Size-resolved source apportionment of aerosol particles using polycapillary X-ray lens with a plateau in its focal spot

A laboratory micro X-ray fluorescence spectrometer based on a special polycapillary X-ray lens (PXRL) was used to carry out the source apportionment of aerosol particles. In the curve of the distribution of the X-ray intensity in the focal spot of the special PXRL, there was a plateau with a diameter of 21.3 μm in which the distribution of the X-ray intensity was homogeneous. The gain in flux density in the plateau of the PXRL is 1490. The uniformity of this plateau was 2.9%. This was helpful for the quantitative X-ray fluorescence analysis of a single aerosol particle with smaller size than that of the plateau of the PXRL. The fingerprint database of aerosol particles with given sizes from various air pollution sources was established with the single particle analysis method. The size-resolved source apportionment of aerosol particles in haze in Beijing city was performed with this fingerprint database.     

Aerosol-induced lung injuries observed by synchrotron radiation X-ray phase-contrast imaging technique

Adverse health effects are associated with the inhalation of a variety of atmospheric particles. To study the lung injuries caused by aerosol PM_2.5, synchrotron radiation (SR) X-ray phase-contrast imaging technique was used. Nude mice were inoculated with PM_2.5 samples collected from suburban area (JD), industrial area (BS) and traffic tunnel (DPQ) of Shanghai. From X-ray phase-contrast images of lung tissues, apart from blood vessels and structures of alveoli, even hemorrhage spots of several microns caused by the inflammation were clearly observed. The studies showed that the PM_2.5 samples collected from the traffic tunnel (DPQ) produced higher level of lung injury, followed by the aerosol samples collected from industrial area (BS) and suburban area (JD). Our studies also helped us to understand the process of lung injuries caused by aerosol particles.     

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.     

扫描电子显微镜结合热电离质谱测定单微粒中铀同位素比值

单微粒铀同位素分析是核保障环境监测技术的重要手段。作为现阶段应用最可靠且广泛的微粒分析技术之一,裂变径迹-热电离质谱(FT-TIMS)技术需依赖反应堆辐照,分析步骤繁琐,效率较低。扫描电子显微镜结合热电离质谱(SEM-TIMS)在保持原有TIMS的高测量精密度的同时,由扫描电子显微镜结合X射线能量色散谱仪(SEM-EDX)完成含铀微粒的寻找和鉴别,由微操作系统进行微粒转移,缩短了分析流程,提高了分析效率。本文应用建立的SEM-TIMS分析方法对已知同位素组成的单分散铀氧化物标准微粒进行了测量,测量结果与其标称值一致。     

Preparation and characterization of Ag-coated cenospheres by magnetron sputtering method

In this paper, we show the feasibility of the magnetron sputtering deposition technique to grow 10-100-nm thick, uniform, continuous and well adhesive silver films on cenosphere particles so that the properties of the core particles can be suitably modified. Experiments were conducted with a magnetron sputtering deposition system in which a newly designed sample stage equipped with an ultrasonic vibration generator was used for the tumbling of cenosphere particles. The cenosphere particles are characterized by X-ray diffraction (XRD) analysis, field emission scanning electron microscope (FE-SEM) and inductively coupled plasma-atom emission spectrometer (ICP-AES) before and after the coating process. All results show the metal film has been successfully coated onto cenosphere particles. Under the given conditions, up to 3.0 wt.% silver was deposited on cenosphere particles measured by ICP-AES. The FE-SEM results indicate that at the micro-scale the relatively uniform, compact and well adhesive silver films with about 51 nm thickness were successfully deposited on cenosphere particles. The XRD analytic result indicates that the nanometer metal film has a face-centered cubic structure.     

