脉动相对湿度方法观测由体相及界面控制的气溶胶传质过程

设计搭建了可以控制样品室内相对湿度发生脉动式变化的压力控制装置。将这种装置与真空红外快速扫描技术联用,采集的时间分辨傅里叶变换红外光谱可以提供在亚秒时间尺度内,脉动相对湿度的准确数值以及湿度变化过程中气溶胶颗粒的含水量。分析这些数据可以了解相对湿度脉动变化过程中气溶胶的动态吸湿特性。选择硝酸钠,硫酸镁和硝酸镁三种无机盐气溶胶为研究对象,比较了他们在相对湿度发生脉动变化和准稳态变化条件下的吸湿特性。结果发现,实验0.12 s的时间分辨率下不足以观察到水在硝酸钠气溶胶和环境之间的传质受阻过程。而对于老化的硫酸镁气溶胶颗粒,胶态的形成减缓了水的扩散速率,体相传质成为速控步骤。对于老化的硝酸镁气溶胶颗粒,由于在颗粒表面难溶物的生成和富集,使得界面水的传质速率成为气溶胶与环境发生传质的决定性因素。这证明脉动压力变化装置与快速扫描真空红外联用可以有效便捷地观测区分体相和界面控制的气溶胶传质过程。     

Synchrotron radiation X-ray fluorescence used to studying the migration of chemical elements in biogeochemical food chains

Synchrotron radiation X-ray fluorescence makes it possible to determine the multielemental composition of atmospheric aerosols and other components of biogeochemical chains. From these data, a close interrelation between the concentration of elements in atmospheric aerosols and tissues (liver, bone tissues) of small mammals of the Central Urals and in tissues (hair, bone tissues) of wild animals of Gornyi Altai has been revealed by correlation analysis. A similar interrelation has been established for the elemental composition of atmospheric aerosols and food, the elemental composition of atmospheric aerosols, and other components of biogeocenosis (plants, mushrooms and soil). It is assumed that atmospheric aerosols play an important role in the global cycling of chemical elements.     

从MODIS数据反演粗细粒子气溶胶

陆地气溶胶一般由粗粒子和细粒子气溶胶组成,二者的光学特性并不相似,如何利用卫星观测数据获取粗粒子和细粒子气溶胶是反演中所面临的重要问题.基于AERONET/PHOTONS北京站地面观测数据,本文分析得到了北京地区的气溶胶模式(包括气溶胶复折射指数和谱分布函数),结果表明北京地区的气溶胶呈明显的粗细粒子混合的双峰分布,粗...     

Scattering and propagation of UV pulses in soot aerosols

Scattering and propagation of a UV pulse in soot aerosols are studied using generalized multi-sphere Mie theory (GMM) and a two-frequency mutual coherence function. Soot aerosols are obtained by the diffusion-limited aggregation (DLA) model. Scattering characteristics of aggregate structures in soot aerosols are analyzed by GMM theory in detail. Scattering intensities versus scattering angles are given and discussed. The effects of different-positions of the aggregate on the scattering intensities, scattering cross section, extinction cross section, absorption cross section and asymmetry factor are computed and compared. The two-frequency mutual coherence functions of UV pulses in soot aerosols are simulated, and the effects of optical distance, frequency difference are analyzed.     

Morphology of single-wall carbon nanotube aggregates generated by electrospray of aqueous suspensions

Airborne single-wall carbon nanotubes (SWCNTs) have a high tendency to agglomerate due to strong interparticle attractive forces. The SWCNT agglomerates generally have complex morphologies with an intricate network of bundles of nanotubes and nanoropes, which limits their usefulness in many applications. It is thus desirable to produce SWCNT aerosol particles that have well-defined, unagglomerated fibrous morphologies. We present a method to generate unagglomerated, fibrous particles of SWCNT aerosols using capillary electrospray of aqueous suspensions. The effects of the operating parameters of capillary electrospray such as strength of buffer solution, capillary diameter, flow rate, and colloidal particle concentration on the size distributions of SWCNT aerosols were investigated. Results showed that electrospray from a suspension of higher nanotube concentration produced a bimodal distribution of SWCNT aerosols. Monodisperse SWCNT aerosols below 100 nm were mostly non-agglomerated single fibers, while polydisperse aerosols larger than 100 nm had two distinct morphologies: a ribbon shape and the long, straight fiber. Possible mechanisms are suggested to explain the formation of the different shapes, which could be used to produce SWCNT aerosols with different morphologies.     

