Abstract: To obtain the fundamental data of CO₂/N₂ gas mixture hydrate formation kinetics and CO₂ separation and sequestration mechanisms, the gas hydrate formation process by a binary CO₂/N₂ gas mixture (50:50) in fine sediments (150-250 μm) was investigated in a semibatch vessel at variable temperatures(273, 275, and 277 K)and pressures (5.8-7.8 MPa). During the gas hydrate reaction process, the changes in the gaseous phase composition were determined by gas chromatography. The results indicate that the gas hydrate formation process of the binary CO₂/N₂ gas mixture in fine sediments can be reduced to two stages. Firstly, the dissolved gas containing a large amount of CO₂ formed gas hydrates, and then gaseous N₂ participated in the gas hydrate formation. In the second stage, all the dissolved gas was consumed. Thus, both gaseous CO₂ and N₂ diffused into sediment. The first stage in different experiments lasted for 5-15 h, and >60% of the gas was consumed in this period. The gas consumption rate was greater in the first stage than in the second stage. After the completion of gas hydrate formation, the CO₂ content in the gas hydrate was more than that in the gas phase. This indicates that CO₂ formed hydrate easily than N₂ in the binary mixture. Higher operating pressures and lower temperatures increased the gas consumption rate of the binary gas mixture in gas hydrate formation.

Key words: Gas hydrate, Formation, Sediments, CO₂/N₂ mixture

摘要： To obtain the fundamental data of CO₂/N₂ gas mixture hydrate formation kinetics and CO₂ separation and sequestration mechanisms, the gas hydrate formation process by a binary CO₂/N₂ gas mixture (50:50) in fine sediments (150-250 μm) was investigated in a semibatch vessel at variable temperatures(273, 275, and 277 K)and pressures (5.8-7.8 MPa). During the gas hydrate reaction process, the changes in the gaseous phase composition were determined by gas chromatography. The results indicate that the gas hydrate formation process of the binary CO₂/N₂ gas mixture in fine sediments can be reduced to two stages. Firstly, the dissolved gas containing a large amount of CO₂ formed gas hydrates, and then gaseous N₂ participated in the gas hydrate formation. In the second stage, all the dissolved gas was consumed. Thus, both gaseous CO₂ and N₂ diffused into sediment. The first stage in different experiments lasted for 5-15 h, and >60% of the gas was consumed in this period. The gas consumption rate was greater in the first stage than in the second stage. After the completion of gas hydrate formation, the CO₂ content in the gas hydrate was more than that in the gas phase. This indicates that CO₂ formed hydrate easily than N₂ in the binary mixture. Higher operating pressures and lower temperatures increased the gas consumption rate of the binary gas mixture in gas hydrate formation.

关键词: Gas hydrate, Formation, Sediments, CO₂/N₂ mixture