Two methods, rapidly depressurizing to 0.1 MPa at a constant temperature and rising temperature under equilibrium P, T conditions, were used to study the dissociation of pure CH4 hydrate formed below the ice point. At...Two methods, rapidly depressurizing to 0.1 MPa at a constant temperature and rising temperature under equilibrium P, T conditions, were used to study the dissociation of pure CH4 hydrate formed below the ice point. At a constant temperature with rapidly depressurizing to 0.1 MPa, CH4 hydrate dissociated rapidly at initial dissociation and then the dissociation rate gradually decreased. However, the dissociation of CH4 hydrate at temperatures of 261 to 266 K was much faster than that at temperatures of 269 to 272 K, indicating its anomalous preservation. Under an equilibrium P, T conditions, rising temperature had extensively controlling impact on dissociation of CH4 hydrate at equilibrium pressures of 2.31, 2.16 and 1.96 MPa. In this study, we report the effect of pressure on CH4 hydrate dissociation, especially the effect of equilibrium pressure on dissociation at various melting temperatures. And we find that the ice particles size of CH4 hydrate formed may dominant the CH4 hydrate dissociation. Dissociation of CH4 hydrate formed from ice particles of smaller than 250 μm may not have an anomalous preservation below the ice point, while particles larger than 250 μm may have more extensive anomalous preservation.展开更多
The replacement process of CH4 from CH4 hydrate formed in NaCl solution by using pressurized CO2 was investigated with a self-designed device at temperatures of 271.05, 273.15 and 275.05 K and a constant pressure of 3...The replacement process of CH4 from CH4 hydrate formed in NaCl solution by using pressurized CO2 was investigated with a self-designed device at temperatures of 271.05, 273.15 and 275.05 K and a constant pressure of 3.30 MPa. The mass fraction of the NaCl solution was either 0.5 wt% or 1.0 wt%. The effects of temperature and concentration of NaCl solution on the replacement process were investigated. Experimental results showed that high temperature was favorable to the replacement reaction but high NaCl concentration had a negative effect on the replacement process. Based on the experimental data, kinetic models of CH4 hydrate decomposition and CO2 hydrate formation in NaCl solution were established. The calculated activation energies suggested that both CH4 hydrate decomposition and CO2 hydrate formation are dominated by diffusion in the hydrate phase.展开更多
Termodynamic data on methane hydrate formation in the presence of ammonia are very important for upgrading of ammonia synthesis vent gas using hydrate formation. This paper is focused on the formation conditions of me...Termodynamic data on methane hydrate formation in the presence of ammonia are very important for upgrading of ammonia synthesis vent gas using hydrate formation. This paper is focused on the formation conditions of methane hydrate in the presence of ammonia and the effects of gas-liquid ratio and temperature on the separation of vent gas by hydrate formation. Equilibrium data for methane hydrate within an ammonia mole concentration range from 1% to 5 % were obtained. The experimental results indicated that ammonia has an inhibitive effect on hydrate formation. The higher the ammonia concentration, the higher is the pressure reguired for methane hydrate formation would be. The primary experimental results showed that when volume ratio of gas to liquid was 80:1 and temperature was 283.15 K, total mole fraction of (H2+N2) in gas phase could reach 96.9 %.展开更多
In addition to the temperature and pressure conditions,the pore fluid composition and migration behavior are also crucial to control hydrate decomposition in the exploitation process.In this work,to investigate the ef...In addition to the temperature and pressure conditions,the pore fluid composition and migration behavior are also crucial to control hydrate decomposition in the exploitation process.In this work,to investigate the effects of these factors,a series of depressurization experiments were carried out in a visible one-dimensional reactor,using hydrate reservoir samples with water saturations ranging from 20%to 65%.The results showed a linear relationship between gas production rates and gas saturations of the reservoir,suggesting that a larger gas-phase space was conducive to hydrate decomposition and gas outflow.Therefore,the rapid water production in the early stage of hydrate exploitation could release more gas-phase space in the water-rich reservoir,which in turn improved the gas production efficiency.Meanwhile,the spatiotemporal evolution of pore fluids could lead to partial accelerated decomposition or secondary formation of hydrates.In the unsealed reservoir,the peripheral water infiltration kept reservoir at a high water saturation,which hindered the overall production process and caused higher water production.Importantly,depressurization assisted with the N2 sweep could displace the pore water rapidly.According to the results,it is recommended that using the short-term N2 sweep as an auxiliary means in the early stage of depressurization to expand the gas-phase space in order to achieve the highest production efficiency.展开更多
基金supported by the Key Projector of Chinese Academy of Science (No. KZCX-YW-330)the National Science Fund Fostering Talents in Basic Research to Glaciology and Geocryology (Grant No. J0630966)
文摘Two methods, rapidly depressurizing to 0.1 MPa at a constant temperature and rising temperature under equilibrium P, T conditions, were used to study the dissociation of pure CH4 hydrate formed below the ice point. At a constant temperature with rapidly depressurizing to 0.1 MPa, CH4 hydrate dissociated rapidly at initial dissociation and then the dissociation rate gradually decreased. However, the dissociation of CH4 hydrate at temperatures of 261 to 266 K was much faster than that at temperatures of 269 to 272 K, indicating its anomalous preservation. Under an equilibrium P, T conditions, rising temperature had extensively controlling impact on dissociation of CH4 hydrate at equilibrium pressures of 2.31, 2.16 and 1.96 MPa. In this study, we report the effect of pressure on CH4 hydrate dissociation, especially the effect of equilibrium pressure on dissociation at various melting temperatures. And we find that the ice particles size of CH4 hydrate formed may dominant the CH4 hydrate dissociation. Dissociation of CH4 hydrate formed from ice particles of smaller than 250 μm may not have an anomalous preservation below the ice point, while particles larger than 250 μm may have more extensive anomalous preservation.
