Experimental Evaluation of the Optical Properties of Porous Silica/Carbon Composite Particles

Light scattering by porous spheroidal silica and several silica/carbon composite particles having different carbon contents was systematically investigated using a laser particle counter coupled with a pulse height analyzer (LPC-PHA). A new and simple method for the measurements of the effective complex refractive index of silica/carbon composite particles using a conventional LPC-PHA system and a differential mobility analyzer was introduced and tested. Challenge particles, from pure silica to silica/carbon compounds having a gradually increasing porous structure, were prepared by spray-drying methods for use in testing of the inversion method. By representing the deviation of the real part of the refractive index of a porous silica particle versus the size on a topographical map, the inversion method for the determination of the real part of the refractive indices was found to have a satisfactory precision. Furthermore, the method can be applied to the measurement of the complex refractive index of silica/carbon composite particles by extending the best fitting method to complex refractive indices. The effective complex refractive index of silica/carbon composite particles as a function of their carbon content is reported. Both the real and imaginary parts of the complex refractive index were increased with increasing carbon content of the composite particles.     

Measuring the effective density, porosity, and refractive index of carbonaceous particles by tandem aerosol techniques

The physical properties of carbonaceous aerosol particles are often of interest but are difficult to determine from a single measurement. In this study, we used tandem aerosol measurement techniques to measure the effective physical properties, namely the effective density, porosity, and effective complex refractive index of spheroid aggregated and porous carbonaceous aerosol particles. An in-flight measurement system, composed of a differential mobility analyzer (DMA) followed by either an aerosol particle mass analyzer (APM) or a laser particle counter-pulse height analyzer (LPC–PHA), was constructed and used to examine shape-controlled and porosity-controlled carbonaceous particles produced by a spray-drying process. The effective density and porosity were inferred from tandem measurements in which particles were first mobility-classified by the DMA and subsequently mass classified in the APM. The effective refractive index of the particles was inferred from tandem DMA–LPC–PHA measurements in conjunction with Mie Theory. The measured effective density and porosity of the carbonaceous particles ranged from 695.0 to 1399.9 kg/cm³ and 15.2% to 64.3%, respectively. Furthermore, the real and imaginary parts of the effective complex refractive index were between 1.430 and 1.736 and between 0.035 and 0.125, respectively. Both the real and imaginary parts decreased with increasing particle porosity.     

Smoke Characterization and Feasibility of the Moment Method for Spacecraft Fire Detection

The Smoke Aerosol Measurement Experiment (SAME) has been conducted twice by the National Aeronautics and Space Administration and provided real-time aerosol data in a spacecraft micro-gravity environment. Flight experiment results have been recently analyzed with respect to comparable ground-based experiments. The ground tests included an electrical mobility analyzer as a reference instrument for measuring particle size distributions of the smoke produced from overheating five common spacecraft materials. Repeatable sample surface temperatures were obtained with the SAME ground-based hardware, and measurements were taken with the aerosol instruments returned from the International Space Station comprising two commercial smoke detectors, three aerosol instruments, which measure moments of the particle size distribution, and a thermal precipitator for collecting smoke particles for transmission electron microscopy (TEM). Moment averages from the particle number concentration (zeroth moment), the diameter concentration (first moment), and the mass concentration (third moment) allowed calculation of the count mean diameter and the diameter of average mass of smoke particles. Additional size distribution information, including geometric mean diameter and geometric standard deviations, can be calculated if the particle size distribution is assumed to be lognormal. Both unaged and aged smoke particle size distributions from ground experiments were analyzed to determine the validity of the lognormal assumption. Comparisons are made between flight experiment particle size distribution statistics generated by moment calculations and microscopy particle size distributions (using projected area equivalent diameter) from TEM grids, which have been returned to the Earth.

