Ky. Song et al., SOLUBILITY MEASUREMENTS OF METHANE AND ETHANE IN WATER AT AND NEAR HYDRATE CONDITIONS, Fluid phase equilibria, 128(1-2), 1997, pp. 249-259
The isobaric solubility of pure methane and ethane gases in liquid wat
er was measured under different conditions, including hydrate formatio
n points, using a ramping method in which measurements are made throug
h the entire and continuous hydrate formation/decomposition cycle. The
work was conducted for methane at 3.45 MPa (500 psia) and temperature
s ranging from 17.0 to 0.0 degrees C (290.2 to 273.2 K), and for ethan
e at 0.66 MPa (95 psia) and a temperature range of 17.0 to 0.0 degrees
C (290.2 to 273.2 K). The isobaric solubilities obtained show a signi
ficant divergence from (normal) Henry's law solubility as the temperat
ure is lowered, The increase in the solubility is presumably the resul
t of the onset of a sorption process that traps the gas molecules in t
he water structure. Several sub-processes were observed as the hydrate
formation was taking place: (1) the dissolution of the gas in the liq
uid water, or interstitial solubility, (2) the onset of the sorption s
ub-process and build-up of the hydrate precursors, (3) the catastrophi
c formation and the existence of the solid phase with its slushy chara
cteristics, and (4) the solidification of the hydrates, therefore caus
ing the total plugging of the experimental cell.