Abstract
Using the CO2 replacement method to exploit natural gas hydrates and store CO2 has great significance in energy access and environmental protection. Herein, the molecular dynamic method is utilized to analyze and evaluate the CH4-CO2 replacement at different constant temperatures and pressures. For optimization, various temperature oscillations are introduced in the CH4-CO2 replacement. It illustrates that increasing the temperature can improve the amounts of CH4 escape and CO2 capture but is unfavorable to the long-term CO2 storage and hydrate stability. The effects of pressure are not as significant and definite as those of temperature. Appropriate temperature oscillations can achieve comprehensive improvements, which benefit from both the deep diffusion of CO2 in the higher temperature stage and the rapid rebuilding of CO2 hydrate within just nanoseconds caused by the memory effects in the lower temperature stage. The results also reveal that the optimal lower temperature duration and frequency should be moderate. Decreasing the lower temperature value can distinctly enhance CO2 capture and hydrate stability. This study can help understand the mechanisms of CH4-CO2 replacement under different temperature and pressure conditions, especially at temperature transitions, and proposes a potentially effective method to achieve large-scale carbon sequestration in the hydrate.
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