Copyright 2015 American Association for Aerosol Research     

Experimental investigation of pressure drop in packed beds of irregular shaped wood particles

The knowledge of the pressure drop across a packed bed of irregular shaped wood particles is of great importance for achieving optimal control and maximum efficiency in many applications, such as wood drying, pyrolysis, gasification and combustion. In this work the effect of porosity, average particle size and main particle orientation on the pressure drop in a packed bed is investigated. To this end, particle size distributions and porosities are determined experimentally.Based on the experimental results obtained in this study, the form coefficient C and the permeability K of the Forcheimer equation are calculated for different packed beds. The Ergun equation requires an average equivalent particle diameter that is derived from the measured particle size distribution. This equivalent diameter and the corresponding bed porosity are used in the well known Ergun equation in order to derive adapted shape factors A and B.Since a change in bed porosity and particle size, caused by the degradation of the wood particles and gravity, can be expected in a reacting packed bed, a set of shape factors for use with the Ergun equation is determined that are independent of porosity and particle diameter and fit the experimental data very well.     

Characterization of Particulate Matter Morphology and Volatility from a Compression-Ignition Natural-Gas Direct-Injection Engine

The particulate matter (PM) emitted from a single-cylinder compression-ignition, natural-gas engine fitted with a High-Pressure Direct-Injection (HPDI) system distinctly different from a duel fuel engine was investigated, and characterized by size distribution, morphology, mass-mobility exponent, effective density, volatility, mixing state, and primary particle size using transmission electron microscopy (TEM), and tandem measurements from differential mobility analyzers (DMA) and a centrifugal particle mass analyzer (CPMA). Six engine conditions were selected with varying load, speed, exhaust gas recirculation (EGR) fraction, and fuel delivery strategy. An increase in engine load increased both the number concentration and the geometric mean diameter of the particulate. The fraction of the number of purely volatile particles to total number of particles (number volatile fraction, NVF) was found to decrease as load increased, although at the lower speed, partially premixed mode, the lowest NVF. All size distributions were also found to be unimodal. The size-segregated ratio of the mass of internally mixed volatile material to total particle mass (mass volatile fraction, MVF) decreased with load and with particle mobility-equivalent diameter. A roughly constant amount of volatile material is likely produced at each engine mode, and the decrease in MVF is due to the increase in PM number with load. Effective density and mass-mobility exponent of the non-volatile soot at the different engine loads were the same or slightly higher than soot from traditional diesel engines. Denuded effective density trends were observed to collapse to approximately the same line, although engine modes with higher MVFs had slightly higher effective densities suggesting that the soot structures have collapsed into more dense shapes—a suspicion that is confirmed with TEM images. TEM results also indicated that primary particle size first decreases from low to medium load, then increases from medium to high load. An increase in EGR was also seen to increase primary particle size. Coefficients were determined for a relation that gives primary particle diameter as a function of projected area equivalent diameter. A decrease in load or speed results in a stronger correlation.

Copyright 2015 American Association for Aerosol Research     

Single-scattering properties of tri-axial ellipsoidal mineral dust aerosols: A database for application to radiative transfer calculations

This paper presents a user-friendly database software package of the single-scattering properties of individual dust-like aerosol particles for application to radiative transfer calculations in a spectral region from ultraviolet (UV) to far-infrared (far-IR). To expand the degree of morphological freedom of the commonly used spheroidal and spherical models, tri-axial ellipsoids were assumed to be the overall shape of dust-like aerosol particles. A combination of four computational methods, including the Lorenz–Mie theory, the T-matrix method, the discrete dipole approximation, and an improved geometric optics method, was employed to compute the phase matrix, extinction efficiency and single-scattering albedo of ellipsoids with various aspect ratios and sizes. The scattering property database was developed for 42 particle shapes specified in terms of two aspect ratios, 69 refractive indices and 471 size parameters. Additionally, accompanying software, based on interpolation, was developed to provide the single-scattering properties for user-specified aspect ratios, refractive indices and size parameters. The software package allows for the derivation of the bulk optical properties for a given distribution of particle microphysical parameters (i.e., refractive index, size parameter and two aspect ratios). The array-oriented single-scattering property data sets are stored in the NetCDF format.     

