The temperature dependence of combined homogeneous and heterogeneous crystal nucleation is examined within the framework of the classical theory. It is demonstrated that nucleation can have a local maximum rate at one or two temperatures. The physical parameters which cause large changes in the structure of the nucleation curve are elucidated. Also, the influence of saturation effects on the structure of nucleation curves is illustrated. The utilization of these results for the interpretation of experiments and for the production of controlled crystal nucleation in glass is considered. 相似文献
The homogeneous particle nucleation in a free turbulent jet is simulated at Reynolds numbers of 3400 and 34,000 by using large eddy simulation (LES) coupled with our newly developed equivalent mean nucleation method (EMNM) for the present study. The simulated velocity field, passive scalar concentration, and nucleated particle concentration are compared with various available measurements in the literature. Both the simulated mean velocity and mean scalar concentration show self-similarity properties and agree well with the experimental measurements quantitatively in the literature. Using the EMNM, it is found that the nucleation primarily occurs in a very narrow region around the jet centerline. It is also found that the position of maximum nucleation is a function of the vapor temperature and concentration at the jet exit and its surrounding background (i.e., T0, T∞, c0, and c∞), and the function varies monotonically with respect to these four parameters. Present numerical simulation and analysis also show that the group, (where is the mean particle number concentration, u0 is the jet velocity, and d is the jet exit diameter), is constant along the axial direction of the jet, which was first observed in the experiment of Lesniewski, T. K., and Friedlander, S. K. (1998). Particle Nucleation and Growth in a Free Turbulent Jet. Proc. R. Soc. Lond. A, 454:2477–2504. However, a different physical explanation of the fact is provided. In this study, it is found that the maximum nucleation occurs around 20d away from the jet exit, other than in the shear layer (less than 5d), which was supposed by Lesniewski, T. K., and Friedlander, S. K. (1998). On the basis of the additional simulated results, more comprehensive and reasonable explanations of their measurement data are provided. In this study, an efficient and rigorous numerical method is presented to simulate the homogeneous particle nucleation in a free turbulent jet, and this has provided a deeper and thorough understanding of the process. 相似文献
The formation of aerosol particles by homogeneous nucleation in a supersaturated vapor has been studied experimentally and theoretically. In the laboratory, a particle-free gas at room temperature is continuously mixed with a high-temperature gas containing dibutylphthalate vapor in a new device for the study of aerosol nucleation called a particle size magnifier. A highly supersaturated vapor is rapidly formed in the mixing zone of the particle size magnifier, and the resulting number concentrations of aerosol particles are measured under various temperatures, mixing ratios, and mixing methods. Measured number concentrations are compared with those predicted by the classical and Lothe-Pound nucleation theories. The measured concentrations lie between the predictions of the two theories, and the trends with temperature and saturation ratio are consistent with either nucleation theory, provided vapor depletion is considered. 相似文献
Summary: Non‐Newtonian fluid behavior has significant influence on quantities in chemical engineering like power input, mixing time, heat transfer etc. In the laminar flow region, the concept of effective viscosity by Metzner and Otto is well established. In the transition region between laminar and turbulent flow, the existing concepts use three and even more empirical parameters to determine the specific power input. Here, a unified and general but simple approach is introduced to calculate the power input for shear thinning fluids over the whole flow region using just one empirical parameter. The Metzner‐Otto relation is obtained as a limiting case for the laminar region. The empirical parameter of the new approach is related to the Metzner‐Otto constant. The concept is validated for eight different stirrer systems. Mixing time and maximum shear rate and heat transfer can also be calculated using this approach. The new concept presented should also be applicable for other apparatuses, e.g., static mixers.
Comparison of experimental data and a curve calculated according to the new method (solid line). 相似文献
A SiAlON ceramic with yttria as a sintering aid has been fabricated and subjected to a 1-h heat treatment at 1150°C. Microstructural characterization by analytical electron microscopy and diffraction analysis indicates that the residual intergranular phase crystallizes into a metastable hexagonal phase (Y2SiAlO5N) and mullite. The mullite appears as a characteristically shaped precipitate forming with a definite orientation relationship on the (10 1 0) facets of SiAlON grains. The absence of a residual amorphous film between the precipitate and the SiAlON indicates that the precipitation occurred in a heterogeneous manner on the surface of the SiAlON. 相似文献
Nucleation rate is a very sensitive function of the temperature and vapor mole fraction. Analytical approximation schemes for the mean nucleation rate in turbulent flows are derived using Laplace’s approximation method. The schemes only require the derivative of the nucleation rate function and the probability density function (pdf) of the vapor mole fraction and/or temperature at the point of maximum nucleation rate. Based on the relation between the mole fraction and temperature, i.e., linearly correlated or not, different approximation schemes are developed. Numerical examples are constructed to investigate the accuracy of these approximation. In the examples, the pdfs of mole fraction and/or temperature in various turbulent flows are assumed to come from the beta distribution with five distinct forms. The mean nucleation rate of dibutyl phthalate (DBP) aerosol in these turbulent flows are calculated from the approximation schemes, and compared with exact numerical integration. The relative errors are less than 1% for cases when nucleation rate diminishes at the bounds of temperature fluctuations, and no more than 50% for all studied examples. Furthermore, the approximation schemes are not sensitive to the precise form of the pdfs. Hence, these developed approximation schemes can be used to estimate the mean nucleation rate in a broad range of turbulent flows conveniently.
