甲烷水合物膜生长动力学研究

Study on Growth Kinetics of Methane Hydrate Film

采用水中悬浮气泡法测定了温度为273.4～279.4K、压力为3.60～11.90MPa范围内甲烷微小气泡表面水合物膜生长动力学数据.应用无因次Gibbs自由能差(-?Gexp/RT)作为推动力,提出了具物理意义的水合物膜生长动力学模型,并回归得到甲烷水合物膜生长动力学反应级数为1.60,表观活化能为55.95kJ?mol-1,指前因子为1.65×1011mm2?s-1.同时考察了温度和压力对甲烷水合物膜生长速率的影响.

Film growth kinetics data of methane hydrate were measured by a suspended gas bubble in water over the temperature and pressure ranges of 273.4～279.4 K and 3.60～11.90 MPa, respectively. The dimensionless Gibbs free energy difference （-△G^exp/RT） was used as the driving force to correlate the experimental data and a model involving parameters of physical significance for hydrate film growth kinetics was proposed. The reaction order （n = 1.60）, apparent activation energy （55.95 kJ·mol^-1） and pre-exponential factor （1.65×10^11 mm^2·s^-1） of methane hydrate film growth kinetics was regressed. Meanwhile the influences of temperature and pressure upon the film growth rate of methane hydrate were also discussed.