TRANSPARENTE POLYMERE MEHRPHASENSYSTEME

Usually two phase polymer blends are not transparent because of differences in the refractive indices of their components and the resulting light scattering. By means of model calculations on the basis of the Mie-theory, the conditions for transparency in two-phase polymer blends are investigated. The models used are homogeneous spheres or spheres with a core-shell morphology imbedded in the polymer matrix. The light scattering of these particles is calculated as a function of diameter, refractive index, wavelength and particlecomposition. Results are presented that show the limits of diameter and difference in the refractive indices between matrix and particle for homogeneous particles to obtain transparency. In the case of large differences in the refractive indices or of large diameters the use of spheres with a core-shell morphology is favourable. Depending on the refractive indices of the respective phases, there exists an optimal composition of these spheres to obtain transparent polymer-blends. Another way to transparency is the minimization of light scattering by interparticle interferences, which can be achieved by special types of block-copolymers.     

Measurements of Particle Loss Functions in a Differential Mobility Analyzer (TSI,Model 3071) for Different Flow Rates

Particle losses in a differential mobility analyzer (TSI, Model 3071) caused by diffusive deposition and Brownian diffusion are measured for particles in the diameter size range between 3 and 100 nm. For small sampling and aerosol flow rates (0.3 liters/min) at 20 nm, nearly 50% of the primary particles are lost; and for 2 liters/min, the particle losses have to be considered in the diameter size range below 30 nm (50% at 7 nm). From the measured penetration values, an effective tube length is derived which is useful to calculate particle losses for other flow rates through the analyzer.     

基于Lattice-Boltzmann方法的纳米颗粒多孔介质导热特性

为研究气凝胶纳米颗粒的导热特性,提出了一种基于随机统计原理的构造气凝胶多孔介质介观尺度三维物理模型的方法。模型中颗粒空间分布、粒径分布及孔隙率可以根据实际气凝胶微尺度结构数据调整。基于所构造的物理模型,采用D3Q15LBM进行了数值模拟。分析了颗粒尺寸、孔隙率等因素对气凝胶导热性能的影响规律,即在既定孔隙率下,热导率随粒径增大而减小;既定粒径下,随孔隙率的递增热导率先下降后上升;颗粒尺寸不均匀性对热导率的影响甚大。模拟与实验结果相吻合。研究工作对优化气凝胶导热性能,提高其有效热导率的预测精度具有参考价值。     

Determination of Arbitrary Moments of Aerosol Size Distributions from Measurements with a Differential Mobility Analyzer

A method to determine arbitrary moments of aerosol size distributions from differential mobility analyzer measurements has been proposed. The proposed method is based on a modification of the algorithm developed by Knutson and Whitby to calculate the moments of electrical mobility distributions. For this modification, the electrical mobility and the charge distribution have been approximately expressed by power functions of the particle diameter. To evaluate the validity of the approximation, we have carried out numerical simulations for typical size distributions. We have found that for typical narrowly distributed aerosols such as polystyrene latex particles and particles that arise in the tandem differential mobility analyzer configuration, the distribution parameters can be accurately determined by this method. For a log-normally distributed aerosol, the accuracy of the distribution parameters determined by this method has been evaluated as a function of the geometric standard deviation. We have also compared the accuracy of the proposed method with other existing methods in the case of the asymmetric Gaussian distribution.     

The optical properties of two-phase polymer systems: Single scattering in monodisperse,non-absorbing systems

Two-phase polymer systems have achieved commercial importance due mainly to the improvement in impact strength brought about by the addition of dispersed rubber particles to a normally brittle glassy polymer. Rubber-reinforced polystyrene and ABS plastics are two familiar examples. An important drawback of this class of materials is their lack of transparency, caused by the scattering of light at the interface between the phases. The theory of light scattering by spherical particles indicates that the degree of scattering (turbidity) is a function of the amount of dispersed phase present, its particle size, the ratio of refractive indices of the phases, and the wavelength of light. Quantitative predictions of the effects of the above parameters on the transparency of two-phase systems can be made, providing answers to the questions “How close must the refractive indices be?” and “What size must the dispersed-phase particles be?” for a given level of transparency. Calculations for typical polymer pairs reveal that at a given dispersed-phase level, a maximum in turbidity is obtained roughly in the range of particle sizes thought to be necessary for good impact strength. Also, if the refractive indices are matched at a particular temperature, small particle sizes greatly increase the temperature range over which scattering is minimized.     