基金support received from the National Natural Science Foundation of China (20476058,20676146)Ministry of Science and Technology of China (2006AA09A208,2009CB219504)Specialized Research Fund for the Doctoral Program of Higher Education (20070425001)
文摘The replacement process of CH4 from CH4 hydrate formed in NaCl solution by using pressurized CO2 was investigated with a self-designed device at temperatures of 271.05, 273.15 and 275.05 K and a constant pressure of 3.30 MPa. The mass fraction of the NaCl solution was either 0.5 wt% or 1.0 wt%. The effects of temperature and concentration of NaCl solution on the replacement process were investigated. Experimental results showed that high temperature was favorable to the replacement reaction but high NaCl concentration had a negative effect on the replacement process. Based on the experimental data, kinetic models of CH4 hydrate decomposition and CO2 hydrate formation in NaCl solution were established. The calculated activation energies suggested that both CH4 hydrate decomposition and CO2 hydrate formation are dominated by diffusion in the hydrate phase.
基金support received from the National Natural Science Foundation of China (20476058, 20676146)Ministry of Science and Technology of China (2006AA09A208, 2009CB219504)Specialized Research Fund for the Doctoral Program of Higher Education (20070425001) aregratefully acknowledged
文摘Termodynamic data on methane hydrate formation in the presence of ammonia are very important for upgrading of ammonia synthesis vent gas using hydrate formation. This paper is focused on the formation conditions of methane hydrate in the presence of ammonia and the effects of gas-liquid ratio and temperature on the separation of vent gas by hydrate formation. Equilibrium data for methane hydrate within an ammonia mole concentration range from 1% to 5 % were obtained. The experimental results indicated that ammonia has an inhibitive effect on hydrate formation. The higher the ammonia concentration, the higher is the pressure reguired for methane hydrate formation would be. The primary experimental results showed that when volume ratio of gas to liquid was 80:1 and temperature was 283.15 K, total mole fraction of (H2+N2) in gas phase could reach 96.9 %.
基金financially supported by the National Natural Science Foundation of China,China(Nos.52004136,22127812,U20B6005)China Postdoctoral Science Foundation,China(Nos.2020M670347,2021T140382)Guangdong MEPP Fund(No.GDNRC[2021]055).
文摘In addition to the temperature and pressure conditions,the pore fluid composition and migration behavior are also crucial to control hydrate decomposition in the exploitation process.In this work,to investigate the effects of these factors,a series of depressurization experiments were carried out in a visible one-dimensional reactor,using hydrate reservoir samples with water saturations ranging from 20%to 65%.The results showed a linear relationship between gas production rates and gas saturations of the reservoir,suggesting that a larger gas-phase space was conducive to hydrate decomposition and gas outflow.Therefore,the rapid water production in the early stage of hydrate exploitation could release more gas-phase space in the water-rich reservoir,which in turn improved the gas production efficiency.Meanwhile,the spatiotemporal evolution of pore fluids could lead to partial accelerated decomposition or secondary formation of hydrates.In the unsealed reservoir,the peripheral water infiltration kept reservoir at a high water saturation,which hindered the overall production process and caused higher water production.Importantly,depressurization assisted with the N2 sweep could displace the pore water rapidly.According to the results,it is recommended that using the short-term N2 sweep as an auxiliary means in the early stage of depressurization to expand the gas-phase space in order to achieve the highest production efficiency.