Selective adsorption of supercritical carbon dioxide and methane binary mixture in shale kerogen nanopores

The adsorption of carbon dioxide and methane binary mixture in shale kerogen nanopores and the underlying mechanism significantly affect the supercritical carbon dioxide enhanced shale gas development project. In this study, we investigated the adsorption properties of carbon dioxide and methane in shale kerogen using grand canonical Monte Carlo (GCMC) method. Shale kerogen was fabricated based on Ungerer molecular model and its parameters were validated. The effects of temperature, pressure, mole fraction on the adsorption isotherms, average isosteric heat, potential energy distribution, and adsorption selectivity of binary mixture were discussed. The results show that the absolute adsorption capacity of methane in binary mixture decreases as temperature increases, but increases as mole fraction increases. Compared with methane, carbon dioxide is in lower energy absorption sites, which indicates the adsorption capacity of carbon dioxide in shale kerogen is stronger than that of methane. The adsorption selectivity of carbon dioxide over methane first decreases as pressure increases until pressure reaches critical pressure (7.38 MPa for carbon dioxide), and then stays at around 3.8 as pressure continues to rise. Adsorption selectivity and desorption quantity are used to reveal that the optimal injection depth for supercritical carbon dioxide enhanced shale gas development project is 1000-2500 m. This study will reveal the mechanism of the adsorption of methane in kerogen and provide some fundamental data for supercritical carbon dioxide enhanced shale gas development project.