Copyright 2014 American Association for Aerosol Research 相似文献
The prediction of the diffusion of a spray in a gaseous environment is still a difficult problem to solve, even when the droplets are small enough to be considered a passive contaminant. The present work proposes to use a simulation of the random trajectories of the individual particles based on the method proposed by Ormancey (1983), and Ormancey and Martinon (1983). It is applied to the case of a nozzle of finite dimensions discharging passive particles in homogeneous turbulent airstream at a low enough concentration to avoid neighboring effects. The results of this simulation compare favorably with those of an experiment designed to test the method. They are also in agreement with the Lagrangian diffusion theory of Taylor (1936). 相似文献
The mixing and diffusion of monodisperse aerosols from a turbulent free stream into the wake created by a solid sphere were studied experimentally and analytically. Experimental measurements with regard to wake velocity profiles and momentum transport were taken in a tubular flow system by hot-wire anemometry. Particle concentration profiles, measured in the wake by means of a screen collection technique, were used to calculate mixing and diffusion parameters for the aerosols used. Experimental results are presented for the mean velocity and particle concentration profiles, wake centerline velocity and particle concentration, wake velocity and concentration half widths, and momentum and particle diffusivities. It is shown that the experimental results may be reasonably described in terms of two phenomenological theories, i.e., Prandtl's mixing length and constant diffusivity in the radial cross section of the wake. Certain departures from predicted concentration behavior are empirically analyzed resulting in the ability to predict overall particle mixing and diffusion characteristics in a turbulent wake. 相似文献
Bio-inspired and single site metal complex catalysts have been discussed to direct towards a rational design of solid heterogeneous catalysts. When concepts derived from catalytic antibodies, molecular imprinting and molecular recognition, and site isolation and modification by appropriate ligands are combined, with new techniques to prepare, tailor made solid materials, catalysts can be prepared that improve reaction rate and selectivity by increasing the concentration and activation of reactants in the vicinity of the active sites, and by stabilizing transition states or intermediate products. It is also shown that enzymatic, homogeneous and hetergeneous catalysts can be combined to perform “one-pot” cascade reactions. 相似文献
The interfacial tension of 2, 4-dichlorophenol/acidic solution, 23 ergs/cm2, was calculated from Nielsen's equations which combine homogeneous nucleation theory and diffusion controlled growth. The parameters measured were induction periods in the millisecond range and the technique employed was photographing the appearance of turbidity on a film moving at 50cm/sec velocity. The calculated value was compared with direct measurements of 2, 4-dichlorophenol's surface tension in air and in solution. 相似文献
Aerosol processes that produce titania particles by reacting gaseous precursors (such as titanium tetrachloride) initially must mix the precursor into the oxidizer at elevated temperatures to initiate the formation of product. Oftentimes the rate of reaction is sufficiently large as to be mixing limited. Thus the rate of mixing of the reacting species will control the chemistry and morphological properties of the particles that are produced. The interplay between mixing, nucleation, and growth in these systems is difficult to observe experimentally due to the small time scales that are involved and the spatial limitations of most diagnostics. An alternative approach is direct numerical simulation (DNS). DNS refers to a class of numerical solutions of the three-dimensional time-dependent governing equations for a particular system in which no turbulence modeling assumptions are made. To within the precision of the numerical algorithm, DNS can be thought of as a numerical experiment. Here we apply DNS to the mixing, reaction, nucleation, and growth of titania particles formed from the reaction of titanium tetrachloride with oxygen. The simulation solves for the velocity, species concentration, and eight moments of the particle size distribution using a combination of a pseudospectral method (for the velocity) and a compact finite difference scheme (for all of the scalars). The results show that increasing the rate of mixing increases the rate of particle formation while decreasing the variance in the particle size distribution. However, for a given extent of reaction, poorer mixing leads to larger mean particle sizes and larger standard deviations. The results are most easily interpreted in terms of the reaction volume between the unmixed reactants, where most of the reaction occurs. Based on this analysis, we present rules of thumb for controlling the particle size distribution in aerosol reactors. 相似文献
We examine the nucleated (with barrier) activation of perfectly wetting (zero contact angle) particles ranging from essentially bulk size down to approximately 1-nm mass diameter. While similar studies trace back to the pioneering work of Fletcher, we present here a novel approach to the analysis based on general area constructions that enable key thermodynamic properties, including surface and bulk contributions to nucleation work, to be interpreted geometrically with reference to the Kelvin curve. The kinetics of activation are described in more detail in terms of the mean first passage time (MFPT) for barrier crossing. MFPT theory and benchmark calculations are used to develop and test a new approximate-but-simpler-to-use analytic expression for the barrier crossing rate. The present study is motivated by recent condensation particle counter (CPC) studies that appear to finally establish the long-predicted detection of “sub-Kelvin” particles in the nano-size regime. Corresponding states thermodynamic and kinetic scaling approaches are used to facilitate the correlation and selection of optimal CPC working fluids and operating conditions based on a new metric for heterogeneous nucleation, the signal-to-noise ratio, and physical and chemical properties. Copyright 2012 American Association for Aerosol Research 相似文献