Absorption of ultrasonics in aerosols

A two crystal transmission and receiving system is used to investigate the ultrasonic absorption of various aerosols. Absorption coefficients of the medium between the crystals are obtained by substituting electrical attenuation for acoustic attenuation. A photoextinction-sedimentation technique for measuring size of particles suspending in liquids is used to determine the size distribution curves of the aerosols. The investigation included magnesium oxide and stearic acid aerosols and lycoperdon spores.     

黑碳团簇气溶胶混合生长的红外吸收特性及长波辐射效应

黑碳气溶胶是当前气溶胶辐射强迫评估中最不确定的因子.本文通过构建黑碳的微物理模型,分别模拟了新鲜状态的黑碳气溶胶和混合生长(老化)后被硫酸盐包裹的黑碳气溶胶,利用叠加T矩阵方法计算获得了具有团簇形态和多成分混合的黑碳气溶胶红外吸收特性,通过大气辐射传输模型模拟了黑碳气溶胶的长波辐射强迫,分析了典型理化参数的敏感性.发现黑碳混合生长可以显著增强其大气层顶的长波辐射强迫,最高可达3倍.而且,包裹黑碳的硫酸盐半径越大,将明显增强大气层顶的黑碳长波辐射强迫.这些发现将有助于降低黑碳气溶胶气候效应评估的不确定性.     

Determination of Fluorescence Cross‐Sections of Biological Aerosols

Biological aerosols like pollen or bacteria can be differentiated from non‐biological aerosols as dust by fluorescence. Several organic substances contained in biological particles emit fluorescence light if they are illuminated with ultraviolet light. An instrument has been developed which generates aerosols of individual bacteria, illuminates them with light in the range of wavelengths from 220 to 570 nm and detects the spectra of fluorescence. The instrument has been tested on different species of bacteria showing that their fluorescence spectra are different.     

Atomic Absorption Spectrometry of Fire-Extinguishing Aerosols

The process of extinguishing a propane-air flame by aerosols of salt solutions has been investigated with the use of an atomic absorption spectrometer. The method of comparing aerosols in terms of the extinguishing efficiency has been evaluated. The changes in the flame temperature and spectra at different jet heights under the influence of aerosols of water and K₂CO₃ and Al(NO₃)₃ solutions have been shown.     

近红外波段气溶胶的衰减特性研究

在已知大气气溶胶折射率和气溶胶谱分布的基础上, 对近红外波段的气溶胶衰减特性进行了研究。利用Mie散射理论计算并讨论了气溶胶的消光、散射、吸收效率因子随尺度参数的变化和消光系数随半径和波长的变化, 并且在MATLAB中对各种变化情况进行了仿真。结果表明, 三种气溶胶粒子的消光和散射能力依次为沙尘性粒子, 水溶性粒子, 烟煤。消光系数在粒子半径和入射波长相近时达到最大, 并且粒子半径对消光、散射、吸收系数的影响比入射波长更明显。这些结论可以为红外辐射在大气中的衰减计算和分析提供依据。     

Can aerosols be trapped in open flows?

The fate of aerosols in open flows is relevant in a variety of physical contexts. Previous results are consistent with the assumption that such finite-size particles always escape in open chaotic advection. Here we show that a different behavior is possible. We analyze the dynamics of aerosols both in the absence and presence of gravitational effects, and both when the dynamics of the fluid particles is hyperbolic and nonhyperbolic. Permanent trapping of aerosols much heavier than the advecting fluid is shown to occur in all these cases. This phenomenon is determined by the occurrence of multiple vortices in the flow and is predicted to happen for realistic particle-fluid density ratios.     

