Fungal spores and pollen in particulate matter collected during agricultural activities in the Po Valley (Italy)

Airborne particulate matter (PM) containing fungal spores and pollen grains was sampled within a monitoring campaign of wheat threshing, plowing and sowing agricultural operations. Fungal spores and pollen grains were detected and identified on morphological basis. No studies were previously available about fungal spore and pollen content in agricultural PM in the Po Valley. Sampling was conducted in a Po Valley farmland in Mezzano (Ferrara, Italy). The organic particles collected were examined by scanning electron microscopy with energy dispersive X-ray spectrometer. Fungal spores and pollen grains were identified when possible at the level of species. The most frequent components of the organic particles sampled were spores of Aspergillus sp., which could represent a risk of developing allergies and aspergillosis for crop farmers.     

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.     

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。     

Identification of sources of lead in the atmosphere by chemical speciation using X-ray absorption near-edge structure (XANES) spectroscopy

Sources of Pb pollution in the local atmosphere together with Pb species, major ions, and heavy metal concentrations in a size-fractionated aerosol sample from Higashi-Hiroshima(Japan) have been determined by X-ray absorption near-edge structure(XANES) spectroscopy, ion chromatography, and ICP-MS/AES, respectively. About 80% of total Pb was concentrated in fine aerosol particles. Lead species in the coarse aerosol particles were PbC2O4, 2PbCO3·Pb(OH)2, and Pb(NO3)2, whereas Pb species in the fine aerosol particles were PbC2O4, PbSO4, and Pb(NO3)2. Chemical speciation and abundance data suggested that the source of Pb in the fine aerosol particles was different from that of the coarse ones. The dominant sources of Pb in the fine aerosol particles were judged to be fly ash from a municipal solid waste incinerator and heavy oil combustion. For the coarse aerosol particles, road dust was considered to be the main Pb source. In addition to Pb species, elemental concentrations in the aerosols were also determined. The results suggested that Pb species in size-fractionated aerosols can be used to identify the origin of aerosol particles in the atmosphere as an alternative to Pb isotope ratio measurement.     

北京大气气溶胶表面无机组分的静态飞行时间二次离子质谱研究

采用特定的样品处理方式,利用静态飞行时间二次离子质谱(Static-TOF-SIMS)技术,对使用通用型大气污染物采样仪VAPS(URG-3000K)采集于非导电性的滤膜(聚碳酸酯滤膜)上的大气气溶胶细粒子(PM_2.5)与粗粒子(PM_2.5～10)的表面无机组分进行了探索性的比较分析.结果表明:大气气溶胶细粒子与粗粒子的表面无机组分组成特征具有明显的差异;气溶胶细粒子表面存在着大气中二次形成的亲水性化合物,会对其表面的疏水性/亲水性特征产生影响,从而影响其大气化学行为;气溶胶粗粒子表面存在氟化物,对生态环境和人体健康具有潜在的危害性,应该重视对气溶胶中氟污染的研究与控制;静态飞行时间二次离子质谱可以成为研究大气气溶胶表面化学组成特征的有利分析手段.      

