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。     

Gold解谱算法在放射性气溶胶监测中的应用

介绍了一种在线式气溶胶监测方法,该方法利用γ放射性测量分析气溶胶中的放射性核素种类,在后期能谱处理中利用Gold解谱算法确定入射射线的能量和比例。为了得到解谱所需的响应矩阵,利用蒙特卡罗方法计算了测量装置对不同能量γ射线的响应能谱,并测试了算法的应用效果。提出了一种改进方法,克服了当响应矩阵较大时Gold算法计算较慢的运算速度问题。测试结果表明,改进算法能够在保证计算结果一致的情况下大幅提高运算速度。     

γ谱法监测环境中放射性气溶胶

为了更有效地对环境中放射性气溶胶进行监测,探讨了γ谱法测量放射性气溶胶的监测方法。该方法将环境中气溶胶颗粒过滤到滤膜之上,利用配以闪烁体探测器的γ谱仪测量过滤膜上的γ放射性气溶胶颗粒的γ能谱,通过γ能谱解析来获得环境样品中放射性核素类型及其活度。实验结果表明:该方法可有效地监测放射性气溶胶,对环境样品中放射性核素具有一定的鉴别能力。     

滤纸吸附氡子体气溶胶能谱的研究

通过使用在线监测仪在氡室中对氡子体气溶胶能谱进行测量,获取了滤纸吸附氡子体气溶胶能谱,研究了氡子体α能谱重叠的原因,找到了描述给定测量时间滤纸吸附氡子体气溶胶能谱的方法。采用离散化法处理滤纸上氡子体的累积过程,建立累积模型。该模型可以准确描述累积过程,得到给定取样时间下滤纸吸附氡子体气溶胶的累积能谱,为更准确地模拟氡子体的α粒子能谱提出了可行性方案。     

一种γ能谱光滑效果评价方法

在γ能谱数据处理中需要对测量能谱进行光滑以降低统计涨落。实际应用中,针对不同的γ能谱,需要对各种能谱光滑算法的光滑效果进行科学的比较和评价,选择最佳的能谱光滑算法及最佳光滑参数。文章从γ能谱计数的统计涨落规律出发,提出了一种评价能谱光滑算法效果的方法,给出了评价参数,并计算了光滑效果的等效测量时间。根据实验测量的γ能谱数据,采用5点三次多项式拟合最小二乘法对不同光滑次数的光滑效果进行了对比,优选了光滑算法的光滑次数参数,并给出了等效测量时间,提高了谱数据处理的精度和准确度。     

滤膜对放射性气溶胶α能谱测量拖尾影响

滤膜是放射性气溶胶测量系统中重要组成部分,由于滤膜本身的特性造成天然放射性气溶胶α能谱拖尾会干扰人工放射性气溶胶测量结果,甚至会造成测量结果错误。通过实验分别测试相同滤膜(混合纤维)不同孔径和相同孔径不同滤膜对α能谱测量拖尾的影响。实验表明,用小流量(5 L·min-1)系统采集天然放射性气溶胶时,选用和天然放射性气溶胶最大粒径(0.5μm)相当大小孔径的混合纤维滤膜(0.45μm)时,α能谱拖尾最小,加大抽气流量(20 L·min~(-1)),α能谱拖尾最小的混合纤维滤膜孔径略有减小(0.3μm);相同孔径下(0.45μm),混合纤维滤膜相比聚四氟乙烯滤膜和聚醚砜滤膜,对α能谱测量拖尾影响最小。本文为减小天然放射性气溶胶测量时α能谱拖尾选取合适滤膜提供了重要依据。     

大气气溶胶样品中放射性核素分析(Ⅰ)气溶胶样品中放射性γ能谱分析方法

介绍了一种利用HPGeγ谱仪测量和研究大气气溶胶放射性的方法。用气溶胶采样器收集大气气溶胶样品,将滤材样品压制成片状,通过对γ能谱的分析,确定了样品中放射性核素的种类,并计算其在大气中的浓度。由于气溶胶样品活度水平很低,在测量时样品需要放在探测器表面,在数据处理过程中还需进行级联符合相加效应校正。     

基于蒙特卡罗方法对光子束剂量沉积核的研究

用蒙特卡罗的程序BEAMnrc模拟西门子加速器6 MV光子束,由BEAMdp子程序分析得到不同射野的能谱分布和平均能量,并建立相应模拟源(能谱源与单能源),由DOSXYZnrc子程序使用模拟源笔形束,在标准水模体中计算最大剂量深度处的剂量沉积核,以比较不同源对剂量沉积的影响。结果表明,不同射野下获得的能谱源对剂量沉积的差异较小,最大百分剂量差1.47%;使用平均能量的单能源剂量差别较大,最大达6.28%。而对于利用同一射野下能谱源和单能源计算的剂量核进行比较,最大百分剂量差在9%以上,甚至达到13.2%。由此可见,剂量沉积核具有光子能量依赖性,由于加速器产生的光子束是具有能谱分布的,只利用某一单能源来进行剂量计算会造成较大的误差,使用能谱源计算剂量沉积核会更为准确。     