利用HITRAN资料研究黑碳和沙尘气溶胶粒子的光学特性

在IDL程序语言中实现Mie理论的数值算法,利用HITRAN资料提供的气溶胶粒子复折射指数,计算分析了沙尘、黑炭2种气溶胶粒子在不同半径（1μm,2.5μm和10μm）时,对波长为400nm和860nm光的散射效率以及散射相函数矩阵元素。结果表明：黑炭与沙尘有明显的光学性质差别,沙尘粒子不仅散射效率大于黑碳,而且后向散射比黑碳粒子强。 2种粒子对400 nm和860 nm太阳光的偏振也不同,可以利用此特性鉴别这2种气溶胶。     

A 2D fixed-sectional approach to model the coagulation of (highly) charged aerosols

Many simulations of charged aerosols are limited to moderately charged aerosols. In order to simulate highly charged aerosols, a 2D extension of the fixed-sectional approach, capable of dealing with negative values, is derived which is more efficient than standard 2D sectional models. Assuming that the charge and the volume of the aerosol particles are independent of each other, this model preserves the 0th and 1st moment in both dimensions. The relaxed grid requirements allow to include higher charges in the simulation without increasing the computational effort or reducing accuracy of the obtained results.     

气体和气溶胶在多孔介质中迁移的数值模拟

为了研究多孔介质对气体和气溶胶的封闭能力,用数值方法模拟了气体和气溶胶在多孔介质中的迁移.考虑了渗透、吸附过滤、扩散、热传导等因素,在柱对称坐标下用双孔双渗模型进行了数值模拟,并与实验结果进行了比较.计算结果显示,多孔介质对气溶胶有较强的阻挡作用,模拟实验结果也证明了这一点.     

Vacuum Ultraviolet Photoionization Mass Spectra of Typical Organics Contained in Ambient Aerosols

This paper reports an investigation on typical organics contained in ambient aerosols with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer (VUV-ATOFMS). The VUV-ATOFMS utilizes a vacuum ultraviolet krypton lamp as an ionization source. The single- and multi-constituent particles generated with typical atmospheric organics (n-eicosane, n-triacontane, 1-pentadecanol, 1-eicosanol, hexanoic acid, decanoic acid, heptadecanoic acid, oleic acid, succinic acid, pyrene, vanillin, benzoic acid, terephthalic acid, and D-galactose) are analyzed with VUV-ATOFMS. The time-of-flight mass spectra of all organic particles are obtained except hexanoic acid. The mass spectra reveal that the detection efficiencies for a certain compound contained in multi-constituent and single-constituent particles are different. These discrepancies may result from the different evaporation dynamics of aerosols in both atomization and vaporization processes. The pyrene has the strongest signal intensity in single- or multi-constituent aerosols, indicating that the VUV-ATOFMS performs well in detecting polycyclic aromatic hydrocarbons. These experimental results present a view on the VUV-photoionization mass spectra of the 14 typical organics contained in ambient aerosols.     

Optical characterization of metallic aerosols

Airborne metallic particulates from industry and urban sources are highly conducting aerosols. The characterization of these pollutant particles is important for environment monitoring and protection. Because these metallic particulates are highly reflective, their effect on local weather or regional radiation budget may also need to be studied. In this work, light scattering characteristics of these metallic aerosols are studied using exact solutions on perfectly conducting spherical and cylindrical particles. It is found that for perfectly conducting spheres and cylinders, when scattering angle is larger than 90° the linear polarization degree of the scattered light is very close to zero. This light scattering characteristics of perfectly conducting particles is significantly different from that of other aerosols. When these perfectly conducting particles are immersed in an absorbing medium, this light scattering characteristics does not show significant change. Therefore, measuring the linear polarization of scattered lights at backward scattering angles can detect and distinguish metallic particulates from other aerosols. This result provides a great potential of metallic aerosol detection and monitoring for environmental protection.     