鹤山气溶胶光学性质和单颗粒化学组分的研究

2014年10~11月在广东省鹤山大气超级站利用单颗粒气溶胶质谱仪（SPAMS）、积分式浊度仪和黑碳仪在线观测了单颗粒气溶胶的化学组成与气溶胶光学特征.采用Art-2a分类法将单颗粒分为9类：有机碳-硫酸盐/硝酸盐颗粒（OC-Sulfate/Nitrate）、元素碳-硫酸盐/硝酸盐颗粒（EC-Sulfate/Nitrate）、元素碳有机碳-硫酸盐/硝酸盐颗粒（ECOC-Sulfate/Nitrate）、高分子有机碳颗粒（HOC）、海盐颗粒（Sea-salt）、硅酸盐颗粒（Si-rich）、左旋葡聚糖颗粒（Lev）、钾-硫酸盐/硝酸盐颗粒（K-Sulfate/Nitrate）、金属颗粒（Metal）.从清洁期到灰霾期气溶胶的吸收系数、散射系数和单次散射反照率（SSA）显著升高,气溶胶消光能力增强,同时EC-Sulfate/Nitrate颗粒占比从34.8%降至31%,OC-Sulfate/Nitrate颗粒从9.9%增加至23.6%,K-Sulfate/Nitrate二次颗粒从8.5%增加至14%,且灰霾期OC-Sulfate/Nitrate颗粒与硫酸盐、硝酸盐和铵盐的混合程度增强,因此老化的OC-Sulfate/Nitrate颗粒和二次组分颗粒对气溶胶消光系数的增加有重要贡献.在大气相对湿度从50%增加到70%以上的过程中,气溶胶散射系数和吸收系数升高,消光系数由326.1Mm^-1增加到362.9Mm^-1,SSA有所下降,PM_2.5质量消光效率由4.98增加到5.99,EC-Sulfate/Nitrate颗粒和K-Sulfate/Nitrate二次颗粒占比下降,而OC-Sulfate/Nitrate颗粒的占比由7.79%增加到14.29%,且OC-Sulfate/Nitrate颗粒中富含硫酸盐、硝酸盐和铵盐,表明高相对湿度下老化的OC-Sulfate/Nitrate颗粒数目增多对气溶胶消光系数的增强有重要影响.     

中国3个AERONET站点气溶胶大小的识别及特征分析

?ngstr?m波长指数a是判断气溶胶粒子大小的重要参数,但当气溶胶尺度分布不满足Junge分布时,仅用a不能很好的反映气溶胶粒子的尺度信息.利用Mie散射理论和AERONET站点实测资料分析说明在0.750.6;当a2>0.3时,多以粗粒子为主,Vfine/Vtotal<0.4.利用Gobbi气溶胶图解法分析显示SACOL站AOD的大值主要是由于沙尘气溶胶的影响造成的;香河站沙尘和细粒子气溶胶都会产生大值AOD,并且图解法可以很好的区分这两种情况;太湖站受沙尘的影响较小,大值AOD绝大多数是由于细粒子气溶胶造成的.     

南京北郊重金属气溶胶粒子来源分析

通过2013年1~12月使用在线单颗粒气溶胶质谱仪(SPAMS)在南京北郊对含有Cu、As、Pb、Cd、V、Co、Cr、Zn、Ni、Ba和Hg这11种重金属气溶胶粒子进行连续观测,并结合自适应共振理论神经网络算法(ART-2a)对其化学特征进行了分析,结果表明,南京北郊重金属气溶胶粒子来源按照化学组成特征可分为5类:工业排放(35.7%)、生物质燃烧(34.45%)、交通排放(13.6%)、化石燃料燃烧(11.03%)和矿尘(4.07%),其中,含Pb、Cd和Cr气溶胶粒子主要来源于工业排放,含Cu、Co和Hg气溶胶粒子主要来源于生物质燃烧,含V、Zn和Ba气溶胶粒子主要来源于交通排放,含As和Ni气溶胶粒子主要来源于化石燃料燃烧.     

南京秋冬季非难熔性亚微米颗粒物来源解析

利用Aerodyne高分辨率飞行时间气溶胶质谱仪（HR-ToF-AMS）对南京北郊秋冬季非难熔性亚微米气溶胶（NR-PM₁）的化学组分（包括有机物、硝酸盐、硫酸盐、铵盐和氯化物）和特征进行实时在线监测,并利用多元线性模型（ME-2）对其中复杂的有机物进行来源解析.观测期间,有机物、硝酸盐、硫酸盐、铵盐、氯化物对NR-PM₁的贡献分别为42%,28%,15%,13%和2%.有机物解析出6类有机气溶胶：烃类有机气溶胶（HOA）、烹饪类有机气溶胶（COA）、生物质燃烧有机气溶胶（BBOA）、高氧化有机气溶胶（MO-OOA）、低氧化有机气溶胶（LO-OOA）、液相反应生成氧化有机气溶胶（aq-OOA）,平均浓度分别占总有机气溶胶的18%,14%,19%,19%,11%和19%.通过不同污染事件的对比结果表明,本次观测期间二次气溶胶在污染时期占比会明显上升并且液相反应对二次组分的形成有显著的促进作用.     

