PHYSICAL ANALOGS AND PERFORMANCE OF A BOX MODEL FOR COMPOSITION AND GROWTH OF H2SO4/H2O AND HNO3/H2SO4/H2O AEROSOL IN THE STRATOSPHERE

A physical box model simulating the aerosol particle evolution along air mass trajectories is developed to provide a tool for interpreting the local observations of stratospheric aerosols (i.e., polar stratospheric clouds). The model calculates the composition and the size distributions of H₂SO₄/H₂O and HNO₃/H₂SO₄/H₂O liquid droplets. The parameterization of the physical processes affecting the dynamics of HNO₃ and H₂SO₄ solid hydrates and ice particle size distributions is also included, but not used. This work is restricted to some speculations about the liquid to solid transition, according to existing theories. The evolution of liquid particles is simulated taking into account nucleation, diffusive condensation/evaporation and coagulation. This paper reports the physical and numerical details of the model, which are discussed within the framework of the current understanding of the stratospheric aerosol physics. Performance and limitations of the model are discussed on the basis of the evolution of particle size, and composition along synthetic air mass thermal histories. Size distributions and size-dependent acid weight fractions of the liquid stratospheric aerosols consisting of HNO₃/H₂SO₄/H₂O are calculated in the cases of air mass thermal histories with different cooling rates and with rapid temperature fluctuations.     

Calibration Correction of an Active Scattering Spectrometer Probe to Account for Refractive Index of Stratospheric Aerosols: Comparison of Results with Inertial Impaction

Real-time particle size spectra are being acquired on our research aircraft with relative ease and speed by techniques that make use of the real-time interaction of laser light with aerosols and cloud droplets. The results are, however, sometimes ambiguous, because the optical “signatures” of the particles depend on their refractive indices in addition to physical dimensions. The calibration supplied by the manufacturer is based on instrument response to a specific test aerosol, e.g., latex spheres (refractive index = 1.59). Such a calibration is strictly valid only for sample aerosols of refractive index and shape similar to the test aerosol. Whenever the sample aerosol differs from the test aerosol, a calibration correction is in order. Of concern here is the use of an active scattering spectrometer probe (ASAS-X), to measure sulfuric acid aerosols on high-flying U-2 and ER-2 research aircraft. Correcting the calibration of the ASAS-X for dilute sulfuric acid droplets (refractive index = 1.44) that predominate the stratospheric aerosol changes the inferred sizes by up to 32% per size interval from that determined from the nominal calibration. This results in an average increase in particle surface area and volume of 42 ± 10% and 71 ± 19%, respectively. The calibration correction of the optical spectrometer probe for stratospheric aerosol is validated by independent and simultaneous sampling of the particles with impactors. Sizing and counting of particles on microphotographs of scanning electron microscope images give results on total particle surface areas and volumes. After the calibration correction, the optical spectrometer data (averaged over four size distributions) agree with the impactor results (similarly averaged) to within a few percent. We conclude that the optical properties, or chemical makeup, of the sample aerosol must be known for accurate size analysis by optical aerosol spectrometers.     

Heterogeneous Reactions of Chlorine Nitrate and Dinitrogen Pentoxide on Sulfuric Acid Surfaces Representative of Global Stratospheric Aerosol Particles

