Occurrence State and Controlling Factors of Methane in Deep Marine Shale: A Case Study from Silurian Longmaxi Formation in Sichuan Basin, SW China

Deep marine shale is the primary carrier of shale gas resources in Southwestern China. Because the occurrence and gas content of methane vary with burial conditions, understanding the microscopic mechanism of methane occurrence in deep marine shale is critical for effective shale gas exploitation. The temperature and pressure conditions in deep shale exceed the operating limits of experimental equipment; thus, few studies have discussed the microscopic occurrence mechanism of shale gas in deep marine shale. This study applies molecular simulation technology to reveal the methane’s microscopic occurrence mechanism, particularly the main controlling factor of adsorbed methane in deep marine shale. Two types of simulation models are also proposed. The Grand Canonical Monte Carlo (GCMC) method is used to simulate the adsorption behavior of methane molecules in these two models. The results indicate that the isosteric adsorption heat of methane in both models is below 42 kJ/mol, suggesting that methane adsorption in deep shale is physical adsorption. Adsorbed methane concentrates on the pore wall surface and forms a double-layer adsorption. Furthermore, adsorbed methane can transition to single-layer adsorption if the pore size is less than 1.6 nm. The total adsorption capacity increases with rising pressure, although the growth rate decreases. Excess adsorption capacity is highly sensitive to pressure and can become negative at high pressures. Methane adsorption capacity is determined by pore size and adsorption potential, while accommodation space and adsorption potential are influenced by pore size and mineral type. Under deep marine shale reservoir burial conditions, with burial depth deepening, the effect of temperature on shale gas occurrence is weaker than pressure. Higher temperatures inhibit shale gas occurrence, and high pressure enhances shale gas preservation. Smaller pores facilitate the occurrence of adsorbed methane, and larger pores have larger total methane adsorption capacity. Deep marine shale with high formation pressure and high clay mineral content is conducive to the microscopic accumulation of shale gas in deep marine shale reservoirs. This study discusses the microscopic occurrence state of deep marine shale gas and provides a reference for the exploration and development of deep shale gas.