文摘
The structural identification and guest compositions of the mixed CO2 and N2 hydrates at low temperatureconditions were investigated by both theoretical predictions and experimental measurements. From the modelcalculations, at very low temperatures, the highly CO2-concentrated hydrates over 95 mol % CO2 on thebasis of water-free concentration could coexist with the gas mixtures of low CO2 concentrations in equilibrium.X-ray diffraction measurements of the hydrates formed with the gas mixture of 3.16 mol % CO2 and balancedN2 indicate that the formed hydrates at all conditions considered in this study were identified as structure I,whereas the model predicts a structural transition to structure II around 220 K. However, it was also foundthat the formed hydrate samples contain a considerable amount of hexagonal ice resulting from incompleteconversion of ice to the hydrates. The compositional analysis suggests that a favorable encaging of CO2 inthe mixed hydrate can be obtained by the hydrate formation at low temperatures and relative amount of CO2molecules in the mixed hydrates increases with a decrease of temperature.