Heat transfer in aggregative and particulate liquid-fluidized beds

Wall-to-bed heat transfer in liquid fluidized beds, particulately and aggregatively fluidized, was studied. Glass particles fluidized with water gave particulate fluidization and lead particles with water gave aggregative fluidization. Local heat transfer coefficients and bed temperature profiles were measured. Heat transfer coefficients were found to be strongly dependent on particle size and porosity and increased with increasing particle size, but were independent of the height of the heater surface from the grid. Any variations in local bed properties, such as porosity do not affect wall-to-bed heat transfer. The heat transfer coefficients show a characteristic, maximum at porosities near 0.7 for both systems. Bed temperature profiles deviate considerably from open-pipe values.A two-resistance model for the heat transfer resistance agrees well with the data. Bed resistance is modeled by a radial eddy diffusivity, which indicates the mixing effectiveness in the core of the bed. Glass beds (particulate) show a maximum mixing effectiveness at porosities near 0.7 and the mixing effectiveness increases with particle diameter. Lead beds (aggregative) show two maxima in mixing effectiveness, the first between porosities of 0.5 and 0.6, and the second between porosities of 0.7 and 0.8. Mixing is greatest at an intermediate particle size in the case of lead beds. In both systems the fraction of the total resistance in the bed core increases as porosity decreases towards packed bed conditions.     

Design and characterization of a novel single-particle polar nephelometer

A new polar nephelometer (PN) has been developed to measure simultaneously the scattering angular distributions from 11.7° to 168.3° for individual particles in planes parallel and perpendicular to the polarization of the incident laser beam. Each detection plane had 21 silicon photodiode detectors to detect scattered light at a rate of 100 Hz. Laboratory experiments to validate the performance of the instrument were conducted using nearly mono-disperse spherical particles (polystyrene latex [PSL] and nigrosine) and nonspherical particles (sodium chloride [NaCl] and soot). The observed scattering angular distributions for individual PSL particles were in good agreement with the results of simulations based on Mie theory. Complex refractive index values for nigrosine particles were determined by comparing the observed scattering angular distributions with the results of simulations. Clear differences between the measured scattering angular distributions and the results of simulations based on Mie theory assuming spherical particles were observed for NaCl particles (mobility diameters of 500 and 700 nm) and propane soot particles (mobility diameters of 300, 500, and 700 nm). These results are reasonably explained by theoretical predictions. We also conducted initial observations of ambient particles in Nagoya city, Japan. Scattering angular distributions for particles with a mobility diameter of 500 nm and an average effective density of 1.4 or 0.3 g/cm³, which were selected with a combination of differential mobility analyzer and aerosol mass particle analyzer, were measured using the PN. As results, scattering angular distributions for nearly spherical inorganic and organic particles with an average effective density of around 1.4 g/cm³ were found to be distinguishable from nonspherical particles with an average effective density of around 0.3 g/cm³. This study has demonstrated that our PN has the potential to distinguish between spherical and nonspherical particles.

