Homogeneous nucleation of carbon dioxide in supersonic nozzles I : experiments and classical theories

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Dingilian , K K , Halonen , R , Tikkanen , V , Reischl , B , Vehkamaki , H & Wyslouzil , B E 2020 , ' Homogeneous nucleation of carbon dioxide in supersonic nozzles I : experiments and classical theories ' , Physical Chemistry Chemical Physics , vol. 22 , no. 34 , pp. 19282-19298 . https://doi.org/10.1039/d0cp02279a

Title: Homogeneous nucleation of carbon dioxide in supersonic nozzles I : experiments and classical theories
Author: Dingilian, Kayane K.; Halonen, Roope; Tikkanen, Valtteri; Reischl, Bernhard; Vehkamaki, Hanna; Wyslouzil, Barbara E.
Contributor: University of Helsinki, INAR Physics
University of Helsinki, INAR Physics
University of Helsinki, INAR Physics
University of Helsinki, Institute for Atmospheric and Earth System Research (INAR)
Date: 2020-09-14
Language: eng
Number of pages: 17
Belongs to series: Physical Chemistry Chemical Physics
ISSN: 1463-9076
URI: http://hdl.handle.net/10138/332972
Abstract: We studied the homogeneous nucleation of carbon dioxide in the carrier gas argon for concentrations of CO(2)ranging from 2 to 39 mole percent using three experimental methods. Position-resolved pressure trace measurements (PTM) determined that the onset of nucleation occurred at temperatures between 75 and 92 K with corresponding CO(2)partial pressures of 39 to 793 Pa. Small angle X-ray scattering (SAXS) measurements provided particle size distributions and aerosol number densities. Number densities of approximately 10(12)cm(-3), and characteristic times ranging from 6 to 13 mu s, resulted in measured nucleation rates on the order of 5 x 10(17)cm(-3)s(-1), values that are consistent with other nucleation rate measurements in supersonic nozzles. Finally, we used Fourier transform infrared (FTIR) spectroscopy to identify that the condensed CO(2)particles were crystalline cubic solids with either sharp or rounded corners. Molecular dynamics simulations, however, suggest that CO(2)forms liquid-like critical clusters before transitioning to the solid phase. Furthermore, the critical clusters are not in thermal equilibrium with the carrier gas. Comparisons with nucleation theories were therefore made assuming liquid-like critical clusters and incorporating non-isothermal correction factors.
Subject: MOLECULAR-DYNAMICS
VAPOR-PHASE
MONOETHANOLAMINE MEA
CO2 CAPTURE
GAS
CONDENSATION
TEMPERATURE
EQUILIBRIA
PRESSURES
DENSITY
116 Chemical sciences
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