Homogeneous nucleation of n-propanol, n-butanol, and n-pentanol in a supersonic nozzle

Gharibeh, Murad; Kim, Yoojeong; Dieregsweiler, Uta; Wyslouzil, Barbara E.; Ghosh, David; Strey, R.

doi:10.1063/1.1858438

Cited by 40 publications

(35 citation statements)

References 25 publications

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“…We use the apparatus described in our previous work 15,17 to prepare the gas mixtures and maintain continuous stable supersonic flow in our nozzles. Summarizing briefly, the condensable of interest is vaporized, diluted with the carrier gas, and flows through the supersonic nozzle before it is exhausted to the atmosphere by vacuum pumps.…”

Section: Experiments and Data Analysismentioning

confidence: 99%

Isothermal Nucleation Rates of n-Propanol, n-Butanol, and n-Pentanol in Supersonic Nozzles: Critical Cluster Sizes and the Role of Coagulation

Mullick¹,

Bhabhe²,

Manka

et al. 2014

J. Phys. Chem. B

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We follow the nucleation of n-alcohols, n-propanol through n-pentanol, in two sets of supersonic nozzles having differing linear expansion rates. Combining the data from static pressure trace measurements with small-angle X-ray scattering we report the experimental nucleation rates and critical cluster sizes. For n-propanol, position resolved measurements clearly confirm that coagulation of the 2-10 nm size (radius) droplets occurs on the time scale of the experiment but that the effect of coagulation on the results is minimal. Under the conditions of the current experiments, our results suggest that alcohols have critical clusters that range from the dimer (n-pentanol) to the hexamer (n-propanol). We then compare the experimental results with classical nucleation theory (CNT), the Girshick-Chiu variant of CNT (GC), and the mean field kinetic nucleation theory (MKNT). Both CNT and MKNT underestimate the nucleation rates by up to 5 and 7 orders of magnitude, respectively, while GC theory predicts rates within 2 orders of magnitude. Correspondingly, the critical cluster size for all alcohols is overpredicted by factors of 2-9 with agreement improving with increasing chain length. An interesting byproduct of our experiments is that we find that the coagulation rate is enhanced by a factor of 3 over the value one would calculate for the free molecule regime.

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Section: Experiments and Data Analysismentioning

confidence: 99%

Isothermal Nucleation Rates of n-Propanol, n-Butanol, and n-Pentanol in Supersonic Nozzles: Critical Cluster Sizes and the Role of Coagulation

Mullick¹,

Bhabhe²,

Manka

et al. 2014

J. Phys. Chem. B

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“…8 uses the same data sets as above but only isotherms obeying Hale's condition T / T c Ͻ 0.5 are plotted; plus the data set of Gharibeh et al 46 ͑2005͒ from supersonic nozzle measurements at much lower temperatures ͑T nucl = 207-239 K͒ is included to increase the range of the plot. The Hale plot given in Fig.…”

Section: ͑4͒mentioning

confidence: 99%

Homogeneous nucleation rate measurements of 1-propanol in helium: The effect of carrier gas pressure

Brus

Ždı́mal

Stratmann

2006

The Journal of Chemical Physics

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Kinetics of homogeneous nucleation in supersaturated vapor of 1-propanol was studied using an upward thermal diffusion cloud chamber. Helium was used as a noncondensable carrier gas and the influence of its pressure on observed nucleation rates was investigated. The isothermal nucleation rates were determined by a photographic method that is independent on any nucleation theory. In this method, the trajectories of growing droplets are recorded using a charge coupled device camera and the distribution of local nucleation rates is determined by image analysis. The nucleation rate measurements of 1-propanol were carried out at four isotherms 260, 270, 280, and 290 K. In addition, the pressure dependence was investigated on the isotherms 290 K (50, 120, and 180 kPa) and 280 K (50 and 120 kPa). The isotherm 270 K was measured at 25 kPa and the isotherm 260 K at 20 kPa. The experiments confirm the earlier observations from several thermal diffusion chamber investigations that the homogeneous nucleation rate of 1-propanol tends to increase with decreasing total pressure in the chamber. In order to reduce the possibility that the observed phenomenon is an experimental artifact, connected with the generally used one-dimensional description of transfer processes in the chamber, a recently developed two-dimensional model of coupled heat, mass, and momentum transfer inside the chamber was used and results of both models were compared. It can be concluded that the implementation of the two-dimensional model does not explain the observed effect. Furthermore the obtained results were compared both to the predictions of the classical theory and to the results of other investigators using different experimental devices. Plotting the experimental data on the so-called Hale plot shows that our data seem to be consistent both internally and also with the data of others. Using the nucleation theorem the critical cluster sizes were obtained from the slopes of the individual isotherms and compared with the Kelvin prediction. The influence of total pressure on the observed isothermal nucleation rate was studied in another experiment, where not only temperature but also supersaturation was kept constant as the total pressure was changed. It was shown that the dependence of the nucleation rate on pressure gets stronger as pressure decreases.

