Thermodynamic data and modeling of the water and ammonia-water phase diagrams up to 2.2 GPa for planetary geophysics (original) (raw)

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Research Article| October 08 2010

Mathieu Choukroun;

1Jet Propulsion Laboratory,

California Institute of Technology

, 4800 Oak Grove Dr., MS 79-24, Pasadena, California 91103,

USA

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Olivier Grasset

2UMR-CNRS 6112-Planétologie et Géodynamique,

Université de Nantes

, 2 rue de la Houssinière, 44322 Nantes Cedex 3,

France

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J. Chem. Phys. 133, 144502 (2010)

We present new experimental data on the liquidus of ice polymorphs in the H2O–NH3 system under pressure, and use all available data to develop a new thermodynamic model predicting the phase behavior in this system in the ranges (0–2.2 GPa; 175–360 K; 0–33 wt % NH3⁠). Liquidus data have been obtained with a cryogenic optical sapphire-anvil cell coupled to a Raman spectrometer. We improve upon pre-existing thermodynamic formulations for the specific volumes and heat capacities of the solid and liquid phase in the pure H2O phase diagram to ensure applicability of the model in the low-temperature metastable domain down to 175 K. We compute the phase equilibria in the pure H2O system with this new model. Then we develop a pressure-temperature dependent activity model to describe the effect of ammonia on phase transitions. We show that aqueous ammonia solutions behave as regular solutions at low pressures, and as close-to-ideal solutions at pressure above 600 MPa. The computation of phase equilibria in the H2O–NH3 system shows that ice III cannot exist at concentrations above 5–10 wt % NH3 (depending on pressure), and ice V is not expected to form above 25%–27% NH3⁠. We eventually address the applications of this new model for thermal and evolution models of icy satellites.

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