-）和碳质组分（OC、EC）,探讨霾污染的特征、来源及硫酸盐形成机制.结果表明,采样期间南京北郊PM_2.5平均浓度（103.22±48.5）µg/m³.污染天二次硫酸盐的形成与NO₂对SO₂的氧化相关性较强,而O₃的氧化作用影响较小;清洁天则相反.污染天,具有酸度缓冲作用的矿物粉尘使得气溶胶颗粒物总体呈弱碱性,而碱性环境下又更利于二次硫酸盐的形成.南京北郊早春二次污染严重,SOC主要由大气中碳氢化合物与O₃发生光氧化反应生成.污染天主要排放源为机动车尾气排放,其次是生物质和煤炭燃烧;清洁天主要排放源为煤炭燃烧和扬尘,机动车尾气影响较小.     

安徽省持续性区域霾污染的时空分布特征

根据天气和气候特征,将安徽省分为沿淮淮北、江淮之间和沿江江南3个子区,并定义了持续性区域性霾过程.基于气象、环保及遥感资料,分析了安徽省持续性区域性霾过程及相应的气溶胶污染的时空分布特征.结果表明,江淮之间和沿江江南区域性霾日数自1980年开始总体呈增多趋势,沿淮淮北2000年开始增加趋势明显;1980年以来,城市持续性霾过程呈增多趋势,但城市之间差异较大;2000年之后持续性区域性霾过程明显增多,最长过程可达10d以上.62%以上的持续性区域性霾过程出现在冬季;江淮之间次数最多,沿江江南次数最少.区域性霾天气常对应着大范围的高湿、小风情况,并伴随着高浓度气溶胶污染,其光学厚度大于0.9,约是晴空天的2.3倍,气溶胶主要集中在400m以下,如近地面区域性霾天的消光系数是普通霾天的2~2.5倍,晴空天的3~5倍;地面PM_2.5污染而言,区域性霾天至少有一个或以上的城市AQI会达到轻度以上污染等级的概率超过了75%.     

Source apportionment of PM2.5 light extinction in an urban atmosphere in China

Haze in China is primarily caused by high pollution of atmospheric fine particulates (PM_2.5). However, the detailed source structures of PM_2.5 light extinction have not been well established, especially for the roles of various organic aerosols, which makes haze management lack specified targets. This study obtained the mass concentrations of the chemical compositions and the light extinction coefficients of fine particles in the winter in Dongguan, Guangdong Province, using high time resolution aerosol observation instruments. We combined the positive matrix factor (PMF) analysis model of organic aerosols and the multiple linear regression method to establish a quantitative relationship model between the main chemical components, in particular the different sources of organic aerosols and the extinction coefficients of fine particles with a high goodness of fit (R² = 0.953). The results show that the contribution rates of ammonium sulphate, ammonium nitrate, biomass burning organic aerosol (BBOA), secondary organic aerosol (SOA) and black carbon (BC) were 48.1%, 20.7%, 15.0%, 10.6%, and 5.6%, respectively. It can be seen that the contribution of the secondary aerosols is much higher than that of the primary aerosols (79.4% versus 20.6%) and are a major factor in the visibility decline. BBOA is found to have a high visibility destroying potential, with a high mass extinction coefficient, and was the largest contributor during some high pollution periods. A more detailed analysis indicates that the contribution of the enhanced absorption caused by BC mixing state was approximately 37.7% of the total particle absorption and should not be neglected.     

Assessment of column aerosol optical properties using ground-based sun-photometer at urban Harbin, Northeast China

Aerosol plays a key role in determining radiative balance, regional climate and human health. Severe air pollution over Northeast China in recent years urges more comprehensive studies to figure out the adverse effects caused by excessive aerosols. In this study, column aerosol measurements over urban Harbin, a metropolis located at the highest latitude in Northeast China, during May 2016 to March 2017 were conducted using a CIMEL sun-photometer to analyze local aerosol properties and its variation from different aspects. According to the observations, aerosol optical depth at 440 nm (AOD₄₄₀) ranges from 0.07 up to 1.54, and the large variability in both AOD₄₄₀ and Angstrom Exponent (AE_440–870) indicates the frequent change of aerosol types due of different emission sources. Coarse mode particles dominated Harbin during the studying period because of the long-range transported dust and probably the suspended snow crystals in winter. As the wavelength increases, relatively consistent decrease trends of single scattering albedo (SSA) and asymmetry factor (ASY) were observed in spring, autumn, and winter, indicating the presence of absorbing polluted aerosols. Mixed type (MIX) aerosol dominated the study region with a total percentage of 34%, and biomass burning and urban industry (BB/UI), clean continental (CC), and desert dust (DD) aerosols were found to be 31%, 27%, and 8%, respectively. The current work fills up the optical characteristics of aerosols in Harbin, and will contribute to the in-depth understanding of local aerosol variation and regional climate change over Northeast China.     

河北香河亚微米气溶胶组分特性、来源及其演变规律分析

霾的形成发展与细颗粒物化学组分变化紧密相关.本文利用颗粒物化学组分监测仪(ACSM)、黑碳仪等对河北香河夏季亚微米气溶胶(PM1)化学组分、来源及其演变规律进行详细分析.结果表明,PM1平均占到PM2.5的约71%,PM1主要分布在20~80μg·m-3间;观测期间有显著的秸秆燃烧事件,秸秆燃烧时段PM1质量浓度显著升高,其中有机物质量分数迅速升高,平均约占到47%;秸秆燃烧使得大气气溶胶由弱碱性转变为弱酸性;整个观测期间,正交矩阵因子分解法(PMF)共识别出4类有机气溶胶,分别为两种一次有机气溶胶(类烃类有机气溶胶和生物质燃烧有机气溶胶)和两种二次有机气溶胶(低挥发、高氧化性的有机气溶胶和低氧化、半挥发性的有机气溶胶),有机气溶胶氧化程度较高.其中二次有机气溶胶的贡献远大于一次有机气溶胶,平均占到有机物的~69%,而去除秸秆燃烧时段后PMF结果中未解析出生物质燃烧有机气溶胶.