有机气溶胶的来源与形成研究现状

介绍了有机气溶胶来源与形成的研究现状,从有机气溶胶的化学组成特征、一次有机气溶胶的来源和二次有机气溶胶的形成机制论述其研究进展.一次有机气溶胶主要来源于烹调油烟、机动车排放、生物质燃烧、工业或民用燃油锅炉释放出的有机物,还有道路扬尘、沥青、刹车尘、轮胎屑、室外香烟烟雾、以及高等植物蜡、细菌活动和草本植物等.大气中的半挥发性有机物可通过物理和化学吸附形成二次有机气溶胶,一些挥发性有机物可通过气相化学反应转化为低挥发性的物质并形成二次有机气溶胶,其主要前体物是芳香族化合物,如苯、甲苯、二甲苯,以及烯烃、烷烃、环烷烃、萜烯和生物排放的非饱和氧化物.     

沙尘暴事件中大气颗粒物化学组分的浓度变化和硫酸盐的形成

应用电感耦合等离子体原子发射光谱、质谱和离子色谱分析了2002年3月28日-4月8日在山东长岛县采集的共11对粗、细大气颗粒物样品的化学组成,探讨4月6-8日沙尘暴事件中大气颗粒物化学组分的变化和硫酸盐的形成.沙尘暴事件应区分前锋和后续部分,前锋与大气中各种污染物相互作用,具有硫富集的特征.后续部分较好地保持了长距离传输风沙尘本身的特征.硫酸盐的形成机理可能是多相氧化而不是简单的酸碱中和.硫酸铵是首先生成的含硫物种,这是细颗粒主导的形成过程.硫酸铵逐渐转化为其他硫酸盐,硫的成分也逐渐向粗颗粒转移.在沙尘暴事件中含硫污染物不但有一个从气相向颗粒物转变的过程,也有一个从细颗粒向粗颗粒转化的过程.      

鹤山大气超级站旱季单颗粒气溶胶化学特征研究

利用单颗粒气溶胶飞行时间质谱等仪器在鹤山大气超级站开展综合观测,结合ART-2a自适应共振神经网络聚类算法,将2013年11月4日~2013年12月30日期间监测到的1637330个细颗粒分成9类: EC-Fresh颗粒、EC-Nitrate/Sulfate颗粒、K-EC颗粒、Ca-EC颗粒、ECOC颗粒、OC-Levoglucosan颗粒、OC-Nitrate/Sulfate颗粒、K-Nitrate/Sulfate颗粒和Metal-rich颗粒.结果表明:该大气超级站所在地区旱季霾日有利于与水溶性二次无机组分混合的EC-Nitrate/Sulfate颗粒、K-Nitrate/Sulfate颗粒的累积;晴朗天更有利于二次有机组分在气溶胶颗粒中生成,雨天受当地排放源的影响显著,含有较高EC-Fresh和K-EC颗粒.相关性的研究发现,EC-Nitrate/Sulfate颗粒与能见度有良好的相关性,它们对霾的形成有至关重要的作用.     

北京2010年10月一次典型灰霾过程光学特性分析

利用探空资料、NECP再分析资料、AERONET气溶胶反演资料等分析了北京地区一次典型灰霾天气过程的成因及气溶胶光学特性参数变化情况.结果表明:此次灰霾期间,稳定的环流形势、湿润的环境及逆温结构的存在是灰霾得以持续和发展的重要原因.灰霾期间AOD、PM2.5浓度逐渐增大,能见度逐渐降低,这可能与局地气溶胶的累积和相对湿度的增大有关,使气溶胶粒子的消光性增强.气溶胶的体积谱表现为双峰型结构,细粒子体积浓度峰值远大于粗粒子浓度峰值,且细粒子浓度峰值逐日增大,Angstrom波长指数在1.2~1.4之间,两参数均可表明此次灰霾过程的污染粒子以气溶胶细粒子为主;灰霾期间SSA逐日增大,表明气溶胶粒子的散射性逐渐增强,SSA随波长的变化主要呈现两种变化趋势,这与当日主控粒子的尺度有关.因气溶胶的作用,使到达地面的辐射通量减小.这些光学特性参量的变化为了解北京地区灰霾期间气溶胶特性及其气候效应提供了参考.     