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“…In previous works, 30,36 it was verified that the simulations using classical nucleation theory for predictions of J theor in systems with alcohols are very sensitive to the initial data and give results higher in orders of magnitude when compared with experiment. Under the assumption that the nucleation theory describes the location of nucleation peak and its shape correctly, it is possible to distribute the experimentally obtained number of droplets along the whole nucleation zone using the maximum value of nucleation rate J max exp :…”

Section: Data Interpretationmentioning

confidence: 82%

“…13 According to Eq. (36), the values of Le lie between 4.8 and 5.7 for all nucleation temperatures considered in this work. Consistently with Lihavainen's results, 13 these values of Le indicate that the nucleation zone lies along the symmetry axis, as it is possible to see in Fig.…”

Section: Resultsmentioning

confidence: 97%

Description of fluid dynamics and coupled transports in models of a laminar flow diffusion chamber

Trávníčková

Havlica

Ždı́mal

2013

The Journal of Chemical Physics

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The aim of this study is to assess how much the results of nucleation experiments in a laminar flow diffusion chamber (LFDC) are influenced by the complexity of the model of the transport properties. The effects of the type of fluid dynamic model (the steady state compressible Navier-Stokes system for an ideal gas/parabolic profile approximation) and the contributions of the coupled terms describing the Dufour effects and thermodiffusion on the predicted magnitude of the nucleation maxima and its location were investigated. This study was performed on the model of the homogeneous nucleation of an n-butanol-He vapor mixture in a LFDC. The isothermal dependencies of the nucleation rate on supersaturation were determined at three nucleation temperatures: 265 K, 270 K, and 280 K. For this purpose, the experimental LFDC data measured by A. P. Hyvärinen et al. [J. Chem. Phys. 124, 224304 (2006)] were reevaluated using transport models at different levels of complexity. Our results indicate that the type of fluid dynamical model affects both the position of the nucleation maxima in the LFDC and the maximum value of the nucleation rate. On the other hand, the Dufour effects and thermodiffusion perceptibly influence only the value of the maximal nucleation rate. Its position changes only marginally. The dependence of the maximum experimental nucleation rate on the saturation ratio and nucleation temperature was acquired for each case. Based on this dependence, we presented a method for the comparison and evaluation of the uncertainties of simpler models' solutions for the results, where we assumed that the model with Navier-Stokes equations and both coupled effects taken into account was the basis. From this comparison, it follows that an inappropriate choice of mathematical models could lead to relative errors of the order of several hundred percent in the maximum experimental nucleation rate. In the conclusion of this study, we also provide some general recommendations concerning the proper choice and setting of the mathematical model of transport processes in the LFDC.

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Homogeneous nucleation of n-propanol, n-butanol, and n-pentanol in a supersonic nozzle

Cited by 40 publications

References 25 publications

Isothermal Nucleation Rates of n-Propanol, n-Butanol, and n-Pentanol in Supersonic Nozzles: Critical Cluster Sizes and the Role of Coagulation

Isothermal Nucleation Rates of n-Propanol, n-Butanol, and n-Pentanol in Supersonic Nozzles: Critical Cluster Sizes and the Role of Coagulation

Homogeneous nucleation rate measurements of 1-propanol in helium: The effect of carrier gas pressure

Description of fluid dynamics and coupled transports in models of a laminar flow diffusion chamber

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