Identification of origin of single aerosol particles using polycapillary X-ray lens

A micro X-ray fluorescence (Micro-XRF) spectrometer based on a polycapillary focusing X-ray lens (PFXRL) and a laboratory X-ray source was designed to carry out the XRF analysis of single aerosol particles. The minimum detection limit (MDL) of this Micro-XRF spectrometer was 9 ppm for the Fe-Kα. The percentage of the particles of vehicle exhaust among aerosol particles was studied in Beijing, Chinese capital, during the test of odd-even driving restrictions for Beijing 2008 Olympics Games. This Micro-XRF spectrometer had potential applications in the analysis of single aerosol particles.     

基于扫描核探针技术的大气气溶胶单颗粒物源识别与解析方法研究与应用

将高分辨、高灵敏的扫描核探针(SNM)技术与人工神经网络(ANN)模式识别方法相结合,以单个气溶胶颗粒物化学表征为基础,开展大气气溶胶源识别与解析的新方法研究。摸索出单颗粒气溶胶SNM靶样的制备方法。建立了SNM多站多参量分析模式的数据获取系统和分析条件。用SNM测定了单个大气气溶胶粒子的元素谱特征。基于标准的误差反向传输神经网络算法,建立ANN模式识别系统,直接对单个气溶胶粒子的SNM分析能谱模式进行识别,判别其来源,计算源的贡献率。将建立的方法初步应用于上海市大气PM10源识别与解析研究。结果表明该方法解析能力强,解析结果客观,具有查找未知污染源、解析低浓度污染源的特点。     

Source apportionment of single aerosol particles in the atmosphere of Shanghai city

A nuclear microprobe with high spatial resolution and high analytical sensitivity was applied to analyze atmospheric aerosol at five monitoring sites in Shanghai city.Meantime,a new pattern recognition technique,which used the micro-PIXE spectrum of a single aerosol particle as its fingerprint.was developed to identify the origin of the particle.The results showed that the major contributors to the atmosphere pollution were soil dust(31.6%) ,building dust(30.8%),and the next were vehicle exhaust(13.7%),metallurgic industry excrements(5.6%).oil combustion(5%) and coal combustion(2.3%).Besides these ,about 10% of the particles could not be identified.Based on the cluster analysis of these particles.they could be divided into eight groups.By inference,they might belong to some sub-pollution sources from soil dust,building dust and metallurgic industry excrements.Moreover,some new pollution sources from tyres and chemical plants were also revealed.     

Aerosol composition and source apportionment in Santiago de Chile

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp<2 μm) and coarse mode aerosol (210 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m⁻³. Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m³ PM₁₀). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM₁₀ aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO₂. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of several heavy metals such as Zn, Cu and others. A factor with molybdenum, arsenic, copper and sulfur was observed frequently, and it results from emissions of copper smelters.     

PIXE and PIGE techniques for the analysis of Antarctic ice dust and continental sediments

An analytical procedure has been implemented in this work for an accurate geochemical characterization and quantitative analysis of the fine dust (particles diameter < 5 μm) trapped in Antarctic ice cores and the fine fraction of potential source areas (PSA) sediments by size selection, filtering and PIXE-PIGE combined measurements. The underestimation of concentrations of the lighter elements, like Na, Mg, Al and Si, due to X-ray self-absorption inside each individual aerosol particle, was also evaluated and the analytical overall accuracy tested by means of measurements performed on size selected certified mineral standards.     

核分析相关技术用于上海市大气污染特征研究

本文研究了近年来上海市区和郊区大气气溶胶颗粒物的污染状况,采用的多种核分析方法及相关技术有质子激发X荧光分析(PIXE)、激光粒径谱仪(LPS)、同步辐射X射线吸收精细结构(XAFS)和扩展X射线吸收谱精细结构(EXAFS)分析等先进技术.充分发挥核分析技术高灵敏度、快速无损、多元素微量微区同时分析的优势,从大气颗粒物的形貌特征、粒径分布、质量浓度、元素浓度、化学价态等入手,对上海大气可吸入颗粒物PM23和PM1o展开多方位的综合研究.     