Copyright © 2016 American Association for Aerosol Research     

Brownian diffusion effect on nanometer aerosol classification in electrical mobility spectrometer

A multi-channel differential mobility analyzer (MCDMA) or aerosol spectrometer is widely used for classifying and measuring nanometer aerosol particles in the size range from 1 nm to 1 μm because of its better time response than a typical differential mobility analyzer. In the present study, the effect of Brownian diffusion on electrical mobility classification and trajectory of nanometer aerosol particles in an electrical mobility spectrometer developed at Chiang Mai University has been analytically investigated. Th Brownian diffusion of particles inside the spectrometer increased with decreasing particle size and flow rates of aerosol and clean sheath air, and with increasing inner electrode voltage, and also decreased with decreasing operating pressure. The particle trajectories considering Brownian diffusion motion inside the spectrometer were found to be broader than those under no Brownian diffusion. Smaller particles were found to have higher degree of broadening of trajectory than the larger particles. Brownian diffusion effect was found to be significant for particles smaller than 10 nm.     

Modeling of the scattering and radiative properties of nonspherical dust-like aerosols

The optical and radiative properties of dust particles in solar and thermal infrared regions are investigated. Dust particles are assumed to be spheres and spheroids for a comparison aimed at understanding the nonsphericity effect of these particles on the radiation at the top of a dusty atmosphere. The classical Lorenz–Mie theory is employed to compute the optical properties of spherical dust particles. To compute the single-scattering properties of spheroidal dust particles, a combination of the T-matrix method and an approximate method is used in the present study. In the approximate method, applicable to large particles, the geometric optics method is applied to the computation of the scattering phase matrix. A combination of the solution from the geometric optics method and the contribution of the so-called edge effect is used to compute the extinction efficiency of a spheroidal particle whose absorption efficiency is computed by adding the so-called above- and below-edge effect (a term from the well-known complex angular momentum theory) to the geometric optics result. Numerical results show that the results from the T-matrix method and the present approximate approach converge at a size parameter of 50 for computing the integrated scattering properties (i.e., the extinction efficiency, single-scattering albedo, and asymmetry factor). Additionally, the phase functions computed from the two methods are quite similar for size parameters larger than 40 although some considerable differences may still be noticed for other phase matrix elements. Furthermore, the effect of surface roughness on the single-scattering properties of spheroidal particles is discussed. The present radiative transfer simulations illustrate the nonsphericity effect of dust particles is significant at short wavelengths, however, not at the thermal infrared wavelengths.     

Study of gradual porous metallic membranes obtained by powder sedimentation

In our preliminary studies the possibility of obtaining sintered porous materials with gradual structure by sedimentation of metallic powder was demonstrated. In this paper we continued our studies on the influencing factors of the sedimentation of metallic powders. Irregular and spherical nickel particles were used having a grain size in the 2–90 μm range measured by the laser scattering particle size analyzer. The particles with irregular shape and larger diameter can sediment faster than the spherical and the smaller diameter particles. The sedimentation rate is also influenced by the sedimentation medium and the quantity of the dispersant agent. Deviations from Stokes law was observed in the case of the irregular particles. The gradual structure is influenced by the sintering regime and the powders characteristics too. The obtained structures were characterized by scanning electron microscopy and mercury porosimetry. The permeability and the filtration fineness were also determined.     

Rapid,Size-Resolved Aerosol Hygroscopic Growth Measurements: Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP)

We report on a new instrument developed to perform rapid, size-resolved aerosol hygroscopicity measurements. The differential aerosol sizing and hygroscopicity spectrometer probe (DASH-SP) employs differential mobility analysis in-concert with multiple humidification and optical sizing steps to determine dry optical size and hygroscopic growth factors for size-selected aerosols simultaneously at three elevated relative humidities. The DASH-SP has been designed especially for aircraft-based measurements, with time resolution as short as a few seconds. The minimum particle diameter detected with 50% efficiency in the optical particle counters (OPCs) is 135 ± 8 nm, while the maximum detectable particle diameter is in excess of 1 μm. An iterative data processing algorithm quantifies growth factors and “effective” refractive indices for humidified particles using an empirically derived three-dimensional surface (OPC pulse height–refractive index–particle size), based on a calculated value of the “effective” dry particle refractive index. Excellent agreement is obtained between DASH-SP laboratory data and thermodynamic model predictions for growth factor dependence on relative humidity for various inorganic salts. Growth factor data are also presented for several organic acids. Oxalic, malonic, glutaric, and glyoxylic acids grow gradually with increasing relative humidity up to 94%, while succinic and adipic acids show no growth. Airborne measurements of hygroscopic growth factors of ship exhaust aerosol during the 2007 Marine Stratus/Stratocumulus Experiment (MASE II) field campaign off the central coast of California are presented as the first report of the aircraft integration of the DASH-SP.     