利用不同的湿度调节方法研究醋酸镁气溶胶中水的传质过程

利用一种自制的湿度调节设备与真空红外光谱仪相结合, 提出了一种研究醋酸镁气溶胶的吸湿性和传质动力学的新方法。湿度调节装置通过改变纯水汽压力来调节样品室的相对湿度,这样可以实现湿度以不同的速度发生变化。与红外光谱手段相结合,湿度缓慢变化,让气溶胶时刻处于准稳态过程,可以研究气溶胶在热力学稳态的吸湿性质。湿度脉冲式改变,可以研究气溶胶的动态吸湿性质以及传质动力学过程。红外光谱的扫描方式随着湿度的改变速度进行调节。由于实验中的相对湿度由纯水气提供,因此通过对红外方光谱中纯水气的特征吸收峰面积的定量计算获得与光谱同步的相对湿度值。研究发现,当湿度稳定在一个高湿度时,醋酸根和液态水的峰面积在持续下降。并且首次发现经过一个准稳态的湿度循环后(1.05×104 s),在80%RH条件下,水峰面积由1.5降低至1.1。通过改变实验方案并对其结果进行对比可知,在高湿度条件下,醋酸镁发生水解,生成的醋酸由于样品室内的负压而挥发,因此引起气溶胶含水量下降。采用脉冲发式快速改变样品室的湿度,一个湿度脉冲循环需要10 s。计算脉冲循环过程中气溶胶的含水量发现,在湿度高于70%RH时,气溶胶含水量没有减少。但是加湿过程的水传输比去湿过程的水传输快。这些现象说明醋酸镁的水解速率小于湿度的脉冲改变速率。在湿度快速变化的过程中,气溶胶液滴表面难溶物的形成引起水传输发生受阻现象。     

气溶胶生长过程的微观动力学研究

气溶胶作为大气颗粒物的重要成分对大气环境以及人体健康均有重要影响.其中气溶胶的吸湿性作为影响其在大气中存活时间以及物理化学性质的重要因素受到广泛关注.目前对于气溶胶颗粒的吸湿性研究较为简单,对于气溶胶颗粒物微观结构对吸湿性的影响较少.本文根据Langmuir吸附模型、Fick扩散定律建立了单颗粒的气-粒作用模型,分析了气溶胶颗粒物的均匀分布结构(H2O/C2H2O4)以及非均匀分布结构(H2O/C2H2O4/H2SO4)对其吸湿性的不同影响。研究结果发现,气溶胶颗粒物的非均匀分布结构会影响其吸湿过程的快慢;对于理想流体构成的气溶胶分子,由于分子之间不存在分子间相互作用,因此气-粒间的水分子交换更快,颗粒物外侧浓度首先升高,接着在浓度差的作用下,内侧颗粒逐渐向外扩散,直至达到平衡;相较与大尺寸的颗粒,在相同体积比的条件下,小颗粒由于气溶胶颗粒物的接触角大,因此表面张力大,水分更难流失;此外,由于大尺寸的气溶胶颗粒物表面积体积比较小,因此颗粒失水速度低,需要更多的时间达到相平衡。     

适用于测量大气气溶胶吸收系数的光声光谱系统的研究

外部噪声和环境温湿度变化对光声池性能的影响是光声光谱技术在实际大气气溶胶吸收测量应用中遇到的主要问题。详细分析了环境温湿度变化引起的共振频率漂移对光声信号的影响,提出了抑制流动噪声和采样泵振动噪声的方法,研制完成了一套测量大气气溶胶吸收的光声光谱系统,探测极限为1.4×10-8 W·cm-1·Hz-1/2。利用NO₂气体在532 nm的吸收对光声池进行了标定,并对实际大气气溶胶的吸收特性进行了测量,结果表明光声光谱测量系统可以满足自然悬浮状态下的气溶胶吸收系数的实时测量。     

Quantitative IBBCEAS measurements of I2 in the presence of aerosols

An instrument implementing Incoherent BroadBand Cavity-Enhanced Absorption Spectroscopy (IBBCEAS) for quantitative measurements of molecular iodine (I₂) at ambient pressure and in the presence of aerosols is presented. The instrument is based on a LED emitting in the green spectral region around 500–550 nm, exciting a multitude of rovibronic transitions in the I₂ B ← X electronic absorption spectrum. I₂ was generated using a permeation device and was mixed with a dilution flow of Ar and another flow containing NaCl aerosols. Retrieval of the mirror reflectivity, necessary for quantitative IBBCEAS measurements, was not pursued in this study. Instead, calibrated I₂ flows were used, and a differential optical absorption spectroscopy type of algorithm was implemented for the data analysis. This approach has several benefits, in particular when light extinction due to aerosols is substantial. Estimated detection limits are roughly 0.04 nmol/l without aerosols and 0.4 nmol/l in the presence of aerosols (10¹⁰ particles/l with 60–70 nm mean diameter, leading to I ₀/I _aerosols ≈ 5.4). A drop in measured I₂ concentration in relation to the expected mixing ratio was observed when using the highest aerosol concentration, likely due to adsorption of I₂ onto aerosols.