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First-principles calculation of H/D isotopic fractionation between hydrous minerals and water

Abstract : Hydrogen fractionation laws between selected hydrous minerals (brucite, kaolinite, lizardite, and gibbsite) and perfect water gas have been computed from first-principles quantum-mechanical calculations. The β-factor of each phase was calculated using the harmonic phonon dispersion curves obtained within density functional theory. All the fractionation laws show the same shape, with a minimum between 200 °C (brucite) and 500 °C (gibbsite). At low temperatures, the mineral/liquid water fractionation laws have been obtained using the experimental gas/liquid water fractionation laws. The resulting fractionation laws systematically overestimate measurements by 15‰ at low temperatures to 8‰ at ≈400 °C. Based on this general agreement, all calculated laws were empirically corrected with reference to brucite/water data. These considerations suggest that the experimental or natural calibrations by Xu and Zheng (1999) and Horita et al. (2002) (brucite/water), Gilg and Sheppard (1996) (kaolinite/water), Wenner and Taylor (1973) (lizardite/water), and in some extents Vitali et al. (2001) (gibbsite/water) are representative of equilibrium fractionations. Besides, internal isotopic fractionation of hydrogen between inner-surface and inner hydroxyl groups has been computed for kaolinite and lizardite. The obtained fractionation is large, of opposite sign for the two systems (respectively, -23‰ and +63‰ at 25 °C) and is linear in T-2. Internal fractionation of hydrogen in TO phyllosilicates might thus be used in geothermometry.
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Submitted on : Friday, March 11, 2022 - 7:26:17 AM
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Merlin Méheut, Michele Lazzeri, Etienne Balan, Francesco Mauri. First-principles calculation of H/D isotopic fractionation between hydrous minerals and water. GEOCHIMICA ET COSMOCHIMICA ACTA, 2010, 74, pp.3874-3882. ⟨10.1016/j.gca.2010.04.020⟩. ⟨insu-03605315⟩

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