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Knowledge of carbon isotope fractionation is needed in order to discuss the formation and dissociation of naturally occurring CO 2 hydrates. We investigated carbon isotope fractionation during CO 2 hydrate formation and measured the three-phase equilibria of 12 CO 2 -H 2 O and 13 CO 2 -H 2 O systems. From a crystal structure viewpoint, the difference in the Raman spectra of hydrate-bound 12 CO 2 and 13 CO 2 was revealed, although their unit cell size was similar. The δ 13 C of hydrate-bound CO 2 was lower than that of the residual CO 2 (1.0-1.5‰) in a formation temperature ranging between 226 K and 278 K. The results show that the small difference between equilibrium pressures of ~0.01 MPa in 12 CO 2 and 13 CO 2 hydrates causes carbon isotope fractionation of ~1‰. However, the difference between equilibrium pressures in the 12 CO 2 -H 2 O and 13 CO 2 -H 2 O systems was smaller than the standard uncertainties of measurement; more accurate pressure measurement is required for quantitative discussion.

Carbon Isotope Fractionation during the Formation of CO2 Hydrate and Equilibrium Pressures of 12CO2 and 13CO2 Hydrates