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L W -H Equilibrium Measurements and Unified Predictions of
LW-H Equilibrium Measurements andUnified Predictions of Hydrate-Containing Phase Equilibriafor Methane, Ethane, Propaneand Their Mixtures S. O. Yang, Y. S. Kim, S. K. Ryu and C. S. Lee Thermodynamics and Properties Laboratory Dept. of Chemical Engineering, Korea University Motivation The methane hydrate as a possible energy resource or the CO2 hydrate as a deep-ocean sequestration Necessity for reliable solubility data in water-rich phase of hydrate-containing systems (H-LW). Measurement of solubility using indirect method for sparingly soluble gas components. Necessity for comprehensive calculation methods Unified method to the hydrate-containing systems The applicability of Nonrandom lattice fluid hydrogen bonding theory (You et al. 1994a, 1994b; Lee et al., 2001) Computation of Hydrate Phase Equilibria Equality of Chemical potential(or fugacity) where ? or ? denotes V, LW, LC or Ice phase. is obtained from EOS and from vapor pressure and saturated molar volume(Sloan et al., 1976) H-LW-V, H-I-V, H-LW-LC : Yang et al.(2000), Present work (Mixture) H-LW-V, H-I-V : Klauda and Sandler (2000) H-Lc, H-V, H-LW : Yang et al.(2000, 2001), Present work (Mixture) H-Lc, H-V : Sloan(1976) Computation of Hydrate Phase Equilibria is obtained from (Holder et al.,1980) H-LW-V, H-I-V : Holder et al.(1980), Sloan (1998) H-V, H-LC : Anderson and Prausnitz(1986), Munck et al.(1988) is obtained from the statistical model by van der Waals and Platteeuw (1959). Chemical Potential in Fluid Phase Nonrandom Lattice Fluid Hydrogen Bonding Theory NLF EOS by You et al. [1994 a, b] Expansion to associating system using Veytsman statistics[1990] by Yeom et al. [1999] A normalization of Veytsman statistics by Lee et al. [2001] Parameters for NLF-HB theory Pure species : energy and size parameters Hydrogen-bonding energy and entropy for H2O-H2O interaction Binary interac
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