Highly time-resolved aerosol characteristics during springtime in Weizhou Island

A single particle aerosol mass spectrometer was deployed to measure the changes of single particle species and sizes during March 2015 in Weizhou Island of the Beibu Gulf, Guangxi province, South China. In this campaign, a total of 3,100,597 particles were sized, and 25.8%particles with both positive and negative mass spectrum were collected and 24.8%characterized in combination with the ART-2 a neural network algorithm. The distribution of sized particles was mainly in from 520 to 600 nm, and the diameters ranging from 340 to1000 nm accounted for above 90%. Eight types of particles were classified: Elemental Carbon containing(EC), Organic Carbon containing(OC), EC and OC combined containing particles,Na containing particles, K containing particles(K), Levoglucosan containing particles,mineral containing particles, and Heavy Metal containing particles(HM). EC, OC and K were the major containing particles, which accounted for 84.3% in the eight types particles. The relative ratio and size distribution of the three types were EC(48.1%, 620 nm), OC(12.7%,440 nm), and K(23.5%, 600 nm), respectively. The three types of particles were a bit increasing ratios compared with those in clean periods during haze pollution periods.Combined with the back-trajectory results from the Hysplit-4 model and local pollution sources revealed that the ambient air quality on the Weizhou Island may be influenced by biomass burning in the Indochina Peninsula(biomass burning in the Indochina Peninsula)from the transportation on higher level atmospheric layer and by mainland of south China located northeast of Weizhou Island on the ground.     

PM_(2.5)和PM_(2.5~10)资料同化及在南京青奥会期间的应用试验

建立了面向PM_(2.5)和PM10观测资料的三维变分同化系统,并在南京地区青奥会期间进行了同化和预报试验.同化系统的控制变量为PM_(2.5)和PM_(2.5~10)(PM10中扣除PM_(2.5)后剩余部分),利用南京地区2014年8月的WRF-Chem模拟结果,估计了PM_(2.5)和PM_(2.5~10)的背景误差协方差,发现在水平和垂直方向上PM_(2.5)的相关系数随距离的衰减均小于PM_(2.5~10),这可能与PM_(2.5)粒径小、生命史长,在大气中传播地更远有关.利用南京及周边区域的134个监测站PM_(2.5)和PM_(10)逐时观测资料,对青奥会期间(2014年8月16~28日)进行滚动同化和预报试验,并利用模式最内层观测资料进行检验分析,结果表明同化对初始场有显著改进,PM_(2.5)和PM10的相关系数均提高53%以上,均方根误差降低55%以上,平均偏差则降低了90%左右;同化试验对其后的预报场也有明显改进,正效应可以持续到20h以后,模式对PM10的预报效果好于PM_(2.5).     

Organic aerosol molecular composition and gas–particle partitioning coefficients at a Mediterranean site (Corsica)

Molecular speciation of atmospheric organic matter was investigated during a short summer field campaign performed in a citrus fruit field in northern Corsica(June 2011). Aimedat assessing the performance on the field of newly developed analytical protocols, this work focuses on the molecular composition of both gas and particulate phases and provides an insight into partitioning behavior of the semi-volatile oxygenated fraction. Limonene ozonolysis tracers were specifically searched for, according to gas chromatography–mass spectrometry(GC–MS) data previously recorded for smog chamber experiments. A screening of other oxygenated species present in the field atmosphere was also performed. About sixty polar molecules were positively or tentatively identified in gas and/or particle phases. These molecules comprise a wide range of branched and linear, mono and di-carbonyls(C_3–C7),mono and di-carboxylic acids(C_3–C_18), and compounds bearing up to three functionalities.Among these compounds, some can be specifically attributed to limonene oxidation and others can be related to α- or β-pinene oxidation. This provides an original snapshot of the organic matter composition at a Mediterranean site in summer. Furthermore, for compounds identified and quantified in both gaseous and particulate phases, an experimental gas/particle partitioning coefficient was determined. Several volatile products, which are not expected in the particulate phase assuming thermodynamic equilibrium, were nonetheless present in significant concentrations. Hypotheses are proposed to explain these observations, such as the possible aerosol viscosity that could hinder the theoretical equilibrium to be rapidly reached.     

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.     

标准气溶胶发生系统的建立与性能评估

针对气溶胶测量仪器校准和实验室气溶胶光学特性研究的需求,搭建了一套标准气溶胶发生系统,并对其性能开展了测试研究.系统采用恒定流量的雾化器产生气溶胶,经过扩散干燥管干燥以及电荷中和器带电中和后,产生标准气溶胶粒子.利用氯化钠样品对系统的性能进行了测试,结果表明,当样品溶液浓度增加时,系统雾化产生粒子的数浓度和粒径均随之增加;当载气气压增加,系统雾化产生粒子的数浓度随之增加,而粒径随之减小.在测试时间内,系统发生的多分散气溶胶粒子的几何平均粒径波动小于1%,总粒子数浓度波动小于2%,单分散气溶胶粒子数浓度的稳定性好于4%.     