Increasing evidence from field measurements, modeling studies, and laboratory experiments suggests that heterogeneous reactions on stratospheric sulfate aerosol particles can change the partitioning in the nitrogen and chlorine families and thereby affect global ozone levels. In this study, a Knudsen cell flow reactor was used to measure the uptake of ClONO₂ and N₂O₅ by sulfuric acid solutions representative of background and volcanic stratospheric aerosol particles. The uptake coefficient (γ) of chlorine nitrate on 50–75 wt% H₂SO₄ at 223 K was found to be markedly dependent on the acid concentration, with γ ranging from about 1 × 10⁻² to 1 × 10⁻⁴. These results are in good agreement with literature reports and the data fit the expression log γ= 1.87 – 0.074 × (wt% H₂SO₄). This reaction will thus have its largest impact when stratospheric temperatures are low and sulfuric acid aerosols are most dilute. Uptake of N₂O₅ was studied on solutions with compositions in the range 58–96 wt% H₂SO₄ at temperatures from 193 to 303 K. N₂O₅ reacted readily on sulfuric acid surfaces with uptake coefficients of about 0.06. The uptake coefficient was found to be independent of the sulfuric acid concentration and the solution temperature over the ranges studied. These results suggest that the reaction of N₂O₅ with H₂O will occur readily on sulfuric acid aerosol particles for most stratospheric conditions.     

Calibration of an Aerosol Composition Mass Spectrometer with Sulfuric Acid Water Aerosol

The first quantitative chemical analysis of polar stratospheric cloud particles has recently been performed using a balloon-borne aerosol composition mass spectrometer (ACMS). A similar spectrometer is presently used in a large cryo-chamber experiment to study low temperature aerosols. All experiments require prior to their employment an accurate calibration to convert mass spectrometer signals into molecular species contained in the aerosols. For the calibration, pure H 2 SO 4 /H 2 O droplets are generated having known composition and diameters between 0.4 w m and 1 w m. The size distribution and the number concentration can be controlled. A flow reactor with a rotating inner glass cylinder placed in a H 2 SO 4 /H 2 O bath solution of known concentration is used to condition the droplets. The residence time of the particles in the flow reactor is long enough that the droplets adopt the composition of the bath solution before entering the ACMS. The result is a linear relationship between the mole ratio of the H 2 SO 4 /H 2 O droplets and the mass spectrometer count rate ratio of water to sulfuric acid. The evaluation takes the dissociation of H 2 SO 4 inside the ACMS into account. The calibration error varies between 3 and 4 wt. % H 2 SO 4 for stratospheric particles with a composition of 30-70 wt. % H 2 SO 4 . Besides the calibration of the instrument, the analysis of the aerosols is a valuable diagnostic tool to investigate impurities in the particles.     

Aerosolbildung durch spontane Phasenübergänge bei Absorptions- und Kondensationsprozessen

Formation of aerosols by spontaneous condensation or desublimation in condensers or absorbers often causes serious problems in industrial processes. The fine aerosol particles, formed under special operating conditions, remain suspended in gases and are carried over into downstream stages or lead to high pollutant concentrations in the exhaust gas. The present paper describe under what conditions aerosols are formed. The characteristic behaviour of aerosols is discussed with the aid of experiments and computer simulation.     

荧光性微粒在气溶胶及微粒技术中应用的研究

以荧色物作标记微粒是微粒技术研究中的一项新方法.荧色物具有很高的分析灵敏度,用通常的荧光光度比色仪,可将其浓度测至1×10~(-10)g/ml;若采用Bergund-Liu气溶胶发生器,就可以得到已知直径及浓度的荧光性标准微粒,这对于研究微粒的空气动力学行为以及对于处理微粒状物料设备的标定是十分有效的.本文介绍了单分散气溶胶发生器,通过实验得出了使用荧光性微粒的一些重要条件,其中包括;溶剂的选择、微粒的发生与捕集、微粒中荧色物的提取及分析.文中还比较了两种常用的荧色物(荧光素钠及若丹明B)用于微粒技术的可能性,并应用这一技术对一种轴流式旋风分离器作了研究,得到了微粒在分离器各部位沉积情况的数据,它表明,该旋风分离器的分高效率和Stokes数间有一定的函数关系.     

Charge distributions and coagulation of radioactive aerosols

The self-charging of radioactive aerosols will be reduced by background ions, such as those produced by radioactive gases. The sources of these background ions and their production rates are specified for a reactor containment atmosphere during a possible nuclear accident. Previous theory is extended to calculate the charging of a polydisperse radioactive aerosol. Gaussian approximations to charge distributions on an aerosol of a given size, and are shown to give a good representation of the exact numerical charge distributions of a Cs aerosol at normal temperatures, and also for highly radioactive aerosol containing ¹³¹I in a containment atmosphere.

