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  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 103 (1995), S. 1714-1717 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We present homogeneous nucleation rates in the binary mixture n-nonane/methane in the supercritical regime, measured in a new pulse expansion tube at pressures up to 40 bar, at a temperature of 240 K. It is shown that both n-nonane and methane are present in the critical cluster. The critical supersaturation of n-nonane decreases from 30 at 10 bar, down to 6 at 40 bar total pressure. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 102 (1995), S. 4531-4537 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A thermodynamic model of the formation free energy of a droplet, based on a real equation of state, has been implemented in the binary classical nucleation theory to analyze homogeneous nucleation of mixtures of n-nonane and methane in the coexistence region at high pressures. The composition of the critical nucleus is computed by solving the Kelvin equations, the chemical potentials, and molar volumes being evaluated from the Redlich–Kwong–Soave equation of state. Real gas behavior appears to have a strong effect on nucleation due to mutual interactions between methane and nonane molecules. Numerical calculations show an increasing concentration of methane in critical clusters with increasing pressure at fixed temperature and supersaturation. As a consequence, the surface tension of the critical droplets, which is evaluated by means of the Parachor method, is lowered, having a strong increasing effect on the nucleation rate; a 10 bar increase of total pressure leads to an increase of the nucleation rate of several orders of magnitude. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 3
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 8535-8544 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Nucleation rate data, obtained from expansion wave tube experiments, are reported for several vapor–gas mixtures at high pressure. Results are given for water–vapor in the presence of helium and nitrogen gas, and for n-nonane in helium and methane. For all these mixtures, carrier gas pressures of 10, 25, and 40 bar have been applied, with temperatures ranging from 230 to 250 K. An extended form of the nucleation theorem (in terms of the derivative of the nucleation rate with respect to carrier gas pressure) is derived, which appears to be very helpful in the interpretation of high pressure data. It can be used to obtain the carrier gas content of the critical nucleus directly from the pressure dependence of experimental nucleation rates. Combining this method with the theoretical considerations of part I of this paper [J. Chem. Phys. 111, 8524 (1999), preceding paper]: the nucleation behavior of water at high pressures of both helium and nitrogen can quantitatively be understood. For n-nonane in helium our "pressure perturbation approach" is also valid. For n-nonane in methane, however, this approach fails because of the high methane solubility in the liquid phase. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 8524-8534 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A theoretical approach is presented that accounts for the influence of high pressure background gases on the vapor-to-liquid nucleation process. The key idea is to treat the carrier gas pressure as a perturbation parameter that modifies the properties of the nucleating substance. Two important mechanisms are identified in this respect: With increasing carrier gas pressure, the saturated vapor density tends to increase (enhancement effect), whereas the surface tension generally decreases. Several routes to obtain data for these pressure effects are outlined, in particular for the vapor–gas mixtures that have been studied experimentally. (The results of these expansion wave tube experiments are presented in Paper II of this paper [J. Chem. Phys. 111, 8535 (1999), following paper.]) Using classical nucleation theory, a criterion is then derived for the "pressure perturbation" approach to be valid: xgeq(very-much-less-than)(S−1)/S, where xgeq is the carrier gas solubility in the liquid phase, and S is the supersaturation ratio. For the semiphenomenological Kalikmanov–Van Dongen model, the implications of the enhancement effect and surface tension decrease are briefly discussed. We also illustrate how these two effects can be obtained from (binary) density functional theory. Results of the latter for a mixture of Lennard-Jones particles are presented, with potential parameters that are characteristic for n-hexane with several carrier gases. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 5
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 8116-8123 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Nucleation rate measurements of water in the presence of nitrogen as a carrier gas are reported at total pressures near 10, 25, and 40 bar, and temperatures of 230 and 250 K. The results were obtained using our pulse-expansion wave tube, particularly suited for high pressure nucleation research. Enhanced fugacity of water vapor in the mixture, due to the presence of nitrogen, was quantitatively taken into account. Values of the enhancement factors as a function of pressure and temperature were correlated from accurate gravimetric measurements available in literature. The results demonstrate a strong influence of nitrogen pressure on the nucleation behavior of water, when temperature and supersaturation are kept fixed. The effect is associated with a decrease of the surface tension of water, due to the adsorption of nitrogen onto the liquid surface. A tentative model is presented that qualitatively describes this decreasing surface tension with pressure. The competition between the opposing effects of enhanced fugacity and decreasing surface tension is identified as a complicating factor in detecting pressure effects on nucleation. This conclusion is expected to hold for other vapor/carrier gas systems as well. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 6
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 4152-4156 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Within the scope of joint experiments by the international Nucleation Workshop Group, nucleation experiments on n-pentanol were carried out using a pulse-expansion wave tube. Data were obtained for nucleation at temperatures between 240 K and 260 K. Total pressures of the carrier gas (helium) during nucleation varied from 89 to 109 kPa. The results are presented in tabular form, to facilitate future comparison. Our results are consistent with existing data by Hrubý et al. Comparisons are made to the Kinetic Classical Theory (KCT) as well as to the semiphenomenological theory by Kalikmanov and Van Dongen (KvD–SPT). Although both theories predict nucleation rates that are apparently too low in the temperature range of interest, the KvD–SPT is approximately two orders of magnitude closer to the experimental results. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 7
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 3553-3558 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The first quantitative experimental results are presented on homogeneous nucleation and droplet growth in a multicomponent gas-vapor mixture. Using the pulse-expansion wave tube technique, we investigated the condensation behavior of natural gas consisting of over 30 components. Data were obtained in the pressure range between 6 and 24 bar and at temperatures ranging from 221 to 237 K. The observed droplet growth rates are quantitatively explained using a multicomponent model for diffusion controlled growth. The nucleation rate data are for the moment mainly presented as a challenge to theoreticians, although some qualitative arguments are presented that could be helpful in the interpretation. The data appear to agree at least qualitatively with theoretical values (according to the revised binary classical nucleation theory) for a mixture of n-octane and methane, a model mixture which also shows the same macroscopic phase behavior as natural gas. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
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