气溶胶中钋-210的分析

采用α能谱示踪法进行了大气气溶胶中的210Po分析方法研究。气溶胶滤膜样品经剪碎后加入209Po示踪剂,在硝酸-硫酸-高氯酸体系中湿式消化,用0.5 mol/L盐酸反复浸取,在高温高速搅拌的水浴中置入银片自沉积,样品源银片在α能谱仪上测量。建立的分析测量方法,对于采样体积大于500m3的气溶胶样品,探测下限可达0.01 m Bq/m3,回收率接近95%。本方法经多项质量控制措施验证,现已在国家辐射监控点大气气溶胶测量和铀矿污染源监测项目中得到应用。     

220Rn子体气溶胶粒径分布测量的方法研究

应用ELPI系统、α谱仪和能量甄别法测量程序,建立了1套²²⁰Rn子体气溶胶活度粒径分布的测量方法;利用该方法收集了南华大学²²⁰Rn实验室不同粒径的²²⁰Rn子体气溶胶,并进行了²²⁰Rn子体气溶胶活度粒径分布测量。实验结果表明：ThB气溶胶的活度中位粒径(AMAD)平均值为237 nm,ThC气溶胶的AMAD平均值为245 nm。该方法简便易行、测量周期短,能实时得到²²⁰Rn子体气溶胶粒子数粒径分布的情况,能同时得到ThB和ThC气溶胶的活度粒径分布情况,且能谱法的测量精度也相对较高。     

Study of emission episodes of urban aerosols by ion beam analytical techniques

The quantitative elemental composition and morphology of over 500 atmospheric aerosol particles were determined by nuclear microscopy and scanning electron microscopy (SEM). The samples originated from eight sampling campaigns, when hourly variation and sources of the urban aerosol elemental components were studied in Debrecen between 2007 and 2010. Aerosol which could be connected to heavy metal pollution episodes and high aerosol pollution levels deposits were selected for the nuclear microprobe study.Ion beam analytical methods (micro-PIXE and STIM) provided the elemental composition of coarse (particles with aerodynamic diameter between 2.5 and 10 μm) aerosols while the morphology of the different particle types was determined by SEM.Through the elemental composition, elemental correlations and morphology different particle types were identified and attributed to different anthropogenic sources like biomass burning, oil combustion, traffic or industry.     

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.     

Micro-PIXE study of Ag in digestive glands of a nano-Ag fed arthropod (Porcellio scaber, Isopoda, Crustacea)

Micro-proton induced X-ray emission (micro-PIXE) method was applied to study the micro-localization of silver (Ag) in digestive glands of a terrestrial arthropod (Porcellio scaber) after feeding on silver nanoparticles (nano-Ag) dosed food. The aim of our work was to assess whether feeding on nano-Ag results in the assimilation of silver (Ag) in digestive gland cells. To study micro-localization and elemental distribution of Ag, the animals were fed on food dosed with nanoparticles for 14 days under controlled laboratory conditions. At the end of the feeding exposure, the animals were dissected and digestive glands prepared for micro-PIXE analyses and TEM investigation. The results obtained by micro-PIXE documented high amounts of Ag inside S-cells of the digestive gland epithelium; however, TEM investigation did not show particle aggregates inside digestive gland cells. Also no adverse effect on feeding behavior was recorded what is a measure of toxic effects. We explain the presence of Ag inside the cells as a result of the assimilation of dissoluted Ag ions from ingested nano-Ag particles. Assimilation of excessive amounts of ingested metal ions in S-cells is a well known metal detoxification mechanism in isopods. We discuss the advantages of using micro-PIXE for the micro-localization of elements in biological tissue in studies of interactions between nanoparticles and biological systems.     

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.     

Three-dimensional measurement of elemental distribution in minute samples by combination of in-air micro-PIXE and STIM

A technique of measuring three-dimensional (3D) distribution of trace elements in a minute sample was studied using the in-air micro-PIXE (Particle Induced X-ray Emission) system. A 3D distribution was acquired by means of reconstructing numbers of projection images of the sample obtained by micro-PIXE analyses from different directions. This is basically the same technique as X-ray CT (Computed Tomography). However, when this technique was applied to the in-air micro-PIXE analysis, the X-ray yields should be corrected in taking account of such parameters as the X-ray production cross section, the X-ray attenuation coefficient, the energy of an incident particle, and the 3D densities of major elements in the analysis sample. In this study, STIM (Scanning Transmission Ion Microscopy)-CT was used to obtain the 3D density map of the sample. Corrected 3D distributions of sulfur and iron in a minute test sample were successfully measured with this technique in combination of STIM-CT and in-air micro-PIXE.     

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.     

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.     

The use of the maximum entropy method for the improvement of the spatial resolution of the micro-PIXE maps

The deconvolution procedure based on the maximum-entropy method is applied to improve both resolution and noise characteristics of micro-PIXE maps. The procedure is simple to execute, fast, easily automated and assumes no a priori information. The best improvement is observed for data with low statistics. Special emphasis is given to the difficulties and limitations of processing micro-PIXE data. Examples of applications for biomedical samples are presented.     

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。