Mathematics – Logic
Scientific paper
Apr 2006
adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=2006gecoa..70.1904p&link_type=abstract
Geochimica et Cosmochimica Acta, Volume 70, Issue 8, p. 1904-1913.
Mathematics
Logic
1
Scientific paper
We have developed a simple, yet accurate theoretical method for calculating the reduced isotope partition function ratio (RIPFR) for hydrogen of water at elevated pressures. This approach requires only accurate equations of state (EOS) for pure isotopic end-members (H2O and D2O), which are available in the literature. The effect of pressure or density on the RIPFR of water was calculated relative to that of ideal-gas water at infinitely low pressure for the temperature range from 0 to 527 °C. For gaseous and low-pressure (ca. ⩽15 MPa) supercritical phases of water, the RIPFR increases slightly (1 1.3‰) with pressure or density in a fashion similar to those of many other geologic materials. However, in liquid and high-pressure (>20 MPa) supercritical phases, the RIPFR of water decreases (0.5 6‰) with increasing pressure (or density) to 100 MPa. This rather unique phenomenon is ascribed to the inverse molar volume isotope effects (MVIE) of liquid and high-density supercritical waters, V (D2O) > V (H2O), while other substances including minerals show the normal MVIE. These theoretical predictions were experimentally confirmed by Horita et al. [Horita, J., Cole, D.R., Polyakov, V.B., Driesner, T., 2002. Experimental and theoretical study of pressure effects on hydrogen isotope fractionation in the system brucite water at elevated temperatures. Geochim. Cosmochim. Acta66, 3769 3788.] for the system brucite water. Although the P T ranges for the EOS of normal and heavy waters are rather limited, our modeling indicates that the RIPFR of water continues to decrease with pressure above 100 MPa. The method developed here can be applied to any other geologic fluids, if accurate EOS for their isotopic end-members is available. These results have important implications for the interpretation of high-pressure isotopic partitioning in the Earth, the outer planets, and their moons.
Cole Daniel R.
Horita Juske
Polyakov Veniamin B.
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