气溶胶单粒子成分和粒径的实时测量

利用气溶胶飞行时间激光质谱仪测定了两种芳香烃气溶胶的质谱,发现芳香族化合物产生的气溶胶粒子容易形成分子离子峰,对苯二酚还发生分子离子反应.对室内外空气中的气溶胶粒子的粒径进行实时检测的结果表明,室内外空气中的气溶胶粒子多以细粒子为主.实验结果表明,该仪器在大气气溶胶污染监测及相关研究领域具有重要的实用价值.     

基于模糊聚类的彩色图像分割算法

提出了基于HSV空间的模糊聚类彩色图像分割算法。运用模糊C方法（FCM fuzzy clustering measure模糊聚类方法）对颜色量化后的图像进行聚类,结合了彩色图像的色彩和空间信息的特点,并且对聚类结果进行了合并优化,去除了聚类过于细小的部分。     

气溶胶飞行时间质谱仪分析间-二甲苯光氧化颗粒相产物

在自制的烟雾腔内,用紫外光照射间-二甲苯、亚硝酸甲酯、一氧化氮和清洁空气的混合物,可以启动间-二甲苯和羟基自由基(OH)的光氧化反应和一系列的后续反应,产生非挥发性和半挥发性有机化合物.半挥发性有机化合物可以在气态和粒子态之间进行分配,产生二次有机气溶胶粒子.采用实时测量气溶胶粒子粒径大小和化学成分的气溶胶飞行时间质谱仪快速、实时地测量了这些粒子的尺度、它们的分子成分和粒径分布.通过化学分析,得到酚、醛、酮和羧酸等重要的间-二甲苯光氧化产物,为讨论间-二甲苯光氧化反应机理提供了新的信息.     

基于快速高斯核函数模糊聚类算法的图像分割

对模糊聚类算法通过引入高斯核函数,平滑图像像素灰度值,从而增强图像分割的抗干扰能力和鲁棒性,并结合阈值模糊聚类算法,提高了图像分割的速度。首先利用阈值模糊聚类法划分初始输入空间,得到模糊规则数及初始聚类中心;然后用高斯核函数平滑图像的像素灰度值;最后用标准模糊聚类算法求解并优化模糊隶属度和聚类中心。将本算法应用于添加噪声的嫦娥一号采集的月球地面灰度图像和Lena灰度图像进行图像分割,仿真结果验证了本方法的鲁棒性、有效性和实用性。     

基于聚类算法的模糊神经网络MCP预测方法研究

本文提出采用聚类算法的模糊神经网络来预测MCP。该预测模型结构简单,是数据驱动的模型,通过对输入输出数据对的模糊C均值聚类确定模糊规则的数目,解决了全连接模糊神经网络模糊规则数目难以确定以及网络复杂所带来的训练时间长的问题。     

基于自适应布谷鸟搜索的模糊聚类算法

由于布谷鸟算法的步长控制因子和发现概率在算法运行过程中保持固定,影响算法的整体寻优效率和寻优精度,为此提出一种自适应设置步长控制因子和发现概率的布谷鸟搜索算法,并利用它优化模糊聚类随机选取初始聚类中心影响聚类效果的缺陷。首先根据搜索阶段的不同自动调节两个参数,使全局和局部的搜索能力达到最平衡的状态,提高整体的搜索效率;然后用改进的布谷鸟搜索算法优化模糊聚类算法,使得算法达到更好的聚类效果。在对比实验中验证了改进后的自适应布谷鸟搜索算法在寻优速度和精度上效果更优。通过比较4种算法在UCI数据集上的聚类效果,验证了改进后的算法在聚类准确率和稳定性上都有所提升。     

基于改进的模糊C-均值聚类算法的接线箱分配设计与应用

为了解决工程设计中接线箱分配最优化的问题,通过分析和比较各种聚类方法,对模糊C-均值聚类算法进行改进和参数设置,通过初始化、迭代、解模糊及分裂等步骤,实现了接线箱的自动分配功能。并设计了一种基于改进的模糊C-均值聚类算法的接线箱分配辅助软件,可以根据不同要求自动分配接线箱的功能,给出了软件流程,分析了实验结果,并在某设计院项目接线箱的实际布置中成功应用。     

基于引力的网格聚类算法

数据挖掘中的聚类在各行各业都有广泛应用,本文提出了基于网格的万有引力聚类算法(GGBCA),通过网格聚类(GBCA)的思想生成一系列的高密度网格,然后对高密度网格进行万有引力聚类,该算法考虑了类的大小对聚类结果的影响,提高了聚类效果。     

基于加权模糊聚类方法的多模型建模

针对化工过程软测量模型的多样性,提出基于一种加权模糊聚类方法的多模型建模方法。将输入向量与输出的相关性作为加权系数,构建加权模糊聚类算法,对样本空间的输入数据进行聚类,然后用与输入变量对应的子模型进行输出估计,子模型输出作为系统模型的最终输出。该方法能够实现对输入数据更加合理的划分,提高软测量模型的精度。将该方法应用于双酚A生产过程的质量指标软测量建模,仿真结果表明了该方法的可行性和有效性。     