SPM analysis on groups of single aerosol particles around steel plant

Several methods for preparing samples of dispersed single aeroslo particles used in scanning proton microprobe(SPM) analysis were tested.Many elements such as Al,Si,S,Cl,Ca,Ti,Cr,Mn,Fe,Ni,Cu and Zn in the groups of different single aerosol particles from the Capital Steel Plant area were analyzed by SPM,The distributions of elemental contents in the group of single particles were mapped with three dimensional contour and the isometric.A new approach to study the group of different single aerosol particles for air pollution is developed in the present work.The results are significant to assessing the environmental impact of the dispersed single aerosol particles.     

质子非卢瑟福背散射测量气溶胶样品中氢、碳、氮和氧的含量

气溶胶样品中Z＞12以上元素含量的质子荧光(PIXE)分析是北京师范大学GIC4117串列加速器的主要应用领域之一。为弥补PIXE无法分析H、C、N和O等轻元素之不足，在PIXE靶室160°散射角安装金硅面垒探测器，用质子非卢瑟福背散射分析（PNBS）方法对核孔膜采集的气溶胶样品中H、C、N和O等轻元素的含量进行测量。测量得到的气溶胶样品中H和Si元素含量与质子前角散射（PESA）和PIXE的分析结果相近，表明PNBS可用于核孔膜采集的气溶胶样品的分析。     

Analysis of C, N and O in aerosol collected on an organic backing using internal blank measurements and variable beam size

A method with low MDL (minimum detection limit) was developed for analysis of carbon (C), nitrogen (N) and oxygen (O) in aerosol samples collected on an organic backing. An accelerator-produced beam of protons interacting with the sample and the detection of elastically scattered protons (PESA; particle elastic scattering analysis) and emitted X-rays (PIXE; particle-induced X-ray emission) were the basic components of the setup. The method is based on measurement of internal blank concentrations, i.e. measurement of the blank concentration outside the aerosol deposit in each sample, and the use of two sizes of the beam in order to improve the MDL of the analysis. Large beam size covering the entire aerosol deposit was used to obtain quantitative analysis with PIXE. Small beam was used to obtain relative elemental concentrations with PESA and PIXE, which were transformed to absolute values by the aid of large-beam analysis. The small-size-beam served two purposes: to make internal blank measurements feasible and to improve the signal ratio of aerosol-deposit to backing. Compared with the traditional way of analysis, using a beam that is larger than the deposit and specially prepared blank samples, the new method reduced the MDL of C, N and O by a factor of 130, 70 and 90, respectively. The new method was applied to aerosol samples collected in the upper troposphere and the lowermost stratosphere from the CARIBIC platform. As far as the authors know, these measurements are the first quantitative determinations of C, N and O in the aerosol of this part of the atmosphere. The results show that these elements together with sulfur are major components of the aerosol.     

Characterization and source identification of fine particulate matter in the atmosphere of downtown Shanghai using μ-SXRF and ICP-MS

To investigate the characteristic and sources of the free particulate matter (PM2.5), and the major sources affecting particulate air pollution in Shanghai, China, the individual aerosol particles were analyzed using the synchrotron radiation micro-beam X-ray fluorescence analysis (μ-SXRF), and the PM2.5 multi-elements were determined by the inductively coupled plasma mass spectrometer (ICP-MS). The results show that the mass concentration and chemical elements have seasonal variation, and the enrichment factors show that the chemical elements in the inhalable particles could come from the earth crust and anthropogenic pollution. The extent of metal pollution was assessed by comparing the measured concentrations with those reported in the literature. Nine categories of PM2.5 pollution sources identified at the center of Shanghai show that the vehicle exhaust, emission of metallurgic industry and coal combustion are important.     

Nondestructive measurement of the weight of kernels in a simulated cylindrical fuel compact for HTGR using X-ray computed tomography

The TRISO-coated fuel particle for the high temperature gas-cooled reactor (HTGR) is composed of a nuclear fuel kernel and outer coating layers. The coated particles are mixed with graphite matrix to make HTGR fuel element. Weight of fuel kernels contained in the element is one of the important items for evaluating the characteristics of fuel element, which is generally measured by chemical analysis or gamma-ray spectrometer. The chemical analysis is a destructive method, and gamma-ray spectrometer requires elaborate reference sample for the measurement. In this study, X-ray computed tomography (CT) is suggested to measure the weight of kernels in an element. The three-dimensional (3D) density information is acquired by the X-ray CT for a simulated compact including simulated TRISO-coated particles with ZrO₂ kernels. The volume of kernels as well as the number of kernels in the simulated compact was calculated from the 3D density information. The weight of kernels in the simulated compact was calculated from the volume of kernels and the average density of kernels. It was also calculated from the number of kernels and the average weight of kernels for comparison.     