Extensive calculations are performed for charge-induced modifications to Brownian coagulation rates between steady-state size distributions of these radioactive aerosols, and also between small-sized radioactive aerosol and larger (non-radioactive) aerosol. The results show considerable enhancements of the coagulation rates between large and small-sized aerosol, but also a strong suppression of coagulation between large particles. Rate modifications calculated using the Gaussian approximations are generally close to the exact values. Time-dependent calculations for a monodisperse -decaying aerosol reveal enhancements in coagulation rates even when the average charge on the aerosol is positive. Our results are relevant to behaviour in a dusty plasma.     

Fungal aerosols: A review

Fungal aerosols are important in the spread of plant, animal and human diseases. The development of this area of aerobiology is reviewed in relation to its influence on, and interaction with, the growth of aerosol science. Physical characteristics of airborne fungal spores relevant to their liberation, flight and deposition are discussed. Some samplers and sampling techniques especially suited to fungal aerosols are described.     

Effects of temperature and humidity on the growth and optical properties of sulphuric acid—water droplets in the stratosphere

Theoretical calculations of the optical properties of equilibrium size sulphuric acid-water solution droplets under stratospheric conditions are presented. We evaluate the changes in the physical properties of the aerosol particles which accompany fluctuations in environmental temperature and humidity, and present them in tabular and graphical form. These results are used in conjunction with Mie scattering theory to show how the aerosol backscatter at 0.6943 μm wavelength and the aerosol extinction at 1.0 μm wavelength are affected by variations in the stratospheric temperature and humidity.     

Aerosol formation by heterogeneous nucleation in wet scrubbing processes

The phenomenon of aerosol formation is often watched in industrial wet scrubbing processes especially if strong acid gases are absorbed in aqueous solutions. Although the basic principles of aerosol formation are well known in general, there exist nearly no specific rules for the design of industrial processes in which aerosol formation can be expected. There are two reasons for the fragmentary knowledge concerning aerosol formation in wet scrubbing processes. Firstly, it is a very complex task to describe the formation and the growth of aerosols theoretically under typical conditions of industrial processes. Secondly, no reliable experimental data, especially for the validation of theoretical work, has been available to date. To bridge this gap, a semi-technical wet scrubbing plant has been developed and erected in which the formation and the growth of aerosols under realistic conditions can be studied and the characteristic aerosol parameters can be measured in situ. It is shown that HCl-aerosols are formed in a quench cooler for hot flue gases of about 200°C even at low HCl feed concentrations of about l000 mg m⁻³, but only in the presence of foreign nuclei. The aerosol droplets in the quench cooler grow up to 1–1.5 μm and can be enlarged in a direct-contact-cooling column up to about 2.5 μm. Furthermore, a strategy for aerosol evaporation is discussed.     

Maschinentechnik beim Füllen von Anstrichmitteln

Machines for Filling Coating Materials To start with, the aerosol filling technique is reviewed. The filling of colours in aerosols is treated at a greater detail. Further, the requirements which are to be set on filling machines and their constructional materials are given. Finally, the filling systems and future marketing prospects are explained.     

A new splitting wavelet method for solving the general aerosol dynamics equation

In this paper, a new and robust splitting wavelet method has been developed to solve the general aerosol dynamics equation. The considered models are the nonlinear integro-partial differential equations on time, size and space, which describe different processes of atmospheric aerosols including condensation, nucleation, coagulation, deposition, sources as well as turbulent mixing. The proposed method reduces the complex general aerosol dynamic equation to two one-dimensional splitting equations in each time interval, and further the wavelet method and the upstream finite difference method are proposed for solving the particle size directional and the spatial directional splitting equations. By the method, the aerosol size spectrum is represented by a combination of Daubechies’ wavelets and substituted into the size-directional splitting equation at each time step. The class of Daubechies’ wavelets in the wavelet-Galerkin scheme as trial and weight functions has the advantages of both compact support and orthonormality which can efficiently simulate the sharp shape distribution of aerosols along the particle size direction. Numerical experiments are given to show the efficient performance of the method.     

