Prediction Phase Equilibrium of Gas Hydrate in the Presence of Alcohol Organic Inhibitors Using an UNIQUAC Activity Coefficient Model
摘要
In the oil and gas sector, organic alcohol inhibitors are pivotal for mitigating hydrate formation. In this paper, we developed a three-dimensional predictive model for the phase equilibrium surface of gas hydrate, specifically focusing on temperature, pressure, and alcohol concentration within alcohol inhibitor aqueous solutions. This model integrates the Chen-Guo model with the Benedict-Webb-Rubin-Starling (BWRS) equation of state and the universal quasichemical (UNIQUAC) activity coefficient model, while accounting for interactions among various inhibitors. Using this model, we predicted the phase equilibrium surfaces for methane hydrate in the presence of four prevalent alcohol inhibitors: methanol (MeOH), ethanol (EtOH), ethylene glycol (EG), and diethylene glycol (DEG). The predicted surfaces closely align with the experimental data from prior studies. Compared to the models by Mohammadi, Li, and Hsieh, our model exhibits superior accuracy for methane hydrate systems that include methanol or ethylene glycol, achieving an absolute mean relative deviation in temperature (AADR-T) of only 0.18% and 0.25%, respectively. Furthermore, in systems with mixed binary alcohol inhibitors, the model shows enhanced interaction considerations, reducing the AADR-T from 0.30% to 0.18% and thus improving prediction accuracy by 40%. Additionally, we analyzed the distribution characteristics of these three-dimensional phase equilibrium surfaces in terms of chemical factors and Clausius-Clapeyron linear behavior. Notably, the phase equilibrium pressure-temperature (p-T) curve exhibits a downward shift as the molar fraction of inhibitors increases, particularly when pressures exceed 20 MPa. Moreover, the surface plots of 1/T versus lnp suggest a roughly linear relationship within the pressure range of 3 to 20 MPa.