Abstract
We conducted homogeneous nucleation experiments for dilute binary H2O-CO2 mixtures in Ar-N2 carrier gas with different CO2/H2O ratios at temperatures of 57 and 75K and total pressures of ∼40 and 70Pa, respectively. Direct experimental information on the number and type of molecules in the clusters and on the cluster number concentration is obtained by mass spectrometric detection of nucleating clusters that form in the uniform region of Laval expansions. Only homo-molecular water clusters are observed in the mass spectra. However, as the CO2/H2O ratio increases, a significant increase in the nucleation rate is observed. A simple kinetic model suggests that this acceleration of nucleation is due to the formation of short-lived, transient hetero-molecular H2O-CO2 dimers. Comparison with homogeneous binary nucleation of toluene-CO2 and unary nucleation of H2O shows that nucleation becomes more efficient in systems with stronger intermolecular interactions and a larger number of degrees of freedom. Such studies at the molecular level will improve our understanding of homogeneous nucleation mechanisms in atmospheric and industrial processes.
Published Version
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