基于SPAMS的兰州市2018年冬季沙尘天气过程细颗粒物污染特征及来源研究

2018年11月22日-12月1日,兰州市经历了一次远距离传输的沙尘天气过程,为了解此次沙尘天气过程时段细颗粒物污染特征及其污染来源变化特征,本研究基于单颗粒气溶胶质谱仪（SPAMS）细颗粒物自动采集数据,并结合常规污染物自动监测数据和气象因子数据对沙尘天气前后及其过境期间细颗粒物化学组分及污染来源变化情况进行了分析,同时利用后向轨迹模型（HYSPLIT）研究了沙尘气溶胶的输送路径.研究结果表明：受沙尘天气过境影响,兰州市PM₁₀浓度大幅升高,PM_2.5/PM₁₀最小值仅为0.13,SO₂、NO₂、CO质量浓度出现明显降低,而O₃质量浓度在沙尘过境时有所升高;细颗粒物质量浓度与MASS数浓度变化趋势基本一致,细颗粒物的变化趋势可一定程度上反映大气细颗粒物的污染状况;利用自适应共振神经网络法分类后经人工合并将所采集到的细颗粒分为9类：OC、EC、HOC、OCEC、MD、HM、K、Na、LEV;所选时间段内SPAMS采集到的OC（24.8%）类颗粒物数量最多,沙尘过境时MD、LEV、Na类颗粒物占比不同程度增大,其余颗粒物占比减小;沙尘过境时扬尘源、生物质燃烧源、工业工艺源、餐饮及其它源贡献率增加,其中扬尘源增幅最大,而其余源贡献占比减小;后向轨迹HYSPLIT模型输送路径结果显示沙尘天气过程的起源地为塔克拉玛干沙漠,传输方向为经新疆的塔里木盆地塔克拉玛干沙漠进入青海中部,最后影响兰州地区.     

天津城区大气气溶胶复折射指数的反演及消光贡献分析

气溶胶的复折射指数是直接影响其散射特性和吸收特性的基本物理量之一.为深入研究城市大气气溶胶的复折射指数特征,引入一种具有高时间分辨率优点的反演方法来反演气溶胶复折射指数.依据辐射传输理论,将天津大气边界层观测站观测到的高精度散射系数、吸收系数和数浓度谱分布数据利用查表法代入Mie理论气溶胶粒子群消光计算公式,对大气气溶胶复折射指数进行反演.结果表明:①天津城区2011年4月观测地点0.55 μm波长处的气溶胶复折射指数实部平均值为1.64,虚部平均值为0.015.②气溶胶复折射指数实部和虚部均有明显日变化规律,实部和虚部均与相对湿度呈正相关,与风速呈负相关.③利用反演得到的复折射指数对不同粒径大气气溶胶的消光特性进行计算发现,对散射特性而言,>0.25~1.00 μm粒子对散射系数的贡献率达86%;对吸收特性而言,>0.25~2.50 μm粒子对吸收系数的贡献率为53%,>2.50~32.00 μm粒子对吸收系数的贡献率为47%.研究显示,>0.25~1.00和>1.00~32.00 μm的粒子对吸收系数的贡献率均较高,但对散射系数而言,>0.25~1.00 μm的粒子贡献率较高,因此综合考虑气溶胶散射系数、吸收系数和消光系数,控制>0.25~1.00 μm的气溶胶粒子数浓度可有效改善大气能见度.      

深圳市城区VOCs对PM2.5和O3耦合生成影响研究

为了探究珠江三角洲城市大气PM_2.5和O₃的协同污染特征,在深圳市大学城开展了秋季光化学反应活跃季大气污染加强观测.发现O₃日最大8h平均值(O₃_8h)和PM_2.5在日间具有较强的正相关关系,且O₃_8h与典型挥发性有机物(VOCs)甲醛的相关性显著高于NO₂.利用气溶胶质谱仪在线测量了亚微米气溶胶化学组成,并利用正交矩阵因子模型(PMF)对其中有机气溶胶进行来源解析,解析出5类因子,其中二次有机气溶胶(SOA)占总有机物浓度的50%.通过对污染物之间的相关性分析发现,O₃_8h和SOA具有良好的相关性,但与硝酸盐(NO₃^-)未表现出相关性,说明VOCs在深圳城区大气PM_2.5和O₃耦合生成过程中的作用比NOx明显,VOCs减排是深圳市协同控制PM_2.5和O₃污染的关键.     