De-agglomeration mechanisms of TiO2 aerosol agglomerates in PWR steam generator tube rupture conditions

A steam generator tube rupture (SGTR) in a pressurized water reactor (PWR) might be a major source of accidental release of radioactive aerosols into the environment during severe accident due to its potential to by-pass the reactor containment. In the ARTIST program, tests were carried out at flow conditions typical to SGTR events to determine the retention of dry aerosol particles inside a steam generator tube. The experiments with TiO₂ agglomerates showed that for high velocities in the range of 100-350 m/s, the average particle size at the outlet of the tube was significantly smaller than at the inlet due to particle de-agglomeration. Earlier, particle de-agglomeration has not been considered significant in nuclear reactor severe accidents. However, the tests in ARTIST program have shown that there is a possibility that TiO₂ aerosol particles de-agglomerate inside a tube and in the expansion zone after the tube exit under SGTR conditions.In this investigation, we measured TiO₂ aerosol de-agglomeration in the tube with very high flow velocities with two different TiO₂ aerosols. The de-agglomeration was determined by measuring the size of the agglomerates at the inlet and outlet of the test section. The test section was composed of tubes with three different lengths, 0.20, 2.0 and 4.0 m, followed by an expansion zone.The main results were: (i) the de-agglomerate process was relatively insensitive to the initial particle size distribution, (ii) the agglomerates were observed to de-agglomerate in all the tubes, and the resulting particle size distributions were similar for both TiO₂ aerosols, (iii) at high flow rates, increasing the gas mass flow rate did not produce further de-agglomeration, and (iv) the agglomerates did not de-agglomerate to primary particles. Instead, after de-agglomeration the particles had a median outer diameter D_c = 1.1 μm. Based on analysis using computational fluid dynamics (CFDs), the de-agglomeration was caused by the turbulent shear stresses due to the fluid velocity difference across the agglomerates in the viscous subrange of turbulence.It has to be noted that the particles used in this investigation were TiO₂ agglomerates, and not prototypical nuclear aerosols with significantly different characteristics. Therefore, the results of this investigation cannot be directly used to determine whether the nuclear aerosol particles may de-agglomerate in SGTR sequences. However, this investigation highlights the possibility of particle de-agglomeration under SGTR conditions, and identifies the mechanism of the de-agglomeration inside the broken tube and when the aerosol is discharged to an open space.     

严重事故下吸湿性气溶胶的自然去除研究

反应堆发生严重事故时,堆芯释放出的吸湿性气溶胶会在潮湿的安全壳内增大,从而影响其自然去除过程。本文理论推导了吸湿性气溶胶的增大模型并通过多种方法对其进行了验证。模型计算结果表明,气溶胶的增大过程由于受到溶解度的限制而存在临界湿度值,在该临界值以下时气溶胶不发生吸湿,但这未被其他严重事故分析程序所考虑。同时,基于某三代先进压水堆的特定严重事故工况,本文分析了干颗粒半径及湿度对气溶胶的平衡半径和自然去除系数的影响。结果表明:气溶胶的自然去除系数随干颗粒半径的增大将先减小后增加,并在1 μm时达到最小值;相同湿度下,干颗粒半径对气溶胶半径的最大增大比例的影响不大;湿度的增加对不同干颗粒半径气溶胶去除系数的影响不同。      

Estimating particle size effects in X-ray fluorescence spectrometry

The influence of size of particles on the X-ray fluorescence intensity for powdered substances with different sized particles is estimated, based on a simple modification of the Berry-Furuta-Rhodes formulae. Analytical expressions are obtained for the model of a powder substance consisting of particles of various sizes distributed randomly in the sample volume. The results of calculations by these expressions agree fairly well with experimental data for binary powder mixtures. The particle size effect on X-ray fluorescence for the powders presented is considerably more than one could be predicted by the models proposed earlier.     

Analysis of atmospheric aerosols by PIXE: the importance of real time and complementary measurements

Particle-Induced X-ray Emission (PIXE) has been used for more than 30 yr in many urban and background air pollution studies. The technique has certainly contributed to the understanding of source-receptor relationship for aerosol particles as well as to aerosol physics and chemistry. In the last few years, where aerosol issues were strongly linked to global climate change through the relationship between aerosol and atmospheric radiation points to new challenges in atmospheric sciences, where PIXE could play an important role. Also the recognition for the inter-relationship between aerosol and liquid and gas phases in the atmosphere makes important to integrate PIXE aerosol analysis with other complementary measurements. The use of Nephelometers and Aethalometers to measure scattering and absorption of radiation by aerosol particles can be done in parallel with particle filter collection for PIXE analysis. Parallel measurements of trace gases using traditional monitors as well as with new techniques such as Differential Optical Absorption Spectroscopy (DOAS) that can provide concentration of O₃, SO₂, NO₃, NO₂, HCHO, HNO₃, Benzene, Toluene, and Xylene, is also important for both urban and remote aerosol studies. They provide information that allows a much richer interpretation of PIXE data. Recently developed instruments that provide real time aerosol data such as the Tapered Element Oscillating Microbalance (TEOM) PM₁₀ monitor and automatic real time organic and elemental carbon analyzers provide extremely useful data to complement PIXE aerosol analysis. The concentrations of trace elements measured by PIXE comprise only 10–30% of the aerosol mass, leaving the organic aerosol characterization and measurement with an important role. The aerosol source apportionment provided by PIXE analysis can be extended with other aerosol measurements such as scattering and absorption, estimating for example, the radiative impact of each discriminated aerosol source. The aerosol bulk PIXE measurements can be complemented with soluble concentrations provided by Ion Chromatography (IC) and Inductively Coupled Plasma-Mass Spectrometry (ICP-MS). Recent developments in remote sensing techniques and products also enhance significantly regional aerosol studies. Three-dimensional air mass trajectories should be integrated in aerosol studies for urban and remote areas. The applications of these techniques to study urban aerosols from São Paulo and Santiago de Chile have broadened extensively the scientific scope of these studies.     

