Homogeneous water nucleation and droplet growth in methane and carbon dioxide mixtures at 235 K and 10 bar

Abstract

Homogeneous nucleation rates and droplet growth rates of water in pure methane and mixtures of methane and carbon dioxide were measured in an expansion wave tube at 235 K and 10 bar. The nucleation rate in pure methane is three orders of magnitude higher than literature nucleation rates of water in low-pressure helium or argon. Addition of carbon dioxide to the carrier gas mixture increases the rates even more. Specifically, rates in a mixture of methane and 3% carbon dioxide are a factor of 10 higher than the rates in pure methane. With 25% carbon dioxide, the rates are four orders of magnitude higher than the rates in pure methane. An application of the nucleation theorem shows that the critical cluster consists of 22 water molecules and 5 methane molecules, for nucleation in pure methane. Growth rates of water droplets were measured in methane and in methane-carbon dioxide mixtures at 243 K and 11.5 bar. At equal temperature, pressure and water vapor fraction, the growth rate of the squared droplet radius is about 20% lower in the mixture with 25% carbon dioxide than in pure methane. The lower growth rate is caused by a smaller diffusion coefficient of water in the mixture with carbon dioxide; the difference of the diffusion coefficients is qualitatively reproduced by the empirical Fuller correlation combined with Blanc's law.