Measurement of size-dependent dynamic shape factors of quartz particles in two flow regimes

Understanding and modeling the behavior of quartz dust particles, commonly found in the atmosphere, requires knowledge of many relevant particle properties, including particle shape. This study uses a single particle mass spectrometer, a differential mobility analyzer, and an aerosol particle mass analyzer to measure quartz aerosol particles mobility (d_m), vacuum aerodynamic, and volume equivalent diameters, mass, composition, effective density, and dynamic shape factor as a function of particle size, in both the free molecular and transition flow regimes. The results clearly demonstrate that dynamic shape factors can vary significantly as a function of particle size. For the quartz samples studied here, the dynamic shape factors increase with size, indicating that larger particles are significantly more aspherical than smaller particles. In addition, dynamic shape factors measured in the free-molecular (χ_v) and transition (χ_t) flow regimes can be significantly different, and these differences vary with the size of the quartz particles. For quartz, χ_v of small (d_m < 200 nm) particles is 1.25, while χ_v of larger particles (d_m ～ 440 nm) is 1.6, with a continuously increasing trend with particle size. In contrast, χ_t of small particles starts at 1.1 increasing slowly to 1.34 for 550 nm diameter particles. The multidimensional particle characterization approach used here goes beyond determination of average properties for each size, to provide additional information about how the particle dynamic shape factor may vary even for particles with the same mass and volume equivalent diameter.

© 2016 American Association for Aerosol Research     

The effect of particle morphology on unipolar diffusion charging of nanoparticle agglomerates in the transition regime

We investigated the effect of particle morphology on unipolar diffusion charging of nanoparticle agglomerates consisting of multiple primary spheres. In the unipolar diffusion charging of non-spherical agglomerates, geometric surface area and electrical capacitance of particles, which are related to particle morphology, are known as important parameters to determine mean charge per particle. From mobility analysis we found that the geometric surface area of chain-like agglomerates is only larger than that of spherical particles with the same mobility diameter for mobility size range below d_m=80 nm. We estimated the electrical capacitance of agglomerates with a newly developed model based on electrostatics and mobility theories. The results show that the electrical capacitance of chain-like agglomerates becomes significantly larger compared to that of spheres with the same mobility diameter as particles become larger. Our analysis results indicate that loose agglomerates have larger mean charge per particle compared to compact particles with the same mobility diameter because the electrical capacitance of agglomerates becomes larger as particle morphology becomes looser. Our experimental data show that mean charge per particle for silver agglomerates is larger than that for fully coalesced silver spheres with the same mobility diameter as agglomerates by about 24%. The experimental data is in good agreement with estimates of mean charge per particle for silver agglomerates.     

Laboratory Verification of PH-CPC's Ability to Monitor Atmospheric Sub-3 nm Clusters

Gas-to-particle conversion takes readily place in the atmosphere. Detecting the initial clusters, which act as embryos for the newly formed particles, is beyond traditional aerosol instrumentation. Charged atmospheric clusters can be measured with air ion spectrometers, but typical state-of-the-art condensation particle counters, which detect both neutral and charged clusters, only see particles larger than 2.5 nm in diameter. In this study we present a modified pulse-height condensation particle counter (PH-CPC) and confirm by laboratory verification that it is capable of detecting charged clusters with electrical mobility equivalent diameter down to ～1 nm. We show how the detection efficiency and the pulse heights depend on the calibration particle size, polarity and composition. The effect of butanol supersaturation on the PH-CPC counting efficiency is also discussed. Furthermore, we developed an inversion method for the data to obtain true particle size distribution from the measurement signal.