Soller slits automatic focusing method for multi-element fluorescence detector

In X-ray absorption fine structure(XAFS) experiments,Soller slits are widely used as filter devices in order to improve the signal to noise ratio.Performing high accuracy manual focusing operations is a time-consuming process;therefore,this work introduces an automatic focusing method for Soller slits in multi-element fluorescence detectors.This method establishes a relation model between the fluorescence intensity distribution and the coordinates of the fluorescence excitation point.According to this relation model,the actual coordinates of the fluorescence excitation point can be deduced from the detected fluorescence intensity distribution and used in focusing operations.This method has proven to be feasible in an XAFS experiment at the BL14W1 beamline of the Shanghai Synchrotron Radiation Facility.     

一种用于SPM分析的大气气溶胶单颗粒样品的制备方法

介绍了一种用于扫描质子微探针分析的大气气溶胶单颗粒样品的制备方法。通过实验摸索出一种适合于支撑颗粒物的材料聚乙烯醇缩丁醛(PVB)。大气颗粒物被直接采集在PVB薄膜上从而制成样品,保持了颗粒物的原始信息。用显微镜观察了采集的颗粒物,颗粒物之间完全分开,颗粒物间距合适。样品的扫描质子微探针试验结果表明,所制成的单颗粒样品能经受住质子束的长久轰击。对PVB薄膜的本底测试表明,这种膜的本底很小,不会对被测颗粒物的元素产生干扰。     

MAPPIX: A software package for off-line micro-pixe single particle aerosol analysis

In the framework of a multiannual experiment performed at Baia Terra Nova, Antarctica, size-segregated aerosol samples were collected by using a 12-stage SDI impactor (Hillamo design). Approximately 2800 particles, belonging to the first four supermicrometric SDI stages – 8.39, 4.08, 2.68, 1.66 μm dynamic aerosol diameter cuts – were analyzed at the INFN-LNL micro-PIXE facility, a three lens Oxford Microprobe (OM) product, installed in the early nineties. Four regions on each of the 12 sub-samples were measured; 60 aerosol particles were detected on average in each of the analyzed regions.The off-line single aerosol particle (SAP) analysis of such big amount of data required software that is able to rapidly handle the acquired data, with a simple and fast area selection procedure; the subsequent automated PIXE spectra analysis with a specialized code was also needed.The MAPPIX 2.0 software was designed to make easier and faster the user jobs during the SAP analysis. The package is composed of two separate routines: the first one is devoted to data format conversion (OM-LMF file format to MAPPIX format), while the second one is devoted to micro-PIXE maps graphical presentation and aerosol particle selection procedure.The MAPPIX data format and software features will be discussed; a short report of the speed performances will be presented.     

严重事故下多组分吸湿性气溶胶的重力沉降研究

严重事故时,安全壳内的多组分吸湿性气溶胶将在高湿度的条件下吸水增大,从而影响其重力沉降行为。通过理论分析,本文推导了多组分吸湿性气溶胶颗粒平衡粒径的物理模型,并通过实验结果进行验证。该模型重点关注溶解度对吸湿过程的影响,解释了多组分吸湿性颗粒粒径增大曲线不连续的原因。同时,分析了典型千兆瓦级压水堆核电厂中相对湿度、干粒径及非吸湿性组分质量分数对重力沉降去除系数的影响。结果表明,只有当气溶胶颗粒增大到一定程度后,其重力沉降速度才会明显的提高;对于干粒径超过0.01 μm的纯吸湿性气溶胶颗粒,只有超过一定湿度后其才会因吸湿而加速沉降,且该湿度下限随着干粒径的增大而减小;随着事故的进行,气溶胶颗粒中的非吸湿性组分质量分数逐渐增加,上述湿度下限将增加,且同湿度下吸湿对重力沉降的促进作用减弱。      

