Journal
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
Volume 24, Issue 11, Pages -Publisher
MDPI
DOI: 10.3390/ijms24119321
Keywords
gas hydrates; carbon dioxide; phase equilibria; ice; quadruple point; measurement
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Using the CO2-H2O system, a new method for determining the non-variant equilibrium of the four phases (vapor-aqueous solution-ice-gas hydrate) in P-T coordinates has been proposed and validated. The method involves direct measurement of parameters after gas hydrate and ice phase formation.
Precise data on the non-variant equilibrium of the four phases (vapor-aqueous solution-ice-gas hydrate) in P-T coordinates are highly desired for developing accurate thermodynamic models and can be used as reference points (similar to the triple point of water). Using the two-component hydrate-forming system CO2-H2O, we have proposed and validated a new express procedure for determining the temperature and pressure of the lower quadruple point Q(1). The essence of the method is the direct measurement of these parameters after the successive formation of the gas hydrate and ice phases in the initial two-phase gas-water solution system under intense agitation of the fluids. After relaxation, the system occurs in the same equilibrium state (T = 271.60 K, P = 1.044 MPa), regardless of the initial parameters and the order of crystallization of the CO2 hydrate and ice phases. Considering the combined standard uncertainties (+/- 0.023 K, +/- 0.021 MPa), the determined P and T values agree with the results of other authors obtained by a more sophisticated indirect method. Validating the developed approach for systems with other hydrate-forming gases is of great interest.
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