On-Line Chemical Analysis of Individual Alkali-Containing Aerosol Particles by Surface Ionization Combined with Time-of-Flight Mass Spectrometry

An aerosol mass spectrometer for measurements of the alkali metal content in individual submicron aerosol particles is presented. The instrument combines surface ionization of individual particles on a hot platinum surface with orthogonal acceleration time-of-flight mass spectrometry. The instrument simultaneously provides the content of different alkali metal elements in single particles with high sensitivity. The instrument is characterized in laboratory experiments, and determination of the alkali metal content is demonstrated for particle diameters of 50–500 nm. The technique is demonstrated in ambient air measurements at an urban background site, and sea spray particles and particles originating from biomass burning are identified based on their content of sodium and potassium. Possible further improvements and applications of the technique are discussed.     

The Elucidation of Charge-Transfer-Induced Matrix Effects in Environmental Aerosols Via Real-Time Aerosol Mass Spectral Analysis of Individual Airborne Particles

Matrix effects in real-time aerosol mass spectrometry (RTAMS) were investigated using Standard Reference Materials (SRMs) obtained from the National Institute of Standards and Technology (NIST). Suppression of major component ions by much less concentrated species was observed. Attempts were made to mimic the ion suppression using binary systems but were unsuccessful. Data are presented that suggest the origin of the matrix effect is charge transfer induced neutralization in the ablation plume.     

Characterization of Organic Particles from Incense Burning Using an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer

Incense burning is a common ritual in Asian communities both indoors in residential homes and outdoors in temple premises. Organic particles from burning of incense sticks, incense coils, and mosquito coils after extensive dilution (>1000×) were characterized by the Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The obtained mass spectra in general resemble those reported for biomass burning aerosols. Ion peaks with m/z values higher than 100 accounted for 15%–25% of the organic signals in the unit-mass-resolution (UMR) mass spectra. In the high-resolution (HR) mass spectra, the ion peaks at m/z 60 and 73 are found to be related to the sugar anhydrides as in particles from other biomass burning processes. In addition, the ion peaks at m/z 107, 121, 137, 151, 167, and 181, some of which (e.g., m/z 137 and 167) have been observed in particles from biomass burning but not yet assigned, were assigned to lignin-related components. Elemental analysis from the HR data reveals that a large portion of particulate organics from incense burning are oxygenated (O/C between 0.3 and 0.5) and unsaturated (and/or cyclic) in nature. Results from this study also highlight that mass spectra from HR-ToF-AMS measurements concerning primary emissions such as incense burning contain very useful information in the high m/z (>100) region about the chemical characteristics of those primary organic particles.

Copyright 2012 American Association for Aerosol Research     

Source Apportionment of Individual Carbonaceous Particles Using 14C and Laser Microprobe Mass Spectrometry

An exploratory study of laser microprobe mass spectra of individual atmospheric soot particles has been made in search of a potential combustion source tracer index. A tentative “cluster ratio index” (CRI = C₄ ^?/C₂ ^?) has been found and compared with bulk measurements of ¹⁴C in a set of ambient samples exhibiting varying impacts from woodburning and motor vehicle exhaust. A CRI-¹⁴C calibration curve resulted, and it led to the conclusion that, at the present level of precision, three particles (or agglomerates) of micrometer size or about 3 pg of carbon would be required for discrimination between the two pure sources. Mixture samples, such as those reported here, would require about 40 times as much. Classification of small set of individual particles from the mixed source ambient samples, suggests preservation of carbonaceous source identity at the single particle level.     

Development of an Aerosol Mass Spectrometer for Size and Composition Analysis of Submicron Particles

The importance of atmospheric aerosols in regulating the Earth's climate and their potential detrimental impact on air quality and human health has stimulated the need for instrumentation which can provide real-time analysis of size resolved aerosol, mass, and chemical composition. We describe here an aerosol mass spectrometer (AMS) which has been developed in response to these aerosol sampling needs and present results which demonstrate quantitative mea surement capability for a laboratory-generated pure component NH₄ NO₃ aerosol. The instrument combines standard vacuum and mass spectrometric technologies with recently developed aerosol sampling techniques. A unique aerodynamic aerosol inlet (developed at the University of Minnesota) focuses particles into a narrow beam and efficiently transports them into vacuum where aerodynamic particle size is determined via a particle time-of-flight (TOF) measurement. Time-resolved particle mass detection is performed mass spectrometrically following particle flash vaporization on a resistively heated surface. Calibration data are presented for aerodynamic particle velocity and particle collection efficiency measurements. The capability to measure aerosol size and mass distributions is compared to simultaneous measurements using a differential mobility analyzer (DMA) and condensation particle counter (CPC). Quantitative size classification is demonstrated for pure component NH₄ NO₃ aerosols having mass concentrations 0.25_mu g m -3. Results of fluid dynamics calculations illustrating the performance of the aerodynamic lens are also presented and compared to the measured performance. The utility of this AMS as both a laboratory and field portable instrument is discussed.     