用于HL-2A装置的新型硬X射线探测器

介绍了一种应用于托卡马克等离子诊断领域的新型硬X射线探测器,该探测器主要由硅酸钇镥(Lutetium-yttrium Oxyorthosilicate,LYSO)闪烁体和硅光电倍增管(Silicon Photomultiplier,Si PM)组成。基于项目应用需求,对探测器的选型和基于粒子输运蒙特卡罗仿真软件GEANT4的探测器设计加以阐述,并搭建了前端的探测系统,在HL-2A托卡马克装置上进行了现场诊断实验。实现了硬X射线空间能谱和辐射强度分布的诊断测量。实验表明该探测器阵列具有10 ms的时间分辨率,同时具有结构紧凑、使用方便等特点,能够满足等离子体诊断中硬X射线动态能谱和强度分布测量的诊断需求。     

鼓泡过滤多分散气溶胶特性的矩估计分析

池式鼓泡过滤是核电站严重事故场景以及缓解措施中一种典型的放射性气溶胶滞留过程,评估气溶胶在该条件下的去除特性对事故后期的源项评估和制定相应的缓解措施具有重要意义。针对鼓泡过滤多分散气溶胶这一背景,本文假设气溶胶的尺度分布满足对数正态分布,考虑布朗扩散、重力沉降以及惯性碰撞3种机制对气溶胶在气泡内沉降的影响,利用矩方法得到了气溶胶尺度分布的3个分布参数（N、d_pg、σ_g）与其初始值、气泡上升高度以及沉降系数之间的解析关系。通过与精确解对比,对数正态矩方法推导的解析解表现出良好的预测精度。本文得到的解析解可在不需要气溶胶尺度分布具体信息而仅需要一些初始分布参数的情况下对气溶胶的去除特性进行快速评估。     

X射线源针孔成像方法可行性研究

为检验利用针孔成像对X射线源进行研究的可行性，对X射线针孔成像系统进行优化设计，搭建了1套X射线源针孔成像装置。从理论上对X射线源的位置和强度发生变化时图像的相应变化进行了计算和预估，并用实验加以验证。结果表明，像斑中心位置的移动和像斑灰度值的变化分别与X射线源位置和强度的变化在一定范围内存在线性关系，由此证明了利用针孔成像对X射线源进行空间定位及定量研究的可行性。本文结果对X射线源针孔成像的系统设计具有参考意义。     

Behavior of Sodium Oxide Aerosol in a Closed Chamber

The behavior of sodium oxide aerosol in a closed chamber was studied for the safety analysis of a Na-cooled fast reactor. The experimental apparatus and techniques are first described. The aerosol was released during a short time by blowing air onto heated Na in a 1 m³ chamber. The maximum mass concentration of the aerosol in the form of Na₂O ranged of 0.05 ～ 10g/m³. The particle size distribution, the aerosol mass concentration and the mass deposition rates were measured as a function of time.

It was found that the mass median diameter of the aerosol was related to the maximum mass concentration. To determine the character of the behavior of sodium oxide aerosol in the chamber, the density of the aerosol material and the thickness of the boundary layer through which the particles deposit on the chamber wall were observed. The initial half-time of the aerosol mass concentration was compared with the values numerically calculated under certain assumptions.     

爆轰条件下的气溶胶粒径分布及Ag质量分数与粒径的关系

用货币银化爆实验研究了爆轰条件下气溶胶生成量及粒径分布规律.实验结果表明,爆炸后气溶胶粒子粒度分布的变化,主要取决于布朗凝并以及重力沉降相结合的过程,相对稳定气相中的气溶胶粒度主要分布在1.8μm左右;用中子活化法分析不同粒径的气溶胶粒子中Ag的质量分数,结果表明,Ag存在着明显的分凝效应;经过SEM和XRD方法分析,10μm以下的Ag气溶胶粒子多以由较小的多晶聚合体逐级凝并成较大的聚合体结构存在,平均晶粒尺寸为27.3nm.     

Characteristic X-rays induced by electrons and positrons from β-emitting radioisotopes

We have investigated the use of energetic electrons and positrons from low intensity ⁹⁰Sr and ²²Na radioactive sources respectively to produce characteristic radiation and compare the emission efficiencies of each kind of particle. A new proposed experimental set-up for radioisotope-excited X-ray fluorescence analysis is of the transparent source type and provides at least a ten-time increase in the intensity of characteristic X-rays emitted by the sample as compared to a standard radioactive source arrangement. Theoretically derived expressions for β-particle penetration, transport and emission processes in a sample are presented, and experimental results of absolute characteristic X-ray yields induced by electrons and positrons from 31 pure chemical elements, from titanium to lead, have been included. The advantages of energetic β-particles in comparison with other radiation sources are also discussed, in fact, a remarkable feature observed being that radiation yield changes by less than an order of magnitude across the whole range of the target atomic numbers herein considered.