北京地区不同时段平均PM2.5浓度与MODIS气溶胶光学厚度相关性分析

利用2014年北京市12个空气质量监测站的逐小时PM_(2.5)地面观测资料,以及Terra和Aqua卫星的MODIS气溶胶光学厚度(AOD)产品,在时间和空间数据匹配的基础上,研究了PM_(2.5)的5 h(10:00—14:00)和24 h(0:00—23:00)两种时段平均浓度及两颗卫星平均AOD的时空分布特征,并建立了AOD与不同时段平均PM_(2.5)浓度之间的回归模型.结果表明:PM_(2.5)的5 h平均浓度和24 h平均浓度值均在城区高、郊区低,最低值位于定陵站;匹配后逐时PM_(2.5)浓度的日变化呈"双峰型",最低值出现在下午,但北京西北部郊区的定陵和昌平镇站因局地山谷风环流和外部排放源的影响,其"双峰型"波动趋势较城区站偏弱,最低值出现在上午;AOD的空间分布特征与PM_(2.5)浓度分布一致,但在郊区由于污染水平分布不均,卫星采集的样本可能来自于周围的清洁大气,导致AOD的最小值在郊区站点明显低于城区站点;两颗卫星平均的AOD与5h PM_(2.5)平均浓度的决定系数高于AOD与24 h PM_(2.5)平均浓度的决定系数;AOD与PM_(2.5)的相关系数在城区高于郊区,郊区排放源分布不均和强的局地系统性环流是造成其相关系数低的重要原因.     

乌鲁木齐市MODIS气溶胶光学厚度与PM10浓度关系模型研究

为了建立乌鲁木齐市近地面PM10浓度监测的关系模型,利用乌鲁木齐市2013年3—11月、2014年3—11月MODIS AOD产品与同期地面观测的PM10质量浓度进行相关分析,结果表明二者直接相关程度较低(r=0.433,p0.01);然后以WRF模式模拟的大气边界层高度及地面观测的相对湿度数据对AOD进行垂直、湿度订正后,二者相关性得到较大程度提高(r=0.630,p0.01);按照季节分类统计和订正春、夏、秋季的相关系数r分别为0.779、0.393、0.523,均大于统计学上99%的置信度要求,其中春季的订正最为有效,可用性更高;最后,建立全年和各季AOD-PM10最优拟合模型并反演乌鲁木齐市地面PM10质量浓度,全年和三季的反演结果与实测数据的相关系数分别为0.757、0.748、0.652、0.715(p0.01);同时基于卫星遥感AOD反演得到的PM10质量浓度的空间分布与AOD呈现出整体的一致性,并且3个季节AOD平均值表现为:春季秋季夏季.证实了卫星遥感AOD经过垂直和湿度订正后,可以作为辅助监测乌鲁木齐市PM10地面浓度分布的一个有效手段.     

混合基质3D打印可见光催化系统对病毒气溶胶的去除

利用3D打印灵活可控的特点和复合材料混合打印的优势，将可见光响应的ZnO/g-C₃N₄催化剂掺入ABS塑料，利用3D打印制成催化剂均匀稳定分布的光催化系统，使用流体动力学仿真模拟对反应器结构进行优化设计，用于处理相对密闭的室内空间中的病毒气溶胶.结果表明，病毒气溶胶比细菌气溶胶具有更强的抗逆性，添加螺旋导流板可以显著提升反应器传质性能并有效改善系统光催化效果，以提高对病毒气溶胶的去除率.以商业LED灯为光源的螺旋式反应器对高浓度病毒气溶胶（MS2、PhiX174噬菌体）和细菌气溶胶（大肠杆菌）具有高效去除效果，在3.75min停留时间可以实现对气溶胶的完全去除.     

超声雾化法捕集气溶胶的试验研究

核设施退役过程,放射性气溶胶浓度较高,需要进行处理,以降低工作人员辐照风险。研究捕集剂配方、雾化通入量等对模拟气溶胶捕集效果的影响,结果表明:捕集剂配方对气溶胶捕集的效果差异明显;粒径越小的气溶胶粒子被雾化捕集的速度较慢;捕集剂通入量在0.06 kg/m3以下,对气溶胶捕集效果影响显著。对等离子切割解体设备产生的241Am、239Pu污染气溶胶进行雾化捕集,初始污染水平为136 Bq/m3的气溶胶经雾化捕集后可降至1.23 Bq/m3,捕集的效果显著。     

Acid-catalyzed heterogeneous reaction of 3-methyl-2-buten-1-ol with hydrogen peroxide

Acid-catalyzed heterogeneous oxidation with hydrogen peroxide(H2O2) has been suggested to be a potential pathway for secondary organic aerosol(SOA) formation from isoprene and its oxidation products. However, knowledge of the chemical mechanism and kinetics for this process is still incomplete. 3-Methyl-2-buten-1-ol(MBO321), an aliphatic alcohol structurally similar to isoprene, is emitted by pine forests and widely used in the manufacturing industries. Herein the uptake of MBO321 into H2SO4–H2O2mixed solution was investigated using a flow-tube reactor coupled to a mass spectrometer. The reactive uptake coefficients(γ) were acquired for the first time and were found to increase rapidly with increasing acid concentration. Corresponding aqueous-phase reactions were performed to further study the mechanism of this acid-catalyzed reaction. MBO321 could convert to 2-methyl-3-buten-2-ol(MBO232) and yield isoprene in acidic media. Organic hydroperoxides(ROOHs) were found to be generated through the acid-catalyzed route,which could undergo a rearrangement reaction and result in the formation of acetone and acetaldehyde. Organosulfates, which have been proposed to be SOA tracer compounds in the atmosphere, were also produced during the oxidation process. These results suggest that the heterogeneous acid-catalyzed reaction of MBO321 with H2O2 may contribute to SOA mass under certain atmospheric conditions.