An Empirical Method for the Determination of the Complex Refractive Index of Size-Fractionated Atmospheric Aerosols for Radiative Transfer Calculations

To adequately assess the effects of atmospheric aerosols on climate, their optical constants (scattering and absorption coefficients) must be known. The absorption and scattering coefficients of the aerosols are derived from the real and imaginary parts of the complex refractive index and are dependent on their size and chemical composition. Because aerosol properties vary significantly with location, it is difficult to assign values for the absorption and scattering of solar radiation by aerosols in models of global climate change. This study reports a new method of collecting size-fractionated atmospheric aerosol samples for the purpose of directly measuring their transmission and reflectance spectra followed by the determination of the complex refractive index across the entire atmospherically relevant spectral range. The samples were collected with a modified Sierra high-volume cascade impactor with the usual filter collection surfaces replaced with Teflon sheets machined to hold quartz (ultraviolet [UV]/visible transparent) and/or silver chloride (infrared transparent) sample collection plates. Reflectance and transmission spectra can be obtained on the aerosol samples directly as a function of wavelength, from 280 nm to 2.5 m, with an integrating sphere coupled to an UV/visible or a Fourier transform infrared (FTIR) spectrophotometer. The effective real and imaginary components of the refractive index of the bulk sample material can then be approximated, as a function of wavelength, from the sample spectra. Preliminary results are presented for carbon soot samples generated in the laboratory and for standard diesel soot samples in the UV/visible spectral range. These are compared to results obtained for size-fractionated atmospheric aerosol samples collected near Pasco, WA, West Mesa, AZ, and Argonne, IL.     

Development of polydisperse aerosol generation and measurement procedures for wind tunnel evaluation of size-selective aerosol samplers

Accurate development and evaluation of inlets for representatively collecting ambient particulate matter typically involves the use of monodisperse particles in aerosol wind tunnels. However, the resource requirements of using monodisperse aerosols for inlet evaluation creates the need for more rapid and less-expensive techniques to enable determination of size-selective performance in aerosol wind tunnels. The goal of recent wind tunnel research at the U.S. EPA was to develop and validate the use of polydisperse aerosols, which provide more rapid, less resource-intensive test results, which still meet data quality requirements necessary for developing and evaluating ambient aerosol inlets. This goal was successfully achieved through comprehensive efforts regarding polydisperse aerosol generation, dispersion, collection, extraction, and analysis over a wide range of aerodynamic particle sizes. Using proper experimental techniques, a sampler’s complete size-selective efficiency curve can be estimated with polydisperse aerosols in a single test, as opposed to the use of monodisperse aerosols, which require conducting multiple tests using several different particle sizes. While this polydisperse aerosol technique is not proposed as a regulatory substitute for use of monodisperse aerosols, the use of polydisperse aerosols is advantageous during an inlet’s development where variables of sampling flow rate and inlet geometry are often iteratively evaluated before a final inlet design can be successfully achieved. Complete Standard Operating Procedures for the generation, collection, and analysis of polydisperse calibration aerosols are available from EPA as downloadable files. The described experimental methods will be of value to other researchers during the development of ambient sampling inlets and size-selective evaluation of the inlets in aerosol wind tunnels.

