Abstract
A new, rigorous framework centered around the multi-scale GHC equation of state is presented for predicting bulk density and phase equilibrium for light gas–water mixtures at conditions where hexagonal ice and structure I hydrate phases can exist. The novel aspects of this new framework include (1) the use of internal energies of departure for ice and empty hydrate respectively to determine densities, (2) contributions to the standard state fugacity of water in ice and empty hydrate from lattice structure, (3) computation of these structural contributions to standard state fugacity from compressibility factors and EOS parameters alone, and (4) the direct calculation of gas occupancy from phase equilibrium. Numerical results for densities and equilibrium for systems involving ice and/or gas hydrates predicted by this GHC-based framework are compared to predictions of other equations of state, density correlations, and experimental data where available. Results show that this new GHC-based EOS framework accurately predicts the densities of hexagonal water ice and structure I gas hydrates as well as phase equilibrium for methane–water and CO2–water mixtures.
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