Characterization of aerosol optical properties, chemical composition and mixing states in the winter season in Shanghai, China

Physical and chemical properties of ambient aerosols at the single particle level were studied in Shanghai from December 22 to 28, 2009. A Cavity-Ring-Down Aerosol Extinction Spectrometer（CRD-AES） and a nephelometer were deployed to measure aerosol light extinction and scattering properties, respectively. An Aerosol Time-of-Flight Mass Spectrometer（ATOFMS）was used to detect single particle sizes and chemical composition. Seven particle types were detected. Air parcels arrived at the sampling site from the vicinity of Shanghai until mid-day of December 25, when they started to originate from North China. The aerosol extinction,scattering, and absorption coefficients all dropped sharply when this cold, clean air arrived.Aerosol particles changed from a highly aged type before this meteorological shift to a relatively fresh type afterwards. The aerosol optical properties were dependent on the wind direction.Aerosols with high extinction coefficient and scattering Angstrom exponent（SAE） were observed when the wind blew from the west and northwest, indicating that they were predominantly fine particles. Nitrate and ammonium correlated most strongly with the change in aerosol optical properties. In the elemental carbon/organic carbon（ECOC） particle type, the diurnal trends of single scattering albedo（SSA） and elemental carbon（EC） signal intensity had a negative correlation. We also found a negative correlation（r =-0.87） between high mass-OC particle number fraction and the SSA in a relatively clean period, suggesting that particulate aromatic components might play an important role in light absorption in urban areas.     

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.     

Size distribution and chemical composition of secondary organic aerosol formed from Cl-initiated oxidation of toluene

Secondary organic aerosol (SOA) formed from Cl-initiated oxidation of toluene was investigated in a home-made smog chamber. The size distribution and chemical composition of SOA particles were measured using aerodynamic particle sizer spectrometer and the aerosol laser time-of-flight mass spectrometer (ALTOFMS), respectively. According to a large number of single aerosol diameter and mass spectra, the size distribution and chemical composition of SOA were obtained statistically. Experimental results showed that SOA particles created by Cl-initiated oxidation of toluene is predominantly in the form of fine particles, which have diameters less than 2.5 m (i.e., PM2.5), and glyoxal, benzaldehyde, benzyl alcohol, benzoquinone, benzoic acid, benzyl hydroperoxide and benzyl methyl nitrate are the major products components in the SOA. The possible reaction mechanisms leading to these products are also proposed.     

Characteristics of secondary inorganic aerosol and sulfate species in size-fractionated aerosol particles in Shanghai

Sulfate, nitrate and ammonium(SNA) are the dominant species in secondary inorganic aerosol, and are considered an important factor in regional haze formation. Size-fractionated aerosol particles for a whole year were collected to study the size distribution of SNA as well as their chemical species in Shanghai. SNA mainly accumulated in fine particles and the highest average ratio of SNA to particulate matter(PM) was observed to be 47% in the fine size fraction(0.49–0.95 μm). Higher sulfur oxidation ratio and nitrogen oxidation ratio values were observed in PM of fine size less than 0.95 μm. Ion balance calculations indicated that more secondary sulfate and nitrate would be generated in PM of fine size(0.49–0.95 μm). Sulfur K-edge X-ray absorption near-edge structure(XANES) spectra of typical samples were analyzed. Results revealed that sulfur mainly existed as sulfate with a proportion(atomic basis) more than 73% in all size of PM and even higher at 90% in fine particles. Sulfate mainly existed as(NH4)2SO4 and gypsum in PM of Shanghai. Compared to non-haze days, a dramatic increase of(NH4)2SO4 content was found in fine particles on haze days only, which suggested the promoting impact of(NH4)2SO4 on haze formation. According to the result of air mass backward trajectory analysis, more(NH4)2SO4 would be generated during the periods of air mass stagnation. Based on XANES, analysis of sulfate species in size-fractionated aerosol particles can be an effective way to evaluate the impact of sulfate aerosols on regional haze formation.