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Binary Nucleation of n-butanol and Deuterium Oxide Conducted in Supersonic Nozzles

Mullick, Kelley Anne
http://rave.ohiolink.edu/etdc/view?acc_num=osu1324247960

Abstract Details

2012, Doctor of Philosophy, Ohio State University, Chemical and Biomolecular Engineering.
Nucleation is the first step in the formation of a more stable liquid phase from a supersaturated vapor phase. This process is important in a wide range of industrial and natural settings ranging from particle production in combustion to smog formation in a polluted atmosphere. In most cases, more than one species participates and the nucleation rates are enhanced over the rate expected for a single compound. The focus of this work is binary nucleation from deuterium oxide (D2O)/n-butanol vapor mixtures. This system is interesting because alcohols are known to enhance both particle formation relative to pure D2O and because bulk n-butanol and D2O liquid mixtures exhibit a large miscibility gap. To investigate particle formation in this binary system, pressure trace measurements (PTM) were conducted for a series of mixtures in two supersonic nozzles with different expansion rates. The experiments yielded the temperature, pressure, mass fraction of the condensate, gas velocity, and the characteristic nucleation time. Small Angle X-ray Scattering (SAXS) measurements were used to determine the aerosol number densities and droplet radii. The binary nucleation rates were obtained by combining the results from both experiments. After the experimental nucleation rates were determined, the critical cluster sizes for the mixtures were estimated using the first nucleation theorem (Kashchiev, 1982; Vehkamäki and Ford, 2000; Tanimura, 2011). The excess energies were calculated using the second nucleation theorem (Ford, 1997; Vehkamäki and Ford, 2000; Tanimura, 2011). The critical cluster sizes and excess energies for D2O were compared to previous measurements (Kim et al., 2004). In addition, the nucleation rates and critical cluster sizes of the homologous series of n-alcohols, n-propanol through n-pentanol, were determined. Alcohols are good compounds to investigate because their physical properties are well characterized and even in supersonic nozzle experiments, condensation occurs above the triple point. Furthermore, hydrogen bonding enhances the stability of subcritical clusters in the vapor phase. The results suggest that under the conditions of the current experiments, these alcohols have critical clusters that range from the dimer (n-pentanol) to the hexamer (n-propanol).
Barbara Wyslouzil (Advisor)
Isamu Kusaka (Committee Member)
James Rathman (Committee Member)
217 p.
Chemical Engineering
binary nucleation; surface enrichment; nonidealty; critical cluster; excess energy; d2O; butanol;

Recommended Citations

Citations

  • Mullick, K. A. (2012). Binary Nucleation of n-butanol and Deuterium Oxide Conducted in Supersonic Nozzles [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1324247960

    APA Style (7th edition)

  • Mullick, Kelley. Binary Nucleation of n-butanol and Deuterium Oxide Conducted in Supersonic Nozzles. 2012. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1324247960.

    MLA Style (8th edition)

  • Mullick, Kelley. "Binary Nucleation of n-butanol and Deuterium Oxide Conducted in Supersonic Nozzles." Doctoral dissertation, Ohio State University, 2012. http://rave.ohiolink.edu/etdc/view?acc_num=osu1324247960

    Chicago Manual of Style (17th edition)

osu1324247960
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© 2012, all rights reserved.
This open access ETD is published by The Ohio State University and OhioLINK.