Effect of Vaporizer Temperature on Ambient Non-Refractory Submicron Aerosol Composition and Mass Spectra Measured by the Aerosol Mass Spectrometer

Aerodyne Aerosol Mass Spectrometers (AMS) are routinely operated with a constant vaporizer temperature (T_vap) of 600°C in order to facilitate quantitative detection of non-refractory submicron (NR-PM₁) species. By analogy with other thermal desorption instruments, systematically varying T_vap may provide additional information regarding NR-PM₁ chemical composition and relative volatility, and was explored during two ambient studies. The performance of the AMS generally and the functional integrity of the vaporizer were not negatively impacted during vaporizer temperature cycling (VTC) periods. NR-PM₁ species signals change substantially as T_vap decreases with that change being consistent with previous relative volatility measurements: large decreases in lower volatility components (e.g., sulfate, organic aerosol [OA]) with little, if any, decrease in higher volatility components (e.g., nitrate, ammonium) as T_vap decreases. At T_vap < 600°C, slower evaporation was observed as a shift in particle time-of-flight distributions and an increase in “particle beam blocked” (background) concentrations. Some chemically reduced (i.e., C_xH_y⁺) OA ions at higher m/z are enhanced at lower T_vap, indicating that this method may improve the analysis of some chemically reduced OA systems. The OA spectra changes dramatically with T_vap; however, the observed trends cannot easily be interpreted to derive volatility information. Reducing T_vap increases the relative O:C and CO₂⁺, contrary to what is expected from measured volatility. This is interpreted as continuing decomposition of low volatility species that decreases more slowly (as T_vap decreases) than does the evaporation of reduced species. The reactive vaporizer surface and the inability to reach T_vap much below 200°C of the standard AMS limit the ability of this method to study the volatility of oxidized OA species.

Copyright 2015 American Association for Aerosol Research     

Unipolar Charging of Nanosized Aerosol Particles Using Soft X-ray Photoionization

A unipolar charging device based on a soft X-ray (<9.5 keV) photoionization was developed to investigate the charging efficiency of aerosol nanoparticles. Unipolar charging using a 241 Am charger was also evaluated as a comparison with the characteristics obtained by X-ray charging. The production rate and the concentration of ions generated by the X-ray and 241 Am unipolar chargers were estimated from ion current measurements. Theoretical calculations by the unipolar diffusion charging theory were also carried out and the calculated data were compared with the experimental results. For acquiring a high number of standard nanoparticles, the classification of monodisperse nanoparticles from polydisperse aerosol particles using the X-ray unipolar charger and a differential mobility analyzer (DMA) was also evaluated. The ion production rate of the X-ray unipolar charger was at least 5.5 times higher than that of the 241 Am unipolar charger and the ion concentration was about three times higher. Therefore, the X-ray unipolar charger showed a higher capability for charging aerosol particles of 10-40 nm size in diameter than the 241 Am charger. The charging state of particles produced by the X-ray unipolar charger was in good agreement with theoretical calculations. The X-ray unipolar charger developed herein has potential for use in charging a high number concentration of nanoparticles for use in nanotechnology investigations.     

Detection and Analysis of Aerosol Particles by Laser-Induced Breakdown Spectroscopy

Laser-induced breakdown spectroscopy (LIBS) was evaluated as a means for quantitative analysis of the size, mass, and composition of individual micron-to submicron-sized aerosol particles over a range of well-characterized experimental conditions. Conditional data analysis was used to identify LIBS spectra that correspond to discrete aerosol particles under low aerosol particle loadings. The size distributions of monodisperse particle source flows were measured using the LIBS technique for calcium- and magnesium-based aerosols. The resulting size distributions were in good agreement with independently measured size distribution data. A lower size detection limit of 175 nm was determined for the calcium- and magnesium-based particles, which corresponds to a detectable mass of approximately 3 femtograms. In addition, the accuracy of the LIBS technique for the interference-free analysis of different particle types was verified using a binary aerosol system of calcium-based and chromium particles.     

Bipolar Charging of Ultrafine Aerosol Particles

The stationary bipolar charging characteristics of aerosol particles in the size range between 4.5 and 40 nm have been studied using a new technique whereby the particles neutralized by a ²⁴¹Am radioactive source are enlarged and directly observed in an electric field. The number ratio of charged particles to total particles obtained in this study was found to deviate from the charge distribution obtained from Boltzmann's law and to agree well with that calculated with the bipolar charging theory of Fuchs using his values for the ion properties. The ratio of positively charged to negatively charged particles was found to be approximately 0.35:0.65.