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。     

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.     

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.     

单分散微米级铀氧化物微粒的制备

铀微粒同位素分析在核保障环境监测中发挥着重要作用。为保证准确测量单个微粒中铀同位素比,需使用丰度已知且尺寸适宜的标准微粒。通过将铀标准物溶解,并将溶液雾化形成液滴,再经蒸发溶剂、热分解一系列步骤,制得所需微粒。建立了1套以振动孔气溶胶发生器为核心的单分散铀氧化物微粒的制备装置。经扫描电子显微镜观测,制备的微粒呈球形;能谱分析表明,微粒为铀氧化物;微粒粒径主要集中在1.1μm左右,由于液滴的分裂与结合,导致了一定数量的较小和较大微粒存在;经二次离子质谱测定,其丰度值与标称值吻合,不同微粒间校正因子波动较小,能够满足实际测量的要求。     

A high sensitivity elemental analysis methodology for upper tropospheric aerosol

In this study, a sampling and analysis tool for aerosol particles has been developed. Its purpose is to characterize upper tropospheric aerosols, where concentrations are low. Since measurements will be made from an airplane, a time resolution of one hour is desirable. These conditions require efficient sampling and analysis with low detection limits. To accomplish this, our sampler uses impaction, concentrating the aerosol deposit on a small area. The impactor has 14 parallel sampling lines which are used sequentially to achieve the time resolution. The elemental analysis is done with Particle-Induced X-ray Emission (PIXE), profiting from its high absolute sensitivity. The aerosol is expected to contain primarily sulphur (S) and emphasis is placed on this element, however the multi-elemental nature of PIXE is of course used. Several substrates have been investigated regarding minimum detection limits. Scanning Transmission Ion Microscopy (STIM) analysis has been conducted on two outdoor aerosol samples, rendering three-dimensional images and mass distribution profiles. The setup was tested at ground level with high time resolution (5 min). Results show that the detection capabilities are excellent.     

Use of silicon drift detectors for the detection of medium-light elements in PIXE

In order to fully exploit in PIXE the superior performance of silicon drift detectors especially for the detection of low- and medium-energy X-rays, avoiding in particular the negative effects of backscattered particles, we developed a custom spectrometer based on a 10 mm² chip with a thermoelectric Peltier cooler and home-designed front-end electronics, coupled to a weakly focusing polycapillary lens.This paper briefly describes the detector + lens assembly and reports the results of first tests carried out at an external beam line of the LABEC laboratory in Florence. Excellent energy resolution is achieved under real operating conditions in a PIXE run (measured FWHM at 1 keV is 81 eV with a count-rate of 480 cps) and also the lineshapes are very good (FW1/10M over FWHM ratio is 2.1). As a whole, our preliminary tests gave encouraging results and also helped to point out some aspects which it is worthwhile to investigate further (e.g. how X-ray peak intensity ratios may be affected by inaccurate lens alignment), in order to profit fully from such a good performance of the spectrometer.     

北京地区大气中7Be、137Cs和131I活度浓度分布规律初步研究

介绍了全面禁止核试验条约（CTBT）国际监测系统（IMS）北京核素台站和北京放射性核素实验室的大气气溶胶取样和测量过程;对核素台站和放射性核素实验室的大气气溶胶的长期监测数据进行了统计分析,得到了⁷Be、¹³⁷Cs和¹³¹I活度浓度的分布特点和规律,为深入研究大气中相关放射性核素浓度分布规律奠定了基础。     

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.     

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.