Supercritical carbon dioxide enhanced natural gas recovery from kerogen micropores

Abstract

As the global energy demand increases, a sustainable and environmentally friendly methane (CH4) extraction technique must be developed to assist in the transition off of fossil fuels. In recent years, supercritical carbon dioxide (CO2) has been poised as a candidate for enhanced gas recovery (EGR) from CH4-rich source rocks, potentially with the reservoir serving as a carbon sink for CO2. However, the underlying molecular-scale mechanisms of CO2-EGR processes are still poorly understood. Using constant chemical potential molecular dynamics (CμMD), this study investigates the CH4 recovery process via supercritical CO2 injection into immature (Type I-A) and overmature (Type II-D) kerogens in real-time and at reservoir conditions (365 K and 275 bar). A pseudo-second order (PSO) rate law was used to quantify the adsorption and desorption kinetics of CO2 and CH4. The kinetics of simultaneous adsorption/desorption are rapid in immature kerogen due to better connected pore volume facilitating fluid diffusion, whereas in overmature kerogen, the structural heterogeneity hinders fluid diffusion. Estimated second order kinetic rate coefficients reveal that CO2 adsorption and CH4 desorption in Type I-A are about two times and an order of magnitude faster, respectively, compared to those of in Type II-D. Furthermore, overmature Type II-D kerogen contains inaccessible micropores which prevent full recovery of CH4. For every CH4 molecule replaced, at least two and six CO2 molecules are adsorbed in Type-II-D and Type I-A kerogens, respectively. Overall, this study shows that CO2 injection can achieve 90 % and 65 % CH4 recovery in Type I-A and Type II-D kerogens, respectively.