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Title: Vapor phase nucleation of the short-chain n-alkanes (n-pentane, n-hexane and n-heptane): Experiments and Monte Carlo simulations

Abstract

We measured the nucleation rates of n-pentane through n-heptane in a supersonic nozzle at temperatures ranging from ca. 109 K to 168 K. For n-pentane and n-hexane, these are the first nucleation rate measurements that have been made, and the trends in the current data agree well with those in the earlier work of Ghosh et al. for longer chain alkanes. Complementary Monte Carlo simulations, using the transferable potentials for phase equilibria-united atom potentials, suggest that despite the high degree of supercooling, the critical clusters remain liquid like under experimental conditions for n-pentane through n-heptane, but adopt more ordered structures for n-octane and n-nonane. For all three alkanes, the experimental and simulated nucleation rates are offset by ~3 orders of magnitude when plotted as a function of ln S/(Tc/T – 1)1.5. Explicitly accounting for the surface tension difference between the real and model substances, or alternatively using the Hale scaling parameter, Ω, consistent with the model potential, increases the offset to ~6 orders of magnitude.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. The Ohio State Univ., Columbus, OH (United States)
  2. Louisiana State Univ., Baton Rouge, LA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1506524
Alternate Identifier(s):
OSTI ID: 1433040
Grant/Contract Number:  
AC02-06CH11357; CHE-1464924; CHE-1052015; EPS-1003897
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 148; Journal Issue: 14; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ogunronbi, Kehinde E., Sepehri, Aliasghar, Chen, Bin, and Wyslouzil, Barbara E. Vapor phase nucleation of the short-chain n-alkanes (n-pentane, n-hexane and n-heptane): Experiments and Monte Carlo simulations. United States: N. p., 2018. Web. doi:10.1063/1.5023567.
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Ogunronbi, Kehinde E., Sepehri, Aliasghar, Chen, Bin, & Wyslouzil, Barbara E. Vapor phase nucleation of the short-chain n-alkanes (n-pentane, n-hexane and n-heptane): Experiments and Monte Carlo simulations. United States. https://doi.org/10.1063/1.5023567
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Ogunronbi, Kehinde E., Sepehri, Aliasghar, Chen, Bin, and Wyslouzil, Barbara E. Fri . "Vapor phase nucleation of the short-chain n-alkanes (n-pentane, n-hexane and n-heptane): Experiments and Monte Carlo simulations". United States. https://doi.org/10.1063/1.5023567. https://www.osti.gov/servlets/purl/1506524.
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@article{osti_1506524,
title = {Vapor phase nucleation of the short-chain n-alkanes (n-pentane, n-hexane and n-heptane): Experiments and Monte Carlo simulations},
author = {Ogunronbi, Kehinde E. and Sepehri, Aliasghar and Chen, Bin and Wyslouzil, Barbara E.},
abstractNote = {We measured the nucleation rates of n-pentane through n-heptane in a supersonic nozzle at temperatures ranging from ca. 109 K to 168 K. For n-pentane and n-hexane, these are the first nucleation rate measurements that have been made, and the trends in the current data agree well with those in the earlier work of Ghosh et al. for longer chain alkanes. Complementary Monte Carlo simulations, using the transferable potentials for phase equilibria-united atom potentials, suggest that despite the high degree of supercooling, the critical clusters remain liquid like under experimental conditions for n-pentane through n-heptane, but adopt more ordered structures for n-octane and n-nonane. For all three alkanes, the experimental and simulated nucleation rates are offset by ~3 orders of magnitude when plotted as a function of ln S/(Tc/T – 1)1.5. Explicitly accounting for the surface tension difference between the real and model substances, or alternatively using the Hale scaling parameter, Ω, consistent with the model potential, increases the offset to ~6 orders of magnitude.},
doi = {10.1063/1.5023567},
journal = {Journal of Chemical Physics},
number = 14,
volume = 148,
place = {United States},
year = {Fri Apr 13 00:00:00 EDT 2018},
month = {Fri Apr 13 00:00:00 EDT 2018}
}
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https://doi.org/10.1063/1.5023567
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