© 2018 American Association for Aerosol Research     

Aerosole und ihre technische Bedeutung

Aerosols and Their Technical Significance Aerosols occur in many technical processes. For example, aerosols are formed to generate products of highly disperse solids in gas phase processes. Particle formation and growth in the aerosol state decisively determine the product properties by the size, shape, and structure of the particles. Undesired aerosol formation can also occur in technical processes. These undesired aerosols pollut process gases or products or increase the pollutant content of exhaust gases. If undesired aerosol formation cannot be avoided, efficient separation techniques have to be used. Efficient separators are also required to recover fine product particles from the gas phase. Moreover, aerosols, whether desired or undesired, have to be measured and characterized. This requires high performing measuring techniques. The paper outlines the technical significance of aerosols.     

湿式氨法烟气脱硫中气溶胶的形成特性研究

气溶胶的形成是湿式氨法烟气脱硫过程存在的主要问题,通过测试分析氨法脱硫前后细颗粒的浓度与粒径分布、颗粒形态及其组成的变化特性,探讨了氨法脱硫中气溶胶的形成机理,并考察了影响气溶胶颗粒形成的主要因素。结果表明:氨水挥发逸出的气态NH3与烟气中SO2发生气相反应是气溶胶形成的主要原因,气溶胶含(NH4)2SO4、(NH4)2SO3、NH4HSO3等组分,粒径集中在0.07～0.70μm范围内,氨法脱硫系统对其难以有效脱除;氨水脱硫液温度及其浓度、烟气中SO2浓度、液气比等对气溶胶形成具有重要影响,形成量随氨水脱硫液及烟气中SO2浓度升高而增多,在保持NH3:SO2化学计量比不变的情况下,随液气比增大,气溶胶颗粒形成量减少。最后,对气溶胶颗粒的控制措施提出了建议。     

Ternary nucleation applied to gas to particle conversion

Atmospheric aerosol formation involving three gaseous components is considered with an emphasis on systems in which one component is water. Analytic methods discussed qualitatively are physical equilibrium phase diagram analysis and heteromolecular nucleation. The possibility of chemical reactions before or after nucleation is considered. Atmospheric applications are discussed.

Additional experimental measurements of thermodynamic parameters, such as the equilibrium vapor pressure of low volatile products and the surface tension of ternary systems are strongly recommended for further studies of ternary aerosols.     

The Use of Nonlinear Acoustics as an Energy-Efficient Technique for Aerosol Removal

This article is a feasibility study on using nonlinear acoustic effects, acoustic streaming and acoustic radiation pressure, for aerosol removal in an air duct. Unlike previous research, which used acoustics solely to cause aerosol agglomeration prior to aerosol removal in traditional duct collection systems, this article considers the acoustic streaming effect, which is significant but was previously neglected. Monodispersed polystyrene spheres with diameters ranging from 0.3 to 6 μm were tested. The proposed system removed 12–20% of the submicron aerosols and 25–32% of the micron aerosols when the airflow rate was approximately 90 L/min. Acoustic streaming introduces stagnation points on the surface of the air duct and removes the aerosols by deposition. Acoustic radiation pressure causes aerosols to form agglomerates. This enhances inertial impaction and/or gravitational sedimentation, which further enhances the removal efficiency of micron aerosols. The particle-removal efficiency is proportional to the duration that the aerosols are exposed to the acoustic field. The pressure drop due to the nonlinear acoustic effects is negligible; thus, power consumption is minimal. This system has the potential to be developed into an energy-efficient technique for aerosol removal.

Copyright 2014 American Association for Aerosol Research     

The characterization of aerosols distributed with respect to size and chemical composition

Aerosols are often distributed with respect to size and chemical composition, and these variables play an important part in determining the effects of the aerosol in air pollution and meteorology. The characteristics of such complex aerosols can be described by means of a probability density function, and an equation for the dynamics of the function can be derived. This equation provides a link between the aerosol, and gas phase chemical reaction and condensation processes.

The development of information collecting and processing systems for the atmospheric aerosol makes it desirable to develop, in parallel, methods for defining the quantity of information. The unit of information, defined in terms of certain integral functions of the probability density function, is introduced and discussed.